40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size...

Code of Federal Regulations, 2011 CFR

2011-07-01

... 40 Protection of Environment 5 2011-07-01 2011-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass...

40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size...

Code of Federal Regulations, 2010 CFR

2010-07-01

... 40 Protection of Environment 5 2010-07-01 2010-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass...

Evolution of size-segregated aerosol mass concentration during the Antarctic summer at Northern Foothills, Victoria Land

NASA Astrophysics Data System (ADS)

Illuminati, Silvia; Bau, Sébastien; Annibaldi, Anna; Mantini, Caterina; Libani, Giulia; Truzzi, Cristina; Scarponi, Giuseppe

2016-01-01

Within the framework of the Italian National Programm for Antarctic Research (PNRA), the first direct gravimetric measurements of size-segregated aerosol fractions were carried out at Faraglione Camp, ˜3-km far from the Italian station "M. Zucchelli" (Terra Nova Bay, Ross Sea), during the 2014-2015 austral summer. A six-stage high-volume cascade impactor with size classes between 10 μm and 0.49 μm, and, in parallel, for comparison purposes, a PM10 high-volume sampler (50% cut-off aerodynamic diameter of 10 μm) were used. A 10-day sampling strategy was adopted. Aerosol mass measurements were carried out before and after exposure by using a microbalance specifically designed for the filter weight and placed inside a glove bag in order to maintain stable temperature and humidity conditions during weighing sessions. Measured atmospheric concentrations (referred to the "actual air conditions" of mean temperature of 268 K and mean pressure of 975 hPa) of size-segregated aerosol fractions showed the following values, given as size range, means (interquartile range): Dp < 0.49 μm, 0.33 (0.26-0.34) μg m-3; 0.49-0.95 μm, 0.20 (0.19-0.24) μg m-3; 0.95-1.5 μm, 0.16 (0.13-0.21) μg m-3; 1.5-3.0 μm 0.075 (0.05-0.11) μg m-3; 3.0-7.2 μm 0.12 (0.02-0.19) μg m-3; 7.2-10 μm 0.06 (0.01-0.03) μg m-3. The average mass concentration of the total PM10 at Faraglione Camp for the entire sampling period was 0.92 (0.67-1.1) μg m-3. Although a great variability, the aerosol mass concentration showed a tri-modal distribution, with an accumulation mode (in the range 0.1-1.0 μm) and two coarse modes (CM1 in the range 1.0-3.0 μm, and CM2 in the range 3.0-10 μm). From 50% to 90% of the PM10 mass comes from particles of a size smaller than 1.0 μm. The two coarse modes represented from ˜5% to ˜35% of the PM10, showing opposite seasonal trends (CM1 decreased while CM2 increased). During summer, PM10 mass concentration increased to a maximum of ˜1.6 μg m-3 at mid-December, while

Process evaluation of sea salt aerosol concentrations at remote marine locations

NASA Astrophysics Data System (ADS)

Struthers, H.; Ekman, A. M.; Nilsson, E. D.

2011-12-01

Sea salt, an important natural aerosol, is generated by bubbles bursting at the surface of the ocean. Sea salt aerosol contributes significantly to the global aerosol burden and radiative budget and are a significant source of cloud condensation nuclei in remote marine areas (Monahan et al., 1986). Consequently, changes in marine aerosol abundance is expected to impact on climate forcing. Estimates of the atmospheric burden of sea salt aerosol mass derived from chemical transport and global climate models vary greatly both in the global total and the spatial distribution (Texor et al. 2006). This large uncertainty in the sea salt aerosol distribution in turn contributes to the large uncertainty in the current estimates of anthropogenic aerosol climate forcing (IPCC, 2007). To correctly attribute anthropogenic climate change and to veraciously project future climate, natural aerosols including sea salt must be understood and accurately modelled. In addition, the physical processes that determine the sea salt aerosol concentration are susceptible to modification due to climate change (Carslaw et al., 2010) which means there is the potential for feedbacks within the climate/aerosol system. Given the large uncertainties in sea salt aerosol modelling, there is an urgent need to evaluate the process description of sea salt aerosols in global models. An extremely valuable source of data for model evaluation is the long term measurements of PM10 sea salt aerosol mass available from a number of remote marine observation sites around the globe (including the GAW network). Sea salt aerosol concentrations at remote marine locations depend strongly on the surface exchange (emission and deposition) as well as entrainment or detrainment to the free troposphere. This suggests that the key parameters to consider in any analysis include the sea surface water temperature, wind speed, precipitation rate and the atmospheric stability. In this study, the sea salt aerosol observations

The Potential of The Synergy of Sunphotometer and Lidar Data to Validate Vertical Profiles of The Aerosol Mass Concentration Estimated by An Air Quality Model

NASA Astrophysics Data System (ADS)

Siomos, N.; Filioglou, M.; Poupkou, A.; Liora, N.; Dimopoulos, S.; Melas, D.; Chaikovsky, A.; Balis, D. S.

2016-06-01

Vertical profiles of the aerosol mass concentration derived by the Lidar/Radiometer Inversion Code (LIRIC), that uses combined sunphotometer and lidar data, were used in order to validate the aerosol mass concentration profiles estimated by the air quality model CAMx. Lidar and CIMEL measurements performed at the Laboratory of Atmospheric Physics of the Aristotle University of Thessaloniki, Greece (40.5N, 22.9E) from the period 2013-2014 were used in this study.

Physicochemical Characterization of Capstone Depleted Uranium Aerosols I: Uranium Concentration in Aerosols as a Function of Time and Particle Size

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

Parkhurst, MaryAnn; Cheng, Yung-Sung; Kenoyer, Judson L.

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols weremore » evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time particularly within the first minute after the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.« less

Changes in ground-level PM mass concentration and column aerosol optical depth over East Asia during 2004-2014

NASA Astrophysics Data System (ADS)

Nam, J.; Kim, S. W.; Park, R.; Yoon, S. C.; Sugimoto, N.; Park, J. S.; Hong, J.

2015-12-01

Multi-year records of moderate resolution imaging spectroradiometer (MODIS), ground-level particulate matter (PM) mass concentration, cloud-aerosol lidar with orthogonal polarization (CALIOP), and ground-level lidar were analyzed to investigate seasonal and annual changes of aerosol optical depth (AOD) and PM mass concentration over East Asia. Least mean square fit method is applied to detect the trends and their magnitudes for each selected regions and stations. Eleven-year MODIS measurements show generally increasing trends in both AOD (1.18 % yr-1) and Ångström exponent (0.98 % yr-1), especially over the east coastal industrialized region in China. Monthly variation of AOD show maximum value at April-July, which were related to the progress of summer monsoon rain band and stationary continental air mass on the northeast of Asia. Increasing trends of AOD were found for eight cites in China (0.80 % yr-1) and Seoul site, Korea (0.40 % yr-1), whereas no significant change were shown in Gosan background site (0.04 % yr-1) and decreasing trend at five background sites in Japan (-0.42 % yr-1). Contrasting to AOD trend, all fifteen sites in China (-1.28 % yr-1), Korea (-2.77 % yr-1), and Japan (-2.03 % yr-1) showed decreasing trend of PM10 mass concentration. Also, PM2.5 mass concentration at Beijing, Seoul, Rishiri, and Oki show significant decreasing trend of -1.16 % yr-1. To further discuss the opposite trend of surface PM mass concentration and column AOD, we investigate vertical aerosol profile from lidar measurements. AOD estimated for planetary boundary layer (surface~1.5 km altitude; AODPBL) from CALIOP measurements over East China show decreasing trend of -1.71 % yr-1 over the period of 2007-2014, wherever AOD estimated for free troposphere (1.5 km~5 km altitude; AODFT) show increasing trend of 2.92 % yr-1. In addition, ground-level lidar measurements in Seoul show decreasing AODPBL trend of -2.57 % yr-1, whereas, AODFT show no significant change (-0.44 % yr

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.

Photochemical aging of aerosol particles in different air masses arriving at Baengnyeong Island, Korea

NASA Astrophysics Data System (ADS)

Kang, Eunha; Lee, Meehye; Brune, William H.; Lee, Taehyoung; Park, Taehyun; Ahn, Joonyoung; Shang, Xiaona

2018-05-01

Atmospheric aerosol particles are a serious health risk, especially in regions like East Asia. We investigated the photochemical aging of ambient aerosols using a potential aerosol mass (PAM) reactor at Baengnyeong Island in the Yellow Sea during 4-12 August 2011. The size distributions and chemical compositions of aerosol particles were measured alternately every 6 min from the ambient air or through the highly oxidizing environment of a potential aerosol mass (PAM) reactor. Particle size and chemical composition were measured by using the combination of a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Inside the PAM reactor, O3 and OH levels were equivalent to 4.6 days of integrated OH exposure at typical atmospheric conditions. Two types of air masses were distinguished on the basis of the chemical composition and the degree of aging: air transported from China, which was more aged with a higher sulfate concentration and O : C ratio, and the air transported across the Korean Peninsula, which was less aged with more organics than sulfate and a lower O : C ratio. For both episodes, the particulate sulfate mass concentration increased in the 200-400 nm size range when sampled through the PAM reactor. A decrease in organics was responsible for the loss of mass concentration in 100-200 nm particles when sampled through the PAM reactor for the organics-dominated episode. This loss was especially evident for the m/z 43 component, which represents less oxidized organics. The m/z 44 component, which represents further oxidized organics, increased with a shift toward larger sizes for both episodes. It is not possible to quantify the maximum possible organic mass concentration for either episode because only one OH exposure of 4.6 days was used, but it is clear that SO2 was a primary precursor of secondary aerosol in northeast Asia, especially during long-range transport from China. In addition

Estimation of atmospheric columnar organic matter (OM) mass concentration from remote sensing measurements of aerosol spectral refractive indices

NASA Astrophysics Data System (ADS)

Zhang, Ying; Li, Zhengqiang; Sun, Yele; Lv, Yang; Xie, Yisong

2018-04-01

Aerosols have adverse effects on human health and air quality, changing Earth's energy balance and lead to climate change. The components of aerosol are important because of the different spectral characteristics. Based on the low hygroscopic and high scattering properties of organic matter (OM) in fine modal atmospheric aerosols, we develop an inversion algorithm using remote sensing to obtain aerosol components including black carbon (BC), organic matter (OM), ammonium nitrate-like (AN), dust-like (DU) components and aerosol water content (AW). In the algorithm, the microphysical characteristics (i.e. volume distribution and complex refractive index) of particulates are preliminarily separated to fine and coarse modes, and then aerosol components are retrieved using bimodal parameters. We execute the algorithm using remote sensing measurements of sun-sky radiometer at AERONET site (Beijing RADI) in a period from October of 2014 to January of 2015. The results show a reasonable distribution of aerosol components and a good fit for spectral feature calculations. The mean OM mass concentration in atmospheric column is account for 14.93% of the total and 56.34% of dry and fine-mode aerosol, being a fairly good correlation (R = 0.56) with the in situ observations near the surface layer.

Long-Term Observations on Aerosol Elemental Carbon and Mass Concentrations in Winter-Time in New Delhi: Implications for Local Source Changes

NASA Astrophysics Data System (ADS)

Aggarwal, S. G.; Singh, K.; Singh, N.; Gupta, P. K.

2009-12-01

Fossil-fuel and bio-fuel burning are the two major sources identified for high carbonaceous aerosol loadings in several mega cities in India. In the last decade, according to a report from the Central Pollution Control Board (CPCB, 1999), the vehicular emission (mostly diesel-powered engines) was contributed to ~67% of the total air pollution load in New Delhi. Therefore, a policy decision was taken by the government, and most of the diesel-powered engines were converted to compressed natural gas (CNG) -powered engines by 2003. To better understand the effect of these changes on air quality, we collected high volume aerosol samples (total suspended particles, TSP) mostly for a day basis at our institute building in New Delhi almost everyday during winter season (November to January) from 2002 to 2008. We found very high mean aerosol loading, i.e., 488±47 μg m-3 in 2002 winter, which dropped significantly to 280±73 μg m-3 in 2003 winter. Thereafter, a steadily increased trend of aerosol mass loadings was observed, i.e., 339±112, 339±120, 412±107 and 444±55 μg m-3 in 2004, 2005, 2006 and 2007 winters, respectively. Similar trend was also observed for elemental carbon (EC) concentration in TSP, which was peaked in 2002 (47±11 μg m-3) and minimized in 2003 (32±6 μg m-3), and then gradually increased to 41±8 μg m-3 in 2007 winter. These decline trends of aerosol mass and EC concentrations in 2003 can be explained well, because of the conversion of diesel engine to CNG engines of public transport facilities. However, again increase in aerosol mass and EC concentrations possibly because of a high increase in road traffic in recent years. According to the economic survey of New Delhi 2008-09, the number of vehicles (which includes all types of engines, i.e., petrol, diesel and CNG) has grown from ~3.3 millions in 1997-98 to ~5.6 millions in 2007-08. The influence of engine types and vehicle population on aerosol loading can also be explained well by SO2 and

Background aerosol over the Himalayas and Tibetan Plateau: observed characteristics of aerosol mass loading

NASA Astrophysics Data System (ADS)

Liu, Bin; Cong, Zhiyuan; Wang, Yuesi; Xin, Jinyuan; Wan, Xin; Pan, Yuepeng; Liu, Zirui; Wang, Yonghong; Zhang, Guoshuai; Wang, Zhongyan; Wang, Yongjie; Kang, Shichang

2017-01-01

To investigate the atmospheric aerosols of the Himalayas and Tibetan Plateau (HTP), an observation network was established within the region's various ecosystems, including at the Ngari, Qomolangma (QOMS), Nam Co, and Southeastern Tibetan (SET) stations. In this paper we illustrate aerosol mass loadings by integrating in situ measurements with satellite and ground-based remote sensing datasets for the 2011-2013 period, on both local and large scales. Mass concentrations of these surface atmospheric aerosols were relatively low and varied with land cover, showing a general tendency of Ngari and QOMS (barren sites) > Nam Co (grassland site) > SET (forest site). Daily averages of online PM2.5 (particulates with aerodynamic diameters below 2.5 µm) at these sites were sequentially 18.2 ± 8.9, 14.5 ± 7.4, 11.9 ± 4.9 and 11.7 ± 4.7 µg m-3. Correspondingly, the ratios of PM2.5 to total suspended particles (TSP) were 27.4 ± 6.65, 22.3 ± 10.9, 37.3 ± 11.1 and 54.4 ± 6.72 %. Bimodal mass distributions of size-segregated particles were found at all sites, with a relatively small peak in accumulation mode and a more notable peak in coarse mode. Diurnal variations in fine-aerosol masses generally displayed a bi-peak pattern at the QOMS, Nam Co and SET stations and a single-peak pattern at the Ngari station, controlled by the effects of local geomorphology, mountain-valley breeze circulation and aerosol emissions. Dust aerosol content in PM2.1 samples gave fractions of 26 % at the Ngari station and 29 % at the QOMS station, or ˜ 2-3 times that of reported results at human-influenced sites. Furthermore, observed evidence confirmed the existence of the aerodynamic conditions necessary for the uplift of fine particles from a barren land surface. Combining surface aerosol data and atmospheric-column aerosol optical properties, the TSP mass and aerosol optical depth (AOD) of the Multi-angle Imaging Spectroradiometer (MISR) generally decreased as land cover changed from

A new method for assessing the contribution of Primary Biological Atmospheric Particles to the mass concentration of the atmospheric aerosol.

PubMed

Perrino, Cinzia; Marcovecchio, Francesca

2016-02-01

Primary Biologic Atmospheric Particles (PBAPs) constitute an interesting and poorly investigated component of the atmospheric aerosol. We have developed and validated a method for evaluating the contribution of overall PBAPs to the mass concentration of atmospheric particulate matter (PM). The method is based on PM sampling on polycarbonate filters, staining of the collected particles with propidium iodide, observation at epifluorescence microscope and calculation of the bioaerosol mass using a digital image analysis software. The method has been also adapted to the observation and quantification of size-segregated aerosol samples collected by multi-stage impactors. Each step of the procedure has been individually validated. The relative repeatability of the method, calculated on 10 pairs of atmospheric PM samples collected side-by-side, was 16%. The method has been applied to real atmospheric samples collected in the vicinity of Rome, Italy. Size distribution measurements revealed that PBAPs was mainly in the coarse fraction of PM, with maxima in the range 5.6-10 μm. 24-h samples collected during different period of the year have shown that the concentration of bioaerosol was in the range 0.18-5.3 μg m(-3) (N=20), with a contribution to the organic matter in PM10 in the range 0.5-31% and to the total mass concentration of PM10 in the range 0.3-18%. The possibility to determine the concentration of total PBAPs in PM opens up interesting perspectives in terms of studying the health effects of these components and of increasing our knowledge about the composition of the organic fraction of the atmospheric aerosol. Copyright © 2015 Elsevier Ltd. All rights reserved.

Relating Aerosol Mass and Optical Depth in the Summertime Continental Boundary Layer

NASA Astrophysics Data System (ADS)

Brock, C. A.; Wagner, N.; Middlebrook, A. M.; Attwood, A. R.; Washenfelder, R. A.; Brown, S. S.; McComiskey, A. C.; Gordon, T. D.; Welti, A.; Carlton, A. G.; Murphy, D. M.

2014-12-01

Aerosol optical depth (AOD), the column-integrated ambient aerosol light extinction, is determined from satellite and ground-based remote sensing measurements. AOD is the parameter most often used to validate earth system model simulations of aerosol mass. Relating aerosol mass to AOD, however, is problematic due to issues including aerosol water uptake as a function of relative humidity (RH) and the complicated relationship between aerosol physicochemical properties and light extinction. Measurements of aerosol microphysical, chemical, and optical properties help to constrain the relationship between aerosol mass and optical depth because aerosol extinction at ambient RH is a function of the abundance, composition and size distribution of the aerosol. We use vertical profiles of humidity and dry aerosol extinction observed in the southeastern United States (U.S.) to examine the relationship between submicron aerosol mass concentration and extinction at ambient RH. We show that the κ-Köhler parameterization directly, and without additional Mie calculations, describes the change in extinction with varying RH as a function of composition for both aged aerosols typical of the polluted summertime continental boundary layer and the biomass burning aerosols we encountered. We calculate how AOD and the direct radiative effect in the eastern U.S. have likely changed due to trends in aerosol composition in recent decades. We also examine the sensitivity of AOD to the RH profile and to aerosol composition, size distribution and abundance.

Vertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events

NASA Astrophysics Data System (ADS)

Mamali, Dimitra; Marinou, Eleni; Sciare, Jean; Pikridas, Michael; Kokkalis, Panagiotis; Kottas, Michael; Binietoglou, Ioannis; Tsekeri, Alexandra; Keleshis, Christos; Engelmann, Ronny; Baars, Holger; Ansmann, Albert; Amiridis, Vassilis; Russchenberg, Herman; Biskos, George

2018-05-01

In situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 µm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.

The link between organic aerosol mass loading and degree of oxygenation: an α-pinene photooxidation study

NASA Astrophysics Data System (ADS)

Pfaffenberger, L.; Barmet, P.; Slowik, J. G.; Praplan, A. P.; Dommen, J.; Prévôt, A. S. H.; Baltensperger, U.

2013-07-01

A series of smog chamber (SC) experiments was conducted to identify factors responsible for the discrepancy between ambient and SC aerosol degree of oxygenation. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer is used to compare mass spectra from α-pinene photooxidation with ambient aerosol. Composition is compared in terms of the fraction of particulate CO2+, a surrogate for carboxylic acids, vs. the fraction of C2H3O+, a surrogate for aldehydes, alcohols and ketones, as well as in the Van Krevelen space, where the evolution of the atomic hydrogen-to-carbon ratio (H : C) vs. the atomic oxygen-to-carbon ratio (O : C) is investigated. Low (near-ambient) organic mass concentrations were found to be necessary to obtain oxygenation levels similar to those of low-volatility oxygenated organic aerosol (LV-OOA) commonly identified in ambient measurements. The effects of organic mass loading and OH (hydroxyl radical) exposure were decoupled by inter-experiment comparisons at the same integrated OH concentration. An OH exposure between 3 and 25 × 107 cm-3 h is needed to increase O : C by 0.05 during aerosol aging. For the first time, LV-OOA-like aerosol from the abundant biogenic precursor α-pinene was produced in a smog chamber by oxidation at typical atmospheric OH concentrations. Significant correlation between measured secondary organic aerosol (SOA) and reference LV-OOA mass spectra is shown by Pearson's R2 values larger than 0.90 for experiments with low organic mass concentrations between 1.2 and 18 μg m-3 at an OH exposure of 4 × 107 cm-3 h, corresponding to about two days of oxidation time in the atmosphere, based on a global mean OH concentration of ~ 1 × 106 cm-3. α-Pinene SOA is more oxygenated at low organic mass loadings. Because the degree of oxygenation influences the chemical, volatility and hygroscopic properties of ambient aerosol, smog chamber studies must be performed at near-ambient concentrations to accurately simulate

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.; Kourtchev, I.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2013-05-01

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 ca. 1 350 000 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 characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS) and was also found to comprise organic aerosol as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and 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 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA) comprised 18%, "biomass 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%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal 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 aerosol mass and non-refractory total PM1, respectively).

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.

PM 2.5 mass concentrations in comparison with aerosol optical depths over the Arabian Sea and Indian Ocean during winter monsoon

NASA Astrophysics Data System (ADS)

Ramachandran, S.

An analysis of PM 2.5 mass concentrations and 0.5 μm aerosol optical depths (AODs) during the Northeast winter monsoon seasons of 1996-2000 is performed and intercompared. AODs are found to show diurnal variations over Coastal India (CI) (west coast) while they are relatively smooth over the Arabian Sea (AS) (5-20°N) and tropical Indian Ocean (TIO) (5°N-20°S). PM 2.5, PM 10 and total mass concentrations show less variations in a day over these oceanic regions. Columnar AODs are found to increase with an increase in the marine boundary layer aerosol concentrations over CI and AS while an opposite trend is seen over TIO. The yearly-mean AODs and mass concentrations are found to increase over CI and AS, over TIO the mass concentrations increased while the AODs decreased during 1996-2000. It is found from the 7-days air back trajectory analyses that at different altitudes air masses can originate from different source regions leading to changes in chemical, physical and optical characteristics of the aerosol between the surface and column. The differences in the surface and columnar measurements could also occur due to changes in the meteorological conditions, wind patterns, in addition to changes in production and subsequently the transport of aerosols. Least-squares fits to the above intercomparison resulted in intercepts of 0.24 and 0.22 over CI and AS indicating that the background AODs over these oceanic regions are higher. An examination of the daily-mean wind speeds and PM 2.5 mass concentrations yielded an index of wind dependence of 0.04 for AS and 0.07 for TIO. The background PM 2.5 mass concentrations are also found to be high at 36 and 25 μg m -3 over AS and TIO, respectively, indicating a stronger influence from the continent. Frequency distribution figures show that 28% of the PM 2.5 values over CI lie in the 60-80 μg m -3 range. Over AS the dominant mode of distribution is 40-60 μg m -3 with a peak value of 42%. Over TIO PM 2.5 values are found to

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 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

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

DOE PAGES

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-03-02

We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles 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 bymore » 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

Source contributions to black carbon mass fractions in aerosol particles over the northwestern Pacific

NASA Astrophysics Data System (ADS)

Koga, Seizi; Maeda, Takahisa; Kaneyasu, Naoki

Aerosol particle number size distributions above 0.3 μm in diameter and black carbon mass concentrations in aerosols were observed on Chichi-jima of the Ogasawara Islands in the northwestern Pacific from January 2000 to December 2002. Chichi-jima is suitable to observe polluted air masses from East Asia in winter and clean air masses over the western North Pacific in summer. In winter, aerosols over Chichi-jima were strongly affected by anthropogenic emissions in East Asia. The form of energy consumption in East Asia varies in various regions. Hence, each source region is expected to be characterized by an individual black carbon mass fraction. A three-dimensional Eulerian transport model was used to estimate contribution rates to air pollutants from each source region in East Asia. Because the Miyake-jima eruption began at the end of June 2000, the influence of smokes from Miyake-jima was also considered in the model calculation. The results of model calculations represent what must be noticed about smokes from volcanoes including Miyake-jima to interpret temporal variations of sulfur compounds over the northwestern Pacific. To evaluate black carbon mass fractions in anthropogenic aerosols as a function of source region, the relationships between the volume concentration of aerosol particles and the black carbon mass concentration in the winter were classified under each source region in East Asia. Consequently, the black carbon mass fractions in aerosols from China, Japan and the Korean Peninsula, and other regions were estimated to be 9-13%, 5-7%, and 4-5%, respectively.

In Situ Measurements of Aerosol Mass Concentration and Spectral Absorption at Three Location in and Around Mexico City

NASA Astrophysics Data System (ADS)

Chaudhry, Z.; Martins, V.; Li, Z.

2006-12-01

As a result of population growth and increasing industrialization, air pollution in heavily populated urban areas is one of the central environmental problems of the century. As a part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) study, Nuclepore filters were collected in two size ranges (PM10 and PM2.5) at 12 hour intervals at three location in Mexico during March, 2006. Sampling stations were located at the Instituto Mexicano del Petroleo (T0), at the Rancho La Bisnago in the State of Hidalgo (T2) and along the Gulf Coast in Tampico (Tam). Each filter was analyzed for mass concentration, aerosol scattering and absorption efficiencies. Mass concentrations at T0 ranged from 47 to 179 μg/m3 for PM10 with an average concentration of 96 μg/m3, and from 20 to 93 μg/m3 for PM2.5 with an average concentration of 41 μg/m3. Mass concentrations at T2 ranged from 12 to 154 μg/m3 for PM10 with an average concentration of 51 μg/m3, and from 7 to 50 μg/m3 for PM2.5 with an average concentration of 25 μg/m3. Mass concentrations at Tam ranged from 34 to 80 μg/m3 for PM10 with an average concentration of 52 μg/m3, and from 8 to 23 μg/m3 for PM2.5 with an average concentration of 13 μg/m3. While some of the extreme values are likely linked to local emissions, regional air pollution episodes also played important roles. Each of the sampling stations experienced a unique atmospheric condition. The site at T0 was influenced by urban air pollution and dust storms, the site at T2 was significantly less affected by air pollution but more affected by regional dust storms and local dust devils while Tam was influenced by air pollution, dust storms and the natural marine environment. The spectral mass absorption efficiency was measured from 350 to 2500 nm and shows large differences between the absorption properties of soil dust, black carbon, and organic aerosols. The strong spectral differences observed can be related to differences in

Latitudinal distribution of aerosol black carbon and its mass fraction to composite aerosols over peninsular India during winter season

NASA Astrophysics Data System (ADS)

Moorthy, K. Krishna; Babu, S. Suresh; Badarinath, K. V. S.; Sunilkumar, S. V.; Kiranchand, T. R.; Ahmed, Y. Nazeer

2007-04-01

During a land campaign to characterise the spatial distribution of aerosols over peninsular India during the winter season, extensive, collocated, and spatially resolved measurements of mass concentration of the composite aerosols (MT) as well as that (MB) of aerosol Black Carbon (BC) were made over different environments (coastal, industrial, urban, village, remote, semiarid) of the western peninsular India. High concentrations of BC, >2.5 μg m-3, were observed along the west coast, from ~8°N up to 14.5°N, and moderate values (1.0 to 2.5 μg m-3) over inland regions from 15 to 18°N. Latitudinally, BC concentration decreased from south to north, @~160 ng m-3 for every degree increase in latitude. The spatial pattern of BC mass fraction differed from that of MB, with regions of high (8 to 16%) ratios spreading more interior, implying higher fractional load of BC at locations where the BC concentrations remain lower.

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).

A Water Mass Tracer Detected in Aerosols Demonstrates Ocean-Atmosphere Mass Transfer and Links Sea Spray Aerosol to Source Waters

NASA Astrophysics Data System (ADS)

Pendergraft, M.; Grimes, D. J.; Giddings, S. N.; Feddersen, F.; Prather, K. A.; Santander, M.; Lee, C.; Beall, C.

2016-12-01

During September and October of 2015 the Cross Surfzone/Inner-shelf Dye Exchange (CSIDE) project released rhodamine WT dye to study nearshore water movement and exchange offshore along a Southern California sandy beach. We utilized this opportunity to investigate ocean-atmosphere mass transfer via sea spray aerosol and linkage to source waters. Aerosol-concentrating sampling equipment was deployed at beachside and inland locations during three dye releases. Concentrated aerosol samples were analyzed for dye content using fluorescence spectroscopy. Here we present the ocean and atmosphere conditions associated with the presence and absence of dye in aerosol samples. Dye was identified in aerosol samples collected 0.1-0.3 km from the shoreline for 6 hs during the first and third dye releases of the CSIDE project. During these releases the dye persisted in the waters upwind of the sampling equipment. Dye was not detected in aerosol samples collected during the second release during which dye was moved away from waters upwind of the sampling equipment. Recovery of a chemical tracer in sea spray aerosol allows direct linkage to a known source area in the ocean that is independent of, but supported by, wind data. Our observations demonstrate: a tight ocean-atmosphere spatial coupling; a short residence time of coastal marine constituents before transfer to the atmosphere; that the ocean is both a sink for and a source of atmospheric and terrestrial material; and that human inputs to the ocean can return to us in sea spray aerosol.

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-08-01

Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-02-01

Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57' E, 30°46' N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ˜ 2.0 µg m-3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O / C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O / C ratio of 0.72), and an average O / C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated

Investigation of the CCN Activity, BC and UVBC Mass Concentrations of Biomass Burning Aerosols during the 2013 BASELInE Campaign

NASA Technical Reports Server (NTRS)

Hsiao, Ta-Chih; Ye, Wei-Cheng; Wang, Sheng-Hsiang; Tsay, Si-Chee; Chen, Wei-Nai; Lin, Neng-Huei; Lee, Chung-Te; Hung, Hui-Ming; Chuang, Ming-Tung; Chantara, Somporn

2015-01-01

Biomass-burning (BB) aerosols, acting as cloud condensation nuclei (CCN), can influence cloud microphysical and radiative properties. In this study, we present CCN measured near the BB source regions over northern Southeast Asia (Doi Ang Khang, Thailand) and at downwind receptor areas (Lulin Atmospheric Background Station, Taiwan), focusing exclusively on 13-20 March 2013 as part of 2013 spring campaign of the Seven SouthEast Asian Studies (7-SEAS) intensive observation. One of the campaigns objectives is to characterize BB aerosols serving as CCN in SouthEast Asia (SEA). CCN concentrations were measured by a CCN counter at 5 supersaturation (SS) levels: 0.15%, 0.30%, 0.45%, 0.60%, and 0.75%. In addition, PM2.5 and black carbon mass concentrations were analyzed by using a tapered element oscillating microbalance and an aethalometer. It was found the number-size distributions and the characteristics of hygroscopicity (e.g., activation ratio and k) of BB aerosols in SEA have a strong diurnal pattern, and different behaviors of patterns were characterized under two distinct weather systems. The overall average value was low (0.05-0.1) but comparable with previous CCN studies in other BB source regions. Furthermore, a large fraction of UV-absorbing organic material (UVBC) and high Delta-C among BB aerosols were also observed, which suggest the existence of substantial particulate organic matter in fresh BB aerosols. These data provide the most extensive characterization of BB aerosols in SEA until now.

Spatial variability of carbonaceous aerosol concentrations in East and West Jerusalem.

PubMed

von Schneidemesser, Erika; Zhou, Iiabin; Stone, Elizabeth A; Schauer, James I; Shpund, Jacob; Brenner, Shmuel; Qasrawi, Radwan; Abdeen, Ziad; Sarnat, Jeremy A

2010-03-15

Carbonaceous aerosol concentrations and sources were compared during a year long study at two sites in East and West Jerusalem that were separated by a distance of approximately 4 km. One in six day 24-h PM(2.5) elemental and organic carbon concentrations were measured, along with monthly average concentrations of particle-phase organic compound tracers for primary and secondary organic aerosol sources.Tracer compounds were used in a chemical mass balance ICMB) model to determine primary and secondary source contributions to organic carbon. The East Jerusalem sampling site at Al Quds University experienced higher concentrations of organic carbon (OC) and elemental carbon (EC) compared to the West Jerusalem site at Hebrew University. The annual average concentrations of OC and EC at the East Jerusalem site were 5.20 and 2.19 μg m(-3), respectively, and at the West Jerusalem site were 4.03 and 1.14 μg m(-3), respectively. Concentrations and trends of secondary organic aerosol and vegetative detritus were similar at both sites, but large differences were observed in the concentrations of organic aerosol from fossil fuel combustion and biomass burning, which was the cause of the large differences in OC and EC concentrations observed at the two sites.

Evaluation of species-dependent detection efficiencies in the aerosol mass spectrometer

USDA-ARS?s Scientific Manuscript database

Mass concentrations of chemical species calculated from the aerosol mass spectrometer (AMS) depend on two factors: particle collection efficiency (CE) and relative ionization efficiency (RIE, relative to the primary calibrant ammonium nitrate). While previous studies have characterized CE, RIE is re...

Reconstruction of Aerosol Concentration and Composition from Glacier Ice Cores

NASA Astrophysics Data System (ADS)

Vogel, Alexander; Dällenbach, Kaspar; El-Haddad, Imad; Wendl, Isabel; Eichler, Anja; Schwikowski, Margit

2017-04-01

Reconstruction of the concentration and composition of natural aerosol in an undisturbed atmosphere enables the evaluation of the understanding of aerosol-climate effects, which is currently based on highly uncertain emission inventories of the biosphere under pre-industrial conditions. Understanding of the natural state of the pre-industrial atmosphere and evaluating the atmospheric perturbations by anthropogenic emissions, and their potential feedbacks, is essential for accurate model predictions of the future climate (Boucher et al., 2013). Here, we present a new approach for the chemical characterization of the organic fraction preserved in cold-glacier ice cores. From this analysis historic trends of atmospheric organic aerosols are reconstructed, allowing new insights on organic aerosol composition and mass in the pre-industrial atmosphere, which can help to improve climate models through evaluation of our current understanding of aerosol radiative effects. We present results from a proof-of-principal study, analyzing an 800 year ice core record from the Lomonosovfonna glacier ice core, drilled in 2009 in Svalbard, Norway, using a setup that has until then only been applied on offline measurements of aerosol filter extracts (Dällenbach et al., 2016): The melted ice was nebulized and dried, such that aerosols are formed from the soluble and insoluble organic and inorganic compounds that are preserved in the ice. To improve the sensitivity, the aerosol stream was then enriched by the application of an online aerosol concentrator, before the aerosol was analyzed by electron ionization within a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). We were able to demonstrate that this setup is a quantitative method toward nitrate and sulfate when internal inorganic standards of NH415NO3 and (NH4)234SO4 are added to the sample. Comparison between AMS and IC measurements of nitrate and sulfate resulted in an excellent agreement. The analysis of

Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

NASA Technical Reports Server (NTRS)

Igel, Adele L.; Van Den Heever, Susan C.; Naud, Catherine M.; Saleeby, Stephen M.; Posselt, Derek J.

2013-01-01

An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.

Mass spectrometric airborne measurements of submicron aerosol and cloud residual composition in tropic deep convection during ACRIDICON-CHUVA

NASA Astrophysics Data System (ADS)

Schulz, Christiane; Schneider, Johannes; Mertes, Stephan; Kästner, Udo; Weinzierl, Bernadett; Sauer, Daniel; Fütterer, Daniel; Walser, Adrian; Borrmann, Stephan

2015-04-01

Airborne measurements of submicron aerosol and cloud particles were conducted in the region of Manaus (Amazonas, Brazil) during the ACRIDICON-CHUVA campaign in September 2014. ACRIDICON-CHUVA aimed at the investigation of convective cloud systems in order to get a better understanding and quantification of aerosol-cloud-interactions and radiative effects of convective clouds. For that, data from airborne measurements within convective cloud systems are combined with satellite and ground-based data. We used a C-ToF-AMS (Compact-Time-of-Flight-Aerosol-Mass-Spectrometer) to obtain information on aerosol composition and vertical profiles of different aerosol species, like organics, sulphate, nitrate, ammonium and chloride. The instrument was operated behind two different inlets: The HASI (HALO Aerosol Submicrometer Inlet) samples aerosol particles, whereas the CVI (Counterflow Virtual Impactor) samples cloud droplets and ice particles during in-cloud measurements, such that cloud residual particles can be analyzed. Differences in aerosol composition inside and outside of clouds and cloud properties over forested or deforested region were investigated. Additionally, the in- and outflow of convective clouds was sampled on dedicated cloud missions in order to study the evolution of the clouds and the processing of aerosol particles. First results show high organic aerosol mass concentrations (typically 15 μg/m3 and during one flight up to 25 μg/m3). Although high amounts of organic aerosol in tropic air over rainforest regions were expected, such high mass concentrations were not anticipated. Next to that, high sulphate aerosol mass concentrations (about 4 μg/m3) were measured at low altitudes (up to 5 km). During some flights organic and nitrate aerosol was observed with higher mass concentrations at high altitudes (10-12 km) than at lower altitudes, indicating redistribution of boundary layer particles by convection. The cloud residuals measured during in

Variations of the aerosol concentration and chemical composition over the arid steppe zone of Southern Russia in summer

NASA Astrophysics Data System (ADS)

Artamonova, M. S.; Gubanova, D. P.; Iordanskii, M. A.; Lebedev, V. A.; Maksimenkov, L. O.; Minashkin, V. M.; Obvintsev, Y. I.; Chketiani, O. G.

2016-12-01

Variations in the surface aerosol over the arid steppe zone of Southern Russia have been measured. The parameters of atmospheric aerosol (mass concentration, both dispersed and elemental compositions) and meteorological parameters were measured in Tsimlaynsk raion (Rostov oblast). The chemical composition of aerosol particles in the atmospheric surface layer has been determined, and the coefficients of enrichment of elements with respect to clarkes in the Earth's crust have been calculated. It is shown that, in summer, arid aerosols are transported from both alkaline and sandy soils of Kalmykia to the air basin over the observation zone. Aerosol particles in the surface air layer over this region have been found to contain the products of combustion of oil, coal, and ethylized fuel. These combustion products make a small contribution to the total mass concentration of atmospheric aerosol; however, they are most hazardous to the health of people because of their sizes and heavy-metal contents. A high concentration of submicron sulfur-containing aerosol particles of chemocondensation nature has been recorded. Sources of aerosol of both natural and anthropogenic origins in southern Russia are discussed.

Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia

NASA Astrophysics Data System (ADS)

Schneider, J.; Freutel, F.; Zorn, S. R.; Chen, Q.; Farmer, D. K.; Jimenez, J. L.; Martin, S. T.; Artaxo, P.; Wiedensohler, A.; Borrmann, S.

2011-11-01

The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker fragments places upper limits of 7.5% for amino acids and 5.6% for carbohydrates on the contribution of primary biological aerosol particles (PBAP) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m-3. Carbohydrates and proteins (composed of amino acids) make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAP mass fraction of about 20% to the submicron organic aerosol measured in Amazonia during AMAZE-08.

