Technical note: Relating functional group measurements to carbon types for improved model-measurement comparisons of organic aerosol composition

NASA Astrophysics Data System (ADS)

Takahama, Satoshi; Ruggeri, Giulia

2017-04-01

Functional group (FG) analysis provides a means by which functionalization in organic aerosol can be attributed to the abundances of its underlying molecular structures. However, performing this attribution requires additional, unobserved details about the molecular mixture to provide constraints in the estimation process. We present an approach for conceptualizing FG measurements of organic aerosol in terms of its functionalized carbon atoms. This reformulation facilitates estimation of mass recovery and biases in popular carbon-centric metrics that describe the extent of functionalization (such as oxygen to carbon ratio, organic mass to organic carbon mass ratio, and mean carbon oxidation state) for any given set of molecules and FGs analyzed. Furthermore, this approach allows development of parameterizations to more precisely estimate the organic carbon content from measured FG abundance. We use simulated photooxidation products of α-pinene secondary organic aerosol previously reported by Ruggeri et al. (2016) and FG measurements by Fourier transform infrared (FT-IR) spectroscopy in chamber experiments by Sax et al. (2005) to infer the relationships among molecular composition, FG composition, and metrics of organic aerosol functionalization. We find that for this simulated system, ˜ 80 % of the carbon atoms should be detected by FGs for which calibration models are commonly developed, and ˜ 7 % of the carbon atoms are undetectable by FT-IR analysis because they are not associated with vibrational modes in the infrared. Estimated biases due to undetected carbon fraction for these simulations are used to make adjustments in these carbon-centric metrics such that model-measurement differences are framed in terms of unmeasured heteroatoms (e.g., in hydroperoxide and nitrate groups for the case studied in this demonstration). The formality of this method provides framework for extending FG analysis to not only model-measurement but also instrument

Lidar determination of the composition of atmosphere aerosols

NASA Technical Reports Server (NTRS)

Wright, M. L.

1980-01-01

Theoretical and experimental studies of the feasibility of using DIfferential SCatter (DISC) lidar to measure the composition of atmospheric aerosols are described. This technique involves multiwavelength measurements of the backscatter cross section of aerosols in the middle infrared, where a number of materials display strong restrahlen features that significantly modulate the backscatter spectrum. The theoretical work indicates that a number of materials of interest, including sulfuric acid, ammonium sulfate, and silicates, can be discriminated among with a CO2 lidar. An initial evaluation of this procedure was performed in which cirrus clouds and lower altitude tropospheric aerosols were developed. The observed ratio spectrum of the two types of aerosol displays structure that is in crude accord with theoretical expectations.

The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore-Washington, D.C. region

NASA Astrophysics Data System (ADS)

Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

2016-01-01

In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type - such as composition, size, and hygroscopicity - and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD-Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km, decreasing to 35 ng m-3 in the free troposphere (above

Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

NASA Astrophysics Data System (ADS)

Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

2013-12-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

Influence of aerosol chemical composition on N2O5 uptake: airborne regional measurements in northwestern Europe

NASA Astrophysics Data System (ADS)

Morgan, W. T.; Ouyang, B.; Allan, J. D.; Aruffo, E.; Di Carlo, P.; Kennedy, O. J.; Lowe, D.; Flynn, M. J.; Rosenberg, P. D.; Williams, P. I.; Jones, R.; McFiggans, G. B.; Coe, H.

2015-01-01

Aerosol chemical composition was found to influence nighttime atmospheric chemistry during a series of airborne measurements in northwestern Europe in summer conditions, which has implications for regional air quality and climate. The uptake of dinitrogen pentoxide, γ (N2O5), to particle surfaces was found to be modulated by the amount of water content and ammonium nitrate present in the aerosol. The conditions prevalent in this study suggest that the net uptake rate of N2O5 to atmospheric aerosols was relatively efficient compared to previous studies, with γ (N2O5) values in the range 0.01-0.03. This is likely a consequence of the elevated relative humidity in the region, which promotes greater aerosol water content. Increased nitrate concentrations relative to particulate water were found to suppress N2O5 uptake. The results presented here contrast with previous ambient studies of N2O5 uptake, which have generally taken place in low-nitrate environments in the USA. Comparison of the N2O5 uptake derived from the measurements with a parameterised scheme that is based on the ratio of particulate water to nitrate yielded reasonably good agreement in terms of the magnitude and variation in uptake, provided the effect of chloride was neglected. An additional suppression of the parameterised uptake is likely required to fully capture the variation in N2O5 uptake, which could be achieved via the known suppression by organic aerosol. However, existing parameterisations representing the suppression by organic aerosol were unable to fully represent the variation in N2O5 uptake. These results provide important ambient measurement constraint on our ability to predict N2O5 uptake in regional and global aerosol models. N2O5 uptake is a potentially important source of nitrate aerosol and a sink of the nitrate radical, which is the main nocturnal oxidant in the atmosphere. The results further highlight the importance of ammonium nitrate in northwestern Europe as a key component

Experimental investigation of aerosol composition and growth rates

NASA Astrophysics Data System (ADS)

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

2017-04-01

(CPCs) grow the particles internally, after which they are detected optically. By changing the condensing liquid, depending on the aerosol particle composition, they are activated differently. By combining the electrical size selection with CPCs with different liquids, information about particle composition can be determined. The project includes laboratory studies and field measurements in different locations (one rural site and two urban sites). I wish to acknowledge the Austrian Science Fund (FWF; Grant No J3951 - N36).

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.

Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

NASA Astrophysics Data System (ADS)

Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

2015-02-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, coating by heterogeneous uptake of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the resulting aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent in a soil whose aggregates are dispersed by wet sieving during analysis. We reconstruct the undispersed size distribution of the original soil that is subject to wind erosion. An empirical constraint upon the relative emission of clay and silt is applied that further differentiates the soil and aerosol mineral composition. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the extension brings the model into better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

Influence of aerosol chemical composition on N2O5 uptake: airborne regional measurements in North-Western Europe

NASA Astrophysics Data System (ADS)

Morgan, W. T.; Ouyang, B.; Allan, J. D.; Aruffo, E.; Di Carlo, P.; Kennedy, O. J.; Lowe, D.; Flynn, M. J.; Rosenberg, P. D.; Williams, P. I.; Jones, R.; McFiggans, G. B.; Coe, H.

2014-07-01

Aerosol chemical composition was found to influence nighttime atmospheric chemistry during a series of airborne measurements in North-Western Europe in summer conditions, which has implications for regional air quality and climate. The uptake of dinitrogen pentoxide, γ (N2O5), to particle surfaces was found to be modulated by the amount of water content and ammonium nitrate present in the aerosol. The conditions prevalent in this study suggest that the net uptake rate of N2O5 to atmospheric aerosols was relatively efficient compared to previous studies, with γ (N2O5) values in the range 0.01-0.03. This is likely a consequence of the elevated relative humidity in the region, which promotes greater aerosol water content. Increased nitrate concentrations relative to particulate water were found to suppress N2O5 uptake. The results presented here contrast with previous ambient studies of N2O5 uptake, which have generally taken place in low-nitrate environments in the USA. Comparison of the N2O5 uptake derived from the measurements with a parameterised scheme that is based on the ratio of particulate water to nitrate yielded reasonably good agreement in terms of the magnitude and variation in uptake, provided the effect of chloride was neglected. An additional suppression of the parameterised uptake is likely required to fully capture the variation in N2O5 uptake, which could be achieved via the known suppression by organic aerosol. However, existing parameterisations representing the suppression by organic aerosol were unable to fully represent the variation in N2O5 uptake. These results provide important ambient measurement constraint on our ability to predict N2O5 uptake in regional and global aerosol models. N2O5 uptake is a potentially important source of nitrate aerosol and a sink of the nitrate radical, which is the main nocturnal oxidant in the atmosphere. The results further highlight the importance of ammonium nitrate in North-Western Europe as a key

Persistence of organic carbon in heated aerosol residuals measured during Tropical Composition Cloud and Climate Coupling (TC4)

NASA Astrophysics Data System (ADS)

Thornberry, T.; Froyd, K. D.; Murphy, D. M.; Thomson, D. S.; Anderson, B. E.; Thornhill, K. L.; Winstead, E. L.

2010-05-01

The Particle Analysis by Laser Mass Spectrometry (PALMS) single particle mass spectrometer was used to analyze the composition of the nonvolatile fraction of atmospheric aerosol in a number of different environments. The mass spectra of individual particles sampled through an inlet section heated to 300°C were compared to unheated particles during flights of the NASA DC-8 aircraft during the Tropical Composition Cloud and Climate Coupling (TC4) mission. Comparisons are presented of measurements made in the marine boundary layer, the free troposphere, and the continental boundary layer over the Colombian jungle. The heated section completely removed sulfate from the aerosols except for sodium sulfate and related compounds in sea salt particles. Organic material in sea salt particles was observed to be less volatile than chlorine. Biomass burning particles were more likely to survive heating than other mixed sulfate-organic particles. For all particle types, there was a significant contribution to the residues from carbonaceous material other than elemental carbon. These results demonstrate the remaining compositional complexity of aerosol residuals that survive heating in a thermal denuder.

Airborne Atmospheric Aerosol Measurement System

NASA Astrophysics Data System (ADS)

Ahn, K.; Park, Y.; Eun, H.; Lee, H.

2015-12-01

It is important to understand the atmospheric aerosols compositions and size distributions since they greatly affect the environment and human health. Particles in the convection layer have been a great concern in global climate changes. To understand these characteristics satellite, aircraft, and radio sonde measurement methods have usually been used. An aircraft aerosol sampling using a filter and/or impactor was the method commonly used (Jay, 2003). However, the flight speed particle sampling had some technical limitations (Hermann, 2001). Moreover, the flight legal limit, altitude, prohibited airspace, flight time, and cost was another demerit. To overcome some of these restrictions, Tethered Balloon Package System (T.B.P.S.) and Recoverable Sonde System(R.S.S.) were developed with a very light optical particle counter (OPC), impactor, and condensation particle counter (CPC). Not only does it collect and measure atmospheric aerosols depending on altitudes, but it also monitors the atmospheric conditions, temperature, humidity, wind velocity, pressure, GPS data, during the measurement (Eun, 2013). In this research, atmospheric aerosol measurement using T.B.P.S. in Ansan area is performed and the measurement results will be presented. The system can also be mounted to an unmanned aerial vehicle (UAV) and create an aerial particle concentration map. Finally, we will present measurement data using Tethered Balloon Package System (T.B.P.S.) and R.S.S (Recoverable Sonde System).

Synchronised Aerosol Mass Spectrometer Measurements across Europe

NASA Astrophysics Data System (ADS)

Nemitz, Eiko

2010-05-01

Up to twelve Aerodyne Aerosol Mass Spectrometers (AMSs) were operated simultaneously at rural and background stations (EMEP and EUSAAR sites) across Europe. Measurements took place during three intensive periods, in collaboration between the European EUCAARI IP and the EMEP monitoring activities under the UNECE Convention for Long-Range Transboundary Air Pollution (CLRTAP) during three contrasting months (May 2008, Sep/Oct 2008, Feb/Mar 2009). These measurements were conducted, analysed and quality controlled carefully using a unified protocol, providing the largest spatial database of aerosol chemical composition measured with a unified online technique to date, and a unique snapshots of the European non-refractory submicron aerosol climatology. As campaign averages over all active monitoring sites, organics represent 28 to 43%, sulphate 18 to 25%, ammonium 13 to 15% and nitrate 15 to 36% of the resolved aerosol mass, with the highest relative nitrate contribution during the Feb/Mar campaign. The measurements demonstrate that in NW Europe (e.g. Ireland, UK, The Netherlands, Germany, Switzerland) the regional submicron aerosol tends to be neutralised and here nitrates make a major contribution to the aerosol mass. By contrast, periods with low nitrate and acidic aerosol were observed at sites in S and E Europe (e.g. Greece, Finland), presumably due to a combination of larger SO2 point sources in Easter Europe, smaller local NH3 sources and, in the case of Greece, higher temperatures. While at the more marine and remote sites (Ireland, Scotland, Finland) nitrate concentrations were dominated by episodic transport phenomena, at continental sites (Switzerland, Germany, Hungary) nitrate followed a clear diurnal cycle, reflecting the thermodynamic behaviour of ammonium nitrate. The datasets clearly shows spatially co-ordinated, large-scale pollution episodes of organics, sulphate and nitrate, the latter being most pronounced during the Feb/Mar campaign. At selected

Aerosol measurements during COPE: composition, size, and sources of CCN and INPs at the interface between marine and terrestrial influences

NASA Astrophysics Data System (ADS)

Taylor, Jonathan W.; Choularton, Thomas W.; Blyth, Alan M.; Flynn, Michael J.; Williams, Paul I.; Young, Gillian; Bower, Keith N.; Crosier, Jonathan; Gallagher, Martin W.; Dorsey, James R.; Liu, Zixia; Rosenberg, Philip D.

2016-09-01

Heavy rainfall from convective clouds can lead to devastating flash flooding, and observations of aerosols and clouds are required to improve cloud parameterisations used in precipitation forecasts. We present measurements of boundary layer aerosol concentration, size, and composition from a series of research flights performed over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) of summer 2013. We place emphasis on periods of southwesterly winds, which locally are most conducive to convective cloud formation, when marine air from the Atlantic reached the peninsula. Accumulation-mode aerosol mass loadings were typically 2-3 µg m-3 (corrected to standard cubic metres at 1013.25 hPa and 273.15 K), the majority of which was sulfuric acid over the sea, or ammonium sulfate inland, as terrestrial ammonia sources neutralised the aerosol. The cloud condensation nuclei (CCN) concentrations in these conditions were ˜ 150-280 cm-3 at 0.1 % and 400-500 cm-3 at 0.9 % supersaturation (SST), which are in good agreement with previous Atlantic measurements, and the cloud drop concentrations at cloud base ranged from 100 to 500 cm-3. The concentration of CCN at 0.1 % SST was well correlated with non-sea-salt sulfate, meaning marine sulfate formation was likely the main source of CCN. Marine organic aerosol (OA) had a similar mass spectrum to previous measurements of sea spray OA and was poorly correlated with CCN. In one case study that was significantly different to the rest, polluted anthropogenic emissions from the southern and central UK advected to the peninsula, with significant enhancements of OA, ammonium nitrate and sulfate, and black carbon. The CCN concentrations here were around 6 times higher than in the clean cases, and the cloud drop number concentrations were 3-4 times higher. Sources of ice-nucleating particles (INPs) were assessed by comparing different parameterisations used to predict INP concentrations, using measured

Application of Aerosol Hygroscopicity Measured at the Atmospheric Radiation Measurement Program's Southern Great Plains Site to Examine Composition and Evolution

NASA Technical Reports Server (NTRS)

Gasparini, Roberto; Runjun, Li; Collins, Don R.; Ferrare, Richard A.; Brackett, Vincent G.

2006-01-01

A Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) was used to measure submicron aerosol size distributions, hygroscopicity, and occasionally volatility during the May 2003 Aerosol Intensive Operational Period (IOP) at the Central Facility of the Atmospheric Radiation Measurement Program's Southern Great Plains (ARM SGP) site. Hygroscopic growth factor distributions for particles at eight dry diameters ranging from 0.012 micrometers to 0.600 micrometers were measured throughout the study. For a subset of particle sizes, more detailed measurements were occasionally made in which the relative humidity or temperature to which the aerosol was exposed was varied over a wide range. These measurements, in conjunction with backtrajectory clustering, were used to infer aerosol composition and to gain insight into the processes responsible for evolution. The hygroscopic growth of both the smallest and largest particles analyzed was typically less than that of particles with dry diameters of about 0.100 micrometers. It is speculated that condensation of secondary organic aerosol on nucleation mode particles is largely responsible for the minimal hygroscopic growth observed at the smallest sizes considered. Growth factor distributions of the largest particles characterized typically contained a nonhygroscopic mode believed to be composed primarily of dust. A model was developed to characterize the hygroscopic properties of particles within a size distribution mode through analysis of the fixed size hygroscopic growth measurements. The performance of this model was quantified through comparison of the measured fixed size hygroscopic growth factor distributions with those simulated through convolution of the size-resolved concentration contributed by each of the size modes and the mode-resolved hygroscopicity. This transformation from sizeresolved hygroscopicity to mode-resolved hygroscopicity facilitated examination of changes in the hygroscopic

Predicting the mineral composition of dust aerosols: Insights from elemental composition measured at the Izaña Observatory

NASA Astrophysics Data System (ADS)

Pérez García-Pando, Carlos; Miller, Ron L.; Perlwitz, Jan P.; Rodríguez, Sergio; Prospero, Joseph M.

2016-10-01

Regional variations of dust mineral composition are fundamental to climate impacts but generally neglected in climate models. A challenge for models is that atlases of soil composition are derived from measurements following wet sieving, which destroys the aggregates potentially emitted from the soil. Aggregates are crucial to simulating the observed size distribution of emitted soil particles. We use an extension of brittle fragmentation theory in a global dust model to account for these aggregates. Our method reproduces the size-resolved dust concentration along with the approximately size-invariant fractional abundance of elements like Fe and Al in the decade-long aerosol record from the Izaña Observatory, off the coast of West Africa. By distinguishing between Fe in structural and free forms, we can attribute improved model behavior to aggregation of Fe and Al-rich clay particles. We also demonstrate the importance of size-resolved measurements along with elemental composition analysis to constrain models.

Long term aerosol and trace gas measurements in Central Amazonia

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Barbosa, Henrique M. J.; Ferreira de Brito, Joel; Carbone, Samara; Rizzo, Luciana V.; Andreae, Meinrat O.; Martin, Scot T.

2016-04-01

The central region of the Amazonian forest is a pristine region in terms of aerosol and trace gases concentrations. In the wet season, Amazonia is actually one of the cleanest continental region we can observe on Earth. A long term observational program started 20 years ago, and show important features of this pristine region. Several sites were used, between then ATTO (Amazon Tall Tower Observatory) and ZF2 ecological research site, both 70-150 Km North of Manaus, receiving air masses that traveled over 1500 km of pristine tropical forests. The sites are GAW regional monitoring stations. Aerosol chemical composition (OC/EC and trace elements) is being analysed using filters for fine (PM2.5) and coarse mode aerosol as well as Aerodyne ACSM (Aerosol Chemical Speciation Monitors). VOCs are measured using PTR-MS, while CO, O3 and CO2 are routinely measured. Aerosol absorption is being studied with AE33 aethalometers and MAAP (Multi Angle Absorption Photometers). Aerosol light scattering are being measured at several wavelengths using TSI and Ecotech nephelometers. Aerosol size distribution is determined using scanning mobility particle sizer at each site. Lidars measure the aerosol column up to 12 Km providing the vertical profile of aerosol extinction. The aerosol column is measures using AERONET sun photometers. In the wet season, organic aerosol comprises 75-85% of fine aerosol, and sulfate and nitrate concentrations are very low (1-3 percent). Aerosols are dominated by biogenic primary particles as well as SOA from biogenic precursors. Black carbon in the wet season accounts for 5-9% of fine mode aerosol. Ozone in the wet season peaks at 10-12 ppb at the middle of the day, while carbon monoxide averages at 50-80 ppb. Aerosol optical thickness (AOT) is a low 0.05 to 0.1 at 550 nm in the wet season. Sahara dust transport events sporadically enhance the concentration of soil dust aerosols and black carbon. In the dry season (August-December), long range transported

Predicting the Mineral Composition of Dust Aerosols. Part 1; Representing Key Processes

NASA Technical Reports Server (NTRS)

Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

2015-01-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

NASA Astrophysics Data System (ADS)

Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

2015-10-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

The Influence of Chemical Composition and Relative Humidity on the Optical Properties of Aerosols During the Southern Oxidant and Aerosol Study (SOAS)

NASA Astrophysics Data System (ADS)

Attwood, A. R.; Washenfelder, R. A.; Brock, C. A.; Brown, S. S.; Hu, W.; Campuzano Jost, P.; Day, D. A.; Palm, B. B.; Simoes de Sa, S.; Jimenez, J. L.

2013-12-01

Atmospheric particles are produced from a wide variety of both anthropogenic and natural sources and play an important role in the Earth's radiative budget by direct scattering and absorption of radiation. To address this impact, in situ measurements of aerosol optical, chemical and hygroscopic properties were performed during the Southern Oxidant and Aerosol Study (SOAS), which took place in the summer of 2013. Ground based measurements of sub-micron aerosol in the southeastern United States were made to investigate the influence of chemical composition and hygroscopicity on aerosol optical properties. We report the wavelength dependence of aerosol extinction cross sections measured with a novel broadband cavity enhanced spectrometer covering a wavelength range of 360-420 nm using two light emitting diodes (LED) and a separate cavity ring down (CRDS) channel. The sensitivity of the relative humidity dependence of extinction based on the type of aerosol present is examined and we show that the optical properties and hygroscopicity of aerosols are greatly influenced by the fraction of sulfate and organics within the particles. Additional data analysis from the SOAS campaign will be presented. The results, thus far, illustrate that the variability in aerosol chemical composition can impact visibility and climate forcing in this region.

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Russell, P. B.; Bergstrom, Robert W.; Schmid, B.; Livingston, J. M.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net short-wave flux at the tropopause by combining satellite-derived aerosol optical depth (AOD) maps with model aerosol properties determined via closure analyses in TARFOX and ACE 2. We exclude African dust, primarily by restricting latitudes to 25-60 N. The analyses use in situ aerosol composition measurements and air- and ship-borne sun-photometer measurements of AOD spectra. The aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. Its midvisible single-scattering albedo is 0.9. which is in the range obtained from in situ measurements of scattering and absorption in both TARFOX and ACE 2. Combining satellite-derived AOD maps with the aerosol model yields maps of 24-hour average net radiative flux changes. For simultaneous AVHRR, radiance measurements exceeded the sunphotometer AODs by about 0.04. However. shipboard sunphotometer and AVHRR AODs agreed Within 0.02 for data acquired during satellite overflights on two other days. We discuss attempts to demonstrate column closure within the MBL by comparing shipboard sunphotometer AODs and values calculated from simultaneous shipboard in-situ aerosol size distribution measurements. These comparisons were mostly unsuccessful, but they illustrate the difficulties inherent in this type of closure analysis. Specifically, AODs derived from near-surface in-situ size distribution measurements are extremely sensitive to the assumed hygroscopic growth model that itself requires an assumption of particle composition as a function of height and size, to the radiosonde-measured relative humidity, and to the vertical profile of particle number. We investigate further the effects of hygroscopic particle growth within the MBL by using shipboard lidar aerosol backscatter profiles together with the sunphotometer AOD.

Spectrally-resolved measurements of aerosol extinction at ultraviolet and visible wavelengths

NASA Astrophysics Data System (ADS)

Flores, M.; Washenfelder, R. A.; Brock, C. A.; Brown, S. S.; Rudich, Y.

2012-12-01

Aerosols play an important role in the Earth's radiative budget. Aerosol extinction includes both the scattering and absorption of light, and these vary with wavelength, aerosol diameter, and aerosol composition. Historically, aerosol absorption has been measured using filter-based or extraction methods that are prone to artifacts. There have been few investigations of ambient aerosol optical properties at the blue end of the visible spectrum and into the ultraviolet. Brown carbon is particularly important in this spectral region, because it both absorbs and scatters light, and encompasses a large and variable group of organic compounds from biomass burning and secondary organic aerosol. We have developed a laboratory instrument that combines new, high-power LED light sources with high-finesse optical cavities to achieve sensitive measurements of aerosol optical extinction. This instrument contains two broadband channels, with spectral coverage from 360 - 390 nm and 385 - 420 nm. Using this instrument, we report aerosol extinction in the ultraviolet and near-visible spectral region as a function of chemical composition and structure. We have measured the extinction cross-sections between 360 - 420 nm with 0.5 nm resolution using different sizes and concentrations of polystyrene latex spheres, ammonium sulfate, and Suwannee River fulvic acid. Fitting the real and imaginary part of the refractive index allows the absorption and scattering to be determined.

Aerosol Classification from High Spectral Resolution Lidar Measurements

NASA Astrophysics Data System (ADS)

Burton, S. P.; Hair, J. W.; Ferrare, R. A.; Hostetler, C. A.; Kahnert, M.; Vaughan, M. A.; Cook, A. L.; Harper, D. B.; Berkoff, T.; Seaman, S. T.; Collins, J. E., Jr.; Fenn, M. A.; Rogers, R. R.

2015-12-01

The NASA Langley airborne High Spectral Resolution Lidars, HSRL-1 and HSRL-2, have acquired large datasets of vertically resolved aerosol extinction, backscatter, and depolarization during >30 airborne field missions since 2006. The lidar measurements of aerosol intensive parameters like lidar ratio and color ratio embed information about intrinsic aerosol properties, and are combined to qualitatively classify HSRL aerosol measurements into aerosol types. Knowledge of aerosol type is important for assessing aerosol radiative forcing, and can provide useful information for source attribution studies. However, atmospheric aerosol is frequently not a single pure type, but instead is a mixture, which affects the optical and radiative properties of the aerosol. We show that aerosol intensive parameters measured by lidar can be understood using mixing rules for cases of external mixing. Beyond coarse classification and mixing between classes, variations in the lidar aerosol intensive parameters provide additional insight into aerosol processes and composition. This is illustrated by depolarization measurements at three wavelengths, 355 nm, 532 nm, and 1064 nm, made by HSRL-2. Particle depolarization ratio is an indicator of non-spherical particles. Three cases each have a significantly different spectral dependence of the depolarization ratio, related to the size of the depolarizing particles. For two dust cases, large non-spherical particles account for the depolarization of the lidar light. The spectral dependence reflects the size distribution of these particles and reveals differences in the transport histories of the two plumes. For a smoke case, the depolarization is inferred to be due to the presence of small coated soot aggregates. Interestingly, the depolarization at 355 nm is similar for this smoke case compared to the dust cases, having potential implications for the upcoming EarthCARE satellite, which will measure particle depolarization ratio only at 355 nm.

Organic Functional Group Composition of Submicron Aerosol Particles at Alert, Nunavut, during 2012-2014

NASA Astrophysics Data System (ADS)

Russell, L. M.; Leaitch, W. R.; Liu, J.; Desiree, T. S.; Huang, L.; Sharma, S.; Chivulescu, A.; Veber, D.; Zhang, W.

2016-12-01

Long-term measurements of submicron aerosol particle chemical composition and size distributions are essential for evaluating whether global climate models correctly transport particles from lower latitudes to polar regions, especially in the winter months when satellite retrieval of aerosol properties is limited. In collaboration with ongoing measurements by the Dr. Neil Trivett Global Atmospheric Watch observatory at Alert, Nunavut (82.5°N; elevation 185 m-ASL), we measured the organic functional group composition of submicron aerosol particles sampled from the 10-m inlet from April 2012 to October 2014. The sampling site is approximately 10 km from the Alert station, and vehicle traffic is restricted except when filter sampling is stopped, making the impact of local emissions on submicron particle mass concentrations small. The organic functional group (OFG) composition is measured by Fourier Transform Infrared spectroscopy of samples collected on pre-loaded Teflon filters and stored and shipped frozen to La Jolla, California, for analysis. Samples were collected weekly to complement the twice hourly online measurements of non-refractory organic and inorganic composition by an Aerodyne ACSM. Organic components are shown to contribute a substantial fraction of the measured aerosol submicron mass year round. These measurements illustrate the seasonal contributions to the aerosol size distribution from OFG and illustrate the potential sources of the OFG at this remote site. The three largest OFG sources are transported fossil fuel combustion emissions from lower latitudes, sea spray and other marine particles, and episodic contributions from wildfires, volcanoes, and other high-latitude events. These sources are similar to those identified from earlier OFG measurements at Barrow, Alaska, and during the ICEALOT cruise in the Arctic Ocean.

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

Biomass burning aerosols characterization from ground based and profiling measurements

NASA Astrophysics Data System (ADS)

Marin, Cristina; Vasilescu, Jeni; Marmureanu, Luminita; Ene, Dragos; Preda, Liliana; Mihailescu, Mona

2018-04-01

The study goal is to assess the chemical and optical properties of aerosols present in the lofted layers and at the ground. The biomass burning aerosols were evaluated in low level layers from multi-wavelength lidar measurements, while chemical composition at ground was assessed using an Aerosol Chemical Speciation Monitor (ACSM) and an Aethalometer. Classification of aerosol type and specific organic markers were used to explore the potential to sense the particles from the same origin at ground base and on profiles.

Predicting the mineral composition of dust aerosols – Part 1: Representing key processes

DOE PAGES

Perlwitz, J. P.; Perez Garcia-Pando, C.; Miller, R. L.

2015-10-21

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accountsmore » for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. Finally, a

Sources of atmospheric aerosol from long-term measurements (5 years) of chemical composition in Athens, Greece.

PubMed

Paraskevopoulou, D; Liakakou, E; Gerasopoulos, E; Mihalopoulos, N

2015-09-15

To identify the sources of aerosols in Greater Athens Area (GAA), a total of 1510 daily samples of fine (PM 2.5) and coarse (PM 10-2,5) aerosols were collected at a suburban site (Penteli), during a five year period (May 2008-April 2013) corresponding to the period before and during the financial crisis. In addition, aerosol sampling was also conducted in parallel at an urban site (Thissio), during specific, short-term campaigns during all seasons. In all these samples mass and chemical composition measurements were performed, the latest only at the fine fraction. Particulate organic matter (POM) and ionic masses (IM) are the main contributors of aerosol mass, equally contributing by accounting for about 24% of the fine aerosol mass. In the IM, nss-SO4(-2) is the prevailing specie followed by NO3(-) and NH4(+) and shows a decreasing trend during the 2008-2013 period similar to that observed for PM masses. The contribution of water in fine aerosol is equally significant (21 ± 2%), while during dust transport, the contribution of dust increases from 7 ± 2% to 31 ± 9%. Source apportionment (PCA and PMF) and mass closure exercises identified the presence of six sources of fine aerosols: secondary photochemistry, primary combustion, soil, biomass burning, sea salt and traffic. Finally, from winter 2012 to winter 2013 the contribution of POM to the urban aerosol mass is increased by almost 30%, reflecting the impact of wood combustion (dominant fuel for domestic heating) to air quality in Athens, which massively started in winter 2013. Copyright © 2015 Elsevier B.V. All rights reserved.

Secondary Aerosol Formation over the ESCOMPTE Area: Results from airborne Aerosol and Trace Gas Measurements

NASA Astrophysics Data System (ADS)

van Dingenen, R.; Martins-Dos Santos, S.; Putaud, J. P.; Allet, C.; Bretton, E.; Perros, P.

2003-04-01

From June 10th to July 14th 2001, the ESCOMPTE campaign took place in the Marseille-Berre area in Southern France. The goal of the campaign was to produce a high quality 3-D data base from emissions, transport and air composition measurements during urban photochemical pollution episodes at the meso-scale. The CAATER AEROPLUM project was embedded within this international field campaign. AEROPLUM aimed at mapping size distributions of aerosols and photo-oxidants in the mixed layer over the ESCOMPTE domain, using the ARAT Fokker 27 as measurement platform. Aircraft sub-micrometer aerosol measurements are validated during overpasses against ground-based measurements, carried out with similar instrumentation. We will present and discuss data during periods of seabreeze, transporting coastal industrial and urban pollution land-inwards. This leads to intense photochemical activity, evidenced by elevated O_3 concentrations and aerosol levels.

Combined use of optical and electron microscopic techniques for the measurement of hygroscopic property, chemical composition, and morphology of individual aerosol particles.

PubMed

Ahn, Kang-Ho; Kim, Sun-Man; Jung, Hae-Jin; Lee, Mi-Jung; Eom, Hyo-Jin; Maskey, Shila; Ro, Chul-Un

2010-10-01

In this work, an analytical method for the characterization of the hygroscopic property, chemical composition, and morphology of individual aerosol particles is introduced. The method, which is based on the combined use of optical and electron microscopic techniques, is simple and easy to apply. An optical microscopic technique was used to perform the visual observation of the phase transformation and hygroscopic growth of aerosol particles on a single particle level. A quantitative energy-dispersive electron probe X-ray microanalysis, named low-Z particle EPMA, was used to perform a quantitative chemical speciation of the same individual particles after the measurement of the hygroscopic property. To validate the analytical methodology, the hygroscopic properties of artificially generated NaCl, KCl, (NH(4))(2)SO(4), and Na(2)SO(4) aerosol particles of micrometer size were investigated. The practical applicability of the analytical method for studying the hygroscopic property, chemical composition, and morphology of ambient aerosol particles is demonstrated.

Chemistry and Composition of Atmospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Kolb, Charles E.; Worsnop, Douglas R.

2012-05-01

For more than two decades a cadre of physical chemists has focused on understanding the formation processes, chemical composition, and chemical kinetics of atmospheric aerosol particles and droplets with diameters ranging from a few nanometers to ˜10,000 nm. They have adapted or invented a range of fundamental experimental and theoretical tools to investigate the thermochemistry, mass transport, and chemical kinetics of processes occurring at nanoscale gas-liquid and gas-solid interfaces for a wide range of nonideal, real-world substances. State-of-the-art laboratory methods devised to study molecular spectroscopy, chemical kinetics, and molecular dynamics also have been incorporated into field measurement instruments that are deployed routinely on research aircraft, ships, and mobile laboratories as well as at field sites from megacities to the most remote jungle, desert, and polar locations. These instruments can now provide real-time, size-resolved aerosol particle physical property and chemical composition data anywhere in Earth's troposphere and lower stratosphere.

Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

PubMed

Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

2015-10-06

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

Intercomparisons of airborne measurements of aerosol ionic chemical composition during TRACE-P and ACE-Asia

NASA Astrophysics Data System (ADS)

Ma, Y.; Weber, R. J.; Maxwell-Meier, K.; Orsini, D. A.; Lee, Y.-N.; Huebert, B. J.; Howell, S. G.; Bertram, T.; Talbot, R. W.; Dibb, J. E.; Scheuer, E.

2004-08-01

As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P) and the Asian Aerosol Characterization Experiment (ACE-Asia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the particle into liquid sampler (PILS) for measurement of a suite of fine particle a mist chamber/ion chromatograph (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and micro-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r2 of 0.95), but were systematically different by 10 ± 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low-turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an r2 of 0.78 and a relative difference of 39% ± 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 μm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% ± 6% and correlated with an r2 of 0.87. Most ionic compounds were within ±30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30-40%.

Intercomparisons of Airborne Measurements of Aerosol Ionic Chemical Composition during TRACE-P and ACE-Asia

NASA Technical Reports Server (NTRS)

Ma, Y.; Weber, R. J.; Maxwell-Meier, K.; Orsini, D. A.; Lee, Y.-N.; Huebert, B. J.; Howell, S. G.; Bertram, T.; Talbot, R. W.

2003-01-01

As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P), and the Asian Aerosol Characterization Experiment (ACEAsia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the Particle Into Liquid Sampler (PILS) for measurement of a suite of fine particle ionic compounds and a mist chamber (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and multi-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r(sup 2) of 0.95), but were systematically different by 10 +/- 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an 3 of 0.78 and a relative difference of 39% +/- 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 pm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% +/- 6% and correlated with an r(sup 2) of 0.87. Most ionic compounds were within f 30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30-40%.

Aerosol Optical Properties and Chemical Composition Measured on the Ronald H. Brown During ACE-Asia

NASA Astrophysics Data System (ADS)

Quinn, P. K.; Bates, T. S.; Miller, T. L.; Coffman, D.

2001-12-01

Measurements of aerosol chemical, physical, and optical properties were made onboard the NOAA R/V Ronald H. Brown during the ACE-Asia Intensive Field Program to characterize Asian aerosol as it was transported across the Pacific Ocean. The ship traveled across the Pacific from Hawaii to Japan and into the East China Sea and the Sea of Japan. Trajectories indicate that remote marine air masses were sampled on the transit to Japan. In the ACE-Asia study region air masses from Japan, China, Mongolia, and the Korea Peninsula were sampled. A variety of aerosol types were encountered including those of marine, volcanic, crustal, and industrial origin. Presented here, for the different air masses encountered, are aerosol optical properties (scattering and absorption coefficients, single scattering albedo, Angstrom Exponent, and aerosol optical depth) and chemical composition (major ions, total organic and black carbon, and trace elements). Scattering by submicron aerosol (55 % RH and 550 nm) was less than 20 1/Mm during the transit from Hawaii to Japan. In continental air masses, values ranged from 60 to 320 1/Mm with the highest submicron scattering coefficients occurring during prefrontal conditions with a low marine boundary layer height and trajectories from Japan. For the continental air masses, the ratio of scattering by submicron to sub-10 micron aerosol during polluted conditions averaged 0.8 and during a dust event 0.41. Aerosol optical depth (500 nm) ranged from 0.08 during the Pacific transit to 1.3 in the prefrontal conditions described above. Optical depths during dust events ranged from 0.2 to 0.6. Submicron non-sea salt (nss) sulfate concentrations ranged from 0.5 ug/m-3 during the Pacific transit to near 30 ug/m-3 during the prefrontal conditions described above. Black carbon to total carbon mass ratios in air masses from Asia averaged 0.18 with highest values (0.32) corresponding to trajectories crossing the Yangtze River valley.

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

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.

Organic component vapor pressures and hygroscopicities of aqueous aerosol measured by optical tweezers.

PubMed

Cai, Chen; Stewart, David J; Reid, Jonathan P; Zhang, Yun-hong; Ohm, Peter; Dutcher, Cari S; Clegg, Simon L

2015-01-29

Measurements of the hygroscopic response of aerosol and the particle-to-gas partitioning of semivolatile organic compounds are crucial for providing more accurate descriptions of the compositional and size distributions of atmospheric aerosol. Concurrent measurements of particle size and composition (inferred from refractive index) are reported here using optical tweezers to isolate and probe individual aerosol droplets over extended timeframes. The measurements are shown to allow accurate retrievals of component vapor pressures and hygroscopic response through examining correlated variations in size and composition for binary droplets containing water and a single organic component. Measurements are reported for a homologous series of dicarboxylic acids, maleic acid, citric acid, glycerol, or 1,2,6-hexanetriol. An assessment of the inherent uncertainties in such measurements when measuring only particle size is provided to confirm the value of such a correlational approach. We also show that the method of molar refraction provides an accurate characterization of the compositional dependence of the refractive index of the solutions. In this method, the density of the pure liquid solute is the largest uncertainty and must be either known or inferred from subsaturated measurements with an error of <±2.5% to discriminate between different thermodynamic treatments.

