Biomass burning and its effects on fine aerosol acidity, water content and nitrogen partitioning

NASA Astrophysics Data System (ADS)

Bougiatioti, Aikaterini; Nenes, Athanasios; Paraskevopoulou, Despina; Fourtziou, Luciana; Stavroulas, Iasonas; Liakakou, Eleni; Myriokefalitakis, Stelios; Daskalakis, Nikos; Weber, Rodney; Kanakidou, Maria; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos

2017-04-01

Aerosol acidity is an important property that drives the partitioning of semi-volatile species, the formation of secondary particulate matter and metal and nutrient solubility. Aerosol acidity varies considerably between aerosol types, RH, temperature, the degree of atmospheric chemical aging and may also change during transport. Among aerosol different sources, sea salt and dust have been well studied and their impact on aerosol acidity and water uptake is more or less understood. Biomass burning (BB) on the other hand, despite its significance as a source in a regional and global scale, is much less understood. Currently, there is no practical and accurate enough method, to directly measure the pH of in-situ aerosol. The combination of thermodynamic models, with targeted experimental observations can provide reliable predictions of aerosol particle water and pH, using as input the concentration of gas/aerosol species, temperature (T), and relative humidity (RH). As such an example, ISORROPIA-II (Fountoukis and Nenes, 2007) has been used for the thermodynamic analysis of measurements conducted in downtown Athens during winter 2013, in order to evaluate the effect of BB on aerosol water and acidity. Biomass burning, especially during night time, was found to contribute significantly to the increased organics concentrations, but as well to the BC component associated with wood burning, particulate nitrates, chloride, and potassium. These increased concentrations were found to impact on fine aerosol water, with Winorg having an average concentration of 11±14 μg m-3 and Worg 12±19 μg m-3 with the organic component constituting almost 38% of the total calculated submicron water. When investigating the fine aerosol acidity it was derived that aerosol was generally acidic, with average pH during strong BB influence of 2.8±0.5, value similar to the pH observed for regional aerosol influenced by important biomass burning episodes at the remote background site of

Light absorption by secondary organic aerosol from α-pinene: Effects of oxidants, seed aerosol acidity, and relative humidity

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

Song, Chen; Gyawali, Madhu; Zaveri, Rahul A.

2013-10-25

It is well known that light absorption from dust and black carbon aerosols has a warming effect on climate while light scattering from sulfate, nitrate, and sea salt aerosols has a cooling effect. However, there are large uncertainties associated with light absorption and scattering by different types of organic aerosols, especially in the near-UV and UV spectral regions. In this paper, we present the results from a systematic laboratory study focused on measuring light absorption by secondary organic aerosols (SOAs) generated from dark α-pinene + O 3 and α-pinene + NO x + O 3 systems in the presence ofmore » neutral and acidic sulfate seed aerosols. Light absorption was monitored using photoacoustic spectrometers at four different wavelengths: 355, 405, 532, and 870 nm. Significant light absorption at 355 and 405 nm was observed for the SOA formed from α-pinene + O 3 + NO 3 system only in the presence of highly acidic sulfate seed aerosols under dry conditions. In contrast, no absorption was observed when the relative humidity was elevated to greater than 27% or in the presence of neutral sulfate seed aerosols. Organic nitrates in the SOA formed in the presence of neutral sulfate seed aerosols were found to be nonabsorbing, while the light-absorbing compounds are speculated to be aldol condensation oligomers with nitroxy organosulfate groups that are formed in highly acidic sulfate aerosols. Finally and overall, these results suggest that dark α-pinene + O 3 and α-pinene + NO x + O 3 systems do not form light-absorbing SOA under typical atmospheric conditions.« less

Effects of aerosol formulation to amino acids and fatty acids contents in Haruan extract.