Continuous dry dispersion of multi-walled carbon nanotubes to aerosols with high concentrations of individual fibers

NASA Astrophysics Data System (ADS)

Simonow, Barbara Katrin; Wenzlaff, Daniela; Meyer-Plath, Asmus; Dziurowitz, Nico; Thim, Carmen; Thiel, Jana; Jandy, Mikolaj; Plitzko, Sabine

2018-06-01

The assessment of the toxicity of airborne nanofibers is an important task. It relies on toxicological inhalation studies and validated exposure measurement techniques. Both require nanofiber-containing aerosols of known morphological composition and controlled fraction of individual fibers. Here, a dry powder dispersion method is presented that operates with mixtures of nanofibers and microscale beads. Aerosolization experiments of mixtures of multi-walled carbon nanotubes (MWCNTs) and glass beads that were continuously fed into a Venturi nozzle enabled high generation rates of aerosols composed of individual and agglomerate nanofiber structures. The aerosol process achieved good stability over more than 2 h with respect to concentration and aerodynamic size distribution. Its operation duration is limited only by the reservoir volume of the cyclone used to separate the beads from the aerosol. The aerosol concentration can be controlled by changing the mass ratio of MWCNTs and glass beads or by adapting the mass feed rate to the nozzle. For two agglomerated MWCNT materials, aerosol concentrations ranged from 1700 to 64,000 nano-objects per cm3. Comprehensive scanning electron microscope analysis of filter samples was performed to categorize and determine the morphological composition of the aerosol, its fiber content as well as fiber length and diameter distributions. High fractions of individual fibers of up to 34% were obtained, which shows the setup to be capable of dispersing also highly tangled MWCNT agglomerates effectively.

Effects of diesel exhaust aftertreatment devices on concentrations and size distribution of aerosols in underground mine air.

PubMed

Bugarski, Aleksandar D; Schnakenberg, George H; Hummer, Ion A; Cauda, Emanuele; Janisko, Samuel I; Patts, Larry D

2009-09-01

Three types of uncatalyzed diesel particulate filter (DPF) systems, three types of high-temperature disposable filter elements (DFEs), and one diesel oxidation catalytic converter (DOC) were evaluated in underground mine conditions for their effects on the concentrations and size distributions of diesel aerosols. Those effects were compared with the effects of a standard muffler. The experimental work was conducted directly in an underground environment using a unique diesel laboratory developed in an underground experimental mine. The DPF systems reduced total mass of aerosols in the mine air approximately 10-fold for light-load and 20-fold or more for high-load test conditions. The DFEs offered similar reductions in aerosol mass concentrations. The efficiency of the new DFEs significantly increased with accumulation of operating time and buildup of diesel particulate matter in the porous structure of the filter elements. A single laundering process did not exhibit substantial effects on performance of the filter element The effectiveness of DPFs and DFEs in removing aerosols by number was strongly influenced by engine operating mode. The concentrations of nucleation mode aerosols in the mine air were found to be substantially higher for both DPFs and DFEs when the engine was operated at high-load modes than at low-load modes. The effects of the DOC on mass and number concentrations of aerosols in mine air were relatively minor when compared to those of the DPF and DFE systems.

Mass spectrometry of atmospheric aerosols--recent developments and applications. Part II: On-line mass spectrometry techniques.

PubMed

Pratt, Kerri A; Prather, Kimberly A

2012-01-01

Many of the significant advances in our understanding of atmospheric particles can be attributed to the application of mass spectrometry. Mass spectrometry provides high sensitivity with fast response time to probe chemically complex particles. This review focuses on recent developments and applications in the field of mass spectrometry of atmospheric aerosols. In Part II of this two-part review, we concentrate on real-time mass spectrometry techniques, which provide high time resolution for insight into brief events and diurnal changes while eliminating the potential artifacts acquired during long-term filter sampling. In particular, real-time mass spectrometry has been shown recently to provide the ability to probe the chemical composition of ambient individual particles <30 nm in diameter to further our understanding of how particles are formed through nucleation in the atmosphere. Further, transportable real-time mass spectrometry techniques are now used frequently on ground-, ship-, and aircraft-based studies around the globe to further our understanding of the spatial distribution of atmospheric aerosols. In addition, coupling aerosol mass spectrometry techniques with other measurements in series has allowed the in situ determination of chemically resolved particle effective density, refractive index, volatility, and cloud activation properties. Copyright © 2011 Wiley Periodicals, Inc.

Laser Ablation-Aerosol Mass Spectrometry-Chemical Ionization Mass Spectrometry for Ambient Surface Imaging

DOE PAGES

Berry, Jennifer L.; Day, Douglas A.; Elseberg, Tim; ...

2018-02-20

Mass spectrometry imaging is becoming an increasingly common analytical technique due to its ability to provide spatially resolved chemical information. In this paper, we report a novel imaging approach combining laser ablation with two mass spectrometric techniques, aerosol mass spectrometry and chemical ionization mass spectrometry, separately and in parallel. Both mass spectrometric methods provide the fast response, rapid data acquisition, low detection limits, and high-resolution peak separation desirable for imaging complex samples. Additionally, the two techniques provide complementary information with aerosol mass spectrometry providing near universal detection of all aerosol molecules and chemical ionization mass spectrometry with a heated inletmore » providing molecular-level detail of both gases and aerosols. The two techniques operate with atmospheric pressure interfaces and require no matrix addition for ionization, allowing for samples to be investigated in their native state under ambient pressure conditions. We demonstrate the ability of laser ablation-aerosol mass spectrometry-chemical ionization mass spectrometry (LA-AMS-CIMS) to create 2D images of both standard compounds and complex mixtures. Finally, the results suggest that LA-AMS-CIMS, particularly when combined with advanced data analysis methods, could have broad applications in mass spectrometry imaging applications.« less

Laser Ablation-Aerosol Mass Spectrometry-Chemical Ionization Mass Spectrometry for Ambient Surface Imaging

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

Berry, Jennifer L.; Day, Douglas A.; Elseberg, Tim

Mass spectrometry imaging is becoming an increasingly common analytical technique due to its ability to provide spatially resolved chemical information. In this paper, we report a novel imaging approach combining laser ablation with two mass spectrometric techniques, aerosol mass spectrometry and chemical ionization mass spectrometry, separately and in parallel. Both mass spectrometric methods provide the fast response, rapid data acquisition, low detection limits, and high-resolution peak separation desirable for imaging complex samples. Additionally, the two techniques provide complementary information with aerosol mass spectrometry providing near universal detection of all aerosol molecules and chemical ionization mass spectrometry with a heated inletmore » providing molecular-level detail of both gases and aerosols. The two techniques operate with atmospheric pressure interfaces and require no matrix addition for ionization, allowing for samples to be investigated in their native state under ambient pressure conditions. We demonstrate the ability of laser ablation-aerosol mass spectrometry-chemical ionization mass spectrometry (LA-AMS-CIMS) to create 2D images of both standard compounds and complex mixtures. Finally, the results suggest that LA-AMS-CIMS, particularly when combined with advanced data analysis methods, could have broad applications in mass spectrometry imaging applications.« less

Estimation of columnar concentrations of absorbing and scattering fine mode aerosol components using AERONET data

NASA Astrophysics Data System (ADS)

Choi, Yongjoo; Ghim, Young Sung

2016-11-01

Columnar concentrations of absorbing and scattering components of fine mode aerosols were estimated using Aerosol Robotic Network (AERONET) data for a site downwind of Seoul. The study period was between March 2012 and April 2013 including the period of the Distributed Regional Aerosol Gridded Observation Networks (DRAGON)-Asia campaign in March to May 2012. The Maxwell Garnett mixing rule was assumed for insoluble components embedded in a host solution, while the volume average mixing rule was assumed for the aqueous solution of soluble components. During the DRAGON-Asia campaign the surface concentrations of major components of fine particles were measured. The columnar mass fractions of black carbon (BC), organic carbon (OC), mineral dust (MD), and ammonium sulfate (AS) were 1.5, 5.9, 6.6, and 52%, respectively, which were comparable to the mass fractions measured at the surface for BC, OC, and secondary inorganic aerosols at 2.3, 18, and 55%. The vertical distributions of BC and AS were investigated by employing the concept of a column height. While the column height for BC was similar to the planetary boundary layer (PBL) height, that for AS was 4.4 times higher than the PBL height and increased with air temperature from March to May. The monthly variations of the columnar mass concentrations during the study period were generally well explained in term of meteorology and emission characteristics. However, certain variations of MD were different from those typically observed primarily because only fine mode aerosols were considered.

Aircraft-based Aerosol Size and Composition Measurements during ACE-Asia and CRYSTAL-FACE using an Aerodyne Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Bahreini, R.; Jimenez, J.; Delia, A.; Flagan, R. C.; Seinfeld, J. H.; Jayne, J. T.; Worsnop, D. R.

2002-12-01

An Aerodyne Aerosol Mass Spectrometer (AMS) was deployed in an aircraft for the first time during the ACE-Asia field campaign. The AMS was operated on board the CIRPAS Twin Otter aircraft to measure the size-resolved chemical composition of the submicron aerosols in the outflow from Eastern Asia. Research flights were carried out from March 31 to May 1, 2001 in an area that covered 127 E-135 E and 32 N-38 N on longitude and latitude, respectively. The submicron aerosol was typically distributed in distinct layers (from the boundary layer to ~ 3700 m). This is consistent with other on-board measurements. The aerosol in the pollution layers was mainly composed of sulfate, ammonium, and organics separated by cleaner layers. Sub-micron nitrate aerosols were also detected in some layers. Since the molar ratio of positive to negative ions did not exceed one on most of the constant altitude legs of the flights, the particles were not completely neutralized. Sulfate and organics concentrations of up to 10 and 5 ug m-3 (STP), respectively, were measured on some pollution layers. AMS measurements of sulfate concentration and NH4/SO4 mass ratio (~0.16 on average) are consistent with previously reported measurements at Cheju Island, South Korea [Charmichael et al., 1997; Chen et al., 1997] and Sapporo, Japan [Kaneyasu et al., 1995]. The mass-weighed size distribution of the sub-micron sulfate was relatively constant from day to day and layer to layer, with an aerodynamic mode at 350-500 nm (vacuum aerodynamic diameter) and FWHM ~ 400 nm on most of the layers. Furthermore, the ratios between SO4/ NH4/ NO3/ Organics were approximately independent of size in the sub-micron size range. Comparisons of AMS data to other on-board aerosol measurements will be presented. In particular, the AMS mass concentration correlates well with the aerosol volume determined by the on-board Differential Automated Classifying Aerosol Detector (DCAD). In addition, preliminary results of airborne size

Primary and secondary organic aerosols in Fresno, California during wintertime: Results from high resolution aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Ge, Xinlei; Setyan, Ari; Sun, Yele; Zhang, Qi

2012-10-01

Organic aerosols (OA) were studied in Fresno, California, in winter 2010 with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). OA dominated the submicron aerosol mass (average = 67%) with an average concentration of 7.9μg m-3 and a nominal formula of C1H1.59N0.014O0.27S0.00008, which corresponds to an average organic mass-to-carbon ratio of 1.50. Three primary OA (POA) factors and one oxygenated OA factor (OOA) representative of secondary OA (SOA) were identified via Positive Matrix Factorization of the high-resolution mass spectra. The three POA factors, which include a traffic-related hydrocarbon-like OA (HOA), a cooking OA (COA), and a biomass burning OA (BBOA) released from residential heating, accounted for an average 57% of the OA mass and up to 80% between 6 - 9 P.M., during which enhanced emissions from evening rush hour traffic, dinner cooking, and residential wood burning were exacerbated by low mixed layer height. The mass-based size distributions of the OA factors were estimated based on multilinear analysis of the size-resolved mass spectra of organics. Both HOA and BBOA peaked at ˜140 nm in vacuum aerodynamic diameter (Dva) while OOA peaked at an accumulation mode of ˜460 nm. COA exhibited a unique size distribution with two size modes centering at ˜200 nm and 450 nm respectively. This study highlights the leading roles played by anthropogenic POA emissions, primarily from traffic, cooking and residential heating, in aerosol pollution in Fresno in wintertime.

Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Dreyfus, Matthew A.

Analytical methods developed to sample and characterize ambient organic aerosols often face the trade-off between long sampling times and the loss of detailed information regarding specific chemical species present. The soft, universal ionization scheme of the Photoionization Aerosol Mass Spectrometer (PIAMS) allows for identification of various chemical compounds by a signature ion, often the molecular ion. The goal of this thesis work is to apply PIAMS to both laboratory and field experiments to answer questions regarding the formation, composition, and behavior of organic aerosols. To achieve this goal, a variety of hardware and software upgrades were administered to PIAMS to optimize the instrument. Data collection and processing software were either refined or built from the ground up to simplify difficult or monotonous tasks. Additional components were added to PIAMS with the intent to automate the instrument, enhance the results, and make the instrument more rugged and user-friendly. These changes, combined with the application of an external particle concentration system (mini-Versatile Aerosol Concentration Enrichment System, m-VACES), allowed PIAMS to be suitable for field measurements of organic aerosols. Two such field campaigns were completed, both at the State of Delaware Air Quality Monitoring Site in Wilmington, Delaware: a one week period in June, 2006, and an 18 day period in October and November of 2007. A sampling method developed was capable of collecting sufficient ambient organic aerosol and analyzing it with a time resolution of 3.5 minutes. Because of this method, short term concentration changes of individual species can be tracked. Combined with meteorological data, the behavior of these species can be analyzed as a function of time or wind direction. Many compounds are found at enhanced levels during the evening/night-time hours; potentially due to the combined effects of temperature inversion, and fresh emissions in a cooler environment

Introduction of the new concept: Potential Aerosol Mass (PAM) for Inorganic and Organic Secondary Aerosol

NASA Astrophysics Data System (ADS)

Kang, E.; Root, M. J.; Brune, W. H.

2006-12-01

A new concept, the Potential Aerosol Mass (PAM), is being developed and tested in the laboratory with the goal of deploying instruments to measure PAM in the atmosphere. PAM can be defined as the maximum aerosol mass that precursor gases can be oxidized to form. In the PAM concept, all precursor gases are oxidized to low volatile compounds with excessive amount of oxidants in a small continuous-flow Teflon cylinder, resulting in aerosol formation. Excessive amounts of OH and O3 are produced by a UV light that shines into the Teflon chamber. For our studies, the aerosol mass is then detected with a real-time aerosol mass measurement instrument, the Rupprecht and Patashnick Tapered Element Oscillating Microbalance (TEOM) and Filter Dynamic Measurement System (FDMS). As a test of the system, SO2 was oxidized to sulfate; the measured and calculated conversion ratios of sulfate aerosol mass to SO2 mass agree to within 10%. We will discuss the results of a series of laboratory tests that have been conducted with α-pinene to determine the variables that most affect its Secondary Organic Aerosol (SOA) yield. We will also discuss the results of some atmospheric measurement tests made at a site on the Penn State University campus.

Ice nucleating particle concentration during a combustion aerosol event

NASA Astrophysics Data System (ADS)

Adams, Mike; O'Sullivan, Daniel; Porter, Grace; Sanchez-Marroquin, Alberto; Tarn, Mark; Harrison, Alex; McQuaid, Jim; Murray, Benjamin

2017-04-01

The formation of ice in supercooled clouds is important for cloud radiative properties, their lifetime and the formation of precipitation. Cloud water droplets can supercool to below -33oC, but in the presence of Ice Nucleating Particles (INPs) freezing can be initiated at much higher temperatures. The concentration of atmospheric aerosols that are active as INPs depends on a number of factors, such as temperature and aerosol composition and concentration. However, our knowledge of which aerosol types serve as INPs is limited. For example, there has been much discussion over whether aerosol from combustion processes are important as INP. This is significant because combustion aerosol have increased in concentration dramatically since pre-industrial times and therefore have the potential to exert a significant anthropogenic impact on clouds and climate. In this study we made measurements of INP concentrations in Leeds over a specific combustion aerosol event in order to test if there was a correlation between INP concentrations and combustion aerosol. The combustion aerosol event was on the 5th November which is a major bonfire and firework event celebrated throughout the UK. During the event we observed a factor of five increase in aerosol and a factor of 10 increase in black carbon, but observed no significant increase in INP concentration. This implies that black carbon and combustion aerosol did not compete with the background INP during this event.

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

Sources and atmospheric processing of winter aerosols in Seoul, Korea: insights from real-time measurements using a high-resolution aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Kim, Hwajin; Zhang, Qi; Bae, Gwi-Nam; Kim, Jin Young; Bok Lee, Seung

2017-02-01

Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 µg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 µg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air

Chemical Characterization of Particulate Matter at the La Porte site Using an Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Silva, P. J.; Worsnop, D.; Canagaratna, M.; Jimenez, J. L.; Delia, A.; Purvis, K.; Davidovits, P.

2001-12-01

During the summer of 2000, a large atmospheric chemistry field campaign took place in the Greater Houston area in conjunction with an EPA supersite. As part of the campaign, we operated an aerosol mass spectrometer from 20 August, 2000 until 15 September, 2000. The aerosol mass spectrometer (AMS) obtained chemical composition data and particle size distributions continuously with 10 minute averaging times. The measured aerosol mass concentration ranged from approximately 2 μ g m-3 to a high of 30 μ g m-3. Ammonium and sulfate were the two dominant chemical species present during most of the study. The mass concentration of particulate nitrate was typically less than a few μ g m-3, with one major nitrate event on 23 August, 2000. Very small amounts of non-sea salt chloride were detected in the particles, typically less than one μ g m-3, again with the largest value detected on 23 August 2000. In addition to the inorganic species, several different organic aerosol types were identified based on simple evaluation of mass spectral and size distribution data. Three organic particle types appear to be from discrete primary sources of organic aerosol. A combustion particle type displays mass spectra similar to those observed from diesel exhaust emissions. The temporal variation of this type shows sharp spikes, consistent with primary sources and sharp plumes that drift pass. A second organic particle type is responsible for the largest particle mass concentrations observed during the entire study, occurring during a fire episode on 5-6 September, 2000. The mass spectra exhibit characteristic peaks representative of markers for compounds from biomass burning, including levoglucosan and dehydroabietic acid. A third organic particle type observed during the study exhibits peaks in the mass spectra that are characteristic of fluorinated hydrocarbons and are similar to mass spectra of pump oil. This particle type contributes several μ g m-3 to the ambient particle mass

Influence of air mass origin on aerosol properties at a remote Michigan forest site

NASA Astrophysics Data System (ADS)

VanReken, T. M.; Mwaniki, G. R.; Wallace, H. W.; Pressley, S. N.; Erickson, M. H.; Jobson, B. T.; Lamb, B. K.

2015-04-01

The northern Great Lakes region of North America is a large, relatively pristine area. To date, there has only been limited study of the atmospheric aerosol in this region. During summer 2009, a detailed characterization of the atmospheric aerosol was conducted at the University of Michigan Biological Station (UMBS) as part of the Community Atmosphere-Biosphere Interactions Experiment (CABINEX). Measurements included particle size distribution, water-soluble composition, and CCN activity. Aerosol properties were strongly dependent on the origin of the air masses reaching the site. For ∼60% of the study period, air was transported from sparsely populated regions to the northwest. During these times aerosol loadings were low, with mean number and volume concentrations of 1630 cm-3 and 1.91 μm3 cm-3, respectively. The aerosol during clean periods was dominated by organics, and exhibited low hygroscopicities (mean κ = 0.18 at s = 0.3%). When air was from more populated regions to the east and south (∼29% of the time), aerosol properties reflected a stronger anthropogenic influence, with 85% greater particle number concentrations, 2.5 times greater aerosol volume, six times more sulfate mass, and increased hygroscopicity (mean к = 0.24 at s = 0.3%). These trends are have the potential to influence forest-atmosphere interactions and should be targeted for future study.

Influence of air mass origin on aerosol properties at a remote Michigan forest site

DOE PAGES

VanReken, T. M.; Mwaniki, G. R.; Wallace, H. W.; ...

2015-02-10

The northern Great Lakes region of North America is a large, relatively pristine area. To date, there has only been limited study of the atmospheric aerosol in this region. During summer 2009, a detailed characterization of the atmospheric aerosol was conducted at the University of Michigan Biological Station (UMBS) as part of the Community Atmosphere–Biosphere Interactions Experiment (CABINEX). Measurements included particle size distribution, water-soluble composition, and CCN activity. Aerosol properties were strongly dependent on the origin of the air masses reaching the site. For ~60% of the study period, air was transported from sparsely populated regions to the northwest. Duringmore » these times aerosol loadings were low, with mean number and volume concentrations of 1630 cm -3 and 1.91 μm 3 cm -3, respectively. The aerosol during clean periods was dominated by organics, and exhibited low hygroscopicities (mean κ = 0.18 at s = 0.3%). When air was from more populated regions to the east and south (~29% of the time), aerosol properties reflected a stronger anthropogenic influence, with 85% greater particle number concentrations, 2.5 times greater aerosol volume, six times more sulfate mass, and increased hygroscopicity (mean к = 0.24 at s = 0.3%). Furthermore, these trends are have the potential to influence forest–atmosphere interactions and should be targeted for future study.« less

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

Seasonal differences in aerosol water may reconcile AOT and surface mass measurements in the Southeast U.S.

NASA Astrophysics Data System (ADS)

Nguyen, T. K. V.; Ghate, V. P.; Carlton, A. M. G.

2015-12-01

Summertime aerosol optical thickness (AOT) in the Southeast U.S. is high and sharply enhanced (2-3 times) compared to wintertime AOT. This seasonal pattern is unique to the Southeast U.S. and is of particular interest because temperatures there have not warmed over the past 100 years, contrasting with trends in other U.S. regions. Some investigators hypothesize the Southeast temperature trend is due to secondary organic aerosols (SOA) formed from interactions of biogenic volatile organic compounds (BVOCs) and anthropogenic emissions that create a cooling haze. However, aerosol measurements made at the surface do not exhibit strong seasonal differences in mass or organic fraction to support this hypothesis. In this work, we attempt to reconcile the spatial and temporal distribution of AOT over the U.S. with surface mass measurements by examining trends in particle-phase liquid water, an aerosol constituent that effectively scatters radiation and is removed from aerosols in mass measurements at routine surface monitoring sites. We employ the thermodynamic model ISORROPIA (v2.1) to estimate surface and aloft aerosol water mass concentrations at locations of Interagency Monitoring of Protected Visual Environments (IMPROVE) sites using measured speciated ion mass concentrations and NCEP North American Regional Reanalysis (NARR) meteorological data. Results demonstrate strong seasonal differences in aerosol water in the eastern compared to the western part of the U.S., consistent with geographic patterns in AOT. The highest mean regional seasonal difference from 2000 to 2007 is 5.5 μg m-3 and occurs the Southeast, while the lowest is 0.44 μg m-3 and occurs in the dry Mountain West. Our findings suggest 1) similarity between spatial trends in aerosol water in the U.S. and previously published AOT data from the MODIS-TERRA instrument and 2) similar interannual trends in mean aerosol water and previously published interannual AOT trends from MISR, MODIS-TERRA, MODIS

Wide-range particle characterization and elemental concentration in Beijing aerosol during the 2013 Spring Festival.

PubMed

Jing, Hui; Li, Yu-Feng; Zhao, Jiating; Li, Bai; Sun, Jialong; Chen, Rui; Gao, Yuxi; Chen, Chunying

2014-09-01

The number and mass concentration, size distribution, and the concentration of 16 elements were studied in aerosol samples during the Spring Festival celebrations in 2013 in Beijing, China. Both the number and mass concentration increased sharply in a wide range from 10 nm to 10 μm during the firecrackers and fireworks activities. The prominent increase of the number concentration was in 50 nm-500 nm with a peak of 1.7 × 10(5)/cm(3) at 150 nm, which is 8 times higher than that after 1.5 h. The highest mass concentration was in 320-560 nm, which is 4 times higher than the control. K, Mg, Sr, Ba and Pb increased sharply during the firework activities in PM10. Although the aerosol emission from firework activities is a short-term air quality degradation event, there may be a substantial hazard arising from the chemical composition of the emitted particles. Copyright © 2014 Elsevier Ltd. All rights reserved.

Aerosol formation by ozonolysis of α- and β-pinene with initial concentrations below 1 ppb

NASA Astrophysics Data System (ADS)

Saathoff, Harald; Naumann, Karl-Heinz; Möhler, Ottmar

2014-05-01

Secondary organic aerosols (SOA) from the oxidation of biogenic volatile organic compounds (BVOC) are a large fraction of the tropospheric aerosol especially over tropical continental regions. The dominant SOA forming compounds are monoterpenes of which pinene is the most abundant. The reactions of monoterpenes with OH radicals, NO3 radicals, and ozone yield secondary organic aerosol mass in highly variable yields. Despite the various studies on SOA formation the influence of temperature and precursor concentrations on SOA yields are still major uncertainties in tropospheric aerosol models. In previous studies we observed a negative temperature dependence of SOA yields for SOA from ozonolysis α-pinene and limonene (Saathoff et al., 2009). However, this study as well as most of the literature data for measured SOA yields is limited to terpene concentrations of several ppb and higher (e.g. Bernard et al., 2012), hence about an order of magnitude higher than terpene concentrations even near their sources. Monoterpene concentrations in and above tropical or boral forests reach values up to a few tenth of a ppb during daytime decreasing rapidly with altitude in the boundary layer (Kesselmeier et al. 2000; Boy et al., 2004). Therefore we investigated the yield of SOA material from the ozonolysis of α- and β-pinene under simulated tropospheric conditions in the large aerosol chamber AIDA on time scales of several hours and for terpene concentrations between 0.1 and 1 ppb. The temperatures investigated were 243, 274, and 296 K with relative humidities ranging from 25% to 41%. The organic aerosol was generated by controlled oxidation with an excess of ozone (220-930 ppb) and the aerosol yield is calculated from size distributions measured with differential mobility analysers (SMPS, TSI, 3071 & 3080N) in the size range between 2 and 820 nm. On the basis of the measured initial particle size distribution, particle number concentration (CPC, TSI, 3775, 3776, 3022), and

Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J.; Healy, R.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; Ehn, M.; Mikkilä, J.; Kulmala, M.; O'Dowd, C. D.

2010-09-01

As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June, 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the N. E. Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were

Impact of radon gas concentration in the aerosoles profile

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

Lukaj, Edmond, E-mail: mondilukaj@yahoo.com; Vila, Floran, E-mail: floranvila@yahoo.com; Mandija, Florian, E-mail: fmandija@yahoo.com

Radon gases relased from building materials and from earth surface are the major responsibility of air ionization. Radon nuclear decay can produce an alpha particle with high energy and Radon progeny. This particle and gamma rays can deliver particles in the air and produce ions with different polarities. This ions, because of induced electric charge, can attach with air aerosols and charge them with their electric charge. The charged aerosols can interact with the other aerosols and ions. Because of this exchange, the air conductivity and the aerosol profiles will change dependently by Radon gas concentration and gamma radiation. Observationsmore » show an increase in concentration of Radon during the night, and a decrease during the daylight time. The Radon gas concentration changed hour by hour can induce aerosol profile to change. This dependency between the aerosol profiles and the Radon gas concentrations is discussed.« less

A qualitative comparison of secondary organic aerosol yields and composition from ozonolysis of monoterpenes at varying concentrations of NO2

NASA Astrophysics Data System (ADS)

Draper, D. C.; Farmer, D. K.; Desyaterik, Y.; Fry, J. L.

2015-11-01

The effect of NO2 on secondary organic aerosol (SOA) formation from ozonolysis of α-pinene, β-pinene, Δ3-carene, and limonene was investigated using a dark flow-through reaction chamber. SOA mass yields were calculated for each monoterpene from ozonolysis with varying NO2 concentrations. Kinetics modeling of the first-generation gas-phase chemistry suggests that differences in observed aerosol yields for different NO2 concentrations are consistent with NO3 formation and subsequent competition between O3 and NO3 to oxidize each monoterpene. α-Pinene was the only monoterpene studied that showed a systematic decrease in both aerosol number concentration and mass concentration with increasing [NO2]. β-Pinene and Δ3-carene produced fewer particles at higher [NO2], but both retained moderate mass yields. Limonene exhibited both higher number concentrations and greater mass concentrations at higher [NO2]. SOA from each experiment was collected and analyzed by HPLC-ESI-MS, enabling comparisons between product distributions for each system. In general, the systems influenced by NO3 oxidation contained more high molecular weight products (MW > 400 amu), suggesting the importance of oligomerization mechanisms in NO3-initiated SOA formation. α-Pinene, which showed anomalously low aerosol mass yields in the presence of NO2, showed no increase in these oligomer peaks, suggesting that lack of oligomer formation is a likely cause of α-pinene's near 0 % yields with NO3. Through direct comparisons of mixed-oxidant systems, this work suggests that NO3 is likely to dominate nighttime oxidation pathways in most regions with both biogenic and anthropogenic influences. Therefore, accurately constraining SOA yields from NO3 oxidation, which vary substantially with the volatile organic compound precursor, is essential in predicting nighttime aerosol production.

A comparison of secondary organic aerosol (SOA) yields and composition from ozonolysis of monoterpenes at varying concentrations of NO2

NASA Astrophysics Data System (ADS)

Draper, D. C.; Farmer, D. K.; Desyaterik, Y.; Fry, J. L.

2015-05-01

The effect of NO2 on secondary organic aerosol (SOA) formation from ozonolysis of α-pinene, β-pinene, Δ3-carene, and limonene was investigated using a dark flow-through reaction chamber. SOA mass yields were calculated for each monoterpene from ozonolysis with varying NO2 concentrations. Kinetics modeling of the first generation gas-phase chemistry suggests that differences in observed aerosol yields for different NO2 concentrations are consistent with NO3 formation and subsequent competition between O3 and NO3 to oxidize each monoterpene. α-pinene was the only monoterpene studied that showed a systematic decrease in both aerosol number concentration and mass concentration with increasing [NO2]. β-pinene and Δ3-carene produced fewer particles at higher [NO2], but both retained moderate mass yields. Limonene exhibited both higher number concentrations and greater mass concentrations at higher [NO2]. SOA from each experiment was collected and analyzed by HPLC-ESI-MS, enabling comparisons between product distributions for each system. In general, the systems influenced by NO3 oxidation contained more high molecular weight products (MW >400 amu), suggesting the importance of oligomerization mechanisms in NO3-initiated SOA formation. α-pinene, which showed anomalously low aerosol mass yields in the presence of NO2, showed no increase in these oligomer peaks, suggesting that lack of oligomer formation is a likely cause of α-pinene's near 0% yields with NO3. Through direct comparisons of mixed-oxidant systems, this work suggests that NO3 is likely to dominate nighttime oxidation pathways in most regions with both biogenic and anthropogenic influences. Therefore, accurately constraining SOA yields from NO3 oxidation, which vary substantially with the VOC precursor, is essential in predicting nighttime aerosol production.

Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-04-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We model the observed ultrafine aerosol growth with a simplified scheme approximating the condensing species as a mixture of effectively non-volatile and semi-volatile species, demonstrate that state-of-the-art organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We find that roughly half of the mass of the condensing mass needs to be distributed proportional to the aerosol surface area (thus implying that the condensation is governed by gas-phase concentration rather than the equilibrium vapour pressure) to explain the observed aerosol growth. We demonstrate the large sensitivity of predicted number concentrations of cloud condensation nuclei (CCN) to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J. C.; Sodeau, J. R.; Healy, R. M.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; O'Dowd, C. D.

2009-12-01

As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the NE Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Black carbon concentrations in polluted air were between 300-400 ng m-3, and in clean marine air were less than 50 ng m-3. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water

Satellite measurement of aerosol mass over land

NASA Technical Reports Server (NTRS)

Fraser, R. S.; Kaufman, Y. J.; Mahoney, R. L.

1984-01-01

The estimation of aerosol optical thickness and mass from satellite observations over land is demonstrated using data from the GOES Visible/IR Spin-Scan Radiometer for the eastern U.S. The post-launch calibration technique is described; the algorithm used to derive optical thickness from the radiance of scattered sunlight (by means of a radiative-transfer model in which the optical characteristics of the aerosol are assumed) is presented; and data on aerosol S for July 31, 1980 are analyzed. The results are presented in a series of graphs and maps and compared with ground-based data. The errors in the optical thickness and columnar mass are estimated as 15 and 40 percent, respectively, and the need for independent-data-set validation of satellite-based mass, transport, and divergence values is indicated.

Electrospray ionizer for mass spectrometry of aerosol particles

DOEpatents

He, Siqin; Hogan, Chris; Li, Lin; Liu, Benjamin Y. H.; Naqwi, Amir; Romay, Francisco

2017-09-19

A device and method are disclosed to apply ESI-based mass spectroscopy to submicrometer and nanometer scale aerosol particles. Unipolar ionization is utilized to charge the particles in order to collect them electrostatically on the tip of a tungsten rod. Subsequently, the species composing the collected particles are dissolved by making a liquid flow over the tungsten rod. This liquid with dissolved aerosol contents is formed into highly charged droplets, which release unfragmented ions for mass spectroscopy, such as time-of-flight mass spectroscopy. The device is configured to operate in a switching mode, wherein aerosol deposition occurs while solvent delivery is turned off and vice versa.

Derivation of Aerosol Columnar Mass from MODIS Optical Depth

NASA Technical Reports Server (NTRS)

Gasso, Santiago; Hegg, Dean A.

2003-01-01

In order to verify performance, aerosol transport models (ATM) compare aerosol columnar mass (ACM) with those derived from satellite measurements. The comparison is inherently indirect since satellites derive optical depths and they use a proportionality constant to derive the ACM. Analogously, ATMs output a four dimensional ACM distribution and the optical depth is linearly derived. In both cases, the proportionality constant requires a direct intervention of the user by prescribing the aerosol composition and size distribution. This study introduces a method that minimizes the direct user intervention by making use of the new aerosol products of MODIS. A parameterization is introduced for the derivation of columnar aerosol mass (AMC) and CCN concentration (CCNC) and comparisons between sunphotometer, MODIS Airborne Simulator (MAS) and in-measurements are shown. The method still relies on the scaling between AMC and optical depth but the proportionality constant is dependent on the MODIS derived r$_{eff}$,\\eta (contribution of the accumulation mode radiance to the total radiance), ambient RH and an assumed constant aerosol composition. The CCNC is derived fkom a recent parameterization of CCNC as a function of the retrieved aerosol volume. By comparing with in-situ data (ACE-2 and TARFOX campaigns), it is shown that retrievals in dry ambient conditions (dust) are improved when using a proportionality constant dependent on r$ {eff}$ and \\eta derived in the same pixel. In high humidity environments, the improvement inthe new method is inconclusive because of the difficulty in accounting for the uneven vertical distribution of relative humidity. Additionally, two detailed comparisons of AMC and CCNC retrieved by the MAS algorithm and the new method are shown. The new method and MAS retrievals of AMC are within the same order of magnitude with respect to the in-situ measurements of aerosol mass. However, the proposed method is closer to the in-situ measurements than

Steady increase of secondary organic aerosol mass concentration and light extinction during the CARES 2010 Field Campaign

NASA Astrophysics Data System (ADS)

Gyawali, M. S.; Arnott, W. P.; Flowers, B. A.; Dubey, M. K.; Atkinson, D. B.; Song, C.; Zaveri, R. A.; Setyan, A.; Zhang, Q.; Mazzoleni, C.; Gorkowski, K.

2011-12-01

We present multispectral (355, 375, 405, 532, 870, 781, and 1047 nm) aerosol light absorption and scattering measurements for the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) campaign in Sacramento, CA and the Sierra Nevada foothills. The short wavelength scattering at both sites gradually increased during the last 10 days of the campaign as diagnosed by a systematic increase in the Ångström exponent of scattering. The UV and near UV enhanced scattering was likely a consequence of the ultra and sub-micron aerosol which began to grow vigorously in the size range where scattering at shorter wavelengths begins to increase. Multispectral aerosol light absorption coefficients suggest the absence of short wavelength light absorption by brown carbon. Aerosol mass spectrometer data also shows the steady increase of secondary organic aerosol during the last 10 days of CARES. The time series of the measurements made between the two sites (T0 and T1) separated by the slope of the foothills are strikingly similar, except for isolated night time episodes of enhanced absorption at T0. This is possibly due to paving events or other nocturnal emissions markers

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

Particle deposition in human respiratory system: deposition of concentrated hygroscopic aerosols.

PubMed

Varghese, Suresh K; Gangamma, S

2009-06-01

In the nearly saturated human respiratory tract, the presence of water-soluble substances in the inhaled aerosols can cause change in the size distribution of the particles. This consequently alters the lung deposition profiles of the inhaled airborne particles. Similarly, the presence of high concentration of hygroscopic aerosols also affects the water vapor and temperature profiles in the respiratory tract. A model is presented to analyze these effects in human respiratory system. The model solves simultaneously the heat and mass transfer equations to determine the size evolution of respirable particles and gas-phase properties within human respiratory tract. First, the model predictions for nonhygroscopic aerosols are compared with experimental results. The model results are compared with experimental results of sodium chloride particles. The model reproduces the major features of the experimental data. The water vapor profile is significantly modified only when a high concentration of particles is present. The model is used to study the effect of equilibrium assumptions on particle deposition. Simulations show that an infinite dilution solution assumption to calculate the saturation equilibrium over droplet could induce errors in estimating particle growth. This error is significant in the case of particles of size greater than 1 mum and at number concentrations higher than 10(5)/cm(3).

Development and characterization of an aircraft aerosol time-of-flight mass spectrometer.

PubMed

Pratt, Kerri A; Mayer, Joseph E; Holecek, John C; Moffet, Ryan C; Sanchez, Rene O; Rebotier, Thomas P; Furutani, Hiroshi; Gonin, Marc; Fuhrer, Katrin; Su, Yongxuan; Guazzotti, Sergio; Prather, Kimberly A

2009-03-01

Vertical and horizontal profiles of atmospheric aerosols are necessary for understanding the impact of air pollution on regional and global climate. To gain further insight into the size-resolved chemistry of individual atmospheric particles, a smaller aerosol time-of-flight mass spectrometer (ATOFMS) with increased data acquisition capabilities was developed for aircraft-based studies. Compared to previous ATOFMS systems, the new instrument has a faster data acquisition rate with improved ion transmission and mass resolution, as well as reduced physical size and power consumption, all required advances for use in aircraft studies. In addition, real-time source apportionment software allows the immediate identification and classification of individual particles to guide sampling decisions while in the field. The aircraft (A)-ATOFMS was field-tested on the ground during the Study of Organic Aerosols in Riverside, CA (SOAR) and aboard an aircraft during the Ice in Clouds Experiment-Layer Clouds (ICE-L). Initial results from ICE-L represent the first reported aircraft-based single-particle dual-polarity mass spectrometry measurements and provide an increased understanding of particle mixing state as a function of altitude. Improved ion transmission allows for the first single-particle detection of species out to approximately m/z 2000, an important mass range for the detection of biological aerosols and oligomeric species. In addition, high time resolution measurements of single-particle mixing state are demonstrated and shown to be important for airborne studies where particle concentrations and chemistry vary rapidly.

Aerosols in polluted versus nonpolluted air masses Long-range transport and effects on clouds

NASA Technical Reports Server (NTRS)

Pueschel, R. F.; Van Valin, C. C.; Castillo, R. C.; Kadlecek, J. A.; Ganor, E.

1986-01-01

To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United States, aerosol and cloud-drop size distributions, elemental composition of aerosols as a function of size, and ionic content of cloud water were measured on Whiteface Mountain, NY, during the summers of 1981 and 1982. In several case studies, the data were cross-correlated with different air mass types - background continental, polluted continental, and maritime - that were advected to the sampling site. The results are the following: (1) Anthropogenic sources hundreds of kilometers upwind cause the small-particle (accumulation) mode number to increase from hundreds of thousands per cubic centimeter and the mass loading to increase from a few to several tens of micrograms per cubic meter, mostly in the form of sulfur aerosols. (2) A significant fraction of anthropogenic sulfur appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (3) Clouds in Atlantic maritime air masses have cloud drop spectra that are markedly different from those measured in continental clouds. The drop concentration is significantly lower, and the drop size spectra are heavily skewed toward large drops. (4) Effects of anthropogenic pollutants on cloud water ionic composition are an increase of nitrate by a factor of 50, an increase of sulfate by more than one order of magnitude, and an increase of ammonium ion by a factor of 7. The net effect of the changes in ionic concentrations is an increase in cloud water acidity. An anion deficit even in maritime clouds suggests an unknown, possibly biogenic, source that could be responsible for a pH below neutral, which is frequently observed in nonpolluted clouds.

