Traffic is a major source of atmospheric nanocluster aerosol

PubMed Central

Kuuluvainen, Heino; Karjalainen, Panu; Keskinen, Jorma; Hillamo, Risto; Niemi, Jarkko V.; Pirjola, Liisa; Timonen, Hilkka J.; Saarikoski, Sanna; Saukko, Erkka; Järvinen, Anssi; Silvennoinen, Henna; Rostedt, Antti; Olin, Miska; Yli-Ojanperä, Jaakko; Nousiainen, Pekka; Kousa, Anu; Dal Maso, Miikka

2017-01-01

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3–3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20–54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)−1 in a roadside environment, 2.6·1015 (kgfuel)−1 in a street canyon, and 2.9·1015 (kgfuel)−1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)−1 to a high value of 4.3·1015 (kgfuel)−1. These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds. PMID:28674021

Traffic is a major source of atmospheric nanocluster aerosol.

PubMed

Rönkkö, Topi; Kuuluvainen, Heino; Karjalainen, Panu; Keskinen, Jorma; Hillamo, Risto; Niemi, Jarkko V; Pirjola, Liisa; Timonen, Hilkka J; Saarikoski, Sanna; Saukko, Erkka; Järvinen, Anssi; Silvennoinen, Henna; Rostedt, Antti; Olin, Miska; Yli-Ojanperä, Jaakko; Nousiainen, Pekka; Kousa, Anu; Dal Maso, Miikka

2017-07-18

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·10 15 (kg fuel ) -1 in a roadside environment, 2.6·10 15 (kg fuel ) -1 in a street canyon, and 2.9·10 15 (kg fuel ) -1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·10 12 (kg fuel ) -1 to a high value of 4.3·10 15 (kg fuel ) -1 These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Micro-scale variability of particulate matter and the influence of urban fabric on the aerosol distribution in two mid-sized German cities

NASA Astrophysics Data System (ADS)

Paas, Bastian; Schneider, Christoph

2016-04-01

Spatial micro-scale variability of particle mass concentrations is an important criterion for urban air quality assessment. The major proportion of the world's population lives in cities, where exceedances of air quality standards occur regularly. Current research suggests that both long-term and even short-term stays, e.g. during commuting or relaxing, at locations with high PM concentrations could have significant impacts on health. In this study we present results from model calculations in comparison to high resolution spatial and temporal measurements. Airborne particles were sampled using an optical particle counter in two inner-city park areas in Aachen and Munster. Both are mid-sized German cities which, however, are characterized by a different topology. The measurement locations represent spots with different degrees of outdoor particle exposure that can be experienced by a pedestrian walking in an intra-urban recreational area. Simulations of aerosol distributions induced by road traffic were conducted using both the German reference dispersion model Austal2000 and the numerical microclimate model ENVI-met. Simulation results reveal details in the distribution of urban particles with highest concentrations of PM10 in direct vicinity to traffic lines. The corresponding concentrations rapidly decline as the distances to the line sources increase. Still, urban fabric and obstacles like shrubs or trees are proved to have a major impact on the aerosol distribution in the area. Furthermore, the distribution of particles was highly dependent of wind direction and turbulence characteristics. The analysis of observational data leads to the hypothesis that besides motor traffic numerous diffuse particle sources e.g. on the ability of surfaces to release particles by resuspension which were dominantly apparent in measured PM(1;10) and PM(0.25;10) data are present in the urban roughness layer. The results highlight that a conclusive picture concerning micro-scale patterns of PM helps to understand the effects of urban fabric and obstacles of both natural and artificial origin (e.g. street furniture, vegetation elements and buildings) on the local patterns of aerosol distribution. Simulation results with Austal2000 and ENVI-met indicate that there is potential to support urban planners in designing urban infrastructure and open spaces with reduced local particle concentrations through modelling. This approach seemingly is i.e. relevant for inner-city recreational areas.

Aerosol removal due to precipitation and wind forcings in Milan urban area

NASA Astrophysics Data System (ADS)

Cugerone, Katia; De Michele, Carlo; Ghezzi, Antonio; Gianelle, Vorne

2018-01-01

Air pollution represents a critical issue in Milan urban area (Northern Italy). Here, the levels of fine particles increase, overcoming the legal limits, mostly in wintertime, due to favourable calm weather conditions and large heating and vehicular traffic emissions. The main goal of this work is to quantify the aerosol removal effect due to precipitation at the ground. At first, the scavenging coefficients have been calculated for aerosol particles with diameter between 0.25 and 3 μm. The average values of this coefficient vary between 2 ×10-5 and 5 ×10-5 s-1. Then, the aerosol removal induced separately by precipitation and wind have been compared through the introduction of a removal index. As a matter of fact, while precipitation leads to a proper wet scavenging of the particles from the atmosphere, high wind speeds cause enhanced particle dispersion and dilution, that locally bring to a tangible decrease of aerosol particles' number. The removal triggered by these two forcings showed comparable average values, but different trends. The removal efficiency of precipitation lightly increases with the increase of particle diameters and vice versa happens with strong winds.

Substantial convection and precipitation enhancements by ultrafine aerosol particles

NASA Astrophysics Data System (ADS)

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei; Giangrande, Scott E.; Li, Zhanqing; Machado, Luiz A. T.; Martin, Scot T.; Yang, Yan; Wang, Jian; Artaxo, Paulo; Barbosa, Henrique M. J.; Braga, Ramon C.; Comstock, Jennifer M.; Feng, Zhe; Gao, Wenhua; Gomes, Helber B.; Mei, Fan; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; de Souza, Rodrigo A. F.

2018-01-01

Ultrafine aerosol particles (smaller than 50 nanometers in diameter) have been thought to be too small to affect cloud formation. Fan et al. show that this is not the case. They studied the effect of urban pollution transported into the otherwise nearly pristine atmosphere of the Amazon. Condensational growth of water droplets around the tiny particles releases latent heat, thereby intensifying atmospheric convection. Thus, anthropogenic ultrafine aerosol particles may exert a more important influence on cloud formation processes than previously believed.

Effective density and mixing state of aerosol particles in a near-traffic urban environment.

PubMed

Rissler, Jenny; Nordin, Erik Z; Eriksson, Axel C; Nilsson, Patrik T; Frosch, Mia; Sporre, Moa K; Wierzbicka, Aneta; Svenningsson, Birgitta; Löndahl, Jakob; Messing, Maria E; Sjogren, Staffan; Hemmingsen, Jette G; Loft, Steffen; Pagels, Joakim H; Swietlicki, Erik

2014-06-03

In urban environments, airborne particles are continuously emitted, followed by atmospheric aging. Also, particles emitted elsewhere, transported by winds, contribute to the urban aerosol. We studied the effective density (mass-mobility relationship) and mixing state with respect to the density of particles in central Copenhagen, in wintertime. The results are related to particle origin, morphology, and aging. Using a differential mobility analyzer-aerosol particle mass analyzer (DMA-APM), we determined that particles in the diameter range of 50-400 nm were of two groups: porous soot aggregates and more dense particles. Both groups were present at each size in varying proportions. Two types of temporal variability in the relative number fraction of the two groups were found: soot correlated with intense traffic in a diel pattern and dense particles increased during episodes with long-range transport from polluted continental areas. The effective density of each group was relatively stable over time, especially of the soot aggregates, which had effective densities similar to those observed in laboratory studies of fresh diesel exhaust emissions. When heated to 300 °C, the soot aggregate volatile mass fraction was ∼10%. For the dense particles, the volatile mass fraction varied from ∼80% to nearly 100%.

The Effect of Particle Composition on Hygroscopicity and Droplet Formation at CARES

NASA Astrophysics Data System (ADS)

Cziczo, D. J.; Pekour, M. S.; Hiranuma, N.; Nelson, D.

2010-12-01

During the June, 2010 Carbonaceous Aerosol and Radiative Effects Study (CARES) a custom made humidity controlled nephelometer, hereafter termed a ‘humidograph’, was deployed with a commercial cloud condensation nucleus counter (CCNC) and the particle analysis by laser mass spectrometry (PALMS) instrument. Other ancillary measurements, such as particle size distributions, were made continuously during the month. The CARES field study took place in the Sacramento, CA area. Early June was characterized by cool, wet weather with predominantly northerly flow and very low particle loading. Very little biomass burning took place and the aerosol was largely sulfate neutralized by ammonia. Later in the month a more typical flow pattern from the Sacramento urban area toward the foothills developed. During this period more biomass burning occurred and organics from anthropogenic and urban sources were present on particles. The aforementioned instruments were located in the town of Cool, CA in the Sierra foothills, approximately 50 kilometers north east of cool. This site was chosen as being on the typical summertime daily flow some hours downstream of the Sacramento urban plume. Using these instruments we were able to correlate water uptake and droplet formation with particle composition. The early period of CARES was characterized by a clear deliquescence of the aerosol at ~80% relative humidity which correlated with an ammonium neutralized sulfate aerosol composition. Few CCN were present although these activated at low supersaturations and represented a large fraction of the total aerosol over ~70 nanometers in diameter. Later in the month deliquescence was not clearly indicated for a more organic-rich and biomass burning influenced aerosol. More CCN were present although activation generally required much higher saturations.

Fluxes of Submicron Organic Aerosol above London Measured by Eddy Covariance using the Aerodyne HR-ToF-AMS

NASA Astrophysics Data System (ADS)

Phillips, G. J.; di Marco, C. F.; Farmer, D.; Kimmel, J. R.; Jimenez, J. L.; Nemitz, E.

2009-12-01

Urban centres are large sources of sub-micron particles. The myriad of emission sources combined with the complex interaction between regional aerosol and the particulate and gaseous photochemistry make for a complex system. It is evident that particulate emissions from cities will affect the regional atmosphere as well as the environment within the urban area. Aerosol particles have been associated with respiratory and cardio-vascular disease and are also linked with the climate through scattering of radiation and indirect effects such as cloud formation. The Aerodyne Aerosol Mass Spectrometer (AMS) provides a powerful tool to elucidate the sources and processing of organic aerosol in the urban atmosphere. Normally this is done through concentration measurements, by statistical analysis of the organic mass spectra, e.g. using Positive Matrix Factorization (PMF). Recently the quadrupole based AMS (Q-AMS) has been used for the micrometeorological measurement of organic aerosol fluxes above several cities, based on high frequency measurements of individual masses (m/z) representative of different organic mass fractions. While providing a major step forward towards quantification of urban organic aerosol emissions and processing, the interpretation of Q-AMS flux data requires assumptions to scale up signals on individual m/z to total organic mass fluxes. In this paper we present chemically-speciated and size-segregated number aerosol fluxes measured using the next generation eddy covariance flux system based on the Aerodyne HR-ToF-AMS, now capable of recording fast-response eddy-covariance time-series of all m/z simultaneously. This allows organic mass fluxes to be calculated more quantitatively and provides 'flux mass spectra' in addition to concentration mass spectra, which produces novel information on the local emission and processing of organic aerosols in the urban environment, while concentration analysis includes the regional background. The measurements were made from the 190 m tall BT Tower in central London, UK, during the REPARTEE-2/CityFlux experiment in autumn 2007 and are interpreted in conjunction with simultaneous measurements of fluxes of CO and CO2 as well as size-segregated particle number fluxes between 60 and 1000 nm using an ultra-high sensitivity aerosol spectrometer, UHSAS (Particle Measurement Systems, now Droplet Measurement Technologies, Boulder, US).

Optoacoustic Spectroscopy to Detect Hydrazine Fuels.

DTIC Science & Technology

1981-07-01

signals in noise. Proc IEEE 58:610 (1970). 303. Rosen, H., A. D. Hansen, L. Gundel, and T. Novakov . Photoacoustic investigation of urban aerosol...Appl Phys 40:5404 (1969). 383. Yasa, Z., N. M. Amer, H. Rosen, A. D. Hansen, and T. Novakov . Photoacous- tic investigation of urban aerosol particles

Cloud residues and interstitial aerosols from non-precipitating clouds over an industrial and urban area in northern China

NASA Astrophysics Data System (ADS)

Li, Weijun; Li, Peiren; Sun, Guode; Zhou, Shengzhen; Yuan, Qi; Wang, Wenxing

2011-05-01

Most studies of aerosol-cloud interactions have been conducted in remote locations; few have investigated the characterization of cloud condensation nuclei (CCN) over highly polluted urban and industrial areas. The present work, based on samples collected at Mt. Tai, a site in northern China affected by nearby urban and industrial air pollutant emissions, illuminates CCN properties in a polluted atmosphere. High-resolution transmission electron microscopy (TEM) was used to obtain the size, composition, and mixing state of individual cloud residues and interstitial aerosols. Most of the cloud residues displayed distinct rims which were found to consist of soluble organic matter (OM). Nearly all (91.7%) cloud residues were attributed to sulfate-related salts (the remainder was mostly coarse crustal dust particles with nitrate coatings). Half the salt particles were internally mixed with two or more refractory particles (e.g., soot, fly ash, crustal dust, CaSO 4, and OM). A comparison between cloud residues and interstitial particles shows that the former contained more salts and were of larger particle size than the latter. In addition, a somewhat high number scavenging ratio of 0.54 was observed during cloud formation. Therefore, the mixtures of salts with OMs account for most of the cloud-nucleating ability of the entire aerosol population in the polluted air of northern China. We advocate that both size and composition - the two influential, controlling factors for aerosol activation - should be built into all regional climate models of China.

Local and regional components of aerosol in a heavily trafficked street canyon in central London derived from PMF and cluster analysis of single-particle ATOFMS spectra.

PubMed

Giorio, Chiara; Tapparo, Andrea; Dall'Osto, Manuel; Beddows, David C S; Esser-Gietl, Johanna K; Healy, Robert M; Harrison, Roy M

2015-03-17

Positive matrix factorization (PMF) has been applied to single particle ATOFMS spectra collected on a six lane heavily trafficked road in central London (Marylebone Road), which well represents an urban street canyon. PMF analysis successfully extracted 11 factors from mass spectra of about 700,000 particles as a complement to information on particle types (from K-means cluster analysis). The factors were associated with specific sources and represent the contribution of different traffic related components (i.e., lubricating oils, fresh elemental carbon, organonitrogen and aromatic compounds), secondary aerosol locally produced (i.e., nitrate, oxidized organic aerosol and oxidized organonitrogen compounds), urban background together with regional transport (aged elemental carbon and ammonium) and fresh sea spray. An important result from this study is the evidence that rapid chemical processes occur in the street canyon with production of secondary particles from road traffic emissions. These locally generated particles, together with aging processes, dramatically affected aerosol composition producing internally mixed particles. These processes may become important with stagnant air conditions and in countries where gasoline vehicles are predominant and need to be considered when quantifying the impact of traffic emissions.

FDATMOS16 non-linear partitioning and organic volatility distributions in urban aerosols

DOE PAGES

Madronich, Sasha; Kleinman, Larry; Conley, Andrew; ...

2015-12-17

Gas-to-particle partitioning of organic aerosols (OA) is represented in most models by Raoult’s law, and depends on the existing mass of particles into which organic gases can dissolve. This raises the possibility of non-linear response of particle-phase OA to the emissions of precursor volatile organic compounds (VOCs) that contribute to this partitioning mass. Implications for air quality management are evident: A strong non-linear dependence would suggest that reductions in VOC emission would have a more-than-proportionate benefit in lowering ambient OA concentrations. Chamber measurements on simple VOC mixtures generally confirm the non-linear scaling between OA and VOCs, usually stated as amore » mass-dependence of the measured OA yields. However, for realistic ambient conditions including urban settings, no single component dominates the composition of the organic particles, and deviations from linearity are presumed to be small. Here we re-examine the linearity question using volatility spectra from several sources: (1) chamber studies of selected aerosols, (2) volatility inferred for aerosols sampled in two megacities, Mexico City and Paris, and (3) an explicit chemistry model (GECKO-A). These few available volatility distributions suggest that urban OA may be only slightly super-linear, with most values of the sensitivity exponent in the range 1.1-1.3, also substantially lower than seen in chambers for some specific aerosols. Furthermore, the rather low values suggest that OA concentrations in megacities are not an inevitable convergence of non-linear effects, but can be addressed (much like in smaller urban areas) by proportionate reductions in emissions.« less

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

NASA Astrophysics Data System (ADS)

Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

Rapid Measurements of Aerosol Ionic Composition and 3-10 nm Particle Size Distributions On The NASA P3 To Better Quantify Processes Affecting Aerosols Advected From East Asia

NASA Technical Reports Server (NTRS)

Weber, Rodney J.

2004-01-01

The Particle Into Liquid Sample (PILS) was deployed on the NASA P3 for airborne measurements of fine particle ionic chemical composition. The data have been quality assured and reside in the NASA data archive. We have analyzed our data to characterize the sources and atmospheric processing of fine aerosol particles advected from the region during the experiments. Fine particle water-soluble potassium was found to serve as a useful aerosol tracer for biomass smoke. Ratios of PILS potassium to sulfate are used as a means of estimating the percent contribution of biomass burning to fine particle mass in mixed plumes advecting from Asia. The high correlations between K+ and NO3(sup -) and NH4(sup +)' indicated that biomass burning was a significant source of these aerosol compounds in the region. It is noteworthy that the air mass containing the highest concentrations of fine particles recorded in all of ACE-Asia and TRACE-P appeared to be advecting from the Bejing/Tientsin urban region and also had the highest K(+), NO3(sup -) and NH4(sup +) concentrations of both studies. Based on K+/SO4(sup 2-) ratio's, we estimated that the plume was composed of approx. 60% biomass burning emissions, possibly from the use of bio-fuels in the urban regions.

Statistical analysis and parameterization of the hygroscopic growth of the sub-micrometer urban background aerosol in Beijing

NASA Astrophysics Data System (ADS)

Wang, Yu; Wu, Zhijun; Ma, Nan; Wu, Yusheng; Zeng, Limin; Zhao, Chunsheng; Wiedensohler, Alfred

2018-02-01

The take-up of water of aerosol particles plays an important role in heavy haze formation over North China Plain, since it is related with particle mass concentration, visibility degradation, and particle chemistry. In the present study, we investigated the size-resolved hygroscopic growth factor (HGF) of sub-micrometer aerosol particles (smaller than 350 nm) on a basis of 9-month Hygroscopicity-Tandem Differential Mobility Analyzer measurement in the urban background atmosphere of Beijing. The mean hygroscopicity parameter (κ) values derived from averaging over the entire sampling period for particles of 50 nm, 75 nm, 100 nm, 150 nm, 250 nm, and 350 nm in diameters were 0.14 ± 0.07, 0.17 ± 0.05, 0.18 ± 0.06, 0.20 ± 0.07, 0.21 ± 0.09, and 0.23 ± 0.12, respectively, indicating the dominance of organics in the sub-micrometer urban aerosols. In the spring, summer, and autumn, the number fraction of hydrophilic particles increased with increasing particle size, resulting in an increasing trend of overall particle hygroscopicity with enhanced particle size. Differently, the overall mean κ values peaked in the range of 75-150 nm and decreased for particles larger than 150 nm in diameter during wintertime. Such size-dependency of κ in winter was related to the strong primary particle emissions from coal combustion during domestic heating period. The number fraction of hydrophobic particles such as freshly emitted soot decreased with increasing PM2.5 mass concentration, indicating aged and internal mixed particles were dominant in the severe particulate matter pollution. Parameterization schemes of the HGF as a function of relative humidity (RH) and particle size between 50 and 350 nm were determined for different seasons and pollution levels. The HGFs calculated from the parameterizations agree well with the measured HGFs at 20-90% RH. The parameterizations can be applied to determine the hygroscopic growth of aerosol particles at ambient conditions for the area of Beijing (ultrafine and fine particles) and the North China plain (fine particles).

Preliminary results of the aerosol optical depth retrieval in Johor, Malaysia

NASA Astrophysics Data System (ADS)

Lim, H. Q.; Kanniah, K. D.; Lau, A. M. S.

2014-02-01

Monitoring of atmospheric aerosols over the urban area is important as tremendous amounts of pollutants are released by industrial activities and heavy traffic flow. Air quality monitoring by satellite observation provides better spatial coverage, however, detailed aerosol properties retrieval remains a challenge. This is due to the limitation of aerosol retrieval algorithm on high reflectance (bright surface) areas. The aim of this study is to retrieve aerosol optical depth over urban areas of Iskandar Malaysia; the main southern development zone in Johor state, using Moderate Resolution Imaging Spectroradiometer (MODIS) 500 m resolution data. One of the important steps is the aerosol optical depth retrieval is to characterise different types of aerosols in the study area. This information will be used to construct a Look Up Table containing the simulated aerosol reflectance and corresponding aerosol optical depth. Thus, in this study we have characterised different aerosol types in the study area using Aerosol Robotic Network (AERONET) data. These data were processed using cluster analysis and the preliminary results show that the area is consisting of coastal urban (65%), polluted urban (27.5%), dust particles (6%) and heavy pollution (1.5%) aerosols.

Aerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines

NASA Astrophysics Data System (ADS)

Kecorius, Simonas; Madueño, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; Müller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, Alfred

2017-12-01

Ultrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors' knowledge, no other studies reported such high number concentration of ultrafine refractory particles under ambient conditions. Inverse modeling of emission factors of refractory particle number size distributions revealed that diesel-fed public utility Jeepneys, commonly used for public transportation, are responsible for 94% of total roadside emitted refractory particle mass. The observed results showed that the majority of urban pollution in Metro Manila is dominated by carbonaceous aerosol. This suggests that PM10 or PM2.5 metrics do not fully describe possible health related effects in this kind of urban environments. Extremely high concentrations of ultrafine particles have been and will continue to induce adverse health related effects, because of their potential toxicity. We imply that in megacities, where the major fraction of particulates originates from the transport sector, PM10 or PM2.5 mass concentration should be complemented by legislative measurements of equivalent black carbon mass concentration.

Analysis of Fine and Coarse mode Aerosol Distributions from AERONET's mini-DRAGON Set-up at Singapore 2012

NASA Astrophysics Data System (ADS)

Salinas Cortijo, S. V.; Chew, B. N.; Muller, A.; Liew, S.

2013-12-01

Aerosol optical depth combined with the Angstrom exponent and its derivative, are often used as a qualitative indicator of aerosol type and particle size regime. In Singapore, the sources of aerosols are mostly from fossil fuel burning (energy stations, incinerators, urban transport etc.) and from industrial and urban areas. However, depending on the time of the year (July-October), there can be a strong bio-mass component originated from uncontrolled forest/plantation fires from the neighboring land masses of Sumatra and Borneo. Unlike urban/fossil fuel aerosols, smoke or bio-mass related aerosol particles are typically characterized by showing a large optical depth and small, sub-micron particle size distributions. Trans-boundary smoke episodes has become an annual phenomenon in this region. Severe episodes were recorded in 1997 and 2006 and other minor episodes happened during 2002, 2004, 2010 and more recently on 2013. On August-September 2012, as part of CRISP participation on the August-September ground campaign of the Southeast Asia Composition, Cloud Climate Coupling Regional Study (SEAC4RS), a Distributed Regional Aerosol Gridded Observation Networks (DRAGON) set of six CIMEL CE-318A automatic Sun-tracking photometers have been deployed at sites located at North (Yishun ITE), East (Temasek Poly), West (NUS and Pandan Reservoir), Central (NEA) and South (St. John's island) of Singapore. In order to fully discriminate bio-mass burning events over other local sources, we perform a spectral discrimination of fine/coarse mode particle regime to all DRAGON sites; subsequently, the fine mode parameters such as optical depth, optical ratio and fine mode Angstrom exponent are used to identify possible bio-mass related events within the data set. Spatio-temporal relationship between sites are also investigated.

Urban organic aerosols measured by single particle mass spectrometry in the megacity of London

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Harrison, R. M.

2011-02-01

During the month of October 2006, as part of the REPARTEE-I experiment (Regent's Park and Tower Environmental Experiment) an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed at an urban background location in the city of London, UK. Fifteen particle types were classified, some of which were accompanied by Aerosol Mass Spectrometer (AMS) quantitative aerosol mass loading measurements (Dall'Osto et al., 2009a, b). In this manuscript the origins and properties of four particle types associated with locally generated aerosols, independent of the air mass type advected into London, are examined. One particle type, originating from lubricating oil (referred to as Ca-EC), was associated with morning rush hour traffic emissions. A second particle type, composed of both inorganic and organic species (called Na-EC-OC), was found enhanced in particle number concentration during evening time periods, and is likely to originate from a source operating at this time of day, or more probably from condensation of semi-volatile species, and contains both primary and secondary components. A third class, internally mixed with organic carbon and sulphate (called OC), was found to spike both in the morning and evenings. The fourth class (SOA-PAH) exhibited maximum frequency during the warmest part of the day, and a number of factors point towards secondary production from traffic-related volatile aromatic compounds. Single particle mass spectra of this particle type showed an oxidized polycyclic aromatic compound signature. Finally, a comparison of ATOFMS particle class data is made with factors obtained by Positive Matrix Factorization from AMS data.. Both the Ca-EC and OC particle types correlate with the AMS HOA primary organic fraction (R2 = 0.65 and 0.50 respectively), and Na-EC-OC, but not SOA-PAH, which correlates weakly with the AMS OOA secondary organic aerosol factor (R2 = 0.35). A detailed analysis was conducted to identify ATOFMS particle type(s) representative of the AMS COA cooking aerosol factor, but no convincing associations were found.

A study of the mixing state of black carbon in urban zone

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Despiau, S.; Putaud, J. P.; Dubovik, O.

2004-02-01

The knowledge of the mixing state of black carbon particle with other aerosol species is critical for adequate simulations of the direct radiative effect of black carbon particles and its effect on climate. This paper reports the investigation of the mixing state of black carbon aerosol in the urban zone. The study uses a combination of in situ and ground-based remote sensing observations conducted during the ESCOMPTE experiment, which took place in industrialized region in France in summer of 2001. The criteria we used for identifying mixing state relies on the known enhancement of absorption for aerosol composed by internal versus external mixtures of black carbon with weakly absorbing aerosol components. First, using in situ aerosol data, we performed Mie computations and reconstructed the single scattering albedo of aerosol for the two different mixing assumptions: black carbon mixed externally or internally with other aerosol species. Then, we compared the obtained values ωo,int and ωo,ext with the retrievals of ωo from independent AERONET Sun-photometric measurements. The aerosol single scattering albedo (ωo,aer.) derived from the AERONET photometer observations (with the mean value equal to 0.84 ± 0.04) was found to be close to ωo,ext reconstructed from in situ observation under assumptions of external mixture. This similarity between AERONET values and external mixture simulations was observed during all the days studied. Our conclusion on external mixture of black carbon aerosol with other particles in urban zone during ESCOMPTE (close to the pollution source) is coherent with observations made during other independent studies reported in a number of recent publications.

Three Dimensional Characterization of Typical Urban and Desert Particles: Implications to Particle Optics

NASA Astrophysics Data System (ADS)

Goel, V.; Mishra, S.; Ahlawat, A. S.; Sharma, C.; Kotnala, R. K.

2017-12-01

Aerosol particles are generally considered as chemically homogeneous spheres in the retrieval techniques of ground and space borne observations which is not accurate approach and can lead to erroneous observations. For better simulation of optical and radiative properties of aerosols, a good knowledge of aerosol's morphology, chemical composition and internal structure is essential. Till date, many studies have reported the morphology and chemical composition of particles but very few of them provide internal structure and spatial distribution of different chemical species within the particle. The research on the effect of particle internal structure and its contribution to particle optics is extremely limited. In present work, we characterize the PM10 particles collected form typical arid (the Thar Desert, Rajasthan, India) and typical urban (New Delhi, India) environment using microscopic techniques. The particles were milled several times to investigate their internal structure. The EDS (Energy Dispersive X-ray Spectroscopy) spectra were recorded after each milling to check the variation in the chemical composition. In arid environment, Fe, Ca, C, Al, and Mg rich shell was observed over a Si rich particle whereas in urban environment, shell of Hg, Ag, C and N was observed over a Cu rich particle. Based on the observations, different model shapes [homogenous sphere and spheroid; heterogeneous sphere and spheroid; core shell] have been considered for assessing the associated uncertainties with the routine modeling of optical properties where volume equivalent homogeneous sphere approximation is considered. The details will be discussed during presentation.

On the spatial distribution and evolution of ultrafine aerosols in urban air

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Alastuey, A.; O'Dowd, C.; Harrison, R. M.; Wenger, J.; Gómez-Moreno, F. J.

2012-07-01

Sources and evolution of ultrafine particles (<0.1 μ m diameter) were investigated both horizontally and vertically in the large urban agglomerate of Barcelona, Spain. Within the SAPUSS project (Solving Aerosol Problems by Using Synergistic Strategies), a large number of instruments was deployed simultaneously at different monitoring sites (road, two urban background, regional background, urban tower 150 μa.s.l., urban background tower site 80 m a.s.l.) during a 4 week period in September-October 2010. Particle number concentrations (N>5nm) are highly correlated with black carbon (BC) at all sites only under strong vehicular traffic influences. By contrast, under clean atmospheric conditions (low condensation sinks, CS) such correlation diverges towards much higher N/BC ratios at all sites, indicating additional sources of particles including secondary production of freshly nucleated particles. This is also evident in the urban background annual mean diurnal trend of N/BC, showing a midday peak in all seasons. Size-resolved aerosol distributions (N10-500) as well as particle number concentrations (N>5nm) allow us to identify two types of nucleation and growth events: a regional type event originating in the whole study region and impacting almost simultaneously the urban city of Barcelona and the surrounding background area; and an urban type which originates only within the city centre but whose growth continues while transported away from the city to the regional background. Furthermore, during these clean air days, higher N are found at tower level than at ground level only in the city centre whereas such a difference is not so pronounced at the remote urban background tower. In other words, this study suggests that the column of air above the city ground level possesses the best compromise between low CS and high vapour source, hence enhancing the concentrations of freshly nucleated particles. By contrast, within stagnant polluted atmospheric conditions, higher N and BC concentrations are always measured at ground level relative to tower level at all sites. Our study suggests that the city centre is a source of both non-volatile traffic primary (29-39%) and secondary freshly nucleated particles (up to 61-71%) at all sites. We suggest that organic compounds evaporating from freshly emitted traffic particles are a possible candidate for new particle formation within the city and urban plume.

Aerosol physicochemical properties in relation to meteorology: Case studies in urban, marine, and arid settings

NASA Astrophysics Data System (ADS)

Wonaschuetz, Anna

Atmospheric aerosols are a highly relevant component of the climate system affecting atmospheric radiative transfer and the hydrological cycle. As opposed to other key atmospheric constituents with climatic relevance, atmospheric aerosol particles are highly heterogeneous in time and space with respect to their size, concentration, chemical composition and physical properties. Many aspects of their life cycle are not understood, making them difficult to represent in climate models and hard to control as a pollutant. Aerosol-cloud interactions in particular are infamous as a major source of uncertainty in future climate predictions. Field measurements are an important source of information for the modeling community and can lead to a better understanding of chemical and microphysical processes. In this study, field data from urban, marine, and arid settings are analyzed and the impact of meteorological conditions on the evolution of aerosol particles while in the atmosphere is investigated. Particular attention is given to organic aerosols, which are a poorly understood component of atmospheric aerosols. Local wind characteristics, solar radiation, relative humidity and the presence or absence of clouds and fog are found to be crucial factors in the transport and chemical evolution of aerosol particles. Organic aerosols in particular are found to be heavily impacted by processes in the liquid phase (cloud droplets and aerosol water). The reported measurements serve to improve the process-level understanding of aerosol evolution in different environments and to inform the modeling community by providing realistic values for input parameters and validation of model calculations.

Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

NASA Astrophysics Data System (ADS)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

NASA Astrophysics Data System (ADS)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S/C-rich secondary particles) and sea salt (Na/Cl-rich). Tar balls from wood combustion were also observed, especially (∼5%) during the LRT pollution episode.

Characterization of urban aerosol in Cork City (Ireland) using aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ovadnevaite, J.; Ceburnis, D.; Martin, D.; Healy, R. M.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2012-11-01

Ambient wintertime background urban aerosol in Cork City, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the 1 200 000 single particles characterized by an Aerosol Time-Of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally-mixed to different proportions with Elemental Carbon (EC), sulphate and nitrate while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was also characterized using a High Resolution Time-Of-Flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS) and was also found to comprise organic matter as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and then chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix and a five-factor solution was found to describe the variance in the data well. Specifically, "Hydrocarbon-like" Organic Aerosol (HOA) comprised 19% of the mass, "Oxygenated low volatility" Organic Aerosols (LV-OOA) comprised 19%, "Biomass wood Burning" Organic Aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "Peat and Coal" Organic Aerosol (PCOA) comprised 21%, and finally, a species type characterized by primary m/z peaks at 41 and 55, similar to previously-reported "Cooking" Organic Aerosol (COA) but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Despite wood, cool and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosols mass and non refractory PM1, respectively).

Apportionment of urban aerosol sources in Chongqing (China) using synergistic on-line techniques

NASA Astrophysics Data System (ADS)

Chen, Yang; Yang, Fumo

2016-04-01

The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Chongqing (southwestern China) have been determined. Aerosol chemical composition analyses were performed using multiple on-line techniques, such as single particle aerosol mass spectrometer (SPAMS) for single particle chemical composition, on-line elemental carbon-organic carbon analyzer (on-line OC-EC), on-line X-ray fluorescence (XRF) for elements, and in-situ Gas and Aerosol Compositions monitor (IGAC) for water-soluble ions in PM2.5. All the datasets from these techniques have been adjusted to a 1-h time resolution for receptor model input. Positive matrix factorization (PMF) has been used for resolving aerosol sources. At least six sources, including domestic coal burning, biomass burning, dust, traffic, industrial and secondary/aged factors have been resolved and interpreted. The synergistic on-line techniques were helpful for identifying aerosol sources more clearly than when only employing the results from the individual techniques. This results are useful for better understanding of aerosol sources and atmospheric processes.

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

NASA Astrophysics Data System (ADS)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

Contribution of bacteria-like particles to PM2.5 aerosol in urban and rural environments

NASA Astrophysics Data System (ADS)

Wolf, R.; El-Haddad, I.; Slowik, J. G.; Dällenbach, K.; Bruns, E.; Vasilescu, J.; Baltensperger, U.; Prévôt, A. S. H.

2017-07-01

We report highly time-resolved estimates of airborne bacteria-like particle concentrations in ambient aerosol using an Aerodyne aerosol mass spectrometer (AMS). AMS measurements with a newly developed PM2.5 and the standard (PM1) aerodynamic lens were performed at an urban background site (Zurich) and at a rural site (Payerne) in Switzerland. Positive matrix factorization using the multilinear engine (ME-2) implementation was used to estimate the contribution of bacteria-like particles to non-refractory organic aerosol. The success of the method was evaluated by a size-resolved analysis of the organic mass and the analysis of single particle mass spectra, which were detected with a light scattering system integrated into the AMS. Use of the PM2.5 aerodynamic lens increased measured bacteria-like concentrations, supporting the analysis method. However, at all sites, the low concentrations of this component suggest that airborne bacteria constitute a minor fraction of non-refractory PM2.5 organic aerosol mass. Estimated average mass concentrations were below 0.1 μg/m3 and relative contributions were lower than 2% at both sites. During rainfall periods, concentrations of the bacteria-like component increased considerably reaching a short-time maximum of approximately 2 μg/m3 at the Payerne site in summer.

Source apportionment of aerosol particles near a steel plant by electron microscopy.

PubMed

Ebert, Martin; Müller-Ebert, Dörthe; Benker, Nathalie; Weinbruch, Stephan

2012-12-01

The size, morphology and chemical composition of 37,715 individual particles collected over 22 sampling days in the vicinity of a large integrated steel production were studied by scanning and transmission electron microscopy. Based on the morphology, chemistry and beam stability the particles were classified into the following fourteen groups: silicates, sea salt, calcium sulfates, calcium carbonates, carbonate-silicate mixtures, sulfate-silicate mixtures, iron oxides, iron mixtures, metal oxide-metals, complex secondary particles, soot, Cl-rich particles, P-rich particles, and other particles. The majority of iron oxide (≈85%) and metal oxide-metal (≈70%) particles as well as ≈20% of the silicate particles are fly ashes from high temperature processes. The emissions from the steel work are dominated by iron oxide particles. For source apportionment, seven source categories and two sectors of local wind direction (industrial and urban background) were distinguished. In both sectors PM₁₀ consists of four major source categories: 35% secondary, 20% industrial, 17% soil and 16% soot in the urban background sector compared to 45% industrial, 20% secondary, 13% soil, and 9% soot in the industrial sector. As the secondary and the soot components are higher in the urban background sector than in the industrial sector, it is concluded that both components predominantly originate from urban background sources (traffic, coal burning, and domestic heating). Abatement measures should not only focus on the steel work but should also include the urban background aerosol.

Effects of the Urban Heat Island on Aerosol pH

NASA Astrophysics Data System (ADS)

Battaglia, M., Jr.; Douglas, S.; Hennigan, C. J.

2017-12-01

The urban heat island (UHI) is a widely observed phenomenon whereby urban environments have higher temperature (T) and lower relative humidity (RH) than surrounding suburban and rural areas. Both of these factors affect the partitioning of semi-volatile species found in the atmosphere, such as nitric acid and ammonia. These species are inherently tied to aerosol pH, which is a key parameter driving some atmospheric chemical processes and environmental effects of aerosols. In this study, we characterized the effect of the UHI on aerosol pH in Baltimore, MD and Chicago, IL. These cities were selected based on differences in climatology, source influences, and atmospheric composition. Meteorological and atmospheric composition data from the urban centers and surrounding rural locations were used as inputs to the ISORROPIA-II aerosol thermodynamic model to compute gas/particle partitioning, aerosol liquid water content, and aerosol pH. Dramatic differences in aerosol liquid water (ALW) content were found in both cities and were attributable to the T and RH differences (UHI effect). The urban-rural differences in ALW result in urban aerosol pH that is systematically lower (more acidic) than rural aerosol pH for identical atmospheric composition. The UHI in Baltimore is most intense during the summer and at night, with differences of up to 1 pH unit predicted during these times. Similarly, the UHI in Chicago is most intense during the summer and at night; however, the atmospheric composition in Chicago shows a mediating effect, with differences of up to 0.65 pH units predicted during these times. These results are likely to have broad implications for chemistry occurring in and around urban atmospheres globally, although the magnitude of the effect may differ based on the UHI characteristic of each urban environment.

Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China, during the 2014 APEC summit

NASA Astrophysics Data System (ADS)

Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

2015-11-01

The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3- / SO42- mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play an important role in alleviating PM levels and achieving the "APEC blue" effect. The evolution of vertical differences between 260 m and the ground level was also investigated. Our results show complex vertical differences during the formation and evolution of severe haze episodes that are closely related to aerosol sources and boundary-layer dynamics.

Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China during 2014 APEC summit

NASA Astrophysics Data System (ADS)

Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

2015-08-01

The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the 325 m Beijing Meteorological Tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition at near ground level using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3-/SO42- mass ratios illustrate an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed by secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors such as SO2, NOx, and volatile organic compounds (VOCs). In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play an important role in alleviating PM levels and achieving the "APEC blue" effect. The evolution of vertical differences between 260 m and the ground level was also investigated. Our results show complex vertical differences during the formation and evolution of severe haze episodes that are closely related to aerosol sources and boundary layer dynamics.

Urban organic aerosols measured by single particle mass spectrometry in the megacity of London

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Harrison, R. M.

2012-05-01

During the month of October 2006, as part of the REPARTEE-I experiment (Regent's Park and Tower Environmental Experiment) an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed at an urban background location in the city of London, UK. Fifteen particle types were classified, some of which were already discussed (Dall'Osto et al., 2009a,b; Harrison et al., 2012). In this manuscript the origins and properties of four unreported particle types postulated to be due to locally generated aerosols, independent of the air mass type advected into London, are examined. One particle type, originating from lubricating oil (referred to as Ca-EC), was associated with morning rush hour traffic emissions. A second particle type, composed of both inorganic and organic species (called Na-EC-OC), was found enhanced in particle number concentration during evening time periods, and is likely to originate from a source operating at this time of day, or more probably from condensation of semi-volatile species. A third class, internally mixed with organic carbon and sulphate (called OC), was found to spike both in the morning and evenings although it could not unambiguously associated with a specific source or atmospheric process. The fourth class (Secondary Organic Aerosols - Polycyclic Aromatic Hydrocarbon; SOA-PAH) exhibited maximum frequency during the warmest part of the day, and a number of factors point towards secondary aerosol production from traffic-related volatile aromatic compounds. Single particle mass spectra of this particle type showed an oxidized polycyclic aromatic compound signature. A comparison of ATOFMS particle class data is then made with factors obtained by Positive Matrix Factorization and PAH signatures obtained from Aerosol Mass Spectrometer (AMS) data (Allan et al., 2010). Both the Ca-EC and OC particle types correlate with primary Hydrocarbon-like Organic Aerosol (HOA, R2 = 0.65 and 0.50 respectively), and Na-EC-OC correlates weakly with the AMS secondary Oxygenated Organic Aerosol (OOA), (R2 = 0.35). Cluster SOA-PAH was found not to correlate with any AMS signal. A detailed analysis was conducted to identify ATOFMS particle type(s) representative of the AMS cooking aerosol factor (COA), but no convincing associations were found. The combined ATOFMS and AMS results of this REPARTEE study do not always provide an entirely coherent interpretation.

The smog-fog-smog cycle and acid deposition

NASA Astrophysics Data System (ADS)

Pandis, Spyros N.; Seinfeld, John H.; Pilinis, Christodoulos

1990-10-01

A model including descriptions of aerosol and droplet microphysics, gas and aqueous-phase chemistry, and deposition is used to study the transformation of aerosol to fog droplets and back to aerosol in an urban environment. Fogs in polluted environments have the potential to increase aerosol sulfate concentrations but at the same time to cause reductions in the aerosol concentration of nitrate, chloride, ammonium and sodium and well as in the total aerosol mass concentration. The sulfate produced during fog episodes favors the aerosol particles that have access to most of the fog liquid water which are usually the large particles. Aerosol scavenging efficiencies of around 80 percent are calculated for urban fogs. Sampling and subsequent mixing of fog droplets of different sizes may result in measured concentrations that are not fully representative of the fogwater chemical composition and can introduce errors in the reported values of the ionic species deposition velocities. Differences in the major ionic species deposition velocities can be explained by their distribution over the droplet size spectrum and can be correlated with the species average diameter. Two different expressions are derived for use in fog models for the calculation of the liquid water deposition velocity during fog growth and dissipation stages.

Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

NASA Astrophysics Data System (ADS)

Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

2011-12-01

Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

CONTINUOUS MEASUREMENT OF FINE AND ULTRAFINE PARTICULATE MATTER, CRITERIA POLLUTANTS AND METEOROLOGICAL CONDITIONS IN URBAN EL PASO, TEXAS

EPA Science Inventory

Continuous measurements of aerosol size distributions were made in El Paso, TX, for a period in winter 1999. Size distribution measurements were performed at two urban locations in El Paso using two pairs of the scanning mobility particle sizer and the aerodynamic particle si...

In Situ Single Particle Measurement of Atmospheric Aging of Carbonaceous Aerosols During CARES

NASA Astrophysics Data System (ADS)

Cahill, J. F.; Suski, K.; Hubbe, J.; Shilling, J.; Zaveri, R. A.; Springston, S. R.; Prather, K. A.

2011-12-01

Atmospheric aging of aerosols through photochemistry, heterogeneous reactions and aqueous processing can change their physical and chemical properties, impacting their gas uptake, radiative forcing, and activation of cloud nuclei. Understanding the timescale and magnitude of this aging process is essential for accurate aerosol-climate modeling and predictions. An aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS) measured single particle mixing state during the Carbonaceous Aerosols and Radiative Effects Study (CARES) in the summer of 2010 over Sacramento, CA. On 6/23/10, flights in the morning and afternoon performed pseudo-Lagrangian sampling of the Sacramento urban plume. Carbonaceous particles from these flights were classified into 'aged' and 'fresh' classes based on their mixing state, with aged particles having more secondary species, such as nitrate and sulfate. In the morning flight, a clear decreasing trend in the ratio of fresh/aged particle types was seen as the flight progressed, whereas in the afternoon flight, the ratio was essentially constant. These data show that in the morning carbonaceous aerosols can become heavily oxidized in a few hours. Further analysis of particle mixing state and the timescale of carbonaceous aerosol aging will be presented

DOE Office of Scientific and Technical Information (OSTI.GOV)

Madronich, Sasha; Kleinman, Larry; Conley, Andrew

Gas-to-particle partitioning of organic aerosols (OA) is represented in most models by Raoult’s law, and depends on the existing mass of particles into which organic gases can dissolve. This raises the possibility of non-linear response of particle-phase OA to the emissions of precursor volatile organic compounds (VOCs) that contribute to this partitioning mass. Implications for air quality management are evident: A strong non-linear dependence would suggest that reductions in VOC emission would have a more-than-proportionate benefit in lowering ambient OA concentrations. Chamber measurements on simple VOC mixtures generally confirm the non-linear scaling between OA and VOCs, usually stated as amore » mass-dependence of the measured OA yields. However, for realistic ambient conditions including urban settings, no single component dominates the composition of the organic particles, and deviations from linearity are presumed to be small. Here we re-examine the linearity question using volatility spectra from several sources: (1) chamber studies of selected aerosols, (2) volatility inferred for aerosols sampled in two megacities, Mexico City and Paris, and (3) an explicit chemistry model (GECKO-A). These few available volatility distributions suggest that urban OA may be only slightly super-linear, with most values of the sensitivity exponent in the range 1.1-1.3, also substantially lower than seen in chambers for some specific aerosols. Furthermore, the rather low values suggest that OA concentrations in megacities are not an inevitable convergence of non-linear effects, but can be addressed (much like in smaller urban areas) by proportionate reductions in emissions.« less

Temporal and spatial variation of morphological descriptors for atmospheric aerosols collected in Mexico City

NASA Astrophysics Data System (ADS)

China, S.; Mazzoleni, C.; Dubey, M. K.; Chakrabarty, R. K.; Moosmuller, H.; Onasch, T. B.; Herndon, S. C.

2010-12-01

We present an analysis of morphological characteristics of atmospheric aerosol collected during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign that took place in Mexico City in March 2006. The sampler was installed on the Aerodyne mobile laboratory. The aerosol samples were collected on nuclepore clear polycarbonate filters mounted in Costar pop-top membrane holders. More than one hundred filters were collected at different ground sites with different atmospheric and geographical characteristics (urban, sub-urban, mountain-top, industrial, etc.) over a month period. Selected subsets of these filters were analyzed for aerosol morphology using a scanning electron microscope and image analysis techniques. In this study we investigate spatial and temporal variations of aerosol shape descriptors, morphological parameters, and fractal dimension. We also compare the morphological results with other aerosol measurements such as aerosol optical properties(scattering and absorption) and size distribution data. Atmospheric aerosols have different morphological characteristics depending on many parameters such as emission sources, atmospheric formation pathways, aging processes, and aerosol mixing state. The aerosol morphology influences aerosol chemical and mechanical interactions with the environment, physical properties, and radiative effects. In this study, ambient aerosol particles have been classified in different shape groups as spherical, irregularly shaped, and fractal-like aggregates. Different morphological parameters such as aspect ratio, roundness, feret diameter, etc. have been estimated for irregular shaped and spherical particles and for different kinds of soot particles including fresh soot, collapsed and coated soot. Fractal geometry and image processing have been used to obtain morphological characteristics of different soot particles. The number of monomers constituting each aggregate and their diameters were measured and used to estimate an ensemble three-dimensional (3-d) fractal dimension. One-dimensional (1-d) and two-dimensional (2-d) fractal geometries have been measured using a power-law scaling relationship between 1-d and 2-d properties of projected images. Temporal variations in fractal dimension of soot-like aggregates have been observed at the mountaintop site and spatial variation of fractal dimension and other morphological descriptors of different shaped particles have been investigated for the different ground sites.

The Unique Properties of Agricultural Aerosols Measured at a Cattle Feeding Operation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hiranuma, Naruki; Brooks, S. D.; Gramann, J.

2011-05-11

Housing roughly 10 million head of cattle in the United States alone, open air cattle feedlots represent a significant but poorly constrained source of atmospheric particles. Here we present a comprehensive characterization of physical and chemical properties of particles emitted from a large representative cattle feedlot in the Southwest United States. In the summer of 2008, measurements and samplings were conducted at the nominally upwind and downwind edges of the facility. A series of far-field measurements and samplings was also conducted 3.5 km north of the facility. Two instruments, a GRIMM Sequential Mobility Particle Sizer (SMPS) and a GRIMM Portablemore » Aerosol Spectrometer (PAS), were used to measure particle size distributions over the range of 0.01 to 25 μm diameter. Raman microspectroscopy (RM) was used to determine the chemical composition of particles on a single particle basis. Volume size distributions of fugitive dust were dominated by coarse mode particles. Twenty-four hour averaged concentrations of PM10 (particulate matter with a diameter of 10 µm or less) were as high as 1200 μg/m3 during the campaign. The primary constituents of the particulate matter were carbonaceous materials, such as humic acid, water soluble organics, and less soluble fatty acids, including stearic acid and tristearin. A significant fraction of the organic particles was composed of internally mixed with salts. Basic characteristics such as size distribution and composition of agricultural aerosols were found to be different than the properties of those found in urban and semi-urban aerosols. Failing to account for such differences will lead to serious errors in estimates of aerosol effects on climate, visibility, and public health.« less

The unique properties of agricultural aerosols measured at a cattle feeding operation

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Brooks, S. D.; Gramann, J.; Auvermann, B. W.

2011-05-01

Housing roughly 10 million head of cattle in the United States alone, open air cattle feedlots represent a significant but poorly constrained source of atmospheric particles. Here we present a comprehensive characterization of physical and chemical properties of particles emitted from a large representative cattle feedlot in the Southwest United States. In the summer of 2008, measurements and samplings were conducted at the nominally upwind and downwind edges of the facility. A series of far-field measurements and samplings was also conducted 3.5 km north of the facility. Two instruments, a GRIMM Sequential Mobility Particle Sizer (SMPS) and a GRIMM Portable Aerosol Spectrometer (PAS), were used to measure particle size distributions over the range of 0.01 to 25 μm diameter. Raman microspectroscopy (RM) was used to determine the chemical composition of particles on a single particle basis. Volume size distributions of fugitive dust were dominated by coarse mode particles. Twenty-four hour averaged concentrations of PM10 (particulate matter with a diameter of 10 μm or less) were as high as 1200 μg m-3 during the campaign. The primary constituents of the particulate matter were carbonaceous materials, such as humic acid, water soluble organics, and less soluble fatty acids, including stearic acid and tristearin. A significant percentage of the organic particles, up to 28 %, were composed of internally mixed with salts. Basic characteristics such as size distribution and composition of agricultural aerosols were found to be different than the properties of those found in urban and semi-urban aerosols. Failing to account for such differences will lead to serious errors in estimates of aerosol effects on climate, visibility, and public health.

Real-Time Characterization of Fluorescent Biological Aerosol Particles for Clear and Haze Episodes in Winter Beijing

NASA Astrophysics Data System (ADS)

Yue, S.; Fu, P.; Ren, H.; Fan, S.; Wei, L.; Hou, S.; Sun, Y.; Wang, Z.

2016-12-01

Primary biological aerosol particles (PBAP) such as pollen, fungal spore, bacteria and virus represent a major subset of particulate compositions for both coarse and fine aerosols. This category of aerosols affects weather, climate and human and plant health. We report the first multi-band quantification of fluorescent biological aerosol particles in Beijing, China in winter. The number concentrations and size distributions of FBAP were acquired by a Wideband Integrated Bioaerosol Sensor (WIBS-4A). Three-hour samples of total suspended particles (TSP) were concurrently collected during a transition of a haze event to a clear period. It was found that the fraction of FBAP in all particles (> 0.8 µm) in pollution episodes (average value: 17%) was slightly higher than that during clear periods (13%). Besides, size-segregated FBAP in different fluorescent channels were less correlated (Pearson correlation coefficient) and existed diverse diurnal trends, indicating various sources of FBAP. Our results provide a better understanding of the roles of biological aerosols in an urban environment that is frequently suffered from severe air pollution.

Aerosol Radiative Forcing in Asian Continental Outflow

NASA Technical Reports Server (NTRS)

Pueschel, R.; Kinne, S.; Redemann, J.; Gore, Warren J. (Technical Monitor)

2000-01-01

Aerosols in elevated layers were sampled with FSSP-probes and wire impactors over the Pacific ocean aboard the NASA DC-8 aircraft. Analyses of particle size and morphology identifies two distinctly different aerosol types for cases when the mid-visible extinctions exceed 0.2/km. Smaller sizes (effective radii of 0.2 um) and moderate absorption (mid-visible single scattering albedo of.935) are typical for urban-industrial pollution. Larger sizes (effective radii of 0.7 um) and weak absorption (mid-visible single scattering albedo of 0.985) identify dust. This aerosol classification is in agreement with its origin as determined by airmass back trajectory analysis. Based on lidar vertical profiling, aerosol dominated by dust and urban-industrial pollution above 3km were assigned mid-visible optical depths of 0.50 and 0.27, respectively. Radiative transfer simulations, considering a 50% cloud-cover below the aerosol layers, suggest (on a daily tP C)C> basis) small reductions (-4W/m2) to the energy budget at the top of the atmosphere for both aerosol types. For c' 0 dust, more backscattering of sunlight (weaker solar absorption) is compensated by a stronger greenhouse effect due to larger sizes. Forced reductions to the energy budget at the surface are 12W/m2 for both aerosol types. In contrast, impacts on heating rates within the aerosol layers are quite different: While urban-industrial aerosol warms the layer (at +0.6K/day as solar heating dominates), dust cools (at -0.5K/day as infrared cooling dominates). Sensitivity tests show the dependence of the aerosol climatic impact on the optical depth, particle size, absorptivity, and altitude of the layers, as well as clouds and surface properties. Climatic cooling can be eliminated (1) for the urban-industrial aerosol if absorption is increased to yield a mid-visible single scattering albedo of 0.89, or if the ocean is replaced by a land surface; (2) for the dust aerosol if the effective radius is increased from 0.7 to 1.2 um. The removal of low-level clouds doubles the cooling at the top of the atmosphere to about -8W/m2.

Atmospheric aerosols in Rome, Italy: sources, dynamics and spatial variations during two seasons

NASA Astrophysics Data System (ADS)

Struckmeier, Caroline; Drewnick, Frank; Fachinger, Friederike; Gobbi, Gian Paolo; Borrmann, Stephan

2016-12-01

Investigations on atmospheric aerosols and their sources were carried out in October/November 2013 and May/June 2014 consecutively in a suburban area of Rome (Tor Vergata) and in central Rome (near St Peter's Basilica). During both years a Saharan dust advection event temporarily increased PM10 concentrations at ground level by about 12-17 µg m-3. Generally, in October/November the ambient aerosol was more strongly influenced by primary emissions, whereas higher relative contributions of secondary particles (sulfate, aged organic aerosol) were found in May/June. Absolute concentrations of anthropogenic emission tracers (e.g. NOx, CO2, particulate polycyclic aromatic hydrocarbons, traffic-related organic aerosol) were generally higher at the urban location. Positive matrix factorization was applied to the PM1 organic aerosol (OA) fraction of aerosol mass spectrometer (HR-ToF-AMS) data to identify different sources of primary OA (POA): traffic, cooking, biomass burning and (local) cigarette smoking. While biomass burning OA was only found at the suburban site, where it accounted for the major fraction of POA (18-24 % of total OA), traffic and cooking were more dominant sources at the urban site. A particle type associated with cigarette smoke emissions, which is associated with a potential characteristic marker peak (m/z 84, C5H10N+, a nicotine fragment) in the mass spectrum, was only found in central Rome, where it was emitted in close vicinity to the measurement location. Regarding secondary OA, in October/November, only a very aged, regionally advected oxygenated OA was found, which contributed 42-53 % to the total OA. In May/June total oxygenated OA accounted for 56-76 % of the OA. Here a fraction (18-26 % of total OA) of a fresher, less oxygenated OA of more local origin was also observed. New particle formation events were identified from measured particle number concentrations and size distributions in May/June 2014 at both sites. While they were observed every day at the urban location, at the suburban location they were only found under favourable meteorological conditions, but were independent of advection of the Rome emission plume. Particles from sources in the metropolitan area of Rome and particles advected from outside Rome contributed 42-70 and 30-58 % to the total measured PM1, respectively. Apart from the general aerosol characteristics, in this study the properties (e.g. emission strength) and dynamics (e.g. temporal behaviour) of each identified aerosol type is investigated in detail to provide a better understanding of the observed seasonal and spatial differences.

Spectral Discrimination of Fine and Coarse Mode Aerosol Optical Depth from AERONET Direct Sun Data of Singapore and South-East Asia

NASA Astrophysics Data System (ADS)

Salinas Cortijo, S.; Chew, B.; Liew, S.

2009-12-01

Aerosol optical depth combined with the Angstrom exponent and its derivative, are often used as a qualitative indicator of aerosol particle size, with Angstrom exp. values greater than 2 indicating small (fine mode) particles associated with urban pollution and bio-mass burning. Around this region, forest fires are a regular occurrence during the dry season, specially near the large land masses of Sumatra and Borneo. The practice of clearing land by burning the primary and sometimes secondary forest, results in a smog-like haze covering large areas of regional cities such as cities Singapore, Kuala Lumpur and sometimes the south of Thailand, often reducing visibility and increasing health problems for the local population. In Singapore, the sources of aerosols are mostly from fossil fuel burning (energy stations, incinerators, urban transport etc.) and from the industrial and urban areas. The proximity to the sea adds a possible oceanic source. However, as stated above and depending on the time of the year, there can be a strong bio-mass component coming from forest fires from various regions of the neighboring countries. Bio-mass related aerosol particles are typically characterized by showing a large optical depth and small, sub-micron particle size distributions. In this work, we analyze three years of direct Sun measurements performed with a multi-channel Cimel Sun-Photometer (part of the AERONET network) located at our site. In order to identify bio-mass burning events in this region, we perform a spectral discrimination between coarse and fine mode optical depth; subsequently, the fine mode parameters such as optical depth, optical ratio and fine mode Angstrom exponents (and its derivative) are used to identify possible bio-mass related events within the data set.

Determination of mixing state and sources of wintertime organic aerosol in Paris using single particle mass spectrometry

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Wiedensohler, A.; Jeong, C.; McGuire, M.; Evans, G. J.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J.

2012-12-01

The size-resolved chemical composition of single particles at an urban background site in Paris, France, was determined using an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) as part of the MEGAPOLI winter campaign in January/February 2010. A variety of mixing states were identified for organic aerosol by mass spectral clustering and apportioned to both fossil fuel and biomass burning sources. The ATOFMS data were scaled in order to produce mass concentration estimates for each organic aerosol particle type identified. Potassium-containing organic aerosol internally mixed with nitrate, associated with local wood burning, was observed to dominate during periods characterised by marine air masses. Sulfate-rich potassium-containing organic aerosol, associated with transboundary transport of biomass burning emissions, dominated during periods influenced by continental air masses. The scaled total mass concentration for potassium-containing particles was well correlated (R2 = 0.79) with concurrent measurements of potassium mass concentration measured with a Particle-Into-Liquid-Sampler (PILS). Another organic particle type, also containing potassium but rich in trimethylamine and sulfate, was detected exclusively during continental air mass events. These particles are postulated to have accumulated gas phase trimethylamine through heterogeneous reaction before arriving at the sampling site. Potential source regions for transboundary organic aerosols have been investigated using the potential source contribution function (PSCF). Comparison with aerosol mass spectrometer (AMS) measurements will also be discussed.

Aerosol properties over the western Mediterranean basin: temporal and spatial variability

NASA Astrophysics Data System (ADS)

Lyamani, H.; Valenzuela, A.; Perez-Ramirez, D.; Toledano, C.; Granados-Muñoz, M. J.; Olmo, F. J.; Alados-Arboledas, L.

2015-03-01

This study focuses on the analysis of Aerosol Robotic Network (AERONET) aerosol data obtained over Alborán Island (35.90° N, 3.03° W, 15 m a.s.l.) in the western Mediterranean from July 2011 to January 2012. Additional aerosol data from the three nearest AERONET stations (Málaga, Oujda and Palma de Mallorca) and the Maritime Aerosol Network (MAN) were also analyzed in order to investigate the temporal and spatial variations of aerosol over this scarcely explored region. High aerosol loads over Alborán were mainly associated with desert dust transport from North Africa and occasional advection of anthropogenic fine particles from central European urban-industrial areas. The fine particle load observed over Alborán was surprisingly similar to that obtained over the other three nearest AERONET stations, suggesting homogeneous spatial distribution of fine particle loads over the four studied sites in spite of the large differences in local sources. The results from MAN acquired over the Mediterranean Sea, Black Sea and Atlantic Ocean from July to November 2011 revealed a pronounced predominance of fine particles during the cruise period.

New Particle Formation in an Urban Atmosphere: The Role of Various Ingredients Investigated in the CLOUD Chamber

NASA Astrophysics Data System (ADS)

Baltensperger, U.; Xiao, M.; Hoyle, C.; Dada, L.; Garmash, O.; Stolzenburg, D.; Molteni, U.; Lehtipalo, K.; El-Haddad, I.; Dommen, J.

2017-12-01

Atmospheric aerosols play an important role on climate via aerosol-radiation interaction and aerosol-cloud interaction. The latter is strongly influenced by new particle formation (NPF). The physical and chemical mechanisms behind the NPF process are still under investigation. Great advancements were made in resolving chemical and physical mechanisms of NPF with a series of experiments conducted at the CLOUD (Cosmics Leaving Outdoor Droplets) chamber facility at CERN (Geneva, Switzerland), including binary nucleation of sulfuric acid - water, ternary nucleation of sulfuric acid - water with ammonia or dimethylamine as well as oxidation products (highly oxygenated molecules, HOMs) from biogenic precursors with and without the presence of sulfuric acid. Here, we investigate possible NPF mechanisms in urban atmospheres, where large populations are exposed to high aerosol concentrations; these mechanisms are still missing and are urgently needed. Urban atmospheres are highly polluted with high concentrations of SO2, ammonia, NOx and volatile organic vapors from anthropogenic activity as well as with high particle concentrations, which provide a high condensation sink for condensable gases. Aromatic hydrocarbons from industrial activities, traffic and residential combustion are present at high concentrations and contribute significantly to photochemical smog in the urban environment.The experiments were conducted at the CLOUD chamber facility during the CLOUD11 campaign in fall 2016. Three aromatic hydrocarbons were selected: toluene, 1,2,4-trimethylbenzene (1,2,4-TMB) and naphthalene (NPT). Experiments were also conducted with mixtures of the three aromatic hydrocarbons to better represent the urban atmosphere. All the experiments were conducted in the presence of sulfuric acid concentrations with or without the addition of ammonia and NOx. New particle formation rates and early growth rates derived for each precursor and their mixture, together with sulfuric acid and with or without the addition of ammonia and NOx will be reported.

Aerosol climatology over the Mexico City basin: Characterization of optical properties

NASA Astrophysics Data System (ADS)

Carabali, Giovanni; Estévez, Héctor Raúl; Valdés-Barrón, Mauro; Bonifaz-Alfonzo, Roberto; Riveros-Rosas, David; Velasco-Herrera, Víctor Manuel; Vázquez-Gálvez, Felipe Adrián

2017-09-01

Climatology of Aerosol Optical Depth (AOD), Single Scattering Albedo (SSA), and aerosol particle-size distribution were analyzed using a 15-year (1999-2014) dataset from AErosol RObotic NETwork (AERONET) observations over the Mexico City (MC) basin. The atmosphere over this site is dominated by two main aerosol types, represented by urban/industrial pollution and biomass-burning particles. Due to the specific meteorological conditions within the basin, seasons are usually classified into three as follows: Dry Winter (DW) (November-February); Dry Spring (DS) (March-April), and the RAiny season (RA) (May-October), which are mentioned throughout this article. Using a CIMEL sun photometer, we conducted continuous observations over the MC urban area from January 1999 to December 2014. Aerosol Optical Depth (AOD), Ångström exponent (α440-870), Single Scattering Albedo (SSA), and aerosol particle-size distribution were derived from the observational data. The overall mean AOD500 during the 1999-2014 period was 0.34 ± 0.07. The monthly mean AOD reached a maximal value of 0.49 in May and a minimal value of 0.27 in February and March. The average α440-870 value for the period studied was 1.50 ± 0.16. The monthly average of α440-870 reached a minimal value of 1.32 in August and a maximal value of 1.61 in May. Average SSA at 440 nm was 0.89 throughout the observation period, indicating that aerosols over Mexico City are composed mainly of absorptive particles. Concentrations of fine- and coarse-mode aerosols over MC were highest in DS season compared with other seasons, especially for particles with radii measuring between 0.1 and 0.2 μm. Results from the Spectral De-convolution Algorithm (SDA) show that fine-mode aerosols dominated AOD variability in MC. In the final part of this article, we present a classification of aerosols in MC by using the graphical method proposed by Gobbi et al. (2007), which is based on the combined analysis of α and its spectral curvature δα.

EVALUATION OF COMPUTER-CONTROLLED SCANNING ELECTRON MICROSCOPY APPLIED TO AN AMBIENT URBAN AEROSOL SAMPLE

EPA Science Inventory

Concerns about the environmental and public health effects of particulate matter (PM) have stimulated interest in analytical techniques capable of measuring the size and chemical composition of individual aerosol particles. Computer-controlled scanning electron microscopy (CCSE...

Distinct high molecular weight organic compound (HMW-OC) types in aerosol particles collected at a coastal urban site

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Healy, R. M.; Wenger, J. C.; O'Dowd, C.; Ovadnevaite, J.; Ceburnis, D.; Harrison, Roy M.; Beddows, D. C. S.

2017-12-01

Organic oligomers were discovered in laboratory-generated atmospheric aerosol over a decade ago. However, evidence for the presence of oligomers in ambient aerosols is scarce and mechanisms for their formation have yet to be fully elucidated. In this work, three unique aerosol particle types internally mixed with High molecular weight organic compounds (HMW-OC) species - likely oligomers - were detected in ambient air using single particle Aerosol Time-Of-Flight Mass Spectrometry (ATOFMS) in Cork (Ireland) during winter 2009. These particle types can be described as follows: (1) HMW-OCs rich in organic nitrogen - possibly containing nitrocatechols and nitroguaiacols - originating from primary emissions of biomass burning particles during evening times; (2) HMW-OCs internally mixed with nitric acid, occurring in stagnant conditions during night time; and (3) HMW-OCs internally mixed with sea salt, likely formed via photochemical reactions during day time. The study exemplifies the power of methodologies capable of monitoring the simultaneous formation of organic and inorganic particle-phase reaction products. Primary emissions and atmospheric aging of different types of HMW-OC contributes to aerosol with a range of acidity, hygroscopic and optical properties, which can have different impacts on climate and health.

Fossil Fuel Combustion-Related Emissions Dominate Atmospheric Ammonia Sources during Severe Haze Episodes: Evidence from 15N-Stable Isotope in Size-Resolved Aerosol Ammonium

NASA Astrophysics Data System (ADS)

Pan, Y.; Tian, S.; Liu, D.; Fang, Y.; Zhu, X.; Zhang, Q.; Zheng, B.; Michalski, G. M.; Wang, Y.

2016-12-01

The reduction of ammonia (NH3) emissions is urgently needed due to its major contributions to nitrogen deposition and particle pollution. However, the relative contributions of individual NH3 sources are unclear, and debate remains over whether agricultural emissions dominate atmospheric NH3 in urban areas. Based on the chemical and isotopic measurements of size-resolved aerosols in urban Beijing, China, we find that the natural abundance of 15N (expressed using δ15N values) of ammonium (NH4+) in fine particles varies with the development of haze episodes, ranging from -37.1‰ to -21.7‰ during clean/dusty days (relative humidity: ˜ 40%), to -13.1‰ to +5.8‰ during hazy days (relative humidity: 70-90%). After factoring the isotope exchange between NH3 gas and aerosol NH4+, the δ15N value of the initial NH3 during hazy days is found to be -14.5‰ to -1.6‰, which indicates fossil fuel-based emissions. These emissions contribute 90% of the total NH3 during hazy days in urban Beijing. This work demonstrates the analysis of δ15N values of aerosol NH4+ to be a promising new tool for partitioning atmospheric NH3 sources, providing policy makers with insights into NH3 emissions and secondary aerosols for regulation in urban environments. This work also shed lights on the sources of nitrogen deposition in downwind ecosystems.

Characteristics of size-segregated carbonaceous aerosols in the Beijing-Tianjin-Hebei region.

PubMed

Guo, Yuhong

2016-07-01

Mass concentrations of organic carbon (OC) and elemental carbon (EC) in size-resolved aerosols were investigated at four sites (three cities and one country) in the Beijing-Tianjin-Hebei region from September 2009 to August 2011. The size distributions of OC and EC presented large evolutions among rural and urban sites, and among four seasons, with highest peaks of OC and EC in fine mode in urban areas during winter. Geometric mean diameters (GMDs) of OC and EC in fine particles at urban sites during winter were lower than those at rural site mainly due to effects of fine particle coagulation and organic compound repartitioning. Fossil fuel emissions were a dominant source of OC and EC in urban areas, while biomass burning was a major source of OC and EC at rural site. Trajectory clustering and CWT analysis showed that regional transport was an important contributor to OC and EC in Beijing.

Measurements of Size Resolved Organic Particulate Mass Using An On-line Aerosol Mass Spectrometer (ams) Laboratory Validation; Analysis Tool Development; and Interpretation of Field Data

NASA Astrophysics Data System (ADS)

Alfarra, M. R.; Coe, H.; Allan, J. D.; Bower, K. N.; Garforth, A. A.; Canagaratna, M.; Worsnop, D.

The aerosol mass spectrometer (AMS) is a quantitative instrument designed to deliver real-time size resolved chemical composition of the volatile and semi volatile aerosol fractions. The AMS response to a wide range of organic compounds has been exper- imentally characterized, and has been shown to compare well with standard libraries of 70 eV electron impact ionization mass spectra. These results will be presented. Due to the scanning nature of the quadrupole mass spectrometer, the AMS provides averaged composition of ensemble of particles rather than single particle composi- tion. However, the mass spectra measured by AMS are reproducible and similar to those of standard libraries so analysis tools can be developed on large mass spectral libraries that can provide chemical composition information about the type of organic compounds in the aerosol. One such tool is presented and compared with laboratory measurements of single species and mixed component organic particles by the AMS. We will then discuss the applicability of these tools to interpreting field AMS data ob- tained in a range of experiments at different sites in the UK and Canada. The data will be combined with other measurements to show the behaviour of the organic aerosol fraction in urban and sub-urban environments.

Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

NASA Astrophysics Data System (ADS)

Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

2012-07-01

Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

On the Chemical Characterization of Organic Matter in Rain at Mexico City.

NASA Astrophysics Data System (ADS)

Montero-Martinez, G.; Andraca-Ayala, G. L.; Hernández-Nagay, D. P.; Mendoza-Trejo, A.; Rivera-Arellano, J.; Rosado-Abon, A.; Roy, P. D.

2016-12-01

The chemical composition of the aerosol plays a central role in atmospheric processes and has influence on the hydrological cycle. Clouds form through the nucleation of water vapor on certain atmospheric aerosol particles, called cloud condensation nuclei (CCN). Also, precipitating particles scavenge some other aerosol particles on their way to the surface. Atmospheric particles are a mixture of organic and inorganic materials, both soluble and insoluble in water. Aerosol chemical characterization indicates a larger variety of compounds in urban areas respect to other regions. Thus, chemical composition of rainwater may represent an important aspect for estimating atmospheric air pollution. It has been recognized that organic species present in aerosol particles are important in the formation of cloud droplets. Therefore, the information about the organic compounds in precipitation samples may be helpful to understand their effects on the formation of clouds and rain, as well as their sources. Organic acids are ubiquitous components of aerosols and have been identified in precipitation water. In this work, preliminary results of the content of soluble organic (neutral and acidic) matter in rainwater samples collected in Mexico City during 2015 will be presented. The organic compounds content was performed by using an ionic chromatographic methodology with gradient elution; so the total amount was evaluated as the sum of four fractions: neutral/basic, mono-, bi-, and poly-acid compounds. The outcomes suggest that most of the amount of organic substances soluble in water is contained by the neutral/basic and mono-acid fractions. Regarding the total amount of water soluble organic compounds, the rain samples collected in Mexico City are in agreement with some others reported for large urban areas.

Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Amato, F.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.

2012-08-01

Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban Environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter <2.5 μm) resolved Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie FP7-EU framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the unique approach used is the simultaneous PIXE measurements at two monitoring sites: urban background (UB) and a street canyon traffic road site (RS). Elements related to primary non exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (secondary sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non exhaust brake dust (Fe-Cu) - 7%), and three types industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%). The validity of the PMF solution of the PIXE data is supported by strong correlations with external single particle mass spectrometry measurements. Beside apportioning the aerosol sources, some important air quality related conclusions can be drawn about the PM2.5 fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial aerosol plumes associated with shipping oil combustion and smelters activities have a higher impact on the more ventilated UB site; (3) a unique source of Pb-Cl (associated with industrial combustion emissions) is found a to be the major (82%) source of Cl in the urban agglomerate; (4) PM2.5 traffic brake dust (Fe-Cu) is mainly primarily emitted and not resuspended, whereas PM2.5 urban crustal dust (Ca) is found mainly resuspended by both traffic vortex and sea breeze; (5) urban dust (Ca) is found the aerosol source most affected by land wetness, reduced by a factor of eight during rainy days and suggesting that wet roads may be a solution for reducing dust concentrations in road sites, far more effective than street sweeping activities.

Spectral Absorption Properties of Aerosol Particles from 350-2500nm

NASA Technical Reports Server (NTRS)

Martins, J. Vanderlei; Artaxo, Paulo; Kaufman, Yoram J.; Castanho, Andrea D.; Remer, Lorraine A.

2009-01-01

The aerosol spectral absorption efficiency (alpha (sub a) in square meters per gram) is measured over an extended wavelength range (350 2500 nm) using an improved calibrated and validated reflectance technique and applied to urban aerosol samples from Sao Paulo, Brazil and from a site in Virginia, Eastern US, that experiences transported urban/industrial aerosol. The average alpha (sub a) values (approximately 3 square meters per gram at 550 nm) for Sao Paulo samples are 10 times larger than alpha (sub a) values obtained for aerosols in Virginia. Sao Paulo aerosols also show evidence of enhanced UV absorption in selected samples, probably associated with organic aerosol components. This extra UV absorption can double the absorption efficiency observed from black carbon alone, therefore reducing by up to 50% the surface UV fluxes, with important implications for climate, UV photolysis rates, and remote sensing from space.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9-0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9-0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

NASA Astrophysics Data System (ADS)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray emissions to particles, addressing the persistent question of the sources of cloud condensation nuclei in clean marine conditions.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Seinfeld, John H.

This project addressed the following research need in the Atmospheric System Research (ASR) Science and Program Plan: "Measurements downwind of urban sources of aerosol particles and precursor gases have shown that the mass concentration of secondary organic aerosol (SOA) can be several-fold greater than can be explained on the basis of current model calculations using observed precursor concentrations. ASR will continue conducting laboratory experiments on both gas-phase and aqueous-phase SOA formation to characterize the particle formation and the organic gases that react to form new organic aerosol material on aerosol seeds. ASR will use these experiments to guide the developmentmore » of comprehensive chemical mechanisms... to guide the development of parameterizations that are simple enough to be applied to aerosol life cycle models."« less

Traffic and nucleation events as main sources of ultrafine particles in high-insolation developed world cities

NASA Astrophysics Data System (ADS)

Brines, M.; Dall'Osto, M.; Beddows, D. C. S.; Harrison, R. M.; Gómez-Moreno, F.; Núñez, L.; Artíñano, B.; Costabile, F.; Gobbi, G. P.; Salimi, F.; Morawska, L.; Sioutas, C.; Querol, X.

2015-05-01

Road traffic emissions are often considered the main source of ultrafine particles (UFP, diameter smaller than 100 nm) in urban environments. However, recent studies worldwide have shown that - in high-insolation urban regions at least - new particle formation events can also contribute to UFP. In order to quantify such events we systematically studied three cities located in predominantly sunny environments: Barcelona (Spain), Madrid (Spain) and Brisbane (Australia). Three long-term data sets (1-2 years) of fine and ultrafine particle number size distributions (measured by SMPS, Scanning Mobility Particle Sizer) were analysed. Compared to total particle number concentrations, aerosol size distributions offer far more information on the type, origin and atmospheric evolution of the particles. By applying k-means clustering analysis, we categorized the collected aerosol size distributions into three main categories: "Traffic" (prevailing 44-63% of the time), "Nucleation" (14-19%) and "Background pollution and Specific cases" (7-22%). Measurements from Rome (Italy) and Los Angeles (USA) were also included to complement the study. The daily variation of the average UFP concentrations for a typical nucleation day at each site revealed a similar pattern for all cities, with three distinct particle bursts. A morning and an evening spike reflected traffic rush hours, whereas a third one at midday showed nucleation events. The photochemically nucleated particles' burst lasted 1-4 h, reaching sizes of 30-40 nm. On average, the occurrence of particle size spectra dominated by nucleation events was 16% of the time, showing the importance of this process as a source of UFP in urban environments exposed to high solar radiation. Nucleation events lasting for 2 h or more occurred on 55% of the days, this extending to > 4 h in 28% of the days, demonstrating that atmospheric conditions in urban environments are not favourable to the growth of photochemically nucleated particles. In summary, although traffic remains the main source of UFP in urban areas, in developed countries with high insolation urban nucleation events are also a main source of UFP. If traffic-related particle concentrations are reduced in the future, nucleation events will likely increase in urban areas, due to the reduced urban condensation sinks.

Development and evaluation of the aerosol dynamics and gas phase chemistry model ADCHEM

NASA Astrophysics Data System (ADS)

Roldin, P.; Swietlicki, E.; Schurgers, G.; Arneth, A.; Lehtinen, K. E. J.; Boy, M.; Kulmala, M.

2011-06-01

The aim of this work was to develop a model suited for detailed studies of aerosol dynamics, gas and particle phase chemistry within urban plumes, from local scale (1 × 1 km2) to regional scale. This article describes and evaluates the trajectory model for Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer (ADCHEM). The model treats both vertical and horizontal dispersion perpendicular to an air mass trajectory (2-space dimensions). The Lagrangian approach enables a more detailed representation of the aerosol dynamics, gas and particle phase chemistry and a finer spatial and temporal resolution compared to that of available regional 3D-CTMs. These features make it among others well suited for urban plume studies. The aerosol dynamics model includes Brownian coagulation, dry deposition, wet deposition, in-cloud processing, condensation, evaporation, primary particle emissions and homogeneous nucleation. The organic mass partitioning was either modeled with a 2-dimensional volatility basis set (2D-VBS) or with the traditional two-product model approach. In ADCHEM these models consider the diffusion limited and particle size dependent condensation and evaporation of 110 and 40 different organic compounds respectively. The gas phase chemistry model calculates the gas phase concentrations of 61 different species, using 130 different chemical reactions. Daily isoprene and monoterpene emissions from European forests were simulated separately with the vegetation model LPJ-GUESS, and included as input to ADCHEM. ADCHEM was used to simulate the ageing of the urban plumes from the city of Malmö in southern Sweden (280 000 inhabitants). Several sensitivity tests were performed concerning the number of size bins, size structure method, aerosol dynamic processes, vertical and horizontal mixing, coupled or uncoupled condensation and the secondary organic aerosol formation. The simulations show that the full-stationary size structure gives accurate results with little numerical diffusion when more than 50 size bins are used between 1.5 and 2500 nm, while the moving-center method is preferable when only a few size bins are selected. The particle number size distribution in the center of the urban plume from Malmö was mainly affected by dry deposition, coagulation and vertical dilution. The modeled PM2.5 mass was dominated by organic material, nitrate, sulfate and ammonium. If the condensation of HNO3 and NH3 was treated as a coupled process (pH independent) the model gave lower nitrate PM2.5 mass than if considering uncoupled condensation. Although the time of ageing from that SOA precursors are emitted until condensable products are formed is substantially different with the 2D-VBS and two product model, the models gave similar total organic mass concentrations.

Traffic aerosol lobar doses deposited in the human respiratory system.

PubMed

Manigrasso, Maurizio; Vernale, Claudio; Avino, Pasquale

2017-06-01

Aerosol pollution in urban environments has been recognized to be responsible for important pathologies of the cardiovascular and respiratory systems. In this perspective, great attention has been addressed to Ultra Fine Particles (UFPs < 100 nm), because they efficiently penetrate into the respiratory system and are capable of translocating from the airways into the blood circulation. This paper describes the aerosol regional doses deposited in the human respiratory system in a high-traffic urban area. The aerosol measurements were carried out on a curbside in downtown Rome, on a street characterized by a high density of autovehicular traffic. Aerosol number-size distributions were measured by means of a Fast Mobility Particle Sizer in the range from 5.6 to 560 nm with a 1 s time resolution. Dosimetry estimates were performed with the Multiple-Path Particle Dosimetry model by means of the stochastic lung model. The exposure scenario close to traffic is represented by a sequence of short-term peak exposures: about 6.6 × 10 10 particles are deposited hourly into the respiratory system. After 1 h of exposure in proximity of traffic, 1.29 × 10 10 , 1.88 × 10 10 , and 3.45 × 10 10 particles are deposited in the head, tracheobronchial, and alveolar regions. More than 95 % of such doses are represented by UFPs. Finally, according to the greater dose estimated, the right lung lobes are expected to be more susceptible to respiratory pathologies than the left lobes.

Elucidating severe urban haze formation in China

NASA Astrophysics Data System (ADS)

Guo, Song; Hu, Min; Zamora, Misti L.; Peng, Jianfei; Shang, Dongjie; Zheng, Jing; Du, Zhuofei; Wu, Zhijun; Shao, Min; Zeng, Limin; Molina, Mario J.; Zhang, Renyi

2014-12-01

As the world's second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China.

Elucidating severe urban haze formation in China

PubMed Central

Guo, Song; Hu, Min; Zamora, Misti L.; Peng, Jianfei; Shang, Dongjie; Zheng, Jing; Du, Zhuofei; Wu, Zhijun; Shao, Min; Zeng, Limin; Molina, Mario J.; Zhang, Renyi

2014-01-01

As the world’s second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China. PMID:25422462

Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site during SAPUSS - diurnal variations and PMF receptor modelling

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Amato, F.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.

2013-04-01

Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter < 2.5 μm) resolved aerosol samples analysed by Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie European Union framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the approach used is the simultaneous sampling at two monitoring sites in Barcelona (Spain) during September-October 2010: an urban background site (UB) and a street canyon traffic road site (RS). Elements related to primary non-exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (regional sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non-exhaust brake dust (Fe-Cu) - 7%), and three types of industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%, percentages presented are average source contributions to the total elemental mass measured). The validity of the PMF solution of the PIXE data is supported by very good correlations with external single particle mass spectrometry measurements. Some important conclusions can be drawn about the PM2.5 mass fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial aerosol plumes associated with shipping oil combustion and smelters activities have a higher impact on the more ventilated UB site; (3) a unique source of Pb-Cl (associated with combustion emissions) is found to be the major (82%) source of fine Cl in the urban agglomerate; (4) the mean diurnal variation of PM2.5 primary traffic non-exhaust brake dust (Fe-Cu) suggests that this source is mainly emitted and not resuspended, whereas PM2.5 urban dust (Ca) is found mainly resuspended by both traffic vortex and sea breeze; (5) urban dust (Ca) is found the aerosol source most affected by land wetness, reduced by a factor of eight during rainy days and suggesting that wet roads may be a solution for reducing urban dust concentrations.

Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Hansen, Kristen J.

An integrated sampling and supercritical fluid extraction (SFE) cell has been designed for whole-sample analysis of organic compounds on tropospheric aerosol particles. The low-volume extraction cell has been interfaced with a sampling manifold for aerosol particle collection in the field. After sample collection, the entire SFE cell was coupled to a gas chromatograph; after on-line extraction, the cryogenically -focused sample was separated and the volatile compounds detected with either a mass spectrometer or a flame ionization detector. A 20-minute extraction at 450 atm and 90 ^circC with pure supercritical CO _2 is sufficient for quantitative extraction of most volatile compounds in aerosol particle samples. A comparison between SFE and thermal desorption, the traditional whole-sample technique for analyses of this type, was performed using ambient aerosol particle samples, as well as samples containing known amounts of standard analytes. The results of these studies indicate that SFE of atmospheric aerosol particles provides quantitative measurement of several classes of organic compounds. SFE provides information that is complementary to that gained by the thermal desorption analysis. The results also indicate that SFE with CO _2 can be validated as an alternative to thermal desorption for quantitative recovery of several organic compounds. In 1989, the organic constituents of atmospheric aerosol particles collected at Niwot Ridge, Colorado, along with various physical and meteorological data, were measured during a collaborative field study. Temporal changes in the composition of samples collected during summertime at the rural site were studied. Thermal desorption-GC/FID was used to quantify selected compounds in samples collected during the field study. The statistical analysis of the 1989 Niwot Ridge data set is presented in this work. Principal component analysis was performed on thirty-one variables selected from the data set in order to ascertain different source and process components, and to examine concentration changes in groups of variables with respect to time of day and meteorological conditions. Seven orthogonal groups of variables resulted from the statistical analysis; the groups serve as molecular markers for different biologic and anthropogenic emission sources. In addition, the results of the statistical analysis were used to investigate how several emission source contributions vary with respect to local atmospheric dynamics. Field studies were conducted in the urban environment in and around Boulder, CO. to characterize the dynamics, chemistry, and emission sources which affect the composition and concentration of different size-fractions of aerosol particles in the Boulder air mass. Relationships between different size fractions of particles and some gas-phase pollutants were elucidated. These field studies included an investigation of seasonal variations in the organic content and concentration of aerosol particles, and how these characteristics are related to local meteorology and to the concentration of some gas-phase pollutants. The elemental and organic composition of aerosol particles was investigated according to particle size in preliminary studies of size-differentiated samples of aerosol particles. In order to aid in future studies of urban aerosol particles, samples were collected at a forest fire near Boulder. Molecular markers specific to wood burning processes will be useful indicators of residential wood burning activities in future field studies.

High concentrations of coarse particles emitted from a cattle feeding operation

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Brooks, S. D.; Gramann, J.; Auvermann, B. W.

2011-08-01

Housing roughly 10 million head of cattle in the United States alone, open air cattle feedlots represent a significant but poorly constrained source of atmospheric particles. Here we present a comprehensive characterization of physical and chemical properties of particles emitted from a large representative cattle feedlot in the Southwest United States. In the summer of 2008, measurements and samplings were conducted at the upwind and downwind edges of the facility. A series of far-field measurements and samplings was also conducted 3.5 km north of the facility. Two instruments, a GRIMM Sequential Mobility Particle Sizer (SMPS) and a GRIMM Portable Aerosol Spectrometer (PAS), were used to measure particle size distributions over the range of 0.01 to 25 μm diameter. Raman microspectroscopy was used to determine the chemical composition of particles on a single particle basis. Volume size distributions of dust were dominated by coarse mode particles. Twenty-four hour averaged concentrations of PM10 (particulate matter with a diameter of 10 μm or less) were as high as 1200 μg m-3 during the campaign. The primary constituents of the particulate matter were carbonaceous materials, such as humic acid, water soluble organics, and less soluble fatty acids, including stearic acid and tristearin. A significant fraction of the organic particles was present in internal mixtures with salts. Basic characteristics such as size distribution and composition of agricultural aerosols were found to be different than the properties of those found in urban and semi-urban aerosols. Failing to account for such differences may lead to errors in estimates of aerosol effects on local air quality, visibility, and public health.

Identification of the sources of primary organic aerosols at urban schools: a molecular marker approach.

PubMed

Crilley, Leigh R; Qadir, Raeed M; Ayoko, Godwin A; Schnelle-Kreis, Jürgen; Abbaszade, Gülcin; Orasche, Jürgen; Zimmermann, Ralf; Morawska, Lidia

2014-08-01

Children are particularly susceptible to air pollution and schools are examples of urban microenvironments that can account for a large portion of children's exposure to airborne particles. Thus this paper aimed to determine the sources of primary airborne particles that children are exposed to at school by analyzing selected organic molecular markers at 11 urban schools in Brisbane, Australia. Positive matrix factorization analysis identified four sources at the schools: vehicle emissions, biomass burning, meat cooking and plant wax emissions accounting for 45%, 29%, 16% and 7%, of the organic carbon respectively. Biomass burning peaked in winter due to prescribed burning of bushland around Brisbane. Overall, the results indicated that both local (traffic) and regional (biomass burning) sources of primary organic aerosols influence the levels of ambient particles that children are exposed at the schools. These results have implications for potential control strategies for mitigating exposure at schools. Copyright © 2014 Elsevier Ltd. All rights reserved.

On the spatial distribution and evolution of ultrafine particles in Barcelona

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Alastuey, A.; O'Dowd, C.; Harrison, R. M.; Wenger, J.; Gómez-Moreno, F. J.

2013-01-01

Sources and evolution of ultrafine particles were investigated both horizontally and vertically in the large urban agglomerate of Barcelona, Spain. Within the SAPUSS project (Solving Aerosol Problems by Using Synergistic Strategies), a large number of instruments was deployed simultaneously at different monitoring sites (road, two urban background, regional background, urban tower 150 m a.s.l., urban background tower site 80 m a.s.l.) during a 4 week period in September-October 2010. Particle number concentrations (N>5 nm) are highly correlated with black carbon (BC) at all sites only under strong vehicular traffic influences. By contrast, under cleaner atmospheric conditions (low condensation sink, CS) such correlation diverges towards much higher N/BC ratios at all sites, indicating additional sources of particles including secondary production of freshly nucleated particles. Size-resolved aerosol distributions (N10-500) as well as particle number concentrations (N>5 nm) allow us to identify three types of nucleation and growth events: (1) a regional type event originating in the whole study region and impacting almost simultaneously the urban city of Barcelona and the surrounding urban background area; (2) a regional type event impacting only the regional background area but not the urban agglomerate; (3) an urban type event which originates only within the city centre but whose growth continues while transported away from the city to the regional background. Furthermore, during these clean air days, higher N are found at tower level than at ground level only in the city centre whereas such a difference is not so pronounced at the remote urban background tower. In other words, this study suggests that the column of air above the city ground level possesses the optimal combination between low CS and high vapour source, hence enhancing the concentrations of freshly nucleated particles. By contrast, within stagnant polluted atmospheric conditions, higher N and BC concentrations are always measured at ground level relative to tower level at all sites. Our study suggests that the city centre of Barcelona is a source of non-volatile traffic primary particles (29-39% of N>5 nm), but other sources, including secondary freshly nucleated particles contribute up to 61-71% of particle number (N>5 nm) at all sites. We suggest that organic compounds evaporating from freshly emitted traffic particles are a possible candidate for new particle formation within the city and urban plume.