Size-Resolved Composition of Organic Aerosol on the California Central Coast

NASA Astrophysics Data System (ADS)

Babila, J. E.; Depew, C. J.; Heinrich, S. E.; Zoerb, M.

2016-12-01

Organic compounds represent a significant mass fraction of submicrometer aerosol and can influence properties such as radiative forcing and cloud formation. Despite their broad importance, a complete description of particle sources and composition is lacking. Here we present measurements of solvent-extracted organic compounds in ambient aerosol in San Luis Obispo, CA. Ambient particles were sampled and size segregated with a micro-orifice uniform deposit impactor (MOUDI). Water and methanol soluble organic carbon was characterized with electrospray ionization mass spectrometry (ESI-MS) and UV/Vis spectroscopy. Particle composition and influences from local and regional sources on the organic fraction will be discussed.

Volatile organic compound measurements at Trinidad Head, California, during ITCT 2K2: Analysis of sources, atmospheric composition, and aerosol residence times

NASA Astrophysics Data System (ADS)

Millet, Dylan B.; Goldstein, Allen H.; Allan, James D.; Bates, Timothy S.; Boudries, Hacene; Bower, Keith N.; Coe, Hugh; Ma, Yilin; McKay, Megan; Quinn, Patricia K.; Sullivan, Amy; Weber, Rodney J.; Worsnop, Douglas R.

2004-12-01

We report hourly in-situ observations of C1-C8 speciated volatile organic compounds (VOCs) obtained at Trinidad Head CA in April and May 2002 as part of the NOAA Intercontinental Transport and Chemical Transformation study. Factor analysis of the VOC data set was used to define the dominant processes driving atmospheric chemical composition at the site, and to characterize the sources for measured species. Strong decreases in background concentration were observed for several of the VOCs during the experiment due to seasonal changes in OH concentration. CO was the most important contributor to the total measured OH reactivity at the site at all times. Oxygenated VOCs were the primary component of both the total VOC burden and of the VOC OH reactivity, and their relative importance was enhanced under conditions when local source contributions were minimal. VOC variability exhibited a strong dependence on residence time (slnX = 1.55τ-0.44, r2 = 0.98; where slnX is the standard deviation of the natural logarithm of the mixing ratio), and this relationship was used, in conjunction with measurements of 222Rn, to estimate the average OH concentration during the study period (6.1 × 105 molec/cm3). We also employed the variability-lifetime relationship defined by the VOC data set to estimate submicron aerosol residence times as a function of chemical composition. Two independent measures of aerosol chemical composition yielded consistent residence time estimates. Lifetimes calculated in this manner were between 3-7 days for aerosol nitrate, organics, sulfate, and ammonium. The lifetime estimate for methane sulfonic acid (˜12 days) was slightly outside of this range. The lifetime of the total aerosol number density was estimated at 9.8 days.

Elemental composition of Arctic soils and aerosols in Ny-Ålesund measured using laser-induced breakdown spectroscopy

NASA Astrophysics Data System (ADS)

Kim, Gibaek; Yoon, Young-Jun; Kim, Hyun-A.; Cho, Hee-joo; Park, Kihong

2017-08-01

Two laser-induced breakdown spectroscopy (LIBS) systems (soil LIBS and aerosol LIBS) were used to determine the elemental composition of soils and ambient aerosols less than 2.5 μm in Ny-Ålesund, Svalbard (the world's most northerly human settlement). For soil LIBS measurements, matrix effects such as moisture content, soil grain size, and surrounding gas on the LIBS response were minimized. When Ar gas was supplied onto the soil sample surfaces, a significant enhancement in LIBS emission lines was observed. Arctic soil samples were collected at 10 locations, and various elements (Al, Ba, C, Ca, Cu, Fe, H, K, Mg, Mn, N, Na, O, Pb, and Si) were detected in soils. The elemental distribution in arctic soils was clearly distinguishable from those in urban and abandoned mining soils in Korea. Moreover, the concentrations of most of anthropogenic metals were fairly low, and localized sources in extremely close proximity affected the elevated level of Cu in the soil samples derived from Ny-Ålesund. The number of elements detected in aerosols (C, Ca, H, K, Mg, Na, and O) was lower than those determined in soils. The elements in aerosols can mainly originate from minerals and sea salts. The elemental distribution in aerosols was also clearly distinguishable from that in soils, suggesting that the resuspension of local soil particles by wind erosion into aerosols was minimal. The daily variation of particle number concentration (RSD = 71%) and the elements in aerosols (RSD = 25%) varied substantially, possibly due to fluctuating air masses and meteorological conditions.

Aerosol Size and Chemical Composition in the Canadian High Arctic

NASA Astrophysics Data System (ADS)

Chang, R. Y. W.; Hayes, P. L.; Leaitch, W. R.; Croft, B.; O'Neill, N. T.; Fogal, P.; Drummond, J. R.; Sloan, J. J.

2015-12-01

Arctic aerosol have a strong annual cycle, with winter months dominated by long range transport from lower latitudes resulting in high mass loadings. Conversely, local emissions are more prominent in the summer months because of the decreased influence of transported aerosol, allowing us to regularly observe both transported and local aerosol. This study will present observations of aerosol chemical composition and particle number size distribution collected at the Polar Environment Artic Research Laboratory and the Alert Global Atmospheric Watch Observatory at Eureka (80N, 86W) and Alert (82N, 62W), Nunavut, respectively. Summer time observations of the number size distribution reveal a persistent mode of particles centered between 30-50 nm, with occasional bursts of smaller particles. The non-refractory aerosol chemical composition, measured by the Canadian Network for the Detection of Atmospheric Change quadrupole aerosol mass spectrometer, is primarily organic, with contributions from both aged and fresher organic aerosol. Factor analysis will be conducted to better understand these sources. The site at Eureka is more susceptible to long range transport since it is at the top of a mountain ridge (610 m above sea level) and will be compared to the site at Alert on an elevated plain (200 m above sea level). This will allow us to determine the relative contributions from processes and sources at the sites at different elevations. Comparisons with aerosol optical depth and GEOS-Chem model output will also be presented to put these surface measurements into context with the overlying and regional atmosphere. Results from this study contribute to our knowledge of aerosol in the high Arctic.

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

NASA Astrophysics Data System (ADS)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilde, S.; Zhang, Y.; Dall'Osto, M.

2014-04-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterized by a less dense urbanization. We present here the results obtained in San Pietro Capofiume, which is located in a sparsely inhabited sector of the Po Valley, Italy. The experiment was carried out in summer 2009 in the framework of the EUCAARI project ("European Integrated Project on Aerosol, Cloud Climate Aerosol Interaction"). For the first time in Europe, six state-of-the-art techniques were used in parallel: (1) on-line TSI aerosol time-of-flight mass spectrometer (ATOFMS), (2) on-line Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), (3) soot particle aerosol mass spectrometer (SP-AMS), (4) on-line high resolution time-of-flight mass spectrometer-thermal desorption aerosol gas chromatograph (HR-ToFMS-TAG), (5) off-line twelve-hour resolution proton nuclear magnetic resonance (H-NMR) spectroscopy, and (6) chemical ionization mass spectrometry (CIMS) for the analysis of gas-phase precursors of secondary aerosol. Data from each aerosol spectroscopic method were analysed individually following ad-hoc tools (i.e. PMF for AMS, Art-2a for ATOFMS). The results obtained from each techniques are herein presented and compared. This allows us to clearly link the modifications in aerosol chemical composition to transitions in air mass origin and meteorological regimes. Under stagnant conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC

Linking Remotely Sensed Aerosol Types to Their Chemical Composition

NASA Technical Reports Server (NTRS)

Dawson, Kyle William; Kacenelenbogen, Meloe S.; Johnson, Matthew S.; Burton, Sharon P.; Hostetler, Chris A.; Meskhidze, Nicholas

2016-01-01

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% +/- 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into 'dark' and 'light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

Linking remotely sensed aerosol types to their chemical composition

NASA Astrophysics Data System (ADS)

Dawson, K. W.; Kacenelenbogen, M. S.; Johnson, M. S.; Burton, S. P.; Hostetler, C. A.; Meskhidze, N.

2016-12-01

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% ± 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into `dark' and `light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

Aerosols, light, and water: Measurements of aerosol optical properties at different relative humidities

NASA Astrophysics Data System (ADS)

Orozco, Daniel

The Earth's atmosphere is composed of a large number of different gases as well as tiny suspended particles, both in solid and liquid state. These tiny particles, called atmospheric aerosols, have an immense impact on our health and on our global climate. Atmospheric aerosols influence the Earth's radiation budget both directly and indirectly. In the direct effect, aerosols scatter and absorb sunlight changing the radiative balance of the Earth-atmosphere system. Aerosols indirectly influence the Earth's radiation budget by modifying the microphysical and radiative properties of clouds as well as their water content and lifetime. In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering coefficient and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground based observations with other optical aerosol measurements techniques such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. This dissertation presents the aerosol hygroscopicity experiment investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (sp) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (Jan 10-Feb 6, 2013), Baltimore, MD (Jul 3-30, 2013), and Golden, CO (Jul 12-Aug 10, 2014). Observations in Porterville and Golden were part of the NASA-sponsored DISCOVER-AQ project. The measured sp under varying RH in the three sites was combined with ground aerosol extinction, PM2:5mass concentrations, particle composition measurements, and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of sp

Airborne Aerosol in Situ Measurements during TCAP: A Closure Study of Total Scattering

DOE PAGES

Kassianov, Evgueni I.; Berg, Larry K.; Pekour, Mikhail S.; ...

2015-07-31

We present here a framework for calculating the total scattering of both non-absorbing and absorbing aerosol at ambient conditions from aircraft data. The synergistically employed aircraft data involve aerosol microphysical, chemical, and optical components and ambient relative humidity measurements. Our framework is developed emphasizing the explicit use of the complementary chemical composition data for estimating the complex refractive index (RI) of particles, and thus obtaining improved ambient size spectra derived from Optical Particle Counter (OPC) measurements. The feasibility of our framework for improved calculations of total aerosol scattering is demonstrated for different ambient conditions with a wide range of relativemore » humidities (from 5 to 80%) using three types of data collected by the U.S. Department of Energy (DOE) G-1 aircraft during the recent Two-Column Aerosol Project (TCAP). Namely, these three types of data employed are: (1) size distributions measured by an Ultra High Sensitivity Aerosol Spectrometer (UHSAS; 0.06-1 µm), a Passive Cavity Aerosol Spectrometer (PCASP; 0.1-3 µm) and a Cloud and Aerosol Spectrometer (CAS; 0.6- >10 µm), (2) chemical composition data measured by an Aerosol Mass Spectrometer (AMS; 0.06-0.6 µm) and a Single Particle Soot Photometer (SP2; 0.06-0.6 µm), and (3) the dry total scattering coefficient measured by a TSI integrating nephelometer at three wavelengths (0.45, 0.55, 0.7 µm) and scattering enhancement factor measured with a humidification system at three RHs (near 45%, 65% and 90%) at a single wavelength (0.525 µm). We demonstrate that good agreement (~10% on average) between the observed and calculated scattering at these three wavelengths can be obtained using the best available chemical composition data for the RI-based correction of the OPC-derived size spectra. We also demonstrate that ignoring the RI-based correction and using non-representative RI values can cause a substantial

Influence of aerosols on surface reaching spectral irradiance and introduction to a new technique for estimating aerosol radiative forcing from spectral flux measurements

NASA Astrophysics Data System (ADS)

Rao, R. R.

2015-12-01

Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. In this study we look into the approach where ground based spectral radiation flux measurements along with an RT model is used to estimate radiative forcing. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and 3nm resolution for around 54 clear-sky days during which AOD range was around 0.1 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. All the measurements were made in the campus of Indian Institute of Science which is in the heart of Bangalore city. The primary study involved in understanding the sensitivity of spectral flux to change in the mass concentration of individual aerosol species (Optical properties of Aerosols and Clouds -OPAC classified aerosol species) using the SBDART RT model. This made us clearly distinguish the region of influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves an iterative process where the mixture of aerosol species are changed in OPAC model and RT model is run as long as the mixture which mimics the measured spectral flux within 2-3% deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model aerosol radiative forcing is estimated. The new method is limited to clear sky scenes and its accuracy to derive an optically equivalent aerosol mixture reduces when diffuse component of flux increases. Our analysis also showed that direct component of spectral flux is

Measurements of Hygroscopicity- and Size-Resolved Sea Spray Aerosol

NASA Astrophysics Data System (ADS)

Phillips, B.; Dawson, K. W.; Royalty, T. M.; Reed, R. E.; Petters, M.; Meskhidze, N.

2015-12-01

Atmospheric aerosols play a central role in many environmental processes by influencing the Earth's radiative balance, tropospheric chemistry, clouds, biogeochemical cycles, and visibility as well as adversely impacting human health. Based on their origin, atmospheric aerosols can be defined as anthropogenic or natural. Recent studies have shown that a large fraction of uncertainty in the radiative effects of anthropogenic aerosols is related to uncertainty in natural—background—aerosols. Marine aerosols are of particular interest due to the abundance of oceans covering the Earth's surface. Despite their importance, limited information is currently available for size- and composition-resolved marine aerosol emission fluxes. Our group has designed and built an instrument for measuring the size- and hygroscopicity-resolved sea spray aerosol fluxes. The instrument was first deployed during spring 2015 at the end of the 560 m pier of the US Army Corps of Engineers' Field Research Facility in Duck, NC. Measurements include 200 nm-sized diameter growth factor (hygroscopicity) distributions, sea spray particle flux measurements, and total sub-micron sized aerosol concentration. Ancillary ocean data includes salinity, pH, sea surface temperature, dissolved oxygen content, and relative fluorescence (proxy for [Chl-a]). Hygroscopicity distribution measurements show two broad peaks, one indicative of organics and sulfates and another suggestive of sea salt. The fraction of 200 nm-sized salt particles having hygroscopicity similar to that of sea-spray aerosol contributes up to ~24% of the distribution on days with high-speed onshore winds and up to ~3% on calm days with winds blowing from the continent. However, the total concentration of sea-spray-like particles originating from offshore versus onshore winds was relatively similar. Changes in the relative contribution of sea-salt to number concentration were caused by a concomitant changes in total aerosol concentration

The impact of aerosol composition on the particle to gas partitioning of reactive mercury.

PubMed

Rutter, Andrew P; Schauer, James J

2007-06-01

A laboratory system was developed to study the gas-particle partitioning of reactive mercury (RM) as a function of aerosol composition in synthetic atmospheric particulate matter. The collection of RM was achieved by filter- and sorbent-based methods. Analyses of the RM collected on the filters and sorbents were performed using thermal extraction combined with cold vapor atomic fluorescence spectroscopy (CVAFS), allowing direct measurement of the RM load on the substrates. Laboratory measurements of the gas-particle partitioning coefficients of RM to atmospheric aerosol particles revealed a strong dependence on aerosol composition, with partitioning coefficients that varied by orders of magnitude depending on the composition of the particles. Particles of sodium nitrate and the chlorides of potassium and sodium had high partitioning coefficients, shifting the RM partitioning toward the particle phase, while ammonium sulfate, levoglucosan, and adipic acid caused the RM to partition toward the gas phase and, therefore, had partitioning coefficients that were lower by orders of magnitude.

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.

Aerosol chemical composition at Cabauw, The Netherlands as observed in two intensive periods in May 2008 and March 2009

NASA Astrophysics Data System (ADS)

Mensah, A. A.; Holzinger, R.; Otjes, R.; Trimborn, A.; Mentel, Th. F.; ten Brink, H.; Henzing, B.; Kiendler-Scharr, A.

2012-05-01

Observations of aerosol chemical composition in Cabauw, the Netherlands, are presented for two intensive measurement periods in May 2008 and March 2009. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and is compared to observations from aerosol size distribution measurements as well as composition measurements with a Monitor for AeRosol and GAses (MARGA) based instrument and a Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS). An overview of the data is presented and the data quality is discussed. In May 2008 enhanced pollution was observed with organics contributing 40% to the PM1 mass. In contrast the observed average mass loading was lower in March 2009 and a dominance of ammonium nitrate (42%) was observed. The semi-volatile nature of ammonium nitrate is evident in the diurnal cycles with maximum concentrations observed in the morning hours in May 2008 and little diurnal variation observed in March 2009. Size dependent composition data from AMS measurements are presented and show a dominance of organics in the size range below 200 nm. A higher O:C ratio of the organics is observed for May 2008 than for March 2009. Together with the time series of individual tracer ions this shows the dominance of OOA over HOA in May 2008.

New Approach for Near-Real-Time Measurement of Elemental Composition of Aerosol Using Laser-Induced Breakdown Spectroscopy

PubMed Central

Diwakar, Prasoon; Kulkarni, Pramod; Birch, M. Eileen

2015-01-01

A new approach has been developed for making near-real-time measurement of elemental composition of aerosols using plasma spectroscopy. The method allows preconcentration of miniscule particle mass (pg to ng) directly from the sampled aerosol stream through electrostatic deposition of charged particles (30–900 nm) onto a flat-tip microneedle electrode. The collected material is subsequently ablated from the electrode and monitored by laser-induced breakdown spectroscopy. Atomic emission spectra were collected using a broadband spectrometer with a wavelength range of 200–980 nm. A single-sensor delay time of 1.3 μs was used in the spectrometer for all elements to allow simultaneous measurement of multiple elements. The system was calibrated for various elements including Cd, Cr, Cu, Mn, Na, and Ti. The absolute mass detection limits for these elements were experimentally determined and found to be in the range of 0.018–5 ng. The electrostatic collection technique has many advantages over other substrate-based methods involving aerosol collection on a filter or its focused deposition using an aerodynamic lens. Because the particle mass is collected over a very small area that is smaller than the spatial extent of the laser-induced plasma, the entire mass is available for analysis. This considerably improves reliability of the calibration and enhances measurement accuracy and precision. Further, the aerosol collection technique involves very low pressure drop, thereby allowing higher sample flow rates with much smaller pumps—a desirable feature for portable instrumentation. Higher flow rates also make it feasible to measure trace element concentrations at part per trillion levels. Detection limits in the range of 18–670 ng m−3 can be achieved for most of the elements studied at a flow rate of 1.5 L min−1 with sampling times of 5 min. PMID:26692632

Photoacoustic measurements of photokinetics in single optically trapped aerosol droplets

NASA Astrophysics Data System (ADS)

Covert, Paul; Cremer, Johannes; Signorell, Ruth; Thaler, Klemens; Haisch, Christoph

2017-04-01

It is well established that interaction of light with atmospheric aerosols has a large impact on the Earth's climate. However, uncertainties in the magnitude of this impact remain large, due in part to broad distributions of aerosol size, composition, and chemical reactivity. In this context, photoacoustic spectroscopy is commonly used to measure light absorption by aerosols. Here, we present photoacoustic measurements of single, optically-trapped nanodroplets to reveal droplet size-depencies of photochemical and physical processes. Theoretical considerations have pointed to a size-dependence in the magnitude and phase of the photoacoustic response from aerosol droplets. This dependence is thought to originate from heat transfer processes that are slow compared to the acoustic excitation frequency. In the case of a model aerosol, our measurements of single particle absorption cross-section versus droplet size confirm these theoretical predictions. In a related study, using the same model aerosol, we also demonstrate a droplet size-dependence of photochemical reaction rates [1]. Within sub-micron sized particles, photolysis rates were observed to be an order of magnitude greater than those observed in larger droplets. [1] J. W. Cremer, K. M. Thaler, C. Haisch, and R. Signorell. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics. Nat. Commun., 7:10941, 2016.

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Bergstrom, Robert A.; Russell, Philip B.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net shortwave flux at the tropopause by combining maps of satellite-derived aerosol optical depth (AOD) with model aerosol properties. We exclude African dust, primarily by restricting latitudes to 25-60 N. Aerosol properties were determined via column closure analyses in two recent experiments, TARFOX and ACE 2. The analyses use in situ measurements of aerosol composition and air- and ship-borne sunphotometer measurements of AOD spectra. The resulting aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. It has a midvisible single- scattering albedo of 0.9, which is in the range obtained from in situ measurements of aerosol scattering and absorption in both TARFOX and ACE 2. Combining seasonal maps of AVHRR-derived midvisible AOD with the aerosol model yields maps of 24-hour average net radiative flux changes at the tropopause. For cloud-free conditions, results range from -9 W/sq m near the eastern US coastline in the summer to -1 W/sq m in the mid-Atlantic during winter; the regional annual average is -3.5 W/sq m. Using a non- absorbing aerosol model increases these values by about 30%. We estimate the effect of clouds using ISCCP cloud-fraction maps. Because ISCCP midlatitude North Atlantic cloud fractions are relatively large, they greatly reduce the computed aerosol-induced flux changes. For example, the regional annual average decreases from -3.5 W/sq m to -0.8 W/sq m. We compare results to previous model calculations for a variety of aerosol types.

North Atlantic Aerosol Radiative Effects Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Bergstrom, Robert W.; Russell, Philip B.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net shortwave flux at the tropopause by combining maps of satellite-derived aerosol optical depth (AOD) with model aerosol properties. We exclude African dust, primarily by restricting latitudes to 25-60 N. Aerosol properties were determined via column closure analyses in two recent experiments, TARFOX and ACE 2. The analyses use in situ measurements of aerosol composition and air- and ship-borne sunphotometer measurements of AOD spectra. The resulting aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. It has a midvisible single-scattering albedo of 0.9, which is in the range obtained from in situ measurements of aerosol scattering and absorption in both TARFOX and ACE 2. Combining seasonal maps of AVHRR-derived midvisible AOD with the aerosol model yields maps of 24-hour average net radiative flux changes at the tropopause. For cloud-free conditions, results range from -9 W/sq m near the eastern US coastline in the summer to -1 W/sq m in the mid-Atlantic during winter; the regional annual average is -3.5 W/sq m. Using a non- absorbing aerosol model increases these values by about 30%. We estimate the effect of clouds using ISCCP cloud-fraction maps. Because ISCCP midlatitude North Atlantic cloud fractions are relatively large, they greatly reduce the computed aerosol-induced flux changes. For example, the regional annual average decreases from -3.5 W/sq m to -0.8 W/sq m. We compare results to previous model calculations for a variety of aerosol types.

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Bergstrom, Robert W.; Schmid, Beat; Livingston, John M.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net shortwave flux at the tropopause by combining maps of satellite-derived aerosol optical depth (AOD) with model aerosol properties. We exclude African dust, primarily by restricting latitudes to 25-60 N. Aerosol properties were determined via column closure analyses in two recent experiments, TARFOX and ACE 2. The analyses use in situ measurements of aerosol composition and air- and ship-borne sunphotometer measurements of AOD spectra. The resulting aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. It has a midvisible single-scattering albedo of 0.9, which is in the range obtained from in situ measurements of aerosol scattering and absorption in both TARFOX and ACE 2. Combining seasonal maps of AVHRR-derived midvisible AOD with the aerosol model yields maps of 24-hour average net radiative flux changes at the tropopause. For cloud-free conditions, results range from -9 W/sq m near the eastern US coastline in the summer to -1 W/sq m in the mid-Atlantic during winter; the regional annual average is -3.5 W/sq m. Using a non- absorbing aerosol model increases these values by about 30%. We estimate the effect of clouds using ISCCP cloud-fraction maps. Because ISCCP midlatitude North Atlantic cloud fractions are relatively large, they greatly reduce the computed aerosol-induced flux changes. For example, the regional annual average decreases from -3.5 W/sq m to -0.8 W/sq m. We compare results to previous model calculations for a variety of aerosol types.

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

The Chemical Composition and Mixing State of Sea Spray Aerosol and Organic Aerosol in the Winter-Spring Arctic

NASA Astrophysics Data System (ADS)

Kirpes, R.; Bondy, A. L.; Bonanno, D.; Moffet, R.; Wang, B.; Laskin, A.; Ault, A. P.; Pratt, K.

2016-12-01

The Arctic region is undergoing rapid transformations and loss of sea ice due to climate change. With increased sea ice fracturing resulting in greater open ocean surface, winter emissions of sea spray aerosol (SSA) are expected to be increasing. Additionally, during the winter-spring transition, Arctic haze contributes to the Arctic aerosol budget. The magnitude of aerosol climate effects depends on the aerosol composition and mixing state (distribution of chemical species within and between particles). However, few studies of aerosol chemistry have been conducted in the winter Arctic, despite it being a time when aerosol impacts on clouds are expected to be significant. To study aerosol composition and mixing state in the winter Arctic, atmospheric particles were collected near Barrow, Alaska in January and February 2014 for off-line individual particle chemical analysis. SSA was the most prevalent particle type observed. Sulfate and nitrate were observed to be internally mixed with SSA and organic aerosol. Greater than 98% of observed SSA particles contained organic content, with 15-35% organic volume fraction on average for individual particles. The SSA organic compounds consisted of carbohydrates, lipids, and fatty acids found in the seawater surface microlayer. SSA was determined to be emitted from open leads, while transported sulfate and nitrate contributed to aging of SSA and organic aerosol. Determining the aerosol chemical composition and mixing state in the winter Arctic will further the understanding of how individual aerosol particles impact climate through radiative effects and cloud formation.

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.

AEROSOL AND GAS MEASUREMENT

EPA Science Inventory

Measurements provide fundamental information for evaluating and managing the impact of aerosols on air quality. Specific measurements of aerosol concentration and their physical and chemical properties are required by different users to meet different user-community needs. Befo...

Temporal variability of the chemical composition of surface aerosol in the Moscow region in 1999-2005 from the results of infrared spectroscopy of aerosol samples

NASA Astrophysics Data System (ADS)

Shukurova, L. M.; Gruzdev, A. N.

2010-06-01

The temporal variability of the chemical composition of surface aerosol with particle diameters of 0.7-2 μm is analyzed. This analysis is based on the results of measurements of infrared transmission spectra of aerosol samples collected with the use of a cascade impactor at the Zvenigorod Scientific Station of the Institute of Atmospheric Physics (IAP) in 1999-2005. Seasonal features of the aerosol chemical composition and its dependence on the particle size are revealed. The interdiurnal variability of the aerosol composition depends on the season, and it manifests itself more strongly in winter and spring. Air-mass changes lead to changes in the relation of sulfates and nitrates in the micron fraction of aerosol. The enrichment of samples in nitrates is especially characteristic of the winter and spring seasons. Compounds containing the NO2 group are often met in the samples of aerosol with particle sizes of 0.7-1.3 μm during the cold time of the year. The estimates of the optical thickness of micron aerosol in the sulfate absorption band are obtained, and optical-thickness variations of some scales are detected. The quantitative characteristics of statistical relations between different chemical components of aerosol inside individual fractions and between chemical components of the micron and submicron fractions are obtained and analyzed.

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.

Airborne High Spectral Resolution Lidar Aerosol Measurements during MILAGRO and TEXAQS/GOMACCS

NASA Technical Reports Server (NTRS)

Ferrare, Richard; Hostetler, Chris; Hair, John; Cook Anthony; Harper, David; Burton, Sharon; Clayton, Marian; Clarke, Antony; Russell, Phil; Redemann, Jens

2007-01-01

Two1 field experiments conducted during 2006 provided opportunities to investigate the variability of aerosol properties near cities and the impacts of these aerosols on air quality and radiative transfer. The Megacity Initiative: Local and Global Research Observations (MILAGRO) /Megacity Aerosol Experiment in Mexico City (MAX-MEX)/Intercontinental Chemical Transport Experiment-B (INTEX-B) joint experiment conducted during March 2006 investigated the evolution and transport of pollution from Mexico City. The Texas Air Quality Study (TEXAQS)/Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) (http://www.al.noaa.gov/2006/) conducted during August and September 2006 investigated climate and air quality in the Houston/Gulf of Mexico region. During both missions, the new NASA Langley airborne High Spectral Resolution Lidar (HSRL) was deployed on the NASA Langley B200 King Air aircraft and measured profiles of aerosol extinction, backscattering, and depolarization to: 1) characterize the spatial and vertical distributions of aerosols, 2) quantify aerosol extinction and optical thickness contributed by various aerosol types, 3) investigate aerosol variability near clouds, 4) evaluate model simulations of aerosol transport, and 5) assess aerosol optical properties derived from a combination of surface, airborne, and satellite measurements.

In situ measurements of angular-dependent light scattering by aerosols over the contiguous United States

NASA Astrophysics Data System (ADS)

Reed Espinosa, W.; Vanderlei Martins, J.; Remer, Lorraine A.; Puthukkudy, Anin; Orozco, Daniel; Dolgos, Gergely

2018-03-01

This work provides a synopsis of aerosol phase function (F11) and polarized phase function (F12) measurements made by the Polarized Imaging Nephelometer (PI-Neph) during the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and the Deep Convection Clouds and Chemistry (DC3) field campaigns. In order to more easily explore this extensive dataset, an aerosol classification scheme is developed that identifies the different aerosol types measured during the deployments. This scheme makes use of ancillary data that include trace gases, chemical composition, aerodynamic particle size and geographic location, all independent of PI-Neph measurements. The PI-Neph measurements are then grouped according to their ancillary data classifications and the resulting scattering patterns are examined in detail. These results represent the first published airborne measurements of F11 and -F12/F11 for many common aerosol types. We then explore whether PI-Neph light-scattering measurements alone are sufficient to reconstruct the results of this ancillary data classification algorithm. Principal component analysis (PCA) is used to reduce the dimensionality of the multi-angle PI-Neph scattering data and the individual measurements are examined as a function of ancillary data classification. Clear clustering is observed in the PCA score space, corresponding to the ancillary classification results, suggesting that, indeed, a strong link exists between the angular-scattering measurements and the aerosol type or composition. Two techniques are used to quantify the degree of clustering and it is found that in most cases the results of the ancillary data classification can be predicted from PI-Neph measurements alone with better than 85 % recall. This result both emphasizes the validity of the ancillary data classification as well as the PI-Neph's ability to distinguish common aerosol types without additional information.

Chemical composition of atmospheric aerosols resolved via positive matrix factorization

NASA Astrophysics Data System (ADS)

Äijälä, Mikko; Junninen, Heikki; Heikkinen, Liine; Petäjä, Tuukka; Kulmala, Markku; Worsnop, Douglas; Ehn, Mikael

2017-04-01

Atmospheric particulate matter is a complex mixture of various chemical species such as organic compounds, sulfates, nitrates, ammonia, chlorides, black carbon and sea salt. As aerosol chemical composition strongly influences aerosol climate effects (via cloud condensation nucleus activation, hygroscopic properties, aerosol optics, volatility and condensation) as well as health effects (toxicity, carcinogenicity, particle morphology), detailed understanding of atmospheric fine particle composition is widely beneficial for understanding these interactions. Unfortunately the comprehensive, detailed measurement of aerosol chemistry remains difficult due to the wide range of compounds present in the atmosphere as well as for the miniscule mass of the particles themselves compared to their carrier gas. Aerosol mass spectrometer (AMS; Canagaratna et al., 2007) is an instrument often used for characterization of non-refractive aerosol types: the near-universal vaporization and ionisation technique allows for measurement of most atmospheric-relevant compounds (with the notable exception of refractory matter such as sea salt, black carbon, metals and crustal matter). The downside of the hard ionisation applied is extensive fragmentation of sample molecules. However, the apparent loss of information in fragmentation can be partly offset by applying advanced statistical methods to extract information from the fragmentation patterns. In aerosol mass spectrometry statistical analysis methods, such as positive matrix factorization (PMF; Paatero, 1999) are usually applied for aerosol organic component only, to keep the number of factors to be resolved manageable, to retain the inorganic components for solution validation via correlation analysis, and to avoid inorganic species dominating the factor model. However, this practice smears out the interactions between organic and inorganic chemical components, and hinders the understanding of the connections between primary and

Wavelength dependence of aerosol backscatter coefficients obtained by multiple wavelength Lidar measurements

NASA Technical Reports Server (NTRS)

Sasano, Y.; Browell, E. V.

1986-01-01

Aerosols are often classified into several general types according to their origins and composition, such as maritime, continental, and stratospheric aerosols, and these aerosol types generally have different characteristics in chemical and physical properties. The present study aims at demonstrating the potential for distinguishing these aerosol types by the wavelength dependence of their backscatter coefficients obtained from quantitative analyses of multiple wavelength lidar signals. Data from the NASA Airborne Differential Abosrption lidar (DIAL) S ystems, which can measure aerosol backscatter profiles at wavelenghts of 300, 600, and 1064 nm and ozone profiles of backscatter coefficients for these three wavelength were derived from the observations of aerosols of different types. Observations were performed over the Atlantic Ocean, the Southwestern United States, and French Guyana.

In Situ Measurement of Aerosol Extinction

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Castaneda, R.; Owano, T. G.; Bear, D.; Gore, Warren J. (Technical Monitor)

2001-01-01

Aerosols are important contributors to the radiative forcing in the atmosphere. Much of the uncertainty in our knowledge of climate forcing is due to uncertainties in the radiative forcing due to aerosols as illustrated in the IPCC reports of the last ten years. Improved measurement of aerosol optical properties, therefore, is critical to an improved understanding of atmospheric radiative forcing. Additionally, attempts to reconcile in situ and remote measurements of aerosol radiative properties have generally not been successful. This is due in part to the fact that it has been impossible to measure aerosol extinction in situ in the past. In this presentation we introduce a new instrument that employs the techniques used in cavity ringdown spectroscopy to measure the aerosol extinction and scattering coefficients in situ. A prototype instrument has been designed and tested in the lab and the field. It is capable of measuring aerosol extinction coefficient to 2x10(exp -6) per meter. This prototype instrument is described and results are presented.

Fine Aerosol Bulk Composition Measured on WP-3D Research Aircraft in Vicinity of the Northeastern United States - Results from NEAQS

NASA Technical Reports Server (NTRS)

Peltier, R. E.; Sullivan, A. P.; Weber, R. J.; Brock, C. A.; Wollny, A. G.; Holloway, J. S.; deGouw, J. A.; Warneke, C.

2007-01-01

During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM(sub 1.0)) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (approximately 60% micro gram /micro gram) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km), but was significantly higher at altitude layers in the free troposphere (above 2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

NASA Astrophysics Data System (ADS)

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

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. 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 relative humidity and temperature 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). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

Atmospheric aerosols: A literature summary of their physical characteristics and chemical composition

NASA Technical Reports Server (NTRS)

Harris, F. S., Jr.

1976-01-01

This report contains a summary of 199 recent references on the characterization of atmospheric aerosols with respect to their composition, sources, size distribution, and time changes, and with particular reference to the chemical elements measured by modern techniques, especially activation analysis.

Regional haze case studies in the southwestern U.S—I. Aerosol chemical composition

NASA Astrophysics Data System (ADS)

Macias, Edward S.; Zwicker, Judith O.; Ouimette, James R.; Hering, Susanne V.; Friedlander, Sheldon K.; Cahill, Thomas A.; Kuhlmey, Gregory A.; Richards, L. Willard

Aerosol chemical composition as a function of particle size was determined in the southwestern U.S.A. during four weeks of sampling in June, July and December, 1979 as a part of project VISITA. Samples were collected at two ground stations about 80 km apart near Page (AZ) and in two aircraft flying throughout the region. Several different size separating aerosol samplers and chemical analysis procedures were intercompared and were used in determining the size distribution and elemental composition of the aerosol. Sulfur was shown to be in the form of water soluable sulfate, highly correlated with ammonium ion, and with an average [NH +4]/[SO 2-4] molar ratio of 1.65. During the summer sampling period, three distinct regimes were observed, each with a different aerosol composition. The first, 24 h sampling ending 30 June, was characterized by a higher than average value of light scattering due to particles (b sp) of 24 × 10 -6m-1 and a fine particulate mass ( Mf) of 8.5 μg m -1. The fine particle aerosol was dominated by sulfate and carbon. Aircraft measurements showed the aerosol was homogeneous throughout the region at that time. The second regime, 5 July, had the highest average bsp of 51 × 10 -6m -1 during the sampling period with Mf of 3.2 μgm -3. The fine particle aerosol had nearly equal concentrations of carbon and ammonium sulfate. For all three regimes, enrichment factor analysis indicated fine and coarse particle Cu, Zn, Cl, Br, and Pb and fine particle K were enriched above crustal concentrations relative to Fe, indicating that these elements were present in the aerosol from sources other than wind blown dust. Particle extinction budgets calculated for the three regimes indicated that fine particles contributed most significantly, with carbon and (NH 4) 2SO 4 making the largest contributions. Fine particle crustal elements including Si did not contribute significantly to the extinction budget during this study. The December sampling was characterized

Stratospheric Aerosol Measurements

NASA Technical Reports Server (NTRS)

Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

1998-01-01

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

NASA Astrophysics Data System (ADS)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-12-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation

Molecular Composition and Volatility of Organic Aerosol in the Southeastern U.S.: Implications for IEPOX Derived SOA.