Vertical profile of elemental concentrations in aerosol particles in the Bermuda area during GCE/CASE/WATOX

NASA Astrophysics Data System (ADS)

Ennis, G.; Sievering, H.

1990-06-01

During the 1988 Global Change Expedition/Coordinated Air-Sea Experiment/Western Atlantic Ocean Experiment (GCE/CASE/WATOX) joint effort, research was conducted to determine elemental concentrations in atmospheric aerosol particles near Bermuda, to construct a three-level (15, 150, and 2600 m ASL) vertical profile of these concentrations, and to ascertain the source of the particles. Samples were collected by the NOAA King Air aircraft and NOAA ship Mt. Mitchell on July 24-28, 1988. Concentration determinations were made for 16 elements through the use of an X ray fluorescence instrument designed for analysis of small-mass samples. A layering effect was found; concentrations of several elements at 150 m were more than twice their respective concentrations at 15 m and 2600 m. Enrichment factors, V/Mn ratio, and correlations between concentrations suggest a Saharan mineral source, despite air mass back trajectories that show no direct continental input for up to 10 days prior to sample collection. Estimated total mineral aerosol concentrations at 15 m, 150 m, and 2600 m are 1.5, 4.1, and 2.1 μg m-3.

Spatial variability of aerosol and black carbon concentrations in the troposphere of the Russian Arctic

NASA Astrophysics Data System (ADS)

Kozlov, Valerii S.; Panchenko, Mikhail V.; Paris, Jean D.; Nédéléc, Philippe; Chernov, Dmitry G.; Shmargunov, Vladimir P.

2015-11-01

A cycle of flights of the Optik TU-134 Flying Laboratory of IAO SB RAS over regions of Western Siberia and the Russian Arctic (55.0-74.8°N, 61.3-82.9°E) was carried out on October 15-17 of 2014 within the framework of the YAK-AEROSIB Russian—French Project. The mass concentrations of submicron aerosol and Black Carbon (BC) in the troposphere up to a height of 8.5 km were measured in the flights. The ranges of variability were 0.3-20 μg/m3 for the aerosol concentration and 0.02-1 μg/m3 for the BC concentration. In the subpolar latitudes of 71-74.8°N, the lower levels of aerosol (0.8-6 μg/m3) and BC (0.02-0.3 μg/m3) were observed. The comparison of the results of airborne sensing in 2008 and 2014 has shown that in the Western Subartic the aerosol and BC concentrations in the vertical profiles up to six times exceeded those observed in the Eastern Subarctic (0.3-1 μg/m3 and 10-50 ng/m3). The excess of the mean integral BC concentrations and the aerosol optical depth was, on average, 2-2.5 times (0.16 mg/m2; 0.02). In the region of the Kara Sea at heights of 0.5-2 and 4-6 km, the excess of the aerosol content in the western sector in comparison with the eastern one was, on average, 2 times, while for the black carbon the excess achieved 7 times at heights of 1-2 km (0.25- 0.035 μg/m3). The mean integral concentrations of aerosol and black carbon ˜ 1.3 times exceeded those in the clearer eastern region of the sea (0.31 mg/m2; 0.049). The obtained estimates indicate the decrease of the aerosol and BC concentrations in the subpolar latitudes of the Russian Federation from the west to the east.

Characterizing aerosol transport into the Canadian High Arctic using aerosol mass spectrometry and Lagrangian modelling

NASA Astrophysics Data System (ADS)

Kuhn, T.; Damoah, R.; Bacak, A.; Sloan, J. J.

2010-05-01

We report the analysis of measurements made using an aerosol mass spectrometer (AMS; Aerodyne Research Inc.) that was installed in the Polar Environment Atmospheric Research Laboratory (PEARL) in summer 2006. PEARL is located in the Canadian high Arctic at 610 m above sea level on Ellesmere Island (80° N 86° W). PEARL is unique for its remote location in the Arctic and because most of the time it is situated within the free troposphere. It is therefore well suited as a receptor site to study the long range tropospheric transport of pollutants into the Arctic. Some information about the successful year-round operation of an AMS at a high Arctic site such as PEARL will be reported here, together with design considerations for reliable sampling under harsh low-temperature conditions. Computational fluid dynamics calculations were made to ensure that sample integrity was maintained while sampling air at temperatures that average -40 °C in the winter and can be as low as -55 °C. Selected AMS measurements of aerosol mass concentration, size, and chemical composition recorded during the months of August, September and October 2006 will be reported. During this period, sulfate was at most times the predominant aerosol component with on average 0.115 μg m-3 (detection limit 0.003 μg m-3). The second most abundant component was undifferentiated organic aerosol, with on average 0.11 μg m-3 detection limit (0.04 μg m-3). The nitrate component, which averaged 0.007 μg m-3, was above its detection limit (0.002 μg m-3), whereas the ammonium ion had an apparent average concentration of 0.02 μg m-3, which was approximately equal to its detection limit. A few episodes having increased mass concentrations and lasting from several hours to several days are apparent in the data. These were investigated further using a statistical analysis to determine their common characteristics. High correlations among some of the components arriving during the short term episodes provide

Real-time analysis of ambient organic aerosols using aerosol flowing atmospheric-pressure afterglow mass spectrometry (AeroFAPA-MS)

NASA Astrophysics Data System (ADS)

Brüggemann, Martin; Karu, Einar; Stelzer, Torsten; Hoffmann, Thorsten

2015-04-01

Organic aerosol accounts for a major fraction of atmospheric aerosols and has implications on the earth's climate and human health. However, due to the chemical complexity its measurement remains a major challenge for analytical instrumentation.1 Here, we present the development, characterization and application of a new soft ionization technique that allows mass spectrometric real-time detection of organic compounds in ambient aerosols. The aerosol flowing atmospheric-pressure afterglow (AeroFAPA) ion source utilizes a helium glow discharge plasma to produce excited helium species and primary reagent ions. Ionization of the analytes occurs in the afterglow region after thermal desorption and results mainly in intact molecular ions, facilitating the interpretation of the acquired mass spectra. In the past, similar approaches were used to detect pesticides, explosives or illicit drugs on a variety of surfaces.2,3 In contrast, the AeroFAPA source operates 'online' and allows the detection of organic compounds in aerosols without a prior precipitation or sampling step. To our knowledge, this is the first application of an atmospheric-pressure glow discharge ionization technique to ambient aerosol samples. We illustrate that changes in aerosol composition and concentration are detected on the time scale of seconds and in the ng-m-3 range. Additionally, the successful application of AeroFAPA-MS during a field study in a mixed forest region in Central Europe is presented. Several oxidation products of monoterpenes were clearly identified using the possibility to perform tandem MS experiments. The acquired data are in agreement with previous studies and demonstrate that AeroFAPA-MS is a suitable tool for organic aerosol analysis. Furthermore, these results reveal the potential of this technique to enable new insights into aerosol formation, growth and transformation in the atmosphere. References: 1) IPCC, 2013: Summary for Policymakers. In: Climate Change 2013: The

Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO 3 − aerosol during the 2013 Southern Oxidant and Aerosol Study

DOE PAGES

Allen, H. M.; Draper, D. C.; Ayres, B. R.; ...

2015-09-25

Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO 3 −) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na + and Ca 2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms bymore » multiphase reactions of HNO 3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH 4NO 3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. In addition, calculation of the rate of the heterogeneous uptake of HNO 3 on mineral aerosol supports the conclusion that aerosol NO 3 − is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO 3 − and HNO 3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.« less

Reactions and mass spectra of complex particles using Aerosol CIMS

NASA Astrophysics Data System (ADS)

Hearn, John D.; Smith, Geoffrey D.

2006-12-01

Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

Mass-spectrometric identification of primary biological particle markers: indication for low abundance of primary biological material in the pristine submicron aerosol of Amazonia

NASA Astrophysics Data System (ADS)

Schneider, J.; Freutel, F.; Zorn, S. R.; Chen, Q.; Farmer, D. K.; Jimenez, J. L.; Martin, S. T.; Artaxo, P.; Wiedensohler, A.; Borrmann, S.

2011-07-01

The abundance of marker compounds for primary biological particles in submicron aerosol was investigated by means of aerosol mass spectrometry. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker peaks were identified. The identified marker peaks were compared with mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the Central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker peaks places upper limits of 7.5 % for amino acids and 5.6 % for carbohydrates on the contribution of primary biological aerosol particles (PBAPs) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m-3. Carbohydrates and protein amino acids make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAPs mass fraction of about 20 % to the submicron organic aerosol.

Spatial and temporal variations of aerosols around Beijing in summer 2006: 2. Local and column aerosol optical properties

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

Matsui, Hitoshi; Koike, Makoto; Kondo, Yutaka

Weather Research and Forecasting (WRF)-chem model calculations were conducted to study aerosol optical properties around Beijing, China, during the Campaign of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006) period. In this paper, we interpret aerosol optical properties in terms of aerosol mass concentrations and their chemical compositions by linking model calculations with measurements. In general, model calculations reproduced observed features of spatial and temporal variations of various surface and column aerosol optical parameters in and around Beijing. Spatial and temporal variations of aerosol absorption, scattering, and extinction coefficient corresponded well to those of elemental carbon (primary aerosol),more » sulfate (secondary aerosol), and the total aerosol mass concentration, respectively. These results show that spatial and temporal variations of the absorption coefficient are controlled by local emissions (within 100 km around Beijing during the preceding 24 h), while those of the scattering coefficient are controlled by regional-scale emissions (within 500 km around Beijing during the preceding 3 days) under synoptic-scale meteorological conditions, as discussed in our previous study of aerosol mass concentration. Vertical profiles of aerosol extinction revealed that the contribution of secondary aerosols and their water uptake increased with altitude within the planetary boundary layer, leading to a considerable increase in column aerosol optical depth (AOD) around Beijing. These effects are the main factors causing differences in regional and temporal variations between particulate matter (PM) mass concentration at the surface and column AOD over a wide region in the northern part of the Great North China Plain.« less

Precipitation effects on aerosol concentration in the background EMEP station of Zarra (Valencia), Spain

NASA Astrophysics Data System (ADS)

Calvo, Ana Isabel; San Martín, Isabel; Castro, Amaya; Alonso-Blanco, Elisabeth; Alves, Célia; Duarte, Márcio; Fernández-González, Sergio; Fraile, Roberto

2014-05-01

Aerosols and precipitation are closely related, presenting a bidirectional influence and constituting an important source of uncertainties on climate change studies. However, they are usually studied independently and in general are only linked to one another for the development or validation of cloud models. The primary and secondary pollutants may be removed by wet and dry deposition. Wet deposition, including in-cloud and below-cloud scavenging processes, can efficiently remove atmospheric aerosols and it is considered a critical process for determining aerosol concentrations in the atmosphere. In this study, aerosols and precipitation data from a background Spanish EMEP (Cooperative Programme for the Monitoring and Evaluation of Long Range Transmission of Air Pollutants in Europe) station located in Zarra, Valencia (Spain) were analyzed (1° 06' W and 39° 05' N, 885 m asl). The effect of precipitation on aerosol concentration was studied and the correlation between the intensity of precipitation and scavenging effect was investigated. In order to evaluate the effects of precipitation on different aerosol size ranges three different aerosol fractions were studied: PM10, PM10-2.5 and PM2.5. In order to eliminate the influence of the air mass changes, only the days in which the air mass of the precipitation day and the previous day had the same origin were considered. Thus, from a total of 3586 rainy days registered from March 2001 to December 2010, 34 precipitation days satisfied this condition and were analyzed. During the period of study, daily precipitation ranged between 0.2 and 28.8 mm, with a mean value of 4 mm. Regarding the origin of the air masses, those from west were dominant at the three height levels investigated (500, 1500 and 3000 m). In order to obtain additional information, aerosol and precipitation chemical composition were also studied in relation to the days of precipitation and the previous days. Furthermore, in order to identify the type

Dust mass concentrations from the UK volcanic ash lidar network compared with in-situ aircraft measurements

NASA Astrophysics Data System (ADS)

Osborne, Martin; Marenco, Franco; Adam, Mariana; Buxmann, Joelle; Haywood, Jim

2018-04-01

The Met Office has recently established a series of 10 lidar / sun-photometer installations across the UK, consolidating their ash / aerosol remote sensing capabilities [1]. In addition to this network, the Met Office have acquired the Civil Contingency Aircraft (MOCCA) which allows airborne in-situ measurements of ash / aerosol scattering and size-distributions. Two case studies are presented in which mass concentrations of Saharan dust are obtained remotely using lidar returns, and are then compared with those obtained in-situ. A thorough analysis of the mass concentration uncertainty will be provided at the conference.

New insights into modeling an organic mass fraction of sea spray aerosol

NASA Astrophysics Data System (ADS)

Meskhidze, N.; Gantt, B.

2010-12-01

As the study of climate change progresses, a need to separate the effects of natural and anthropogenic processes becomes essential in order to correctly forecast the future climate. Due to their massive source regions underlying an atmosphere with low aerosol concentration, marine aerosols derived from sea spray and ocean emitted biogenic volatile organic compounds (BVOCs) are extremely important for the Earth’s radiative budget, regional air quality and biogeochemical cycling of elements. Measurements of freshly-emitted sea spray have revealed that bubble bursting processes, largely responsible for the production of sea salt aerosol, also control sea-to-air transfer of marine organic matter. It has been established that the organic mass fraction of sea spray can be a function of sea-water composition (e.g., concentrations of Chlorophyll-a, [Chl-a], dissolved organic carbon, [DOC], particulate organic carbon, [POC], types of organic carbon, and the amount of surfactants). Current paramaterizations of marine primary organic aerosol emissions use remotely sensed [Chl-a] data as a proxy for oceanic biological activity. However, it has also been shown that the path length, size, and lifetime of bubbles in seawater as well as spatial coverage of seawater surface by streaks or slicks (visible film of a roughly 50 μm thick layer, highly enriched in organics) can have dramatic effect on organic mass fraction of sea spray (OCss). Dynamics of bubble entrainment and the level of microlayer enrichment by organics relative to the underlying bulk water can be controlled by surface wind speed. For bubble entrainment, high winds can increase rising bubble path length and therefore the amount of organics scavenged by the bubble. However, when the surface wind speeds exceed 8 m s-1 breaking of ocean waves can entirely destroy surface organic films and diminish the amount of organics leaving the sea. Despite the probable impact of wind speed, existing parameterizations do not

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

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

Organosulfates and organic acids in Arctic aerosols: speciation, annual variation and concentration levels

NASA Astrophysics Data System (ADS)

Hansen, A. M. K.; Kristensen, K.; Nguyen, Q. T.; Zare, A.; Cozzi, F.; Nøjgaard, J. K.; Skov, H.; Brandt, J.; Christensen, J. H.; Ström, J.; Tunved, P.; Krejci, R.; Glasius, M.

2014-02-01

Sources, composition and occurrence of secondary organic aerosols (SOA) in the Arctic were investigated at Zeppelin Mountain, Svalbard, and Station Nord, northeast Greenland, during the full annual cycle of 2008 and 2010 respectively. We focused on the speciation of three types of SOA tracers: organic acids, organosulfates and nitrooxy organosulfates from both anthropogenic and biogenic precursors, here presenting organosulfate concentrations and compositions during a full annual cycle and chemical speciation of organosulfates in Arctic aerosols for the first time. Aerosol samples were analysed using High Performance Liquid Chromatography coupled to a quadrupole Time-of-Flight mass spectrometer (HPLC-q-TOF-MS). A total of 11 organic acids (terpenylic acid, benzoic acid, phthalic acid, pinic acid, suberic acid, azelaic acid, adipic acid, pimelic acid, pinonic acid, diaterpenylic acid acetate (DTAA) and 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA)), 12 organosulfates and one nitrooxy organosulfate were identified at the two sites. Six out of the 12 organosulfates are reported for the first time. Concentrations of organosulfates follow a distinct annual pattern at Station Nord, where high concentration were observed in late winter and early spring, with a mean total concentration of 47 (±14) ng m-3, accounting for 7 (±2)% of total organic matter, contrary to a considerably lower organosulfate mean concentration of 2 (±3) ng m-3 (accounting for 1 (±1)% of total organic matter) observed during the rest of the year. The organic acids followed the same temporal trend as the organosulfates at Station Nord; however the variations in organic acid concentrations were less pronounced, with a total mean organic acid concentration of 11.5 (±4) ng m-3 (accounting for 1.7 (±0.6)% of total organic matter) in late winter and early spring, and 2.2 (±1) ng m-3 (accounting for 0.9 (±0.4)% of total organic matter) during the rest of the year. At Zeppelin Mountain

Trends in sulfate and organic aerosol mass in the Southeast U.S.: Impact on aerosol optical depth and radiative forcing

NASA Astrophysics Data System (ADS)

Attwood, A. R.; Washenfelder, R. A.; Brock, C. A.; Hu, W.; Baumann, K.; Campuzano-Jost, P.; Day, D. A.; Edgerton, E. S.; Murphy, D. M.; Palm, B. B.; McComiskey, A.; Wagner, N. L.; Sá, S. S.; Ortega, A.; Martin, S. T.; Jimenez, J. L.; Brown, S. S.

2014-11-01

Emissions of SO2 in the United States have declined since the early 1990s, resulting in a decrease in aerosol sulfate mass in the Southeastern U.S. of -4.5(±0.9)% yr-1 between 1992 and 2013. Organic aerosol mass, the other major aerosol component in the Southeastern U.S., has decreased more slowly despite concurrent emission reductions in anthropogenic precursors. Summertime measurements in rural Alabama quantify the change in aerosol light extinction as a function of aerosol composition and relative humidity. Application of this relationship to composition data from 2001 to 2013 shows that a -1.1(±0.7)% yr-1 decrease in extinction can be attributed to decreasing aerosol water mass caused by the change in aerosol sulfate/organic ratio. Calculated reductions in extinction agree with regional trends in ground-based and satellite-derived aerosol optical depth. The diurnally averaged summertime surface radiative effect has changed by 8.0 W m-2, with 19% attributed to the decrease in aerosol water.

Estimation of surface-level PM concentration based on aerosol type classification and near-surface AOD over Korea

NASA Astrophysics Data System (ADS)

Kim, Kwanchul; Noh, Youngmin; Lee, Kwon H.

2016-04-01

Surface-level PM distribution was estimated from the satellite aerosol optical depth (AOD) products, taking the account of aerosol type classification and near-surface AOD over Jeju, Korea. For this purpose, data from various instruments such as satellites, sunphotometer, and Micro-pulse Lidar (MPL) was used during March 2008 and October 2009. Initial analyses of comparison with sunphotometer AOD and PM concentration showed some relatively poor relationship over Jeju, Korea. Since the AERONET L2 data has significant number of observations with high AOT values paired to low surface-level PM values, which were believed to be the effect of long-rage transport aerosols like as Asian dust and biomass burning. Stronger correlations (exceeding R = 0.8) were obtained by screening long-rage transport aerosols and calculating near-surface AOT considering aerosol profiles data from MPL and HYSPLIT air mass trajectory. The relationship found between corrected satellite observed AOD and surface-level PM concentration over Jeju is very similar. An approach to reduce the discrepancy between satellite observed AOD and PM concentration is demonstrated by tuning thresholds used to detect aerosol type from sunphotometer inversion data. Finally, the satellite observed AOD-surface PM concentration correlation is significantly improved. Our study clearly demonstrates that satellite observed AOD is a good surrogate for monitoring PM air quality over Korea.

Variability of aerosol, gaseous pollutants and meteorological characteristics associated with changes in air mass origin 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.

2012-04-01

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 (NR-PM1) 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

Sensitive Detection and Identification of Isovanillin Aerosol Particles at the pg/cm3 Mass Concentration Level using Raman Spectroscopy

DTIC Science & Technology

2017-04-24

Spectroscopy * R. L. Aggarwal1, S. Di Cecca, L. W. Farrar, Shabshelowitz, A...Public Release A compact Raman spectroscopy system with high sensitivity to chemical aerosols has been developed. This system has been used to...this represents the lowest chemical aerosol concentration and signal integration period product ever reported for a Raman spectroscopy system.

Modelling organic aerosol concentrations and properties during ChArMEx summer campaigns of 2012 and 2013 in the western Mediterranean region

NASA Astrophysics Data System (ADS)

Chrit, Mounir; Sartelet, Karine; Sciare, Jean; Pey, Jorge; Marchand, Nicolas; Couvidat, Florian; Sellegri, Karine; Beekmann, Matthias

2017-10-01

In the framework of the Chemistry-Aerosol Mediterranean Experiment, a measurement site was set up at a remote site (Ersa) on Corsica Island in the northwestern Mediterranean Sea. Measurement campaigns performed during the summers of 2012 and 2013 showed high organic aerosol concentrations, mostly from biogenic origin. This work aims to represent the organic aerosol concentrations and properties (oxidation state and hydrophilicity) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Biogenic precursors are isoprene, monoterpenes and sesquiterpenes. In this work, the following model oxidation products of monoterpenes are added: (i) a carboxylic acid (MBTCA) to represent multi-generation oxidation products in the low-NOx regime, (ii) organic nitrate chemistry and (iii) extremely low-volatility organic compounds (ELVOCs) formed by ozonolysis. The model shows good agreement of measurements of organic concentrations for both 2012 and 2013 summer campaigns. The modelled oxidation property and hydrophilic organic carbon properties of the organic aerosols also agree reasonably well with the measurements. The influence of the different chemical processes added to the model on the oxidation level of organics is studied. Measured and simulated water-soluble organic carbon (WSOC) concentrations show that even at a remote site next to the sea, about 64 % of the organic carbon is soluble. The concentrations of WSOC vary with the origins of the air masses and the composition of organic aerosols. The marine organic emissions only contribute to a few percent of the organic mass in PM1, with maxima above the sea.

Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign

NASA Technical Reports Server (NTRS)

DeCarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.;

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

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).

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

Winter monsoon variability and its impact on aerosol concentrations in East Asia.

PubMed

Jeong, Jaein I; Park, Rokjin J

2017-02-01

We investigate the relationship between winter aerosol concentrations over East Asia and variability in the East Asian winter monsoon (EAWM) using GEOS-Chem 3-D global chemical transport model simulations and ground-based aerosol concentration data. We find that both observed and modeled surface aerosol concentrations have strong relationships with the intensity of the EAWM over northern (30-50°N, 100-140°E) and southern (20-30°N, 100-140°E) East Asia. In strong winter monsoon years, compared to weak winter monsoon years, lower and higher surface PM 2.5 concentrations by up to 25% are shown over northern and southern East Asia, respectively. Analysis of the simulated results indicates that the southward transport of aerosols is a key process controlling changes in aerosol concentrations over East Asia associated with the EAWM. Variability in the EAWM is found to play a major role in interannual variations in aerosol concentrations; consequently, changes in the EAWM will be important for understanding future changes in wintertime air quality over East Asia. Copyright © 2016 Elsevier Ltd. All rights reserved.

Long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Xu, J.; Zhang, X.; Liu, Y.; Shichang, K.; Ma, Y.

2017-12-01

An intensive measurement was conducted at a remote, background, and high-altitude site (Qomolangma station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from April 12 to May 12, 2016 to chemically characterize high time-resolved submicron particulate matter (PM1) and obtain the influence of biomass burning emissions to the Himalayas, frequently transported from south Asia during pre-monsoon season. Two high aerosol loading periods were observed during the study. Overall, the average (± 1σ) PM1 mass concentration was 4.44 (± 4.54) µg m-3 for the entire study, comparable with those observed at other remote sites worldwide. Organic aerosols (OA) was the dominant PM1 species (accounting for 54.3% of total PM1 mass on average) and its contribution increased with the increase of total PM1 mass loading. The average size distributions of PM1 species all peaked at an overlapping accumulation mode ( 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transportations. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a biomass burning related OA (BBOA, 43.7%) and two oxygenated OA (Local-OOA and LRT-OOA; 13.9% and 42.4%) represented sources from local emissions and long-range transportations, respectively. Two polluted air mass origins (generally from the west and southwest of QOMS) and two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions were observed, respectively, suggesting the important sources of wildfires from south Asia. One of polluted aerosol plumes was investigated in detail to illustrate the evolution of aerosol characteristics at QOMS driving by different impacts of wildfires, air mass origins, meteorological conditions and

Whole-body nanoparticle aerosol inhalation exposures.

PubMed

Yi, Jinghai; Chen, Bean T; Schwegler-Berry, Diane; Frazer, Dave; Castranova, Vince; McBride, Carroll; Knuckles, Travis L; Stapleton, Phoebe A; Minarchick, Valerie C; Nurkiewicz, Timothy R

2013-05-07

Inhalation is the most likely exposure route for individuals working with aerosolizable engineered nano-materials (ENM). To properly perform nanoparticle inhalation toxicology studies, the aerosols in a chamber housing the experimental animals must have: 1) a steady concentration maintained at a desired level for the entire exposure period; 2) a homogenous composition free of contaminants; and 3) a stable size distribution with a geometric mean diameter < 200 nm and a geometric standard deviation σg < 2.5 (5). The generation of aerosols containing nanoparticles is quite challenging because nanoparticles easily agglomerate. This is largely due to very strong inter-particle forces and the formation of large fractal structures in tens or hundreds of microns in size (6), which are difficult to be broken up. Several common aerosol generators, including nebulizers, fluidized beds, Venturi aspirators and the Wright dust feed, were tested; however, none were able to produce nanoparticle aerosols which satisfy all criteria (5). A whole-body nanoparticle aerosol inhalation exposure system was fabricated, validated and utilized for nano-TiO2 inhalation toxicology studies. Critical components: 1) novel nano-TiO2 aerosol generator; 2) 0.5 m(3) whole-body inhalation exposure chamber; and 3) monitor and control system. Nano-TiO2 aerosols generated from bulk dry nano-TiO2 powders (primary diameter of 21 nm, bulk density of 3.8 g/cm(3)) were delivered into the exposure chamber at a flow rate of 90 LPM (10.8 air changes/hr). Particle size distribution and mass concentration profiles were measured continuously with a scanning mobility particle sizer (SMPS), and an electric low pressure impactor (ELPI). The aerosol mass concentration (C) was verified gravimetrically (mg/m(3)). The mass (M) of the collected particles was determined as M = (Mpost-Mpre), where Mpre and Mpost are masses of the filter before and after sampling (mg). The mass concentration was calculated as C = M

Whole-Body Nanoparticle Aerosol Inhalation Exposures

PubMed Central

Yi, Jinghai; Chen, Bean T.; Schwegler-Berry, Diane; Frazer, Dave; Castranova, Vince; McBride, Carroll; Knuckles, Travis L.; Stapleton, Phoebe A.; Minarchick, Valerie C.; Nurkiewicz, Timothy R.

2013-01-01

Inhalation is the most likely exposure route for individuals working with aerosolizable engineered nano-materials (ENM). To properly perform nanoparticle inhalation toxicology studies, the aerosols in a chamber housing the experimental animals must have: 1) a steady concentration maintained at a desired level for the entire exposure period; 2) a homogenous composition free of contaminants; and 3) a stable size distribution with a geometric mean diameter < 200 nm and a geometric standard deviation σg < 2.5 5. The generation of aerosols containing nanoparticles is quite challenging because nanoparticles easily agglomerate. This is largely due to very strong inter-particle forces and the formation of large fractal structures in tens or hundreds of microns in size 6, which are difficult to be broken up. Several common aerosol generators, including nebulizers, fluidized beds, Venturi aspirators and the Wright dust feed, were tested; however, none were able to produce nanoparticle aerosols which satisfy all criteria 5. A whole-body nanoparticle aerosol inhalation exposure system was fabricated, validated and utilized for nano-TiO2 inhalation toxicology studies. Critical components: 1) novel nano-TiO2 aerosol generator; 2) 0.5 m3 whole-body inhalation exposure chamber; and 3) monitor and control system. Nano-TiO2 aerosols generated from bulk dry nano-TiO2 powders (primary diameter of 21 nm, bulk density of 3.8 g/cm3) were delivered into the exposure chamber at a flow rate of 90 LPM (10.8 air changes/hr). Particle size distribution and mass concentration profiles were measured continuously with a scanning mobility particle sizer (SMPS), and an electric low pressure impactor (ELPI). The aerosol mass concentration (C) was verified gravimetrically (mg/m3). The mass (M) of the collected particles was determined as M = (Mpost-Mpre), where Mpreand Mpost are masses of the filter before and after sampling (mg). The mass concentration was calculated as C = M/(Q*t), where Q is

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

Organosulfates and organic acids in Arctic aerosols: speciation, annual variation and concentration levels

NASA Astrophysics Data System (ADS)

Hansen, A. M. K.; Kristensen, K.; Nguyen, Q. T.; Zare, A.; Cozzi, F.; Nøjgaard, J. K.; Skov, H.; Brandt, J.; Christensen, J. H.; Ström, J.; Tunved, P.; Krejci, R.; Glasius, M.

2014-08-01

Sources, composition and occurrence of secondary organic aerosols in the Arctic were investigated at Zeppelin Mountain, Svalbard, and Station Nord, northeastern Greenland, during the full annual cycle of 2008 and 2010, respectively. Speciation of organic acids, organosulfates and nitrooxy organosulfates - from both anthropogenic and biogenic precursors were in focus. A total of 11 organic acids (terpenylic acid, benzoic acid, phthalic acid, pinic acid, suberic acid, azelaic acid, adipic acid, pimelic acid, pinonic acid, diaterpenylic acid acetate and 3-methyl-1,2,3-butanetricarboxylic acid), 12 organosulfates and 1 nitrooxy organosulfate were identified in aerosol samples from the two sites using a high-performance liquid chromatograph (HPLC) coupled to a quadrupole Time-of-Flight mass spectrometer. At Station Nord, compound concentrations followed a distinct annual pattern, where high mean concentrations of organosulfates (47 ± 14 ng m-3) and organic acids (11.5 ± 4 ng m-3) were observed in January, February and March, contrary to considerably lower mean concentrations of organosulfates (2 ± 3 ng m-3) and organic acids (2.2 ± 1 ng m-3) observed during the rest of the year. At Zeppelin Mountain, organosulfate and organic acid concentrations remained relatively constant during most of the year at a mean concentration of 15 ± 4 ng m-3 and 3.9 ± 1 ng m-3, respectively. However during four weeks of spring, remarkably higher concentrations of total organosulfates (23-36 ng m-3) and total organic acids (7-10 ng m-3) were observed. Elevated organosulfate and organic acid concentrations coincided with the Arctic haze period at both stations, where northern Eurasia was identified as the main source region. Air mass transport from northern Eurasia to Zeppelin Mountain was associated with a 100% increase in the number of detected organosulfate species compared with periods of air mass transport from the Arctic Ocean, Scandinavia and Greenland. The results from this

Validation of LIRIC aerosol concentration retrievals using airborne measurements during a biomass burning episode over Athens

NASA Astrophysics Data System (ADS)

Kokkalis, Panagiotis; Amiridis, Vassilis; Allan, James D.; Papayannis, Alexandros; Solomos, Stavros; Binietoglou, Ioannis; Bougiatioti, Aikaterini; Tsekeri, Alexandra; Nenes, Athanasios; Rosenberg, Philip D.; Marenco, Franco; Marinou, Eleni; Vasilescu, Jeni; Nicolae, Doina; Coe, Hugh; Bacak, Asan; Chaikovsky, Anatoli

2017-01-01

In this paper we validate the Lidar-Radiometer Inversion Code (LIRIC) retrievals of the aerosol concentration in the fine mode, using the airborne aerosol chemical composition dataset obtained over the Greater Athens Area (GAA) in Greece, during the ACEMED campaign. The study focuses on the 2nd of September 2011, when a long-range transported smoke layer was observed in the free troposphere over Greece, in the height range from 2 to 3 km. CIMEL sun-photometric measurements revealed high AOD ( 0.4 at 532 nm) and Ångström exponent values ( 1.7 at 440/870 nm), in agreement with coincident ground-based lidar observations. Airborne chemical composition measurements performed over the GAA, revealed increased CO volume concentration ( 110 ppbv), with 57% sulphate dominance in the PM1 fraction. For this case, we compare LIRIC retrievals of the aerosol concentration in the fine mode with the airborne Aerosol Mass Spectrometer (AMS) and Passive Cavity Aerosol Spectrometer Probe (PCASP) measurements. Our analysis shows that the remote sensing retrievals are in a good agreement with the measured airborne in-situ data from 2 to 4 km. The discrepancies observed between LIRIC and airborne measurements at the lower troposphere (below 2 km), could be explained by the spatial and temporal variability of the aerosol load within the area where the airborne data were averaged along with the different time windows of the retrievals.

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

NASA Astrophysics Data System (ADS)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

Spatial and temporal variations of aerosols around Beijing in summer 2006: 2. Local and column aerosol optical properties

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Fast, J. D.; PöSchl, U.; Garland, R. M.; Andreae, M. O.; Wiedensohler, A.; Sugimoto, N.; Zhu, T.

2010-11-01

Model calculations were conducted using the Weather Research and Forecasting model coupled with chemistry (WRF-chem) for the region around Beijing, China, in the summer of 2006, when the CAREBeijing-2006 intensive campaign was conducted. In this paper, we interpret aerosol optical properties in terms of aerosol mass concentrations and their chemical compositions by linking model calculations with measurements. The model calculations generally captured the observed variability of various surface and column aerosol optical parameters in and around Beijing. At the surface, the spatial and temporal variations of aerosol absorption and scattering coefficients corresponded well to those of elemental carbon and sulfate mass concentrations, respectively, and were controlled by local-scale (<100 km and <24 hours) and regional-scale (<500 km and <3 days) emissions, respectively. The contribution of secondary aerosols and their water uptake increased with altitude within the planetary boundary layer. This variation led to a considerable increase in column aerosol optical depth and was responsible for the differences in regional and temporal variations between surface and column aerosol optical properties around Beijing. These processes are expected to be common in other megacity regions as well. Model calculations, however, underestimated or overestimated the absolute levels of aerosol optical properties in and around Beijing by up to 60%. Sensitivity studies showed that these discrepancies were mostly due to the uncertainties in aerosol mixing state and aerosol density (affecting mass extinction efficiency) in the model calculations. Good agreement with measurements is achieved when these aerosol properties are accurately predicted or assumed; however, significant bias can result when these properties are inadequately treated, even if total aerosol mass concentrations are reproduced well in the model calculations.

[Size distributions of aerosol during the Spring Festival in Nanjing].

PubMed

Wang, Hong-Lei; Zhu, Bin; Shen, Li-Juan; Liu, Xiao-Hui; Zhang, Ze-Feng; Yang, Yang

2014-02-01

In order to investigate the firework burning impacts on spectrum distribution of atmospheric aerosol during the Spring Festival in Nanjing, number concentration and mass concentration of aerosol as well as mass concentration of gas pollutants were measured during January 19-31, 2012. The results indicated that the concentration of aerosol between 10-20 nm decreased, aerosol concentration in the range of 50-100 nm, 100-200 nm and 200-500 nm increased during the firework burning period comparing to those during the non-burning period. However, there was no obvious variation for aerosol between 20-50 nm and 0.5-10 microm. The spectrum distribution of number concentration was bimodal during the non-burning period and unimodal during the burning period, with the peak value shifting to large diameter section. The mass concentration presented a bimodal distribution, the value of PM2.5/PM10 and PM10/PM10 increased by 10% during the burning period. The firework burning events had big influence on the density of aerosol between 1.0-2.1 microm.

Number concentration, size distribution and horizontal mass flux of Asian dust particles collected over free troposphere of Chinese desert region in calm weather condition using balloon borne measurements.

NASA Astrophysics Data System (ADS)

Habib, A.; Chen, B.

2017-12-01

Balloon borne measurements were carried out during calm weather conditions in Taklamakan Desert, which is considered as one of the major source areas of Asian dust (KOSA) particles. Vertical distribution of aerosols number concentration, size distribution, mass concentration and horizontal mass flux due to westerly wind was investigated .Vertical distribution of aerosol number concentration and size distribution at Dunhuang (40 °00'N, 94°30'E) China were observed by optical particle counter (OPC) on August 17, 2001, October 17, 2011, January 11, 2002, April 30, 2002. Five channels (0.3, 0.5, 0.8, 1.2 and 3.6 µm) were used in OPC for particle sizing measurements. Aerosol number concentration in winter season (January 11, 2002) at 3-5 km was very high. Variation of free tropospheric aerosols in April 30, 2002 was noticeable. Many inversions of temperature and aerosol concentration change are found at these inversion points. Super micron range was noticeable in size distribution of all balloon borne measurements. High values of estimated mass concentration of aerosols were observed at the ground atmosphere (1-2 km), and interestingly relatively high concentrations were frequently detected above about 2 km. Wind pattern observed by ERA-interim data sets at 500 and 850 hPa, shows that westerly winds were dominated in Taklamakan Desert during balloon borne observation period. Average horizontal mass flux of background Asian dust due to westerly wind was about in the range of 1219-58.5 μg/m³ tons/km2/day. Most of the profiles showed active transport of aerosols in the westerly dominated region, while, fluxes were found to be very low on January 11, 2002, compared with the other seasons. Vertical profiles of aerosols number concentration showed that significant transport of aerosols was dominated in westerly region (4-7 km). Low horizontal mass flux of aerosols was found in winter season

Calculating Capstone Depleted Uranium Aerosol Concentrations from Beta Activity Measurements

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

Szrom, Fran; Falo, Gerald A.; Parkhurst, MaryAnn

2009-03-01

Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the depleted uranium (DU) source term for the subsequent human health risk assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that themore » equilibrium between the uranium isotopes and their immediate short lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Correction factors for the disrupted equilibrium ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92.« less

Long-term variation of the concentrations of long-lived Rn descendants and cosmogenic 7Be and determination of the MRT of aerosols

NASA Astrophysics Data System (ADS)

Dueñas, C.; Fernández, M. C.; Carretero, J.; Liger, E.; Cañete, S.

During a 6 years period, the atmospheric activity concentrations of the long-lived 222Rn daughters and 7Be concentrations were measured at Málaga (36° 43'40″ N; 4° 28'8″ W). The concentration data of long-lived radon daughters and 7Be together with meteorological variables were used for a comprehensive regression analysis of weekly variation of radioactivity in air. The seasonal variations of the concentrations show similar trend for the long-lived daughters of radon and 7Be concentrations. The activity concentrations were observed to be higher during the summer months than in other seasons. From the ratio between the activity concentrations of 210Po and 210Pb, a mean residence time of aerosol particles in the atmosphere of about 31 days was obtained. The average concentrations values of 210Pb and 7Be over the 6 years period have been found to be 510 and 4.6 mBq m -3, respectively. A mean aerosol mass concentrations of (46.6±7.8) μg m -3 was also determined during the period of measurements. The 7Be/ 210Pb activity ratios varied between 11 and 8.4. Correlation study has been carried out between the aerosol mass and concentrations of these tracers.

Relationships among particle number, surface area, and respirable mass concentrations in automotive engine manufacturing.

PubMed

Heitbrink, William A; Evans, Douglas E; Ku, Bon Ki; Maynard, Andrew D; Slavin, Thomas J; Peters, Thomas M

2009-01-01

This study investigated the relationships between particle number, surface area, and respirable mass concentration measured simultaneously in a foundry and an automotive engine machining and assembly center. Aerosol concentrations were measured throughout each plant with a condensation particle counter for number concentration, a diffusion charger for active surface area concentration, and an optical particle counter for respirable mass concentration. At selected locations, particle size distributions were characterized with the optical particle counter and an electrical low pressure impactor. Statistical analyses showed that active surface area concentration was correlated with ultrafine particle number concentration and weakly correlated with respirable mass concentration. Correlation between number and active surface area concentration was stronger during winter (R2 = 0.6 for both plants) than in the summer (R2 = 0.38 and 0.36 for the foundry and engine plant respectively). The stronger correlation in winter was attributed to use of direct-fire gas fired heaters that produced substantial numbers of ultrafine particles with a modal diameter between 0.007 and 0.023 mu m. These correlations support findings obtained through theoretical analysis. Such analysis predicts that active surface area increasingly underestimates geometric surface area with increasing particle size, particularly for particles larger than 100 nm. Thus, a stronger correlation between particle number concentration and active surface area concentration is expected in the presence of high concentrations of ultrafine particles. In general, active surface area concentration may be a concentration metric that is distinct from particle number concentration and respirable mass concentration. For future health effects or toxicological studies involving nano-materials or ultrafine aerosols, this finding needs to be considered, as exposure metrics may influence data interpretation.