Impact of particle emissions of new laser printers on modeled office room

NASA Astrophysics Data System (ADS)

Koivisto, Antti J.; Hussein, Tareq; Niemelä, Raimo; Tuomi, Timo; Hämeri, Kaarle

2010-06-01

In this study, we present how an indoor aerosol model can be used to characterize particle emitter and predict influence of the source on indoor air quality. Particle size-resolved emission rates were quantified and the source's influence on indoor air quality was estimated by using office model simulations. We measured particle emissions from three modern laser printers in a flow-through chamber. Measured parameters were used as input parameters for an indoor aerosol model, which we then used to quantify the particle emission rates. The same indoor aerosol model was used to simulate the effect of the particle emission source inside an office model. The office model consists of a mechanically ventilated empty room and the particle source. The aerosol from the ventilation air was a filtered urban background aerosol. The effect of the ventilation rate was studied using three different ventilation ratios 1, 2 and 3 h -1. According to the model, peak emission rates of the printers exceeded 7.0 × 10 8 s -1 (2.5 × 10 12 h -1), and emitted mainly ultrafine particles (diameter less than 100 nm). The office model simulation results indicate that a print job increases ultrafine particle concentration to a maximum of 2.6 × 10 5 cm -3. Printer-emitted particles increased 6-h averaged particle concentration over eleven times compared to the background particle concentration.

Characterization of a Quadrotor Unmanned Aircraft System for Aerosol-Particle-Concentration Measurements.

PubMed

Brady, James M; Stokes, M Dale; Bonnardel, Jim; Bertram, Timothy H

2016-02-02

High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking.

SEM Imaging and Chemical Analysis of Aerosol Particles from Surface and Hi-altitudes in New Jersey.

NASA Astrophysics Data System (ADS)

Bandamede, M.; Boaggio, K.; Bancroft, L.; Hurler, K.; Magee, N. B.

2016-12-01

We report on Scanning Electron Microscopy analysis of aerosol particle morphology and chemistry. The work includes the first comparative SEM analysis of aerosol particles captured by balloon at high altitude. The particles were acquired in an urban/suburban environment in central New-Jersey. Particles were sampled from near the surface using ambient air filtration and at high-altitudes using a novel balloon-borne instrument (ICE-Ball, see abstract by K. Boaggio). Particle images and 3D geometry are acquired by a Hitachi SU-5000 SEM, with resolution to approximately 3 nm. Elemental analysis on particles is provided by Energy Dispersive X-Ray Spectroscopy (EDS, EDAX, Inc.). Uncoated imaging is conducted in low vacuum within the variable-pressure SEM, which provides improved detection and analysis of light-element compositions including Carbon. Preliminary results suggest that some similar particle types and chemical species are sampled at both surface and high-altitude. However, as expected, particle morphologies, concentrations, chemistry, and apparent origin vary significantly at different altitudes and under different atmospheric flow regimes. Improved characterization of high-altitude aerosol particles, and differences from surface particulate composition, may advance inputs for atmospheric cloud and radiation models.

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China.

PubMed

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Li, Lei

2018-02-01

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer (AMS) and Single Particle Aerosol Mass Spectrometer (SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2-1.0μm, accounting for over 97% of the total particles measured by both instruments. Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH 4 + was obtained by AMS, while extremely low value of NH 4 + was detected by SPAMS. Contrarily, high particle number counts of NO 3 - and Cl - were given by SPAMS while low concentrations of NO 3 - and Cl - were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments. Copyright © 2017. Published by Elsevier B.V.

Diurnal and seasonal trends and source apportionment of redox-active metals in Los Angeles using a novel online metal monitor and Positive Matrix Factorization (PMF)

NASA Astrophysics Data System (ADS)

Mousavi, Amirhosein; Sowlat, Mohammad H.; Sioutas, Constantinos

2018-02-01

In the present study, we identified the sources of four redox-active metals, including Iron (Fe), Chromium (Cr), Cupper (Cu), and Manganese (Mn) and quantified the contribution of these sources to PM2.5 concentrations in central Los Angeles, California, by employing time-resolved measurements (i.e., a time resolution of 2 h) with a recently developed online metal monitor and Positive Matrix Factorization (PMF). Size distribution of ambient PM (14 nm-10 μm) was measured using the Scanning Mobility Particle Sizer (SMPS) and Optical Particle Sizer (OPS). Auxiliary variables were also collected, including elemental (EC) and organic carbon (OC), gaseous pollutants (NO2 and O3), meteorological parameters (including relative humidity (RH) and temperature), and traffic data (for heavy- (HDVs) and light-duty vehicles (LDVs)). A 4-factor solution was found to be optimum for the chemically-speciated dataset, whereas a 5-factor solution appeared to be most plausible for the size distribution data. The factors included fresh traffic, soil/road dust, urban background aerosol, secondary aerosol, and nucleation (only resolved for the size distribution data). Fresh traffic was the major contributor to Fe and Cu concentrations, whereas Cr was mostly found in the urban background aerosol (reflecting a mixture of small local sources as well as aged traffic emissions), and Mn mostly came from both soil/road dust and was to a lesser degree found in urban background aerosol. Secondary aerosol did not contribute to the concentrations of any of these metals, but was associated with very high loading of OC, as expected. Even though the urban background aerosol and secondary aerosol appeared to be characterized by "aged" particles and have a rather homogeneous spatial distribution, the reactions and processes involved in their formation are entirely different. Our results provide insights into the sources of redox-active metals in central Los Angeles. They also underscore the benefits of novel measurement techniques for PM-bound metals, which could enhance our understanding of the sources of atmospheric aerosols by providing us with measurements with finer time resolutions that otherwise would not have been possible using traditional filter-based measurement techniques.

Hygroscopic properties of ultrafine particles at an urban site in northern Japan during the summer of 2011

NASA Astrophysics Data System (ADS)

Jung, Jinsang; Kawamura, Kimitaka

2013-04-01

To investigate the hygroscopic property of ultrafine particles, hygroscopic growth factors [g(RH)] of size-segregated atmospheric particles were measured at an urban site in Sapporo, northern Japan, during the summer of 2011. Hygroscopic growth factors at 85% RH [g(85%)] of freshly formed nucleation mode particles ranged from 1.11 to 1.28 with an average of 1.16 ± 0.06. These values are similar to those of secondary organic aerosols, suggesting that low volatile organic vapors are important to the growth of nucleated clusters into quasi-stable aerosol particles larger than 3 nm. Higher g(85%) values (range: 1.21-1.31, AVG: 1.27 ± 0.04) were obtained for grown Aitken mode nucleated particles. This result may indicate that the growth of freshly formed nucleation mode particles to the Aitken mode particles at the urban site can be attributed to condensation not only of low volatility organic vapors but also of highly water-soluble inorganic compounds like sulfuric acid. Diel variations in the number concentrations of less-hygroscopic particles [g(85%) <1.05] were similar to those in NO concentrations, suggesting that less-hygroscopic particles are mainly produced by local anthropogenic emissions such as traffic. Higher g(85%) values (1.27 ± 0.05) were obtained at a dry particle diameter of 120 nm when the air masses originated from downwind areas of the Asian continent, whereas lower g(85%) values (1.19 ± 0.06) were obtained when clean marine air masses arrived in the urban site. These results indicate that the hygroscopic property of large Aitken and small accumulation mode particles (80-165 nm) are highly influenced by the long-range transport of atmospheric particles.

Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

NASA Technical Reports Server (NTRS)

Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

2013-01-01

Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

Aerosol and Urban Land Use Effect on Rainfall Around Cities in Indo-Gangetic Basin From Observations and Cloud Resolving Model Simulations

NASA Astrophysics Data System (ADS)

Sarangi, Chandan; Tripathi, S. N.; Qian, Yun; Kumar, Shailendra; Ruby Leung, L.

2018-04-01

Coupling of urban land use land cover (LULC) and aerosol loading on rainfall around cities in the Gangetic Basin (GB) is examined here. Long-term observations illustrate more rainfall at urban core and climatological downwind regions compared to the upwind regions of Kanpur, a metropolitan area located in central GB. In addition, analysis of a 15 day cloud resolving simulation using the Weather Research and Forecasting model also illustrated similar rainfall pattern around other major cities in the GB. Interestingly, the enhancement of downwind rainfall was greater than that over urban regions, and it was positively associated with both the urban area of the city and ambient aerosol loading during the propagating storm. Further, to gain a process-level understanding, a typical storm that propagated northwestward across Kanpur was simulated using Weather Research and Forecasting under three different scenarios. Case 1 has realistic LULC representation of Kanpur, while the grids representing the Kanpur urban region were replaced by cropland LULC pattern in Case 2. Comparison illustrated that urban heat island effect caused convergence of winds and moisture in the lower troposphere, which enhances convection over urban region and induced more rainfall over the urban core compared to upwind regions. Case 3 is similar to Case 1 but lower aerosol concentration (by a factor of 100) over the storm region. Analysis shows that aerosol-induced microphysical changes delay the initiation of warm rain (over the upwind region) but enhance ice phase particle formation in latter stages (over the urban and downwind regions) resulting in increase in downwind rainfall.

Seasonal variabilities in chemical compounds and acidity of aerosol particles at urban site in the west Pacific.

PubMed

Pan, Xiaole; Uno, Itsushi; Wang, Zhe; Yamamoto, Shigekazu; Hara, Yukari; Wang, Zifa

2018-06-01

Mass concentrations of chemical compounds in both PM 2.5 (particle aerodynamic diameter, Dp < 2.5 μm) and PM 2.5-10 (2.5 < Dp < 10 μm), and acidity of aerosol particles were measured at an urban site in western Japan using a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-12) throughout 2014. Mass concentrations of both PM 2.5 and sulfate had distinct seasonal variabilities with maxima in spring and winter, mostly due to long-range transport with the prevailing westerly wind. Mass concentration of nitrate in PM 2.5 (fNO 3 ) showed an obvious warm-season-low and cold-season-high pattern as a result of both gas-aerosol phase equilibrium processes under high temperature conditions as well as transport. Nitrate in PM 2.5-10 (cNO 3 ) increased during long-range transport of dust, implying the great importance of heterogeneous processes at the surface of coarse mode particles. In this study, Δ[H + ] (derived from the difference in pH of extract liquid with/without sampling) was used to indicate the acidity of particles. We found that acidity of particles in PM 2.5 (fΔH) was mostly positive with a maximum in August because of the large fraction of nitrate and sulfate. Acidity of particles in PM 2.5-10 (cΔH) was negative in winter and spring due to presence of alkaline matter from crustal sources. This study highlights the great importance of anthropogenic pollutants on the acidity of particles in the western Pacific Ocean and further impact on the marine environment and climate. Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Petäjä, T

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. Themore » formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.« less

Experimental investigation of aerosol composition and growth rates

NASA Astrophysics Data System (ADS)

Wimmer, Daniela; Winkler, Paul; Kulmala, Markku; Petäjä, Tuukka

2017-04-01

Atmospheric aerosol particles have relevant influence on human lives. Human health is affected, as by breathing in the aerosol particles, they deposit in the lungs causing various health problems. Also they interfere indirectly and directly with sunlight, which affects the climate on Earth. Primary aerosol particles originate for example from anthropogenic sources, such as Diesel cars or natural sources such as dessert dust. Secondary aerosol particles are formed via condensation of low volatile gas phase compounds. First, small clusters consisting of a few gas molecules only are formed, which can then grow to bigger aerosol particles. These then form seeds for cloud droplets. The chemical composition of the cloud particles determines whether the cloud absorbs or scatters sunlight more. Intensive experimental and theoretical work has been put into understanding the details of the initial processes leading to the natural formation of these secondary aerosol particles. According to modelling studies, aerosol particles formed via the nucleation process are responsible for about 50% of the global cloud condensation nuclei concentration. With currently used methods, the chemical composition of small molecular clusters (up to 2nm in diameter) can be resolved. Also standard methods to determine aerosol particle composition at sizes >10 nm are available. Within this project, the aerosol particle composition in the 2-4 nm size range will be investigated experimentally. The setup will consist of a combination of an electrical method that allows determine the electrical mobility of the particles which then can be converted to a diameter. By letting the charged particles travel through a changing electrical field, they travel at different speeds according to their mobility. That allows to particles with certain mobilities, which then can be converted to a diameter. After the size selection, the particles are counted by means of optical detection. Condensation particle counters (CPCs) grow the particles internally, after which they are detected optically. By changing the condensing liquid, depending on the aerosol particle composition, they are activated differently. By combining the electrical size selection with CPCs with different liquids, information about particle composition can be determined. The project includes laboratory studies and field measurements in different locations (one rural site and two urban sites). I wish to acknowledge the Austrian Science Fund (FWF; Grant No J3951 - N36).

Gas- and particle-phase chemical composition measurements onboard the G-1 research aircraft during the GoAmazon campaign.

NASA Astrophysics Data System (ADS)

Shilling, J.; Pekour, M. S.; Fortner, E.; Hubbe, J. M.; Longo, K.; Martin, S. T.; Mei, F.; Springston, S. R.; Tomlinson, J. M.; Wang, J.

2014-12-01

The Green Ocean Amazon (GoAmazon) campaign conducted from January 2014 - December 2015 in the vicinity of Manaus, Brazil, was designed to study the aerosol lifecycle and aerosol-cloud interactions in both pristine and anthropogenically influenced conditions. As part of this campaign, the DOE G-1 research aircraft was deployed from February 17th - March 25th 2014 and September 6th - October 5th 2014 to investigate aerosol and cloud properties aloft. An Aerodyne High Resolution Aerosol Mass Spectrometer (AMS) and an Ionicon Proton Transfer Reaction Mass Spectrometer (PTRMS) were part of the G-1 research aircraft payload and were used to investigate aerosol gas- and particle-phase chemical composition. Here we present preliminary analysis of the aerosol and gas phase chemical composition. PTR-MS measurements show that isoprene and its oxidation products are the dominant VOCs during research flights. HR-AMS measurements reveal that the particle phase is dominated by organic material with smaller concentrations of sulfate and nitrate observed. Organic particle concentrations are enhanced when encountering the urban plume from Manaus. During the wet season, we observe increased concentrations of organic particle when passing through low-altitude clouds. PMF analysis of the organic mass spectra shows that the chemical composition of the particles observed in-cloud is distinctly different from particles observed outside clouds. We will also compare measurements made during the wet and dry seasons.

Changes of ns-soot mixing states and shapes in an urban area during CalNex

NASA Astrophysics Data System (ADS)

Adachi, Kouji; Buseck, Peter R.

2013-05-01

Aerosol particles from megacities influence the regional and global climate as well as the health of their occupants. We used transmission electron microscopes (TEMs) to study aerosol particles collected from the Los Angeles area during the 2010 CalNex campaign. We detected major amounts of ns-soot, defined as consisting of carbon nanospheres, sulfate, sea salt, and organic aerosol (OA) and lesser amounts of brochosome particles from leaf hoppers. Ns-soot-particle shapes, mixing states, and abundances varied significantly with sampling times and days. Within plumes having high CO2 concentrations, much ns-soot was compacted and contained a relatively large number of carbon nanospheres. Ns-soot particles from both CalNex samples and Mexico City, the latter collected in 2006, had a wide range of shapes when mixed with other aerosol particles, but neither sets showed spherical ns-soot nor the core-shell configuration that is commonly used in optical calculations. Our TEM observations and light-absorption calculations of modeled particles indicate that, in contrast to ns-soot particles that are embedded within other materials or have the hypothesized core-shell configurations, those attached to other aerosol particles hardly enhance their light absorption. We conclude that the ways in which ns-soot mixes with other particles explain the observations of smaller light amplification by ns-soot coatings than model calculations during the CalNex campaign and presumably in other areas.

Satellite and in-situ monitoring of urban air pollution in relation with children's asthma

NASA Astrophysics Data System (ADS)

Dida, Mariana R.; Zoran, Maria A.

2013-10-01

Urban air pollution and especially aerosols have significant negative health effects on urban population, of which children are most exposed for the rapid increase of asthma disease. An allergic reaction to different allergens is a major contributor to asthma in urban children, but new research suggests that the allergies are just one part of a more complex story. Very early exposure to certain components of air pollution can increase the risk of developing of different allergies by age 7. The epidemiological research on the mutagenic effects of airborne particulate matter pointed their capability to reach deep lung regions, being vehicles of toxic substances. The current study presents a spatio-temporal analysis of the aerosol concentrations in relation with meteorological parameters in two size fractions (PM10 and PM2.5) and possible health effects in Bucharest metropolitan area. Both in-situ monitoring data as well as MODIS Terra/Aqua time-series satellite data of particle matter PM2.5 and PM10 concentrations have been used to qualitatively assess distribution of aerosols in the greater metropolitan are of Bucharest comparative with some other little towns in Romania during 2010- 2011 period. It was found that PM2.5 and PM10 aerosols exhibit their highest concentration mostly in the central part of the towns, mainly due to road traffic as well as in the industrialized parts outside of city's centre. Pediatric asthma can be managed through medications prescribed by a healthcare provider, but the most important aspect is to avoid urban locations with high air pollution concentrations of air particles and allergens.

Weighted Flow Algorithms (WFA) for stochastic particle coagulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

DeVille, R.E.L., E-mail: rdeville@illinois.edu; Riemer, N., E-mail: nriemer@illinois.edu; West, M., E-mail: mwest@illinois.edu

2011-09-20

Stochastic particle-resolved methods are a useful way to compute the time evolution of the multi-dimensional size distribution of atmospheric aerosol particles. An effective approach to improve the efficiency of such models is the use of weighted computational particles. Here we introduce particle weighting functions that are power laws in particle size to the recently-developed particle-resolved model PartMC-MOSAIC and present the mathematical formalism of these Weighted Flow Algorithms (WFA) for particle coagulation and growth. We apply this to an urban plume scenario that simulates a particle population undergoing emission of different particle types, dilution, coagulation and aerosol chemistry along a Lagrangianmore » trajectory. We quantify the performance of the Weighted Flow Algorithm for number and mass-based quantities of relevance for atmospheric sciences applications.« less

Weighted Flow Algorithms (WFA) for stochastic particle coagulation

NASA Astrophysics Data System (ADS)

DeVille, R. E. L.; Riemer, N.; West, M.

2011-09-01

Stochastic particle-resolved methods are a useful way to compute the time evolution of the multi-dimensional size distribution of atmospheric aerosol particles. An effective approach to improve the efficiency of such models is the use of weighted computational particles. Here we introduce particle weighting functions that are power laws in particle size to the recently-developed particle-resolved model PartMC-MOSAIC and present the mathematical formalism of these Weighted Flow Algorithms (WFA) for particle coagulation and growth. We apply this to an urban plume scenario that simulates a particle population undergoing emission of different particle types, dilution, coagulation and aerosol chemistry along a Lagrangian trajectory. We quantify the performance of the Weighted Flow Algorithm for number and mass-based quantities of relevance for atmospheric sciences applications.

Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

NASA Astrophysics Data System (ADS)

Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

2014-12-01

Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could reflect differences in their viscosity.

Development and evaluation of the aerosol dynamic and gas phase chemistry model ADCHEM

NASA Astrophysics Data System (ADS)

Roldin, P.; Swietlicki, E.; Schurgers, G.; Arneth, A.; Lehtinen, K. E. J.; Boy, M.; Kulmala, M.

2010-08-01

The aim of this work was to develop a model ideally suited for detailed studies on aerosol dynamics, gas and particle phase chemistry within urban plumes, from local scale (1×1 km2) to regional or global scale. This article describes and evaluates the trajectory model for Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer (ADCHEM), which has been developed and used at Lund University since 2007. The model treats both vertical and horizontal dispersion perpendicular to an air mass trajectory (2-space dimensions), which is not treated in Lagrangian box-models (0-space dimensions). The Lagrangian approach enables a more detailed representation of the aerosol dynamics, gas and particle phase chemistry and a finer spatial and temporal resolution compared to that of available regional 3D-CTMs. These features make it among others ideally suited for urban plume studies. The aerosol dynamics model includes Brownian coagulation, dry deposition, wet deposition, in-cloud processing, condensation, evaporation, primary particle emissions and homogeneous nucleation. The gas phase chemistry model calculates the gas phase concentrations of 63 different species, using 119 different chemical reactions. Daily isoprene and monoterpene emissions from European forests were simulated separately with the vegetation model LPJ-GUESS, and included as input to ADCHEM. ADCHEM was used to simulate the ageing of the urban plumes from the city of Malmö in Southern Sweden (280 000 inhabitants). Several sensitivity tests were performed concerning the number of size bins, size structure method, coupled or uncoupled condensation, the volatility basis set (VBS) or traditional 2-product model for secondary organic aerosol formation, different aerosol dynamic processes and vertical and horizontal mixing. The simulations show that the full-stationary size structure gives accurate results with little numerical diffusion when more than 50 size bins are used between 1.5 and 2500 nm, while the moving-center method is preferable when only a few size bins are selected. The particle number size distribution in the center of the urban plume from Malmö is mainly affected by dry deposition, coagulation and condensation, and is relatively insensitive to moderate variations in the vertical and horizontal mixing, as long as the mixing height is relatively uniform. The modeled PM2.5 was dominated by organics, nitrate, sulfate and ammonium. If treating the condensation of HNO3 and NH3 as a coupled process (pH independent) the model gave lower nitrate PM2.5 values than if considering uncoupled condensation. However, both methods gave similar and significant temporal variation in the particulate nitrate content, primarily due to fluctuation in the relative humidity.

NMOC, ozone, and organic aerosol in the southeastern United States, 1999-2007: 3. Origins of organic aerosol in Atlanta, Georgia, and surrounding areas

NASA Astrophysics Data System (ADS)

Blanchard, C. L.; Hidy, G. M.; Tanenbaum, S.; Edgerton, E. S.

2011-02-01

Carbonaceous compounds constitute a major fraction of the fine particle mass at locations throughout North America; much of the condensed-phase organic carbon (OC) is produced in the atmosphere from NMOC reactions as "secondary" OC (SOC). Ten years of particulate carbon and speciated non-methane organic compound (NMOC) data combined with other measurements from Southeastern Aerosol Research and Characterization (SEARCH) and other sites provide insight into the association between elemental carbon (EC), OC and NMOCs. Data are analyzed to characterize the OC and SOC contrasts between urban Atlanta, Georgia, and nearby non-urban conditions in the Southeast. Analysis of the monitoring record indicates that the mean Atlanta urban excess of total carbon (TC) is 2.1-2.8 μg m -3. The OC/EC ratio of the Atlanta urban excess is in the range 1.3 to 1.8, consistent with OC/EC ratios observed in motor vehicle emissions and a fossil carbon source of urban excess TC. Carbon isotope analysis of a subset of particle samples demonstrates that the urban excess is mainly fossil in origin, even though the majority of the TC is modern at both urban and non-urban sites. Temperature-dependent partitioning of OC between gas and condensed phases cannot explain the observed diurnal and seasonal variations of OC/CO, EC/CO, and OC/EC ratios. Alternatively, a hypothesis involving vertical mixing of OC-enriched air from aloft is supported by the seasonal and diurnal OC, isopentane, aromatic and isoprene observations at the ground. A statistical model is applied to indicate the relative significance of aerometric factors affecting OC and EC concentrations, including meteorological and pollutant associations. The model results demonstrate strong linkages between fine particle carbon and pollutant indicators of source emissions compared with meteorological factors; the model results show weaker dependence of OC on meteorological factors than is the case for ozone (O 3) concentrations.

Characterization of Cooking-Related Aerosols

NASA Astrophysics Data System (ADS)

Niedziela, R. F.; Blanc, L. E.

2010-12-01

The temperatures at which food is cooked are usually high enough to drive oils and other organic compounds out of materials which are being prepared for consumption. As these compounds move away from the hot cooking surface and into the atmosphere, they can participate in chemical reactions or condense to form particles. Given the high concentration of cooking in urban areas, cooking-related aerosols likely contribute to the overall amount of particulate matter on a local scale. Reported here are results for the mid-infrared optical characterization of aerosols formed during the cooking of several meat and vegetable samples in an inert atmosphere. The samples were heated in a novel aerosol generator that is designed to collect particles formed immediately above the cooking surface and inject them into a laminar aerosol flow cell. Preliminary results for the chemical processing of cooking-related aerosols in synthetic air will also be presented.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

NASA Astrophysics Data System (ADS)

Enroth, Joonas; Mikkilä, Jyri; Németh, Zoltán; Kulmala, Markku; Salma, Imre

2018-04-01

Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a volatility-hygroscopicity tandem differential mobility analyser (VH-TDMA) system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014-2015. The probability density function of the hygroscopic growth factor (HGF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033) independently of the particle size and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF) also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The hygroscopic particles were ordinarily volatile. They could be composed of moderately transformed aged combustion particles consisting of partly oxygenated organics, inorganic salts and soot. The larger particles contained internally mixed non-volatile chemical species as a refractory residual in 20-25 % of the aerosol material (by volume).

Size distribution of ions in atmospheric aerosols

NASA Astrophysics Data System (ADS)

Krivácsy, Z.; Molnár, Á.

The aim of this paper is to present data about the concentration and size distribution of ions in atmospheric aerosol under slightly polluted urban conditions in Hungary. Concentration of inorganic cations (ammonium, sodium, potassium, calcium, magnesium), inorganic anions (sulfate, nitrate, chloride, carbonate) and organic acids (oxalic, malonic, succinic, formic and acetic acid) for 8 particle size range between 0.0625 and 16 μm were determined. As was the case for ammonium, sulfate and nitrate, the organic acids were mostly found in the fine particle size range. Potassium and chloride were rather uniformly distributed between fine and coarse particles. Sodium, calcium, magnesium and carbonate were practically observed in the coarse mode. The results obtained for the summer and the winter half-year were also compared. The mass concentrations were recalculated in equivalents, and the ion balance was found to be reasonable in most cases. Measurement of the pH of the aerosol extracts indicates that the aerosol is acidic in the fine mode, but alkaline in the coarse particle size range.

Biogenic Aerosols—Effects on Clouds and Climate (BAECC) Final Campaign Summary

DOE Office of Scientific and Technical Information (OSTI.GOV)

Petäjä, T; Moisseev, D; Sinclair, V

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the Northern latitudes throughout the United States, Canada, Russia, and Scandinavia, are, of all biomes, among the most active areas of atmospheric aerosol formation. Themore » formation of aerosol particles and their growth to cloud condensation nuclei sizes in these areas are associated with biogenic volatile organic emissions (BVOC) from vegetation and soil.« less

Urban aerosol particles of Santiago, Chile:. organic content and molecular characterization

NASA Astrophysics Data System (ADS)

Didyk, Borys M.; Simoneit, Bernd R. T.; Alvaro Pezoa, L.; Luis Riveros, M.; Anselmo Flores, A.

Santiago, Chile has developed a significant problem of atmospheric contamination with high levels of total suspended aerosol particles consisting of a high PM-10 fraction. This is associated with a growing economy, rapid urban expansion, increasing rate of motorization and expanding industrial activity. The organic contribution to atmospheric suspended particles (PM-10) in Santiago has been quantitated, characterized and related to its input sources in this report. The average organic content of 38% is significantly lower from pre-regulatory levels of 71% and in the range reported for other urban centers. Molecular markers indicate that a predominant proportion of the organic compounds associated with the particluate matter are derived from uncombusted diesel, uncombusted lubricating oil and other petrochemical fuel use. A significant organic contribution from natural plant wax hydrocarbons is also detected, suggesting biomass fuel use, open burning of vegetation in incidental fires or agricultural practices and resuspension of weathered vegetation debris. Aromatic hydrocarbon fractions indicate the presence of pyrogenic PAH formed by high-temperature combustion processes of petrochemical fuels with a significant contribution of retene indicative of conifer wood combustion. Maturity indicators, based on methylphenanthrene indexes, also indicate the simultaneous concurrence of high- and low-temperature combustion processes and confirm a significant contribution of non-petrochemical-sourced organic compounds to the atmospheric aerosols. Benzopyrene ratios indicate that Santiago aerosols are freshly generated and do not have an extensive solar exposure. The present study provides a reference baseline for the organic components relating to air quality in Santiago, and will permit the assessment of the environmental effectiveness of corrective measures related to energy usage and transport administration.

Overview of balloon-borne aerosol measurements with the aerosol counter LOAC, with focus on the ChArMEx 2013 campaign

NASA Astrophysics Data System (ADS)

Dulac, François; Renard, Jean-Baptiste

LOAC (Light Optical Aerosol Counter) is a new small optical particle counter/sizer of 250 grams designed to fly under all kinds of balloons. The measurements are conducted at two scattering angles: the first one, at 12°, is used to determine the aerosol particle concentrations in 19 size classes within a diameter range of 0.2-100 mm; the second angle, at 60°, is used to discriminate between different types of particles dominating different size classes. The sensor particularly discriminates wet or liquid particles, mineral dust, soot carbon particles and salts. Comparisons with measurements from other sensors at the surface are shown. We shall give a quick review of balloon-borne experiences since 2011 with LOAC under all kinds of balloons including tethered, sounding, open stratospheric, and new boundary-layer pressurized drifting balloons (BLBP) from CNES. Observation domains include the atmospheric surface layer, the boundary layer, the free troposphere and the lower stratosphere up to more than 35 km in altitude. Operations encompass a variety of environments including the Arctic (Reykjavik, Island, and Kiruna, Sweden), Brazil (Sao Paolo), the western Mediterranean Basin, southwestern France, peri-urban (Ile de France) and urban areas (Paris and Vienna). Results from the various campaigns will be illustrated including the study of fog events, urban aerosols, Saharan dust transport over France, stratospheric soot... Emphasis will be put on the ChArMEx campaign (the Chemistry-Aerosol Mediterranean Experiment) performed in summer 2013 in the Mediterranean basin: 19 LOAC flights have been performed under meteorological balloons and 12 under low altitude drifting balloons, most of them from Minorca Island (Spain) in June and early July and others from Levant Island (south of France) in late July and early August. Most of the flights were coupled with ozone concentration measurements (see presentation by F. Gheusi et al.). LOAC balloons were especially, but not only, dedicated to study the various Saharan dust events that occurred during the campaign. In particular, a series of flights were conducted every 12 hours during the 15-19 June dust event. Forest fire smoke from North America was also sampled in late June over Minorca, as well as anthropogenic polluted layers in various occasions. LOAC data are used to identify the various turbid layers with the help of coincident lidar and sun photometer remote sensing measurements in Menorca and air mass trajectories. The sounding flights allow one to determine the vertical extent of the various aerosol layers, and to follow the particle size distribution and the concentration evolution along the vertical. The low altitude drifting balloons, which stayed roughly at constant altitude between 350 and 3330 m up to more than 25 h, allow us to study the time-evolution of the aerosol concentrations in the same air mass. Under both balloon types, LOAC has detected larges particles up to 30 mum in diameter. The flights drifting within dust layers indicate that there is a relatively stable particle size distribution during transport over the sea, with no clear sedimentation loss of large particles.

A Study of The Direct Aerosol Forcing At Ground Level For A Pollution Event During The Escompte Campaign

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Dubuisson, P.; Putaud, J. P.; van Dingenen, R.; Despiau, S.

Radiative forcing by aerosol particles is one of the largest source of uncertainties in predicting climate change (IPCC, 2001). Indeed, quantitative estimates of this effect are still uncertain due to little knowledge of these atmospheric particles. Atmospheric particles influence the Earth's radiation balance both directly and indirectly. The indi- rect effect denotes the effect of aerosols acting as cloud condensation nuclei, possibly modifying cloud albedo and cloud lifetime. The direct effect is due to scattering and absorption of radiation and each of these processes depends mainly on the refractive index and the size distribution of aerosol particles. During the ESCOMPTE campaign, which took place in coastal Mediterranean area during the summer 2001, we estimated these aerosol micro-physical properties during a pollution event at two different sites. The first is an urban site (the city of Marseille), and the second is a rural area located fifty kilometers inland. The aerosol size distribution was measured with an SMPS for the particles with radii < 1 µm, and an optical counter for r > 1 µm. The chemi- cal composition (including different ionic compounds , dust, elemental and organic carbon) was deduced from chromatography analysis. The aerosol optical properties calculated from measured aerosol physical and chemical properties at ground level (from Mie theory) are used as input to a shortwave radiative transfer model. Then, this model is used to calculate the diurnally averaged direct aerosol forcing at surface and to compare this values with those measured from the ARAT aircraft and surface pyranometer during the campaign.

Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

NASA Astrophysics Data System (ADS)

Zhang, Y. M.; Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Gong, S. L.; Shen, X. J.; Yang, S.

2011-07-01

Size-resolved aerosol number and mass concentrations and the mixing ratios of O3 and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM1) and sulphate; nitrate and ammonium were more minor contributors.

Overview of atmospheric aerosol studies in Malaysia: Known and unknown

NASA Astrophysics Data System (ADS)

Kanniah, Kasturi Devi; Kaskaoutis, Dimitris G.; San Lim, Hwee; Latif, Mohd Talib; Kamarul Zaman, Nurul Amalin Fatihah; Liew, Juneng

2016-12-01

Atmospheric aerosols particularly those originated from anthropogenic sources can affect human health, air quality and the regional climate system of Southeast Asia (SEA). Population growth, and rapid urbanization associated with economic development in the SEA countries including Malaysia have resulted in high aerosol concentrations. Moreover, transboundary smoke plumes add more aerosols to the atmosphere in Malaysia. Nevertheless, the aerosol monitoring networks and/or field studies and research campaigns investigating the various aerosol properties are not so widespread over Malaysia. In the present work, we summarize and discuss the results of previous studies that investigated the aerosol properties over Malaysia by means of various instrumentation and techniques, focusing on the use of remote sensing data to examine atmospheric aerosols. Furthermore, we identify gaps in this research field and recommend further studies to bridge these knowledge gaps. More specifically gaps are identified in (i) monitoring aerosol loading and composition over urban areas, (ii) examining the influence of dust, (iii) assessing radiative effects of aerosols, (iv) measuring and modelling fine particles and (v) quantifying the contribution of long range transport of aerosols. Such studies are crucial for understanding the optical, physical and chemical properties of aerosols and their spatio-temporal characteristics over the region, which are useful for modelling and prediction of aerosols' effects on air quality and climate system.

A study of remotely sensed aerosol properties from ground-based sun and sky scanning radiometers

NASA Astrophysics Data System (ADS)

Giles, David M.

Aerosol particles impact human health by degrading air quality and affect climate by heating or cooling the atmosphere. The Indo-Gangetic Plain (IGP) of Northern India, one of the most populous regions in the world, produces and is impacted by a variety of aerosols including pollution, smoke, dust, and mixtures of them. The NASA Aerosol Robotic Network (AERONET) mesoscale distribution of Sun and sky-pointing instruments in India was established to measure aerosol characteristics at sites across the IGP and around Kanpur, India, a large urban and industrial center in the IGP, during the 2008 pre-monsoon (April-June). This study focused on detecting spatial and temporal variability of aerosols, validating satellite retrievals, and classifying the dominant aerosol mixing states and origins. The Kanpur region typically experiences high aerosol loading due to pollution and smoke during the winter and high aerosol loading due to the addition of dust to the pollution and smoke mixture during the pre-monsoon. Aerosol emissions in Kanpur likely contribute up to 20% of the aerosol loading during the pre-monsoon over the IGP. Aerosol absorption also increases significantly downwind of Kanpur indicating the possibility of the black carbon emissions from aerosol sources such as coal-fired power plants and brick kilns. Aerosol retrievals from satellite show a high bias when compared to the mesoscale distributed instruments around Kanpur during the pre-monsoon with few high quality retrievals due to imperfect aerosol type and land surface characteristic assumptions. Aerosol type classification using the aerosol absorption, size, and shape properties can identify dominant aerosol mixing states of absorbing dust and black carbon particles. Using 19 long-term AERONET sites near various aerosol source regions (Dust, Mixed, Urban/Industrial, and Biomass Burning), aerosol absorption property statistics are expanded upon and show significant differences when compared to previous work. The sensitivity of absorption properties is evaluated and quantified with respect to aerosol retrieval uncertainty. Using clustering analysis, aerosol absorption and size relationships provide a simple method to classify aerosol mixing states and origins and potentially improve aerosol retrievals from ground-based and satellite-based instrumentation.

Aeolian Dust and Forest Fire Smoke in Urban Air

NASA Astrophysics Data System (ADS)

Brimblecombe, P.

2006-12-01

Particles of aeolian dust and forest fire smoke are now regularly detected in urban air. Although dusts are common on the Asian Pacific Rim and forest fire smoke characteristic of South East Asia they also frequently detected elsewhere. In the past dust was treated as though it was fairly inert and reactions on the surface limited to the neutralizing ability of alkaline minerals. More recent work shows that that dust has a complex organic chemistry. Observations in China found fatty acids from urban areas (oleic acid and linoleic acid from cooking) on dust derived aerosols. The fatty acids and PAHs decreased sharply after dust storms, suggesting a role for dust in removal processes. When silica particles absorb unsaturated compounds they can react with ozone and release compounds such as formaldehyde. Particles from forest fires have a similarly complex chemistry and the acid-alkaline balance may vary depend on the balance of removal rates of alkaline materials (ammonia, potassium carbonate) and inorganic and organic acids. Airborne dust and forest fire soot can contain humic like substances (HULIS) either as primary material or as secondary oxidation products of the surface of soot. This paper will report on the role polluted air masses in the generation humic materials, particularly those that are surface active. These materials of high molecular weight oxygen rich organic compounds, which exhibit a range of properties of importance in aerosols: they can form complexes with metal ions and thus enhance their solubility, photosensitize the oxidation of organic compounds and lower the surface tension of aqueous aerosols. HULIS can be oxidized to form a range of simpler acids such as formic, acetic and oxalic acid. Dust and forest fire smoke particles have a different composition and size range to that of typical urban combustion particles, so it is likely that the health impacts will be different, yet current regulation often does not recognize any significant difference.

Geochemistry of aerosols from an urban site, Varanasi, in the Eastern Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Ram, Kirpa; Norra, Stefan; Zirzov, Felix; Singh, Sunita; Mehra, Manisha; Nanad Tripathi, Sachichida

2016-04-01

PM2.5 aerosol samples were collected from an urban site, Varanasi, in the eastern Indo-Gangetic Plain on weekly basis during 19 March to 29 May 2015 (n=12), along with daily samples (n=8) during 11 to 18 March 2015 to study the geochemical and morphological features of aerosols. Samples were collected with a low volume sampler (Leckel GmbH, Germany) on the terrace of the Institute of Environment and Sustainable Development building, located in the Banaras Hindu University campus in the southern part of the city. Samples were analyzed for element concentration by Inductively Coupled Plasma Mass Spectrometry and particle morphology by Scanning Electron Microscope. PM2.5 concentration ranged between 22.3 and 70.5 μgm-3 in daily samples, whereas those varied between 52.0 and 106 μgm-3 in weekly samples. Lead, potassium, aluminum, zinc and iron have conspicuously higher concentrations with Pb concentration exceeding above the annual limit of 50 ngm-3 in four samples. First results show a trend of corresponding concentrations of chemical elements originated from anthropogenic and geogenic sources. The biogenic particles are a minor fraction of the total particulate aerosols. The Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) back trajectory analysis of air parcels indicate that the air mass for the low loaded days originate from eastern directions including the region of the gulf of Bengal, where as high aerosols concentrations in cases of air masses arriving from north-western direction transporting the air pollutants from the Gangetic Plain towards Varanasi. Black carbon (BC) concentration, measured using an microaethalometer (AE-51), exhibit a strong variability (4.4 to 8.4 μg m-3) in the University campus which are ˜20-40% lower than those measured in the Varanasi city. The carbon content was found to be high with soot particles constituting the largest part in these samples and exist as single particle as well as attachment to other particles. The Cluster analysis shows a mixture of geogenic and anthropogenic emission sources, though their contribution could not be quantified in the present study. Thus further investigations are started with continuous aerosol sampling in Varanasi.

The simulations of sulfuric acid concentration and new particle formation in an urban atmosphere in China

NASA Astrophysics Data System (ADS)

Wang, Z. B.; Hu, M.; Mogensen, D.; Yue, D. L.; Zheng, J.; Zhang, R. Y.; Liu, Y.; Yuan, B.; Li, X.; Shao, M.; Zhou, L.; Wu, Z. J.; Wiedensohler, A.; Boy, M.

2013-11-01

Simulations of sulfuric acid concentration and new particle formation are performed by using the zero-dimensional version of the model MALTE (Model to predict new Aerosol formation in the Lower TropospherE) and measurements from the Campaign of Air Quality Research in Beijing and Surrounding areas (CAREBeijing) in 2008. Chemical reactions from the Master Chemical Mechanism version 3.2 (MCM v3.2) are used in the model. High correlation (slope = 0.72, R = 0.74) between the modelled and observed sulfuric acid concentrations is found during daytime (06:00-18:00). The aerosol dynamics are simulated by the University of Helsinki Multicomponent Aerosol (UHMA) model including several nucleation mechanisms. The results indicate that the model is able to predict the on- and offset of new particle formation in an urban atmosphere in China. In addition, the number concentrations of newly formed particles in kinetic-type nucleation including homogenous homomolecular (J=K[H2SO4]2) and homogenous heteromolecular nucleation involving organic vapours (J=Khet[H2SO4][Org]) are in satisfactory agreement with the observations. However, the specific organic compounds that possibly participate in the nucleation process should be investigated in further studies. For the particle growth, only a small fraction of the oxidized total organics condense onto the particles in polluted environments. Meanwhile, the OH and O3 oxidation mechanism contribute 5.5% and 94.5% to the volume concentration of small particles, indicating the particle growth is more controlled by the precursor gases and their oxidation by O3.

Functional exploratory data analysis for high-resolution measurements of urban particulate matter.

PubMed

Ranalli, M Giovanna; Rocco, Giorgia; Jona Lasinio, Giovanna; Moroni, Beatrice; Castellini, Silvia; Crocchianti, Stefano; Cappelletti, David

2016-09-01

In this work we propose the use of functional data analysis (FDA) to deal with a very large dataset of atmospheric aerosol size distribution resolved in both space and time. Data come from a mobile measurement platform in the town of Perugia (Central Italy). An OPC (Optical Particle Counter) is integrated on a cabin of the Minimetrò, an urban transportation system, that moves along a monorail on a line transect of the town. The OPC takes a sample of air every six seconds and counts the number of particles of urban aerosols with a diameter between 0.28 μm and 10 μm and classifies such particles into 21 size bins according to their diameter. Here, we adopt a 2D functional data representation for each of the 21 spatiotemporal series. In fact, space is unidimensional since it is measured as the distance on the monorail from the base station of the Minimetrò. FDA allows for a reduction of the dimensionality of each dataset and accounts for the high space-time resolution of the data. Functional cluster analysis is then performed to search for similarities among the 21 size channels in terms of their spatiotemporal pattern. Results provide a good classification of the 21 size bins into a relatively small number of groups (between three and four) according to the season of the year. Groups including coarser particles have more similar patterns, while those including finer particles show a more different behavior according to the period of the year. Such features are consistent with the physics of atmospheric aerosol and the highlighted patterns provide a very useful ground for prospective model-based studies. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Airborne Particles: What We Have Learned About Their Role in Climate from Remote Sensing, and Prospects for Future Advances

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.

2013-01-01

Desert dust, wildfire smoke, volcanic ash, biogenic and urban pollution particles, all affect the regional-scale climate of Earth in places and at times; some have global-scale impacts on the column radiation balance, cloud properties, atmospheric stability structure, and circulation patterns. Remote sensing has played a central role in identifying the sources and transports of airborne particles, mapping their three-dimensional distribution and variability, quantifying their amount, and constraining aerosol air mass type. The measurements obtained from remote sensing have strengths and limitations, and their value for characterizing Earths environment is enhanced immensely when they are combined with direct, in situ observations, and used to constrain aerosol transport and climate models. A similar approach has been taken to study the role particles play in determining the climate of Mars, though based on far fewer observations. This presentation will focus what we have learned from remote sensing about the impacts aerosol have on Earths climate; a few points about how aerosols affect the climate of Mars will also be introduced, in the context of how we might assess aerosol-climate impacts more generally on other worlds.

The variability of biomass burning and its influence on regional aerosol properties during the wheat harvest season in North China

NASA Astrophysics Data System (ADS)

Wang, Lili; Xin, Jinyuan; Li, Xingru; Wang, Yuesi

2015-04-01

The spatial-temporal variation of biomass burning in June during the wheat harvest season in the North China (32-41°N, 111-120°E) and its influence on the regional aerosol optical depth (AOD) and the chemical compositions of size-segregated aerosols in the urban environment were investigated to evaluate the effectiveness of the burn ban policy and the influence on regional pollution. Fire events that occurred in early and middle June accounted for approximately 89% of the events during the month, and fire points located in mid-eastern China (32.5-35.5°N, 114-120°E) comprised 71%. The occurrences exhibit oscillatory changes with a minimum in 2008 (during the Beijing Olympics) and a peak and explosive growth in 2012. Under high relative humidity and south winds, fire emissions from straw burning combined with high urban/industrial emissions to produce intensive regional haze pollution in the North Plain. The formation of secondary inorganic particles was intensified due to the interactions of smoke plumes and urban/industrial pollutants in an urban environment. Higher concentrations and percentages (79%) of sulfate, nitrate, ammonium, and organic carbon in the fine particles under high relative humidity conditions contributed to a deteriorated urban visibility. Therefore, stronger management and a comprehensive ban on wheat straw burning in June are urgently needed, especially during years when the south wind is dominant.

Theoretical analysis of the influence of aerosol size distribution and physical activity on particle deposition pattern in human lungs.

PubMed

Voutilainen, Arto; Kaipio, Jari P; Pekkanen, Juha; Timonen, Kirsi L; Ruuskanen, Juhani

2004-01-01

A theoretical comparison of modeled particle depositions in the human respiratory tract was performed by taking into account different particle number and mass size distributions and physical activity in an urban environment. Urban-air data on particulate concentrations in the size range 10 nm-10 microm were used to estimate the hourly average particle number and mass size distribution functions. The functions were then combined with the deposition probability functions obtained from a computerized ICRP 66 deposition model of the International Commission on Radiological Protection to calculate the numbers and masses of particles deposited in five regions of the respiratory tract of a male adult. The man's physical activity and minute ventilation during the day were taken into account in the calculations. Two different mass and number size distributions of aerosol particles with equal (computed) <10 microm particle mass concentrations gave clearly different deposition patterns in the central and peripheral regions of the human respiratory tract. The deposited particle numbers and masses were much higher during the day (0700-1900) than during the night (1900-0700) because an increase in physical activity and ventilation were temporally associated with highly increased traffic-derived particles in urban outdoor air. In future analyses of the short-term associations between particulate air pollution and health, it would not only be important to take into account the outdoor-to-indoor penetration of different particle sizes and human time-activity patterns, but also actual lung deposition patterns and physical activity in significant microenvironments.

Variation of aerosol characteristics in the detail scale of time and space

NASA Astrophysics Data System (ADS)

Mukai, S.; Nakata, M.; Sano, I.

2012-04-01

In this work, we intend to demonstrate the spatial and temporal variation of atmospheric aerosols around AERONET/Osaka site. Osaka is the second big city in Japan and a typical Asian urban area. It is well known that the aerosol distribution in Asia is complicated due to the increasing emissions of anthropogenic aerosols in association with economic growth and in addition behavior of natural dusts significantly varies with the seasons. Therefore local spatially and temporally resolved measurements of atmospheric particles in Asian urban city are meaningful. We equip various ground measurement devices of atmosphere in the campus of Kinki University (KU). The data supplied by the Cimel instrument are analyzed with a standard AERONET (Aerosol Robotics Network) processing system. It provides us with Aerosol optical thickness (AOT), the Ångström exponent and so on. We set up a PM sampler and a standard instrument of NIES/LIDAR network attached to our AERONET site. The PM sampler provides particle information about the concentrations of PM2.5, PM10 and OBC separately. In addition to the simultaneous measurements, we make observation of the air quality at several locations in the neighbour-hood using portable sun-photometers (Solar-Light Company Microtops-2). The simultaneous measurements of aerosols and numerical model simulations indicate that the spatial and temporal factors influence the characterization of atmospheric particles especially in dust event. Then we observe the air quality at such several locations within a few 10 km area from KU, as Izumi and Nara, in ordinal days and dust days. Izumi site locates near industrial area and Nara is in the east of KU beyond the mountain-Ikoma. It is found from the simultaneous measurements at these three sites that AOT at Izumi in ordinal days is the highest and Nara's lowest. It indicates that the Ikoma-mountains block off the polluted air from the west. However in dust days, AOT at Nara is as large as that at Higashi-Osaka. We guess dust aerosols are transported over the mountains because dust aerosols exist higher than usual. In order to investigate change of aerosol properties before and after dust event, we analyze particulate matter with scanning electron microscope (SEM) coupled with energy dispersive X-ray analyzer (EDX). It is found from the scaling of particle size and ratio of major and minor axis for PM2.5 sampling on 21 March, 2010 when dust event occurred that at the peak of dust event nonspherical particles with large particle size are dominant. A componential analysis also presents temporal variation of aerosol properties. Sulfur is major component before dust comes but Si becomes major component with dust event.

Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

PubMed

Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

2014-09-15

The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic aerosol factor (AMS_PMF_COA) to oxidized organic aerosol, chloride and locally produced nitrate, indicating that AMS_PMF_COA cannot be attributed to primary cooking emissions only. Overall, there are clear benefits from factor analysis applied to results obtained from multiple techniques, which allows better association of aerosols with sources and atmospheric processes. Copyright © 2014 Elsevier B.V. All rights reserved.

An automated online instrument to quantify aerosol-bound reactive oxygen species (ROS) for ambient measurement and health-relevant aerosol studies

NASA Astrophysics Data System (ADS)

Wragg, Francis P. H.; Fuller, Stephen J.; Freshwater, Ray; Green, David C.; Kelly, Frank J.; Kalberer, Markus

2016-10-01

The adverse health effects associated with ambient aerosol particles have been well documented, but it is still unclear which aerosol properties are most important for their negative health impact. Some studies suggest the oxidative effects of particle-bound reactive oxygen species (ROS) are potential major contributors to the toxicity of particles. Traditional ROS measurement techniques are labour-intensive, give poor temporal resolution and generally have significant delays between aerosol sampling and ROS analysis. However, many oxidising particle components are reactive and thus potentially short-lived. Thus, a technique to quantify particle-bound ROS online would be beneficial to quantify also the short-lived ROS components. We introduce a new portable instrument to allow online, continuous measurement of particle-bound ROS using a chemical assay of 2'7'-dichlorofluorescein (DCFH) with horseradish peroxidase (HRP), via fluorescence spectroscopy. All components of the new instrument are attached to a containing shell, resulting in a compact system capable of automated continuous field deployment over many hours or days. From laboratory measurements, the instrument was found to have a detection limit of ˜ 4 nmol [H2O2] equivalents per cubic metre (m3) air, a dynamic range up to at least ˜ 2000 nmol [H2O2] equivalents per m3 air and a time resolution of ≤ 12 min. The instrument allows for ˜ 16 h automated measurement if unattended and shows a fast response to changes in concentrations of laboratory-generated oxidised organic aerosol. The instrument was deployed at an urban site in London, and particulate ROS levels of up to 24 nmol [H2O2] equivalents per m3 air were detected with PM2.5 concentrations up to 28 µg m-3. The new and portable Online Particle-bound ROS Instrument (OPROSI) allows fast-response quantification; this is important due to the potentially short-lived nature of particle-bound ROS as well as fast-changing atmospheric conditions, especially in urban environments. The instrument design allows for automated operation and extended field operation with twice-daily presence of an operator. As well as having sensitivity suitable for ambient level measurement, the instrument is also suitable at concentrations such as those required for laboratory and chamber toxicological studies.

Aerosol composition and source apportionment in Santiago de Chile

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (2

LOAC: a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles - Part 2: First results from balloon and unmanned aerial vehicle flights

NASA Astrophysics Data System (ADS)

Renard, Jean-Baptiste; Dulac, François; Berthet, Gwenaël; Lurton, Thibaut; Vignelles, Damien; Jégou, Fabrice; Tonnelier, Thierry; Jeannot, Matthieu; Couté, Benoit; Akiki, Rony; Verdier, Nicolas; Mallet, Marc; Gensdarmes, François; Charpentier, Patrick; Mesmin, Samuel; Duverger, Vincent; Dupont, Jean-Charles; Elias, Thierry; Crenn, Vincent; Sciare, Jean; Zieger, Paul; Salter, Matthew; Roberts, Tjarda; Giacomoni, Jérôme; Gobbi, Matthieu; Hamonou, Eric; Olafsson, Haraldur; Dagsson-Waldhauserova, Pavla; Camy-Peyret, Claude; Mazel, Christophe; Décamps, Thierry; Piringer, Martin; Surcin, Jérémy; Daugeron, Daniel

2016-08-01

In the companion (Part I) paper, we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosol Counter), based on scattering measurements at angles of 12 and 60°. That allows for some typology identification of particles (droplets, carbonaceous, salts, and mineral dust) in addition to size-segregated counting in a large diameter range from 0.2 µm up to possibly more than 100 µm depending on sampling conditions (Renard et al., 2016). Its capabilities overpass those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronic-sized absorbing carbonaceous particles in polluted air to very coarse particles (> 10-20 µm in diameter) in desert dust plumes or fog and clouds. LOAC's light and compact design allows measurements under all kinds of balloons, on-board unmanned aerial vehicles (UAVs) and at ground level. We illustrate here the first LOAC airborne results obtained from a UAV and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Vienna (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediterranean (during the Chemistry-Aerosol Mediterranean Experiment - ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in south-western France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes.

LOAC: a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles - Part 2: First results from balloon and unmanned aerial vehicle flights

NASA Astrophysics Data System (ADS)

Renard, J.-B.; Dulac, F.; Berthet, G.; Lurton, T.; Vignelles, D.; Jégou, F.; Tonnelier, T.; Thaury, C.; Jeannot, M.; Couté, B.; Akiki, R.; Verdier, N.; Mallet, M.; Gensdarmes, F.; Charpentier, P.; Mesmin, S.; Duverger, V.; Dupont, J. C.; Elias, T.; Crenn, V.; Sciare, J.; Giacomoni, J.; Gobbi, M.; Hamonou, E.; Olafsson, H.; Dagsson-Waldhauserova, P.; Camy-Peyret, C.; Mazel, C.; Décamps, T.; Piringer, M.; Surcin, J.; Daugeron, D.

2015-09-01

In the companion paper (Renard et al., 2015), we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosol Counter) based on scattering measurements at angles of 12 and 60° that allows some topology identification of particles (droplets, carbonaceous, salts, and mineral dust) in addition to size segregated counting in a large diameter range from 0.2 up to possibly more than 100 μm depending on sampling conditions. Its capabilities overpass those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronic-sized absorbing carbonaceous particles in polluted air to very coarse particles (> 10-20 μm in diameter) in desert dust plumes or fog and clouds. LOAC's light and compact design allows measurements under all kinds of balloons, on-board unmanned aerial vehicles (UAV) and at ground level. We illustrate here the first LOAC airborne results obtained from an unmanned aerial vehicle (UAV) and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Vienna (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediterranean (during the Chemistry-Aerosol Mediterranean Experiment - ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in south-western France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes.

LOAC: a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles - Part 2: First results from balloon and unmanned aerial vehicle flights

NASA Astrophysics Data System (ADS)

Renard, J.-B.; Dulac, F.; Berthet, G.; Lurton, T.; Vignelle, D.; Jégou, F.; Tonnelier, T.; Thaury, C.; Jeannot, M.; Couté, B.; Akiki, R.; Mineau, J.-L.; Verdier, N.; Mallet, M.; Gensdarmes, F.; Charpentier, P.; Mesmin, S.; Duverger, V.; Dupont, J.-C.; Elias, T.; Crenn, V.; Sciare, J.; Giacomoni, J.; Gobbi, M.; Hamonou, E.; Olafsson, H.; Dagsson-Waldhauserova, P.; Camy-Peyret, C.; Mazel, C.; Décamps, T.; Piringer, M.; Surcin, J.; Daugeron, D.

2015-01-01

In a companion (Part 1) paper (Renard et al., 2015), we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosols Counter) based on scattering measurements at angles of 12 and 60°. that allows some speciation of particles (droplets, carbonaceous, salts, and mineral dust) in addition to size segregated counting in a large diameter range from 0.2 up to possibly more than 100 μm depending on sampling conditions. Its capabilities overwhelm those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronic-sized absorbing carbonaceous particles in polluted air to very coarse particles (> 10-20 μm in diameter) in desert dust plumes or fog and clouds. LOAC light and compact design allows measurements under all kinds of balloons, on-board unmanned aerial vehicles (UAV) and at ground level. We illustrate here the first LOAC airborne results obtained from an unmanned aerial vehicle (UAV) and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Wien (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediterranean (during the Chemistry-Aerosol Mediterranean Experiment - ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in south-western France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes.

Determinants of aerosol lung-deposited surface area variation in an urban environment.

PubMed

Reche, Cristina; Viana, Mar; Brines, Mariola; Pérez, Noemí; Beddows, David; Alastuey, Andrés; Querol, Xavier

2015-06-01

Ultrafine particles are characterized by a high surface area per mass. Particle surface has been reported to play a significant role in determining the toxicological activity of ultrafine particles. In light of this potential role, the time variation of lung deposited surface area (LDSA) concentrations in the alveolar region was studied at the urban background environment of Barcelona (Spain), aiming to asses which processes and sources govern this parameter. Simultaneous data on Black Carbon (BC), total particle number (N) and particle number size distribution were correlated with LDSA. Average LDSA concentrations in Barcelona were 37 ± 26 μm(2)cm(-3), levels which seem to be characteristic for urban environments under traffic influence across Europe. Results confirm the comparability between LDSA data provided by the online monitor and those calculated based on particle size distributions (by SMPS), and reveal that LDSA concentrations are mainly influenced by particles in the size range 50-200 nm. A set of representative daily cycles for LDSA concentrations was obtained by means of a k-means cluster technique. The contribution of traffic emissions to daily patterns was evidenced in all the clusters, but was quantitatively different. Traffic events under stable atmospheric conditions increased mean hourly background LDSA concentrations up to 6 times, attaining levels higher than 200 μm(2)cm(-3). However, under warm and relatively clean atmospheric conditions, the traffic rush hour contribution to the daily LDSA mean appeared to be lower and the contribution of new urban particle formation events (by photochemically induced nucleation) was detected. These nucleation events were calculated to increase average background LDSA concentrations by 15-35% (maximum LDSA levels=45-50 μm(2)cm(-3)). Thereby, it may be concluded that in the urban background of Barcelona road traffic is the main source increasing the aerosol surface area which can deposit on critical regions of the human lung, followed by nucleation episodes. Copyright © 2015 Elsevier B.V. All rights reserved.

Characterization of key aerosol, trace gas and meteorological properties and particle formation and growth processes dependent on air mass origins in coastal Southern Spain

NASA Astrophysics Data System (ADS)

Diesch, J.; Drewnick, F.; Sinha, V.; Williams, J.; Borrmann, S.

2011-12-01

The chemical composition and concentration of aerosols at a certain site can vary depending on season, the air mass source region and distance from sources. Regardless of the environment, new particle formation (NPF) events are one of the major sources for ultrafine particles which are potentially hazardous to human health. Grown particles are optically active and efficient CCN resulting in important implications for visibility and climate (Zhang et al., 2004). The study presented here is intended to provide information about various aspects of continental, urban and marine air masses reflected by wind patterns of the air arriving at the measurement site. Additionally we will be focusing on NPF events associated with different types of air masses affecting their emergence and temporal evolution. Measurements of the ambient aerosol, various trace gases and meteorological parameters were performed within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from mid-November to mid-December 2008 at the atmospheric research station "El Arenosillo" located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean. Number and mass as well as PAH and black carbon concentrations were measured in PM1 and size distribution instruments covered the size range 6 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (AMS). In order to evaluate the characteristics of different air masses linking local and regional sources as well as NPF processes, characteristic air mass types were classified dependent on backwards trajectory pathways and local meteorology. Large nuclei mode concentrations in the number size distribution were found within continental and urban influenced air mass types due to frequently occurring NPF events. Exploring individual production and sink variables, sulfuric acid was found to be the main particle formation contributor. The AMS analysis showed inorganic sulfate species being substantially higher during the growth stages of urban compared to continentally influenced events that are characterized by lower PM1 mass concentrations mainly composed of oxidized organics. The lowest average PM1 mass and number concentrations (2 μg m-3, 1000 cm-3) were found in marine air mass types characterized by the highest sulfate PM1-fraction (54%, 0.91 μg m-3) and volume size distributions probably dominated by sodium chloride particles from sea spray. Two to five times higher submicron aerosol mass concentrations were observed in continental (2.5 μg m-3) and urban (4.2 μg m-3) air mass types mainly consisting of organic species that were further evaluated using Positive Matrix Factorization (PMF). Zhang, Q. et al. (2004), Environ. Sci. Technol., 38, 4797-4809.

Characteristics of size-resolved atmospheric inorganic and carbonaceous aerosols in urban Shanghai

NASA Astrophysics Data System (ADS)

Ding, X. X.; Kong, L. D.; Du, C. T.; Zhanzakova, A.; Fu, H. B.; Tang, X. F.; Wang, L.; Yang, X.; Chen, J. M.; Cheng, T. T.

2017-10-01

Size-segregated aerosol particles were collected with a 10-stage Micro-Orifice Uniform Deposit Impactor (MOUDI) at an urban site in Shanghai, China for four non-consecutive months representing four seasons from 2015 to 2016. Chemical composition, including water-soluble ions as well as organic carbon (OC), elemental carbon (EC) and secondary organic carbon (SOC) of size-resolved (0.056-18 μm) atmospheric aerosols in four seasons and in different polluted cases were studied. The size distributions of sulfate, nitrate and ammonium (SNA) and carbonaceous aerosol (OC, EC and SOC) were discussed and the potential sources of PM1.8-associated secondary species (SO42-, NO3-, SNA and SOC) in different seasons were identified by potential source contribution function (PSCF) model. Results showed that atmospheric ultrafine and fine particle pollution in Shanghai were very serious during the study period. Most of the water-soluble ions tended to be enriched in fine particles, especially being abundant in the droplet mode in polluted cases. Compared with sulfate, size distributions of nitrate and ammonium presented more significant seasonal variations and showed distinctive characteristics in polluted days. Abundant nitrate was concentrated in fine particles in cold seasons (spring and winter), whereas it was enriched in coarse mode during summer and autumn. The droplet mode sulfate with high concentration did not result in the aggravation of air pollution, while the nucleation mode sulfate may have made a great contribution to the air pollution in urban Shanghai. It was also found that the formation of air pollution in urban Shanghai had a significant link with nitrate and ammonium, especially with nitrate and ammonium in condensation mode and droplet mode, and the contribution of sulfate to the pollution formation in Shanghai would somehow be surpassed by the increasing nitrate and ammonium. OC and EC concentrations from spring to winter were found to be 11.10, 7.10, 12.30, 20.16, and 3.73, 2.84, 4.63, 7.10 μg m-3, respectively, distinctly presenting the summer minima and winter maxima in this study. The maximum OC/EC was in the droplet mode and the minimum was in the nucleation mode for both clean and polluted days. The great contribution of SOC to OC in droplet mode and the occurrence of PM pollution necessarily had an important bearing on the SOC formation in droplet mode particles. Particle acidity may play a key role in secondary organic aerosol formation and the particles with the size of 0.056-0.1 μm was the most sensitive particles to acid catalysis in SOA formation. The similar PSCF results of PM1.8-associated SOC to those of SO42-, NO3- and SNA indicated possible connections between the formation of SOC and secondary inorganic species in PM.

Aerosol Production from Charbroiled and Wet-Fried Meats

NASA Astrophysics Data System (ADS)

Niedziela, R. F.; Blanc, L. E.

2012-12-01

Previous work in our laboratory focused on the chemical and optical characterization of aerosols produced during the dry-frying of different meat samples. This method yielded a complex ensemble of particles composed of water and long-chain fatty acids with the latter dominated by oleic, stearic, and palmitic acids. The present study examines how wet-frying and charbroiling cooking methods affect the physical and chemical properties of their derived aerosols. Samples of ground beef, salmon, chicken, and pork were subject to both cooking methods in the laboratory, with their respective aerosols swept into a laminar flow cell where they were optically analyzed in the mid-infrared and collected through a gas chromatography probe for chemical characterization. This presentation will compare and contrast the nature of the aerosols generated in each cooking method, particularly those produced during charbroiling which exposes the samples, and their drippings, to significantly higher temperatures. Characterization of such cooking-related aerosols is important because of the potential impact of these particles on air quality, particularly in urban areas.

Properties of aerosols and formation mechanisms over southern China during the monsoon season

NASA Astrophysics Data System (ADS)

Chen, Weihua; Wang, Xuemei; Blake Cohen, Jason; Zhou, Shengzhen; Zhang, Zhisheng; Chang, Ming; Chan, Chuen-Yu

2016-10-01

Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May-June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 µm). Sulfate was found to be strongly correlated with aerosol water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.

Metrological assessment of a portable analyzer for monitoring the particle size distribution of ultrafine particles.

PubMed

Stabile, Luca; Cauda, Emanuele; Marini, Sara; Buonanno, Giorgio

2014-08-01

Adverse health effects caused by worker exposure to ultrafine particles have been detected in recent years. The scientific community focuses on the assessment of ultrafine aerosols in different microenvironments in order to determine the related worker exposure/dose levels. To this end, particle size distribution measurements have to be taken along with total particle number concentrations. The latter are obtainable through hand-held monitors. A portable particle size distribution analyzer (Nanoscan SMPS 3910, TSI Inc.) was recently commercialized, but so far no metrological assessment has been performed to characterize its performance with respect to well-established laboratory-based instruments such as the scanning mobility particle sizer (SMPS) spectrometer. The present paper compares the aerosol monitoring capability of the Nanoscan SMPS to the laboratory SMPS in order to evaluate whether the Nanoscan SMPS is suitable for field experiments designed to characterize particle exposure in different microenvironments. Tests were performed both in a Marple calm air chamber, where fresh diesel particulate matter and atomized dioctyl phthalate particles were monitored, and in microenvironments, where outdoor, urban, indoor aged, and indoor fresh aerosols were measured. Results show that the Nanoscan SMPS is able to properly measure the particle size distribution for each type of aerosol investigated, but it overestimates the total particle number concentration in the case of fresh aerosols. In particular, the test performed in the Marple chamber showed total concentrations up to twice those measured by the laboratory SMPS-likely because of the inability of the Nanoscan SMPS unipolar charger to properly charge aerosols made up of aggregated particles. Based on these findings, when field test exposure studies are conducted, the Nanoscan SMPS should be used in tandem with a condensation particle counter in order to verify and correct the particle size distribution data. Published by Oxford University Press on behalf of the British Occupational Hygiene Society 2014.

Reduced ultrafine particle levels in São Paulo's atmosphere during shifts from gasoline to ethanol use.

PubMed

Salvo, Alberto; Brito, Joel; Artaxo, Paulo; Geiger, Franz M

2017-07-18

Despite ethanol's penetration into urban transportation, observational evidence quantifying the consequence for the atmospheric particulate burden during actual, not hypothetical, fuel-fleet shifts, has been lacking. Here we analyze aerosol, meteorological, traffic, and consumer behavior data and find, empirically, that ambient number concentrations of 7-100-nm diameter particles rise by one-third during the morning commute when higher ethanol prices induce 2 million drivers in the real-world megacity of São Paulo to substitute to gasoline use (95% confidence intervals: +4,154 to +13,272 cm -3 ). Similarly, concentrations fall when consumers return to ethanol. Changes in larger particle concentrations, including US-regulated PM2.5, are statistically indistinguishable from zero. The prospect of increased biofuel use and mounting evidence on ultrafines' health effects make our result acutely policy relevant, to be weighed against possible ozone increases. The finding motivates further studies in real-world environments. We innovate in using econometrics to quantify a key source of urban ultrafine particles.The biofuel ethanol has been introduced into urban transportation in many countries. Here, by measuring aerosols in São Paulo, the authors find that high ethanol prices coincided with an increase in harmful nanoparticles by a third, as drivers switched from ethanol to cheaper gasoline, showing a benefit of ethanol.

Emission of intermediate, semi and low volatile organic compounds from traffic and their impact on secondary organic aerosol concentrations over Greater Paris

NASA Astrophysics Data System (ADS)

Sartelet, K.; Zhu, S.; Moukhtar, S.; André, M.; André, J. M.; Gros, V.; Favez, O.; Brasseur, A.; Redaelli, M.

2018-05-01

Exhaust particle emissions are mostly made of black carbon and/or organic compounds, with some of these organic compounds existing in both the gas and particle phases. Although emissions of volatile organic compounds (VOC) are usually measured at the exhaust, emissions in the gas phase of lower volatility compounds (POAvapor) are not. However, these gas-phase emissions may be oxidised after emission and enhance the formation of secondary organic aerosols (SOA). They are shown here to contribute to most of the SOA formation in Central Paris. POAvapor emissions are usually estimated from primary organic aerosol emissions in the particle phase (POA). However, they could also be estimated from VOC emissions for both gasoline and diesel vehicles using previously published measurements from chamber measurements. Estimating POAvapor from VOC emissions and ageing exhaust emissions with a simple model included in the Polyphemus air-quality platform compare well to measurements of SOA formation performed in chamber experiments. Over Greater Paris, POAvapor emissions estimated using POA and VOC emissions are compared using the HEAVEN bottom-up traffic emissions model. The impact on the simulated atmospheric concentrations is then assessed using the Polyphemus/Polair3D chemistry-transport model. Estimating POAvapor emissions from VOC emissions rather than POA emissions lead to lower emissions along motorway axes (between -50% and -70%) and larger emissions in urban areas (up to between +120% and +140% in Central Paris). The impact on total organic aerosol concentrations (gas plus particle) is lower than the impact on emissions: between -8% and 25% along motorway axes and in urban areas respectively. Particle-phase organic concentrations are lower when POAvapor emissions are estimated from VOC than POA emissions, even in Central Paris where the total organic aerosol concentration is higher, because of different assumptions on the emission volatility distribution, stressing the importance of characterizing not only the emission strength, but also the emission volatility distribution.

Fossil Fuel Combustion-Related Emissions Dominate Atmospheric Ammonia Sources during Severe Haze Episodes: Evidence from (15)N-Stable Isotope in Size-Resolved Aerosol Ammonium.

PubMed

Pan, Yuepeng; Tian, Shili; Liu, Dongwei; Fang, Yunting; Zhu, Xiaying; Zhang, Qiang; Zheng, Bo; Michalski, Greg; Wang, Yuesi

2016-08-02

The reduction of ammonia (NH3) emissions is urgently needed due to its role in aerosol nucleation and growth causing haze formation during its conversion into ammonium (NH4(+)). However, the relative contributions of individual NH3 sources are unclear, and debate remains over whether agricultural emissions dominate atmospheric NH3 in urban areas. Based on the chemical and isotopic measurements of size-resolved aerosols in urban Beijing, China, we find that the natural abundance of (15)N (expressed using δ(15)N values) of NH4(+) in fine particles varies with the development of haze episodes, ranging from -37.1‰ to -21.7‰ during clean/dusty days (relative humidity: ∼ 40%), to -13.1‰ to +5.8‰ during hazy days (relative humidity: 70-90%). After accounting for the isotope exchange between NH3 gas and aerosol NH4(+), the δ(15)N value of the initial NH3 during hazy days is found to be -14.5‰ to -1.6‰, which indicates fossil fuel-based emissions. These emissions contribute 90% of the total NH3 during hazy days in urban Beijing. This work demonstrates the analysis of δ(15)N values of aerosol NH4(+) to be a promising new tool for partitioning atmospheric NH3 sources, providing policy makers with insights into NH3 emissions and secondary aerosols for regulation in urban environments.

Hygroscopic properties of atmospheric particles emitted during wintertime biomass burning episodes in Athens

NASA Astrophysics Data System (ADS)

Psichoudaki, Magda; Nenes, Athanasios; Florou, Kalliopi; Kaltsonoudis, Christos; Pandis, Spyros N.

2018-04-01

This study explores the Cloud Condensation Nuclei (CCN) activity of atmospheric particles during intense biomass burning periods in an urban environment. During a one-month campaign in the center of Athens, Greece, a CCN counter coupled with a Scanning Mobility Particle Sizer (SMPS) and a high resolution Aerosol Mass Spectrometer (HR-AMS) were used to measure the size-resolved CCN activity and composition of the atmospheric aerosols. During the day, the organic fraction of the particles was more than 50%, reaching almost 80% at night, when the fireplaces were used. Positive Matrix Factorization (PMF) analysis revealed 4 factors with biomass burning being the dominant source after 18:00 until the early morning. The CCN-based overall hygroscopicity parameter κ ranged from 0.15 to 0.25. During the night, when the biomass burning organic aerosol (bbOA) dominated, the hygroscopicity parameter for the mixed organic/inorganic particles was on average 0.16. The hygroscopicity of the biomass-burning organic particles was 0.09, while the corresponding average value for all organic particulate matter during the campaign was 0.12.

The optical properties, physical properties and direct radiative forcing of urban columnar aerosols in the Yangtze River Delta, China

NASA Astrophysics Data System (ADS)

Zhuang, Bingliang; Wang, Tijian; Liu, Jane; Che, Huizheng; Han, Yong; Fu, Yu; Li, Shu; Xie, Min; Li, Mengmeng; Chen, Pulong; Chen, Huimin; Yang, Xiu-qun; Sun, Jianning

2018-02-01

The optical and physical properties as well as the direct radiative forcings (DRFs) of fractionated aerosols in the urban area of the western Yangtze River Delta (YRD) are investigated with measurements from a Cimel sun photometer combined with a radiation transfer model. Ground-based observations of aerosols have much higher temporal resolutions than satellite retrievals. An initial analysis reveals the characteristics of the optical properties of different types of fractionated aerosols in the western YRD. The total aerosols, mostly composed of scattering components (93.8 %), have mean optical depths of 0.65 at 550 nm and refractive index of 1.44 + 0.0084i at 440 nm. The fine aerosols are approximately four times more abundant and have very different compositions from coarse aerosols. The absorbing components account for only ˜ 4.6 % of fine aerosols and 15.5 % of coarse aerosols and have smaller sizes than the scattering aerosols within the same mode. Therefore, fine particles have stronger scattering than coarse ones, simultaneously reflecting the different size distributions between the absorbing and scattering aerosols. The relationships among the optical properties quantify the aerosol mixing and imply that approximately 15 and 27.5 % of the total occurrences result in dust- and black-carbon-dominating mixing aerosols, respectively, in the western YRD. Unlike the optical properties, the size distributions of aerosols in the western YRD are similar to those found at other sites over eastern China on a climatological scale, peaking at radii of 0.148 and 2.94 µm. However, further analysis reveals that the coarse-dominated particles can also lead to severe haze pollution over the YRD. Observation-based estimations indicate that both fine and coarse aerosols in the western YRD exert negative DRFs, and this is especially true for fine aerosols (-11.17 W m-2 at the top of atmosphere, TOA). A higher absorption fraction leads directly to the negative DRF being further offset for coarse aerosols (-0.33 W m-2) at the TOA. Similarly, the coarse-mode DRF contributes to only 13.3 % of the total scattering aerosols but > 33.7 % to the total absorbing aerosols. A sensitivity analysis states that aerosol DRFs are not highly sensitive to their profiles in clear-sky conditions. Most of the aerosol properties and DRFs have substantial seasonality in the western YRD. The results further reveal the contributions of each component of the different size particles to the total aerosol optical depths (AODs) and DRFs. Additionally, these results can be used to improve aerosol modelling performance and the modelling of aerosol effects in the eastern regions of China.

[Study on transition metals in airborne particulate matter in Shanghai city's subway].

PubMed

Bao, Liang-Man; Lei, Qian-Tao; Tan, Ming-Guang; Li, Xiao-Lin; Zhang, Gui-Lin; Liu, Wei; Li, Yan

2014-06-01

PM10 and PM2.5 aerosol particle samples were collected at a subway station in Shanghai and their morphology, chemical composition and transition metal species were studied. The mass concentrations of PM10 and PM2.5 inside the subway station were significantly higher than those measured in aboveground ambient air. The PM levels inside subway were much higher than the state control limit. The aerosol composition in the metro station was quite different from that of the aboveground urban particles. Concentrations of Fe, Mn and Cr were higher than the averages of aboveground urban air particles by factors of 8, 2, and 2, respectively, showing a substantial enrichment in subway. Scanning electron microscope (SEM) analysis showed that the subway particles had flat surfaces in combination with parallel scratches and sharp edges and looked like metal sheets or flakes. Furthermore, analysis of the atomic composition of typical subway particles by energy dispersive X-Ray (EDX) spectroscopy showed that oxygen and iron dominated the mass of the particles. The X-ray absorption near-edge structure (XANES) spectroscopy results showed that a fraction (> 26%) of the total iron in the PM10 was in the form of pure Fe, while in the street particles Fe(III) was shown to be a significant fraction of the total iron. The work demonstrated that the underground subway stations in Shanghai were an important microenvironment for exposure to transition metal aerosol for the people taking subway train for commuting every day and those who work in the subway stations, and the metal particle exposure for people in the subway station should not be ignored.

Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

NASA Astrophysics Data System (ADS)

Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

2017-12-01

Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

Simulation of the effects of aerosol on mixed-phase orographic clouds using the WRF model with a detailed bin microphysics scheme

NASA Astrophysics Data System (ADS)

Xiao, Hui; Yin, Yan; Jin, Lianji; Chen, Qian; Chen, Jinghua

2015-08-01

The Weather Research Forecast (WRF) mesoscale model coupled with a detailed bin microphysics scheme is used to investigate the impact of aerosol particles serving as cloud condensation nuclei and ice nuclei on orographic clouds and precipitation. A mixed-phase orographic cloud developed under two scenarios of aerosol (a typical continental background and a relatively polluted urban condition) and ice nuclei over an idealized mountain is simulated. The results show that, when the initial aerosol condition is changed from the relatively clean case to the polluted scenario, more droplets are activated, leading to a delay in precipitation, but the precipitation amount over the terrain is increased by about 10%. A detailed analysis of the microphysical processes indicates that ice-phase particles play an important role in cloud development, and their contribution to precipitation becomes more important with increasing aerosol particle concentrations. The growth of ice-phase particles through riming and Wegener-Bergeron-Findeisen regime is more effective under more polluted conditions, mainly due to the increased number of droplets with a diameter of 10-30 µm. Sensitivity tests also show that a tenfold increase in the concentration of ice crystals formed from ice nucleation leads to about 7% increase in precipitation, and the sensitivity of the precipitation to changes in the concentration and size distribution of aerosol particles is becoming less pronounced when the concentration of ice crystals is also increased.

Uncertainty in Predicting CCN Activity of Aged and Primary Aerosols

NASA Astrophysics Data System (ADS)

Zhang, Fang; Wang, Yuying; Peng, Jianfei; Ren, Jingye; Collins, Don; Zhang, Renyi; Sun, Yele; Yang, Xin; Li, Zhanqing

2017-11-01

Understanding particle CCN activity in diverse atmospheres is crucial when evaluating aerosol indirect effects. Here aerosols measured at three sites in China were categorized as different types for attributing uncertainties in CCN prediction in terms of a comprehensive data set including size-resolved CCN activity, size-resolved hygroscopic growth factor, and chemical composition. We show that CCN activity for aged aerosols is unexpectedly underestimated 22% at a supersaturation (S) of 0.2% when using κ-Kohler theory with an assumption of an internal mixture with measured bulk composition that has typically resulted in an overestimate of the CCN activity in previous studies. We conclude that the underestimation stems from neglect of the effect of aging/coating on particle hygroscopicity, which is not considered properly in most current models. This effect enhanced the hygroscopicity parameter (κ) by between 11% (polluted conditions) and 30% (clean days), as indicated in diurnal cycles of κ based on measurements by different instruments. In the urban Beijing atmosphere heavily influenced by fresh emissions, the CCN activity was overestimated by 45% at S = 0.2%, likely because of inaccurate assumptions of particle mixing state and because of variability of chemical composition over the particle size range. For both fresh and aged aerosols, CCN prediction exhibits very limited sensitivity to κSOA, implying a critical role of other factors like mixing of aerosol components within and between particles in regulating CCN activity. Our findings could help improving CCN parameterization in climate models.

Seasonal dependence of aerosol processing in urban Philadelphia

NASA Astrophysics Data System (ADS)

Avery, A. M.; Waring, M. S.; DeCarlo, P. F.

2017-12-01

Urban aerosols pose an important threat to human health due to the conflation of emissions and concentrated population exposed. Winter and summer aerosol and trace gas measurements were taken in downtown Philadelphia in 2016. Measurements included aerosol composition and size with an Aerodyne Aerosol Mass Spectrometer (AMS), particle size distributions with an SMPS, and an aethalometer. Trace gas measurements of O3, NO, CH4, CO, and CO2 were taken concurrently. Sampling in seasonal extremes provided contrast in aerosol and trace gas composition, aerosol processing, and emission factors. Inorganic aerosol components contributed approximately 60% of the submicron aerosol mass, while summertime aerosol composition was roughly 70% organic matter. Positive Matrix Factorization (PMF) on the organic aerosol (OA) matrix revealed three factors in common in each season, including an oxygenated organic aerosol (OOA) factor with different temporal behavior in each season. In summertime, OOA varied diurnally with ozone and daytime temperature, but in the wintertime, it was anti-correlated with ozone and temperature, and instead trended with calculated liquid water, indicating a seasonally-dependent processing of organic aerosol in Philadelphia's urban environment. Due to the inorganic dominant winter aerosol, liquid water much higher (2.65 μg/m3) in winter than in summer (1.54 μg/m3). Diurnally varying concentrations of background gas phase species (CH4, CO2) were higher in winter and varied less as a result of boundary layer conditions; ozone was also higher in background in winter than summer. Winter stagnation events with low windspeed showed large buildup of trace gases CH4, CO, CO2, and NO. Traffic related aerosol was also elevated with black carbon and hydrocarbon-like OA (HOA) plumes of each at 3-5 times higher than the winter the average value for each. Winter ratios of HOA to black carbon were significantly higher in the winter than the summer due to lower temperatures. Aerosol compositional differences in winter and summer indicate Philadelphia resident's aerosol exposures vary significantly with season.

Long-term observations of tropospheric particle number size distributions and equivalent black carbon mass concentrations in the German Ultrafine Aerosol Network (GUAN)

NASA Astrophysics Data System (ADS)

Birmili, W.; Weinhold, K.; Merkel, M.; Rasch, F.; Sonntag, A.; Wiedensohler, A.; Bastian, S.; Schladitz, A.; Löschau, G.; Cyrys, J.; Pitz, M.; Gu, J.; Kusch, T.; Flentje, H.; Quass, U.; Kaminski, H.; Kuhlbusch, T. A. J.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ries, L.; Wirtz, K.; Fiebig, M.

2015-11-01

The German Ultrafine Aerosol Network (GUAN) is a cooperative atmospheric observation network, which aims at improving the scientific understanding of aerosol-related effects in the troposphere. The network addresses research questions dedicated to both, climate and health related effects. GUAN's core activity has been the continuous collection of tropospheric particle number size distributions and black carbon mass concentrations at seventeen observation sites in Germany. These sites cover various environmental settings including urban traffic, urban background, rural background, and Alpine mountains. In association with partner projects, GUAN has implemented a high degree of harmonisation of instrumentation, operating procedures, and data evaluation procedures. The quality of the measurement data is assured by laboratory intercomparisons as well as on-site comparisons with reference instruments. This paper describes the measurement sites, instrumentation, quality assurance and data evaluation procedures in the network as well as the EBAS repository, where the data sets can be obtained (doi:10.5072/guan).

Long-term observations of tropospheric particle number size distributions and equivalent black carbon mass concentrations in the German Ultrafine Aerosol Network (GUAN)

NASA Astrophysics Data System (ADS)

Birmili, Wolfram; Weinhold, Kay; Rasch, Fabian; Sonntag, André; Sun, Jia; Merkel, Maik; Wiedensohler, Alfred; Bastian, Susanne; Schladitz, Alexander; Löschau, Gunter; Cyrys, Josef; Pitz, Mike; Gu, Jianwei; Kusch, Thomas; Flentje, Harald; Quass, Ulrich; Kaminski, Heinz; Kuhlbusch, Thomas A. J.; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ries, Ludwig; Gerwig, Holger; Wirtz, Klaus; Fiebig, Markus

2016-08-01

The German Ultrafine Aerosol Network (GUAN) is a cooperative atmospheric observation network, which aims at improving the scientific understanding of aerosol-related effects in the troposphere. The network addresses research questions dedicated to both climate- and health-related effects. GUAN's core activity has been the continuous collection of tropospheric particle number size distributions and black carbon mass concentrations at 17 observation sites in Germany. These sites cover various environmental settings including urban traffic, urban background, rural background, and Alpine mountains. In association with partner projects, GUAN has implemented a high degree of harmonisation of instrumentation, operating procedures, and data evaluation procedures. The quality of the measurement data is assured by laboratory intercomparisons as well as on-site comparisons with reference instruments. This paper describes the measurement sites, instrumentation, quality assurance, and data evaluation procedures in the network as well as the EBAS repository, where the data sets can be obtained (doi:10.5072/guan).

Denuder/filter sampling of organic acids and organosulfates at urban and boreal forest sites: Gas/particle distribution and possible sampling artifacts

NASA Astrophysics Data System (ADS)

Kristensen, Kasper; Bilde, Merete; Aalto, Pasi P.; Petäjä, Tuukka; Glasius, Marianne

2016-04-01

Carboxylic acids and organosulfates comprise an important fraction of atmospheric secondary organic aerosols formed from both anthropogenic and biogenic precursors. The partitioning of these compounds between the gas and particle phase is still unclear and further research is warranted to better understand the abundance and effect of organic acids and organosulfates on the formation and properties of atmospheric aerosols. This work compares atmospheric aerosols collected at an urban and a boreal forest site using two side-by-side sampling systems; a high volume sampler (HVS) and a low volume (LVS) denuder/filter sampling system allowing for separate collection of gas- and particle-phase organics. All particle filters and denuder samples were collected at H.C. Andersen Boulevard (HCAB), Copenhagen, Denmark in the summer of 2010, and at the remote boreal forest site at Hyytiälä forestry field station in Finland in the summer of 2012. The chemical composition of gas- and particle-phase secondary organic aerosol was investigated by ultra-high performance liquid chromatography/electrospray ionization quadrupole time-of-flight mass spectrometry (UPLC/ESI-Q-TOFMS), with a focus on carboxylic acids and organosulfates. Results show gas-phase concentrations higher than those observed in the particle phase by a factor of 5-6 in HCAB 2010 and 50-80 in Hyytiälä 2012. Although abundant in the particle phase, no organosulfates were detected in the gas phase at either site. Through a comparison of samples collected by the HVS and the LVS denuder/filter sampling system we evaluate the potential artifacts associated with sampling of atmospheric aerosols. Such comparison shows that particle phase concentrations of semi-volatile organic acids obtained from the filters collected by HVS are more than two times higher than concentrations obtained from filters collected using LVS denuder/filter system. In most cases, higher concentrations of organosulfates are observed in particles collected by HVS compared to samples collected by LVS denuder/filter sampling system. The present study shows that volatile organics may absorb onto filter materials in the HVS (and similar sampling systems without denuder) and furthermore undergo subsequent on-filter oxidation and sulfation resulting in formation of both organic acids and organosulfates.

Determination of the refractive index of insoluble organic extracts from atmospheric aerosol over the visible wavelength range using optical tweezers

NASA Astrophysics Data System (ADS)

Shepherd, Rosalie H.; King, Martin D.; Marks, Amelia A.; Brough, Neil; Ward, Andrew D.

2018-04-01

Optical trapping combined with Mie spectroscopy is a new technique used to record the refractive index of insoluble organic material extracted from atmospheric aerosol samples over a wide wavelength range. The refractive index of the insoluble organic extracts was shown to follow a Cauchy equation between 460 and 700 nm for organic aerosol extracts collected from urban (London) and remote (Antarctica) locations. Cauchy coefficients for the remote sample were for the Austral summer and gave the Cauchy coefficients of A = 1.467 and B = 1000 nm2 with a real refractive index of 1.489 at a wavelength of 589 nm. Cauchy coefficients for the urban samples varied with season, with extracts collected during summer having Cauchy coefficients of A = 1.465 ± 0.005 and B = 4625 ± 1200 nm2 with a representative real refractive index of 1.478 at a wavelength of 589 nm, whilst samples extracted during autumn had larger Cauchy coefficients of A = 1.505 and B = 600 nm2 with a representative real refractive index of 1.522 at a wavelength of 589 nm. The refractive index of absorbing aerosol was also recorded. The absorption Ångström exponent was determined for woodsmoke and humic acid aerosol extract. Typical values of the Cauchy coefficient for the woodsmoke aerosol extract were A = 1.541 ± 0.03 and B = 14 800 ± 2900 nm2, resulting in a real refractive index of 1.584 ± 0.007 at a wavelength of 589 nm and an absorption Ångström exponent of 8.0. The measured values of refractive index compare well with previous monochromatic or very small wavelength range measurements of refractive index. In general, the real component of the refractive index increases from remote to urban to woodsmoke. A one-dimensional radiative-transfer calculation of the top-of-the-atmosphere albedo was applied to model an atmosphere containing a 3 km thick layer of aerosol comprising pure water, pure insoluble organic aerosol, or an aerosol consisting of an aqueous core with an insoluble organic shell. The calculation demonstrated that the top-of-the-atmosphere albedo increases by 0.01 to 0.04 for pure organic particles relative to water particles of the same size and that the top-of-the-atmosphere albedo increases by 0.03 for aqueous core-shell particles as volume fraction of the shell material increases to 25 %.

C1-C2 alkyl aminiums in urban aerosols: Insights from ambient and fuel combustion emission measurements in the Yangtze River Delta region of China.

PubMed

Shen, Wenchao; Ren, Lili; Zhao, Yi; Zhou, Luyu; Dai, Liang; Ge, Xinlei; Kong, Shaofei; Yan, Qin; Xu, Honghui; Jiang, Yujun; He, Jun; Chen, Mindong; Yu, Huan

2017-11-01

We measured low molar-mass alkyl aminiums (methylaminium, dimethylaminium, ethylaminium and diethylaminium) in urban aerosols in the Yangtze River Delta region of eastern China in August 2014 and from November 2015 to May 2016. After examining artifact formation on sample filters, methylaminium, dimethylaminium and ethylaminium concentrations were quantified. The three C1-C2 aminiums exhibited a unimodal size distribution that maximized between 0.56 and 1.0 μm. Their concentrations in PM 2.5 were 5.7 ± 3.2 ng m -3 , 7.9 ± 5.4 ng m -3 and 20.3 ± 16.6 ng m -3 , respectively, with higher concentrations during the daytime and in warm seasons. On new particle growth days, amine uptake to particles larger than 56 nm was barely enhanced. The molar ratios of individual aminium/NH 4 + in PM 2.5 were on the order of 10 -4 and 10 -3 . Aminiums were thus far less to out-compete ammonium (NH 4 + ) in neutralizing acidic species in particle sizes down to 56 nm. Abundant nitrate (NO 3 - /SO 4 2- molar ratio = ∼3) and its correlation to methylaminium and ethylaminium implied that nitrate might be more important aminium salt than sulfate in urban aerosols of this area. Direct measurement of particle-phase amine emission from coal and biomass burning showed that coal burning is an important atmospheric amine source, considering coal burning is top-ranked particulate matter source in China. Copyright © 2017 Elsevier Ltd. All rights reserved.