PubMed

Lopez-Hilfiker, F D; Mohr, C; D'Ambro, E L; Lutz, A; Riedel, T P; Gaston, C J; Iyer, S; Zhang, Z; Gold, A; Surratt, J D; Lee, B H; Kurten, T; Hu, W W; Jimenez, J; Hallquist, M; Thornton, J A

2016-03-01

We present measurements as part of the Southern Oxidant and Aerosol Study (SOAS) during which atmospheric aerosol particles were comprehensively characterized. We present results utilizing a Filter Inlet for Gases and AEROsol coupled to a chemical ionization mass spectrometer (CIMS). We focus on the volatility and composition of isoprene derived organic aerosol tracers and of the bulk organic aerosol. By utilizing the online volatility and molecular composition information provided by the FIGAERO-CIMS, we show that the vast majority of commonly reported molecular tracers of isoprene epoxydiol (IEPOX) derived secondary organic aerosol (SOA) is derived from thermal decomposition of accretion products or other low volatility organics having effective saturation vapor concentrations <10(-3) μg m(-3). In addition, while accounting for up to 30% of total submicrometer organic aerosol mass, the IEPOX-derived SOA has a higher volatility than the remaining bulk. That IEPOX-SOA, and more generally bulk organic aerosol in the Southeastern U.S. is comprised of effectively nonvolatile material has important implications for modeling SOA derived from isoprene, and for mechanistic interpretations of molecular tracer measurements. Our results show that partitioning theory performs well for 2-methyltetrols, once accretion product decomposition is taken into account. No significant partitioning delays due to aerosol phase or viscosity are observed, and no partitioning to particle-phase water or other unexplained mechanisms are needed to explain our results.

A model for studying the composition and chemical effects of stratospheric aerosols

NASA Technical Reports Server (NTRS)

Tabazadeh, Azadeh; Turco, Richard P.; Jacobson, Mark Z.

1994-01-01

We developed polynomial expressions for the temperature dependence of the mean binary and water activity coefficients for H2SO4 and HNO3 solutions. These activities were used in an equilibrium model to predict the composition of stratospheric aerosols under a wide range of environmental conditions. For typical concentrations of H2O, H2SO4, HNO3, HCl, HBr, HF, and HOCl in the lower stratosphere, the aerosol composition is estimated as a function of the local temperature and the ambient relative humidity. For temperatures below 200 K, our results indicate that (1) HNO3 contributes a significant mass fraction to stratospheric aerosols, and (2) HCl solubility is considerably affected by HNO3 dissolution into sulfate aerosols. We also show that, in volcanically disturbed periods, changes in stratospheric aerosol composition can significantly alter the microphysics that leads to the formation of polar stratospheric clouds. The effects caused by HNO3 dissolution on the physical and chemical properties of stratospheric aerosols are discussed.

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

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

2011-03-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in Southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources were reflected through three factors: two biomass burning factors and a highly chemically processed long range transport factor. The biomass burning factors were separated by PMF due to differences in chemical processing which were caused in part by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

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

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

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

Constraining Upper Troposphere/Lower Stratosphere Aerosol Physical Processes with High-Altitude Aircraft Measurements

NASA Technical Reports Server (NTRS)

Jensen, Eric; Rosenlof, Karen H.; Thornberry, Troy

2018-01-01

Interest in a more complete understanding of the sources, composition and microphysics of stratospheric aerosol particles has intensified during recent years for several reasons: (1) small volcanic eruptions have been recognized as a driver of short-term changes in climate forcing; (2) emissions of sulfur dioxide (SO2) and other aerosol precursors have shifted to south Asia and other low latitude regions with intense vertical transport; (3) organic material has been recognized as a key contributor to lower stratospheric aerosol mass; and (4) interest in possible solar radiation management (geoengineering) through significant enhancements in stratospheric aerosols has intensified. To address stratospheric aerosol science issues, we are proposing a NASA Earth Ventures mission to NASA to provide extensive high-altitude aircraft measurements of critical gas-phase and aerosol properties at multiple locations across the planet. In this presentation, we will discuss the objectives of the proposed campaign, the measurements provided, the sampling strategy, and the modeling and analysis approaches that would be used to address specific science questions.

Org Areo Boreal Forest Sources, compositions and properties of newly formed and regional organic aerosol in a boreal forest during the Biogenic Aerosol: Effects on Clouds and Climate Campaign

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

Thornton, Joel A

The major goals of this project were to make unique measurements, as part of the DOE sponsored Biogenic Aerosol Effects on Clouds and Climate (BAECC) campaign, of the volatility and molecular composition of organic aerosol, as well as gas-phase concentrations of oxygenated organic compounds that interact and affect organic aerosol. In addition, we aimed to conduct a similar set of measurements as part of a collaborative set of environmental simulation chamber experiments at PNNL, the aim of which was to simulate the atmospheric oxidation of key biogenic volatile organic compounds (BVOC) and study the associated formation and evolution of secondarymore » organic aerosol (SOA). The target BVOC were a set of monoterpenes, isoprene, and related intermediates such as IEPOX. The ultimate goal of such measurements are to develop a more detailed mechanistic understanding of the sensitivity of SOA mass formation and lifetime to precursor and environmental conditions. Molecular composition and direct volatility measurements provide robust tracers of chemical processing and properties. As such, meeting these goals will allow for stronger constraints on the types of processes and their fundamental descriptions needed to simulate aerosol particle number and size, and cloud nucleating ability in regional and global earth system models.« 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

Insight into global trends in aerosol composition from 2005 to 2015 inferred from the OMI Ultraviolet Aerosol Index

NASA Astrophysics Data System (ADS)

Hammer, Melanie S.; Martin, Randall V.; Li, Chi; Torres, Omar; Manning, Max; Boys, Brian L.

2018-06-01

Observations of aerosol scattering and absorption offer valuable information about aerosol composition. We apply a simulation of the Ultraviolet Aerosol Index (UVAI), a method of detecting aerosol absorption from satellite observations, to interpret UVAI values observed by the Ozone Monitoring Instrument (OMI) from 2005 to 2015 to understand global trends in aerosol composition. We conduct our simulation using the vector radiative transfer model VLIDORT with aerosol fields from the global chemical transport model GEOS-Chem. We examine the 2005-2015 trends in individual aerosol species from GEOS-Chem and apply these trends to the UVAI simulation to calculate the change in simulated UVAI due to the trends in individual aerosol species. We find that global trends in the UVAI are largely explained by trends in absorption by mineral dust, absorption by brown carbon, and scattering by secondary inorganic aerosol. Trends in absorption by mineral dust dominate the simulated UVAI trends over North Africa, the Middle East, East Asia, and Australia. The UVAI simulation resolves observed negative UVAI trends well over Australia, but underestimates positive UVAI trends over North Africa and Central Asia near the Aral Sea and underestimates negative UVAI trends over East Asia. We find evidence of an increasing dust source from the desiccating Aral Sea that may not be well represented by the current generation of models. Trends in absorption by brown carbon dominate the simulated UVAI trends over biomass burning regions. The UVAI simulation reproduces observed negative trends over central South America and West Africa, but underestimates observed UVAI trends over boreal forests. Trends in scattering by secondary inorganic aerosol dominate the simulated UVAI trends over the eastern United States and eastern India. The UVAI simulation slightly overestimates the observed positive UVAI trends over the eastern United States and underestimates the observed negative UVAI trends over

Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

NASA Astrophysics Data System (ADS)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-08-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosols (OA) indicated that highly oxidized secondary OA (SOA) showed decreases similar to those of SIA during APEC. However, primary OA (POA) from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging

Composition and physical properties of the Asian Tropopause Aerosol Layer and the North American Tropospheric Aerosol Layer: Composition of ATAL and NATAL

DOE PAGES

Yu, Pengfei; Toon, Owen B.; Neely, Ryan R.; ...

2015-04-10

Recent studies revealed layers of enhanced aerosol scattering in the upper troposphere and lower stratosphere over Asia (Asian Tropopause Aerosol Layer (ATAL)) and North America (North American Tropospheric Aerosol Layer (NATAL)). We use a sectional aerosol model (Community Aerosol and Radiation Model for Atmospheres (CARMA)) coupled with the Community Earth System Model version 1 (CESM1) to explore the composition and optical properties of these aerosol layers. The observed aerosol extinction enhancement is reproduced by CESM1/CARMA. Both model and observations indicate a strong gradient of the sulfur-to-carbon ratio from Europe to the Asia on constant pressure surfaces. We found that themore » ATAL is mostly composed of sulfates, surface-emitted organics, and secondary organics; the NATAL is mostly composed of sulfates and secondary organics. In conclusion, the model also suggests that emission increases in Asia between 2000 and 2010 led to an increase of aerosol optical depth of the ATAL by 0.002 on average which is consistent with observations.« less

Composition and physical properties of the Asian Tropopause Aerosol Layer and the North American Tropospheric Aerosol Layer: Composition of ATAL and NATAL

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

Yu, Pengfei; Toon, Owen B.; Neely, Ryan R.

Recent studies revealed layers of enhanced aerosol scattering in the upper troposphere and lower stratosphere over Asia (Asian Tropopause Aerosol Layer (ATAL)) and North America (North American Tropospheric Aerosol Layer (NATAL)). We use a sectional aerosol model (Community Aerosol and Radiation Model for Atmospheres (CARMA)) coupled with the Community Earth System Model version 1 (CESM1) to explore the composition and optical properties of these aerosol layers. The observed aerosol extinction enhancement is reproduced by CESM1/CARMA. Both model and observations indicate a strong gradient of the sulfur-to-carbon ratio from Europe to the Asia on constant pressure surfaces. We found that themore » ATAL is mostly composed of sulfates, surface-emitted organics, and secondary organics; the NATAL is mostly composed of sulfates and secondary organics. In conclusion, the model also suggests that emission increases in Asia between 2000 and 2010 led to an increase of aerosol optical depth of the ATAL by 0.002 on average which is consistent with observations.« less

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.

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

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

Influence of aerosols on surface reaching spectral irradiance and introduction to a new technique of estimating aerosol radiative forcing from high resolution spectral flux measurements

NASA Astrophysics Data System (ADS)

Rao, Roshan

2016-04-01

Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. We look into the approach where ground based spectral radiation flux measurement is made and along with an Radtiative transfer (RT) model, radiative forcing is estimated. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and a 3nm resolution during around 54 clear-sky days during which AOD range was around 0.01 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. The primary study involved in understanding the sensitivity of spectral flux due to change in individual aerosol species (Optical properties of Aerosols and Clouds (OPAC) classified aerosol species) using the SBDART RT model. This made us clearly distinguish the influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves matching different combinations of aerosol species in OPAC model and RT model as long as the combination which gives the minimum root mean squared deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model, aerosol radiative forcing is estimated. Also an alternate method to estimate the spectral SSA is discussed. Here, the RT model, the observed spectral flux and spectral AOD is used. Spectral AOD is input to RT model and SSA is varied till the minimum root mean squared difference between observed and simulated spectral flux from RT model is obtained. The methods discussed are limited to clear sky scenes and its accuracy to derive

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.

Overview of Aerosol Distribution

NASA Technical Reports Server (NTRS)

Kaufman, Yoram

2005-01-01

Our knowledge of atmospheric aerosols (smoke, pollution, dust or sea salt particles, small enough to be suspended in the air), their evolution, composition, variability in space and time and interaction with clouds and precipitation is still lacking despite decades of research. Understanding the global aerosol system is fundamental for progress in climate change and hydrological cycle research. While a single instrument was used to demonstrate 50 years ago that the global CO2 levels are rising, posing threat of global warming, we need an array of satellites and field measurements coupled with chemical transport models to understand the global aerosol system. This complexity of the aerosol problem results from their short lifetime (1 week) and variable chemical composition. A new generation of satellites provides exciting opportunities to measure the global distribution of aerosols, distinguishing natural from anthropogenic aerosol and measuring their interaction with clouds and climate. I shall discuss these topics and application of the data to air quality monitoring.

Chemical Thermodynamics of Aqueous Atmospheric Aerosols: Modeling and Microfluidic Measurements

NASA Astrophysics Data System (ADS)

Nandy, L.; Dutcher, C. S.

2017-12-01

Accurate predictions of gas-liquid-solid equilibrium phase partitioning of atmospheric aerosols by thermodynamic modeling and measurements is critical for determining particle composition and internal structure at conditions relevant to the atmosphere. Organic acids that originate from biomass burning, and direct biogenic emission make up a significant fraction of the organic mass in atmospheric aerosol particles. In addition, inorganic compounds like ammonium sulfate and sea salt also exist in atmospheric aerosols, that results in a mixture of single, double or triple charged ions, and non-dissociated and partially dissociated organic acids. Statistical mechanics based on a multilayer adsorption isotherm model can be applied to these complex aqueous environments for predictions of thermodynamic properties. In this work, thermodynamic analytic predictive models are developed for multicomponent aqueous solutions (consisting of partially dissociating organic and inorganic acids, fully dissociating symmetric and asymmetric electrolytes, and neutral organic compounds) over the entire relative humidity range, that represent a significant advancement towards a fully predictive model. The model is also developed at varied temperatures for electrolytes and organic compounds the data for which are available at different temperatures. In addition to the modeling approach, water loss of multicomponent aerosol particles is measured by microfluidic experiments to parameterize and validate the model. In the experimental microfluidic measurements, atmospheric aerosol droplet chemical mimics (organic acids and secondary organic aerosol (SOA) samples) are generated in microfluidic channels and stored and imaged in passive traps until dehydration to study the influence of relative humidity and water loss on phase behavior.

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.

Day-night differences in the composition and sources of carbonaceous aerosol at a polluted regional background site in the Netherlands

NASA Astrophysics Data System (ADS)

Dusek, Ulrike; Broekema, Elise; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro

2017-04-01

The origin of carbonaceous aerosol differs during day- and night-time, because emissions from major sources such as traffic, biomass combustion, and secondary organic aerosol formation show a distinct diurnal pattern. Moreover, photochemical processing and evaporation of semi-volatile organic compounds are enhanced during day-time, due to the availability of sunlight and higher temperatures. Assessing day-night differences in sources and chemical composition can give an indication of the importance of local/regional carbon sources and processing, since day-night differences should be averaged out during long-range transport. If local sources dominate, one could expect a strong diurnal variation in the source profile, but if long-range transport dominates the diurnal variation would be much weaker. In this study we measure the isotopic (14C and 13C) and detailed chemical composition of the organic fraction of the aerosol on high volume PM2.5 filter samples that were collected separately during day and night time. Radiocarbon (14C) measurements are used to estimate three main aerosol sources of organic and elemental carbon (OC and EC): Fossil fuel combustion (ff), biomass combustion (bb), and biogenic sources (bio). The detailed chemical and stable isotopic composition are measured at different desorption temperatures from the filter, which separates the more and less refractory organic compounds. The composition of the organic aerosol is measured using an thermal-desporption Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) method (Holzinger et al, 2010) and the stable isotopic composition is measured using a thermal desorption IRMS method (Dusek et al., 2013). Source apportionment results using 14C show that the contribution of fossil fuel combustion to EC and OC is higher during day-time than during night-time. This is valid for all seasons. During night-time biomass combustion plays a bigger role as a source of carbonaceous aerosol. Even in

Classifying aerosol type using in situ surface spectral aerosol optical properties

NASA Astrophysics Data System (ADS)

Schmeisser, Lauren; Andrews, Elisabeth; Ogren, John A.; Sheridan, Patrick; Jefferson, Anne; Sharma, Sangeeta; Kim, Jeong Eun; Sherman, James P.; Sorribas, Mar; Kalapov, Ivo; Arsov, Todor; Angelov, Christo; Mayol-Bracero, Olga L.; Labuschagne, Casper; Kim, Sang-Woo; Hoffer, András; Lin, Neng-Huei; Chia, Hao-Ping; Bergin, Michael; Sun, Junying; Liu, Peng; Wu, Hao

2017-10-01

Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE), absorption Ångström exponent (AAE) and single scattering albedo (SSA) from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes.Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type) and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station.The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol), marine polluted (carbonaceous aerosol mixed with sea salt) and continental dust/biomass sites

Spatio-temporal aerosol particle distributions in the UT/LMS measured by the IAGOS-CARIBIC Observatory

NASA Astrophysics Data System (ADS)

Assmann, Denise; Hermann, Markus; Weigelt, Andreas; Martinsson, Bengt; Brenninkmeijer, Carl; Rauthe-Schöch, Armin; van Velthoven, Peter; Bönisch, Harald; Zahn, Andreas

2017-04-01

Submicrometer aerosol particles in the upper troposphere and lowermost stratosphere (UT/LMS) influence the Earth`s radiation budget directly and, more important, indirectly, by acting as cloud condensation nuclei and by changing trace gas concentrations through heterogeneous chemical processes. Since 1997, regular in situ UT/LMS aerosol particle measurements have been conducted by the Leibniz Institute for Tropospheric Research, Leipzig, Germany and the University of Lund, Sweden, using the the CARIBIC (now IAGOS-CARIBIC) observatory (www.caribic-atmospheric.com) onboard a passenger aircraft. Submicrometer aerosol particle number concentrations and the aerosol particle size distribution are measured using three condensation particle counters and one optical particle size spectrometer. Moreover, particle elemental composition is determined using an aerosol impactor sampler and post-flight ion beam analysis (PIXE, PESA) of the samples in the laboratory. Based on this unique data set, including meteorological analysis, we present representative spatio-temporal distributions of particle number, surface, volume and elemental concentrations in an altitude of 8-12 km covering a large fraction of the northern hemisphere. We discuss the measured values in the different size regimes with respect to sources and sinks in different regions. Additionally, we calculated highly resolved latitudinal and longitudinal cross sections of the particle number size distribution, probability density functions and trends in particle number concentrations, but also in elemental composition, determined from our regular measurements over more than a decade. Moreover, we generated seasonal contour plots for particle number concentrations, the potential temperature, and the equivalent latitude. The results are interpreted with respect to aerosol microphysics and transport using CARIBIC trace gas data like ozone and water vapour. The influence of clouds in the troposphere and the different

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

NASA Astrophysics Data System (ADS)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

2014-11-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

Development of Portable Aerosol Mobility Spectrometer for Personal and Mobile Aerosol Measurement

PubMed Central

Kulkarni, Pramod; Qi, Chaolong; Fukushima, Nobuhiko

2017-01-01

We describe development of a Portable Aerosol Mobility Spectrometer (PAMS) for size distribution measurement of submicrometer aerosol. The spectrometer is designed for use in personal or mobile aerosol characterization studies and measures approximately 22.5 × 22.5 × 15 cm and weighs about 4.5 kg including the battery. PAMS uses electrical mobility technique to measure number-weighted particle size distribution of aerosol in the 10–855 nm range. Aerosol particles are electrically charged using a dual-corona bipolar corona charger, followed by classification in a cylindrical miniature differential mobility analyzer. A condensation particle counter is used to detect and count particles. The mobility classifier was operated at an aerosol flow rate of 0.05 L/min, and at two different user-selectable sheath flows of 0.2 L/min (for wider size range 15–855 nm) and 0.4 L/min (for higher size resolution over the size range of 10.6–436 nm). The instrument was operated in voltage stepping mode to retrieve the size distribution, which took approximately 1–2 minutes, depending on the configuration. Sizing accuracy and resolution were probed and found to be within the 25% limit of NIOSH criterion for direct-reading instruments (NIOSH 2012). Comparison of size distribution measurements from PAMS and other commercial mobility spectrometers showed good agreement. The instrument offers unique measurement capability for on-person or mobile size distribution measurements of ultrafine and nanoparticle aerosol. PMID:28413241

Micrometeorological flux measurements of aerosol and gases above Beijing

NASA Astrophysics Data System (ADS)

Nemitz, Eiko; Langford, Ben; Mullinger, Neil; Cowan, Nicholas; Coyle, Mhairi; Acton, William Joe; Lee, James; Fu, Pingqing

2017-04-01

Air pollution is estimated to cause 1.6 million premature deaths in China every year and in the winter 2016/17 Beijing had to issue health alerts and put in place ad hoc limitations on industrial and vehicular activity. Much of this pollution is attributed to emissions from industrial processes and in particular coal combustion. By contrast, the diffuse pollutant sources within the city are less well understood. This includes, e.g., emissions from the Beijing traffic fleet, the sewage system, food preparation, solid fuel combustion in the streets and small industrial processes. Within the framework of a major UK-Chinese collaboration to study air pollution and its impact on human health in Beijing, we therefore measured fluxes of a large range of pollutants from a height of 102 m on the 325 m meteorological tower at the Institute of Atmospheric Physics. Several instruments were mounted at 102 m: fluxes of CO2 and H2O were measured with an infrared gas analyser (LiCOR 7500) and fluxes of ozone with a combination of a relative fast-response ozone analyser (ROFI) and a 2B absolute O3 instrument. Total particle number fluxes were measured with a condensation particle counter (TSI CPC 3785), and size-segregated fluxes over the size range 0.06 to 20 μm with a combination of an optical Ultrafine High Sensitivity Aerosol Spectrometer (UHSAS) and an Aerodynamic Particle Sizer Spectrometer (TSI APS3321). Ammonia (NH3) fluxes were measured for the first time above the urban environment using an Aerodyne compact quantum cascade laser (QCL). In addition, composition resolved aerosol fluxes were measured with an Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS), operated in a measurement container at the bottom of the tower, which subsampled from a 120 m long copper tube (15 mm OD). The analysis so far suggests that, due to often low wind speeds, fluxes were at times de-coupled from the surface. Fluxes normalised by CO2, a tracer for the amount of fossil fuel consumed, should be

Comparison of Modeled Backscatter using Measured Aerosol Microphysics with Focused CW Lidar Data over Pacific

NASA Technical Reports Server (NTRS)

Srivastava, Vandana; Clarke, Antony D.; Jarzembski, Maurice A.; Rothermel, Jeffry

1997-01-01

During NASA's GLObal Backscatter Experiment (GLOBE) II flight mission over the Pacific Ocean in May-June 1990, extensive aerosol backscatter data sets from two continuous wave, focused CO2 Doppler lidars and an aerosol microphysics data set from a laser optical particle counter (LOPC) were obtained. Changes in aerosol loading in various air masses with associated changes in chemical composition, from sulfuric acid and sulfates to dustlike crustal material, significantly affected aerosol backscatter, causing variation of about 3 to 4 orders of magnitude. Some of the significant backscatter features encountered in different air masses were the low backscatter in subtropical air with even lower values in the tropics near the Intertropical Convergence Zone (ITCZ), highly variable backscatter in the ITCZ, mid-tropospheric aerosol backscatter background mode, and high backscatter in an Asian dust plume off the Japanese coast. Differences in aerosol composition and backscatter for northern and southern hemisphere also were observed. Using the LOPC measurements of physical and chemical aerosol properties, we determined the complex refractive index from three different aerosol mixture models to calculate backscatter. These values provided a well-defined envelope of modeled backscatter for various atmospheric conditions, giving good agreement with the lidar data over a horizontal sampling of approximately 18000 km in the mid-troposphere.

Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

NASA Astrophysics Data System (ADS)

Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

2009-02-01

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ=0.05-0.45. The overall median value of κ≍0.15 was only half of the value typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm). The CCN measurement results were fully consistent with aerosol mass spectrometry (AMS) data, which showed that the organic mass fraction (Xm,org) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a close linear correlation with Xm,org and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which is consistent with laboratory measurements of secondary organic aerosols and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size-dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=0.1 Xm,org+0.6 Xm,inorg), and the CCN number concentrations predicted with κp were in fair agreement with the measurement results. The median CCN number concentrations at S=0.1-0.82% ranged from NCCN,0.10≍30 cm-3 to NCCN,0.82≍150 cm-3, the median concentration of aerosol particles larger than 30 nm was NCN,30≍180 cm-3, and the corresponding integral CCN efficiencies were in the range of NCCN,0

Characterization of aerosols and fibers emitted from composite materials combustion.

PubMed

Chivas-Joly, C; Gaie-Levrel, F; Motzkus, C; Ducourtieux, S; Delvallée, A; De Lagos, F; Nevé, S Le; Gutierrez, J; Lopez-Cuesta, J-M

2016-01-15

This work investigates the aerosols emitted during combustion of aircraft and naval structural composite materials (epoxy resin/carbon fibers and vinyl ester/glass fibers and carbon nanotubes). Combustion tests were performed at lab-scale using a modified cone calorimeter. The aerosols emitted have been characterized using various metrological devices devoted to the analysis of aerosols. The influence of the nature of polymer matrices, the incorporation of fibers and carbon nanotubes as well as glass reinforcements on the number concentration and the size distribution of airborne particles produced, was studied in the 5 nm-10 μm range. Incorporation of carbon fibers into epoxy resin significantly reduced the total particle number concentration. In addition, the interlaced orientation of carbon fibers limited the particles production compared to the composites with unidirectional one. The carbon nanotubes loading in vinyl ester resin composites influenced the total particles production during the flaming combustion with changes during kinetics emission. Predominant populations of airborne particles generated during combustion of all tested composites were characterized by a PN50 following by PN(100-500). Copyright © 2015 Elsevier B.V. All rights reserved.

Calibrations and Comparisons of Aerosol Spectrometers linking Ground and Airborne Measurements

NASA Astrophysics Data System (ADS)

Williamson, C.; Brock, C. A.; Erdesz, F.

2015-12-01

The nucleation-mode aerosol size spectrometer (NMASS), a fast-time response instrument measuring aerosol size distributions between 5 and 60nm, is to sample in the boundary layer and free troposphere on NASA's Atmospheric Tomography mission (ATom), providing contiguous data with global coverage in all four seasons. In preparation for this the NMASS is calibrated for the expected flight conditions and compatibility studies are made with ground-based instrumentation. The NMASS is comprised of 5 parallel condensation particle counters (CPCs) using perfluoro-tributylamine as a working fluid. Understanding the variation of CPC counting efficiencies with respect to the chemical composition of the sample is important for accurate data analysis and can be used to give indirect information about sample chemical composition. This variation is strongly dependent on the working fluid. The absolute responses and associated variations of the NMASS to ammonium sulfate and limonene ozonolysis products, compounds pertinent to the composition of particles nucleated in the free troposphere and boundary later, are compared to those of butanol, diethylene-glycol and water based CPCs, which are more commonly used in ground-based measurements. While fast time-response is key to measuring aerosol size distributions on flights, high size-resolution is often prioritized for ground-based measurements, and so a scanning mobility particle sizer (SMPS) is commonly used. Inter-comparison between NMASS and SMPS data is non-trivial because of the different working principles and resolutions of the instruments and yet it is vital, for example, for understanding the sources of particles observed during flights and the global relevance of phenomena observed from field stations and in chambers. We report compatibility studies on inversions of data from the SMPS and NMASS, evaluating temporal and spatial resolution and sources of uncertainty.

Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

NASA Astrophysics Data System (ADS)

Forestieri, Sara D.; Cornwell, Gavin C.; Helgestad, Taylor M.; Moore, Kathryn A.; Lee, Christopher; Novak, Gordon A.; Sultana, Camille M.; Wang, Xiaofei; Bertram, Timothy H.; Prather, Kimberly A.; Cappa, Christopher D.

2016-07-01

The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative

Nature, Origin, Potential Composition, and Climate Impact of the Asian Tropopause Aerosol Layer (ATAL)

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Thomason, L. W.; Natarajan, M.; Bedka, K.; Wienhold, F.; Bian J.; Martinsson, B.

2015-01-01

Satellite observations from SAGE II and CALIPSO indicate that summertime aerosol extinction has more than doubled in the Asian Tropopause Aerosol Layer (ATAL) since the late 1990s. Here we show remote and in-situ observations, together with results from a chemical transport model (CTM), to explore the likely composition, origin, and radiative forcing of the ATAL. We show in-situ balloon measurements of aerosol backscatter, which support the high levels observed by CALIPSO since 2006. We also show in situ measurements from aircraft, which indicate a predominant carbonaceous contribution to the ATAL (Carbon/Sulfur ratios of 2- 10), which is supported by the CTM results. We show that the peak in ATAL aerosol lags by 1 month the peak in CO from MLS, associated with deep convection over Asia during the summer monsoon. This suggests that secondary formation and growth of aerosols in the upper troposphere on monthly timescales make a significant contribution to ATAL. Back trajectory calculations initialized from CALIPSO observations provide evidence that deep convection over India is a significant source for ATAL through the vertical transport of pollution to the upper troposphere.

iSPEX: everybody can measure atmospheric aerosols with a smartphone spectropolarimeter

NASA Astrophysics Data System (ADS)

Snik, F.; Heikamp, S.; de Boer, J.; Keller, C. U.; van Harten, G.; Smit, J. M.; Rietjens, J. H. H.; Hasekamp, O.; Stam, D. M.; Volten, H.; iSPEX Team

2012-04-01

An increasing amount people carry a mobile phone with internet connection, camera and large computing power. iSPEX, a spectropolarimetric add-on with complementary app, instantly turns a smartphone into a scientific instrument to measure dust and other aerosols in our atmosphere. A measurement involves scanning the blue sky, which yields the angular behavior of the degree of linear polarization as a function of wavelength, which can unambiguously be interpreted in terms of size, shape and chemical composition of the aerosols in the sky directly above. The measurements are tagged with location and pointing information, and submitted to a central database where they will be interpreted and compiled into an aerosol map. Through crowdsourcing, many people will thus be able to contribute to a better assessment of health risks of particulate matter and of whether or not volcanic ash clouds are dangerous for air traffic. It can also contribute to the understanding of the relationship between atmospheric aerosols and climate change. We will give a live presentation of the first iSPEX prototype. Furthermore, we will present the design and the plans for producing the iSPEX add-on, app and website. We aim to distribute thousands of iSPEX units, such that a unique network of aerosol measurement equipment is created. Many people will thus contribute to the solution of several urgent social and scientific problems, and learn about the nature of light, remote sensing and the issues regarding atmospheric aerosols in the process. In particular we focus on school classes where smartphones are usually considered a nuisance, whereas now they can be a crucial part of various educational programs in science class.

The Global Aerosol Synthesis and Science Project (GASSP): Measurements and Modeling to Reduce Uncertainty

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

Reddington, C. L.; Carslaw, K. S.; Stier, P.

The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in situ measurements of the particle size distribution, number concentration, and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, tomore » create an extensive global dataset of aerosol in situ microphysical and chemical measurements, and to develop new ways to assess the uncertainty associated with comparing sparse point measurements with low-resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modelers and nonspecialist users. Available measurements are extensive, but they are biased to polluted regions of the Northern Hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model–data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.« less

The Global Aerosol Synthesis and Science Project (GASSP): Measurements and Modeling to Reduce Uncertainty

DOE PAGES

Reddington, C. L.; Carslaw, K. S.; Stier, P.; ...

2017-09-01

The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in situ measurements of the particle size distribution, number concentration, and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, tomore » create an extensive global dataset of aerosol in situ microphysical and chemical measurements, and to develop new ways to assess the uncertainty associated with comparing sparse point measurements with low-resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modelers and nonspecialist users. Available measurements are extensive, but they are biased to polluted regions of the Northern Hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model–data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.« less

On the competition among aerosol number, size and composition in predicting CCN variability: a multi-annual field study in an urbanized desert.

PubMed

Crosbie, E; Youn, J-S; Balch, B; Wonaschütz, A; Shingler, T; Wang, Z; Conant, W C; Betterton, E A; Sorooshian, A

2015-02-10

A 2-year data set of measured CCN (cloud condensation nuclei) concentrations at 0.2 % supersaturation is combined with aerosol size distribution and aerosol composition data to probe the effects of aerosol number concentrations, size distribution and composition on CCN patterns. Data were collected over a period of 2 years (2012-2014) in central Tucson, Arizona: a significant urban area surrounded by a sparsely populated desert. Average CCN concentrations are typically lowest in spring (233 cm -3 ), highest in winter (430 cm -3 ) and have a secondary peak during the North American monsoon season (July to September; 372 cm -3 ). There is significant variability outside of seasonal patterns, with extreme concentrations (1 and 99 % levels) ranging from 56 to 1945 cm -3 as measured during the winter, the season with highest variability. Modeled CCN concentrations based on fixed chemical composition achieve better closure in winter, with size and number alone able to predict 82% of the variance in CCN concentration. Changes in aerosol chemical composition are typically aligned with changes in size and aerosol number, such that hygroscopicity can be parameterized even though it is still variable. In summer, models based on fixed chemical composition explain at best only 41% (pre-monsoon) and 36% (monsoon) of the variance. This is attributed to the effects of secondary organic aerosol (SOA) production, the competition between new particle formation and condensational growth, the complex interaction of meteorology, regional and local emissions and multi-phase chemistry during the North American monsoon. Chemical composition is found to be an important factor for improving predictability in spring and on longer timescales in winter. Parameterized models typically exhibit improved predictive skill when there are strong relationships between CCN concentrations and the prevailing meteorology and dominant aerosol physicochemical processes, suggesting that similar findings could

Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

NASA Astrophysics Data System (ADS)

Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

2009-10-01

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ≍0.1-0.4 (0.16±0.06 arithmetic mean and standard deviation). The overall median value of κ≍0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (forg) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a negative linear correlation with forg (R2=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=κorg×forg +κinorg×finorg). The CCN number concentrations predicted with κp were in fair agreement with the measurement results (~20% average deviation). The median CCN number concentrations at S=0

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

Sources and composition of submicron organic mass in marine aerosol particles

DOE PAGES

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; ...

2014-11-27

Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

Sources and composition of submicron organic mass in marine aerosol particles

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

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.

Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

Aerosol algorithm evaluation within aerosol-CCI

NASA Astrophysics Data System (ADS)

Kinne, Stefan; Schulz, Michael; Griesfeller, Jan

Properties of aerosol retrievals from space are difficult. Even data from dedicated satellite sensors face contaminations which limit the accuracy of aerosol retrieval products. Issues are the identification of complete cloud-free scenes, the need to assume aerosol compositional features in an underdetermined solution space and the requirement to characterize the background at high accuracy. Usually the development of aerosol is a slow process, requiring continuous feedback from evaluations. To demonstrate maturity, these evaluations need to cover different regions and seasons and many different aerosol properties, because aerosol composition is quite diverse and highly variable in space and time, as atmospheric aerosol lifetimes are only a few days. Three years ago the ESA Climate Change Initiative started to support aerosol retrieval efforts in order to develop aerosol retrieval products for the climate community from underutilized ESA satellite sensors. The initial focus was on retrievals of AOD (a measure for the atmospheric column amount) and of Angstrom (a proxy for aerosol size) from the ATSR and MERIS sensors on ENVISAT. The goal was to offer retrieval products that are comparable or better in accuracy than commonly used NASA products of MODIS or MISR. Fortunately, accurate reference data of ground based sun-/sky-photometry networks exist. Thus, retrieval assessments could and were conducted independently by different evaluation groups. Here, results of these evaluations for the year 2008 are summarized. The capability of these newly developed retrievals is analyzed and quantified in scores. These scores allowed a ranking of competing efforts and also allow skill comparisons of these new retrievals against existing and commonly used retrievals.

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.

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.

All-year-round aerosol chemical composition at Dome C, Antarctica

NASA Astrophysics Data System (ADS)

Udisti, Roberto; Becagli, Silvia; Frosini, Daniele; Galli, Gaia; Ghedini, Costanza; Rugi, Francesco; Severi, Mirko; Traversi, Rita

2010-05-01

induced) controlling the MSA-H2SO4 ratio from DMS. Since, in summer, DMS in route toward central Antarctica is subjected to larger atmospheric concentrations of OH (and/or BrO) radical, lower temperatures and lower humidity, all conditions promoting the preferential H2SO4 formation, non-sea-salt sulphate is assumed to be the most reliable biogenic marker at Dome C. A further insight from ice-core stratigraphies is concerning the sea salt sodium (ssNa) content in snow precipitation as a reliable marker of sea-ice extent, via frost-flower formation at the pack-ice seasonal growth. This interpretation faces with the classical view that consider higher sea-spray production as caused by an increase in zonal wind intensity. Sea spray originated from frost flowers can be distinguished from sea spray coming from bulk sea-water by the lower sulphate/sodium ratio (caused by mirabilite - Na2SO4 10H20 - precipitation occurring when sea-ice temperature falls below -8°C). High resolution aerosol measurement can allow to identify different sea-spray sources and quantify frost flowers contribution to the annual ssNa budget. Finally, dust recorded in ice cores can be used as a valuable proxy for changes in hydrological cycles in the dust source areas and transport processes (pathways and scavenging). The geochemical characterization of dust in the present-day aerosol, compared with chemical composition of soils collected in South America and Australia, allows identifying the major dust source area (South America) and reconstructing pathways of atmospheric circulation. South America role in feeding dust aerosol at Dome C was supported also by comparing aerosol composition with satellite observations (dust plumes on the source sites) and back-trajectory analysis (air masses reaching Antarctica) during massive dust-storm events.

Predicting the Mineral Composition of Dust Aerosols. Part 2; Model Evaluation and Identification of Key Processes with Observations

NASA Technical Reports Server (NTRS)

Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

2015-01-01

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

Spatio-temporal aerosol particle distributions in the UT/LMS measured by the IAGOS-CARIBIC Observatory

NASA Astrophysics Data System (ADS)

Assmann, D. N.; Hermann, M.; Weigelt, A.; Martinsson, B. G.; Brenninkmeijer, C. A. M.; Rauthe-Schoech, A.; van Velthoven, P. J. F.; Boenisch, H.; Zahn, A.

2016-12-01

Submicrometer aerosol particles in the upper troposphere and lowermost stratosphere (UT/LMS) influence the Earth`s radiation budget directly and, more important, indirectly, by acting as cloud condensation nuclei and by changing trace gas concentrations through heterogeneous chemical processes. Since 1997, regular in situ UT/LMS aerosol particle measurements have been conducted by the Leibniz Institute for Tropospheric Research, Leipzig, Germany and the University of Lund, Sweden, using the the CARIBIC (now IAGOS-CARIBIC) observatory (www.caribic-atmospheric.com) onboard a passenger aircraft. Submicrometer aerosol particle number concentrations and the aerosol particle size distribution are measured using three condensation particle counters and one optical particle size spectrometer. Moreover, particle elemental composition is determined using an aerosol impactor sampler and post-flight ion beam analysis (PIXE, PESA) of the samples in the laboratory. Based on this unique data set, including meteorological analysis, we present representative spatio-temporal distributions of particle number, surface, volume, and elemental concentrations in an altitude of 8-12 km covering a large fraction of the northern hemisphere. We discuss the measured values in the different size regimes with respect to sources and sinks in different regions. Additionally, we calculated highly resolved latitudinal and longitudinal cross sections of the particle number size distribution, probability density functions and trends in particle number concentrations, but also in elemental composition, determined from our regular measurements over more than a decade. Moreover, we present the seasonality of particle number concentration in an equivelent latitude - potential temperature coordinate framework (see figure). The results are interpreted with respect to aerosol microphysics and transport using CARIBIC trace gas data like ozone and water vapour. The influence of clouds in the troposphere and

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.