MCS precipitation and downburst intensity response to increased aerosol concentrations

NASA Astrophysics Data System (ADS)

Clavner, M.; Cotton, W. R.; van den Heever, S. C.

2015-12-01

Mesoscale convective systems (MCSs) are important contributors to rainfall in the High Plains of the United States as well as producers of severe weather such as hail, tornados and straight-line wind events known as derechos. Past studies have shown that changes in aerosol concentrations serving as cloud condensation nuclei (CCN) alter the MCS hydrometeor characteristics which in turn modify precipitation yield, downdraft velocity, cold-pool strength, storm propagation and the potential for severe weather to occur. In this study, the sensitivity of MCS precipitation characteristics and convective downburst velocities associated with a derecho to changes in CCN concentrations were examined by simulating a case study using the Regional Atmospheric Modeling System (RAMS). The case study of the 8 May 2009 "Super-Derecho" MCS was chosen since it produced a swath of widespread wind damage in association with an embedded large-scale bow echo, over a broad region from the High Plains of western Kansas to the foothills of the Appalachians. The sensitivity of the storm to changes in CCN concentrations was examined by conducting a set of three simulations which differed in the initial aerosol concentration based on output from the 3D chemical transport model, GEOS-Chem. Results from this study indicate that while increasing CCN concentrations led to an increase in precipitation rates, the changes to the derecho strength were not linear. A moderate increase in aerosol concentration reduced the derecho strength, while the simulation with the highest aerosol concentrations increased the derecho intensity. These changes are attributed to the impact of enhanced CCN concentration on the production of convective downbursts. An analysis of aerosol loading impacts on these MCS features will be presented.

Enhancement of PM2.5 Concentrations by Aerosol-Meteorology Interactions Over China

NASA Astrophysics Data System (ADS)

Zhang, Xin; Zhang, Qiang; Hong, Chaopeng; Zheng, Yixuan; Geng, Guannan; Tong, Dan; Zhang, Yuxuan; Zhang, Xiaoye

2018-01-01

Aerosol-meteorology interactions can change surface aerosol concentrations via different mechanisms such as altering radiation budget or cloud microphysics. However, few studies investigated the impacts of different mechanisms on temporal and spatial distribution of PM2.5 concentrations over China. Here we used the fully coupled Weather Research and Forecasting model with online chemistry (WRF-Chem) to quantify the enhancement of PM2.5 concentrations by aerosol-meteorology feedback in China in 2014 for different seasons and separate the relative impacts of aerosol radiation interactions (ARIs) and aerosol-cloud interactions (ACIs). We found that ARIs and ACIs could increase population-weighted annual mean PM2.5 concentration over China by 4.0 μg/m3 and 1.6 μg/m3, respectively. We found that ARIs play a dominant role in aerosol-meteorology interactions in winter, while the enhancement of PM2.5 concentration by ARIs and ACIs is comparable in other three seasons. ARIs reduced the wintertime monthly mean wind speed and planetary boundary layer (PBL) height by up to 0.1 m/s and 160 m, respectively, but increased the relative humidity by up to 4%, leading to accumulation of pollutants within PBL. Also, ARIs reduced dry deposition velocity of aerosols by up to 20%, resulting in an increase in PM2.5 lifetime and concentrations. ARIs can increase wintertime monthly mean surface PM2.5 concentration by a maximum of 30 μg/m3 in Sichuan Basin. ACIs can also increase PM2.5 concentration with more significant impacts in wet seasons via reduced wet scavenging and enhanced in-cloud chemistry. Dominant processes in PM2.5 enhancement are also clarified in different seasons. Results show that physical process is more important than chemical processes in winter in ARIs, while chemical process of secondary inorganic aerosols production may be crucial in wet seasons via ACIs.

High summertime aerosol organic functional group concentrations from marine and seabird sources at Ross Island, Antarctica, during AWARE

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

Liu, Jun; Dedrick, Jeramy; Russell, Lynn M.

Observations of the organic components of the natural aerosol are scarce in Antarctica, which limits our understanding of natural aerosols and their connection to seasonal and spatial patterns of cloud albedo in the region. From November 2015 to December 2016, the ARM West Antarctic Radiation Experiment (AWARE) measured submicron aerosol properties near McMurdo Station at the southern tip of Ross Island. Submicron organic mass (OM), particle number, and cloud condensation nuclei concentrations were higher in summer than other seasons. The measurements included a range of compositions and concentrations that likely reflected both local anthropogenic emissions and natural background sources. We isolated themore » natural organic components by separating a natural factor and a local combustion factor. The natural OM was 150 times higher in summer than in winter. The local anthropogenic emissions were not hygroscopic and had little contribution to the CCN concentrations. Natural sources that included marine sea spray and seabird emissions contributed 56 % OM in summer but only 3 % in winter. The natural OM had high hydroxyl group fraction (55 %), 6 % alkane, and 6 % amine group mass, consistent with marine organic composition. In addition, the Fourier transform infrared (FTIR) spectra showed the natural sources of organic aerosol were characterized by amide group absorption, which may be from seabird populations. Finally, carboxylic acid group contributions were high in summer and associated with natural sources, likely forming by secondary reactions.« less

High summertime aerosol organic functional group concentrations from marine and seabird sources at Ross Island, Antarctica, during AWARE

DOE PAGES

Liu, Jun; Dedrick, Jeramy; Russell, Lynn M.; ...

2018-01-18

Observations of the organic components of the natural aerosol are scarce in Antarctica, which limits our understanding of natural aerosols and their connection to seasonal and spatial patterns of cloud albedo in the region. From November 2015 to December 2016, the ARM West Antarctic Radiation Experiment (AWARE) measured submicron aerosol properties near McMurdo Station at the southern tip of Ross Island. Submicron organic mass (OM), particle number, and cloud condensation nuclei concentrations were higher in summer than other seasons. The measurements included a range of compositions and concentrations that likely reflected both local anthropogenic emissions and natural background sources. We isolated themore » natural organic components by separating a natural factor and a local combustion factor. The natural OM was 150 times higher in summer than in winter. The local anthropogenic emissions were not hygroscopic and had little contribution to the CCN concentrations. Natural sources that included marine sea spray and seabird emissions contributed 56 % OM in summer but only 3 % in winter. The natural OM had high hydroxyl group fraction (55 %), 6 % alkane, and 6 % amine group mass, consistent with marine organic composition. In addition, the Fourier transform infrared (FTIR) spectra showed the natural sources of organic aerosol were characterized by amide group absorption, which may be from seabird populations. Finally, carboxylic acid group contributions were high in summer and associated with natural sources, likely forming by secondary reactions.« less

Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

NASA Astrophysics Data System (ADS)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-04-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

Boundary layer aerosol size distribution, mass concentration and mineralogical composition in Morocco and at Cape Verde Islands during SAMUM I-II

NASA Astrophysics Data System (ADS)

Kandler, K.; Lieke, K.

2009-04-01

The Saharan Mineral Dust Experiment (SAMUM) is dedicated to the understanding of the radiative effects of mineral dust. Two major field experiments were performed: A first joint field campaign took place at Ouarzazate and near Zagora, southern Morocco, from May 13 to June 7, 2006. Aircraft and ground based measurements of aerosol physical and chemical properties were carried out to collect a data set of surface and atmospheric columnar information within a major dust source. This data set combined with satellite data provides the base of the first thorough columnar radiative closure tests in Saharan dust. A second field experiment was conducted during January-February 2008, in the Cape Verde Islands region, where about 300 Tg of mineral dust are transported annually from Western Africa across the Atlantic towards the Caribbean Sea and the Amazon basin. Along its transport path, the mineral dust is expected to influence significantly the radiation budget - by direct and indirect effects - of the subtropical North Atlantic. We are lacking a radiative closure in the Saharan air plume. One focus of the investigation within the trade wind region is the spatial distribution of mixed dust/biomass/sea salt aerosol and their physical and chemical properties, especially with regard to radiative effects. We report on measurements of size distributions, mass concentrations and mineralogical composition conducted at the Zagora (Morocco) and Praia (Cape Verde islands) ground stations. The aerosol size distribution was measured from 20 nm to 500

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.

Changes in organic aerosol composition with aging inferred from aerosol mass spectra

NASA Astrophysics Data System (ADS)

Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.

2011-07-01

Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows for the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C) (Van Krevelen, 1950). Heald et al. (2010) examined the evolution of total OA in the Van Krevelen diagram. In this work total OA is deconvolved into components that correspond to primary (HOA and others) and secondary (OOA) organic aerosols. By deconvolving total OA into different components, we remove physical mixing effects between secondary and primary aerosols which allows for examination of the evolution of OOA components alone in the Van Krevelen space. This provides a unique means of following ambient secondary OA evolution that is analogous to and can be compared with trends observed in chamber studies of secondary organic aerosol formation. The triangle plot in Ng et al. (2010) indicates that f44 of OOA components increases with photochemical age, suggesting the importance of acid formation in OOA evolution. Once they are transformed with the new parameterization, the triangle plot of the OOA components from all sites occupy an area in Van Krevelen space which follows a ΔH:C/ΔO:C slope of ~ -0.5. This slope suggests that ambient OOA aging results in net changes in chemical composition that are equivalent to the addition of both acid and alcohol/peroxide functional groups without fragmentation (i.e. C-C bond breakage), and/or the addition of acid groups with fragmentation. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.

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

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1987-01-01

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1986-01-01

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Characterization of ambient aerosols at the San Francisco International Airport using BioAerosol Mass Spectrometry

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

Steele, P T; McJimpsey, E L; Coffee, K R

2006-03-16

The BioAerosol Mass Spectrometry (BAMS) system is a rapidly fieldable, fully autonomous instrument that can perform correlated measurements of multiple orthogonal properties of individual aerosol particles. The BAMS front end uses optical techniques to nondestructively measure a particle's aerodynamic diameter and fluorescence properties. Fluorescence can be excited at 266nm or 355nm and is detected in two broad wavelength bands. Individual particles with appropriate size and fluorescence properties can then be analyzed more thoroughly in a dual-polarity time-of-flight mass spectrometer. Over the course of two deployments to the San Francisco International Airport, more than 6.5 million individual aerosol particles were fullymore » analyzed by the system. Analysis of the resulting data has provided a number of important insights relevant to rapid bioaerosol detection, which are described here.« less

Aerosol Enhancements in the Upper Troposphere Over The Amazon Forest: Do Amazonian Clouds Produce Aerosols?

NASA Astrophysics Data System (ADS)

Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Dollner, M.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Krüger, M. L.; Machado, L.; Mertes, S.; Pöhlker, C.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Weinzierl, B.; Wendisch, M.

2015-12-01

The German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. The aircraft was equipped with about 30 remote sensing and in-situ instruments for meteorological, trace gas, aerosol, cloud, precipitation, and solar radiation measurements. Fourteen research flights were conducted during this campaign. Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with concentrations after normalization to standard conditions often exceeding those in the boundary layer (BL). This behavior was consistent between several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were found to be depleted in aerosol particles, whereas enhanced aerosol number and mass concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. This suggests that aerosol production takes place in the UT based on volatile and condensable material brought up by deep convection. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new

Spinning-disk generation and drying of monodisperse solid aerosols with output concentrations sufficient for single-breath inhalation studies.

PubMed

Byron, P R; Hickey, A J

1987-01-01

The air-driven spinning-disk aerosol generator was modified to allow the production of monodisperse dry spherical aerosols of disodium fluorescein (as model solute) in high output concentrations. Output concentrations were determined by filtration. Optical and aerodynamic size distributions were determined microscopically (after electrostatic precipitation) and by cascade impaction. The generator housing allowed the entrainment of 25-microns primary aqueous solution droplets in a 10-L X min-1 downward flow of dry, filtered air. Internal equipment surfaces were machined flush and polished to minimize aerosol losses. Primary droplets were dried within a stainless steel pipe encased in a tube furnace. Water vapor was removed by diffusion drying. Disk-driven air, satellite droplets, and additional dilution air were vented to waste without using a vacuum. Generator yields were increased by reducing the size of the satellite droplet extraction gap. Aerosols were generated reproducibly by delivering aqueous solutions at a rate of 0.2 mL X min-1 to the center of the disk and spinning at 1000 rps. Dry aerosols, with mass median aerodynamic diameters of 2, 4.9, and 9 microns, were produced in concentrations of 0.89, 5.48, and 54.6 micrograms X L-1 from aqueous solutions containing 0.0374, 0.584, and 3.4% solute by weight. Geometric standard deviations were less than 1.2 in all cases. Concentrations are several times higher than others in the literature and are suitable for single-breath inhalation studies of therapeutic aerosol deposition and effect.

Characterization of submicron aerosols at a rural site in Pearl River Delta of China using an Aerodyne High-Resolution Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Huang, X.-F.; He, L.-Y.; Hu, M.; Canagaratna, M. R.; Kroll, J. H.; Ng, N. L.; Zhang, Y.-H.; Lin, Y.; Xue, L.; Sun, T.-L.; Liu, X.-G.; Shao, M.; Jayne, J. T.; Worsnop, D. R.

2010-11-01

The Pearl River Delta (PRD) region in South China is one of the most economically developed regions in China, but it is also noted for its severe air pollution due to industrial/metropolitan emissions. In order to continuously improve the understanding and quantification of air pollution in this region, an intensive campaign was executed in PRD during October-November 2008. Here, we report and analyze Aerodyne High-Resolution Aerosol Mass Spectrometer measurements at Kaiping, a rural site downwind of the highly-polluted central PRD area, to characterize the general features of submicron particulate pollution in the regional air. The mean measured PM1 mass concentration was 33.1 ± 18.1 μg m-3 during the campaign and composed of organic matter (33.8%), sulfate (33.7%), ammonium (14.0%), nitrate (10.7%), black carbon (6.7%), and chloride (1.1%), which is characterized by high fractions of inorganic ions due to huge emissions of SO2 and NOx in PRD. The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at ~450 nm in vacuum aerodynamic diameter. Calculations based on high-resolution organic mass spectra indicate that C, H, O, and N on average contributed 56.6, 7.0, 35.1, and 1.3% to the total organic mass, respectively, corresponding to an organic matter mass to organic carbon mass ratio (OM/OC) of 1.77 ± 0.08. Based on the high-resolution organic mass spectral dataset observed, Positive Matrix Factorization (PMF) analysis differentiated the organic aerosol into three components, i.e., biomass burning (BBOA) and two oxygenated (LV-OOA and SV-OOA) organic aerosols, which on average accounted for 24.5, 39.6 and 35.8% of the total organic mass, respectively. The BBOA showed strong features of biomass burning emissions and has been mainly attributed to field rice straw burning after harvest. The LV-OOA and SV-OOA were found to correspond to more aged (and thus less-volatile) and fresher (and semi-volatile) secondary

Aerosol Vacuum-Assisted Plasma Ionization (Aero-VaPI) Coupled to Ion Mobility-Mass Spectrometry

NASA Astrophysics Data System (ADS)

Blair, Sandra L.; Ng, Nga L.; Zambrzycki, Stephen C.; Li, Anyin; Fernández, Facundo M.

2018-02-01

In this communication, we report on the real-time analysis of organic aerosol particles by Vacuum-assisted Plasma Ionization-Mass Spectrometry (Aero-VaPI-MS) using a home-built VaPI ion source coupled to a Synapt G2-S HDMS ion mobility-mass spectrometry (IM-MS) system. Standards of organic molecules of interest in prebiotic chemistry were used to generate aerosols. Monocaprin and decanoic acid aerosol particles were successfully detected in both the positive and negative ion modes, respectively. A complex aerosol mixture of different sizes of polymers of L-malic acid was also examined through ion mobility (IM) separations, resulting in the detection of polymers of up to eight monomeric units. This noncommercial plasma ion source is proposed as a low cost alternative to other plasma ionization platforms used for aerosol analysis, and a higher-performance alternative to more traditional aerosol mass spectrometers. VaPI provides robust online ionization of organics in aerosols without extensive ion activation, with the coupling to IM-MS providing higher peak capacity and excellent mass accuracy. [Figure not available: see fulltext.

Retrieve Aerosol Concentration Based On Surface Model and Distribution of Concentration of PM2.5 ——A Case Study of Beijing

NASA Astrophysics Data System (ADS)

Cui, H.

2017-12-01

As China's economy continues to grow, urbanization continues to advance, along with growth in all areas to pollutant emissions in the air industry, air quality also continued to deteriorate. Aerosol concentrations as a measure of air quality of the most important part of are more and more people's attention. Traditional monitoring stations measuring aerosol concentration method is accurate, but time-consuming and can't be done simultaneously measure a large area, can only rely on data from several monitoring sites to predict the concentration of the panorama. Remote Sensing Technology retrieves aerosol concentrations being by virtue of their efficient, fast advantages gradually into sight. In this paper, by the method of surface model to start with the physical processes of atmospheric transport, innovative aerosol concentration coefficient proposed to replace the traditional aerosol concentrations, pushed to a set of retrieval of aerosol concentration coefficient method, enabling fast and efficient Get accurate air pollution target area. At the same paper also monitoring data for PM2.5 in Beijing were analyzed from different angles, from the perspective of the data summarized in Beijing PM2.5 concentration of time, space, geographical distribution and concentration of PM2.5 and explored the relationship between aerosol concentration coefficient and concentration of PM2.5.

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-01-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

A novel continuous powder aerosolizer (CPA) for inhalative administration of highly concentrated recombinant surfactant protein-C (rSP-C) surfactant to preterm neonates.

PubMed

Pohlmann, G; Iwatschenko, P; Koch, W; Windt, H; Rast, M; de Abreu, M Gama; Taut, F J H; De Muynck, C

2013-12-01

In pulmonary medicine, aerosolization of substances for continuous inhalation is confined to different classes of nebulizers with their inherent limitations. Among the unmet medical needs is the lack of an aerosolized surfactant preparation for inhalation by preterm neonates, to avoid the risks associated with endotracheal intubation and surfactant bolus instillation. In the present report, we describe a high-concentration continuous powder aerosolization system developed for delivery of inhalable surfactant to preterm neonates. The developed device uses a technique that allows efficient aerosolization of dry surfactant powder, generating a surfactant aerosol of high concentration. In a subsequent humidification step, the heated aerosol particles are covered with a surface layer of water. The wet surfactant aerosol is then delivered to the patient interface (e.g., nasal prongs) through a tube. The performance characteristics of the system are given as mass concentration, dose rate, and size distribution of the generated aerosol. Continuous aerosol flows of about 0.84 L/min can be generated from dry recombinant surfactant protein-C surfactant, with concentrations of up to 12 g/m(3) and median particle sizes of the humidified particles in the range of 3 to 3.5 μm at the patient interface. The system has been successfully used in preclinical studies. The device with its continuous high-concentration delivery is promising for noninvasive delivery of surfactant aerosol to neonates and has the potential for becoming a versatile disperser platform closing the gap between continuously operating nebulizers and discontinuously operating dry powder inhaler devices.

Evaluation of the impact of long-range transport and aerosol concentration temporal variations at the eastern coast of the Baltic Sea.

PubMed

Ovadnevaite, J; Kvietkus, K; Sakalys, J

2007-09-01

Ambient particles vary greatly in their ability to affect visibility, climate and human health. The fine fraction of aerosol is responsible for greater and wider effects on human health; thus, investigation of this fraction is very important. Continuous measurements of PM2.5 (particulate matter below 2.5 microm in size) concentrations at the Preila monitoring station started in 2003. During a period of 2 years, the episodes of high daily and semi-hourly concentrations of PM2.5 were measured. These episodes did not depend on the season or time of day. The substantial role of long-range transport of pollutants to these increases in concentration was shown using chemical and statistical analysis. It was found that most of the severe episodes occurred when air masses came from a specific site besides it was established that air masses of different origin were characterized by different mixing layer depth. Lower mixing depth was observed in air masses characterized by higher observed concentrations at the measuring site and vice versa. PM2.5 concentrations showed diurnal and seasonal variations whose pattern reflected the regional origin of the aerosol. The regional pollution level was evaluated by the statistical analysis of PM2.5 concentrations. The background annual average of PM2.5 mass concentration for the eastern coast of the Baltic Sea was 15.1 +/- 0.8 microg m(-3).

Measurements of Semi-volatile Aerosol and Its Effect on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

NASA Astrophysics Data System (ADS)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2013-12-01

Semi-volatile compounds, including particle-bound water, comprise a large part of aerosol mass and have a significant influence on aerosol lifecycle and its optical properties. Understanding the properties of semi-volatile compounds, especially those pertaining to gas/aerosol partitioning, is of critical importance for our ability to predict concentrations and properties of ambient aerosol. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of temperature and relative humidity on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). In parallel to these measurements, a long residence time temperature-stepping thermodenuder and a variable residence time constant temperature thermodenuder in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. It was found that both temperature and relative humidity have a strong effect on aerosol optical properties. The variable residence time thermodenuder data suggest that aerosol equilibrated fairly quickly, within 2 s, in contrast to other ambient observations. Preliminary analysis show that approximately 50% and 90% of total aerosol mass evaporated at temperatures of 100 C and 180C, respectively. Evaporation varied substantially with ambient aerosol loading and composition and meteorology. During course of this study, T50 (temperatures at which 50% aerosol mass evaporates) varied from 60 C to more than 120 C.

Mass or total surface area with aerosol size distribution as exposure metrics for inflammatory, cytotoxic and oxidative lung responses in rats exposed to titanium dioxide nanoparticles.

PubMed

Noël, A; Truchon, G; Cloutier, Y; Charbonneau, M; Maghni, K; Tardif, R

2017-04-01

There is currently no consensus on the best exposure metric(s) for expressing nanoparticle (NP) dose. Although surface area has been extensively studied for inflammatory responses, it has not been as thoroughly validated for cytotoxicity or oxidative stress effects. Since inhaled NPs deposit and interact with lung cells based on agglomerate size, we hypothesize that mass concentration combined with aerosol size distribution is suitable for NP risk assessment. The objective of this study was to evaluate different exposure metrics for inhaled 5 nm titanium dioxide aerosols composed of small (SA < 100 nm) or large (LA > 100 nm) agglomerates at 2, 7, and 20 mg/m 3 on rat lung inflammatory, cytotoxicity, and oxidative stress responses. We found a significant positive correlation ( r = 0.98, p < 0.01) with the inflammatory reaction, measured by the number of neutrophils and the mass concentration when considering all six (SA + LA) aerosols. This correlation was similar ( r = 0.87) for total surface area. Regarding cytotoxicity and oxidative stress responses, measured by lactate dehydrogenase and 8-isoprostane, respectively, and mass or total surface area as an exposure metric, we observed significant positive correlations only with SA aerosols for both the mass concentration and size distribution ( r > 0.91, p < 0.01), as well as for the total surface area ( r > 0.97, p < 0.01). These data show that mass or total surface area concentrations alone are insufficient to adequately predict oxidant and cytotoxic pulmonary effects. Overall, our study indicates that considering NP size distribution along with mass or total surface area concentrations contributes to a more mechanistic discrimination of pulmonary responses to NP exposure.

Impact of aerosol size representation on modeling aerosol-cloud interactions

DOE PAGES

Zhang, Y.; Easter, R. C.; Ghan, S. J.; ...

2002-11-07

In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach.more » The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).« less

Potential source identification for aerosol concentrations over a site in Northwestern India

NASA Astrophysics Data System (ADS)

Payra, Swagata; Kumar, Pramod; Verma, Sunita; Prakash, Divya; Soni, Manish

2016-03-01

The collocated measurements of aerosols size distribution (ASD) and aerosol optical thickness (AOT) are analyzed simultaneously using Grimm aerosol spectrometer and MICROTOP II Sunphotometer over Jaipur, capital of Rajasthan in India. The contrast temperature characteristics during winter and summer seasons of year 2011 are investigated in the present study. The total aerosol number concentration (TANC, 0.3-20 μm) during winter season was observed higher than in summer time and it was dominated by fine aerosol number concentration (FANC < 2 μm). Particles smaller than 0.8 μm (at aerodynamic size) constitute ~ 99% of all particles in winter and ~ 90% of particles in summer season. However, particles greater than 2 μm contribute ~ 3% and ~ 0.2% in summer and winter seasons respectively. The aerosols optical thickness shows nearly similar AOT values during summer and winter but corresponding low Angstrom Exponent (AE) values during summer than winter, respectively. In this work, Potential Source Contribution Function (PSCF) analysis is applied to identify locations of sources that influenced concentrations of aerosols over study area in two different seasons. PSCF analysis shows that the dust particles from Thar Desert contribute significantly to the coarse aerosol number concentration (CANC). Higher values of the PSCF in north from Jaipur showed the industrial areas in northern India to be the likely sources of fine particles. The variation in size distribution of aerosols during two seasons is clearly reflected in the log normal size distribution curves. The log normal size distribution curves reveals that the particle size less than 0.8 μm is the key contributor in winter for higher ANC.

A thermal desorption mass spectrometer for freshly nucleated secondary aerosol particles

NASA Astrophysics Data System (ADS)

Held, A.; Gonser, S. G.

2012-04-01

Secondary aerosol formation in the atmosphere is observed in a large variety of locations worldwide, introducing new particles to the atmosphere which can grow to sizes relevant for health and climate effects of aerosols. The chemical reactions leading to atmospheric secondary aerosol formation are not yet fully understood. At the same time, analyzing the chemical composition of freshly nucleated particles is still a challenging task. We are currently finishing the development of a field portable aerosol mass spectrometer for nucleation particles with diameters smaller than 30 nm. This instrument consists of a custom-built aerosol sizing and collection unit coupled to a time-of-flight mass spectrometer (TOF-MS). The aerosol sizing and collection unit is composed of three major parts: (1) a unipolar corona aerosol charger, (2) a radial differential mobility analyzer (rDMA) for aerosol size separation, and (3) an electrostatic precipitator for aerosol collection. After collection, the aerosol sample is thermally desorbed, and the resulting gas sample is transferred to the TOF-MS for chemical analysis. The unipolar charger is based on corona discharge from carbon fibres (e.g. Han et al., 2008). This design allows efficient charging at voltages below 2 kV, thus eliminating the potential for ozone production which would interfere with the collected aerosol. With the current configuration the extrinsic charging efficiency for 20 nm particles is 32 %. The compact radial DMA similar to the design of Zhang et al. (1995) is optimized for a diameter range from 1 nm to 100 nm. Preliminary tests show that monodisperse aerosol samples (geometric standard deviation of 1.09) at 10 nm, 20 nm, and 30 nm can easily be separated from the ambient polydisperse aerosol population. Finally, the size-segregated aerosol sample is collected on a high-voltage biased metal filament. The collected sample is protected from contamination using a He sheath counterflow. Resistive heating of the

A study of photochemical againg of ambient air using Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions

NASA Astrophysics Data System (ADS)

Lee, T.; Son, J.; Kim, J.; Kim, S.; Sung, K.; Park, G.; Link, M.; Park, T.; Kim, K.; Kang, S.; Ban, J.; Kim, D. S.

2016-12-01

Recent research proposed that Secondary Aerosol (SA) is important class of predicting future climate change scenarios, health effect, and a general air quality. However, there has been lack of studies to investigate SA formation all over the world. This study tried to focus on understanding potential secondary aerosol formation and its local impact by the photochemical aging of inorganic and organic aerosols in the ambient air using the Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions. PAM chamber manufactured by Aerodyne make an oxidizing environment that simulates oxidation processes on timescales of 12-15 hrs in the atmosphere. Chemical compositions of ambient aerosol and aerosol that was aged in the PAM chamber were alternately measured every 2-minutes using the High Resolution-Time of Flight-Aerosol Mass Spectrometer (HR-ToF-AMS). HR-ToF-AMS provides non-refractory aerosol mass concentrations including nitrate, sulfate, hydrocarbon-like and oxygenated organic aerosol in real time. This study includes a residence area of mixture of sources, a forest site of dominant source of biogenic VOCs, an underground parking lot of dominant vehicle emission, and laboratory experiment of vehicle emissions under different fuels and speeds using the chassis dynamometer. As a result, it was revealed that gasoline and LPG vehicle relatively made more potential SA than diesel vehicle.

Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

NASA Astrophysics Data System (ADS)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-07-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based

Comparison of two estimation methods for surface area concentration using number concentration and mass concentration of combustion-related ultrafine particles

NASA Astrophysics Data System (ADS)

Park, Ji Young; Raynor, Peter C.; Maynard, Andrew D.; Eberly, Lynn E.; Ramachandran, Gurumurthy

Recent research has suggested that the adverse health effects caused by nanoparticles are associated with their surface area (SA) concentrations. In this study, SA was estimated in two ways using number and mass concentrations and compared with SA (SA meas) measured using a diffusion charger (DC). Aerosol measurements were made twice: once starting in October 2002 and again starting in December 2002 in Mysore, India in residences that used kerosene or liquefied petroleum gas (LPG) for cooking. Mass, number, and SA concentrations and size distributions by number were measured in each residence. The first estimation method (SA PSD) used the size distribution by number to estimate SA. The second method (SA INV) used a simple inversion scheme that incorporated number and mass concentrations while assuming a lognormal size distribution with a known geometrical standard deviation. SA PSD was, on average, 2.4 times greater (range = 1.6-3.4) than SA meas while SA INV was, on average, 6.0 times greater (range = 4.6-7.7) than SA meas. The logarithms of SA PSD and SA INV were found to be statistically significant predictors of the logarithm of SA meas. The study showed that particle number and mass concentration measurements can be used to estimate SA with a correction factor that ranges between 2 and 6.

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

Quantification of marine aerosol subgrid variability and its correlation with clouds based on high-resolution regional modeling: Quantifying Aerosol Subgrid Variability

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

Lin, Guangxing; Qian, Yun; Yan, Huiping

One limitation of most global climate models (GCMs) is that with the horizontal resolutions they typically employ, they cannot resolve the subgrid variability (SGV) of clouds and aerosols, adding extra uncertainties to the aerosol radiative forcing estimation. To inform the development of an aerosol subgrid variability parameterization, here we analyze the aerosol SGV over the southern Pacific Ocean simulated by the high-resolution Weather Research and Forecasting model coupled to Chemistry. We find that within a typical GCM grid, the aerosol mass subgrid standard deviation is 15% of the grid-box mean mass near the surface on a 1 month mean basis.more » The fraction can increase to 50% in the free troposphere. The relationships between the sea-salt mass concentration, meteorological variables, and sea-salt emission rate are investigated in both the clear and cloudy portion. Under clear-sky conditions, marine aerosol subgrid standard deviation is highly correlated with the standard deviations of vertical velocity, cloud water mixing ratio, and sea-salt emission rates near the surface. It is also strongly connected to the grid box mean aerosol in the free troposphere (between 2 km and 4 km). In the cloudy area, interstitial sea-salt aerosol mass concentrations are smaller, but higher correlation is found between the subgrid standard deviations of aerosol mass and vertical velocity. Additionally, we find that decreasing the model grid resolution can reduce the marine aerosol SGV but strengthen the correlations between the aerosol SGV and the total water mixing ratio (sum of water vapor, cloud liquid, and cloud ice mixing ratios).« less

Comparison of MADE3-simulated and observed aerosol distributions with a focus on aerosol vertical profiles

NASA Astrophysics Data System (ADS)

Kaiser, Christopher; Hendricks, Johannes; Righi, Mattia; Jöckel, Patrick

2016-04-01

The reliability of aerosol radiative forcing estimates from climate models depends on the accuracy of simulated global aerosol distribution and composition, as well as on the models' representation of the aerosol-cloud and aerosol-radiation interactions. To help improve on previous modeling studies, we recently developed the new aerosol microphysics submodel MADE3 that explicitly tracks particle mixing state in the Aitken, accumulation, and coarse mode size ranges. We implemented MADE3 into the global atmospheric chemistry general circulation model EMAC and evaluated it by comparison of simulated aerosol properties to observations. Compared properties include continental near-surface aerosol component concentrations and size distributions, continental and marine aerosol vertical profiles, and nearly global aerosol optical depth. Recent studies have shown the specific importance of aerosol vertical profiles for determination of the aerosol radiative forcing. Therefore, our focus here is on the evaluation of simulated vertical profiles. The observational data is taken from campaigns between 1990 and 2011 over the Pacific Ocean, over North and South America, and over Europe. The datasets include black carbon and total aerosol mass mixing ratios, as well as aerosol particle number concentrations. Compared to other models, EMAC with MADE3 yields good agreement with the observations - despite a general high bias of the simulated mass mixing ratio profiles. However, BC concentrations are generally overestimated by many models in the upper troposphere. With MADE3 in EMAC, we find better agreement of the simulated BC profiles with HIPPO data than the multi-model average of the models that took part in the AeroCom project. There is an interesting difference between the profiles from individual campaigns and more "climatological" datasets. For instance, compared to spatially and temporally localized campaigns, the model simulates a more continuous decline in both total

Analysis of DIAL/HSRL aerosol backscatter and extinction profiles during the SEAC4RS campaign with an aerosol assimilation system

NASA Astrophysics Data System (ADS)

Weaver, C. J.; da Silva, A. M., Jr.; Colarco, P. R.; Randles, C. A.

2015-12-01

We retrieve aerosol concentrations and optical information from vertical profiles of airborne 532 nm extinction and 532 and 1064 nm backscatter measurements made during the SEAC4RS summer 2013 campaign. The observations are from the High Spectral Resolution Lidar (HSRL) Airborne Differential Absorption Lidar (DIAL) on board the NASA DC-8. Instead of retrieving information about aerosol microphysical properties such as indexes of refraction, we seek information more directly applicable to an aerosol transport model - in our case the Goddard Chemistry Aerosol Radiation and Transport (GOCART) module used in the GEOS-5 Earth modeling system. A joint atmosphere/aerosol mini-reanalysis was performed for the SEAC4RS period using GEOS-5. The meteorological reanalysis followed the MERRA-2 atmospheric reanalysis protocol, and aerosol information from MODIS, MISR, and AERONET provided a constraint on the simulated aerosol optical depth (i.e., total column loading of aerosols). We focus on the simulated concentrations of 10 relevant aerosol species simulated by the GOCART module: dust, sulfate, and organic and black carbon. Our first retrieval algorithm starts with the SEAC4RS mini-reanalysis and adjusts the concentration of each GOCART aerosol species so that differences between the observed and simulated backscatter and extinction measurements are minimized. In this case, too often we are unable to simulate the observations by simple adjustment of the aerosol concentrations. A second retrieval approach adjusts both the aerosol concentrations and the optical parameters (i.e., assigned mass extinction efficiency) associated with each GOCART species. We present results from DC-8 flights over smoke from forest fires over the western US using both retrieval approaches. Finally, we compare our retrieved quantities with in-situ observations of aerosol absorption, scattering, and mass concentrations at flight altitude.

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.

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

Constraining Aerosol Optical Models Using Ground-Based, Collocated Particle Size and Mass Measurements in Variable Air Mass Regimes During the 7-SEAS/Dongsha Experiment

NASA Technical Reports Server (NTRS)

Bell, Shaun W.; Hansell, Richard A.; Chow, Judith C.; Tsay, Si-Chee; Wang, Sheng-Hsiang; Ji, Qiang; Li, Can; Watson, John G.; Khlystov, Andrey

2012-01-01

During the spring of 2010, NASA Goddard's COMMIT ground-based mobile laboratory was stationed on Dongsha Island off the southwest coast of Taiwan, in preparation for the upcoming 2012 7-SEAS field campaign. The measurement period offered a unique opportunity for conducting detailed investigations of the optical properties of aerosols associated with different air mass regimes including background maritime and those contaminated by anthropogenic air pollution and mineral dust. What appears to be the first time for this region, a shortwave optical closure experiment for both scattering and absorption was attempted over a 12-day period during which aerosols exhibited the most change. Constraints to the optical model included combined SMPS and APS number concentration data for a continuum of fine and coarse-mode particle sizes up to PM2.5. We also take advantage of an IMPROVE chemical sampler to help constrain aerosol composition and mass partitioning of key elemental species including sea-salt, particulate organic matter, soil, non sea-salt sulphate, nitrate, and elemental carbon. Our results demonstrate that the observed aerosol scattering and absorption for these diverse air masses are reasonably captured by the model, where peak aerosol events and transitions between key aerosols types are evident. Signatures of heavy polluted aerosol composed mostly of ammonium and non sea-salt sulphate mixed with some dust with transitions to background sea-salt conditions are apparent in the absorption data, which is particularly reassuring owing to the large variability in the imaginary component of the refractive indices. Extinctive features at significantly smaller time scales than the one-day sample period of IMPROVE are more difficult to reproduce, as this requires further knowledge concerning the source apportionment of major chemical components in the model. Consistency between the measured and modeled optical parameters serves as an important link for advancing remote

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.

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

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

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses.

PubMed

Kahn, Ralph A; Berkoff, Tim A; Brock, Charles; Chen, Gao; Ferrare, Richard A; Ghan, Steven; Hansico, Thomas F; Hegg, Dean A; Martins, J Vanderlei; McNaughton, Cameron S; Murphy, Daniel M; Ogren, John A; Penner, Joyce E; Pilewskie, Peter; Seinfeld, John H; Worsnop, Douglas R

2017-10-01

A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ . The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling , help interrelate remote-sensing, in situ, and modeling aerosol-type definitions , and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable , even if aerosol loading varies.

Aerosol chemical composition in cloud events by high resolution time-of-flight aerosol mass spectrometry.

PubMed

Hao, Liqing; Romakkaniemi, Sami; Kortelainen, Aki; Jaatinen, Antti; Portin, Harri; Miettinen, Pasi; Komppula, Mika; Leskinen, Ari; Virtanen, Annele; Smith, James N; Sueper, Donna; Worsnop, Douglas R; Lehtinen, Kari E J; Laaksonen, Ari

2013-03-19

This study presents results of direct observations of aerosol chemical composition in clouds. A high-resolution time-of-flight aerosol mass spectrometer was used to make measurements of cloud interstitial particles (INT) and mixed cloud interstitial and droplet residual particles (TOT). The differences between these two are the cloud droplet residuals (RES). Positive matrix factorization analysis of high-resolution mass spectral data sets and theoretical calculations were performed to yield distributions of chemical composition of the INT and RES particles. We observed that less oxidized hydrocarbon-like organic aerosols (HOA) were mainly distributed into the INT particles, whereas more oxidized low-volatile oxygenated OA (LVOOA) mainly in the RES particles. Nitrates existed as organic nitrate and in chemical form of NH(4)NO(3). Organic nitrates accounted for 45% of total nitrates in the INT particles, in clear contrast to 26% in the RES particles. Meanwhile, sulfates coexist in forms of acidic NH(4)HSO(4) and neutralized (NH(4))(2)SO(4). Acidic sulfate made up 64.8% of total sulfates in the INT particles, much higher than 10.7% in the RES particles. The results indicate a possible joint effect of activation ability of aerosol particles, cloud processing, and particle size effects on cloud formation.

Simultaneous aerosol mass spectrometry and chemical ionisation mass spectrometry measurements during a biomass burning event in the UK: insights into nitrate chemistry

NASA Astrophysics Data System (ADS)

Reyes-Villegas, Ernesto; Priestley, Michael; Ting, Yu-Chieh; Haslett, Sophie; Bannan, Thomas; Le Breton, Michael; Williams, Paul I.; Bacak, Asan; Flynn, Michael J.; Coe, Hugh; Percival, Carl; Allan, James D.