Investigation of the tracers for plastic-enriched waste burning aerosols

NASA Astrophysics Data System (ADS)

Kumar, Sudhanshu; Aggarwal, Shankar G.; Gupta, Prabhat K.; Kawamura, Kimitaka

2015-05-01

To better identify the tracers for open-waste burning (OWB) aerosols, we have conducted aerosol sampling at 2 landfill sites, i.e., Okhla and Bhalswa in New Delhi. The metals such as, As, Cd, Sb and Sn, which have been observed almost negligible in remote aerosols, are found abundantly in these OWB aerosol samples (n = 26), i.e., 60 ± 65, 41 ± 53, 537 ± 847 and 1325 ± 1218 ng m-3, respectively. Samples (n = 20) collected at urban locations in New Delhi, i.e., at Employees' State Insurance (ESI) hospital and National Physical Laboratory (NPL) also show high abundances of these metals in the particles. Filter samples are also analyzed for water-soluble dicarboxylic acids (C2-C12) and related compounds (oxocarboxylic acids and α-dicarbonyls). Terephthalic acid (tPh) was found to account for more than 77% of total diacids determined in OWB aerosols. However, such a high abundance of tPh is not observed in aerosols collected at urban sites. Instead, phthalic acid (Ph) was found as the third/fourth most abundant diacid (∼3%) following C2 (>70%) and C4 (>12%) in these waste burning influenced urban aerosols. A possible secondary formation pathway of Ph by photo-degradation of phthalate ester (di-2-ethylhexyl phthalate) in plastic-waste burning aerosol is suggested. Ionic composition of OWB aerosols showed that Cl- is the most abundant ion (40 ± 8% of total ions determined). The correlation studies of the potential metals with the organic tracers of garbage burning, i.e., phthalic, isophthalic and terephthalic acids show that especially Sn can be used as marker for tracing the plastic-enriched waste burning aerosols.

Identification of aerosol types over an urban site based on air-mass trajectory classification

NASA Astrophysics Data System (ADS)

Pawar, G. V.; Devara, P. C. S.; Aher, G. R.

2015-10-01

Columnar aerosol properties retrieved from MICROTOPS II Sun Photometer measurements during 2010-2013 over Pune (18°32‧N; 73°49‧E, 559 m amsl), a tropical urban station in India, are analyzed to identify aerosol types in the atmospheric column. Identification/classification is carried out on the basis of dominant airflow patterns, and the method of discrimination of aerosol types on the basis of relation between aerosol optical depth (AOD500 nm) and Ångström exponent (AE, α). Five potential advection pathways viz., NW/N, SW/S, N, SE/E and L have been identified over the observing site by employing the NOAA-HYSPLIT air mass back trajectory analysis. Based on AE against AOD500 nm scatter plot and advection pathways followed five major aerosol types viz., continental average (CA), marine continental average (MCA), urban/industrial and biomass burning (UB), desert dust (DD) and indeterminate or mixed type (MT) have been identified. In winter, sector SE/E, a representative of air masses traversed over Bay of Bengal and Eastern continental Indian region has relatively small AOD (τpλ = 0.43 ± 0.13) and high AE (α = 1.19 ± 0.15). These values imply the presence of accumulation/sub-micron size anthropogenic aerosols. During pre-monsoon, aerosols from the NW/N sector have high AOD (τpλ = 0.61 ± 0.21), and low AE (α = 0.54 ± 0.14) indicating an increase in the loading of coarse-mode particles over Pune. Dominance of UB type in winter season for all the years (i.e. 2010-2013) may be attributed to both local/transported aerosols. During pre-monsoon seasons, MT is the dominant aerosol type followed by UB and DD, while the background aerosols are insignificant.

Characterization of organic compounds in the PM2.5 aerosols in winter in an industrial urban area

NASA Astrophysics Data System (ADS)

Mikuška, P.; Křůmal, K.; Večeřa, Z.

2015-03-01

Urban aerosol particles in the fine fraction (PM2.5) were collected over the sampling interval of 24-hrs on quartz filters in Ostrava (Czech Republic) in winter 2012. The collected aerosols were analysed for selected organic compounds that serve as tracers of the main emission sources. The campaign was carried out under two different meteorological scenarios. During a smog episode due to high concentration of aerosols in the first part of the campaign, high concentrations of PM2.5 aerosols (mean concentration of 159 μg m-3) and PAHs bound to particles were found, while in the second part of the campaign, after the smog episode, much lower concentrations of aerosols (mean concentration of 49.3 μg m-3) were observed. Analysis of the source specific molecular markers and diagnostic ratios of PAHs, hopanes and alkanes imply that combustion of coniferous wood and coal in residential heating and traffic belong to the biggest emission sources of organic compounds associated with the PM2.5 aerosols collected during the winter campaign in Ostrava-Radvanice. The industrial production of coke and iron is another important contributor to the concentrations of BaP and other carcinogenic PAHs. The level of air pollution in Ostrava-Radvanice was considerably determined by the overall meteorological situation during the campaign. The highest concentrations of PM2.5 and bound organic compounds were found during a smog episode characterized by poor dispersion conditions due to temperature inversion and weak north-eastern wind, while during the subsequent period characterized by north-west or west wind, the concentrations of aerosols and bound organic compounds were much lower. Transboundary transport of polluted air from the Silesian Voivodeship could have contributed to the pollution in the Moravian-Silesian region during the smog episode.

The Effect of Aerosol on Gravity Wave Characteristics above the Boundary Layer over a Tropical Location

NASA Astrophysics Data System (ADS)

Rakshit, G.; Jana, S.; Maitra, A.

2017-12-01

The perturbations of temperature profile over a location give an estimate of the potential energy of gravity waves propagating through the atmosphere. Disturbances in the lower atmosphere due to tropical deep convection, orographic effects and various atmospheric disturbances generates of gravity waves. The present study investigates the gravity wave energy estimated from fluctuations in temperature profiles over the tropical location Kolkata (22°34' N, 88°22' E). Gravity waves are most intense during the pre-monsoon period (March-June) at the present location, the potential energy having high values above the boundary layer (2-4 km) as observed from radiosonde profiles. An increase in temperature perturbation, due to high ambient temperature in the presence of heat absorbing aerosols, causes an enhancement in potential energy. As the present study location is an urban metropolitan city experiencing high level of pollution, pollutant aerosols can go much above the normal boundary layer during daytime due to convection causing an extended boundary layer. The Aerosol Index (AAI) obtained from Global Ozone Monitoring Experiment-2 (GOME-2) on MetOp-A platform at 340 nm and 380 nm confirms the presence of absorbing aerosol particles over the present location. The Hysplit back trajectory analysis shows that the aerosol particles at those heights are of local origin and are responsible for depleting liquid water content due to cloud burning. The aerosol extinction coefficient obtained from CALIPSO data exhibits an increasing trend during 2006-2016 accompanied by a similar pattern of gravity wave energy. Thus the absorbing aerosols have a significant role in increasing the potential energy of gravity wave at an urban location in the tropical region.

Surface aerosol and rehabilitation properties of ground-level atmosphere in the mountains of the North Caucasus

NASA Astrophysics Data System (ADS)

Reps, Valentina; Efimenko, Natalia; Povolotskaya, Nina; Abramtsova, Anna; Ischenko, Dmitriy; Senik, Irina; Slepikh, Victor

2017-04-01

The rehabilitative properties (RP) of ground-level atmosphere (GA) of Russian resorts are considered as natural healing resources and received state legal protection [1]. Due to global urbanization the chemical composition and particle size distribution of the surface aerosol are changing rapidly. However, the influence of surface aerosol on the RP of GA has been insufficiently studied. At the resort region of the North Caucasus complex monitoring (aerosol, trace gases NOx, CO, O3, CH4; periodically - heavy metals) is performed at two high levels (860 masl - a park zone of a large mountain resort, 2070 masl - alpine grassland, the net station). The results of the measurements are used in programs of bioclimatic, landscape and medical monitoring to specify the influence of aerosol on rehabilitation properties of the environment and human adaptative reserves. The aerosol particles of size range 500-1000 nm are used as a marker of the pathogenic effect of aerosol [2]. In the conditions of regional urbanization and complicated mountain atmospheric circulation the influence of aerosol on RP of GA and the variability of heart rhythm with the volunteers at different heights were investigated. At the height of 860 masl (urbanized resort) there have been noticed aerosol variations in the range of 0,04-0,35 particles/cm3 (slightly aerosol polluted), in mountain conditions - background pollution aerosol level. The difference of bioclimatic conditions at the specified high-rise levels has been referred to the category of contrasts. The natural aero ionization ∑(N+)+(N-) varied from 960 ion/cm3 to 1460 ion/cm3 in the resort park (860 m); from 1295 ion/cm3 to 4850 ion/cm3 on the Alpine meadow (2070 m); from 1128 ion/cm3 to 3420 ion/cm3 - on the tested site near the edge of the pinewood (1720 m). In the group of volunteers the trip from low-hill terrain zone (860 m) to the lower zone of highlands (2070 m) caused the activation of neuro and humoral regulation, vegetative and central parts of nervous system, psychoemotional status, normalization of frequency spectrum of brain activity and organism adaptation level. The researches are still being conducted. References: 1. The federal law "About Natural Medical Resources, Medical and Improving Areas and Resorts" from 23.02.1995 № 26-fl. 2. The technique of balneological assessment of forest-park landscapes of mountain territories for the purposes of climate-landscape therapy in case of resort treatment of the contingent subject to FMBA of Russia: Handbook for doctors//Registration number 82-15 from 17.12.2015 - Pyatigorsk:MHRF:FMBA of Russia, 2015. -26 p.

Formation of nitrogen-containing oligomers by methylglyoxal and amines in simulated evaporating cloud droplets.

PubMed

De Haan, David O; Hawkins, Lelia N; Kononenko, Julia A; Turley, Jacob J; Corrigan, Ashley L; Tolbert, Margaret A; Jimenez, Jose L

2011-02-01

Reactions of methylglyoxal with amino acids, methylamine, and ammonium sulfate can take place in aqueous aerosol and evaporating cloud droplets. These processes are simulated by drying droplets and bulk solutions of these compounds (at low millimolar and 1 M concentrations, respectively) and analyzing the residuals by scanning mobility particle sizing, nuclear magnetic resonance, aerosol mass spectrometry (AMS), and electrospray ionization MS. The results are consistent with imine (but not diimine) formation on a time scale of seconds, followed by the formation of nitrogen-containing oligomers, methylimidazole, and dimethylimidazole products on a time scale of minutes to hours. Measured elemental ratios are consistent with imidazoles and oligomers being major reaction products, while effective aerosol densities suggest extensive reactions take place within minutes. These reactions may be a source of the light-absorbing, nitrogen-containing oligomers observed in urban and biomass-burning aerosol particles.

Observed aerosol effects on marine cloud nucleation and supersaturation

NASA Astrophysics Data System (ADS)

Russell, Lynn M.; Sorooshian, Armin; Seinfeld, John H.; Albrecht, Bruce A.; Nenes, Athanasios; Leaitch, W. Richard; Macdonald, Anne Marie; Ahlm, Lars; Chen, Yi-Chun; Coggon, Matthew; Corrigan, Ashley; Craven, Jill S.; Flagan, Richard C.; Frossard, Amanda A.; Hawkins, Lelia N.; Jonsson, Haflidi; Jung, Eunsil; Lin, Jack J.; Metcalf, Andrew R.; Modini, Robin; Mülmenstädt, Johannes; Roberts, Greg C.; Shingler, Taylor; Song, Siwon; Wang, Zhen; Wonaschütz, Anna

2013-05-01

Aerosol particles in the marine boundary layer include primary organic and salt particles from sea spray and combustion-derived particles from ships and coastal cities. These particle types serve as nuclei for marine cloud droplet activation, although the particles that activate depend on the particle size and composition as well as the supersaturation that results from cloud updraft velocities. The Eastern Pacific Emitted Aerosol Cloud Experiment (EPEACE) 2011 was a targeted aircraft campaign to assess how different particle types nucleate cloud droplets. As part of E-PEACE 2011, we studied the role of marine particles as cloud droplet nuclei and used emitted particle sources to separate particle-induced feedbacks from dynamical variability. The emitted particle sources included shipboard smoke-generated particles with 0.05-1 μm diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke) and combustion particles from container ships with 0.05-0.2 μm diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components) [1]. Three central aspects of the collaborative E-PEACE results are: (1) the size and chemical composition of the emitted smoke particles compared to ship-track-forming cargo ship emissions as well as background marine particles, with particular attention to the role of organic particles, (2) the characteristics of cloud track formation for smoke and cargo ships, as well as the role of multi-layered low clouds, and (3) the implications of these findings for quantifying aerosol indirect effects. For comparison with the E-PEACE results, the preliminary results of the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) 2012 provided evidence of the cloud-nucleating roles of both marine organic particles and coastal urban pollution, with simultaneous measurements of the effective supersaturations of the clouds in the California coastal region.

Optical properties of size-resolved particles at a Hong Kong urban site during winter

NASA Astrophysics Data System (ADS)

Gao, Yuan; Lai, Senchao; Lee, Shun-Cheng; Yau, Pui Shan; Huang, Yu; Cheng, Yan; Wang, Tao; Xu, Zheng; Yuan, Chao; Zhang, Yingyi

2015-03-01

Visibility degradation in Hong Kong is related to the city's serious air pollution problems. To investigate the aerosols' optical properties and their relationship with the chemical composition and size distribution of the particles, a monitoring campaign was conducted at an urban site in the early winter period (from October to December, 2010). The particle light scattering coefficient (Bsp) and absorption coefficient (Bap) were measured. Two collocated Micro-Orifice Uniform Deposit Impactor samplers (MOUDI110, MSP, USA) with nominal 50% cut-off aerodynamic diameters of 18, 10, 5.6, 3.2, 1.8, 1, 0.56, 0.32, 0.18, 0.1, and 0.056 μm were used to collect size-resolved particle samples. The average Bsp and Bap were 201.96 ± 105.82 Mm- 1 and 39.91 ± 19.16 Mm- 1, with an average single scattering albedo (ωo) of 0.82 ± 0.07. The theoretical method of light extinction calculation was used to determine the extinction of the size-resolved particulate matters (PM). The reconstructed light scattering coefficient correlated well with the measured scattering value in the Hong Kong urban area. Droplet mode (0.56-1.8 μm) particles contributed most to the particle light extinction (~ 69%). Organic matter, ammonium sulphate and elemental carbon were the key components causing visibility degradation in the droplet (0.56-1.8 μm) and condensation (0.1-0.56 μm) size ranges. Five sources contributing to particle light extinction have been identified using positive matrix factorisation (PMF). Traffic/engine exhausts and secondary aerosols accounted for ~ 36% and ~ 32% of particle light extinction, respectively, followed by sea salt (15%). The remaining sources, soil/fugitive dust and tire dust, contributed by ~ 10% and 7%, respectively, to particle light extinction.

COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thornton, Joel A.; Worsnop, Douglas

2016-09-22

This project was part of a collaborative campaign, including the participation of scientists from seven research groups as part of the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London to study wintertime sources of urban particulate matter. The UW contribution by PI Thornton’s group was to make the first deployment of a chemical ionization mass spectrometer instrument (MOVI-CI-ToFMS) to measure both particle and gas phase organic acids. The new instrument ran nearly continuously during the ClearfLo WINTER IOP at the Detlingmore » site, producing a first-ever data set of molecular composition information that can be used for source apportionment and process studies. The UW group published a paper in Environmental Science and Technology and contributed to another (Bohnenstengel et al BAMS 2015) detailing a direct molecular connection between biomass/biofuel burning particles and aerosol light absorption. The ES&T paper (Mohr, et al ES&T 2013) has received 42 citations in just 3 years indicative of its significant impact on the field. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal.« less

Effects of Siberian wildfires on the chemical composition and acidity of atmospheric aerosols of remote urban, rural and background territories.

PubMed

Smolyakov, Boris S; Makarov, Valeriy I; Shinkorenko, Marina P; Popova, Svetlana A; Bizin, Mikhail A

2014-05-01

Extensive forest fires occurred during the summer of 2012 in Siberia. This work presents the influence of long-range atmospheric smoke on the aerosol properties at urban, suburban and background sites, which are located 400-800 km from the fire source. The higher levels of submicron particles (PM1), organic (OC), secondary organic (SOC) and elemental (EC) carbon were observed at all sampling sites, whereas an increase in ionic species HCOO(-), K(+), NO3(-), and Cl(-) and a decrease in pH was higher at the background and suburban sites in comparison with the urban site. Other natural and anthropogenic factors appear to be more significant for ions Ca(2+) + Mg(2+), HCO3(-), NH4(+), SO4(2-) and Na(+). The present study indicates that the impact of remote fires on the aerosol characteristics depends on their background (without fires) levels at the sampling sites. Copyright © 2014 Elsevier Ltd. All rights reserved.

Submicron particles influenced by mixed biogenic and anthropogenic emissions: high-resolution aerosol mass spectrometry results from the Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Setyan, A.; Zhang, Q.; Merkel, M.; Knighton, W. B.; Sun, Y.; Song, C.; Shilling, J. E.; Onasch, T. B.; Herndon, S. C.; Worsnop, D. R.; Fast, J. D.; Zaveri, R. A.; Berg, L. K.; Wiedensohler, A.; Flowers, B. A.; Dubey, M. K.; Subramanian, R.

2012-02-01

The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project (~40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 μg m-3 on average) and dominated by organics (80 % of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at ˜400 nm in vacuum aerodynamic diameter (Dva), and a condensation mode at ~150 nm, while organics generally displayed a broad distribution in 60-600 nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a~nominal formula of C1H1.38N0.004O0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90 % of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high-resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly due to local traffic. Twenty three periods of urban plumes from T0 (Sacramento) to T1 (Cool) were identified using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The average PM1 mass loading was much higher in urban plumes (3.9 μg m-3) than in air masses dominated by biogenic SOA (1.8 μg m-3). The change in OA mass relative to CO (Δ OA/Δ CO) varied in the range of 5-196 μg m-3 ppm-1, reflecting large variability in SOA production. The highest Δ OA/Δ CO were reached when urban plumes arrived at Cool in the presence of a~high concentration of biogenic volatile organic compounds (BVOCs = isoprene + monoterpenes + 2-methyl-3-buten-2-ol [MBO] + methyl chavicol). This ratio, which was 77 μg m-3 ppm-1 on average when BVOCs > 2 ppb, is much higher than when urban plumes arrived in a low biogenic VOCs environment (28 μg m-3 ppm-1 when BVOCs < 0.7 ppb) or during other periods dominated by biogenic SOA (40 μg m-3 ppm-1). The results from this study demonstrate that SOA formation is enhanced when anthropogenic emissions interact with biogenic precursors.

Estimation of particulate matter from simulation and measurements

NASA Astrophysics Data System (ADS)

Nakata, Makiko; Nakano, Tomio; Okuhara, Takaaki; Sano, Itaru; Mukai, Sonoyo

2011-11-01

The particulate matter is a typical indicator of small particles in the atmosphere. In addition to providing impacts on climate and environment, these small particles can bring adverse effects on human health. Then an accurate estimation of particulate matter is an urgent subject. We set up SPM sampler attached to our AERONET (Aerosol Robotics Network) station in urban city of Higashi-Osaka in Japan. The SPM sampler provides particle information about the concentrations of various SPMs (e.g., PM10 and PM2.5) separately. The AEROENT program is world wide ground based sunphotometric observation networks by NASA and provides the spectral information about aerosol optical thickness (AOT) and Angstrom exponent (α). Simultaneous measurements show that a linear correlation definitely exists between AOT and PM2.5. These results indicate that particulate matter can be estimated from AOT. However AOT represents integrated values of column aerosol amount retrieved from optical property, while particulate matter concentration presents in-situ aerosol loading on the surface. Then simple way using linear correlation brings the discrepancy between observed and estimated particulate matter. In this work, we use cluster information about aerosol type to reduce the discrepancy. Our improved method will be useful for retrieving particulate matter from satellite measurements.

Hygroscopic growth of size-resolved, emission-source classified, aerosol particles sampled across the United States

NASA Astrophysics Data System (ADS)

Shingler, T.; Crosbie, E. C.; Ziemba, L. D.; Anderson, B. E.; Campuzano Jost, P.; Jimenez, J. L.; Mikoviny, T.; Wisthaler, A.; Sorooshian, A.

2014-12-01

The hygroscopic growth of atmospheric aerosol particles is a key air quality parameter, impacting the radiation budget, visibility, and cloud formation. During the DC3 and SEAC4RS field campaigns (>300 total flight hours), measurements were made over 32 US states, Canada, the Pacific Ocean, and the Gulf of Mexico, between the surface and 41,000 feet ASL. The aircraft research payloads included a suite of in-situ aerosol and gas phase instruments. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) and the Langley Aerosol Research Group Experiment (LARGE) humidified nephelometer instrument applied different techniques to measure water uptake by aerosol particles at prescribed relative humidity values. Size-resolved growth factor (GF ≡ Dp,wet/Dp,dry) measurements by the DASH-SP are compared to bulk scattering measurements (f(RH) ≡ σscat,wet/σscat,dry) by the LARGE instrument. Spatial location and volatile organic compound tracers such as isoprene and acetonitrile are used to classify the origin of distinct air masses, including: forest fires, biogenic-emitting forests, agricultural use lands, marine boundary layer, urban, and rural background. Analyses of GF results by air mass origin are reported and results are compared with f(RH) measurements. A parameterization between the f(RH) and GF measurements and its potential uses are discussed.

Evaluation and modelling of the size fractionated aerosol particle number concentration measurements nearby a major road in Helsinki - Part I: Modelling results within the LIPIKA project

NASA Astrophysics Data System (ADS)

Pohjola, M. A.; Pirjola, L.; Karppinen, A.; Härkönen, J.; Korhonen, H.; Hussein, T.; Ketzel, M.; Kukkonen, J.

2007-08-01

A field measurement campaign was conducted near a major road "Itäväylä" in an urban area in Helsinki in 17-20 February 2003. Aerosol measurements were conducted using a mobile laboratory "Sniffer" at various distances from the road, and at an urban background location. Measurements included particle size distribution in the size range of 7 nm-10 μm (aerodynamic diameter) by the Electrical Low Pressure Impactor (ELPI) and in the size range of 3-50 nm (mobility diameter) by Scanning Mobility Particle Sizer (SMPS), total number concentration of particles larger than 3 nm detected by an ultrafine condensation particle counter (UCPC), temperature, relative humidity, wind speed and direction, driving route of the mobile laboratory, and traffic density on the studied road. In this study, we have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI used in combination with an aerosol process model MONO32. For model comparison purposes, one of the cases was additionally computed using the aerosol process model UHMA, combined with the CAR-FMI model. The vehicular exhaust emissions, and atmospheric dispersion and transformation of fine and ultrafine particles was evaluated within the distance scale of 200 m (corresponding to a time scale of a couple of minutes). We computed the temporal evolution of the number concentrations, size distributions and chemical compositions of various particle size classes. The atmospheric dilution rate of particles is obtained from the roadside dispersion model CAR-FMI. Considering the evolution of total number concentration, dilution was shown to be the most important process. The influence of coagulation and condensation on the number concentrations of particle size modes was found to be negligible on this distance scale. Condensation was found to affect the evolution of particle diameter in the two smallest particle modes. The assumed value of the concentration of condensable organic vapour of 1012 molecules cm-3 was shown to be in a disagreement with the measured particle size evolution, while the modelling runs with the concentration of condensable organic vapour of 109-1010 molecules cm-3 resulted in particle sizes that were closest to the measured values.

Source characterization of urban particles from meat smoking activities in Chongqing, China using single particle aerosol mass spectrometry.

PubMed

Chen, Yang; Wenger, John C; Yang, Fumo; Cao, Junji; Huang, Rujin; Shi, Guangming; Zhang, Shumin; Tian, Mi; Wang, Huanbo

2017-09-01

A Single Particle Aerosol Mass Spectrometer (SPAMS) was deployed in the urban area of Chongqing to characterize the particles present during a severe particulate pollution event that occurred in winter 2014-2015. The measurements were made at a time when residents engaged in traditional outdoor meat smoking activities to preserve meat before the Chinese Spring Festival. The measurement period was predominantly characterized by stagnant weather conditions, highly elevated levels of PM 2.5 , and low visibility. Eleven major single particle types were identified, with over 92.5% of the particles attributed to biomass burning emissions. Most of the particle types showed appreciable signs of aging in the stagnant air conditions. To simulate the meat smoking activities, a series of controlled smoldering experiments was conducted using freshly cut pine and cypress branches, both with and without wood logs. SPAMS data obtained from these experiments revealed a number of biomass burning particle types, including an elemental and organic carbon (ECOC) type that proved to be the most suitable marker for meat smoking activities. The traditional activity of making preserved meat in southwestern China is shown here to be a major source of particulate pollution. Improved measures to reduce emissions from the smoking of meat should be introduced to improve air quality in regions where smoking meat activity prevails. Copyright © 2017 Elsevier Ltd. All rights reserved.

Aerosol Number Size Distribution and Type Classification from 4-Year Polarization Optical Particle Counter (POPC) Measurements at Urban-Mountain Site in Seoul

NASA Astrophysics Data System (ADS)

Park, H. J.; Kim, S. W.; Kobayashi, H.; Nishizawa, T.

2017-12-01

The Polarization Optical Particle Counter (POPC), unlike general OPCs, has the advantage capable of classifying the aerosol types (e.g., dust, anthropogenic pollution), because it measures particle number, size and depolarization ratio (DPR; the sphericity information of single particle) for 4 size bins with diameter (0.5-1, 1-3, 3-5, 5-10 μm). In this study, we investigate the temporal variations of particle number and volume size distributions with DPR values and classify aerosol types such as dust, anthropogenic pollution, from 4-year (2013-2016) POPC data at Seoul National University campus in Seoul, Korea. Coarse mode particles from 5-10 μm with relatively high DPR values (0.25-0.3) were distinctly appeared in in both spring (March-May) and winter (December-February) due to frequent transport of Asian dust particles. In summer (June -August), however, both aerosol number concentration and DPR value were decreased in all size bins due to the influences of relatively clean maritime airmass and frequent precipitations. In autumn (September - November), the particle number concentration in all size bins was the lowest. To classify the aerosol types, we investigate particle number and volume size distributions and DPR value for clean, dust-dominant and anthropogenic pollution-dominant cases, which were selected by PM10, PM2.5 mass concentrations and its ratio, because those parameters are clearly different among aerosol types (Kobayashi et al., 2014, Pan et al., 2016). Non-spherical coarse mode particles (Dp > 2.5 μm, 0.1 < DPR < 0.6) were dominantly observed during the dust-dominant period, while both spherical fine mode and coarse mode particles (Dp < 1 μm and Dp = 2-4 μm, DPR < 0.1) were dominantly appeared during the pollution event. The aerosol type classifications with these criteria values were successfully applied to the extreme Asian dust event from February 22 to 24, 2015. The results showed that pollution-dominant airmass preceded by the appearance of a major mineral dust plume. Co-located aerosol lidar measurements also revealed that spherical pollution particles were observed near the surface prior to a major plume of non-spherical mineral dust.

MAX-DOAS retrieval of aerosol extinction properties in Madrid, Spain

NASA Astrophysics Data System (ADS)

Wang, Shanshan; Cuevas, Carlos A.; Frieß, Udo; Saiz-Lopez, Alfonso

2017-04-01

We present Multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements performed in the urban environment of Madrid, Spain, from March to September 2015. The O4 absorption in the ultraviolet (UV) spectral region was used to retrieve the aerosol extinction profile using an inversion algorithm. The results show a good agreement between the hourly retrieved aerosol optical depth (AOD) and the correlative Aerosol Robotic Network (AERONET) product. Higher AODs are found in the summer season due to the more frequent occurrence of Saharan dust intrusions. The surface aerosol extinction coefficient as retrieved by the MAX-DOAS measurements was also compared to in situ PM2:5 concentrations. The level of agreement between both measurements indicates that the MAX-DOAS retrieval has the ability to characterize the extinction of aerosol particles near the surface. The retrieval algorithm was also used to study a case of severe dust intrusion on 12 May 2015. The capability of the MAX-DOAS retrieval to recognize the dust event including an elevated particle layer is investigated along with air mass back-trajectory analysis.

The fluorescence properties of aerosol larger than 0.8 μm in an urban and a PBA-dominated location

NASA Astrophysics Data System (ADS)

Gabey, A. M.; Stanley, W. R.; Gallagher, M. W.; Kaye, P. H.

2011-01-01

Dual-wavelength Ultraviolet light-induced fluorescence (UV-LIF) measurements were performed on ambient environmental aerosol in Manchester, UK (urban city centre, winter) and Borneo, Malaysia (remote, tropical), which are taken to represent environments with negligible and significant primary biological aerosol (PBA) influences, respectively. Single-particle fluorescence intensity and optical equivalent diameter were measured with a Wide Issue Bioaerosol Sensor, version 3 (WIBS3) in the diameter range 0.8 μm≤DP≤20 μm for 2-3 weeks and filters were analysed using energy dispersive X-ray (EDX) spectroscopy, which revealed mostly non-PBA dominated particle sizes larger than 1 μm in Manchester. The WIBS3 features three fluorescence channels: Fluorescence excited at 280 nm is recorded at 310-400 nm and 400-600 nm and fluorescence excited at 370 nm is detected at 400-600 nm. In Manchester the primary size mode of fluorescent and non-fluorescent material was at 1.2 μm. In Borneo non-fluorescent material peaked at 1.2 μm and fluorescent at 3-4 μm. The fluorescence intensity at 400-600 nm generally increased with DP at both sites, as did the 310-400 nm intensity in Borneo. In Manchester the 310-400 m fluorescence decreased at DP>4 μm, suggesting this channel offers additional discrimination between fluorescent particle types. Finally, the ratio of fluorescence intensity in two pairs of channels was investigated as a function of particle diameter and this varied significantly between the two environments, demonstrating that the fluorescent aerosol in each can in principle be distinguished using a combination of fluorescence and elastic scattering measurements.

Fine particulate matter characteristics and its impact on visibility impairment at two urban sites in Korea: Seoul and Incheon

NASA Astrophysics Data System (ADS)

Kim, Young J.; Kim, Kyung W.; Kim, Shin D.; Lee, Bo K.; Han, Jin S.

In order to investigate the causes of visibility degradation in the metropolitan area of Seoul, extensive chemical and optical monitoring of aerosol was conducted at two urban sites; Junnong, Seoul and Yonghyun, Incheon during several seasonal intensive monitoring periods between August 2002 and August 2004. Light extinction, scattering, and absorption coefficients were measured simultaneously with a transmissometer, a nephelometer, and an aethalometer, respectively. Continuous aerosol chemical measurement was also made with Sunset elemental carbon/organic carbon (EC/OC) analyzers and on-line ion monitors. The mean light extinction budget for five major aerosol components; ammonium sulfate, ammonium nitrate, fine carbonaceous particles (EC and OC), fine soil, and coarse particle was estimated based on the measurement results. Investigation of the haze level revealed that PM 2.5 mass concentrations at Junnong and Yonghyun measured under the Worst20% condition were approximately twice those of the Best20% condition. The worst visibility condition was well correlated with increases in mass concentrations of sulfate and nitrate, and EC particles. The mass concentration of aerosol components for the Worst20% was measured to be approximately two- to four-fold higher than those for the Best20%. Degree of visibility degradation was also analyzed based on the air mass pathway information obtained using the HYSPLIT model. Average light extinction coefficients under continental air flow condition at the Junnong and Yonghyun sites were the highest values of 704±414 and 773±546 Mm -1, respectively due to increased loading of fine particles. Visibility was greatly improved at both sites when atmosphere was impacted by air mass originated from Pacific Ocean.

Remote Sensing of Aerosol Over the Land from the Earth Observing System MODIS Instrument

NASA Technical Reports Server (NTRS)

Kaufman, Yoram; Tanre, Didier; Remer, Lorraine; Einaudi, Franco (Technical Monitor)

2000-01-01

On Dec 18, 1999, NASA launched the Moderate-Resolution Imaging Spectroradiometer (MODIS) instrument on the Earth Observing System (EOS) Terra mission, in a spectacular launch. The mission will provide morning (10:30 AM) global observations of aerosol and other related parameters. It will be followed a year later by a MODIS instrument on EOS Aqua for afternoon observations (1:30 PM). MODIS will measure aerosol over land and ocean with its eight 500 m and 250 m channels in the solar spectrum (0-41 to 2.2 micrometers). Over the land MODIS will measure the total column aerosol loading, and distinguish between submicron pollution particles and large soil particles. Standard daily products of resolution of ten kilometers and global mapped eight day and monthly products on a 1x1 degree global scale will be produced routinely and make available for no or small reproduction charge to the international community. Though the aerosol products will not be available everywhere over the land, it is expected that they will be useful for assessments of the presence, sources and transport of urban pollution, biomass burning aerosol, and desert dust. Other measurements from MODIS will supplement the aerosol information, e.g., land use change, urbanization, presence and magnitude of biomass burning fires, and effect of aerosol on cloud microphysics. Other instruments on Terra, e.g. Multi-angle Imaging SpectroRadiometer (MISR) and the Clouds and the Earth's Radiant Energy System (CERES), will also measure aerosol, its properties and radiative forcing in tandem with the MODIS measurements. During the Aqua period, there are plans to launch in 2003 the Pathfinder Instruments for Cloud and Aerosol Spaceborne Observations (PICASSO) mission for global measurements of the aerosol vertical structure, and the PARASOL mission for aerosol characterization. Aqua-MODIS, PICASSO and PARASOL will fly in formation for detailed simultaneous characterization of the aerosol three-dimensional field, which will feed and evaluate global aerosol transport and climate models. In this talk, some examples of the MODIS measurements will be shown.

Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Despiau, S.; Dubovik, O.; Putaud, J. P.

2003-10-01

Microphysical and optical properties of the main aerosol species on a peri-urban site have been investigated during the ESCOMPTE experiment. Ammonium sulfate (AS), nitrate (N), black carbon (BC), particulate organic matter (POM), sea salt (SS) and mineral aerosol (D) size distributions have been used, associated with their refractive index, to compute, from the Mie theory, the key radiative aerosol properties as the extinction coefficient Kext, the mass extinction efficiencies σext, the single scattering albedo ω0 and the asymmetry parameter g at the wavelength of 550 nm. Optical computations show that 90% of the light extinction is due to anthropogenic aerosol and only 10% is due to natural aerosol (SS and D). 44±6% of the extinction is due to (AS) and 40±6% to carbonaceous particles (20±4% to BC and 21±4% to POM). Nitrate aerosol has a weak contribution of 5±2%. Computations of the mass extinction efficiencies σext, single scattering albedo ω0 and asymmetry parameter g indicate that the optical properties of the anthropogenic aerosol are often quite different from those yet published and generally used in global models. For example, the (AS) mean specific mass extinction presents a large difference with the value classically adopted at low relative humidity ( h<60%) (2.6±0.5 instead of 6 m 2 g -1 at 550 nm). The optical properties of the total aerosol layer, including all the aerosol species, indicate a mean observed single-scattering albedo ω0=0.85±0.05, leading to an important absorption of the solar radiation and an asymmetry parameter g=0.59±0.05 which are in a reasonably good agreements with the AERONET retrieval of ω0 (=0.86±0.05) and g (=0.64±0.05) at this wavelength.

Complex anthropogenic sources of platinum group elements in aerosols on Cape Cod, USA.

PubMed

Sen, Indra S; Peucker-Ehrenbrink, Bernhard; Geboy, Nicholas

2013-09-17

Platinum group elements (PGE) of anthropogenic origin have been reported in rainwater, snow, roadside soil and vegetation, industrial waste, and urban airborne particles around the world. As recent studies have shown that PGE are bioavailable in the environment and pose health risks at chronic levels, the extent of PGE pollution is of global concern. In this study, we report PGE concentrations and osmium isotope ((187)Os/(188)Os) ratios of airborne particles (particulate matter, PM10) collected in Woods Hole, a small coastal village on Cape Cod, Massachusetts, U.S.A. The sampling site is more than 100 km away from the nearest urban centers (Boston, Providence) and has no large industrial emission center within a 30 km radius. The study reveals that, although PGE concentrations in rural airborne particulate matter are orders of magnitude lower than in urban aerosols, 69% of the total osmium is of anthropogenic origin. Anthropogenic PGE signatures in airborne particles are thus not restricted to large cities with high traffic flows and substantial industries; they can also be found in rural environments. We further conclude that the combination of Pt/Rh concentration ratios and (187)Os/(188)Os composition can be used to trace PGE sources. The Pt/Rh and (187)Os/(188)Os composition of Woods Hole aerosols indicate that the anthropogenic PGE fraction is primarily sourced from ore smelting processes, with possible minor contributions from fossil fuel burning and automobile catalyst-derived materials. Our results further substantiate the use of (187)Os/(188)Os in source apportionment studies on continental scales.

Aerosol composition and microstructure in the smoky atmosphere of Moscow during the August 2010 extreme wildfires

NASA Astrophysics Data System (ADS)

Popovicheva, O. B.; Kistler, M.; Kireeva, E. D.; Persiantseva, N. M.; Timofeev, M. A.; Shoniya, N. K.; Kopeikin, V. M.

2017-01-01

This is a comprehensive study of the physicochemical characterization of multicomponent aerosols in the smoky atmosphere of Moscow during the extreme wildfires of August 2010 and against the background atmosphere of August 2011. Thermal-optical analysis, liquid and ion chromatography, IR spectroscopy, and electron microscopy were used to determine the organic content (OC) and elemental content (EC) of carbon, organic/inorganic and ionic compounds, and biomass burning markers (anhydrosaccharides and the potassium ion) and study the morphology and elemental composition of individual particles. It has been shown that the fires are characterized by an increased OC/EC ratio and high concentrations of ammonium, potassium, and sulfate ions in correlation with an increased content of levoglucosan as a marker of biomass burning. The organic compounds containing carbonyl groups point to the process of photochemical aging and the formation of secondary organic aerosols in the urban atmosphere when aerosols are emitted from forest fires. A cluster analysis of individual particles has indicated that when the smokiest atmosphere is characterized by prevailing soot/tar ball particles, which are smoke-emission micromarkers.

Internally mixed sea salt, soot, and sulfates at Macao, a coastal city in South China.

PubMed

Li, Weijun; Shao, Longyi; Shen, Rongrong; Yang, Shusheng; Wang, Zhishi; Tang, Uwa

2011-11-01

Direct observation of the mixing state of aerosol particles in a coastal urban city is critical to understand atmospheric processing and hygroscopic growth in humid air. Morphology, composition, and mixing state of individual aerosol particles from Macao, located south of the Pearl River Delta (PRD) and 100 km west of Hong Kong, were investigated using scanning electron microscopy (SEM) and transmission electron microscopy coupled with energy-dispersive X-ray spectrometry (TEM/EDX). SEM images show that soot and roughly spherical particles are prevalent in the samples. Based on the compositions of individual aerosol particles, aerosol particles with roughly spherical shape are classified into coarse Na-rich and fine S-rich particles. TEM/EDX indicates that each Na-rich particle consists of a Na-S core and NaNO3 shell. Even in the absence of heavy pollution, the marine sea salt particles were completely depleted in chloride, and Na-related sulfates and nitrates were enriched in Macao air. The reason could be that SO2 from the polluted PRD and ships in the South China Sea and NO2 from vehicles in the city sped up the chlorine depletion in sea salt through heterogeneous reactions. Fresh soot particles from vehicular emissions mainly occur near curbside. However, there are many aged soot particles in the sampling site surrounded by main roads 200 to 400 m away, suggesting that the fresh soot likely underwent a quick aging. Overall, secondary nitrates and sulfates internally mixed with soot and sea salt particles can totally change their surface hygroscopicity in coastal cities.

Influence of measurement frequency on the evaluation of short-term dose of sub-micrometric particles during indoor and outdoor generation events

NASA Astrophysics Data System (ADS)

Manigrasso, M.; Stabile, L.; Avino, P.; Buonanno, G.

2013-03-01

Aerosol generation events due to combustion processes are characterized by high particle emissions in the nucleation mode range. Such particles are characterized by very short atmospheric lifetimes, leading to rapid decay in time and space from the emission point. Therefore, the deposited fraction of inhaled particles (dose) also changes. In fact, close to the emission source, high short-term peak exposures occur. The related exposure estimates should therefore rely on measurements of aerosol number-size distributions able to track rapid aerosol dynamics. In order to study the influence of the time resolution on such estimates, simultaneous measurements were carried out via Scanning Mobility Particle Sizer (SMPS) and Fast Mobility Particle Sizer (FMPS) spectrometers during particle generation events in both indoor (cooking activities) and outdoor (airstrip and urban street canyons) microenvironments. Aerosol size distributions in the range 16-520 nm were measured by SMPS and FMPS at frequencies of 0.007 s-1 and 1 s-1, respectively. Based on the two datasets, respiratory dosimetry estimates were made on the basis of the deposition model of the International Commission on Radiological Protection. During cooking activities, SMPS measurements give an approximate representation of aerosol temporal evolution. Consequently, the related instant doses can be approximated to a fair degree. In the two outdoor microenvironments considered, aerosol size distributions change rapidly: the FMPS is able to follow such evolution, whereas the SMPS is not. The high short-term peak concentrations, and the consequent respiratory doses, evidenced by FMPS data are hardly described by SMPS, which is unable to track the fast aerosol changes. The health relevance of such short peak exposures has not been thoroughly investigated in scientific literature, therefore, in the present paper highly time-resolved and size-resolved dosimetry estimates were provided in order to deepen this aspect.

Aerosol studies during the ESCOMPTE experiment: an overview

NASA Astrophysics Data System (ADS)

Cachier, Hélène; Aulagnier, Fabien; Sarda, Roland; Gautier, François; Masclet, Pierre; Besombes, Jean-Luc; Marchand, Nicolas; Despiau, Serge; Croci, Delphine; Mallet, Marc; Laj, Paolo; Marinoni, Angela; Deveau, Pierre-Alexandre; Roger, Jean-Claude; Putaud, Jean-Philippe; Van Dingenen, Rita; Dell'Acqua, Alessandro; Viidanoja, Jyrkki; Martins-Dos Santos, Sebastiao; Liousse, Cathy; Cousin, Frédéric; Rosset, Robert; Gardrat, Eric; Galy-Lacaux, Corinne

2005-03-01

The "Expérience sur Site pour COntraindre les Modèles de Pollution atmosphérique et de Transport d'Emissions" (ESCOMPTE) experiment took place in the Southern part of France in the Marseilles/Fos-Berre region during 6 weeks in June and July 2001. One task was to document the regional sources of atmospheric particles and to gain some insight into the aerosol transformations in the atmosphere. For this purpose, seven sites were chosen and equipped with the same basic instrumentation to obtain the chemical closure of the bulk aerosol phase and size-segregated samples. Some specific additional experiments were conducted for the speciation of the organic matter and the aerosol size distribution in number. Finally, four multiwavelength sun-photometers were also deployed during the experiment. Interestingly, in this region, three intense aerosol sources (urban, industrial and biogenic) are very active, and data show consistent results, enlightening an important background of particles over the whole ESCOMPTE domain. Notable is the overwhelming importance of the carbonaceous fraction (comprising primary and secondary particles), which is always more abundant than sulphates. Particle size studies show that, on average, more than 90% of the mean regional aerosol number is found on a size range smaller than 300 nm in diameter. The most original result is the evidence of the rapid formation of secondary aerosols occurring in the whole ESCOMPTE domain. This formation is much more important than that usually observed at these latitudes since two thirds of the particulate mass collected off source zones is estimated to be generated during atmospheric transport. On the other hand, the marine source has poor influence in the region, especially during the overlapping pollution events of Intensive Observation Periods (IOP). Preliminary results from the 0D and 3D versions of the MesoNH-aerosol model show that, with optimised gas and particle sources, the model accounts satisfactorily for the measured aerosol concentrations. The formation of secondary particles in the model is currently underway; initial encouraging results show that the model accounts for the formation of secondary species, such as sulphate and organic particles. Finally, radiative calculations suggest that the role of the fine aerosol fraction is predominant mostly due to the presence of black carbon (BC) particles, which could induce a regional atmospheric heating.

Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-09-01

Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental-scale emissions.

Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

NASA Astrophysics Data System (ADS)

Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

2016-04-01

The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle arises mainly from fossil fuel sources, whereas OC in larger particles from 200 nm to 1 μm has higher contribution from biomass burning/other sources. Moreover, there is a clear distinction in source contribution between the more volatile OC fraction and the more refractory fraction. The more refractory fraction is enriched in 13C by 1 to 2 ‰ for both small and large particles. These results show that the fossil fuel combustion is associated to a larger degree with more volatile carbon, whereas biomass burning is the main source of the more refractory particles. According to our source apportionment, the more volatile carbon fraction in the smallest particles is almost completely from fossil fuels, whereas the more refractory carbon fraction in the large size range is almost complete from biomass burning. The more refractory small particles and the less refractory large particles are roughly an even mix of these two sources. The detailed chemical speciation of the carbonaceous aerosol will be presented as well. Acknowledgements This study was funded by the Dutch Science Foundation (NWO grants Nr. 820.01.001, and 834.08.002).

Characterization of Dust Properties during ACE-Asia and PRIDE: A Column Satellite-Surface Perspective

NASA Technical Reports Server (NTRS)

Lau, William K. M. (Technical Monitor); Tsay, Si-Chee; Hsu, N. Christina; Herman, Jay R.; Ji, Q. Jack

2002-01-01

Many recent field experiments are designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentration over particular pathways around the globe. For example, the ACE-Asia (Aerosol Characterization Experiment-Asia) was conducted from March-May 2001 in the vicinity of the Taklimakan and Gobi deserts, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). The PRIDE (Puerto RIco Dust Experiment, July 2000) was designed to measure the properties of Saharan dust transported across the Atlantic Ocean to the Caribbean. Dust particles typically originate in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of dust aerosols is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the ocean. During ACE-Asia and PRIDE we had measured aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from ground-based remote sensing. The inclusion of flux measurements permits the determination of aerosol radiative flux in addition to measurements of loading and optical depth. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. We will present the results and discuss their implications in regional climatic effects.

Type-segregated aerosol effects on regional monsoon activity: A study using ground-based experiments and model simulations

NASA Astrophysics Data System (ADS)

Vijayakumar, K.; Devara, P. C. S.; Sonbawne, S. M.

2014-12-01

Classification of observed aerosols into key types [e.g., clean-maritime (CM), desert-dust (DD), urban-industrial/biomass-burning (UI/BB), black carbon (BC), organic carbon (OC) and mixed-type aerosols (MA)] would facilitate to infer aerosol sources, effects, and feedback mechanisms, not only to improve the accuracy of satellite retrievals but also to quantify the assessment of aerosol radiative impacts on climate. In this paper, we report the results of a study conducted in this direction, employing a Cimel Sun-sky radiometer at the Indian Institute of Tropical Meteorology (IITM), Pune, India during 2008 and 2009, which represent two successive contrasting monsoon years. The study provided an observational evidence to show that the local sources are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle over Pune, a tropical urban station in India. The results revealed the absence of CM aerosols in the pre-monsoon as well as in the monsoon seasons of 2009 as opposed to 2008. Higher loading of dust aerosols is observed in the pre-monsoon and monsoon seasons of 2009; majority may be coated with fine BC aerosols from local emissions, leading to reduction in regional rainfall. Further, significant decrease in coarse-mode AOD and presence of carbonaceous aerosols, affecting the aerosol-cloud interaction and monsoon-rain processes via microphysics and dynamics, is considered responsible for the reduction in rainfall during 2009. Additionally, we discuss how optical depth, contributed by different types of aerosols, influences the distribution of monsoon rainfall over an urban region using the Monitoring Atmospheric Composition and Climate (MACC) aerosol reanalysis. Furthermore, predictions of the Dust REgional Atmospheric Model (DREAM) simulations combined with HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) cluster model are also discussed in support of the observed features.

Dust episodes in Beirut and their effect on the chemical composition of coarse and fine particulate matter.

PubMed

Jaafar, Malek; Baalbaki, Rima; Mrad, Raya; Daher, Nancy; Shihadeh, Alan; Sioutas, Constantinos; Saliba, Najat A

2014-10-15

Particles captured during dust episodes in Beirut originated from both the African and Arabian deserts. This particular air mixture showed an increase, over non-dust episodes, in particle volume distribution which was mostly noticed for particles ranging in sizes between 2.25 and 5 μm. It also resulted in an increase in average mass concentration by 48.5% and 14.6%, for the coarse and fine fractions, respectively. Chemical analysis of major aerosol components accounted for 93% of fine PM and 71% of coarse PM. Crustal material (CM) dominated the coarse PM fraction, contributing to 39 ± 15% of the total mass. Sea salt (SS) (11 ± 10%) and secondary ions (SI) (11 ± 7%) were the second most abundant elements. In the fine fraction, SI (36 ± 14%) were the most abundant PM constituent, followed by organic matter (OM) (33 ± 7%) and CM (13 ± 2%). Enrichment factors (EF) and correlation coefficients show that biogenic and anthropogenic sources contribute to the elemental composition of particles during dust episodes. This study emphasizes on the role played by the long-range transport of aerosols in changing the chemical composition of the organic and inorganic constituents of urban coarse and fine PM. The chemical reactions between aged urban and dust aerosols are enhanced during transport, leading to the formation of organo-nitrogenated and -sulfonated compounds. Their oligomeric morphologies are further confirmed by SEM-EDX measurements. Copyright © 2014 Elsevier B.V. All rights reserved.

Solar dimming and urban aerosol distribution in New York Metropolitan area

NASA Astrophysics Data System (ADS)

Hannon, P.; Liepert, B.; Chillrud, S. N.

2004-12-01

One impact of human activities on the urban and suburban environment is the dimming of sunlight due to urban air pollution and intensified haze. The spreading of urban aerosol and the optical efficiency depends on the size distribution of the particles and the vertical distribution. Reduced transparency of the atmosphere leads to an increase in scattered light compared to direct sunlight and an overall reduced total solar flux at the surface due to absorption in the atmosphere and backscattering of light to space. The modified solar flux cools the surface and suppresses evaporation and turbulent mass exchange in urban and suburban areas. Increase in diffuse sunlight can also have a positive effect on plant productivity due to increased actinic flux. Hence consequences for the biogeochemical cycles can be expected in urban and suburban areas. The quantification and variability of these effects were investigated in a pilot project in summer 2003 and 2004 where measurements of Aerosol Optical Thickness (AOT) at several wavelengths and particle number concentration for multiple size ranges were made in pilot fashion with the initial goal of better understanding horizontal and vertical distribution of aerosols near a major metropolitan center. Large spatial variability of atmospheric transparency in the New York Metropolitan area was observed in transects through New York City and Long Island to New Jersey in a field campaign in July 2003. Vertical profiles of AOT and particle number concentration were collected on board hot-air balloon flights in July 2004 that were launched from rural/suburban New Jersey. One evening flight was made in clear conditions and 4 evening flights where made under varying hazy conditions with the sunphotometer looking west. One sunrise flight was made in hazy conditions with the sunphotometer looking east through the city. Here we highlight a few results from two evening flights; additional data and plans of future work will be discussed in the poster. On July 6, during clear conditions, AOT at 500 nm is very low (depth integrated mean of 0.07) and fairly constant as a function of altitude (-0.003 change per 100 meters). Particle number concentration in the 0.3 - 0.5 μ m size range are also relatively low but have a steeper vertical gradient than AOT and abruptly drops to near zero above the boundary layer (1200 meters on that flight). The mean AOT at 500 nm (0.5) is a factor of 7 higher on the hazy evening of July 20th and its vertical gradient is also ca. a factor of 7 higher (-0.02 per 100 meters). Particle number concentrations in the the 0.3 - 0.5 μ m size range on this hazy evening were a factor of 3 to 4 higher than the clear evening and fairly constant with altitude, only appreciably dropping off above 1600 meters.

Chemical characteristics of soluble aerosols over the central Himalayas: insights into spatiotemporal variations and sources.

PubMed

Tripathee, Lekhendra; Kang, Shichang; Rupakheti, Dipesh; Cong, Zhiyuan; Zhang, Qianggong; Huang, Jie

2017-11-01

In order to investigate the spatial and temporal variations of aerosols and its soluble chemical compositions of the data gap zone in the central Himalayan region, aerosol samples were collected at four sites. The sampling location were characterized by four different categories, such as urban (Bode), semi-urban site in the northern Indo-Gangetic Plain (Lumbini), rural (Dhunche), and semiarid rural (Jomsom). A total of 230 aerosol samples were collected from four representative sites for a yearlong period and analyzed for water-soluble inorganic ions (WSIIs). The annual average aerosol mass concentration followed the sequence as Bode (238.24 ± 162.24 μg/m 3 )> Lumbini (161.14 ± 105.95 μg/m 3 )> Dhunche (112.40 ± 40.30 μg/m 3 )> Jomsom (78.85 ± 34.28 μg/m 3 ), suggesting heavier particulate pollution in the urban and semi-urban sites. The total soluble ions contributed to 12.61-28.19% of TSP aerosol mass. The results revealed that SO 4 2- and NO 3 - were the major anion and Ca 2+ and NH 4 + were the major cation influencing the aerosol composition over the central Himalayas. Calcium played a major role in neutralizing aerosol acidity followed by NH 4 + at all the sites. The major compound of aerosol was (NH 4 ) 2 SO 4 and NH 4 HSO 4 in the central Himalayas. Clear seasonality was observed at three observation sites, with higher concentrations during non-monsoon (dry periods) and lower during monsoon (wet period), suggesting washing out of aerosol particles by heavy precipitation during monsoon. In contrast, semiarid sites did not show the clear seasonal trend due to limited precipitation. Stationary sources were predominant over the mobile sources mostly in the remote sites. Principal component analysis confirmed that the major sources of WSIIs in the region were industrial emissions, fossil fuel and biomass burning, and crustal fugitive dusts. Nevertheless, transboundary aerosol transport over the region from polluted cities from south Asia could not be ignored as indicated by the clusters of air mass backward trajectory analysis.

Partitioning of magnetic particles in PM10, PM2.5 and PM1 aerosols in the urban atmosphere of Barcelona (Spain).

PubMed

Revuelta, María Aránzazu; McIntosh, Gregg; Pey, Jorge; Pérez, Noemi; Querol, Xavier; Alastuey, Andrés

2014-05-01

A combined magnetic-chemical study of 15 daily, simultaneous PM10-PM2.5-PM1 urban background aerosol samples has been carried out. The magnetic properties are dominated by non-stoichiometric magnetite, with highest concentrations seen in PM10. Low temperature magnetic analyses showed that the superparamagnetic fraction is more abundant when coarse, multidomain particles are present, confirming that they may occur as an oxidized outer shell around coarser grains. A strong association of the magnetic parameters with a vehicular PM10 source has been identified. Strong correlations found with Cu and Sb suggests that this association is related to brake abrasion emissions rather than exhaust emissions. For PM1 the magnetic remanence parameters are more strongly associated with crustal sources. Two crustal sources are identified in PM1, one of which is of North African origin. The magnetic particles are related to this source and so may be used to distinguish North African dust from other sources in PM1. Copyright © 2014 Elsevier Ltd. All rights reserved.

One year online chemical speciation of submicron particulate matter (PM1) sampled at a French industrial and coastal site

NASA Astrophysics Data System (ADS)

Zhang, Shouwen; Riffault, Véronique; Dusanter, Sébastien; Augustin, Patrick; Fourmentin, Marc; Delbarre, Hervé

2015-04-01

The harbor of Dunkirk (Northern France) is surrounded by different industrial plants (metallurgy, petrochemistry, food processing, power plant, etc.), which emit gaseous and particulate pollutants such as Volatile Organic Compounds (VOCs), oxides of nitrogen (NOx) and sulfur (SO2), and submicron particles (PM1). These emissions are poorly characterized and their impact on neighboring urban areas has yet to be assessed. Studies are particularly needed in this type of complex environments to get a better understanding of PM1sources, especially from the industrial sector, their temporal variability, and their transformation. Several instruments, capable of real-time measurements (temporal resolution ≤ 30 min), were deployed at a site located downwind from the industrial area of Dunkirk for a one-year duration (July 2013-September 2014). An Aerosol Chemical Speciation Monitor (ACSM) and an Aethalometer monitored the main chemical species in the non-refractory submicron particles and black carbon, respectively. Concomitant measurements of trace gases and wind speed and direction were also performed. This dataset was analyzed considering four wind sectors, characteristics of marine, industrial, industrial-urban, and urban influences, and the different seasons. We will present a descriptive analysis of PM1, showing strong variations of ambient concentrations, as well as evidences of SO2 to SO4 gas-particle conversion when industrial plumes reached the monitoring site. The organic fraction measured by ACSM (37% of the total mass on average) was analyzed using a source-receptor model based on Positive Matrix Factorization (PMF) to identify chemical signatures of main emission sources and to quantify the contribution of each source to the PM1 budget given the wind sector. Four main factors were identified: hydrocarbon organic aerosol (HOA), oxygenated organic aerosol (OOA), biomass burning organic aerosol (BBOA) and cooking-like organic aerosol (COA). Overall, the total PM1 mass loading was dominated by secondary inorganic species and OOA. The seasonal variations of different identified factors will be discussed as well as the influence of ship emissions.

Religious Burning as a Major Source of Atmospheric Fine Aerosols in Lhasa city in the Tibetan Plateau

NASA Astrophysics Data System (ADS)

Liu, S.; Cui, Y.; Zhixuan, B.; Bian, J.; McKeen, S. A.; Watts, L. A.; Ciciora, S. J.; Gao, R. S.

2017-12-01

Measurements of aerosols in the Tibetan Plateau are scant due to the high altitude and harsh climate. To bridge this gap, we carried out the first field measurements of aerosol size distributions in Lhasa, a major city in the Tibetan Plateau that has been experiencing fast urbanization and reduced air quality. Aerosol number size distribution was continuously measured using an optical particle size spectrometer near the center of Lhasa city during the Asian summer monsoon season in 2016. The mass concentration of fine particles was modulated by boundary layer dynamics, with an average of 11 µg m-3 and the high values exceeding 50 µg m-3 during religious holidays. Daytime high concentration coincided with the religious burning of biomass and incense in the temples during morning hours, which produced heavy smoke. Factor analysis revealed a factor that is likely induced by religious burning. The factor contributed 34% of the campaign-average fine particle mass and the contribution reached up to 80% during religious holidays. The mass size distribution of aerosols produced from religious burnings peaked at 500 nm, indicating that these particles could efficiently decrease visibility and promote health risk. Because of its significance, our results suggest that more attention should be paid to religious burning, a currently under-studied source, in the Tibetan Plateau and in other regions of the world where religious burnings are frequently practiced.

Urban air quality assessment using monitoring data of fractionized aerosol samples, chemometrics and meteorological conditions.

PubMed

Yotova, Galina I; Tsitouridou, Roxani; Tsakovski, Stefan L; Simeonov, Vasil D

2016-01-01

The present article deals with assessment of urban air by using monitoring data for 10 different aerosol fractions (0.015-16 μm) collected at a typical urban site in City of Thessaloniki, Greece. The data set was subject to multivariate statistical analysis (cluster analysis and principal components analysis) and, additionally, to HYSPLIT back trajectory modeling in order to assess in a better way the impact of the weather conditions on the pollution sources identified. A specific element of the study is the effort to clarify the role of outliers in the data set. The reason for the appearance of outliers is strongly related to the atmospheric condition on the particular sampling days leading to enhanced concentration of pollutants (secondary emissions, sea sprays, road and soil dust, combustion processes) especially for ultra fine and coarse particles. It is also shown that three major sources affect the urban air quality of the location studied-sea sprays, mineral dust and anthropogenic influences (agricultural activity, combustion processes, and industrial sources). The level of impact is related to certain extent to the aerosol fraction size. The assessment of the meteorological conditions leads to defining of four downwind patterns affecting the air quality (Pelagic, Western and Central Europe, Eastern and Northeastern Europe and Africa and Southern Europe). Thus, the present study offers a complete urban air assessment taking into account the weather conditions, pollution sources and aerosol fractioning.

Incorporation of new particle formation and early growth treatments into WRF/Chem: Model improvement, evaluation, and impacts of anthropogenic aerosols over East Asia

NASA Astrophysics Data System (ADS)

Cai, Changjie; Zhang, Xin; Wang, Kai; Zhang, Yang; Wang, Litao; Zhang, Qiang; Duan, Fengkui; He, Kebin; Yu, Shao-Cai

2016-01-01

New particle formation (NPF) provides an important source of aerosol particles and cloud condensation nuclei, which may result in enhanced cloud droplet number concentration (CDNC) and cloud shortwave albedo. In this work, several nucleation parameterizations and one particle early growth parameterization are implemented into the online-coupled Weather Research and Forecasting model coupled with chemistry (WRF/Chem) to improve the model's capability in simulating NPF and early growth of ultrafine particles over East Asia. The default 8-bin over the size range of 39 nm-10 μm used in the Model for Simulating Aerosol Interactions and Chemistry aerosol module is expanded to the 12-bin over 1 nm-10 μm to explicitly track the formation and evolution of new particles. Although model biases remain in simulating H2SO4, condensation sink, growth rate, and formation rate, the evaluation of July 2008 simulation identifies a combination of three nucleation parameterizations (i.e., COMB) that can best represent the atmospheric nucleation processes in terms of both surface nucleation events and the resulting vertical distribution of ultrafine particle concentrations. COMB consists of a power law of Wang et al. (2011) based on activation theory for urban areas in planetary boundary layer (PBL), a power law of Boy et al. (2008) based on activation theory for non-urban areas in PBL, and the ion-mediated nucleation parameterization of YU10 for above PBL. The application and evaluation of the improved model with 12-bin and the COMB nucleation parameterization in East Asia during January, April, July, and October in 2001 show that the model has an overall reasonably good skill in reproducing most observed meteorological variables and surface and column chemical concentrations. Relatively large biases in simulated precipitation and wind speeds are due to inaccurate surface roughness and limitations in model treatments of cloud formation and aerosol-cloud-precipitation interactions. Large biases in the simulated surface concentrations of PM10, NOx, CO, SO2, and VOCs at some sites are due in part to possible underestimations of emissions and in part to inaccurate meteorological predictions. The simulations of 2001 show that anthropogenic aerosols can increase aerosol optical depth by 64.0-228.3%, CDNC by 40.2-76.4%, and cloud optical thickness by 14.3-25.3%; they can reduce surface net shortwave radiation by up to 42.5-52.8 W m-2, 2-m temperature by up to 0.34-0.83 °C, and PBL height by up to 76.8-125.9 m. Such effects are more significant than those previously reported for the U.S. and Europe.

Aged particles derived from emissions of coal-fired power plants: The TERESA field results

PubMed Central

Kang, Choong-Min; Gupta, Tarun; Ruiz, Pablo A.; Wolfson, Jack M.; Ferguson, Stephen T.; Lawrence, Joy E.; Rohr, Annette C.; Godleski, John; Koutrakis, Petros

2013-01-01

The Toxicological Evaluation of Realistic Emissions Source Aerosols (TERESA) study was carried out at three US coal-fired power plants to investigate the potential toxicological effects of primary and photochemically aged (secondary) particles using in situ stack emissions. The exposure system designed successfully simulated chemical reactions that power plant emissions undergo in a plume during transport from the stack to receptor areas (e.g., urban areas). Test atmospheres developed for toxicological experiments included scenarios to simulate a sequence of atmospheric reactions that can occur in a plume: (1) primary emissions only; (2) H2SO4 aerosol from oxidation of SO2; (3) H2SO4 aerosol neutralized by gas-phase NH3; (4) neutralized H2SO4 with secondary organic aerosol (SOA) formed by the reaction of α-pinene with O3; and (5) three control scenarios excluding primary particles. The aged particle mass concentrations varied significantly from 43.8 to 257.1 μg/m3 with respect to scenario and power plant. The highest was found when oxidized aerosols were neutralized by gas-phase NH3 with added SOA. The mass concentration depended primarily on the ratio of SO2 to NOx (particularly NO) emissions, which was determined mainly by coal composition and emissions controls. Particulate sulfate (H2SO4 + neutralized sulfate) and organic carbon (OC) were major components of the aged particles with added SOA, whereas trace elements were present at very low concentrations. Physical and chemical properties of aged particles appear to be influenced by coal type, emissions controls and the particular atmospheric scenarios employed. PMID:20462390

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

NASA Astrophysics Data System (ADS)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Relation between aerosol particles and their optical properties: a case study for São Paulo-Brazil

NASA Astrophysics Data System (ADS)

Miranda, Regina; Andrade, Maria de Fatima

2013-04-01

Brazil has a territory of 8.5 million km2 and a population of more than 160 million inhabitants, distributed throughout 26 states. Brazillian capital-cities with millions inhabitants and vehicles have several problems concerning air pollution. São Paulo, capital of São Paulo State, with more than 19 million inhabitants, 7 million vehicles, as well as the major industrial and technological park of the country, has high concentrations of air pollutants, especially in the winter. Air pollution, high building density, and a lack of green areas, combined with the proliferation of asphalt and concrete surfaces, have resulted in a greater number of urban heat island effects, fewer drizzle events, and rainfall events of greater intensity. São Paulo has an extensive air quality monitoring network, which has shown that ozone levels often exceed the NAAQS limit during spring and summer, and that concentrations of inhalable particles exceed the NAAQS limit mainly during the winter, from June to August. Aerosols are produced by a variety of processes, creating differences in their physicochemical properties and hence in their ability to scatter and absorb solar radiation. For most urban areas in Brazil, vehicles are considered the principal source of particles emitted to the atmosphere. Particles have been monitored in the winter of 2012 in São Paulo using a MOUDI (Micro Orifice Uniform Deposit Impactor), in order to have the mass distribution of the aerosol. The concentrations of coarse particles can still be larger than those of fine particles, although the difference between both has become smaller than in the past. The samples collected were analyzed by gravimetry for mass concentration, optical reflectance for Black Carbon concentration and X-ray Fluorescence for elementar characterization. Optical properties were obtained from Aeronet (Aerosol Robotic Network, http://aeronet.gsfc.nasa.gov/) for São Paulo city. It was found that a high fraction of elements was derived from mineral dust (Al, Si, Ca, Fe), anthropogenic particles and the burning of diesel (S), as well as from industries and residual oil combustion. Considering the trace element values obtained through EDXRF analysis, Angstron coefficients and Aerosol Optical Thickness (AOT 500 nm) were correlated (Pearson Correlation) to particulate and chemical elements. Soil elements have a positive correlation, fine particles are strong correlated to AOT. Elements like Fe, Si and Ca are usually related to larger particles and lower Angstron coefficients.

Evolution of multispectral aerosol optical properties in a biogenically-influenced urban environment during the CARES campaign

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Zaveri, R. A.; Song, C.; Pekour, M.; Flowers, B.; Dubey, M. K.; Setyan, A.; Zhang, Q.; Harworth, J. W.; Radney, J. G.; Atkinson, D. B.; China, S.; Mazzoleni, C.; Gorkowski, K.; Subramanian, R.; Jobson, B. T.; Moosmüller, H.

2013-03-01

Ground-based aerosol measurements made in June 2010 within Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area are used to investigate the evolution of multispectral optical properties as the urban aerosols aged and interacted with biogenic emissions. Along with black carbon and non-refractory aerosol mass and composition observations, spectral absorptio (βabs), scattering (βsca), and extinction (βext) coefficients for wavelengths ranging from 355 to 1064 nm were measured at both sites using photoacoustic (PA) instruments with integrating nephelometers and using cavity ring-down (CRD) instruments. The daytime average Ångström exponent of absorption (AEA) was ~1.6 for the wavelength pair 405 and 870 nm at T0, while it was ~1.8 for the wavelength pair 355 and 870 nm at T1, indicating a modest wavelength-dependent enhancement of absorption at both sites throughout the study. The measured and Mie theory calculations of multispectral βsca showed good correlation (R2=0.85-0.94). The average contribution of supermicron aerosol (mainly composed of sea salt particles advected in from the Pacific Ocean) to the total scattering coefficient ranged from less than 20% at 405 nm to greater than 80% at 1064 nm. From 22 to 28 June, secondary organic aerosol mass increased significantly at both sites due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the short wavelength scattering coefficients at both sites gradually increased due to increase in the size of submicron aerosols. At the same time, BC mass-normalized absorption cross-section (MAC) values for ultraviolet wavelengths at T1 increased by ~60% compared to the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for 870 nm wavelength were identical at both sites. These results suggest formation of moderately brown secondary organic aerosols formed in biogenically-influenced urban air.

Size evolution of ultrafine particles: Differential signatures of normal and episodic events.

PubMed

Joshi, Manish; Khan, Arshad; Anand, S; Sapra, B K

2016-01-01

The effect of fireworks on the aerosol number characteristics of atmosphere was studied for an urban mega city. Measurements were made at 50 m height to assess the local changes around the festival days. Apart from the increase in total number concentration and characteristic accumulation mode, short-term increase of ultrafine particle concentration was noted. Total number concentration varies an order of magnitude during the measurement period in which peak occurs at a frequency of approximately one per day. On integral scale, it seems not possible to distinguish an episodic (e.g. firework bursting induced aerosol emission) and a normal (ambient atmospheric changes) event. However these events could be differentiated on the basis of size evolution analysis around number concentration peaks. The results are discussed relative to past studies and inferences are drawn towards aerosol signatures of firework bursting. The short-term burst in ultrafine particle concentration can pose an inhalation hazard. Copyright © 2015 Elsevier Ltd. All rights reserved.

Long-range-transported bioaerosols captured in snow cover on Mount Tateyama, Japan: impacts of Asian-dust events on airborne bacterial dynamics relating to ice-nucleation activities

NASA Astrophysics Data System (ADS)

Maki, Teruya; Furumoto, Shogo; Asahi, Yuya; Lee, Kevin C.; Watanabe, Koichi; Aoki, Kazuma; Murakami, Masataka; Tajiri, Takuya; Hasegawa, Hiroshi; Mashio, Asami; Iwasaka, Yasunobu

2018-06-01

The westerly wind travelling at high altitudes over eastern Asia transports aerosols from the Asian deserts and urban areas to downwind areas such as Japan. These long-range-transported aerosols include not only mineral particles but also microbial particles (bioaerosols), that impact the ice-cloud formation processes as ice nuclei. However, the detailed relations of airborne bacterial dynamics to ice nucleation in high-elevation aerosols have not been investigated. Here, we used the aerosol particles captured in the snow cover at altitudes of 2450 m on Mt Tateyama to investigate sequential changes in the ice-nucleation activities and bacterial communities in aerosols and elucidate the relationships between the two processes. After stratification of the snow layers formed on the walls of a snow pit on Mt Tateyama, snow samples, including aerosol particles, were collected from 70 layers at the lower (winter accumulation) and upper (spring accumulation) parts of the snow wall. The aerosols recorded in the lower parts mainly came from Siberia (Russia), northern Asia and the Sea of Japan, whereas those in the upper parts showed an increase in Asian dust particles originating from the desert regions and industrial coasts of Asia. The snow samples exhibited high levels of ice nucleation corresponding to the increase in Asian dust particles. Amplicon sequencing analysis using 16S rRNA genes revealed that the bacterial communities in the snow samples predominately included plant associated and marine bacteria (phyla Proteobacteria) during winter, whereas during spring, when dust events arrived frequently, the majority were terrestrial bacteria of phyla Actinobacteria and Firmicutes. The relative abundances of Firmicutes (Bacilli) showed a significant positive relationship with the ice nucleation in snow samples. Presumably, Asian dust events change the airborne bacterial communities over Mt Tateyama and carry terrestrial bacterial populations, which possibly induce ice-nucleation activities, thereby indirectly impacting climate change.

Observations of Aerosol Optical Properties over 15 AERONET Sites in Southeast Asia

NASA Astrophysics Data System (ADS)

Chan, J. D.; Lagrosas, N.; Uy, S. N.; Holben, B. N.; Dorado, S.; Tobias, V., Jr.; Anh, N. X.; Po-Hsiung, L.; Janjai, S.; Salinas Cortijo, S. V.; Liew, S. C.; Lim, H. S.; Lestari, P.

2014-12-01

Mean column-integrated optical properties from ground sun photometers of the Aerosol Robotic Network (AERONET) are studied to provide an overview of the characteristics of aerosols over the region as part of the 7 Southeast Asian Studies (7-SEAS) mission. The 15 AERONET sites with the most available level 2 data products are selected from Thailand (Chiang Mai, Mukdahan, Songkhla and Silpakorn University), Malaysia (University Sains Malaysia), Laos (Vientiane), Vietnam (Bac Giang, Bac Lieu and Nha Trang), Taiwan (National Cheng Kung University and Central Weather Bureau Taipei), Singapore, Indonesia (Bandung) and the Philippines (Manila Observatory and Notre Dame of Marbel University). For all 15 sites, high angstrom exponent values (α>1) have been observed. Chiang Mai and USM have the highest mean Angstrom exponent indicating the dominance of fine particles that can be ascribed to biomass burning and urbanization. Sites with the lowest Angstrom exponent values include Bac Lieu (α=1.047) and Manila Observatory (α=1.021). From the average lognormal size distribution curves, Songkhla and NDMU show the smallest annual variation in the fine mode region, indicating the observed fine aerosols are local to the sites. The rest of the sites show high variation which could be due to large scale forcings (e.g., monsoons and biomass burnings) that affect aerosol properties in these sites. Both high and low single scattering albedo at 440 nm (ω0440) values are found in sites located in major urban areas. Silpakorn University, Manila Observatory and Vientiane have all mean ω0440 < 0.90. Singapore and CWB Taipei have ω0440 > 0.94. The discrepancy in ω0 suggests different types of major emission sources present in urban areas. The absorptivity of urban aerosols can vary depending on the strength of traffic emissions, types of fuel combusted and automobile engines used, and the effect of biomass burning aerosols during the dry season. High aerosol optical depth values (τa550 > 0.4) are mainly found over inland sites north of Songkhla and south of China on mainland Asia. Major pollution types in the region include biomass burning smoke and urban aerosols. The highest average τa550 is measured in Bac Giang, which has been studied to be greatly affected by aerosol sources from Eastern China during the later parts of the year.

Monthly and seasonal variations of aerosol optical properties and direct radiative forcing over Zanjan, Iran

NASA Astrophysics Data System (ADS)

Gharibzadeh, Maryam; Alam, Khan; Abedini, Yousefali; Bidokhti, Abbasali Aliakbari; Masoumi, Amir

2017-11-01

Aerosol optical properties and radiative forcing over Zanjan in northwest of Iran has been analyzed during 2010-2013. The aerosol optical and radiative properties are less studied over Zanjan, and therefore, require a careful and in depth analysis. The optical properties like Aerosol Optical Depth (AOD), Ångström Exponent (AE), ASYmmetry parameter (ASY), Single Scattering Albedo (SSA), and Aerosol Volume Size Distribution (AVSD) have been evaluated using the ground-based AErosol RObotic NETwork (AERONET) data. Higher AOD while relatively lower AE were observed in the spring and summer, which showed the presence of coarse mode particles in these seasons. An obvious increase of coarse mode particles in AVSD distribution, as well as a higher value of SSA represented considerable addition of coarse mode particles like dust into the atmosphere of Zanjan in these two seasons. Increase in AE, while a decrease in AOD was detected in the winter and fall. The presence of fine particles indicates the dominance of particles like urban-industrial aerosols from local sources especially in the winter. The Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model was utilized to calculate the Aerosol Radiative Forcing (ARF) at the Top of the Atmosphere (TOA), earth's surface and within the atmosphere. The annual averaged ARF values were -13.47 W m-2 and -36.1 W m-2 at the TOA and earth's surface, respectively, which indicate a significant cooling effect. Likewise, the ARF efficiencies at the TOA and earth's surface were -65.08 W m-2 and -158.43 W m-2, respectively. The annual mean atmospheric ARF and heating rate within the atmosphere were 22.63 W m-2 and 0.27 Kday-1 respectively, represented the warming effect within the atmosphere. Finally, a good agreement was found between AERONET retrieved ARF and SBDART simulated ARF.

Study of particulate matter from Primary/Secondary Marine Aerosol and anthropogenic sources collected by a self-made passive sampler for the evaluation of the dry deposition impact on built heritage.

PubMed

Morillas, Héctor; Maguregui, Maite; García-Florentino, Cristina; Marcaida, Iker; Madariaga, Juan Manuel

2016-04-15

Dry deposition is one of the most dangerous processes that can take place in the environment where the compounds that are suspended in the atmosphere can react directly on different surrounding materials, promoting decay processes. Usually this process is related with industrial/urban fog and/or marine aerosol in the coastal areas. Particularly, marine aerosol transports different types of salts which can be deposited on building materials and by dry deposition promotes different decay pathways. A new analytical methodology based on the combined use of Raman Spectroscopy and SEM-EDS (point-by-point and imaging) was applied. For that purpose, firstly evaporated seawater (presence of Primary Marine Aerosol (PMA)) was analyzed. After that, using a self-made passive sampler (SMPS), different suspended particles coming from marine aerosol (transformed particles in the atmosphere (Secondary Marine Aerosol (SMA)) and metallic airborne particulate matter coming from anthropogenic sources, were analyzed. Finally in order to observe if SMA and metallic particles identified in the SMPS can be deposited on a building, sandstone samples from La Galea Fortress (Getxo, north of Spain) located in front of the sea and in the place where the passive sampler was mounted were analyzed. Copyright © 2016 Elsevier B.V. All rights reserved.

Morphology and mixing of black carbon particles collected in central California during the CARES field study

DOE PAGES

Moffet, Ryan C.; O'Brien, Rachel E.; Alpert, Peter A.; ...

2016-11-23

Aerosol absorption is strongly dependent on the internal heterogeneity (mixing state) and morphology of individual particles containing black carbon (BC) and other non-absorbing species. Here, we examine an extensive microscopic data set collected in the California Central Valley during the CARES 2010 field campaign. During a period of high photochemical activity and pollution buildup, the particle mixing state and morphology were characterized using scanning transmission X-ray microscopy (STXM) at the carbon K-edge. Observations of compacted BC core morphologies and thick organic coatings at both urban and rural sites provide evidence of the aged nature of particles, highlighting the importance ofmore » highly aged particles at urban sites during periods of high photochemical activity. Based on the observation of thick coatings and more convex BC inclusion morphology, either the aging was rapid or the contribution of fresh BC emissions at the urban site was relatively small compared to background concentrations. Most particles were observed to have the BC inclusion close to the center of the host. However, host particles containing inorganic rich inclusions had the BC inclusion closer to the edge of the particle. Furthermore, these measurements of BC morphology and mixing state provide important constraints for the morphological effects on BC optical properties expected in aged urban plumes.« less

Morphology and mixing of black carbon particles collected in central California during the CARES field study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moffet, Ryan C.; O'Brien, Rachel E.; Alpert, Peter A.

Aerosol absorption is strongly dependent on the internal heterogeneity (mixing state) and morphology of individual particles containing black carbon (BC) and other non-absorbing species. Here, we examine an extensive microscopic data set collected in the California Central Valley during the CARES 2010 field campaign. During a period of high photochemical activity and pollution buildup, the particle mixing state and morphology were characterized using scanning transmission X-ray microscopy (STXM) at the carbon K-edge. Observations of compacted BC core morphologies and thick organic coatings at both urban and rural sites provide evidence of the aged nature of particles, highlighting the importance ofmore » highly aged particles at urban sites during periods of high photochemical activity. Based on the observation of thick coatings and more convex BC inclusion morphology, either the aging was rapid or the contribution of fresh BC emissions at the urban site was relatively small compared to background concentrations. Most particles were observed to have the BC inclusion close to the center of the host. However, host particles containing inorganic rich inclusions had the BC inclusion closer to the edge of the particle. Furthermore, these measurements of BC morphology and mixing state provide important constraints for the morphological effects on BC optical properties expected in aged urban plumes.« less

Religious burning as a potential major source of atmospheric fine aerosols in summertime Lhasa on the Tibetan Plateau

NASA Astrophysics Data System (ADS)

Cui, Yu Yan; Liu, Shang; Bai, Zhixuan; Bian, Jianchun; Li, Dan; Fan, Kaiyu; McKeen, Stuart A.; Watts, Laurel A.; Ciciora, Steven J.; Gao, Ru-Shan

2018-05-01

We carried out field measurements of aerosols in Lhasa, a major city in the Tibetan Plateau that has been experiencing fast urbanization and industrialization. Aerosol number size distribution was continuously measured using an optical particle size spectrometer near the center of Lhasa city during the Asian summer monsoon season in 2016. The mass concentration of fine particles was modulated by boundary layer dynamics, with an average of 11 μg m-3 and the high values exceeding 50 μg m-3 during religious holidays. Daytime high concentration coincided with the religious burning of biomass and incense in the temples during morning hours, which produced heavy smoke. Factor analysis revealed a factor that likely represented religious burning. The factor contributed 34% of the campaign-average fine particle mass and the contribution reached up to 80% during religious holidays. The mass size distribution of aerosols produced from religious burnings peaked at ∼500 nm, indicating that these particles could efficiently decrease visibility and promote health risk. Because of its significance, our results suggest that further studies of religious burning, a currently under-studied source, are needed in the Tibetan Plateau and in other regions of the world where religious burnings are frequently practiced.

Aerosol Remote Sensing from Space -- What We've Learned, Where We're Heading

NASA Technical Reports Server (NTRS)

Kahn, Ralph

2010-01-01

The MISR and MODIS instruments aboard the NASA Earth Observing System's Terra Satellite have been collecting data containing information about the state of Earth's atmosphere and surface for over ten years. Among the retrieved quantities are amount and type of wildfire smoke, desert dust, volcanic effluent, urban and industrial pollution particles, and other aerosols. However, the broad scientific challenges of understanding aerosol impacts on climate and health place different, and very exacting demands on our measurement capabilities. And these data sets, though much more advanced in many respects than previous aerosol data records, are imperfect. In this presentation, I will summarize current understanding of MISR and MODIS aerosol product strengths and limitations, discuss how they relate to the bigger aerosol science questions we must address, and give my view of what we will need to do to progress.

Aerosol Remote Sensing from Space - Where We Stand, Where We're Heading

NASA Technical Reports Server (NTRS)

Kahn, Ralph

2011-01-01

The MISR and MODIS instruments aboard the NASA Earth Observing System's Terra Satellite have been collecting data containing information about the state of Earth's atmosphere and surface for over eleven years. Among the retrieved quantities are amount and type of wildfire smoke, desert dust, volcanic effluent, urban and industrial pollution particles, and other aerosols. However, the broad scientific challenges of understanding aerosol impacts on climate and health place different, and very exacting demands on our measurement capabilities. And these data sets, though much more advanced in many respects than previous aerosol data records, are imperfect. In this presentation, I will summarize current understanding of MISR and MODIS aerosol product strengths and limitations, discuss how they relate to the bigger aerosol science questions we must address, and give my view of the way forward.

Aerosol Remote Sensing from Space - Where We Stand, Where We're Heading

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.

2013-01-01

The MISR and MODIS instruments aboard the NASA Earth Observing System's Terra Satellite have been collecting data containing information about the state of Earth's atmosphere and surface for over eleven years. Among the retrieved quantities are amount and type of wildfire smoke, desert dust, volcanic effluent, urban and industrial pollution particles, and other aerosols. However, the broad scientific challenges of understanding aerosol impacts on climate and health place different, and very exacting demands on our measurement capabilities. And these data sets, though much more advanced in many respects than previous aerosol data records, are imperfect. In this presentation, I will summarize current understanding of MISR and MODIS aerosol product strengths and limitations, discuss how they relate to the bigger aerosol science questions we must address, and give my view of the way forward.

Modelling of strong heterogeneities in aerosol single scattering albedos over a polluted region

NASA Astrophysics Data System (ADS)

Mallet, M.; Pont, V.; Liousse, C.

2005-05-01

To date, most models dedicated to the investigation of aerosol direct or semi-direct radiative forcings have assumed the various aerosol components to be either completely externally mixed or homogeneously internally mixed. Some recent works have shown that a core-shell treatment of particles should be more realistic, leading to significant differences in the radiative impact as compared to only externally or well-internally mixed states. To account for these studies, an optical module, ORISAM-RAD, has been developed for computing aerosol radiative properties under the hypothesis of internally mixed particles with a n-layer spherical concentric structure. Mesoscale simulations using ORISAM-RAD, coupled with the 3D mesoscale model Meso-NH-C, have been performed for one selected day (06/24/2001) during the ESCOMPTE experiment in the Marseilles-Fos/Berre region, which illustrate the ability of this new module to reproduce spatial heterogeneities of measured single scattering albedo (ωo), due to industrial and/or urban pollution plumes.

Optical and Chemical Characterization of Aerosols Produced from Cooked Meats

NASA Astrophysics Data System (ADS)

Niedziela, R. F.; Foreman, E.; Blanc, L. E.

2011-12-01

Cooking processes can release a variety compounds into the air immediately above a cooking surface. The distribution of compounds will largely depend on the type of food that is being processed and the temperatures at which the food is prepared. High temperatures release compounds from foods like meats and carry them away from the preparation surface into cooler regions where condensation into particles can occur. Aerosols formed in this manner can impact air quality, particularly in urban areas where the amount of food preparation is high. Reported here are the results of laboratory experiments designed to optically and chemically characterize aerosols derived from cooking several types of meats including ground beef, salmon, chicken, and pork both in an inert atmosphere and in synthetic air. The laboratory-generated aerosols are studied using a laminar flow cell that is configured to accommodate simultaneous optical characterization in the mid-infrared and collection of particles for subsequent chemical analysis by gas chromatography. Preliminary optical results in the visible and ultra-violet will also be presented.

Baseline Maritime Aerosol: Methodology to Derive the Optical Thickness and Scattering Properties

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Smirnov, Alexander; Holben, Brent N.; Dubovik, Oleg; Einaudi, Franco (Technical Monitor)

2001-01-01

Satellite Measurements of the global distribution of aerosol and their effect on climate should be viewed in respect to a baseline aerosol. In this concept, concentration of fine mode aerosol particles is elevated above the baseline by man-made activities (smoke or urban pollution), while coarse mode by natural processes (e.g. dust or sea-spray). Using 1-3 years of measurements in 10 stations of the Aerosol Robotic network (ACRONET we develop a methodology and derive the optical thickness and properties of this baseline aerosol for the Pacific and Atlantic Oceans. Defined as the median for periods of stable optical thickness (standard deviation < 0.02) during 2-6 days, the median baseline aerosol optical thickness over the Pacific Ocean is 0.052 at 500 am with Angstrom exponent of 0.77, and 0.071 and 1.1 respectively, over the Atlantic Ocean.

Size distributions of aerosol and water-soluble ions in Nanjing during a crop residual burning event.

PubMed

Wang, Honglei; Zhu, Bin; Shen, Lijuan; Kang, Hanqing

2012-01-01

To investigate the impact on urban air pollution by crop residual burning outside Nanjing, aerosol concentration, pollution gas concentration, mass concentration, and water-soluble ion size distribution were observed during one event of November 4-9, 2010. Results show that the size distribution of aerosol concentration is bimodal on pollution days and normal days, with peak values at 60-70 and 200-300 nm, respectively. Aerosol concentration is 10(4) cm(-3) x nm(-1) on pollution days. The peak value of spectrum distribution of aerosol concentration on pollution days is 1.5-3.3 times higher than that on a normal day. Crop residual burning has a great impact on the concentration of fine particles. Diurnal variation of aerosol concentration is trimodal on pollution days and normal days, with peak values at 03:00, 09:00 and 19:00 local standard time. The first peak is impacted by meteorological elements, while the second and third peaks are due to human activities, such as rush hour traffic. Crop residual burning has the greatest impact on SO2 concentration, followed by NO2, O3 is hardly affected. The impact of crop residual burning on fine particles (< 2.1 microm) is larger than on coarse particles (> 2.1 microm), thus ion concentration in fine particles is higher than that in coarse particles. Crop residual burning leads to similar increase in all ion components, thus it has a small impact on the water-soluble ions order. Crop residual burning has a strong impact on the size distribution of K+, Cl-, Na+, and F- and has a weak impact on the size distributions of NH4+, Ca2+, NO3- and SO4(2-).

COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

DOE Office of Scientific and Technical Information (OSTI.GOV)

Worsnop, Douglas R.

2014-07-28

This project funded the participation of scientists from seven research groups, running more than thirty instruments, in the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London. The primary science questions for the ClearfLo Winter IOP were, 1) what is the urban increment of particulate matter (PM) and other pollutants in the greater London area, and, 2) what is the contribution of solid fuel use for home heating to wintertime PM? An additional motivation for the Detling measurements was the question ofmore » whether coatings on black carbon particles enhance absorption. The following four key accomplishments have been identified so far: 1) Chemical, physical and optical characterization of PM from local and regional sources (Figures 2, 4, 5 and 6). 2) Measurement of urban increment in particulate matter and gases in London (Figure 3). 3) Measurement of optical properties and chemical composition of coatings on black carbon containing particles indicates absorption enhancement. 4) First deployment of chemical ionization instrument (MOVI-CI-TOFMS) to measure both particle-phase and gas-phase organic acids. (See final report from Joel Thornton, University of Washington, for details.) Analysis of the large dataset acquired in Detling is ongoing and will yield further key accomplishments. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal. The measurement of absorption enhancement by coatings on black carbon will contribute to improved modeling of the direct radiative properties of PM.« less

Ion chemistry and source identification of coarse and fine aerosols in an urban area of eastern central India

NASA Astrophysics Data System (ADS)

Verma, Santosh K.; Deb, Manas K.; Suzuki, Yukio; Tsai, Ying I.