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

NASA Technical Reports Server (NTRS)

Weber, Rodney J.

2004-01-01

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

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.

MAESTRO Measurements of Atmospheric Aerosol

NASA Astrophysics Data System (ADS)

McElroy, Tom; Drummond, James; Zou, Jason

2014-05-01

MAESTRO (Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) is now in its 11th year on orbit as part of the Atmospheric Chemistry Experiment on the Canadian Space Agency's SCISAT satellite. MAESTRO data analysis has been dogged by a deficiency in accurate timing between the measurements made by the partner instrument, the ACE-FTS (Atmospheric Chemistry Experiment, Fourier Transform Spectrometer), that provides the atmospheric pressure-temperature profile and observation tangent altitudes used in the MAESTRO data analysis. Attempts have been made to use apparent air column density and oxygen A-band absorption as a mechanism to line up the tangent heights, but to no avail. A new product is now being produced, based on matching the modeled ozone slant columns from the ACE-FTS retrievals with the MAESTRO slant column measurements. The approach is very promising and indicates that a valuable product from the MAESTRO wavelength-dependent aerosol extinction likely result. The usefulness of the profile matching technique will be demonstrated and some aerosol absorption profiles will be presented in comparison with measurements made by the ACE Imager aerosol profile results. While the process optimizes the comparison between ACE-FTS ozone profile data and that from MAESTRO, it does not detract from the higher vertical resolution information provided by MAESTRO.

Systematic Relationships Between Lidar Observables and Sizes And Mineral Composition Of Dust Aerosols

NASA Technical Reports Server (NTRS)

Van Diedenhoven, Bastiaan; Stangl, Alexander; Perlwitz, Jan; Fridlind, Ann M.; Chowdhary, Jacek; Cairns, Brian

2015-01-01

The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

Characteristics and Composition of Atmospheric Aerosols in Phimai, Central Thailand During BASE-ASIA

NASA Technical Reports Server (NTRS)

Li, Can; Tsay, Si-Chee; Hsu, N. Christina; Kim, Jin Young; Howell, Steven G.; Huebert, Barry J.; Ji, Qiang; Jeong, Myeong-Jae; Wang, Sheng-Hsiang; Hansell, Richard A.;

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

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

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

2011-05-11

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

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

NASA Astrophysics Data System (ADS)

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

2011-05-01

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

Composition and spectral characteristics of ambient aerosol at Mauna Loa Observatory

NASA Technical Reports Server (NTRS)

Johnson, Stanley A.; Kumar, Romesh

1991-01-01

The spectral and the chemical characteristics of ambient aerosol at Mauna Loa Observatory (Hawaii) were determined in aerosol particles continuously sampled during an 8-day period in August 1986. During this period, the chemical species in the ambient aerosol varied considerably. During the major fraction of the sampling period, the aerosol was acidic due to predominance of (NH4)3H(SO4)2, NH4HSO4, or H2SO4. Aerosol samples showed much higher absorbance at 9.1 microns than at 10.6 microns. Moreover, changes in chemical composition from the neutral (NH4)2SO4 aerosol to more acidic sulphate forms were accompanied by substantial changes in the samples' absorbance at 9.1 microns (with lesser changes in the 10.6-micron absorptions).

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

Aerosol composition and sources in the Central Arctic Ocean during ASCOS

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Leck, C.; Graus, M.; Müller, M.; Paatero, J.; Burkhart, J. F.; Stohl, A.; Orr, L. H.; Hayden, K.; Li, S.-M.; Hansel, A.; Tjernström, M.; Leaitch, W. R.; Abbatt, J. P. D.

2011-05-01

Measurements of submicron aerosol chemical composition were made in the Central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.042 and 0.046 μg m-3, respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33 % and 36 % of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47 % of the sulphate apportioned to marine biogenic sources and 48 % to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25 ± 0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it was more processed and had been present longer in the atmosphere than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources.

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

Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

NASA Technical Reports Server (NTRS)

Gorzelska, K.; Talbot, R. W.; Klemm, K.; Lefer, B.; Klemm, O.; Gregory, G. L.; Anderson, B.; Barrie, L. A.

1994-01-01

Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

Long-term Aerosol Lidar Measurements At CNR-IMAA

NASA Astrophysics Data System (ADS)

Mona, L.; Amodeo, A.; D'Amico, G.; Pandolfi, M.; Pappalardo, G.

2006-12-01

Actual estimations of the aerosol effect on the radiation budget are affected by a large uncertainties mainly due to the high inhomogeneity and variability of atmospheric aerosol, in terms of concentration, shape, size distribution, refractive index and vertical distribution. Long-term measurements of vertical profiles of aerosol optical properties are needed to reduce these uncertainties. At CNR-IMAA (40° 36'N, 15° 44' E, 760 m above sea level), a lidar system for aerosol study is operative since May 2000 in the framework of EARLINET (European Aerosol Research Lidar Network). Until August 2005, it provided independent measurements of aerosol extinction and backscatter at 355 nm and aerosol backscatter profiles at 532 nm. After an upgrade of the system, it provides independent measurements of aerosol extinction and backscatter profiles at 355 and 532 nm, and of aerosol backscatter profiles at 1064 nm and depolarization ratio at 532 nm. For these measurements, lidar ratio at 355 and 532 nm and Angstrom exponent profiles at 355/532 nm are also obtained. Starting on May 2000, systematic measurements are performed three times per week according to the EARLINET schedule and further measurements are performed in order to investigate particular events, like dust intrusions, volcanic eruptions and forest fires. A climatological study has been carried out in terms of the seasonal behavior of the PBL height and of the aerosol optical properties calculated inside the PBL itself. In the free troposphere, an high occurrences of Saharan dust intrusions (about 1 day of Saharan dust intrusion every 10 days) has been observed at CNR-IMAA because of the short distance from the Sahara region. During 6 years of observations, very peculiar cases of volcanic aerosol emitted by Etna volcano and aerosol released by large forest fires burning occurred in Alaska and Canada have been observed in the free troposphere at our site. Particular attention is devoted to lidar ratio both for the

Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Gitelson, A.; Karnieli, A.; Ganor, E. (Editor); Fraser, R. S.; Nakajima, T.; Mattoo, S.; Holben, B. N.

1994-01-01

Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate

Monitoring and tracking the trans-Pacific transport of aerosols using multi-satellite aerosol optical depth composites

NASA Astrophysics Data System (ADS)

Naeger, Aaron R.; Gupta, Pawan; Zavodsky, Bradley T.; McGrath, Kevin M.

2016-06-01

The primary goal of this study was to generate a near-real time (NRT) aerosol optical depth (AOD) product capable of providing a comprehensive understanding of the aerosol spatial distribution over the Pacific Ocean, in order to better monitor and track the trans-Pacific transport of aerosols. Therefore, we developed a NRT product that takes advantage of observations from both low-earth orbiting and geostationary satellites. In particular, we utilize AOD products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Suomi National Polar-orbiting Partnership (NPP) Visible Infrared Imaging Radiometer Suite (VIIRS) satellites. Then, we combine these AOD products with our own retrieval algorithms developed for the NOAA Geostationary Operational Environmental Satellite (GOES-15) and Japan Meteorological Agency (JMA) Multi-functional Transport Satellite (MTSAT-2) to generate a NRT daily AOD composite product. We present examples of the daily AOD composite product for a case study of trans-Pacific transport of Asian pollution and dust aerosols in mid-March 2014. Overall, the new product successfully tracks this aerosol plume during its trans-Pacific transport to the west coast of North America as the frequent geostationary observations lead to a greater coverage of cloud-free AOD retrievals equatorward of about 35° N, while the polar-orbiting satellites provide a greater coverage of AOD poleward of 35° N. However, we note several areas across the domain of interest from Asia to North America where the GOES-15 and MTSAT-2 retrieval algorithms can introduce significant uncertainties into the new product.

Sources and composition of submicron organic mass in marine aerosol particles

NASA Astrophysics Data System (ADS)

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

2014-11-01

The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of

Tying Biological Activity to Changes in Sea Spray Aerosol Chemical Composition via Single Particle Analyses

NASA Astrophysics Data System (ADS)

Sultana, C. M.; Lee, C.; Collins, D. B.; Axson, J. L.; Laskina, O.; Grandquist, J. R.; Grassian, V. H.; Prather, K. A.

2014-12-01

In remote marine environments, sea spray aerosols (SSA) often represent the greatest aerosol burden, thus having significant impacts on direct radiative interactions and cloud processes. Previous studies have shown that SSA is a complex mixture of inorganic salts and an array of dissolved and particulate organic components. Enrichment of SSA organic content is often correlated to seawater chlorophyll concentrations, a measure of oceanic biological activity. As the physical and chemical properties of aerosols control their radiative effects, recent studies conducted by the Center for Aerosol Impacts on Climate and the Environment have endeavored to further elucidate the ties between marine biological activity and primary SSA chemical composition using highly time resolved single particle analyses. A series of experiments performed in the recently developed Marine Aerosol Reference Tank evaluated the effect of changing marine microbial populations on SSA chemical composition, which was monitored via an aerosol time-of-flight mass spectrometer and a variety of offline spectroscopic and microscopic techniques. Each experiment was initiated using unfiltered and untreated seawater, thus maintaining a high level of biogeochemical complexity. This study is the first of its kind to capture daily changes in the primary SSA mixing state over the growth and death of a natural phytoplankton bloom. Increases in organic aerosol types (0.4-3 μm), internally and externally mixed with sea salt, could not be correlated to chlorophyll concentrations. Maximum production of these populations occurred two to four days after the in vivo chlorophyll fluorescence peaked in intensity. This work is in contrast to the current paradigm of correlating SSA organic content to seawater chlorophyll concentration.

Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

NASA Astrophysics Data System (ADS)

May, A. A.; McMeeking, G. R.; Lee, T.; Taylor, J. W.; Craven, J. S.; Burling, I.; Sullivan, A. P.; Akagi, S.; Collett, J. L.; Flynn, M.; Coe, H.; Urbanski, S. P.; Seinfeld, J. H.; Yokelson, R. J.; Kreidenweis, S. M.

2014-10-01

Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California; coastal plain ecosystem in South Carolina) and from open burning of over 15 individual plant species in the laboratory. We report emission ratios and emission factors for refractory black carbon (rBC) and submicron nonrefractory aerosol and compare field and laboratory measurements to assess the representativeness of our laboratory-measured emissions. Laboratory measurements of organic aerosol (OA) emission factors for some fires were an order of magnitude higher than those derived from any of our aircraft observations; these are likely due to higher-fuel moisture contents, lower modified combustion efficiencies, and less dilution compared to field studies. Nonrefractory inorganic aerosol emissions depended more strongly on fuel type and fuel composition than on combustion conditions. Laboratory and field measurements for rBC were in good agreement when differences in modified combustion efficiency were considered; however, rBC emission factors measured both from aircraft and in the laboratory during the present study using the Single Particle Soot Photometer were generally higher than values previously reported in the literature, which have been based largely on filter measurements. Although natural variability may account for some of these differences, an increase in the BC emission factors incorporated within emission inventories may be required, pending additional field measurements for a wider variety of fires.

Aerosol volatility in a boreal forest environment

NASA Astrophysics Data System (ADS)

Häkkinen, S. A. K.; ńijälä, M.; Lehtipalo, K.; Junninen, H.; Virkkula, A.; Worsnop, D. R.; Kulmala, M.; Petäjä, T.; Riipinen, I.

2012-04-01

Climate and health effects of atmospheric aerosols are determined by their properties such as their chemical composition. Aerosol chemical composition can be studied indirectly by measuring volatility of aerosol particles. The volatility of submicron aerosol particles (20-500 nm) was studied in a boreal forest site at SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations II) station (Vesala et al., 1998) in Hyytiälä, Finland, during 01/2008-05/2010. The instrument used for the measurements was VDMPS (Volatility Differential Mobility Particle Sizer), which consists of two separate instruments: DMPS (Differential Mobility Particle Sizer, Aalto et al., 2001) and TD (Thermodenuder, Wehner et al., 2002). Aerosol evaporation was examined by heating the aerosol and comparing the total aerosol mass before and after heating. In the VDMPS system ambient aerosol sample was heated up to temperatures ranging from 80 °C to 280 °C. The higher the heating temperature was the more aerosol material was evaporated. There was a non-volatile residual present in aerosol particles when heated up to 280 °C. This residual explained (20±8)% of the total aerosol mass. Aerosol non-volatile mass fraction was highest during winter and smallest during summer months. The role of black carbon in the observed non-volatile residual was determined. Black carbon explained 40 to 90% of the non-volatile mass. Especially during colder seasons noticeable amount of non-volatile material, something else than black carbon, was observed. According to Kalberer et al. (2004) some atmospheric organic species can form polymers that have high evaporation temperatures. Also low-volatile organic salts may contribute to the non-volatile aerosol (Smith et al., 2010). Aerosol mass composition measured directly with AMS (Aerosol Mass Spectrometer, Jayne et al., 2000) was analyzed in order to examine the properties of the non-volatile material (other than black carbon). The AMS measurements were performed

Aircraft-borne aerosol chemical composition measurements in the lower to middle troposphere over southern West Africa: Biomass burning, urban outflow plumes, and long-range transport.

NASA Astrophysics Data System (ADS)

Batenburg, Anneke; Schulz, Christiane; Schneider, Johannes; Sauer, Daniel; Schlager, Hans; Borrmann, Stephan

2017-04-01

During the DACCIWA field campaign in June and July 2016, aircraft-borne in-situ aerosol chemical composition measurements were performed over southern West Africa (SWA). This presentation will focus on the submicron particle measurements done with a Compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) on board of the DLR Falcon aircraft during twelve research flights from Lomé, Togo, covering the altitude range from the boundary layer (BL) to the middle troposphere (12 km). A preliminary analysis of the results shows typical baseline total non-refractory aerosol mass loadings of 1.5 to 2.8 μg m-3 in the BL, and 0.4 to 1.1 μg m-3above. Up to half of the baseline aerosol mass in the BL appears to consist of sulphate, compared to only 10 to 35 % above the BL; organic matter dominates in the middle troposphere. During several flights, the DLR Falcon crossed a pronounced and seemingly widespread aerosol layer at 2—4.5 km altitude, partly in or slightly above the BL. The AMS data indicate that about half of the non-refractory aerosol mass in the middle of this layer consisted of organic matter. We consider it likely that these aerosol particles were produced by biomass burning in Central Africa. Emissions from cities and industrial areas were also intercepted, as well as enhancements in some species at higher altitudes. Trajectory analysis suggests that an increase of the organics to more than 2.5 μg m-3 observed at 8 km during one flight came from the Arabian Peninsula. Several ammonium peaks during the same flight at higher altitudes were traced back to the Asian Summer Monsoon Anticyclone (ASMA).

Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Metcalf, A. R.; Dutcher, C. S.

2014-12-01

Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

LASE measurements of aerosols and water vapor during TARFOX

NASA Technical Reports Server (NTRS)

Ferrare, Richard A.; Ismail, Syed; Browell, Edward V.; Brackett, Vincent G.; Kooi, Susan A.; Clayton, Marian B.; Melfi, Harvey; Whiteman, David N.; Schwenner, Geary; Evans, Keith D.;

Boundary Layer Aerosol Composition over Sierra Nevada Mountains using 9.11- and 10.59-micron CW Lidars and Modeled Backscatter from Size Distribution Data

NASA Technical Reports Server (NTRS)

Cutten, D. R.; Jarzembski, M. A.; Srivastava, V.; Pueschel, R. F.; Howard, S. D.; McCaul, E. W., Jr.

2003-01-01

An inversion technique has been developed to determine volume fractions of an atmospheric aerosol composed primarily of ammonium sulfate and ammonium nitrate and water combined with fixed concentration of elemental and organic carbon. It is based on measured aerosol backscatter obtained with 9.11 - and 10.59-micron wavelength continuous wave CO2 lidars and modeled backscatter from aerosol size distribution data. The technique is demonstrated during a flight of the NASA DC-8 aircraft over the Sierra Nevada Mountain Range, California on 19 September, 1995. Volume fraction of each component and effective complex refractive index of the composite particle were determined assuming an internally mixed composite aerosol model. The volume fractions were also used to re-compute aerosol backscatter, providing good agreement with the lidar-measured data. The robustness of the technique for determining volume fractions was extended with a comparison of calculated 2.1,-micron backscatter from size distribution data with the measured lidar data converted to 2.1,-micron backscatter using an earlier derived algorithm, verifying the algorithm as well as the backscatter calculations.

Airborne Sunphotometer Studies of Aerosol Properties and Effects, Including Closure Among Satellite, Suborbital Remote, and In situ Measurements

NASA Technical Reports Server (NTRS)

Russlee, Philip B.; Schmid, B.; Redemann, J.; Livingston, J. M.; Bergstrom, R. W.; Ramirez, S. A.; Hipskind, R. Stephen (Technical Monitor)

2001-01-01

Airborne sunphotometry has been used to measure aerosols from North America, Europe, and Africa in coordination with satellite and in situ measurements in TARFOX (1996), ACE-2 (1997), PRIDE (2000), and SAFARI 2000. Similar coordinated measurements of Asian aerosols are being conducted this spring in ACE-Asia and are planned for North American aerosols this summer in CLAMS. This paper summarizes the approaches used, key results, and implications for aerosol properties and effects, such as single scattering albedo and regional radiative forcing. The approaches exploit the three-dimensional mobility of airborne sunphotometry to access satellite scenes over diverse surfaces (including open ocean with and without sunglint) and to match exactly the atmospheric layers sampled by airborne in situ measurements and other radiometers. These measurements permit tests of the consistency, or closure, among such diverse measurements as aerosol size-resolved chemical composition; number or mass concentration; light extinction, absorption, and scattering (total, hemispheric back and 180 deg.); and radiative fluxes. In this way the airborne sunphotometer measurements provide a key link between satellite and in situ measurements that helps to understand any discrepancies that are found. These comparisons have led to several characteristic results. Typically these include: (1) Better agreement among different types of remote measurements than between remote and in situ measurements. (2) More extinction derived from transmission measurements than from in situ measurements. (3) Larger aerosol absorption inferred from flux radiometry than from in situ measurements. Aerosol intensive properties derived from these closure studies have been combined with satellite-retrieved fields of optical depth to produce fields of regional radiative forcing. We show results for the North Atlantic derived from AVHRR optical depths and aerosol intensive properties from TARFOX and ACE-2. Companion papers

Satellite stratospheric aerosol measurement validation

NASA Technical Reports Server (NTRS)

Russell, P. B.; Mccormick, M. P.

1984-01-01

The validity of the stratospheric aerosol measurements made by the satellite sensors SAM II and SAGE was tested by comparing their results with each other and with results obtained by other techniques (lider, dustsonde, filter, and impactor). The latter type of comparison required the development of special techniques that convert the quantity measured by the correlative sensor (e.g. particle backscatter, number, or mass) to that measured by the satellite sensor (extinction) and quantitatively estimate the uncertainty in the conversion process. The results of both types of comparisons show agreement within the measurement and conversion uncertainties. Moreover, the satellite uncertainty is small compared to aerosol natural variability (caused by seasonal changes, volcanoes, sudden warmings, and vortex structure). It was concluded that the satellite measurements are valid.

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

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.

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements: Evaluation of Aerosol Measurements from SAGE II, HALOE, and Balloonborne Optical Particle Counters

NASA Technical Reports Server (NTRS)

Hervig, Mark; Deshler, Terry; Moddrea, G. (Technical Monitor)

2002-01-01

Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.

Aerosol carbon isotope composition over Baltic Sea

NASA Astrophysics Data System (ADS)

Garbaras, Andrius; Pabedinskas, Algirdas; Masalaite, Agne; Petelski, Tomasz; Gorokhova, Elena; Sapolaite, Justina; Ezerinskis, Zilvinas; Remeikis, Vidmantas

2017-04-01

Particulate carbonaceous matter is significant contributor to ambient particulate matter originating from intervening sources which contribution is difficult to quantify due to source diversity, chemical complexity and processes during atmospheric transport. Carbon isotope analysis can be extremely useful in source apportionment of organic matter due to the unique isotopic signatures associated with anthropocentric (fossil fuel), continental (terrestrial plants) and marine sources, and is particularly effective when these sources are mixed (Ceburnis et al., 2011;Ceburnis et al., 2016). We will present the isotope ratio measurement results of aerosol collected during the cruise in the Baltic Sea. Sampling campaign of PM10 and size segregated aerosol particles was performed on the R/V "Oceania" in October 2015. Air mass back trajectories were prevailing both from the continental and marine areas during the sampling period. The total carbon concentration varied from 1 µg/m3 to 8 µg/m3. Two end members (δ13C = -25‰ and δ13C = -28 ‰ ) were established from the total stable carbon isotope analysis in PM10 fraction. δ13C analysis in size segregated aerosol particles revealed δ13C values being highest in the 1 - 2.5 µm range (δ13C = -24.9 ‰ ) during continental transport, while lowest TC δ13C values (δ13C ≈ -27 ‰ ) were detected in the size range D50 <1 µm during stormy weather when air mass trajectory prevailed from the western direction. These measurements revealed that simplified isotope mixing model can not be applied for the aerosol source apportionment (Masalaite et al., 2015) in the perturbed marine environment. Additionally, concentration of bacteria and fungi were measured in size segregated and PM10 aerosol fraction. We were able to relate aerosol source δ13C end members with the abundance of bacteria and fungi over Baltic Sea combining air mass trajectories, stable isotope data, fungi and bacteria concentrations. Ceburnis, D., Garbaras, A

Phase Partitioning of Soluble Trace Gases with Size-Resolved Aerosols during the Nitrogen, Aerosol Composition, and Halogens on a Tall Tower (NACHTT) Campaign

NASA Astrophysics Data System (ADS)

Young, A.; Keene, W. C.; Pszenny, A.; Sander, R.; Maben, J. R.; Warrick-Wriston, C.; Bearekman, R.

2011-12-01

During February and March 2011, size-resolved and bulk aerosol were sampled at 22 m above the surface over nominal 12-hour (daytime and nighttime) intervals from the Boulder Atmospheric Observatory tower (40.05 N, 105.01 W, 1584-m elevation). Samples were analyzed for major organic and inorganic ionic constituents by high performance ion chromatography (IC). Soluble trace gases (HCl, HNO3, NH3, HCOOH, and CH3COOH) were sampled in parallel over 2-hour intervals with tandem mist chambers and analyzed on site by IC. NH4+, NO3-, and SO42- were the major ionic components of aerosols (median values of 57.7, 34.5, and 7.3 nmol m-3 at STP, respectively, N = 45) with 86%, 82%, and 82%, respectively, associated with sub-μm size fractions. Cl- and Na+ were present at significant concentrations (median values of 6.8 and 6.6 nmol m-3, respectively) but were associated primarily with super-μm size fractions (75% and 78%, respectively). Median values (and ranges) for HCl, HNO3, and NH3 were 21 (<20-1257), 120 (<45-1638), and 5259 (<1432-48,583) pptv, respectively. Liquid water contents of size-resolved aerosols and activity coefficients for major ionic constituents were calculated with the Extended Aerosol Inorganic Model II and IV (E-AIM) based on the measured aerosol composition, RH, temperature, and pressure. Size-resolved aerosol pHs were inferred from the measured phase partitioning of HCl, HNO3, and NH3. Major controls of phase partitioning and associated chemical dynamics will be presented.

Characterization of aerosol composition and sources in the greater Atlanta area by aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Ng, N. L.; Xu, L.; Suresh, S.; Weber, R. J. J.; Baumann, K.; Edgerton, E. S.

2014-12-01

An important and uncertain aspect of biogenic secondary organic aerosol (SOA) formation is that it is often associated with anthropogenic pollution tracers. Prior studies in Atlanta suggested that 70-80% of the carbon in water-soluble organic carbon (WSOC) is modern, yet it is well-correlated with the anthropogenic CO. In this study, we deployed a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) at multiple sites in different seasons (May 2012-February 2013) to characterize the sources and chemical composition of aerosols in the greater Atlanta area. This area in the SE US is ideal to investigate anthropogenic-biogenic interactions due to high natural and anthropogenic emissions. These extensive field studies are part of the Southeastern Center for Air Pollution and Epidemiology study (SCAPE). The HR-ToF-AMS is deployed at four sites (~ 3 weeks each) in rotation: Jefferson Street (urban), Yorkville (rural), roadside site (near Highway 75/85), and Georgia Tech site (campus), with the urban and rural sites being part of the SEARCH network. We obtained seven HR-ToF-AMS datasets in total. During the entire measurement period, the ACSM is stationary at the GIT site and samples continuously. We perform positive matrix factorization (PMF) analysis on the HR-ToF-AMS and ACSM data to deconvolve the OA into different components. While the diurnal cycle of the total OA is flat as what have been previously observed, the OA factors resolved by PMF analysis show distinctively different diurnal trends. We find that the "more-oxidized oxygenated OA" (MO-OOA) constitutes a major fraction of OA at all sites. In summer, OA is dominated by SOA, e.g., isoprene-OA and OOA with different degrees of oxidation. In contrary, biomass burning OA is more prominent in winter data. By comparing HR-ToF-AMS and ACSM data during the same sampling periods, we find that the aerosol time series are highly correlated, indicating the

Aerosol counterflow two-jets unit for continuous measurement of the soluble fraction of atmospheric aerosols.

PubMed

Mikuska, Pavel; Vecera, Zbynek

2005-09-01

A new type of aerosol collector employing a liquid at laboratory temperature for continuous sampling of atmospheric particles is described. The collector operates on the principle of a Venturi scrubber. Sampled air flows at high linear velocity through two Venturi nozzles "atomizing" the liquid to form two jets of a polydisperse aerosol of fine droplets situated against each other. Counterflow jets of droplets collide, and within this process, the aerosol particles are captured into dispersed liquid. Under optimum conditions (air flow rate of 5 L/min and water flow rate of 2 mL/min), aerosol particles down to 0.3 microm in diameter are quantitatively collected in the collector into deionized water while the collection efficiency of smaller particles decreases. There is very little loss of fine aerosol within the aerosol counterflow two-jets unit (ACTJU). Coupling of the aerosol collector with an annular diffusion denuder located upstream of the collector ensures an artifact-free sampling of atmospheric aerosols. Operation of the ACTJU in combination with on-line detection devices allows in situ automated analysis of water-soluble aerosol species (e.g., NO2-, NO3-)with high time resolution (as high as 1 s). Under the optimum conditions, the limit of detection for particulate nitrite and nitrate is 28 and 77 ng/m(3), respectively. The instrument is sufficiently rugged for its application at routine monitoring of aerosol composition in the real time.

Size-resolved chemical composition of aerosol emitted by Erebus volcano, Antarctica

NASA Astrophysics Data System (ADS)

Ilyinskaya, E.; Oppenheimer, C.; Mather, T. A.; Martin, R. S.; Kyle, P. R.

2010-03-01

Persistent, open-vent degassing of Erebus volcano, Antarctica, is a significant point source of gases and aerosol to the austral polar troposphere. We report here on the chemical composition and size distribution of the Erebus aerosol, focusing on the water-soluble fraction. The aerosol was sampled at the rim of the active crater using a cascade impactor, which collected and sized particles in 14 size bins from >10 to 0.01 μm. The soluble fraction of the Erebus aerosol is distinct from other volcanic sources in several respects. It is dominated by chloride-bearing particles (over 30% of total mass) and has an unusually high Cl-/SO42- molar ratio of 3.5. Coarse particles contribute little to the total mass of the soluble fraction. Elevated concentrations of F-, Cl-, Br-, and SO42- are found in a narrow particle size fraction of 0.1-0.25 μm. The detection of particulate Br- reinforces our understanding of the potential for quiescent volcanic emissions to deplete tropospheric ozone. The small aerosol size reflects the low atmospheric temperature and humidity, which inhibit particle growth. Halide-alkali metal salts (Na, K)(Cl, F) appear to be the most abundant species in the aerosol. The concentration of Pb is high compared to other volcanoes; its exsolution may be promoted by the high abundance of halogens in Erebus magma. Despite the previously reported high NOx content in the plume, we did not detect significant quantities of nitrate in the near-vent aerosol. Our findings emphasize the potential regional significance of emissions from Erebus for understanding the Antarctic atmospheric composition and glaciochemical records.

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

NASA Astrophysics Data System (ADS)

Trivitayanurak, W.; Palmer, P. I.; Barkley, M. P.; Robinson, N. H.; Coe, H.; Oram, D. E.

2012-01-01

We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands) was a net exporter of primary organic aerosol (42 kT) and black carbon aerosol (11 kT). We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA), with Borneo being a net exporter of SOA (15 kT). SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%), with smaller contributions from gas-phase oxidation (15%) and advection into the regions (14%). We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD) data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where the model

Chemical Composition and Oxidation State of Iron-Containing Aerosol Particles Over West Antarctic Peninsula

NASA Astrophysics Data System (ADS)

Fan, S.; Yu, S.; Lai, B.; Gao, Y.

2017-12-01

Iron is a limiting micronutrient element critical for the marine ecosystem. In the extensive high-nutrient low-chlorophyll (HNLC) regions of the Southern Ocean, the activities of phytoplankton are partly controlled by iron (Fe) from different sources, including atmospheric deposition. Among important properties of atmospheric Fe are the elemental composition and Fe oxidation state of Fe-containing aerosol particles, as these properties affect aerosol Fe solubility. To explore these issues, aerosol samples were collected at Palmer Station in West Antarctic Peninsula. Samples were analyzed by submicron synchrotron-based X-ray fluorescence (XRF) and X-ray absorption near edge structure (XANES) spectroscopy for the Fe oxidation state and elemental composition of aerosol particles. The morphological information of aerosol particles was also observed by the high-resolution fluorescence microscopy, revealing possible sources and formation processes of iron-containing particles. More detailed results will be discussed in this presentation.

Influence of aqueous chemistry on the chemical composition of fog water and interstitial aerosol in Fresno

NASA Astrophysics Data System (ADS)

Kim, Hwajin; Ge, Xinlei; Collier, Sonya; Xu, Jianzhong; Sun, Yele; Wang, Youliang; Herckes, Pierre; Zhang, Qi

2015-04-01

A measurement study was conducted in the Central Valley (Fresno) of California in January 2010, during which radiation fog events were frequently observed. Fog plays important roles in atmospheric chemistry by scavenging aerosol particles and trace gases and serving as a medium for various aqueous-phase reactions. Understanding the effects of fog on the microphysical and chemical processing of aerosol particles requires detailed information on their chemical composition. In this study, we characterized the chemical composition of fog water and interstitial aerosol particles to study the effects of fog processing on aerosol properties. Fog water samples were collected during the 2010 Fresno campaigns with a Caltech Active Strand Cloud water Collector (CASCC) while interstitial submicron aerosols were characterized in real time with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and a scanning Mobility Particle Sizer (SMPS). The fog water samples were later analyzed using the HR-ToF-AMS, ion chromatography, and a total carbon analyzer. The chemical composition and characteristics of interstitial particles during the fog events were compared to those of dissolved inorganic and organic matter in fog waters. Compared to interstitial aerosols, fog water is composed of a higher fraction of ammonium nitrate and oxygenated organics, due to aqueous formation of secondary aerosol species as well as enhanced gas-to-particle partitioning of water soluble species under water rich conditions. Sulfate is formed most efficiently in fog water although its contribution to total dissolved mass is relatively low. The HR-ToF-AMS mass spectra of organic matter in fog water (FOM) are very similar to that of oxygenated organic aerosols (OOA) derived from positive matrix factorization (PMF) of the HR-ToF-AMS spectra of ambient aerosol (r2 = 0.96), but FOM appears to contain a large fraction of acidic functional groups than OOA. FOM is also enriched of

Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

NASA Astrophysics Data System (ADS)

Wollny, A. G.; Garland, R.; Pöschl, U.

2009-04-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

Chemical composition of aerosol particles and light extinction apportionment before and during the heating season in Beijing, China

NASA Astrophysics Data System (ADS)

Wang, Qingqing; Sun, Yele; Jiang, Qi; Du, Wei; Sun, Chengzhu; Fu, Pingqing; Wang, Zifa

2015-12-01

Despite extensive efforts into characterization of the sources and formation mechanisms of severe haze pollution in the megacity of Beijing, the response of aerosol composition and optical properties to coal combustion emissions in the heating season remain poorly understood. Here we conducted a 3 month real-time measurement of submicron aerosol (PM1) composition by an Aerosol Chemical Speciation Monitor and particle light extinction by a Cavity Attenuated Phase Shift extinction monitor in Beijing, China, from 1 October to 31 December 2012. The average (±σ) PM1 concentration was 82.4 (±73.1) µg/m3 during the heating period (HP, 15 November to 31 December), which was nearly 50% higher than that before HP (1 October to 14 November). While nitrate and secondary organic aerosol (SOA) showed relatively small changes, organics, sulfate, and chloride were observed to have significant increases during HP, indicating the dominant impacts of coal combustion sources on these three species. The relative humidity-dependent composition further illustrated an important role of aqueous-phase processing for the sulfate enhancement during HP. We also observed great increases of hydrocarbon-like OA (HOA) and coal combustion OA (CCOA) during HP, which was attributed to higher emissions at lower temperatures and coal combustion emissions, respectively. The relationship between light extinction and chemical composition was investigated using a multiple linear regression model. Our results showed that the largest contributors to particle extinction were ammonium nitrate (32%) and ammonium sulfate (28%) before and during HP, respectively. In addition, the contributions of SOA and primary OA to particle light extinction were quantified. The results showed that the OA extinction was mainly caused by SOA before HP and by SOA and CCOA during HP, yet with small contributions from HOA and cooking aerosol for the entire study period. Our results elucidate substantial changes of aerosol

The chemical composition of cirrus forming aerosol: Lessons from the MACPEX field study

NASA Astrophysics Data System (ADS)

Cziczo, D. J.; Froyd, K. D.; Murphy, D. M.

2012-12-01

Cirrus clouds are an important factor in the Earth's climate system. These clouds exert a large radiative forcing due to their extensive global coverage and high altitude despite minimal physical and optical thickness. During the Mid-latitude Aerosol and Cloud Properties EXperiment (MACPEX) we measured chemical and physical properties of the aerosols on which cirrus ice crystals formed in situ and in real time using a laser ablation single particle mass spectrometry technique deployed aboard the NASA WB-57 research aircraft. Ice residual particles were also collected for off-line laboratory investigation including electron microscopy. Flights spanned from the Gulf of Mexico to the mid-latitudes over the United States. In most cases heterogeneous freezing was the inferred mechanism of cloud formation and aerosol composition had a significant impact on the nucleation of the ice phase. Mineral dust and some metallic particles were highly enhanced in the ice phase when compared to their abundance outside of cloud. Particles such as soot and biological material, previously suggested as ice nuclei, were not found either due to an inability to nucleate ice or low abundance. Atmospheric implications of these measurements and more advanced future analyses will be discussed.

Aerosol Absorption Measurements in MILAGRO.

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Arnott, W. P.; Paredes-Miranda, L.; Barnard, J. C.

2007-12-01

During the month of March 2006, a number of instruments were used to determine the absorption characteristics of aerosols found in the Mexico City Megacity and nearby Valley of Mexico. These measurements were taken as part of the Department of Energy's Megacity Aerosol Experiment - Mexico City (MAX-Mex) that was carried out in collaboration with the Megacity Interactions: Local and Global Research Observations (MILAGRO) campaign. MILAGRO was a joint effort between the DOE, NSF, NASA, and Mexican agencies aimed at understanding the impacts of a megacity on the urban and regional scale. A super-site was operated at the Instituto Mexicano de Petroleo in Mexico City (designated T-0) and at the Universidad Technologica de Tecamac (designated T-1) that was located about 35 km to the north east of the T-0 site in the State of Mexico. A third site was located at a private rancho in the State of Hidalgo approximately another 35 km to the northeast (designated T-2). Aerosol absorption measurements were taken in real time using a number of instruments at the T-0 and T-1 sites. These included a seven wavelength aethalometer, a multi-angle absorption photometer (MAAP), and a photo-acoustic spectrometer. Aerosol absorption was also derived from spectral radiometers including a multi-filter rotating band spectral radiometer (MFRSR). The results clearly indicate that there is significant aerosol absorption by the aerosols in the Mexico City megacity region. The absorption can lead to single scattering albedo reduction leading to values below 0.5 under some circumstances. The absorption is also found to deviate from that expected for a "well-behaved" soot anticipated from diesel engine emissions, i.e. from a simple 1/lambda wavelength dependence for absorption. Indeed, enhanced absorption is seen in the region of 300-450 nm in many cases, particularly in the afternoon periods indicating that secondary organic aerosols are contributing to the aerosol absorption. This is likely due

Characterizing the Asian Tropopause Aerosol Layer using in situ balloon measurements: the BATAL campaigns of 2014-2017

NASA Astrophysics Data System (ADS)

Fairlie, T. D.; Vernier, J. P.; Deshler, T.; Pandit, A. K.; Ratnam, M. V.; Gadhavi, H. S.; Liu, H.; Natarajan, M.; Jayaraman, A.; Kumar, S.; Singh, A. K.; Stenchikov, G. L.; Wienhold, F.; Vignelles, D.; Bedka, K. M.; Avery, M. A.