2018-03-01

Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality such as bonfires and fireworks. High aerosol and gas concentrations generated from public bonfires or fireworks were measured in order to understand the night-time chemical processes and their atmospheric implications. Nitrogen chemistry was observed during Bonfire Night with nitrogen containing compounds in both gas and aerosol phases and further N2O5 and ClNO2 concentrations, which depleted early next morning due to photolysis of NO3 radicals and ceasing production. Particulate organic oxides of nitrogen (PONs) concentrations of 2.8 µg m-3 were estimated using the m / z 46 : 30 ratios from aerosol mass spectrometer (AMS) measurements, according to previously published methods. Multilinear engine 2 (ME-2) source apportionment was performed to determine organic aerosol (OA) concentrations from different sources after modifying the fragmentation table and it was possible to identify two PON factors representing primary (pPON_ME2) and secondary (sPON_ME2) contributions. A slight improvement in the agreement between the source apportionment of the AMS and a collocated AE-31 Aethalometer was observed after modifying the prescribed fragmentation in the AMS organic spectrum (the fragmentation table) to determine PON sources, which resulted in an r2 = 0.894 between biomass burning organic aerosol (BBOA) and babs_470wb compared to an r2 = 0.861 obtained without the modification. Correlations between OA sources and measurements made using time-of-flight chemical ionisation mass spectrometry with an iodide adduct ion were performed in order to determine possible gas tracers to be used in future ME-2 analyses to constrain solutions. During Bonfire Night, strong correlations (r2) were observed between BBOA and methacrylic acid (0.92), acrylic acid (0.90), nitrous acid (0.86), propionic acid, (0.85) and hydrogen cyanide (0.76). A series of

Concurrent Temporal and Spatial Trends in Sulfate and Organic Mass Concentrations Measured in the IMPROVE Monitoring Program

NASA Astrophysics Data System (ADS)

Malm, William C.; Schichtel, Bret A.; Hand, Jenny L.; Collett, Jeffrey L.

2017-10-01

Recent modeling and field studies have highlighted a relationship between sulfate concentrations and secondarily formed organic aerosols related to isoprene and other volatile biogenic gaseous emissions. The relationship between these biogenic emissions and sulfate is thought to be primarily associated with the effect of sulfate on aerosol acidity, increased aerosol water at high relative humidities, and aerosol volume. The Interagency Monitoring of Protected Visual Environments (IMPROVE) program provides aerosol concentration levels of sulfate (SO4) and organic carbon (OC) at 136 monitoring sites in rural and remote areas of the United States over time periods of between 15 and 28 years. This data set allows for an examination of relationships between these variables over time and space. The relative decreases in SO4 and OC were similar over most of the eastern United States, even though concentrations varied dramatically from one region to another. The analysis implied that for every unit decrease in SO4 there was about a 0.29 decrease in organic aerosol mass (OA = 1.8 × OC). This translated to a 2 μg/m3 decrease in biogenically derived secondary organic aerosol over 15 years in the southeastern United States. The analysis further implied that 35% and 27% in 2001 and 2015, respectively, of average total OA may be biogenically derived secondary organic aerosols and that there was a small but significant decrease in OA not linked to changes in SO4 concentrations. The analysis yields a constraint on ambient SO4-OC relationships that should help to refine and improve regional-scale chemical transport models.

Aerosol generation and measurement of multi-wall carbon nanotubes

NASA Astrophysics Data System (ADS)

Myojo, Toshihiko; Oyabu, Takako; Nishi, Kenichiro; Kadoya, Chikara; Tanaka, Isamu; Ono-Ogasawara, Mariko; Sakae, Hirokazu; Shirai, Tadashi

2009-01-01

Mass production of some kinds of carbon nanotubes (CNT) is now imminent, but little is known about the risk associated with their exposure. It is important to assess the propensity of the CNT to release particles into air for its risk assessment. In this study, we conducted aerosolization of a multi-walled CNT (MWCNT) to assess several aerosol measuring instruments. A Palas RBG-1000 aerosol generator applied mechanical stress to the MWCNT by a rotating brush at feed rates ranging from 2 to 20 mm/h, which the MWCNT was fed to a two-component fluidized bed. The fluidized bed aerosol generator was used to disperse the MWCNT aerosol once more. We monitored the generated MWCNT aerosol concentrations based on number, area, and mass using a condensation particle counter and nanoparticle surface area monitor. Also we quantified carbon mass in MWCNT aerosol samples by a carbon monitor. The shape of aerosolized MWCNT fibers was observed by a scanning electron microscope (SEM). The MWCNT was well dispersed by our system. We found isolated MWCNT fibers in the aerosols by SEM and the count median lengths of MWCNT fibers were 4-6 μm. The MWCNT was quantified by the carbon monitor with a modified condition based on the NIOSH analytical manual. The MWCNT aerosol concentration (EC mass base) was 4 mg/m3 at 2 mm/h in this study.

Effect of high concentrations of inorganic seed aerosols on secondary organic aerosol formation in the m-xylene/NO x photooxidation system

NASA Astrophysics Data System (ADS)

Lu, Zifeng; Hao, Jiming; Takekawa, Hideto; Hu, Lanhua; Li, Junhua

High concentrations (>15 μm 3 cm -3) of CaSO 4, Ca(NO 3) 2 and (NH 4) 2SO 4 were selected as surrogates of dry neutral, aqueous neutral and dry acidic inorganic seed aerosols, respectively, to study the effects of inorganic seeds on secondary organic aerosol (SOA) formation in irradiated m-xylene/NO x photooxidation systems. The results indicate that neither ozone formation nor SOA formation is significantly affected by the presence of neutral aerosols (both dry CaSO 4 and aqueous Ca(NO 3) 2), even at elevated concentrations. The presence of high concentrations of (NH 4) 2SO 4 aerosols (dry acidic) has no obvious effect on ozone formation, but it does enhance SOA generation and increase SOA yields. In addition, the effect of dry (NH 4) 2SO 4 on SOA yield is found to be positively correlated with the (NH 4) 2SO 4 surface concentration, and the effect is pronounced only when the surface concentration reaches a threshold value. Further, it is proposed that the SOA generation enhancement is achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of dry (NH 4) 2SO 4 seed aerosols.

A rocket-borne mass analyzer for charged aerosol particles in the mesosphere

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

Knappmiller, Scott; Robertson, Scott; Sternovsky, Zoltan

2008-10-15

An electrostatic mass spectrometer for nanometer-sized charged aerosol particles in the mesosphere has been developed and tested. The analyzer is mounted on the forward end of a rocket and has a slit opening for admitting a continuous sample of air that is exhausted through ports at the sides. Within the instrument housing are two sets of four collection plates that are biased with positive and negative voltages for the collection of negative and positive aerosol particles, respectively. Each collection plate spans about an order of magnitude in mass which corresponds to a factor of 2 in radius. The number densitymore » of the charge is calculated from the current collected by the plates. The mean free path for molecular collisions in the mesosphere is comparable to the size of the instrument opening; thus, the analyzer performance is modeled by a Monte Carlo computer code that finds the aerosol particles trajectories within the instrument including both the electrostatic force and the forces from collisions of the aerosol particles with air molecules. Mass sensitivity curves obtained using the computer models are near to those obtained in the laboratory using an ion source. The first two flights of the instrument returned data showing the charge number densities of both positive and negative aerosol particles in four mass ranges.« less

Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

NASA Astrophysics Data System (ADS)

Elser, Miriam; Bozzetti, Carlo; El-Haddad, Imad; Maasikmets, Marek; Teinemaa, Erik; Richter, Rene; Wolf, Robert; Slowik, Jay G.; Baltensperger, Urs; Prévôt, André S. H.

2016-06-01

Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero ≤ 2.5 µm) in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR)-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning), and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded regional background

Spatial and temporal distributions of aerosol concentrations and depositions in Asia during the year 2010.

PubMed

Park, Soon-Ung; Lee, In-Hye; Joo, Seung Jin

2016-01-15

Aerosol Modeling System (AMS) that is consisted of the Asian Dust Aerosol Model2 (ADAM2) and the Community Multi-scale Air Quality (CMAQ) modeling system has been employed to document the spatial distributions of the monthly and the annual averaged concentration of both the Asian dust (AD) aerosol and the anthropogenic aerosol (AA), and their total depositions in the Asian region for the year 2010. It is found that the annual mean surface aerosol (PM10) concentrations in the Asian region affect in a wide region as a complex mixture of AA and AD aerosols; they are predominated by the AD aerosol in the AD source region of northern China and Mongolia with a maximum concentration exceeding 300 μg m(-3); AAs are predominated in the high pollutant emission regions of southern and eastern China and northern India with a maximum concentration exceeding 110 μg m(-3); while the mixture of AA and AD aerosols is dominated in the downwind regions extending from the Yellow Sea to the Northwest Pacific Ocean. It is also found that the annual total deposition of aerosols in the model domain is found to be 485 Tg (372 Tg by AD aerosol and 113 Tg by AA), of which 66% (319 Tg) is contributed by the dry deposition (305 Tg by AD aerosol and 14 Tg by AA) and 34% (166 Tg) by the wet deposition (66 Tg by AD aerosol and 100 Tg by AA), suggesting about 77% of the annual total deposition being contributed by the AD aerosol mainly through the dry deposition process and 24% of it by AA through the wet deposition process. The monthly mean aerosol concentration and the monthly total deposition show a significant seasonal variation with high in winter and spring, and low in summer. Copyright © 2015 Elsevier B.V. All rights reserved.

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

Vertically-resolved profiles of mass concentrations and particle backscatter coefficients of Asian dust plumes derived from lidar observations of silicon dioxide.

PubMed

Noh, Youngmin; Müller, Detlef; Shin, Sung-Kyun; Shin, Dongho; Kim, Young J

2016-01-01

This study presents a method to retrieve vertically-resolved profiles of dust mass concentrations by analyzing Raman lidar signals of silicon dioxide (quartz) at 546nm. The observed particle plumes consisted of mixtures of East Asian dust with anthropogenic pollution. Our method for the first time allows for extracting the contribution of the aerosol component "pure dust" contained in the aerosol type "polluted dust". We also propose a method that uses OPAC (Optical Properties of Aerosols and Clouds) and the mass concentrations profiles of dust in order to derive profiles of backscatter coefficients of pure dust in mixed dust/pollution plumes. The mass concentration of silicon dioxide (quartz) in the atmosphere can be estimated from the backscatter coefficient of quartz. The mass concentration of dust is estimated by the weight percentage (38-77%) of mineral quartz in Asian dust. The retrieved dust mass concentrations are classified into water soluble, nucleation, accumulation, mineral-transported and coarse mode according to OPAC. The mass mixing ratio of 0.018, 0.033, 0.747, 0.130 and 0.072, respectively, is used. Dust extinction coefficients at 550nm were calculated by using OPAC and prescribed number concentrations for each of the 5 components. Dust backscatter coefficients were calculated from the dust extinction coefficients on the basis of a lidar ratio of 45±3sr at 532nm. We present results of quartz-Raman measurements carried out on the campus of the Gwangju Institute of Science and Technology (35.10°N, 126.53°E) on 15, 16, and 21 March 2010. Copyright © 2015 Elsevier Ltd. All rights reserved.

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.

Implementing marine organic aerosols into the GEOS-Chem model

DOE PAGES

Gantt, B.; Johnson, M. S.; Crippa, M.; ...

2015-03-17

Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Modelmore » predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.« less

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

NASA Technical Reports Server (NTRS)

Johnson, Matthew S.

2015-01-01

Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field 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 (2Aerosol mass (PM 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3. Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An

Effect of Vaporizer Temperature on Ambient Non-Refractory Submicron Aerosol Composition and Mass Spectra Measured by the Aerosol Mass Spectrometer

EPA Science Inventory

Aerodyne Aerosol Mass Spectrometers (AMS) are routinely operated with a constant vaporizer temperature (Tvap) of 600^oC in order to facilitate quantitative detection of non-refractory submicron (NR-PM1) species. By analogy with other thermal desorption instrument...

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry

PubMed Central

Farmer, D. K.; Matsunaga, A.; Docherty, K. S.; Surratt, J. D.; Seinfeld, J. H.; Ziemann, P. J.; Jimenez, J. L.

2010-01-01

Organonitrates (ON) are important products of gas-phase oxidation of volatile organic compounds in the troposphere; some models predict, and laboratory studies show, the formation of large, multifunctional ON with vapor pressures low enough to partition to the particle phase. Organosulfates (OS) have also been recently detected in secondary organic aerosol. Despite their potential importance, ON and OS remain a nearly unexplored aspect of atmospheric chemistry because few studies have quantified particulate ON or OS in ambient air. We report the response of a high-resolution time-of-flight aerosol mass spectrometer (AMS) to aerosol ON and OS standards and mixtures. We quantify the potentially substantial underestimation of organic aerosol O/C, commonly used as a metric for aging, and N/C. Most of the ON-nitrogen appears as ions in the AMS, which are typically dominated by inorganic nitrate. Minor organonitrogen ions are observed although their identity and intensity vary between standards. We evaluate the potential for using fragment ratios, organonitrogen ions, ions, the ammonium balance of the nominally inorganic ions, and comparison to ion-chromatography instruments to constrain the concentrations of ON for ambient datasets, and apply these techniques to a field study in Riverside, CA. OS manifests as separate organic and sulfate components in the AMS with minimal organosulfur fragments and little difference in fragmentation from inorganic sulfate. The low thermal stability of ON and OS likely causes similar detection difficulties for other aerosol mass spectrometers using vaporization and/or ionization techniques with similar or larger energy, which has likely led to an underappreciation of these species. PMID:20194777

Changes in organic aerosol composition with aging inferred from aerosol mass spectra

NASA Astrophysics Data System (ADS)

Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.

2011-03-01

Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C). Heald et al. (2010) suggested that the bulk composition of OA line up in the Van Krevelen diagram with a slope ~ -1; such slope can potentially arise from the physical mixing of HOA and OOA, and/or from chemical aging of these components. In this study, we find that the OOA components from all sites occupy an area in the Van Krevelen space, with the evolution of OOA following a shallower slope of ~ -0.5, consistent with the additions of both acid and alcohol functional groups without fragmentation, and/or the addition of acid groups with C-C bond breakage. The importance of acid formation in OOA evolution is consistent with increasing f44 in the triangle plot with photochemical age. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.

Strong influence of deposition and vertical mixing on secondary organic aerosol concentrations in CMAQ and CAMx

NASA Astrophysics Data System (ADS)

Shu, Qian; Koo, Bonyoung; Yarwood, Greg; Henderson, Barron H.

2017-12-01

Differences between two air quality modeling systems reveal important uncertainties in model representations of secondary organic aerosol (SOA) fate. Two commonly applied models (CMAQ: Community Multiscale Air Quality; CAMx: Comprehensive Air Quality Model with extensions) predict very different OA concentrations over the eastern U.S., even when using the same source data for emissions and meteorology and the same SOA modeling approach. Both models include an option to output a detailed accounting of how each model process (e.g., chemistry, deposition, etc.) alters the mass of each modeled species, referred to as process analysis. We therefore perform a detailed diagnostic evaluation to quantify simulated tendencies (Gg/hr) of each modeled process affecting both the total model burden (Gg) of semi-volatile organic compounds (SVOC) in the gas (g) and aerosol (a) phases and the vertical structures to identify causes of concentration differences between the two models. Large differences in deposition (CMAQ: 69.2 Gg/d; CAMx: 46.5 Gg/d) contribute to significant OA bias in CMAQ relative to daily averaged ambient concentration measurements. CMAQ's larger deposition results from faster daily average deposition velocities (VD) for both SVOC (g) (VD,cmaq = 2.15 × VD,camx) and aerosols (VD,cmaq = 4.43 × Vd,camx). Higher aerosol deposition velocity would be expected to cause similar biases for inert compounds like elemental carbon (EC), but this was not seen. Daytime low-biases in EC were also simulated in CMAQ as expected but were offset by nighttime high-biases. Nighttime high-biases were a result of overly shallow mixing in CMAQ leading to a higher fraction of EC total atmospheric mass in the first layer (CAMx: 5.1-6.4%; CMAQ: 5.6-6.9%). Because of the opposing daytime and nighttime biases, the apparent daily average bias for EC is reduced. For OA, there are two effects of reduced vertical mixing: SOA and SVOC are concentrated near the surface, but SOA yields are reduced

The influence of continental air masses on the aerosols and nutrients deposition over the western North Pacific

NASA Astrophysics Data System (ADS)

Fu, Jiangping; Wang, Bo; Chen, Ying; Ma, Qingwei

2018-01-01

The air masses transported from East Asia have a strong impact on the aerosol properties and deposition in the marine boundary layer of the western North Pacific (WNP) during winter and spring. We joined a cruise between 17 Mar. and 22 Apr. 2014 and investigated the changes of aerosol composition and size distribution over the remote WNP and marginal seas. Although the secondary aerosol species (SO42-, NO3- and NH4+) in remote WNP were influenced significantly by the continental transport, NH4+ concentrations were lower than 2.7 μg m-3 in most sampling days and not correlated with non-sea-salt (nss)-SO42- suggesting that the ocean could be a primary source of NH4+. Moderate Cl- depletion (23%) was observed in remote WNP, and the inverse relationship between Cl- depletion percentages and nss-K+ in aerosols suggested that the transport of biomass burning smoke from East Asia might be a vital extra source of Cl-. Both Asian dust and haze events were encountered during the cruise. Asian dust carried large amounts of crustal elements such as Al and Ti to the WNP, and the dusty Fe deposition may double its background concentration in seawater. Differently, a dramatic increase of dry deposition flux of dissolved particulate inorganic nitrogen was observed during the haze event. Our study reveals that the transport of different continental air masses may have distinct biogeochemical impacts on the WNP by increasing the fluxes of different nutrient elements and potentially changing the nutrient stoichiometry.

Future aerosol concentrations in Europe: Effects of changing meteorology and emissions

NASA Astrophysics Data System (ADS)

Coleman, Liz; Martin, Damien; Radalescu, Razvan; O'Dowd, Colin

2013-05-01

The ambient particulate matter concentrations are assessed using annual simulations for model validation period 2006, and for future time-slice years 2030, 2050 and 2100 under RCP scenario 6.0. Meteorological initial and boundary conditions are procured from ECHAM5-HAMMOC global simulations. The contribution of natural and anthropogenic processes to aerosol concentrations are assessed with particular emphasis on accumulation mode sea salt, organic enrichment thereof and future levels of secondary organic aerosol from isoprene.

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.

Origin of atmospheric aerosols at the Pierre Auger Observatory using studies of air mass trajectories in South America

NASA Astrophysics Data System (ADS)

Aab, A.; Abreu, P.; Aglietta, M.; Ahlers, M.; Ahn, E. J.; Albuquerque, I. F. M.; Allekotte, I.; Allen, J.; Allison, P.; Almela, A.; Alvarez Castillo, J.; Alvarez-Muñiz, J.; Alves Batista, R.; Ambrosio, M.; Aminaei, A.; Anchordoqui, L.; Andringa, S.; Antičić, T.; Aramo, C.; Arqueros, F.; Asorey, H.; Assis, P.; Aublin, J.; Ave, M.; Avenier, M.; Avila, G.; Badescu, A. M.; Barber, K. B.; Bardenet, R.; Bäuml, J.; Baus, C.; Beatty, J. J.; Becker, K. H.; Bellido, J. A.; BenZvi, S.; Berat, C.; Bertou, X.; Biermann, P. L.; Billoir, P.; Blanco, F.; Blanco, M.; Bleve, C.; Blümer, H.; Boháčová, M.; Boncioli, D.; Bonifazi, C.; Bonino, R.; Borodai, N.; Brack, J.; Brancus, I.; Brogueira, P.; Brown, W. C.; Buchholz, P.; Bueno, A.; Buscemi, M.; Caballero-Mora, K. S.; Caccianiga, B.; Caccianiga, L.; Candusso, M.; Caramete, L.; Caruso, R.; Castellina, A.; Cataldi, G.; Cazon, L.; Cester, R.; Cheng, S. H.; Chiavassa, A.; Chinellato, J. A.; Chudoba, J.; Cilmo, M.; Clay, R. W.; Cocciolo, G.; Colalillo, R.; Collica, L.; Coluccia, M. R.; Conceição, R.; Contreras, F.; Cooper, M. J.; Coutu, S.; Covault, C. E.; Criss, A.; Cronin, J.; Curutiu, A.; Dallier, R.; Daniel, B.; Dasso, S.; Daumiller, K.; Dawson, B. R.; de Almeida, R. M.; De Domenico, M.; de Jong, S. J.; De La Vega, G.; de Mello Junior, W. J. M.; de Mello Neto, J. R. T.; De Mitri, I.; de Souza, V.; de Vries, K. D.; del Peral, L.; Deligny, O.; Dembinski, H.; Dhital, N.; Di Giulio, C.; Di Matteo, A.; Diaz, J. C.; Díaz Castro, M. L.; Diep, P. N.; Diogo, F.; Dobrigkeit, C.; Docters, W.; D'Olivo, J. C.; Dong, P. N.; Dorofeev, A.; dos Anjos, J. C.; Dova, M. T.; Ebr, J.; Engel, R.; Erdmann, M.; Escobar, C. O.; Espadanal, J.; Etchegoyen, A.; Facal San Luis, P.; Falcke, H.; Fang, K.; Farrar, G.; Fauth, A. C.; Fazzini, N.; Ferguson, A. P.; Fick, B.; Figueira, J. M.; Filevich, A.; Filipčič, A.; Foerster, N.; Fox, B. D.; Fracchiolla, C. E.; Fraenkel, E. D.; Fratu, O.; Fröhlich, U.; Fuchs, B.; Gaior, R.; Gamarra, R. F.; Gambetta, S.; García, B.; Garcia Roca, S. T.; Garcia-Gamez, D.; Garcia-Pinto, D.; Garilli, G.; Gascon Bravo, A.; Gemmeke, H.; Ghia, P. L.; Giammarchi, M.; Giller, M.; Gitto, J.; Glaser, C.; Glass, H.; Gomez Albarracin, F.; Gómez Berisso, M.; Gómez Vitale, P. F.; Gonçalves, P.; Gonzalez, J. G.; Gookin, B.; Gorgi, A.; Gorham, P.; Gouffon, P.; Grebe, S.; Griffith, N.; Grillo, A. F.; Grubb, T. D.; Guardincerri, Y.; Guarino, F.; Guedes, G. P.; Hansen, P.; Harari, D.; Harrison, T. A.; Harton, J. L.; Haungs, A.; Hebbeker, T.; Heck, D.; Herve, A. E.; Hill, G. C.; Hojvat, C.; Hollon, N.; Holt, E.; Homola, P.; Hörandel, J. R.; Horvath, P.; Hrabovský, M.; Huber, D.; Huege, T.; Insolia, A.; Isar, P. G.; Jansen, S.; Jarne, C.; Josebachuili, M.; Kadija, K.; Kambeitz, O.; Kampert, K. H.; Karhan, P.; Kasper, P.; Katkov, I.; Kégl, B.; Keilhauer, B.; Keivani, A.; Kemp, E.; Kieckhafer, R. M.; Klages, H. O.; Kleifges, M.; Kleinfeller, J.; Knapp, J.; Krause, R.; Krohm, N.; Krömer, O.; Kruppke-Hansen, D.; Kuempel, D.; Kunka, N.; La Rosa, G.; LaHurd, D.; Latronico, L.; Lauer, R.; Lauscher, M.; Lautridou, P.; Le Coz, S.; Leão, M. S. A. B.; Lebrun, D.; Lebrun, P.; Leigui de Oliveira, M. A.; Letessier-Selvon, A.; Lhenry-Yvon, I.; Link, K.; López, R.; Lopez Agüera, A.; Louedec, K.; Lozano Bahilo, J.; Lu, L.; Lucero, A.; Ludwig, M.; Lyberis, H.; Maccarone, M. C.; Malacari, M.; Maldera, S.; Maller, J.; Mandat, D.; Mantsch, P.; Mariazzi, A. G.; Marin, V.; Mariş, I. C.; Marquez Falcon, H. R.; Marsella, G.; Martello, D.; Martin, L.; Martinez, H.; Martínez Bravo, O.; Martraire, D.; Masías Meza, J. J.; Mathes, H. J.; Matthews, J.; Matthews, J. A. J.; Matthiae, G.; Maurel, D.; Maurizio, D.; Mayotte, E.; Mazur, P. O.; Medina, C.; Medina-Tanco, G.; Melissas, M.; Melo, D.; Menichetti, E.; Menshikov, A.; Messina, S.; Meyhandan, R.; Mićanović, S.; Micheletti, M. I.; Middendorf, L.; Minaya, I. A.; Miramonti, L.; Mitrica, B.; Molina-Bueno, L.; Mollerach, S.; Monasor, M.; Monnier Ragaigne, D.; Montanet, F.; Morales, B.; Morello, C.; Moreno, J. C.; Mostafá, M.; Moura, C. A.; Muller, M. A.; Müller, G.; Münchmeyer, M.; Mussa, R.; Navarra, G.; Navarro, J. L.; Navas, S.; Necesal, P.; Nellen, L.; Nelles, A.; Neuser, J.; Nhung, P. T.; Niechciol, M.; Niemietz, L.; Niggemann, T.; Nitz, D.; Nosek, D.; Nožka, L.; Oehlschläger, J.; Olinto, A.; Oliveira, M.; Ortiz, M.; Pacheco, N.; Pakk Selmi-Dei, D.; Palatka, M.; Pallotta, J.; Palmieri, N.; Parente, G.; Parra, A.; Pastor, S.; Paul, T.; Pech, M.; Pȩkala, J.; Pelayo, R.; Pepe, I. M.; Perrone, L.; Pesce, R.; Petermann, E.; Petrera, S.; Petrolini, A.; Petrov, Y.; Piegaia, R.; Pierog, T.; Pieroni, P.; Pimenta, M.; Pirronello, V.; Platino, M.; Plum, M.; Pontz, M.; Porcelli, A.; Preda, T.; Privitera, P.; Prouza, M.; Quel, E. J.; Querchfeld, S.; Quinn, S.; Rautenberg, J.; Ravel, O.; Ravignani, D.; Revenu, B.; Ridky, J.; Riggi, S.; Risse, M.; Ristori, P.; Rivera, H.; Rizi, V.; Roberts, J.; Rodrigues de Carvalho, W.; Rodriguez Cabo, I.; Rodriguez Fernandez, G.; Rodriguez Martino, J.; Rodriguez Rojo, J.; Rodríguez-Frías, M. D.; Ros, G.; Rosado, J.; Rossler, T.; Roth, M.; Rouillé-d'Orfeuil, B.; Roulet, E.; Rovero, A. C.; Rühle, C.; Saffi, S. J.; Saftoiu, A.; Salamida, F.; Salazar, H.; Salesa Greus, F.; Salina, G.; Sánchez, F.; Sanchez-Lucas, P.; Santo, C. E.; Santos, E.; Santos, E. M.; Sarazin, F.; Sarkar, B.; Sarmento, R.; Sato, R.; Scharf, N.; Scherini, V.; Schieler, H.; Schiffer, P.; Schmidt, A.; Scholten, O.; Schoorlemmer, H.; Schovánek, P.; Schröder, F. G.; Schulz, A.; Schulz, J.; Sciutto, S. J.; Scuderi, M.; Segreto, A.; Settimo, M.; Shadkam, A.; Shellard, R. C.; Sidelnik, I.; Sigl, G.; Sima, O.; Śmiałkowski, A.; Šmída, R.; Snow, G. R.; Sommers, P.; Sorokin, J.; Spinka, H.; Squartini, R.; Srivastava, Y. N.; Stanič, S.; Stapleton, J.; Stasielak, J.; Stephan, M.; Straub, M.; Stutz, A.; Suarez, F.; Suomijärvi, T.; Supanitsky, A. D.; Šuša, T.; Sutherland, M. S.; Swain, J.; Szadkowski, Z.; Szuba, M.; Tapia, A.; Tartare, M.; Taşcău, O.; Thao, N. T.; Tiffenberg, J.; Timmermans, C.; Tkaczyk, W.; Todero Peixoto, C. J.; Toma, G.; Tomankova, L.; Tomé, B.; Tonachini, A.; Torralba Elipe, G.; Torres Machado, D.; Travnicek, P.; Tridapalli, D. B.; Trovato, E.; Tueros, M.; Ulrich, R.; Unger, M.; Valdés Galicia, J. F.; Valiño, I.; Valore, L.; van Aar, G.; van den Berg, A. M.; van Velzen, S.; van Vliet, A.; Varela, E.; Vargas Cárdenas, B.; Varner, G.; Vázquez, J. R.; Vázquez, R. A.; Veberič, D.; Verzi, V.; Vicha, J.; Videla, M.; Villaseñor, L.; Wahlberg, H.; Wahrlich, P.; Wainberg, O.; Walz, D.; Watson, A. A.; Weber, M.; Weidenhaupt, K.; Weindl, A.; Werner, F.; Westerhoff, S.; Whelan, B. J.; Widom, A.; Wieczorek, G.; Wiencke, L.; Wilczyńska, B.; Wilczyński, H.; Will, M.; Williams, C.; Winchen, T.; Wundheiler, B.; Wykes, S.; Yamamoto, T.; Yapici, T.; Younk, P.; Yuan, G.; Yushkov, A.; Zamorano, B.; Zas, E.; Zavrtanik, D.; Zavrtanik, M.; Zaw, I.; Zepeda, A.; Zhou, J.; Zhu, Y.; Zimbres Silva, M.; Ziolkowski, M.; Curci, G.

2014-11-01

The Pierre Auger Observatory is making significant contributions towards understanding the nature and origin of ultra-high energy cosmic rays. One of its main challenges is the monitoring of the atmosphere, both in terms of its state variables and its optical properties. The aim of this work is to analyse aerosol optical depth τa(z) values measured from 2004 to 2012 at the observatory, which is located in a remote and relatively unstudied area of Pampa Amarilla, Argentina. The aerosol optical depth is in average quite low - annual mean τa(3.5 km) ∼ 0.04 - and shows a seasonal trend with a winter minimum - τa(3.5 km) ∼ 0.03 -, and a summer maximum - τa(3.5 km) ∼ 0.06 -, and an unexpected increase from August to September - τa(3.5 km) ∼ 0.055. We computed backward trajectories for the years 2005 to 2012 to interpret the air mass origin. Winter nights with low aerosol concentrations show air masses originating from the Pacific Ocean. Average concentrations are affected by continental sources (wind-blown dust and urban pollution), whilst the peak observed in September and October could be linked to biomass burning in the northern part of Argentina or air pollution coming from surrounding urban areas.

MASS SPECTROMETRY OF INDIVIDUAL AEROSOL PARTICLES. (R823980)

EPA Science Inventory

Typically, in real-time aerosol mass spectrometry (RTAMS), individual airborne particles
are ablated and ionized with a single focused laser pulse. This technique yields information that
permits bulk characterization of the particle, but information about the particle's sur...

Comprehensive characterization of PM2.5 aerosols in Singapore

NASA Astrophysics Data System (ADS)

Balasubramanian, R.; Qian, W.-B.; Decesari, S.; Facchini, M. C.; Fuzzi, S.

2003-08-01

A comprehensive characterization of PM2.5 aerosols collected in Singapore from January through December 2000 is presented. The annual average mass concentration of PM2.5 was 27.2 μg/m3. The atmospheric loading of PM2.5 was elevated sporadically from March through May, mainly due to advection of biomass burning (deliberate fires to clear plantation areas) impacted air masses from Sumatra, Indonesia. Satellite images of the area, trajectory calculations, and surface wind direction data are in support of the transport of pyrogenic products from Sumatra toward Singapore. Aerosol samples collected during the dry season were analyzed for water-soluble ions, water-soluble organic compounds (WSOC), elemental carbon (EC), organic carbon, and trace elements using a number of analytical techniques. The major components were sulfate, EC, water-soluble carbonaceous materials, and water-insoluble carbonaceous materials. Aerosol WSOC were characterized based on a combination of chromatographic separations by ion exchange chromatography, functional group investigation by proton nuclear magnetic resonance, and total organic carbon determination. The comprehensive chemical characterization of PM2.5 particles revealed that both non-sea-salt sufate (nss-SO42-) and carbonaceous aerosols mainly contributed to the increase in the mass concentration of aerosols during the smoke haze period. Using a mass closure test (a mass balance), we determined whether the physical measurement of gravimetric fine PM concentration of a sample is equal to the summed concentrations of the individually identified chemical constituents (measured or inferred) in the sample. The sum of the determined groups of aerosol components and the gravimetrically determined mass agreed reasonably well. Principal component analysis was performed from the combined data set, and five factors were observed: a soil dust component, a metallurgical industry factor, a factor representing emissions from biomass burning and

Estimation of surface-level PM2.5 concentration using aerosol optical thickness through aerosol type analysis method

NASA Astrophysics Data System (ADS)

Chen, Qi-Xiang; Yuan, Yuan; Huang, Xing; Jiang, Yan-Qiu; Tan, He-Ping

2017-06-01

Surface-level particulate matter is closely related to column aerosol optical thickness (AOT). Previous researches have successfully used column AOT and different meteorological parameters to estimate surface-level PM concentration. In this study, the performance of a selected linear model that estimates surface-level PM2.5 concentration was evaluated following the aerosol type analysis method (ATAM) for the first time. We utilized 443 daily average data for Xuzhou, Jiangsu province, collected using Aerosol Robotic Network (AERONET) during the period October 2013 to April 2016. Several parameters including atmospheric boundary layer height (BLH), relative humidity (RH), and effective radius of the aerosol size distribution (Ref) were used to assess the relationship between the column AOT and PM2.5 concentration. By including the BLH, ambient RH, and effective radius, the correlation (R2) increased from 0.084 to 0.250 at Xuzhou, and with the use of ATAM, the correlation increased further to 0.335. To compare the results, 450 daily average data for Beijing, pertaining to the same period, were utilized. The study found that model correlations improved by varying degrees in different seasons and at different sites following ATAM. The average urban industry (UI) aerosol ratios at Xuzhou and Beijing were 0.792 and 0.451, respectively, demonstrating poorer air conditions at Xuzhou. PM2.5 estimation at Xuzhou showed lower correlation (R2 = 0.335) compared to Beijing (R2 = 0.407), and the increase of R2 at Xuzhou and Beijing site following use of ATAM were 33.8% and 12.4%, respectively.

Black Carbon Concentration from Worldwide Aerosol Robotic Network (AERONET)

NASA Technical Reports Server (NTRS)

Schuster, Greg; Dubovik, Oleg; Holben, Brent; Clothiaux, Eugene

2008-01-01

Worldwide black carbon concentration measurements are needed to assess the efficacy of the carbon emissions inventory and transport model output. This requires long-term measurements in many regions, as model success in one region or season does not apply to all regions and seasons. AERONET is an automated network of more than 180 surface radiometers located throughout the world. The sky radiance measurements obtained by AERONET are inverted to provide column-averaged aerosol refractive indices and size distributions for the AERONET database, which we use to derive column-averaged black carbon concentrations and specific absorptions that are constrained by the measured radiation field. This provides a link between AERONET sky radiance measurements and the elemental carbon concentration of transport models without the need for an optics module in the transport model. Knowledge of both the black carbon concentration and aerosol absorption optical depth (i.e., input and output of the optics module) will enable improvements to the transport model optics module.

Satellite measurements of aerosol mass and transport

NASA Technical Reports Server (NTRS)

Fraser, R. S.; Kaufman, Y. J.; Mahoney, R. L.

1984-01-01

The aerosol optical thickness over land is derived from satellite measurements of the radiance of scattered sunlight. These data are used to estimate the columnar mass density of particulate sulfur on a day with a large amount of sulfur. The horizontal transport of the particulate sulfur is calculated using wind vectors measured with rawins.

Outdoor and indoor aerosol size, number, mass and compositional dynamics at an urban background site during warm season

NASA Astrophysics Data System (ADS)

Talbot, N.; Kubelova, L.; Makes, O.; Cusack, M.; Ondracek, J.; Vodička, P.; Schwarz, J.; Zdimal, V.

2016-04-01

This paper describes the use of a unique valve switching system that allowed for high temporal resolution indoor and outdoor data to be collected concurrently from online C-ToF-AMS, SMPS and OC/EC, and offline BLPI measurements. The results reveal near real-time dynamic aerosol behaviour along a migration path from an outdoor to indoor environment. An outdoor reduction in NR-PM1 mass concentration occurred daily from AM (06:00-12:00) to PM (12:00-18:00). SO4 (26%-37%) [AM/PM] increased proportionally during afternoons at the expense of NO3 (18%-7%). The influences of mixing height, temperature and solar radiation were considered against the mean mass concentration loss for each species. Losses were then calculated according to species via a basic input/output model. NO3 lost the most mass during afternoon periods, which we attribute to the accelerated dissociation of NH4NO3 through increasing temperature and decreasing relative humidity. Indoor/outdoor (I/O) ratios varied from 0.46 for <40 nm to 0.65 for >100 nm. These ratios were calculated using average SMPS PNC measurements over the full campaign and corroborated using a novel technique of calculating I/O penetration ratios through the indoor migration of particles during a new particle formation event. This ratio was then used to observe changes in indoor composition relative to those outdoors. Indoor sampling was carried out in an undisturbed room with no known sources. Indoor concentrations were found to be proportional to those outdoors, with organic matter [2.7 μg/m3] and SO4 [1.7 μg/m3] being the most prominent species. These results are indicative of fairly rapid aerosol penetration, a source-free indoor environment and small afternoon I/O temperature gradients. Fine fraction NO3 was observed indoors in both real-time AMS PM1 and off-line BLPI measurements. Greater mass concentration losses were observed from filter measurements, highlighting an important time dependency factor when investigating semi

Progress Toward a Global, EOS-Era Aerosol Air Mass Type Climatology

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.

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 eleven years. 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. The next frontier in assessing aerosol radiative forcing of climate is aerosol type, and in particular, the absorption properties of major aerosol air masses. This presentation will focus on the prospects for constraining aerosol type globally, and the steps we are taking to apply a combination of satellite and suborbital data to this challenge.

The relationship between aerosol particles chemical composition and optical properties to identify the biomass burning contribution to fine particles concentration: a case study for São Paulo city, Brazil.

PubMed

de Miranda, Regina Maura; Lopes, Fabio; do Rosário, Nilton Évora; Yamasoe, Marcia Akemi; Landulfo, Eduardo; de Fatima Andrade, Maria

2016-12-01

The air quality in the Metropolitan Area of São Paulo (MASP) is primarily determined by the local pollution source contribution, mainly the vehicular fleet, but there is a concern about the role of remote sources to the fine mode particles (PM 2.5 ) concentration and composition. One of the most important remote sources of atmospheric aerosol is the biomass burning emissions from São Paulo state's inland and from the central and north portions of Brazil. This study presents a synergy of different measurements of atmospheric aerosol chemistry and optical properties in the MASP in order to show how they can be used as a tool to identify particles from local and remote sources. For the clear identification of the local and remote source contribution, aerosol properties measurements at surface level were combined with vertical profiles information. Over 15 days in the austral winter of 2012, particulate matter (PM) was collected using a cascade impactor and a Partisol sampler in São Paulo City. Mass concentrations were determined by gravimetry, black carbon concentrations by reflectance, and trace element concentrations by X-ray fluorescence. Aerosol optical properties were studied using a multifilter rotating shadowband radiometer (MFRSR), a Lidar system and satellite data. Optical properties, concentrations, size distributions, and elemental composition of atmospheric particles were strongly related and varied according to meteorological conditions. During the sampling period, PM mean mass concentrations were 17.4 ± 10.1 and 15.3 ± 6.9 μg/m 3 for the fine and coarse fractions, respectively. The mean aerosol optical depths at 415 nm and Ångström exponent (AE) over the whole period were 0.29 ± 0.14 and 1.35 ± 0.11, respectively. Lidar ratios reached values of 75 sr. The analyses of the impacts of an event of biomass burning smoke transport to the São Paulo city revealed significant changing on local aerosol concentrations and optical parameters

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry.