2010-01-01

This work focuses on size segregated atmospheric aerosol mass concentrations and water soluble inorganic components in Chhattisgarh, the eastern central India. Investigation on the monitoring of ambient air levels of atmospheric particulates were done around a large source of primary anthropogenic particulate emissions: the industrial area and coal based power plants. Chemical characterization was carried out for aerosol samples collected in urban area, Raipur, (21°14'N, 81°38'E) of Chhattisgarh region over a period of one year, using cascade impactor. Annual mean of mass concentration for coarse (PM 2.5-10) and fine (PM 2.5) aerosols were monitored to be 238.1 ± 89.9 and 167.0 ± 75.3 µg m - 3 respectively This work deals with the seasonal variation and meteorological influences of inorganic components of the aerosols viz. NO 3-, Cl - and SO 42-, Mg 2+, Na +, K +, Ca 2+ and NH 4+. The annual mean concentration of the inorganic components were monitored to be 3.8 ± 2.5, 8.9 ± 2.7, 10.2 ± 1.5, 2.6 ± 0.6, 8.7 ± 7.2, 4.6 ± 1.8, 16.4 ± 6.9 and 0.4 ± 0.5 µg m - 3 respectively in coarse particles and 8.2 ± 7.1, 6.8 ± 3.6, 46.5 ± 32.8, 1.7 ± 0.6, 7.4 ± 3.6, 5.9 ± 3.4, 10.2 ± 2.9, and 8.8 ± 7.7 µg m - 3 respectively in fine particles, for the above ions. The average distribution of nitrate and sulphate in PM 2.5-10 were found to be 1.6 and 4.2% and in PM 2.5 were 4.9 and 27.9% respectively indicating the dominance of sulphate in both PM 2.5-10 and PM 2.5 particles. Here, industrial emission plays important role for contribution of PM 2.5 particle loading in the atmosphere. The cation-anion rational analysis indicated that the PM 2.5-10 particles were mostly neutralized and PM 2.5 particle were acidic. The major ions were mainly in the form of NaCl > CaSO 4 > K 2SO 4 > MgSO 4 > KCl > NH 4Cl > Ca(NO 3) 2 > KNO 3 > MgCl 2 > Mg(NO 3) 2 > NH 4NO 3 > (NH 4) 2SO 4 in coarse aerosol particles and (NH 4) 2SO 4 > K 2SO 4 > CaSO 4 > NaCl > NH 4NO 3 > CaCl 2 > KNO 3 > MgCl 2 > Ca(NO 3) 2 > KCl > NH 4Cl in fine particles.

Changes in the physico-chemical properties of Amazonian aerosols from background conditions due to urban impacts in Central Amazonia.

NASA Astrophysics Data System (ADS)

Artaxo, P.; Barbosa, H. M.; Brito, J.; Carbone, S.; Fiorese, C.; Andre, B.; Rizzo, L. V.; Ditas, F.; Pöhlker, C.; Pöhlker, M. L.; Saturno, J.; Holanda, B. A.; Wang, J.; Souza, R. A. F. D.; Machado, L.; Andreae, M. O.; Martin, S. T.

2016-12-01

The GoAmazon 2014/15 experiment (Observations and Modeling of the Green Ocean Amazon) was a great opportunity to study how urbanization can change aerosol properties under pristine conditions in a tropical rain forest. The experiment took place from January 2014 to December 2015 in the vicinity of Manaus, Brazil, where several sampling stations were operated. Natural biogenic aerosol properties were studied in 3 sampling stations upwind of Manaus (ATTO (T0a), ZF2 (T0z) and EMBRAPA (T0e)). Urban impacted aerosols were analysed in two downwind sampling stations at Tiwa (T2) and Manacapuru (T3). Properties analysed were size distribution, scattering and absorption, composition, vertical profiles and others. Remote sensing measurements were done using AERONET and MODIS, while extensive ground based measurements were done in all sampling stations. Remote sensing measurements shows important changes in aerosol optical depth (AOD), especially in the aerosol absorption component. It was also observed a reduction in cloud droplet size downwind of Manaus for liquid phase clouds. Changes in particle number and size were also very significant, that reflected in changes in the aerosol radiative forcing (RF) before and after Manaus plume. In the dry season, an average RF of -24 w/m² was observed upwind, while -17 w/m² was observed downwind, due to large scale biomass burning aerosols. Single scattering albedo (SSA) at 550 nm changed from a high value of 0.96 upwind to 0.84 downwind due to the increase in absorbing aerosols in the wet season. In the dry season, SSA at 550nm changed from 0.95 to 0.87. Aerosol composition showed a large dominance of organic aerosols for all sites, accounting for 65-75% of PM1 non refractory aerosol. Most of these were secondary organic aerosol (SOA), with very low sulfate and nitrate concentrations. The influence of the Manaus plume on aerosol properties was more intense during the wet season, because in the dry season a significant amount of large scale biomass burning aerosol was observed for all GoAmazon 2014/15 sites.

Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-04-01

Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental scale emissions.

Chemical and physical properties of biomass burning aerosols and their CCN activity: A case study in Beijing, China.

PubMed

Wu, Zhijun; Zheng, Jing; Wang, Yu; Shang, Dongjie; Du, Zhoufei; Zhang, Yuanhang; Hu, Min

2017-02-01

Biomass burning emits large amounts of both trace gases and particles into the atmosphere. It plays a profound role in regional air quality and climate change. In the present study, an intensive campaign was carried out at an urban site in Beijing, China, in June 2014, which covered the winter wheat harvest season over the North China Plain (NCP). Meanwhile, two evident biomass-burning events were observed. A clear burst in ultrafine particles (below 100nm in diameter, PM 1 ) and subsequent particle growth took place during the events. With the growth of the ultrafine particles, the organic fraction of PM 1 increased significantly. The ratio of oxygen to carbon (O:C), which had an average value of 0.23±0.04, did not show an obvious enhancement, indicating that a significant chemical aging process of the biomass-burning aerosols was not observed during the course of events. This finding might have been due to the fact that the biomass-burning events occurred in the late afternoon and grew during the nighttime, which is associated with a low atmospheric oxidation capacity. On average, organics and black carbon (BC) were dominant in the biomass-burning aerosols, accounting for 60±10% and 18±3% of PM 1 . The high organic and BC fractions led to a significant suppression of particle hygroscopicity. Comparisons among hygroscopicity tandem differential mobility analyzer (HTDMA)-derived, cloud condensation nuclei counter (CCNc)-derived, and aerosol mass spectrometer-based hygroscopicity parameter (κ) values were consistent. The mean κ values of biomass-burning aerosols derived from both HTDMA and CCNc measurements were approximately 0.1, regardless of the particle size, indicating that the biomass-burning aerosols were less active. The burst in particle count during the biomass-burning events resulted in an increased number of cloud condensation nuclei (CCN) at supersaturation (SS)=0.2-0.8%. Copyright © 2016 Elsevier B.V. All rights reserved.

Steps Toward an EOS-Era Aerosol Type Climatology

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.

2012-01-01

We still have a way to go to develop a global climatology of aerosol type from the EOS-era satellite data record that currently spans more than 12 years of observations. We have demonstrated the ability to retrieve aerosol type regionally, providing a classification based on the combined constraints on particle size, shape, and single-scattering albedo (SSA) from the MISR instrument. Under good but not necessarily ideal conditions, the MISR data can distinguish three-to-five size bins, two-to-four bins in SSA, and spherical vs. non-spherical particles. However, retrieval sensitivity varies enormously with scene conditions. So, for example, there is less information about aerosol type when the mid-visible aerosol optical depth (AOD) is less that about 0.15 or 0.2, or when the range of scattering angles observed is reduced by solar geometry, even though the quality of the AOD retrieval itself is much less sensitive to these factors. This presentation will review a series of studies aimed at assessing the capabilities, as well as the limitations, of MISR aerosol type retrievals involving wildfire smoke, desert dust, volcanic ash, and urban pollution, in specific cases where suborbital validation data are available. A synthesis of results, planned upgrades to the MISR Standard aerosol algorithm to improve aerosol type retrievals, and steps toward the development of an aerosol type quality flag for the Standard product, will also be covered.

Optical and microphysical properties of atmospheric aerosols in Moldova

NASA Astrophysics Data System (ADS)

Aculinin, Alexandr; Smicov, Vladimir

2010-05-01

Measurements of aerosol properties in Kishinev, Moldova are being carried out within the framework of the international AERONET program managed by NASA/GSFC since 1999. Direct solar and sky diffuse radiances are measured by using of sunphotometer Cimel-318. Aerosol optical properties are retrieved from measured radiances by using of smart computational procedures developed by the AERONET's team. The instrument is situated at the ground-based solar radiation monitoring station giving the opportunity to make simultaneous spectral (win sunphotometer) and broadband (with the set of sensors from radiometric complex) solar radiation. Detailed description of the station and investigations in progress can be found at the http://arg.phys.asm.md. Ground station is placed in an urban environment of Kishinev city (47.00N; 28.56E; 205 m a.s.l). Summary of aerosol optical and microphysical properties retrieved from direct solar and diffuse sky radiance observations at Moldova site from September 1999 to June 2009 are presented below. Number of measurements (total): 1695 Number of measurements (for ?o, n, k): 223 Range of aerosol optical depth (AOD) @440 nm: 0.03 < ?(440) < 2.30, < ?(440)>=0.25 Range of Ångström parameter < α440_870 >: 0.14 < α < 2.28 Asymmetry factor (440/670/870/1020): 0.70/0.63/0.59/0.58 ±0.04 Refraction (n) and absorption (k) indices@440 nm: 1.41 ± 0.06; 0.009 ± 0.005 Single scattering albedo < ?o >(440/670/870/1020): 0.93/0.92/0.90/0.89 ±0.04 Parameters of volume particle size distribution function: (fine mode) volume median radius r v,f , μm: 0.17 ± 0.06 particle volume concentration Cv,f, μm3/μm2: 0.04 ± 0.03 (coarse mode) volume median radius rv,c , μm: 3.08 ± 0.64 particle volume concentration Cv,c, μm3/μm2: 0.03 ± 0.03 Climatic norms of AOD@500 nm and Ångström parameter < α440_870 > at the site of observation are equal to 0.21 ± 0.06 and 1.45 ± 0.14, respectively. The aerosol type in Moldova may be considered as 'urban-industrial and mixed' in accordance with the classification of aerosol type models systematized and developed by AERONET team (O.Dubovik et al., 2002, J. Atmosph. Sci., 59, 590-608) on the basis of datasets acquired from worldwide observations at the network of sunphotometers. It should be noted the presence of increased value of absorption index and reduced values of albedo. This may be due to influence of absorptive aerosols (soot). These aerosols are originated from local dust sources and exhausts from intensive urban traffic, from sources of biomass and household garbage burning both in and around the city, and from long-range transport over regions with high loading of aerosols (dust, smoke).

Evaluation of a coupled dispersion and aerosol process model against measurements near a major road

NASA Astrophysics Data System (ADS)

Pohjola, M. A.; Pirjola, L.; Karppinen, A.; Härkönen, J.; Ketzel, M.; Kukkonen, J.

2007-02-01

A field measurement campaign was conducted near a major road "Itäväylä" in an urban area in Helsinki in 17-20 February 2003. Aerosol measurements were conducted using a mobile laboratory "Sniffer" at various distances from the road, and at an urban background location. Measurements included particle size distribution in the size range of 7 nm-10 μm (aerodynamic diameter) by the Electrical Low Pressure Impactor (ELPI) and in the size range of 3-50 nm (mobility diameter) by Scanning Mobility Particle Sizer (SMPS), total number concentration of particles larger than 3 nm detected by an ultrafine condensation particle counter (UCPC), temperature, relative humidity, wind speed and direction, driving route of the mobile laboratory, and traffic density on the studied road. In this study, we have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI used in combination with an aerosol process model MONO32. The vehicular exhaust emissions, and atmospheric dispersion and transformation of fine and ultrafine particles was evaluated within the distance scale of 200 m (corresponding to a time scale of a couple of minutes). We computed the temporal evolution of the number concentrations, size distributions and chemical compositions of various particle size classes. The atmospheric dilution rate of particles is obtained from the roadside dispersion model CAR-FMI. Considering the evolution of total number concentration, dilution was shown to be the most important process. The influence of coagulation and condensation on the number concentrations of particle size modes was found to be negligible at this distance scale. Condensation was found to affect the evolution of particle diameter in the two smallest particle modes. The assumed value of the concentration of condensable organic vapour of 1012 molecules cm-3 was shown to be in a disagreement with the measured particle size evolution, while the modelling runs with the concentration of condensable organic vapour of 109-1010 molecules cm-3 resulted in particle sizes that were closest to the measured values.

Aerosol optical properties and direct radiative forcing based on measurements from the China Aerosol Remote Sensing Network (CARSNET) in eastern China

NASA Astrophysics Data System (ADS)

Che, Huizheng; Qi, Bing; Zhao, Hujia; Xia, Xiangao; Eck, Thomas F.; Goloub, Philippe; Dubovik, Oleg; Estelles, Victor; Cuevas-Agulló, Emilio; Blarel, Luc; Wu, Yunfei; Zhu, Jun; Du, Rongguang; Wang, Yaqiang; Wang, Hong; Gui, Ke; Yu, Jie; Zheng, Yu; Sun, Tianze; Chen, Quanliang; Shi, Guangyu; Zhang, Xiaoye

2018-01-01

Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71-0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (˜ 0.40-0.60) than in January and February (0.71-0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ˜ 0.04-0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was -93 ± 44 to -79 ± 39 W m-2 at the Earth's surface and ˜ -40 W m-2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80°) under cloud-free conditions. The fine mode composed a major contribution of the absorbing particles in the classification scheme based on SSA, fine-mode fraction and extinction Angström exponent. This study contributes to our understanding of aerosols and regional climate/air quality, and the results will be useful for validating satellite retrievals and for improving climate models and remote sensing algorithms.

LOAC (Light Optical Particle Counter): a new small aerosol counter with particle characterization capabilities for surface and airborne measurements

NASA Astrophysics Data System (ADS)

Renard, Jean-Baptiste; Berthet, Gwenael; Jégou, Fabrice; Jeannot, Matthieu; Jourdain, Line; Dulac, François; Mallet, Marc; Dupont, Jean-Charles; Thaury, Claire; Tonnelier, Thierry; Verdier, Nicolas; Charpentier, Patrick

2013-04-01

The determination of the size distribution of tropospheric and stratospheric aerosols with conventional optical counters is difficult when different natures of particles are present (droplets, soot, mineral dust, secondary organic or mineral particles...). Also, a light and cheap aerosol counter that can be used at ground, onboard drones or launched under all kinds of atmospheric balloons can be very useful during specific events as volcanic plumes, desert dust transport or local pollution episodes. These goals can be achieved thanks to a new generation of aerosol counter, called LOAC (Light Optical Aerosol Counter). The instrument was developed in the frame of a cooperation between French scientific laboratories (CNRS), the Environnement-SA and MeteoModem companies and the French Space Agency (CNES). LOAC is a small optical particle counter/sizer of ~250 grams, having a low electrical power consumption. The measurements are conducted at two scattering angles. The first one, at 12°, is used to determine the aerosol particle concentrations in 19 size classes within a diameter range of 0.3-100 micrometerers. At such an angle close to forward scattering, the signal is much more intense and the measurements are the least sensitive to the particle nature. The second angle is at 60°, where the scattered light is strongly dependent on the particle refractive index and thus on the nature of the aerosols. The ratio of the measurements at the two angles is used to discriminate between the different types of particles dominating the nature of the aerosol particles in the different size classes. The sensor particularly discriminates wet or liquid particles, soil dust and soot. Since 2011, we have operated LOAC in various environments (Arctic, Mediterranean, urban and peri-urban…) under different kinds of balloons including zero pressure stratospheric, tethered, drifting tropospheric, and meteorological sounding balloons. For the last case, the total weight of the gondola including the PTU sonde, transmission and batteries is below 1 kg. The results obtained during these flights and related campaigns such as the ground-based winter campaign Paris-Fog in Ile de France (fog life circle) and the Pre-ChArMEx/TRAQA summer campaign on the French Mediterranean coast will be presented, as well as future campaigns in which LOAC is involved, especially ChArMEx, (flights in the lower troposphere above the Mediterranean Sea), and Strateole (long duration flights in the tropical stratosphere). Balloon operation of LOAC will tentatively been shown during EGU.

Dust aerosol properties and radiative forcing observed in spring during 2001-2014 over urban Beijing, China.

PubMed

Yu, Xingna; Lü, Rui; Kumar, K Raghavendra; Ma, Jia; Zhang, Qiuju; Jiang, Yilun; Kang, Na; Yang, Suying; Wang, Jing; Li, Mei

2016-08-01

The ground-based characteristics (optical and radiative properties) of dust aerosols measured during the springtime between 2001 and 2014 were investigated over urban Beijing, China. The seasonal averaged aerosol optical depth (AOD) during spring of 2001-2014 was about 0.78 at 440 nm. During dust days, higher AOD occurred associated with lower Ångström exponent (AE). The mean AE440-870 in the springtime was about 1.0, indicating dominance of fine particles over the region. The back-trajectory analysis revealed that the dust was transported from the deserts of Inner Mongolia and Mongolia arid regions to Beijing. The aerosol volume size distribution showed a bimodal distribution pattern, with its highest peak observed in coarse mode for all episodes (especially for dust days with increased volume concentration). The single scattering albedo (SSA) increased with wavelength on dust days, indicating the presence of more scattering particles. Furthermore, the complex parts (real and imaginary) of refractive index showed distinct characteristics with lower imaginary values (also scattering) on dust days. The shortwave (SW; 0.2-4.0 μm) and longwave (LW; 4-100 μm) aerosol radiative forcing (ARF) values were computed from the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model both at the top of atmosphere (TOA) and the bottom of atmosphere (BOA) during dust and non-dust (dust free) days, and the corresponding heating rates and forcing efficiencies were also estimated. The SW (LW) ARF, therefore, produced significant cooling (warming) effects at both the TOA and the BOA over Beijing.

Airborne ultrafine particles in a naturally ventilated metro station: Dominant sources and mixing state determined by particle size distribution and volatility measurements.

PubMed

Mendes, Luís; Gini, Maria I; Biskos, George; Colbeck, Ian; Eleftheriadis, Konstantinos

2018-08-01

Ultrafine particle number concentrations and size distributions were measured on the platform of a metro station in Athens, Greece, and compared with those recorded at an urban background station. The volatility of the sampled particles was measured in parallel, providing further insights on the mixing state and composition of the sampled particles. Particle concentration exhibited a mean value of 1.2 × 10 4 # cm -3 and showed a weak correlation with train passage frequency, but exhibited a strong correlation with urban background particle concentrations. The size distribution appears to be strongly influenced by outdoor conditions, such as the morning traffic rush hour and new particle formation events observed at noon. The aerosol in the metro was externally mixed throughout the day, with particle populations being identified (1) as fully refractory particles being more dominant during the morning traffic rush hours, (2) as core-shell structure particles having a non-volatile core coated with volatile material, and (3) fully volatile particles. The evolution of particle volatility and size throughout the day provide additional support that most nanoparticles in the metro station originate from outdoor urban air. Copyright © 2018 Elsevier Ltd. All rights reserved.

Constraints on Global Aerosol Types: Past, Present, and Near-Future

NASA Astrophysics Data System (ADS)

Kahn, Ralph

2014-05-01

Although the recent IPCC fifth assessment report (AR5) suggests that confidence in estimated direct aerosol radiative forcing (DARF) is high, indications are that there is little agreement among current climate models about the global distribution of aerosol single-scattering albedo (SSA). SSA must be associated with specific surface albedo and aerosol optical depth (AOD) values to calculate DARF with confidence, and global-scale constraints on aerosol type, including SSA, are poor at present. Yet, some constraints on aerosol type have been demonstrated for several satellite instruments, including the NASA Earth Observing System's Multi-angle Imaging SpectroRadiometer (MISR). The time-series of approximately once-weekly, global MISR observations has grown to about 14 years. The MISR capability amounts to three-to-five bins in particle size, two-to-four bins in SSA, and spherical vs. non-spherical particle distinctions, under good retrieval conditions. As the record of coincident, suborbital validation data has increased steadily, it has become progressively more feasible to assess and to improve the operational algorithm constraints on aerosol type. This presentation will discuss planned refinements to the MISR operational algorithm, and will highlight recent efforts at using MISR results to help better represent wildfire smoke, volcanic ash, and urban pollution in climate models.

Lidar Remote Sensing for Industry and Environment Monitoring

NASA Technical Reports Server (NTRS)

Singh, Upendra N. (Editor); Itabe, Toshikazu (Editor); Sugimoto, Nobuo (Editor)

2000-01-01

Contents include the following: 1. Keynote paper: Overview of lidar technology for industrial and environmental monitoring in Japan. 2. lidar technology I: NASA's future active remote sensing mission for earth science. Geometrical detector consideration s in laser sensing application (invited paper). 3. Lidar technology II: High-power femtosecond light strings as novel atmospheric probes (invited paper). Design of a compact high-sensitivity aerosol profiling lidar. 4. Lasers for lidars: High-energy 2 microns laser for multiple lidar applications. New submount requirement of conductively cooled laser diodes for lidar applications. 5. Tropospheric aerosols and clouds I: Lidar monitoring of clouds and aerosols at the facility for atmospheric remote sensing (invited paper). Measurement of asian dust by using multiwavelength lidar. Global monitoring of clouds and aerosols using a network of micropulse lidar systems. 6. Troposphere aerosols and clouds II: Scanning lidar measurements of marine aerosol fields at a coastal site in Hawaii. 7. Tropospheric aerosols and clouds III: Formation of ice cloud from asian dust particles in the upper troposphere. Atmospheric boundary layer observation by ground-based lidar at KMITL, Thailand (13 deg N, 100 deg. E). 8. Boundary layer, urban pollution: Studies of the spatial correlation between urban aerosols and local traffic congestion using a slant angle scanning on the research vessel Mirai. 9. Middle atmosphere: Lidar-observed arctic PSC's over Svalbard (invited paper). Sodium temperature lidar measurements of the mesopause region over Syowa Station. 10. Differential absorption lidar (dIAL) and DOAS: Airborne UV DIAL measurements of ozone and aerosols (invited paper). Measurement of water vapor, surface ozone, and ethylene using differential absorption lidar. 12. Space lidar I: Lightweight lidar telescopes for space applications (invited paper). Coherent lidar development for Doppler wind measurement from the International Space Station. 13. Space lidar II: Using coherent Doppler lidar to estimate river discharge. 14. Poster session: Lidar technology, optics for lidar. Laser for lidar. Middle atmosphere observations. Tropospheric observations (aerosols, clouds). Boundary layer, urban pollution. Differential absorption lidar. Doppler lidar. and Space lidar.

Columnar aerosol optical properties at AERONET sites in northern, central and southern Mexico

NASA Astrophysics Data System (ADS)

Carabali, Giovanni; Estévez, Hector; Florean-Cruz, Claudia; Navarro-Medina, Abigail; Valdés-Barrón, Mauro; Bonifaz-Alfonzo, Roberto; Riveros-Rosas, David; Velasco-Herrera, Víctor; Vázquez-Gálvez, Felipe

2017-04-01

The column-integrated optical properties of aerosol in the north, central and southern Mexico were investigated based on Sun/sky radiometer measurements made at Aerosol Robotic Network (AERONET) sites. Characterization of aerosol properties in these Mexico regions is important due to natural and anthropogenic significant events that occurred: dust storms from Sonora desert, biomass burning from south forest areas and urban/industrial from Mexico City due to the increases in fossil fuel combustion. Some cities in northern Mexico located near desert areas are affected by the dust from Sonora and Chihuahua deserts. These particles are suspended in the atmosphere due to strong wind activity that creates dust storms. In the central part of the Mexican territory, urban air pollution is one of the biggest problems. Mexico City is the most important urban area that face seriously environmental problem generated by daily anthropogenic emissions from activities of some 21 million people and the vast amount of industry. On the other hand, biomass burning in the Yucatan Peninsula, Southern Mexico, and Guatemala is an important source of anthropogenic aerosol in the troposphere (Crutzen and Andrade, 1990). The pollution from these fires affects air quality locally and is transported over the Gulf of Mexico to the United States (Wang et al., 2006). The aim of this work is to study the optical properties of different types of aerosols by analyzing a 5-year (2005-2010) data set from AErosol RObotic NETwork (AERONET). Time series of Angstrom exponent (α) and aerosol optical depth (τ) in 7 wavelengths from 340 to 1020 nm are shown. Additionally, a graphical framework to classify aerosol properties using direct sun-photometer observations in the different regions of Mexico is presented. That aerosol classification was made by applying the method described by Gobbi et al (2007), which relies on the combined analysis of α and its spectral curvature δα.

Size-resolved particulate water-soluble organic compounds in the urban, mountain and marine atmosphere

NASA Astrophysics Data System (ADS)

Wang, G.; Kawamura, K.; Xie, M.; Hu, S.; Zhou, B.; Li, J.; Cao, J.; An, Z.

2010-07-01

Primary (i.e., sugars and sugar alcohols) and secondary water-soluble organic compounds (WSOCs) (i.e., dicarboxylic acids and aromatic acids) were characterised on a molecular level in size-segregated aerosols from the urban and mountain atmosphere of China and from the marine atmosphere in the outflow region of East Asia. Levoglucosan is the most abundant WSOCs in the urban and mountain atmosphere, whose accumulated concentrations in all stages are 1-3 orders of magnitude higher than those of marine aerosols. In contrast, malic, succinic and phthalic acids are dominant in the marine aerosols, which are 3-6 times more abundant than levoglucosan. This suggests that a continuous formation of secondary organic aerosols is occurring in the marine atmosphere during the long-range transport of air mass from inland China to the North Pacific. Sugars and sugar-alcohols, except for levoglucosan, gave a bimodal size distribution in the urban and mountain areas, peaking at 0.7-1.1 μm and >3.3 μm, and a unimodal distribution in the marine region, peaking at >3.3 μm. In contrast, levoglucosan and all the secondary WSOCs, except for benzoic and azelaic acids, showed a unimodal size distribution with a peak at 0.7-1.1 μm. Geometric mean diameters (GMDs) of the WSOCs in fine particles (<2.1 μm) at the urban site are larger in winter than in spring, due to an enhanced coagulation effect under the development of an inversion layer. However, GMDs of levoglucosan and most of the secondary WSOCs in the coarse mode are larger in the mountain and marine air and smaller in the urban air. This is most likely caused by an enhanced hygroscopic growth due to the high humidity of the mountain and marine atmosphere.

Global Monitoring of Air Pollution Using Spaceborne Sensors

NASA Technical Reports Server (NTRS)

Chu, D. A.; Kaufman, Y. J.; Tanre, D.; Remer, L. A.; Einaudi, Franco (Technical Monitor)

2000-01-01

The MODIS sensor onboard EOS-Terra satellite provides not only daily global coverage but also high spectral (36 channels from 0.41 to 14 microns wavelength) and spatial (250m, 500m and 1km) resolution measurements. A similar MODIS instrument will be also configured into EOS-Aqua satellite to be launched soon. Using the complementary EOS-Terra and EOS-Aqua sun-synchronous orbits (10:30 AM and 1:30 PM equator-crossing time respectively), it enables us also to study the diurnal changes of the Earth system. It is unprecedented for the derivation of aerosol properties with such high spatial resolution and daily global converge. Aerosol optical depth and other aerosol properties, e.g., Angstrom coefficient over land and particle size over ocean, are derived as standard products at a spatial resolution of 10 x 10 sq km. The high resolution results are found surprisingly useful in detecting aerosols in both urban and rural regions as a result of urban/industrial pollution and biomass burning. For long-lived aerosols, the ability to monitoring the evolution of these aerosol events could help us to establish an system of air quality especially for highly populated areas. Aerosol scenarios with city pollution and biomass burning will be presented. Also presented are the method used in the derivation of aerosol optical properties and preliminary results will be presented, and issue as well as obstacles in validating aerosol optical depth with AERONET ground-based observations.

Formation and Growth of New Organic Aerosol Particles over the Deepwater Horizon Oil Spill

NASA Astrophysics Data System (ADS)

Brock, C. A.; Murphy, D. M.; Bahreini, R.; Middlebrook, A. M.; De Gouw, J. A.

2011-12-01

Aerosol size distributions were measured in June 2010 downwind of the surface oil slick produced by the Deepwater Horizon oil spill in the Gulf of Mexico. Rapid condensation of partially oxidized hydrocarbons was responsible for formation of a plume of secondary organic aerosol downwind of the spill region. New particles were nucleated upwind of the freshest surface oil but downwind of oil that surfaced less than 100 hours previously. These new particles grew by condensation at rates of ~20 nm hr-1; preexisting accumulation mode particles grew by ~10 nm hr-1. The gas-phase concentration of a condensing species necessary to support the observed growth rate assuming irreversible adsorption with unit accommodation coefficient is estimated to be ~0.04-0.09 μg m-3 (~3-8 pptv). The ratio of growth rates for newly formed particles to accumulation mode particles was consistent within error limits with irreversible condensation. Because new particle formation did not occur in areas away from the <100 hr-old oil slick, these results indicate that the oxidation products of VOC species, probably C14-C16 compounds, were directly involved in the growth of the new particles. While a unique and extreme environment, the oil spill plume provides insight into similar processes that may occur in urban and industrial areas where petrochemical products are produced and consumed.

Functional characterization of the water-soluble organic carbon of size fractionated aerosol in the Southern Mississippi Valley

NASA Astrophysics Data System (ADS)

Chalbot, M.-C. G.; Brown, J.; Chitranshi, P.; Gamboa da Costa, G.; Pollock, E. D.; Kavouras, I. G.

2014-02-01

The chemical content of the water soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to: (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for the period when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5% of particle mass for particles with dp > 0.96 μm and 10% of particle mass for particles with dp < 0.96 μm. Non-exchangeable aliphatic (H-C), unsaturated aliphatic (H-C-C=), oxygenated saturated aliphatic (H-C-O), acetalic (O-CH-O) and aromatic (Ar-H) protons were determined by proton nuclear magnetic resonance. The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m-3 for particles with 0.96 < dp < 1.5 μm to 73.9 ± 12.3 nmol m-3 for particles with dp < 0.49 μm, resulting in molar H / C ratios of 0.48 ± 0.05 to 0.92 ± 0.09 observed in combustion-related organic aerosol. The R-H was the most abundant group representing about 45% of measured total non-exchangeable organic hydrogen concentration followed by H-C-O (27%) and H-C-C= (26%). Levoglucosan, amines, ammonium and methanosulfonate were tentatively identified in NMR fingerprints of fine particles. Sucrose, fructose, glucose, formate and acetate were associated with coarse particles. These qualitative differences of 1H-NMR profiles for different particle sizes indicated the possible contribution of biological aerosol and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing δ13C abundance from -26.81 ± 0.18‰ for the smallest particles to -25.93 ± 0.31‰ for the largest particles and the relative distribution of the functional groups as compared to those previously observed for marine, biomass burning and secondary organic aerosol. The latter also allowed for the differentiation of urban combustion-related aerosol and biological particles. The five types of organic hydrogen accounted for the majority of WSOC for particles with dp > 3.0 μm and dp < 0.96 μm.

Functional characterization of the water-soluble organic carbon of size-fractionated aerosol in the southern Mississippi Valley

NASA Astrophysics Data System (ADS)

Chalbot, M.-C. G.; Brown, J.; Chitranshi, P.; Gamboa da Costa, G.; Pollock, E. D.; Kavouras, I. G.

2014-06-01

The chemical content of water-soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for periods when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5% of particle mass for particles with dp > 0.96 μm and 10% of particle mass for particles with dp < 0.96 μm. Non-exchangeable aliphatic (H-C), unsaturated aliphatic (H-C-C=), oxygenated saturated aliphatic (H-C-O), acetalic (O-CH-O) and aromatic (Ar-H) protons were determined by proton nuclear magnetic resonance (1H-NMR). The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m-3 for particles with 1.5 < dp < 3.0 μm to 73.9 ± 12.3 nmol m-3 for particles with dp < 0.49 μm. The molar H / C ratios varied from 0.48 ± 0.05 to 0.92 ± 0.09, which were comparable to those observed for combustion-related organic aerosol. The R-H was the most abundant group, representing about 45% of measured total non-exchangeable organic hydrogen concentrations, followed by H-C-O (27%) and H-C-C= (26%). Levoglucosan, amines, ammonium and methanesulfonate were identified in NMR fingerprints of fine particles. Sucrose, fructose, glucose, formate and acetate were associated with coarse particles. These qualitative differences of 1H-NMR profiles for different particle sizes indicated the possible contribution of biological aerosols and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing δ13C abundance from -26.81 ± 0.18‰ for the smallest particles to -25.93 ± 0.31‰ for the largest particles and the relative distribution of the functional groups as compared to those previously observed for marine, biomass burning and secondary organic aerosol. The latter also allowed for the differentiation of urban combustion-related aerosol and biological particles. The five types of organic hydrogen accounted for the majority of WSOC for particles with dp > 3.0 μm and dp < 0.96 μm.

Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements

NASA Technical Reports Server (NTRS)

Limbacher, J.; Patadia, F.; Petrenko, M.; Martin, M. Val; Chin, M.; Gaitley, B.; Garay, M.; Kalashnikova, O.; Nelson, D.; Scollo, S.

2011-01-01

As the aerosol products from the NASA Earth Observing System's Multi-angle Imaging SpectroRadiometer (MISR) mature, we are placing greater focus on ways of using the aerosol amount and type data products, and aerosol plume heights, to constrain aerosol transport models. We have demonstrated the ability to map aerosol air-mass-types regionally, and have identified product upgrades required to apply them globally, including the need for a quality flag indicating the aerosol type information content, that varies depending upon retrieval conditions. We have shown that MISR aerosol type can distinguish smoke from dust, volcanic ash from sulfate and water particles, and can identify qualitative differences in mixtures of smoke, dust, and pollution aerosol components in urban settings. We demonstrated the use of stereo imaging to map smoke, dust, and volcanic effluent plume injection height, and the combination of MISR and MODIS aerosol optical depth maps to constrain wildfire smoke source strength. This talk will briefly highlight where we stand on these application, with emphasis on the steps we are taking toward applying the capabilities toward constraining aerosol transport models, planet-wide.

Assessing the role of anthropogenic and biogenic sources on PM1 over southern West Africa using aircraft measurements

NASA Astrophysics Data System (ADS)

Brito, Joel; Freney, Evelyn; Dominutti, Pamela; Borbon, Agnes; Haslett, Sophie L.; Batenburg, Anneke M.; Colomb, Aurelie; Dupuy, Regis; Denjean, Cyrielle; Burnet, Frederic; Bourriane, Thierry; Deroubaix, Adrien; Sellegri, Karine; Borrmann, Stephan; Coe, Hugh; Flamant, Cyrille; Knippertz, Peter; Schwarzenboeck, Alfons

2018-01-01

As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, an airborne campaign was designed to measure a large range of atmospheric constituents, focusing on the effect of anthropogenic emissions on regional climate. The presented study details results of the French ATR42 research aircraft, which aimed to characterize gas-phase, aerosol and cloud properties in the region during the field campaign carried out in June/July 2016 in combination with the German Falcon 20 and the British Twin Otter aircraft. The aircraft flight paths covered large areas of Benin, Togo, Ghana and Côte d'Ivoire, focusing on emissions from large urban conurbations such as Abidjan, Accra and Lomé, as well as remote continental areas and the Gulf of Guinea. This paper focuses on aerosol particle measurements within the boundary layer (< 2000 m), in particular their sources and chemical composition in view of the complex mix of both biogenic and anthropogenic emissions, based on measurements from a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) and ancillary instrumentation. Background concentrations (i.e. outside urban plumes) observed from the ATR42 indicate a fairly polluted region during the time of the campaign, with average concentrations of carbon monoxide of 131 ppb, ozone of 32 ppb, and aerosol particle number concentration ( > 15 nm) of 735 cm-3 stp. Regarding submicron aerosol composition (considering non-refractory species and black carbon, BC), organic aerosol (OA) is the most abundant species contributing 53 %, followed by SO4 (27 %), NH4 (11 %), BC (6 %), NO3 (2 %) and minor contribution of Cl (< 0.5 %). Average background PM1 in the region was 5.9 µg m-3 stp. During measurements of urban pollution plumes, mainly focusing on the outflow of Abidjan, Accra and Lomé, pollutants are significantly enhanced (e.g. average concentration of CO of 176 ppb, and aerosol particle number concentration of 6500 cm-3 stp), as well as PM1 concentration (11.9 µg m-3 stp). Two classes of organic aerosols were estimated based on C-ToF-AMS: particulate organic nitrates (pONs) and isoprene epoxydiols secondary organic aerosols (IEPOX-SOA). Both classes are usually associated with the formation of particulate matter through complex interactions of anthropogenic and biogenic sources. During DACCIWA, pONs have a fairly small contribution to OA (around 5 %) and are more associated with long-range transport from central Africa than local formation. Conversely, IEPOX-SOA provides a significant contribution to OA (around 24 and 28 % under background and in-plume conditions). Furthermore, the fractional contribution of IEPOX-SOA is largely unaffected by changes in the aerosol composition (particularly the SO4 concentration), which suggests that IEPOX-SOA concentration is mainly driven by pre-existing aerosol surface, instead of aerosol chemical properties. At times of large in-plume SO4 enhancements (above 5 µg m-3), the fractional contribution of IEPOX-SOA to OA increases above 50 %, suggesting only then a change in the IEPOX-SOA-controlling mechanism. It is important to note that IEPOX-SOA constitutes a lower limit to the contribution of biogenic OA, given that other processes (e.g. non-IEPOX isoprene, monoterpene SOA) are likely in the region. Given the significant contribution to aerosol concentration, it is crucial that such complex biogenic-anthropogenic interactions are taken into account in both present-day and future scenario models of this fast-changing, highly sensitive region.

Lidar remote sensing of laser-induced incandescence on light absorbing particles in the atmosphere.

PubMed

Miffre, Alain; Anselmo, Christophe; Geffroy, Sylvain; Fréjafon, Emeric; Rairoux, Patrick

2015-02-09

Carbon aerosol is now recognized as a major uncertainty on climate change and public health, and specific instruments are required to address the time and space evolution of this aerosol, which efficiently absorbs light. In this paper, we report an experiment, based on coupling lidar remote sensing with Laser-Induced-Incandescence (LII), which allows, in agreement with Planck's law, to retrieve the vertical profile of very low thermal radiation emitted by light-absorbing particles in an urban atmosphere over several hundred meters altitude. Accordingly, we set the LII-lidar formalism and equation and addressed the main features of LII-lidar in the atmosphere by numerically simulating the LII-lidar signal. We believe atmospheric LII-lidar to be a promising tool for radiative transfer, especially when combined with elastic backscattering lidar, as it may then allow a remote partitioning between strong/less light absorbing carbon aerosols.

EVALUATION OF COMPUTER-CONTROLLED SCANNING ELECTRON MICROSCOPY APPLIED TO AN AMBIENT URBAN AEROSOL SAMPLE

EPA Science Inventory

Recent interest in monitoring and speciation of particulate matter has led to increased application of scanning electron microscopy (SEM) coupled with energy-dispersive x-ray analysis (EDX) to individual particle analysis. SEM/EDX provides information on the size, shape, co...

Aerosol particle shrinkage event phenomenology in a South European suburban area during 2009-2015

NASA Astrophysics Data System (ADS)

Alonso-Blanco, E.; Gómez-Moreno, F. J.; Núñez, L.; Pujadas, M.; Cusack, M.; Artíñano, B.

2017-07-01

A high number of aerosol particle shrinkage cases (70) have been identified and analyzed from an extensive and representative database of aerosol size distributions obtained between 2009 and 2015 at an urban background site in Madrid (Spain). A descriptive classification based on the process from which the shrinkage began is proposed according which shrinkage events were divided into three groups: (1) NPF + shrinkage (NPF + S) events, (2) aerosol particle growth process + shrinkage (G + S) events, and (3) pure shrinkage (S) events. The largest number of shrinkages corresponded to the S-type followed by NPF + S, while the G + S events were the least frequent group recorded. Duration of shrinkages varied widely from 0.75 to 8.5 h and SR from -1.0 to -11.1 nm h-1. These processes typically occurred in the afternoon, around 18:00 UTC, caused by two situations: i) a wind speed increase usually associated with a change in the wind direction (over 60% of the observations) and ii) the reduction of photochemical activity at the end of the day. All shrinkages were detected during the warm period, mainly between May and August, when local meteorological conditions (high solar irradiance and temperature and low relative humidity), atmospheric processes (high photochemical activity) and availability of aerosol-forming precursors were favorable for their development. As a consequence of these processes, the particles concentration corresponding to the Aitken mode decreased into the nucleation mode. The accumulation mode did not undergo significant changes during these processes. In some cases, a dilution of the particulate content in the ambient air was observed. This work, goes further than others works dealing with aerosol particles shrinkages, as it incorporates as a main novelty a classification methodology for studying these processes. Moreover, compared to other studies, it is supported by a high and representative number of observations. Thus, this study contributes to get a better understanding of this type of atmospheric aerosol transformations and its features.

Aerosol optical extinction during the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ) 2014 summertime field campaign, Colorado, USA

NASA Astrophysics Data System (ADS)

Dingle, Justin H.; Vu, Kennedy; Bahreini, Roya; Apel, Eric C.; Campos, Teresa L.; Flocke, Frank; Fried, Alan; Herndon, Scott; Hills, Alan J.; Hornbrook, Rebecca S.; Huey, Greg; Kaser, Lisa; Montzka, Denise D.; Nowak, John B.; Reeves, Mike; Richter, Dirk; Roscioli, Joseph R.; Shertz, Stephen; Stell, Meghan; Tanner, David; Tyndall, Geoff; Walega, James; Weibring, Petter; Weinheimer, Andrew

2016-09-01

Summertime aerosol optical extinction (βext) was measured in the Colorado Front Range and Denver metropolitan area as part of the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ) campaign during July-August 2014. An Aerodyne cavity attenuated phase shift particle light extinction monitor (CAPS-PMex) was deployed to measure βext (at average relative humidity of 20 ± 7 %) of submicron aerosols at λ = 632 nm at 1 Hz. Data from a suite of gas-phase instrumentation were used to interpret βext behavior in various categories of air masses and sources. Extinction enhancement ratios relative to CO (Δβext / ΔCO) were higher in aged urban air masses compared to fresh air masses by ˜ 50 %. The resulting increase in Δβext / ΔCO for highly aged air masses was accompanied by formation of secondary organic aerosols (SOAs). In addition, the impacts of aerosol composition on βext in air masses under the influence of urban, natural oil and gas operations (O&G), and agriculture and livestock operations were evaluated. Estimated non-refractory mass extinction efficiency (MEE) values for different air mass types ranged from 1.51 to 2.27 m2 g-1, with the minimum and maximum values observed in urban and agriculture-influenced air masses, respectively. The mass distribution for organic, nitrate, and sulfate aerosols presented distinct profiles in different air mass types. During 11-12 August, regional influence of a biomass burning event was observed, increasing the background βext and estimated MEE values in the Front Range.

Increases in wintertime PM2.5 sodium and chloride linked to snowfall and road salt application

NASA Astrophysics Data System (ADS)

Kolesar, Katheryn R.; Mattson, Claire N.; Peterson, Peter K.; May, Nathaniel W.; Prendergast, Rashad K.; Pratt, Kerri A.

2018-03-01

The application of salts and salty brines to roads is common practice during the winter in many urban environments. Road salts can become aerosolized, thereby injecting sodium and chloride particulate matter (PM) into the atmosphere. Here, data from the United States Environmental Protection Agency Chemical Speciation Monitoring Network were used to assess temporal trends of sodium and chloride PM2.5 (PM < 2.5 μm) at 25 locations across the United States to investigate the ubiquity of road salt aerosols. Sodium and chloride PM2.5 concentrations were an average of three times higher in the winter, as compared to the summer, for locations with greater than 25 cm of average annual snowfall. Winter urban chloride PM2.5 concentrations attributed to road salt can even sometimes rival those of coastal sea spray aerosol-influenced sites. In most snow-influenced cities, chloride and sodium PM2.5 concentrations were positively correlated with snowfall; however, this relationship is complicated by differences in state and local winter maintenance practices. This study highlights the ubiquity of road salt aerosols in the United States and their potential impact on wintertime urban air quality, particularly due to the potential for multiphase reactions to liberate chlorine from the particle-phase. Since road salt application is a common practice in wintertime urban environments across the world, it is imperative that road salt application emissions, currently not included in inventories, and its impacts be investigated through measurements and modeling.

Size distributions of hydrophilic and hydrophobic fractions of water-soluble organic carbon in an urban atmosphere in Hong Kong

NASA Astrophysics Data System (ADS)

Wang, Nijing; Yu, Jian Zhen

2017-10-01

Water-soluble organic carbon (WSOC) is a significant part of ambient aerosol and plays an active role in contributing to aerosol's effect on visibility degradation and radiation budget through its interactions with atmospheric water. Size-segregated aerosol samples in the range of 0.056-18 μm were collected using a ten-stage impactor sampler at an urban site in Hong Kong over one-year period. The WSOC samples were separated into hydrophilic (termed WSOC_h) and hydrophobic fractions (i.e., the humic-like substances (HULIS) fraction) through solid-phase extraction procedure. Carbon in HULIS accounted for 40 ± 14% of WSOC. The size distribution of HULIS was consistently characterized in all seasons with a dominant droplet mode (46-71%) and minor condensation (9.0-18%) and coarse modes (20-35%). The droplet mode had a mass median aerodynamic diameter in the range of 0.7-0.8 μm. This size mode showed the largest seasonal variation in abundance, lowest in the summer (0.41 μg/m3) and highest in the winter (3.3 μg/m3). WSOC_h also had a dominant droplet mode, but was more evenly distributed among different size modes. Inter-species correlations within the same size mode suggest that the condensation-mode HULIS was partly associated with combustion sources and the droplet-mode was strongly associated with secondary sulfate formation and biomass burning particle aging processes. There is evidence to suggest that the coarse-mode HULIS largely originated from coagulation of condensation-mode HULIS with coarse soil/sea salt particles. The formation process and possible sources of WSOC_h was more complicated and multiple than HULIS and need further investigation. Our measurements indicate that WSOC components contributed a dominant fraction of water-soluble aerosol mass in particles smaller than 0.32 μm while roughly 20-30% in the larger particles.

Chemical composition, source, and process of urban aerosols during winter haze formation in Northeast China.

PubMed

Zhang, Jian; Liu, Lei; Wang, Yuanyuan; Ren, Yong; Wang, Xin; Shi, Zongbo; Zhang, Daizhou; Che, Huizheng; Zhao, Hujia; Liu, Yanfei; Niu, Hongya; Chen, Jianmin; Zhang, Xiaoye; Lingaswamy, A P; Wang, Zifa; Li, Weijun

2017-12-01

The characteristics of aerosol particles have been poorly evaluated even though haze episodes frequently occur in winter in Northeast China. OC/EC analysis, ion chromatography, and transmission electron microscopy (TEM) were used to investigate the organic carbon (OC) and elemental carbon (EC), and soluble ions in PM 2.5 and the mixing state of individual particles during a severe wintertime haze episode in Northeast China. The organic matter (OM), NH 4 + , SO 4 2- , and NO 3 - concentrations in PM 2.5 were 89.5 μg/m 3 , 24.2 μg/m 3 , 28.1 μg/m 3 , and 32.8 μg/m 3 on the haze days, respectively. TEM observations further showed that over 80% of the haze particles contained primary organic aerosols (POAs). Based on a comparison of the data obtained during the haze formation, we generate the following synthetic model of the process: (1) Stable synoptic meteorological conditions drove the haze formation. (2) The early stage of haze formation (light or moderate haze) was mainly caused by the enrichment of POAs from coal burning for household heating and cooking. (3) High levels of secondary organic aerosols (SOAs), sulfates, and nitrates formation via heterogeneous reactions together with POAs accumulation promoted to the evolution from light or moderate to severe haze. Compared to the severe haze episodes over the North China Plain, the PM 2.5 in Northeast China analyzed in the present study contained similar sulfate, higher SOA, and lower nitrate contents. Our results suggest that most of the POAs and secondary particles were likely related to emissions from coal-burning residential stoves in rural outskirts and small boilers in urban areas. The inefficient burning of coal for household heating and cooking should be monitored during wintertime in Northeast China. Copyright © 2017 Elsevier Ltd. All rights reserved.

The fluorescence properties of aerosol larger than 0.8 μm in urban and tropical rainforest locations

NASA Astrophysics Data System (ADS)

Gabey, A. M.; Stanley, W. R.; Gallagher, M. W.; Kaye, P. H.

2011-06-01

UV-LIF measurements were performed on ambient aerosol in Manchester, UK (urban city centre, winter) and Borneo, Malaysia (remote, tropical) using a Wide Issue Bioaerosol Spectrometer, version 3 (WIBS3). These sites are taken to represent environments with minor and significant primary biological aerosol (PBA) influences respectively, and the urban dataset describes the fluorescent background aerosol against which PBA must be identified by researchers using LIF. The ensemble aerosol at both sites was characterised over 2-3 weeks by measuring the fluorescence intensity and optical equivalent diameter (DP) of single particles sized 0.8 ≤ DP ≤ 20 μm. Filter samples were also collected for a subset of the Manchester campaign and analysed using energy dispersive X-Ray (EDX) spectroscopy and environmental scanning electron microscopy (ESEM), which revealed mostly non-PBA at D ≤ 1 μm. The WIBS3 features three fluorescence channels: the emission following a 280 nm excitation is recorded at 310-400 nm (channel F1) and 400-600 nm (F2), and fluorescence excited at 350 nm is detected at 400-600 nm (F3). In Manchester the primary size mode of fluorescent and non-fluorescent material was present at 0.8-1.2 μm, with a secondary fluorescent mode at 2-4 μm. In Borneo non-fluorescent material peaked at 0.8-1.2 μm and fluorescent at 3-4 μm. Agreement between fluorescent number concentrations in each channel differed at the two sites, with F1 and F3 reporting similar concentrations in Borneo but F3 outnumbering F1 by a factor of 2-3 across the size spectrum in Manchester. The fluorescence intensity in each channel generally rose with DP at both sites with the exception of F1 intensity in Manchester, which peaked at DP = 4 μm, causing a divergence between F1 and F3 intensity at larger DP. This divergence and the differing fluorescent particle concentrations demonstrate the additional discrimination provided by the F1 channel in Manchester. The relationships between fluorescence intensities in different pairs of channels were also investigated as a function of DP. Differences between these metrics were apparent at each site and provide some distinction between the two datasets. Finally, particle selection criteria based on the Borneo dataset were applied to identify a median concentration of 10 "Borneo-like" fluorescent particles per litre in Manchester.

Source Apportionment of Atmospheric Particles by Electron Probe X-Ray Microanalysis and Receptor Models.

NASA Astrophysics Data System (ADS)

van Borm, Werner August

Electron probe X-ray microanalysis (EPXMA) in combination with an automation system and an energy-dispersive X-ray detection system was used to analyse thousands of microscopical particles, originating from the ambient atmosphere. The huge amount of data was processed by a newly developed X-ray correction method and a number of data reduction procedures. A standardless ZAF procedure for EPXMA was developed for quick semi-quantitative analysis of particles starting from simple corrections, valid for bulk samples and modified taking into account the particle finit diameter, assuming a spherical shape. Tested on a limited database of bulk and particulate samples, the compromise between calculation speed and accuracy yielded for elements with Z > 14 accuracies on concentrations less than 10% while absolute deviations remained below 4 weight%, thus being only important for low concentrations. Next, the possibilities for the use of supervised and unsupervised multivariate particle classification were investigated for source apportionment of individual particles. In a detailed study of the unsupervised cluster analysis technique several aspects were considered, that have a severe influence on the final cluster analysis results, i.e. data acquisition, X-ray peak identification, data normalization, scaling, variable selection, similarity measure, cluster strategy, cluster significance and error propagation. A supervised approach was developed using an expert system-like approach in which identification rules are builded to describe the particle classes in a unique manner. Applications are presented for particles sampled (1) near a zinc smelter (Vieille-Montagne, Balen, Belgium), analyzed for heavy metals, (2) in an urban aerosol (Antwerp, Belgium), analyzed for over 20 elements and (3) in a rural aerosol originating from a swiss mountain area (Bern). Thus is was possible to pinpoint a number of known and unknown sources and characterize their emissions in terms of particles abundance and particle composition. Alternatively, the bulk analysis of filters (total, fine and coarse mode) using Particle Induced X -Ray Emission (PIXE) and the application of a receptor modeling approach provided for complementary information on a macroscopical level. A computer program was developed incorporating an absolute factor analysis based receptor modeling procedure. Source profiles and contributions are described by elemental concentrations and an atmospheric mass balance is put forward. The latter method was applied in a two year study of the Antwerp urban aerosol and for the swiss aerosol, revealing a number of previously known and unknown sources. Both methods were successfully combined to increase the source resolution.

Aerosol mixingstate, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lance, Sara; Raatikainen, T.; Onasch, Timothy B.

2013-05-15

Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. K¨ohler theory is used to evaluate the characteristic water uptake coefficient, k*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions, (forg), are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which kAMS is inferred and compared against k*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated withmore » an increased k* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% +/- 0.06%. We also find that at 0600-0800 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as “internally-mixed”. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning “rush hour”, and the entire campaign. We show that k* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for k* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the AMS. Measured k* typically ranges from 0.2 to 0.35, and organics typically make up 60-85% of the aerosol mass in the size range studied. Despite some disagreement between kAMS and kCCNc, we show that kAMS is able to describe CCN concentrations reasonably well, especially at the highest CCN concentrations. This is consistent with other CCN studies carried out in urban environments, and is partly due to the fact that the highest CCN concentrations occur during the daytime when the aerosol is internally-mixed and the organic fraction is relatively low. During the early morning rush hour, however, failing to account for the aerosol mixing state results in systematic overestimation of CCN concentrations by 50-100%.« less

Characteristics of Aerosol Transport from Asia to the West Coast of North America

NASA Astrophysics Data System (ADS)

Brock, C. A.; Bahreini, R.; Middlebrook, A. M.; Atlas, E. L.; Blake, D. R.; Brioude, J.; Cooper, O. R.; de Gouw, J. A.; Holloway, J. S.; Lack, D. A.; Langridge, J. M.; Meinardi, S.; Nowak, J. B.; Peischl, J.; Perring, A.; Pollack, I. B.; Roberts, J. M.; Ryerson, T. B.; Schwarz, J. P.; Spackman, J. R.; Trainer, M.; Trytko, J.; Warneke, C.

2010-12-01

During the CalNex field program of May and June 2010, the NOAA WP-3D aircraft observed several layers of enhanced trace gas mixing ratios and aerosol concentrations at altitudes ranging from 1 to 4 km over southern and central California. The submicron aerosol composition within these layers was dominated by partially neutralized sulfate, while nitrate, organic matter and black carbon were only minor constituents. The particle layers were associated with trace gases, such as benzene and sulfur dioxide, consistent with anthropogenic fossil fuel emissions, and were not associated with enhancements of the biomass burning tracer acetonitrile. The particle size distribution was dominated by a single accumulation mode that is characteristic of a well aged aerosol. Transport modeling indicates an Asian source for these layers of pollution. Dew point temperatures within the layers were less than -15 degrees Celsius, indicating desiccation by precipitation during transport. Taken together, these observations are consistent with those from earlier studies in which was diagnosed the removal of primary and organic particles by precipitation scavenging during uplift from the polluted Asian boundary layer into the free troposphere. Oxidation of residual sulfur dioxide that remained following transport through the cloud system may have resulted in the observed sulfate-rich aerosol. The repeated observation of such layers suggests that wet scavenging frequently modifies the chemical and optical characteristics of aerosols emitted in urban regions in Asia and transported in the free troposphere across the Pacific.

Atmospheric aerosols parameters behavior and its association with meteorological activities variables over western Indian tropical semi-urban site i.e., Udaipur

NASA Astrophysics Data System (ADS)

Vyas, B. M.; Saxenna, Abhishek; Panwar, Chhagan

2016-05-01

The present study has been focused to the identify the role of meteorological processes on changing the monthly variation of AOD at 550nm, Angstrom Exponent Coefficient (AEC, 440/670nm) and Cloud Effective Radius (CER, μm) measured during January, 2005 to December 2013 over western Indian location i.e., Udaipur (24.6° N, 73.7° E, 560 m amsl). The monthly variation of AOD 550nm, AEC and during entire study period have shown the strong combined influence of different local surface meteorological parameters in varying amplitude with different nature. The higher values of wind speed, ambient surface temperature, planetary boundary layer, and favorable wind direction coming from desert and oceanic region (W and SW) may be recognize as some of possible factor to exhibit the higher aerosols loading of bigger aerosol size particles in pre-monsoon. These meteorological factors seem also to be plausible responsible factors for drastically reducing the cloud effective radius in pre-monsoon season. In contrary to this, in winter, lower atmospheric aerosols burden and more abundance of fine size particles along with increasing the CER sizes also seem to be influenced and governed by the adverse nature of meteorological conditions such lowering the PBL, T, WS as well as with air pollutants transportation by wind from the N and NE region, of high aerosols loading of fine size particles as anthropogenic aerosols located far away to the observing site.

Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing

NASA Astrophysics Data System (ADS)

Ren, Jingye; Zhang, Fang; Wang, Yuying; Collins, Don; Fan, Xinxin; Jin, Xiaoai; Xu, Weiqi; Sun, Yele; Cribb, Maureen; Li, Zhanqing

2018-05-01

Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (NCCN). In this study, we predict NCCN under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external-internal size-resolved, abbreviated as EI-SR scheme). The resulting ratios of predicted-to-measured NCCN (RCCN_p/m) were 0.90 - 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT-BK scheme) shows good closure with RCCN_p/m of 1.0 -1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT-SR scheme) achieves better closure than the INT-BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI-SR and INT-SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. NCCN is significantly underestimated (with RCCN_p/m of 0.66 - 0.75) when using the schemes of external mixtures with bulk (EXT-BK scheme) or size-resolved composition (EXT-SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the κorg exceeds 0.1.

Global aerosol typing from a combination of A-Train satellite observations in clear-sky and above clouds

NASA Astrophysics Data System (ADS)

Kacenelenbogen, M. S.; Russell, P. B.; Vaughan, M.; Redemann, J.; Shinozuka, Y.; Livingston, J. M.; Zhang, Q.

2014-12-01

According to the 5th Assessment Report of the Intergovernmental Panel on Climate Change (IPCC), the model estimates of Radiative Forcing due to aerosol-radiation interactions (RFari) for individual aerosol types are less certain than the total RFari [Boucher et al., 2013]. For example, the RFari specific to Black Carbon (BC) is uncertain due to an underestimation of its mass concentration near source regions [Koch et al., 2009]. Several recent studies have evaluated chemical transport model (CTM) predictions using observations of aerosol optical properties such as Aerosol Optical Depth (AOD) or Single Scattering Albedo (SSA) from satellite or ground-based instruments (e.g., Huneeus et al., [2010]). However, most passive remote sensing instruments fail to provide a comprehensive assessment of the particle type without further analysis and combination of measurements. To improve the predictions of aerosol composition in CTMs, we have developed an aerosol classification algorithm (called Specified Clustering and Mahalanobis Classification, SCMC) that assigns an aerosol type to multi-parameter retrievals by spaceborne, airborne or ground based passive remote sensing instruments [Russell et al., 2014]. The aerosol types identified by our scheme are pure dust, polluted dust, urban-industrial/developed economy, urban-industrial/developing economy, dark biomass smoke, light biomass smoke and pure marine. First, we apply the SCMC method to five years of clear-sky space-borne POLDER observations over Greece. We then use the aerosol extinction and SSA spectra retrieved from a combination of MODIS, OMI and CALIOP clear-sky observations to infer the aerosol type over the globe in 2007. Finally, we will extend the spaceborne aerosol classification from clear-sky to above low opaque water clouds using a combination of CALIOP AOD and backscatter observations and OMI absorption AOD values from near-by clear-sky pixels.

Cloud condensation nuclei activity and hygroscopicity of fresh and aged cooking organic aerosol

NASA Astrophysics Data System (ADS)

Li, Yanwei; Tasoglou, Antonios; Liangou, Aikaterini; Cain, Kerrigan P.; Jahn, Leif; Gu, Peishi; Kostenidou, Evangelia; Pandis, Spyros N.

2018-03-01

Cooking organic aerosol (COA) is potentially a significant fraction of organic particulate matter in urban areas. COA chemical aging experiments, using aerosol produced by grilling hamburgers, took place in a smog chamber in the presence of UV light or excess ozone. The water solubility distributions, cloud condensation nuclei (CCN) activity, and corresponding hygroscopicity of fresh and aged COA were measured. The average mobility equivalent activation diameter of the fresh particles at 0.4% supersaturation ranged from 87 to 126 nm and decreased for aged particles, ranging from 65 to 88 nm. Most of the fresh COA had water solubility less than 0.1 g L-1, even though the corresponding particles were quite CCN active. After aging, the COA fraction with water solubility greater than 0.1 g L-1 increased more than 2 times. Using the extended Köhler theory for multiple partially soluble components in order to predict the measured activation diameters, the COA solubility distribution alone could not explain the CCN activity. Surface tensions less than 30 dyn cm-1 were required to explain the measured activation diameters. In addition, COA particles appear to not be spherical, which can introduce uncertainties into the corresponding calculations.

Where There’s Smoke, There’s Science

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aiken, Allison; Dubey, Manvendra

Cloaking urban areas and wildfire zones, tiny smoke particles suspended in the atmosphere have a sizeable effect on our climate. But the exact effect of many of these aerosols-such as how much sunlight they absorb, thus warming Earth, or reflecting back to space and so cooling Earth-is very uncertain.

Time resolved aerosol monitoring in the urban centre of Soweto

NASA Astrophysics Data System (ADS)

Formenti, P.; Annegarn, H. J.; Piketh, S. J.

1998-03-01

A programme of aerosol sampling was conducted from 1982 to 1984 in the urban area of Soweto, Johannesburg, South Africa. The particulate matter (aerodynamic diameter <15 μm) was collected using a two hours time resolution single stage streaker sampler and elemental concentrations were resolved via Particle Induced X-ray Emission (PIXE) analysis. Samples have been selected for analysis from an aerosol sample archive to establish base-line atmospheric conditions that existed in Soweto prior to large scale electrification, and to establish source apportionment of crustal elements between coal smoke and traffic induced road dust, based on chemical elemental measurements. A novel technique is demonstrated for processing PIXE-derived time sequence elemental concentration vectors. Slowly varying background components have been extracted from sulphur and crustal aerosol components, using alternatively two digital filters: a moving minimum, and a moving average. The residuals of the crustal elements, assigned to locally generated aerosol components, were modelled using surrogate tracers: sulphur as a surrogate for coal smoke; and Pb as a surrogate for traffic activity. Results from this source apportionment revealed coal emissions contributed between 40% and 50% of the aerosol mineral matter, while 18-22% originated from road dust. Background aerosol, characteristic of the regional winter aerosol burden over the South African Highveld, was between 12% and 21%. Minor contributors identified included a manganese smelter, located 30 km from the sampling site, and informal trash burning, as the source of intermittent heavy metals (Cu, Zn). Elemental source profiles derived for these various sources are presented.

Size-resolved aerosol chemical analysis of extreme haze pollution events during early 2013 in urban Beijing, China.

PubMed

Tian, Shili; Pan, Yuepeng; Liu, Zirui; Wen, Tianxue; Wang, Yuesi

2014-08-30

Using size-resolved filter sampling and chemical characterization, high concentrations of water-soluble ions, carbonaceous species and heavy metals were found in both fine (PM2.1) and coarse (PM2.1-9) particles in Beijing during haze events in early 2013. Even on clear days, average mass concentration of submicron particles (PM1.1) was several times higher than that previously measured in most of abroad urban areas. A high concentration of particulate matter on haze days weakens the incident solar radiation, which reduces the generation rate of secondary organic carbon in PM1.1. We show that the peak mass concentration of particles shifted from 0.43-0.65μm on clear days to 0.65-1.1μm on lightly polluted days and to 1.1-2.1μm on heavily polluted days. The peak shifts were also found for the following species: organic carbon, elemental carbon, NH4(+), SO4(2-), NO3(-), K, Cu, Zn, Cd and Pb. Our findings demonstrate that secondary inorganic aerosols (36%) and organic matter (26%) dominated the fine particle mass on heavily polluted days, while their contribution reduced to 29% and 18%, respectively, on clear days. Besides fine particles, anthropogenic chemical species also substantially accumulated in the coarse mode, which suggests that particles with aerodynamic diameter larger than 2.1μm cannot be neglected during severe haze events. Copyright © 2014 Elsevier B.V. All rights reserved.

Source apportionment of PM2.5 light extinction in an urban atmosphere in China.

PubMed

Lan, Zijuan; Zhang, Bin; Huang, Xiaofeng; Zhu, Qiao; Yuan, Jinfeng; Zeng, Liwu; Hu, Min; He, Lingyan

2018-01-01

Haze in China is primarily caused by high pollution of atmospheric fine particulates (PM 2.5 ). However, the detailed source structures of PM 2.5 light extinction have not been well established, especially for the roles of various organic aerosols, which makes haze management lack specified targets. This study obtained the mass concentrations of the chemical compositions and the light extinction coefficients of fine particles in the winter in Dongguan, Guangdong Province, using high time resolution aerosol observation instruments. We combined the positive matrix factor (PMF) analysis model of organic aerosols and the multiple linear regression method to establish a quantitative relationship model between the main chemical components, in particular the different sources of organic aerosols and the extinction coefficients of fine particles with a high goodness of fit (R 2 =0.953). The results show that the contribution rates of ammonium sulphate, ammonium nitrate, biomass burning organic aerosol (BBOA), secondary organic aerosol (SOA) and black carbon (BC) were 48.1%, 20.7%, 15.0%, 10.6%, and 5.6%, respectively. It can be seen that the contribution of the secondary aerosols is much higher than that of the primary aerosols (79.4% versus 20.6%) and are a major factor in the visibility decline. BBOA is found to have a high visibility destroying potential, with a high mass extinction coefficient, and was the largest contributor during some high pollution periods. A more detailed analysis indicates that the contribution of the enhanced absorption caused by BC mixing state was approximately 37.7% of the total particle absorption and should not be neglected. Copyright © 2017. Published by Elsevier B.V.

Field characterization of the PM2.5 Aerosol Chemical Speciation Monitor: insights into the composition, sources, and processes of fine particles in eastern China

NASA Astrophysics Data System (ADS)

Zhang, Yunjiang; Tang, Lili; Croteau, Philip L.; Favez, Olivier; Sun, Yele; Canagaratna, Manjula R.; Wang, Zhuang; Couvidat, Florian; Albinet, Alexandre; Zhang, Hongliang; Sciare, Jean; Prévôt, André S. H.; Jayne, John T.; Worsnop, Douglas R.

2017-12-01

A PM2.5-capable aerosol chemical speciation monitor (Q-ACSM) was deployed in urban Nanjing, China, for the first time to measure in situ non-refractory fine particle (NR-PM2.5) composition from 20 October to 19 November 2015, along with parallel measurements of submicron aerosol (PM1) species by a standard Q-ACSM. Our results show that the NR-PM2.5 species (organics, sulfate, nitrate, and ammonium) measured by the PM2.5-Q-ACSM are highly correlated (r2 > 0.9) with those measured by a Sunset Lab OC  /  EC analyzer and a Monitor for AeRosols and GAses (MARGA). The comparisons between the two Q-ACSMs illustrated similar temporal variations in all NR species between PM1 and PM2.5, yet substantial mass fractions of aerosol species were observed in the size range of 1-2.5 µm. On average, NR-PM1-2.5 contributed 53 % of the total NR-PM2.5, with sulfate and secondary organic aerosols (SOAs) being the two largest contributors (26 and 27 %, respectively). Positive matrix factorization of organic aerosol showed similar temporal variations in both primary and secondary OAs between PM1 and PM2.5, although the mass spectra were slightly different due to more thermal decomposition on the capture vaporizer of the PM2.5-Q-ACSM. We observed an enhancement of SOA under high relative humidity conditions, which is associated with simultaneous increases in aerosol pH, gas-phase species (NO2, SO2, and NH3) concentrations and aerosol water content driven by secondary inorganic aerosols. These results likely indicate an enhanced reactive uptake of SOA precursors upon aqueous particles. Therefore, reducing anthropogenic NOx, SO2, and NH3 emissions might not only reduce secondary inorganic aerosols but also the SOA burden during haze episodes in China.

Effects of mineral dust on global atmospheric nitrate concentrations

NASA Astrophysics Data System (ADS)

Karydis, V. A.; Tsimpidi, A. P.; Pozzer, A.; Astitha, M.; Lelieveld, J.

2016-02-01

This study assesses the chemical composition and global aerosol load of the major inorganic aerosol components, focusing on mineral dust and aerosol nitrate. The mineral dust aerosol components (i.e., Ca2+, Mg2+, K+, Na+) and their emissions are included in the ECHAM5/MESSy Atmospheric Chemistry model (EMAC). Gas/aerosol partitioning is simulated using the ISORROPIA-II thermodynamic equilibrium model that considers K+, Ca2+, Mg2+, NH4+, Na+, SO42-, NO3-, Cl-, and H2O aerosol components. Emissions of mineral dust are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide. Presence of metallic ions can substantially affect the nitrate partitioning into the aerosol phase due to thermodynamic interactions. The model simulates highest fine aerosol nitrate concentration over urban and industrialized areas (1-3 µg m-3), while coarse aerosol nitrate is highest close to deserts (1-4 µg m-3). The influence of mineral dust on nitrate formation extends across southern Europe, western USA, and northeastern China. The tropospheric burden of aerosol nitrate increases by 44 % when considering interactions of nitrate with mineral dust. The calculated global average nitrate aerosol concentration near the surface increases by 36 %, while the coarse- and fine-mode concentrations of nitrate increase by 53 and 21 %, respectively. Other inorganic aerosol components are affected by reactive dust components as well (e.g., the tropospheric burden of chloride increases by 9 %, ammonium decreases by 41 %, and sulfate increases by 7 %). Sensitivity tests show that nitrate aerosol is most sensitive to the chemical composition of the emitted mineral dust, followed by the soil size distribution of dust particles, the magnitude of the mineral dust emissions, and the aerosol state assumption.

Particle growth in an isoprene-rich forest: Influences of urban, wildfire, and biogenic air masses

NASA Astrophysics Data System (ADS)

Gunsch, Matthew J.; Schmidt, Stephanie A.; Gardner, Daniel J.; Bondy, Amy L.; May, Nathaniel W.; Bertman, Steven B.; Pratt, Kerri A.; Ault, Andrew P.

2018-04-01

Growth of freshly nucleated particles is an important source of cloud condensation nuclei (CCN) and has been studied within a variety of environments around the world. However, there remains uncertainty regarding the sources of the precursor gases leading to particle growth, particularly in isoprene-rich forests. In this study, particle growth events were observed from the 14 total events (31% of days) during summer measurements (June 24 - August 2, 2014) at the Program for Research on Oxidants PHotochemistry, Emissions, and Transport (PROPHET) tower within the forested University of Michigan Biological Station located in northern Michigan. Growth events were observed within long-range transported air masses from urban areas, air masses impacted by wildfires, as well as stagnant, forested/regional air masses. Growth events observed during urban-influenced air masses were prevalent, with presumably high oxidant levels, and began midday during periods of high solar radiation. This suggests that increased oxidation of biogenic volatile organic compounds (BVOCs) likely contributed to the highest observed particle growth in this study (8 ± 2 nm h-1). Growth events during wildfire-influenced air masses were observed primarily at night and had slower growth rates (3 ± 1 nm h-1). These events were likely influenced by increased SO2, O3, and NO2 transported within the smoke plumes, suggesting a role of NO3 oxidation in the production of semi-volatile compounds. Forested/regional air mass growth events likely occurred due to the oxidation of regionally emitted BVOCs, including isoprene, monoterpenes, and sesquiterpenes, which facilitated multiday growth events also with slower rates (3 ± 2 nm h-1). Intense sulfur, carbon, and oxygen signals in individual particles down to 20 nm, analyzed by transmission electron microscopy with energy dispersive X-ray spectroscopy (TEM-EDX), suggest that H2SO4 and secondary organic aerosol contributed to particle growth. Overall, aerosol growth was frequently observed in a range of air masses (urban, wildfire, forested) and oxidant conditions (day vs. night), with rates ranging from 0.8 to 10.2 nm h-1.

The Impact of Aerosol Sources and Aging on CCN Formation in the Houston-Galveston-Gulf of Mexico Region

NASA Astrophysics Data System (ADS)

Quinn, P.; Bates, T.; Coffman, D.; Covert, D.

2007-12-01

The impact of anthropogenic aerosol on cloud properties, cloud lifetime, and precipitation processes is one of the largest uncertainties in our current understanding of climate change. Aerosols affect cloud properties by serving as cloud condensation nuclei (CCN) thereby leading to the formation of cloud droplets. The process of cloud drop activation is a function of both the size and chemistry of the aerosol particles which, in turn, depend on the source of the aerosol and transformations that occur downwind. In situ field measurements that can lead to an improved understanding of the process of cloud drop formation and simplifying parameterizations for improving the accuracy of climate models are highly desirable. During the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources, aging, chemistry, and size in the activation of particles to form cloud droplets. Here, we use the correlation between variability in critical diameter for activation (determined empirically from measured CCN concentrations and the number size distribution) and aerosol composition to quantify the impact of composition on particle activation. Variability in aerosol composition is parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA) for particle diameters less than 200 nm (vacuum aerodynamic). The HOA mass fraction in this size range is lowest for marine aerosol and higher for aerosol impacted by anthropogenic emissions. Combining all data collected at 0.44 percent supersaturation (SS) reveals that composition (defined in this way) explains 40 percent of the variance in the critical diameter. As expected, the dependence of activation on composition is strongest at lower SS. At the same time, correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during GoMACCS, composition plays a dominant role in determining the fraction of particles that are activated to form cloud droplets. Using Kohler theory, we estimate the error that results in calculated CCN concentrations if the organic fraction of the aerosol is neglected (i.e., a fully soluble composition of ammonium sulfate is assumed) for the range of organic mass fractions and mean diameters observed during GoMACCS. We then relate this error to the source and age of the aerosol. At 0.22 and 0.44 percent SS, the error is considerable for anthropogenic aerosol sampled near the source region as this aerosol has, on average, a high POM mass fraction and smaller particle mean diameter. The error is lower for more aged aerosol as it has a lower POM mass fraction and larger mean particle diameter. Hence, the percent error in calculated CCN concentration is expected to be larger for younger, organic- rich aerosol and smaller for aged, sulfate rich aerosol and for marine aerosol. We extend this analysis to continental and marine data sets recently reported by Dusek et al. [Science, 312, 1375, 2006] and Hudson [Geophys. Res., Lett., 34, L08801, 2007].

[Seasonal Variation Characteristics and Potential Source Contribution of Sulfate, Nitrate and Ammonium in Beijing by Using Single Particle Aerosol Mass Spectrometry].

PubMed

Liu, Lang; Zhang, Wen-jie; Du, Shi-yong; Hou, Lu-jian; Han, Bin; Yang, Wen; Chen, Min-dong; Bai, Zhi-peng

2016-05-15

Single particle aerosol mass spectrometry (SPAMS) was deployed to continuously observe the aerosol particles of Beijing urban area from 2013-12 to 2014-11, and the hourly average data of sulfate, nitrate and ammonium (SNA) were obtained using the characteristic ion tracer method. The mixing state and size distribution of SNA were analyzed. In addition, based on Hysplit 48 h back air mass trajectory results in combination with Concentration Weighted Trajectory method (CWT), we obtained the seasonal potential source contribution area of SNA. The results showed that the mixture of sulfate, nitrate and ammonium in spring and summer was more stable than that in autumn and winter. The size distribution of sulfate and nitrate was very similar. The size distribution characteristics of SNA followed the order of autumn > summer > spring > winter. The potential source region of SNA had similar spatial distribution characteristics, and the potential source region of SNA was mainly located in Beijing and south areas, especially at Tianjin, Langfang, Hengshui, Baoding and Shijiazhuang.

The Carbon Aerosol / Particles Nucleation with a Lidar: Numerical Simulations and Field Studies

NASA Astrophysics Data System (ADS)

Miffre, Alain; Anselmo, Christophe; Francis, Mirvatte; David, Gregory; Rairoux, Patrick

2016-06-01

In this contribution, we present the results of two recent papers [1,2] published in Optics Express, dedicated to the development of two new lidar methodologies. In [1], while the carbon aerosol (for example, soot particles) is recognized as a major uncertainty on climate and public health, we couple lidar remote sensing with Laser-Induced-Incandescence (LII) to allow retrieving the vertical profile of very low thermal radiation emitted by the carbon aerosol, in agreement with Planck's law, in an urban atmosphere over several hundred meters altitude. In paper [2], awarded as June 2014 OSA Spotlight, we identify the optical requirements ensuring an elastic lidar to be sensitive to new particles formation events (NPF-events) in the atmosphere, while, in the literature, all the ingredients initiating nucleation are still being unrevealed [3]. Both papers proceed with the same methodology by identifying the optical requirements from numerical simulation (Planck and Kirchhoff's laws in [1], Mie and T-matrix numerical codes in [2]), then presenting lidar field application case studies. We believe these new lidar methodologies may be useful for climate, geophysical, as well as fundamental purposes.

Is there an aerosol signature of aqueous processing?

NASA Astrophysics Data System (ADS)

Ervens, B.; Sorooshian, A.

2017-12-01

The formation of aerosol mass in cloud water has been recognized as a substantial source of atmospheric aerosol mass. While sulfate formation can be relatively well constrained, the formation of secondary organic aerosol mass in the aqueous phase (aqSOA) is much more complex due to the multitude of precursors and variety in chemical processes. Aqueous phase processing adds aerosol mass to the droplet mode, which is formed due to mass addition to activated particles in clouds. In addition, it has been shown that aqSOA mass has specific characteristics in terms of oxidation state and hygroscopicity that might help to distinguish it from other SOA sources. Many models do not include detailed chemical mechanisms of sulfate and aqSOA formation and also lack details on the mass distribution of newly formed mass. Mass addition inside and outside clouds modifies different parts of an aerosol population and consequently affects predictions of properties and lifetime of particles. Using a combination of field data analysis and model studies for a variety of air masses, we will show which chemical and physical aerosol properties can be used, in order to identify an `aqueous phase signature' in processed aerosol populations. We will discuss differences in this signature in clean (e.g., background), moderately polluted (e.g., urban) and highly polluted (e.g., biomass burning) air masses and suggest air-mass-specific chemical and/or physical properties that will help to quantify the aqueous-phase derived aerosol mass.

Aerosol particles generated by diesel-powered school buses at urban schools as a source of children’s exposure

PubMed Central

Hochstetler, Heather A.; Yermakov, Mikhail; Reponen, Tiina; Ryan, Patrick H.; Grinshpun, Sergey A.

2015-01-01

Various heath effects in children have been associated with exposure to traffic-related particulate matter (PM), including emissions from school buses. In this study, the indoor and outdoor aerosol at four urban elementary schools serviced by diesel-powered school buses was characterized with respect to the particle number concentrations and size distributions as well as the PM2.5 mass concentrations and elemental compositions. It was determined that the presence of school buses significantly affected the outdoor particle size distribution, specifically in the ultrafine fraction. The time-weighted average of the total number concentration measured outside the schools was significantly associated with the bus and the car counts. The concentration increase was consistently observed during the morning drop-off hours and in most of the days during the afternoon pick-up period (although at a lower degree). Outdoor PM2.5 mass concentrations measured at schools ranged from 3.8 to 27.6 µg m−3. The school with the highest number of operating buses exhibited the highest average PM2.5 mass concentration. The outdoor mass concentrations of elemental carbon (EC) and organic carbon (OC) were also highest at the school with the greatest number of buses. Most (47/55) correlations between traffic-related elements identified in the outdoor PM2.5 were significant with elements identified in the indoor PM2.5. Significant associations were observed between indoor and outdoor aerosols for EC, EC/OC, and the total particle number concentration. Day-to-day and school-to-school variations in Indoor/Outdoor (I/O) ratios were related to the observed differences in opening windows and doors, which enhanced the particle penetration, as well as indoor activities at schools. Overall, the results on I/O ratio obtained in this study reflect the sizes of particles emitted by diesel-powered school bus engines (primarily, an ultrafine fraction capable of penetrating indoors). PMID:25904818

Aerosol particles generated by diesel-powered school buses at urban schools as a source of children's exposure

NASA Astrophysics Data System (ADS)

Hochstetler, Heather A.; Yermakov, Mikhail; Reponen, Tiina; Ryan, Patrick H.; Grinshpun, Sergey A.

2011-03-01

Various heath effects in children have been associated with exposure to traffic-related particulate matter (PM), including emissions from school buses. In this study, the indoor and outdoor aerosol at four urban elementary schools serviced by diesel-powered school buses was characterized with respect to the particle number concentrations and size distributions as well as the PM2.5 mass concentrations and elemental compositions. It was determined that the presence of school buses significantly affected the outdoor particle size distribution, specifically in the ultrafine fraction. The time-weighted average of the total number concentration measured outside the schools was significantly associated with the bus and the car counts. The concentration increase was consistently observed during the morning drop-off hours and in most of the days during the afternoon pick-up period (although at a lower degree). Outdoor PM2.5 mass concentrations measured at schools ranged from 3.8 to 27.6 μg m-3. The school with the highest number of operating buses exhibited the highest average PM2.5 mass concentration. The outdoor mass concentrations of elemental carbon (EC) and organic carbon (OC) were also highest at the school with the greatest number of buses. Most (47/55) correlations between traffic-related elements identified in the outdoor PM2.5 were significant with elements identified in the indoor PM2.5. Significant associations were observed between indoor and outdoor aerosols for EC, EC/OC, and the total particle number concentration. Day-to-day and school-to-school variations in Indoor/Outdoor (I/O) ratios were related to the observed differences in opening windows and doors, which enhanced the particle penetration, as well as indoor activities at schools. Overall, the results on I/O ratio obtained in this study reflect the sizes of particles emitted by diesel-powered school bus engines (primarily, an ultrafine fraction capable of penetrating indoors).

Aerosol particles generated by diesel-powered school buses at urban schools as a source of children's exposure.

PubMed

Hochstetler, Heather A; Yermakov, Mikhail; Reponen, Tiina; Ryan, Patrick H; Grinshpun, Sergey A

2011-03-01

Various heath effects in children have been associated with exposure to traffic-related particulate matter (PM), including emissions from school buses. In this study, the indoor and outdoor aerosol at four urban elementary schools serviced by diesel-powered school buses was characterized with respect to the particle number concentrations and size distributions as well as the PM2.5 mass concentrations and elemental compositions. It was determined that the presence of school buses significantly affected the outdoor particle size distribution, specifically in the ultrafine fraction. The time-weighted average of the total number concentration measured outside the schools was significantly associated with the bus and the car counts. The concentration increase was consistently observed during the morning drop-off hours and in most of the days during the afternoon pick-up period (although at a lower degree). Outdoor PM2.5 mass concentrations measured at schools ranged from 3.8 to 27.6 µg m -3 . The school with the highest number of operating buses exhibited the highest average PM2.5 mass concentration. The outdoor mass concentrations of elemental carbon (EC) and organic carbon (OC) were also highest at the school with the greatest number of buses. Most (47/55) correlations between traffic-related elements identified in the outdoor PM2.5 were significant with elements identified in the indoor PM2.5. Significant associations were observed between indoor and outdoor aerosols for EC, EC/OC, and the total particle number concentration. Day-to-day and school-to-school variations in Indoor/Outdoor (I/O) ratios were related to the observed differences in opening windows and doors, which enhanced the particle penetration, as well as indoor activities at schools. Overall, the results on I/O ratio obtained in this study reflect the sizes of particles emitted by diesel-powered school bus engines (primarily, an ultrafine fraction capable of penetrating indoors).

Black carbon in aerosol during BIBLE B

NASA Astrophysics Data System (ADS)

Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

2003-02-01

The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

Black carbon in aerosol during BIBLE B

NASA Astrophysics Data System (ADS)

Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

2002-02-01

The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

On the influence of Aerosols in measurement of electric field from Earth surface using a Field-Mill

NASA Astrophysics Data System (ADS)

Ghosh, Abhijit; Sundar De, Syam; Paul, Suman; Hazra, Pranab; Guha, Gautam

2016-07-01

Aerosol particles influence the electrical conductivity of air. The value is reduced through the removal of small ions responsible for the conductivity. The metropolitan city, Kolkata (latitude 22.56° N, longitude 88.5° E) is densely populated surrounded by various types of Industries. Air is highly invaded by pollutant particles here for which the city falls under small-scale fair-weather condition where electric field and air-earth current get perturbed by ionization and different aerosols produced locally. Fine particles having diameter < 0.1 μm (Aitken nuclei) are distributed in air which decreases the electrical conductivity and increases the columnar resistance. Aerosol particles steadily change the status at different times of the day through coagulation, sedimentation, charge-transfer initiated by precipitation. The diurnal variation of potential gradient is caused mainly due to urbanization, emission from industry and traffic. The rate of production of haze (atmospheric suspension) and their vertical transportation control the daily variation of atmospheric potential. The nuclei of pollutant particles combine with ions and decrease the concentration of small ions thereby reducing the conductivity. The pollutants, influenced by CO _{2} and other green house gas emission from fossil fuels are also responsible for the variation of electric field. Variation in consumption of Oil and Gasoline due to traffic in the city contributes a high Aitken count and there are changes in atmospheric dispersion following reduction of conductivity of the medium. Outcome of some important measurement of potential gradient and air-earth current will be presented. Different parameters like air-conductivity, relative abundance of smoke, visibility would offer new signatures of aerosol-influence on electric potential gradient. Some of those will be reported here.

Urban light pollution - The effect of atmospheric aerosols on astronomical observations at night

NASA Astrophysics Data System (ADS)

Joseph, J. H.; Kaufman, Y. J.; Mekler, Y.

1991-07-01

The transfer of diffuse city light from a localized source through a dust-laden atmosphere with optical depth less than 0.5 has been analyzed in the source-observer plane on the basis of an approximate treatment. The effect on several types of astronomical observation at night has been studied, considering different size distributions and amounts as well as particle shapes of the aerosols. The analysis is made in terms of the signal-to-noise ratios for a given amount of aerosol. The model is applied to conditions at the Wise Astronomical Observatory in the Negev desert, and limiting backgrounds for spectroscopy, photometry, and photography of stars and extended objects have been calculated for a variety of signal-to-noise ratios. Applications to observations with different equipment at various distances from an urban area of any size are possible. Due to the use of signal-to-noise ratios, the conclusions are different for the different experimental techniques used in astronomy.

Urban light pollution - The effect of atmospheric aerosols on astronomical observations at night

NASA Technical Reports Server (NTRS)

Joseph, Joachim H.; Mekler, Yuri; Kaufman, Yoram J.

1991-01-01

The transfer of diffuse city light from a localized source through a dust-laden atmosphere with optical depth less than 0.5 has been analyzed in the source-observer plane on the basis of an approximate treatment. The effect on several types of astronomical observation at night has been studied, considering different size distributions and amounts as well as particle shapes of the aerosols. The analysis is made in terms of the signal-to-noise ratios for a given amount of aerosol. The model is applied to conditions at the Wise Astronomical Observatory in the Negev desert, and limiting backgrounds for spectroscopy, photometry, and photography of stars and extended objects have been calculated for a variety of signal-to-noise ratios. Applications to observations with different equipment at various distances from an urban area of any size are possible. Due to the use of signal-to-noise ratios, the conclusions are different for the different experimental techniques used in astronomy.

Multiday production of condensing organic aerosol mass in urban and forest outflow

DOE PAGES

Lee-Taylor, J.; Hodzic, A.; Madronich, S.; ...

2014-07-03

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1–2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products ofmore » both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

Aerosol Optical Properties over Northwestern European Seas

NASA Astrophysics Data System (ADS)

Avgousta Floutsi, Athina; Korras Carraca, Marios Bruno; Matsoukas, Christos; Riva, Riccardo; Biskos, George

2017-04-01

Atmospheric aerosols, both natural and anthropogenic, can affect the regional and global climate through their direct, indirect, and semi-direct effects on the radiative energy budget of the Earth-atmosphere system. In order to quantify these effects it is necessary to determine the aerosol load. An effective way to do this is by measuring the aerosol optical depth (AOD). Besides AOD, the Fine mode Fraction (AOD of particles smaller than 1 μm / total AOD, FF) is a useful parameter for the characterization of the aerosol and provides a good proxy for particle size. In this study, we investigate the spatial and temporal variability of the AOD and FF over the Western and Northwestern European Seas (43° N - 67° N, 10° W - 31° E), where significant sources of both natural and anthropogenic particles are located. Anthropogenic particles (mostly fine mode) originate from ship activity, or from urban-industrial and biomass-burning processes in the European countries. The natural, coarse mode particles are primarily sea salt. The study is performed using Collection 006 Level-3 mean daily aerosol data from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument on board Aqua satellite, available in 1° × 1° resolution (ca. 100 km × 100 km) over the period 2002- 2014. Our results indicate significant spatial variability of the aerosol load over the study region. The highest AOD values (up to 0.32 on annual level) are observed over the English Channel and the coasts of the Netherlands and Germany. In these regions the highest FF values are also observed (up to 0.77), indicating a relatively large contribution of anthropogenic particles to the aerosol load. Offshore, both AOD and FF are lower compared to coastal regions, indicating the predominance of maritime aerosols (sea salt). The data also show a clear seasonal cycle, with larger aerosol load during spring and summer (AOD up to 0.60), and lower during autumn and winter (AOD up to 0.30). A similar pattern is observed for FF indicating a larger contribution of anthropogenic particles during spring and summer compared to autumn and winter. The highest FF values (up to 0.80- 0.85) are observed over the Baltic Sea during summer while year-round the lowest values are observed in remote maritime areas, mostly in the northern part of our study region, highlighting the predominance of sea salt particles. The AOD exhibits a generally decreasing trend (slope between -0.18 to 0.05 per decade). Positive values are observed over the northwestern ocean areas (sea salt dominated), while over most of our study region the slope is of the order of -0.02 to -0.05 per decade. These trends are possibly associated with a reduction of the anthropogenic emissions.

High Resolution Mass Spectrometry of Seasonal Aerosol Samples From an Urban Location in the Italian Po Valley

NASA Astrophysics Data System (ADS)

Mahon, Brendan; Giorio, Chiara; Gallimore, Peter J.; Zielinski, Arthur T.; Tapparo, Andrea; Kalberer, Markus

2016-04-01

The Po Valley in Northern Italy represents one of the most polluted environments in Europe, with PM2.5 and ozone concentrations regularly exceeding 100μg/m3 and 50ppb respectively. Particularly during winter, prolonged inversion conditions together with biomass burning and anthropogenic emissions regularly lead to severe air pollution events. Over the course of several months in 2013-14, we carried out a sampling program at a city-centre site in Padova, Italy, collecting 24-hour high-volume aerosol filter samples, 18 in winter (mid December - mid March) and 20 in summer (late May - late July). Utilising high-resolution Orbitrap mass spectrometry techniques, we have characterised these sample sets to examine the long-term variation in aerosol composition over the sampling campaign and to determine the effect of anthropogenic gaseous pollutants such as NOx and SO2 on the composition of organic particle components. The results showed that between ca. 450-700 ions were measured in each sample in both the summer and winter sample sets, however the majority (90%) of ions in the winter samples were below 300m/z and below 380m/z in the summer samples. A much higher percentage of CHO-only ions were found in winter (ca. 27%) compared to the summer samples (ca. 6%), indicating a higher degree of photochemical reactions taking place involving pollutants such as NOx and SO2 in summer. Our results represent the first long term data set of high-resolution measurements of aerosol composition and demonstrate that this technique is an important tool in evaluating the composition of aerosol particles in complex polluted urban areas.