2017-12-01

We present in situ balloon observations of the Asian Tropopause Aerosol Layer (ATAL), a summertime accumulation of aerosols in the upper troposphere and lower stratosphere (UTLS), associated with Asian Summer Monsoon (ASM). The ATAL was first revealed by CALIPSO satellite data, and has been linked with deep convection of boundary layer pollution into the UTLS. The ATAL has potential implications for regional cloud properties, radiative transfer, and chemical processes in the UTLS. The "Balloon measurements of the Asian Tropopause Aerosol Layer (BATAL)" field campaigns to India and Saudi Arabia in were designed to characterize the physical and optical properties of the ATAL, to explore its composition, and its relationship with clouds in the UTLS. We launched 55 balloon flights from 4 locations, in summers 2014-2016. We return to India to make more balloon flights in summer 2017. Balloon payloads range from 500g to 50 kg, making measurements of meteorological parameters, ozone, water vapor, aerosol optical properties, concentration, volatility, and composition in the UTLS region. This project represents the most important effort to date to study UTLS aerosols during the ASM, given few in situ observations. We complement the in situ data presented with 3-d chemical transport simulations, designed to further explore the ATAL's chemical composition, the sensitivity of such to scavenging in parameterized deep convection, and the relative contribution of regional vs. rest-of-the-world pollution sources. The BATAL project has been a successful partnership between institutes in the US, India, Saudi Arabia, and Europe, and continues for the next 3-4 years, sponsored by the NASA Upper Atmosphere Research program. This partnership may provide a foundation for potential high-altitude airborne measurement studies during the ASM in the future.

The reaction probability of N2O5 with sulfuric acid aerosols at stratospheric temperatures and compositions

NASA Technical Reports Server (NTRS)

Fried, Alan; Henry, Bruce E.; Calvert, Jack G.; Mozurkewich, Michael

1994-01-01

We have measured the rate of reaction of N2O5 with H2O on monodisperse, submicrometer H2SO4 particles in a low-temperature flow reactor. Measurements were carried out at temperatures between 225 K and 293 K on aerosol particles with sizes and compositions comparable to those found in the stratosphere. At 273 K, the reaction probability was found to be 0.103 +/- 0.0006, independent of H2SO4 composition from 64 to 81 wt%. At 230 K, the reaction probability increased from 0.077 for compositions near 60% H2SO4 to 0.146 for compositions near 70% H2SO4. Intermediate conditions gave intermediate results except for low reaction probabilities of about 0.045 at 260 K on aerosols with about 78% H2SO4. The reaction probability did not depend on particle size. These results imply that the reaction occurs essentially at the surface of the particle. A simple model for this type of reaction that reproduces the general trends observed is presented. the presence of formaldehyde did not affect the reaction rate.

Predicting the mineral composition of dust aerosols – Part 2: Model evaluation and identification of key processes with observations

DOE PAGES

Perlwitz, J. P.; Perez Garcia-Pando, C.; Miller, R. L.

2015-10-21

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second methodmore » approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. In conclusion, the importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.« less

Airborne Cavity Ring-Down Measurement of Aerosol Extinction and Scattering During the Aerosol IOP

NASA Technical Reports Server (NTRS)

Strawa, A. W.; Ricci, K.; Provencal, R.; Schmid, B.; Covert, D.; Elleman, R.; Arnott, P.

2003-01-01

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300 Mm-1 with an estimated precision of 0.1 Min-1 for 1550 nm light and 0.2 Mm-1 for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects.= We present comparisons between the Cadenza measurements and those friom a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Biomass burning aerosol over the Amazon during SAMBBA: impact of chemical composition on radiative properties

NASA Astrophysics Data System (ADS)

Morgan, William; Allan, James; Flynn, Michael; Darbyshire, Eoghan; Hodgson, Amy; Liu, Dantong; O'shea, Sebastian; Bauguitte, Stephane; Szpek, Kate; Langridge, Justin; Johnson, Ben; Haywood, Jim; Longo, Karla; Artaxo, Paulo; Coe, Hugh

2014-05-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. Globally, biomass burning aerosols are thought to exert a small warming effect but with the uncertainty being 4 times greater than the central estimate. On regional scales, the impact is substantially greater, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, both in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated

Comparison of Aerosol Classification Results from Airborne High Spectral Resolution Lidar (HSRL) Measurements and the Calipso Vertical Feature Mask

NASA Technical Reports Server (NTRS)

Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Rogers, R. R.; Obland, M. D.; Butler, C. F.; Cook, A. L.; Harper, D. B.; Froyd, K. D.;

Pinatubo Aerosol Evolution: Using Composite Data Sets to Build the Global- to Micro-Scale Picture and Assess Consistency of Different Measurements

NASA Technical Reports Server (NTRS)

Russell, P. B.; Pueschel, R. F.; Livingston, J. M.; Bergstrom, R.; Hamill, P.

1994-01-01

This paper brings together experimental evidence required to build realistic models of the global evolution of physical, chemical, and optical properties of the aerosol resulting from the 1991 Pinatubo volcanic eruption. Such models are needed to compute the effects of the aerosol on atmospheric chemistry, dynamics, radiation, and temperature. Whereas there is now a large and growing body of post-Pinatubo measurements by a variety of techniques, some results are in conflict, and a self-consistent, unified picture is needed, along with an assessment of remaining uncertainties. This paper examines data from photometers, radiometers, impactors, optical counters/sizers, and lidars operated on the ground, aircraft, balloons, and spacecraft. Example data sources include: - Tracking sunphotometers and lidars at Mauna Loa Observatory (MLO) and on the DC-8 - Particle spectrometers and wire impactors on the ER-2 and DC-8 - Dustsondes (particle counters/sizers on balloons) - SAGE II, SAM II, AVHRR, CLAES, and ISAMS sensors on a variety of satellites. We assess the mutual consistency of these disparate data sets and recommend 'consensus" properties and uncertainties in the process of developing a composite data set. Recommended properties include the spatial and temporal evolution of particle chemical composition, shape, wavelength and temperature-dependent refractive index, size distribution, and optical depth spectra. Supporting references are cited and representative data shown.

Pinatubo Aerosol Evolution: Using Composite Data Sets to Build the Global- To Micro-Scale Picture and Assess Consistency of Different Measurements

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Pueschel, R. F.; Livingston, J. M.; Bergstrom, R.; Hamill, P.; Lawless, James G. (Technical Monitor)

1994-01-01

This paper brings together experimental evidence required to build realistic models of the global evolution of physical, chemical, and optical properties of the aerosol resulting from the 1991 Pinatubo volcanic eruption. Such models are needed to compute the effects of the aerosol on atmospheric chemistry, dynamics, radiation, and temperature. Whereas there is now a large and crowing body of post-Pinatubo measurements by a variety of techniques, some results are in conflict, and a self-consistent, unified picture is needed, along with an assessment of remaining uncertainties. This paper examines, data from photometers, radiometers, impactors, optical counter/sizers, and lidars operated on the ground, aircraft, balloons, and spacecraft. Example data sources include: (1) Tracking sunphotometers and lidars at Mauna Loa Observatory (MLO) and on the DC-8. (2) Particle spectrometers and wire impactors on the ER-2 and DC-8. (3) Dustsondes (particle counter/sizers on balloons). and (3) SAGE II, SAM II, AVHRR, CLAES, and ISAMS sensors on a variety of satellites. We assess the mutual consistency of these disparate data sets and recommend 'consensus' properties and uncertainties in the process of developing a composite data set. Recommended properties include the spatial and temporal evolution of particle chemical composition, shape, wavelength-and temperature-dependent refractive index, size distribution, and optical depth spectra. Supporting references are cited and representative data shown.

The Asian Tropopause Aerosol Layer: Balloon-Borne Measurements, Satellite Observations and Modeling Approaches

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Natarajan, M.; Deshler, Terry; Liu, H.; Wegner, T.; Baker, N.; Gadhavi, H.; Jayaraman, A.; Pandit, A.;

ELECTRICAL AEROSOL DETECTOR (EAD) MEASUREMENTS AT THE ST. LOUIS SUPERSITE

EPA Science Inventory

The Model 3070A Electrical Aerosol Detector (EAD) measures a unique aerosol parameter called total aerosol length. Reported as mm/cm3, aerosol length can be thought of as a number concentration times average diameter, or simply as d1 weighting. This measurement falls between nu...

Lidar Measurements of Ozone, Aerosols, and Clouds Observed in the Tropics Near Central America During TC4-Costa Rica

NASA Astrophysics Data System (ADS)

Hair, J. W.; Browell, E.; Butler, C.; Fenn, M.; Notari, A.; Simpson, S.; Ismail, S.; Avery, M.

2007-12-01

Large-scale measurements of ozone and aerosol distributions were made from the NASA DC-8 aircraft during the TC4 (Tropical Composition, Cloud, and Climate Coupling) field experiment conducted from June 28 - August 10, 2007 based in San Jose, Costa Rica. Remote measurements were made with an airborne lidar to provide ozone and multiple-wavelength aerosol and cloud backscatter profiles from near the surface to above the tropopause along the flight track. Aerosol depolarization measurements were also made for the detection of nonspherical aerosols, such as mineral dust, biomass burning, and recent emissions from South American volcanoes. Long-range transport of Saharan dust with depolarizing aerosols was frequently observed in the lower troposphere both over the Caribbean Sea and Pacific Ocean and within the marine boundary layer. In addition, visible and sub-visible cirrus clouds were observed with the multi-wavelength backscatter and depolarization measurements. Initial distributions of ozone, aerosol, and cloud are presented which will be used to interpret large-scale atmospheric processes. In situ measurements of ozone and aerosols made onboard the DC-8 will be compared to the remote lidar measurements. This paper provides a first look at the characteristics of ozone, aerosol, and cloud distributions that were encountered during this field experiment and provide a unique dataset that will be further related through satellite data, backward trajectories, and chemical transport models (CTM) to sources and sinks of ozone, aerosols, and clouds and to dynamical, chemical, and radiative processes.

Effect of SO2 and Photolysis on Photooxidized Diesel Fuel Secondary Organic Aerosol Composition

NASA Astrophysics Data System (ADS)

MacMillan, A. C.; Blair, S. L.; Lin, P.; Laskin, A.; Laskin, J.; Nizkorodov, S.

2014-12-01

Diesel fuel (DSL) and sulfur dioxide (SO2) are important precursors to secondary organic aerosol (SOA) formation. DSL is often co-emitted with SO2 and NO2, thus it is important to understand the possible effects of SO2 on DSL SOA composition. Additionally, DSL SOA composition can be affected by photochemical aging processes such as photolysis. In this study, DSL SOA was first prepared under dry, high-NOx conditions with various concentrations of SO2 by photooxidation in a smog chamber. The SOA was then stripped of excess oxidants and gaseous organics with a denuder train and the resulting particles were photolyzed at various photolysis times in a quartz flow tube. The SOA composition, photochemical aging, properties, and mass concentration, before and after direct photolysis in the flow tube, were examined using several techniques. High-resolution mass spectrometry (HR-MS) was performed on DSL SOA samples to investigate the effect of SO2 on molecular level composition. SOA composition as a function of photolysis time was measured with an aerosol mass spectrometer (AMS). HR-MS results show that organosulfates are produced in DSL SOA. Both AMS and HR-MS results show that photolysis also has an effect on composition; though, this is more apparent in the HR-MS results than in the AMS results. In summary, both the presence of SO2 and solar radiation has an effect on DSL SOA composition.

Measuring Sodium Chloride Contents of Aerosols

NASA Technical Reports Server (NTRS)

Sinha, M. P.; Friedlander, S. K.

1986-01-01

Amount of sodium chloride in individual aerosol particles measured in real time by analyzer that includes mass spectrometer. Analyzer used to determine mass distributions of active agents in therapeutic or diagnostic aerosols derived from saline solutions and in analyzing ocean spray. Aerosol particles composed of sodium chloride introduced into oven, where individually vaporized on hot wall. Vapor molecules thermally dissociated, and some of resulting sodium atoms ionized on wall. Ions leave oven in burst and analyzed by spectrometer, which is set to monitor sodium-ion intensity.

Composition and formation of organic aerosol particles in the Amazon

NASA Astrophysics Data System (ADS)

Pöhlker, C.; Wiedemann, K.; Sinha, B.; Shiraiwa, M.; Gunthe, S. S.; Artaxo, P.; Gilles, M. K.; Kilcoyne, A. L. D.; Moffet, R. C.; Smith, M.; Weigand, M.; Martin, S. T.; Pöschl, U.; Andreae, M. O.

2012-04-01

We applied scanning transmission X-ray microscopy with near edge X-ray absorption fine structure (STXM-NEXAFS) analysis to investigate the morphology and chemical composition of aerosol samples from a pristine tropical environment, the Amazon Basin. The samples were collected in the Amazonian rainforest during the rainy season and can be regarded as a natural background aerosol. The samples were found to be dominated by secondary organic aerosol (SOA) particles in the fine and primary biological aerosol particles (PBAP) in the coarse mode. Lab-generated SOA-samples from isoprene and terpene oxidation as well as pure organic compounds from spray-drying of aqueous solution were measured as reference samples. The aim of this study was to investigate the microphysical and chemical properties of a tropical background aerosol in the submicron size range and its internal mixing state. The lab-generated SOA and pure organic compounds occurred as spherical and mostly homogenous droplet-like particles, whereas the Amazonian SOA particles comprised a mixture of homogeneous droplets and droplets having internal structures due to atmospheric aging. In spite of the similar morphological appearance, the Amazon samples showed considerable differences in elemental and functional group composition. According to their NEXAFS spectra, three chemically distinct types of organic material were found and could be assigned to the following three categories: (1) particles with a pronounced carboxylic acid (COOH) peak similar to those of laboratory-generated SOA particles from terpene oxidation; (2) particles with a strong hydroxy (COH) signal similar to pure carbohydrate particles; and (3) particles with spectra resembling a mixture of the first two classes. In addition to the dominant organic component, the NEXAFS spectra revealed clearly resolved potassium (K) signals for all analyzed particles. During the rainy season and in the absence of anthropogenic influence, active biota is

Aerosol Measurements by the Globally Distributed Micro Pulse Lidar Network

NASA Technical Reports Server (NTRS)

Spinhirne, James; Welton, Judd; Campbell, James; Berkoff, Tim; Starr, David (Technical Monitor)

2001-01-01

Full time measurements of the vertical distribution of aerosol are now being acquired at a number of globally distributed MP (micro pulse) lidar sites. The MP lidar systems provide full time profiling of all significant cloud and aerosol to the limit of signal attenuation from compact, eye safe instruments. There are currently eight sites in operation and over a dozen planned. At all sited there are also passive aerosol and radiation measurements supporting the lidar data. Four of the installations are at Atmospheric Radiation Measurement program sites. The network operation includes instrument operation and calibration and the processing of aerosol measurements with standard retrievals and data products from the network sites. Data products include optical thickness and extinction cross section profiles. Application of data is to supplement satellite aerosol measurements and to provide a climatology of the height distribution of aerosol. The height distribution of aerosol is important for aerosol transport and the direct scattering and absorption of shortwave radiation in the atmosphere. Current satellite and other data already provide a great amount of information on aerosol distribution, but no passive technique can adequately resolve the height profile of aerosol. The Geoscience Laser Altimeter System (GLAS) is an orbital lidar to be launched in early 2002. GLAS will provide global measurements of the height distribution of aerosol. The MP lidar network will provide ground truth and analysis support for GLAS and other NASA Earth Observing System data. The instruments, sites, calibration procedures and standard data product algorithms for the MPL network will be described.

Two-Column Aerosol Project: Aerosol Light Extinction Measurements Field Campaign Report

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

Dubey, Manvendra; Aiken, Allison; Berg, Larry

We deployed Aerodyne Research Inc.’s first Cavity Attenuated Phase Shift extinction (CAPS PMex) monitor (built by Aerodyne) that measures light extinction by using a visible-light-emitting diode (LED) as a light source, a sample cell incorporating two high-reflectivity mirrors centered at the wavelength of the LED, and a vacuum photodiode detector in Cape Cod in 2012/13 for the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Two-Column Aerosol Project (TCAP). The efficacy of this instrument is based on the fact that aerosols are broadband scatterers and absorbers of light. The input LED is square-wave modulated and passedmore » through the sample cell that distorts it due to exponential decay by aerosol light absorption and scattering; this is measured at the detector. The amount of phase shift of the light at the detector is used to determine the light extinction. This extinction measurement provides an absolute value, requiring no calibration. The goal was to compare the CAPS performance with direct measurements of absorption with ARM’s baseline photoacoustic soot spectrometer (PASS-3) and nephelometer instruments to evaluate its performance.« less

Broadband Measurement of Aerosol Extinction in the Visible Range

NASA Astrophysics Data System (ADS)

He, Quanfu; Bluvshtein, Nir; Segev, Lior; Flores, Michel; Rudich, Yinon; Washenfelder, Rebecca; Brown, Steven

2017-04-01

Atmospheric aerosols influence the Earth's radiative budget directly by scattering and absorbing incoming solar radiation. Aerosol direct forcing remains one of the largest uncertainties in quantifying the role that aerosols play in the Earth's radiative budget. The optical properties of aerosols vary as a function of wavelength, but few measurements reported the wavelength dependence of aerosol extinction cross section and complex refractive indices, particularly in the blue and visible spectral range. There is also currently a large gap in our knowledge of how the optical properties evolve as a function of atmospheric aging in the visible spectrum. In this study, we constructed a new and novel laboratory instrument to measure aerosol extinction as a function of wavelength, using cavity enhanced spectroscopy with a white light source. This broadband cavity enhanced spectroscopy (BBCES) covers the 395-700 nm spectral region using a broadband light source and a grating spectrometer with charge-coupled device detector (CCD). We evaluated this BBCES by measuring extinction cross section for aerosols that are pure scattering, slightly absorbing and strongly absorbing atomized from standard materials. We also retrieved the refractive indices from the measured extinction cross sections. Secondary organic aerosols from biogenic and anthropogenic precursors were "aged" to differential time scales (1 to 10 days) in an Oxidation Flow Reactor (OFR) under the combined influence of OH, O3 and UV light. The new BBCES was used to online measure the extinction cross sections of the SOA. This talk will provide a comprehensive understanding of aerosol optical properties alerting during aging process in the 395 - 700 nm spectrum.

Speciated Chemical Composition of Biomass Burning Aerosol from Various Fuels during FIREX

NASA Astrophysics Data System (ADS)

Jen, C.; Hatch, L. E.; Kreisberg, N. M.; Selimovic, V.; Yokelson, R. J.; Barsanti, K.; Goldstein, A. H.

2017-12-01

Biomass burning is the largest global source of atmospheric primary carbonaceous aerosols and the second largest global source of non-methane organic compounds, including volatile and semi-volatile organic compounds that are now understood to be major contributors to secondary particle formation in the atmosphere. As wildfires in forested regions such as the western United States become larger and more frequent, understanding the chemical composition of biomass burning organic aerosol is needed to better predict their increasing impact on human health, air quality, and climate. This study presents emission profiles of chemically speciated intermediate and semi-volatile organic compounds present in biomass burning aerosol particles ≤1.0 μm. Biomass burning organic aerosol (BBOA) samples from a variety of fuel types and burning conditions were collected during the FIREX campaign at the USDA Fire Lab (Missoula, MT). Fuels were primarily selected from vegetation commonly found in the western United States, such as ponderosa pine, lodgepole pine, ceanothus, and chaparral. Collected BBOA was thermally desorbed from the filters and analyzed using online derivatization and 2-dimensional gas chromatography with an electron impact (70 eV) and vacuum ultra violet light (10.5 eV) high resolution time of flight mass spectrometer for compound identification. Emission profiles for specific compounds (e.g., levoglucosan) and families of compounds (e.g., sugars and methoxyphenols) show distinct variations between different fuel types, with major differences between fresh and partially decomposed fuels. Results also illustrate the variability in chemical species between burns conducted under similar conditions. Furthermore, chemical fingerprints, representing ratios of normalized emissions for key chemical compounds, were measured for specific fuels/conditions and could be used in future field studies to help identify contributions of various vegetation to total BBOA and in

Aircraft measurements of aerosol properties during GoAmazon - G1 and HALO inter-comparison

NASA Astrophysics Data System (ADS)

Mei, F.; Cecchini, M. A.; Wang, J.; Tomlinson, J. M.; Comstock, J. M.; Hubbe, J. M.; Pekour, M. S.; Machado, L.; Wendisch, M.; Longo, K.; Martin, S. T.; Schmid, B.; Weinzierl, B.; Krüger, M. L.; Zöger, M.

2015-12-01

Currently, the indirect effects of atmospheric aerosols remain the most uncertain components in forcing of climate change over the industrial period (IPCC, 2013). This large uncertainty is partially a result of our incomplete understanding of the ability of particles to form cloud droplets under atmospherically relevant supersaturations. One objective of the US Department of Energy (DOE) Green Ocean Amazon Project (GoAmazon2014/5) is to understand the influence of the emission from Manaus, a tropical megacity, on aerosol size, concentration, and chemical composition, and their impact on cloud condensation nuclei (CCN) spectrum. The GoAmazon2014/5 study was an international campaign with the collaboration efforts from US, Brazil and Germany. During the intensive operation period, in the dry season (Sep. 1st - Oct. 10th, 2014), aerosol concentration, size distributions, and CCN spectra, both under pristine conditions and inside the Manaus plume, were characterized in-situ from the DOE Gulfstream-1 (G-1) research aircraft and German HALO aircraft during 4 coordinated flights on Sep. 9th, Sep. 16th, Sep 21st and Oct. 1st, 2014. During those four flights, aerosol number concentrations and CCN concentrations at two supersaturations (0.25% and 0.5%) were measured by condensation particle counters (CPCs) and a DMT dual column CCN counter onboard both G-1 and HALO. Aerosol size distribution was also measured by a Fast Integrated Mobility Spectrometer (FIMS) aboard the G-1 and is compared with the size distribution from Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A, DMT), which were deployed both on the G-1 and the HALO. Good agreement between the aerosol properties measured from the two aircraft has been achieved. The vertical profiles of aerosol size distribution and CCN spectrum will be discussed.

Radiative Effects of Aerosol in the Marine Environment: Tales from the Two-Column Aerosol Project

NASA Astrophysics Data System (ADS)

Berg, L. K.; Fast, J. D.; Barnard, J.; Chand, D.; Chapman, E. G.; Comstock, J. M.; Ferrare, R. A.; Flynn, C. J.; Hair, J. W.; Hostetler, C. A.; Hubbe, J.; Johnson, R.; Kassianov, E.; Kluzek, C.; Laskin, A.; Lee, Y.; Mei, F.; Michalsky, J. J.; Redemann, J.; Rogers, R. R.; Russell, P. B.; Sedlacek, A. J.; Schmid, B.; Shilling, J. E.; Shinozuka, Y.; Springston, S. R.; Tomlinson, J. M.; Wilson, J. M.; Zelenyuk, A.; Berkowitz, C. M.

2013-12-01

There is still uncertainty associated with the direct radiative forcing by atmospheric aerosol and its representation in atmospheric models. This is particularly true in marine environments near the coast where the aerosol loading is a function of both naturally occurring and anthropogenic aerosol. These regions are also subject to variable synoptic and thermally driven flows (land-sea breezes) that transport aerosol between the continental and marine environments. The situation is made more complicated due to seasonal changes in aerosol emissions. Given these differences in emissions, we expect significant differences in the aerosol intensive and extensive properties between summer and winter and data is needed to evaluate models over the wide range of conditions. To address this issue, the recently completed Two Column Aerosol Project (TCAP) was designed to measure the key aerosol parameters in two atmospheric columns, one located over Cape Cod, Massachusetts and another approximately 200 km from the coast over the Atlantic Ocean. Measurements included aerosol size distribution, chemical composition, optical properties and vertical distribution. Several aspects make TCAP unique, including the year-long deployment of a suite of surface-based instruments by the US Department of Energy's Atmospheric Radiation Measurement (ARM) Climate Research Facility and two aircraft intensive operations periods supported by the ARM Airborne Facility, one conducted in July 2012 and a second in February 2013. The presentation will include a discussion of the impact of the aerosol optical properties and their uncertainty on simulations of the radiation budget within the TCAP domain in the context of both single column and regional scale models. Data from TCAP will be used to highlight a number of important factors, including diurnal variation in aerosol optical depth measured at the surface site, systematic changes in aerosol optical properties (including scattering, absorption, and

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.

Optical measurement of medical aerosol media parameters

NASA Astrophysics Data System (ADS)

Sharkany, Josif P.; Zhytov, Nikolay B.; Sichka, Mikhail J.; Lemko, Ivan S.; Pintye, Josif L.; Chonka, Yaroslav V.

2000-07-01

The problem of aerosol media parameters measurements are presented in the work and these media are used for the treatment of the patients with bronchial asthma moreover we show the results of the development and the concentration and dispersity of the particles for the long-term monitoring under such conditions when the aggressive surroundings are available. The system for concentration measurements is developed, which consists of two identical photometers permitting to carry out the measurements of the transmission changes and the light dispersion depending on the concentration of the particles. The given system permits to take into account the error, connected with the deposition of the salt particles on the optical windows and the mirrors in the course of the long-term monitoring. For the controlling of the dispersity of the aggressive media aerosols the optical system is developed and used for the non-stop analysis of the Fure-spectra of the aerosols which deposit on the lavsan film. The registration of the information is performed with the help of the rule of the photoreceivers or CCD-chamber which are located in the Fure- plane. With the help of the developed optical system the measurements of the concentration and dispersity of the rock-salt aerosols were made in the medical mines of Solotvino (Ukraine) and in the artificial chambers of the aerosol therapy.

Aerosol composition and sources in the central Arctic Ocean during ASCOS

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Leck, C.; Graus, M.; Müller, M.; Paatero, J.; Burkhart, J. F.; Stohl, A.; Orr, L. H.; Hayden, K.; Li, S.-M.; Hansel, A.; Tjernström, M.; Leaitch, W. R.; Abbatt, J. P. D.

2011-10-01

Measurements of submicron aerosol chemical composition were made over the central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.051 and 0.055 μ g m-3, respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33% and 36% of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47% of the sulphate apportioned to marine biogenic sources and 48% to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25 ± 0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it had a longer photochemical lifetime than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources. In particular, given that the factor does not correlate with common tracers of continental influence, we cannot rule out that the organic factor arises from a primary marine source.

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

NASA Astrophysics Data System (ADS)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

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

NASA Astrophysics Data System (ADS)

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

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

How Well Can Aerosol Measurements from the Terra Morning Polar Orbiting Satellite Represent the Daily Aerosol Abundance and Properties?

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Holben, B. N.; Tanre, D.; Slutzker, I.; Eck, T. F.; Smirnov, A.; Einaudi, Franco (Technical Monitor)

2000-01-01

The Terra mission, launched at the dawn of 1999, and Aqua mission to be launched soon, will possess innovative measurements of the aerosol daily spatial distribution, distinguish between dust, smoke and regional pollution and measure aerosol radiative forcing of climate. Their polar orbit gives daily global coverage, however measurements are acquired at specific time of the day. To what degree can present measurements from Terra taken between 10:00 and 11:30 AM local time, represent the daily average aerosol forcing of climate? Here we answer this question using 7 years of data from the distributed ground based 50-70 instrument Aerosol Robotic Network (AERONET) This (AERONET) half a million measurement data set shows that Terra aerosol measurements represent the daily average values within 5%. The excellent representation is found for large dust particles or small aerosol particles from Fires or regional pollution and for any range of the optical thickness, a measure of the amount of aerosol in the atmosphere.

Sea spray aerosol chemical composition: elemental and molecular mimics for laboratory studies of heterogeneous and multiphase reactions.

PubMed

Bertram, Timothy H; Cochran, Richard E; Grassian, Vicki H; Stone, Elizabeth A

2018-04-03

Sea spray aerosol particles (SSA), formed through wave breaking at the ocean surface, contribute to natural aerosol particle concentrations in remote regions of Earth's atmosphere, and alter the direct and indirect effects of aerosol particles on Earth's radiation budget. In addition, sea spray aerosol serves as suspended surface area that can catalyze trace gas reactions. It has been shown repeatedly that sea spray aerosol is heavily enriched in organic material compared to the surface ocean. The selective enrichment of organic material complicates the selection of representative molecular mimics of SSA for laboratory or computational studies. In this review, we first provide a short introduction to SSA formation processes and discuss chemical transformations of SSA that occur in polluted coastal regions and remote pristine air. We then focus on existing literature of the chemical composition of nascent SSA generated in controlled laboratory experiments and field investigations. We combine the evidence on the chemical properties of nascent SSA with literature measurements of SSA water uptake to assess SSA molecular composition and liquid water content. Efforts to speciate SSA organic material into molecular classes and specific molecules have led to the identification of saccharides, alkanes, free fatty acids, anionic surfactants, dicarboxylic acids, amino acids, proteinaceous matter, and other large macromolecules. However to date, less than 25% of the organic mass of nascent SSA has been quantified at a molecular level. As discussed here, quantitative measurements of size resolved elemental ratios, combined with determinations of water uptake properties, provides unique insight on the concentration of ions within SSA as a function of particle size, pointing to a controlling role for relative humidity and the hygroscopicity of SSA organic material at small particle diameters.

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

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

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.

Size Resolved Measurements of Springtime Aerosol Particles over the Northern South China Sea

NASA Technical Reports Server (NTRS)

Atwood, Samuel A.; Reid, Jeffrey S.; Kreidenweis, Sonia M.; Cliff, Stephen S.; Zhao, Yongjing; Lin, Neng-Huei; Tsay, Si-Chee; Chu, Yu-Chi; Westphal, Douglas L.

2012-01-01

Large sources of aerosol particles and their precursors are ubiquitous in East Asia. Such sources are known to impact the South China Sea (henceforth SCS), a sometimes heavily polluted region that has been suggested as particularly vulnerable to climate change. To help elucidate springtime aerosol transport into the SCS, an intensive study was performed on the remote Dongsha (aka Pratas) Islands Atoll in spring 2010. As part of this deployment, a Davis Rotating-drum Uniform size-cut Monitor (DRUM) cascade impactor was deployed to collect size-resolved aerosol samples at the surface that were analyzed by X-ray fluorescence for concentrations of selected elements. HYSPLIT backtrajectories indicated that the transport of aerosol observed at the surface at Dongsha was occurring primarily from regions generally to the north and east. This observation was consistent with the apparent persistence of pollution and dust aerosol, along with sea salt, in the ground-based dataset. In contrast to the sea-level observations, modeled aerosol transport suggested that the westerly flow aloft (w700 hPa) transported smoke-laden air toward the site from regions from the south and west. Measured aerosol optical depth at the site was highest during time periods of modeled heavy smoke loadings aloft. These periods did not coincide with elevated aerosol concentrations at the surface, although the model suggested sporadic mixing of this free-tropospheric aerosol to the surface over the SCS. A biomass burning signature was not clearly identified in the surface aerosol composition data, consistent with this aerosol type remaining primarily aloft and not mixing strongly to the surface during the study. Significant vertical wind shear in the region also supports the idea that different source regions lead to varying aerosol impacts in different vertical layers, and suggests the potential for considerable vertical inhomogeneity in the SCS aerosol environment.

Characteristics and composition of atmospheric aerosols in Phimai, central Thailand during BASE-ASIA

NASA Astrophysics Data System (ADS)

Li, Can; Tsay, Si-Chee; Hsu, N. Christina; Kim, Jin Young; Howell, Steven G.; Huebert, Barry J.; Ji, Qiang; Jeong, Myeong-Jae; Wang, Sheng-Hsiang; Hansell, Richard A.; Bell, Shaun W.

2013-10-01

Comprehensive measurements of atmospheric aerosols were made in Phimai, central Thailand (15.183°N, 102.565°E, elevation: 206 m) during the BASE-ASIA field experiment from late February to early May in 2006. The observed aerosol loading was sizable for this rural site (mean aerosol scattering: 108 ± 64 Mm-1; absorption: 15 ± 8 Mm-1; PM10 concentration: 33 ± 17 μg m-3), and dominated by submicron particles. Major aerosol compounds included carbonaceous (OC: 9.5 ± 3.6 μg m-3; EC: 2.0 ± 2.3 μg m-3) and secondary species (SO42-: 6.4 ± 3.7 μg m-3, NH4+: 2.2 ± 1.3 μg m-3). While the site was seldom under the direct influence of large forest fires to its north, agricultural fires were ubiquitous during the experiment, as suggested by the substantial concentration of K+ (0.56 ± 0.33 μg m-3). Besides biomass burning, aerosols in Phimai during the experiment were also strongly influenced by industrial and vehicular emissions from the Bangkok metropolitan region and long-range transport from southern China. High humidity played an important role in determining the aerosol composition and properties in the region. Sulfate was primarily formed via aqueous phase reactions, and hygroscopic growth could enhance the aerosol light scattering by up to 60%, at the typical morning RH level of 85%. The aerosol single scattering albedo demonstrated distinct diurnal variation, ranging from 0.86 ± 0.04 in the evening to 0.92 ± 0.02 in the morning. This experiment marks the first time such comprehensive characterization of aerosols was made for rural central Thailand. Our results indicate that aerosol pollution has developed into a regional problem for northern Indochina, and may become more severe as the region's population and economy continue to grow.

Sensitivity of multiangle photo-polarimetry to absorbing aerosol vertical layering and properties: Quantifying measurement uncertainties for ACE requirements

NASA Astrophysics Data System (ADS)

Kalashnikova, O. V.; Garay, M. J.; Davis, A. B.; Natraj, V.; Diner, D. J.; Tanelli, S.; Martonchik, J. V.; JPl Team

2011-12-01

The impact of tropospheric aerosols on climate can vary greatly based upon relatively small variations in aerosol properties, such as composition, shape and size distributions, as well as vertical layering. Multi-angle polarimetric measurements have been advocated in recent years as an additional tool to better understand and retrieve the aerosol properties needed for improved predictions of aerosol radiative forcing on climate. The central concern of this work is the assessment of the effects of absorbing aerosol properties under measurement uncertainties achievable for future generation multi-angle, polarimetric imaging instruments under ACE mission requirements. As guidelines, the on-orbit performance of MISR for multi-angle intensity measurements and the reported polarization sensitivities of a MSPI prototype were adopted. In particular, we will focus on sensitivities to absorbing aerosol layering and observation-constrained refractive indices (resulting in various single scattering albedos (SSA)) of both spherical and non-spherical absorbing aerosol types. We conducted modeling experiments to determine how the measured Stokes vector elements are affected in UV-NIR range by the vertical distribution, mixing and layering of smoke and dust aerosols, and aerosol SSA under the assumption of a black and polarizing ocean surfaces. We use a vector successive-orders-of-scattering (SOS) and VLIDORT transfer codes that show excellent agreement. Based on our sensitivity studies we will demonstrate advantages and disadvantages of wavelength selection in UV-NIR range to access absorbing aerosol properties. Polarized UV channels do not show particular advantage for absorbing aerosol property characterization due to dominating molecular signal. Polarimetric SSA sensitivity is small, however needed to be considered in the future polarimetric retrievals under ACE-defined uncertainty.

Winter measurements of trace gas and aerosol composition at a rural site in southern ontario

NASA Astrophysics Data System (ADS)

Daum, P. H.; Kelly, T. J.; Tanner, R. L.; Tang, X.; Anlauf, K.; Bottenheim, J.; Brice, K. A.; Wiebe, H. A.

This paper reports the results of continuous measurements of concentrations of trace gas and aerosol species at Powassan, Ontario, a rural location in southern Ontario, from 20 January to 24 February 1984. The measurements included aerosol H + , NH 4+, Na +, Ca 2+ , NO 3-, SO 42- and Cl -, gaseous SO 2, NO, NO' y; ( = NO + NO2 + PAN + HNO3), HNO 3, PAN, and O 3. Average values of concentrations for key species during the project were: SO 2, 7.3 ppb; NO y, 7.5 ppb; HNO 3, 0.85 ppb; O 3, 33 ppb; NH 4+ 1.5 ppb; NO 3-, 0.4 ppb; and SO 42-, 0.9 ppb. Concentrations of primary pollutants (e.g. SO 2) were typically much higher, and concentrations of secondary species (e.g. SO 42-) typically lower, than observed at this location in summer. However, clear-air t- NO 3-/SO 42- ratios averaged 5-10 times higher in winter than in summer which suggests that HNO 3 is a more important source of atmospheric acidity, relative to SO 42- aerosol, in winter than in summer. Pollutant concentrations were highly variable; back trajectory calculations indicate that periods of high concentrations of both primary and secondary species were typically associated with air-mass back trajectories from the southern sectors while periods of low concentrations of secondary species were associated with back trajectories from the north. Comparison of these measurements with those at other locations suggests that concentrations at Powassan were characteristic of those prevailing over a much larger, possibly regional, area.

Correlative measurements of the stratospheric aerosols

NASA Astrophysics Data System (ADS)

Santer, R.; Brogniez, C.; Herman, M.; Diallo, S.; Ackerman, M.

1992-12-01

Joint experiments were organized or available during stratospheric flights of a photopolarimeter, referred to as RADIBAL (radiometer balloon). In May 1984, RADIBAL flew simultaneously with another balloonborne experiment conducted by the Institut d'Aeronomie Spatiale de Belgique (IASB), which provides multiwavelength vertical profiles of the aerosol scattering coefficient. At this time, the El Chichon layer was observable quite directly from mountain sites. A ground-based station set up at Pic du Midi allowed an extensive description of the aerosol optical properties. The IASB and the Pic du Midi observations are consistent with the aerosol properties derived from the RADIBAL measurement analysis.

The Global Atmosphere Watch Aerosol Programme

NASA Astrophysics Data System (ADS)

Baltensperger, U.