PubMed

Farmer, D K; Matsunaga, A; Docherty, K S; Surratt, J D; Seinfeld, J H; Ziemann, P J; Jimenez, J L

2010-04-13

Organonitrates (ON) are important products of gas-phase oxidation of volatile organic compounds in the troposphere; some models predict, and laboratory studies show, the formation of large, multifunctional ON with vapor pressures low enough to partition to the particle phase. Organosulfates (OS) have also been recently detected in secondary organic aerosol. Despite their potential importance, ON and OS remain a nearly unexplored aspect of atmospheric chemistry because few studies have quantified particulate ON or OS in ambient air. We report the response of a high-resolution time-of-flight aerosol mass spectrometer (AMS) to aerosol ON and OS standards and mixtures. We quantify the potentially substantial underestimation of organic aerosol O/C, commonly used as a metric for aging, and N/C. Most of the ON-nitrogen appears as NO(x)+ ions in the AMS, which are typically dominated by inorganic nitrate. Minor organonitrogen ions are observed although their identity and intensity vary between standards. We evaluate the potential for using NO(x)+ fragment ratios, organonitrogen ions, HNO(3)+ ions, the ammonium balance of the nominally inorganic ions, and comparison to ion-chromatography instruments to constrain the concentrations of ON for ambient datasets, and apply these techniques to a field study in Riverside, CA. OS manifests as separate organic and sulfate components in the AMS with minimal organosulfur fragments and little difference in fragmentation from inorganic sulfate. The low thermal stability of ON and OS likely causes similar detection difficulties for other aerosol mass spectrometers using vaporization and/or ionization techniques with similar or larger energy, which has likely led to an underappreciation of these species.

Effects of turbulence on mixed-phase deep convective clouds under different basic-state winds and aerosol concentrations

NASA Astrophysics Data System (ADS)

Lee, Hyunho; Baik, Jong-Jin; Han, Ji-Young

2014-12-01

The effects of turbulence-induced collision enhancement (TICE) on mixed-phase deep convective clouds are numerically investigated using a 2-D cloud model with bin microphysics for uniform and sheared basic-state wind profiles and different aerosol concentrations. Graupel particles account for the most of the cloud mass in all simulation cases. In the uniform basic-state wind cases, graupel particles with moderate sizes account for some of the total graupel mass in the cases with TICE, whereas graupel particles with large sizes account for almost all the total graupel mass in the cases without TICE. This is because the growth of ice crystals into small graupel particles is enhanced due to TICE. The changes in the size distributions of graupel particles due to TICE result in a decrease in the mass-averaged mean terminal velocity of graupel particles. Therefore, the downward flux of graupel mass, and thus the melting of graupel particles, is reduced due to TICE, leading to a decrease in the amount of surface precipitation. Moreover, under the low aerosol concentration, TICE increases the sublimation of ice particles, consequently playing a partial role in reducing the amount of surface precipitation. The effects of TICE are less pronounced in the sheared basic-state wind cases than in the uniform basic-state wind cases because the number of ice crystals is much smaller in the sheared basic-state wind cases than in the uniform basic-state wind cases. Thus, the size distributions of graupel particles in the cases with and without TICE show little difference.

Estimating Marine Aerosol Particle Volume and Number from Maritime Aerosol Network Data

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Smirnov, A.; Hsu, N. C.; Munchak, L. A.; Holben, B. N.

2012-01-01

As well as spectral aerosol optical depth (AOD), aerosol composition and concentration (number, volume, or mass) are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN) cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET) inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS) data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The average solution MODIS dataset agrees more closely with MAN than the best solution dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data.

Aerosol characteristics and sources for the Amazon basin during the wet season

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

Artaxo, P.; Maenhaut, W.; Storms, H.

1990-09-20

Fine (< 2.0 {mu}m) and coarse (2.0 - 15 {mu}m) aerosol fractions were collected using stacked filter units, at three sites under the forest canopy and at three levels of a tower inside the jungle. Particle-induced x-ray emission (PIXE) was used to measure concentrations Na, Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sr, Zr, and Pb. Morphological and trace element measurements of individual particles were carried out by automated electron probe x-ray microanalysis. Gravimetric analysis was performed to obtain the fine and coarse aerosol mass concentration. The concentrations ofmore » soil dust related elements (Al, Si, Ti, Fe, Mn) were 5 times larger in the wet season compared to the 1985 ABLE 2A dry season experiment. Biogenic aerosol related elements in the fine fraction showed lower concentrations in the wet season. Fine aerosol mass concentration averaged only 2.1 {plus minus} 0.7 {mu}g m{sup {minus}3}, while the average coarse mass concentration was 6.1 {plus minus} 1.8 {mu}g m{sup {minus}3}. Sulfur concentrations averaged 76 {plus minus} 14 ng m{sup {minus}3} in the fine fraction and 37 {plus minus} 9 ng m{sup {minus}3} in the coarse fraction. Only two factors explained about 90% of the data variability for the fine and coarse aerosol fractions. These were soil dust (represented mainly by Al, Si, Ti, Mn, and Fe) and biogenic aerosol (represented by K, P, Cl, S, Zn, and the aerosol mass concentration). Biogenic particles account for 55-95% of the airborne concentrations and consisted of leaf fragments, pollen grains, fungi, algae, and other types of particles. It is possible that biogenic particles can play an important role in the global aerosol budget and in the global biogeochemical cycles of various elements.« less

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

NASA Astrophysics Data System (ADS)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

Chemical characterization of fine particulate matter in Changzhou, China, and source apportionment with offline aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Ye, Zhaolian; Liu, Jiashu; Gu, Aijun; Feng, Feifei; Liu, Yuhai; Bi, Chenglu; Xu, Jianzhong; Li, Ling; Chen, Hui; Chen, Yanfang; Dai, Liang; Zhou, Quanfa; Ge, Xinlei

2017-02-01

Knowledge of aerosol chemistry in densely populated regions is critical for effective reduction of air pollution, while such studies have not been conducted in Changzhou, an important manufacturing base and populated city in the Yangtze River Delta (YRD), China. This work, for the first time, performed a thorough chemical characterization on the fine particulate matter (PM2.5) samples, collected during July 2015 to April 2016 across four seasons in this city. A suite of analytical techniques was employed to measure the organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), water-soluble inorganic ions (WSIIs), trace elements, and polycyclic aromatic hydrocarbons (PAHs) in PM2.5; in particular, an Aerodyne soot particle aerosol mass spectrometer (SP-AMS) was deployed to probe the chemical properties of water-soluble organic aerosol (WSOA). The average PM2.5 concentration was found to be 108.3 µg m-3, and all identified species were able to reconstruct ˜ 80 % of the PM2.5 mass. The WSIIs occupied about half of the PM2.5 mass (˜ 52.1 %), with SO42-, NO3-, and NH4+ as the major ions. On average, nitrate concentrations dominated over sulfate (mass ratio of 1.21), indicating that traffic emissions were more important than stationary sources. OC and EC correlated well with each other and the highest OC / EC ratio (5.16) occurred in winter, suggesting complex OC sources likely including both secondary and primary ones. Concentrations of eight trace elements (Mn, Zn, Al, B, Cr, Cu, Fe, Pb) can contribute up to ˜ 5.0 % of PM2.5 during winter. PAH concentrations were also high in winter (140.25 ng m-3), which were predominated by median/high molecular weight PAHs with five and six rings. The organic matter including both water-soluble and water-insoluble species occupied ˜ 21.5 % of the PM2.5 mass. SP-AMS determined that the WSOA had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), nitrogen-to-carbon (N / C), and organic

Spatial and Temporal Patterns in the Carbon Isotopic Signal of Leaf Wax Aerosols in Continental Air Masses: Linkages with Ecosystem Discrimination

NASA Astrophysics Data System (ADS)

Weber, J.; Conte, M. H.

2006-12-01

Temporal and spatial variations in the concentration and isotopic composition of atmospheric carbon dioxide can be used to estimate the relative magnitudes of the terrestrial and oceanic carbon sinks. An important model parameter is the terrestrial photosynthetic carbon isotopic fractionation of CO2 (Δ), yet estimating Δ over the large spatial scales required by models remains problematic. Epiculticular leaf waxes appear to closely reflect the plant's carbon isotopic discrimination; therefore, the ablated wax aerosols present in well-mixed continental air masses may be used as a proxy to estimate the magnitude of Δ integrated over large (subcontinental) spatial scales. Over the last several years, we have been conducting time-series studies of wax aerosol molecular and isotopic composition at strategically located sites (Maine, northern Alaska, Florida, Bermuda, Barbados) which receive continental air masses passing over major terrestrial biomes (northern temperate/ecotonal boreal forests, tundra, southern US pine/hardwood forests, North American and north African). In this presentation, we describe and contrast patterns of wax aerosol-derived estimates of Δ at these sites. In North American air masses, estimates of Δ range from 14.5-20.5 using the concentration-weighted average δ13C of wax n-acids and from 13.5-19.5 for the wax n-alcohols. Seasonal trends observed in the Florida (southern US) and Bermuda samples (mixed North American air masses) indicate maximum discrimination in early spring and minimum discrimination during the summer dry season. In northern US and high latitude air masses, seasonal trends are less pronounced but in general temporally offset with highest discrimination occurring during late summer. At Barbados, which is dominated by north African air masses passing over regions largely comprised of arid C4 grasslands, estimated Δ for the wax n-acids is significantly lower (14.0-15.5 per mil), consistent with a higher predominance of C4

Relationship between fluid bed aerosol generator operation and the aerosol produced

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

Carpenter, R.L.; Yerkes, K.

1980-12-01

The relationships between bed operation in a fluid bed aerosol generator and aerosol output were studied. A two-inch diameter fluid bed aerosol generator (FBG) was constructed using stainless steel powder as a fluidizing medium. Fly ash from coal combustion was aerosolized and the influence of FBG operating parameters on aerosol mass median aerodynamic diameter (MMAD), geometric standard deviation (sigma/sub g/) and concentration was examined. In an effort to extend observations on large fluid beds to small beds using fine bed particles, minimum fluidizing velocities and elutriation constant were computed. Although FBG minimum fluidizing velocity agreed well with calculations, FBG elutriationmore » constant did not. The results of this study show that the properties of aerosols produced by a FBG depend on fluid bed height and air flow through the bed after the minimum fluidizing velocity is exceeded.« less

Chemical Composition of African Biomass Burning Aerosols Over the Southeast Atlantic: Aerosol Mass Spectrometer Results from the 2016 and 2017 ORACLES Field Campaigns.

NASA Astrophysics Data System (ADS)

Dobracki, A. N.; Howell, S. G.; Freitag, S.; Smirnow, N.; Podolske, J. R.

2017-12-01

Biomass burning (BB) is one of the largest contributors of anthropogenic aerosols in the atmosphere. During BB events, organic and inorganic gases and particles are emitted into the atmosphere. Because of their abundance, particle size, and radiative properties, BB aerosols play an important role in global climate. Southern Africa produces 30% of the Earth's BB aerosol particles. Organics, Nitrates, sulfates, and refractory black carbon, along with other chemical species are lofted into the free troposphere and transported over the Southeast Atlantic Ocean. However, considerate uncertainty remains in the chemical composition of these plumes with its large variety of organic and inorganic species. As part of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2017 airborne field campaigns, an Aerosol Mass Spectrometer (AMS) was used to sample the chemical composition and chemical structure of the aerosol in this region. Results show constant vertical stratification within the plume over the course of the campaign (August 2017 / September 2016). Using nitrate (NO3) and organic carbon (OC) as two tracers, the structure of the September 2016 plume had a ratio of 1:8 (NO3:OC) in the upper plume (3km-5km), while the lower plume (1km-2.5km) had a ratio of 1:12 (NO3:OC). AMS measurements were supported by carbon monoxide (CO) and carbon dioxide (CO2) measurements. This data revealed a modified combustion efficiency (MCE= ΔCO2/ΔCO2 + ΔCO) of <0.97 in the upper plume, and a higher MCE > 0.97 in the lower plume. An MCE above 0.9 represents efficient burning processes. Additionally, concentrations of C2(H2O)2 (m/z60), a common chemical fragment from breaking up carbohydrates (primarily levoglucosan) emitted by burning biomass only represented <1% of total organics throughout the campaign. These low concentrations are due to efficient combustion rather than oxidation during transport. These results are consistent with earlier studies of

Photochemical Cycling of Humic-Like Substances in Atmospheric Aerosols

NASA Astrophysics Data System (ADS)

Rincon, A. G.; Guzman, M. I.; Hoffmann, M. R.; Colussi, A. J.

2007-12-01

Colored, humic-like substances (HULIS) arising from the biodegradation of organic detritus are widespread in natural surface waters, where they ultimately undergo solar photolysis into small alpha-dicarbonylic species, such as glyoxal, glyoxylic and pyruvic acids. Diversely generated and chemically dissimilar HULIS are also found in the atmospheric aerosol. How are significant levels of colored HULIS produced and sustained in the concentrated aerosol phase under intense solar irradiation? Here, this issue is tackled by investigating the solar photolysis of aqueous pyruvic acid (PA) solutions at concentrations representative of the atmospheric aerosol using UV-absorption, high resolution electrospray mass, and nuclear magnetic resonance spectrometries. Under such conditions, PA is not photodegraded but yields polyfunctional polymers, whose mass and UV-absorption spectra remain unaffected after 3, 8 and 22 h photolysis. Unless diluted, these polymers undergo condensation/polymerization in the post-photolysis period into mass < 700 Da species that absorb in the visible, and are bleached upon resuming irradiation. The re- photolyzed solutions recover the mass and UV-absorption spectra of first photolyzed solutions. Whereas initial pH has no effect on the mechanism of reaction, ammonium bisulfate, a major component of the aerosol, markedly influences these processes. These findings suggest that the chemical identity and concentration levels of complex organic substances in the aerosol are the result of dynamic photochemical processing in the condensed phase.

Comparison of Respirable Mass Concentrations Measured by a Personal Dust Monitor and a Personal DataRAM to Gravimetric Measurements.

PubMed

Halterman, Andrew; Sousan, Sinan; Peters, Thomas M

2017-12-15

In 2016, the Mine Safety and Health Administration required the use of continuous monitors to measure respirable dust in mines and better protect miner health. The Personal Dust Monitor, PDM3700, has met stringent performance criteria for this purpose. In a laboratory study, respirable mass concentrations measured with the PDM3700 and a photometer (personal DataRam, pDR-1500) were compared to those measured gravimetrically for five aerosols of varying refractive index and density (diesel exhaust fume, welding fume, coal dust, Arizona road dust (ARD), and salt [NaCl] aerosol) at target concentrations of 0.38, 0.75, and 1.5 mg m-3. For all aerosols except coal dust, strong, near-one-to-one, linear relationships were observed between mass concentrations measured with the PDM3700 and gravimetrically (diesel fume, slope = 0.99, R2 = 0.99; ARD, slope = 0.98, R2 = 0.99; and NaCl, slope = 0.95, R2 = 0.99). The slope deviated substantially from unity for coal dust (slope = 0.55; R2 = 0.99). Linear relationships were also observed between mass concentrations measured with the pDR-1500 and gravimetrically, but one-to-one behavior was not exhibited (diesel fume, slope = 0.23, R2 = 0.76; coal dust, slope = 0.54, R2 = 0.99; ARD, slope = 0.61, R2 = 0.99; NaCl, slope = 1.14, R2 = 0.98). Unlike the pDR-1500, mass concentrations measured with the PDM3700 appear independent of refractive index and density, suggesting that it could have applications in a variety of occupational settings. © The Author(s) 2017. Published by Oxford University Press on behalf of the British Occupational Hygiene Society.

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.

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses

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

Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses

DOE PAGES

Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles; ...

2017-10-30

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less

On-line analysis of ambient air aerosols using laser-induced breakdown spectroscopy

NASA Astrophysics Data System (ADS)

Carranza, J. E.; Fisher, B. T.; Yoder, G. D.; Hahn, D. W.

2001-06-01

Laser-induced breakdown spectroscopy is developed for the detection of aerosols in ambient air, including quantitative mass concentration measurements and size/composition measurements of individual aerosol particles. Data are reported for ambient air aerosols containing aluminum, calcium, magnesium and sodium for a 6-week sampling period spanning the Fourth of July holiday period. Measured mass concentrations for these four elements ranged from 1.7 parts per trillion (by mass) to 1.7 parts per billion. Ambient air concentrations of magnesium and aluminum revealed significant increases during the holiday period, which are concluded to arise from the discharge of fireworks in the lower atmosphere. Real-time conditional data analysis yielded increases in analyte spectral intensity approaching 3 orders of magnitude. Analysis of single particles yielded composition-based aerosol size distributions, with measured aerosol diameters ranging from 100 nm to 2 μm. The absolute mass detection limits for single particle analysis exceeded sub-femtogram values for calcium-containing particles, and was on the order of 2-3 femtograms for magnesium and sodium-based particles. Overall, LIBS-based analysis of ambient air aerosols is a promising technique for the challenging issues associated with the real-time collection and analysis of ambient air particulate matter data.

Cloud condensation nuclei closure study on summer arctic aerosol

NASA Astrophysics Data System (ADS)

Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

2011-03-01

We present an aerosol - cloud condensation nuclei CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in summer 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration is then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory and an internally mixed aerosol. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one. One possible explanation is that the smaller particles that activate at these supersaturations have a relative larger insoluble organic mass fraction and thus are less good CCN than the larger particles. At 0.20, 0.15 and 0.10% supersaturation, the measured CCN number can be represented with different parameters for the hygroscopicity and density of the particles. For the best agreement of the calculated CCNnumber concentration with the measured one the organic fraction of the aerosol needs to be nearly insoluble (қorg=0.02). However, this is not unambigious and қorg=0.2 is found as an upper limit at 0.1% supersaturation.

Measurements of Organic Composition of Aerosol and Rainwater Samples Using Offline Aerosol Mass Spectrometry

NASA Astrophysics Data System (ADS)

OBrien, R. E.; Ridley, K. J.; Canagaratna, M. R.; Croteau, P.; Budisulistiorini, S. H.; Cui, T.; Green, H. S.; Surratt, J. D.; Jayne, J. T.; Kroll, J. H.

2016-12-01

A thorough understanding of the sources, evolution, and budgets of atmospheric organic aerosol requires widespread measurements of the amount and chemical composition of atmospheric organic carbon in the condensed phase (within particles and water droplets). Collecting such datasets requires substantial spatial and temporal (long term) coverage, which can be challenging when relying on online measurements by state-of-the-art research-grade instrumentation (such as those used in atmospheric chemistry field studies). Instead, samples are routinely collected using relatively low-cost techniques, such as aerosol filters, for offline analysis of their chemical composition. However, measurements made by online and offline instruments can be fundamentally different, leading to disparities between data from field studies and those from more routine monitoring. To better connect these two approaches, and take advantage of the benefits of each, we have developed a method to introduce collected samples into online aerosol instruments using nebulization. Because nebulizers typically require tens to hundreds of milliliters of solution, limiting this technique to large samples, we developed a new, ultrasonic micro-nebulizer that requires only small volumes (tens of microliters) of sample for chemical analysis. The nebulized (resuspended) sample is then sent into a high-resolution Aerosol Mass Spectrometer (AMS), a widely-used instrument that provides key information on the chemical composition of aerosol particulate matter (elemental ratios, carbon oxidation state, etc.), measurements that are not typically made for collected atmospheric samples. Here, we compare AMS data collected using standard on-line techniques with our offline analysis, demonstrating the utility of this new technique to aerosol filter samples. We then apply this approach to organic aerosol filter samples collected in remote regions, as well as rainwater samples from across the US. This data provides

Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; de Sá, S. S.; McKinney, K.; Martin, S. T.; Hu, M.; Budisulistiorini, S. H.; Riva, M.; Surratt, J. D.; St. Clair, J. M.; Isaacman-Van Wertz, G.; Yee, L. D.; Goldstein, A. H.; Carbone, S.; Brito, J.; Artaxo, P.; de Gouw, J. A.; Koss, A.; Wisthaler, A.; Mikoviny, T.; Karl, T.; Kaser, L.; Jud, W.; Hansel, A.; Docherty, K. S.; Alexander, M. L.; Robinson, N. H.; Coe, H.; Allan, J. D.; Canagaratna, M. R.; Paulot, F.; Jimenez, J. L.

2015-10-01

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12-40 ‰) but varies substantially between locations, which is shown to reflect

Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

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

Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accountedmore » by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C 5H 6O + ( m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine f C5H6O ( f C5H6O= C 5H 6O +/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher f C5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. f C5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations

Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

DOE PAGES

Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; ...

2015-10-23

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accountedmore » by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C 5H 6O + ( m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine f C5H6O ( f C5H6O= C 5H 6O +/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher f C5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. f C5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations

Overview of the aerosol measurements in the UTLS during the POSIDON campaign

NASA Astrophysics Data System (ADS)

Gao, R. S.; Liu, S.; Thornberry, T. D.; Rollins, A. W.; Yu, P.; Woods, S.; Bui, T. V.

2017-12-01

The tropical tropopause layer (TTL) is the main gateway for transport of aerosols from the troposphere to the stratosphere. Studies of aerosol properties in the TTL, however, are very limited. During the NASA Pacific Oxidants, Sulfur, Ice, Dehydration, and cONvection (POSIDON) Experiment in Guam in October 2016, we measured aerosol size distributions onboard the NASA WB-57F high altitude research aircraft up to 19 km. Multiple aerosol vertical profiles showed a robust enhancement of aerosols as a function of altitude between 15 and 19 km, with the aerosol number and mass concentrations of 10 cm-3 and 0.1 µg m-3, respectively, for particles in the size range of 140-3000 nm at 17 km altitude. Simulation using a global sectional aerosol model coupled with the Community Earth System Model generally agreed with aerosol observations, suggesting that the aerosol enhancement was likely due to in-situ particle formation and growth. Concurrent SO2 measurement showed that conversion of SO2 to sulfuric acid alone cannot explain the enhanced aerosol layer at TTL, indicating that other precursors or formation pathways exist for efficient aerosol formation. Using the measured mass concentration and an average vertical air velocity, the aerosol mass flux at the tropopause has been estimated. In addition, we investigated the potential aerosol removal processes and found no evidence for aerosol scavenging by ice.

Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

NASA Astrophysics Data System (ADS)

Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

2017-10-01

The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

Chemical composition of Titan's aerosols analogues characterized with a systematic pyrolysis-gas chromatography-mass spectrometry characterization

NASA Astrophysics Data System (ADS)

Szopa, Cyril; Raulin, Francois; Coll, Patrice; Cabane, Michel; GCMS Team

2014-05-01

The in situ chemical characterization of Titan's atmosphere was achieved in 2005 with two instruments present onboard the Huygens atmospheric probe : the Aerosol Collector and Pyrolyzer (ACP) devoted to collect and pyrolyse Titan's aerosols ; the Gas Chromatograph-Mass Spectrometer (GCMS) experiment devoted to analyze gases collected in the atmosphere or coming from the aerosols pyrolysis. The GCMS was developed by Hasso Niemann in the filiation of the quadrupole mass spectrometers he built for several former space missions. The main objectives were to : determine the concentration profile of the most abundant chemical species; seek for minor atmospheric organic species not detected with remote observations ; give a first view of the organic aerosols structure; characterize the condensed volatiles present at the surface (e.g. lakes) in case of survival of the probe to the landing impact. Taking into account for the potential complexity of the gaseous samples to be analyzed, it was decided to couple to the MS analyzer a gas chromatograph capable to separate volatile species from light inorganic molecules and noble gases, to organic compounds including aromatics. This was the first GCMS analyzer that worked in an extraterrestrial environment since the Viking missions on Mars. Even if the GCMS coupling mode did not provide any result of interest, it has been demonstrated to be functional during the Huygens descent. But, the direct MS analysis of the atmosphere, and the pyrolysis-MS analysis of aerosols allowed to make great discoveries which are still of primary importance to describe the Titan's lower atmosphere composition. This contribution aims at presenting this instrument that worked in the Titan's atmosphere, and summarizing the most important discoveries it allowed.

Influence of the Surf Zone on the Marine Aerosol Concentration in a Coastal Area

NASA Astrophysics Data System (ADS)

Tedeschi, Gilles; van Eijk, Alexander M. J.; Piazzola, Jacques; Kusmierczyk-Michulec, Jolanta T.

2017-01-01

Sea-salt aerosol concentrations in the coastal zone are assessed with the numerical aerosol-transport model MACMod that applies separate aerosol source functions for open ocean and the surf zone near the sea-land transition. Numerical simulations of the aerosol concentration as a function of offshore distance from the surf zone compare favourably with experimental data obtained during a surf-zone aerosol experiment in Duck, North Carolina in autumn 2007. Based on numerical simulations, the effect of variations in aerosol production (source strength) and transport conditions (wind speed, air-sea temperature difference), we show that the surf-zone aerosols are replaced by aerosols generated over the open ocean as the airmass advects out to sea. The contribution from the surf-generated aerosol is significant during high wind speeds and high wave events, and is significant up to 30 km away from the production zone. At low wind speeds, the oceanic component dominates, except within 1-5 km of the surf zone. Similar results are obtained for onshore flow, where no further sea-salt aerosol production occurs as the airmass advects out over land. The oceanic aerosols that are well-mixed throughout the boundary layer are then more efficiently transported inland than are the surf-generated aerosols, which are confined to the first few tens of metres above the surface, and are therefore also more susceptible to the type of surface (trees or grass) that determines the deposition velocity.

Chemical composition of aerosols over peninsular India during winter

NASA Astrophysics Data System (ADS)

Nair, Prabha R.; George, Susan K.; Sunilkumar, S. V.; Parameswaran, K.; Jacob, Salu; Abraham, Annamma

As a part of the campaign conducted for the spatial characterization of aerosols over peninsular India measurements of aerosol mass loading, optical depth and chemical composition have been carried out during the winter month of February 2004. The aerosol characteristics showed significant variation with locations. The aerosol mass loading as well as the optical depth showed high values along the western coastal regions compared to inland locations. Ions of SO 4 and NO 3 are observed to be the major anions present over the entire region with higher mass concentrations at the coastal and close-to-forest regions. The mass fraction of non-sea-salt sulphate was larger at the interior locations. Compared to that in the inland/close-to-forest locations the concentration of Cl and Na are found to be 2-3 times larger in the coastal region. The mass fraction of non-sea-salt K was largest at locations close to forests. Among the metallic components, Fe, Cu, Ca, Zn, Pb etc, which are of continental origin, are found to dominate over inland locations. These measurements over the land are compared with those observed over the Arabian Sea and Indian Ocean during the Indian Ocean Experiment.

Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield

NASA Astrophysics Data System (ADS)

Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; Brune, W. H.; Hunter, J. F.; Kroll, J. H.; Cummings, M. J.; Brogan, J. F.; Parmar, Y.; Worsnop, D. R.; Kolb, C. E.; Davidovits, P.

2015-03-01

We performed a systematic intercomparison study of the chemistry and yields of secondary organic aerosol (SOA) generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0 × 108 to 2.2 × 1010 molec cm-3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2 × 106 to 2 × 107 molec cm-3 over exposure times of several hours. The OH concentration in the chamber experiments is close to that found in the atmosphere, but the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. In most cases, for a specific SOA type the most-oxidized chamber SOA and the least-oxidized flow reactor SOA have similar mass spectra, oxygen-to-carbon and hydrogen-to-carbon ratios, and carbon oxidation states at integrated OH exposures between approximately 1 × 1011 and 2 × 1011 molec cm-3 s, or about 1-2 days of equivalent atmospheric oxidation. This observation suggests that in the range of available OH exposure overlap for the flow reactor and chambers, SOA elemental composition as measured by an aerosol mass spectrometer is similar whether the precursor is exposed to low OH concentrations over long exposure times or high OH concentrations over short exposure times. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The influence of sulfate seed

Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield

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

Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.

We performed a systematic intercomparison study of the chemistry and yields of secondary organic aerosol (SOA) generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0 × 10 8 to 2.2 × 10 10 molec cm -3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2 × 10 6 to 2 × 10 7 molec cm -3 over exposure times of severalmore » hours. The OH concentration in the chamber experiments is close to that found in the atmosphere, but the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. In most cases, for a specific SOA type the most-oxidized chamber SOA and the least-oxidized flow reactor SOA have similar mass spectra, oxygen-to-carbon and hydrogen-to-carbon ratios, and carbon oxidation states at integrated OH exposures between approximately 1 × 10 11 and 2 × 10 11 molec cm -3 s, or about 1–2 days of equivalent atmospheric oxidation. This observation suggests that in the range of available OH exposure overlap for the flow reactor and chambers, SOA elemental composition as measured by an aerosol mass spectrometer is similar whether the precursor is exposed to low OH concentrations over long exposure times or high OH concentrations over short exposure times. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The

Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield

DOE PAGES

Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; ...

2015-03-18

We performed a systematic intercomparison study of the chemistry and yields of secondary organic aerosol (SOA) generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0 × 10 8 to 2.2 × 10 10 molec cm -3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2 × 10 6 to 2 × 10 7 molec cm -3 over exposure times of severalmore » hours. The OH concentration in the chamber experiments is close to that found in the atmosphere, but the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. In most cases, for a specific SOA type the most-oxidized chamber SOA and the least-oxidized flow reactor SOA have similar mass spectra, oxygen-to-carbon and hydrogen-to-carbon ratios, and carbon oxidation states at integrated OH exposures between approximately 1 × 10 11 and 2 × 10 11 molec cm -3 s, or about 1–2 days of equivalent atmospheric oxidation. This observation suggests that in the range of available OH exposure overlap for the flow reactor and chambers, SOA elemental composition as measured by an aerosol mass spectrometer is similar whether the precursor is exposed to low OH concentrations over long exposure times or high OH concentrations over short exposure times. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The

Parametric uncertainties in global model simulations of black carbon column mass concentration

NASA Astrophysics Data System (ADS)

Pearce, Hana; Lee, Lindsay; Reddington, Carly; Carslaw, Ken; Mann, Graham

2016-04-01

Previous studies have deduced that the annual mean direct radiative forcing from black carbon (BC) aerosol may regionally be up to 5 W m-2 larger than expected due to underestimation of global atmospheric BC absorption in models. We have identified the magnitude and important sources of parametric uncertainty in simulations of BC column mass concentration from a global aerosol microphysics model (GLOMAP-Mode). A variance-based uncertainty analysis of 28 parameters has been performed, based on statistical emulators trained on model output from GLOMAP-Mode. This is the largest number of uncertain model parameters to be considered in a BC uncertainty analysis to date and covers primary aerosol emissions, microphysical processes and structural parameters related to the aerosol size distribution. We will present several recommendations for further research to improve the fidelity of simulated BC. In brief, we find that the standard deviation around the simulated mean annual BC column mass concentration varies globally between 2.5 x 10-9 g cm-2 in remote marine regions and 1.25 x 10-6 g cm-2 near emission sources due to parameter uncertainty Between 60 and 90% of the variance over source regions is due to uncertainty associated with primary BC emission fluxes, including biomass burning, fossil fuel and biofuel emissions. While the contributions to BC column uncertainty from microphysical processes, for example those related to dry and wet deposition, are increased over remote regions, we find that emissions still make an important contribution in these areas. It is likely, however, that the importance of structural model error, i.e. differences between models, is greater than parametric uncertainty. We have extended our analysis to emulate vertical BC profiles at several locations in the mid-Pacific Ocean and identify the parameters contributing to uncertainty in the vertical distribution of black carbon at these locations. We will present preliminary comparisons of

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

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

NASA Technical Reports Server (NTRS)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Aqueous-phase photooxidation of levoglucosan - a mechanistic study using aerosol time-of-flight chemical ionization mass spectrometry (Aerosol ToF-CIMS)

NASA Astrophysics Data System (ADS)

Zhao, R.; Mungall, E. L.; Lee, A. K. Y.; Aljawhary, D.; Abbatt, J. P. D.

2014-09-01

Levoglucosan (LG) is a widely employed tracer for biomass burning (BB). Recent studies have shown that LG can react rapidly with hydroxyl (OH) radicals in the aqueous phase despite many mass balance receptor models assuming it to be inert during atmospheric transport. In the current study, aqueous-phase photooxidation of LG by OH radicals was performed in the laboratory. The reaction kinetics and products were monitored by aerosol time-of-flight chemical ionization mass spectrometry (Aerosol ToF-CIMS). Approximately 50 reaction products were detected by the Aerosol ToF-CIMS during the photooxidation experiments, representing one of the most detailed product studies yet performed. By following the evolution of mass defects of product peaks, unique trends of adding oxygen (+O) and removing hydrogen (-2H) were observed among the products detected, providing useful information for determining potential reaction mechanisms and sequences. Additionally, bond-scission reactions take place, leading to reaction intermediates with lower carbon numbers. We introduce a data analysis framework where the average oxidation state (OSc) is plotted against a novel molecular property: double-bond-equivalence-to-carbon ratio (DBE/#C). The trajectory of LG photooxidation on this plot suggests formation of polycarbonyl intermediates and their subsequent conversion to carboxylic acids as a general reaction trend. We also determined the rate constant of LG with OH radicals at room temperature to be 1.08 ± 0.16 × 109 M-1 s-1. By coupling an aerosol mass spectrometer (AMS) to the system, we observed a rapid decay of the mass fraction of organic signals at mass-to-charge ratio 60 (f60), corresponding closely to the LG decay monitored by the Aerosol ToF-CIMS. The trajectory of LG photooxidation on a f44-f60 correlation plot matched closely to literature field measurement data. This implies that aqueous-phase photooxidation might be partially contributing to aging of BB particles in the

Cloud condensation nuclei closure study on summer arctic aerosol

NASA Astrophysics Data System (ADS)

Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

2011-11-01

We present an aerosol - cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

NASA Astrophysics Data System (ADS)

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy; Eastman, Ryan; Luke, Edward

2018-01-01

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (Na). These terms are then parameterized, and by assuming that on seasonal time scales Na is in steady state, the budget equation is rearranged to form a diagnostic equation for Na based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-Section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter Na concentrations are made using the simplified steady state model and seasonal mean observed variables. These are found to match well with the observed Na. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g., precipitation rate and free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in Na, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.

Submicron particle mass concentrations and sources in the Amazonian wet season (AMAZE-08)

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

Chen, Q.; Farmer, D. K.; Rizzo, L. V.

Real-time mass spectra of non-refractory component of submicron aerosol particles were recorded in a tropical rainforest in the central Amazon basin during the wet season of 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE-08). Organic components accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. Ammonium was present in sufficient quantities to halfway neutralize sulfate. In this acidic, isoprene-dominated, low-NOx environment the high-resolution mass spectra as well as mass closures with ion chromatography measurements did not provide evidence for significant contributions of organosulfate species, at least atmore » concentrations above uncertainty levels. Positive-matrix factorization of the time series of particle mass spectra identified four statistical factors to account for the variance of the signal intensities of the organic constituents: a factor HOA having a hydrocarbon-like signature and identified as regional emissions of primary organic material, a factor OOA-1 associated with fresh production of secondary organic material by a mechanism of BVOC oxidation followed by gas-to-particle conversion, a factor OOA-2 consistent with reactive uptake of isoprene oxidation products, especially epoxydiols by acidic particles, and a factor OOA-3 associated with long range transport and atmospheric aging. The OOA-1, -2, and -3 factors had progressively more oxidized signatures. Diameter-resolved mass spectral markers also suggested enhanced reactive uptake of isoprene oxidation products to the accumulation mode for the OOA-2 factor, and such size partitioning can be indicative of in-cloud process. The campaign-average factor loadings were in a ratio of 1.1:1.0 for the OOA-1 compared to the OOA-2 pathway, suggesting the comparable importance of gas-phase compared to particle-phase (including cloud waters) production pathways of secondary organic material

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

NASA Astrophysics Data System (ADS)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-11-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

NASA Astrophysics Data System (ADS)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-07-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Novel characterization of the aerosol and gas-phase composition of aerosolized jet fuel.

PubMed

Tremblay, Raphael T; Martin, Sheppard A; Fisher, Jeffrey W

2010-04-01

Few robust methods are available to characterize the composition of aerosolized complex hydrocarbon mixtures. The difficulty in separating the droplets from their surrounding vapors and preserving their content is challenging, more so with fuels, which contain hydrocarbons ranging from very low to very high volatility. Presented here is a novel method that uses commercially available absorbent tubes to measure a series of hydrocarbons in the vapor and droplets from aerosolized jet fuels. Aerosol composition and concentrations were calculated from the differential between measured total (aerosol and gas-phase) and measured gas-phase concentrations. Total samples were collected directly, whereas gas-phase only samples were collected behind a glass fiber filter to remove droplets. All samples were collected for 1 min at 400 ml min(-1) and quantified using thermal desorption-gas chromatography-mass spectrometry. This method was validated for the quantification of the vapor and droplet content from 4-h aerosolized jet fuel exposure to JP-8 and S-8 at total concentrations ranging from 200 to 1000 mg/m(3). Paired samples (gas-phase only and total) were collected every approximately 40 min. Calibrations were performed with neat fuel to calculate total concentration and also with a series of authentic standards to calculate specific compound concentrations. Accuracy was good when compared to an online GC-FID (gas chromatography-flame ionization detection) technique. Variability was 15% or less for total concentrations, the sum of all gas-phase compounds, and for most specific compound concentrations in both phases. Although validated for jet fuels, this method can be adapted to other hydrocarbon-based mixtures.

Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Zhang, Xinghua; Xu, Jianzhong; Kang, Shichang; Liu, Yanmei; Zhang, Qi

2018-04-01

An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical evolution) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m-3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). The average size distributions of PM1 species all peaked at an overlapping accumulation mode (˜ 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

Numerical simulation of advection fog formation on multi-disperse aerosols due to combustion-related pollutants

NASA Technical Reports Server (NTRS)

Hung, R. J.; Liaw, G. S.

1980-01-01

The effects of multi-disperse distribution of the aerosol population are presented. Single component and multi-component aerosol species on the condensation/nucleation processes which affect the reduction in visibility are described. The aerosol population with a high particle concentration provided more favorable conditions for the formation of a denser fog than the aerosol population with a greater particle size distribution when the value of the mass concentration of the aerosols was kept constant. The results were used as numerical predictions of fog formation. Two dimensional observations in horizontal and vertical coordinates, together with time-dependent measurements were needed as initial values for the following physical parameters: (1)wind profiles; (2) temperature profiles; (3) humidity profiles; (4) mass concentration of aerosol particles; (5) particle size distribution of aerosols; and (6) chemical composition of aerosols. Formation and dissipation of advection fog, thus, can be forecasted numerically by introducing initial values obtained from the observations.

Aqueous aerosol SOA formation: impact on aerosol physical properties.