Highly Acidic Ambient Particles, Soluble Metals, and Oxidative Potential: A Link between Sulfate and Aerosol Toxicity.

PubMed

Fang, Ting; Guo, Hongyu; Zeng, Linghan; Verma, Vishal; Nenes, Athanasios; Weber, Rodney J

2017-03-07

Soluble transition metals in particulate matter (PM) can generate reactive oxygen species in vivo by redox cycling, leading to oxidative stress and adverse health effects. Most metals, such as those from roadway traffic, are emitted in an insoluble form, but must be soluble for redox cycling. Here we present the mechanism of metals dissolution by highly acidic sulfate aerosol and the effect on particle oxidative potential (OP) through analysis of size distributions. Size-segregated ambient PM were collected from a road-side and representative urban site in Atlanta, GA. Elemental and organic carbon, ions, total and water-soluble metals, and water-soluble OP were measured. Particle pH was determined with a thermodynamic model using measured ionic species. Sulfate was spatially uniform and found mainly in the fine mode, whereas total metals and mineral dust cations were highest at the road-side site and in the coarse mode, resulting in a fine mode pH < 2 and near neutral coarse mode. Soluble metals and OP peaked at the intersection of these modes demonstrating that sulfate plays a key role in producing highly acidic fine aerosols capable of dissolving primary transition metals that contribute to aerosol OP. Sulfate-driven metals dissolution may account for sulfate-health associations reported in past studies.

Aerosol optical properties and types over the tropical urban region of Hyderabad, India

NASA Astrophysics Data System (ADS)

Kharol, Shailesh Kumar; Kaskaoutis, D. G.; Rani Sharma, Anu; Kvs, Badarinath; Kambezidis, H. D.

India is densely populated, industrialized and in the recent years has witnessed an impressive economic development. Aerosols over and around India not only affect the Indian monsoon but also the global climate. The growing population coupled with revolution in industry has resulted in higher demands for energy and transport. With more and more urbanization the usage pattern of fossil and bio-fuels are leading to changes in aerosol properties, which may cause changes in precipitation and can decelerate the hydrological cycle. Over urban areas of India aerosol emissions from fossil fuels such as coal, petrol and diesel oil dominate. Further-more, the Indian subcontinent exhibits different land characteristics ranging from vegetated areas and forests to semiarid and arid environments and tall mountains. India experiences large seasonal climatic variations, which result in extreme temperatures, rainfall and relative humidity. These meteorological and climatic features introduce large variabilities in aerosol op-tical and physico-chemical characteristics at spatial and temporal scales. In the present study, seasonal variations in aerosol properties and types were analysed over tropical urban region of Hyderabad, India during October 2007-September 2008 using MICROTOPS II sun photometer measurements. Higher aerosol optical depth (AOD) values are observed in premonsoon, while the variability of the ˚ngstrüm exponent (α) seems to be more pronounced with higher values A in winter and premonsoon and lower in the monsoon periods. The AOD at 500 nm (AOD500 ) is very large over Hyderabad, varying from 0.46±0.17 in postmonsoon to 0.65±0.22 in premon-soon periods. A discrimination of the different aerosol types over Hyderabad is also attempted using values of AOD500 and α380-870. Such discrimination is rather difficult to interpret since a single aerosol type can partly be identified only under specific conditions (e.g. anthropogenic emissions, biomass burning or dust outbreaks), while the presence of mixed aerosols, without dominance of the coarse or accumulation mode is the usual situation. According to the analysis the three individual components of differing origin, composition and optical characteristics are, a) an urban/industrial aerosol type composed of aerosols produced locally and all year round by combustion activities in the city or long-range transported (mainly in spring) biomass burning, b) an aerosol type of mineral origin raised by the wind in the deserts (mainly in premonsoon) or constitutes coarse-mode aerosols under high relative humidity conditions mainly in the monsoon period, and c) an aerosol type with a marine influence under background conditions occurred in monsoon and postmonsoon periods. Nevertheless, the mixed or undetermined aerosol type dominates with percentages varying from 44.3% (premonsoon) to 72.9% (postmonsoon). Spec-tral AOD and α data are analyzed to obtain information about the adequacy of the simple use of the ˚ngstrüm exponent for characterizing the aerosols. This is achieved by taking advantage A of the spectral variation of lnAOD vs lnλ, the so-called curvature. The results show that the spectral curvature can be effectively used as a tool for aerosol types discrimination, since the fine-mode aerosols exhibit negative curvature, while the coarse-mode particles positive. The present study is among the first over Hyderabad focusing on the seasonal pattern of aerosol properties and types and aiming at associating them with local emissions, regional climatology and long-range transport. Keywords: AOD, aerosol types; sun photometer; back trajectories; Hyderabad; India

Size Distribution, Chemical Composition and Optical Properties of Atmospheric Dust in Israel: A Comparison of Urban and Desert Aerosols under Clear and Dusty Conditions.

DTIC Science & Technology

1980-02-01

size distribution and aerosol particle concentrations during a winter period in Mitzpe Ramon. Negev desert. Fig. 5 Comparison of normalized frequency...Israel. The upper two samples are from Mitzpe Ramon in the Negev desert. The bottom three are from Tel Aviv. The lighter of the three Tel Aviv samples (the...shown show much higher imaginary indices than do those from the Negev desert or the two American desert localities (Lindberg et al., 1976). Fig. 12

CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions

NASA Astrophysics Data System (ADS)

Thalman, Ryan; de Sá, Suzane S.; Palm, Brett B.; Barbosa, Henrique M. J.; Pöhlker, Mira L.; Lizabeth Alexander, M.; Brito, Joel; Carbone, Samara; Castillo, Paulo; Day, Douglas A.; Kuang, Chongai; Manzi, Antonio; Ng, Nga Lee; Sedlacek, Arthur J., III; Souza, Rodrigo; Springston, Stephen; Watson, Thomas; Pöhlker, Christopher; Pöschl, Ulrich; Andreae, Meinrat O.; Artaxo, Paulo; Jimenez, Jose L.; Martin, Scot T.; Wang, Jian

2017-10-01

During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ˜ 0. 15 is consistent with the largely uniform and high O : C value (˜ 0. 8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through multivariable linear regression. For the SOA factors, the variation of the κ value with O : C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O : C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O : C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O : C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase in κorg with O : C, as observed during this and earlier field studies. This finding helps better understand and reconcile the differences in the relationships between κorg and O : C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.

Urban particle size distributions during two contrasting dust events originating from Taklimakan and Gobi Deserts.

PubMed

Zhao, Suping; Yu, Ye; Xia, Dunsheng; Yin, Daiying; He, Jianjun; Liu, Na; Li, Fang

2015-12-01

The dust origins of the two events were identified using HYSPLIT trajectory model and MODIS and CALIPSO satellite data to understand the particle size distribution during two contrasting dust events originated from Taklimakan and Gobi deserts. The supermicron particles significantly increased during the dust events. The dust event from Gobi desert affected significantly on the particles larger than 2.5 μm, while that from Taklimakan desert impacted obviously on the particles in 1.0-2.5 μm. It is found that the particle size distributions and their modal parameters such as VMD (volume median diameter) have significant difference for varying dust origins. The dust from Taklimakan desert was finer than that from Gobi desert also probably due to other influencing factors such as mixing between dust and urban emissions. Our findings illustrated the capacity of combining in situ, satellite data and trajectory model to characterize large-scale dust plumes with a variety of aerosol parameters. Copyright © 2015 Elsevier Ltd. All rights reserved.

Monthly and diurnal variations in aerosol size distributions, downwind of the Seoul metropolitan area

NASA Astrophysics Data System (ADS)

Kim, B. S.; Choi, Y.; Ghim, Y. S.

2014-12-01

The size distribution of aerosols is a physical property. However, since major aerosol types such as mineral dust, secondary inorganic ions, and carbonaceous aerosols are typically in specific size ranges, we can estimate the chemical composition of aerosols from the size distribution. We measured the mass size distribution of aerosols using an optical particle counter (Grimm Model 1.109) for a year from February 2013 to February 2014 at intervals of 10 minutes. The optical particle counter measures number concentrations between 0.25 and 32 μm in 31 bins and converts them into mass concentrations assuming a sphere and densities of aerosols in urban environment which originate from traffic and other combustion sources and are secondarily formed from photochemical reactions. The measurement site is at the rooftop of the five-story building on the hill (37.34 °N, 127.27 °E, 167 m above sea level), about 35 km southeast of downtown Seoul, the downwind area of which is affected by prevailing northwesterlies. There are no major emission sources nearby except a 4-lane road running about 1.4 km to the west. We tried to characterize the bimodal property of the mass size distribution, consisting of fine and coarse modes, in terms of mass concentration and mean diameter. Monthly and diurnal variations in mass concentration and mean diameter of each mode were investigated to estimate major aerosol types as well as major factors causing those variations.

Seasonality of major aerosol species and their transformations in Cairo megacity

NASA Astrophysics Data System (ADS)

Favez, Olivier; Cachier, Hélène; Sciare, Jean; Alfaro, Stéphane C.; El-Araby, Tarek M.; Harhash, Maha A.; Abdelwahab, Magdy M.

Bulk aerosols sampled on a weekly basis at two Cairo (Egypt) urban sites from January 2003 to May 2006 were analysed for their chemical composition of major aerosol species (elemental carbon, water soluble/insoluble organic carbon, nitrate, sulphate, ammonium, chloride, sodium and calcium). Data subsequently obtained constitute one of the longest and more detailed dataset related to Cairo aerosols, and offer the opportunity to investigate seasonal trends. Dust aerosols (derived from calcium measurements) displayed maximum concentrations in spring and winter, due to frequent dust storms, but also high background concentration levels (˜50 μg m -3) all year long. Within these particles, about 40% on average of Ca 2+ was found to be associated with SO 42-, NO 3- and/or Cl -, pointing out "dust anthropization" processes and their subsequent climatic impact on a regional scale. Seasonal variations of non-dust aerosols, equally distributed between carbonaceous aerosols and ions, were also observed, with concentrations of the order of 100 μg m -3 in autumn and winter, and of 60 μg m -3 in spring and summer. High concentration levels of non-sea-salt chloride (up to 15 μg m -3 on a monthly basis), likely of industrial origin, were observed in autumn and winter. During the autumn "Black Cloud" event, biomass burning aerosols originating from rice straw burning in the Nile Delta have shown to account for 12%, 35% and 50% of Cairo EC, WIOC and WSOC mass concentrations, respectively. Finally, relatively low WSOC/OC ratios (˜1/3) were obtained all the year long, calling for more investigation on the water-solubility of organic aerosols originating from the burning of agricultural waste, and on that of secondary organic aerosols formed in dry urban atmospheres.

A synergetic approach for estimating the local direct aerosol forcing: Application to an urban zone during the Expérience sur Site pour Contraindre les Modèles de Pollution et de Transport d'Emission (ESCOMPTE) experiment

NASA Astrophysics Data System (ADS)

Roger, J. C.; Mallet, M.; Dubuisson, P.; Cachier, H.; Vermote, E.; Dubovik, O.; Despiau, S.

2006-07-01

A method dedicated to the investigation of direct radiative forcing of the main anthropogenic aerosol species (ammonium sulfate, black carbon, particulate organic matter) is presented. We computed the direct radiative aerosol forcing at the top of atmosphere (TOA), at the bottom of atmosphere (BOA), and into the atmospheric layer (ATM). The methodology is based on chemical, photometric, and satellite measurements. We first determined the optical properties of the main aerosol species and then computed their direct radiative impact at local scale. The method was applied to a periurban zone during the Expérience sur Site pour Contraindre les Modèles de Pollution et de Transport d'Emission experiment. Optical computations indicate that the single scattering albedo, for the total aerosol population in the external mixture, is equal to 0.83 ± 0.04 at 550 nm, indicative of a strong absorption of the solar radiation. At the same time the mean asymmetry parameter is equal to 0.59 ± 0.04, and the mean aerosol optical thickness is equal to 0.30 ± 0.02, at 550 nm. The anthropogenic urban aerosol layer reduces significantly the daily surface illumination (-24 W m-2 > ΔFBOA > -47.5 W m-2) by reflection to space (-6 W m-2 > ΔFTOA > -9 W m-2) and by absorption of the solar radiation into the atmosphere (17 W m-2 < ΔFATM < 39 W m-2). The available resulting energy in the atmospheric column heats the lowermost part of the atmosphere from 1.1°K d-1 to 2.8°K d-1. Our study shows that the black carbon particles have a large contribution to the BOA forcing (almost 50% of the total daily forcing), whereas the ammonium sulfate particles contribute only to about 10%. Conversely, the TOA daily forcing is mostly driven by the ammonium sulfate aerosol (around 50%).

Using the Aerosol Single Scattering Albedo and Angstrom Exponent from AERONET to Determine Aerosol Origins and Mixing States over the Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Slutsker, I.; Smirnov, A.; Schafer, J. S.; Dickerson, R. R.; Thompson, A. M.; Tripathi, S. N.; Singh, R. P.; Ghauri, B.

2012-12-01

Aerosol mixtures—whether dominated by dust, carbon, sulfates, nitrates, sea salt, or mixtures of them—complicate the retrieval of remotely sensed aerosol properties from satellites and possibly increase the uncertainty of the aerosol radiative impact on climate. Major aerosol source regions in South Asia include the Thar Desert as well as agricultural lands, Himalayan foothills, and large urban centers in and near the Indo-Gangetic Plain (IGP). Over India and Pakistan, seasonal changes in meteorology, including the monsoon (June-September), significantly affect the transport, lifetime, and type of aerosols. Strong monsoonal winds can promote long range transport of dust resulting in mixtures of dust and carbonaceous aerosols, while more stagnant synoptic conditions (e.g., November-January) can prolong the occurrence of urban/industrial pollution, biomass burning smoke, or mixtures of them over the IGP. Aerosol Robotic Network (AERONET) Sun/sky radiometer data are analyzed to show the aerosol optical depth (AOD) seasonality and aerosol dominant mixing states. The Single Scattering Albedo (SSA) and extinction Angstrom exponent (EAE) relationship has been shown to provide sound clustering of dominant aerosol types using long term AERONET site data near known source regions [Giles et al., 2012]. In this study, aerosol type partitioning using the SSA (440 nm) and EAE (440-870 nm) relationship is further developed to quantify the occurrence of Dust, Mixed (e.g., dust and carbonaceous aerosols), Urban/Industrial (U/I) pollution, and Biomass Burning (BB) smoke. Based on EAE thresholds derived from the cluster analysis (for AOD440nm>0.4), preliminary results (2001-2010) for Kanpur, India, show the overall contributions of each dominant particle type (rounded to the nearest 10%): 10% for Dust (EAE≤0.25), 60% for Mixed (0.251.25). In the IGP, BB aerosols may have varying sizes (e.g., corresponding to 1.2

Characterization of particle number size distribution and new particle formation in Southern China.

PubMed

Huang, Xiaofeng; Wang, Chuan; Peng, Jianfei; He, Lingyan; Cao, Liming; Zhu, Qiao; Cui, Jie; Wu, Zhijun; Hu, Min

2017-01-01

Knowledge of particle number size distribution (PND) and new particle formation (NPF) events in Southern China is essential for mitigation strategies related to submicron particles and their effects on regional air quality, haze, and human health. In this study, seven field measurement campaigns were conducted from December 2013 to May 2015 using a scanning mobility particle sizer (SMPS) at four sites in Southern China, including three urban sites and one background site. Particles were measured in the size range of 15-615nm, and the median particle number concentrations (PNCs) were found to vary in the range of 0.3×10 4 -2.2×10 4 cm -3 at the urban sites and were approximately 0.2×10 4 cm -3 at the background site. The peak diameters at the different sites varied largely from 22 to 102nm. The PNCs in the Aitken mode (25-100nm) at the urban sites were up to 10 times higher than they were at the background site, indicating large primary emissions from traffic at the urban sites. The diurnal variations of PNCs were significantly influenced by both rush hour traffic at the urban sites and NPF events. The frequencies of NPF events at the different sites were 0%-30%, with the highest frequency occurring at an urban site during autumn. With higher SO 2 concentrations and higher ambient temperatures being necessary, NPF at the urban site was found to be more influenced by atmospheric oxidizing capability, while NPF at the background site was limited by the condensation sink. This study provides a unique dataset of particle number and size information in various environments in Southern China, which can help understand the sources, formation, and the climate forcing of aerosols in this quickly developing region, as well as help constrain and validate NPF modeling. Copyright © 2016. Published by Elsevier B.V.

Role of snow and cold environment in the fate and effects of nanoparticles and select organic pollutants from gasoline engine exhaust.

PubMed

Nazarenko, Yevgen; Kurien, Uday; Nepotchatykh, Oleg; Rangel-Alvarado, Rodrigo B; Ariya, Parisa A

2016-02-01

Exposure to vehicle exhaust can drive up to 70 % of excess lifetime cancer incidences due to air pollution in urban environments. Little is known about how exhaust-derived particles and organic pollutants, implicated in adverse health effects, are affected by freezing ambient temperatures and the presence of snow. Airborne particles and (semi)volatile organic constituents in dilute exhaust were studied in a novel low-temperature environmental chamber system containing natural urban snow under controlled cold environmental conditions. The presence of snow altered the aerosol size distributions of dilute exhaust in the 10 nm to 10 μm range and decreased the number density of the nanoparticulate (<100 nm) fraction of exhaust aerosols, yet increased the 100-150 nm fraction. Upon 1 hour exhaust exposure, the total organic carbon increased in the natural snow from 0.218 ± 0.014 to 0.539 ± 0.009 mg L(-1), and over 40 additional (semi)volatile organic compounds and a large number of exhaust-derived carbonaceous and likely organic particles were identified. The concentrations of benzene, toluene, ethylbenzene, and xylenes (BTEX) increased from near the detection limit to 52.48, 379.5, 242.7, and 238.1 μg kg(-1) (± 10 %), respectively, indicating the absorption of exhaust-derived toxic organic compounds by snow. The alteration of exhaust aerosol size distributions at freezing temperatures and in the presence of snow, accompanied by changes of the organic pollutant content in snow, has potential to alter health effects of human exposure to vehicle exhaust.

Variations of aerosol size distribution, chemical composition and optical properties from roadside to ambient environment: A case study in Hong Kong, China

NASA Astrophysics Data System (ADS)

Zhang, Qian; Ning, Zhi; Shen, Zhenxing; Li, Guoliang; Zhang, Junke; Lei, Yali; Xu, Hongmei; Sun, Jian; Zhang, Leiming; Westerdahl, Dane; Gali, Nirmal Kumar; Gong, Xuesong

2017-10-01

This study investigated the ;roadside-to-ambient; evolution of particle physicochemical and optical properties in typical urban atmospheres of Hong Kong through collection of chemically-resolved PM2.5 data and PM2.5 size distribution at a roadside and an ambient site. Roadside particle size distribution showed typical peaks in the nuclei mode (30-40 nm) while ambient measurements peaked in the Aitken mode (50-70 nm), revealing possible condensation and coagulation growth of freshly emitted particles during aging processes. Much higher levels of anthropogenic chemical components, i.e. nitrate, sulfate, ammonium, organic carbon (OC) and elemental carbon (EC), but lower levels of OC/EC and secondary inorganic aerosols (SIA)/EC ratios appeared in roadside than ambient particles. The high OC/EC and SIA/EC ratios in ambient particles implied high contributions from secondary aerosols. Black carbon (BC), a strong light absorbing material, showed large variations in optical properties when mixed with other inorganic and organic components. Particle-bound polycyclic aromatic hydrocarbons (p-PAHs), an indicator of brown carbon (BrC), showed significant UV-absorbing ability. The average BC and p-PAHs concentrations were 3.8 and 87.6 ng m-3, respectively, at the roadside, but were only 1.5 and 18.1 ng m-3 at the ambient site, suggesting BC and p-PAHs concentrations heavily driven by traffic emissions. In contrast, PM2.5 UV light absorption coefficients (babs-BrC,370nm) at the ambient site (4.2 Mm-1) and at the roadside site (4.1 Mm-1) were similar, emphasizing that particle aging processes enhanced UV light-absorbing properties, a conclusion that was also supported by the finding that the Absorption Ångström coefficient (AAC) value at UV wavelengths (AAC_UV band) at the ambient site were ∼1.7 times higher than that at the roadside. Both aqueous reaction and photochemically produced secondary organic aerosol (SOA) for ambient aerosols contributed to the peak values of babs-BrC,370nm in ambient particles at midnight and around noon, highlighting that secondary BrC had different sources and particle aging in the atmosphere affected BrC and BC properties and related aerosol light absorption.

Characterizing the composition and evolution of and urban particles in Chongqing (China) during summertime

NASA Astrophysics Data System (ADS)

Chen, Yang; Yang, Fumo; Mi, Tian; Cao, Junji; Shi, Guangming; Huang, Rujin; Wang, Huanbo; Chen, Jun; Lou, Shengrong; Wang, Qiyuan

2017-05-01

Urban particles were investigated using a single particle aerosol mass spectrometer (SPAMS) in Chongqing during the summertime (from 07/05/2014 to 08/06/2014). Chemical composition, mixing state, and atmospheric behavior of urban particles were studied. The major particle types include ECOC (Elemental-Carbon-Organic-Carbon 20.6%), OC (20.1%), KSec (K-Secondary) (13.3%), BB (Biomass burning, 11.9%), NaK (sodium-potassium-rich, 7.3%), Al-rich (4.0%), Fe-rich (3.2%), Ca-rich (1.4%), Ca-EC (1.6%), and NaKPb (0.5%). EC, ECOC, OC, and Ca-EC were prevalent in the condensation mode (< 0.7 μm), while KSec, EC, NaK were significant in both the droplet mode (0.7-1.1 μm) and coarse mode. Increases in aged groups such as EC, KSec, and NaK were observed in the afternoon. Case studies suggested that wet scavenging (rain) rates of different single particle types followed an order of NaKPb > Fe-rich > EC > Ca-EC > Ca-rich > KSec > OC > NaK > ECOC > Al-rich > BB. Increased number fraction of EC and KSec were correlated with the increase of odd oxygen (Ox = O3 + NO2). EC, OC, and ECOC were enriched at higher relative humidity. The findings of this study on the mixing state, temporal variation, processing, and evolution of single particles provide new insight into the atmospheric behavior and impacts of urban particles.

Scattering and absorption characteristics of aerosols at an urban megacity over IGB: Implications to radiative forcing

NASA Astrophysics Data System (ADS)

Srivastava, A. K.; Bisht, D. S.; Singh, Sachchidanand; Kishore, N.; Soni, V. K.; Singh, Siddhartha; Tiwari, S.

2018-06-01

Aerosol scattering and absorption characteristics were investigated at an urban megacity Delhi in the western Indo-Gangetic Basin (IGB) during the period from October 2011 to September 2012 using different in-situ measurements. The scattering coefficient (σsp at 550 nm) varied between 71 and 3014 Mm-1 (mean 710 ± 615 Mm-1) during the entire study period, which was about ten times higher than the absorption coefficient (σabs at 550 nm 67 ± 40 Mm-1). Seasonally, σsp and σabs were substantially higher during the winter/post-monsoon periods, which also gave rise to single scattering albedo (SSA) by 5%. The magnitude of SSA (at 550 nm) varied between 0.81 and 0.94 (mean: 0.89 ± 0.05). Further, the magnitude of scattering Ångström exponent (SAE) and back-scattering Ångström exponent (BAE) showed a wide range from -1.20 to 1.57 and -1.13 to 0.87, respectively which suggests large variability in aerosol sizes and emission sources. Relatively higher aerosol backscatter fraction (b at 550 nm) during the monsoon (0.25 ± 0.10) suggests more inhomogeneous scattering, associated with the coarser dust particles. However, lower value of b during winter (0.13 ± 0.02) is associated with more isotropic scattering due to dominance of smaller size particles. This is further confirmed with the estimated asymmetry parameter (AP at 550 nm), which exhibits opposite trend with b. The aerosol optical parameters were used in a radiative transfer model to estimate aerosol radiative forcing. A mean radiative forcing of -61 ± 22 W m-2 (ranging from -111 to -40 W m-2) was observed at the surface and 42 ± 24 W m-2 (ranging from 18 to 87 W m-2) into the atmosphere, which can give rise to the mean atmospheric heating rate of 1.18 K day-1.

PM2.5 soluble brown-carbon measured in contrasting urban and rural environments

NASA Astrophysics Data System (ADS)

Weber, R.; Zhang, X.

2011-12-01

An instrument was developed to continuously measure the light absorption spectra and carbon mass of soluble PM2.5 components by coupling a particle-into-liquid sampler (PILS), UV-VIS (200-800nm) spectrophotometer with long-path absorption cell and total organic carbon (TOC) analyzer. The analytical system has also been used to measure brown carbon in aqueous extracts from integrated filters. Measurements have been conducted at a number of locations, including urban sites in Los Angeles, Atlanta and smaller urban and rural locations in the southeastern US. At all locations a characteristic brown carbon absorption spectra was observed, where soluble chromophores produce an increasing absorption with decreasing wavelength, starting from mid-visible and extending into the near UV. Incomplete combustion from biomass and fossil fuel burning and secondary processes have been identified as sources of soluble brown carbon. During summer when biomass burning impacts were minimal, mass absorption efficiencies calculated relative to ambient particle water-soluble organic carbon (WSOC) were highest in Los Angeles and correlated with the daily production of secondary organic aerosol. Nitro-aromatics were identified as a component of the brown carbon. In contrast, the Atlanta secondary aerosol was significantly less light-absorbing, and unlike Los Angeles the diurnal trend in brown carbon largely tracked primary sources. Absorption Angstrom exponents varied between 3 and 7 with fresh Los Angeles secondary organic aerosol associated with smaller exponents, indicting greater absorption into the visible spectrum. The southeastern US regional/rural brown carbon was the least absorbing per WSOC mass in the UV and with largest Angstrom exponents (7) the least absorbing at higher wavelengths. A correlation between the regional brown carbon and fine particle oxalate suggested an aqueous phase heterogeneous source for these chromophores. Compared to pure black carbon, brown carbon was optically significant at low wavelengths (365 nm) and most important in rural regions due to low black carbon concentrations.

Submicron aerosol and trace gas composition near Manaus as observed during GoAmazon2014/5

NASA Astrophysics Data System (ADS)

Ferreira De Brito, J.; Wurm, F.; Liu, Y.; de Sá, S. S.; Carbone, S.; Rizzo, L. V.; Cirino, G. G.; Barbosa, H. M.; Souza, R. A. F. D.; Martin, S. T.; Artaxo, P.

2014-12-01

The Amazon Basin, during the wet season, has one of the lowest aerosol concentrations worldwide, with air masses covering thousands of kilometers of pristine forest with negligible human impact. The atmosphere in such regions is strongly coupled with the biosphere through primary biological aerosols, biogenic salts and secondary aerosols from oxidation of biogenic VOCs. The natural environment is strongly modified nearby urbanized areas, in particular Manaus, a city of nearly two million people. The urban pollution plume has high concentrations of oxides of nitrogen and sulfur, carbon monoxide, particle concentrations, and soot, among other pollutants, strongly contrasting with the clean air masses reaching the city. Such unique location provides the ideal laboratory to study the isolated urban emission, as well the pristine environment by perturbing it in a relatively known fashion. The GoAmazon experiment was designed with these questions in mind, combining remote sensing, in situand airborne measurements. This manuscript describes the measurements currently taking place at the T2 site, near Manaus, frequently impacted by relatively fresh emissions from the city. This presentation focuses on aerosol properties and trace gas composition at the T2 site. PM1 mass concentration from March up to July 2014 has been observed to be dominated by organics (1.51 μg m-3), followed by BC (0.83 μg m-3), SO4 (0.17 μg m-3), NO3 (0.08 μg m-3) and NH4 (0.06 μg m-3). Mean aerosol number concentration was 3600 cm-3, with a mean geometric diameter of 70 nm. As for the trace gases, initial estimates of isoprene average ambient concentration is 0.95 ppb, whereas MVK+MACR has been estimated to be 0.76 ppb. Average mixing ratios of toluene, benzene and C8 aromatics were 0.31 ppb, 0.16 ppb and 0.15 ppb, respectively, correlating relatively well with markers of anthropogenic activities, such as BC. Such measurements will carry on throughout GoAmazon 2014/5, providing a unique dataset to understand the aerosol life cycle and the impact of urban emission in the heart of the Amazon Forest.

Spectral solar attenuation due to aerosol loading over an urban area in India

NASA Astrophysics Data System (ADS)

Latha, K. Madhavi; Badarinath, K. V. S.

2005-06-01

Anthropogenic activities in urban areas are sources for atmospheric aerosols and are increasing due to population explosion and migration. Many large cities in the developing world are presently plagued by high levels of atmospheric pollution and long-term effect of urban aerosol on climate is an important topic. In the present study, ground-based measurements of solar irradiance, aerosol loading and black carbon (BC) aerosol concentration have been analyzed during different aerosol loading conditions during 2003 over an urban environment. BC aerosols concentration has been observed to be enhanced during high aerosol optical depth day suggesting influence of local anthropogenic activities. The analysis of wind fields over the study area during the measurement period is from north with continental air mass prevailing over the region. Spectral measurements of solar irradiance exhibited variations based on aerosol loading in urban atmosphere. Relative attenuations caused by aerosols have been found to be of the order of 21% and 17% on the irradiance on visible and near infrared respectively.

Single Aerosol Particle Studies Using Optical Trapping Raman And Cavity Ringdown Spectroscopy

NASA Astrophysics Data System (ADS)

Gong, Z.; Wang, C.; Pan, Y. L.; Videen, G.

2017-12-01

Due to the physical and chemical complexity of aerosol particles and the interdisciplinary nature of aerosol science that involves physics, chemistry, and biology, our knowledge of aerosol particles is rather incomplete; our current understanding of aerosol particles is limited by averaged (over size, composition, shape, and orientation) and/or ensemble (over time, size, and multi-particles) measurements. Physically, single aerosol particles are the fundamental units of any large aerosol ensembles. Chemically, single aerosol particles carry individual chemical components (properties and constituents) in particle ensemble processes. Therefore, the study of single aerosol particles can bridge the gap between aerosol ensembles and bulk/surface properties and provide a hierarchical progression from a simple benchmark single-component system to a mixed-phase multicomponent system. A single aerosol particle can be an effective reactor to study heterogeneous surface chemistry in multiple phases. Latest technological advances provide exciting new opportunities to study single aerosol particles and to further develop single aerosol particle instrumentation. We present updates on our recent studies of single aerosol particles optically trapped in air using the optical-trapping Raman and cavity ringdown spectroscopy.

Evolution of vehicle exhaust particles in the atmosphere.

PubMed

Canagaratna, Manjula R; Onasch, Timothy B; Wood, Ezra C; Herndon, Scott C; Jayne, John T; Cross, Eben S; Miake-Lye, Richard C; Kolb, Charles E; Worsnop, Douglas R

2010-10-01

Aerosol mass spectrometer (AMS) measurements are used to characterize the evolution of exhaust particulate matter (PM) properties near and downwind of vehicle sources. The AMS provides time-resolved chemically speciated mass loadings and mass-weighted size distributions of nonrefractory PM smaller than 1 microm (NRPM1). Source measurements of aircraft PM show that black carbon particles inhibit nucleation by serving as condensation sinks for the volatile and semi-volatile exhaust gases. Real-world source measurements of ground vehicle PM are obtained by deploying an AMS aboard a mobile laboratory. Characteristic features of the exhaust PM chemical composition and size distribution are discussed. PM mass and number concentrations are used with above-background gas-phase carbon dioxide (CO2) concentrations to calculate on-road emission factors for individual vehicles. Highly variable ratios between particle number and mass concentrations are observed for individual vehicles. NRPM1 mass emission factors measured for on-road diesel vehicles are approximately 50% lower than those from dynamometer studies. Factor analysis of AMS data (FA-AMS) is applied for the first time to map variations in exhaust PM mass downwind of a highway. In this study, above-background vehicle PM concentrations are highest close to the highway and decrease by a factor of 2 by 200 m away from the highway. Comparison with the gas-phase CO2 concentrations indicates that these vehicle PM mass gradients are largely driven by dilution. Secondary aerosol species do not show a similar gradient in absolute mass concentrations; thus, their relative contribution to total ambient PM mass concentrations increases as a function of distance from the highway. FA-AMS of single particle and ensemble data at an urban receptor site shows that condensation of these secondary aerosol species onto vehicle exhaust particles results in spatial and temporal evolution of the size and composition of vehicle exhaust PM on urban and regional scales.

Influence of haze pollution on water-soluble chemical species in PM2.5 and size-resolved particles at an urban site during fall.

PubMed

Yu, Geun-Hye; Zhang, Yan; Cho, Sung-Yong; Park, Seungshik

2017-07-01

To investigate the influence of haze on the chemical composition and formation processes of ambient aerosol particles, PM 2.5 and size-segregated aerosol particles were collected daily during fall at an urban site of Gwangju, Korea. During the study period, the total concentration of secondary ionic species (SIS) contributed an average of 43.9% to the PM 2.5 , whereas the contribution of SIS to the PM 2.5 during the haze period was 62.3%. The NO 3 - and SO 4 2- concentrations in PM 2.5 during the haze period were highly elevated, being 13.4 and 5.0 times higher than those during non-haze period, respectively. The PM, NO 3 - , SO 4 2- , oxalate, water-soluble organic carbon (WSOC), and humic-like substances (HULIS) had tri-modal size distributions peaks at 0.32, 1.0, and 5.2μm during the non-haze and haze periods. However, during the non-haze period they exhibited dominant size distributions at the condensation mode peaking at 0.32μm, while on October 21 when the heaviest haze event occurred, they had predominant droplet mode size distributions peaking at 1.00μm. Moreover, strong correlations of WSOC and HULIS with SO 4 2- , oxalate, and K + at particle sizes of <1.8μm indicate that secondary processes and emissions from biomass burning could be responsible for WSOC and HULIS formations. It was found that the factors affecting haze formation could be the local stable synoptic conditions, including the weak surface winds and high surface pressures, the long-range transportation of haze from eastern China and upwind regions of the Korean peninsula, as well as the locally emitted and produced aerosol particles. Copyright © 2016. Published by Elsevier B.V.

Can Aerosol Offset Urban Heat Island Effect?

NASA Astrophysics Data System (ADS)

Jin, M. S.; Shepherd, J. M.

2009-12-01

The Urban Heat Island effect (UHI) refers to urban skin or air temperature exceeding the temperatures in surrounding non-urban regions. In a warming climate, the UHI may intensify extreme heat waves and consequently cause significant health and energy problems. Aerosols reduce surface insolation via the direct effect, namely, scattering and absorbing sunlight in the atmosphere. Combining the National Aeronautics and Space Administration (NASA) AERONET (AErosol RObotic NETwork) observations over large cities together with Weather Research and Forecasting Model (WRF) simulations, we find that the aerosol direct reduction of surface insolation range from 40-100 Wm-2, depending on seasonality and aerosol loads. As a result, surface skin temperature can be reduced by 1-2C while 2-m surface air temperature by 0.5-1C. This study suggests that the aerosol direct effect is a competing mechanism for the urban heat island effect (UHI). More importantly, both aerosol and urban land cover effects must be adequately represented in meteorological and climate modeling systems in order to properly characterize urban surface energy budgets and UHI.

Linking Load, Fuel, and Emission Controls to Photochemical Production of Secondary Organic Aerosol from a Diesel Engine.

PubMed

Jathar, Shantanu H; Friedman, Beth; Galang, Abril A; Link, Michael F; Brophy, Patrick; Volckens, John; Eluri, Sailaja; Farmer, Delphine K

2017-02-07

Diesel engines are important sources of fine particle pollution in urban environments, but their contribution to the atmospheric formation of secondary organic aerosol (SOA) is not well constrained. We investigated direct emissions of primary organic aerosol (POA) and photochemical production of SOA from a diesel engine using an oxidation flow reactor (OFR). In less than a day of simulated atmospheric aging, SOA production exceeded POA emissions by an order of magnitude or more. Efficient combustion at higher engine loads coupled to the removal of SOA precursors and particle emissions by aftertreatment systems reduced POA emission factors by an order of magnitude and SOA production factors by factors of 2-10. The only exception was that the retrofitted aftertreatment did not reduce SOA production at idle loads where exhaust temperatures were low enough to limit removal of SOA precursors in the oxidation catalyst. Use of biodiesel resulted in nearly identical POA and SOA compared to diesel. The effective SOA yield of diesel exhaust was similar to that of unburned diesel fuel. While OFRs can help study the multiday evolution, at low particle concentrations OFRs may not allow for complete gas/particle partitioning and bias the potential of precursors to form SOA.

Aerosol Remote Sensing from Space - Where We Stand, Where We're Heading

NASA Technical Reports Server (NTRS)

Kahn, Ralph

2012-01-01

The MISR and MODIS instruments aboard the NASA Earth Observing System's Terra Satellite have been collecting data containing information about the state of Earth's atmosphere and surface for over twelve years. Among the retrieved quantities are the amount and type of wildfire smoke, desert dust, volcanic effluent, urban and industrial pollution particles, and other aerosols. Data from these instruments have been used to develop a global, monthly climatology of aerosol amount that is widely used as a constraint on climate models, including those used for the 2007 IPCC assessment report. However, the broad scientific challenges of understanding aerosol impacts on climate and health place different, and very exacting demands on our measurement capabilities. And these data sets, though much more advanced in many respects than previous aerosol data records, are imperfect. The next frontier in assessing aerosol radiative forcing of climate is aerosol type, and in particular, the absorption properties of major aerosol air masses. In this presentation, I will summarize current understanding of MISR and MODIS aerosol product strengths and limitations, discuss how they relate to the bigger aerosol science questions we must address, and give my view of the way forward.

Detecting Aerosol Effect on Deep Precipitation Systems: A Modeling Study

NASA Astrophysics Data System (ADS)

Li, X.; Tao, W.; Khain, A.; Kummerow, C.; Simpson, J.

2006-05-01

Urban cities produce high concentrations of anthropogenic aerosols. These aerosols are generally hygroscopic and may serve as Cloud Condensation Nuclei (CCN). This study focuses on the aerosol indirect effect on the deep convective systems over the land. These deep convective systems contribute to the majority of the summer time rainfall and are important for local hydrological cycle and weather forecast. In a companion presentation (Tao et al.) in this session, the mechanisms of aerosol-cloud-precipitation interactions in deep convective systems are explored using cloud-resolving model simulations. Here these model results will be analyzed to provide guidance to the detection of the impact of aerosols as CCN on summer time, deep convections using the currently available observation methods. The two-dimensional Goddard Cumulus Ensemble (GCE) model with an explicit microphysical scheme has been used to simulate the aerosol effect on deep precipitation systems. This model simulates the size distributions of aerosol particles, as well as cloud, rain, ice crystals, snow, graupel, and hail explicitly. Two case studies are analyzed: a midlatitude summer time squall in Oklahoma, and a sea breeze convection in Florida. It is shown that increasing the CCN number concentration does not affect the rainfall structure and rain duration in these two cases. The total surface rainfall rate is reduced in the squall case, but remains essentially the same in the sea breeze case. For the long-lived squall system with a significant portion of the stratiform rain, the surface rainfall PDF (probability density function) distribution is more sensitive to the change of the initial CCN concentrations compared with the total surface rainfall. The possibility of detecting the aerosol indirect effect in deep precipitation systems from the space is also studied in this presentation. The hydrometeors fields from the GCE model simulations are used as inputs to a microwave radiative transfer model. It is found that Tb at higher frequencies (35 GHz and 85 GHz) are quite sensitive to the CCN concentration variations. This is because the higher frequency brightness temperatures are sensitive to large, ice-phase particles. In a clean environment, the deep convections produce larger cloud particles. When these cloud particles are transported above the freezing level by strong updrafts, they form larger precipitable ice particles (snow, graupel and hail) compared with dirty environment simulations. These larger ice particles result in significantly colder brightness temperatures at high frequencies in the clean scenario simulations.

Morphologies and elemental compositions of local biomass burning particles at urban and glacier sites in southeastern Tibetan Plateau: Results from an expedition in 2010.

PubMed

Hu, Tafeng; Cao, Junji; Zhu, Chongshu; Zhao, Zhuzi; Liu, Suixin; Zhang, Daizhou

2018-07-01

Many studies indicate that the atmospheric environment over the southern part of the Tibetan Plateau is influenced by aged biomass burning particles that are transported over long distances from South Asia. However, our knowledge of the particles emitted locally (within the plateau region) is poor. We collected aerosol particles at four urban sites and one remote glacier site during a scientific expedition to the southeastern Tibetan Plateau in spring 2010. Weather and backward trajectory analyses indicated that the particles we collected were more likely dominated by particles emitted within the plateau. The particles were examined using an electron microscope and identified according to their sizes, shapes and elemental compositions. At three urban sites where the anthropogenic particles were produced mainly by the burning of firewood, soot aggregates were in the majority and made up >40% of the particles by number. At Lhasa, the largest city on the Tibetan Plateau, tar balls and mineral particles were also frequently observed because of the use of coal and natural gas, in addition to biofuel. In contrast, at the glacier site, large numbers of chain-like soot aggregates (~25% by number) were noted. The morphologies of these aggregates were similar to those of freshly emitted ones at the urban sites; moreover, physically or chemically processed ageing was rarely confirmed. These limited observations suggest that the biomass burning particles age slowly in the cold, dry plateau air. Anthropogenic particles emitted locally within the elevated plateau region may thus affect the environment within glaciated areas in Tibet differently than anthropogenic particles transported from South Asia. Copyright © 2018 Elsevier B.V. All rights reserved.

Field comparison of portable and stationary instruments for outdoor urban air exposure assessments

NASA Astrophysics Data System (ADS)

Viana, M.; Rivas, I.; Reche, C.; Fonseca, A. S.; Pérez, N.; Querol, X.; Alastuey, A.; Álvarez-Pedrerol, M.; Sunyer, J.

2015-12-01

The performance of three portable monitors (micro-aethalometer AE51, DiscMini, Dusttrak DRX) was assessed for outdoor air exposure assessment in a representative Southern European urban environment. The parameters evaluated were black carbon, particle number concentration, alveolar lung-deposited surface area, mean particle diameter, PM10, PM2.5 and PM1. The performance was tested by comparison with widely used stationary instruments (MAAP, CPC, SMPS, NSAM, GRIMM aerosol spectrometer). Results evidenced a good agreement between most portable and stationary instruments, with R2 values mostly >0.80. Relative differences between portable and stationary instruments were mostly <20%, and <10% between different units of the same instrument. The only exception was found for the Dusttrak DRX measurements, for which occasional concentration jumps in the time series were detected. Our results validate the performance of the black carbon, particle number concentration, particle surface area and mean particle diameter monitors as indicative instruments (tier 2) for outdoor air exposure assessment studies.

Physico-chemical characterization of African urban aerosols (Abidjan in Cote d'Ivoire and Cotonou in Benin) and their toxic effects in human bronchial epithelial cells during the dry season 2016.

NASA Astrophysics Data System (ADS)

Adon, Jacques; Liousse, Cathy; Yoboue, Veronique; Baeza, Armelle; Akpo, Aristide; Bahino, Julien; Chiron, Christelle; Galy-Lacaux, Corinne; Keita, Sékou

2017-04-01

This study is a contribution to the WP2-DACCIWA program with the aim to characterize particulate pollution on domestic fire site, traffic sites and waste burning site of two West-African capitals (Abidjan, Cote d'Ivoire and Cotonou, Benin) and to study aerosol biological impacts on lung inflammation. Such an impact is still largely unknown, especially for the particles emitted by intense African traffic sources and domestic fires. In this context, fundamental research of this study is centered on the following key scientific question: what is the link between aerosol size differentiated composition and inflammation markers for the main combustion sources prevailing in South West Africa during dry and wet seasons? To tackle this question, intensive campaigns in Abidjan and Cotonou have been conducted in July 2015, January and July 2016, and January 2017. In this paper, we will present our first results for the campaign of January 2016. In terms of aerosol size differentiated composition, main aerosol components (mass, black carbon, organic carbon, water soluble particles ...) were measured. We may notice that PM measured for all the sites is generally higher than WHO norms. Organic carbon and dust particles are the two more important contributors for the ultra-fine and fine particle sizes with more organic carbon in Abidjan and dust particles in Cotonou respectively. In terms of in vitro biological studies on sampled aerosols on these sites, size-fractionated PM from the different sampling sites were compared for their ability to induce a proinflammatory response characterized by the release of the cytokine IL-6 by human bronchial epithelial cells. PM from waste burning site did not induce significant IL-6 release whatever the size fraction whereas PM from domestic fire were the most reactive especially the ultra-fine fraction. Ultra-fine particles from traffic (Abidjan and Cotonou) always induced a dose-dependent IL-6 release. A tentative cross-analysis between physico-chemical and toxicological results will be proposed.

Characteristics and aging of traffic-derived particles in a highway tunnel at a coastal city in southern China.

PubMed

Hou, Cong; Shao, Longyi; Hu, Wei; Zhang, Daizhou; Zhao, Chengmei; Xing, Jiaoping; Huang, Xiaofeng; Hu, Min

2018-04-01

Road traffic is one of the major sources of particulate matters in the atmosphere. Tunnels provide a semi-closed place to measure traffic-derived particles before the particles were photo-chemically modified in the open air. In this study, aerosol particles were collected in a tunnel, and an urban site for comparison at a coastal city in south China. The particles were analyzed by using a transmission electron microscope coupled with an energy-dispersive X-ray spectrometry. There were four groups of particles according to sources: tailpipe-emitted particles, wear debris, road dust, and secondary particles. Tailpipe-emitted particles included soot, organic, and a part of sulfate and metal particles. Wear debris were characterized by their distinct metal components. Road dust was composed of mineral particles and fly ash. Secondary particles were some sulfate particles and mixture particles. Sulfate particles were further divided into two subtypes: with and without organic coating. Sulfate particles with organic coating accounted for 56.2% of total sulfate particles in the tunnel, while the percentage was 36.9% at the urban site, indicating that sulfate particles were more easily coated by organics in the tunnel than the urban site. However, the aging degree of sulfate particles in the tunnel was weaker than that at the urban site, which was attributed to the absence of photochemical reactions in the tunnel environment. Some mixture particles had a core-shell structure (C-S particles). The composition and morphologies of the cores of the C-S particles were similar to those of mineral, metal, and mixture particles. The shells of the C-S particles were mainly composed of organics. The C-S particles were more aged than the sulfate particles with coating in the tunnel environment, suggesting that mineral and metal components could efficiently enhance particle aging in the absence of photochemical reactions. Copyright © 2017 Elsevier B.V. All rights reserved.

Atmospheric particulate mercury at the urban and forest sites in central Poland.

PubMed

Siudek, Patrycja; Frankowski, Marcin; Siepak, Jerzy

2016-02-01

Particulate mercury concentrations were investigated during intensive field campaigns at the urban and forest sites in central Poland, between April 2013 and October 2014. For the first time, quantitative determination of total particulate mercury in coarse (PHg2.2) and fine (PHg0.7) aerosol samples was conducted in Poznań and Jeziory. The concentrations in urban fine and coarse aerosol fractions amounted to < MDL ± 77.1 pg m(-3) and < MDL ± 604.9 pg m(-3), respectively. Aerosol samples collected during the whole study period showed statistically significant differences for particulate mercury concentrations. A strong impact of meteorological conditions (wind velocity, air mass direction, air temperature, and precipitation amount) on particulate mercury concentrations was also observed. In particular, higher variation and concentration range of PHg0.7 and PHg2.2 was reported for wintertime measurements. An increase in atmospheric particulate mercury during the cold season in the study region indicated that coal combustion, i.e., residential and industrial heating, is the main contribution factor for the selected particle size modes. Coarse particulate Hg at the urban site during summer was mainly attributed to anthropogenic sources, with significant contribution from resuspension processes and long-range transport. The highest values of PHg0.7 and PHg2.2 were found during westerly and southerly wind events, reflecting local emission from highly polluted areas. The period from late fall to spring showed that advection from the southern part of Poland was the main factor responsible for elevated Hg concentrations in fine and coarse particles in the investigated region. Moreover, September 2013 could be given as an example of the influence of additional urban activities which occurred approx. 10 m from the sampling site-construction works connected with replacement of the road surface, asphalting, etc. The concentrations of particulate Hg (>600.0 pg m(-3)) were much higher than during the following months when any similar situation did not occur. Our investigations confirmed that Hg in urban aerosol samples was predominantly related to local industrial and commercial emissions, whereas the main source of Hg in particulate matter collected at the forest site was connected with regional anthropogenic processes. This paper provides the results of the first long-term measurements of size-fractionated particulate mercury conducted in central Poland, which could be an important insight into atmospheric Hg processes within such a scarcely investigated part of Europe.

Chemical and Microphysical Properties of Particles in Aged Forest Fire Plumes From Alaska and Western Canada Observed Over the Northeastern U.S.

NASA Astrophysics Data System (ADS)

Brock, C. A.; Wollny, A. G.; Cooper, O. R.; Fehsenfeld, F. C.; de Gouw, J. A.; Hudson, P. K.; Matthew, B. M.; Middlebrook, A. M.; Murphy, D. M.; Simsons, C.; Stohl, A.; Warneke, C.; Peltier, R.; Sulivan, A.; Weber, R. J.; Wilson, J. C.

2004-12-01

During the Intercontinental Transport and Chemical Transformation - New England Air Quality Study (ITCT-NEAQS 2004) in July and August 2004 several forest fires plumes were observed over the northeastern U.S. and southeastern Canada. Satellite data and trajectory analyses indicate that the plumes originated from forest fires burning in Alaska and western Canada. In-situ measurements of the aged forest fire smoke were made on board the NOAA WP-3D research aircraft during several flights over a period of 2 weeks. Concentrations of volatile organic compounds (VOCs) and the chemical composition of single aerosol particles in air masses containing forest fire smoke show significant differences compared to background air or to pollution from urban and industrial sources and unambiguously identify the smoke plumes. Particle size distributions from 0.004 to 8 um were measured with one second resolution in the aged forest fire smoke. The smoke was characterized by mass-weighted diameters between 0.6 and 1 um--much larger than secondary particles typical of urban and industrial sources. Particle volume concentrations were among the highest seen within the ITCT-NEAQS 2004 project, and regional visibility and air quality were significantly affected by the transported smoke. Quantitative compositional measurements were made of the non-refractory fraction of submicron particles, as well as of submicron inorganic ionic compounds and water soluble organic mass, within the forest fire plumes. The submicron aerosol particles in the biomass plumes were largely carbonaceous with very little sulfate, ammonium, or nitrate. A fraction of this carbonaceous material was soluble in water and likely contained oxygenated organic species.

An operational MODIS aerosol retrieval algorithm at high spatial resolution, and its application over a complex urban region

NASA Astrophysics Data System (ADS)

Wong, Man Sing; Nichol, Janet E.; Lee, Kwon Ho

2011-03-01

Aerosol retrieval algorithms for the MODerate Resolution Imaging Spectroradiometer (MODIS) have been developed to estimate aerosol and microphysical properties of the atmosphere, which help to address aerosol climatic issues at global scale. However, higher spatial resolution aerosol products for urban areas have not been well-researched mainly due to the difficulty of differentiating aerosols from bright surfaces in urban areas. Here, an aerosol retrieval algorithm using the MODIS 500-m resolution bands is described, to retrieve aerosol properties over Hong Kong and the Pearl River Delta region. The rationale of our technique is to first estimate the aerosol reflectances by decomposing the top-of-atmosphere reflectances from surface reflectances and Rayleigh path reflectances. For the determination of surface reflectances, a Minimum Reflectance Technique (MRT) is used, and MRT images are computed for different seasons. For conversion of aerosol reflectance to aerosol optical thickness (AOT), comprehensive Look Up Tables specific to the local region are constructed, which consider aerosol properties and sun-viewing geometry in the radiative transfer calculations. Four local aerosol types, namely coastal urban, polluted urban, dust, and heavy pollution, were derived using cluster analysis on 3 years of AERONET measurements in Hong Kong. The resulting 500 m AOT images were found to be highly correlated with ground measurements from the AERONET (r2 = 0.767) and Microtops II sunphotometers (r2 = 0.760) in Hong Kong. This study further demonstrates the application of the fine resolution AOT images for monitoring inter-urban and intra-urban aerosol distributions and the influence of trans-boundary flows. These applications include characterization of spatial patterns of AOT within the city, and detection of regional biomass burning sources.

Semi-continuous measurement of PM 2.5 ionic composition at several rural locations in the United States

NASA Astrophysics Data System (ADS)

Lee, Taehyoung; Yu, Xiao-Ying; Kreidenweis, Sonia M.; Malm, William C.; Collett, Jeffrey L.

To improve understanding of the nature and variability of the ionic fraction of atmospheric fine aerosol particles in non-urban environments, one to two month measurement campaigns were conducted at several rural locations in the United States. Study sites included Yosemite National Park (NP) (July-September 2002), Bondville, Illinois (February 2003), San Gorgonio Wilderness Area, California (April and July 2003), Grand Canyon National Park, Arizona (May 2003), Brigantine National Wildlife Refuge (NWR), New Jersey (November 2003), and Great Smoky Mountains National Park, Tennessee (July/August 2004). PM 2.5 ion composition was measured at 15 min intervals using a Particle-Into-Liquid-Sampler (PILS) coupled to two ion chromatographs. Comparisons of PILS measurements with parallel traditional 24 h denuder/filter-pack measurements reveal generally good agreement between the two techniques for major species, although PILS measurements of PM 2.5 NH 4+ are biased low by approximately 4-20%. High time resolution PILS aerosol concentration measurements provide better estimates of the range of aerosol concentrations at the rural locations than the 24 h integrated filter data. Ratios of peak 15 min to 24 h nitrate concentrations, for example, ranged from 1.7 at Brigantine NWR to 7.0 at Great Smoky Mountains NP. A strong influence of diurnal upslope/downslope transport patterns was observed on aerosol concentrations at several locations, including Yosemite NP, San Gorgonio Wilderness Area, and Great Smoky Mountains NP, with peak concentrations typically occurring during afternoon upslope transport. High time resolution aerosol composition measurements also provide new insight into relationships between individual aerosol species and the influence of environmental conditions on aerosol composition. Observations at several locations revealed important information about mechanisms of particle nitrate formation. At Yosemite and Grand Canyon National Parks, for example, evidence was observed for reaction of nitric acid or its precursors with sea salt or soil dust. Observations from several sites also revealed the importance of aerosol acidity (Great Smoky Mountains NP, Bondville) and temperature/humidity (San Gorgonio) on fine particle ammonium nitrate formation.

Characterization of traffic-related ambient fine particulate matter (PM2.5) in an Asian city: Environmental and health implications

NASA Astrophysics Data System (ADS)

Zhang, Zhi-Hui; Khlystov, Andrey; Norford, Leslie K.; Tan, Zhen-Kang; Balasubramanian, Rajasekhar

2017-07-01

Vehicular traffic emission is an important source of particulate pollution in most urban areas. The detailed chemical speciation of traffic-related PM2.5 (fine particles) is relatively sparse in the literature, especially in Asian cities. To fill this knowledge gap, we carried out an intensive field study in Singapore from November 2015 to February 2016. PM2.5 samples were collected concurrently at a typical roadside microenvironment and at an urban background site. A detailed chemical speciation of PM2.5 samples was conducted to gain insights into the emission characteristics of traffic-related fine aerosols. Analyses of diagnostic ratios and molecular markers of selected chemical species were explored for source attribution of different classes of chemical constituents in traffic-related PM2.5. The human health risk due to inhalation of the particulate-bound PAHs (polycyclic aromatic hydrocarbons) and toxic trace elements was estimated for both adults and children. The overall results of the study indicate that gasoline-powered vehicles make a higher contribution to traffic-related fine aerosol components such as organic carbon (OC), particle-bound PAHs and particulate ammonium than that of diesel-powered vehicles. However, both types of vehicles contribute to traffic-related EC emissions significantly. The combustion of petroleum fuels and lubricating oil make significant contributions to the emission of n-alkanes and hopanes into the urban atmosphere, respectively. The study further reveals that some toxic trace elements are emitted from non-exhaust sources and that aromatic acids represent an important component of secondary organic aerosols. The emission of toxic trace elements from non-exhaust sources is of particular concern as they could pose a higher carcinogenic risk to both adults and children than other chemical species.

Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS

NASA Astrophysics Data System (ADS)

Hamilton, J. F.; Webb, P. J.; Lewis, A. C.; Hopkins, J. R.; Smith, S.; Davy, P.

2004-08-01

Partially oxidised organic compounds associated with PM2.5 aerosol collected in London, England, have been analysed using direct thermal desorption coupled to comprehensive gas chromatography-time of flight mass spectrometry (GCXGC-TOF/MS). Over 10000 individual organic components were isolated from around 10µg of aerosol material in a single procedure and with no sample pre-treatment. Chemical functionalities observed using this analytical technique ranged from alkanes to poly-oxygenated species. The chemical band structures commonly used in GCXGC for group type identifications overlap for this sample type, and have required mass spectrometry as an additional level of instrument dimensionality. An investigation of oxygenated volatile organic compounds (o-VOC) contained within urban aerosol has been performed and in a typical sample around 130 o-VOCs were identified based on retention behaviour and spectral match. In excess of 100 other oxygenated species were also observed but lack of mass spectral library or pure components prevents positive identification. Many of the carbonyl species observed could be mechanistically linked to gas phase aromatic hydrocarbon oxidation and there is good agreement in terms of speciation between the urban samples analysed here and those degradation products observed in smog chamber experiments of aromatic oxidation. The presence of partially oxidised species such as linear chain aldehydes and ketones and cyclic products such as furanones suggests that species generated early in the oxidative process may undergo gas to particle partitioning despite their relatively high volatility.

Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS

NASA Astrophysics Data System (ADS)

Hamilton, J.; Webb, P.; Lewis, A.; Hopkins, J.; Smith, S.; Davy, P.

2004-03-01

Partially oxidised organic compounds associated with PM2.5 aerosol collected in London, England, have been analysed using direct thermal desorption coupled to comprehensive gas chromatography-time of flight mass spectrometry (GCXGC-OF/MS). Over 10 000 individual organic components were isolated from around 10 μg of aerosol material in a single procedure and with no sample pre-treatment. Chemical functionalities observed using this analytical technique ranged from alkanes to poly-oxygenated species. The chemical band structures commonly used in GCXGC for group type identifications overlap for this sample type, and have required mass spectrometry as an additional level of instrument dimensionality. An investigation of oxygenated volatile organic compounds (o-VOC) contained within urban aerosol has been performed and in a typical sample around 130 o-VOCs were identified based on retention behaviour and spectral match. In excess of 100 other oxygenated species were also observed but lack of mass spectral library or pure components prevents positive identification. Many of the carbonyl species observed could be mechanistically linked to gas phase aromatic hydrocarbon oxidation and there is good agreement in terms of speciation between the urban samples analysed here and those degradation products observed in smog chamber experiments of aromatic oxidation. The presence of partially oxidised species such as linear chain aldehydes and ketones and cyclic products such as furanones suggests that species generated relatively early in the oxidative process may undergo gas to particle partitioning despite their relatively high volatility.

Introducing MISR Version 23: Resolution and Content Improvements to MISR Aerosol and Land Surface Product

NASA Astrophysics Data System (ADS)

Garay, M. J.; Bull, M. A.; Witek, M. L.; Diner, D. J.; Seidel, F.

2017-12-01

Since early 2000, the Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has been providing operational Level 2 (swath-based) aerosol optical depth (AOD) and particle property retrievals at 17.6 km spatial resolution and atmospherically corrected land surface products at 1.1 km resolution. A major, multi-year development effort has led to the release of updated operational MISR Level 2 aerosol and land surface retrieval products. The spatial resolution of the aerosol product has been increased to 4.4 km, allowing more detailed characterization of aerosol spatial variability, especially near local sources and in urban areas. The product content has been simplified and updated to include more robust measures of retrieval uncertainty and other fields to benefit users. The land surface product has also been updated to incorporate the Version 23 aerosol product as input and to improve spatial coverage, particularly over mountainous terrain and snow/ice-covered surfaces. We will describe the major upgrades incorporated in Version 23, present validation of the aerosol product, and describe some of the applications enabled by these product updates.

CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: Seasonal and diel variations and impact of anthropogenic emissions

DOE PAGES

Thalman, Ryan; de Sá, Suzane S.; Palm, Brett B.; ...

2017-10-05

During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60km downwind of the city of Manaus, Brazil, in central Amazonia for one year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely duemore » to an increase in sulfate volume fraction. Also, during both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ~0.15 is consistent with the largely uniform and high O:C value (~0.8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O:C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O:C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF analysis of AMS spectra, were estimated through multi-variable linear regression. For the SOA factors, the variation of the κ value with O:C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O:C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O:C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O:C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase of κorg with O:C, as observed during this and earlier field studies. Our finding helps better understand and reconcile the differences in the relationships between κorg and O:C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.« less

CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: Seasonal and diel variations and impact of anthropogenic emissions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thalman, Ryan; de Sá, Suzane S.; Palm, Brett B.

During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60km downwind of the city of Manaus, Brazil, in central Amazonia for one year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely duemore » to an increase in sulfate volume fraction. Also, during both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ~0.15 is consistent with the largely uniform and high O:C value (~0.8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O:C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O:C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF analysis of AMS spectra, were estimated through multi-variable linear regression. For the SOA factors, the variation of the κ value with O:C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O:C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O:C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O:C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase of κorg with O:C, as observed during this and earlier field studies. Our finding helps better understand and reconcile the differences in the relationships between κorg and O:C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.« less

Multiday production of condensing organic aerosol mass in urban and forest outflow

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee-Taylor, J.; Hodzic, A.; Madronich, S.

2015-01-16

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

Multiday production of condensing organic aerosol mass in urban and forest outflow

DOE PAGES

Lee-Taylor, J.; Hodzic, A.; Madronich, S.; ...

2015-01-16

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. Here, the results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

Aerosol Chemistry over a High Altitude Station at Northeastern Himalayas, India

PubMed Central

Chatterjee, Abhijit; Adak, Anandamay; Singh, Ajay K.; Srivastava, Manoj K.; Ghosh, Sanjay K.; Tiwari, Suresh; Devara, Panuganti C. S.; Raha, Sibaji

2010-01-01

Background There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. Methodology/Principal Findings An extensive aerosol sampling program was conducted in Darjeeling (altitude ∼2200 meter above sea level (masl), latitude 27°01′N and longitude 88°15′E), a high altitude station in northeastern Himalayas, during January–December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5±20.8 µg m−3 and 19.6±11.1 µg m−3 respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH4NO3 in fine mode aerosol during winter and as NaNO3 in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO2 during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO4 2− in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. Conclusions/Significance The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over northeastern Himalayas, and should be useful to policy makers in making control strategies. PMID:20585397

Aerosol chemistry over a high altitude station at northeastern Himalayas, India.

PubMed

Chatterjee, Abhijit; Adak, Anandamay; Singh, Ajay K; Srivastava, Manoj K; Ghosh, Sanjay K; Tiwari, Suresh; Devara, Panuganti C S; Raha, Sibaji

2010-06-16

There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. An extensive aerosol sampling program was conducted in Darjeeling (altitude approximately 2200 meter above sea level (masl), latitude 27 degrees 01'N and longitude 88 degrees 15'E), a high altitude station in northeastern Himalayas, during January-December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5+/-20.8 microg m(-3) and 19.6+/-11.1 microg m(-3) respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH(4)NO(3) in fine mode aerosol during winter and as NaNO(3) in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO(2) during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO(4)(2-) in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over northeastern Himalayas, and should be useful to policy makers in making control strategies.

In situ airborne measurements of aerosol optical properties during photochemical pollution events

NASA Astrophysics Data System (ADS)

Mallet, M.; van Dingenen, R.; Roger, J. C.; Despiau, S.; Cachier, H.

2005-02-01

Dry aerosol optical properties (scattering, absorbing coefficients, and single scattering albedo) were derived from in situ airborne measurements during two photochemical pollution events (25 and 26 June) observed during the Experience sur Site pour Contraindre les Modeles de Pollution atmospherique et de Transport d'Emissions (ESCOMPTE) experiment. Two flights were carried out during daytime (one during the morning and one at noon) over a domain, allowing the investigation of how an air pollution event affects the particle optical properties. Both horizontal distribution and vertical profiles are presented. Results from the horizontal mapping show that plumes of enhanced scattering and absorption are formed in the planetary boundary layer (PBL) during the day in the sea breeze-driven outflow of the coastal urban-industrial area of Marseille-Fos de Berre. The domain-averaged scattering coefficient (at 550 nm) over land σs changes from 35 (28) Mm-1 during land breeze to 63 (43) Mm-1 during sea breeze on 25 June (26 June), with local maxima reaching > 100 Mm-1. The increase in the scattering coefficient is associated with new particle formation, indicative of secondary aerosol formation. Simultaneously, the domain-averaged absorption coefficient increases from 5.6 (3.4) Mm-1 to 9.3 (8.0) Mm-1. The pollution plume leads to strong gradients in the single scattering albedo ωo over the domain studied, with local values as low as 0.73 observed inside the pollution plume. The role of photochemistry and secondary aerosol formation during the 25 June case is shown to increase ωo and to make the aerosol more `reflecting' while the plume moves away from the sources. The lower photochemical activity, observed in the 26 June case, induces a relatively higher contribution of black carbon, making the aerosol more absorbing. Results from vertical profiles at a single near-urban location in the domain indicate that the changes in optical properties happen almost entirely within the PBL. No significant variation of σs, σa, and ωo is observed in the upper layer (1-3 km), where the aerosol optical properties are considered to be well mixed.

Microfluidic electrochemical sensor for on-line monitoring of aerosol oxidative activity.

PubMed

Sameenoi, Yupaporn; Koehler, Kirsten; Shapiro, Jeff; Boonsong, Kanokporn; Sun, Yele; Collett, Jeffrey; Volckens, John; Henry, Charles S

2012-06-27

Particulate matter (PM) air pollution has a significant impact on human morbidity and mortality; however, the mechanisms of PM-induced toxicity are poorly defined. A leading hypothesis states that airborne PM induces harm by generating reactive oxygen species in and around human tissues, leading to oxidative stress. We report here a system employing a microfluidic electrochemical sensor coupled directly to a particle-into-liquid sampler (PILS) system to measure aerosol oxidative activity in an on-line format. The oxidative activity measurement is based on the dithiothreitol (DTT) assay, where, after being oxidized by PM, the remaining reduced DTT is analyzed by the microfluidic sensor. The sensor consists of an array of working, reference, and auxiliary electrodes fabricated in a poly(dimethylsiloxane)-based microfluidic device. Cobalt(II) phthalocyanine-modified carbon paste was used as the working electrode material, allowing selective detection of reduced DTT. The electrochemical sensor was validated off-line against the traditional DTT assay using filter samples taken from urban environments and biomass burning events. After off-line characterization, the sensor was coupled to a PILS to enable on-line sampling/analysis of aerosol oxidative activity. Urban dust and industrial incinerator ash samples were aerosolized in an aerosol chamber and analyzed for their oxidative activity. The on-line sensor reported DTT consumption rates (oxidative activity) in good correlation with aerosol concentration (R(2) from 0.86 to 0.97) with a time resolution of approximately 3 min.

Elemental composition of Arctic soils and aerosols in Ny-Ålesund measured using laser-induced breakdown spectroscopy

NASA Astrophysics Data System (ADS)

Kim, Gibaek; Yoon, Young-Jun; Kim, Hyun-A.; Cho, Hee-joo; Park, Kihong

2017-08-01

Two laser-induced breakdown spectroscopy (LIBS) systems (soil LIBS and aerosol LIBS) were used to determine the elemental composition of soils and ambient aerosols less than 2.5 μm in Ny-Ålesund, Svalbard (the world's most northerly human settlement). For soil LIBS measurements, matrix effects such as moisture content, soil grain size, and surrounding gas on the LIBS response were minimized. When Ar gas was supplied onto the soil sample surfaces, a significant enhancement in LIBS emission lines was observed. Arctic soil samples were collected at 10 locations, and various elements (Al, Ba, C, Ca, Cu, Fe, H, K, Mg, Mn, N, Na, O, Pb, and Si) were detected in soils. The elemental distribution in arctic soils was clearly distinguishable from those in urban and abandoned mining soils in Korea. Moreover, the concentrations of most of anthropogenic metals were fairly low, and localized sources in extremely close proximity affected the elevated level of Cu in the soil samples derived from Ny-Ålesund. The number of elements detected in aerosols (C, Ca, H, K, Mg, Na, and O) was lower than those determined in soils. The elements in aerosols can mainly originate from minerals and sea salts. The elemental distribution in aerosols was also clearly distinguishable from that in soils, suggesting that the resuspension of local soil particles by wind erosion into aerosols was minimal. The daily variation of particle number concentration (RSD = 71%) and the elements in aerosols (RSD = 25%) varied substantially, possibly due to fluctuating air masses and meteorological conditions.

Chemical composition and mass closure of ambient coarse particles at traffic and urban-background sites in Thessaloniki, Greece.

PubMed

Grigoratos, Theodoros; Samara, Constantini; Voutsa, Dimitra; Manoli, Evangelia; Kouras, Athanasios

2014-06-01

Concentrations and chemical composition of the coarse particle fraction (PMc) were investigated at two urban sites in the city of Thessaloniki, Greece, through concurrent sampling of PM10 and PM2.5 during the warm and the cold months of the year. PMc levels at the urban-traffic site (UT) were among the highest found in literature worldwide exhibiting higher values in the cold period. PMc levels at the urban-background site (UB) were significantly lower exhibiting a reverse seasonal trend. Concentration levels of minerals and most trace metals were also higher at the UT site suggesting a stronger impact from traffic-related sources (road dust resuspension, brake and tire abrasion, road wear). According to the chemical mass closure obtained, minerals (oxides of Si, Al, Ca, Mg, Fe, Ti, and K) dominated the PMc profile, regardless of the site and the period, with organic matter and secondary inorganic aerosols (mainly nitrate) also contributing considerably to the PMc mass, particularly in the warm period. The influence of wind speed to dilution and/or resuspension of coarse particles was investigated. The source of origin of coarse particles was also investigated using surface wind data and atmospheric back-trajectory modeling. Finally, the contribution of resuspension to PMc levels was estimated for air quality management perspectives.

The Regional Environmental Impacts of Atmospheric Aerosols over Egypt

NASA Astrophysics Data System (ADS)

Zakey, Ashraf; Ibrahim, Alaa

2015-04-01

Identifying the origin (natural versus anthropogenic) and the dynamics of aerosols over Egypt at varying temporal and spatial scales provide valuable knowledge on the regional climate impacts of aerosols and their ultimate connections to the Earth's regional climate system at the MENA region. At regional scale, Egypt is exposed to air pollution with levels exceeding typical air-quality standards. This is particularly true for the Nile Delta region, being at the crossroads of different aerosol species originating from local urban-industrial and biomass-burning activities, regional dust sources, and European pollution from the north. The Environmental Climate Model (EnvClimA) is used to investigate both of the biogenic and anthropogenic aerosols over Egypt. The dominant natural aerosols over Egypt are due to the sand and dust storms, which frequently occur during the transitional seasons (spring and autumn). In winter, the maximum frequency reaches 2 to 3 per day in the north, which decreases gradually southward with a frequency of 0.5-1 per day. Monitoring one of the most basic aerosol parameters, the aerosol optical depth (AOD), is a main experimental and modeling task in aerosol studies. We used the aerosol optical depth to quantify the amount and variability of aerosol loading in the atmospheric column over a certain areas. The aerosols optical depth from the model is higher in spring season due to the impacts of dust activity over Egypt as results of the westerly wind, which carries more dust particles from the Libyan Desert. The model result shows that the mass load of fine aerosols has a longer life-time than the coarse aerosols. In autumn season, the modelled aerosol optical depth tends to increase due to the biomass burning in the delta of Egypt. Natural aerosol from the model tends to scatter the solar radiation while most of the anthropogenic aerosols tend to absorb the longwave solar radiation. The overall results indicate that the AOD is lowest in winter due to airborne particles washed out by rain events. Conversely, the AOD increases in summer because particle accumulation is favored by the absence of precipitation during this season. Moreover, in summer, photochemical processes in the atmosphere lead to slight increases in the values of aerosol optical characteristics, despite lower wind speeds [hence less wind-blown dust] relative to other seasons. This study has been conducted under the PEER 2-239 research project titled "the Impact of Biogenic and Anthropogenic Atmospheric Aerosols to Climate in Egypt". Project website: CleanAirEgypt.org

Particulate air pollution from combustion and construction in coastal and urban areas of China.

PubMed

Chen, Bing; Chen, Jinsheng; Zhao, Jinping; Zhang, Fuwang

2011-11-01

In China, the areas that are undergoing rapid urban growth are faced with increasingly more complicated air pollution problems. Sources of air pollution need to be identified and their contributions quantified. In this study, PM2.5 (particulate matter with aerodynamic diameters < or =2.5 microm), PM2.5-10 (particulate matter with aerodynamic diameters 2.5-10 microm), organic carbon (OC), and elemental carbon (EC) concentrations were measured from April to July 2009 at four selected areas in Xiamen (the downtown area, an industrial park, a suburb, and one remote site). The contributions of carbonaceous aerosols to PM2.5 and PM2.5-10 were 20-30% and 10-20%, respectively, indicating that finer particles contained more carbonaceous aerosols. The EC concentrations in PM2.5 at the downtown, industrial, suburb, and remote sites were 2.16 +/- 0.61, 2.05 +/- 0.45, 1.69 +/- 0.54, and 0.65 +/- 0.43 microg m-3, respectively, showing a decrease from the urban and industrial hotspots to the surrounding areas. These data show that carbonaceous aerosols emitted from the combustion of fossil fuels in urban and industrial hotspots influence air quality at the regional scale. Higher levels of PM2.5 and PM2.5-10 were observed at the suburb site compared to the urban and industrial sites. Peak EC concentrations in PM2.5 were observed during the morning and evening rush hours. However, peak PM2.5 levels at the suburb site were observed around noon, which coincides with construction work hours, instead of the morning and evening rush hours when emissions from combustion dominated. These findings indicate that both fuel combustion and construction have exacerbated air pollution in coastal and urban areas in China.

Coagulation effect on the activity size distributions of long lived radon progeny aerosols and its application to atmospheric residence time estimation techniques.

PubMed

Anand, S; Mayya, Y S

2015-03-01

The long lived naturally occurring radon progeny species in the atmosphere, namely (210)Pb, (210)Bi and (210)Po, have been used as important tracers for understanding the atmospheric mixing processes and estimating aerosol residence times. Several observations in the past have shown that the activity size distribution of these species peaks at larger particle sizes as compared to the short lived radon progeny species - an effect that has been attributed to the process of coagulation of the background aerosols to which they are attached. To address this issue, a mathematical equation is derived for the activity-size distribution of tracer species by formulating a generalized distribution function for the number of tracer atoms present in coagulating background particles in the presence of radioactive decay and removal. A set of these equations is numerically solved for the progeny chain using Fuchs coagulation kernel combined with a realistic steady-state aerosol size spectrum that includes nucleation, accumulation and coarse mode components. The important findings are: (i) larger shifts in the modal sizes of (210)Pb and (210)Po at higher aerosol concentrations such as that found in certain Asian urban regions (ii) enrichment of tracer specific activity on particles as compared to that predicted by pure attachment laws (iii) sharp decline of daughter-to-parent activity ratios for decreasing particle sizes. The implication of the results to size-fractionated residence time estimation techniques is highlighted. A coagulation corrected graphical approach is presented for estimating the residence times from the size-segregated activity ratios of (210)Bi and (210)Po with respect to (210)Pb. The discrepancy between the residence times predicted by conventional formula and the coagulation corrected approach for specified activity ratios increases at higher atmospheric aerosol number concentrations (>10(10) #/m(3)) for smaller sizes (<1 μm). The results are further discussed. Copyright © 2014 Elsevier Ltd. All rights reserved.

Temporal variability in aerosol composition at an urban site, Varanasi in the eastern Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Ram, Kirpa; Norra, Stefan; Yuan, Chen; Venkata Satish, Rangu; Rastogi, Neeraj

2017-04-01

PM2.5 aerosol samples (n=31) were collected from an urban site, Varanasi (25° 28'N, 83°0' E) in the eastern Indo-Gangetic Plain during May 2015 to March 2016 using a mini-volume sampler (Leckel GmbH, Germany) at a flow rate of 200 l/hr. The PM2.5 samples were integrated for 7 days and were analyzed for organic and elemental carbon (OC & EC), water-soluble OC (WSOC), organic and inorganic nitrogen (ON & IN) and water-soluble inorganic species (WSIS) to study the geochemical behavior of aerosols. The mass concentration of OC and EC varies from 4.2 to 105.2 (average: 32.8) μg m-3 and 1.2 to 7.0 (average: 4.6) μg m-3 during the study period with total carbonaceous aerosols (TCA=1.6*OC+EC), on an average, accounting for ˜59% of PM2.5 mass. Relatively high WSOC/OC ratio (average: 0.55±0.18; range 0.18-0.86) indicate a significant contribution from the secondary organic aerosols at Varanasi. The concentration of ON varies from less than detection limit to 5.3 (average: 2.4) μg m-3 which contribute to ˜12% of WSOC highlighting the presence of nitro-organic compounds in aerosols at Varanasi. The average WSIS contribution to PM2.5 is only 17% with a strong seasonal variability (range: 4-36%). Generally, carbonaceous and inorganic aerosol concentration is higher during winter, fall and post-monsoon that those in the summer when dust aerosol contribution is significant (as high as 75% of PM2.5 mass). This study highlights the role of nitro-organic compounds in secondary organic aerosols which is lacking in Indian aerosols. Furthermore, these aerosol samples could be very important for the study of particle morphology and composition using scanning-electron Microscope-Energy Dispersive X-ray due to lower impaction in the mini-volume sampler.

Dust Concentrations and Composition During African Dust Incursions in the Caribbean Region

NASA Astrophysics Data System (ADS)

Mayol-Bracero, O. L.; Santos-Figueroa, G.; Morales-Garcia, F.

2016-12-01

The World Health Organization (WHO) indicates that exposure to PM10 concentrations higher than 50 µg/m³ 24-hour mean in both developed and developing countries could have an adverse impact on public health. Recent studies showed that in the Caribbean region the PM10 concentrations often exceed the WHO guidelines for PM10. These exceedances are largely driven by the presence of African Dust particles that reach the Caribbean region every year during the summer months. These dust particles also influence the Earth's radiative budget directly by scattering solar radiation in the atmosphere and indirectly by affecting cloud formation and, thus, cloud albedo. In order to have a better understanding of the impacts of African Dust on public health and climate, we determine the concentration of dust particles, the carbonaceous fraction (total, elemental and organic carbon: TC, EC, and OC) and water-soluble ions (e.g., Na+, Cl-, Ca+2, NH4+, SO4-2) of aerosol samples in the presence and absence of African Dust. Samples were collected using a Hi-Vol and Stacked-Filter Units for the sampling of total suspended particles (TSP) at two stations in Puerto Rico: a marine site located at Cabezas de San Juan (CSJ) Nature Reserve, in Fajardo, and an urban site located at the University of Puerto Rico, in San Juan. The presence of African Dust was supported with Saharan Air Layer (SAL) imagery and with the results from the air mass backward trajectories calculated with the NOAA Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT). Preliminary results showed that the total mass concentration of aerosols obtained at the urban site is about two times that at the marine site for SFU samples during African Dust incursions. The average dust concentration obtained at CSJ for Hi Vol samples was 22 µg/m³ during the summer 2015. African Dust concentrations, TC, EC, OC, and ionic speciation results for the marine and urban sites will be presented at the conference.

Aerosol mass spectrometry: particle-vaporizer interactions and their consequences for the measurements

NASA Astrophysics Data System (ADS)

Drewnick, F.; Diesch, J.-M.; Faber, P.; Borrmann, S.

2015-09-01

The Aerodyne aerosol mass spectrometer (AMS) is a frequently used instrument for on-line measurement of the ambient sub-micron aerosol composition. With the help of calibrations and a number of assumptions on the flash vaporization and electron impact ionization processes, this instrument provides robust quantitative information on various non-refractory ambient aerosol components. However, when measuring close to certain anthropogenic or marine sources of semi-refractory aerosols, several of these assumptions may not be met and measurement results might easily be incorrectly interpreted if not carefully analyzed for unique ions, isotope patterns, and potential slow vaporization associated with semi-refractory species. Here we discuss various aspects of the interaction of aerosol particles with the AMS tungsten vaporizer and the consequences for the measurement results: semi-refractory components - i.e., components that vaporize but do not flash-vaporize at the vaporizer and ionizer temperatures, like metal halides (e.g., chlorides, bromides or iodides of Al, Ba, Cd, Cu, Fe, Hg, K, Na, Pb, Sr, Zn) - can be measured semi-quantitatively despite their relatively slow vaporization from the vaporizer. Even though non-refractory components (e.g., NH4NO3 or (NH4)2SO4) vaporize quickly, under certain conditions their differences in vaporization kinetics can result in undesired biases in ion collection efficiency in thresholded measurements. Chemical reactions with oxygen from the aerosol flow can have an influence on the mass spectra for certain components (e.g., organic species). Finally, chemical reactions of the aerosol with the vaporizer surface can result in additional signals in the mass spectra (e.g., WO2Cl2-related signals from particulate Cl) and in conditioning or contamination of the vaporizer, with potential memory effects influencing the mass spectra of subsequent measurements. Laboratory experiments that investigate these particle-vaporizer interactions are presented and are discussed together with field results, showing that measurements of typical continental or urban aerosols are not significantly affected, while measurements of semi-refractory aerosol in the laboratory, close to anthropogenic sources or in marine environments, can be biased by these effects.

Chemical characterization and source apportionment of fine particulate matter in Yangzhou, China, using offline aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Li, L.; Ge, X.; Xu, J.; Ye, Z.

2016-12-01

In recent years, Aerodyne Aerosol Mass Spectrometer (AMS) has been widely used for online and real-time monitoring of fine aerosol particles all over the world. However, due to the high cost and complex maintenance, the AMS was typically deployed for short-term intense field measurements, limiting its ability in elucidating the long-term behaviors and dominant sources of regional fine particles (PM2.5). In this study, we collected daily PM2.5 filter samples across a relatively long period (November 2015 to April 2016, in total >100 samples) using a high-volume sampler, in urban Yangzhou - a city in the Yangtze River Delta region, China. These samples were analyzed by using a suite of analytical techniques, for the water-soluble inorganic ions (WSIs), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and total nitrogen (TN), trace metal elements, etc. More importantly, an Aerodyne soot particle aerosol mass spectrometer (SP-AMS) was for the first time introduced for the offline characterization of the PM2.5 samples collected in this region. In particular, Positive matrix factorization was conducted on the SP-AMS determined water-soluble fraction of organic aerosols (WSOA), and three distinct sources were separated, including a primary OA (POA), a less oxygenated OA (LOOA), and a more oxygenated OA (MOOA). Chemical characteristics and evolution processes of these OA subcomponents were further discussed. Our results are useful for the air pollution management in the YRD region, and the technique developed can be applied elsewhere as well.

Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

NASA Astrophysics Data System (ADS)

Xu, L.; Williams, L. R.; Young, D. E.; Allan, J. D.; Coe, H.; Massoli, P.; Fortner, E.; Chhabra, P.; Herndon, S.; Brooks, W. A.; Jayne, J. T.; Worsnop, D. R.; Aiken, A. C.; Liu, S.; Gorkowski, K.; Dubey, M. K.; Fleming, Z. L.; Visser, S.; Prévôt, A. S. H.; Ng, N. L.

2016-02-01

The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.

Characterization of Fine Particulate Matter (PM) and Secondary PM Precursor Gases in the Mexico City Metropolitan Area

DOE Office of Scientific and Technical Information (OSTI.GOV)

Molina, Luisa T.; Molina, Mario J.; Volkamer, Rainer

2008-10-31

This project was one of three collaborating grants funded by DOE/ASP to characterize the fine particulate matter (PM) and secondary PM precursors in the Mexico City Metropolitan Area (MCMA) during the MILAGRO Campaign. The overall effort of MCMA-2006, one of the four components, focused on i) examination of the primary emissions of fine particles and precursor gases leading to photochemical production of atmospheric oxidants and secondary aerosol particles; ii) measurement and analysis of secondary oxidants and secondary fine PM production, with particular emphasis on secondary organic aerosol (SOA), and iii) evaluation of the photochemical and meteorological processes characteristic of themore » Mexico City Basin. The collaborative teams pursued the goals through three main tasks: i) analyses of fine PM and secondary PM precursor gaseous species data taken during the MCMA-2002/2003 campaigns and preparation of publications; ii) planning of the MILAGRO Campaign and deployment of the instrument around the MCMA; and iii) analysis of MCMA-2006 data and publication preparation. The measurement phase of the MILAGRO Campaign was successfully completed in March 2006 with excellent participation from the international scientific community and outstanding cooperation from the Mexican government agencies and institutions. The project reported here was led by the Massachusetts Institute of Technology/Molina Center for Energy and the Environment (MIT/MCE2) team and coordinated with DOE/ASP-funded collaborators at Aerodyne Research Inc., University of Colorado at Boulder and Montana State University. Currently 24 papers documenting the findings from this project have been published. The results from the project have improved significantly our understanding of the meteorological and photochemical processes contributing to the formation of ozone, secondary aerosols and other pollutants. Key findings from the MCMA-2003 include a vastly improved speciated emissions inventory from on-road vehicles: the MCMA motor vehicles produce abundant amounts of primary PM, elemental carbon, particle-bound polycyclic aromatic hydrocarbons, carbon monoxide and a wide range of air toxics; the feasibility of using eddy covariance techniques to measure fluxes of volatile organic compounds in an urban core and a valuable tool for validating local emissions inventory; a much better understanding of the sources and atmospheric loadings of volatile organic compounds; the first spectroscopic detection of glyoxal in the atmosphere; a unique analysis of the high fraction of ambient formaldehyde from primary emission sources; characterization of ozone formation and its sensitivity to VOCs and NO x; a much more extensive knowledge of the composition, size distribution and atmospheric mass loadings of both primary and secondary fine PM, including the fact that the rate of MCMA SOA production greatly exceeded that predicted by current atmospheric models; evaluations of significant errors that can arise from standard air quality monitors for O 3 and NO 2; and the implementation of an innovative Markov Chain Monte Carlo method for inorganic aerosol modeling as a powerful tool to analyze aerosol data and predict gas phase concentrations where these are unavailable. During the MILAGRO Campaign the collaborative team utilized a combination of central fixed sites and a mobile laboratory deployed throughout the MCMA to representative urban and boundary sites to measure trace gases and fine particles. Analysis of the extensive 2006 data sets has confirmed the key findings from MCMA-2002/2003; additionally MCMA-2006 provided more detailed gas and aerosol chemistry and wider regional scale coverage. Key results include an updated 2006 emissions inventory; extension of the flux system to measure fluxes of fine particles; better understanding of the sources and apportionment of aerosols, including contribution from biomass burning and industrial sources; a comprehensive evaluation of metal containing particles in a complex urban environment; identification of a close correlation between the rate of production of SOA and “Odd Oxygen” (O 3 + NO 3) and primary organic PM with CO in the urban plume; a more sophisticated understanding of the relationship between ozone formation and ozone precursors: while ozone production in the urban area is VOC-limited, the response is mostly NOx-limited in the surrounding mountain. Comparison of the findings from 2003 and 2006 also confirm that the VOC levels have decreased during the three-year period, while NO x levels remain the same. The results from the 2002/2003 and 2006 have been presented at international conferences and communicated to Mexican government officials. In addition, a large number of graduate students and post-doctoral associates were involved in the project. All data sets and publications are available to the scientific community.« less

Variability of air ion concentrations in urban Paris

NASA Astrophysics Data System (ADS)

Dos Santos, V. N.; Herrmann, E.; Manninen, H. E.; Hussein, T.; Hakala, J.; Nieminen, T.; Aalto, P. P.; Merkel, M.; Wiedensohler, A.; Kulmala, M.; Petäjä, T.; Hämeri, K.

2015-12-01

Air ion concentrations influence new particle formation and consequently the global aerosol as potential cloud condensation nuclei. We aimed to evaluate air ion concentrations and characteristics of new particle formation events (NPF) in the megacity of Paris, France, within the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric Pollution and climate effects, and Integrated tools for assessment and mitigation) project. We measured air ion number size distributions (0.8-42 nm) with an air ion spectrometer and fine particle number concentrations (> 6 nm) with a twin differential mobility particle sizer in an urban site of Paris between 26 June 2009 and 4 October 2010. Air ions were size classified as small (0.8-2 nm), intermediate (2-7 nm), and large (7-20 nm). The median concentrations of small and large ions were 670 and 680 cm-3, respectively, (sum of positive and negative polarities), whereas the median concentration of intermediate ions was only 20 cm-3, as these ions were mostly present during new particle formation bursts, i.e. when gas-to-particle conversion produced fresh aerosol particles from gas phase precursors. During peaks in traffic-related particle number, the concentrations of small and intermediate ions decreased, whereas the concentrations of large ions increased. Seasonal variations affected the ion population differently, with respect to their size and polarity. NPF was observed in 13 % of the days, being most frequent in spring and late summer (April, May, July, and August). The results also suggest that NPF was favoured on the weekends in comparison to workdays, likely due to the lower levels of condensation sinks in the mornings of weekends (CS weekdays 09:00: 18 × 10-3 s-1; CS weekend 09:00: 8 × 10-3 s-1). The median growth rates (GR) of ions during the NPF events varied between 3 and 7 nm h-1, increasing with the ion size and being higher on workdays than on weekends for intermediate and large ions. The median GR of small ions on the other hand were rather similar on workdays and weekends. In general, NPF bursts changed the diurnal cycle of particle number as well as intermediate and large ions by causing an extra peak between 09:00 and 14:00. On average, during the NPF bursts the concentrations of intermediate ions were 8.5-10 times higher than on NPF non-event days, depending on the polarity, and the concentrations of large ions and particles were 1.5-1.8 and 1.2 times higher, respectively. Because the median concentrations of intermediate ions were considerably higher on NPF event days in comparison to NPF non-event days, the results indicate that intermediate ion concentrations could be used as an indication for NPF in Paris. The results suggest that NPF was a source of ions and aerosol particles in Paris and therefore contributed to both air quality degradation and climatic effects, especially in the spring and summer.

Multisite study of particle number concentrations in urban air.