2003-04-01

The Global Atmosphere Watch (GAW) programme is a WMO sponsored activity and currently supported by about 80 WMO member countries. It is the goal of GAW to develop and maintain long-term measurements of atmospheric constituents in order to detect trends, develop aerosol predictive capabilities and understand proc- esses. With respect to aerosols, the objective of GAW is to support a global network determining the spatio-temporal distribution of aerosol properties related to climate forcing and air quality up to multi-decadal time scales. The GAW network consists of 22 Global stations and some 300 Regional stations. The Scientific Advisory Group (SAG) for Aerosols will soon publish their recommendations for aerosol measurements. Each site should have an acceptable aerosol sampling inlet. Regional stations measure aerosol optical depth, as well as the aerosol light scattering and absorption coefficient. If possible these should be complemented by routine mass concentration and composition measurements in two aerosol size fractions. At Global stations, a larger number of measurements are desirable. These include the Regional parameters list above as well as the light scattering, hemispheric backscat- tering, and absorption coefficients at various wavelengths, aerosol number concen- tration, cloud condensation nuclei (CCN) concentration at 0.5% supersaturation, and diffuse, global and direct solar radiation. Additional parameters such as the aerosol size distribution, detailed size fractionated chemical composition, dependence of aerosol properties on relative humidity, CCN concentration at various supersatura- tions, and the vertical distribution of aerosol properties should be measured intermit- tently at Global stations. Examples from the Jungfraujoch (Swiss Alps, 3580 m asl) will be given, where many of the parameters listed above are measured. Data are delivered to and made available by the World Data Centre for Aerosols (WDCA, located in Ispra, Italy http

Comparison of Methods for Predicting the Compositional Dependence of the Density and Refractive Index of Organic-Aqueous Aerosols.

PubMed

Cai, Chen; Miles, Rachael E H; Cotterell, Michael I; Marsh, Aleksandra; Rovelli, Grazia; Rickards, Andrew M J; Zhang, Yun-Hong; Reid, Jonathan P

2016-08-25

Representing the physicochemical properties of aerosol particles of complex composition is of crucial importance for understanding and predicting aerosol thermodynamic, kinetic, and optical properties and processes and for interpreting and comparing analysis methods. Here, we consider the representations of the density and refractive index of aqueous-organic aerosol with a particular focus on the dependence of these properties on relative humidity and water content, including an examination of the properties of solution aerosol droplets existing at supersaturated solute concentrations. Using bulk phase measurements of density and refractive index for typical organic aerosol components, we provide robust approaches for the estimation of these properties for aerosol at any intermediate composition between pure water and pure solute. Approximately 70 compounds are considered, including mono-, di- and tricarboxylic acids, alcohols, diols, nitriles, sulfoxides, amides, ethers, sugars, amino acids, aminium sulfates, and polyols. We conclude that the molar refraction mixing rule should be used to predict the refractive index of the solution using a density treatment that assumes ideal mixing or, preferably, a polynomial dependence on the square root of the mass fraction of solute, depending on the solubility limit of the organic component. Although the uncertainties in the density and refractive index predictions depend on the range of subsaturated compositional data available for each compound, typical errors for estimating the solution density and refractive index are less than ±0.1% and ±0.05%, respectively. Owing to the direct connection between molar refraction and the molecular polarizability, along with the availability of group contribution models for predicting molecular polarizability for organic species, our rigorous testing of the molar refraction mixing rule provides a route to predicting refractive indices for aqueous solutions containing organic molecules

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

NASA Astrophysics Data System (ADS)

Cao, Li-Ming; Huang, Xiao-Feng; Li, Yuan-Yuan; Hu, Min; He, Ling-Yan

2018-02-01

Aerosol pollution has been a very serious environmental problem in China for many years. The volatility of aerosols can affect the distribution of compounds in the gas and aerosol phases, the atmospheric fates of the corresponding components, and the measurement of the concentration of aerosols. Compared to the characterization of chemical composition, few studies have focused on the volatility of aerosols in China. In this study, a thermodenuder aerosol mass spectrometer (TD-AMS) system was deployed to study the volatility of non-refractory submicron particulate matter (PM1) species during winter in Shenzhen. To our knowledge, this paper is the first report of the volatilities of aerosol chemical components based on a TD-AMS system in China. The average PM1 mass concentration during the experiment was 42.7±20.1 µg m-3, with organic aerosol (OA) being the most abundant component (43.2 % of the total mass). The volatility of chemical species measured by the AMS varied, with nitrate showing the highest volatility, with a mass fraction remaining (MFR) of 0.57 at 50 °C. Organics showed semi-volatile characteristics (the MFR was 0.88 at 50 °C), and the volatility had a relatively linear correlation with the TD temperature (from the ambient temperature to 200 °C), with an evaporation rate of 0.45 % °C-1. Five subtypes of OA were resolved from total OA using positive matrix factorization (PMF) for data obtained under both ambient temperature and high temperatures through the TD, including a hydrocarbon-like OA (HOA, accounting for 13.5 %), a cooking OA (COA, 20.6 %), a biomass-burning OA (BBOA, 8.9 %), and two oxygenated OAs (OOAs): a less-oxidized OOA (LO-OOA, 39.1 %) and a more-oxidized OOA (MO-OOA, 17.9 %). Different OA factors presented different volatilities, and the volatility sequence of the OA factors at 50 °C was HOA (MFR of 0.56) > LO-OOA (0.70) > COA (0.85) ≈ BBOA (0.87) > MO-OOA (0.99), which was not completely consistent with the sequence of their O

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

NASA Astrophysics Data System (ADS)

Dhomse, S. S.; Emmerson, K. M.; Mann, G. W.; Bellouin, N.; Carslaw, K. S.; Chipperfield, M. P.; Hommel, R.; Abraham, N. L.; Telford, P.; Braesicke, P.; Dalvi, M.; Johnson, C. E.; O'Connor, F.; Morgenstern, O.; Pyle, J. A.; Deshler, T.; Zawodny, J. M.; Thomason, L. W.

2014-10-01

We use a stratosphere-troposphere composition-climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC

Analysis of reflectance spectra of UV-absorbing aerosol scenes measured by SCIAMACHY

NASA Astrophysics Data System (ADS)

de Graaf, M.; Stammes, P.; Aben, E. A. A.

2007-01-01

Reflectance spectra from 280-1750 nm of typical desert dust aerosol (DDA) and biomass burning aerosol (BBA) scenes over oceans are presented, measured by the space-borne spectrometer Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY). DDA and BBA are both UV-absorbing aerosols, but their effect on the top-of-atmosphere (TOA) reflectance is different due to differences in the way mineral aerosols and smoke reflect and absorb radiation. Mineral aerosols are typically large, inert particles, found in warm, dry continental air. Smoke particles, on the other hand, are usually small particles, although often clustered, chemically very active and highly variable in composition. Moreover, BBA are hygroscopic and over oceans BBA were invariably found in cloudy scenes. TOA reflectance spectra of typical DDA and BBA scenes were analyzed, using radiative transfer simulations, and compared. The DDA spectrum was successfully simulated using a layer with a bimodal size distribution of mineral aerosols in a clear sky. The spectrum of the BBA scene, however, was determined by the interaction between cloud droplets and smoke particles, as is shown by simulations with a model of separate aerosol and cloud layers and models with internally and externally mixed aerosol/cloud layers. The occurrence of clouds in smoke scenes when sufficient water vapor is present usually prevents the detection of optical properties of these aerosol plumes using space-borne sensors. However, the Absorbing Aerosol Index (AAI), a UV color index, is not sensitive to scattering aerosols and clouds and can be used to detect these otherwise obscured aerosol plumes over clouds. The amount of absorption of radiation can be expressed using the absorption optical thickness. The absorption optical thickness in the DDA case was 0.42 (340 nm) and 0.14 (550 nm) for an aerosol layer of optical thickness 1.74 (550 nm). In the BBA case the absorption optical thickness was 0.18 (340 nm) and 0

Where and What Is Pristine Marine Aerosol?

NASA Astrophysics Data System (ADS)

Russell, L. M.; Frossard, A. A.; Long, M. S.; Burrows, S. M.; Elliott, S.; Bates, T. S.; Quinn, P.

2014-12-01

The sources and composition of atmospheric marine aerosol particles have been measured by functional group composition (from Fourier transform infrared spectroscopy) to identify the organic composition of the pristine primary marine (ocean-derived) particles as 65% hydroxyl, 21% alkane, 6% amine, and 7% carboxylic acid functional groups [Frossard et al., 2014a,b]. Pristine but non-primary components from photochemical reactions (likely from biogenic marine vapor emissions) add carboxylic acid groups. Non-pristine contributions include shipping effluent in seawater and ship emissions, which add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. The pristine primary marine (ocean-derived) organic aerosol composition is nearly identical to model generated primary marine aerosol particles from bubbled seawater, indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the generated primary marine aerosol particles remained nearly constant over a broad range of chlorophyll-a concentrations, the generated primary marine aerosol particle alkane group fraction increased with chlorophyll-a concentrations. In addition, the generated primary marine aerosol particles have a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater hydroxyl group peak location is closer to that of polysaccharides. References Cited Frossard, Amanda A., Lynn M. Russell, Paola Massoli, Timothy S. Bates, and Patricia K. Quinn, "Side-by-Side Comparison of Four Techniques Explains the Apparent Differences in the Organic Composition of Generated and Ambient Marine Aerosol Particles," Aerosol Science and Technology - Aerosol Research Letter

Ground-based Network and Supersite Measurements for Studying Aerosol Properties and Aerosol-Cloud Interactions

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee; Holben, Brent N.

2008-01-01

From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations contain large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite datasets. The development and deployment of AERONET (AErosol RObotic NETwork) sunphotometer network and SMART-COMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile supersite are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To characterize the regional natural and anthropogenic aerosols, AERONET is an internationally federated network of unique sunphotometry that contains more than 250 permanent sites worldwide. Since 1993, there are more than 480 million aerosol optical depth observations and about 15 sites have continuous records longer than 10 years for annual/seasonal trend analyses. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instrument into three categories: flux radiometer, radiance sensor and in-situ probe. Through participation in many satellite remote-sensing/retrieval and validation projects over eight years, SMART-COMMIT have gradually refine( and been proven vital for field deployment. In this paper, we will demonstrate the

Aerosol optical properties along the northeast coast of North America during the New England Air Quality Study-Intercontinental Transport and Chemical Transformation 2004 campaign and the influence of aerosol composition

NASA Astrophysics Data System (ADS)

Wang, Wei; Rood, Mark J.; Carrico, Christian M.; Covert, David S.; Quinn, Patricia K.; Bates, Timothy S.

2007-05-01

Optical and hygroscopic properties of submicrometer diameter aerosol particles were measured on board the NOAA R/V Ronald H. Brown as part of the NEAQS-ITCT field campaign. The campaign occurred along the northeast coast of North America during the summer of 2004. A scanning relative humidity (RH) nephelometry system (humidograph) measured total light scattering and backscattering coefficients (σsp and σbsp, respectively) at three wavelengths (λs) and RH = 26% and while RH was scanned between 40% and 85%. These measurements were combined with aerosol light absorption and composition measurements to describe σsp, σbsp, single scattering albedo (ω), Ångström exponent (å), and hemispheric backscatter fraction (b) at a low reference RH of 26 ± 4% and the aerosol's hygroscopic properties based on its optical response up to 85% RH. Humidogram curve structure was dominated by hygroscopic growth without hysteresis (76% frequency). Dependence of the aerosol's σsp values with changes in RH, fσsp(RH, 26), was observed to decrease with increasing mass fraction of particulate organic matter (POM, FO). Statistical analyses indicated that increasing FO resulted in a less hygroscopic aerosol, while increasing molar equivalence ratio (ER) resulted in lower hysteresis factors based on the aerosols' optical responses at a 0.95 confidence level. ω showed little RH dependence while å and b decreased with increasing RH values. Values for å(λ1, λ2), b, and fσsp(82, 26) increased with increasing λ values. Sensitivities of top of the atmosphere aerosol radiative forcing to changes in ω, b, and σsp with RH were also estimated.

Aerosol Chemical Speciation Monitor (ACSM) Instrument Handbook

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

Watson, Thomas B.

The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) measures particle mass loading and chemical composition in real time for non-refractory sub-micron aerosol particles. The ACSM is designed for long-term unattended deployment and routine monitoring applications.

Retrieval of the complex refractive index of aerosol droplets from optical tweezers measurements.

PubMed

Miles, Rachael E H; Walker, Jim S; Burnham, Daniel R; Reid, Jonathan P

2012-03-07

The cavity enhanced Raman scattering spectrum recorded from an aerosol droplet provides a unique fingerprint of droplet radius and refractive index, assuming that the droplet is homogeneous in composition. Aerosol optical tweezers are used in this study to capture a single droplet and a Raman fingerprint is recorded using the trapping laser as the source for the Raman excitation. We report here the retrieval of the real part of the refractive index with an uncertainty of ± 0.0012 (better than ± 0.11%), simultaneously measuring the size of the micrometre sized liquid droplet with a precision of better than 1 nm (< ± 0.05% error). In addition, the equilibrium size of the droplet is shown to depend on the laser irradiance due to optical absorption, which elevates the droplet temperature above that of the ambient gas phase. Modulation of the illuminating laser power leads to a modulation in droplet size as the temperature elevation is altered. By measuring induced size changes of <1 nm, we show that the imaginary part of the refractive index can be retrieved even when less than 10 × 10(-9) with an accuracy of better than ± 0.5 × 10(-9). The combination of these measurements allows the complex refractive index of a droplet to be retrieved with high accuracy, with the possibility of making extremely sensitive optical absorption measurements on aerosol samples and the testing of frequently used mixing rules for treating aerosol optical properties. More generally, this method provides an extremely sensitive approach for measuring refractive indices, particularly under solute supersaturation conditions that cannot be accessed by simple bulk-phase measurements.

Biomass burning influences on atmospheric composition: A case study to assess the impact of aerosol data assimilation

NASA Astrophysics Data System (ADS)

Keslake, Tim; Chipperfield, Martyn; Mann, Graham; Flemming, Johannes; Remy, Sam; Dhomse, Sandip; Morgan, Will

2016-04-01

The C-IFS (Composition Integrated Forecast System) developed under the MACC series of projects and to be continued under the Copernicus Atmospheric Monitoring System, provides global operational forecasts and re-analyses of atmospheric composition at high spatial resolution (T255, ~80km). Currently there are 2 aerosol schemes implemented within C-IFS, a mass-based scheme with externally mixed particle types and an aerosol microphysics scheme (GLOMAP-mode). The simpler mass-based scheme is the current operational system, also used in the existing system to assimilate satellite measurements of aerosol optical depth (AOD) for improved forecast capability. The microphysical GLOMAP scheme has now been implemented and evaluated in the latest C-IFS cycle alongside the mass-based scheme. The upgrade to the microphysical scheme provides for higher fidelity aerosol-radiation and aerosol-cloud interactions, accounting for global variations in size distribution and mixing state, and additional aerosol properties such as cloud condensation nuclei concentrations. The new scheme will also provide increased aerosol information when used as lateral boundary conditions for regional air quality models. Here we present a series of experiments highlighting the influence and accuracy of the two different aerosol schemes and the impact of MODIS AOD assimilation. In particular, we focus on the influence of biomass burning emissions on aerosol properties in the Amazon, comparing to ground-based and aircraft observations from the 2012 SAMBBA campaign. Biomass burning can affect regional air quality, human health, regional weather and the local energy budget. Tropical biomass burning generates particles primarily composed of particulate organic matter (POM) and black carbon (BC), the local ratio of these two different constituents often determining the properties and subsequent impacts of the aerosol particles. Therefore, the model's ability to capture the concentrations of these two

Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

NASA Astrophysics Data System (ADS)

Fu, P. Q.; Kawamura, K.; Chen, J.; Charrière, B.; Sempéré, R.

2013-02-01

Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m-3 (mean 47.6 ng m-3), accounting for 1.8-11.0% (4.8%) of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA) tracers formed from the oxidation of biogenic volatile organic compounds (VOCs) such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052-53.3 ng m-3 (9.2 ng m-3), followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 10.7% (up to 26.2%) of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8%) and α-pinene SOC (2.9%). In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

NASA Astrophysics Data System (ADS)

Fu, P. Q.; Kawamura, K.; Chen, J.; Charrière, B.; Sempéré, R.

2012-08-01

Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m-3 (mean 47.6 ng m-3), accounting for 1.8-11.0% (4.8%) of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA) tracers formed from the oxidation of biogenic volatile organic compounds (VOCs) such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052-53.3 ng m-3 (9.2 ng m-3), followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 10.7% (up to 26.2%) of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8%) and α-pinene SOC (2.9%). In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

NASA Technical Reports Server (NTRS)

Ghan, Stephen J.; Rissman, Tracey A.; Ellman, Robert; Ferrare, Richard A.; Turner, David; Flynn, Connor; Wang, Jian; Ogren, John; Hudson, James; Jonsson, Haflidi H.;

Measurements of the absorption coefficient of stratospheric aerosols

NASA Technical Reports Server (NTRS)

Ogren, J. A.; Ahlquist, N. C.; Clarke, A. D.; Charlson, R. J.

1981-01-01

The absorption coefficients of stratospheric aerosols are measured using a variation on the integrating plate method. The technique is based on the decrease in the transparency of a substrate when an absorbing aerosol is deposited on it. A Lambert scatterer is placed behind the substrate to integrate forward scattered light and minimize the effect of scattering on the measurement. The low pressure in the stratosphere is used for the direct impaction of particles onto a narrow strip of opal glass. The eight samples collected had a median value of 4 x 10 to the -9th m with an uncertainty of + or - 5 x 10 to the -9th m. If this absorption is due to graphitic carbon, then its concentration is estimated at about 0.4 ng/cu m, or about 0.25% of the total aerosol mass concentration. Estimates of the aerosol scattering coefficients based on satellite extinction inversions result in an aerosol single-scattering albedo in the range of 0.96-1.0.

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.

Radiative Flux Changes by Aerosols from North America, Europe, and Africa over the Atlantic Ocean: Measurements and Calculations from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Russell, P. B.; Hignett, P.; Livingston, J. M.; Schmid, B.; Chien, A.; Bergstrom, R.; Durkee, P. A.; Hobbs, P. V.; Bates, T. S.; Quinn, P. K.;

Chemical composition of individual aerosol particles from working areas in a nickel refinery.

PubMed

Höflich, B L; Wentzel, M; Ortner, H M; Weinbruch, S; Skogstad, A; Hetland, S; Thomassen, Y; Chaschin, V P; Nieboer, E

2000-06-01

Individual aerosol particles (n = 1170) collected at work stations in a nickel refinery were analyzed by wavelength-dispersive electron-probe microanalysis. By placing arbitrary restrictions on the contents of sulfur and silicon, the particles could be divided into four main groups. Scanning electron images indicated that most of the particles examined were relatively small (< or = 2 microm, equivalent projected area diameter), and that their morphology suggested formation from a melt. There was an absence of well-defined phases and simple stoichiometries, indicating that exposures to pure substances such as nickel subsulfide or specific oxides appeared not to occur. Although the elemental composition of particles varied greatly, a rough association was evident with the known elemental content of the refinery intermediates. The implications of the findings for aerosol speciation measurements, toxicological studies and interpretation of adverse health effects are explored.

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

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

Cappa, Christopher D; Atkinson, Dean B

The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements ismore » facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?« less

Biogenic influence on the composition and growth of summertime Arctic aerosol

NASA Astrophysics Data System (ADS)

Willis, M. D.; Burkart, J.; Thomas, J. L.; Koellner, F.; Schneider, J.; Bozem, H.; Hoor, P. M.; Aliabadi, A. A.; Schulz, H.; Herber, A. B.; Leaitch, R.; Abbatt, J.

2016-12-01

The summertime Arctic lower troposphere is a relatively pristine background aerosol environment dominated by nucleation and Aitken mode particles. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties and therefore radiative balance and climate. We present aircraft-based observations of submicron aerosol composition from an aerosol mass spectrometer made during the NETCARE 2014 summertime arctic campaign, based in the Canadian High Arctic, at Resolute Bay, NU (74°N). Under stable and regionally influenced atmospheric conditions with low carbon monoxide and black carbon concentrations (< 100 ppbv and < 50 ng/m3, respectively), we observed organic aerosol (OA)-to-sulfate ratios ranging from 0.5 to > 6 with evidence for enhancement within the lower boundary layer. Methanesulfonic acid (MSA), a marker for the contribution of ocean-derived biogenic sulphur, was also observed in submicron aerosol. MSA-to-sulfate ratios ranged from near zero to 0.3 and tended to increase within the lower boundary layer, suggesting a contribution to aerosol loading from the ocean. In one notable case while flying in the lower boundary layer above open water in Lancaster Sound, we observed growth of small particles, <20 nm in diameter, into sizes above 50 nm. Aerosol growth was correlated with the presence of organic species, trimethylamine, and MSA in particles 80 nm and larger, where the organics were similar to those previously observed in marine settings. The organic-rich aerosol contributed significantly to particles active as cloud condensation nuclei (CCN, supersaturation = 0.6%). Our results highlight the potential importance of secondary organic aerosol formation and its role in growing nucleation mode aerosol into CCN-active sizes in this remote marine environment.

Size-resolved measurements of mixing state and cloud-nucleating ability of aerosols in Nanjing, China

NASA Astrophysics Data System (ADS)

Ma, Yan; Li, Shizheng; Zheng, Jun; Khalizov, Alexei; Wang, Xing; Wang, Zhen; Zhou, Yaoyao

2017-09-01

An integrated aerosol analytical system was deployed in Nanjing, a megacity in the Yangtze River Delta, to measure size-resolved aerosol mixing states, effective densities, cloud condensation nucleus (CCN) activities, and chemical composition in August 2013. It was found that aerosols were predominantly internally mixed. The average effective densities were 1.38 ± 0.09, 1.48 ± 0.08, and 1.53 ± 0.07 g cm-3 for 50, 80, and 120 nm particles, respectively. Although black carbon (BC) represented only 0.3%, 1.6%, and 3.3% of the particle mass, on average, it was present in 7%, 38%, and 47% of the total particle number concentration at 50, 80, and 120 nm, respectively, indicating that BC particles may contribute significantly to the total atmospheric aerosol population. Externally mixed BC was only occasionally observed with an effective density of 0.67-0.97 g cm-3. Aerosols sampled generally exhibited a relatively high CCN activity and hygroscopicity (κ = 0.35 ± 0.13). Both newly formed particles and freshly emitted BC particles were observed to age rapidly from photochemical processes, with a significant enhancement in the particle CCN activity and an increase in the effective density. Aerosols influenced by four different air masses presented similar CCN activation, indicating that CCN activation would be primarily dependent on the particle size rather than the particle origin (and hence original composition). Our results suggest that under highly active photochemical conditions as encountered in this study, particles from both local sources and regional transport can be rapidly converted into efficient CCN by photochemical aging, thereby making important contributions to the atmospheric CCN budget and exerting profound implications on aerosol indirect climate forcing.

A Comparison of Aerosol Measurements from OCO-2 and MODIS

NASA Astrophysics Data System (ADS)

Nelson, R. R.; O'Dell, C.

2016-12-01

The goal of OCO-2 is to use hyperspectral measurements of reflected near-infrared sunlight to retrieve carbon dioxide with high accuracy and precision. This is only possible, however, if the light-path modification effects caused by clouds and aerosols are properly quantified. Even tiny amounts of clouds or aerosols can induce sufficient light-path modifications to lead to large errors in the estimated CO2 column-mean (XCO2). Therefore, it is imperative to evaluate the accuracy of the OCO-2 retrieved aerosol parameters. In this study, we compare OCO-2 retrieved aerosol parameters to Aqua-MODIS observations co-located in time and space. We find that there are significant disagreements between the aerosol information derived from MODIS and the retrieved aerosol parameters from OCO-2. These results are unsurprising, as previous comparisons to AERONET have also been poor. However, the tight co-location between Aqua and OCO-2 in the Afternoon Constellation allows us to examine the potential synergistic use of OCO-2 and MODIS measurements to more accurately constrain aerosol properties, potentially leading to a more accurate CO2 measurement. Specifically, we used select MODIS aerosol properties as the a priori for the OCO-2 retrievals and present the results here. Future studies include investigating the possibility of ingesting the MODIS radiances directly into the OCO-2 retrieval algorithm to further improve OCO-2's aerosol scheme and the resulting measurements.

Characterizing Organic Aerosol Processes and Climatically Relevant Properties via Advanced and Integrated Analyses of Aerosol Mass Spectrometry Datasets from DOE Campaigns and ACRF Measurements. Final report for DE-SC0007178

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

Zhang, Qi

Organic aerosols (OA) are an important but poorly characterized component of the earth’s climate system. Enormous complexities commonly associated with OA composition and life cycle processes have significantly complicated the simulation and quantification of aerosol effects. To unravel these complexities and improve understanding of the properties, sources, formation, evolution processes, and radiative properties of atmospheric OA, we propose to perform advanced and integrated analyses of multiple DOE aerosol mass spectrometry datasets, including two high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) datasets from intensive field campaigns on the aerosol life cycle and the Aerosol Chemical Speciation Monitor (ACSM) datasets from long-term routinemore » measurement programs at ACRF sites. In this project, we will focus on 1) characterizing the chemical (i.e., composition, organic elemental ratios), physical (i.e., size distribution and volatility), and radiative (i.e., sub- and super-saturated growth) properties of organic aerosols, 2) examining the correlations of these properties with different source and process regimes (e.g., primary, secondary, urban, biogenic, biomass burning, marine, or mixtures), 3) quantifying the evolutions of these properties as a function of photochemical processing, 4) identifying and characterizing special cases for important processes such as SOA formation and new particle formation and growth, and 5) correlating size-resolved aerosol chemistry with measurements of radiative properties of aerosols to determine the climatically relevant properties of OA and characterize the relationship between these properties and processes of atmospheric aerosol organics. Our primary goal is to improve a process-level understanding of the life cycle of organic aerosols in the Earth’s atmosphere. We will also aim at bridging between observations and models via synthesizing and translating the results and insights generated from

Elemental and iron isotopic composition of aerosols collected in a parking structure.

PubMed

Majestic, Brian J; Anbar, Ariel D; Herckes, Pierre

2009-09-01

The trace metal contents and iron isotope composition of size-resolved aerosols were determined in a parking structure in Tempe, AZ, USA. Particulate matter (PM)<2.5 microm in diameter (the fine fraction) and PM>2.5 microm were collected. Several air toxics (e.g., arsenic, cadmium, and antimony) were enriched above the crustal average, implicating automobiles as an important source. Extremely high levels of fine copper (up to 1000 ng m(-3)) were also observed in the parking garage, likely from brake wear. The iron isotope composition of the aerosols were found to be +0.15+/-0.03 per thousand and +0.18+/-0.03 per thousand for the PM<2.5 microm and PM>2.5 microm fractions, respectively. The similarity of isotope composition indicates a common source for each size fraction. To better understand the source of iron in the parking garage, the elemental composition in four brake pads (two semi-metallic and two ceramic), two tire tread samples, and two waste oil samples were determined. Striking differences in the metallic and ceramic brake pads were observed. The ceramic brake pads contained 10-20% copper by mass, while the metallic brake pads contained about 70% iron, with very little copper. Both waste oil samples contained significant amounts of calcium, phosphorous, and zinc, consistent with the composition of some engine oil additives. Differences in iron isotope composition were observed between the source materials; most notably between the tire tread (average=+0.02 per thousand) and the ceramic brake linings (average=+0.65 per thousand). Differences in isotopic composition were also observed between the metallic (average=+0.18 per thousand) and ceramic brake pads, implying that iron isotope composition may be used to resolve these sources. The iron isotope composition of the metallic brake pads was found to be identical to the aerosols, implying that brake dust is the dominant source of iron in a parking garage.

A Comparison of Aerosol Optical Property Measurements Made During the DOE Aerosol Intensive Operating Period and Their Effects on Regional Climate

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Hallar, A. G.; Arnott, W. P.; Covert, D.; Elleman, R.; Ogren, J.; Schmid, B.; Luu, A.

2004-01-01

The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult to measure aerosol properties. One of the main purposes of the DOE Aerosol Intensive Operating Period (IOP) flown in May, 2003 was to assess our ability to measure absorption coefficient in situ. This paper compares measurements of aerosol optical properties made during the IOP. Measurements of aerosol absorption coefficient were made by Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter (U. Washington) and on the DOE Cessna 172 (NOAA-C,MDL). Aerosol absorption coefficient was also measured by a photoacoustic instrument (DRI) that was operated on an aircraft for the first time during the IOP. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-AkC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Measurements of absorption coefficient from all of these instruments during appropriate periods are compared. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model.

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

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

Improved Tandem Measurement Techniques for Aerosol Particle Analysis

NASA Astrophysics Data System (ADS)

Rawat, Vivek Kumar

Non-spherical, chemically inhomogeneous (complex) nanoparticles are encountered in a number of natural and engineered environments, including combustion systems (which produces highly non-spherical aggregates), reactors used in gas-phase materials synthesis of doped or multicomponent materials, and in ambient air. These nanoparticles are often highly diverse in size, composition and shape, and hence require determination of property distribution functions for accurate characterization. This thesis focuses on development of tandem mobility-mass measurement techniques coupled with appropriate data inversion routines to facilitate measurement of two dimensional size-mass distribution functions while correcting for the non-idealities of the instruments. Chapter 1 provides the detailed background and motivation for the studies performed in this thesis. In chapter 2, the development of an inversion routine is described which is employed to determine two dimensional size-mass distribution functions from Differential Mobility Analyzer-Aerosol Particle Mass analyzer tandem measurements. Chapter 3 demonstrates the application of the two dimensional distribution function to compute cumulative mass distribution function and also evaluates the validity of this technique by comparing the calculated total mass concentrations to measured values for a variety of aerosols. In Chapter 4, this tandem measurement technique with the inversion routine is employed to analyze colloidal suspensions. Chapter 5 focuses on application of a transverse modulation ion mobility spectrometer coupled with a mass spectrometer to study the effect of vapor dopants on the mobility shifts of sub 2 nm peptide ion clusters. These mobility shifts are then compared to models based on vapor uptake theories. Finally, in Chapter 6, a conclusion of all the studies performed in this thesis is provided and future avenues of research are discussed.

Retrieval of Aerosol Absorption Properties from Satellite Observations

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, Pawan K.; Jethva, H.; Ahn, Chang-Woo

2012-01-01

The Angstrom Absorption Exponent (AAE) is a parameter commonly used to characterize the wavelength-dependence of aerosol absorption optical depth (AAOD). It is closely related to aerosol composition. Black carbon (BC) containing aerosols yield AAE values near unity whereas Organic carbon (OC) aerosol particles are associated with values larger than 2. Even larger AAE values have been reported for desert dust aerosol particles. Knowledge of spectral AAOD is necessary for the calculation of direct radiative forcing effect of aerosols and for inferring aerosol composition. We have developed a satellitebased method of determining the spectral AAOD of absorbing aerosols. The technique uses multi-spectral measurements of upwelling radiation from scenes where absorbing aerosols lie above clouds as indicated by the UV Aerosol Index. For those conditions, the satellite measurement can be explained, using an approximations of Beer's Law (BL), as the upwelling reflectance at the cloud top attenuated by the absorption effects of the overlying aerosol layer. The upwelling reflectance at the cloud-top in an aerosol-free atmospheric column is mainly a function of cloud optical depth (COD). In the proposed method of AAE derivation, the first step is determining COD which is retrieved using a previously developed color-ratio based approach. In the second step, corrections for molecular scattering effects are applied to both the observed ad the calculated cloud reflectance terms, and the spectral AAOD is then derived by an inversion of the BL approximation. The proposed technique will be discussed in detail and application results making use of OMI multi-spectral measurements in the UV-Vis. will be presented.

Nitrogen, Aerosol Composition, and Halogens on a Tall Tower (NACHTT): Overview of a wintertime air chemistry field study in the front range urban corridor of Colorado

NASA Astrophysics Data System (ADS)

Brown, Steven S.; Thornton, Joel A.; Keene, William C.; Pszenny, Alexander A. P.; Sive, Barkley C.; Dubé, William P.; Wagner, Nicholas L.; Young, Cora J.; Riedel, Theran P.; Roberts, James M.; VandenBoer, Trevor C.; Bahreini, Roya; Öztürk, Fatma; Middlebrook, Ann M.; Kim, Saewung; Hübler, Gerhard; Wolfe, Daniel E.

2013-07-01

The Nitrogen, Aerosol Composition, and Halogens on a Tall Tower (NACHTT) field experiment took place during late winter, 2011, at a site 33 km north of Denver, Colorado. The study included fixed-height measurements of aerosols, soluble trace gases, and volatile organic compounds near surface level, as well as vertically resolved measurements of nitrogen oxides, aerosol composition, soluble gas-phase acids, and halogen species from 3 to 270 m above ground level. There were 1928 individual profiles during the three-week campaign to characterize trace gas and aerosol distributions in the lower levels of the boundary layer. Nitrate and ammonium dominated the ionic composition of aerosols and originated primarily from local or regional sources. Sulfate and organic matter were also significant and were associated primarily with longer-range transport to the region. Aerosol chloride was associated primarily with supermicron size fractions and was always present in excess of gas-phase chlorine compounds. The nighttime radical reservoirs, nitryl chloride, ClNO2, and nitrous acid, HONO, were both consistently present in nighttime urban air. Nitryl chloride was especially pronounced in plumes from large point sources sampled aloft at night. Nitrous acid was typically most concentrated near the ground surface and was the dominant contributor (80%) to diurnally averaged primary OH radical production in near-surface air. Large observed mixing ratios of light alkanes, both in near-surface air and aloft, were attributable to local emissions from oil and gas activities.

Aerosol microphysics simulations of the Mt. Pinatubo eruption with the UKCA composition-climate model

NASA Astrophysics Data System (ADS)

Dhomse, S. S.; Emmerson, K. M.; Mann, G. W.; Bellouin, N.; Carslaw, K. S.; Chipperfield, M. P.; Hommel, R.; Abraham, N. L.; Telford, P.; Braesicke, P.; Dalvi, M.; Johnson, C. E.; O'Connor, F.; Morgenstern, O.; Pyle, J. A.; Deshler, T.; Zawodny, J. M.; Thomason, L. W.

2014-01-01

We have enhanced the capability of a microphysical aerosol-chemistry module to simulate the atmospheric aerosol and precursor gases for both tropospheric and stratospheric conditions. Using the Mount Pinatubo eruption (June 1991) as a test case, we evaluate simulated aerosol properties in a composition-climate model against a range of satellite and in-situ observations. Simulations are performed assuming an injection of 20 Tg SO2 at 19-27 km in tropical latitudes, without any radiative feedback from the simulated aerosol. In both quiescent and volcanically perturbed conditions, simulated aerosol properties in the lower stratosphere show reasonable agreement with the observations. The model captures the observed timing of the maximum aerosol optical depth (AOD) and its decay timescale in both tropics and Northern Hemisphere (NH) mid-latitudes. There is also good qualitative agreement with the observations in terms of spatial and temporal variation of the aerosol effective radius (Reff), which peaks 6-8 months after the eruption. However, the model shows significant biases against some observational data sets. Simulated AOD and Surface Area Density (SAD) in the tropics are substantially higher than the gap-filled satellite data products during the first 6 months after the eruption. The model shows consistently weaker enhancement in Reff compared to satellite and in-situ measurements. Simulated aerosol particle size distribution is also compared to NH mid-latitude in-situ balloon sounding measurements of size-resolved number concentrations. Before the eruption, the model captures the observed profiles of lower stratospheric particle number concentrations with radii larger than 5, 150 and 250 nm (N5, N150 and N250) very well. However, in the first 6 months after the eruption, the model shows high bias in N5 concentrations in the lower stratosphere, suggesting too strong nucleation. Following particle growth via condensation and coagulation, this bias in the finest

Relations Between Cloud Condensation Nuclei And Aerosol Optical Properties Relevant to Remote Sensing: Airborne Measurements in Biomass Burning, Pollution and Dust Aerosol Over North America

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A.; Howell, S.; Kapustin, V.; McNaughton, C.; Zhou, J.; Decarlo, P.; Jimenez, J.; Roberts, G.; Tomlinson, J.; Collins, D.

2008-12-01

Remote sensing of the concentration of cloud condensation nuclei (CCN) would help investigate the indirect effect of tropospheric aerosols on clouds and climate. In order to assess its feasibility, this paper evaluates the spectral-based retrieval technique for aerosol number and seeks one for aerosol solubility, using in-situ aircraft measurements of aerosol size distribution, chemical composition, hygroscopicity, CCN activity and optical properties. Our statistical analysis reveals that the CCN concentration over Mexico can be optically determined to a relative error of <20%, smaller than that for the mainland US and the surrounding oceans (~a factor of 2). Mexico's advantage is four-fold. Firstly, many particles originating from the lightly regulated industrial combustion and biomass burning are large enough to significantly affect light extinction, elevating the correlation between extinction and CCN number in absence of substantial dust. Secondly, the generally low ambient humidity near the major aerosol sources limits the error in the estimated response of particle extinction to humidity changes. Thirdly, because many CCN contain black carbon, light absorption also provides a measure of the CCN concentration. Fourthly, the organic fraction of volatile mass of submicron particles (OMF) is anti-correlated with the wavelength dependence of extinction due to preferential anion uptake by coarse dust, which provides a potential tool for remote-sensing OMF and the particle solubility.