PubMed

Febriyenti; Bai-Baie, Saringat Bin; Laila, Lia

2012-01-01

Haruan (Channa striatus) extract was formulated to aerosol for wound and burn treatment. Haruan extract is containing amino acids and fatty acids that important for wound healing process. The purpose of this study is to observe the effect of formulation and other excipients in the formula to amino acids and fatty acids content in Haruan extract before and after formulated into aerosol. Precolumn derivatization with 6-aminoquinolyl-N-hydroxysuccinimidyl carbamate (AQC) method is used for amino acids analysis. Fatty acids in Haruan extract were esterified using transesterification method to form FAMEs before analyzed using GC. Boron trifluoride-methanol reagent is used for transesterification. Tyrosine and methionine concentrations were different after formulated. The concentrations were decrease. There are six fatty acids have amount that significantly different after formulated into concentrate and aerosol. Contents of these fatty acids were increase. Generally, fatty acids which had content increased after formulated were the long-chain fatty acids. This might be happen because of chain extension process. Saponification and decarboxylation would give the chain extended product. Therefore contents of long-chain fatty acids were increase. Generally, the aerosol formulation did not affect the amino acids concentrations in Haruan extract while some long-chain fatty acids concentrations were increase after formulated into concentrate and aerosol.

Stratospheric Sulfuric Acid and Black Carbon Aerosol Measured During POLARIS and its Role in Ozone Chemistry

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Pueschel, R. F.; Drdla, K.; Verma, S.; Gore, Warren J. (Technical Monitor)

1998-01-01

Stratospheric aerosol can affect the environment in three ways. Sulfuric acid aerosol have been shown to act as sites for the reduction of reactive nitrogen and chlorine and as condensation sites to form Polar Stratospheric Clouds, under very cold conditions, which facilitate ozone depletion. Recently, modeling studies have suggested a link between BCA (Black Carbon Aerosol) and ozone chemistry. These studies suggest that HNO3, NO2, and O3 may be reduced heterogeneously on BCA particles. The ozone reaction converts ozone to oxygen molecules, while HNO3 and NO2 react to form NOx. Finally, a buildup of BCA could reduce the single-scatter albedo of aerosol below a value of 0.98, a critical value that has been postulated to change the effect of stratospheric aerosol from cooling to warming. Correlations between measured BCA amounts and aircraft usage have been reported. Attempts to link BCA to ozone chemistry and other stratospheric processes have been hindered by questions concerning the amount of BCA that exists in the stratosphere, the magnitude of reaction probabilities, and the scarcity of BCA measurements. The Ames Wire Impactors (AWI) participated in POLARIS as part of the complement of experiments on the NASA ER-2. One of our main objectives was to determine the amount of aerosol surface area, particularly BCA, available for reaction with stratospheric constituents and assess if possible, the importance of these reactions. The AWI collects aerosol and BCA particles on thin Palladium wires that are exposed to the ambient air in a controlled manner. The samples are returned to the laboratory for subsequent analysis. The product of the AWI analysis is the size, surface area, and volume distributions, morphology and elemental composition of aerosol and BCA. This paper presents results from our experiments during POLARIS and puts these measurements in the context of POLARIS and other missions in which we have participated. It describes modifications to the AWI data

Volatility of organic aerosol: evaporation of ammonium sulfate/succinic acid aqueous solution droplets.

PubMed

Yli-Juuti, Taina; Zardini, Alessandro A; Eriksson, Axel C; Hansen, Anne Maria K; Pagels, Joakim H; Swietlicki, Erik; Svenningsson, Birgitta; Glasius, Marianne; Worsnop, Douglas R; Riipinen, Ilona; Bilde, Merete

2013-01-01

Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol.