PubMed

Harrison, Roy M; Jones, Alan M

2005-08-15

Particle number concentration data are reported from a total of eight urban site locations in the United Kingdom. Of these, six are central urban background sites, while one is an urban street canyon (Marylebone Road) and another is influenced by both a motorway and a steelworks (Port Talbot). The concentrations are generally of a similar order to those reported in the literature, although higher than those in some of the other studies. Highest concentrations are at the Marylebone Road site and lowest are at the Port Talbot site. The central urban background locations lie somewhere between with concentrations typically around 20 000 cm(-3). A seasonal pattern affects all sites, with highest concentrations in the winter months and lowest concentrations in the summer. Data from all sites show a diurnal variation with a morning rush hour peak typical of an anthropogenic pollutant. When the dilution effects of windspeed are accounted for, the data show little directionality at the central urban background sites indicating the influence of sources from all directions as might be expected if the major source were road traffic. At the London Marylebone Road site there is high directionality driven by the air circulation in the street canyon, and at the Port Talbot site different diurnal patterns are seen for particle number count and PM10 influenced by emissions from road traffic (particle number count) and the steelworks (PM10) and local meteorological factors. Hourly particle number concentrations are generally only weakly correlated to NO(x) and PM10, with the former showing a slightly closer relationship. Correlations between daily average particle number count and PM10 were also weak. Episodes of high PM10 concentration in summer typically show low particle number concentrations consistent with transport of accumulation mode secondary aerosol, while winter episodes are frequently associated with high PM10 and particle number count arising from poor dispersion of local primary emissions.

Observations of fine and coarse particle nitrate at several rural locations in the United States

NASA Astrophysics Data System (ADS)

Lee, Taehyoung; Yu, Xiao-Ying; Ayres, Benjamin; Kreidenweis, Sonia M.; Malm, William C.; Collett, Jeffrey L.

Nitrate comprises an important part of aerosol mass at many non-urban locations during some times of the year. Little is known, however, about the chemical form and size distribution of particulate nitrate in these environments. While submicron ammonium nitrate is often assumed to be the dominant species, this assumption is rarely tested. Properties of aerosol nitrate were characterized at several IMPROVE monitoring sites during a series of field studies. Study sites included Bondville, Illinois (February 2003), San Gorgonio Wilderness Area, California (April and July 2003), Grand Canyon National Park, Arizona (May 2003), Brigantine National Wildlife Refuge, New Jersey (November 2003), and Great Smoky Mountains National Park, Tennessee (July/August 2004). Nitrate was found predominantly in submicron ammonium nitrate particles during the Bondville and San Gorgonio (April) campaigns. Coarse mode nitrate particles, resulting from reactions of nitric acid or its precursors with sea salt or soil dust, were more important at Grand Canyon and Great Smoky Mountains. Both fine and coarse mode nitrate were important during the studies at Brigantine and San Gorgonio (July). These results, which complement earlier findings about the importance of coarse particle nitrate at Yosemite and Big Bend National Parks, suggest a need to more closely examine common assumptions regarding the importance of ammonium nitrate at non-urban sites, to include pathways for coarse mode nitrate formation in regional models, and to consider impacts of coarse particle nitrate on visibility. Because coarse particle nitrate modes often extend well below 2.5 μm aerodynamic diameter, measurements of PM 2.5 nitrate in these environments should not automatically be assumed to contain only ammonium nitrate.

Hydroxymethanesulfonic acid in size-segregated aerosol particles at nine sites in Germany

NASA Astrophysics Data System (ADS)

Scheinhardt, S.; van Pinxteren, D.; Müller, K.; Spindler, G.; Herrmann, H.

2013-12-01

In the course of two field campaigns, size-segregated particle samples were collected at nine sites in Germany, including traffic, urban, rural, marine, and mountain sites. During the chemical characterisation of the samples some of them were found to contain an unknown substance that was later on identified as hydroxymethanesulfonic acid (HMSA). HMSA is known to be formed during the reaction of S(IV) (HSO3- or SO32-) with formaldehyde in the aqueous phase. Due to its stability, HMSA may can act as a reservoir species for S(IV) in the atmosphere and is therefore of interest for the understanding of atmospheric sulphur chemistry. However, no HMSA data are available for atmospheric particles from Central Europe and even on a worldwide scale, data are scarce. Thus, the present study now provides a representative dataset with detailed information on HMSA concentrations in size-segregated Central European aerosol particles. HMSA mass concentrations in this dataset were highly variable: HMSA was found in 224 out of 738 samples (30%), sometimes in high mass concentrations exceeding those of oxalic acid. In average over all 154 impactor runs, 31.5 ng m-3 HMSA were found in PM10, contributing 0.21% to the total mass. The results show that the particle diameter, the sampling location, the sampling season and the air mass origin impact the HMSA mass concentration. Highest concentrations were found in the particle fraction 0.42-1.2 μm, at urban sites, in winter and with eastern (continental) air masses, respectively. The results suggest that HMSA is formed during aging of pollution plumes. A positive correlation of HMSA with sulphate, oxalate and PM is found (R2 > 0.4). The results furthermore suggest that the fraction of HMSA in PM slightly decreases with increasing pH.

Hydroxymethanesulfonic acid in size-segregated aerosol particles at nine sites in Germany

NASA Astrophysics Data System (ADS)

Scheinhardt, S.; van Pinxteren, D.; Müller, K.; Spindler, G.; Herrmann, H.

2014-05-01

In the course of two field campaigns, size-segregated particle samples were collected at nine sites in Germany, including traffic, urban, rural, marine and mountain sites. During the chemical characterisation of the samples some of them were found to contain an unknown substance that was later identified as hydroxymethanesulfonic acid (HMSA). HMSA is known to be formed during the reaction of S(IV) (HSO3- or SO32-) with formaldehyde in the aqueous phase. Due to its stability, HMSA can act as a reservoir species for S(IV) in the atmosphere and is therefore of interest for the understanding of atmospheric sulfur chemistry. However, no HMSA data are available for atmospheric particles from central Europe, and even on a worldwide scale data are scarce. Thus, the present study now provides a representative data set with detailed information on HMSA concentrations in size-segregated central European aerosol particles. HMSA mass concentrations in this data set were highly variable: HMSA was found in 224 out of 738 samples (30%), sometimes in high mass concentrations exceeding those of oxalic acid. On average over all 154 impactor runs, 31.5 ng m-3 HMSA was found in PM10, contributing 0.21% to the total mass. The results show that the particle diameter, the sampling location, the sampling season and the air mass origin impact the HMSA mass concentration. Highest concentrations were found in the particle fraction 0.42-1.2 μm, at urban sites, in winter and with eastern (continental) air masses, respectively. The results suggest that HMSA is formed during aging of pollution plumes. A positive correlation of HMSA with sulfate, oxalate and PM is found (R2 > 0.4). The results furthermore suggest that the fraction of HMSA in PM slightly decreases with increasing pH.

The formation of nitrogen-containing organic oxidation products in a heavily polluted urban environment

NASA Astrophysics Data System (ADS)

Chen, Q.; Cheng, X.; Zheng, Y.; Li, Y.; Zhu, T.; Zhang, Q.; Canagaratna, M. R.; Nowark, J.; Worsnop, D. R.

2017-12-01

Nitrogen-containing organic oxidation products are important species that may contribute to secondary organic aerosol and to redistribute nitrogen oxides through photolysis and oxidation. We deployed a nitrate ion chemical ionization time-of-flight mass spectrometer and a long time-of-flight aerosol mass spectrometer in Beijing for various seasons to study the nitrogen-containing organic species in both gas and particle phases. High concentrations of nitrated phenols were observed in both winter and summer, due to contributions from both primary and secondary sources. The concentrations of gaseous dinitrophenols tracked the severe haze events and correlated well with many highly oxygenated organic molecules. We also identified mass spectral tracers for quantifying organic nitrates. Significant photochemical production of nitrate and organic nitrates were evident during severe haze events, which may contribute to persistent particle formation. The findings are consistent with observed high OH turnover rates, highlighting the importance of gaseous oxidation pathways on persistent particle formation during haze.

Study of atmospheric aerosols by IBA techniques: The LABEC experience

NASA Astrophysics Data System (ADS)

Lucarelli, F.; Calzolai, G.; Chiari, M.; Nava, S.; Carraresi, L.

2018-02-01

At the 3 MV Tandetron accelerator of the LABEC laboratory of INFN (Florence, Italy) an external beam facility is fully dedicated to PIXE-PIGE measurements of the elemental composition of atmospheric aerosols. All the elements with Z > 10 are simultaneously detected by PIXE typically in one minute. This setup allows us an easy automatic positioning, changing and scanning of samples collected by different kinds of devices: long series of daily PM (Particulate Matter) samples can be analysed in short times, as well as size-segregated and high time-resolution aerosol samples. Thanks to the capability of detecting all the crustal elements, PIXE-PIGE analyses are unrivalled in the study of mineral dust: consequently, they are very effective in the study of natural aerosols, like, for example, Saharan dust intrusions. Among the detectable elements there are also important markers of anthropogenic sources, which allow effective source apportionment studies in polluted urban environments using a multivariate method like Positive Matrix Factorization (PMF). Examples regarding recent monitoring campaigns, performed in urban and remote areas, both daily and with high time resolution (hourly samples), as well as with size selection, are presented. The importance of the combined use of the Particle Induced Gamma Ray emission technique (PIGE) and of other complementary (non-nuclear) techniques is highlighted.

Presenting SAPUSS: Solving Aerosol Problem by Using Synergistic Strategies in Barcelona, Spain

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Alastuey, A.; Minguillon, M. C.; Alier, M.; Amato, F.; Brines, M.; Cusack, M.; Grimalt, J. O.; Karanasiou, A.; Moreno, T.; Pandolfi, M.; Pey, J.; Reche, C.; Ripoll, A.; Tauler, R.; Van Drooge, B. L.; Viana, M.; Harrison, R. M.; Gietl, J.; Beddows, D.; Bloss, W.; O'Dowd, C.; Ceburnis, D.; Martucci, G.; Ng, N. L.; Worsnop, D.; Wenger, J.; Mc Gillicuddy, E.; Sodeau, J.; Healy, R.; Lucarelli, F.; Nava, S.; Jimenez, J. L.; Gomez Moreno, F.; Artinano, B.; Prévôt, A. S. H.; Pfaffenberger, L.; Frey, S.; Wilsenack, F.; Casabona, D.; Jiménez-Guerrero, P.; Gross, D.; Cots, N.

2013-09-01

This paper presents the summary of the key objectives, instrumentation and logistic details, goals, and initial scientific findings of the European Marie Curie Action SAPUSS project carried out in the western Mediterranean Basin (WMB) during September-October in autumn 2010. The key SAPUSS objective is to deduce aerosol source characteristics and to understand the atmospheric processes responsible for their generations and transformations - both horizontally and vertically in the Mediterranean urban environment. In order to achieve so, the unique approach of SAPUSS is the concurrent measurements of aerosols with multiple techniques occurring simultaneously in six monitoring sites around the city of Barcelona (NE Spain): a main road traffic site, two urban background sites, a regional background site and two urban tower sites (150 m and 545 m above sea level, 150 m and 80 m above ground, respectively). SAPUSS allows us to advance our knowledge sensibly of the atmospheric chemistry and physics of the urban Mediterranean environment. This is well achieved only because of both the three dimensional spatial scale and the high sampling time resolution used. During SAPUSS different meteorological regimes were encountered, including warm Saharan, cold Atlantic, wet European and stagnant regional ones. The different meteorology of such regimes is herein described. Additionally, we report the trends of the parameters regulated by air quality purposes (both gaseous and aerosol mass concentrations); and we also compare the six monitoring sites. High levels of traffic-related gaseous pollutants were measured at the urban ground level monitoring sites, whereas layers of tropospheric ozone were recorded at tower levels. Particularly, tower level night-time average ozone concentrations (80 ± 25 μg m-3) were up to double compared to ground level ones. The examination of the vertical profiles clearly shows the predominant influence of NOx on ozone concentrations, and a source of ozone aloft. Analysis of the particulate matter (PM) mass concentrations shows an enhancement of coarse particles (PM2.5-10) at the urban ground level (+64%, average 11.7 μg m-3) but of fine ones (PM1) at urban tower level (+28%, average 14.4 μg m-3). These results show complex dynamics of the size-resolved PM mass at both horizontal and vertical levels of the study area. Preliminary modelling findings reveal an underestimation of the fine accumulation aerosols. In summary, this paper lays the foundation of SAPUSS, an integrated study of relevance to many other similar urban Mediterranean coastal environment sites.

Improved MODIS aerosol retrieval in urban areas using a land classification approach and empirical orthogonal functions

NASA Astrophysics Data System (ADS)

Levitan, Nathaniel; Gross, Barry

2016-10-01

New, high-resolution aerosol products are required in urban areas to improve the spatial coverage of the products, in terms of both resolution and retrieval frequency. These new products will improve our understanding of the spatial variability of aerosols in urban areas and will be useful in the detection of localized aerosol emissions. Urban aerosol retrieval is challenging for existing algorithms because of the high spatial variability of the surface reflectance, indicating the need for improved urban surface reflectance models. This problem can be stated in the language of novelty detection as the problem of selecting aerosol parameters whose effective surface reflectance spectrum is not an outlier in some space. In this paper, empirical orthogonal functions, a reconstruction-based novelty detection technique, is used to perform single-pixel aerosol retrieval using the single angular and temporal sample provided by the MODIS sensor. The empirical orthogonal basis functions are trained for different land classes using the MODIS BRDF MCD43 product. Existing land classification products are used in training and aerosol retrieval. The retrieval is compared against the existing operational MODIS 3 KM Dark Target (DT) aerosol product and co-located AERONET data. Based on the comparison, our method allows for a significant increase in retrieval frequency and a moderate decrease in the known biases of MODIS urban aerosol retrievals.

Absorption of visible radiation in atmosphere containing mixtures of absorbing and nonabsorbing particles

NASA Technical Reports Server (NTRS)

Ackerman, T. P.; Toon, O. B.

1981-01-01

The presence of a strongly absorbing material, tentatively identified as graphitic carbon, or 'soot', is indicated by measurements of single-scattering albedo of tropospheric aerosols. Although theoretical calculations based on models of the ways in which soot may mix with other aerosol materials yield the single-scattering albedo values of 0.6, accounted for by a minimum 20% soot by volume, in urban regions and 0.8, yielded by 1-5% soot by volume, in rural settings, it is found that these same values can be produced by similar amounts of the iron oxide magnetite. Magnetite is shown to be indistinguishable from soot by optical measurements performed on bulk samples, and calculation of various mixtures of soot indicate the difficulty of determining aerosol composition by optical scattering techniques.

Aerosol optical properties of Western Mediterranean basin from multi-year AERONET data

NASA Astrophysics Data System (ADS)

Benkhalifa, Jamel; Léon, Jean François; Chaabane, Mabrouk

2017-11-01

Aerosol optical properties including the total and coarse mode aerosol extinction optical depth (AODt and AODc respectively), Angstrom exponent (AE), size distribution, single scattering albedo (SSA) were examined using long-term ground-based radiometric measurements at 9 sites in the Western Mediterranean: Oujda, Malaga, Barcelona, Carpentras, Rome Tor Vergata, Ersa, Ispra, Venice and Evora, during the 4-year study period (2010-2013). The South-North gradient in the fraction of AODc represents the signature of the increasing influence of coarse particles on the optical properties at southern stations. This fraction has a daily mean ranging from 48 ± 18% at the southern site Oujda and to 8 ± 8% at Ispra. The low average AE444-870 value (<0.7) at Oujda confirms the major influence of large dust particles. Conversely, the AOD at urban stations are dominated by fine mode particles. The Angstrom Exponent (AE444-870) above 1.5 in Ispra and Venice indicates an atmospheric situation corresponding to the urban pollution controlled by small particles. We have analyzed the intrinsic dust optical properties by selecting the dusty days corresponding to a total optical depth above 0.3 and a fraction of the coarse mode optical depth above 30%. For these cases, the mean AODt during dusty days was shown to be close to 0.4. During dusty days, the coarse mode fraction represents 88% of the total volume at Oudja and above 83% for all other sites. There is a weak variability in the mean coarse mode volume median radius, showing an average of 1.98 ± 0.1. A maximum in the AODc was observed in the summer of 2012, with particular high events on June 27. The forward trajectory starting at Evora on June 27 clearly indicates that all the sites were affected by such dust events in the following days.

Atmospheric ammonia and its impacts on regional air quality over the megacity of Shanghai, China.

PubMed

Wang, Shanshan; Nan, Jialiang; Shi, Chanzhen; Fu, Qingyan; Gao, Song; Wang, Dongfang; Cui, Huxiong; Saiz-Lopez, Alfonso; Zhou, Bin

2015-10-30

Atmospheric ammonia (NH3) has great environmental implications due to its important role in ecosystem and global nitrogen cycle, as well as contribution to secondary particle formation. Here, we report long-term continuous measurements of NH3 at different locations (i.e. urban, industrial and rural) in Shanghai, China, which provide an unprecedented portrait of temporal and spatial characteristics of atmospheric NH3 in and around this megacity. In addition to point emission sources, air masses originated from or that have passed over ammonia rich areas, e.g. rural and industrial sites, increase the observed NH3 concentrations inside the urban area of Shanghai. Remarkable high-frequency NH3 variations were measured at the industrial site, indicating instantaneous nearby industrial emission peaks. Additionally, we observed strong positive exponential correlations between NH4(+)/(NH4(+)+NH3) and sulfate-nitrate-ammonium (SNA) aerosols, PM2.5 mass concentrations, implying a considerable contribution of gas-to-particle conversion of ammonia to SNA aerosol formation. Lower temperature and higher humidity conditions were found to favor the conversion of gaseous ammonia to particle ammonium, particularly in autumn. Although NH3 is currently not included in China's emission control policies of air pollution precursors, our results highlight the urgency and importance of monitoring gaseous ammonia and improving its emission inventory in and around Shanghai.

Gas and particulate phase products from the ozonolysis of acenaphthylene

NASA Astrophysics Data System (ADS)

Riva, Matthieu; Healy, Robert M.; Tomaz, Sophie; Flaud, Pierre-Marie; Perraudin, Emilie; Wenger, John C.; Villenave, Eric

2016-10-01

Polycyclic aromatic hydrocarbons (PAHs) are recognized as important secondary organic aerosol (SOA) precursors in the urban atmosphere. In this work, the gas-phase ozonolysis of acenaphthylene was investigated in an atmospheric simulation chamber using a proton transfer reaction time-of-flight-mass spectrometer (PTR-TOF-MS) and an aerosol time-of-flight-mass spectrometer (ATOFMS) for on-line characterization of the oxidation products in the gas and particle phases, respectively. SOA samples were also collected on filters and analyzed by ultra performance liquid chromatography/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) and gas chromatography/electron impact ionization-mass spectrometry (GC/EI-MS). The major gas-phase products included a range of oxygenated naphthalene derivatives such as 1,8-naphthalic anhydride, naphthalene 1,8-dicarbaldehyde and naphthaldehyde, as well as a secondary ozonide. Possible reaction mechanisms are proposed for the formation of these products and favoured pathways have been suggested. Many of these products were also found in the particle phase along with a range of oligomeric compounds. The same range of gas and particle phase products was observed in the presence and absence of excess cyclohexane, an OH scavenger, indicating that OH radical production from the ozonolysis of acenaphthylene is negligible. SOA yields in the range 23-37% were determined and indicate that acenaphthylene ozonolysis may contribute to part of the SOA observed in urban areas.

Atmospheric ammonia and its impacts on regional air quality over the megacity of Shanghai, China

PubMed Central

Wang, Shanshan; Nan, Jialiang; Shi, Chanzhen; Fu, Qingyan; Gao, Song; Wang, Dongfang; Cui, Huxiong; Saiz-Lopez, Alfonso; Zhou, Bin

2015-01-01

Atmospheric ammonia (NH3) has great environmental implications due to its important role in ecosystem and global nitrogen cycle, as well as contribution to secondary particle formation. Here, we report long-term continuous measurements of NH3 at different locations (i.e. urban, industrial and rural) in Shanghai, China, which provide an unprecedented portrait of temporal and spatial characteristics of atmospheric NH3 in and around this megacity. In addition to point emission sources, air masses originated from or that have passed over ammonia rich areas, e.g. rural and industrial sites, increase the observed NH3 concentrations inside the urban area of Shanghai. Remarkable high-frequency NH3 variations were measured at the industrial site, indicating instantaneous nearby industrial emission peaks. Additionally, we observed strong positive exponential correlations between NH4+/(NH4++NH3) and sulfate-nitrate-ammonium (SNA) aerosols, PM2.5 mass concentrations, implying a considerable contribution of gas-to-particle conversion of ammonia to SNA aerosol formation. Lower temperature and higher humidity conditions were found to favor the conversion of gaseous ammonia to particle ammonium, particularly in autumn. Although NH3 is currently not included in China’s emission control policies of air pollution precursors, our results highlight the urgency and importance of monitoring gaseous ammonia and improving its emission inventory in and around Shanghai. PMID:26514559

Studies of Physicochemical Processes in Atmospheric Particles and Acid Deposition.

NASA Astrophysics Data System (ADS)

Pandis, Spyros N.

A comprehensive chemical mechanism for aqueous -phase atmospheric chemistry was developed and its detailed sensitivity analysis was performed. The main aqueous-phase reaction pathways for the system are the oxidation of S(IV) to S(VI) by H_2O_2 , OH, O_2 (catalysed by Fe ^{3+} and Mn^ {2+}), O_3 and HSO_sp{5}{-}. The gas-phase concentrations of SO_2, H_2O_2, HO _2, OH, O_3 HCHO, NH_3, HNO_3 and HCl and the liquid water content of the cloud are of primary importance. The Lagrangian model predictions for temperature profile, fog development, liquid water content, gas-phase concentrations of SO_2 , HNO_3, and NH_3 , pH, aqueous-phase concentrations of SO _sp{4}{2-}, NH _sp{4}{+} and NO _sp{3}{-}, and finally deposition rates of the above ions match well the observed values. A third model was developed to study the distribution of acidity and solute concentration among the various droplet sizes in a fog or a cloud. Significant solute concentration differences can occur in aqueous droplets inside a fog or a cloud. Fogs in polluted environments have the potential to increase aerosol sulfate concentrations, but at the same time to cause reductions in the aerosol concentration of nitrate, chloride, ammonium and sodium as well as in the total aerosol mass concentration. The sulfate producd during fog episodes favors the aerosol particles that have access to most of the fog liquid water. Aerosol scavenging efficiencies of around 80% were calculated for urban fogs. Sampling and subsequent mixing of fog droplets of different sizes may result in measured concentrations that are not fully representative of the fogwater chemical composition. Isoprene and beta-pinene, at concentration levels ranging from a few ppb to a few ppm were reacted photochemically with NO_ {x} in the Caltech outdoor smog chamber facility. Aerosol formation from the isoprene photooxidation was found to be negligible even under extreme ambient conditions due to the relatively high vapor pressure of its condensable products. Aerosol carbon yield from the beta -pinene photooxidation is as high as 8% and depends strongly on the initial HC/NO_{x} ratio. Monoterpene photooxidation can be a significant source of secondary aerosol in rural environments and in urban areas with extended natural vegetation. (Abstract shortened with permission of author.).

Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

NASA Astrophysics Data System (ADS)

Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

2013-11-01

Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

NASA Astrophysics Data System (ADS)

Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

2013-06-01

Multiwavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentrations profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analyzed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical to distinguish between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

Chemical, optical and radiative characteristics of aerosols during haze episodes of winter in the North China Plain

NASA Astrophysics Data System (ADS)

Ding, Jing; Zhang, Yufen; Han, Suqin; Xiao, Zhimei; Wang, Jiao; Feng, Yinchang

2018-05-01

Aerosol and water vapor radiative forcings, shortwave atmospheric heating rates and longwave atmospheric cooling rates were determined based on in situ physical and chemical measurements of aerosol, associated with the Mie theory and a radiative transfer model, LOWTRAN7, during the two haze episodes in the winter of 2013 in Tianjin, China. The aerosol types considered in LOWTRAN7 included rural, urban, marine, desert and custom aerosols. The default ratio of the absorption coefficient to the extinction coefficient for urban aerosol in LOWTRAN7 was approximately double of those found in this work, implying the weaker absorption ability of aerosols in the North China Plain (NCP). Moreover, the aerosol is assumed to be evenly distributed below 1 km of planetary boundary layer (PBL) on hazy days in LOWTRAN7. If the default urban aerosol optical properties and extinction profile in LOWTRAN7 is employed directly, a larger energy imbalance between the atmosphere and surface is generated and the warming effect of the aerosol is magnified. Hence, modified urban aerosol optical properties were established to replace the corresponding parameters' database in LOWTRAN7. The aerosol extinction profiles were obtained based on a 255-m meteorological tower and observed results from the studies about Tianjin. In the NCP, the aerosol had little impact on atmospheric counter radiation. The water vapor is the crucial factor that affects atmospheric counter radiation. Both modified high shortwave heating rates and longwave cooling rates occur near the surface due to the abundance of aerosol and water vapor. The modified net atmospheric heating rate near the surface is 1.2 K d-1 on hazy days and 0.3 K d-1 on non-hazy days. Compared with the default urban aerosol optical properties and its vertical distribution in LOWTRAN7, the feedback effect of the modified urban aerosol on the boundary layer may not necessarily result in a stable lower atmosphere, but depends on the aerosol light absorption ability and its vertical distribution.

Concentrations and size distributions of fine aerosol particles measured at roof level in urban zone

NASA Astrophysics Data System (ADS)

Despiau, S.; Croci, D.

2007-05-01

During the experimental Field Experiments to Constrain Models of Atmospheric Pollution and Transport of Emissions (ESCOMPTE) campaign in June-July 2001, concentrations and size distributions of fine particles (14-722 nm) were measured at roof level in downtown Marseille (France). Part of the campaign was dedicated to the study of aerosol behavior in relation to strong photochemical events (which were identified as "IOP" days) and their regional modeling. The analysis of the concentration variations and the evolution of average diurnal size distribution showed that an "IOP day" is not characterized by a specific concentration or its variation, nor by a specific evolution of the average size distribution. The morning traffic rush is detected at roof level by a net increase in particle concentration over the whole size range measured, indicating a production of ultrafine particles by the traffic but also the raising to roof level of particles of the accumulation mode. The increase is observed about 1 hour after the traffic peak at street level, which is characterized by strong increases in NOx and CO concentrations. The corresponding flux of particles at roof level has been estimated around 3 × 104 cm-2 s-1. A specific signature characterized by a strong and rapid burst of concentration (factor 2 to 4 in 15 min) of particles between 25 and 50 nm, independent of the traffic source, has been detected on six occasions during the campaign. These events occur systematically around noon, in cases of strong radiation, low relative humidity, and common wind direction. Despite the high-diameter value of these particles, it is suggested that they could result from a specific "secondary aerosol process" event involving ozone, biogenic, and/or anthropogenic gas precursors like iodine and VOCs.

Apparatus for rapid measurement of aerosol bulk chemical composition

DOEpatents

Lee, Yin-Nan E.; Weber, Rodney J.

2003-01-01

An apparatus and method for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution are provided. The apparatus includes a modified particle size magnifier for producing activated aerosol particles and a collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical methods. The method provided for on-line measurement of chemical composition of aerosol particles includes exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

Apparatus for rapid measurement of aerosol bulk chemical composition

DOEpatents

Lee, Yin-Nan E.; Weber, Rodney J.; Orsini, Douglas

2006-04-18

An apparatus for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution is provided. The apparatus includes an enhanced particle size magnifier for producing activated aerosol particles and an enhanced collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical means. Methods for on-line measurement of chemical composition of aerosol particles are also provided, the method including exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; and flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

Spectral Optical Properties of the Polluted Atmosphere of Mexico City (Spring-Summer 1992)

NASA Technical Reports Server (NTRS)

Vasilyev, O. B.; Contreras, A. Leyva; Valazquez, A. Muhlia; Peralta-Fabi, R.; Ivlev, L. S.; Kovalenko, A. P.; Vasilyev, A. V.; Jukov, V. M.; Welch, Ronald M.

1995-01-01

A joint Mexican, Russian, and American research effort has been initiated to develop new methods to remotely sense atmospheric parameters using ground-based, aircraft, and satellite observations. As a first step in this program, ground-based spectrophotometric measurements of the direct solar radiation have been obtained for the extremely polluted Mexico City atmosphere for the period of April-June 1992. These observations were made at more than 1300 channels in the spectral range of 0.35-0.95 microns. In the UltraViolet (UV) portions of the spectrum (e.g., 0.35 microns), aerosol optical thicknesses were found to range between 0.6 and 1.2; in the visible portion of the spectrum (e. g., 0.5 microns) they ranged from 0.5 to 0.8; and in the Near-Infrared (NIR) spectra (e.g., 0.85 micron), values of 0.3 - 0.5 were found. Applying a Spectral Optical Depth (SOD) model of tau(lambda) = C + A(lambda(sup -varies as), values of 1.55 less than varies as less than 1.85 were obtained for polluted, cloudless days, with values of 1.25 less than varies as less than 1.60 on days with haze. The aerosol particles in the polluted Mexico City atmosphere were found to be strongly absorbing, with a single-scattering albedo of 0.7 - 0.9 in the UV, 0.6 - 0.8 in the visible portion of the spectrum, and 0.4 - 0.7 in the NIR. These values are possibly consistent with a high soot concentration, contributed both by vehicular traffic and heavy industry. Analysis of the measured aerosol SOD using the optical parameters of an urban aerosol model pemiits the concentration of aerosol particles to be estimated in the vertical column; a maximum value of 3 x 10(exp 9) 1/sq cm was found. This concentration of aerosol particles exceeds that found in most other regions of the globe by at least an order of magnitude. Near the ground the aerosol size distributions measured using an optical particle counter were found to be strongly multimodal.

Coarse and fine aerosol source apportionment in Rio de Janeiro, Brazil

NASA Astrophysics Data System (ADS)

Godoy, Maria Luiza D. P.; Godoy, José Marcus; Roldão, Luiz Alfredo; Soluri, Daniela S.; Donagemma, Raquel A.

The metropolitan area of Rio de Janeiro is one of the twenty biggest urban agglomerations in the world, with 11 million inhabitants in the metropolitan area, and has a high population density, with 1700 hab. km -2. For this aerosol source apportionment study, the atmospheric aerosol sampling was performed at ten sites distributed in different locations of the metropolitan area from September/2003 to December/2005, with sampling during 24 h on a weekly basis. Stacked filter units (SFU) were used to collect fine and coarse aerosol particles with a flow rate of 17 L min -1. In both size fractions trace elements were analyzed by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) as well as water-soluble species by Ion-Chromatography (IC). Also gravimetric analysis and reflectance measurements provided aerosol mass and black carbon concentrations. Very good detection limits for up to 42 species were obtained. Mean annual PM 10 mass concentration ranged from 20 to 37 μg m -3, values that are within the Brazilian air quality standards. Receptor models such as principal factor analysis, cluster analysis and absolute principal factor analysis were applied in order to identify and quantify the aerosol sources. For fine and coarse modes, circa of 100% of the measured mass was quantitatively apportioned to relatively few identified aerosol sources. A very similar and consistent source apportionment was obtained for both fine and coarse modes for all 10 sampling sites. Soil dust is an important component, accounting for 22-72% and for 25-48% of the coarse and fine mass respectively. On the other hand, anthropogenic sources as vehicle traffic and oil combustion represent a relatively high contribution (52-75%) of the fine aerosol mass. The joint use of ICP-MS and IC analysis of species in aerosols has proven to be reliable and feasible for the analysis of large amount of samples, and the coupling with receptor models provided an excellent method for quantitative aerosol source apportionment in large urban areas.

Retrieval of AOD and PM2.5 Concentrations over Urban Areas of Shenyang City using MODIS Data

NASA Astrophysics Data System (ADS)

Wang, Z.

2016-12-01

Atmospheric aerosols play an important part in the Earth's radiation balance as well as global climate change, aerosols also have very important impact on environment as well as human and other organisms' health, PM2.5 and other small particle aerosols, can enter bronchi directly, thus causing bronchitis, cardiovascular disease, asthma and so on.Detection of AOD by satellite and remote sensing is currently one of the hotest issues , diffierent from the traditional monitoring method, this method has much more advantanges, for emample wide area coverage, fast and convenient etc. So it is possible for people to know the regional changes of AOD real time over large area. Now, detection aerosol by RS technology has reached a high level in marine and dense vegetation land areas, but result is not ideal for urban areas, the higher surface reflectance in urban areas is a bottleneck of AOD retrieval. Focus on the high surface reflectance and low accuracy of the AOD products of urban areas, this paper propose an algorithm coupled with surface reflectance to get red band surface reflectance, based on Dens Dark Vegetation algorithm and geometrical optics model theory, to distinguish urban reflectivity from other targets. Considering the appropriate aerosol model which adapt to season and other proper parameters, this paper uses 6S model to establish look-up table, thus retrieve AOD for urban as well as other high reflectance areas. This paper take Shenyang region as pilot area, then retrieve the AOD and PM2.5 concentration of Shenyang in 2015 based on MODIS data, thus get 1km resolution distribution map, and then analyzed the results in spatial, intensity and temporal. At last, real-time monitoring data from the ground monitor station is used to verify the outcome, the results have good accuracy and the the correlation reached 0.9004 when the weather is sunny. The research shows that this algorithm has relatively higher precision and certain universality. This method has better applicability to retrieve AOD and PM2.5 concentration by remote sensing in Shenyang and Liaoning Provience, and owes guiding and reference significance, and it has a high value in terms of atmospheric environment monitoring.

Relationship Between Aerosol Number Size Distribution and Atmospheric Electric Potential Gradient in an Urban Area

NASA Astrophysics Data System (ADS)

Wright, Matthew; Matthews, James; Bacak, Asan; Silva, Hugo; Priestley, Michael; Percival, Carl; Shallcross, Dudley

2016-04-01

Small ions are created in the atmosphere by ground based radioactive decay and solar and cosmic radiation ionising the air. The ionosphere is maintained at a high potential relative to the Earth due to global thunderstorm activity, a current from the ionosphere transfers charge back to the ground through the weakly ionised atmosphere. A potential gradient (PG) exists between the ionosphere and the ground that can be measured in fair weather using devices such as an electric field mill. PG is inversely-proportional to the conductivity of the air and therefore to the number of ions of a given electrical mobility; a reduction of air ions will cause an increase of PG. Aerosols in the atmosphere act as a sink of air ions with an attachment rate dependent on aerosol size distribution and ion mobility. These relationships have been used to infer high particulate, and hence pollution, levels in historic datasets of atmospheric PG. A measurement campaign was undertaken in Manchester, UK for three weeks in July and August where atmospheric PG was measured with an electric field mill (JCI131, JCI Chilworth) on a second floor balcony, aerosol size distribution measured with a scanning mobility particle sizer (SMPS, TSI3936), aerosol concentration measured with a condensation particle counter (CPC, Grimm 5.403) and local meteorological measurements taken on a rooftop measurement site ~200 m away. Field mill and CPC data were taken at 1 s intervals and SMPS data in 2.5 minute cycles. Data were excluded for one hour either side of rainfall as rainclouds and droplets can carry significant charge which would affect PG. A quantity relating to the attachment of ions to aerosol (Ion Sink) was derived from the effective attachment coefficient of the aerosols. Further measurements with the field mill and CPC were taken at the same location in November 2015 when bonfire events would be expected to increase aerosol concentrations. During the summer measurements, particle number count (PNC) from the CPC and SMPS were very closely correlated. PG was closely related to PNC and the ion sink parameter both with the overall trend, and especially during 'peak' events of high concentration. The data were averaged to a diurnal cycle and the average daily cycle showed variability in PG and PNC consistent with the urban environment including a peak at rush hour and a minimum during the night. Lomb-Scargle periodograms provided the spectral content and daily and weekly peaks were apparent in PG and PNC data. Cross correlation analysis indicates that the best temporal correlation exists between PG and ion sink rate.

Use of Lead Isotopes to Identify Sources of Metal and Metalloid Contaminants in Atmospheric Aerosol from Mining Operations

PubMed Central

Félix, Omar I.; Csavina, Janae; Field, Jason; Rine, Kyle P.; Sáez, A. Eduardo; Betterton, Eric A.

2014-01-01

Mining operations are a potential source of metal and metalloid contamination by atmospheric particulate generated from smelting activities, as well as from erosion of mine tailings. In this work, we show how lead isotopes can be used for source apportionment of metal and metalloid contaminants from the site of an active copper mine. Analysis of atmospheric aerosol shows two distinct isotopic signatures: one prevalent in fine particles (< 1 μm aerodynamic diameter) while the other corresponds to coarse particles as well as particles in all size ranges from a nearby urban environment. The lead isotopic ratios found in the fine particles are equal to those of the mine that provides the ore to the smelter. Topsoil samples at the mining site show concentrations of Pb and As decreasing with distance from the smelter. Isotopic ratios for the sample closest to the smelter (650 m) and from topsoil at all sample locations, extending to more than 1 km from the smelter, were similar to those found in fine particles in atmospheric dust. The results validate the use of lead isotope signatures for source apportionment of metal and metalloid contaminants transported by atmospheric particulate. PMID:25496740

Ion balance and acidity of size-segregated particles during haze episodes in urban Beijing

NASA Astrophysics Data System (ADS)

Tian, Shili; Pan, Yuepeng; Wang, Yuesi

2018-03-01

In this study, we investigated how the ion balance causes variations in size segregated aerosol acidity and atmospheric processing on clean versus hazy days using a 9-stage sampler. We calculated the ratios (in charge equivalents, RC/A) between measured cations (Na+, NH4+, K+, Mg2 +, and Ca2 +) and anions (SO42 -, NO3- and Cl-) for different aerosol size fractions. The ratios were typically close to unity in the accumulation mode (0.65-2.1 μm), and increased significantly when the particle size increased or decreased. In the coarse size range (aerodynamic diameter > 2.1 μm), high RC/A values were most likely caused by the undetermined CO32- and HCO3- content of the mineral dust. In contrast, the high RC/A values for submicron aerosols (< 1.1 μm) were likely caused by the presence of water-soluble organic anions. The RC/A values for all size fractions were lower on hazy days than clean days, indicating that aerosol acidity was enhanced on polluted days. Simiar temporal trend between RC/A and in-situ pH indicated that RC/A was a good indicator of aerosol acidity in fine mode aerosol. The SO42 - and NO3- contents in fine particles were completely neutralized as the RC/A values for PM2.1 approached unity, and mean values of RC/A were 1.34 and 1.16 during the transition and polluted periods, respectively. The lowest RC/A values were observed in the size fraction with the highest concentrations of SO42 -, NO3- and NH4+ (SNA) and concentrations of SNA increased with the increasing aerosol acidity. Significant correlations between [NO3-]/[SO42 -] and [NH4+]/[SO42 -] during NH4+-rich conditions in fine size fractions indicated fine mode NO3- in Beijing was mainly formed by gas-phase homogeneous reaction between the ambient NH3 and HNO3.

Assessment of capabilities of multiangle imaging photo-polarimetry for atmospheric correction in presence of absorbing aerosols

NASA Astrophysics Data System (ADS)

Kalashnikova, O. V.; Garay, M. J.; Xu, F.; Seidel, F. C.; Diner, D. J.

2015-12-01

Satellite remote sensing of ocean color is a critical tool for assessing the productivity of marine ecosystems and monitoring changes resulting from climatic or environmental influences. Yet water-leaving radiance comprises less than 10% of the signal measured from space, making correction for absorption and scattering by the intervening atmosphere imperative. Traditional ocean color retrieval algorithms utilize a standard set of aerosol models and the assumption of negligible water-leaving radiance in the near-infrared. Modern improvements have been developed to handle absorbing aerosols such as urban particulates in coastal areas and transported desert dust over the open ocean, where ocean fertilization can impact biological productivity at the base of the marine food chain. Even so, imperfect knowledge of the absorbing aerosol optical properties or their height distribution results in well-documented sources of error. In the UV, the problem of UV-enhanced absorption and nonsphericity of certain aerosol types are amplified due to the increased Rayleigh and aerosol optical depth, especially at off-nadir view angles. Multi-angle spectro-polarimetric measurements have been advocated as an additional tool to better understand and retrieve the aerosol properties needed for atmospheric correction for ocean color retrievals. The central concern of the work to be described is the assessment of the effects of absorbing aerosol properties on water leaving radiance measurement uncertainty by neglecting UV-enhanced absorption of carbonaceous particles and by not accounting for dust nonsphericity. In addition, we evaluate the polarimetric sensitivity of absorbing aerosol properties in light of measurement uncertainties achievable for the next generation of multi-angle polarimetric imaging instruments, and demonstrate advantages and disadvantages of wavelength selection in the UV/VNIR range. The phase matrices for the spherical smoke particles were calculated using a standard Mie code, while those for non-spherical dust particles were calculated using the numerical approach described by Dubovik et al., 2006. A vector Markov Chain radiative transfer code including bio-optical models was used to evaluate TOA and water leaving radiances.

Long- and/or short-range transportation of local Asian aerosols in DRAGON-Osaka Experiment

NASA Astrophysics Data System (ADS)

Nakata, M.; Sano, I.; Mukai, S.; Holben, B. N.

2013-12-01

This work intends to demonstrate the spatial and temporal variation of atmospheric particles in East Asia, especially around AERONET (Aerosol Robotics Network) -Osaka site during Dragon Asia period in the spring of 2012, named Dragon-Osaka. It is known that the air pollution in East Asia becomes to be severe due to both the increasing emissions of the anthropogenic aerosols associated with economic growth and the complicated behavior of natural aerosols. Thus the precise observations of atmospheric particles in East Asia are desired. Osaka is the second big city in Japan and a typical Asian urban area. The population of the region is around 20 millions including neighbor prefectures. Therefore, air quality in the region is slightly bad compared to remote area due to industries and auto mobiles. In recent years, Asian dusts and anthropogenic small particles transported from China and cover those cities throughout year. AERONET Osaka site was established in 2002 on the campus of Kinki University. Nowadays, LIDAR (Light Detection and Ranging), an SPM sampler (SPM-613D, Kimoto Electric, Japan) and others are available on the roof of a building. The site data are useful for algorithm development of aerosol retrieval over busy city. On the other hand, human activities in this region also emit the huge amount of pollutions, thus it is needed to investigate the local distribution of aerosols in this region. In order to investigate change of aerosol properties, PM-individual analysis is made with scanning electron microscope (SEM) coupled with energy dispersive X-ray analyzer (EDX). SEM/EDX is an effective instrument to observe the surface microstructure and analyze the chemical composition of such materials as metals, powders, biological specimens, etc. We used sampling data from the SPM sampler at AERONET Osaka site. During a period of DRAGON-Asia, high concentrations of air pollutant were observed on the morning of March 11 in Fukue Island in the East China Sea. On the same day afternoon, large value of PM mass concentration was measured in Osaka. It is found from the simultaneous measurements of atmospheric particles, especially those on March 11, which present the maximum efficiency of DRAGON-Osaka, and numerical model simulations indicate that the long- and/or short- range transportation factors influence the characterization of atmospheric particles.

A three-dimensional sectional representation of aerosol mixing state for simulating optical properties and cloud condensation nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ching, Ping Pui; Zaveri, Rahul A.; Easter, Richard C.

2016-05-27

Light absorption by black carbon (BC) particles emitted from fossil fuel combustion depends on the how thickly they are coated with non-refractory species such as ammonium, sulfate, nitrate, organics, and water. The cloud condensation nuclei (CCN) activation property of a particle depends on its dry size and the hygroscopicities of all the individual species mixed together. It is therefore necessary to represent both size and mixing state of aerosols to reliably predict their climate-relevant properties in atmospheric models. Here we describe and evaluate a novel sectional framework in the Model for Simulating Aerosol Interactions and Chemistry, referred to as MOSAIC-mix,more » that represents the mixing state by resolving aerosol dry size (Ddry), BC dry mass fraction (wBC), and hygroscopicity (κ). Using ten idealized urban plume scenarios in which different types of aerosols evolve over 24 hours under a range of atmospherically relevant environmental conditions, we examine errors in CCN concentrations and optical properties with respect to a more explicit aerosol mixing state representation. We find that only a small number of wBC and κ bins are needed to achieve significant reductions in the errors, and propose a configuration consisting of 24 Ddry bins, 2 wBC bins, and 2 κ bins that gives 24-hour average errors of about 5% or less in CCN concentrations and optical properties, 3-4 times lower than those from size-only-resolved simulations. These results show that MOSAIC-mix is suitable for use in regional and global models to examine the effects of evolving aerosol mixing states on aerosol-radiation-cloud feedbacks.« less

Aircraft-borne aerosol chemical composition measurements in the lower to middle troposphere over southern West Africa: Biomass burning, urban outflow plumes, and long-range transport.

NASA Astrophysics Data System (ADS)

Batenburg, Anneke; Schulz, Christiane; Schneider, Johannes; Sauer, Daniel; Schlager, Hans; Borrmann, Stephan

2017-04-01

During the DACCIWA field campaign in June and July 2016, aircraft-borne in-situ aerosol chemical composition measurements were performed over southern West Africa (SWA). This presentation will focus on the submicron particle measurements done with a Compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) on board of the DLR Falcon aircraft during twelve research flights from Lomé, Togo, covering the altitude range from the boundary layer (BL) to the middle troposphere (12 km). A preliminary analysis of the results shows typical baseline total non-refractory aerosol mass loadings of 1.5 to 2.8 μg m-3 in the BL, and 0.4 to 1.1 μg m-3above. Up to half of the baseline aerosol mass in the BL appears to consist of sulphate, compared to only 10 to 35 % above the BL; organic matter dominates in the middle troposphere. During several flights, the DLR Falcon crossed a pronounced and seemingly widespread aerosol layer at 2—4.5 km altitude, partly in or slightly above the BL. The AMS data indicate that about half of the non-refractory aerosol mass in the middle of this layer consisted of organic matter. We consider it likely that these aerosol particles were produced by biomass burning in Central Africa. Emissions from cities and industrial areas were also intercepted, as well as enhancements in some species at higher altitudes. Trajectory analysis suggests that an increase of the organics to more than 2.5 μg m-3 observed at 8 km during one flight came from the Arabian Peninsula. Several ammonium peaks during the same flight at higher altitudes were traced back to the Asian Summer Monsoon Anticyclone (ASMA).

Natural and Anthropogenic Aerosols in the World's Megacities and Climate Impacts

NASA Astrophysics Data System (ADS)

Kafatos, M.; Singh, R.; El-Askary, H.; Qu, J.

2005-12-01

The world's megacities are the sites of production of a variety of aerosols and are themselves affected by natural and human-induced aerosols. In particular, sources of aerosols impacting cities include: industrial and automobile emission; sand and dust storms from, e.g., the Sahara and Gobi Deserts; as well as fire-induced aerosols. Improving the ability of various stakeholder organizations to respond effectively to high concentrations of aerosols, with special emphasis on mineral dust from dust storms; smoke from controlled burns, wild fires and agricultural burning; and anthropogenic aerosols, would be an important goal not just to understand climate forcings but also to be able to better respond to the increasing amounts of aerosols at global and regional levels. Cities and surrounding areas are affected without good estimates of the current and future conditions of the aerosols and their impact on regional and global climate. Remotely sensed (RS) NASA, NOAA and international platform data can be used to characterize the properties of aerosol clouds and special hazard events such as sand and dust storms (SDS). Aerosol analysis and prediction-model capabilities from which stakeholders can choose the tools that best match their needs and technological expertise are important. Scientists validating mesoscale and aerosol-transport models, aerosol retrievals from satellite measurements are indispensable for robust climate predictions. Here we give two examples of generic SDS cases and urban pollution and their possible impact on climate: The Sahara desert is a major source of dust aerosols dust transport is an important climatic process. The aerosols in the form of dust particles reflect the incoming solar radiation to space, thereby reducing the amount of radiation available to the ground, known as `direct' radiative forcing of aerosols. The aerosols also change the cloud albedo and microphysical properties of clouds, known as `indirect' radiative forcing of aerosols. The highest boundary layer heights are associated with regions where the sensible heat flux is greatest, and latent heat flux is smallest due to lack of vegetation. Boundary layer heights in the deserts may be systematically higher than the slightly wetter regions at the edges of deserts. Latent heat flux model runs and MODIS observations of dust storms affecting the Nile Delta and Cairo indicate strong influence on the local weather and climate forcings. In the Indo-Gangetic, during the pre-monsoon period, dust storms form. We have examined SDS transport using RS data acquired from NASA's MODIS MISR instruments and from sun photometer measurements. The aerosol optical depth and size of the dust particles are found to be significantly higher during such dust storm events. Moreover, our results clearly show that power plants in this region are the key point source of air pollutants. The detailed analysis of aerosol parameters show the existence of absorbing and non-absorbing aerosols emitted from these plants. The combined effects of urban aerosols with dust aerosols in India and Cairo not only affect megacities, they also have long-term climate impacts. We will also discuss how the assimilation of RS data into mesoscale models can improve these models and predictability of hazards and effects on megacities, such as SDS events, and forest fires, all sources of aerosols. Therefore RS data can improve the prediction of climate forcings by aerosols.

Dust Aerosols at the Source Region During ACE-ASIA: A Surface/Satellite Perspective

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee; Lau, William K. M. (Technical Monitor)

2001-01-01

ACE (Aerosol Characterization Experiment)-Asia is designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentrations over eastern Asia and along the rim of the western Pacific. The phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian dust is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of dust aerosol radiative flux in addition to measurements of loading and optical thickness. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

Characterization of Dust Properties at the Source Region During ACE-Asia

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee; Lau, William (Technical Monitor)

2001-01-01

ACE (Aerosol Characterization Experiment)-Asia is designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally-occurring aerosols, which often exist in high concentrations over eastern Asia and along the rim of the western Pacific. The phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, east coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian dust is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of dust aerosol radiative flux in addition to measurements of loading and optical thickness. At the time of the Terra/MODIS overpass, these ground-based observations can provide valuable data to compare with MODIS retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

Aerosol Meteorology of Maritime Continent for the 2012 7SEAS Southwest Monsoon Intensive Study - Part 2: Philippine Receptor Observations of Fine-Scale Aerosol Behavior

NASA Technical Reports Server (NTRS)

Reid, Jeffrey S.; Lagrosas, Nofel D.; Jonsson, Haflidi H.; Reid, Elizabeth A.; Atwood, Samuel A.; Boyd, Thomas J.; Ghate, Virendra P.; Xian, Peng; Posselt, Derek J.; Simpas, James B.;

Aerosol meteorology of Maritime Continent for the 2012 7SEAS southwest monsoon intensive study – Part 2: Philippine receptor observations of fine-scale aerosol behavior

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reid, Jeffrey S.; Lagrosas, Nofel D.; Jonsson, Haflidi H.

The largest 7 Southeast Asian Studies (7SEAS) operations period within the Maritime Continent (MC) occurred in the August–September 2012 biomass burning season. Data included were observations aboard the M/Y Vasco, dispatched to the Palawan Archipelago and Sulu Sea of the Philippines for September 2012. At these locations, the Vasco observed MC smoke and pollution entering the southwest monsoon (SWM) monsoonal trough. Here we describe the research cruise findings and the finer-scale aerosol meteorology of this convectively active region. This 2012 cruise complemented a 2-week cruise in 2011 and was generally consistent with previous findings in terms of how smoke emission and transportmore » related to monsoonal flows, tropical cyclones (TC), and the covariance between smoke transport events and the atmosphere's thermodynamic structure. Biomass burning plumes were usually mixed with significant amounts of anthropogenic pollution. Also key to aerosol behavior were squall lines and cold pools propagating across the South China Sea (SCS) and scavenging aerosol particles in their path. However, the 2012 cruise showed much higher modulation in aerosol frequency than its 2011 counterpart. Whereas in 2011 large synoptic-scale aerosol events transported high concentrations of smoke into the Philippines over days, in 2012 measured aerosol events exhibited a much shorter-term variation, sometimes only 3$-$12 h. Strong monsoonal flow reversals were also experienced in 2012. Nucleation events in cleaner and polluted conditions, as well as in urban plumes, were observed. Perhaps most interestingly, several cases of squall lines preceding major aerosol events were observed, as opposed to 2011 observations where these lines largely scavenged aerosol particles from the marine boundary layer. Combined, these observations indicate pockets of high and low particle counts that are not uncommon in the region. These perturbations are difficult to observe by satellite and very difficult to model. Indeed, the Navy Aerosol Analysis and Prediction System (NAAPS) simulations captured longer period aerosol events quite well but largely failed to capture the timing of high-frequency phenomena. Ultimately, the research findings of these cruises demonstrate the real world challenges of satellite-based missions, significant aerosol life cycle questions such as those the future Aerosol/Clouds/Ecosystems (ACE) will investigate, and the importance of small-scale phenomena such as sea breezes, squall lines, and nucleation events embedded within SWM patterns in dominating aerosol life cycle and potential relationships to clouds.« less

Aerosol meteorology of Maritime Continent for the 2012 7SEAS southwest monsoon intensive study - Part 2: Philippine receptor observations of fine-scale aerosol behavior

NASA Astrophysics Data System (ADS)

Reid, Jeffrey S.; Lagrosas, Nofel D.; Jonsson, Haflidi H.; Reid, Elizabeth A.; Atwood, Samuel A.; Boyd, Thomas J.; Ghate, Virendra P.; Xian, Peng; Posselt, Derek J.; Simpas, James B.; Uy, Sherdon N.; Zaiger, Kimo; Blake, Donald R.; Bucholtz, Anthony; Campbell, James R.; Chew, Boon Ning; Cliff, Steven S.; Holben, Brent N.; Holz, Robert E.; Hyer, Edward J.; Kreidenweis, Sonia M.; Kuciauskas, Arunas P.; Lolli, Simone; Oo, Min; Perry, Kevin D.; Salinas, Santo V.; Sessions, Walter R.; Smirnov, Alexander; Walker, Annette L.; Wang, Qing; Yu, Liya; Zhang, Jianglong; Zhao, Yongjing

2016-11-01

The largest 7 Southeast Asian Studies (7SEAS) operations period within the Maritime Continent (MC) occurred in the August-September 2012 biomass burning season. Data included were observations aboard the M/Y Vasco, dispatched to the Palawan Archipelago and Sulu Sea of the Philippines for September 2012. At these locations, the Vasco observed MC smoke and pollution entering the southwest monsoon (SWM) monsoonal trough. Here we describe the research cruise findings and the finer-scale aerosol meteorology of this convectively active region. This 2012 cruise complemented a 2-week cruise in 2011 and was generally consistent with previous findings in terms of how smoke emission and transport related to monsoonal flows, tropical cyclones (TC), and the covariance between smoke transport events and the atmosphere's thermodynamic structure. Biomass burning plumes were usually mixed with significant amounts of anthropogenic pollution. Also key to aerosol behavior were squall lines and cold pools propagating across the South China Sea (SCS) and scavenging aerosol particles in their path. However, the 2012 cruise showed much higher modulation in aerosol frequency than its 2011 counterpart. Whereas in 2011 large synoptic-scale aerosol events transported high concentrations of smoke into the Philippines over days, in 2012 measured aerosol events exhibited a much shorter-term variation, sometimes only 3-12 h. Strong monsoonal flow reversals were also experienced in 2012. Nucleation events in cleaner and polluted conditions, as well as in urban plumes, were observed. Perhaps most interestingly, several cases of squall lines preceding major aerosol events were observed, as opposed to 2011 observations where these lines largely scavenged aerosol particles from the marine boundary layer. Combined, these observations indicate pockets of high and low particle counts that are not uncommon in the region. These perturbations are difficult to observe by satellite and very difficult to model. Indeed, the Navy Aerosol Analysis and Prediction System (NAAPS) simulations captured longer period aerosol events quite well but largely failed to capture the timing of high-frequency phenomena. Ultimately, the research findings of these cruises demonstrate the real world challenges of satellite-based missions, significant aerosol life cycle questions such as those the future Aerosol/Clouds/Ecosystems (ACE) will investigate, and the importance of small-scale phenomena such as sea breezes, squall lines, and nucleation events embedded within SWM patterns in dominating aerosol life cycle and potential relationships to clouds.

Satellite and ground-based remote sensing of aerosols during intense haze event of October 2013 over lahore, Pakistan

NASA Astrophysics Data System (ADS)

Tariq, Salman; Zia, ul-Haq; Ali, Muhammad

2016-02-01

Due to increase in population and economic development, the mega-cities are facing increased haze events which are causing important effects on the regional environment and climate. In order to understand these effects, we require an in-depth knowledge of optical and physical properties of aerosols in intense haze conditions. In this paper an effort has been made to analyze the microphysical and optical properties of aerosols during intense haze event over mega-city of Lahore by using remote sensing data obtained from satellites (Terra/Aqua Moderate-resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO)) and ground based instrument (AErosol RObotic NETwork (AERONET)) during 6-14 October 2013. The instantaneous highest value of Aerosol Optical Depth (AOD) is observed to be 3.70 on 9 October 2013 followed by 3.12 on 8 October 2013. The primary cause of such high values is large scale crop residue burning and urban-industrial emissions in the study region. AERONET observations show daily mean AOD of 2.36 which is eight times higher than the observed values on normal day. The observed fine mode volume concentration is more than 1.5 times greater than the coarse mode volume concentration on the high aerosol burden day. We also find high values (~0.95) of Single Scattering Albedo (SSA) on 9 October 2013. Scatter-plot between AOD (500 nm) and Angstrom exponent (440-870 nm) reveals that biomass burning/urban-industrial aerosols are the dominant aerosol type on the heavy aerosol loading day over Lahore. MODIS fire activity image suggests that the areas in the southeast of Lahore across the border with India are dominated by biomass burning activities. A Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model backward trajectory showed that the winds at 1000 m above the ground are responsible for transport from southeast region of biomass burning to Lahore. CALIPSO derived sub-types of aerosols with vertical profile taken on 10 October 2013 segregates the wide spread aerosol burden as smoke, polluted continental and dust aerosols.

Seasonal variations in the physico-chemical characteristics of aerosols in North Taiwan

NASA Astrophysics Data System (ADS)

Chou, Charles

2014-05-01

From 2007 to 2012, this study investigated the mass concentration and chemical composition of ambient aerosols (i.e. PM10, PM2.5, and PMc = PM10-PM2.5) at Cape Fuguei, Yangminshan, and NTU (National Taiwan University) stations in northern Taiwan. It was found that the concentration and composition of aerosols exhibited significant seasonal variations but without an inter-annual trend during the study period. Moderate correlations (R2 = 0.4-0.6) were observed among the aerosol concentrations at the respective stations, indicating that the aerosol concentrations were dominated by factors on regional scales. During the seasons of northeasterly winter monsoons, long range transport of dust and particulate air pollutants from the Asia Continent had negatively impacted the atmospheric environment in this area. On the other hand, as a highly developed urban area, Taipei has substantial local emissions of air pollutants that should have transported to the surrounding areas of Taipei basin and caused deterioration of air quality and visibility in Cape Fuguei and Yangminshan. The results indicated that the major components of aerosols in Taipei include sulfate, sea salts, dust, and organic matters. In addition, contributions from nitrate, ammonium, and elemental carbon were also significant. In terms of mass concentration, most of the sea salts and dust particles existed in the coarse mode of aerosols, whereas sulfate and EC were confined within PM2.5. This suggests that the dust and sea salts particles were externally mixed with EC and sulfate in the aerosols over Taipei area. Further, it was found that nitrate were closely associated with sea salts in aerosols, suggesting the reaction between nitric acid and sea salt particles. Different seasonality was observed for sea salt and dust: sea salts peaked in fall and dust reached the maximal level in springtime, implying their sources were regulated by independent seasonal factors. Particulate pollutants (i.e. sulfate, nitrate, OM and EC) were consistently reaching their respective maxima in spring, agreeing with dust particle, suggesting the influences of long range transport of air pollutants. This study also found that both the mass fraction of OM in aerosols and OC/EC ratio exhibited peaks in summertime. Secondary organic aerosols (SOA) produced from photochemical reactions and heteo-nucleation were among the major factors controlling the seasonal variations of aerosol concentration in Taipei area. Because the formation of SOA could alter the interactions between aerosols and cloud/fog and, in turn, have potential impacts upon the regional radiation budget, this study suggests conduct an in-depth study upon the relationship between cloud condensation nuclei (CCN) and SOA in this region.

Stereoscopic Retrieval of Smoke Plume Heights and Motion from Space-Based Multi-Angle Imaging, Using the MISR INteractive eXplorer(MINX)

NASA Technical Reports Server (NTRS)

Nelson, David L.; Kahn, Ralph A.

2014-01-01

Airborne particles desert dust, wildfire smoke, volcanic effluent, urban pollution affect Earth's climate as well as air quality and health. They are found in the atmosphere all over the planet, but vary immensely in amount and properties with season and location. Most aerosol particles are injected into the near-surface boundary layer, but some, especially wildfire smoke, desert dust and volcanic ash, can be injected higher into the atmosphere, where they can stay aloft longer, travel farther, produce larger climate effects, and possibly affect human and ecosystem health far downwind. So monitoring aerosol injection height globally can make important contributions to climate science and air quality studies. The Multi-angle Imaging Spectro-Radiometer (MISR) is a space borne instrument designed to study Earths clouds, aerosols, and surface. Since late February 2000 it has been retrieving aerosol particle amount and properties, as well as cloud height and wind data, globally, about once per week. The MINX visualization and analysis tool complements the operational MISR data products, enabling users to retrieve heights and winds locally for detailed studies of smoke plumes, at higher spatial resolution and with greater precision than the operational product and other space-based, passive remote sensing techniques. MINX software is being used to provide plume height statistics for climatological studies as well as to investigate the dynamics of individual plumes, and to provide parameterizations for climate modeling.

Volatility Properties of Internally- and Externally-Mixed Ambient Aerosols at an Anthropogenically-influenced Forest Site in Southeastern USA

NASA Astrophysics Data System (ADS)

Khlystov, A.; Subramanian, R.

2015-12-01

Secondary organic aerosol (SOA) from biogenic sources has a significant contribution to ambient aerosol loadings in Southeastern USA and thus contributes to adverse health effects of air pollution and influences regional and global climate. Volatility properties of biogenic SOA determine its concentration, reactivity, and lifetime, but are still largely unknown. As part of a larger study to assess the effect of biogenic SOA on aerosol optical properties, a set of instruments, including scanning mobility sizers (SMPS), single particle soot photometer (SP2), and a thermodenuder, was deployed during June 2015 at a Duke Forest site near Chapel Hill, NC. The site is characterized by a significant contribution of both biogenic and urban (mostly traffic) sources. Measurements of changes in aerosol volume and optical size upon heating in the thermodenuder at different temperatures are used to derive volatility properties of the ambient aerosol. A limited set of experiments was carried out using the tandem differential mobility analysis (TDMA) approach to investigate whether the ambient aerosol at the Duke Forest site is internally mixed with respect to its volatility properties. In this presentation we will discuss equilibrium and kinetic aspects of aerosol volatility observed during this study and implications of external vs. internal mixing for derivation of bulk volatility properties of ambient aerosol.

CCN Activity of Organic Aerosols Observed Downwind of Urban Emissions during CARES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mei, Fan; Setyan, Ari; Zhang, Qi

2013-12-17

During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of CCN-active particles (K CCN) with diameter from 100 to 170 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites in earlier studies. The low K CCN value was due to the high organic volume fraction, averaged over 80% at the T1more » site. The derived K CCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size selected particles with diameter between 100 and 171nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (K org) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For vast majority of the cases, an increase of K org from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from K CCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m/z 44 (f 44) and O:C were compared to results from previous studies. Overall, the relationships between K org and f 44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in smog chamber. Compared to the relationship between K org and f 44, the relationship between K org and O:C exhibits more significant differences among different studies, suggesting korg may be better parameterized using f 44. A least squares fit yielded K org = 2.10 (±0.07) × f 44 -0.11 (±0.01) with the Pearson R 2 value of 0.71. One possible explanation for the stronger correlation between K org and f 44 is that the m/z 44 signal (mostly contributed by the CO 2 + ion) is more closely related to organic acids, which may dominate the overall korg due to their relatively high water solubility and hygroscopicity.« less

Connecting Water Quality With Air Quality Through Microbial Aerosols

NASA Astrophysics Data System (ADS)

Dueker, M. Elias

Aerosol production from surface waters results in the transfer of aquatic materials (including nutrients and bacteria) to air. These materials can then be transported by onshore winds to land, representing a biogeochemical connection between aquatic and terrestrial systems not normally considered. In urban waterfront environments, this transfer could result in emissions of pathogenic bacteria from contaminated waters. Despite the potential importance of this link, sources, near-shore deposition, identity and viability of microbial aerosols are largely uncharacterized. This dissertation focuses on the environmental and biological mechanisms that define this water-air connection, as a means to build our understanding of the biogeochemical, biogeographical, and public health implications of the transfer of surface water materials to the near-shore environment in both urban and non-urban environments. The effects of tidal height, wind speed and fog on coastal aerosols and microbial content were first quantified on a non-urban coast of Maine, USA. Culture-based, culture-independent, and molecular methods were used to simultaneously sample microbial aerosols while monitoring meteorological parameters. Aerosols at this site displayed clear marine influence and high concentrations of ecologically-relevant nutrients. Coarse aerosol concentrations significantly increased with tidal height, onshore wind speed, and fog presence. Tidal height and fog presence did not significantly influence total microbial aerosol concentrations, but did have a significant effect on culturable microbial aerosol fallout. Molecular analyses of the microbes settling out of near-shore aerosols provided further evidence of local ocean to terrestrial transport of microbes. Aerosol and surface ocean bacterial communities shared species and in general were dominated by organisms previously sampled in marine environments. Fog presence strengthened the microbial connection between water and land through air by increasing microbial aerosol settling rates and enhancing viability of aerosolized marine microbes. Using methods developed for the non-urban site, the role of local environment and winds in mediating water-air connections was further investigated in the urban environment. The local environment, including water surfaces, was an important source of microbial aerosols at urban sites. Large portions of the urban waterfront microbial aerosol communities were aquatic and, at a highly polluted Superfund waterfront, were closely related to bacteria previously described in environments contaminated with hydrocarbons, heavy metals, sewage and other industrial waste. Culturable urban aerosols and surface waters contained bacterial genera known to include human pathogens and asthma agents. High onshore winds strengthened this water-air connection by playing both a transport and production role. The microbial connection between water and air quality outlined by this dissertation highlights the need for information on the mechanisms that deliver surface water materials to terrestrial systems on a much larger scale. Moving from point measurements to landscape-level analyses will allow for the quantitative assessment of implications for this microbial water-air-land transfer in both urban and non-urban arenas.

Regional Aerosol Forcing over India: Preliminary Results from the South West Asian Aerosol-Monsoon Interactions (SWAAMI) Aircraft Experiment

NASA Astrophysics Data System (ADS)

Morgan, W.; Brooks, J.; Fox, C.; Haslett, S.; Liu, D.; Kompalli, S. K.; Pathak, H.; Manoj, M. R.; Allan, J. D.; Haywood, J. M.; Highwood, E.; Langridge, J.; Nanjundaiah, R. S.; Krishnamoorthy, K.; Babu, S. S.; Satheesh, S. K.; Turner, A. G.; Coe, H.

2016-12-01

Aerosol particles from multiple sources across the Indian subcontinent build up to form a dense and extensive haze across the region in advance of the monsoon. These aerosols are thought to perturb the regional radiative balance and hydrological cycle, which may have a significant impact on the monsoon circulation, as well as influencing the associated cloud and rainfall of the system. However the nature and magnitude of such impacts are poorly understood or constrained. Major uncertainties relevant to the regional aerosol burden include its vertical distribution, the relative contribution of different pollution sources and natural emissions and the role of absorbing aerosol species (black carbon and mineral dust). The South West Asian Aerosol-Monsoon Interactions (SWAAMI) project sought to address these major uncertainties by conducting an airborne experiment during June/July 2016 on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft. Based out of Lucknow in the), The aircraft conducted multiple flights from Lucknow in the heart of the Indo-Gangetic Plain (IGP) in advance of the monsoon and during the onset phase. The spatial and vertical distribution of aerosol was evaluated across northern India, encompassing drier desert-like regions to the west, heavily populated urban and industrial centres over the IGP and air masses in outflow regions to the south-east towards the Bay of Bengal. Principal measurements included aerosol chemical composition using an Aerodyne Aerosol Mass Spectrometer and a DMT Single Particle Soot Photometer, alongside a Leosphere backscatter LIDAR. Sulphate was a major contributor to the aerosol burden across India, while the organic aerosol was elevated and more dominant over the most polluted regions of the IGP. Substantial aerosol concentrations were frequently observed up to altitudes of approximately 6km, with notable changes in aerosol chemical and physical properties when comparing different layers between there and the surface. Black carbon concentrations were enhanced at lower altitudes (approximately 0-2km), with reduced concentrations above this. Further observations will be presented and used to characterise the regional aerosol burden and its associated interactions with the monsoon.

Using Smart Planning to Mitigate Drought in Urban Areas: A Seasonal Simulation of the Impact of Urbanization on Precipitation in the Indianapolis Region

NASA Astrophysics Data System (ADS)

Schmid, P. E.; Niyogi, D.

2012-12-01

The Indianapolis region exhibits a precipitation distribution indicative of urban weather modification: negative bias upwind and positive bias downwind. The causes for such a distribution within an urban area arise from a combination of land-surface heterogeneity and urban aerosol-cloud interaction. This study investigates the causes of the precipitation distribution with a 120-day simulation using the Regional Atmospheric Modeling System (RAMS) coupled with the Town Energy Budget (TEB) model. Using a nested grid with a maximum resolution of 500m, a seasonal simulation of May through August, 2008 is conducted. Land surface conditions are varied, removing, expanding, and intensifying the Indianapolis urban area. Aerosol conditions are scaled by a three-dimensional combination of MODIS and CALIPSO observations, and varied in concentration and plume extent. Results from the study demonstrate the paradigm of urban precipitation modification on a seasonal time scale. The boundary between the rural and urban land surfaces weakens approaching systems upwind, decreasing precipitation in the city center. A larger urban extent diminishes the systems further. The aerosol plume downwind increases cloud lifetimes via cloud-nucleating aerosol, then invigorates precipitation via large drizzle-invigorating aerosols. The overall effect reproduces the observed negative precipitation bias upwind and positive bias downwind of the urban center. A lower concentration of aerosols leads to a higher proportion of stratiform rain over a larger area, whereas a higher concentration of aerosols leads to more convective rain and heavy rain events. This manifests in a weekly cycle of precipitation with rain most likely on weekends, and with less frequent but heavier rain events most likely during midweek, when aerosol concentrations are the highest. More intense urbanization, via both land surface and aerosol effects, creates more frequent heavy rainfall events and exacerbates dry-periods, potentially leading to premature drought onset. The wetter than average May, June, and July received more total rainfall from the heavy rainfall events, while the dry August became drier due to lack of stratiform precipitation. Smart planning solutions can partially mitigate the urban precipitation problem. In a simulation where a more intense urban Indianapolis is surrounded by a greenbelt and green roofs are implemented in the city, the urban precipitation bias becomes less significant. Upwind, the greenbelt provides surface moisture and mitigates how much precipitation systems weaken. Downwind, the greenbelt slows the transport of drizzle-invigorating aerosol, reducing the heavy rain events. The green roofs reduce the urban-rural gradient and slow the initial weakening of systems.

Ammonium Nitrate Formation near the Colorado Front Range

NASA Astrophysics Data System (ADS)

Middlebrook, A. M.; Bahreini, R.; Brock, C. A.; Brown, S. S.; Cozic, J.; Frost, G. J.; Langford, A. O.; Lerner, B. M.; Matthew, B.; McKeen, S. A.; Neuman, J.; Nowak, J. B.; Peischl, J. W.; Quinn, P.; Ryerson, T. B.; Schultz, K.; Stark, H.; Trainer, M.; Wagner, N.; Williams, E. J.; Wollny, A. G.

2009-12-01

A significant air quality issue during wintertime temperature inversions along the Colorado Front Range urban corridor is the infamous “Brown Cloud” which is dominated by ammonium nitrate particles. Aerosol composition, size distribution, and gas phase measurements were obtained along with meteorology in Boulder-based ground studies during the winters of 2005 and 2009 and in an airborne survey over the Colorado Front Range urban corridor and northeastern Colorado on April 1, 2008. New in these campaigns was the fast time response data which showed that nitric acid was partitioned mainly into the aerosol phase as ammonium nitrate. During the survey flight, ammonium nitrate mass concentrations were highest on the west side of the urban corridor whereas nitrogen oxide concentrations were highest directly west and south of Denver. Nitric acid concentrations were highest south of the city. The calculated equilibrium gas phase ammonia was highest close to the ground directly around large feed lots near Brush and west of Greeley. These differences are consistent with what is known about the locations of emission sources, the predominant flow during the experiments, and the chemistry. Indeed, the ammonia emissions in the northern part of the region are sufficiently high to cause ammonium nitrate formation to be limited by nitric acid whereas in the southern part of the region ammonium nitrate formation was limited by low ammonia emissions. Although NOx (NO + NO2) emissions in the region are much larger than those for ammonia, NOx must be converted into nitric acid in order for ammonium nitrate to form. In the survey data, aerosol nitrate was correlated with the daytime nitric acid production rate but with higher slopes in the northern parts of the region. In the longer Boulder datasets, the calculated daytime production rate was slow and comparable to nighttime heterogeneous production via N2O5 hydrolysis. During periods of low aerosol surface area, daytime and nighttime production of nitric acid resulted in freshly formed ammonium nitrate particles. These results suggest that reductions in NOx emissions along the northern part of the region are likely to decrease the prevalence of the Brown Cloud.

High Resolution Aerosol Data from MODIS Satellite for Urban Air Quality Studies

NASA Technical Reports Server (NTRS)

Chudnovsky, A.; Lyapustin, A.; Wang, Y.; Tang, C.; Schwartz, J.; Koutrakis, P.

2013-01-01

The Moderate Resolution Imaging Spectroradiometer (MODIS) provides daily global coverage, but the 10 km resolution of its aerosol optical depth (AOD) product is not suitable for studying spatial variability of aerosols in urban areas. Recently, a new Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm was developed for MODIS which provides AOD at 1 km resolution. Using MAIAC data, the relationship between MAIAC AOD and PM(sub 2.5) as measured by the 27 EPA ground monitoring stations was investigated. These results were also compared to conventional MODIS 10 km AOD retrievals (MOD04) for the same days and locations. The coefficients of determination for MOD04 and for MAIAC are R(exp 2) =0.45 and 0.50 respectively, suggested that AOD is a reasonably good proxy for PM(sub 2.5) ground concentrations. Finally, we studied the relationship between PM(sub 2.5) and AOD at the intra-urban scale (10 km) in Boston. The fine resolution results indicated spatial variability in particle concentration at a sub-10 kilometer scale. A local analysis for the Boston area showed that the AOD-PM(sub 2.5) relationship does not depend on relative humidity and air temperatures below approximately 7 C. The correlation improves for temperatures above 7 - 16 C. We found no dependence on the boundary layer height except when the former was in the range 250-500 m. Finally, we apply a mixed effects model approach to MAIAC aerosol optical depth (AOD) retrievals from MODIS to predict PM(sub 2.5) concentrations within the greater Boston area. With this approach we can control for the inherent day-to-day variability in the AOD-PM(sub 2.5) relationship, which depends on time-varying parameters such as particle optical properties, vertical and diurnal concentration profiles and ground surface reflectance. Our results show that the model-predicted PM(sub 2.5) mass concentrations are highly correlated with the actual observations (out-of-sample R(exp 2) of 0.86). Therefore, adjustment for the daily variability in the AOD-PM(sub 2.5) relationship provides a means for obtaining spatially-resolved PM(sub 2.5) concentrations.

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

NASA Technical Reports Server (NTRS)

Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

1980-01-01

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Environment Partitioning and Reactivity of Polybrominated Diphenylethers

NASA Technical Reports Server (NTRS)

Hua, Inez; Iraci, Laura T.; Jafvert, Chad; Bezares-Cruz, Juan

2004-01-01

Polybrominated diphenyl ethers (PBDEs) are an important class of flame retardants. Annual global demand for these compounds was over 67,000 metric tons in 2001. PBDEs have recently been extensively investigated as environmental contaminants because they have been detected in air, sediment, and tissue samples from urban and remote areas. Important issues include quantifying PBDE partitioning in various environmental compartments, and elucidating transformation pathways. The partitioning of PBDE congeners to aerosols was estimated for 16 sites in the United States, Canada, and Mexico. The aerosol particles were PM2.5, the total suspended particle (TSP) concentration varied between 3.0 - 55.4 micro g/cubic meter, and the organic fraction ranged from 11 - 41%; these data are published values for each site. It is estimated that the largest fraction of each PBDE associated with the aerosol particles occurs in Mexico City, and the smallest fraction in Colorado Plateau. Although the organic fraction in Mexico City is about 60% of that observed in the Colorado Plateau, the TSP is larger by a factor of about 18.5, and it is the difference in TSP that strongly influences the fraction of particle-bound PBDE in this case. PBDE partitioning to PM2.5 particles also varies seasonally because of temperature variations. For the less brominated congeners the percentage that is particle-bound is relatively low, regardless of air temperature. In contrast, the heavier congeners exhibit a significant temperature dependence: as the temperature decreases (fall, winter) the percentage of PBDE that is particle-bound increases. The partitioning calculations complement experimental data indicating that decabromodiphenyl ether (DBDE) dissolved in hexane transforms very rapidly when irradiated with solar light. DBDE is the most highly brominated PBDE congener (10 bromine atoms) and occurs in the commercial formulation which is subject to the largest global demand.

Environmental Partitioning and Reactivity of Polybrominated Diphenylethers

NASA Astrophysics Data System (ADS)

Hua, I.; Iraci, L.; Jafvert, C.; Bezares-Cruz, J.

2004-05-01

Polybrominated diphenyl ethers (PBDEs) are an important class of flame retardants. Annual global demand for these compounds was over 67,000 metric tons in 2001. PBDEs have recently been extensively investigated as environmental contaminants because they have been detected in air, sediment, and tissue samples from urban and remote areas. Important issues include quantifying PBDE partitioning in various environmental compartments, and elucidating transformation pathways. The partitioning of PBDE congeners to aerosols was estimated for 16 sites in the United States, Canada, and Mexico. The aerosol particles were PM2.5, the total suspended particle (TSP) concentration varied between 3.0 - 55.4 μ g m-3, and the organic fraction ranged from 11 - 41%; these data are published values for each site. It is estimated that the largest fraction of each PBDE associated with the aerosol particles occurs in Mexico City, and the smallest fraction in Colorado Plateau. Although the organic fraction in Mexico City is about 60% of that observed in the Colorado Plateau, the TSP is larger by a factor of about 18.5, and it is the difference in TSP that strongly influences the fraction of particle-bound PBDE in this case. PBDE partitioning to PM2.5 particles also varies seasonally because of temperature variations. For the less brominated congeners, the percentage that is particle-bound is relatively low, regardless of air temperature. In contrast, the heavier congeners exhibit a significant temperature dependence: as the temperature decreases (fall, winter) the percentage of PBDE that is particle-bound increases. The partitioning calculations complement experimental data indicating that decabromodiphenyl ether (DBDE) dissolved in hexane transforms very rapidly when irradiated with solar light. DBDE is the most highly brominated PBDE congener (10 bromine atoms) and occurs in the commercial formulation which is subject to the largest global demand.

Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Huang, X.-F.; He, L.-Y.; Hu, M.; Canagaratna, M. R.; Sun, Y.; Zhang, Q.; Zhu, T.; Xue, L.; Zeng, L.-W.; Liu, X.-G.; Zhang, Y.-H.; Jayne, J. T.; Ng, N. L.; Worsnop, D. R.

2010-09-01

As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008), an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008). The campaign mean PM1 mass concentration was 63.1 ± 39.8 μg m-3; the mean composition consisted of organics (37.9%), sulfate (26.7%), ammonium (15.9%), nitrate (15.8%), black carbon (3.1%), and chloride (0.87%). The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF) analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA), cooking-related (COA), and two oxygenated organic aerosols (OOA-1 and OOA-2), which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C) compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses contained a large fraction of primary HOA and COA species, probably due to stronger influences from local emissions. The lowest concentration levels for all major species were obtained during the Olympic game days (8 to 24 August 2008), possibly due to the effects of both strict emission controls and favorable meteorological conditions.

Micrometeorological flux measurements of aerosol and gases above Beijing

NASA Astrophysics Data System (ADS)

Nemitz, Eiko; Langford, Ben; Mullinger, Neil; Cowan, Nicholas; Coyle, Mhairi; Acton, William Joe; Lee, James; Fu, Pingqing

2017-04-01

Air pollution is estimated to cause 1.6 million premature deaths in China every year and in the winter 2016/17 Beijing had to issue health alerts and put in place ad hoc limitations on industrial and vehicular activity. Much of this pollution is attributed to emissions from industrial processes and in particular coal combustion. By contrast, the diffuse pollutant sources within the city are less well understood. This includes, e.g., emissions from the Beijing traffic fleet, the sewage system, food preparation, solid fuel combustion in the streets and small industrial processes. Within the framework of a major UK-Chinese collaboration to study air pollution and its impact on human health in Beijing, we therefore measured fluxes of a large range of pollutants from a height of 102 m on the 325 m meteorological tower at the Institute of Atmospheric Physics. Several instruments were mounted at 102 m: fluxes of CO2 and H2O were measured with an infrared gas analyser (LiCOR 7500) and fluxes of ozone with a combination of a relative fast-response ozone analyser (ROFI) and a 2B absolute O3 instrument. Total particle number fluxes were measured with a condensation particle counter (TSI CPC 3785), and size-segregated fluxes over the size range 0.06 to 20 μm with a combination of an optical Ultrafine High Sensitivity Aerosol Spectrometer (UHSAS) and an Aerodynamic Particle Sizer Spectrometer (TSI APS3321). Ammonia (NH3) fluxes were measured for the first time above the urban environment using an Aerodyne compact quantum cascade laser (QCL). In addition, composition resolved aerosol fluxes were measured with an Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS), operated in a measurement container at the bottom of the tower, which subsampled from a 120 m long copper tube (15 mm OD). The analysis so far suggests that, due to often low wind speeds, fluxes were at times de-coupled from the surface. Fluxes normalised by CO2, a tracer for the amount of fossil fuel consumed, should be less sensitive to transport effects. However, not only fluxes, but also these CO2-ratioed fluxes are highly variable in both space and time, indicating a complex mix of sources, which will be further investigated. The organic aerosol fluxes were the largest we have recorded to date at any urban measurement site. Nitrate, sulphate, chloride and ammonium all showed emissions that followed a similar diurnal cycle as the organic aerosol. Much of this aerosol is likely to have been formed by chemistry below the measurement height, but it nevertheless indicates significant sources of the precursor gases within the footprint. Comparing the measured fluxes of gas-phase NH3 and aerosol NH4+, at 102 m the aerosol phase makes a significant contribution to the reduced nitrogen emission.

Variability of aerosol, gaseous pollutants and meteorological characteristics associated with continental, urban and marine air masses at the SW Atlantic coast of Iberia

NASA Astrophysics Data System (ADS)

Diesch, J.-M.; Drewnick, F.; Zorn, S. R.; von der Weiden-Reinmüller, S.-L.; Martinez, M.; Borrmann, S.

2011-12-01

Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM1 and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) and a weather station provided meteorological parameters. Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m-3 and 1000 cm-3. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM1-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54%) was detected in marine air masses and was to a high degree not neutralized. In addition small concentrations of methanesulfonic acid (MSA), a product of biogenic dimethyl sulfate (DMS) emissions could be identified in the particle phase. In all air masses passing the continent the organic aerosol fraction dominated the total NR-PM1. For this reason, using Positive Matrix Factorization (PMF) four organic aerosol (OA) classes that can be associated with various aerosol sources and components were identified: a highly-oxygenated OA is the major component contributing an average of 43% of the particulate organic mass while the semi-volatile OA accounts for 23%. A hydrocarbon-like OA mainly resulting from industries, traffic and shipping emissions as well as particles from wood burning emissions also contribute to total OA dependent on the air mass origin. The variability of ozone is not only affected by different types of air masses but also significantly by the diurnal variation as a consequence of the solar radiation as well as local meteorological parameters.

Urban PM in Eastern Germany: Source apportionment and contributions from different spatial scales

NASA Astrophysics Data System (ADS)

van Pinxteren, D.; Fomba, K. W.; Mothes, F.; Spindler, G.; Herrmann, H.

2017-12-01

Understanding the contributions of particulate matter (PM) sources and the source areas impacting total PM levels in a city are important requirements for further developing clean air policies and efficient abatement strategies. This presentation reports on two studies in Eastern Germany providing a detailed picture of present-day urban PM sources and discriminating contributions of local, regional and long-range sources. The "Leipzig Aerosol 2013-15" study yielded contributions of 12 sources to coarse, fine, and ultrafine particles, resolved by Positive Matrix Factorization (PMF) from comprehensive chemical speciation of 5-stage Berner impactor samples at 4 different sites in the Leipzig area. Dominant winter-time sources were traffic exhaust and non-exhaust emissions, secondary aerosol formation, and combustion emissions from both biomass and coal burning with different relative importance in different particle size ranges. Local sources dominated PM levels in ultrafine and coarse particles (60% - 80%) while high mass concentrations in accumulation mode particles mainly resulted from regional import into the city (70%). The "PM-East" study compiled PM10 mass and constituents' concentrations at 10 urban and rural sites in Eastern Germany during winter 2016/17, which included a 3-week episode of frequent exceedances of the PM10 limit value. PMF source apportionment is performed for a subset of the sites, including the city of Berlin. Contributions from short-, mid-, and long-range sources, including trans-boundary pollution import from neighbouring countries, are quantitatively assessed by advanced back trajectory statistical methods. Data analysis in PM-East is ongoing and final results will be available by November. Funding is acknowledged from 4 federal states of Germany: Berlin Senate Department for Environment, Transport and Climate Protection; Saxon State Office for Environment, Agriculture and Geology; State Agency for Environment, Nature Conservation and Geology Mecklenburg-Vorpommern; and Brandenburg State Office for Environment.

The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

PubMed

Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

2015-06-24

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

Wintertime aerosol in Las Vegas, Nevada

NASA Astrophysics Data System (ADS)

Brown, Steven G.

Numerous studies have found adverse health effects in subjects who live next to major roadways due to air pollution; in particular, there can be severe impacts on lung function and development in children living and/or attending school next to major roadways due to their exposure to air pollutants, including particulate matter (PM) or aerosol. The composition of aerosol at an elementary school next to a major freeway in Las Vegas, Nevada during winter 2008 was measured using a suite of measurements. An Aerodyne High Resolution Aerosol Mass Spectrometer (HR-AMS) was used to quantify the composition of non-refractory PM1 aerosol, including organic matter (OM); an Aethalometer was used to quantify black carbon (BC); a Sunset OCEC analyzer was used to measure organic and elemental carbon (OC, EC); and a particle-into-liquid system (PILS) coupled to two ion chromatographs (IC) was used to measure fine particle ions. Hi-volume PM2.5 samplers were used to collect aerosol on quartz fiber filters at between 2 and 24 hour intervals during the study, a subset of which were analyzed for PAHs and the biomass burning tracer levoglucosan. Data were analyzed by positive matrix factorization (PMF) to determine the amount of fresh, hydrocarbon-like organic aerosol (HOA), more oxidized OA (low-volatility and semi-volatile OA [LV-OOA, SV-OOA]) and biomass burning OA (BBOA). PM1 aerosol was predominantly carbonaceous, with OM plus BC accounting for 74% of the overall average 6.9 mug/m3 of PM measured. BC had a diurnal pattern similar to traffic volume, while OM was higher in the evening compared to the morning. OM was a mixture of fresh HOA, urban- and regional-scale OOA, and BBOA; in the evening, SV-OOA and BBOA peaked, while HOA concentrations were on average the same in the morning and evening, similar to BC. OM/OC ratios were low (1.52 +/-0.14 on average) during the morning rush hour (average OM = 2.4 mug/m3) when vehicular emissions dominate this near-road measurement site, and even lower (1.46 +/- 0.10) in the evening (average OM=6.3 mug/m3), when a combination of vehicular and fresh residential biomass burning emissions was typically present during a period characterized by strong atmospheric stability. While nitrate and sulfate had size distributions typical of secondary species with a sharp peak in particle diameter between 400 nm and 500 nm, OM had a broader distribution between 100 nm and 400 nm diameter particles, reflecting its combination of fresh, smaller particles and aged, larger particles. OM concentrations were on average similar between periods when the sampling site was upwind and downwind of the freeway, though during the morning OM concentrations were higher under downwind conditions, as was the fraction of HOA.

Mechanical Properties of the Surface Material of Comet 67P/Churyumov-Gerasimenko Measured By the Casse Instrument Onboard the Philae Lander

NASA Astrophysics Data System (ADS)

Knapmeyer, M.; Fischer, H. H.; Seidensticker, K. J.; Arnold, W.; Faber, C.; Möhlmann, D.; Thiel, K.

2014-12-01

Satellite remote sensing of ocean color is a critical tool for assessing the productivity of marine ecosystems and monitoring changes resulting from climatic or environmental influences. Yet water-leaving radiance comprises less than 10% of the signal measured from space, making correction for absorption and scattering by the intervening atmosphere imperative. Traditional ocean color retrieval algorithms utilize a standard set of aerosol models and the assumption of negligible water-leaving radiance in the near-infrared. Modern improvements have been developed to handle absorbing aerosols such as urban particulates in coastal areas and transported desert dust over the open ocean, where ocean fertilization can impact biological productivity at the base of the marine food chain. Even so, imperfect knowledge of the absorbing aerosol optical properties or their height distribution results in well-documented sources of error. In the UV, the problem of UV-enhanced absorption and nonsphericity of certain aerosol types are amplified due to the increased Rayleigh and aerosol optical depth, especially at off-nadir view angles. Multi-angle spectro-polarimetric measurements have been advocated as an additional tool to better understand and retrieve the aerosol properties needed for atmospheric correction for ocean color retrievals. The central concern of the work to be described is the assessment of the effects of absorbing aerosol properties on water leaving radiance measurement uncertainty by neglecting UV-enhanced absorption of carbonaceous particles and by not accounting for dust nonsphericity. In addition, we evaluate the polarimetric sensitivity of absorbing aerosol properties in light of measurement uncertainties achievable for the next generation of multi-angle polarimetric imaging instruments, and demonstrate advantages and disadvantages of wavelength selection in the UV/VNIR range. The phase matrices for the spherical smoke particles were calculated using a standard Mie code, while those for non-spherical dust particles were calculated using the numerical approach described by Dubovik et al., 2006. A vector Markov Chain radiative transfer code including bio-optical models was used to evaluate TOA and water leaving radiances.

Fluorescence lifetime imaging of optically levitated aerosol: a technique to quantitatively map the viscosity of suspended aerosol particles.