Aerosol composition and the contribution of SOA formation over Mediterranean forests

NASA Astrophysics Data System (ADS)

Freney, Evelyn; Sellegri, Karine; Chrit, Mounir; Adachi, Kouji; Brito, Joel; Waked, Antoine; Borbon, Agnès; Colomb, Aurélie; Dupuy, Régis; Pichon, Jean-Marc; Bouvier, Laetitia; Delon, Claire; Jambert, Corinne; Durand, Pierre; Bourianne, Thierry; Gaimoz, Cécile; Triquet, Sylvain; Féron, Anaïs; Beekmann, Matthias; Dulac, François; Sartelet, Karine

2018-05-01

As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), a series of aerosol and gas-phase measurements were deployed aboard the SAFIRE ATR42 research aircraft in summer 2014. The present study focuses on the four flights performed in late June early July over two forested regions in the south of France. We combine in situ observations and model simulations to aid in the understanding of secondary organic aerosol (SOA) formation over these forested areas in the Mediterranean and to highlight the role of different gas-phase precursors. The non-refractory particulate species measured by a compact aerosol time-of-flight mass spectrometer (cToF-AMS) were dominated by organics (60 to 72 %) followed by a combined contribution of 25 % by ammonia and sulfate aerosols. The contribution from nitrate and black carbon (BC) particles was less than 5 % of the total PM1 mass concentration. Measurements of non-refractory species from off-line transmission electron microscopy (TEM) showed that particles have different mixing states and that large fractions (35 %) of the measured particles were organic aerosol containing C, O, and S but without inclusions of crystalline sulfate particles. The organic aerosol measured using the cToF-AMS contained only evidence of oxidized organic aerosol (OOA), without a contribution of fresh primary organic aerosol. Positive matrix factorization (PMF) on the combined organic-inorganic matrices separated the oxidized organic aerosol into a more-oxidized organic aerosol (MOOA), and a less-oxidized organic aerosol (LOOA). The MOOA component is associated with inorganic species and had higher contributions of m/z 44 than the LOOA factor. The LOOA factor is not associated with inorganic species and correlates well with biogenic volatile organic species measured with a proton-transfer-reaction mass spectrometer, such as isoprene and its oxidation products (methyl vinyl ketone, MVK; methacroleine, MACR; and isoprene hydroxyhydroperoxides

Airborne Sunphotometer, Airborne in-situ, Space-borne, and Ground-Based Measurements of Troposoheric Aerosol in Ace-2

NASA Technical Reports Server (NTRS)

Schmid, Beat; Collins, D.; Gasso, S.; Ostrom, E.; Powell, D.; Welton, E.; Durkee, P.; Livingstron, J.; Russell, P.; Flagan, R.;

Retrievals of aerosol optical and microphysical properties from Imaging Polar Nephelometer scattering measurements

NASA Astrophysics Data System (ADS)

Reed Espinosa, W.; Remer, Lorraine A.; Dubovik, Oleg; Ziemba, Luke; Beyersdorf, Andreas; Orozco, Daniel; Schuster, Gregory; Lapyonok, Tatyana; Fuertes, David; Vanderlei Martins, J.

2017-03-01

A method for the retrieval of aerosol optical and microphysical properties from in situ light-scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high-accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3 to 177°. The resulting retrieval produces particle size distributions (PSDs) that agree, within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, with a refractive index that is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represents the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the real refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs.

Development and first application of an Aerosol Collection Module (ACM) for quasi online compound specific aerosol measurements

NASA Astrophysics Data System (ADS)

Hohaus, Thorsten; Kiendler-Scharr, Astrid; Trimborn, Dagmar; Jayne, John; Wahner, Andreas; Worsnop, Doug

2010-05-01

Atmospheric aerosols influence climate and human health on regional and global scales (IPCC, 2007). In many environments organics are a major fraction of the aerosol influencing its properties. Due to the huge variety of organic compounds present in atmospheric aerosol current measurement techniques are far from providing a full speciation of organic aerosol (Hallquist et al., 2009). The development of new techniques for compound specific measurements with high time resolution is a timely issue in organic aerosol research. Here we present first laboratory characterisations of an aerosol collection module (ACM) which was developed to allow for the sampling and transfer of atmospheric PM1 aerosol. The system consists of an aerodynamic lens system focussing particles on a beam. This beam is directed to a 3.4 mm in diameter surface which is cooled to -30 °C with liquid nitrogen. After collection the aerosol sample can be evaporated from the surface by heating it to up to 270 °C. The sample is transferred through a 60cm long line with a carrier gas. In order to test the ACM for linearity and sensitivity we combined it with a GC-MS system. The tests were performed with octadecane aerosol. The octadecane mass as measured with the ACM-GC-MS was compared versus the mass as calculated from SMPS derived total volume. The data correlate well (R2 0.99, slope of linear fit 1.1) indicating 100 % collection efficiency. From 150 °C to 270 °C no effect of desorption temperature on transfer efficiency could be observed. The ACM-GC-MS system was proven to be linear over the mass range 2-100 ng and has a detection limit of ~ 2 ng. First experiments applying the ACM-GC-MS system were conducted at the Jülich Aerosol Chamber. Secondary organic aerosol (SOA) was formed from ozonolysis of 600 ppbv of b-pinene. The major oxidation product nopinone was detected in the aerosol and could be shown to decrease from 2 % of the total aerosol to 0.5 % of the aerosol over the 48 hours of

Long-term aerosol measurements in Gran Canaria, Canary Islands: Particle concentration, sources and elemental composition

NASA Astrophysics Data System (ADS)

Gelado-Caballero, MaríA. D.; López-GarcíA, Patricia; Prieto, Sandra; Patey, Matthew D.; Collado, Cayetano; HéRnáNdez-Brito, José J.

2012-02-01

There are very few sets of long-term measurements of aerosol concentrations over the North Atlantic Ocean, yet such data is invaluable in quantifying atmospheric dust inputs to this ocean region. We present an 8-year record of total suspended particles (TSP) collected at three stations on Gran Canaria Island, Spain (Taliarte at sea level, Tafira 269 m above sea level (a.s.l.) and Pico de la Gorra 1930 m a.s.l.). Using wet and dry deposition measurements, the mean dust flux was calculated at 42.3 mg m-2 d-1. Air mass back trajectories (HYSPLIT, NOAA) suggested that the Sahara desert is the major source of African dust (dominant during 32-50% of days), while the Sahel desert was the major source only 2-10% of the time (maximum in summer). Elemental composition ratios of African samples indicate that, despite the homogeneity of the dust in collected samples, some signatures of the bedrocks can still be detected. Differences were found for the Sahel, Central Sahara and North of Sahara regions in Ti/Al, Mg/Al and Ca/Al ratios, respectively. Elements often associated with pollution (Pb, Cd, Ni, Zn) appeared to share a common origin, while Cu may have a predominantly local source, as suggested by a decrease in the enrichment factor (EF) of Cu during dust events. The inter-annual variability of dust concentrations is investigated in this work. During winter, African dust concentration measurements at the Pico de la Gorra station were found to correlate with the North Atlantic Oscillation (NAO) index.

Validation of Satellite Aerosol Retrievals from AERONET Ground-Based Measurements

NASA Technical Reports Server (NTRS)

Holben, Brent; Remer, Lorraine; Torres, Omar; Zhao, Tom; Smith, David E. (Technical Monitor)

2001-01-01

Accurate and comprehensive assessment of the parameters that control key atmospheric and biospheric processes including assessment of anthropogenic effects on climate change is a fundamental measurement objective of NASA's EOS program (King and Greenstone, 1999). Satellite assessment programs and associated global climate models require validation and additional parameterization with frequent reliable ground-based observations. A critical and highly uncertain element of the measurement program is characterization of tropospheric aerosols requiring basic observations of aerosols optical and microphysical properties. Unfortunately as yet we do not know the aerosol burden man is contributing to the atmosphere and thus we will have no definitive measure of change for the future. This lack of aerosol assessment is the impetus for some of the EOS measurement activities (Kaufman et al., 1997; King et al., 1999) and the formation of the AERONET program (Holben et al., 1998). The goals of the AERONET program are to develop long term monitoring at globally distributed sites providing critical data for multiannual trend changes in aerosol loading and optical properties with the specific goal of providing a data base for validation of satellite derived aerosol optical properties. The AERONET program has evolved into an international federated network of approximately 100 ground-based remote sensing monitoring stations to characterize the optical and microphysical properties of aerosols.

Insights into Submicron Aerosol Composition and Sources from the WINTER Aircraft Campaign Over the Eastern US.

NASA Astrophysics Data System (ADS)

Schroder, J. C.; Campuzano Jost, P.; Day, D. A.; Fibiger, D. L.; McDuffie, E. E.; Blake, N. J.; Hills, A. J.; Hornbrook, R. S.; Apel, E. C.; Weinheimer, A. J.; Campos, T. L.; Brown, S. S.; Jimenez, J. L.

2015-12-01

The WINTER aircraft campaign was a recent field experiment to probe the sources and evolution of gas pollutants and aerosols in Northeast US urban and industrial plumes during the winter. A highly customized Aerodyne aerosol mass spectrometer (AMS) was flown on the NCAR C-130 to characterize submicron aerosol composition and evolution. Thirteen research flights were conducted covering a wide range of conditions, including rural, urban, and marine environments during day and night. Organic aerosol (OA) was a large component of the submicron aerosol in the boundary layer. The fraction of OA (fOA) was smaller (35-40%) than in recent US summer campaigns (~60-70%). Biomass burning was observed to be an important source of OA in the boundary layer, which is consistent with recent wintertime studies that show a substantial contribution of residential wood burning to the OA loadings. OA oxygenation (O/C ratio) shows a broad distribution with a substantial fraction of smaller O/C ratios when compared to previous summertime campaigns. Since measurements were rarely made very close to primary sources (i.e. directly above urban areas), this is consistent with oxidative chemistry being slower during winter. SOA formation and aging in the NYC plume was observed during several flights and compared with summertime results from LA (CalNex) and Mexico City (MILAGRO). Additionally, an oxidation flow reactor (OFR) capable of oxidizing ambient air up to several equivalent days of oxidation was deployed for the first time in an aircraft platform. The aerosol outflow of the OFR was sampled with the AMS to provide real-time snapshots of the potential for aerosol formation and aging. For example, a case study of a flight through the Ohio River valley showed evidence of oxidation of SO2 to sulfate. The measured sulfate enhancements were in good agreement with our OFR chemical model. OFR results for SOA will be discussed.

Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign

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

Lee, Y. -N.; Springston, S.; Jayne, J.

2014-01-01

The chemical composition of aerosol particles ( D p ≤ 1.5 μm) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated bymore » non-sea-salt SO 4 2−, followed by Na +, Cl −, Org (total organics), NH 4 +, and NO 3 −, in decreasing order of importance; CH 3SO 3 − (MSA), Ca 2+, and K + rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH 4 + to SO 4 2− equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl − deficits caused by both HNO 3 and H 2SO 4, but for the most part were externally mixed with particles, mainly SO 4 2−. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH 3 is present between 72° W and 76° W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31° S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol concentrations were negligible. Finally, the very low levels of CH 3SO 3 − observed as well as the correlation between SO 4 2− and NO 3 − (which is thought primarily anthropogenic) suggest a limited contribution of DMS to SO 4 2− aerosol

Twilight sky brightness measurements as a useful tool for stratospheric aerosol investigations

NASA Astrophysics Data System (ADS)

Mateshvili, Nina; Fussen, Didier; Vanhellemont, Filip; Bingen, Christine; KyröLä, Erkki; Mateshvili, Iuri; Mateshvili, Giuli

2005-05-01

In this paper we demonstrate how twilight sky brightness measurements can be used to obtain information about stratospheric aerosols. Beside this, the measurements of the distribution and the variability of the twilight sky brightness may help to understand how the stratospheric aerosols affect the radiation field, which is important for correct calculations of photodissociation rates. Multispectral measurements of twilight sky brightness were carried out in Abastumani Observatory (41.8°N, 42.8°E), Georgia, South Caucasus, during the period (1991-1993) when the level of stratospheric aerosols was substantially enhanced after the 1991 Mount Pinatubo eruption. The twilight sky brightness was measured at 9 wavelengths (422, 474, 496, 542, 610, 642, 678, 713, and 820 nm) for solar zenith angles from 89° to 107°. There are clear indications of a growth of the stratospheric aerosol layer after the eruption of Mount Pinatubo that manifests itself by "humps" in twilight sky brightness dependences versus solar zenith angle. Similar features were obtained using a radiative transfer code constrained by the SAGE II aerosol optical thicknesses. It is shown how an enhancement of stratospheric aerosol loading perturbs the twilight sky brightness due to light scattering and absorption in the aerosol layer. The influence of ozone variations and background stratospheric aerosols on twilight sky brightness has also been analyzed. The optical thicknesses of the stratospheric aerosol layer obtained from the twilight measurements of 1990-1993 show a good agreement with SAGE II results. The spectral variations of the stratospheric aerosol extinction for pre-Pinatubo and post-Pinatubo measurements reflect the aerosol growth after the eruption. Finally, the utilization of twilight sky brightness measurements for validation of satellite-based measurements of the stratospheric aerosol is proposed.

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

International Workshop on Stratospheric Aerosols: Measurements, Properties, and Effects

NASA Technical Reports Server (NTRS)

Pueschel, Rudolf F. (Editor)

1991-01-01

Following a mandate by the International Aerosol Climatology Program under the auspices of International Association of Meteorology and Atmospheric Physics International Radiation Commission, 45 scientists from five nations convened to discuss relevant issues associated with the measurement, properties, and effects of stratospheric aerosols. A summary is presented of the discussions on formation and evolution, transport and fate, effects on climate, role in heterogeneous chemistry, and validation of lidar and satellite remote sensing of stratospheric aerosols. Measurements are recommended of the natural (background) and the volcanically enhanced aerosol (sulfuric acid and silica particles), the exhaust of shuttle, civil aviation and supersonic aircraft operations (alumina, soot, and ice particles), and polar stratospheric clouds (ice, condensed nitric and hydrochloric acids).

Lidar Measurements of the Vertical Distribution of Aerosol Optical and Physical Properties over Central Asia

DOE PAGES

Chen, Boris B.; Sverdlik, Leonid G.; Imashev, Sanjar A.; ...

2013-01-01

The vertical structure of aerosol optical and physical properties was measured by Lidar in Eastern Kyrgyzstan, Central Asia, from June 2008 to May 2009. Lidar measurements were supplemented with surface-based measurements of PM 2.5 and PM 10 mass and chemical composition in both size fractions. Dust transported into the region is common, being detected 33% of the time. The maximum frequency occurred in the spring of 2009. Dust transported to Central Asia comes from regional sources, for example, Taklimakan desert and Aral Sea basin, and from long-range transport, for example, deserts of Arabia, Northeast Africa, Iran, and Pakistan. Regional sourcesmore » are characterized by pollution transport with maximum values of coarse particles within the planetary boundary layer, aerosol optical thickness, extinction coefficient, integral coefficient of aerosol backscatter, and minimum values of the Ångström exponent. Pollution associated with air masses transported over long distances has different characteristics during autumn, winter, and spring. During winter, dust emissions were low resulting in high values of the Ångström exponent (about 0.51) and the fine particle mass fraction (64%). Dust storms were more frequent during spring with an increase in coarse dust particles in comparison to winter. The aerosol vertical profiles can be used to lower uncertainty in estimating radiative forcing.« less

A Strategy to Assess Aerosol Direct Radiative Forcing of Climate Using Satellite Radiation Measurements

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Tanre, Didier; Einaudi, Franco (Technical Monitor)

2001-01-01

Atmospheric aerosols have a complex internal chemical composition and optical properties. Therefore it is difficult to model their impact on redistribution and absorption of solar radiation, and the consequent impact on atmospheric dynamics and climate. The use in climate models of isolated aerosol parameters retrieved from satellite data (e.g. optical thickness) may result in inconsistent calculations, if the model assumptions differ from these of the satellite retrieval schemes. Here we suggest a strategy to assess the direct impact of aerosol on the radiation budget at the top and bottom of the atmosphere using satellite and ground based measurements of the spectral solar radiation scattered by the aerosol. This method ensures consistent use of the satellite data and increases its accuracy. For Kaufman and Tanre: Strategy for aerosol direct forcing anthropogenic aerosol in the fine mode (e.g. biomass burning smoke and urban pollution) consistent use of satellite derived optical thickness can yield the aerosol impact on the spectral solar flux with accuracy an order of magnitude better than the optical thickness itself. For example, a simulated monthly average smoke optical thickness of 0.5 at 0.55 microns (forcing of 40-50 W/sq m) derived with an error of 20%, while the forcing can be measured directly with an error of only 0-2 W/sq m. Another example, the effect of large dust particles on reflection of solar flux can be derived three times better than retrievals of optical thickness. Since aerosol impacts not only the top of the atmosphere but also the surface irradiation, a combination of satellite and ground based measurements of the spectral flux, can be the most direct mechanism to evaluate the aerosol effect on climate and assimilate it in climate models. The strategy is applied to measurements from SCAR-B and the Tarfox experiments. In SCAR-B aircraft spectral data are used to derive the 24 hour radiative forcing of smoke at the top of the atmosphere of

Inorganic Salt Interference on CO2+ in Aerodyne AMS and ACSM Organic Aerosol Composition Studies.

PubMed

Pieber, Simone M; El Haddad, Imad; Slowik, Jay G; Canagaratna, Manjula R; Jayne, John T; Platt, Stephen M; Bozzetti, Carlo; Daellenbach, Kaspar R; Fröhlich, Roman; Vlachou, Athanasia; Klein, Felix; Dommen, Josef; Miljevic, Branka; Jiménez, José L; Worsnop, Douglas R; Baltensperger, Urs; Prévôt, André S H

2016-10-04

Aerodyne aerosol mass spectrometer (AMS) and Aerodyne aerosol chemical speciation monitor (ACSM) mass spectra are widely used to quantify organic aerosol (OA) elemental composition, oxidation state, and major environmental sources. The OA CO 2 + fragment is among the most important measurements for such analyses. Here, we show that a non-OA CO 2 + signal can arise from reactions on the particle vaporizer, ion chamber, or both, induced by thermal decomposition products of inorganic salts. In our tests (eight instruments, n = 29), ammonium nitrate (NH 4 NO 3 ) causes a median CO 2 + interference signal of +3.4% relative to nitrate. This interference is highly variable between instruments and with measurement history (percentiles P 10-90 = +0.4 to +10.2%). Other semi-refractory nitrate salts showed 2-10 times enhanced interference compared to that of NH 4 NO 3 , while the ammonium sulfate ((NH 4 ) 2 SO 4 ) induced interference was 3-10 times lower. Propagation of the CO 2 + interference to other ions during standard AMS and ACSM data analysis affects the calculated OA mass, mass spectra, molecular oxygen-to-carbon ratio (O/C), and f 44 . The resulting bias may be trivial for most ambient data sets but can be significant for aerosol with higher inorganic fractions (>50%), e.g., for low ambient temperatures, or laboratory experiments. The large variation between instruments makes it imperative to regularly quantify this effect on individual AMS and ACSM systems.

Measurement of the aerosol absorption coefficient with the nonequilibrium process

NASA Astrophysics Data System (ADS)

Li, Liang; Li, Jingxuan; Bai, Hailong; Li, Baosheng; Liu, Shanlin; Zhang, Yang

2018-02-01

On the basis of the conventional Jamin interferometer,the improved measuring method is proposed that using a polarization type reentrant Jamin interferometer measures atmospheric aerosol absorption coefficient under the photothermal effect.The paper studies the relationship between the absorption coefficient of atmospheric aerosol particles and the refractive index change of the atmosphere.In Matlab environment, the variation curves of the output voltage of the interferometer with different concentration aerosol samples under stimulated laser irradiation were plotted.Besides, the paper also studies the relationship between aerosol concentration and the time required for the photothermal effect to reach equilibrium.When using the photothermal interferometry the results show that the time required for the photothermal effect to reach equilibrium is also increasing with the increasing concentration of aerosol particles,the absorption coefficient and time of aerosol in the process of nonequilibrium are exponentially changing.

Raman Lidar Measurements of Aerosol Optical Properties Performed at CNR- IMAA

NASA Astrophysics Data System (ADS)

Mona, L.; Amodeo, A.; Cornacchia, C.; D'Amico, G.; Madonna, F.; Pandolfi, M.; Pappalardo, G.

2005-12-01

The lidar system for tropospheric aerosol study, located at CNR-IMAA in Tito Scalo, Potenza (40 °36'N, 15°44' E, 760 m above sea level), is a Raman/elastic lidar system operational since May 2000 in the framework of EARLINET (European Aerosol Research LIdar NETwork), the first lidar network for tropospheric aerosol study on continental scale. It provides independent measurements of aerosol extinction and backscatter coefficient profiles at 355 nm and aerosol backscatter profiles at 532 nm. Both the IMAA aerosol lidar system and the used algorithms for the retrieval of aerosol optical parameters have been successfully tested with different intercomparison exercises in the frame of the EARLINET quality assurance program. In the frame of EARLINET, regular measurements are performed three times per week, allowing to study the aerosol content typically present in the planetary boundary layer over Potenza. Particular attention is devoted to Saharan dust intrusions in Europe, and Saharan dust forecasts are distributed to all EARLINET stations. The large dataset of Saharan dust optical properties profiles collected at IMAA allowed to study the contribution of dust particles to the aerosol load typically present in our area as well as to investigate transformations of aerosol optical properties during the transport. Several intensive measurement campaigns have been performed at IMAA with this system to study optical properties of different types of aerosol, and how the transport and modification mechanisms and the water content affect these optical properties. In particular, direct transport of volcanic aerosol emitted in 2002 during the Etna eruptions was observed, and in summer 2004, aerosol layers related to forest fires smoke or pollution plume transported from Alaska, Canada and North America were observed at IMAA during the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) field campaign. Moreover, this system has been used

An Investigation of Aerosol Measurements from the Halogen Occultation Experiment: Validation, Size Distributions, Composition, and Relation to Other Chemical Species

NASA Technical Reports Server (NTRS)

Deshler, Terry; Hervig, Mark E.

1998-01-01

The efforts envisioned within the original proposal (accepted February 1994) and the extension of this proposal (accepted February 1997) included measurement validations, the retrieval of aerosol size distributions and distribution moments, aerosol correction studies, and investigations of polar stratospheric clouds. A majority of the results from this grant have been published. The principal results from this grant are discussed.

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.

Raman Lidar Measurements of Aerosol Extinction and Backscattering. Report 1; Methods and Comparisons

NASA Technical Reports Server (NTRS)

Ferrare, R. A.; Melfi, S. H.; Whiteman, D. N.; Evans, K. D.; Leifer, R.

1998-01-01

This paper examines the aerosol backscattering and extinction profiles measured at night by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site in April 1994. These lidar data are used to derive aerosol profiles for altitudes between 0.0 1 5 and 5 km. Since this lidar detects Raman scattering from nitrogen and oxygen molecules as well as the elastic scattering from molecules and aerosols, it measures both aerosol backscattering and extinction simultaneously. The aerosol extinction/backscattering ratio varied between approximately 30 sr and 75 sr at 351 nm. Aerosol optical thicknesses derived by integrating the lidar profiles of aerosol extinction measured at night between 0. I and 5 km are found to be about 10-40% lower than those measured by a Sun photometer during the day. This difference is attributed to the contribution by stratospheric aerosols not included in the lidar estimates as well as to diurnal differences in aerosol properties and concentrations. Aerosol profiles close to the surface were acquired by pointing the lidar nearly horizontally. Measurements of aerosol scattering from a tower-mounted nephelometer are found to be 40% lower than lidar measurements of aerosol extinction over a wide range of relative humidities even after accounting for the difference in wavelengths. The reasons for this difference are not clear but may be due to the inability of the nephelometer to accurately measure scattering by large particles.

Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2, and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements

NASA Technical Reports Server (NTRS)

Livingston, John M.; Kapustin, Vladimir N.; Schmid, Beat; Russell, Philip B.; Quinn, Patricia K.; Bates, Timothy S.; Durkee, Philip A.; Smith, Peter J.; Freudenthaler, Volker; Wiegner, Matthias

2000-01-01

Analyses of aerosol optical depth (AOD) and columnar water vapor (CWV) measurements acquired with NASA Ames Research Center's six-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V (research vehicle) Professor Vodyanitskiy during the second Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA (National Oceanographic and Atmospheric Administration)-14/AVHRR (Advanced Very High Resolution Radiometer) satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering measured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from

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.

Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements

NASA Technical Reports Server (NTRS)

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

2011-01-01

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

Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

Treesearch

A. A. May; G. R. McMeeking; T. Lee; J. W. Taylor; J. S. Craven; I. Burling; A. P. Sullivan; S. Akagi; J. L. Collett; M. Flynn; H. Coe; S. P. Urbanski; J. H. Seinfeld; R. J. Yokelson; S. M. Kreidenweis

2014-01-01

Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California...

Stratospheric Aerosol and Gas Experiment (SAGE) II and III Aerosol Extinction Measurements in the Arctic Middle and Upper Troposphere

NASA Technical Reports Server (NTRS)

Treffeisen, R. E.; Thomason, L. W.; Strom, J.; Herber, A. B.; Burton, S. P.; Yamanouchi, T.

2006-01-01

In recent years, substantial effort has been expended toward understanding the impact of tropospheric aerosols on Arctic climate and chemistry. A significant part of this effort has been the collection and documentation of extensive aerosol physical and optical property data sets. However, the data sets present significant interpretive challenges because of the diverse nature of these measurements. Among the longest continuous records is that by the spaceborne Stratospheric Aerosol and Gas Experiment (SAGE) II. Although SAGE tropospheric measurements are restricted to the middle and upper troposphere, they may be able to provide significant insight into the nature and variability of tropospheric aerosol, particularly when combined with ground and airborne observations. This paper demonstrates the capacity of aerosol products from SAGE II and its follow-on experiment SAGE III to describe the temporal and vertical variations of Arctic aerosol characteristics. We find that the measurements from both instruments are consistent enough to be combined. Using this combined data set, we detect a clear annual cycle in the aerosol extinction for the middle and upper Arctic troposphere.

Street canyon aerosol pollutant transport measurements.

PubMed

Longley, I D; Gallagher, M W; Dorsey, J R; Flynn, M; Bower, K N; Allan, J D

2004-12-01

Current understanding of dispersion in street canyons is largely derived from relatively simple dispersion models. Such models are increasingly used in planning and regulation capacities but are based upon a limited understanding of the transport of substances within a real canyon. In recent years, some efforts have been made to numerically model localised flow in idealised canyons (e.g., J. Appl. Meteorol. 38 (1999) 1576-89) and stepped canyons (Assimakopoulos V. Numerical modelling of dispersion of atmospheric pollution in and above urban canopies. PhD thesis, Imperial College, London, 2001) but field studies in real canyons are rare. To further such an understanding, a measurement campaign has been conducted in an asymmetric street canyon with busy one-way traffic in central Manchester in northern England. The eddy correlation method was used to determine fluxes of size-segregated accumulation mode aerosol. Measurements of aerosol at a static location were made concurrently with measurements on a platform lift giving vertical profiles. Size-segregated measurements of ultrafine and coarse particle concentrations were also made simultaneously at various heights. In addition, a small mobile system was used to make measurements of turbulence at various pavement locations within the canyon. From this data, various features of turbulent transport and dispersion in the canyon will be presented. The concentration and the ventilation fluxes of vehicle-related aerosol pollutants from the canyon will be related to controlling factors. The results will also be compared with citywide ventilation data from a separate measurement campaign conducted above the urban canopy.

Single particle measurements of the chemical composition of cirrus ice residue during CRYSTAL-FACE

NASA Astrophysics Data System (ADS)

Cziczo, D. J.; Murphy, D. M.; Hudson, P. K.; Thomson, D. S.

2004-02-01

The first real-time, in situ, investigation of the chemical composition of the residue of cirrus ice crystals was performed during July 2002. This study was undertaken on a NASA WB-57F high-altitude research aircraft as part of CRYSTAL-FACE, a field campaign which sought to further our understanding of the relation of clouds, water vapor, and climate by characterizing, among other parameters, anvil cirrus formed about the Florida peninsula. A counter flow virtual impactor (CVI) was used to separate cirrus ice from the unactivated interstitial aerosol particles and evaporate condensed-phase water. Residual material, on a crystal-by-crystal basis, was subsequently analyzed using the NOAA Aeronomy Laboratory's Particle Analysis by Laser Mass Spectrometry (PALMS) instrument. Sampling was performed from 5 to 15 km altitude and from 12° to 28° north latitude within cirrus originating over land and ocean. Chemical composition measurements provided several important results. Sea salt was often incorporated into cirrus, consistent with homogeneous ice formation by aerosol particles from the marine boundary layer. Size measurements showed that large particles preferentially froze over smaller ones. Meteoritic material was found within ice crystals, indicative of a relation between stratospheric aerosol particles and tropospheric clouds. Mineral dust was the dominant residue observed in clouds formed during a dust transport event from the Sahara, consistent with a heterogeneous freezing mechanism. These results show that chemical composition and size are important determinants of which aerosol particles form cirrus ice crystals.

Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2 and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements

NASA Technical Reports Server (NTRS)

Livingston, John M.; Kapustin, Vladimir N.; Schmid, Beat; Russell, Philip B.; Quinn, Patricia K.; Bates, Timothy S.; Durkee, Philip A.; Smith, Peter J.; Freudenthaler, Volker; Wiegner, Matthias;

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

Characterizing the Asian Tropopause Aerosol Layer (ATAL) Using Satellite Observations, Balloon Measurements and a Chemical Transport Model

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.;

A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

DOE PAGES

Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; ...

2016-11-25

Here, we present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography–mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arrangedmore » into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level

A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

NASA Astrophysics Data System (ADS)

Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, Jose L.

2016-11-01

We present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography-mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level resolution on

Retrieval of aerosol profiles combining sunphotometer and ceilometer measurements in GRASP code

NASA Astrophysics Data System (ADS)

Román, R.; Benavent-Oltra, J. A.; Casquero-Vera, J. A.; Lopatin, A.; Cazorla, A.; Lyamani, H.; Denjean, C.; Fuertes, D.; Pérez-Ramírez, D.; Torres, B.; Toledano, C.; Dubovik, O.; Cachorro, V. E.; de Frutos, A. M.; Olmo, F. J.; Alados-Arboledas, L.

2018-05-01

In this paper we present an approach for the profiling of aerosol microphysical and optical properties combining ceilometer and sun/sky photometer measurements in the GRASP code (General Retrieval of Aerosol and Surface Properties). For this objective, GRASP is used with sun/sky photometer measurements of aerosol optical depth (AOD) and sky radiances, both at four wavelengths and obtained from AErosol RObotic NETwork (AERONET), and ceilometer measurements of range corrected signal (RCS) at 1064 nm. A sensitivity study with synthetic data evidences the capability of the method to retrieve aerosol properties such as size distribution and profiles of volume concentration (VC), especially for coarse particles. Aerosol properties obtained by the mentioned method are compared with airborne in-situ measurements acquired during two flights over Granada (Spain) within the framework of ChArMEx/ADRIMED (Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) 2013 campaign. The retrieved aerosol VC profiles agree well with the airborne measurements, showing a mean bias error (MBE) and a mean absolute bias error (MABE) of 0.3 μm3/cm3 (12%) and 5.8 μm3/cm3 (25%), respectively. The differences between retrieved VC and airborne in-situ measurements are within the uncertainty of GRASP retrievals. In addition, the retrieved VC at 2500 m a.s.l. is shown and compared with in-situ measurements obtained during summer 2016 at a high-atitude mountain station in the framework of the SLOPE I campaign (Sierra Nevada Lidar AerOsol Profiling Experiment). VC from GRASP presents high correlation (r = 0.91) with the in-situ measurements, but overestimates them, MBE and MABE being equal to 23% and 43%.

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.;

Lidar characterizations of atmospheric aerosols and clouds

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Burton, S. P.

2017-12-01

Knowledge of the vertical profile, composition, concentration, and size distribution of aerosols is required to quantify the impacts of aerosols on human health, global and regional climate, clouds and precipitation. In particular, radiative forcing due to anthropogenic aerosols is the most uncertain part of anthropogenic radiative forcing, with aerosol-cloud interactions (ACI) as the largest source of uncertainty in current estimates of global radiative forcing. Improving aerosol transport model predictions of the vertical profile of aerosol optical and microphysical characteristics is crucial for improving assessments of aerosol radiative forcing. Understanding how aerosols and clouds interact is essential for investigating the aerosol indirect effect and ACI. Through its ability to provide vertical profiles of aerosol and cloud distributions as well as important information regarding the optical and physical properties of aerosols and clouds, lidar is a crucial tool for addressing these science questions. This presentation describes how surface, airborne, and satellite lidar measurements have been used to address these questions, and in particular how High Spectral Resolution Lidar (HSRL) measurements provide profiles of aerosol properties (backscatter, extinction, depolarization, concentration, size) important for characterizing radiative forcing. By providing a direct measurement of aerosol extinction, HSRL provides more accurate aerosol measurement profiles and more accurate constraints for models than standard retrievals from elastic backscatter lidar, which loses accuracy and precision at lower altitudes due to attenuation from overlying layers. Information regarding particle size and abundance from advanced lidar retrievals provides better proxies for cloud-condensation-nuclei (CCN), which are required for assessing aerosol-cloud interactions. When combined with data from other sensors, advanced lidar measurements can provide information on aerosol and

Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

NASA Astrophysics Data System (ADS)

Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

2015-04-01

Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined here as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1-0.15 and 0.9-1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.

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

Towards retrievals of aerosol chemical composition from satellite observations by POLDER/PARASOL polarimeter

NASA Astrophysics Data System (ADS)

Li, L.; Dubovik, O.; Derimian, Y.; Lapyonok, T.; Schuster, G. L.; Ducos, F.

2016-12-01

The information about composition of aerosols has a great importance for monitoring and understanding of climate and environment dynamics. Such information can be obtained using situ measurements or chemical transport models. However, in situ sampling has limited spatial and temporal coverage, while estimations have large uncertainties. The present work enables the monitoring of aerosol chemical species from space-borne observations, providing observationally-based results with spatial and temporal coverage. Following the ideas of Schuster et al.(2005, 2009, 2016), we retrieve chemical composition directly from remote sensing measurements without intermediate retrieval of the refractive index (in contrast with Schuster's approach). This approach is expected to reduce the influence of modeling uncertainties, and to provide additional constraints in situations where remote sensing observations do not have enough spectral sensitivity to refractive index. One of principal difficulties is the identification of an adequate model for linking refractive index to chemical composition. Therefore, the initial effort of this work has focused on identifying an optimal "chemical composition to refractive index" conversion model. With that purpose, we first tested the retrieval approach using a simplified volume-weighting model and updated by the Maxwell Garnett mixing model. This concept was incorporated into the GRASP algorithm designed to retrieve an extended set of atmospheric parameters from remote sensing observations. Then a series of sensitivity tests using synthetic data of POLDER/PARASOL were conducted, and followed by inversion of real PARASOL observations. The sensitivity tests showed that these two models allow the retrieval to distinguish amongst the assumed chemical species. Results obtained from real PARASOL data demonstrated good agreement with the optical characteristics provided by AERONET (e.g., r2 of AOT 0.9). The obtained patterns of chemical component

RELATIONSHIP BETWEEN MEASURED WATER VAPOR GROWTH AND CHEMISTRY OF ATMOSPHERIC AEROSOL FOR GRAND CANYON, ARIZONA, IN WINTER 1990.

EPA Science Inventory

Size-resolved aerosol growth measurements (growth = moist particle diameter/dry particle diameter) and chemical composition monitoring were conducted during a 3 month period in the winter of 1990 at the South Rim of Grand Canyon National Park, AZ as part of the Navajo Generating ...

Satellite Observations of the Effect of Natural and Anthropogenic Aerosols on Clouds

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.

2006-01-01

Our knowledge of atmospheric aerosols (smoke, pollution, dust or sea salt particles, small enough to be suspended in the air), their evolution, composition, variability in space and time and interaction with clouds and precipitation is still lacking despite decades of research. Understanding the global aerosol system is critical to quantifying anthropogenic climate change, to determine climate sensitivity from observations and to understand the hydrological cycle. While a single instrument was used to demonstrate 50 years ago that the global CO2 levels are rising, posing threat of global warming, we need an array of satellites and field measurements coupled with chemical transport models to understand the global aerosol system. This complexity of the aerosol problem results from their short lifetime (1 week) and variable chemical composition. A new generation of satellites provides exciting opportunities to measure the global distribution of aerosols, distinguishing natural from anthropogenic aerosol and measuring their interaction with clouds and climate.

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

Light Source Effects on Aerosol Photoacoustic Spectroscopy Measurements

PubMed Central

Radney, James G.; Zangmeister, Christopher D.

2016-01-01

Photoacoustic spectroscopy measurements of flame-generated soot aerosol coated with small amounts of water yielded absorption enhancements that were dependent on the laser used: quasi-continuous wave (Q-CW, ≈ 650 ps pulse duration and 78 MHz repetition rate) versus continuous wave (CW). Water coating thickness was controlled by exposing the aerosol to a set relative humidity (RH). At ≈ 85 % RH, the mass of the soot particles increased by an amount comparable to a monolayer of water being deposited and enhanced the measured absorption by 36 % and 15 % for the Q-CW and CW lasers, respectively. Extinction measurements were also performed using a cavity ring-down spectrometer (extinction equals the sum of absorption and scattering) with a CW laser and negligible enhancement was observed at all RH. These findings demonstrate that source choice can impact measurements of aerosols with volatile coatings and that the absorption enhancements at high RH previously measured by Radney and Zangmeister (2015) [1] are the result of laser source used (Q-CW) and not from an increase in the particle absorption cross section. PMID:28066027

Aerosol optical properties measurements by a CAPS single scattering albedo monitor: Comparisons between summer and winter in Beijing, China

NASA Astrophysics Data System (ADS)

Han, Tingting; Xu, Weiqi; Li, Jie; Freedman, Andrew; Zhao, Jian; Wang, Qingqing; Chen, Chen; Zhang, Yingjie; Wang, Zifa; Fu, Pingqing; Liu, Xingang; Sun, Yele

2017-02-01

Aerosol optical properties were measured in Beijing in summer and winter using a state-of-the-art cavity attenuated phase shift single scattering albedo monitor (CAPS PMssa) along with aerosol composition measurements by aerosol mass spectrometers and aethalometers. The SSA directly measured by the CAPS PMssa showed overall agreements with those derived from colocated measurements. However, substantial differences were observed during periods with low SSA values in both summer and winter, suggesting that interpretation of low SSA values needs to be cautious. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 336 (±343) Mm-1 and 44 (±41) Mm-1, respectively, during wintertime, which were approximately twice those observed in summer, while the average SSA was relatively similar, 0.86 (±0.06) and 0.85 (±0.04) in summer and winter, respectively. Further analysis showed that the variations in SSA can be approximately parameterized as a function of mass fraction of secondary particulate matter (fSPM), which is SSA = 0.74 + 0.19 × fSPM (fSPM > 0.3, r2 = 0.85). The contributions of aerosol species to extinction coefficients during the two seasons were also estimated. Our results showed that the light extinction was dominantly contributed by ammonium sulfate (30%) and secondary organic aerosol (22%) in summer, while organic aerosol was the largest contributor (51%) in winter. Consistently, SPM played the major role in visibility degradation in both seasons by contributing 70% of the total extinction.