Volatility of Organic Aerosol: Evaporation of Ammonium Sulfate/Succinic Acid Aqueous Solution Droplets

PubMed Central

2013-01-01

Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol. PMID:24107221

Dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls in fine aerosols over central Alaska: Implications for sources and atmospheric processes

NASA Astrophysics Data System (ADS)

Deshmukh, Dhananjay K.; Mozammel Haque, Md.; Kawamura, Kimitaka; Kim, Yongwon

2018-04-01

The presence of water-soluble dicarboxylic acids in atmospheric aerosols has a significant influence on the regional radiative forcing through direct aerosol effect and cloud formation process. Fine aerosol (PM2.5) samples collected in central Alaska (Fairbanks: 64.51°N and 147.51°W) during summer of 2009 were measured for water-soluble diacids (C2-C12), oxoacids (C2-C9) and α-dicarbonyls (C2-C3) as well as elemental carbon (EC), organic carbon (OC) and water-soluble OC (WSOC) to assess their sources and formation processes. We found the predominance of oxalic acid (C2) followed by malonic (C3) and succinic acid (C4) in Alaskan aerosols. Higher C3/C4 diacid ratios (ave. 1.2) in Alaskan aerosols than those reported for fresh aerosols emitted from fossil fuel combustion (ave. 0.35) and biomass burning (0.51-0.66) suggest that organic aerosols in central Alaska were photochemically processed. The relatively high correlations of major diacids and related compounds with levoglucosan (r = 0.80-0.99) than those with 2-methylglyceric acid (r = 0.59-0.98) suggest that they were significantly produced from biomass burning emission. Strong correlations of C2 with normal-chain saturated diacids (C3-C9: r = 0.80-0.98), glyoxylic acid (ωC2: r = 0.95) and methylglyoxal (MeGly: r = 0.88), together with strong correlations of solar radiation with ratio of C2 to C2-C12 diacids (r = 0.83), ωC2 (r = 0.80) and MeGly (r = 0.82) suggest that oxalic acid in PM2.5 aerosol was produced by the photooxidation of higher homologous diacids, glyoxylic acid and methylglyoxal in the atmosphere of central Alaska. These results reveal that photochemical processing of organic precursors mainly produced from biomass burning control the water-soluble organic chemical composition of fine aerosols in central Alaska.

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

Broadband measurements of aerosol extinction in the ultraviolet spectral region

NASA Astrophysics Data System (ADS)

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

2013-04-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We determined aerosol extinction cross sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross sections over the 360-420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with the literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (± 0.03) + 0.19 (± 0.08)i at 360 nm and 1.63 (± 0.03) + 0.21 (± 0.05)i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (± 0.02) + 0.07 (± 0.06)i at 360 nm and 1.66 (± 0.02) + 0.06 (± 0.04)i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross section, and complex refractive index as a function of wavelength.

Broadband measurements of aerosol extinction in the ultraviolet spectral region

NASA Astrophysics Data System (ADS)

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

2013-01-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross-sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We determined aerosol extinction cross-sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross-sections over the 360-420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (±0.03) + 0.19 (±0.08) i at 360 nm and 1.53 (±0.03) + 0.21 (±0.05) i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (±0.02) + 0.07 (±0.06) i at 360 nm and 1.66 (±0.02) + 0.06 (±0.04) i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross-section, and complex refractive index as a function of wavelength.

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

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.

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.

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...

Compound Specific Isotope Analysis of Fatty Acids in Southern African Aerosols

NASA Astrophysics Data System (ADS)

Billmark, K. A.; Macko, S. A.; Swap, R. J.

2003-12-01

This study, conducted as a part of the Southern African Regional Science Initiative (SAFARI 2000), applied compound specific isotope analysis to describe aerosols at source regions and rural locations. Stable carbon isotopic compositions of individual fatty acids were determined for aerosol samples collected at four sites throughout southern Africa. Mongu, Zambia and Skukuza, South Africa were chosen for their location within intense seasonal Miombo woodland savanna and bushveld savanna biomass burning source regions, respectively. Urban aerosols were collected at Johannesburg, South Africa and rural samples were collected at Sua Pan, Botswana. Fatty acid isotopic compositions varied temporally. Urban aerosols showed significant isotopic enrichment of selected short chain fatty acids (C < 20) compared to aerosols produced during biomass combustion. Sua Pan short chain fatty acid signatures were significantly different from the other non-urban sites, which suggests that sources other than biomass combustion products, such as organic eolian material, impact the Sua Pan aerosol profile. However, a high degree of correlation between Sua Pan and Skukuza long chain fatty acid δ 13C values confirm atmospheric linkages between the two areas and that isotopic signatures of combusted fatty acids are unaltered during atmospheric transport highlighting their potential for use as a conservative tracer.