PubMed

Fitzgerald, C; Hosny, N A; Tong, H; Seville, P C; Gallimore, P J; Davidson, N M; Athanasiadis, A; Botchway, S W; Ward, A D; Kalberer, M; Kuimova, M K; Pope, F D

2016-08-21

We describe a technique to measure the viscosity of stably levitated single micron-sized aerosol particles. Particle levitation allows the aerosol phase to be probed in the absence of potentially artefact-causing surfaces. To achieve this feat, we combined two laser based techniques: optical trapping for aerosol particle levitation, using a counter-propagating laser beam configuration, and fluorescent lifetime imaging microscopy (FLIM) of molecular rotors for the measurement of viscosity within the particle. Unlike other techniques used to measure aerosol particle viscosity, this allows for the non-destructive probing of viscosity of aerosol particles without interference from surfaces. The well-described viscosity of sucrose aerosol, under a range of relative humidity conditions, is used to validate the technique. Furthermore we investigate a pharmaceutically-relevant mixture of sodium chloride and salbutamol sulphate under humidities representative of in vivo drug inhalation. Finally, we provide a methodology for incorporating molecular rotors into already levitated particles, thereby making the FLIM/optical trapping technique applicable to real world aerosol systems, such as atmospheric aerosols and those generated by pharmaceutical inhalers.

High Spatial Resolution of Atmospheric Particle Mixing State and Its Links to Particle Evolution in a Metropolitan Area

NASA Astrophysics Data System (ADS)

Ye, Q.; Gu, P.; Li, H.; Robinson, E. S.; Apte, J.; Sullivan, R. C.; Robinson, A. L.; Presto, A. A.; Donahue, N.

2017-12-01

Traditional air quality studies in urban areas have mostly relied on very few monitoring locations either at urban background sites or at roadside sites.However, air pollution is highly complex and dynamic and will undergo complicated transformations. Therefore, results from one or two monitoring sites may not be sufficient to address the spatial gradients of pollutants and their evolution after atmosphere processing on a local scale. Our study, as part of the Center for Air, Climate, and Energy Solutions, performed stratified mobile sampling of atmospheric particulate matter with high spatial resolution to address intra-city variability of atmospheric particle composition and mixing state. A suite of comprehensive real-time instrumentations including a state-of-the-art aerosol mass spectrometer with single particle measurement capability are deployed on the mobile platform. Our sampling locations covered a wide variety of places with substantial differences in emissions and land use types including tunnels, inter-state highways, commercial areas, residential neighborhood, parks, as well as locations upwind and downwind of the city center. Our results show that particles from traffic emissions and restaurant cookings are two major contributors to fresh particles in the urban environment. In addition, there are large spatial variabilities of source-specific particles and we identify the relevant physicochemical processes governing transformation of particle composition, size and mixing state. We also combine our results with demographic data to study population exposure to particles of specific sources. This work will help evaluate the performance of existing modeling tools for air quality and population exposure studies.

Global combustion sources of organic aerosols: model comparison with 84 AMS factor-analysis data sets

NASA Astrophysics Data System (ADS)

Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

2016-07-01

Emissions of organic compounds from biomass, biofuel, and fossil fuel combustion strongly influence the global atmospheric aerosol load. Some of the organics are directly released as primary organic aerosol (POA). Most are emitted in the gas phase and undergo chemical transformations (i.e., oxidation by hydroxyl radical) and form secondary organic aerosol (SOA). In this work we use the global chemistry climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) with a computationally efficient module for the description of organic aerosol (OA) composition and evolution in the atmosphere (ORACLE). The tropospheric burden of open biomass and anthropogenic (fossil and biofuel) combustion particles is estimated to be 0.59 and 0.63 Tg, respectively, accounting for about 30 and 32 % of the total tropospheric OA load. About 30 % of the open biomass burning and 10 % of the anthropogenic combustion aerosols originate from direct particle emissions, whereas the rest is formed in the atmosphere. A comprehensive data set of aerosol mass spectrometer (AMS) measurements along with factor-analysis results from 84 field campaigns across the Northern Hemisphere are used to evaluate the model results. Both the AMS observations and the model results suggest that over urban areas both POA (25-40 %) and SOA (60-75 %) contribute substantially to the overall OA mass, whereas further downwind and in rural areas the POA concentrations decrease substantially and SOA dominates (80-85 %). EMAC does a reasonable job in reproducing POA and SOA levels during most of the year. However, it tends to underpredict POA and SOA concentrations during winter indicating that the model misses wintertime sources of OA (e.g., residential biofuel use) and SOA formation pathways (e.g., multiphase oxidation).

Chemical characteristics of size-resolved aerosols in winter in Beijing.

PubMed

Sun, Kang; Qu, Yu; Wu, Qiong; Han, Tingting; Gu, Jianwei; Zhao, Jingjing; Sun, Yele; Jiang, Qi; Gao, Ziqi; Hu, Min; Zhang, Yuanhang; Lu, Keding; Nordmann, Stephan; Cheng, Yafang; Hou, Li; Ge, Hui; Furuuchi, Masami; Hata, Mitsuhiko; Liu, Xingang

2014-08-01

Size-resolved aerosols were continuously collected by a Nano Sampler for 13 days at an urban site in Beijing during winter 2012 to measure the chemical composition of ambient aerosol particles. Data collected by the Nano Sampler and an ACSM (Aerodyne Aerosol Chemical Speciation Monitor) were compared. Between the data sets, similar trends and strong correlations were observed, demonstrating the validity of the Nano Sampler. PM₁₀ and PM₂.₅ concentrations during the measurement were 150.5 ± 96.0 μg/m³ (mean ± standard variation) and 106.9 ± 71.6 μg/m³, respectively. The PM₂.₅/PM₁₀ ratio was 0.70 ± 0.10, indicating that PM₂.₅ dominated PM₁₀. The aerosol size distributions showed that three size bins of 0.5-1, 1-2.5 and 2.5-10 μm contributed 21.8%, 23.3% and 26.0% to the total mass concentration (TMC), respectively. OM (organic matter) and SIA (secondary ionic aerosol, mainly SO₄(2-), NO₃(-) and NH₄(+)) were major components of PM₂.₅. Secondary compounds (SIA and secondary organic carbon) accounted for half of TMC (about 49.8%) in PM₂.₅, and suggested that secondary aerosols significantly contributed to the serious particulate matter pollution observed in winter. Coal burning, biomass combustion, vehicle emissions and SIA were found to be the main sources of PM₂.₅. Mass concentrations of water-soluble ions and undetected materials, as well as their fractions in TMC, strikingly increased with deteriorating particle pollution conditions, while OM and EC (elemental carbon) exhibited different variations, with mass concentrations slightly increasing but fractions in TMC decreasing. Copyright © 2014. Published by Elsevier B.V.

Molecular Characterization of Organosulfates in Urban Aerosols during the Spring Festival by FT-ICR Mass Spectrometry

NASA Astrophysics Data System (ADS)

Xie, Q.; Fu, P.

2017-12-01

Aerosol particles collected at daytime and nighttime in Beijing during the spring festival, including the episodes of various gradient level pollution and short-term pollution raised by fireworks, were analyzed using 15T Fourier transform ion cyclotron resonance mass spectrometry (FT-ICRMS). Organosulfates (OSs), tracers for secondary organic aerosol formation, were identified through accurate mass measurements. Both the total number and the arbitrary abundance of OSs were consistent with the total OC concentrations of the aerosol samples. Nitrooxy-organosulfates were more abundant in the nighttime than those in the daytime due to high NOX concentrations at night. Although all subgroups OSs increased with the deterioration of air quality, especially for the relative abundance of aromatic OSs with high double bond equivalents, the percentage contributions of aliphatic OSs with low degree of unsaturation decreased. It was worth to note that aliphatic OSs with a wide range in carbon-chain length of C6-40 were identified in this study. The candidates for their potential precursors were alkanes and fatty acids. Moreover, a large number of aromatic OSs, about two thirds of OSs, were detected. The rapid formation of these compounds in New Year's Eve with plentiful aromatics from firework burning suggests that they may be derived from PAHs. The high carbon and oxygen contents of OSs may indicate the presence of dimmers, even polymers. Our results support the important contribution of anthropogenic precursors to OSs in ambient aerosols on the basis of aromatic and aliphatic OSs, which may have a significant impact on the hygroscopic properties of ambient aerosol particles.

Formation kinetics and abundance of organic nitrates in α-pinene ozonolysis

NASA Astrophysics Data System (ADS)

Berkemeier, Thomas; Ammann, Markus; Pöschl, Ulrich; Shiraiwa, Manabu

2016-04-01

Formation of organic nitrates affects the total atmospheric budget of oxidized nitrogen (NOy) and alters the total aerosol mass yield from secondary sources. We investigated the formation of organic nitrate species during ozonolysis of α-pinene and subsequent formation of secondary organic aerosols (SOA) using the short-lived radioactive tracer 13N inside an aerosol flow reactor (Ammann et al., 2001). The results represent direct measurements of the organic nitrate content of α-pinene secondary aerosol and give insight into the kinetics of organic nitrate formation. Organic nitrates constituted up to 40 % of aerosol mass with a pronounced influence during the initial period of particle growth. Kinetic modelling, as well as additional experiments using OH scavengers and UV irradiation, suggests that organic peroxy radicals (RO2) from the reaction of α-pinene with secondarily produced OH are important intermediates in the organic nitrate formation process. Direct oxidation of α-pinene by NO3 was found to be a less efficient pathway for formation of particle phase nitrate. The organic nitrate content decreased very slightly with an increase of relative humidity on the experimental time scale. The experiments show a tight correlation between organic nitrate content and SOA number concentrations, implying that organic nitrates play an important role in nucleation and growth of nanoparticles. Since present in large amounts in organic aerosol, organic nitrates deposited in the lung might have implications for human health as they release nitric acid upon hydrolysis, especially in regions influenced by urban pollution and large sources of monoterpene SOA precursors. References Ammann et al. (2001) Radiochimica Acta 89, 831.

Long-range Transported African Dust in the Caribbean Region: Dust Concentrations and Water-soluble Ions

NASA Astrophysics Data System (ADS)

Santos-Figueroa, G.; Avilés-Piñeiro, G. M.; Mayol-Bracero, O. L.

2017-12-01

Long-range transported African dust (LRTAD) particles reach the Caribbean region every year during the summer months causing an increase in PM10 concentrations and by consequence degradation of air quality. During African dust (AD) incursions at the Caribbean region, PM10 concentration could exceeds the exposure limit of 50 µg/m³ 24-hour mean established by the World Health Organization (WHO). To have a better understanding of the impacts of AD particles to climate and public health at the Caribbean region it is necessary to study and determine the spatial and temporal distribution of dust particles. In order to address this, aerosols samples were collected during and absence of AD incursions during the summer of 2017 using a Hi-Volume (Hi-Vol) sampler for total suspended particles (TSP) at two sampling stations in Puerto Rico. The first station is a marine site located at Cabezas de San Juan (CSJ) Nature Reserve in Fajardo, and the second station is an urban site located at the Facundo Bueso (FB) building at the University of Puerto Rico-Rio Piedras. Aerosol samples were collected using Whatman 41 grade filters from which we determined the concentration of dust particles and the water-soluble ions (e.g., Na+, NH4+, Ca+2, Cl-, SO4-2) in the presence and absence of LRTAD particles. Saharan Air Layer (SAL) imagery, the results from the air mass backward trajectories calculated with the NOAA Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT), and the spectral coefficients from measurements at CSJ were used to monitor and confirm the presence of air masses coming from North Africa. Average dust concentrations using the Stacked-Filter Units (SFUs) at CSJ are around 4 μg/m3. LRTAD concentrations and ionic speciation results using the Hi-Vol for the marine and urban sites will be presented at the conference.

Modeling particle nucleation and growth over northern California during the 2010 CARES campaign

NASA Astrophysics Data System (ADS)

Lupascu, A.; Easter, R.; Zaveri, R.; Shrivastava, M.; Pekour, M.; Tomlinson, J.; Yang, Q.; Matsui, H.; Hodzic, A.; Zhang, Q.; Fast, J. D.

2015-11-01

Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10-40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20-30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.

Vertical distribution of aerosol optical properties in the Po Valley during the 2012 summer campaigns

NASA Astrophysics Data System (ADS)

Bucci, Silvia; Cristofanelli, Paolo; Decesari, Stefano; Marinoni, Angela; Sandrini, Silvia; Größ, Johannes; Wiedensohler, Alfred; Di Marco, Chiara F.; Nemitz, Eiko; Cairo, Francesco; Di Liberto, Luca; Fierli, Federico

2018-04-01

Studying the vertical distribution of aerosol particle physical and chemical properties in the troposphere is essential to understand the relative importance of local emission processes vs. long-range transport for column-integrated aerosol properties (e.g. the aerosol optical depth, AOD, affecting regional climate) as well as for the aerosol burden and its impacts on air quality at the ground. The main objective of this paper is to investigate the transport of desert dust in the middle troposphere and its intrusion into the planetary boundary layer (PBL) over the Po Valley (Italy), a region considered one of the greatest European pollution hotspots for the frequency that particulate matter (PM) limit values are exceeded. Events of mineral aerosol uplift from local (soil) sources and phenomena of hygroscopic growth at the ground are also investigated, possibly affecting the PM concentration in the region as well. During the PEGASOS 2012 field campaign, an integrated observing-modelling system was set up based on near-surface measurements (particle concentration and chemistry), vertical profiling (backscatter coefficient profiles from lidar and radiosoundings) and Lagrangian air mass transport simulations by FLEXPART model. Measurements were taken at the San Pietro Capofiume supersite (44°39' N, 11°37' E; 11 m a.s.l.), located in a rural area relatively close to some major urban and industrial emissive areas in the Po Valley. Mt. Cimone (44°12' N, 10°42' E; 2165 m a.s.l.) WMO/GAW station observations are also included in the study to characterize regional-scale variability. Results show that, in the Po Valley, aerosol is detected mainly below 2000 m a.s.l. with a prevalent occurrence of non-depolarizing particles ( > 50 % throughout the campaign) and a vertical distribution modulated by the PBL daily evolution. Two intense events of mineral dust transport from northern Africa (19-21 and 29 June to 2 July) are observed, with layers advected mainly above 2000 m, but subsequently sinking and mixing in the PBL. As a consequence, a non-negligible occurrence of mineral dust is observed close to the ground ( ˜ 7 % of occurrence during a 1-month campaign). The observations unambiguously show Saharan dust layers intruding the Po Valley mixing layer and directly affecting the aerosol concentrations near the surface. Finally, lidar observations also indicate strong variability in aerosol on shorter timescales (hourly). Firstly, these highlight events of hygroscopic growth of anthropogenic aerosol, visible as shallow layers of low depolarization near the ground. Such events are identified during early morning hours at high relative humidity (RH) conditions (RH > 80 %). The process is observed concurrently with high PM1 nitrate concentration (up to 15 µg cm-3) and hence mainly explicable by deliquescence of fine anthropogenic particles, and during mineral dust intrusion episodes, when water condensation on dust particles could instead represent the dominant contribution. Secondly, lidar images show frequent events (mean daily occurrence of ˜ 22 % during the whole campaign) of rapid uplift of mineral depolarizing particles in afternoon-evening hours up to 2000 m a.s.l. height. The origin of such particles cannot be directly related to long-range transport events, being instead likely linked to processes of soil particle resuspension from agricultural lands.

Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, L.; Williams, L. R.; Young, D. E.

The composition of PM 1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM 1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between themore » two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM 1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.« less

Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

DOE PAGES

Xu, L.; Williams, L. R.; Young, D. E.; ...

2016-02-02

The composition of PM 1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM 1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between themore » two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM 1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.« less

Particle size distribution of aerosols sprayed from household hand-pump sprays containing fluorine-based and silicone-based compounds.

PubMed

Kawakami, Tsuyoshi; Isama, Kazuo; Ikarashi, Yoshiaki

2015-01-01

Japan has published safety guideline on waterproof aerosol sprays. Furthermore, the Aerosol Industry Association of Japan has adopted voluntary regulations on waterproof aerosol sprays. Aerosol particles of diameter less than 10 µm are considered as "fine particles". In order to avoid acute lung injury, this size fraction should account for less than 0.6% of the sprayed aerosol particles. In contrast, the particle size distribution of aerosols released by hand-pump sprays containing fluorine-based or silicone-based compounds have not been investigated in Japan. Thus, the present study investigated the aerosol particle size distribution of 16 household hand-pump sprays. In 4 samples, the ratio of fine particles in aerosols exceeded 0.6%. This study confirmed that several hand-pump sprays available in the Japanese market can spray fine particles. Since the hand-pump sprays use water as a solvent and their ingredients may be more hydrophilic than those of aerosol sprays, the concepts related to the safety of aerosol-sprays do not apply to the hand pump sprays. Therefore, it may be required for the hand-pump spray to develop a suitable method for evaluating the toxicity and to establish the safety guideline.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles.

PubMed

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-04-22

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30-500 nm, number concentration in range of 5 × 10²-10⁷ /cm³. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles

PubMed Central

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-01-01

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30–500 nm, number concentration in range of 5 × 102–5 × 107 /cm3. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles. PMID:28441740

The Green Ocean Amazon Experiment (GoAmazon2014/5) Observes Pollution Affecting Gases, Aerosols, Clouds, and Rainfall over the Rain Forest

DOE Office of Scientific and Technical Information (OSTI.GOV)

Martin, S. T.; Artaxo, P.; Machado, L.

The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) experiment took place around the urban region of Manaus in central Amazonia across two years. The urban pollution plume was used to study the susceptibility of gases, aerosols, clouds, and rainfall to human activities in a tropical environment. Many aspects of air quality, weather, terrestrial ecosystems, and climate work differently in the tropics than in the more thoroughly studied USA, employed an unparalleled suite of measurements at nine ground sites and onboard two aircraft to investigate the flow of background air into Manaus, the emissions into the air over themore » city, and the advection of the pollution downwind of the city. Herein, to visualize this train of processes and its effects, observations aboard a low-flying aircraft are presented. Comparative measurements within and adjacent to the plume followed the emissions of biogenic volatile organic carbon compounds (BVOCs) from the tropical forest, their transformations by the atmospheric oxidant cycle, alterations of this cycle by the influence of the pollutants, transformations of the chemical products into aerosol particles, the relationship of these particles to cloud condensation nuclei (CCN) activity, and the differences in cloud properties and rainfall for background compared to polluted conditions. The observations of the GoAmazon2014/5 experiment illustrate how the hydrologic cycle, radiation balance, and carbon recycling may be affected by present-day as well as future economic development and pollution over the Amazonian tropical forest.« less

Spatial Variability of Sources and Mixing State of Atmospheric Particles in a Metropolitan Area.

PubMed

Ye, Qing; Gu, Peishi; Li, Hugh Z; Robinson, Ellis S; Lipsky, Eric; Kaltsonoudis, Christos; Lee, Alex K Y; Apte, Joshua S; Robinson, Allen L; Sullivan, Ryan C; Presto, Albert A; Donahue, Neil M

2018-05-30

Characterizing intracity variations of atmospheric particulate matter has mostly relied on fixed-site monitoring and quantifying variability in terms of different bulk aerosol species. In this study, we performed ground-based mobile measurements using a single-particle mass spectrometer to study spatial patterns of source-specific particles and the evolution of particle mixing state in 21 areas in the metropolitan area of Pittsburgh, PA. We selected sampling areas based on traffic density and restaurant density with each area ranging from 0.2 to 2 km 2 . Organics dominate particle composition in all of the areas we sampled while the sources of organics differ. The contribution of particles from traffic and restaurant cooking varies greatly on the neighborhood scale. We also investigate how primary and aged components in particles mix across the urban scale. Lastly we quantify and map the particle mixing state for all areas we sampled and discuss the overall pattern of mixing state evolution and its implications. We find that in the upwind and downwind of the urban areas, particles are more internally mixed while in the city center, particle mixing state shows large spatial heterogeneity that is mostly driven by emissions. This study is to our knowledge, the first study to perform fine spatial scale mapping of particle mixing state using ground-based mobile measurement and single-particle mass spectrometry.

Real-Time Ultrafine Aerosol Measurements from Wastewater Treatment Facilities.

PubMed

Piqueras, P; Li, F; Castelluccio, V; Matsumoto, M; Asa-Awuku, A

2016-10-18

Airborne particle emissions from wastewater treatment plants (WWTP) have been associated with health repercussions but particulate quantification studies are scarce. In this study, particulate matter (PM) number concentrations and size distributions in the ultrafine range (7-300 nm) were measured from two different sources: a laboratory-scale aerobic bioreactor and the activated sludge aeration basins at Orange County Sanitation District (OCSD). The relationships between wastewater parameters (total organic carbon (TOC), chemical oxygen demand (COD), and total suspended solids (TSS)), aeration flow rate and particle concentrations were also explored. A significant positive relationship was found between particle concentration and WWTP variables (COD: r(10) = 0.876, p <.001, TOC: r(10) = 0.664, p <.05, TSS: r(10) = 0.707, p <.05, aeration flow rate: r(8) = 0.988, p <.0001). A theoretical model was also developed from empirical data to compare real world WWTP aerosol number emission fluxes with laboratory data. Aerosol number fluxes at OCSD aerated basins (9.8 × 10 4 lbs/min·cm 2 ) and the bioreactor (7.95 × 10 4 lbs/min·cm 2 ) were calculated and showed a relatively small difference (19%). The ultrafine size distributions from both systems were consistent, with a mode of ∼48 nm. The average mass concentration (7.03 μg/cm 3 ) from OCSD was relatively small compared to other urban sources. However, the in-tank average number concentration of airborne particles (14 480 lbs/cm 3 ) was higher than background ambient concentrations.

Variability in optical properties of atmospheric aerosols and their frequency distribution over a mega city "New Delhi," India.

PubMed

Tiwari, S; Tiwari, Suresh; Hopke, P K; Attri, S D; Soni, V K; Singh, Abhay Kumar

2016-05-01

The role of atmospheric aerosols in climate and climate change is one of the largest uncertainties in understanding the present climate and in capability to predict future climate change. Due to this, the study of optical properties of atmospheric aerosols over a mega city "New Delhi" which is highly polluted and populated were conducted for two years long to see the aerosol loading and its seasonal variability using sun/sky radiometer data. Relatively higher mean aerosol optical depth (AOD) (0.90 ± 0.38) at 500 nm and associated Angstrom exponent (AE) (0.82 ± 0.35) for a pair of wavelength 400-870 nm is observed during the study period indicating highly turbid atmosphere throughout the year. Maximum AOD value is observed in the months of June and November while minimum is in transition months March and September. Apart from this, highest value of AOD (AE) value is observed in the post-monsoon [1.00 ± 0.42 (1.02 ± 0.16)] season followed by the winter [0.95 ± 0.36 (1.02 ± 0.20)] attributed to significance contribution of urban as well as biomass/crop residue burning aerosol which is further confirmed by aerosol type discrimination based on AOD vs AE. During the pre-monsoon season, mostly dust and mixed types aerosols are dominated. AODs value at shorter wavelength observed maximum in June and November while at longer wavelength maximum AOD is observed in June only. For the better understanding of seasonal aerosol modification process, the aerosol curvature effect is studied which show a strong seasonal dependency under a high turbid atmosphere, which are mainly associated with various emission sources. Five days air mass back trajectories were computed. They suggest different patterns of particle transport during the different seasons. Results suggest that mixtures of aerosols are present in the urban environment, which affect the regional air quality as well as climate. The present study will be very much useful to the modeler for validation of satellite data with observed data during estimation of radiative effect.

Aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing in Guangzhou during the 2006 Pearl River Delta campaign.

PubMed

Jung, Jinsang; Lee, Hanlim; Kim, Young J; Liu, Xingang; Zhang, Yuanhang; Gu, Jianwei; Fan, Shaojia

2009-08-01

Optical and chemical aerosol measurements were obtained from 2 to 31 July 2006 at an urban site in the metropolitan area of Guangzhou (China) as part of the Program of Regional Integrated Experiment of Air Quality over Pearl River Delta (PRIDE-PRD2006) to investigate aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing. During the PRIDE-PRD2006 campaign, the average contributions of ammonium sulfate, organic mass by carbon (OMC), elemental carbon (EC), and sea salt (SS) to total PM(2.5) mass were measured to be 36.5%, 5.7%, 27.1%, 7.8%, and 3.7%, respectively. Compared with the clean marine period, (NH(4))(2)SO(4), NH(4)NO(3), and OMC were all greatly enhanced (by up to 430%) during local haze periods via the accumulation of a secondary aerosol component. The OMC dominance increased when high levels of biomass burning influenced the measurement site while (NH(4))(2)SO(4) and OMC did when both biomass burning and industrial emissions influenced it. The effect of aerosol water content on the total light-extinction coefficient was estimated to be 34.2%, of which 25.8% was due to aerosol water in (NH(4))(2)SO(4), 5.1% that in NH(4)NO(3), and 3.3% that in SS. The average mass-scattering efficiency (MSE) of PM(10) particles was determined to be 2.2+/-0.6 and 4.6+/-1.7m(2)g(-1) under dry (RH<40%) and ambient conditions, respectively. The average single-scattering albedo (SSA) was 0.80+/-0.08 and 0.90+/-0.04 under dry and ambient conditions, respectively. Not only are the extinction and scattering coefficients greatly enhanced by aerosol water content, but MSE and SSA are also highly sensitive. It can be concluded that sulfate and carbonaceous aerosol, as well as aerosol water content, play important roles in the processes that determine visibility impairment and radiative forcing in the ambient atmosphere of the Guangzhou urban area.

Direct identification of trace metals in fine and ultrafine particles in the Detroit urban atmosphere.

PubMed

Utsunomiya, Satoshi; Jensen, Keld A; Keeler, Gerald J; Ewing, Rodney C

2004-04-15

Exposure to airborne particulates containing low concentrations of heavy metals, such as Pb, As, and Se, may have serious health effects. However, little is known about the speciation and particle size of these airborne metals. Fine- and ultrafine particles with heavy metals in aerosol samples from the Detroit urban area, Michigan, were examined in detail to investigate metal concentrations and speciation. The characterization of individual particles was completed using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with conventional high-resolution TEM techniques. The trace elements, Pb, As, La, Ce, Sr, Zn, Cr, Se, Sn, Y, Zr, Au, and Ag, were detected, and the elemental distributions were mapped in situ atthe nanoscale. The crystal structures of the particles containing Pb, Sr, Zn, and Au were determined from their electron diffraction patterns. Based on the characterization of the representative trace element particles, the potential health effects are discussed. Most of the trace element particles detected in this study were within a range of 0.01-1.0 microm in size, which has the longest atmospheric residence time (approximately 100 days). Increased chemical reactivity owing to the size of nanoparticles may be expected for most of the trace metal particles observed.

Chemical composition of PM2.5 at an urban site of Chengdu in southwestern China

NASA Astrophysics Data System (ADS)

Tao, Jun; Cheng, Tiantao; Zhang, Renjian; Cao, Junji; Zhu, Lihua; Wang, Qiyuan; Luo, Lei; Zhang, Leiming

2013-07-01

PM2.5 aerosols were sampled in urban Chengdu from April 2009 to January 2010, and their chemical compositions were characterized in detail for elements, water soluble inorganic ions, and carbonaceous matter. The annual average of PM2.5 was 165 μg m-3, which is generally higher than measurements in other Chinese cities, suggesting serious particulate pollution issues in the city. Water soluble ions contributed 43.5% to the annual total PM2.5 mass, carbonaceous aerosols including elemental carbon and organic carbon contributed 32.0%, and trace elements contributed 13.8%. Distinct daily and seasonal variations were observed in the mass concentrations of PM2.5 and its components, reflecting the seasonal variations of different anthropogenic and natural sources. Weakly acidic to neutral particles were found for PM2.5. Major sources of PM2.5 identified from source apportionment analysis included coal combustion, traffic exhaust, biomass burning, soil dust, and construction dust emissions. The low nitrate: sulfate ratio suggested that stationary emissions were more important than vehicle emissions. The reconstructed masses of ammonium sulfate, ammonium nitrate, particulate carbonaceous matter, and fine soil accounted for 79% of the total measured PM2.5 mass; they also accounted for 92% of the total measured particle scattering.

Operational remote sensing of tropospheric aerosol over land from EOS moderate resolution imaging spectroradiometer

NASA Astrophysics Data System (ADS)

Kaufman, Y. J.; Tanré, D.; Remer, L. A.; Vermote, E. F.; Chu, A.; Holben, B. N.

1997-07-01

Daily distribution of the aerosol optical thickness and columnar mass concentration will be derived over the continents, from the EOS moderate resolution imaging spectroradiometer (MODIS) using dark land targets. Dark land covers are mainly vegetated areas and dark soils observed in the red and blue channels; therefore the method will be limited to the moist parts of the continents (excluding water and ice cover). After the launch of MODIS the distribution of elevated aerosol concentrations, for example, biomass burning in the tropics or urban industrial aerosol in the midlatitudes, will be continuously monitored. The algorithm takes advantage of the MODIS wide spectral range and high spatial resolution and the strong spectral dependence of the aerosol opacity for most aerosol types that result in low optical thickness in the mid-IR (2.1 and 3.8 μm). The main steps of the algorithm are (1) identification of dark pixels in the mid-IR; (2) estimation of their reflectance at 0.47 and 0.66 μm; and (3) derivation of the optical thickness and mass concentration of the accumulation mode from the detected radiance. To differentiate between dust and aerosol dominated by accumulation mode particles, for example, smoke or sulfates, ratios of the aerosol path radiance at 0.47 and 0.66 μm are used. New dynamic aerosol models for biomass burning aerosol, dust and aerosol from industrial/urban origin, are used to determine the aerosol optical properties used in the algorithm. The error in the retrieved aerosol optical thicknesses, τa is expected to be Δτa = 0.05±0.2τa. Daily values are stored on a resolution of 10×10 pixels (1 km nadir resolution). Weighted and gridded 8-day and monthly composites of the optical thickness, the aerosol mass concentration and spectral radiative forcing are generated for selected scattering angles to increase the accuracy. The daily aerosol information over land and oceans [Tanré et al., this issue], combined with continuous aerosol remote sensing from the ground, will be used to study aerosol climatology, to monitor the sources and sinks of specific aerosol types, and to study the interaction of aerosol with water vapor and clouds and their radiative forcing of climate. The aerosol information will also be used for atmospheric corrections of remotely sensed surface reflectance. In this paper, examples of applications and validations are provided.

New particle formation events as a source for cloud condensation nuclei in an urban environment

NASA Astrophysics Data System (ADS)

Wonaschütz, Anna; Burkart, Julia; Wagner, Robert; Reischl, Georg; Steiner, Gerhard; Hitzenberger, Regina

2014-05-01

Nucleation and growth events have been observed in many remote, urban and rural environments. The new particles can contribute significantly to cloud condensation nuclei concentrations, after growing into the appropriate size range (Kerminen et al., 2012). Several studies have attempted to quantify this contribution (e.g. Asmi et al., 2011, Matsui et al., 2013), but only a limited number of them to date have used simultaneous measurements of CCN concentrations and particle size distributions for this purpose (e.g. Levin et al., 2012). In this study, a data set from an urban background station, consisting of 22 months of size distribution and 12 months of CCN concentration measurements (Burkart et al., 2011, Burkart et al., 2012) with 10 months of overlapping measurements is combined to explore the variability of CCN concentrations, their possible causes, and the contribution of nucleation and growth events to CCN concentrations. Consistent with observations in many other locations, nucleation and growth events occur on 30% of all days in spring and summer, on 11% of days in fall and on 4% of days in winter. This suggests a potentially large source of CCN from nucleation and growth events, particularly in the warm season. We acknowledge funding from FWF (Austrian Science Fund) P19515-N20 References: Asmi E., Kivekas, N., Kerminen, V. M., Komppula, M., Hyvarinen, A. P., Hatakka, J., Viisanen, Y., and Lihavainen, H.: Secondary new particle formation in Northern Finland Pallas site between the years 2000 and 2010, Atmos. Chem. Phys., 11, 12959-12972, doi: 10.5194/acp-11-12959-2011, 2011 Burkart J., Steiner, G., Reischl, G., and Hitzenberger, R.: Long-term study of cloud condensation nuclei (CCN) acticvation of the atmospheric aerosol in Vienna, Atmos. Environ., 45, 5751-5759, doi: 10.1016/j.atmosenv.2011.07.022, 2011. Burkart J., Hitzenberger, R., Reischl, G., Bauer, H., Leder, K., and Puxbaum, H.: Activation of "synthetic ambient" aerosols - relation to chemical composition of particles < 100 nm, Atmos. Environ., 54, 583-591, doi: 10.1016/j.atmosenv.2012.01.063, 2012. Kerminen V.-M., Paramonov, M., Anttila, T., Riipinen, I., Fountoukis, C., Korhonen, H., Asmi, E., Laakso, L., Lihavainen, H., Swietlicki, E., Svenningsson, B., Asmi, A., Pandis, S. N., Kulmala, M., and Petäjä, T.: Cloud condensation nuclei production associated with atmospheric nucleation: a synthesis based on existing literature and new results, Atmos. Chem. Phys., 12, 12037-12059, doi: 10.5194/acp-12-12037-2012, 2012. Levin, E. J. T., Prenni, A. J., Petters, M. D., Kreidenweis, S. M., Sullivan, R. C., Atwood, S. A., Ortega, J., DeMott, P. J., and Smith, J. N.: An annual cycle of size-resolved aerosol hygroscopicity at a forested site in Colorado, J. Geophys. Res., 117, 06201, doi:10.1029/2011JD016854, 2012. Matsui, H., Koike, M., Kondo, Y., Takegawa, N., Wiedensohler, A., Fast, J. D., and Zaveri, R. A.: Impact of new particle formation on the concentrations of aerosols and cloud condensation nuclei around Beijing, J. Geophys. Res., 116, 19208, doi:10.1029/2011JD016025, 2011.

Internally mixed black carbon in the Indo-Gangetic Plain and its effect on absorption enhancement

NASA Astrophysics Data System (ADS)

Thamban, Navaneeth M.; Tripathi, S. N.; Moosakutty, Shamjad P.; Kuntamukkala, Pavan; Kanawade, V. P.

2017-11-01

We present the systematic analysis of individual black carbon (BC) mixing state and its impact on radiative forcing from an urban Indian city, Kanpur, located in Indo-Gangetic Plain (IGP). Simultaneous measurements using Single Particle Soot Photometer (SP2), Photo-Acoustic Soot Spectrometer (PASS-3) and High-Resolution Time-of-Flight Aerosol Mass Spectrometer (AMS) were conducted from 8 January 2015 to 28 February 2015 at Kanpur. BC mass and number concentrations varied between 0.7 and 17 μg/m3 and 277-5866 #/cm3 with a mean of 4.06 μg/m3 and 1314 #/cm3, respectively. The diurnal variation of BC mass concentration showed a traffic hour peak during both the morning and late night. The mean fraction of "thickly coated BC" particles (fTCBC) was found to be 61.6%, indicating that a large fraction of BC particles was internally mixed. The fTCBC increased after sunrise with a peak at about noontime, indicating that the formation of secondary organic aerosol under active photochemistry can enhance organic coating on a core of black carbon. High-resolution positive matrix factorization (HR-PMF) factors showed distinct characteristics with fTCBC. While primary organic aerosols like cooking organic aerosols (COA) and biomass burning organic aerosols (BBOA) were negatively correlated with fTCBC (r = - 0.78 and - 0.51, respectively), aged low volatile oxygenated organic aerosol (LVOOA) was forming a coating over BC (r = 0.6). Similar positive correlation of fTCBC with inorganic species like ammonium (r = 0.58) and nitrate (r = 0.47) further suggested that BC appears to be largely coated with LVOOA, ammonium, and nitrate. A positive correlation between the fTCBC and the mass absorption cross-section at 781 nm (MAC781) was also observed (r = 0.58). Our results suggest that the observed fTCBC could amplify the MAC781 approximately by a factor of 1.8, which may catalyze the positive radiative forcing in the IGP.

Primary sources and secondary formation of organic aerosols in Beijing, China.

PubMed

Guo, Song; Hu, Min; Guo, Qingfeng; Zhang, Xin; Zheng, Mei; Zheng, Jun; Chang, Chih Chung; Schauer, James J; Zhang, Renyi

2012-09-18

Ambient aerosol samples were collected at an urban site and an upwind rural site of Beijing during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. Contributions of primary particles and secondary organic aerosols (SOA) were estimated by chemical mass balance (CMB) modeling and tracer-yield method. The apportioned primary and secondary sources explain 73.8% ± 9.7% and 79.6% ± 10.1% of the measured OC at the urban and rural sites, respectively. Secondary organic carbon (SOC) contributes to 32.5 ± 15.9% of the organic carbon (OC) at the urban site, with 17.4 ± 7.6% from toluene, 9.7 ± 5.4% from isoprene, 5.1 ± 2.0% from α-pinene, and 2.3 ± 1.7% from β-caryophyllene. At the rural site, the secondary sources are responsible for 38.4 ± 14.4% of the OC, with the contributions of 17.3 ± 6.9%, 13.9 ± 9.1%, 5.6 ± 1.9%, and 1.7 ± 1.0% from toluene, isoprene, α-pinene, and β-caryophyllene, respectively. Compared with other regions in the world, SOA in Beijing is less aged, but the concentrations are much higher; between the sites, SOA is more aged and affected by regional transport at the urban site. The high SOA loading in Beijing is probably attributed to the high regional SOC background (~2 μg m(-3)). The toluene SOC concentration is high and comparable at the two sites, implying that some anthropogenic components, at least toluene SOA, are widespread in Beijing and represents a major factor in affecting the regional air quality. The aerosol gaseous precursor concentrations and temperature correlate well with SOA, both affecting SOA formation. The significant SOA enhancement with increasing water uptake and acidification indicates that the aqueous-phase reactions are largely responsible SOA formation in Beijing.

Reactive intermediates revealed in secondary organic aerosol formation from isoprene

PubMed Central

Surratt, Jason D.; Chan, Arthur W. H.; Eddingsaas, Nathan C.; Chan, ManNin; Loza, Christine L.; Kwan, Alan J.; Hersey, Scott P.; Flagan, Richard C.; Wennberg, Paul O.; Seinfeld, John H.

2010-01-01

Isoprene is a significant source of atmospheric organic aerosol; however, the oxidation pathways that lead to secondary organic aerosol (SOA) have remained elusive. Here, we identify the role of two key reactive intermediates, epoxydiols of isoprene (IEPOX = β-IEPOX + δ-IEPOX) and methacryloylperoxynitrate (MPAN), which are formed during isoprene oxidation under low- and high-NOx conditions, respectively. Isoprene low-NOx SOA is enhanced in the presence of acidified sulfate seed aerosol (mass yield 28.6%) over that in the presence of neutral aerosol (mass yield 1.3%). Increased uptake of IEPOX by acid-catalyzed particle-phase reactions is shown to explain this enhancement. Under high-NOx conditions, isoprene SOA formation occurs through oxidation of its second-generation product, MPAN. The similarity of the composition of SOA formed from the photooxidation of MPAN to that formed from isoprene and methacrolein demonstrates the role of MPAN in the formation of isoprene high-NOx SOA. Reactions of IEPOX and MPAN in the presence of anthropogenic pollutants (i.e., acidic aerosol produced from the oxidation of SO2 and NO2, respectively) could be a substantial source of “missing urban SOA” not included in current atmospheric models. PMID:20080572

Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols

PubMed Central

Mills, Jessica B.; Park, Jae Hong; Peters, Thomas M.

2016-01-01

We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride, NaCl, and spark generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <103; Medium, 103–104; and High, >104 particles/cm3). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared to those measured with reference instruments, a scanning mobility particle sizer (SMPS) and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 21% of those measured by reference instruments for polydisperse aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +130% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm but caution should be exercised when particles larger than 300 nm are present. PMID:23473056

Sources and chemical composition of atmospheric fine and coarse particles in the Helsinki area

NASA Astrophysics Data System (ADS)

Pakkanen, Tuomo A.; Loukkola, Kati; Korhonen, Christina H.; Aurela, Minna; Mäkelä, Timo; Hillamo, Risto E.; Aarnio, Päivi; Koskentalo, Tarja; Kousa, Anu; Maenhaut, Willy

During April 1996-June 1997 size-segregated atmospheric aerosol particles were collected at an urban and a rural site in the Helsinki area by utilising virtual impactors (VI) and Berner low-pressure impactors (BLPI). In addition, VI samples were collected at a semi-urban site during October 1996-May 1997. The average PM 2.3 (fine particle) concentrations at the urban and rural sites were 11.8 and 8.4 μg/m 3, and the PM 2.3-15 (coarse particle) concentrations were 12.8 and about 5 μg/m 3, respectively. The difference in fine particle mass concentrations suggests that on average, more than one third of the fine mass at the urban site is of local origin. Evaporation of fine particle nitrate from the VI Teflon filters during sampling varied similarly at the three sites, the average evaporation being about 50-60%. The average fine particle concentrations of the chemical components (25 elements and 13 ions) appeared to be fairly similar at the three sites for most components, which suggests that despite the long-range transport, the local emissions of these components were relatively evenly distributed in the Helsinki area. Exceptions were the average fine particles Ba, Fe, Sb and V concentrations that were clearly highest at the urban site pointing to traffic (Ba, Fe, Sb) and to combustion of heavy fuel oil (V) as the likely local sources. The average coarse particle concentrations for most components were highest at the urban site and lowest at the rural site. Average chemical composition of fine particles was fairly similar at the urban and rural sites: non-analysed fraction (mainly carbonaceous material and water) 43% and 37%, sulphate 21% and 25%, crustal matter 12% and 13%, nitrate 12% and 11%, ammonium 9% and 10% and sea-salt 2.5% and 3.2%, respectively. At the semi-urban site also, the average fine particle composition was similar. At the urban site, the year round average composition of coarse particles was dominated by crustal matter (59%) and the non-analysed components (28%, mainly carbonaceous material and water), while the other contributions were much lower: sea-salt 7%, nitrate 4% and sulphate 2%. At the rural site, the coarse samples were collected in spring and summer and the percentage was clearly lower for crustal matter (37%) and sea-salt (3%) but higher for the not-analysed fraction (51%). At the semi-urban site, the average composition of coarse particles was nearly identical to that at the urban site. Correlations between the chemical components were calculated separately for fine and coarse particles. In urban fine particles sulphate, ammonium, Tl, oxalate and PM 2.3 mass correlated with each other and originated mainly from long-range transport. The sea-salt ions Na +, Cl - and Mg 2+ formed another group and still another group was formed by the organic anions oxalate, malonate, succinate, glutarate and methane sulphonate. Ni and V correlated strongly pointing to combustion of heavy fuel oil as the likely source. In addition, some groups with lower correlations were detected. At the rural and semi-urban sites, the correlating components were rather similar to those at the urban site, although differences were also observed.

Effect of vehicular traffic, remote sources and new particle formation on the activation properties of cloud condensation nuclei in the megacity of São Paulo, Brazil

NASA Astrophysics Data System (ADS)

Souto-Oliveira, Carlos Eduardo; de Fátima Andrade, Maria; Kumar, Prashant; Juliano da Silva Lopes, Fábio; Babinski, Marly; Landulfo, Eduardo

2016-11-01

Atmospheric aerosol is the primary source of cloud condensation nuclei (CCN). The microphysics and chemical composition of aerosols can affect cloud development and the precipitation process. Among studies conducted in Latin America, only a handful have reported the impact of urban aerosol on CCN activation parameters such as activation ratio (AR) and activation diameter (Dact). With over 20 million inhabitants, the Metropolitan Area of São Paulo (MASP) is the largest megacity in South America. To our knowledge, this is the first study to assess the impact that remote sources and new particle formation (NPF) events have on CCN activation properties in a South American megacity. The measurements were conducted in the MASP between August and September 2014. We measured the CCN within the 0.2-1.0 % range of supersaturation, together with particle number concentration (PNC) and particle number distribution (PND), as well as trace-element concentrations and black carbon (BC). NPF events were identified on 35 % of the sampling days. Combining multivariate analysis in the form of positive matrix factorization (PMF) with an aerosol profile from lidar and HYSPLIT model analyses allowed us to identify the main contribution of vehicular traffic on all days and sea salt and biomass burning from remote regions on 28 and 21 % of the sampling days, respectively. The AR and Dact parameters showed distinct patterns for daytime with intense vehicular traffic and nighttime periods. For example, CCN activation was lower during the daytime than during the nighttime periods, a pattern that was found to be associated mainly with local road-traffic emissions. A decrease in CCN activation was observed on the NPF event days, mainly due to high concentrations of particles with smaller diameters. We also found that aerosols from sea salt, industrial emissions, and biomass burning had minor effects on Dact. For example, nights with biomass burning and vehicular emissions showed slightly lower CCN activation properties than sea-salt, industrial and non-event nights. Our results show that particulate matter from local vehicular emissions during the daytime has a greater effect on CCN activation parameters than that from remote sources.

On the competition among aerosol number, size and composition in predicting CCN variability: a multi-annual field study in an urbanized desert.

PubMed

Crosbie, E; Youn, J-S; Balch, B; Wonaschütz, A; Shingler, T; Wang, Z; Conant, W C; Betterton, E A; Sorooshian, A

2015-02-10

A 2-year data set of measured CCN (cloud condensation nuclei) concentrations at 0.2 % supersaturation is combined with aerosol size distribution and aerosol composition data to probe the effects of aerosol number concentrations, size distribution and composition on CCN patterns. Data were collected over a period of 2 years (2012-2014) in central Tucson, Arizona: a significant urban area surrounded by a sparsely populated desert. Average CCN concentrations are typically lowest in spring (233 cm -3 ), highest in winter (430 cm -3 ) and have a secondary peak during the North American monsoon season (July to September; 372 cm -3 ). There is significant variability outside of seasonal patterns, with extreme concentrations (1 and 99 % levels) ranging from 56 to 1945 cm -3 as measured during the winter, the season with highest variability. Modeled CCN concentrations based on fixed chemical composition achieve better closure in winter, with size and number alone able to predict 82% of the variance in CCN concentration. Changes in aerosol chemical composition are typically aligned with changes in size and aerosol number, such that hygroscopicity can be parameterized even though it is still variable. In summer, models based on fixed chemical composition explain at best only 41% (pre-monsoon) and 36% (monsoon) of the variance. This is attributed to the effects of secondary organic aerosol (SOA) production, the competition between new particle formation and condensational growth, the complex interaction of meteorology, regional and local emissions and multi-phase chemistry during the North American monsoon. Chemical composition is found to be an important factor for improving predictability in spring and on longer timescales in winter. Parameterized models typically exhibit improved predictive skill when there are strong relationships between CCN concentrations and the prevailing meteorology and dominant aerosol physicochemical processes, suggesting that similar findings could be possible in other locations with comparable climates and geography.

Characterization of Dust Properties Near Source Region During ACE-Asia: A Column Satellite-Surface Perspective

NASA Technical Reports Server (NTRS)

Tsay, S. -C.; Ji, Q.; Chu, A.; Hsu, C.; Holben, B.; Campbell, J.; Welton, E. J.; Shu, P. K.

2002-01-01

Many recent field experiments are designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentrations over eastern/southeastern Asia and along the rim of the western Pacific. For example, the ACE-Asia was conducted from March-May 2001 in the vicinity of the Taklimakan and Gobi deserts, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian aerosols is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of aerosol radiative flux in addition to measurements of loading and optical depth. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

Characteristics, sources and evolution of fine aerosol (PM1) at urban, coastal and forest background sites in Lithuania

NASA Astrophysics Data System (ADS)

Masalaite, A.; Holzinger, R.; Remeikis, V.; Röckmann, T.; Dusek, U.

2017-01-01

The chemical and isotopic composition of organic aerosol (OA) samples collected on PM1 filters was determined as a function of desorption temperature to investigate the main sources of organic carbon and the effects of photochemical processing on atmospheric aerosol. The filter samples were collected at an urban (54°38‧ N, 25°18‧ E), coastal (55°55‧ N, 21°00‧ E) and forest (55°27‧ N, 26°00' E) site in Lithuania in March 2013. They can be interpreted as winter-time samples because the monthly averaged temperature was -4 °C. The detailed chemical composition of organic compounds was analysed with a thermal desorption PTR-MS. The mass concentration of organic aerosol at the forest site was roughly by a factor of 30 lower than at the urban and coastal site. This fact could be an indication that in this cold month the biogenic secondary organic aerosol (SOA) formation was very low. Moreover, the organic aerosol collected at the forest site was more refractory and contained a larger fraction of heavy molecules with m/z > 200. The isotopic composition of the aerosol was used to differentiate the two main sources of organic aerosol in winter, i.e. biomass burning (BB) and fossil fuel (FF) combustion. Organic aerosol from biomass burning is enriched in 13C compared to OA from fossil fuel emissions. δ13COC values of the OA samples showed a positive correlation with the mass fraction of several individual organic compounds. Most of these organic compounds contained nitrogen indicating that organic nitrogen compounds formed during the combustion of biomass may be indicative of BB. Other compounds that showed negative correlations with δ13COC were possibly indicative of FF. These compounds included heavy hydrocarbons and were on the average less oxidized than the bulk organic carbon. The correlation of δ13COC and the O/C ratio was positive at low but negative at high desorption temperatures at the forest site. We propose that this might be due to photochemical processing of OA. This processing can lead to accumulation of carbon in the more refractory organic fraction that is depleted in 13C compared with the less refractory organic fraction. Detailed laboratory experiments are necessary to further investigate the aging of aerosol particles before firm conclusions can be drawn.

Anthropogenic Osmium in Airborne Particles from Woods Hole, Massachusetts, USA

NASA Astrophysics Data System (ADS)

Peucker-Ehrenbrink, B.; Sen, I. S.; Geboy, N.

2012-12-01

The global geochemical cycle of osmium has been significantly disturbed by the introduction of automobile exhaust catalysts to convert noxious gas emissions into more benign forms. Anthropogenic osmium has been reported in rainwater, snow, and in the urban airborne particles from around the world to reveal global-scale osmium pollution [1, 2]. In this study, we report on the platinum group element (PGE) concentrations and osmium isotope ratios of airborne particles (PM10) collected in Woods Hole, a small coastal town in Massachusetts to better understand inputs of anthropogenic osmium to rural environments. We further investigate the use of osmium isotopes to track sources of airborne particles and support source apportionment studies on a continental scale. The samples used in this study were collected at Woods Hole Oceanographic Institution over one year (2008-2009). From this collection twelve samples for which the backward air mass trajectories have been determined were selected for osmium isotope analyses. Our results show that the osmium and platinum concentrations are an order of magnitude lower when compared to downtown Boston [2]. The average Os, Pt and Ir concentrations are 0.006±0.012, 0.019±0.023, and 0.685±0.634 pg m-3, respectively. The 187Os/188Os of the aerosols range from 0.275 to 0.788. As continental crust is radiogenic (187Os/188Os >1) and PGE ore bodies generally have unradiogenic 187Os/188Os (~0.2), the unradiogenic 187Os/188Os signature of the aerosols indicates anthropogenic contributions. With 95% of the total osmium mobilization on land being attributed to human activities [3], it is clear that human imprint on airborne particles is not restricted to urban centers with high traffic flows, but also affects rural environments. Aerosol particles that have backward air mass trajectories from the Southwest, the densely populated and industrialized Eastern seaboard, are characterized by unradiogenic osmium, while air masses from the North have radiogenic signatures. Our results suggest that 187Os/188Os has potential for source apportionment studies. [1] Rauch et al. (2005), Environ. Sci. Technol., 39, p. 9464-9470 [2] Chen et al. (2009), PNAS, 106, p. 7724-7728 [3] Sen and Peucker-Ehrenbrink (2012), Environ. Sci. Technol., dx.doi.org/10.102/es301261x

Composition and major sources of organic compounds in urban aerosols

NASA Astrophysics Data System (ADS)

Bi, Xinhui; Simoneit, Bernd R. T.; Sheng, Guoying; Ma, Shexia; Fu, Jiamo

Total suspended particles (TSP), collected during June 2002 to July 2003 in Guangzhou, a typical economically developed city in South China, were analyzed for the organic compound compositions using gas chromatography-mass spectrometry (GC/MS). Over 140 organic compounds were detected in the aerosols and grouped into different classes including n-alkanes, hopanoids, polycyclic aromatic hydrocarbons, alkanols, fatty acids, dicarboxylic acids excluding oxalic acid, polyols/polyacids, lignin products, phytosterols, phthalates and water-soluble sugars. The total amounts of the identified organic compounds including unresolved complex mixture (UCM) ranged from 3112 ng/m 3 in spring to 5116 ng/m 3 in winter, comprising on seasonal average 2.8% of TSP. Primary organic compounds peaked in winter although there are no heating systems burning fuels in Guangzhou. The highest saccharide levels occurred in fall due to agricultural activities. This study demonstrated that utilization of fossil fuels, biomass burning, soil resuspension and plastic/refuse burning are the major contributors to the identified organic compounds in the urban atmosphere of South China.

Adaptation of an aerosol retrieval algorithm using multi-wavelength and multi-pixel information of satellites (MWPM) to GOSAT/TANSO-CAI

NASA Astrophysics Data System (ADS)

Hashimoto, M.; Takenaka, H.; Higurashi, A.; Nakajima, T.

2017-12-01

Aerosol in the atmosphere is an important constituent for determining the earth's radiation budget, so the accurate aerosol retrievals from satellite is useful. We have developed a satellite remote sensing algorithm to retrieve the aerosol optical properties using multi-wavelength and multi-pixel information of satellite imagers (MWPM). The method simultaneously derives aerosol optical properties, such as aerosol optical thickness (AOT), single scattering albedo (SSA) and aerosol size information, by using spatial difference of wavelegths (multi-wavelength) and surface reflectances (multi-pixel). The method is useful for aerosol retrieval over spatially heterogeneous surface like an urban region. In this algorithm, the inversion method is a combination of an optimal method and smoothing constraint for the state vector. Furthermore, this method has been combined with the direct radiation transfer calculation (RTM) numerically solved by each iteration step of the non-linear inverse problem, without using look up table (LUT) with several constraints. However, it takes too much computation time. To accelerate the calculation time, we replaced the RTM with an accelerated RTM solver learned by neural network-based method, EXAM (Takenaka et al., 2011), using Rster code. And then, the calculation time was shorternd to about one thouthandth. We applyed MWPM combined with EXAM to GOSAT/TANSO-CAI (Cloud and Aerosol Imager). CAI is a supplement sensor of TANSO-FTS, dedicated to measure cloud and aerosol properties. CAI has four bands, 380, 674, 870 and 1600 nm, and observes in 500 meters resolution for band1, band2 and band3, and 1.5 km for band4. Retrieved parameters are aerosol optical properties, such as aerosol optical thickness (AOT) of fine and coarse mode particles at a wavelenth of 500nm, a volume soot fraction in fine mode particles, and ground surface albedo of each observed wavelength by combining a minimum reflectance method and Fukuda et al. (2013). We will show the results and discuss the accuracy of the algorithm for various surface types. Our future work is to extend the algorithm for analysis of GOSAT-2/TANSO-CAI-2 and GCOM/C-SGLI data.

Metagenomic analysis of the airborne environment in urban spaces.

PubMed

Be, Nicholas A; Thissen, James B; Fofanov, Viacheslav Y; Allen, Jonathan E; Rojas, Mark; Golovko, George; Fofanov, Yuriy; Koshinsky, Heather; Jaing, Crystal J

2015-02-01

The organisms in aerosol microenvironments, especially densely populated urban areas, are relevant to maintenance of public health and detection of potential epidemic or biothreat agents. To examine aerosolized microorganisms in this environment, we performed sequencing on the material from an urban aerosol surveillance program. Whole metagenome sequencing was applied to DNA extracted from air filters obtained during periods from each of the four seasons. The composition of bacteria, plants, fungi, invertebrates, and viruses demonstrated distinct temporal shifts. Bacillus thuringiensis serovar kurstaki was detected in samples known to be exposed to aerosolized spores, illustrating the potential utility of this approach for identification of intentionally introduced microbial agents. Together, these data demonstrate the temporally dependent metagenomic complexity of urban aerosols and the potential of genomic analytical techniques for biosurveillance and monitoring of threats to public health.

Markedly enhanced direct radiative forcing of black carbon particles under polluted urban environments

NASA Astrophysics Data System (ADS)

Peng, Jianfei; Hu, Min; Guo, Song; Du, Zhuofei; Zheng, Jing; Shang, Dongjie; Zamora, Misti; Zeng, Liming; Shao, Min; Wu, Yusheng; Zheng, Jun; Wang, Yuan; Collins, Don; Zhang, Renyi

2016-04-01

Black carbon (BC) particles, produced from incomplete fossil fuel combustion and biomass burning, are ubiquitous in the atmosphere and have profound impacts on air quality, human health, weather, and climate. For example, in areas identified as aerosol hotspots, which include many urban centers and megacities worldwide, solar heating by BC particles has been shown to be comparable to warming due to the greenhouse gases2. Although BC represents a key short-lived climate forcer, its direct radiative forcing remains highly uncertain. In particular, the available results of absorption enhancement of BC particles during atmospheric aging are conflicting from the previous studies, leading to a large uncertainty in global radiative transfer calculation. Here, we quantified the aging and variation in the optical properties of BC particles under ambient conditions in Beijing, China and Houston, US, using a novel chamber approach. BC aging exhibits two distinct stages - initial transformation from a fractal to spherical morphology with little absorption variation and the subsequent growth of fully compact particles with a maximum absorption enhancement factor of 2.4. The variation in BC direct radiative forcing is highly dependent of the rate and timescale of aging, with an estimated increase of 0.45 (0.21 - 0.80) W m-2 from fresh to fully aged particles. Our results reveal a high climatic impact in polluted environments due to rapid aging and a clear distinction between urban cities in developed and developing countries for BC particles, highlighting a larger than recognized co-benefit in air quality improvement and climate protection by BC mediation.

Gas phase emissions from cooking processes and their secondary aerosol production potential

NASA Astrophysics Data System (ADS)

Klein, Felix; Platt, Stephen; Bruns, Emily; Termime-roussel, Brice; Detournay, Anais; Mohr, Claudia; Crippa, Monica; Slowik, Jay; Marchand, Nicolas; Baltensperger, Urs; Prevot, Andre; El Haddad, Imad

2014-05-01

Long before the industrial evolution and the era of fossil fuels, high concentrations of aerosol particles were alluded to in heavily populated areas, including ancient Rome and medieval London. Recent radiocarbon measurements (14C) conducted in modern megacities came as a surprise: carbonaceous aerosol (mainly organic aerosol, OA), a predominant fraction of particulate matter (PM), remains overwhelmingly non-fossil despite extensive fossil fuel combustion. Such particles are directly emitted (primary OA, POA) or formed in-situ in the atmosphere (secondary OA, SOA) via photochemical reactions of volatile organic compounds (VOCs). Urban levels of non-fossil OA greatly exceed the levels measured in pristine environments strongly impacted by biogenic emissions, suggesting a contribution from unidentified anthropogenic non-fossil sources to urban OA. Positive matrix factorization (PMF) techniques applied to ambient aerosol mass spectrometer (AMS, Aerodyne) data identify primary cooking emissions (COA) as one of the main sources of primary non-fossil OA in major cities like London (Allan et al., 2010), New York (Sun et al., 2011) and Beijing (Huang et al., 2010). Cooking processes can also emit VOCs that can act as SOA precursors, potentially explaining in part the high levels of oxygenated OA (OOA) identified by the AMS in urban areas. However, at present, the chemical nature of these VOCs and their secondary aerosol production potential (SAPP) remain virtually unknown. The approach adopted here involves laboratory quantification of PM and VOC emission factors from the main primary COA emitting processes and their SAPP. Primary emissions from deep-fat frying, vegetable boiling, vegetable frying and meat cooking for different oils, meats and vegetables were analysed under controlled conditions after ~100 times dilution. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a high resolution proton transfer time-of-flight mass spectrometer (PTR-ToF-MS) were used to quantify OA and VOC emissions, respectively. SOA production potential of the different emissions was quantified by introducing them into the PSI mobile smog chamber and a potential aerosol chamber (PAM) where they were photochemically aged. The measurements of primary emissions suggest that the COA factor identified in ambient atmospheric aerosols is mostly related to fat release from frying with vegetable oils or grilling fatty-meats. In contrast, vegetable cooking (boiling and frying) was associated with significant VOC emissions. The VOC emissions from frying consist mainly of aldehydes which are formed through breaking of fatty acids. Gas phase composition, emission factors and SAPP from all these processes will be presented. This work was supported by the Swiss National Science Foundation as well as the Swiss Federal Office for the Environment. The research leading to these results has received funding from the European Community's Seventh Framework Programme (FP7/2007-2013) under grant agreement n.° 290605 (COFUND: PSI-FELLOW). J. Allan et al, Atmos. Chem. Phys. 10, 647-668 (2010) X.-F. Huang et al, Atmos. Chem. Phys. 10, 8933-8945 (2010) Y.-L. Sun et al, Atmos. Chem. Phys. 11, 1581-1602 (2011)

Modeling particle nucleation and growth over northern California during the 2010 CARES campaign

NASA Astrophysics Data System (ADS)

Lupascu, A.; Easter, R.; Zaveri, R.; Shrivastava, M.; Pekour, M.; Tomlinson, J.; Yang, Q.; Matsui, H.; Hodzic, A.; Zhang, Q.; Fast, J. D.

2015-07-01

Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4 while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapors parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates were predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10-40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. Differences among the three simulations for the 40-100 nm particle diameter range are mostly associated with the timing of the peak total tendencies that shift the morning increase and afternoon decrease in particle number concentration by up to two hours. We found that newly formed particles could explain up to 20-30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ∼ 36 %.

Simultaneous factor analysis of organic particle and gas mass spectra: AMS and PTR-MS measurements at an urban site

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Vlasenko, A.; McGuire, M.; Evans, G. J.; Abbatt, J. P. D.

2009-03-01

During the winter component of the SPORT (Seasonal Particle Observations in the Region of Toronto) field campaign, particulate non-refractory chemical composition and concentration of selected volatile organic compounds (VOCs) were measured by an Aerodyne time-of-flight aerosol mass spectrometer (AMS) and a proton transfer reaction-mass spectrometer (PTR-MS), respectively. Sampling was performed in downtown Toronto ~15 m from a major road. The mass spectra from the AMS and PTR-MS were combined into a unified dataset, which was analyzed using positive matrix factorization (PMF). The two instruments were given equal weight in the PMF analysis by application of a scaling factor to the uncertainties of each instrument. A residual based metric, Δesc, was used to evaluate the relative weight. The PMF analysis yielded a 5-factor solution that included factors characteristic of regional transport, local traffic emissions, charbroiling, and oxidative processing. The unified dataset provides information on particle and VOC sources and atmospheric processing that cannot be obtained from the datasets of the individual instruments, such as apportionment of oxygenated VOCs to direct emission sources vs. secondary reaction products, improved correlation of oxygenated aerosol factors with photochemical age, and increased detail regarding the composition of oxygenated organic aerosol factors. This analysis represents the first application of PMF to a unified AMS/PTR-MS dataset.

Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties

DOE PAGES

Willis, Megan D.; Healy, Robert M.; Riemer, Nicole; ...

2016-04-14

The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) inmore » two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Lastly, significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.« less

Mineral dust aerosols promote the formation of toxic nitropolycyclic aromatic compounds

PubMed Central

Kameda, Takayuki; Azumi, Eri; Fukushima, Aki; Tang, Ning; Matsuki, Atsushi; Kamiya, Yuta; Toriba, Akira; Hayakawa, Kazuichi

2016-01-01

Atmospheric nitrated polycyclic aromatic hydrocarbons (NPAHs), which have been shown to have adverse health effects such as carcinogenicity, are formed in part through nitration reactions of their parent polycyclic aromatic hydrocarbons (PAHs) in the atmosphere. However, little is known about heterogeneous nitration rates of PAHs by gaseous NO2 on natural mineral substrates, such as desert dust aerosols. Herein by employing kinetic experiments using a flow reactor and surface analysis by Fourier transform infrared spectroscopy with pyridine adsorption, we demonstrate that the reaction is accelerated on acidic surfaces of mineral dust, particularly on those of clay minerals. In support of this finding, we show that levels of ambient particle-associated NPAHs in Beijing, China, significantly increased during heavy dust storms. These results suggest that mineral dust surface reactions are an unrecognized source of toxic organic chemicals in the atmosphere and that they enhance the toxicity of mineral dust aerosols in urban environments. PMID:27075250

Measurements of gas and particle polycyclic aromatic hydrocarbons (PAHs) in air at urban, rural and near-roadway sites

NASA Astrophysics Data System (ADS)

Pratt, G. C.; Herbrandson, C.; Krause, M. J.; Schmitt, C.; Lippert, C. J.; McMahon, C. R.; Ellickson, K. M.

2018-04-01

We measured polycyclic aromatic hydrocarbons (PAHs) in gas and particle phases over two years using high volume samplers equipped with quartz fiber filters and XAD-4 at a rural site, an urban site, and a site adjacent to a heavily trafficked roadway. Overall results were generally as expected, in that concentrations increased from rural to urban to near-roadway sites, and PAHs with high vapor pressures (liquid subcooled, PoL) and low octanol-air partition coefficients (Koa) were mainly in the gas phase, while those with low PoL and high Koa were predominantly in the particle phase. Intermediate PAHs existed in both phases with the phase distribution following a seasonal pattern of higher gas phase concentrations in summer due to temperature effects. The overall pattern of phase distribution was consistent with PAH properties and ambient conditions and was similar at all three sites. The particle-bound fraction (ϕ) was well-described empirically by nonlinear regressions with log Koa and log PoL as predictors. Adsorption and absorption models underestimated the particle-bound fraction for most PAHs. The dual aerosol-air/soot-air model generally represented the gas-particle partitioning better than the other models across all PAHs, but there was a tendency to underestimate the range in the particle-bound fraction seen in measurements. There was a statistically insignificant tendency for higher PAHs in the particle phase at the near roadway site, and one piece of evidence that PAHs may be enriched on ultrafine particles at the near roadway site. Understanding the phase and particle size distributions of PAHs in highly polluted, high exposure microenvironments near traffic sources will help shed light on potential health effects.

Mass and number size distributions of particulate matter components: comparison of an industrial site and an urban background site.

PubMed

Taiwo, Adewale M; Beddows, David C S; Shi, Zongbo; Harrison, Roy M

2014-03-15

Size-resolved composition of particulate matter (PM) sampled in the industrial town of Port Talbot (PT), UK was determined in comparison to a typical urban background site in Birmingham (EROS). A Micro-Orifice Uniform Deposit Impactor (MOUDI) sampler was deployed for two separate sampling campaigns with the addition of a Grimm optical spectrometer at the PT site. MOUDI samples were analysed for water-soluble anions (Cl(-), NO₃(-) and SO₄(2-)) and cations (Na(+), NH4(+), K(+), Mg(2+) and Ca(2+)) and trace metals (Al, V, Cr, Mn, Fe, Cu, Zn, Sb, Ba and Pb). The PM mass distribution showed a predominance of fine particle (PM₂.₅) mass at EROS whereas the PT samples were dominated by the coarse fraction (PM₂.₅₋₁₀). SO₄(2-), Cl(-), NH4(+), Na(+), NO₃(-), and Ca(2+) were the predominant ionic species at both sites while Al and Fe were the metals with highest concentrations at both sites. Mean concentrations of Cl(-), Na(+), K(+), Ca(2+), Mg(2+), Cr, Mn, Fe and Zn were higher at PT than EROS due to industrial and marine influences. The contribution of regional pollution by sulphate, ammonium and nitrate was greater at EROS relative to PT. The traffic signatures of Cu, Sb, Ba and Pb were particularly prominent at EROS. Overall, PM at EROS was dominated by secondary aerosol and traffic-related particles while PT was heavily influenced by industrial activities and marine aerosol. Profound influences of wind direction are seen in the 72-hour data, especially in relation to the PT local sources. Measurements of particle number in 14 separate size bins plotted as a function of wind direction and speed are highly indicative of contributing sources, with local traffic dominant below 0.5 μm, steelworks emissions from 0.5 to 15 μm, and marine aerosol above 15 μm. Copyright © 2013 Elsevier B.V. All rights reserved.

Isotopic mass independent signature of black crusts: a proxy for atmospheric aerosols formation in the Paris area (France).

NASA Astrophysics Data System (ADS)

Genot, Isabelle; Martin, Erwan; Yang, David Au; De Rafelis, Marc; Cartigny, Pierre; Wing, Boswell; Le Gendre, Erwann; Bekki, Slimane

2016-04-01

In view of the negative forcing of the sulfate aerosols on climate, a more accurate understanding of the formation of these particles is crucial. Indeed, despite the knowledge of their effects, uncertainties remain regarding the formation of sulfate aerosols, particularly the oxidation processes of S-bearing gases. Since the discovery of oxygen and sulfur mass independent fractionation (O- and S-MIF) processes on Earth, the sulfate isotopic composition became essential to investigate the atmospheric composition evolution and its consequences on the climate and the biosphere. Large amount of S-bearing compounds (SO2 mainly) is released into the atmosphere by anthropogenic and natural sources. Their oxidation in the atmosphere generates sulfate aerosols, H2SO4, which precipitate on the earth surface mainly as acid rain. One consequence of this precipitation is the formation of black crust on buildings made of carbonate stones. Indeed the chemical alteration of CaCO3 by H2SO4 leads to gypsum (CaSO4·2H2O) concretions on building walls. Associated to other particles, gypsum forms black-crusts. Therefore, black crusts acts as 'sulfate aerosol traps', meaning that their isotopic composition reveals the composition and thus the source and formation processes of sulfate aerosols in the atmosphere in a specific region. In this study we collected 37 black crusts on a 300km NW-SE profile centered on Paris (France). In our samples, sulfate represent 40wt.% and other particles 60wt.% of the black crusts. After sulfate extraction from each samples we measured their O- and S-isotopes composition. Variations of about 10‰ in δ18O and δ34S are observed and both O-MIF (Δ17O from 0 to 1.4‰) and S-MIF (Δ33S from 0 to -0.3‰) compositions have been measured. In regards to these compositions we can discuss the source and formation (oxidation pathways) of the sulfate aerosols in troposphere above the Paris region that covers urban, rural and coastal environments. Furthermore, this study shows for the first time O- and S-MIF signature in black crusts. Finally, we demonstrate that black crusts can be considered as a good 'sulfate aerosols traps', which can be widely used to study the sulfate aerosol formation, fate and sink in the troposphere.

Spaceborne Remote Sensing of Aerosol Type: Global Distribution, Model Evaluation and Translation into Chemical Speciation

NASA Astrophysics Data System (ADS)

Kacenelenbogen, M. S.; Tan, Q.; Johnson, M. S.; Burton, S. P.; Redemann, J.; Hasekamp, O. P.; Dawson, K. W.; Hair, J. W.; Ferrare, R. A.; Butler, C. F.; Holben, B. N.; Beyersdorf, A. J.; Ziemba, L. D.; Froyd, K. D.; Dibb, J. E.; Shingler, T.; Sorooshian, A.; Jimenez, J. L.; Campuzano Jost, P.; Jacob, D.; Kim, P. S.; Travis, K.; Lacagnina, C.

2016-12-01

It is essential to evaluate and refine aerosol classification methods applied to passive satellite remote sensing. We have developed an aerosol classification algorithm (called Specified Clustering and Mahalanobis Classification, SCMC) that assigns an aerosol type to multi-parameter retrievals by spaceborne, airborne or ground-based passive remote sensing instruments [1]. The aerosol types identified by our scheme are pure dust, polluted dust, urban-industrial/developed economy, urban-industrial/developing economy, dark biomass smoke, light biomass smoke and pure marine. We apply the SCMC method to inversions from the ground-based AErosol RObotic NETwork (AERONET [2]) and retrievals from the space-borne Polarization and Directionality of Earth's Reflectances instrument (POLDER, [3]). The POLDER retrievals that we use differ from the standard POLDER retrievals [4] as they make full use of multi-angle, multispectral polarimetric data [5]. We analyze agreement in the aerosol types inferred from both AERONET and POLDER and evaluate GEOS-Chem [6] simulations over the globe. Finally, we use in-situ observations from the SEAC4RS airborne field experiment to bridge the gap between remote sensing-inferred qualitative SCMC aerosol types and their corresponding quantitative chemical speciation. We apply the SCMC method to airborne in-situ observations from the NASA Langley Aerosol Research Group Experiment (LARGE, [7]) and the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP, [8]) instruments; we then relate each coarsely defined SCMC type to a sum of percentage of individual aerosol species, using in-situ observations from the Particle Analysis by Laser Mass Spectrometry (PALMS, [9]), the Soluble Acidic Gases and Aerosol (SAGA, [10]), and the High - Resolution Time - of - Flight Aerosol Mass Spectrometer (HR ToF AMS, [11]). [1] Russell P. B., et al., JGR, 119.16 (2014) [2] Holben B. N., et al., RSE, 66.1 (1998) [3] Tanré D., et al., AMT, 4.7 (2011) [4] Deuzé J. L., et al., JGR, 106.D5 (2001) [5] Hasekamp O. P., et al., JGR, 116.D14 (2011) [6] Bey I., et al., JGR, 106.D19 (2001) [7] Ziemba L. D., et al., GRL, 40.2 (2013) [8] Sorooshian A., et al., AST, 42.6 (2008) [9] Murphy D. M., et al., JGR, 111.D23 (2006) [10] Dibb J. E., et al., JGR, 108.D21 (2003) [11] DeCarlo P. F., et al., AC, 78.24 (2006)

Dicarboxylic acids, metals and isotopic compositions of C and N in atmospheric aerosols from inland China: implications for dust and coal burning emission and secondary aerosol formation

NASA Astrophysics Data System (ADS)

Wang, G.; Xie, M.; Hu, S.; Gao, S.; Tachibana, E.; Kawamura, K.

2010-07-01

Dicarboxylic acids (C2-C10), metals, elemental carbon (EC), organic carbon (OC), and stable isotopic compositions of total carbon (TC) and total nitrogen (TN) were determined for PM10 samples collected at three urban and one suburban sites of Baoji, an inland city of China, during winter and spring 2008. Oxalic acid (C2) was the dominant diacid, followed by succinic (C4) and malonic (C3) acids. Total diacids in the urban and suburban areas were 1546±203 and 1728±495 ng m-3 during winter and 1236±335 and 1028±193 ng m-3 during spring. EC in the urban and the suburban atmospheres were 17±3.8 and 8.0±2.1 μg m-3 during winter and 20±5.9 and 7.1±2.7 μg m-3 during spring, while OC at the urban and suburban sites were 74±14 and 51±7.9 μg m-3 in winter and 51±20 and 23±6.1 μg m-3 in spring. Secondary organic carbon (SOC) accounted for 38±16% of OC in winter and 28±18% of OC in spring, suggesting an enhanced photochemical production of secondary organic aerosols in winter under an inversion layer development. Total metal elements in winter and spring were 34±10 and 61±27 μg m-3 in the urban air and 18±7 and 32±23 μg m-3 in the suburban air. A linear correlation (r2>0.8 in winter and r2>0.6 in spring) was found between primary organic carbon (POC) and Ca2+/Fe, together with a strong dependence of pH value of sample extracts on water-soluble inorganic carbon, suggesting fugitive dust as an important source of the airborne particles. Polycyclic aromatic hydrocarbons (PAHs), sulfate, and Pb in the samples well correlated each other (r2>0.6) in winter, indicating an importance of emissions from coal burning for house heating. Stable carbon isotope compositions of TC (δ13C) became higher with an increase in the concentration ratios of C2/OC due to aerosol aging. In contrast, nitrogen isotope compositions of TN (δ15N) became lower with an increases in the mass ratios of NH4+/PM10 and NO3-/PM10, which is possibly caused by an enhanced adsorption and/or condensation of gaseous NH3 and HNO3 onto particles.

Deposition flux of aerosol particles and 15 polycyclic aromatic hydrocarbons in the North China Plain.

PubMed

Wang, Xilong; Liu, Shuzhen; Zhao, Jingyu; Zuo, Qian; Liu, Wenxin; Li, Bengang; Tao, Shu

2014-04-01

The present study examined deposition fluxes of aerosol particles and 15 polycyclic aromatic hydrocarbons (PAHs) associated with the particles in the North China Plain. The annual mean deposition fluxes of aerosol particles and 15 PAHs were 0.69 ± 0.46 g/(m(2) ×d) and 8.5 ± 6.2 μg/(m(2) ×d), respectively. Phenanthrene, fluoranthene, pyrene, chrysene, benzo[b]fluoranthene, and benzo[k]fluoranthene were the dominant PAHs bound to deposited aerosol particles throughout the year. The total concentration of 15 PAHs in the deposited aerosol particles was the highest in winter but lowest in spring. The highest PAH concentration in the deposited aerosol particles in winter was because the heating processes highly increased the concentration in atmospheric aerosol particles. Low temperature and weak sunshine in winter reduced the degradation rate of deposited aerosol particle-bound PAHs, especially for those with low molecular weight. The lowest PAH concentration in deposited aerosol particles in spring resulted from the frequently occurring dust storms, which diluted PAH concentrations. The mean deposition flux of PAHs with aerosol particles in winter (16 μg/[m(2) ×d]) reached 3 times to 5 times that in other seasons (3.5-5.0 μg/[m(2) ×d]). The spatial variation of the deposition flux of PAHs with high molecular weight (e.g., benzo[a]pyrene) was consistent with their concentrations in the atmospheric aerosol particles, whereas such a phenomenon was not observed for those with low molecular weight (e.g., phenanthrene) because of their distinct hydrophobicity, Henry's law constant, and the spatially heterogeneous meteorological conditions. © 2013 SETAC.

The optical properties of absorbing aerosols with fractal soot aggregates: Implications for aerosol remote sensing

NASA Astrophysics Data System (ADS)

Cheng, Tianhai; Gu, Xingfa; Wu, Yu; Chen, Hao; Yu, Tao

2013-08-01

Applying sphere aerosol models to replace the absorbing fine-sized dominated aerosols can potentially result in significant errors in the climate models and aerosol remote sensing retrieval. In this paper, the optical properties of absorbing fine-sized dominated aerosol were modeled, which are taking into account the fresh emitted soot particles (agglomerates of primary spherules), aged soot particles (semi-externally mixed with other weakly absorbing aerosols), and coarse aerosol particles (dust particles). The optical properties of the individual fresh and aged soot aggregates are calculated using the superposition T-matrix method. In order to quantify the morphology effect of absorbing aerosol models on the aerosol remote sensing retrieval, the ensemble averaged optical properties of absorbing fine-sized dominated aerosols are calculated based on the size distribution of fine aerosols (fresh and aged soot) and coarse aerosols. The corresponding optical properties of sphere absorbing aerosol models using Lorenz-Mie solutions were presented for comparison. The comparison study demonstrates that the sphere absorbing aerosol models underestimate the absorption ability of the fine-sized dominated aerosol particles. The morphology effect of absorbing fine-sized dominated aerosols on the TOA radiances and polarized radiances is also investigated. It is found that the sphere aerosol models overestimate the TOA reflectance and polarized reflectance by approximately a factor of 3 at wavelength of 0.865 μm. In other words, the fine-sized dominated aerosol models can cause large errors in the retrieved aerosol properties if satellite reflectance measurements are analyzed using the conventional Mie theory for spherical particles.

Fluorescence spectra of atmospheric aerosol at Adelphi, Maryland, USA: measurement and classification of single particles containing organic carbon

NASA Astrophysics Data System (ADS)

Pinnick, Ronald G.; Hill, Steven C.; Pan, Yong-Le; Chang, Richard K.

We measured laser-induced fluorescence spectra from individual supermicron-sized atmospheric particles drawn into our laboratory at Adelphi, MD, an urban site in the Washington, DC metroplex. A virtural impactor concentrator is used along with an aerodynamic-focusing-nozzle which forms, within an optical chamber, a focused aerosol jet where single aerosol particles can be interrogated on-the-fly with a pulsed 266-nm-wavelength laser. Sample rates are a few liter per minute, and are size dependent. Crossed-diode laser beams indicate when a particle is traversing the sample region and are used to trigger the UV laser to fire and the gated intensified CCD to record the fluorescence spectrum. Our breadboard fluorescence particle spectrometer measures particles in the 3-10 μm diameter size range. Typical trigger rates are a few per second. The usable spectral range is from about 295 to 605 nm. The majority of the particles have very weak fluorescence (on average 8 percent of particles have fluorescence signals above noise). The spectra were grouped using a heirarchical cluster analysis, with parameters chosen so that spectra typically cluster into 4-12 main categories. From the set of all cluster spectra we chose 8 template spectra for reanalyzing all the data. On average, 92 percent (81-94 percent) of the spectra were similar to these templates (using the same thresholds used for the cluster analysis). The major emission bands of the most commonly occurring spectra have peaks: near 460 nm (28 percent of fluorescent particles on average), a very broad hump, and may be humic acids or humic like substances; near 317 nm (on average 24 percent of fluorescent particles); near 321 and 460 nm (a double hump, 12 percent of fluorescent particles); and near 341 nm (8 percent of fluorescent particles). Some of the fluorescence in spectra peaking in the 317-341 nm range is probably from dicyclic aromatics and heterocyclics, including the amino acid tryptophan in biological particles such as bacteria and spores.

Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

NASA Astrophysics Data System (ADS)

Gantt, B.; Kelly, J. T.; Bash, J. O.

2015-11-01

Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.

Aerosol optical properties and radiative effects: Assessment of urban aerosols in central China using 10-year observations

NASA Astrophysics Data System (ADS)

Zhang, Ming; Ma, Yingying; Gong, Wei; Liu, Boming; Shi, Yifan; Chen, ZhongYong

2018-06-01

Poor air quality episodes are common in central China. Here, based on 10 years of ground-based sun-photometric observations, aerosol optical and radiative forcing characteristics were analyzed in Wuhan, the biggest metropolis in central China. Aerosol optical depth (AOD) in the last decade declined significantly, while the Ångström exponent (AE) showed slight growth. Single scattering albedo (SSA) at 440 nm reached the lowest value (0.87) in winter and highest value (0.93) in summer. Aerosol parameters derived from sun-photometric observations were used as input in a radiative transfer model to calculate aerosol radiative forcing (ARF) on the surface in ultraviolet (UV), visible (VIS), near-infrared (NIR), and shortwave (SW) spectra. ARFSW sustained decreases (the absolute values) over the last 10 years. In terms of seasonal variability, due to the increases in multiple scattering effects and attenuation of the transmitted radiation as AOD increased, ARF in summer displayed the largest value (-73.94 W/m2). After eliminating the influence of aerosol loading, the maximum aerosol radiative forcing efficiency in SW range (ARFESW) achieved a value of -64.5 W/m2/AOD in April. The ARFE change in each sub-interval spectrum was related to the change in SSA and effective radius of fine mode particles (Refff), that is, ARFE increased with the decreases in SSA and Refff. The smallest contribution of ARFENIR to ARFESW was 34.11% under strong absorbing and fine particle conditions, and opposite results were found for the VIS range, whose values were always over 51.82%. Finally, due to the serious air pollution and frequency of haze day, aerosol characteristics in haze and clear days were analyzed. The percentage of ARFENIR increased from 35.71% on clear-air days to 37.63% during haze periods, while both the percentage of ARFEUV and ARFENIR in ARFESW kept decreasing. The results of this paper should help us to better understand the effect of aerosols on solar spectral radiation and to develop improved the aerosol models over central China.

Daily behavior of urban Fluorescing Aerosol Particles in northwest Spain

NASA Astrophysics Data System (ADS)

Calvo, A. I.; Baumgardner, D.; Castro, A.; Fernández-González, D.; Vega-Maray, A. M.; Valencia-Barrera, R. M.; Oduber, F.; Blanco-Alegre, C.; Fraile, R.

2018-07-01

Measurements of ambient aerosol particles at the University of León, León, Spain, were made in May and June 2015 with a Wideband Integrated Bioaerosol Spectrometer (WIBS). The WIBS detects Fluorescing Aerosol Particles (FAP) in the size range from 0.5 to 20 μm. These measurements were complemented with an analysis of pollen concentrations assessed with optical microscopy of samples captured with a volumetric Hirst spore trap. The total particle, FAP and pollen concentrations show clear, daily cycles. Whereas the total particle concentrations maximize at 0800 and 2200 UTC, the FAP concentrations have peaks at midnight and 0800 UTC while the pollen has a broad peak between 1200 and 2000 UTC. The FAP larger than 2 μm represent 15-35% of the total particle population in this size range, maximizing at midnight UTC. Similar to what has been found by investigators at other locations, there is a strong positive correlation of the WIBS measured FAP with relative humidity; however, the pollen concentration is positively correlated with the temperature and anti-correlated with the relative humidity. Back trajectory analysis indicates that the largest FAP to total particle fractions are found in air masses arriving from the northeast with the second largest coming from the southwest. Given the location of the university in relation to the city and forested areas, this implies that the higher concentration FAP are coming from rural, probably natural, sources; however, more local, anthropogenic sources cannot be ruled out as a secondary source. The majority of the FAP that are identified from microscopy are fungal spores (Cladosporium, Aspergillus, Alternaria, Oidium) and pollen grains (mainly Poaceae, Quercus, Plantago, Rumex and Urticaceae). A comparison of the fluorescence fingerprints between laboratory generated FAP and the ambient particles showed some similarities; however, a significant fraction of the FAP are those whose fluorescence patterns do not match any of those that have been previously classified in the laboratory.

The MUMBA campaign: measurements of urban, marine and biogenic air

NASA Astrophysics Data System (ADS)

Paton-Walsh, Clare; Guérette, Élise-Andrée; Kubistin, Dagmar; Humphries, Ruhi; Wilson, Stephen R.; Dominick, Doreena; Galbally, Ian; Buchholz, Rebecca; Bhujel, Mahendra; Chambers, Scott; Cheng, Min; Cope, Martin; Davy, Perry; Emmerson, Kathryn; Griffith, David W. T.; Griffiths, Alan; Keywood, Melita; Lawson, Sarah; Molloy, Suzie; Rea, Géraldine; Selleck, Paul; Shi, Xue; Simmons, Jack; Velazco, Voltaire

2017-06-01

The Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign took place in Wollongong, New South Wales (a small coastal city approximately 80 km south of Sydney, Australia) from 21 December 2012 to 15 February 2013. Like many Australian cities, Wollongong is surrounded by dense eucalyptus forest, so the urban airshed is heavily influenced by biogenic emissions. Instruments were deployed during MUMBA to measure the gaseous and aerosol composition of the atmosphere with the aim of providing a detailed characterisation of the complex environment of the ocean-forest-urban interface that could be used to test the skill of atmospheric models. The gases measured included ozone, oxides of nitrogen, carbon monoxide, carbon dioxide, methane and many of the most abundant volatile organic compounds. The aerosol characterisation included total particle counts above 3 nm, total cloud condensation nuclei counts, mass concentration, number concentration size distribution, aerosol chemical analyses and elemental analysis.The campaign captured varied meteorological conditions, including two extreme heat events, providing a potentially valuable test for models of future air quality in a warmer climate. There was also an episode when the site sampled clean marine air for many hours, providing a useful additional measure of the background concentrations of these trace gases within this poorly sampled region of the globe. In this paper we describe the campaign, the meteorology and the resulting observations of atmospheric composition in general terms in order to equip the reader with a sufficient understanding of the Wollongong regional influences to use the MUMBA datasets as a case study for testing a chemical transport model. The data are available from PANGAEA (http://doi.pangaea.de/10.1594/PANGAEA.871982).

Revisiting Atmospheric Lead in NYC - Comparison of Archived Air Filters to Urban Park Sediments and Soils

NASA Astrophysics Data System (ADS)

Chillrud, S. N.; Ross, J. M.; Yan, B.; Bopp, R.

2015-12-01

Urban lake sediments have the potential to be used for reconstructing history of aerosols, providing data before the start of urban air quality monitoring. In a previous study, the similarity between radionuclide and excess Pb inventories (57 g/m^2) in Central Park Lake (CPL) sediments and those same parameters in Central Park soils (CPS) was interpreted to indicate that urban lake sediment cores from CPL represent deposition of atmospheric aerosols over the history of the park, which was constructed in the 1860s. Furthermore, metal ratios and metal chronologies indicated that incineration was the major source of Pb to the NYC atmosphere over the 20th century. In this report, we compare the lake chronologies for metals to a set of archived air filters collected by the Department of Energy's Environmental Measurement Lab (EML). These weekly filters of total suspended particulates (TSP) were collected by a high volume sampler located in lower Manhattan for radionuclides as part of the program focused on documenting radioactive fallout from nuclear weapons testing. Metal concentrations measured in subsamples of the EML filters collected between the 1970s to 1990s showed Pb decreasing more slowly than the records of Pb added to gasoline. Metal ratios in the filters were similar to the ratios measured in CPL sediments; the Pb to Sn ratios were roughly 20:1 and the Pb to Zn ratios were in close to 1. The similarity of the ratios provides additional solid support that the CP Lake sediment cores reflect atmospheric inputs. The enrichment of Pb in the large aerosol particle fraction (TSP), relative to fine PM2.5 fraction, demonstrates that the resuspended NYC soils and their historical contaminant burden, are the primary, current source of Pb to NYC air.

Application of AERONET Single Scattering Albedo and Absorption Angstrom Exponent to Classify Dominant Aerosol Types during DRAGON Campaigns

NASA Astrophysics Data System (ADS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Schafer, J.; Crawford, J. H.; Kim, J.; Sano, I.; Liew, S.; Salinas Cortijo, S. V.; Chew, B. N.; Lim, H.; Smirnov, A.; Sorokin, M.; Kenny, P.; Slutsker, I.

2013-12-01

Aerosols can have major implications on human health by inducing respiratory diseases due to inhalation of fine particles from biomass burning smoke or industrial pollution and on radiative forcing whereby the presence of absorbing aerosol particles (e.g., black carbon) increases atmospheric heating. Aerosol classification techniques have utilized aerosol loading and aerosol properties derived from multi-spectral and multi-angle observations by ground-based (e.g., AERONET) and satellite instrumentation (e.g., MISR). Aerosol Robotic Network (AERONET) data have been utilized to determine aerosol types by implementing various combinations of measured aerosol optical depth or retrieved size and absorption aerosol properties (e.g., Gobbi et al., 2007; Russell et al., 2010). Giles et al. [2012] showed single scattering albedo (SSA) relationship with extinction Angstrom exponent (EAE) can provide an estimate of the general classification of dominant aerosol types (i.e., desert dust, urban/industrial pollution, biomass burning smoke, and mixtures) based on data from ~20 AERONET sites located in known aerosol source regions. In addition, the absorption Angstrom exponent relationship with EAE can provide an indication of the dominant absorbing aerosol type such as dust, black carbon, brown carbon, or mixtures of them. These classification techniques are applied to the AERONET Level 2.0 quality assured data sets collected during Distributed Regional Aerosol Gridded Observational Network (DRAGON) campaigns in Maryland (USA), Japan, South Korea, Singapore, Penang (Malaysia), and California (USA). An analysis of aerosol type classification for DRAGON sites is performed as well as an assessment of the spatial variability of the aerosol types for selected DRAGON campaigns. Giles, D. M., B. N. Holben, T. F. Eck, A. Sinyuk, A. Smirnov, I. Slutsker, R. R. Dickerson, A. M. Thompson, and J. S. Schafer (2012), An analysis of AERONET aerosol absorption properties and classifications representative of aerosol source regions, J. Geophys. Res., 117, D17203, doi:10.1029/2012JD018127. Gobbi, G. P., Y. J. Kaufman, I. Koren, and T. F. Eck (2007), Classification of aerosol properties derived from AERONET direct sun data, Atmos. Chem. Phys., 7, 453-458, doi:10.5194/acp-7-453-2007. Russell, P. B., R. W. Bergstrom, Y. Shinozuka, A. D. Clarke, P. F. DeCarlo, J. L. Jimenez, J. M. Livingston, J. Redemann, O. Dubovik, and A. Strawa (2010), Absorption Ångstrom Exponent in AERONET and related data as an indicator of aerosol composition, Atmos. Chem. Phys., 10, 1155-1169, doi:10.5194/acp-10-1155-2010.