Detection and Measurement of Unhealthy, Environment-Derived Aerosol Materials in an Emergency Department.

PubMed

Choi, Bryan Y; Kobayashi, Leo; Pathania, Shivany; Miller, Courtney B; Locke, Emma R; Stearns, Branden C; Hudepohl, Nathan J; Patefield, Scott S; Suner, Selim; Williams, Kenneth A; Machan, Jason T; Jay, Gregory D

2015-01-01

To measure unhealthy aerosol materials in an Emergency Department (ED) and identify their sources for mitigation efforts. Based on pilot findings of elevated ED particulate matter (PM) levels, investigators hypothesized that unhealthy aerosol materials derive from exogenous (vehicular) sources at ambulance receiving entrances. The Aerosol Environmental Toxicity in Healthcare-related Exposure and Risk program was conducted as an observational study. Calibrated sensors monitored PM and toxic gases at Ambulance Triage Exterior (ATE), Ambulance Triage Desk (ATD), and control Public Triage Desk (PTD) on a 3/3/3-day cycle. Cassette sampling characterized PM; meteorological and ambulance traffic data were logged. Descriptive and multiple linear regression analyses assessed for interactions between aerosol material levels, location, temporal variables, ambulance activity, and meteorological factors. Sensors acquired 93,682 PM0.3, 90,250 PM2.5, and 93,768 PM5 measurements over 366 days to generate a data set representing at least 85.6% of planned measurements. PM0.3, PM2.5, and PM5 mean counts were lowest in PTD; 56%, 224%, and 223% higher in ATD; and 996%, 200%, and 63% higher in ATE, respectively (all p < .001). Qualitative analyses showed similar PM compositions in ATD and ATE. On multiple linear regression analysis, PM0.3 counts correlated primarily with location; PM2.5 and PM5 counts correlated most strongly with location and ambulance presence. PM < 2.5 and toxic gas concentrations at ATD and PTD patient care areas did not exceed hazard levels; PM0.3 counts did not have formal safety thresholds for comparison. Higher levels of PM were linked with ED ambulance areas, although their health impact is unclear. © The Author(s) 2015.

Aerosol classification using EARLINET measurements for an intensive observational period

NASA Astrophysics Data System (ADS)

Papagiannopoulos, Nikolaos; Mona, Lucia; Pappalardo, Gelsomina

2016-04-01

ACTRIS (Aerosols, Clouds and Trace gases Research Infrastructure Network) organized an intensive observation period during summer 2012. This campaign aimed at the provision of advanced observations of physical and chemical aerosol properties, at the delivery of information about the 3D distribution of European atmospheric aerosols, and at the monitoring of Saharan dust intrusions events. EARLINET (European Aerosol Research Lidar Network) participated in the ACTRIS campaign through the addition of measurements according to the EARLINET schedule as well as daily lidar-profiling measurements around sunset by 11 selected lidar stations for the period from 8 June - 17 July. EARLINET observations during this almost two-month period are used to characterize the optical properties and vertical distribution of long-range transported aerosol over the broader area of Mediterranean basin. The lidar measurements of aerosol intensive parameters (lidar ratio, depolarization, Angstrom exponents) are shown to vary with location and aerosol type. A methodology based on EARLINET observations of frequently observed aerosol types is used to classify aerosols into seven separate types. The summertime Mediterranean basin is prone to African dust aerosols. Two major dust events were studied. The first episode occurred from the 18 to 21 of the June and the second one lasted from 28 June to 6 July. The lidar ratio within the dust layer was found to be wavelength independent with mean values of 58±14 sr at 355 nm and 57±11 sr at 532 nm. For the particle linear depolarization ratio, mean values of 0.27±0.04 at 532 nm have been found. Acknowledgements. The financial support for EARLINET in the ACTRIS Research Infrastructure Project by the European Union's Horizon 2020 research and innovation programme under grant agreement no. 654169 and previously under grant agreement no. 262254 in the Seventh Framework Programme (FP7/2007-2013) is gratefully acknowledged.

Size-specific composition of aerosols in the El Chichon volcanic cloud

NASA Technical Reports Server (NTRS)

Woods, D. C.; Chuan, R. L.

1983-01-01

A NASA U-2 research aircraft flew sampling missions in April, May, July, November, and December 1982 aimed at obtaining in situ data in the stratospheric cloud produced from the March-April 1982 El Chichon eruptions. Post flight analyses provided information on the aerosol composition and morphology. The particles ranged in size from smaller than 0.05 m to larger than 20 m diameter and were quite complex in composition. In the April, May, and July samples the aerosol mass was dominated by magmatic and lithic particles larger than about 3 m. The submicron particles consisted largely of sulfuric acid. Halite particles, believed to be related to a salt dome beneath El Chichon, were collected in the stratosphere in April and May. On the July 23 flight, copper-zinc oxide particles were collected. In July, November, and December, in addition to the volcanic ash and acid particles, carbon-rich particles smaller than about 0.1 m aerodynamic diameter were abundant.

Validation of stratospheric aerosol and gas experiments 1 and 2 satellite aerosol optical depth measurements using surface radiometer data

NASA Technical Reports Server (NTRS)

Kent, G. S.; Mccormick, M. P.; Wang, P.-H.

1994-01-01

The stratospheric aerosol measurement 2, stratospheric aerosol and gas experiment (SAGE) 1, and SAGE 2 series of solar occultation satellite instruments were designed for the study of stratospheric aerosols and gases and have been extensively validated in the stratosphere. They are also capable, under cloud-free conditions, of measuring the extinction due to aerosols in the troposphere. Such tropospheric extinction measurements have yet to be validated by appropriate lidar and in situ techniques. In this paper published atmospheric aerosol optical depth measurements, made from high-altitude observatories during volcanically quiet periods, have been compared with optical depths calculated from local SAGE 1 and SAGE 2 extinction profiles. Surface measurements from three such observatories have been used, one located in Hawaii and two within the continental United States. Data have been intercompared on a seasonal basis at wave-lenths between 0.5 and 1.0 micron and found to agree within the range of measurement errors and expected atmospheric variation. The mean rms difference between the optical depths for corresponding satellite and surface measured data sets is 29%, and the mean ratio of the optical depths is 1.09.

SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels

NASA Technical Reports Server (NTRS)

Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas

2008-01-01

Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.

Multi-wavelength aerosol light absorption measurements in the Amazon rainforest

NASA Astrophysics Data System (ADS)

Saturno, Jorge; Chi, Xuguang; Pöhlker, Christopher; Morán, Daniel; Ditas, Florian; Massabò, Dario; Prati, Paolo; Rizzo, Luciana; Artaxo, Paulo; Andreae, Meinrat

2015-04-01

The most important light-absorbing aerosol is black carbon (BC), which is emitted by incomplete combustion of fossil fuels and biomass. BC is considered the second anthropogenic contributor to global warming. Beyond BC, other aerosols like some organics, dust, and primary biological aerosol particles are able to absorb radiation. In contrast to BC, the light absorption coefficient of these aerosols is wavelength dependent. Therefore, multi-wavelength measurements become important in environments where BC is not the predominant light-absorbing aerosol like in the Amazon. The Amazon Tall Tower Observatory (ATTO) site is located in the remote Amazon rainforest, one of the most pristine continental sites in the world during the wet season. In the dry season, winds coming from the southern hemisphere are loaded with biomass burning aerosol particles originated by farming-related deforestation. BC and aerosol number concentration data from the last two years indicate this is the most polluted period. Two different techniques have been implemented to measure the light absorption at different wavelengths; one of them is the 7-wavelengths Aethalometer, model AE30, an instrument that measures the light attenuation on a filter substrate and requires multiple scattering and filter-loading corrections to retrieve the light absorption coefficient. The other method is an offline technique, the Multi-Wavelength Absorbance Analysis (MWAA), which is able to measure reflectance and absorbance by aerosols collected on a filter and, by means of a radiative model, can retrieve the light absorption coefficient. Filters collected during May-September 2014, comprehending wet-to-dry transition and most of the dry season, were analyzed. The results indicate that the Absorption Ångström Exponent (AAE), a parameter that is directly proportional to the wavelength dependence of the aerosol light absorption, is close to 1.0 during the transition period and slightly decreases in the beginning of

Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

2015-11-01

To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

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

-25%, and 34-51% for sulfate, ammonium, and nitrate, respectively. These comparisons are all close to the stated ±30% accuracy of the ACSM except for nitrate. These discrepancies could be due to positive biases in the ACSM nitrate concentrations from interferences at the NO+ (m/z 30) fragment ion and/or negative artifacts in the nitrate filter measurement (from volatilization of NH4NO3) are also possible. The organic matter OM/OC ratios derived from linear regression of ACSM OM vs. Sunset OC/EC analyzer are 4.18 ± 0.04 and 3.59 ± 0.02 for summer and fall, respectively. Linear correlations of the ACSM NR-PM1 plus EC with TEOM PM2.5 mass are strong (r2 > 0.7) with percentage difference of 19% and 80% during summer and fall, respectively. On the other hand, the ACSM NR-PM1 correlation with FRM PM1 is high (r2 > 0.8) with percentage difference of ±47% over three seasons. Correlation of ACSM NR-PM1 plus EC mass with SEMS-MCPC PM1 volume concentration results in an estimation of aerosol density of 1.61 g cm-3 for fall 2012 period. ACSM organic concentrations measured during this study were obtained using relative ionization efficiency (RIE) values observed in Aerodyne Aerosol Mass Spectrometer (AMS). Explicit calibration of the ACSM relative ionizations for ammonium, nitrate, and sulfate, during this study was shown to improve the comparisons between ACSM and collocated measurements for these species. The accuracy of the organic and total mass concentrations would likely also be improved if organic relative ionization efficiency values for the ACSM were available during this study. Laboratory calibrations of ACSM relative ionization efficiencies using organic particles of known composition are recommended for future studies.

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.

2014-07-01

Currently, there are a limited number of field studies that evaluate the long-term performance of the Aerodyne Aerosol Chemical Speciation Monitor (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. Intercomparison of two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21) indicating that ACSM instruments are capable of stable and reproducible operation. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the filter-adjusted continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Correlations of the ACSM NR-PM1 (non-refractory particulate matter with aerodynamic diameter less than or equal to 1 μm) plus elemental carbon (EC) with tapered element oscillating microbalance (TEOM) PM2.5 and Federal Reference Method (FRM) PM1 mass are strong with r2 > 0.7 and r2 > 0.8, respectively. Discrepancies might be attributed to evaporative losses of semi-volatile species from the filter measurements used to adjust the collocated continuous measurements. This suggests that adjusting the ambient aerosol continuous measurements with results from filter analysis introduced additional bias to the measurements. We also recommend to calibrate the ambient aerosol monitoring instruments using aerosol standards rather than gas-phase standards. The fitting approach for ACSM relative ionization for sulfate was shown to improve the comparisons between ACSM and collocated measurements in the absence of calibrated values, suggesting the importance of adding sulfate calibration into the ACSM calibration routine.

Deriving simple empirical relationships between aerodynamic and optical aerosol measurements and their application

USDA-ARS?s Scientific Manuscript database

Different measurement techniques for aerosol characterization and quantification either directly or indirectly measure different aerosol properties (i.e. count, mass, speciation, etc.). Comparisons and combinations of multiple measurement techniques sampling the same aerosol can provide insight into...

Synthesis of Spherical Carbon Nitride-Based Polymer Composites by Continuous Aerosol-Photopolymerization with Efficient Light Harvesting.

PubMed

Poostforooshan, Jalal; Badiei, Alireza; Kolahdouz, Mohammadreza; Weber, Alfred P

2016-08-24

Here we report a novel, facile, and sustainable approach for the preparation of spherical submicrometer carbon nitride-based polymer composites by a continuous aerosol-photopolymerization process. In this regard, spherical mesoporous carbon nitride (SMCN) nanoparticles were initially prepared via a nanocasting approach using spray-drying synthesized spherical mesoporous silica (SMS) nanoparticles as hard templates. In addition to experimental characterization, the effect of porosity on the light absorption enhancement and consequently the generation rate of electron-hole pairs inside the SMCN was simulated using a three-dimensional finite difference time-domain (FDTD) method. To produce the carbon nitride-based polymer composite, SMCN nanoparticles exhibit excellent performance in photopolymerization of butyl acrylate (PBuA) monomer in the presence of n-methyldiethanolamine (MDEA) as a co-initiator in a continuous aerosol-based process. In this one-pot synthesis, SMCN nanoparticles act not only as photoinitiators but at the same time as fillers and templates. The average aerosol residence time in the photoreactor is about 90 s. The presented aerosol-photopolymerization process avoids the need for solvent and surfactant, operates at room temperature, and, more importantly, is suitable to produce the spherical composite with hydrophobic polymers. Furthermore, we simulated the condition of SMCN nanoparticles during illumination in the gas phase process, which can freely rotate. The results demonstrated that the hole (h(+)) density is almost equally distributed in the whole part of the SMCN nanoparticles due to their rotation, leading to efficient light harvesting and more homogeneous photoreaction. The combination of the outstanding features of environmentally friendly SMCN, photopolymerization, and aerosol processing might open new avenues, especially in green chemistry, to produce novel polymer composites with multifunctional properties.

Organic and inorganic markers and stable C-, N-isotopic compositions of tropical coastal aerosols from megacity Mumbai: sources of organic aerosols and atmospheric processing

NASA Astrophysics Data System (ADS)

Aggarwal, S. G.; Kawamura, K.; Umarji, G. S.; Tachibana, E.; Patil, R. S.; Gupta, P. K.

2012-08-01

To better understand the sources of PM10 samples from Mumbai, India, aerosol chemical compositions, i.e. total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4‰, also suggest that biofuel/biomass burning is the dominant source in both summer and winter seasons. Aerosol mass concentrations of major species increased 3-4 times in winter compared to summer, indicating an enhanced emission from these sources in winter season. Photochemical production tracers, C2 diacid and nssSO42- do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for day- (0.37 ± 0.06 (0.28 ± 0.04)) and nighttime (0.38 ± 0.07 (0.28 ± 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant rather the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from -27.0 to -25.4‰ with slightly lower average (-26.5 ± 0.3‰) in summer than in winter (-25.9 ± 0.3‰). Positive correlation between WSOC/TC ratios and δ13C values suggested that the increment in δ13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests

Measurement and Modeling of Vertically Resolved Aerosol Optical Properties and Radiative Fluxes Over the ARM SGP Site

NASA Technical Reports Server (NTRS)

Schmid, B.; Arnott, P.; Bucholtz, A.; Colarco, P.; Covert, D.; Eilers, J.; Elleman, R.; Ferrare, R.; Flagan, R.; Jonsson, H.

2003-01-01

In order to meet one of its goals - to relate observations of radiative fluxes and radiances to the atmospheric composition - the Department of Energy's Atmospheric Radiation Measurement (ARM) program has pursued measurements and modeling activities that attempt to determine how aerosols impact atmospheric radiative transfer, both directly and indirectly. However, significant discrepancies between aerosol properties measured in situ or remotely remain. One of the objectives of the Aerosol Intensive Operational Period (TOP) conducted by ARM in May 2003 at the ARM Southern Great Plains (SGP) site in north central Oklahoma was to examine and hopefully reduce these differences. The IOP involved airborne measurements from two airplanes over the heavily instrumented SGP site. We give an overview of airborne results obtained aboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. The Twin Otter performed 16 research flights over the SGP site. The aircraft carried instrumentation to perform in-situ measurements of aerosol absorption, scattering, extinction and particle size. This included such novel techniques as the photoacoustic and cavity ring-down methods for in-situ absorption (675 nm) and extinction (675 and 1550 nm) and a new multiwavelength, filter-based absorption photometer (467, 530, 660 nm). A newly developed instrument measured cloud condensation nucleus concentration (CCN) concentrations at two supersaturation levels. Aerosol optical depth and extinction (354-2139 nm) were measured with the NASA Ames Airborne Tracking 14-channel sunphotometer. Furthermore, up-and downwelling solar (broadband and spectral) and infrared radiation were measured using seven individual radiometers. Three up-looking radiometers werer mounted on a newly developed stabilized platform, keeping the instruments level up to aircraft pitch and roll angles of approximately 10(exp 0). This resulted in unprecedented continuous vertical profiles

The Composition of Organic Aerosols in Southeast Asia During The 2006 Haze Episode

NASA Astrophysics Data System (ADS)

Jun, H.; Zielinska, B.; Balasubramanian, R.

2007-12-01

The regional smoke haze in Southeast Asia is a recurring air pollution problem. Uncontrolled forest fires from land-clearing activities in Sumatra and Borneo, and to a lesser extent Malaysia, have occurred almost every dry season since the late 1990s. The smoke haze that took place in October 2006 shrouded an estimated 215,000 square miles of land on Indonesia's islands of Sumatra and Borneo, and persisted for several weeks. Satellite pictures showed numerous hotspots in both Sumatra and Kalimantan. The prevailing, South-Southwesterly, winds blew smoke from land and forest fires in central and south Sumatra to Singapore, affecting the regional air quality significantly and reducing atmospheric visibility. During this haze episode, we carried out an intensive field study in Singapore to characterize the composition of organic aerosols, which usually account for a large fraction of airborne particulate matter (PM). A total of 17 PM samples were collected while the hazy atmospheric conditions persisted in Singapore, and subjected to accelerated solvent extraction with dichloromethane and acetone. The extracted compounds were grouped into three major fractions (n-alkanes, polycyclic aromatic hydrocarbons, and polar organic compounds). More than 180 particulate-bound organic compounds were determined using gas chromatography/mass spectrometry (GC-MS). In order to investigate the origin of organic species, the carbon preference indexes as well as diagnostic ratios were used. The compositional differences of organic aerosols between the haze- and non- haze periods will be presented. The atmospheric implications of the composition of organic aerosols of biomass burning origin will be discussed. Keywords: smoke haze, organic aerosols, n-alkanes, polycyclic aromatic hydrocarbons, polar organic compounds

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements

NASA Technical Reports Server (NTRS)

2002-01-01

Under funding from this proposal we evaluated measurements of stratospheric sulfate aerosols from three platforms. Two were satellite platforms providing solar extinction measurements, the Stratospheric Aerosol and Gas Experiment (SAGE) II using wavelengths from 0.386 - 1.02 microns, and the Halogen Occultation Experiment (HALOE) using wavelengths from 2.45 to 5.26 microns. The third set of measurements was from in situ sampling by balloonborne optical particle counters (OPCs). The goal was to determine the consistency among these data sets. This was accomplished through analysis of the existing measurement records, and through additional balloonborne OPC flights coinciding with new SAGE II observations over Laramie, Wyoming. All analyses used the SAGE II v 6.0 data. This project supported two balloon flights per year over Laramie dedicated to SAGE II coincidence. Because logistical factors, such as poor surface weather or unfavorable payload impact location, can make it difficult to routinely obtain close coincidences with SAGE II, we attempt to conduct nearly every Laramie flight (roughly one per month) in conjunction with a SAGE II overpass. The Laramie flight frequency has varied over the years depending on field commitments and funding sources. Current support for the Laramie measurements is from the National Science Foundation in addition to support from this NASA grant. We have also completed a variety of comparisons using aerosol measurements from SAGE II, OPCs, and HALOE. The instruments were compared for their various estimates of aerosol extinction at the SAGE II wavelengths and for aerosol surface area. Additional results, such as illustrated here, can be found in a recently accepted manuscript describing comparisons between SAGE II, HALOE, and OPCs for the period 1982 - 2000. While overall, the impression from these results is encouraging, the agreement of the measurements changes with latitude, altitude, time, and parameter. In the broadest sense

REAL-TIME MEASUREMENTS OF THE CHEMICAL COMPOSITION OF SIZE-RESOLVED PARTICLES DURING A SANTA ANA WIND EPISODE, CALIFORNIA USA. (R826240)

EPA Science Inventory

Size-resolved particle composition, mass and number concentrations, aerosol scattering coefficients, and prevailing meteorological conditions were measured at the Ellen Browning Scripps Memorial Pier located in La Jolla, California on 15 December 1998. Aerosol particles were s...

Aging of Secondary Organic Aerosol from β-Pinene: Changes in Chemical Composition, Density and Morphology

NASA Astrophysics Data System (ADS)

Sarrafzadeh, M.; Hastie, D. R.

2013-12-01

Biogenic volatile organic compounds (VOC) are emitted in large quantities into the atmosphere. These VOC, which includes β-pinene, can react to produce secondary organic aerosols (SOA), which contribute to a substantial fraction of ambient organic aerosols and are known to adversely affect visibility, climate and health. Despite this, the current knowledge regarding the SOA composition, their physical properties and the chemical aging processes they undergo in the atmosphere is limited. In this study, chemical aging of SOA generated from the photooxidation of β-pinene was investigated in the York University smog chamber. The formation and aging of both gas and particle phase products were analyzed using an atmospheric pressure chemical ionization triple quadrupole mass spectrometer. The density of secondary organic matter was also simultaneously measured over the course of the aging experiments, allowing us to improve our understanding in changes in particle composition that may occur. In addition, particle phase and shape was investigated for generated particles from β-pinene oxidation by scanning electron microscope (SEM). Results of this work, including particle density and morphology will be presented as well as comparisons of gas and particle phase products time profiles during aging.

Sea Spray Aerosol Structure and Composition Using Cryogenic Transmission Electron Microscopy

PubMed Central

2016-01-01

The composition and surface properties of atmospheric aerosol particles largely control their impact on climate by affecting their ability to uptake water, react heterogeneously, and nucleate ice in clouds. However, in the vacuum of a conventional electron microscope, the native surface and internal structure often undergo physicochemical rearrangement resulting in surfaces that are quite different from their atmospheric configurations. Herein, we report the development of cryogenic transmission electron microscopy where laboratory generated sea spray aerosol particles are flash frozen in their native state with iterative and controlled thermal and/or pressure exposures and then probed by electron microscopy. This unique approach allows for the detection of not only mixed salts, but also soft materials including whole hydrated bacteria, diatoms, virus particles, marine vesicles, as well as gel networks within hydrated salt droplets—all of which will have distinct biological, chemical, and physical processes. We anticipate this method will open up a new avenue of analysis for aerosol particles, not only for ocean-derived aerosols, but for those produced from other sources where there is interest in the transfer of organic or biological species from the biosphere to the atmosphere. PMID:26878061

Evaluation of a new microphysical aerosol module in the ECMWF Integrated Forecasting System

NASA Astrophysics Data System (ADS)

Woodhouse, Matthew; Mann, Graham; Carslaw, Ken; Morcrette, Jean-Jacques; Schulz, Michael; Kinne, Stefan; Boucher, Olivier

2013-04-01

The Monitoring Atmospheric Composition and Climate II (MACC-II) project will provide a system for monitoring and predicting atmospheric composition. As part of the first phase of MACC, the GLOMAP-mode microphysical aerosol scheme (Mann et al., 2010, GMD) was incorporated within the ECMWF Integrated Forecasting System (IFS). The two-moment modal GLOMAP-mode scheme includes new particle formation, condensation, coagulation, cloud-processing, and wet and dry deposition. GLOMAP-mode is already incorporated as a module within the TOMCAT chemistry transport model and within the UK Met Office HadGEM3 general circulation model. The microphysical, process-based GLOMAP-mode scheme allows an improved representation of aerosol size and composition and can simulate aerosol evolution in the troposphere and stratosphere. The new aerosol forecasting and re-analysis system (known as IFS-GLOMAP) will also provide improved boundary conditions for regional air quality forecasts, and will benefit from assimilation of observed aerosol optical depths in near real time. Presented here is an evaluation of the performance of the IFS-GLOMAP system in comparison to in situ aerosol mass and number measurements, and remotely-sensed aerosol optical depth measurements. Future development will provide a fully-coupled chemistry-aerosol scheme, and the capability to resolve nitrate aerosol.

Urban aerosol hygroscopicity and CCN activity measured during the MAPS-Seoul 2016 campaign

NASA Astrophysics Data System (ADS)

Kim, N.; Park, M.; Yum, S. S.; Kim, D. S.

2016-12-01

While submicron aerosols in atmosphere and their effects on air quality and climate are a rising issue in atmospheric sciences, scientific understanding of them is still limited due to the lack of comprehensive observations. In particular, studies for hygroscopic properties of aerosols, closely related to cloud condensation nuclei (CCN) activity, are essential to aerosol-cloud-interaction study as aerosols can act as CCN, which crucially influence cloud microphysical and radiative properties. Urban aerosol properties were measured at Olympic Park in Seoul, a typical megacity with various anthropogenic sources, during the Megacity Air Pollution Studies (MAPS-Seoul 2016) campaign (9 May- 12 June 2016) for understanding diverse aspects of air quality problem in Korea. Physical properties of aerosols, including aerosol and CCN number concentration, aerosol size distribution and growth factor were measured by CPC, CCNC, SMPS and H-TDMA, respectively. Simultaneously, size-resolved chemical component of aerosol and water-soluble aerosol mass concentration were measured by AMS and PILS-IC. These measurement data are used for comprehensive analysis. A main focus will be on the relationship between overall properties of aerosols and their CCN activity in urban area. Results from MAPS-Seoul 2015 will also be used as reference for comparison with measurements in 2016 campaign. For example, aerosol number concentrations peaked at 0800, 1500 and 2000 LT due to traffic at rush hours and photochemical reaction in the afternoon. This is slightly different from the results of MAPS-Seoul 2015 campaign that showed two dominant peaks in the morning and afternoon.

Global measurements of coarse-mode aerosol size distributions - first results from the Atmospheric Tomography Mission (ATom)

NASA Astrophysics Data System (ADS)

Weinzierl, B.; Dollner, M.; Schuh, H.; Brock, C. A.; Bui, T. V.; Gasteiger, J.; Froyd, K. D.; Schwarz, J. P.; Spanu, A.; Murphy, D. M.; Katich, J. M.; Kupc, A.; Williamson, C.

2016-12-01

Although coarse-mode aerosol (>1 µm diameter), composed mainly of mineral dust and sea-salt, is highly abundant over large regions of the world, these particles form a particularly poorly understood and characterized subset of atmospheric aerosol constituents. The NASA-sponsored Atmospheric Tomography Mission (ATom) is an unprecedented field program that investigates how human emissions affect air quality and climate change. ATom provides a singular opportunity to characterize the global coarse-mode size distribution by continuously profiling between 0.2 and 13 km with the NASA DC-8 research aircraft while traveling from the high Arctic down south the middle of the Pacific Ocean, to the Southern Ocean and back north over the Atlantic Ocean basin in four seasons. For ATom, the DC-8 aircraft has been equipped with multiple instruments to observe the composition of the air. The coarse mode and cloud particle size distribution is measured in-situ with a Cloud, Aerosol, and Precipitation Spectrometer (CAPS) mounted under the wing of the DC-8 research aircraft. The CAPS consists of an optical spectrometer providing size distributions in the size range between 0.5 and 50 µm and an imager detecting number concentration, size and shape of particles between 15 and 930 µm diameter. Early ATom flights indicated complicated vertical layering: over the sea, we regularly observed sea salt aerosol which extended from the ground up to 0.6-1 km altitude. In addition - depending on the location of the measurements - we frequently found layers with coarse mode aerosol originating from deserts and biomass burning aerosol aloft. In this study, we will present first results of coarse mode aerosol observations from the entire first ATom deployment in summer 2016. We will show vertical profiles of coarse mode aerosol number concentration, discuss their interhemispheric differences, and look into the question how frequently coarse-mode aerosol is externally mixed with submicron black

A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

NASA Astrophysics Data System (ADS)

Zhu, S.; Sartelet, K. N.; Seigneur, C.

2015-06-01

The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

A case study of highly time-resolved evolution of aerosol chemical composition and optical properties during severe haze pollution in Shanghai, China

NASA Astrophysics Data System (ADS)

Zhu, W.; Cheng, Z.; Lou, S.

2017-12-01

Despite of extensive efforts into characterization of the sources in severe haze pollution periods in the megacity of Shanghai, the study of aerosol composition, mass-size distribution and optical properties to PM1 in the pollution periods remain poorly understood. Here we conducted a 47days real-time measurement of submicron aerosol (PM1) composition and size distribution by a High-Resolution Time-of-Flight Aerosol Mass spectrometer (HR-TOF-AMS), particle light scattering by a Cavity Attenuated Phase Shift ALBedo monitor (CAPS-ALB) and Photoacoustic Extinctionmeter (PAX) in Shanghai, China, from November 28, 2016 to January 12, 2017. The average PM1 concentration was 85.9(±14.7) μg/m3 during the pollution period, which was nearly 4 times higher than that of clean period. Increased scattering coefficient during EP was associated with higher secondary inorganic aerosols and organics. We also observed organics mass size distribution for different pollution extents showing different distribution characteristics. There were no obvious differences for ammonium nitrate and ammonium sulfate among the pollution periods, which represented single peak distributions, and peaks ranged at 650-700nm and 700nm, respectively. A strong relationship can be expected between PM1 compounds mass concentration size distribution and scattering coefficient, suggesting that chemical composition, size distribution of the particles and their variations could also contribute to the extinction coefficients. Organics and secondary inorganic species to particle light scattering were quantified. The results showed that organics and ammonium nitrate were the largest contribution to scattering coefficients of PM1. The contribution of (NH4)2SO4 to the light scattering exceeded that of NH4NO3 during clean period due to the enhanced sulfate concentrations. Our results elucidate substantial changes of aerosol composition, formation mechanisms, size distribution and optical properties due to local

In Situ Aerosol Profile Measurements and Comparisons with SAGE 3 Aerosol Extinction and Surface Area Profiles at 68 deg North

NASA Technical Reports Server (NTRS)

2005-01-01

Under funding from this proposal three in situ profile measurements of stratospheric sulfate aerosol and ozone were completed from balloon-borne platforms. The measured quantities are aerosol size resolved number concentration and ozone. The one derived product is aerosol size distribution, from which aerosol moments, such as surface area, volume, and extinction can be calculated for comparison with SAGE III measurements and SAGE III derived products, such as surface area. The analysis of these profiles and comparison with SAGE III extinction measurements and SAGE III derived surface areas are provided in Yongxiao (2005), which comprised the research thesis component of Mr. Jian Yongxiao's M.S. degree in Atmospheric Science at the University of Wyoming. In addition analysis continues on using principal component analysis (PCA) to derive aerosol surface area from the 9 wavelength extinction measurements available from SAGE III. Ths paper will present PCA components to calculate surface area from SAGE III measurements and compare these derived surface areas with those available directly from in situ size distribution measurements, as well as surface areas which would be derived from PCA and Thomason's algorithm applied to the four wavelength SAGE II extinction measurements.

Indirect and semi-direct aerosol campaign: The impact of Arctic aerosols on clouds

DOE PAGES

McFarquhar, Greg M.; Ghan, Steven; Verlinde, Johannes; ...

2011-02-01

A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the boundary layer in the vicinity of Barrow, Alaska, was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC). ISDAC's primary aim was to examine the effects of aerosols, including those generated by Asian wildfires, on clouds that contain both liquid and ice. ISDAC utilized the Atmospheric Radiation Measurement Pro- gram's permanent observational facilities at Barrow and specially deployed instruments measuring aerosol, ice fog, precipitation, and radiation. The National Research Council of Canada Convair-580 flew 27 sorties and collected data using an unprecedented 41more » stateof- the-art cloud and aerosol instruments for more than 100 h on 12 different days. Aerosol compositions, including fresh and processed sea salt, biomassburning particles, organics, and sulfates mixed with organics, varied between flights. Observations in a dense arctic haze on 19 April and above, within, and below the single-layer stratocumulus on 8 and 26 April are enabling a process-oriented understanding of how aerosols affect arctic clouds. Inhomogeneities in reflectivity, a close coupling of upward and downward Doppler motion, and a nearly constant ice profile in the single-layer stratocumulus suggests that vertical mixing is responsible for its longevity observed during ISDAC. Data acquired in cirrus on flights between Barrow and Fairbanks, Alaska, are improving the understanding of the performance of cloud probes in ice. Furthermore, ISDAC data will improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and determine the extent to which surface measurements can provide retrievals of aerosols, clouds, precipitation, and radiative heating.« less

Carbon Isotopic Measurements and Aerosol Optical Determinations during CARES: Indications of the Importance of Background Biogenic Aerosols

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Begum, M.; Sturchio, N. C.; Guilderson, T. P.

2011-12-01

High volume size-fractionated aerosol samples were obtained in Cool, CA during the Carbonaceous Aerosol and Radiative Effects Study (CARES) in June of 2010. This site was chosen to study the regional impacts of carbonaceous aerosols originating from the Sacramento area. Samples were collected for 6 to 24 hour time periods on quartz fiber filters by using slotted impactors to allow for collection of sample size cuts above and below one micron. Both total carbon content and carbon isotopic composition, including 13C/12C and 14C, were determined on the samples. In addition, Ångstrom absorption exponents (AAEs) were determined for the region of 300-900 nm on the sub-micron size cut by using state of the art diffuse reflectance UV-visible spectroscopy with integrating sphere technology. The overall carbonaceous aerosol loadings were found to be quite low and relatively constant during the study, suggesting that most of the aerosols at the site were locally formed background aerosols. The 14C data is consistent with a substantial fraction (~80 %) being from modern carbon sources and 13C/12C results indicate that the carbon source was from C-3 plants. This is consistent with a significant fraction of the aerosols in the area arising from secondary formation from biogenic precursor emissions from trees, most likely mono- and sesquiterpenes. These results are compared to past results obtained in Mexico City and discussed in terms of the potential importance of biogenic emissions to UV absorbing aerosols as these are anticipated to increase with climate change. This work was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64328 and Grant No. DE-FG02-07-ER64329 as part of the Atmospheric Systems Research program.

Evaluation of anthropogenic influence on thermodynamics, gas and aerosol composition of city air

NASA Astrophysics Data System (ADS)

Uzhegova, Nina; Belan, Boris; Antokhin, Pavel; Zhidovkhin, Evgenii; Ivlev, Georgii; Kozlov, Artem; Fofonov, Aleksandr

2010-05-01

In the last 40-50 years there is a global tendency of urbanisation, which is a consequence of most countries' economical development. Concurrently, the issue of environment's ecological state has become critical. Urban air pollution is among the most important ecological problems nowadays. World Health Organization (WHO) points out certain "classical" polluting agents: carbon monoxide (CO), nitric oxide (NO), nitrogen dioxide (NO2), sulphur dioxide (SO2), troposphere ozone (O3) (studied here), as well as lead, carbon dioxide (CO2), aldehydes, soot, benzpyrene and dredges (including dust, haze and smoke) [1]. An evaluation of antropogenic component's weight in the thermodynamical conditions and gas and aerosol composition of a city's atmosphere (by the example of Tomsk) is given in this paper. Tomsk is located at the South of West Siberia and is the administrative center of Tomsk region. The city's area is equal to 294,6 km2. Its population is 512.6 thousands of people. The overall number of registered motor vehicles in the city in 2008 was 131 700. That is, every fourth city inhabitant has a personal car. From 2002 to 2008 the number of motor vehicles in Tomsk has increased by 25 thousands units [2]. This increase consists mostly of passenger cars. There is also a positive trend in fuel consumtion by the city's industries and motor vehicles - from 2004 to 2007 it has increased by 10%. Such a quick rate of transport quantity's increase in the city provides reason to suggest an unfavorable ecological situation in Tomsk. For this study we have used the AKV-2 mobile station designed by the SB RAS Institute of Atmospheric Optics. The station's equipment provides the following measurements [3]: air temperature and humidity; aerosol disperse composition in 15 channels with a particle size range of 0.3-20 µm by use of the Grimm-1.108 aerosol spectrometer; NO, NO2, O3, SO2, CO, CO2 concentration. This paper describes a single experiment conducted in Tomsk. Date of

Imaging aerosol viscosity

NASA Astrophysics Data System (ADS)

Pope, Francis; Athanasiadis, Thanos; Botchway, Stan; Davdison, Nicholas; Fitzgerald, Clare; Gallimore, Peter; Hosny, Neveen; Kalberer, Markus; Kuimova, Marina; Vysniauskas, Aurimas; Ward, Andy

2017-04-01

Organic aerosol particles play major roles in atmospheric chemistry, climate, and public health. Aerosol particle viscosity is important since it can determine the ability of chemical species such as oxidants, organics or water to diffuse into the particle bulk. Recent measurements indicate that OA may be present in highly viscous states; however, diffusion rates of small molecules such as water appear not to be limited by these high viscosities. We have developed a technique for measuring viscosity that allows for the imaging of aerosol viscosity in micron sized aerosols through use of fluorescence lifetime imaging of viscosity sensitive dyes which are also known as 'molecular rotors'. These rotors can be introduced into laboratory generated aerosol by adding minute quantities of the rotor to aerosol precursor prior to aerosolization. Real world aerosols can also be studied by doping them in situ with the rotors. The doping is achieved through generation of ultrafine aerosol particles that contain the rotors; the ultrafine aerosol particles deliver the rotors to the aerosol of interest via impaction and coagulation. This work has been conducted both on aerosols deposited on microscope coverslips and on particles that are levitated in their true aerosol phase through the use of a bespoke optical trap developed at the Central Laser Facility. The technique allows for the direct observation of kinetic barriers caused by high viscosity and low diffusivity in aerosol particles. The technique is non-destructive thereby allowing for multiple experiments to be carried out on the same sample. It can dynamically quantify and track viscosity changes during atmospherically relevant processes such oxidation and hygroscopic growth (1). This presentation will focus on the oxidation of aerosol particles composed of unsaturated and saturated organic species. It will discuss how the type of oxidant, oxidation rate and the composition of the oxidized products affect the time