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.

EFFECT OF ACIDITY ON SECONDARY ORGANIC AEROSOL FORMATION FROM ISOPRENE

EPA Science Inventory

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

Size-dependent chemical ageing of oleic acid aerosol under dry and humidified conditions

NASA Astrophysics Data System (ADS)

Al-Kindi, Suad S.; Pope, Francis D.; Beddows, David C.; Bloss, William J.; Harrison, Roy M.

2016-12-01

A chemical reaction chamber system has been developed for the processing of oleic acid aerosol particles with ozone under two relative humidity conditions: dry and humidified to 65 %. The apparatus consists of an aerosol flow tube, in which the ozonolysis occurs, coupled to a scanning mobility particle sizer (SMPS) and an aerosol time-of-flight mass spectrometer (ATOFMS) which measure the evolving particle size and composition. Under both relative humidity conditions, ozonolysis results in a significant decrease in particle size and mass which is consistent with the formation of volatile products that partition from the particle to the gas phase. Mass spectra derived from the ATOFMS reveal the presence of the typically observed reaction products: azelaic acid, nonanal, oxononanoic acid and nonanoic acid, as well as a range of higher molecular weight products deriving from the reactions of reaction intermediates with oleic acid and its oxidation products. These include octanoic acid and 9- and 10-oxooctadecanoic acid, as well as products of considerably higher molecular weight. Quantitative evaluation of product yields with the ATOFMS shows a marked dependence upon both particle size association (from 0.3 to 2.1 µm diameter) and relative humidity. Under both relative humidity conditions, the percentage residual of oleic acid increases with increasing particle size and the main lower molecular weight products are nonanal and oxononanoic acid. Under dry conditions, the percentage of higher molecular weight products increases with increasing particle size due to the poorer internal mixing of the larger particles. Under humidified conditions, the percentage of unreacted oleic acid is greater, except in the smallest particle fraction, with little formation of high molecular weight products relative to the dry particles. It is postulated that water reacts with reactive intermediates, competing with the processes which produce high molecular weight products. Whilst the

Study on Dicarboxylic Acids in Aerosol Samples with Capillary Electrophoresis

PubMed Central

Adler, Heidi; Sirén, Heli

2014-01-01

The research was performed to study the simultaneous detection of a homologous series of α, ω-dicarboxylic acids (C2–C10), oxalic, malonic, succinic, glutaric, adipic, pimelic, suberic, azelaic, and sebacic acids, with capillary electrophoresis using indirect UV detection. Good separation efficiency in 2,6-pyridinedicarboxylic acid as background electrolyte modified with myristyl trimethyl ammonium bromide was obtained. The dicarboxylic acids were ionised and separated within five minutes. For the study, authentic samples were collected onto dry cellulose membrane filters of a cascade impactor (12 stages) from outdoor spring aerosols in an urban area. Hot water and ultrasonication extraction methods were used to isolate the acids from membrane filters. Due to the low concentrations of acids in the aerosols, the extracts were concentrated with solid-phase extraction (SPE) before determination. The enrichment of the carboxylic acids was between 86 and 134% with sample pretreatment followed by 100-time increase by preparation of the sample to 50 μL. Inaccuracy was optimised for all the sample processing steps. The aerosols contained dicarboxylic acids C2–C10. Then, mostly they contained C2, C5, and C10. Only one sample contained succinic acid. In the study, the concentrations of the acids in aerosols were lower than 10 ng/m3. PMID:24729915

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.

Method for characterization of low molecular weight organic acids in atmospheric aerosols using ion chromatography mass spectrometry.