Local environmental pollution strongly influences culturable bacterial aerosols at an urban aquatic superfund site.

PubMed

Dueker, M Elias; O'Mullan, Gregory D; Juhl, Andrew R; Weathers, Kathleen C; Uriarte, Maria

2012-10-16

In polluted environments, when microbial aerosols originate locally, species composition of the aerosols should reflect the polluted source. To test the connection between local environmental pollution and microbial aerosols near an urban waterfront, we characterized bacterial aerosols at Newtown Creek (NTC), a public waterway and Superfund site in a densely populated area of New York, NY, USA. Culturable bacterial aerosol fallout rate and surface water bacterial concentrations were at least an order of magnitude greater at NTC than at a neighboring, less polluted waterfront and a nonurban coastal site in Maine. The NTC culturable bacterial aerosol community was significantly different in taxonomic structure from previous urban and coastal aerosol studies, particularly in relative abundances of Actinobacteria and Proteobacteria. Twenty-four percent of the operational taxonomic units in the NTC overall (air + water) bacterial isolate library were most similar to bacterial 16S rRNA gene sequences previously described in terrestrial or aquatic environments contaminated with sewage, hydrocarbons, heavy metals, and other industrial waste. This study is the first to examine the community composition and local deposition of bacterial aerosols from an aquatic Superfund site. The findings have important implications for the use of aeration remediation in polluted aquatic environments and suggest a novel pathway of microbial exposure in densely populated urban communities containing contaminated soil and water.

Aerosol processing in stratiform clouds in ECHAM6-HAM

NASA Astrophysics Data System (ADS)

Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

2013-04-01

Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the chemical components as well as 5 tracers for aerosol particles in ice crystals. This allows simulations of aerosol processing in warm, mixed-phase (e.g. through the Bergeron-Findeisen process) and ice clouds. The fixed scavenging ratios used for wet deposition in clouds in standard HAM are replaced by an explicit treatment of collision of cloud droplets/ice crystals with interstitial aerosol particles. Nucleation scavenging of aerosol particles by acting as cloud condensation nuclei or ice nuclei, freezing and evaporation of cloud droplets and melting and sublimation of ice crystals are treated explicitly. In extension to previous studies, aerosol particles from evaporating precipitation are released to modes which correspond to their size. Cloud processing of aerosol particles changes their size distribution and hence influences cloud droplet and ice crystal number concentrations as well as precipitation rate, which in turn affects aerosol concentrations. Results will be presented at the conference. Hoose et al., JGR, 2008a, doi: 10.1029/2007JD009251 Hoose et al., ACP, 2008b, doi: 10.5194/acp-8-6939-2008 Stevens et al., 2013, submitted Stier et al., ACP, 2005, doi: 10.5194/acp-5-1125-2005

Imaging aerosol viscosity

NASA Astrophysics Data System (ADS)

Pope, Francis; Athanasiadis, Thanos; Botchway, Stan; Davdison, Nicholas; Fitzgerald, Clare; Gallimore, Peter; Hosny, Neveen; Kalberer, Markus; Kuimova, Marina; Vysniauskas, Aurimas; Ward, Andy

2017-04-01

Organic aerosol particles play major roles in atmospheric chemistry, climate, and public health. Aerosol particle viscosity is important since it can determine the ability of chemical species such as oxidants, organics or water to diffuse into the particle bulk. Recent measurements indicate that OA may be present in highly viscous states; however, diffusion rates of small molecules such as water appear not to be limited by these high viscosities. We have developed a technique for measuring viscosity that allows for the imaging of aerosol viscosity in micron sized aerosols through use of fluorescence lifetime imaging of viscosity sensitive dyes which are also known as 'molecular rotors'. These rotors can be introduced into laboratory generated aerosol by adding minute quantities of the rotor to aerosol precursor prior to aerosolization. Real world aerosols can also be studied by doping them in situ with the rotors. The doping is achieved through generation of ultrafine aerosol particles that contain the rotors; the ultrafine aerosol particles deliver the rotors to the aerosol of interest via impaction and coagulation. This work has been conducted both on aerosols deposited on microscope coverslips and on particles that are levitated in their true aerosol phase through the use of a bespoke optical trap developed at the Central Laser Facility. The technique allows for the direct observation of kinetic barriers caused by high viscosity and low diffusivity in aerosol particles. The technique is non-destructive thereby allowing for multiple experiments to be carried out on the same sample. It can dynamically quantify and track viscosity changes during atmospherically relevant processes such oxidation and hygroscopic growth (1). This presentation will focus on the oxidation of aerosol particles composed of unsaturated and saturated organic species. It will discuss how the type of oxidant, oxidation rate and the composition of the oxidized products affect the time dependent aerosol viscosity. (1) Hosny, N. A., C. Fitzgerald, A. Vysniauskas, T. Athanasiadis, T. Berkemeier, N. Uygur, U. Pöschl, M. Shiraiwa, M. Kalberer, F.D. Pope and M.K. Kuimova (2016) 'Direct imaging of changes in aerosol particle viscosity upon hydration and chemical aging'. Chemical Science, 17, 32194-32203. http://dx.doi.org/doi:10.1039/C5SC02959G

Elucidating Particle Acidity during North China Winter Haze Events

NASA Astrophysics Data System (ADS)

Song, S.; Gao, M.; Sun, Y.; Li, M.; Wang, S.; Wang, Y.; Xu, W.; Zhu, L.; Munger, W.; McElroy, M. B.

2017-12-01

A characteristic feature of North China winter haze pollution is the rapid formation of sulfate. An accurate prediction of particle acidity, or pH, is critical for evaluating the contributions of various aqueous and heterogeneous sulfate production mechanisms (e.g. the reactions involving reactive nitrogen and transition metal ions), and is also important for evaluating the toxicity of atmospheric particles. However, particle acidity during winter haze periods is poorly constrained, and estimates in several recent studies display significant discrepancies, ranging from moderately acidic (pH 4) to neutral (pH 7). In this study, we calculate fine particle pH for several haze episodes during the 2014/2015 winter, using several methods including phase partitioning of ammonia, ion balance, and multiple thermodynamic equilibrium models. Hourly gaseous and particle composition measurements were taken at an urban site in Beijing. We find that the discrepancies in the calculated pH for recent studies are largely due to their differences in assumed methodology. The ion balance method and the reverse modes of thermodynamic models (using only aerosol phase compositions as input) are not suitable for calculating pH in this atmospheric environment. We also find, for the first time, that hydroxymethanesulfonate (HMS), formed from complexation of sulfite and bisulfite with formaldehyde in the aqueous phase, can serve as a tracer of particle pH during winter haze events. Here the concentrations of HMS are quantified using measurement data from an Aerodyne high-resolution aerosol mass spectrometer. HMS is found to contribute a few percent to particle mass during winter haze episodes. The presence of HMS is also identified with data from a single particle aerosol mass spectrometer. Since it may be incorrectly identified as sulfate during the typical chemical composition analysis of fine particles (e.g. ion chromatography), the existence of HMS could explain a significant fraction of the underestimation of sulfate formation in current air quality models. Preliminary results suggest that particle pH values estimated with the HMS tracer, phase partitioning of ammonia, and the forward modes (specifying total concentrations of gas and particle phases) of thermodynamic models are in good agreement.

Real-Time Detection Method And System For Identifying Individual Aerosol Particles

DOEpatents

Gard, Eric Evan; Fergenson, David Philip

2005-10-25

A method and system of identifying individual aerosol particles in real time. Sample aerosol particles are compared against and identified with substantially matching known particle types by producing positive and negative test spectra of an individual aerosol particle using a bipolar single particle mass spectrometer. Each test spectrum is compared to spectra of the same respective polarity in a database of predetermined positive and negative spectra for known particle types and a set of substantially matching spectra is obtained. Finally the identity of the individual aerosol particle is determined from the set of substantially matching spectra by determining a best matching one of the known particle types having both a substantially matching positive spectrum and a substantially matching negative spectrum associated with the best matching known particle type.

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

NASA Astrophysics Data System (ADS)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

2014-11-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in northern Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. The different meteorological regimes also affected the BC mixing state: in periods of enhanced stagnation and recirculation of pollutants, the number fraction of the BC-containing particles determined by ATOFMS was 75% of the total, while in the days of enhanced ventilation of the planetary boundary layer (PBL), such fraction was significantly lower (50%) because of the relative greater influence of non-BC-containing aerosol local sources in the Po Valley. Overall, a full internal mixing between BC and the non-refractory aerosol chemical components was not observed during the experiment in this environment.

Lower tropospheric distributions of O3 and aerosol over Raoyang, a rural site in the North China Plain

NASA Astrophysics Data System (ADS)

Wang, Rui; Xu, Xiaobin; Jia, Shihui; Ma, Ruisheng; Ran, Liang; Deng, Zhaoze; Lin, Weili; Wang, Ying; Ma, Zhiqiang

2017-03-01

The North China Plain (NCP) has become one of the most polluted regions in China, with the rapidly increasing economic growth in the past decades. High concentrations of ambient O3 and aerosol have been observed at urban as well as rural sites in the NCP. Most of the in situ observations of air pollutants have been conducted near the ground so that current knowledge about the vertical distributions of tropospheric O3 and aerosol over the NCP region is still limited. In this study, vertical profiles of O3 and size-resolved aerosol concentrations below 2.5 km were measured in summer 2014 over a rural site in the NCP, using an unmanned aerial vehicle (UAV) equipped with miniature analyzers. In addition, vertical profiles of aerosol scattering property in the lower troposphere and vertical profiles of O3 below 1 km were also observed at the site using a lidar and tethered balloon, respectively. The depths of the mixed layer and residual layer were determined according to the vertical gradients of lidar particle extinction and aerosol number concentration. Average O3 and size-resolved aerosol number concentration in both the mixed and residual layer were obtained from the data observed in seven UAV flights. The results show that during most of the flights the O3 levels above the top of mixed layer were higher than those below. Such a positive gradient in the vertical distribution of O3 makes the residual layer an important source of O3 in the mixed layer, particularly during the morning when the top of mixed layer is rapidly elevated. In contrast to O3, aerosol number concentration was normally higher in the mixed layer than in the residual layer, particularly in the early morning. Aerosol particles were overwhelmingly distributed in the size range < 1 µm, showing slight differences between the mixed and residual layers. Our measurements confirm that the lower troposphere over the rural area of the NCP is largely impacted by anthropogenic pollutants locally emitted or transported from urban areas. Compared with the historic O3 vertical profiles over Beijing from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC), a strong increase in O3 can be found at all heights below 2.5 km in the decade from 2004 to 2014, with the largest enhancement of about 41.6 ppb. This indicates that the lower troposphere over the northern part of the NCP has experienced rapidly worsening photochemical pollution. This worsening trend in photochemical pollution deserves more attention in the future.

Evaluation of PM2.5 surface concentration simulated by Version 1 of the NASA’s MERRA Aerosol Reanalysis over Israel and Taiwan

PubMed Central

Provençal, Simon; Buchard, Virginie; da Silva, Arlindo M.; Leduc, Richard; Barrette, Nathalie; Elhacham, Emily; Wang, Sheng-Hsiang

2018-01-01

Version 1 of the NASA MERRA Aerosol Reanalysis (MERRAero) assimilates bias-corrected aerosol optical depth (AOD) data from MODIS-Terra and MODIS-Aqua, and simulates particulate matter (PM) concentration data to reproduce a consistent database of AOD and PM concentration around the world from 2002 to the end of 2015. The purpose of this paper is to evaluate MERRAero’s simulation of fine PM concentration against surface measurements in two regions of the world with relatively high levels of PM concentration but with profoundly different PM composition, those of Israel and Taiwan. Being surrounded by major deserts, Israel’s PM load is characterized by a significant contribution of mineral dust, and secondary contributions of sea salt particles, given its proximity to the Mediterranean Sea, and sulfate particles originating from Israel’s own urban activities and transported from Europe. Taiwan’s PM load is composed primarily of anthropogenic particles (sulfate, nitrate and carbonaceous particles) locally produced or transported from China, with an additional contribution of springtime transport of mineral dust originating from Chinese and Mongolian deserts. The evaluation in Israel produced favorable results with MERRAero slightly overestimating measurements by 6% on average and reproducing an excellent year-to-year and seasonal fluctuation. The evaluation in Taiwan was less favorable with MERRAero underestimating measurements by 42% on average. Two likely reasons explain this discrepancy: emissions of anthropogenic PM and their precursors are largely uncertain in China, and MERRAero doesn’t include nitrate particles in its simulation, a pollutant of predominately anthropogenic sources. MERRAero nevertheless simulates well the concentration of fine PM during the summer, when Taiwan is least affected by the advection of pollution from China. PMID:29670645

Effect of Ammonia on Glyoxal SOA in Inorganic Aqueous Seed Particles

NASA Astrophysics Data System (ADS)

Waxman, E.; Volkamer, R. M.; Laskin, A.; Laskin, J.; Koenig, T. K.; Baltensperger, U.; Dommen, J.; Prevot, A. S.; Slowik, J.; Maxut, A.; Noziere, B.; Wang, S.; Yu, J.

2014-12-01

Glyoxal (C2H2O2) is a ubiquitous small molecule that is observed in the terrestrial biogenic, urban, marine and arctic atmosphere. It forms secondary organic aerosol (SOA) as a result of multiphase chemical reactions in water. The rate of these reactions is controlled by the effective Henry's law partitioning coefficient (Heff) which is enhanced in the presence of inorganic salts by up to 3 orders of magnitude (Kampf et al., 2013, ES&T). Aerosol particles are among the most concentrated salt solutions on Earth and the SOA formation rate in aerosol water is strongly modified by this 'salting-in' mechanism. We have studied the effect of gas-phase ammonia on the rate of SOA formation in real particles composed of different inorganic salts (sulfate, nitrate, chloride). A series of simulation chamber experiments were conducted at the Paul Scherrer Institut in Switzerland during Summer 2013. The SOA formation rate in experiments with added gas-phase ammonia (NH3) was found to be greatly accelerated compared to experiments without added NH3. Product analysis of particles included online HR-ToF-AMS and offline nano-DESI and LC-MS. We find that imidazole-like oligomer compounds dominate the observed products, rather than high-O/C oligomers containing solely C, H, and O. We further employed isotopically labelled di-substituted 13C glyoxal experiments in order to unambiguously link product formation to glyoxal (and separate it from chamber wall contamination). We present a molecular perspective on the reaction pathways and evaluate the effect of environmental parameters (RH, particle pH, seed chemical composition) on the formation of these imidazole-like oligomer compounds. The implications for SOA formation from photosensitized oxidation chemistry is discussed.

Evaluation of PM2.5 Surface Concentration Simulated by Version 1 of the Nasa's MERRA Aerosol Reanalysis Over Israel and Taiwan

NASA Technical Reports Server (NTRS)

Provencal, Simon; Buchard, Virginie; da Silva, Arlindo M.; Leduc, Richard; Barrette, Nathalie; Elhacham, Emily; Wang, Sheng-Hsiang

2017-01-01

Version 1 of the NASA MERRA Aerosol Reanalysis (MERRAero) assimilates bias-corrected 18 aerosol optical depth (AOD) data from MODIS-Terra and MODIS-Aqua, and simulates particulate 19 matter (PM) concentration data to reproduce a consistent database of AOD and PM concentration around 20 the world from 2002 to the end of 2015. The purpose of this paper is to evaluate MERRAeros simulation 21 of fine PM concentration against surface measurements in two regions of the world with relatively high 22 levels of PM concentration but with profoundly different PM composition, those of Israel and Taiwan. 23 Being surrounded by major deserts, Israels PM load is characterized by a significant contribution of 24 mineral dust, and secondary contributions of sea salt particles, given its proximity to the Mediterranean 25 Sea, and sulfate particles originating from Israels own urban activities and transported from Europe. 26 Taiwans PM load is composed primarily of anthropogenic particles (sulfate, nitrate and carbonaceous 27 particles) locally produced or transported from China, with an additional contribution of springtime 28 transport of mineral dust originating from Chinese and Mongolian deserts. The evaluation in Israel 29 produced favorable results with MERRAero slightly overestimating measurements by 6 on average 30 and reproducing an excellent year-to-year and seasonal fluctuation. The evaluation in Taiwan was less 31 favorable with MERRAero underestimating measurements by 42 on average. Two likely reasons 32 explain this discrepancy: emissions of anthropogenic PM and their precursors are largely uncertain in 33 China, and MERRAero doesnt include nitrate particles in its simulation, a pollutant of predominately 34 anthropogenic sources. MERRAero nevertheless simulates well the concentration of fine PM during the 35 summer, when Taiwan is least affected by the advection of pollution from China.

Impact of the 2009 Attica wild fires on the air quality in urban Athens

NASA Astrophysics Data System (ADS)

Amiridis, V.; Zerefos, C.; Kazadzis, S.; Gerasopoulos, E.; Eleftheratos, K.; Vrekoussis, M.; Stohl, A.; Mamouri, R. E.; Kokkalis, P.; Papayannis, A.; Eleftheriadis, K.; Diapouli, E.; Keramitsoglou, I.; Kontoes, C.; Kotroni, V.; Lagouvardos, K.; Marinou, E.; Giannakaki, E.; Kostopoulou, E.; Giannakopoulos, C.; Richter, A.; Burrows, J. P.; Mihalopoulos, N.

2012-01-01

At the end of August 2009, wild fires ravaged the north-eastern fringes of Athens destroying invaluable forest wealth of the Greek capital. In this work, the impact of these fires on the air quality of Athens and surface radiation levels is examined. Satellite imagery, smoke dispersion modeling and meteorological data confirm the advection of smoke under cloud-free conditions over the city of Athens. Lidar measurements showed that the smoke plume dispersed in the free troposphere and lofted over the city reaching heights between 2 and 4 km. Ground-based sunphotometric measurements showed extreme aerosol optical depth, reaching nearly 6 in the UV wavelength range, accompanied by a reduction up to 70% of solar irradiance at ground. The intensive aerosol optical properties, namely the Ångström exponent, the lidar ratio, and the single scattering albedo, showed typical values for highly absorbing fresh smoke particles. In-situ air quality measurements revealed the impact of the smoke plume down to the surface with a slight delay on both the particulate and gaseous phase. Surface aerosols increase was encountered mainly in the fine mode with prominent elevation of OC and EC levels. Photochemical processes, studied via NO x titration of O 3, were also shown to be different compared to typical urban photochemistry.

Review of Urban Secondary Organic Aerosol Formation from Gasoline and Diesel Motor Vehicle Emissions.

PubMed

Gentner, Drew R; Jathar, Shantanu H; Gordon, Timothy D; Bahreini, Roya; Day, Douglas A; El Haddad, Imad; Hayes, Patrick L; Pieber, Simone M; Platt, Stephen M; de Gouw, Joost; Goldstein, Allen H; Harley, Robert A; Jimenez, Jose L; Prévôt, André S H; Robinson, Allen L

2017-02-07

Secondary organic aerosol (SOA) is formed from the atmospheric oxidation of gas-phase organic compounds leading to the formation of particle mass. Gasoline- and diesel-powered motor vehicles, both on/off-road, are important sources of SOA precursors. They emit complex mixtures of gas-phase organic compounds that vary in volatility and molecular structure-factors that influence their contributions to urban SOA. However, the relative importance of each vehicle type with respect to SOA formation remains unclear due to conflicting evidence from recent laboratory, field, and modeling studies. Both are likely important, with evolving contributions that vary with location and over short time scales. This review summarizes evidence, research needs, and discrepancies between top-down and bottom-up approaches used to estimate SOA from motor vehicles, focusing on inconsistencies between molecular-level understanding and regional observations. The effect of emission controls (e.g., exhaust aftertreatment technologies, fuel formulation) on SOA precursor emissions needs comprehensive evaluation, especially with international perspective given heterogeneity in regulations and technology penetration. Novel studies are needed to identify and quantify "missing" emissions that appear to contribute substantially to SOA production, especially in gasoline vehicles with the most advanced aftertreatment. Initial evidence suggests catalyzed diesel particulate filters greatly reduce emissions of SOA precursors along with primary aerosol.

GoAmazon2014/15. Oxidation Flow Reactor Final Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jimenez, J. L.; Day, D. A.; Hu, W.

The primary goal of the Green Ocean Amazon (GoAmazon2014/5) field campaign was to measure and mechanistically understand the formation of particle number and mass in a region affected by large tropical rainforest biogenic emissions and sometimes anthropogenic influence from a large urban center. As part of the two intensive operational periods (IOPs) and in collaboration with Pacific Northwest National Laboratory (PNNL) and Harvard, the Jimenez Group proposed to deploy a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS), Thermal Denuder (TD), Scanning Mobility Particle Size (SMPS), two oxidation flow reactors (OFR; including supporting O 3, CO/CO 2/CH 4, RH analyzers), and amore » high volume filter sampler (MCV) for the measurement of gas and aerosol chemical, physicochemical, and volatility properties. The two IOPs were conducted during the wet season (February to March, 2014) and dry season (August to October, 2014). This proposal was part of a collaborative proposal involving other university and government laboratories.« less

The Chemical Composition and Mixing State of Sea Spray Aerosol and Organic Aerosol in the Winter-Spring Arctic

NASA Astrophysics Data System (ADS)

Kirpes, R.; Bondy, A. L.; Bonanno, D.; Moffet, R.; Wang, B.; Laskin, A.; Ault, A. P.; Pratt, K.

2016-12-01

The Arctic region is undergoing rapid transformations and loss of sea ice due to climate change. With increased sea ice fracturing resulting in greater open ocean surface, winter emissions of sea spray aerosol (SSA) are expected to be increasing. Additionally, during the winter-spring transition, Arctic haze contributes to the Arctic aerosol budget. The magnitude of aerosol climate effects depends on the aerosol composition and mixing state (distribution of chemical species within and between particles). However, few studies of aerosol chemistry have been conducted in the winter Arctic, despite it being a time when aerosol impacts on clouds are expected to be significant. To study aerosol composition and mixing state in the winter Arctic, atmospheric particles were collected near Barrow, Alaska in January and February 2014 for off-line individual particle chemical analysis. SSA was the most prevalent particle type observed. Sulfate and nitrate were observed to be internally mixed with SSA and organic aerosol. Greater than 98% of observed SSA particles contained organic content, with 15-35% organic volume fraction on average for individual particles. The SSA organic compounds consisted of carbohydrates, lipids, and fatty acids found in the seawater surface microlayer. SSA was determined to be emitted from open leads, while transported sulfate and nitrate contributed to aging of SSA and organic aerosol. Determining the aerosol chemical composition and mixing state in the winter Arctic will further the understanding of how individual aerosol particles impact climate through radiative effects and cloud formation.

Street canyon aerosol pollutant transport measurements.

PubMed

Longley, I D; Gallagher, M W; Dorsey, J R; Flynn, M; Bower, K N; Allan, J D

2004-12-01

Current understanding of dispersion in street canyons is largely derived from relatively simple dispersion models. Such models are increasingly used in planning and regulation capacities but are based upon a limited understanding of the transport of substances within a real canyon. In recent years, some efforts have been made to numerically model localised flow in idealised canyons (e.g., J. Appl. Meteorol. 38 (1999) 1576-89) and stepped canyons (Assimakopoulos V. Numerical modelling of dispersion of atmospheric pollution in and above urban canopies. PhD thesis, Imperial College, London, 2001) but field studies in real canyons are rare. To further such an understanding, a measurement campaign has been conducted in an asymmetric street canyon with busy one-way traffic in central Manchester in northern England. The eddy correlation method was used to determine fluxes of size-segregated accumulation mode aerosol. Measurements of aerosol at a static location were made concurrently with measurements on a platform lift giving vertical profiles. Size-segregated measurements of ultrafine and coarse particle concentrations were also made simultaneously at various heights. In addition, a small mobile system was used to make measurements of turbulence at various pavement locations within the canyon. From this data, various features of turbulent transport and dispersion in the canyon will be presented. The concentration and the ventilation fluxes of vehicle-related aerosol pollutants from the canyon will be related to controlling factors. The results will also be compared with citywide ventilation data from a separate measurement campaign conducted above the urban canopy.

IS THE SIZE DISTRIBUTION OF URBAN AEROSOLS DETERMINED BY THERMODYNAMIC EQUILIBRIUM? (R826371C005)

EPA Science Inventory

A size-resolved equilibrium model, SELIQUID, is presented and used to simulate the size–composition distribution of semi-volatile inorganic aerosol in an urban environment. The model uses the efflorescence branch of aerosol behavior to predict the equilibrium partitioni...

Contribution of Isoprene Epoxydiol to Urban Organic Aerosol: Evidence from Modeling and Measurements

EPA Science Inventory

In a region heavily influenced by anthropogenic and biogenic atmospheric emissions, recent field measurements have attributed one third of urban organic aerosol by mass to isoprene epoxydiols (IEPOX). These aerosols arise from the gas phase oxidation of isoprene, the formation of...

Online single particle analysis of ice particle residuals from mountain-top mixed-phase clouds using laboratory derived particle type assignment

NASA Astrophysics Data System (ADS)

Schmidt, Susan; Schneider, Johannes; Klimach, Thomas; Mertes, Stephan; Schenk, Ludwig Paul; Kupiszewski, Piotr; Curtius, Joachim; Borrmann, Stephan

2017-01-01

In situ single particle analysis of ice particle residuals (IPRs) and out-of-cloud aerosol particles was conducted by means of laser ablation mass spectrometry during the intensive INUIT-JFJ/CLACE campaign at the high alpine research station Jungfraujoch (3580 m a.s.l.) in January-February 2013. During the 4-week campaign more than 70 000 out-of-cloud aerosol particles and 595 IPRs were analyzed covering a particle size diameter range from 100 nm to 3 µm. The IPRs were sampled during 273 h while the station was covered by mixed-phase clouds at ambient temperatures between -27 and -6 °C. The identification of particle types is based on laboratory studies of different types of biological, mineral and anthropogenic aerosol particles. The outcome of these laboratory studies was characteristic marker peaks for each investigated particle type. These marker peaks were applied to the field data. In the sampled IPRs we identified a larger number fraction of primary aerosol particles, like soil dust (13 ± 5 %) and minerals (11 ± 5 %), in comparison to out-of-cloud aerosol particles (2.4 ± 0.4 and 0.4 ± 0.1 %, respectively). Additionally, anthropogenic aerosol particles, such as particles from industrial emissions and lead-containing particles, were found to be more abundant in the IPRs than in the out-of-cloud aerosol. In the out-of-cloud aerosol we identified a large fraction of aged particles (31 ± 5 %), including organic material and secondary inorganics, whereas this particle type was much less abundant (2.7 ± 1.3 %) in the IPRs. In a selected subset of the data where a direct comparison between out-of-cloud aerosol particles and IPRs in air masses with similar origin was possible, a pronounced enhancement of biological particles was found in the IPRs.

Composition of individual aerosol particles above the Israelian Mediterranean coast during the summer time

NASA Astrophysics Data System (ADS)

Ganor, E.; Levin, Z.; Van Grieken, R.

Aerosol particles were collected aboard a ship in Haifa Bay and Tel Aviv, Israel, during the summer time. The aerosol particles (6170) were analyzed as individual particles and classified according to their chemical composition, size, number concentration per cubic centimeter and morphology. Most of the aerosol particles could be classified into four groups. The first contains gypsum from the sea and from industrial sources brought in by land breezes. A second group is characterized by continental aluminosilicate and quartz. A third group consists of sea salt mixed with sulfate particles. The fourth group is characterized by an abundance of sulfate particles, some of which are ammonium sulfate brought by the land breezes. The particles were identified as marine and mineral aerosols which originated in Eastern Europe and the Mediterranean sea, while local aerosols brought by land breeze characterized by phosphate, fly ash and soil particles originated in the Haifa industrial zone. In addition, the aerosols were analyzed for sulfates and nitrates. Aerosols of sea and land breezes differed as follows: (1) Sulfate and nitrate concentrations in the aerosols were 5-10 times higher during land breeze than during sea breeze, and the total content of suspended particles was, respectively, 6-12 times higher. (2) Particle size spectra during land breeze were broader than during sea breeze and their concentrations were about 20 times greater. Analyses of individual particles by electron microscopy revealed that during the sea breeze the aerosols contained calcium sulfate, sodium sulfate and sulfuric acid. The sulfuric acid, of pH 2.5, is due to the long-range transport as previously reported ( Ganor et al., 1993) while the other sulfates are from the sea. This explains the high concentration of sulfates in the atmospheric sea breeze above the Israelian Mediterranean coast during the summertime.

Molecular characterization of organosulfates in organic aerosols from Shanghai and Los Angeles urban areas by nanospray-desorption electrospray ionization high-resolution mass spectrometry.

PubMed

Tao, Shikang; Lu, Xiaohui; Levac, Nicole; Bateman, Adam P; Nguyen, Tran B; Bones, David L; Nizkorodov, Sergey A; Laskin, Julia; Laskin, Alexander; Yang, Xin

2014-09-16

Fine aerosol particles in the urban areas of Shanghai and Los Angeles were collected on days that were characterized by their stagnant air and high organic aerosol concentrations. They were analyzed by nanospray-desorption electrospray ionization mass spectrometry with high mass resolution (m/Δm = 100,000). Solvent mixtures of acetonitrile and water and acetonitrile and toluene were used to extract and ionize polar and nonpolar compounds, respectively. A diverse mixture of oxygenated hydrocarbons, organosulfates, organonitrates, and organics with reduced nitrogen were detected in the Los Angeles sample. A majority of the organics in the Shanghai sample were detected as organosulfates. The dominant organosulfates that were detected at two locations have distinctly different molecular characteristics. Specifically, the organosulfates in the Los Angeles sample were dominated by biogenic products, while the organosulfates of a yet unknown origin found in the Shanghai sample had distinctive characteristics of long aliphatic carbon chains and low degrees of oxidation and unsaturation. The use of the acetonitrile and toluene solvent facilitated the observation of this type of organosulfates, which suggests that they could have been missed in previous studies that relied on sample extraction using common polar solvents. The high molecular weight and low degree of unsaturation and oxidization of the uncommon organosulfates suggest that they may act as surfactants and plausibly affect the surface tension and hygroscopicity of atmospheric particles. We propose that direct esterification of carbonyl or hydroxyl compounds by sulfates or sulfuric acid in the liquid phase could be the formation pathway of these special organosulfates. Long-chain alkanes from vehicle emissions might be their precursors.

The Green Ocean Amazon Experiment (GoAmazon2014/5) Observes Pollution Affecting Gases, Aerosols, Clouds, and Rainfall over the Rain Forest

DOE PAGES

Martin, S. T.; Artaxo, P.; Machado, L.; ...

2017-05-15

The Observations and Modeling of the Green Ocean Amazon 2014–2015 (GoAmazon2014/5) experiment took place around the urban region of Manaus in central Amazonia across 2 years. The urban pollution plume was used to study the susceptibility of gases, aerosols, clouds, and rainfall to human activities in a tropical environment. Many aspects of air quality, weather, terrestrial ecosystems, and climate work differently in the tropics than in the more thoroughly studied temperate regions of Earth. GoAmazon2014/5, a cooperative project of Brazil, Germany, and the United States, employed an unparalleled suite of measurements at nine ground sites and on board two aircraftmore » to investigate the flow of background air into Manaus, the emissions into the air over the city, and the advection of the pollution downwind of the city. Here in this paper, to visualize this train of processes and its effects, observations aboard a low-flying aircraft are presented. Comparative measurements within and adjacent to the plume followed the emissions of biogenic volatile organic carbon compounds (BVOCs) from the tropical forest, their transformations by the atmospheric oxidant cycle, alterations of this cycle by the influence of the pollutants, transformations of the chemical products into aerosol particles, the relationship of these particles to cloud condensation nuclei (CCN) activity, and the differences in cloud properties and rainfall for background compared to polluted conditions. The observations of the GoAmazon2014/5 experiment illustrate how the hydrologic cycle, radiation balance, and carbon recycling may be affected by present-day as well as future economic development and pollution over the Amazonian tropical forest.« less

The Green Ocean Amazon Experiment (GoAmazon2014/5) Observes Pollution Affecting Gases, Aerosols, Clouds, and Rainfall over the Rain Forest

DOE Office of Scientific and Technical Information (OSTI.GOV)

Martin, S. T.; Artaxo, P.; Machado, L.

The Observations and Modeling of the Green Ocean Amazon 2014–2015 (GoAmazon2014/5) experiment took place around the urban region of Manaus in central Amazonia across 2 years. The urban pollution plume was used to study the susceptibility of gases, aerosols, clouds, and rainfall to human activities in a tropical environment. Many aspects of air quality, weather, terrestrial ecosystems, and climate work differently in the tropics than in the more thoroughly studied temperate regions of Earth. GoAmazon2014/5, a cooperative project of Brazil, Germany, and the United States, employed an unparalleled suite of measurements at nine ground sites and on board two aircraftmore » to investigate the flow of background air into Manaus, the emissions into the air over the city, and the advection of the pollution downwind of the city. Here in this paper, to visualize this train of processes and its effects, observations aboard a low-flying aircraft are presented. Comparative measurements within and adjacent to the plume followed the emissions of biogenic volatile organic carbon compounds (BVOCs) from the tropical forest, their transformations by the atmospheric oxidant cycle, alterations of this cycle by the influence of the pollutants, transformations of the chemical products into aerosol particles, the relationship of these particles to cloud condensation nuclei (CCN) activity, and the differences in cloud properties and rainfall for background compared to polluted conditions. The observations of the GoAmazon2014/5 experiment illustrate how the hydrologic cycle, radiation balance, and carbon recycling may be affected by present-day as well as future economic development and pollution over the Amazonian tropical forest.« less

Simulation of aerosol radiative properties with the ORISAM-RAD model during a pollution event (ESCOMPTE 2001)

NASA Astrophysics Data System (ADS)

Mallet, M.; Pont, V.; Liousse, C.; Roger, J. C.; Dubuisson, P.

The aim of this study is to present the organic and inorganic spectral aerosol module-radiative (ORISAM-RAD) module, allowing the 3D distribution of aerosol radiative properties (aerosol optical depth, single scattering albedo and asymmetry parameter) from the ORISAM module. In this work, we test ORISAM-RAD for one selected day (24th June) during the ESCOMPTE (expérience sur site pour contraindre les modèles de pollution atmosphérique et de transport d'emissions) experiment for an urban/industrial aerosol type. The particle radiative properties obtained from in situ and AERONET observations are used to validate our simulations. In a first time, simulations obtained from ORISAM-RAD indicate high aerosol optical depth (AOD)˜0.50-0.70±0.02 (at 440 nm) in the aerosol pollution plume, slightly lower (˜10-20%) than AERONET retrievals. In a second time, simulations of the single scattering albedo ( ωo) have been found to well reproduce the high spatial heterogeneities observed over this domain. Concerning the asymmetry parameter ( g), ORISAM-RAD simulations reveal quite uniform values over the whole ESCOMPTE domain, comprised between 0.61±0.01 and 0.65±0.01 (at 440 nm), in excellent agreement with ground based in situ measurements and AERONET retrievals. Finally, the outputs of ORISAM-RAD have been used in a radiative transfer model in order to simulate the diurnal direct radiative forcing at different locations (urban, industrial and rural). We show that anthropogenic aerosols strongly decrease surface solar radiation, with diurnal mean surface forcings comprised between -29.0±2.9 and -38.6±3.9 W m -2, depending on the sites. This decrease is due to the reflection of solar radiations back to space (-7.3±0.8<Δ FTOA<-12.3±1.2 W m -2) and to its absorption into the aerosol layer (21.1±2.1<Δ FATM<26.3±2.6 W m -2). These values are found to be consistent with those measured at local scale.

Retrieval of Aerosol Properties

NASA Astrophysics Data System (ADS)

de Leeuw, Gerrit; Kinne, Stefan; Léon, Jean-Francois; Pelon, Jacques; Rosenfeld, Daniel; Schaap, Martijn; Veefkind, Pepijn J.; Veihelmann, Ben; Winker, David M.; von Hoyningen-Huene, Wolfgang

Atmospheric aerosol is a suspension of liquid and solid particles in air, i.e. the aerosol includes both particles and its surrounding medium; in practice aerosol is usually referred to as the suspended matter, i.e. the particles or the droplets, depending on their aggregation state.

Ambient in-situ immersion freezing measurements - findings from the ZAMBIS 2014 field campaign for three ice nucleation techniques

NASA Astrophysics Data System (ADS)

Kohn, Monika; Atkinson, James D.; Lohmann, Ulrike; Kanji, Zamin A.

2015-04-01

To estimate the influence of clouds on the Earth's radiation budget, it is crucial to understand cloud formation processes in the atmosphere. A key process, which significantly affects cloud microphysical properties and the initiation of precipitation thus contributing to the hydrological cycle, is the prevailing type of ice nucleation mechanism. In mixed-phase clouds immersion freezing is the dominant ice crystal forming mechanism, whereby ice nucleating particles (INP) first act as cloud condensation nuclei (CCN) and are activated to cloud droplets followed by freezing upon supercooling. There are a number of experimental methods and techniques to investigate the ice nucleating ability in the immersion mode, however most techniques are offline for field sampling or only suitable for laboratory measurements. In-situ atmospheric studies are needed to understand the ice formation processes of 'real world' particles. Laboratory experiments simulate conditions of atmospheric processes like ageing or coating but are still idealized. Our method is able to measure ambient in-situ immersion freezing on single immersed aerosol particles. The instrumental setup consists of the recently developed portable immersion mode cooling chamber (PIMCA) as a vertical extension to the portable ice nucleation chamber (PINC, [1]), where the frozen fraction of activated aerosol particles are detected by the ice optical depolarization detector (IODE, [2]). Two additional immersion freezing techniques based on a droplet freezing array [3,4] are used to sample ambient aerosol particles either in a suspension (fraction larger ~0.6 μm) or on PM10-filters to compare different ice nucleation techniques. Here, we present ambient in-situ measurements at an urban forest site in Zurich, Switzerland held during the Zurich ambient immersion freezing study (ZAMBIS) in spring 2014. We investigated the ice nucleating ability of natural atmospheric aerosol with the PIMCA/PINC immersion freezing setup as well as a droplet freezing method on aerosol particles either collected in a suspension or on PM10-filters to obtain atmospheric IN concentrations based on the measured ambient aerosol. Investigation of physical properties (number and size distribution) and chemical composition as well as the meteorological conditions provide supplementary information that help to understand the nature of particles and air masses that contribute to immersion freezing. Acknowledgements We thank Hannes Wydler and Hansjörg Frei from ETH Zurich for their technical support. Furthermore, the authors want thank Franz Conen from the University of Basel for sharing equipment and training in the drop freezing experiment. References [1] Chou et al. (2011), Atmos. Chem. Phys., 11, 4725-4738. [2] Nicolet et al. (2010), Atmos. Chem. Phys., 10, 313-325. [3] Conen et al. (2012), Atmos. Meas. Tech., 5, 321-327. [4] Stopelli et al. (2014), Atmos. Meas. Tech., 7, 129-134.

Urbanization-induced urban heat island and aerosol effects on climate extremes in the Yangtze River Delta region of China

NASA Astrophysics Data System (ADS)

Zhong, Shi; Qian, Yun; Zhao, Chun; Leung, Ruby; Wang, Hailong; Yang, Ben; Fan, Jiwen; Yan, Huiping; Yang, Xiu-Qun; Liu, Dongqing

2017-04-01

The WRF-Chem model coupled with a single-layer urban canopy model (UCM) is integrated for 5 years at convection-permitting scale to investigate the individual and combined impacts of urbanization-induced changes in land cover and pollutant emissions on regional climate in the Yangtze River Delta (YRD) region in eastern China. Simulations with the urbanization effects reasonably reproduced the observed features of temperature and precipitation in the YRD region. Urbanization over the YRD induces an urban heat island (UHI) effect, which increases the surface temperature by 0.53 °C in summer and increases the annual heat wave days at a rate of 3.7 d yr-1 in the major megacities in the YRD, accompanied by intensified heat stress. In winter, the near-surface air temperature increases by approximately 0.7 °C over commercial areas in the cities but decreases in the surrounding areas. Radiative effects of aerosols tend to cool the surface air by reducing net shortwave radiation at the surface. Compared to the more localized UHI effect, aerosol effects on solar radiation and temperature influence a much larger area, especially downwind of the city cluster in the YRD. Results also show that the UHI increases the frequency of extreme summer precipitation by strengthening the convergence and updrafts over urbanized areas in the afternoon, which favor the development of deep convection. In contrast, the radiative forcing of aerosols results in a surface cooling and upper-atmospheric heating, which enhances atmospheric stability and suppresses convection. The combined effects of the UHI and aerosols on precipitation depend on synoptic conditions. Two rainfall events under two typical but different synoptic weather patterns are further analyzed. It is shown that the impact of urban land cover and aerosols on precipitation is not only determined by their influence on local convergence but also modulated by large-scale weather systems. For the case with a strong synoptic forcing associated with stronger winds and larger spatial convergence, the UHI and aerosol effects are relatively weak. When the synoptic forcing is weak, however, the UHI and aerosol effects on local convergence dominate. This suggests that synoptic forcing plays a significant role in modulating the urbanization-induced land-cover and aerosol effects on individual rainfall event. Hence precipitation changes due to urbanization effects may offset each other under different synoptic conditions, resulting in little changes in mean precipitation at longer timescales.

Urbanization-induced urban heat island and aerosol effects on climate extremes in the Yangtze River Delta region of China

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhong, Shi; Qian, Yun; Zhao, Chun

The WRF-Chem model coupled with a single-layer urban canopy model (UCM) is integrated for 5 years at convection-permitting scale to investigate the individual and combined impacts of urbanization-induced changes in land cover and pollutant emissions on regional climate in the Yangtze River Delta (YRD) region in eastern China. Simulations with the urbanization effects reasonably reproduced the observed features of temperature and precipitation in the YRD region. Urbanization over the YRD induces an urban heat island (UHI) effect, which increases the surface temperature by 0.53 °C in summer and increases the annual heat wave days at a rate of 3.7 d yr −1 in themore » major megacities in the YRD, accompanied by intensified heat stress. In winter, the near-surface air temperature increases by approximately 0.7 °C over commercial areas in the cities but decreases in the surrounding areas. Radiative effects of aerosols tend to cool the surface air by reducing net shortwave radiation at the surface. Compared to the more localized UHI effect, aerosol effects on solar radiation and temperature influence a much larger area, especially downwind of the city cluster in the YRD. Results also show that the UHI increases the frequency of extreme summer precipitation by strengthening the convergence and updrafts over urbanized areas in the afternoon, which favor the development of deep convection. In contrast, the radiative forcing of aerosols results in a surface cooling and upper-atmospheric heating, which enhances atmospheric stability and suppresses convection. The combined effects of the UHI and aerosols on precipitation depend on synoptic conditions. Two rainfall events under two typical but different synoptic weather patterns are further analyzed. It is shown that the impact of urban land cover and aerosols on precipitation is not only determined by their influence on local convergence but also modulated by large-scale weather systems. For the case with a strong synoptic forcing associated with stronger winds and larger spatial convergence, the UHI and aerosol effects are relatively weak. When the synoptic forcing is weak, however, the UHI and aerosol effects on local convergence dominate. This suggests that synoptic forcing plays a significant role in modulating the urbanization-induced land-cover and aerosol effects on individual rainfall event. Hence precipitation changes due to urbanization effects may offset each other under different synoptic conditions, resulting in little changes in mean precipitation at longer timescales.« less

Urbanization-induced urban heat island and aerosol effects on climate extremes in the Yangtze River Delta region of China

DOE PAGES

Zhong, Shi; Qian, Yun; Zhao, Chun; ...

2017-04-27

The WRF-Chem model coupled with a single-layer urban canopy model (UCM) is integrated for 5 years at convection-permitting scale to investigate the individual and combined impacts of urbanization-induced changes in land cover and pollutant emissions on regional climate in the Yangtze River Delta (YRD) region in eastern China. Simulations with the urbanization effects reasonably reproduced the observed features of temperature and precipitation in the YRD region. Urbanization over the YRD induces an urban heat island (UHI) effect, which increases the surface temperature by 0.53 °C in summer and increases the annual heat wave days at a rate of 3.7 d yr −1 in themore » major megacities in the YRD, accompanied by intensified heat stress. In winter, the near-surface air temperature increases by approximately 0.7 °C over commercial areas in the cities but decreases in the surrounding areas. Radiative effects of aerosols tend to cool the surface air by reducing net shortwave radiation at the surface. Compared to the more localized UHI effect, aerosol effects on solar radiation and temperature influence a much larger area, especially downwind of the city cluster in the YRD. Results also show that the UHI increases the frequency of extreme summer precipitation by strengthening the convergence and updrafts over urbanized areas in the afternoon, which favor the development of deep convection. In contrast, the radiative forcing of aerosols results in a surface cooling and upper-atmospheric heating, which enhances atmospheric stability and suppresses convection. The combined effects of the UHI and aerosols on precipitation depend on synoptic conditions. Two rainfall events under two typical but different synoptic weather patterns are further analyzed. It is shown that the impact of urban land cover and aerosols on precipitation is not only determined by their influence on local convergence but also modulated by large-scale weather systems. For the case with a strong synoptic forcing associated with stronger winds and larger spatial convergence, the UHI and aerosol effects are relatively weak. When the synoptic forcing is weak, however, the UHI and aerosol effects on local convergence dominate. This suggests that synoptic forcing plays a significant role in modulating the urbanization-induced land-cover and aerosol effects on individual rainfall event. Hence precipitation changes due to urbanization effects may offset each other under different synoptic conditions, resulting in little changes in mean precipitation at longer timescales.« less

Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yang; Pinterich, Tamara; Wang, Jian

We present rapid measurement of submicron particle size distributions enables the characterization of aerosols with fast changing properties, and is often necessary for measurements onboard mobile platforms (e.g., research aircraft). Aerosol mobility size distribution is commonly measured by a scanning mobility particle sizer (SMPS), which relies on voltage scanning or stepping to classify particles of different sizes, and may take up to several minutes to obtain a complete size spectrum of aerosol particles. The recently developed fast integrated mobility spectrometer (FIMS) with enhanced dynamic size range classifies and detects particles from 10 to ~600 nm simultaneously, allowing submicron aerosol mobilitymore » size distributions to be captured at a time resolution of 1 second. In this study, we present a detailed data inversion routine for deriving aerosol size distribution from FIMS measurements. The inversion routine takes into consideration the FIMS transfer function, particle penetration efficiency in the FIMS, and multiple charging of aerosols. The accuracy of the FIMS measurement is demonstrated by comparing parallel FIMS and SMPS measurements of stable aerosols with a wide range of size spectrum shapes, including ambient aerosols and aerosols classified by a differential mobility analyzer (DMA). The FIMS and SMPS-derived size distributions show excellent agreements for all aerosols tested. In addition, total number concentrations of ambient aerosols were integrated from 1 Hz FIMS size distributions, and compared with those directly measured by a condensation particle counter (CPC) operated in parallel. Finally, the integrated and measured total particle concentrations agree well within 5%.« less

Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer

DOE PAGES

Wang, Yang; Pinterich, Tamara; Wang, Jian

2018-03-30

We present rapid measurement of submicron particle size distributions enables the characterization of aerosols with fast changing properties, and is often necessary for measurements onboard mobile platforms (e.g., research aircraft). Aerosol mobility size distribution is commonly measured by a scanning mobility particle sizer (SMPS), which relies on voltage scanning or stepping to classify particles of different sizes, and may take up to several minutes to obtain a complete size spectrum of aerosol particles. The recently developed fast integrated mobility spectrometer (FIMS) with enhanced dynamic size range classifies and detects particles from 10 to ~600 nm simultaneously, allowing submicron aerosol mobilitymore » size distributions to be captured at a time resolution of 1 second. In this study, we present a detailed data inversion routine for deriving aerosol size distribution from FIMS measurements. The inversion routine takes into consideration the FIMS transfer function, particle penetration efficiency in the FIMS, and multiple charging of aerosols. The accuracy of the FIMS measurement is demonstrated by comparing parallel FIMS and SMPS measurements of stable aerosols with a wide range of size spectrum shapes, including ambient aerosols and aerosols classified by a differential mobility analyzer (DMA). The FIMS and SMPS-derived size distributions show excellent agreements for all aerosols tested. In addition, total number concentrations of ambient aerosols were integrated from 1 Hz FIMS size distributions, and compared with those directly measured by a condensation particle counter (CPC) operated in parallel. Finally, the integrated and measured total particle concentrations agree well within 5%.« less

Development of a remote sensing algorithm to retrieve atmospheric aerosol properties using multiwavelength and multipixel information

NASA Astrophysics Data System (ADS)

Hashimoto, Makiko; Nakajima, Teruyuki

2017-06-01

We developed a satellite remote sensing algorithm to retrieve the aerosol optical properties using satellite-received radiances for multiple wavelengths and pixels. Our algorithm utilizes spatial inhomogeneity of surface reflectance to retrieve aerosol properties, and the main target is urban aerosols. This algorithm can simultaneously retrieve aerosol optical thicknesses (AOT) for fine- and coarse-mode aerosols, soot volume fraction in fine-mode aerosols (SF), and surface reflectance over heterogeneous surfaces such as urban areas that are difficult to obtain by conventional pixel-by-pixel methods. We applied this algorithm to radiances measured by the Greenhouse Gases Observing Satellite/Thermal and Near Infrared Sensor for Carbon Observations-Cloud and Aerosol Image (GOSAT/TANSO-CAI) at four wavelengths and were able to retrieve the aerosol parameters in several urban regions and other surface types. A comparison of the retrieved AOTs with those from the Aerosol Robotic Network (AERONET) indicated retrieval accuracy within ±0.077 on average. It was also found that the column-averaged SF and the aerosol single scattering albedo (SSA) underwent seasonal changes as consistent with the ground surface measurements of SSA and black carbon at Beijing, China.

Evaluation of Aerosol Properties over Ocean from Moderate Resolution Imaging Spectroradiometer (MODIS) during ACE-Asia

NASA Technical Reports Server (NTRS)

Chu, D. A.; Remer, L. A.; Kaufman, Y. J.; Schmid, B.; Redemann, J.; Knobelspiesse, K.; Chern, J.-D.; Livingston, J.; Russell, P. B.; Xiong, X.;

Clear Sky Column Closure Studies of Urban-Marine and Mineral-Dust Aerosols Using Aircraft, Ship, Satellite and Ground-Based Measurements in ACE-2

NASA Technical Reports Server (NTRS)

Schmid, Beat; Russell, Philip B.; Livingston, John M.; Gasso, Santiago; Hegg, Dean A.; Collins, Donald R.; Flagan, Richard C.; Seinfeld, John H.; Oestroem, Elisabeth; Noone, Kevin J.;

Low-cost wind tunnel for aerosol inhalation studies.

PubMed

Chung, I P; Dunn-Rankin, D; Phalen, R F; Oldham, M J

1992-04-01

A low-cost wind tunnel for aerosol studies has been designed, constructed, and evaluated for aerosol uniformity with 2- and 0.46-micron particles. A commercial nebulizer was used to produce the suspended test particles, and a custom-made, four-hole injector was used to introduce the aerosol into the wind tunnel. A commercially available optical particle counter measured the particle concentration. Performance tests of the velocity profile and particle concentration distribution at two flow rates showed that the system performs well for small particles.

Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

NASA Astrophysics Data System (ADS)

Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

2017-12-01

The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

Composition and Morphology of Individual Combustion, Biomass Burning, and Secondary Organic Particle Types Obtained Using ATOFMS and STXM-NEXAFS Measurements (Invited)

NASA Astrophysics Data System (ADS)

Russell, L. M.; Bahadur, R.; Liu, S.; Takahama, S.; Prather, K. A.

2010-12-01

Complementary single particle measurements of organic aerosols using aerosol time-of-flight mass spectrometry (ATOFMS) and Scanning Transmission X-ray Microscopy—Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS) are compared to examine the relationships between particle morphologies and chemical composition of particles having similar sources. ATOFMS measurements from field campaigns in polluted or urban (Riverside/SOAR 2005; Mexico City/MILAGRO 2006; Port of Long Beach 2007) and clean or marine (Arabian Sea/INDOEX 1999; Sea of Japan/ACE-Asia 2001; Trinidad Head/CIFEX 2004) locations illustrate regional differences in the amount and types of organic particles. The majority (≥ 85%) of the number of submicron particles are carbonaceous (including elemental and organic carbon), but represent less than 10% of the number of supermicron particles. Organic carbon (OC) particles are classified into three meta-classes corresponding to (1) combustion-generated OC/EC internalmixtures, (2) biomass burning generated K/OC mixtures, and (3) OC/High MassOC (HMOC) mixtures containing secondary markers of atmospheric processing. Normalized dot products are used to quantify similarity among fragment spectra and indicate that OC particle types are consistent across (and within) platforms. Single particle carbon STXM-NEXAFS measurements during ACE-Asia 2001 and MILAGRO 2006 yield similar source categories based on relative abundances of aromatic, alkane, and carboxylic acid functional groups. All three organic particle types correspond to a variety of very heterogeneous particle morphologies, although the highly oxygenated OC particles with likely secondary organic contributions frequently are nearly spherical, liquid-like particles. Similar particle types are observed at many other locations, including recent measurements at Bakersfield, Tijuana, and the R/V Atlantis as part of CalNex and CalMex. Size-resolved number fractions of the major ATOFMS organic particle types show qualitative agreement with OC particle types from STXM NEXAFS analysis, indicating a correspondence of the OC/EC type with the presence of strong aromatic groups, of the OC/HMOC type with high carboxylic acid groups, and of the biomass burning OC type with aromatic and carbonyl groups. The comparison shows that ATOFMS measurements can be used to establish robust statistics for offline single particle techniques, providing the atmospheric context for the functional group and morphological information obtained from STXM-NEXAFS for an improved understanding of the climate impact of organic aerosols.

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

NASA Astrophysics Data System (ADS)

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-05-01

An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but evaporative phenomena were not sufficient to explain the dependence of aerosol detection on particle diameter. Additional work is needed to correlate experimental data with theory for metal-oxides where thermodynamic property data are sparse relative to pure elements. Lastly, when matrix effects and the diffusion of ions inside the plasma were considered, mass loading was concluded to have had an effect on the dependence of detection efficiency on particle diameter.

Original sounding and drifting balloon-borne measurements in the western Mediterranean with the aerosol counter/sizer LOAC during summer ChArMEx campaigns, with a focus on desert dust events

NASA Astrophysics Data System (ADS)

Renard, Jean-Baptiste; Dulac, François; Vignelles, Damien; Jeannot, Matthieu; Verdier, Nicolas; Chazette, Patrick; Crenn, Vincent; Sciare, Jean; Totems, Julien; Durand, Pierre; Barret, Brice; Jambert, Corinne; Mallet, Marc; Menut, Laurent; Mailler, Sylvain; Basart, Sara; Baldasano, José Maria

2015-04-01

LOAC (Light Optical Aerosol Counter) is a new small optical particle counter/sizer of ~250 grams designed to fly under all kinds of balloons. The measurements are conducted at two scattering angles (12° and 60°), allowing the determination of the aerosol particle concentrations in 19 size classes within a diameter range of ~0.2-100 µm and some identification of the nature of particles dominating different size classes. Following laboratory calibration, the sensor particularly discriminates wet or liquid particles, mineral dust, soot carbon particles and salts. Comparisons with other in situ sensors at the surface and with remote sensing measurements on the vertical were performed to give confidence in measurements. The instrument has been operated at the surface, under all kinds of balloons up to more than 35 km in altitude, including tethered, sounding, open stratospheric and new boundary-layer pressurized drifting balloons (BLPB) from CNES, and was tested on board a small UAV. Operations encompass a variety of environments including the Arctic (Reykjavik, Island, and Kiruna, Sweden), Brazil (Sao Paolo), the western Mediterranean Basin, southwestern France, peri-urban (Ile de France) and urban areas (Paris and Vienna). Presented results are focused on the LOAC balloon-borne measurements performed in the western Mediterranean basin during MISTRALS/ChArMEx campaigns (Mediterranean Integrated Studies aT Regional And Local Scales/the Chemistry-Aerosol Mediterranean Experiment; http://www.mistrals-hjome.org; http://charmex.lsce.ipsl.fr), with a focus on African dust events. Two test flights with a first version of LOAC under sounding balloons were first successfully performed in late June 2012 near Marseille during an intense dust event. In 2013, 19 LOAC flights have been performed under meteorological balloons and 12 under low altitude drifting balloons, most of them from Minorca Island (Spain) in June and early July and others from Levant Island (south of France) in late July and early August . A number of the 2013 flights were coupled with ozone concentration measurements (see presentation of Gheusi et al. in the same session). LOAC balloons were especially, but not only, dedicated to study the various Saharan dust events that occurred during the campaign. In particular, a series of flights were conducted every 12 hours during the 15-19 June dust event. Forest fire smoke from North America was also sampled in late June over Minorca, as well as anthropogenic polluted layers in various occasions. LOAC data (available from ChArMEx database http://mistrals.sedoo.fr/ChArMEx) are interpreted with the help of coincident lidar, sun photometer remote sensing measurements available in Menorca, and satellite products and air mass trajectories. The sounding flights allow us to determine the vertical extent of the various aerosol layers, and to follow the particle size distribution and the concentration evolution along the vertical. The low altitude drifting balloons, which stayed roughly at constant altitude between 350 and 3330 m up to more than 25 h, allow us to study the time-evolution of the aerosol concentrations in the same air mass. Under both balloon types, LOAC has detected larges particles up to ~30 µm in diameter. The flights drifting within dust layers indicate that there is a relatively stable particle size distribution during transport over the sea, with no clear sedimentation loss of large particles. Aerosol simulations with the CHIMERE and NMMB/§BSC chemistry-transport models are compared to LOAC measurements. Acknowledgements: LOAC was developed with support of the French ANR. Balloon operations were performed by CNES and special acknowledgements are addressed to Gilles Dupouy, Françoise Douchin and collaborators for field operations. Alexis Doerenbacher from Météo-France and Claude Basdevant from Ecole Polytechnique are also acknowledged for their helpful contribution in providing balloon-related forecasts, quicklooks and data (http://www.lmd.polytechnique.fr/BAMED/index.html). The LOAC balloon campaigns were mainly funded by CNES, ADEME and CNRS/INSU, with support from CEA and Météo-France.

Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

NASA Astrophysics Data System (ADS)

Logan, Timothy S.

Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the selected four Asian sites. A strongly absorbing mineral dust influence is seen at the Xianghe, Taihu, and SACOL sites during the spring months (MAM) as given by coarse mode dominance. There is a shift towards weakly absorbing pollution (sulfate) and biomass (OC) aerosol dominance in the summer (JJA) and autumn (SON) months as given by a strong fine mode influence. A winter season (DJF) shift toward strongly fine mode, absorbing particles (BC and OC) is observed at Xianghe and Taihu. At Mukdahan, a strong fine mode influence is evident year round with weakly and strongly absorbing biomass particles dominant in the autumn and winter months, respectively, while particles exhibit variable absorption during the spring season. To address SQ2, four cases are selected in Asia to investigate how the optical properties of Asian aerosol plumes change during transport across the remote Pacific Ocean. In addition, six strong smoke events are selected to investigate how the physical and chemical properties of biomass smoke aerosols change during transport in North America. From four selected Asian cases, it was shown by DC-8 aircraft in situ measurements that the Asian plumes contained varying amounts of mineral dust and pollution aerosols during transport. In addition, backward trajectory analysis identified two main dust source regions (Gobi and Taklamakan deserts) and urban/industrial pollution regions in central and eastern China. During the anomalously active wildfire season of 2012 in North America, strong smoke events were observed over the Northern Great Plains region by the Grand Forks, North Dakota, AERONET site and selected as cases. The spectral dependences of absorption aerosol optical depth (AAOD) and o oabs illustrated the varying absorption of the smoke plumes due to carbonaceous particle influences. The AAOD parameter was found to be primarily influenced by aerosol particle size while ooabs was more sensitive to the carbonaceous content. The aerosols likely contain strongly absorbing carbonaceous particles generated from the flaming combustion mode. The cases represented complex mixtures of the flaming and smoldering combustion phases. Lastly, SQ3 is addressed by using a multi-platform dataset from the Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) Graciosa, Azores, 2009-2010 field campaign. The seasonal aerosol particle volume and number size distributions, AOD, and AEAOD during the CAP-MBL campaign have shown that a low overall mean AOD440 of 0.12 denoted a clean environment over this region that typically contains MBL sea salt. In terms of aerosol volume, a bimodal signal was prominent where the coarse mode influence (r ≥ 1 μm) dominated that of the fine mode (r < 1 μm) throughout the year. However, there are considerable continental fine mode aerosols advected to the Azores region during summer months, including Saharan mineral dust, volcanic ash, biomass smoke, and pollution from North American as identified by HYSPLIT backward trajectories. These aerosol types have been shown to have impacts on MBL cloud condensation nuclei (CCN) that are likely different from coarse mode marine aerosols (e.g., sea salt) (Remillard et al. 2014; Wood et al. 2014). The alternating presence of dominant clean air masses with periodic episodes of polluted air masses will provide a substantial variety in aerosol properties during the summer. This will provide a great opportunity to investigate the interactions between aerosol and cloud properties in terms of the aerosol indirect effect (AIE).

An integrated approach to identify the origin of PM10 exceedances.

PubMed

Amodio, M; Andriani, E; de Gennaro, G; Demarinis Loiotile, A; Di Gilio, A; Placentino, M C

2012-09-01

This study was aimed to the development of an integrated approach for the characterization of particulate matter (PM) pollution events in the South of Italy. PM(10) and PM(2.5) daily samples were collected from June to November 2008 at an urban background site located in Bari (Puglia Region, South of Italy). Meteorological data, particle size distributions and atmospheric dispersion conditions were also monitored in order to provide information concerning the different features of PM sources. The collected data allowed suggesting four indicators to characterize different PM(10) exceedances. PM(2.5)/PM(10) ratio, natural radioactivity, aerosol maps and back-trajectory analysis and particle distributions were considered in order to evaluate the contribution of local anthropogenic sources and to determine the different origins of intrusive air mass coming from long-range transport, such as African dust outbreaks and aerosol particles from Central and Eastern Europe. The obtained results were confirmed by applying principal component analysis to the number particle concentration dataset and by the chemical characterization of the samples (PM(10) and PM(2.5)). The integrated approach for PM study suggested in this paper can be useful to support the air quality managers for the development of cost-effective control strategies and the application of more suitable risk management approaches.

Po-Basin Atmospheric Composition during the Pegasos Field Campaign (summer 2012): Evaluation of ninfa/aodeM Simulation with In-Situ e Remote Sensing Observations

NASA Astrophysics Data System (ADS)

Landi, Tony C.; Bonafe, Giovanni; Stortini, Michele; Minguzzi, Enrico; Cristofanelli, Paolo; Marinoni, Angela; Giulianelli, Lara; Sandrini, Silvia; Gilardoni, Stefania; Rinaldi, Matteo; Ricciardelli, Isabella

2014-05-01

Within the EU project PEGASOS one of three field campaigns took place in the Po Valley during the summer of 2012. Photochemistry, particle formation, and particle properties related to diurnal evolution of the PBL were investigated through both in-situ and airborne measurements on board a Zeppelin NT air ship. In addition, 3-D air quality modeling systems were implemented over the Po valley for the summer 2012 to better characterize the atmospheric conditions, in terms of meteorological parameters and chemical composition. In this work, we present a comparison between atmospheric composition simulations carried out by the modeling system NINFA/AODEM with measurements performed during the PEGASOS field campaign for the period 13 June - 12 July 2012. NINFA (Stortini et al., 2007) is based on the chemical transport model CHIMERE (Bessagnet et al., 2008), driven by COSMO-I7, the meteorological Italian Limited Area Model, (Steppeler et al., 2003). Boundary conditions are provided by Prev'air data (www.prevair.org), and emission data input are based on regional, national and European inventory. Besides, a post-processing tool for aerosol optical properties calculation, called AODEM (Landi T. C. 2013) was implemented. Thus, predictions of Aerosol Optical Depth and aerosol extinction coefficient were also used for model comparison to vertical-resolved observations. For this experiment, NINFA/AODEM has been also evaluated by using measurements of size-segregated aerosol samples, number particles concentration and aerosol optical properties collected on hourly basis at the 3 different sampling sites representative of urban background (Bologna), rural background (San Pietro Capofiume) and remote high altitude station (Monte Cimone 2165 ma.s.l.). ). In addition, we focused on new particles formations events and long range transports from Northern Africa observed during the field campaign. References Bessagnet, Bertrand, Laurent Menut, Gabriele Curci, Alma Hodzic, Bruno Guillaume, Catherine Liousse, Sophie Moukhtar, Betty Pun, Christian Seigneur, and Michaël Schulz (2008). "Regional modeling of carbonaceous aerosols over europe-focus on secondary organic aerosols." Journal of Atmospheric Chemistry 61, no. 3 : 175-202. Landi Tony Christian (2013). AODEM: A post-processing tool for aerosol optical properties calculation in the Chemical Transport Models. Book published by LAP - Lambert Academic Publishing ISBN: 978-3-659-31802-3. Steppeler, J., G. Doms, U. Schättler, H. W. Bitzer, A. Gassmann, U. Damrath, and G. Gregoric (2003). "Meso-gamma scale forecasts using the nonhydrostatic model LM." Meteorology and Atmospheric Physics 82, no. 1-4 : 75-96. M. Stortini, M. Deserti, G. Bonafè, and E. Minguzzi. Long-term simulation and validation of ozone and aerosol in the Po Valley. In C.Borrego and E.Renner, editors, Developments in Environmental Sciences, volume 6, pages 768-770. Elsevier, 2007.

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cappa, Christopher D; Atkinson, Dean B

The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements ismore » facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?« less

The effect of organic aerosol material on aerosol reactivity towards ozone

NASA Astrophysics Data System (ADS)

Batenburg, Anneke; Gaston, Cassandra; Thornton, Joel; Virtanen, Annele

2015-04-01

After aerosol particles are formed or emitted into the atmosphere, heterogeneous reactions with gaseous oxidants cause them to 'age'. Aging can change aerosol properties, such as the hygroscopicity, which is an important parameter in how the particles scatter radiation and form clouds. Conversely, heterogeneous reactions on aerosol particles play a significant role in the cycles of various atmospheric trace gases. Organic compounds, a large part of the total global aerosol matter, can exist in liquid or amorphous (semi)solid physical phases. Different groups have shown that reactions with ozone (O3) can be limited by bulk diffusion in organic aerosol, particularly in viscous, (semi)solid materials, and that organic coatings alter the surface interactions between gas and aerosol particles. We aim to better understand and quantify how the viscosity and phase of organic aerosol matter affect gas-particle interactions. We have chosen the reaction of O3 with particles composed of a potassium iodide (KI) core and a variable organic coating as a model system. The reaction is studied in an aerosol flow reactor that consists of a laminar flow tube and a movable, axial injector for the injection of O3. The aerosol-containing air is inserted at the tube's top. The interaction length (and therefore time), between the particles and the O3 can be varied by moving the injector. Alternatively, the production of aerosol particles can be modulated. The remaining O3 concentration is monitored from the bottom of the tube and particle concentrations are measured simultaneously, which allows us to calculate the reactive uptake coefficient γ. We performed exploratory experiments with internally mixed KI and polyethylene glycol (PEG) particles at the University of Washington (UW) in a setup with a residence time around 50 s. Aerosol particles were generated in an atomizer from solutions with varying concentrations of KI and PEG and inserted into the flow tube after they were diluted and humidified and excess flow was ventilated. It proved necessary to separate the particles before the O3 monitor to prevent interference with the optical O3 detection method. Unfortunately, large O3 losses occurred on the used filter, which limited the accuracy of the γ-determinations. Nevertheless, it was found that already a small amount of added PEG considerably reduced the observed γ. Other aerosol separation methods are currently being investigated for the follow-up experiments in Kuopio.

Determination of respirable-sized crystalline silica in different ambient environments in the United Kingdom with a mobile high flow rate sampler utilising porous foams to achieve the required particle size selection

NASA Astrophysics Data System (ADS)

Stacey, Peter; Thorpe, Andrew; Roberts, Paul; Butler, Owen

2018-06-01

Inhalation of respirable crystalline silica (RCS) can cause diseases including silicosis and cancer. Levels of RCS close to an emission source are measured but little is known about the wider ambient exposure from industry emissions or natural sources. The aim of this work is to report the RCS concentrations obtained from a variety of ambient environments using a new mobile respirable (PM4) sampler. A mobile battery powered high flow rate (52 L min-1) sampler was developed and evaluated for particulate aerosol sampling employing foams to select the respirable particle size fraction. Sampling was conducted in the United Kingdom at site boundaries surrounding seven urban construction and demolition and five sand quarry sites. These are compared with data from twelve urban aerosol samples and from repeat measurements from a base line study at a single rural site. The 50% particle size penetration (d50) through the foam was 4.3 μm. Over 85% of predict bias values were with ±10% of the respirable convention, which is based on a log normal curve. Results for RCS from all construction and quarry activities are generally low with a 95 th percentile of 11 μg m-3. Eighty percent of results were less than the health benchmark value of 3 μg m-3 used in some states in America for ambient concentrations. The power cutting of brick and the largest demolition activities gave the highest construction levels. Measured urban background RCS levels were typically below 0.3 μg m-3 and the median RCS level, at a rural background location, was 0.02 μg m-3. These reported ambient RCS concentrations may provide useful baseline values to assess the wider impact of fugitive, RCS containing, dust emissions into the wider environment.

Two extreme types of mixing of dust with urban aerosols observed in Kosa particles: ‘After’ mixing and ‘on-the-way’ mixing

NASA Astrophysics Data System (ADS)

Suzuki, Issei; Igarashi, Yasuhito; Dokiya, Yukiko; Akagi, Tasuku

2010-02-01

Besides well-known episodic Kosa during spring, high concentrations of Ca 2+ in aerosols were observed early in summer as well as in the semi-continuous data of the aerosols at the summit of Mt. Fuji. We further analysed the data to study the chemical characteristics of the high calcium event during early summer. The back trajectory analyses of the event indicated that Ca was transported from arid and semi-arid regions (e.g. the Taklamakan desert) through the westerly-dominated troposphere higher than the height of the summit of Fuji. The amount of SO 42- was always equivalent to that of NH 4+ unlike the case of the normal Kosa period where SO 42- is in excess with respect to NH 4+. This shows the 'after' mixing of unreacted CaCO 3 of Kosa origin with (NH 4) 2SO 4, which was only realized by the downward injection of Kosa particles from higher altitudes to the air masses of different origin. In the case of normal Kosa, the air bearing Kosa particles passed through the polluted area to absorb unneutralized acids ('on-the-way' mixing), whereas in the case of the Kosa-like phenomena in summer, the acids from the polluted area have been neutralized by NH 4+ and become inactive before mixing with CaCO 3 ("after" mixing). We have simplified the chemistry of aerosols using their three major components, Ca 2+, SO 42- and NH 4+, and introduced a new triangle diagram with the three assumed end-members of CaCO 3, CaSO 4 and (NH 4) 2SO 4 to quantify the contribution of the 'after' mixing to the aerosols (AMI; 'after' mixing index). Based on the back trajectories of some high AMI cases, CaCO 3 in Kosa particles was transported through the middle troposphere (5000-7000 m) and descended to meet another air mass where SO 42- had been already neutralized by NH 3.

In Situ Aerosol Detector

NASA Technical Reports Server (NTRS)

Vakhtin, Andrei; Krasnoperov, Lev

2011-01-01

An affordable technology designed to facilitate extensive global atmospheric aerosol measurements has been developed. This lightweight instrument is compatible with newly developed platforms such as tethered balloons, blimps, kites, and even disposable instruments such as dropsondes. This technology is based on detection of light scattered by aerosol particles where an optical layout is used to enhance the performance of the laboratory prototype instrument, which allows detection of smaller aerosol particles and improves the accuracy of aerosol particle size measurement. It has been determined that using focused illumination geometry without any apertures is advantageous over using the originally proposed collimated beam/slit geometry (that is supposed to produce uniform illumination over the beam cross-section). The illumination source is used more efficiently, which allows detection of smaller aerosol particles. Second, the obtained integral scattered light intensity measured for the particle can be corrected for the beam intensity profile inhomogeneity based on the measured beam intensity profile and measured particle location. The particle location (coordinates) in the illuminated sample volume is determined based on the information contained in the image frame. The procedure considerably improves the accuracy of determination of the aerosol particle size.

Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A. D.; Decarlo, P. F.; Jimenez, J. L.; Dunlea, E. J.; Roberts, G. C.; Tomlinson, J. M.; Collins, D. R.; Howell, S. G.; Kapustin, V. N.; McNaughton, C. S.; Zhou, J.

2009-09-01

Remote sensing of cloud condensation nuclei (CCN) would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100 nm particles decreased with increasing organic fraction of non-refractory mass of submicron particles (OMF) as 0.34-0.20×OMF over Central Mexico and 0.47-0.43×OMF over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(-1/3), within measurement uncertainty (~20%). The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0-0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as -0.70×OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust). Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemical composition and CCN activity over Central Mexico.

Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A. D.; Decarlo, P. F.; Jimenez, J. L.; Dunlea, E. J.; Roberts, G. C.; Tomlinson, J. M.; Collins, D. R.; Howell, S. G.; Kapustin, V. N.; McNaughton, C. S.; Zhou, J.

2009-05-01

Remote sensing of cloud condensation nuclei (CCN) would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100-nm particles decreased with the organic fraction of non-refractory mass of submicron particles (OMF) as 10(-0.43-0.44*OMF) over Central Mexico and 10(-0.29-0.70*OMF) over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(-1/3), within measurement uncertainty (~20%). The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0-0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as -0.70*OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust). Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemistry and CCN activity over Central Mexico.

Spatial and seasonal patterns in urban influence on regional concentrations of speciated aerosols across the United States

NASA Astrophysics Data System (ADS)

Hand, J. L.; Schichtel, B. A.; Malm, W. C.; Pitchford, M.; Frank, N. H.

2014-11-01

Monthly, seasonal, and annual mean estimates of urban influence on regional concentrations of major aerosol species were computed using speciated aerosol data from the rural IMPROVE network (Interagency Monitoring of Protected Visual Environments) and the United States Environmental Protection Agency's urban Chemical Speciation Network for the 2008 through 2011 period. Aggregated for sites across the continental United States, the annual mean and one standard error in urban excess (defined as the ratio of urban to nearby rural concentrations) was highest for elemental carbon (3.3 ± 0.2), followed by ammonium nitrate (2.5 ± 0.2), particulate organic matter (1.78 ± 0.08), and ammonium sulfate (1.23 ± 0.03). The seasonal variability in urban excess was significant for carbonaceous aerosols and ammonium nitrate in the West, in contrast to the low seasonal variability in the urban influence of ammonium sulfate. Generally for all species, higher excess values in the West were associated with localized urban sources while in the East excess was more regional in extent. In addition, higher excess values in the western United States in winter were likely influenced not only by differences in sources but also by combined meteorological and topographic effects. This work has implications for understanding the spatial heterogeneity of major aerosol species near the interface of urban and rural regions and therefore for designing appropriate air quality management strategies. In addition, the spatial patterns in speciated mass concentrations provide constraints for regional and global models.

Comparison of mineral dust and droplet residuals measured with two single particle aerosol mass spectrometers

NASA Astrophysics Data System (ADS)

Wonaschütz, Anna; Ludwig, Wolfgang; Zawadowicz, Maria; Hiranuma, Naruki; Hitzenberger, Regina; Cziczo, Daniel; DeMott, Paul; Möhler, Ottmar

2017-04-01

Single Particle mass spectrometers are used to gain information on the chemical composition of individual aerosol particles, aerosol mixing state, and other valuable aerosol characteristics. During the Mass Spectrometry Intercomparison at the Fifth Ice Nucleation (FIN-01) Workshop, the new LAAPTOF single particle aerosol mass spectrometer (AeroMegt GmbH) was conducting simultaneous measurements together with the PALMS (Particle Analysis by Laser Mass Spectrometry) instrument. The aerosol particles were sampled from the AIDA chamber during ice cloud expansion experiments. Samples of mineral dust and ice droplet residuals were measured simultaneously. In this work, three expansion experiments are chosen for a comparison between the two mass spectrometers. A fuzzy clustering routine is used to group the spectra. Cluster centers describing the ensemble of particles are compared. First results show that while differences in the peak heights are likely due to the use of an amplifier in PALMS, cluster centers are comparable.

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

NASA Astrophysics Data System (ADS)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud formation, in the winter Arctic.

Separation and sampling of ice nucleation chamber generated ice particles by means of the counterflow virtual impactor technique for the characterization of ambient ice nuclei.

NASA Astrophysics Data System (ADS)

Schenk, Ludwig; Mertes, Stephan; Kästner, Udo; Schmidt, Susan; Schneider, Johannes; Frank, Fabian; Nillius, Björn; Worringen, Annette; Kandler, Konrad; Ebert, Martin; Stratmann, Frank

2014-05-01

In 2011, the German research foundation (DFG) research group called Ice Nuclei Research Unit (INUIT (FOR 1525, project STR 453/7-1) was established with the objective to achieve a better understanding concerning heterogeneous ice formation. The presented work is part of INUIT and aims for a better microphysical and chemical characterization of atmospheric aerosol particles that have the potential to act as ice nuclei (IN). For this purpose a counterflow virtual impactor (Kulkarni et al., 2011) system (IN-PCVI) was developed and characterized in order to separate and collect ice particles generated in the Fast Ice Nucleus Chamber (FINCH; Bundke et al., 2008) and to release their IN for further analysis. Here the IN-PCVI was used for the inertial separation of the IN counter produced ice particles from smaller drops and interstitial particles. This is realized by a counterflow that matches the FINCH output flow inside the IN-PCVI. The choice of these flows determines the aerodynamic cut-off diameter. The collected ice particles are transferred into the IN-PCVI sample flow where they are completely evaporated in a particle-free and dry carrier air. In this way, the aerosol particles detected as IN by the IN counter can be extracted and distributed to several particle sensors. This coupled setup FINCH, IN-PCVI and aerosol instrumentation was deployed during the INUIT-JFJ joint measurement field campaign at the research station Jungfraujoch (3580m asl). Downstream of the IN-PCVI, the Aircraft-based Laser Ablation Aerosol Mass Spectrometer (ALABAMA; Brands et al., 2011) was attached for the chemical analysis of the atmospheric IN. Also, number concentration and size distribution of IN were measured online (TROPOS) and IN impactor samples for electron microscopy (TU Darmstadt) were taken. Therefore the IN-PCVI was operated with different flow settings than known from literature (Kulkarni et al., 2011), which required a further characterisation of its cut-off-behaviour. Depending on the operation and thus freezing conditions inside FINCH (temperature/supersaturation), IN number concentrations between 1 and 200 per litre were detected by FINCH and a CPC mounted downstream of the IN-PCVI. The ALABAMA spectra of IN showed organic material from biomass burning and mineral dust particles mixed with organic material. The offline electron microscopy revealed that in average 80% of the IN consist of dust and metal oxides. 20 % are carbonaceous material, of which less than 5 % are soot. Bundke, U., Nillius, B., Jaenicke, R., Wetter, T., Klein, H., and Bingemer, H. (2008). The fast ice nucleus chamber finch. Atmospheric Research, 90:180-186. Brands, M., Kamphus, M., Böttger, T., Schneider, J., Drewnick, F., Roth, A., Curtius, J., Voigt, C., Borbon, A., Beekmann, M., Bourdon, A., Perrin, T. and Borrmann, S. (2011). Characterization of a newly developed aircraft-based laser ablation aerosol mass spectrometer (ALABAMA) and first field deployment in urban pollution plumes over Paris during MEGAPOLI 2009. Aerosol Sci. Technol., 45, 46-64. Kulkarni, G., Pekour, M., Afchine, A., Murphy, D. M., and Cziczo, D. J. (2011). Comparison of experimental and numerical studies of the performance characteristics of a pumped counterflow virtual impactor. Aerosol Science and Technology, 45(3):382-392.

Column Aerosol Optical Properties and Aerosol Radiative Forcing During a Serious Haze-Fog Month over North China Plain in 2013 Based on Ground-Based Sunphotometer Measurements

NASA Technical Reports Server (NTRS)

Che, H.; Xia, X.; Zhu, J.; Li, Z.; Dubovik, O.; Holben, Brent N.; Goloub, P.; Chen, H.; Estelles, V.; Cuevas-Agullo, E.

2014-01-01

In January 2013, North China Plain experienced several serious haze events. Cimel sunphotometer measurements at seven sites over rural, suburban and urban regions of North China Plain from 1 to 30 January 2013 were used to further our understanding of spatial-temporal variation of aerosol optical parameters and aerosol radiative forcing (ARF). It was found that Aerosol Optical Depth at 500 nm (AOD500nm) during non-pollution periods at all stations was lower than 0.30 and increased significantly to greater than 1.00 as pollution events developed. The Angstrom exponent (Alpha) was larger than 0.80 for all stations most of the time. AOD500nm averages increased from north to south during both polluted and non-polluted periods on the three urban sites in Beijing. The fine mode AOD during pollution periods is about a factor of 2.5 times larger than that during the non-pollution period at urban sites but a factor of 5.0 at suburban and rural sites. The fine mode fraction of AOD675nm was higher than 80% for all sites during January 2013. The absorption AOD675nm at rural sites was only about 0.01 during pollution periods, while 0.03-0.07 and 0.01-0.03 during pollution and non-pollution periods at other sites, respectively. Single scattering albedo varied between 0.87 and 0.95 during January 2013 over North China Plain. The size distribution showed an obvious tri-peak pattern during the most serious period. The fine mode effective radius in the pollution period was about 0.01-0.08 microns larger than during nonpollution periods, while the coarse mode radius in pollution periods was about 0.06-0.38 microns less than that during nonpollution periods. The total, fine and coarse mode particle volumes varied by about 0.06-0.34 cu microns, 0.03-0.23 cu microns, and 0.03-0.10 cu microns, respectively, throughout January 2013. During the most intense period (1-16 January), ARF at the surface exceeded -50W/sq m, -180W/sq m, and -200W/sq m at rural, suburban, and urban sites, respectively. The ARF readings at the top of the atmosphere were approximately -30W/sq m in rural and -40-60W/sq m in urban areas.

Effects of Airflow and Changing Humidity on the Aerosolization of Respirable Fungal Fragments and Conidia of Botrytis cinerea

PubMed Central

2012-01-01

The purpose of this study was to investigate the aerosolization of particles (micro- and macroconidia and fragments) from Botrytis cinerea cultures in relation to potential human inhalation in indoor environments. The influence of the following factors on the aerosolization of B. cinerea particles was studied: exposure to airflow, relative humidity (rh), changing rh, and plant or building materials. The aerodynamic diameter (da) and the respirable fraction of the aerosolized particles were determined. Conidia and fragments of B. cinerea were not aerosolized as a response to a decrease in the rh. In contrast, both micro- and macroconidia and fungal fragments were aerosolized when exposed to an airflow of 1.5 m s−1 or 0.5 m s−1. Significantly more particles of microconidial size and fragment size were aerosolized at a low rh (18 to 40% rh) than at a higher rh (60 to 80% rh) when cultures were exposed to airflow. The size of the respirable fraction of the aerosolized particles was dependent on the rh but not on the growth material. At high rh, about 30% of the aerosolized particles were of respirable size, while at low rh, about 70% were of respirable size. During low rh, more fungal (1→3)-β-d-glucan and chitinase were aerosolized than during high rh. In conclusion, exposure to external physical forces such as airflow is necessary for the aerosolization of particles from B. cinerea. The amount and size distribution are highly affected by the rh, and more particles of respirable sizes were aerosolized at low rh than at high rh. PMID:22447608

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

Particle Size Distribution of Serratia marcescens Aerosols Created During Common Laboratory Procedures and Simulated Laboratory Accidents

PubMed Central

Kenny, Michael T.; Sabel, Fred L.

1968-01-01

Andersen air samplers were used to determine the particle size distribution of Serratia marcescens aerosols created during several common laboratory procedures and simulated laboratory accidents. Over 1,600 viable particles per cubic foot of air sampled were aerosolized during blending operations. More than 98% of these particles were less than 5 μ in size. In contrast, 80% of the viable particles aerosolized by handling lyophilized cultures were larger than 5 μ. Harvesting infected eggs, sonic treatment, centrifugation, mixing cultures, and dropping infectious material produced aerosols composed primarily of particles in the 1.0- to 7.5-μ size range. Images Fig. 1 PMID:4877498

Simultaneous factor analysis of organic particle and gas mass spectra: AMS and PTR-MS measurements at an urban site

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Vlasenko, A.; McGuire, M.; Evans, G. J.; Abbatt, J. P. D.

2010-02-01

During the winter component of the SPORT (Seasonal Particle Observations in the Region of Toronto) field campaign, particulate non-refractory chemical composition and concentration of selected volatile organic compounds (VOCs) were measured by an Aerodyne time-of-flight aerosol mass spectrometer (AMS) and a proton transfer reaction-mass spectrometer (PTR-MS), respectively. Sampling was performed in downtown Toronto ~15 m from a major road. The mass spectra from the AMS and PTR-MS were combined into a unified dataset, which was analysed using positive matrix factorization (PMF). The two instruments were given balanced weight in the PMF analysis by the application of a scaling factor to the uncertainties of each instrument. A residual based metric, Δesc, was used to evaluate the instrument relative weight within each solution. The PMF analysis yielded a 6-factor solution that included factors characteristic of regional transport, local traffic emissions, charbroiling and oxidative processing. The unified dataset provides information on emission sources (particle and VOC) and atmospheric processing that cannot be obtained from the datasets of the individual instruments: (1) apportionment of oxygenated VOCs to either direct emission sources or secondary reaction products; (2) improved correlation of oxygenated aerosol factors with photochemical age; and (3) increased detail regarding the composition of oxygenated organic aerosol factors. This analysis represents the first application of PMF to a unified AMS/PTR-MS dataset.

Quantifying VOC-Reaction Tracers, Ozone Production, and Continuing Aerosol Production Rates in Urban and Far-Downwind Atmospheres

NASA Technical Reports Server (NTRS)

Chatfield, Robert; Ren, X.; Brune, W.; Fried, A.; Schwab, J.

2008-01-01

We have found a surprisingly informative decomposition of the complex question of smoggy ozone production (basically, [HO2] in a more locally determined field of [NO]) in the process of linked investigations of modestly smoggy Eastern North America (by NASA aircraft, July 2004) and rather polluted Flushing, NYC (Queens College, July, 2001). In both rural and very polluted situations, we find that a simple contour graph parameterization of the local principal ozone production rate can be estimated using only the variables [NO] and j(sub rads) [HCHO]: Po(O3) = c (j(sub rads) [HCHO])(sup a) [HCHO](sup b). Here j(sub rads) is the photolysis of HCHO to radicals, presumably capturing many harder-UV photolytic processes and the principle ozone production is that due to HO2; mechanisms suggest that ozone production due to RO2 is closely correlated, often suggesting a limited range of different proportionality factors. The method immediately suggests a local interpretation for concepts of VOC limitation and NOx limitation. We believe that the product j(sub rads) [HCHO] guages the oxidation rate of observed VOC mixtures in a way that also provides [HO2] useful for the principle ozone production rate k [HO2] [NO], and indeed, all ozone chemical production. The success of the method suggests that dominant urban primary-HCHO sources may transition to secondary plume-HCHO sources in a convenient way. Are there other, simple, near-terminal oxidized VOC's which help guage ozone production and aerosol particle formation? Regarding particles, we report on, to the extent NASA Research resources allow, on appealing relationships between far-downwind (Atlantic PBL) HCHO and very fine aerosol (including sulfate. Since j(sub rads) [HCHO] provides a time-scale, we may understand distant-plume particle production in a more quantitative manner. Additionally we report on a statistical search in the nearer field for relationships between glyoxals (important near-terminal aromatic and isoprene reaction products) and aerosol production, looking for VOC's that might be most implicated. All three variables j(sub rads), [HCHO], and [NO] are relatively easily measured in widespread air pollution monitoring networks, and all are deducible form space-borne observations, though estimation of [NO] from [NO2] (the species observable from space) may require care. We report also on airborne and surface observations of HCHO, suggesting that concentrated (urban) and more diffuse (forest) sources may be distinguishable from space. The use of the 3.58 micron microwindow for HCHO remote sensing should allow much sharper resolution of HCHO than the UV. UV sensing requires large and expensive instruments, but even these seem justified since formaldehyde is so informative.

The effectiveness of an air cleaner in controlling droplet/aerosol particle dispersion emitted from a patient's mouth in the indoor environment of dental clinics.

PubMed

Chen, Chun; Zhao, Bin; Cui, Weilin; Dong, Lei; An, Na; Ouyang, Xiangying

2010-07-06

Dental healthcare workers (DHCWs) are at high risk of occupational exposure to droplets and aerosol particles emitted from patients' mouths during treatment. We evaluated the effectiveness of an air cleaner in reducing droplet and aerosol contamination by positioning the device in four different locations in an actual dental clinic. We applied computational fluid dynamics (CFD) methods to solve the governing equations of airflow, energy and dispersion of different-sized airborne droplets/aerosol particles. In a dental clinic, we measured the supply air velocity and temperature of the ventilation system, the airflow rate and the particle removal efficiency of the air cleaner to determine the boundary conditions for the CFD simulations. Our results indicate that use of an air cleaner in a dental clinic may be an effective method for reducing DHCWs' exposure to airborne droplets and aerosol particles. Further, we found that the probability of droplet/aerosol particle removal and the direction of airflow from the cleaner are both important control measures for droplet and aerosol contamination in a dental clinic. Thus, the distance between the air cleaner and droplet/aerosol particle source as well as the relative location of the air cleaner to both the source and the DHCW are important considerations for reducing DHCWs' exposure to droplets/aerosol particles emitted from the patient's mouth during treatments.