PubMed

Woo, Joseph L; Kim, Derek D; Schwier, Allison N; Li, Ruizhi; McNeill, V Faye

2013-01-01

Organic chemistry in aerosol water has recently been recognized as a potentially important source of secondary organic aerosol (SOA) material. This SOA material may be surface-active, therefore potentially affecting aerosol heterogeneous activity, ice nucleation, and CCN activity. Aqueous aerosol chemistry has also been shown to be a potential source of light-absorbing products ("brown carbon"). We present results on the formation of secondary organic aerosol material in aerosol water and the associated changes in aerosol physical properties from GAMMA (Gas-Aerosol Model for Mechanism Analysis), a photochemical box model with coupled gas and detailed aqueous aerosol chemistry. The detailed aerosol composition output from GAMMA was coupled with two recently developed modules for predicting a) aerosol surface tension and b) the UV-Vis absorption spectrum of the aerosol, based on our previous laboratory observations. The simulation results suggest that the formation of oligomers and organic acids in bulk aerosol water is unlikely to perturb aerosol surface tension significantly. Isoprene-derived organosulfates are formed in high concentrations in acidic aerosols under low-NO(x) conditions, but more experimental data are needed before the potential impact of these species on aerosol surface tension may be evaluated. Adsorption of surfactants from the gas phase may further suppress aerosol surface tension. Light absorption by aqueous aerosol SOA material is driven by dark glyoxal chemistry and is highest under high-NO(x) conditions, at high relative humidity, in the early morning hours. The wavelength dependence of the predicted absorption spectra is comparable to field observations and the predicted mass absorption efficiencies suggest that aqueous aerosol chemistry can be a significant source of aerosol brown carbon under urban conditions.

Indirect effect of changing aerosol concentrations on methane and ozone radiative forcing

NASA Astrophysics Data System (ADS)

Rowlinson, Matthew; Rap, Alexandru; Arnold, Steve; Forster, Piers; Chipperfield, Martyn

2017-04-01

% decreases atmospheric sulpate concentrations by 44% after 2 years, while increasing global OH concentrations by 0.9%. CH4 lifetime is reduced by approximately 50 days as a result, leading to a decrease in CH4 burden of 38ppb. NOx is anticipated to have a similar but much larger effect (Matsui and Koike 2016). The Edwards and Slingo offline radiation model is also used to calculate changes to direct and indirect aerosol forcing. Presented here is the net RF change following 50% emission decrease of each aerosol or precursors, accounting for the direct and indirect aerosol effect as well as indirect effects via oxidation chemistry on the RF due to CH4 and tropospheric O3.

An Intercomparison of Research Scanning Polarimeter Cloud Droplet Number Concentrations with Aerosol Properties over the Atlantic Ocean

NASA Astrophysics Data System (ADS)

Sinclair, K.; van Diedenhoven, B.; Cairns, B.; Alexandrov, M. D.; Ziemba, L. D.; Moore, R.; Crosbie, E.; Hostetler, C. A.

2016-12-01

Cloud droplet number concentration (CDNC) is a key parameter of of liquid clouds and is essential for the understanding of aerosol-cloud interaction. It couples surface aerosol composition and chemistry on the one hand and cloud reflectivity on the other. It impacts radiative forcing, cloud evolution, precipitation, global climate and, through observation, can be used to monitor the cloud albedo effect, or the first indirect effect. The North Atlantic and Marine Ecosystems Study (NAAMES), which is a NASA-led ship and air campaign that takes place off the east coast of Newfoundland, observed many low cloud decks and aerosols over a marine environment. This campaign has completed two of four deployments and provides an excellent opportunity for the Research Scanning Polarimeter (RSP) to cross-validate its approach of sensing CDNC with the Langley Aerosol Research Group Experiment's (LARGE's) Cloud Droplet Probe (CDP). The RSP is an airborne scanning sensor that provides high-precision measurements of polarized and full-intensity radiances at multiple angles over a wide spectral range. Each of the four NAAMES deployments are aligned to a specific annual event in the plankton cycle, along with other variations in environmental conditions. The Fall 2015 and spring 2016 deployments allow us to demonstrate and characterize the RSP's performance over a range of CDNCs and cloud types. We also assess correlations between the RSP CDNC measurements and atmospheric aerosol load. Using the LARGE Cloud Particle Counter (CPC) and Aerosol Mass Spectrometer (AMS), links between the size and type of aerosols and the RSP CDNC retrievals are explored.

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

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

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for Nmore » a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.« less

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

DOE PAGES

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy; ...

2018-01-21

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for Nmore » a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.« less

Atmospheric nuclei in the Pacific midtroposphere: Their nature, concentration, and evolution

NASA Technical Reports Server (NTRS)

Clarke, Antony D.

1993-01-01

An extensive flight series was carried out during May-June 1990 in the remote North and South Pacific free tropospheric aboard the NASA DC-8. Condensation nuclei counters and optical particle counters provided information on aerosol particles with diameters between 0.003 and 7.0 micrometers. Vertical profiles revealed aerosol layers to be a common feature of the free troposphere. Regions with highest aerosol mass tended to have the highest concentrations of surface-derived nuclei but the lowest concentrations of total nuclei. Regions with lowest aerosol mass tended to have the highest concentrations of the smaller 'ultrafine' condensation nuclei with diameters below 0.02 mircometers. Horizontal transects totaling over 35,000 km at about 9 to 10-km altitude exhibited variability of approximately 3 orders of magnitude in both aerosol mass and number concentrations over spatial scales ranging from 1 to 1000 km. At these altitudes an approximate inverse relationship between ultrafine concentrations and the surface area of the larger aerosol was evident. Regions having lowest aerosol mass were characterized by aerosol thermal volatility, indicative of a predominately sulfuric acid composition, and by very high concentrations of ultrafine nuclei, indicative of recent homogeneous nucleation. These conditions were frequently observed but were conspicuously evident above cloud over the intertropical convergence zone. The clean, free troposphere appears to be a significant source region for new tropospheric nuclei. A simplified model of the lifetime, coagulation, and cycling of these nuclei suggests that they constitute a source of cloud condensation nuclei in the lower troposphere.

Inversion of scattered radiance horizon profiles for gaseous concentrations and aerosol parameters

NASA Technical Reports Server (NTRS)

Malchow, H. L.; Whitney, C. K.

1977-01-01

Techniques have been developed and used to invert limb scan measurements for vertical profiles of atmospheric state parameters. The parameters which can be found are concentrations of Rayleigh scatters, ozone, NO2, and aerosols, and aerosol physical properties including a Junge-size distribution parameter and real and imaginary parts of the index of refraction.

Toward Developing a New Occupational Exposure Metric Approach for Characterization of Diesel Aerosols

PubMed Central

Cauda, Emanuele G.; Ku, Bon Ki; Miller, Arthur L.; Barone, Teresa L.

2015-01-01

The extensive use of diesel-powered equipment in mines makes the exposure to diesel aerosols a serious occupational issue. The exposure metric currently used in U.S. underground noncoal mines is based on the measurement of total carbon (TC) and elemental carbon (EC) mass concentration in the air. Recent toxicological evidence suggests that the measurement of mass concentration is not sufficient to correlate ultrafine aerosol exposure with health effects. This urges the evaluation of alternative measurements. In this study, the current exposure metric and two additional metrics, the surface area and the total number concentration, were evaluated by conducting simultaneous measurements of diesel ultrafine aerosols in a laboratory setting. The results showed that the surface area and total number concentration of the particles per unit of mass varied substantially with the engine operating condition. The specific surface area (SSA) and specific number concentration (SNC) normalized with TC varied two and five times, respectively. This implies that miners, whose exposure is measured only as TC, might be exposed to an unknown variable number concentration of diesel particles and commensurate particle surface area. Taken separately, mass, surface area, and number concentration did not completely characterize the aerosols. A comprehensive assessment of diesel aerosol exposure should include all of these elements, but the use of laboratory instruments in underground mines is generally impracticable. The article proposes a new approach to solve this problem. Using SSA and SNC calculated from field-type measurements, the evaluation of additional physical properties can be obtained by using the proposed approach. PMID:26361400

CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

EPA Science Inventory

This chapter surveys the analytical techniques used to determine the concentrations of aerosol mass and its chemical components. The techniques surveyed include mass, major ions (sulfate, nitrate, ammonium), organic carbon, elemental carbon, and trace elements. As reported in...

Atmospheric aerosol composition and source apportionments to aerosol in southern Taiwan

NASA Astrophysics Data System (ADS)

Tsai, Ying I.; Chen, Chien-Lung

In this study, the chemical characteristics of winter aerosol at four sites in southern Taiwan were determined and the Gaussian Trajectory transfer coefficient model (GTx) was then used to identify the major air pollutant sources affecting the study sites. Aerosols were found to be acidic at all four sites. The most important constituents of the particulate matter (PM) by mass were SO 42-, organic carbon (OC), NO 3-, elemental carbon (EC) and NH 4+, with SO 42-, NO 3-, and NH 4+ together constituting 86.0-87.9% of the total PM 2.5 soluble inorganic salts and 68.9-78.3% of the total PM 2.5-10 soluble inorganic salts, showing that secondary photochemical solution components such as these were the major contributors to the aerosol water-soluble ions. The coastal site, Linyuan (LY), had the highest PM mass percentage of sea salts, higher in the coarse fraction, and higher sea salts during daytime than during nighttime, indicating that the prevailing daytime sea breeze brought with it more sea-salt aerosol. Other than sea salts, crustal matter, and EC in PM 2.5 at Jenwu (JW) and in PM 2.5-10 at LY, all aerosol components were higher during nighttime, due to relatively low nighttime mixing heights limiting vertical and horizontal dispersion. At JW, a site with heavy traffic loadings, the OC/EC ratio in the nighttime fine and coarse fractions of approximately 2.2 was higher than during daytime, indicating that in addition to primary organic aerosol (POA), secondary organic aerosol (SOA) also contributed to the nighttime PM 2.5. This was also true of the nighttime coarse fraction at LY. The GTx produced correlation coefficients ( r) for simulated and observed daily concentrations of PM 10 at the four sites (receptors) in the range 0.45-0.59 and biases from -6% to -20%. Source apportionment indicated that point sources were the largest PM 10 source at JW, LY and Daliao (DL), while at Meinung (MN), a suburban site with less local PM 10, SO x and NO x emissions, upwind

Aerosol accumulation intensity and composition variations under different weather conditions in urban environment

NASA Astrophysics Data System (ADS)

Steinberga, Iveta; Bikshe, Janis; Eindorfa, Aiva

2014-05-01

During the last decade aerosol (PM10, PM2.5) mass and composition measurements were done in different urban environments - parallel street canyons, industrial sites and at the background level in Riga, Latvia. Effect of meteorological parameters on the accumulation and ventilation intensity was investigated in order to understand microclimatological parameters affecting aerosol pollution level and chemical composition changes. In comparison to industrial sites (shipping activities, bulk cargo, oil and naphtha processing), urban street canyon aerosol mass concentration was significantly higher, for PM10 number of daily limit exceedances are higher by factor 3.4 - 3.9 in street canyons. Exceedances of PM2.5 annual limits were identified only in street canyons as well. Precipitation intensity, wind speed, days with mist highly correlates with aerosol concentration; in average during the year about 1 - 2 % presence of calm wind days, 20 - 30 days with mist facilitate accumulation of aerosols and mitigating growing of secondary aerosols. It has been assessed that about 25 % of daily exceedances in street canyons are connected with sea salt/street sanding factor. Strong dependency of wind speed and direction were identified in winter time - low winds (0.4 - 1.7 m/s) blowing from south, south-east (cross section of the street) contributing to PM10 concentrations over 100 - 150 ug/m3. Seasonal differences in aerosol concentrations were identified as a result of recombination of direct source impact, specific meteorological and synoptical conditions during the period from January until April when usually dominates extremely high aerosol concentrations. While aerosol mass concentration levels in monitoring sites significantly differs, concentrations of heavy metals (Pb, Ni, Cd, and As) are almost at the same level, even more - concentration of Cd for some years was higher in industrial area where main pollution is caused by oil processing and storage, heavy traffic

Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

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

Vergara-Temprado, Jesús; Murray, Benjamin J.; Wilson, Theodore W.

Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiativemore » flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order

Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Lohmann, U.; Stier, P.; Hoose, C.; Ferrachat, S.; Roeckner, E.; Zhang, J.

2007-03-01

The double-moment cloud microphysics scheme from ECHAM4 has been coupled to the size-resolved aerosol scheme ECHAM5-HAM. ECHAM5-HAM predicts the aerosol mass and number concentrations and the aerosol mixing state. This results in a much better agreement with observed vertical profiles of the black carbon and aerosol mass mixing ratios than with the previous version ECHAM4, where only the different aerosol mass mixing ratios were predicted. Also, the simulated liquid, ice and total water content and the cloud droplet and ice crystal number concentrations as a function of temperature in stratiform mixed-phase clouds between 0 and -35°C agree much better with aircraft observations in the ECHAM5 simulations. ECHAM5 performs better because more realistic aerosol concentrations are available for cloud droplet nucleation and because the Bergeron-Findeisen process is parameterized as being more efficient. The total anthropogenic aerosol effect includes the direct, semi-direct and indirect effects and is defined as the difference in the top-of-the-atmosphere net radiation between present-day and pre-industrial times. It amounts to -1.8 W m-2 in ECHAM5, when a relative humidity dependent cloud cover scheme and present-day aerosol emissions representative for the year 2000 are used. It is larger when either a statistical cloud cover scheme or a different aerosol emission inventory are employed.

Impacts of interannual variation of the East Asian winter monsoon on aerosol concentrations over eastern China

NASA Astrophysics Data System (ADS)

Zhu, J.; Liao, H.; Li, J.; Feng, J.

2012-04-01

China has been experiencing increased concentrations of aerosols, commonly attributed to the large increases in emissions associated with the rapid economic development. We apply a global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) driven by the NASA/GEOS-4 assimilated meteorological data to quantify the impacts of East Asian winter monsoon (EAWM) on the aerosol concentrations over eastern China. We found that the simulated aerosol concentrations over eastern China have strong interannual variation and negative correlations with the strength of EAWM. Model results show that, accounting for sulfate, nitrate, ammonium, black carbon, and organic carbon aerosols, the winter surface layer PM2.5 concentration averaged over eastern China (110°-125°E, 20°-45°N) can be 17.97% (4.78 µg m-3) higher in the weak monsoon years than that in the strong monsoon years. Regionally, the weakening of EAWM is shown to be able to increase PM2.5 concentration in the middle and lower reach of the Yellow River by 12 µg m-3. This point indicates that climate change associated with variation of EAWM has an essential influence on worsening air quality over eastern China. The possible causes of higher aerosol concentrations in the weak monsoon years may be attributed to the changing in wind fields and planetary boundary layer height between the weak and strong monsoon years. Sensitivity studies are performed to identify the role of chemical reaction associated with temperature and humidity on the higher aerosol concentrations in the weak monsoon years over eastern China.

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

2013-11-01

Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding these transformation processes has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a Southeast Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high-resolution aerosol mass spectrometry and Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyl tetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

2013-07-01

Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding the process of these transformations has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a South East Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high resolution aerosol mass spectrometry and fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyltetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

Aerosol elemental concentrations in the tropopause region from intercontinental flights with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform

NASA Astrophysics Data System (ADS)

Papaspiropoulos, Giorgos; Martinsson, Bengt G.; Zahn, Andreas; Brenninkmeijer, Carl A. M.; Hermann, Markus; Heintzenberg, Jost; Fischer, Herbert; van Velthoven, Peter F. J.

2002-12-01

This study with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform investigates the aerosol elemental concentrations at 9-11 km altitude in the northern hemisphere. Measurements from 31 intercontinental flights over a 2-year period between Germany and Sri Lanka/Maldives in the Indian Ocean are presented. Aerosol samples were collected with an impaction technique and were analyzed for the concentration of 18 elements using particle-induced X-ray emission (PIXE). Additional measurements of particle number concentrations, ozone and carbon monoxide concentrations, and meteorological modeling were included in the interpretation of the aerosol elemental concentrations. Particulate sulphur was found to be by far the most abundant element. Its upper tropospheric concentration increased, on average, by a factor of 2 from the tropics to midlatitudes, with another factor 2 higher concentrations in the lowermost stratosphere over midlatitudes. Correlation patterns and source profiles suggest contributions from crustal sources and biomass burning, but not from meteor ablation. Coinciding latitudinal gradients in particulate sulphur concentrations and emissions suggest that fossil fuel combustion is an important source of the aerosol in the upper troposphere and lowermost stratosphere. The measurements indicate aerosol transport along isentropic surfaces across the tropopause into the lowermost stratosphere. As a result of the prolonged residence time, ageing via oxidation of sulphur dioxide in the lowermost stratosphere was found to be a likely high-altitude, strong source that, along with downward transport of stratospheric air, could explain the vertical gradient of particulate sulphur mass concentration around the extratropical tropopause.

Capstone Depleted Uranium Aerosol Biokinetics, Concentrations, and Doses

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

Guilmette, Raymond A.; Miller, Guthrie; Parkhurst, MaryAnn

2009-02-26

One of the principal goals of the Capstone Depleted Uranium (DU) Aerosol Study was to quantify and characterize DU aerosols generated inside armored vehicles by perforation with a DU penetrator. This study consequently produced a database in which the DU aerosol source terms were specified both physically and chemically for a variety of penetrator-impact geometries and conditions. These source terms were used to calculate radiation doses and uranium concentrations for various scenarios as part of the Capstone DU Human Health Risk Assessment (HHRA). This paper describes the scenario-related biokinetics of uranium, and summarizes intakes, chemical concentrations to the organs, andmore » E(50) and HT(50) for organs and tissues based on exposure scenarios for personnel in vehicles at the time of perforation as well as for first responders. For a given exposure scenario (duration time and breathing rates), the range of DU intakes among the target vehicles and shots was not large, about a factor of 10, with the lowest being from a ventilated operational Abrams tank and the highest being for an unventilated Abrams with DU penetrator perforating DU armor. The ranges of committed effective doses were more scenario-dependent than were intakes. For example, the largest range, a factor of 20, was shown for scenario A, a 1-min exposure, whereas, the range was only a factor of two for the first-responder scenario (E). In general, the committed effective doses were found to be in the tens of mSv. The risks ascribed to these doses are discussed separately.« less

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

DOE PAGES

Wang, Jian; Krejci, Radovan; Giangrande, Scott; ...

2016-10-24

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- andmore » ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.« less

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

NASA Astrophysics Data System (ADS)

Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M. J.; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E.; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L.; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A. F.; Springston, Stephen R.; Tomlinson, Jason M.; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N.; Kulmala, Markku; Machado, Luiz A. T.; Artaxo, Paulo; Andreae, Meinrat O.; Petäjä, Tuukka; Martin, Scot T.

2016-11-01

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall.

PubMed

Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M J; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A F; Springston, Stephen R; Tomlinson, Jason M; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N; Kulmala, Markku; Machado, Luiz A T; Artaxo, Paulo; Andreae, Meinrat O; Petäjä, Tuukka; Martin, Scot T

2016-11-17

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

Determination of low-molecular-weight dicarboxylic acids in atmospheric aerosols by injection-port derivatization and gas chromatography-mass spectrometry.

PubMed

Hsu, Ching-Lin; Ding, Wang-Hsien

2009-12-15

A rapid and environmental-friendly injection-port derivatization with gas chromatography-mass spectrometry (GC-MS) method was developed to determine selected low-molecular weight (LMW) dicarboxylic acids (from C2 to C10) in atmospheric aerosol samples. The parameters related to the derivatization process (i.e., type of ion-pair reagent, injection-port temperature and concentration of ion-pair reagent) were optimized. Tetrabutylammonium hydroxide (TBA-OH) 20 mM in methanol gave excellent yield for di-butyl ester dicarboxylate derivatives at injection-port temperature at 300 degrees C. Solid-phase extraction (SPE) method instead of rotary evaporation was used to concentrate analytes from filter extracts. The recovery from filter extracts ranged from 78 to 95% with relative standard deviation (RSD) less than 12%. Limits of quantitation (LOQs) ranged from 25 to 250 pg/m(3). The concentrations of di-carboxylated C2-C5 and total C6-C10 in particles of atmospheric aerosols ranged from 91.9 to 240, 11.3 to 56.7, 9.2 to 49.2, 8.7 to 35.3 and n.d. to 37.8 ng/m(3), respectively. Oxalic acid (C2) was the dominant LMW-dicarboxylic acids detected in aerosol samples. The quantitative results were comparable to the results obtained by the off-line derivatization.

Glyoxal contribution to aerosols over Los Angeles

NASA Astrophysics Data System (ADS)

Balcerak, Ernie

2012-01-01

Laboratory and field studies have indicated that glyoxal (chemical formula OCHCHO), an atmospheric oxidation product of isoprene and aromatic compounds, may contribute to secondary organic aerosols in the atmosphere, which can block sunlight and affect atmospheric chemistry. Some aerosols are primary aerosols, emitted directly into the atmosphere, while others are secondary, formed through chemical reactions in the atmosphere. Washenfelder et al. describe in situ glyoxal measurements from Pasadena, Calif., near Los Angeles, made during summer 2010. They used three different methods to calculate the contribution of glyoxal to secondary atmospheric aerosol and found that it is responsible for 0-0.2 microgram per cubic meter, or 0-4%, of the secondary organic aerosol mass. The researchers also compared their results to those of a previous study that calculated the glyoxal contribution to aerosol for Mexico City. Mexico City had higher levels of organic aerosol mass from glyoxal. They suggest that the lower contribution of glyoxal to aerosol concentrations for Los Angeles may be due to differences in the composition or water content of the aerosols above the two cities. (Journal of Geophysical Research-Atmospheres, doi:10.1029/2011JD016314, 2011)

Characterization of a real-time tracer for Isoprene Epoxydiols-derived Secondary Organic Aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; de Sá, S. S.; Martin, S. T.; Hu, M.; Budisulistiorini, S. H.; Riva, M.; Surratt, J. D.; St. Clair, J. M.; Isaacman-Van Wertz, G.; Yee, L. D.; Goldstein, A. H.; Carbone, S.; Artaxo, P.; de Gouw, J. A.; Koss, A.; Wisthaler, A.; Mikoviny, T.; Karl, T.; Kaser, L.; Jud, W.; Hansel, A.; Docherty, K. S.; Robinson, N. H.; Coe, H.; Allan, J. D.; Canagaratna, M. R.; Paulot, F.; Jimenez, J. L.

2015-04-01

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene low-NO oxidation pathways, was quantified by applying Positive Matrix Factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of OA in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the SOAS study, 78% of IEPOX-SOA is accounted for the measured molecular tracers, making it the highest level of molecular identification of an ambient SOA component to our knowledge. Enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O ( fC5H6O = C5H6O+/OA) across multiple field, chamber and source datasets. A background of ~ 1.7 ± 0.1‰ is observed in studies strongly influenced by urban, biomass-burning and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.8‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7‰). Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12-40‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3‰) observed in non IEPOX-derived isoprene-SOA indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from

PIXE investigation of aerosol composition over the Zambian Copperbelt

NASA Astrophysics Data System (ADS)

Meter, S. L.; Formenti, P.; Piketh, S. J.; Annegarn, H. J.; Kneen, M. A.

1999-04-01

Atmospheric sulphate aerosol concentrations are of interest in climate change studies because of their negative climate forcing potential. Quantification of their forcing strength requires the compilation of global sulphur emission inventories to determine the magnitude of regional sources. We report on measurements of the ambient aerosol concentrations in proximity to a copper refinery in the central African Copperbelt, along the border of Zambia and the Democratic Republic of the Congo. This region is historically regarded as one of the largest African sources of sulphate aerosols. Sulphate is produced by oxidation in the atmosphere of SO 2 emitted during the pyrometallurgical processing of Cu-Co sulphide ores. Since the last quantification of sulphur emissions (late 1960s), there has been large-scale reduction in copper production and more frequent use of the leaching technique with negligible sulphur emissions. Samples were collected over four weeks, November-December 1996, at Kitwe, Zambia. A low volume two-stage time-resolving aerosol sampler (streaker) was used. Coarse and fine mode aerosols were separated at >2.5 and >10 μmad. Hourly elemental concentrations were determined by 3.2 MeV PIXE, and routinely yielded Si, S, K, Ca, Ti, Mn, Fe, Cu and Zn, above detection limits. Si, K, Ca and Fe (major crustal components) dominated the coarse elemental mass. In the fine stage, S and Si accounted for up to 80% of the measured mass, and S alone up to 60%. Time series analysis allowed the division of sulphur and crustal elements (Si, K, Ca, Fe) between (i) background concentrations representative of synoptic scale air masses; and (ii) contributions from local sources, i.e., copper smelter and re-suspended soil dust. Short duration episodes of S concentrations, up to 26 μg/m 3, were found simultaneously with enhanced Cu, Fe and Zn. Contributions from individual pyrometallurgic processes and the cobalt slag dump could be distinguished from the elemental signatures

Aerosol and CCN in southwest Saudi Arabia

NASA Astrophysics Data System (ADS)

Collins, Don; Li, Runjun; Axisa, Duncan; Kucera, Paul; Burger, Roelof

2010-05-01

As part of an ongoing study of the microphysical and dynamical controls on precipitation in southwest Saudi Arabia, a number of surface and aircraft-based instruments were used in summer / fall 2009 to measure the size distribution, hygroscopic properties, and cloud droplet nucleation efficiency of the local aerosol. Submicron size distributions were measured using differential mobility analyzers both on the ground and on board the aircraft, while an aerodynamic particle sizer and a forward scattering spectrometer probe were used to measure the supermicron size distributions on the ground and from on board the aircraft, respectively. Identical continuous flow cloud condensation nuclei counters were used to measure CCN spectra at the surface and aloft and a humidified tandem differential mobility analyzer was operated on the ground to measure size-resolved hygroscopicity. The aerosol in this arid environment is characterized by a persistent accumulation mode having hygroscopic and CCN efficiency properties consistent with a sulfate-rich aged aerosol. The particles in that background aerosol are generally sufficiently large and hygroscopic to activate at those supersaturations expected in the convective clouds responsible for most of the regional precipitation, which consequently acts as a lower bound on the resulting cloud droplet concentrations. Though the concentration, size distribution, and properties of the submicron aerosol generally changed very slowly over periods of several hours, abrupt ~doubling in concentration almost always accompanied the arrival of the sea breeze front that began along the Red Sea. Interestingly, the hygroscopicity and the shape of the size distribution differed little in the pre- and post-sea breeze air masses. The dust-dominated coarse mode typically contributed significantly more to the aerosol mass concentration than did the submicron mode and likely controlled the ice nuclei concentration, though no direct measurements were made

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.

Measurements of aerosol chemical composition in boreal forest summer conditions

NASA Astrophysics Data System (ADS)

ńijälä, M.; Junninen, H.; Ehn, M.; Petäjä, T.; Vogel, A.; Hoffmann, T.; Corrigan, A.; Russell, L.; Makkonen, U.; Virkkula, A.; Mäntykenttä, J.; Kulmala, M.; Worsnop, D.

2012-04-01

Boreal forests are an important biome, covering vast areas of the northern hemisphere and affecting the global climate change via various feedbacks [1]. Despite having relatively few anthropogenic primary aerosol sources, they always contain a non-negligible aerosol population [2]. This study describes aerosol chemical composition measurements using Aerodyne Aerosol Mass Spectrometer (C-ToF AMS, [3]), carried out at a boreal forest area in Hyytiälä, Southern Finland. The site, Helsinki University SMEAR II measurement station [4], is situated at a homogeneous Scots pine (Pinus sylvestris) forest stand. In addition to the station's permanent aerosol, gas phase and meteorological instruments, during the HUMPPA (Hyytiälä United Measurements of Photochemistry and Particles in Air) campaign in July 2010, a very comprehensive set of atmospheric chemistry measurement instrumentation was provided by the Max Planck Institute for chemistry, Johannes Gutenberg-University, University of California and the Finnish Meteorological institute. In this study aerosol chemical composition measurements from the campaign are presented. The dominant aerosol chemical species during the campaign were the organics, although periods with elevated amounts of particulate sulfates were also seen. The overall AMS measured particle mass concentrations varied from near zero to 27 μg/m observed during a forest fire smoke episode. The AMS measured aerosol mass loadings were found to agree well with DMPS derived mass concentrations (r2=0.998). The AMS data was also compared with three other aerosol instruments. The Marga instrument [5] was used to provide a quantitative semi-online measurement of inorganic chemical compounds in particle phase. Fourier Transform Infrared Spectroscopy (FTIR) analysis was performed on daily filter samples, enabling the identification and quantification of organic aerosol subspecies. Finally an Atmospheric Pressure Chemical Ionization Ion Trap Mass Spectrometer (APCI

Elucidating the relationship between aerosol concentration and summertime boundary layer structure in central China.

PubMed

Liu, Lin; Guo, Jianping; Miao, Yucong; Liu, Lin; Li, Jian; Chen, Dandan; He, Jing; Cui, Chunguang

2018-06-11

Wuhan, a megacity in central China, suffers from frequent aerosol pollution and is accompanied by meteorological factors at both synoptic and local scales. Partly due to the lack of appropriate observations of planetary boundary layer (PBL), the associations between synoptic conditions, PBL, and pollution there are not yet fully understood. Thus, systematic analyses were conducted using the fine-resolution soundings, surface meteorological measurements, and aerosol observations in Wuhan during summer for the period 2013-2016, in combination with T-mode principal component analysis and simulations of backward trajectory. The results showed that the variations of boundary layer height (BLH) not only modulated the diurnal variation of PM 2.5 concentration in Wuhan, but also the daily pollution level. Five different synoptic patterns during summer in Wuhan were identified from reanalysis geopotential height fields. Among these synoptic patterns, two types characterized by northeasterly prevailing winds, were found to be associated with heavy pollution in Wuhan. Driven by the northeasterly winds, the polluted air mass from the heavily polluted regions could be easily transported to Wuhan, such as North China Plain and Yangtze River Delta. Such regional transports of pollutants must be partly responsible for the aerosol pollution in Wuhan. In addition, these two synoptic patterns were also featured by the relatively high cloud cover and low boundary layer height in Wuhan, which would favor the occurrence of pollution there. Overall, this study has important implications for understanding the important roles of meteorological factors in modulating aerosol pollution in central China. Copyright © 2018 Elsevier Ltd. All rights reserved.

Sugars in Antarctic aerosol

NASA Astrophysics Data System (ADS)

Barbaro, Elena; Kirchgeorg, Torben; Zangrando, Roberta; Vecchiato, Marco; Piazza, Rossano; Barbante, Carlo; Gambaro, Andrea

2015-10-01

The processes and transformations occurring in the Antarctic aerosol during atmospheric transport were described using selected sugars as source tracers. Monosaccharides (arabinose, fructose, galactose, glucose, mannose, ribose, xylose), disaccharides (sucrose, lactose, maltose, lactulose), alcohol-sugars (erythritol, mannitol, ribitol, sorbitol, xylitol, maltitol, galactitol) and anhydrosugars (levoglucosan, mannosan and galactosan) were measured in the Antarctic aerosol collected during four different sampling campaigns. For quantification, a sensitive high-pressure anion exchange chromatography was coupled with a single quadrupole mass spectrometer. The method was validated, showing good accuracy and low method quantification limits. This study describes the first determination of sugars in the Antarctic aerosol. The total mean concentration of sugars in the aerosol collected at the ;Mario Zucchelli; coastal station was 140 pg m-3; as for the aerosol collected over the Antarctic plateau during two consecutive sampling campaigns, the concentration amounted to 440 and 438 pg m-3. The study of particle-size distribution allowed us to identify the natural emission from spores or from sea-spray as the main sources of sugars in the coastal area. The enrichment of sugars in the fine fraction of the aerosol collected on the Antarctic plateau is due to the degradation of particles during long-range atmospheric transport. The composition of sugars in the coarse fraction was also investigated in the aerosol collected during the oceanographic cruise.

The performance and the characterization of laser ablation aerosol particle time-of-flight mass spectrometry (LAAP-ToF-MS)

NASA Astrophysics Data System (ADS)

Gemayel, Rachel; Hellebust, Stig; Temime-Roussel, Brice; Hayeck, Nathalie; Van Elteren, Johannes T.; Wortham, Henri; Gligorovski, Sasho

2016-05-01

Hyphenated laser ablation-mass spectrometry instruments have been recognized as useful analytical tools for the detection and chemical characterization of aerosol particles. Here we describe the performances of a laser ablation aerosol particle time-of-flight mass spectrometer (LAAP-ToF-MS) which was designed for aerodynamic particle sizing using two 405 nm scattering lasers and characterization of the chemical composition of single aerosol particle via ablation/ionization by a 193 nm excimer laser and detection in a bipolar time-of-flight mass spectrometer with a mass resolving power of m/Δm > 600.

We describe a laboratory based optimization strategy for the development of an analytical methodology for characterization of atmospheric particles using the LAAP-ToF-MS instrument in combination with a particle generator, a differential mobility analyzer and an optical particle counter. We investigated the influence of particle number concentration, particle size and particle composition on the detection efficiency. The detection efficiency is a product of the scattering efficiency of the laser diodes and the ionization efficiency or hit rate of the excimer laser. The scattering efficiency was found to vary between 0.6 and 1.9 % with an average of 1.1 %; the relative standard deviation (RSD) was 17.0 %. The hit rate exhibited good repeatability with an average value of 63 % and an RSD of 18 %. In addition to laboratory tests, the LAAP-ToF-MS was used to sample ambient air during a period of 6 days at the campus of Aix-Marseille University, situated in the city center of Marseille, France. The optimized LAAP-ToF-MS methodology enables high temporal resolution measurements of the chemical composition of ambient particles, provides new insights into environmental science, and a new investigative tool for atmospheric chemistry and physics, aerosol science and health impact studies.

Composition and diurnal variability of the natural Amazonian aerosol

NASA Astrophysics Data System (ADS)

Graham, Bim; Guyon, Pascal; Maenhaut, Willy; Taylor, Philip E.; Ebert, Martin; Matthias-Maser, Sabine; Mayol-Bracero, Olga L.; Godoi, Ricardo H. M.; Artaxo, Paulo; Meixner, Franz X.; Moura, Marcos A. Lima; Rocha, Carlos H. EçA. D'almeida; Grieken, Rene Van; Glovsky, M. Michael; Flagan, Richard C.; Andreae, Meinrat O.

2003-12-01

As part of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA)-Cooperative LBA Airborne Regional Experiment (CLAIRE) 2001 campaign, separate day and nighttime aerosol samples were collected in July 2001 at a ground-based site in Amazonia, Brazil, in order to examine the composition and temporal variability of the natural "background" aerosol. A combination of analytical techniques was used to characterize the elemental and ionic composition of the aerosol. Major particle types larger than ˜0.5 μm were identified by electron and light microscopy. Both the coarse and fine aerosol were found to consist primarily of organic matter (˜70 and 80% by mass, respectively), with the coarse fraction containing small amounts of soil dust and sea-salt particles and the fine fraction containing some non-sea-salt sulfate. Coarse particulate mass concentrations (CPM ≈ PM10 - PM2) were found to be highest at night (average = 3.9 ± 1.4 μg m-3, mean night-to-day ratio = 1.9 ± 0.4), while fine particulate mass concentrations (FPM ≈ PM2) increased during the daytime (average = 2.6 ± 0.8 μg m-3, mean night-to-day ratio = 0.7 ± 0.1). The nocturnal increase in CPM coincided with an increase in primary biological particles in this size range (predominantly yeasts and other fungal spores), resulting from the trapping of surface-derived forest aerosol under a shallow nocturnal boundary layer and a lake-land breeze effect at the site, although active nocturnal sporulation may have also contributed. Associated with this, we observed elevated nighttime concentrations of biogenic elements and ions (P, S, K, Cu, Zn, NH4+) in the CPM fraction. For the FPM fraction a persistently higher daytime concentration of organic carbon was found, which indicates that photochemical production of secondary organic aerosol from biogenic volatile organic compounds may have made a significant contribution to the fine aerosol. Dust and sea-salt-associated elements/ions in the CPM fraction

THE MASS ACCOMMODATION COEFFICIENT OF AMMONIUM NITRATE AEROSOL. (R823514)

EPA Science Inventory

The mass transfer rate of pure ammonium nitrate between the aerosol and gas phases was
quantified experimentally by the use of the tandem differential mobility analyzer/scanning mobility
particle sizer (TDMA/SMPS) technique. Ammonium nitrate particles 80-220 nm in diameter<...

ASSESSMENT OF THE LIQUID WATER CONTENT OF SUMMERTIME AEROSOL IN THE SOUTHEAST UNITED STATES

EPA Science Inventory

The concentration of aerosol liquid water mass represents an important parameter for understanding the physical properties of PM2.5 in the atmosphere. Increases in ambient relative humidity can increase aerosol liquid water and thus the composite particle mass and particle volu...

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.

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.

Bio-Aerosol Detection Using Mass Spectrometry: Public Health Applications

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

Ludvigson, Laura D.

2004-01-01

I recently spent a summer as an intern at the Lawrence Livermore National Laboratory. I worked on a project involving the real-time, reagentless, single cell detection of aerosolized pathogens using a novel mass spectrometry approach called Bio-Aerosol Mass Spectrometry (BAMS). Based upon preliminary results showing the differentiation capabilities of BAMS, I would like to explore the development and use of this novel detection system in the context of both environmental and clinical sample pathogen detection. I would also like to explore the broader public health applications that a system such as BAMS might have in terms of infectious disease preventionmore » and control. In order to appreciate the potential of this instrument, I will demonstrate the need for better pathogen detection methods, and outline the instrumentation, data analysis and preliminary results that lead me toward a desire to explore this technology further. I will also discuss potential experiments for the future along with possible problems that may be encountered along the way.« less

EFFECT OF ACIDITY ON SECONDARY ORGANIC AEROSOL FORMATION FROM ISOPRENE

EPA Science Inventory

The effect of particle-phase acidity on secondary organic aerosol (SOA) formation from isoprene is investigated in a laboratory chamber study, in which the acidity of the inorganic seed aerosol was controlled systematically. The observed enhancement in SOA mass concentration is c...

A New Method Using Single-Particle Mass Spectrometry Data to Distinguish Mineral Dust and Biological Aerosols

NASA Astrophysics Data System (ADS)

Al-Mashat, H.; Kristensen, L.; Sultana, C. M.; Prather, K. A.

2016-12-01

The ability to distinguish types of particles present within a cloud is important for determining accurate inputs to climate models. The chemical composition of particles within cloud liquid droplets and ice crystals can have a significant impact on the timing, location, and amount of precipitation that falls. Precipitation efficiency is increased by the presence of ice crystals in clouds, and both mineral dust and biological aerosols have been shown to be effective ice nucleating particles (INPs) in the atmosphere. A current challenge in aerosol science is distinguishing mineral dust and biological material in the analysis of real-time, ambient, single-particle mass spectral data. Single-particle mass spectrometers are capable of measuring the size-resolved chemical composition of individual atmospheric particles. However, there is no consistent analytical method for distinguishing dust and biological aerosols. Sampling and characterization of control samples (i.e. of known identity) of mineral dust and bacteria were performed by the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) as part of the Fifth Ice Nucleation (FIN01) Workshop at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility in Karlsruhe, Germany. Using data collected by the ATOFMS of control samples, a new metric has been developed to classify single particles as dust or biological independent of spectral cluster analysis. This method, involving the use of a ratio of mass spectral peak areas for organic nitrogen and silicates, is easily reproducible and does not rely on extensive knowledge of particle chemistry or the ionization characteristics of mass spectrometers. This represents a step toward rapidly distinguishing particle types responsible for ice nucleation activity during real-time sampling in clouds. The ability to distinguish types of particles present within a cloud is important for determining accurate inputs to climate models. The chemical composition of particles

Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

NASA Astrophysics Data System (ADS)

Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

2008-12-01

The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

Expanding Single Particle Mass Spectrometer Analyses for the Identification of Microbe Signatures in Sea Spray Aerosol.

PubMed

Sultana, Camille M; Al-Mashat, Hashim; Prather, Kimberly A

2017-10-03

Ocean-derived microbes in sea spray aersosol (SSA) have the potential to influence climate and weather by acting as ice nucleating particles in clouds. Single particle mass spectrometers (SPMSs), which generate in situ single particle composition data, are excellent tools for characterizing aerosols under changing environmental conditions as they can provide high temporal resolution and require no sample preparation. While SPMSs have proven capable of detecting microbes, these instruments have never been utilized to definitively identify aerosolized microbes in ambient sea spray aersosol. In this study, an aerosol time-of-flight mass spectrometer was used to analyze laboratory generated SSA produced from natural seawater in a marine aerosol reference tank. We present the first description of a population of biological SSA mass spectra (BioSS), which closely match the ion signatures observed in previous terrestrial microbe studies. The fraction of BioSS dramatically increased in the largest supermicron particles, consistent with field and laboratory measurements of microbes ejected by bubble bursting, further supporting the assignment of BioSS mass spectra as microbes. Finally, as supported by analysis of inorganic ion signals, we propose that dry BioSS particles have heterogeneous structures, with microbes adhered to sodium chloride nodules surrounded by magnesium-enriched coatings. Consistent with this structure, chlorine-containing ion markers were ubiquitous in BioSS spectra and identified as possible tracers for distinguishing recently aerosolized marine from terrestrial microbes.

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

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.

Concentration Effects and Ion Properties Controlling the Fractionation of Halides during Aerosol Formation

NASA Technical Reports Server (NTRS)

Guzman, Marcelo I.; Athalye, Richa R.; Rodriguez, Jose M.

2012-01-01

During the aerosolization process at the sea surface, halides are incorporated into aerosol droplets, where they may play an important role in tropospheric ozone chemistry. Although this process may significantly contribute to the formation of reactive gas phase molecular halogens, little is known about the environmental factors that control how halides selectively accumulate at the air-water interface. In this study, the production of sea spray aerosol is simulated using electrospray ionization (ESI) of 100 nM equimolar solutions of NaCl, NaBr, NaI, NaNO2, NaNO3, NaClO4, and NaIO4. The microdroplets generated are analyzed by mass spectrometry to study the comparative enrichment of anions (f (Isub x-)) and their correlation with ion properties. Although no correlation exists between f (sub x-) and the limiting equivalent ionic conductivity, the correlation coefficient of the linear fit with the size of the anions R(sub x-), dehydration free-energy ?Gdehyd, and polarizability alpha, follows the order: (R(sub x-)(exp -2)) > (R(sub x-)(exp -1)) >(R(sub x-) > delta G(sub dehyd) > alpha. The same pure physical process is observed in H2O and D2O. The factor f (sub x-) does not change with pH (6.8-8.6), counterion (Li+, Na+, K+, and Cs+) substitution effects, or solvent polarity changes in methanol - and ethanol-water mixtures (0 <= xH2O <= 1). Sodium polysorbate 20 surfactant is used to modify the structure of the interface. Despite the observed enrichment of I- on the air-water interface of equimolar solutions, our results of seawater mimic samples agree with a model in which the interfacial composition is increasingly enriched in I- < Br- < Cl- over the oceanic boundary layer due to concentration effects in sea spray aerosol formation.

Single particle characterization using a light scattering module coupled to a time-of-flight aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Cross, E. S.; Onasch, T. B.; Canagaratna, M.; Jayne, J. T.; Kimmel, J.; Yu, X.-Y.; Alexander, M. L.; Worsnop, D. R.; Davidovits, P.

2008-12-01

We present the first single particle results obtained using an Aerodyne time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS). The instrument was deployed at the T1 ground site approximately 40 km northeast of the Mexico City Metropolitan Area (MCMA) as part of the MILAGRO field study in March of 2006. The instrument was operated as a standard AMS from 12-30 March, acquiring average chemical composition and size distributions for the ambient aerosol, and in single particle mode from 27-30 March. Over a 75-h sampling period, 12 853 single particle mass spectra were optically triggered, saved, and analyzed. The correlated optical and chemical detection allowed detailed examination of single particle collection and quantification within the LS-ToF-AMS. The single particle data enabled the mixing states of the ambient aerosol to be characterized within the context of the size-resolved ensemble chemical information. The particulate mixing states were examined as a function of sampling time and most of the particles were found to be internal mixtures containing many of the organic and inorganic species identified in the ensemble analysis. The single particle mass spectra were deconvolved, using techniques developed for ensemble AMS data analysis, into HOA, OOA, NH4NO3, (NH4)2SO4, and NH4Cl fractions. Average single particle mass and chemistry measurements are shown to be in agreement with ensemble MS and PTOF measurements. While a significant fraction of ambient particles were internal mixtures of varying degrees, single particle measurements of chemical composition allowed the identification of time periods during which the ambient ensemble was externally mixed. In some cases the chemical composition of the particles suggested a likely source. Throughout the full sampling period, the ambient ensemble was an external mixture of combustion-generated HOA particles from local sources (e.g. traffic), with number concentrations peaking

Emission Controls Versus Meteorological Conditions in Determining Aerosol Concentrations in Beijing during the 2008 Olympic Games

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

Gao, Yi; Liu, Xiaohong; Zhao, Chun

A series of emission control measures were undertaken in Beijing and the adjacent provinces in China during the 2008 Beijing Olympic Games on August 8th-24th, 2008. This provides a unique opportunity for investigating the effectiveness of emission controls on air pollution in Beijing. We conducted a series of numerical experiments over East Asia for the period of July to September 2008 using a coupled meteorology-chemistry model (WRF-Chem). Model can generally reproduce the observed variation of aerosol concentrations. Consistent with observations, modeled concentrations of aerosol species (sulfate, nitrate, ammonium, black carbon, organic carbon, total particulate matter) in Beijing were decreased bymore » 30-50% during the Olympic period compared to the other periods in July and August in 2008 and the same period in 2007. Model results indicate that emission controls were effective in reducing the aerosol concentrations by comparing simulations with and without emission controls. However, our analysis suggests that meteorological conditions (e.g., wind direction and precipitation) are at least as important as emission controls in producing the low aerosol concentrations appearing during the Olympic period. Transport from the regions surrounding Beijing determines the temporal variation of aerosol concentrations in Beijing. Based on the budget analysis, we suggest that emission control strategy should focus on the regional scale instead of the local scale to improve the air quality over Beijing.« less

Impacts of Future European Emission Reductions on Aerosol Particle Number Concentrations Accounting for Effects of Ammonia, Amines, and Organic Species.

PubMed

Julin, Jan; Murphy, Benjamin N; Patoulias, David; Fountoukis, Christos; Olenius, Tinja; Pandis, Spyros N; Riipinen, Ilona

2018-01-16

Although they are currently unregulated, atmospheric ultrafine particles (<100 nm) pose health risks because of, e.g., their capability to penetrate deep into the respiratory system. Ultrafine particles, often minor contributors to atmospheric particulate mass, typically dominate aerosol particle number concentrations. We simulated the response of particle number concentrations over Europe to recent estimates of future emission reductions of aerosol particles and their precursors. We used the chemical transport model PMCAMx-UF, with novel updates including state-of-the-art descriptions of ammonia and dimethylamine new particle formation (NPF) pathways and the condensation of organic compounds onto particles. These processes had notable impacts on atmospheric particle number concentrations. All three emission scenarios (current legislation, optimized emissions, and maximum technically feasible reductions) resulted in substantial (10-50%) decreases in median particle number concentrations over Europe. Consistent reductions were predicted in Central Europe, while Northern Europe exhibited smaller reductions or even increased concentrations. Motivated by the improved NPF descriptions for ammonia and methylamines, we placed special focus on the potential to improve air quality by reducing agricultural emissions, which are a major source of these species. Agricultural emission controls showed promise in reducing ultrafine particle number concentrations, although the change is nonlinear with particle size.

Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

DOE PAGES

Parworth, Caroline; Tilp, Alison; Fast, Jerome; ...

2015-04-01

In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

Fine Mode Aerosol over the United Arab Emirates

NASA Astrophysics Data System (ADS)

Ross, K. E.; Piketh, S. J.; Reid, J. S.; Reid, E. A.

2005-12-01

The aerosol loading of the atmosphere over the Arabian Gulf region is extremely diverse and is composed not only of dust, but also of pollution that is derived largely from oil-related activities. Fine mode pollution particles are most efficient at scattering incoming solar radiation and have the potential to act as cloud condensation nuclei (CCN), and may therefore have implications for climate change. The smaller aerosols may also pose a health hazard if present in high concentrations. The United Arab Emirates Unified Aerosol Experiment (UAE2) was designed to investigate aerosol and meteorological characteristics over the region using ground-based, aircraft and satellite measurements, and was conducted in August and September 2004. Aerosol chemical composition has been obtained from filters that were collected at the site of the Mobile Atmospheric Aerosol and Radiation Characterization Observatory (MAARCO) on the coast of the UAE between Abu Dhabi and Dubai. Filter samples were also collected on an airborne platform in order to assess how aerosol chemical composition varies across the region and throughout the depth of the boundary layer. Results of the analysis of the PM2.5 coastal samples show that ammonium sulphate is the most prevalent constituent of the fine mode aerosol in the region (>50% of the mass), followed by organic matter, alumino-silicates, calcium carbonate and black carbon. Source apportionment indicates that most of the fine aerosol mass is derived from fossil fuel combustion, while mineral dust and local vehicle emissions also contribute to the fine aerosol loading. The organic carbon-to-total carbon ratio of the aerosol is 0.65, which is typical of fossil fuel combustion. The dominance of sulphates means that the fine mode aerosol in the region is probably responsible for a negative radiative forcing, and that the polluting emissions significantly elevate the concentration of CCN.

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

Characterization of cumulus cloud fields using trajectories in the center of gravity versus water mass phase space: 2. Aerosol effects on warm convective clouds: Center of Gravity Versus Water Mass 2

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

Heiblum, Reuven H.; Altaratz, Orit; Koren, Ilan

2016-06-07

In Part I of this work a 3D cloud tracking algorithm and phase-space of center of gravity altitude versus cloud liquid water mass (CvM space) were introduced and described in detail. We showed how new physical insight can be gained by following cloud trajectories in the CvM space. Here, this approach is used to investigate aerosol effects on cloud fields of warm cumuli. We show a clear effect of the aerosol loading on the shape and size of CvM clusters. We also find fundamental differences in the CvM space between simulations using bin versus bulk microphysical schemes, with the binmore » scheme precipitation expressing much higher sensitivity to changes in aerosol concentrations. Using the bin microphysical scheme, we find that the increase in cloud center of gravity altitude with increase in aerosol concentrations occurs for a wide range of cloud sizes. This is attributed to reduced sedimentation, increased buoyancy and vertical velocities, and increased environmental instability, all of which are tightly coupled to inhibition of precipitation processes and subsequent feedbacks of clouds on their environment. Many of the physical processes shown here are consistent with processes typically associated with cloud invigoration.« less

Molecular composition of boreal forest aerosol from Hyytiälä, Finland, using ultrahigh resolution mass spectrometry.

PubMed

Kourtchev, Ivan; Fuller, Stephen; Aalto, Juho; Ruuskanen, Taina M; McLeod, Matthew W; Maenhaut, Willy; Jones, Rod; Kulmala, Markku; Kalberer, Markus

2013-05-07

Organic compounds are important constituents of fine particulate matter (PM) in the troposphere. In this study, we applied direct infusion nanoelectrospray (nanoESI) ultrahigh resolution mass spectrometry (UHR-MS) and liquid chromatography LC/ESI-UHR-MS for the analysis of the organic fraction of PM1 aerosol samples collected over a two week period at a boreal forest site (Hyytiälä), southern Finland. Elemental formulas (460-730 in total) were identified with nanoESI-UHR-MS in the negative ionization mode and attributed to organic compounds with a molecular weight below 400. Kendrick Mass Defect and Van Krevelen approaches were used to identify compound classes and mass distributions of the detected species. The molecular composition of the aerosols strongly varied between samples with different air mass histories. An increased number of nitrogen, sulfur, and highly oxygenated organic compounds was observed during the days associated with continental air masses. However, the samples with Atlantic air mass history were marked by a presence of homologous series of unsaturated and saturated C12-C20 fatty acids suggesting their marine origin. To our knowledge, we show for the first time that the highly detailed chemical composition obtained from UHR-MS analyses can be clearly linked to meteorological parameters and trace gases concentrations that are relevant to atmospheric oxidation processes. The additional LC/ESI-UHR-MS analysis revealed 29 species, which were mainly attributed to oxidation products of biogenic volatile compounds BVOCs (i.e., α,β-pinene, Δ3-carene, limonene, and isoprene) supporting the results from the direct infusion analysis.

[A simple testing installation for the production of aerosols with constant bacteria-contaminated concentrations].

PubMed

Herbst, M; Lehmhus, H; Oldenburg, B; Orlowski, C; Ohgke, H

1983-04-01

A simple experimental set for the production and investigation of bacterially contaminated solid-state aerosols with constant concentration is described. The experimental set consists mainly of a fluidized bed-particle generator within a modified chamber for formaldehyde desinfection. The special conditions for the production of a defined concentration of particles and microorganisms are to be found out empirically. In a first application aerosol-sizing of an Andersen sampler is investigated. The findings of Andersen (1) are confirmed with respect to our experimental conditions.

Assessing the impact of industrial source emissions on atmospheric carbonaceous aerosol concentrations using routine monitoring networks.

PubMed

Sheesley, Rebecca J; Schauer, James J; Orf, Marya L

2010-02-01

Industrial sources can have a significant but poorly defined impact on ambient particulate matter concentrations in select areas. Detailed emission profiles are often not available and are hard to develop because of the diversity of emissions across time and space at large industrial complexes. A yearlong study was conducted in an industrial area in Detroit, MI, which combined real-time particle mass (tapered element oscillating microbalance) and black carbon (aetholometer) measurements with molecular marker measurements of monthly average concentrations as well as daily concentrations of select high pollution days. The goal of the study was to use the real-time data to define days in which the particulate matter concentration in the atmosphere was largely impacted by local source emissions and to use daily speciation data to derive emission profiles for the industrial source. When combined with motor vehicle exhaust, wood smoke and road dust profiles, the industrial source profile was used to determine the contribution of the local industrial source to the total organic carbon (OC) concentrations using molecular marker-chemical mass balance modeling (MM-CMB). The MM-CMB analysis revealed that the industrial source had minimal impact on the monthly average carbonaceous aerosol concentration, but contributed approximately 2 microg m(-3), or a little over one-third of the total OC, on select high-impact days.

Toward understanding atmospheric physics impacting the relationship between columnar aerosol optical depth and near-surface PM2.5 mass concentrations in Nevada and California, U.S.A., during 2013

NASA Astrophysics Data System (ADS)

Loría-Salazar, S. Marcela; Panorska, Anna; Arnott, W. Patrick; Barnard, James C.; Boehmler, Jayne M.; Holmes, Heather A.

2017-12-01

Determining the relationship between columnar aerosol optical depth (τext) and surface particulate matter concentrations (PM2.5) is desired to estimate surface aerosol concentrations over broad spatial and temporal scales using satellite remote sensing. However, remote sensing studies incur challenges when surface aerosol pollution (i.e. PM2.5) is not correlated with columnar conditions (i.e., τext). PM2.5 data fusion models that rely on satellite data and statistical relationships of τext and PM2.5 may not be able to capture the physical conditions impacting the relationships that cause columnar and surface aerosols to not be correlated in the western U.S. Therefore, an extensive examination of the atmospheric conditions is required to improve surface estimates of PM2.5 that rely on columnar aerosol measurements. This investigation uses datasets from both routine monitoring networks and models of meteorological variables and aerosol physical parameters to understand the atmospheric conditions under which surface aerosol pollution can be explained by column measurements in California and Nevada during 2013. A novel quadrant method, that utilizes statistical analysis, was developed to investigate the relationship between τext and PM2.5. The results from this investigation show that τext and PM2.5 had a positive association (τext and PM2.5 increase together) when local sources of pollution or wildfires dominated aerosol pollution in the presence of a deep and well-mixed planetary boundary layer (PBL). Moreover, τext and PM2.5 had no association (where the variables are not related) when stable conditions, long-range transport, or entrainment of air from above the PBL were observed. It was found that seasonal categorization of the relationship between τext and PM2.5, an approach commonly used in statistical models to estimate surface concentrations with satellite remote sensing, may not be enough to account for the atmospheric conditions that drive the

Coupling a versatile aerosol apparatus to a synchrotron: Vacuum ultraviolet light scattering, photoelectron imaging, and fragment free mass spectrometry

NASA Astrophysics Data System (ADS)

Shu, Jinian; Wilson, Kevin R.; Ahmed, Musahid; Leone, Stephen R.

2006-04-01

An aerosol apparatus has been coupled to the Chemical Dynamics Beamline of the Advanced Light Source at Lawrence Berkeley National Laboratory. This apparatus has multiple capabilities for aerosol studies, including vacuum ultraviolet (VUV) light scattering, photoelectron imaging, and mass spectroscopy of aerosols. By utilizing an inlet system consisting of a 200μm orifice nozzle and aerodynamic lenses, aerosol particles of ˜50nm-˜1μm in diameter can be sampled directly from atmospheric pressure. The machine is versatile and can probe carbonaceous aerosols generated by a laboratory flame, nebulized solutions of biological molecules, hydrocarbon aerosol reaction products, and synthesized inorganic nanoparticles. The sensitivity of this apparatus is demonstrated by the detection of nanoparticles with VUV light scattering, photoelectron imaging, and charged particle detection. In addition to the detection of nanoparticles, the thermal vaporization of aerosols on a heater tip leads to the generation of intact gas phase molecules. This phenomenon coupled to threshold single photon ionization, accessible with tunable VUV light, allows for fragment-free mass spectrometry of complex molecules. The initial experiments with light scattering, photoelectron imaging, and aerosol mass spectrometry reported here serve as a demonstration of the design philosophy and multiple capabilities of the apparatus.

Estimation of the Cloud condensation nuclei concentration(CCN) and aerosol optical depth(AOD) relation in the Arctic region

NASA Astrophysics Data System (ADS)

Jung, C. H.; Yoon, Y. J.; Ahn, S. H.; Kang, H. J.; Gim, Y. T.; Lee, B. Y.

2017-12-01

Information of the spatial and temporal variations of cloud condensation nuclei (CCN) concentrations is important in estimating aerosol indirect effects. Generally, CCN aerosol is difficult to estimate using remote sensing methods. Although there are many CCN measurements data, extensive measurements of CCN are not feasible because of the complex nature of the operation and high cost, especially in the Arctic region. Thus, there have been many attempts to estimate CCN concentrations from more easily obtainable parameters such as aerosol optical depth (AOD) because AOD has the advantage of being readily observed by remote sensing from space by several sensors. For example, some form of correlation was derived between AOD and the number concentration of cloud condensation nuclei (CCN) through the comparison results from AERONET network and CCN measurements (Andreae 2009). In this study, a parameterization of CCN concentration as a function of AOD at 500 nm is given in the Arctic region. CCN data was collected during the period 2007-2013 at the Zeppelin observatory (78.91° N, 11.89° E, 474 masl). The AERONET network and MODIS AOD data are compared with ground measured CCN measurement and the relations between AOD and CCN are parameterized. The seasonal characteristics as well as long term trends are also considered. Through the measurement, CCN concentration remains high during spring because of aerosol transportation from the mid-latitudes, known as Arctic Haze. Lowest CCN number densities were observed during Arctic autumn and early winter when aerosol long-range transport into the Arctic is not effective and new particle formation ceases. The results show that the relation between AOD and CCN shows a different parameter depending on the seasonal aerosol and CCN characteristics. This seasonal different CCN-AOD relation can be interpreted as many physico-chemical aerosol properties including aerosol size distribution, composition. ReferenceAndreae, M. O. (2009

Aerosol particle and organic vapor concentrations at industrial work sites in Malaysia.

PubMed

Armstrong, R W; Rood, M J; Sani, S; Mohamed, M; Rashid, M; Jab, A T; Landsberger, S

2001-01-01

The objective of this study was to establish baseline data about air pollutants potentially related to nasopharyngeal carcinoma (NPC) in the Federal Territory and Selangor, Malaysia. During 1991-1993, ambient air quality was monitored at 42 work sites representing ten industrial sectors: adhesive manufacturing, foundries, latex processing, metalworking, plywood/veneer milling, ricemilling, rubber tire manufacturing, sawmilling, shoemaking, and textile related industries. At each work site, aerosol particle size distributions and concentrations of formaldehyde, benzene, toluene, isopropyl alcohol, and furfural were measured. Mean aerosol particle concentrations ranged from 61 micrograms/m3 in foundries to 5,578 micrograms/m3 in ricemills, with five industries (adhesives, metalworking, ricemilling, sawmilling, and shoemaking) exceeding the US EPA 24-hr ambient air standard for PM-10. Formaldehyde concentrations exceeded the threshold limit value (TLV) in adhesives factories. Other vapours and elements measured were well below TLVs.

Sea-State Dependence of Aerosol Concentration in the Marine Atmospheric Boundary Layer

NASA Astrophysics Data System (ADS)

Lenain, L.; Melville, W. K.

2016-02-01

While sea spray aerosols represent a large portion of the aerosols present in the marine environment, and despite evidence of the importance of surface wave and wave-breaking related processes in the coupling of the ocean with the atmosphere, sea spray source generation functions are traditionally parameterized by the wind speed at 10m. It is clear that unless the wind and wave field are fully developed, the source function will be a function of both wind and wave parameters. In this study, we report on an air-sea interaction experiment, the ONR phase-resolved High-Resolution Air-Sea Interaction experiments (HIRES), conducted off the coast of Northern California in June 2010. Detailed measurements of aerosol number concentration in the Marine Atmospheric Boundary Layer (MABL), at altitudes ranging from as low as 30m and up to 800m AMSL over a broad range of environmental conditions (significant wave height, Hs, of 2 to 4.5m and wind speed at 10m height, U10, of 10 to 18 m/s) collected from an instrumented research aircraft, are presented. Aerosol number densities and volume are computed over a range of particle diameters from 0.1 to 200 µm, while the surface conditions, i.e. significant wave height, moments of the breaker length distribution Λ(c), and wave breaking dissipation, were measured by a suite of electro-optical sensors that included the NASA Airborne Topographic Mapper (ATM). The sea-state dependence of the aerosol concentration in the MABL is evident, ultimately stressing the need to incorporate wave and wave kinematics in the spray source generation functions that are traditionally primarily parameterized by surface winds. A scaling of the measured aerosol volume distribution by wave and atmospheric state variables is proposed.

A one-dimensional sectional aerosol model integrated with mesoscale meteorological data to study marine boundary layer aerosol dynamics

NASA Astrophysics Data System (ADS)

Caffrey, Peter F.; Hoppel, William A.; Shi, Jainn J.

2006-12-01

The dynamics of aerosols in the marine boundary layer are simulated with a one-dimensional, multicomponent, sectional aerosol model using vertical profiles of turbulence, relative humidity, temperature, vertical velocity, cloud cover, and precipitation provided by 3-D mesoscale meteorological model output. The Naval Research Laboratory's (NRL) sectional aerosol model MARBLES (Fitzgerald et al., 1998a) was adapted to use hourly meteorological input taken from NRL's Coupled Ocean-Atmosphere Prediction System (COAMPS). COAMPS-generated turbulent mixing coefficients and large-scale vertical velocities determine vertical exchange within the marine boundary layer and exchange with the free troposphere. Air mass back trajectories were used to define the air column history along which the meteorology was retrieved for use with the aerosol model. Details on the integration of these models are described here, as well as a description of improvements made to the aerosol model, including transport by large-scale vertical motions (such as subsidence and lifting), a revised sea-salt aerosol source function, and separate tracking of sulfate mass from each of the five sources (free tropospheric, nucleated, condensed from gas phase oxidation products, cloud-processed, and produced from heterogeneous oxidation of S(IV) on sea-salt aerosol). Results from modeling air masses arriving at Oahu, Hawaii, are presented, and the relative contribution of free-tropospheric sulfate particles versus sea-salt aerosol from the surface to CCN concentrations is discussed. Limitations and benefits of the method are presented, as are sensitivity analyses of the effect of large-scale vertical motions versus turbulent mixing.

Light-absorbing Aerosol Properties in the Kathmandu Valley during SusKat-ABC Field Campaign

NASA Astrophysics Data System (ADS)

Kim, S.; Yoon, S.; Kim, J.; Cho, C.; Jung, J.

2013-12-01

Light-absorbing aerosols, such as black carbon (BC), are major contributors to the atmospheric heating and the reduction of solar radiation reaching at the earth's surface. In this study, we investigate light-absorption and scattering properties of aerosols (i.e., BC mass concentration, aerosol solar-absorption/scattering efficiency) in the Kathmandu valley during Sustainable atmosphere for the Kathmandu valley (SusKat)-ABC campaign, from December 2012 to February 2013. Kathmandu City is among the most polluted cities in the world. However, there are only few past studies that provide basic understanding of air pollution in the Kathmandu Valley, which is not sufficient for designing effective mitigation measures (e.g., technological, financial, regulatory, legal and political measures, planning strategies). A distinct diurnal variation of BC mass concentration with two high peaks observed during wintertime dry monsoon period. BC mass concentration was found to be maximum around 09:00 and 20:00 local standard time (LST). Increased cars and cooking activities including substantial burning of wood and other biomass in the morning and in the evening contributed to high BC concentration. Low BC concentrations during the daytime can be explain by reduced vehicular movement and cooking activities. Also, the developmements of the boundary layer height and mountain-valley winds in the Kathmandu Valley paly a crucial role in the temproal variation of BC mass concentrations. Detailed radiative effects of light-absorbing aerosols will be presented.

Physico-chemical properties of aerosols in Sao Paulo, Brazil and mechanisms of secondary organic aerosol formation.

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Ferreira de Brito, Joel; Varanda Rizzo, Luciana; Luiza Godoy, Maria; Godoy, Jose Marcus

2013-04-01

Megacities emissions are increasingly becoming a global issue, where emissions from the transportation sector play an increasingly important role. Sao Paulo is a megacity with a population of about 18 million people, 7 million cars and large-scale industrial emissions. As a result of the vehicular and industrial emissions, the air quality in Sao Paulo is bellow WMO standards for aerosol particles and ozone. Many uncertainties are found on gas- and particulate matter vehicular emission factors and their following atmospheric processes, e.g. secondary organic aerosol formation. Due to the uniqueness of the vehicular fuel in Brazil, largely based on ethanol use, such characterization currently holds further uncertainties. To improve the understanding of the role of this unique emission characteristics, we are running a source apportionment study in Sao Paulo focused on the mechanisms of organic aerosol formation. One of the goals of this study is a quantitative aerosol source apportionment focused on vehicular emissions, including ethanol and gasohol (both fuels used by light-duty vehicles). This study comprises four sampling sites with continuous measurements for one year, where trace elements and organic aerosol are being measured for PM2.5 and PM10 along with real-time NOx, O3, PM10 and CO measurements. Aerosol optical properties and size distribution are being measured on a rotation basis between sampling stations. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to measure in real time VOCs and aerosol composition, respectively. Trace elements were measured using XRF and OC/EC analysis was determined with a Sunset OC/EC instrument. A TSI Nephelometer with 3 wavelengths measure light scattering and a MAAP measure black carbon. Results show aerosol number concentrations ranging between 10,000 and 35,000 cm-3, mostly concentrated in the nucleation and Aitken modes, with a peak in size at 80

Real time measurements of submicrometer aerosols in Seoul, Korea: Sources, characteristics, and processing of organic aerosols during winter time.

NASA Astrophysics Data System (ADS)

Kim, H.; Zhang, Q.

2016-12-01

Highly time-resolved chemical characterization of non-refractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter when persistent air quality problems associated with elevated PM concentrations were observed. The average NR-PM1 concentration was 27.5 µg m-3 and the average mass was dominated by organics (44%), followed by nitrate (24%) and sulfate (10%). Five distinct sources of organic aerosol (OA) were identified from positive matrix factorization (PMF) analysis of the AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA), cooking represented by a cooking OA factor (COA), wood combustion represented by a biomass burning OA factor (BBOA), and secondary aerosol formation in the atmosphere that is represented by a semi-volatile oxygenated OA factor (SVOOA) and a low volatile oxygenated OA factor (LVOOA). These factors, on average, contributed 16, 20, 23, 15 and 26% to the total OA mass, respectively, with primary organic aerosol (POA = HOA + COA + BBOA) accounting for 59% of the OA mass. On average, both primary emissions and secondary aerosol formation are important factors affecting air quality in Seoul during winter, contributing approximately equal. However, differences in the fraction of PM source and properties were observed between high and low loading PM period. For example, during stagnant period with low wind speed (WS) (0.99 ± 0.7 m/s) and high RH (71%), high PM loadings (43.6 ± 12.4 µg m-3) with enhanced fractions of nitrate (27%) and SVOOA (8%) were observed, indicating a strong influence from locally generated secondary aerosol. On the other hand, when low PM loadings (12.6 ± 7.1 µg m-3), which were commonly associated with high WS (1.8 ± 1.1 m/s) and low RH (50 %), were observed, the fraction of regional sources, such as sulfate (12%) and LVOOA (21

Desorption atmospheric pressure photoionization high-resolution mass spectrometry: a complementary approach for the chemical analysis of atmospheric aerosols.

PubMed

Parshintsev, Jevgeni; Vaikkinen, Anu; Lipponen, Katriina; Vrkoslav, Vladimir; Cvačka, Josef; Kostiainen, Risto; Kotiaho, Tapio; Hartonen, Kari; Riekkola, Marja-Liisa; Kauppila, Tiina J

2015-07-15

On-line chemical characterization methods of atmospheric aerosols are essential to increase our understanding of physicochemical processes in the atmosphere, and to study biosphere-atmosphere interactions. Several techniques, including aerosol mass spectrometry, are nowadays available, but they all suffer from some disadvantages. In this research, desorption atmospheric pressure photoionization high-resolution (Orbitrap) mass spectrometry (DAPPI-HRMS) is introduced as a complementary technique for the fast analysis of aerosol chemical composition without the need for sample preparation. Atmospheric aerosols from city air were collected on a filter, desorbed in a DAPPI source with a hot stream of toluene and nitrogen, and ionized using a vacuum ultraviolet lamp at atmospheric pressure. To study the applicability of the technique for ambient aerosol analysis, several samples were collected onto filters and analyzed, with the focus being on selected organic acids. To compare the DAPPI-HRMS data with results obtained by an established method, each filter sample was divided into two equal parts, and the second half of the filter was extracted and analyzed by liquid chromatography/mass spectrometry (LC/MS). The DAPPI results agreed with the measured aerosol particle number. In addition to the targeted acids, the LC/MS and DAPPI-HRMS methods were found to detect different compounds, thus providing complementary information about the aerosol samples. DAPPI-HRMS showed several important oxidation products of terpenes, and numerous compounds were tentatively identified. Thanks to the soft ionization, high mass resolution, fast analysis, simplicity and on-line applicability, the proposed methodology has high potential in the field of atmospheric research. Copyright © 2015 John Wiley & Sons, Ltd.

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.

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

Vertical profiles of fine and coarse aerosol particles over Cyprus: Comparison between in-situ drone measurements and remote sensing observations

NASA Astrophysics Data System (ADS)

Mamali, Dimitra; Marinou, Eleni; Pikridas, Michael; Kottas, Michael; Binietoglou, Ioannis; Kokkalis, Panagiotis; Tsekeri, Aleksandra; Amiridis, Vasilis; Sciare, Jean; Keleshis, Christos; Engelmann, Ronny; Ansmann, Albert; Russchenberg, Herman W. J.; Biskos, George

2017-04-01

Vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) measurements were compared to airborne dried optical particle counter (OPC MetOne; Model 212) measurements during the INUIT-BACCHUS-ACTRIS campaign. The campaign took place in April 2016 and its main focus was the study of aerosol dust particles. During the campaign the NOA Polly-XT Raman lidar located at Nicosia (35.08° N, 33.22° E) was providing round-the-clock vertical profiles of aerosol optical properties. In addition, an unmanned aerial vehicle (UAV) carrying an OPC flew on 7 days during the first morning hours. The flights were performed at Orounda (35.1018° N, 33.0944° E) reaching altitudes of 2.5 km a.s.l, which allows comparison with a good fraction of the recorded lidar data. The polarization lidar photometer networking method (POLIPHON) was used for the estimation of the fine (non-dust) and coarse (dust) mode aerosol mass concentration profiles. This method uses as input the particle backscatter coefficient and the particle depolarization profiles of the lidar at 532 nm wavelength and derives the aerosol mass concentration. The first step in this approach makes use of the lidar observations to separate the backscatter and extinction contributions of the weakly depolarizing non-dust aerosol components from the contributions of the strongly depolarizing dust particles, under the assumption of an externally mixed two-component aerosol. In the second step, sun photometer retrievals of the fine and the coarse modes aerosol optical thickness (AOT) and volume concentration are used to calculate the associated concentrations from the extinction coefficients retrieved from the lidar. The estimated aerosol volume concentrations were converted into mass concentration with an assumption for the bulk aerosol density, and compared with the OPC measurements. The first results show agreement within the experimental uncertainty. This project received funding from the

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

Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in Downtown Atlanta, Georgia

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

2013-12-01

The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was recently developed to provide long-term real-time continuous measurements of ambient non-refractory (i.e., organic, sulfate, ammonium, nitrate, and chloride) submicron particulate matter (NR-PM1). Currently, there are a limited number of field studies that evaluate the long-term performance of the ACSM against established monitoring networks. In this study, we present seasonal intercomparisons of the ACSM with collocated fine aerosol (PM2.5) measurements at the Southeastern Aerosol Research and Characterization (SEARCH) Jefferson Street (JST) site near downtown Atlanta, GA, during 2011-2012. The collocated measurements included a second ACSM, continuous and integrated sulfate, nitrate, and ammonium measurements, as well as a semi-continuous Sunset organic carbon/elemental carbon (OC/EC) analyzer, continuous tapered element oscillating microbalance (TEOM), 24 h integrated Federal Reference Method (FRM) filters, and continuous scanning electrical mobility system-mixing condensation particle counter (SEMS-MCPC). Intercomparison of the two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21); mass concentration for all chemical species agreed within ±27%, indicating that ACSM instruments are capable of stable and reproducible operation. Chemical constituents measured by the ACSM are also compared with those obtained from the continuous measurements from JST. Since the continuous measurement concentrations are adjusted to match the integrated filter measurements, these comparisons reflect the combined uncertainties of the ACSM, continuous, and filter measurements. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Differences between ACSM mass concentrations and the filter-adjusted JST continuous data are 5-27%, 4

A COMPARISON OF CMAQ-BASED AEROSOL PROPERTIES WITH IMPROVE, MODIS, AND AERONET DATA

EPA Science Inventory

We compare select aerosol Properties derived from the Community Multiscale Air Quality (CMAQ) model-simulated aerosol mass concentrations with routine data from the National Aeronautics and Space Administration (NASA) satellite-borne Moderate Resolution Imaging Spectro-radiometer...

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.

Vertical distribution of aerosols in the vicinity of Mexico City during MILAGRO-2006 Campaign

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

Lewandowski, P.A.; Kleinman, L.; Eichinger, W. E.

On 7 March 2006, a mobile, ground-based, vertical pointing, elastic lidar system made a North-South transect through the Mexico City basin. Column averaged, aerosol size distribution (ASD) measurements were made on the ground concurrently with the lidar measurements. The ASD ground measurements allowed calculation of the column averaged mass extinction efficiency (MEE) for the lidar system (1064 nm). The value of column averaged MEE was combined with spatially resolved lidar extinction coefficients to produce total aerosol mass concentration estimates with the resolution of the lidar (1.5 m vertical spatial and 1 s temporal). Airborne ASD measurements from DOE G-1 aircraftmore » made later in the day on 7 March 2006, allowed the evaluation of the assumptions of constant ASD with height and time used for estimating the column averaged MEE. The results showed that the aerosol loading within the basin is about twice what is observed outside of the basin. The total aerosol base concentrations observed in the basin are of the order of 200 {mu}g/m{sup 3} and the base levels outside are of the order of 100 {mu}g/m{sup 3}. The local heavy traffic events can introduce aerosol levels near the ground as high as 900 {mu}g/m{sup 3}. The article presents the methodology for estimating aerosol mass concentration from mobile, ground-based lidar measurements in combination with aerosol size distribution measurements. An uncertainty analysis of the methodology is also presented.« less

Estimating particle speciation concentrations using MISR retrieved aerosol properties in southern California

NASA Astrophysics Data System (ADS)

Meng, X.; Liu, Y.; Diner, D. J.; Garay, M. J.

2016-12-01

Ambient fine particle (PM2.5) has been positively associated with increased mortality and morbidity worldwide. Recent studies highlight the characteristics and differential toxicity of PM2.5 chemical components, which are important for identifying sources, developing targeted particulate matter (PM) control strategies, and protecting public health. Modelling with satellite retrieved data has been proved as the most cost-effective way to estimate ground PM2.5 levels; however, limited studies have predict PM2.5 chemical components with this method. In this study, the experimental MISR 4.4 km aerosol retrievals were used to predict ground-level particle sulfate, nitrite, organic carbon and element carbon concentrations in 16 counties of southern California. The PM2.5 chemical components concentrations were obtained from the National Chemical Speciation Network (CSN) and the Interagency Monitoring of Protected Visual Environments (IMPROVE) network. A generalized additive model (GAM) was developed based on 16-years data (2000-2015) by combining the MISR aerosol retrievals, meteorological variables and geographical indicators together. Model performance was assessed by model fitted R2 and root-mean-square error (RMSE) and 10-fold cross validation. Spatial patterns of sulfate, nitrate, OC and EC concentrations were also examined with 2-D prediction surfaces. This is the first attempt to develop high-resolution spatial models to predict PM2.5 chemical component concentrations with MISR retrieved aerosol properties, which will provide valuable population exposure estimates for future studies on the characteristics and differential toxicity of PM2.5 speciation.

Direct Observations of Isoprene Secondary Organic Aerosol Formation in Ambient Cloud Droplets

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Bell, D.; Thornton, J. A.; Fast, J. D.; Shrivastava, M. B.; Berg, L. K.; Imre, D. G.; Mei, F.; Shilling, J.; Suski, K. J.; Liu, J.; Tomlinson, J. M.; Wang, J.

2017-12-01

Multiphase chemistry of isoprene photooxidation products has been shown to be one of the major sources of secondary organic aerosol (SOA) in the atmosphere. A number of recent studies indicate that aqueous aerosol phase provides a medium for reactive uptake of isoprene photooxidation products, and in particular, isomeric isoprene epoxydiols (IEPOX), with reaction rates and yields being dependent on aerosol acidity, water content, sulfate concentration, and organic coatings. However, very few studies focused on chemistry occurring within actual cloud droplets. We will present data acquired during recent Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) Campaign, which provide direct evidence for IEPOX-SOA formation in cloud droplets. Single particle mass spectrometer, miniSPLAT, and a high-resolution, time-of-flight aerosol mass spectrometer were used to characterize the composition of aerosol particles and cloud droplet residuals, while a high-resolution, time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) was used to characterize gas-phase compounds. We find that the composition of cloud droplet residuals was markedly different than that of aerosol particles sampled outside the cloud. Cloud droplet residuals were comprised of individual particles with high relative fractions of sulfate and nitrate and significant fraction of particles with mass spectra that are nearly identical to those of laboratory-generated IEPOX-SOA particles. The observed cloud-induced formation of IEPOX-SOA was accompanied by simultaneous decrease in measured concentrations of IEPOX and other gas-phase isoprene photooxidation products. Ultimately, the combined cloud, aerosol, and gas-phase measurements conducted during HI-SCALE will be used to develop and evaluate model treatments of aqueous-phase isoprene SOA formation.

Determination of particulate lead during MILAGRO/MCMA-2006 using Aerosol Mass Spectrometry

NASA Astrophysics Data System (ADS)

Salcedo, D.; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

2010-02-01

We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO)/Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ<0.1 s) and ~75% exhibiting slow evaporation (τ~2.4 min) at the T0 urban supersite and a different fraction (70% prompt and 30% slow evaporation) at a site northwest from the metropolitan area (PEMEX site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at T0 (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the compounds generating Pb