PubMed

Brent, Lacey C; Reiner, Jessica L; Dickerson, Russell R; Sander, Lane C

2014-08-05

The structural composition of PM2.5 monitored in the atmosphere is usually divided by the analysis of organic carbon, black (also called elemental) carbon, and inorganic salts. The characterization of the chemical composition of aerosols represents a significant challenge to analysts, and studies are frequently limited to determination of aerosol bulk properties. To better understand the potential health effects and combined interactions of components in aerosols, a variety of measurement techniques for individual analytes in PM2.5 need to be implemented. The method developed here for the measurement of organic acids achieves class separation of aliphatic monoacids, aliphatic diacids, aromatic acids, and polyacids. The selective ion monitoring capability of a triple quadropole mass analyzer was frequently capable of overcoming instances of incomplete separations. Standard Reference Material (SRM) 1649b Urban Dust was characterized; 34 organic acids were qualitatively identified, and 6 organic acids were quantified.

EFFECTS OF ENDOGENOUS AMMONIA ON NEUTRALIZATION OF INHALED SULFURIC ACID AEROSOLS

EPA Science Inventory

Nine male beagle dogs were exposed by inhalation to 0, 6 and 10.5 mg/cu.m sulfuric acid aerosols with normal ammonia, increased blood ammonia, and increased inhaled ammonia to determine whether the addition of ammonia affected the toxicity of sulfuric acid aerosols. Exhaled conce...

Measurements of Acidic Gases and Aerosol Species Aboard the NASA DC-8 Aircraft During the Pacific Exploratory Mission in the Tropics (PEM-Tropics A)

NASA Technical Reports Server (NTRS)

Talbot, Robert W.; Dibb, Jack E.

1999-01-01

We received funding to provide measurements of nitric acid (HNO3), formic acid (HCOOH), acetic acid (CH3COOH), and the chemical composition of aerosols aboard the NASA Ames DC-8 research aircraft during the PEM-Tropics A mission. These measurements were successfully completed and the final data resides in the electronic archive (ftp-gte.larc.nasa.gov) at NASA Langley Research Center. For the PEM-Tropics A mission the University of New Hampshire group was first author of four different manuscripts. Three of these have now appeared in the Journal of Geophysical Research-Atmospheres, included in the two section sections on PEM-Tropics A. The fourth manuscript has just recently been submitted to this same journal as a stand alone paper. All four of these papers are included in this report. The first paper (Influence of biomass combustion emissions on the distribution of acidic trace gases over the Southern Pacific basin during austral springtime) describes the large-scale distributions of HNO3, HCOOH, and CH3COOH. Arguments were presented to show, particularly in the middle tropospheric region, that biomass burning emissions from South America and Africa were a major source of acidic gases over the South Pacific basin. The second paper (Aerosol chemical composition and distribution during the Pacific Exploratory Mission (PEM) Tropics) covers the aerosol aspects of our measurement package. Compared to acidic gases, O3, and selected hydrocarbons, the aerosol chemistry showed little influence from biomass burning emissions. The data collected in the marine boundary layer showed a possible marine source of NH3 to the troposphere in equatorial areas. This source had been speculated on previously, but our data was the first collected from an airborne platform to show its large-scale features. The third paper (Constraints on the age and dilution of Pacific Exploratory Mission-Tropics biomass burning plumes from the natural radionuclide tracer Pb-210) utilized the unexpectedly

Measurements of Gases and Aerosols during 2010Cal-Mex

NASA Astrophysics Data System (ADS)

Zheng, J.; Zhang, R.; Molina, L.

2012-04-01

The major goal of the collaborative Cal-Mex 2010 research project is to assess the sources and processing of emissions along the California-Mexico border region and their effects on regional air quality and climate in order to provide scientific information to decision makers of both nations when addressing these two inter-related issues. During the Cal-Mex 2010 field study, the TAMU teams have collected extensive data sets from Tijuana/San Diego border, including volatile organic compounds (VOCs), gaseous sulfuric acid (H2SO4) and a suite set of physical and chemical parameters of aerosols. This comprehensive data set requires additional effort to process and analyze the measurements of gases and aerosols during Cal-Mex 2010. In this talk, preliminary data analysis of gases and aerosols will be presented, including VOCs and particle mixing states, morphology, and effective densities.

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.

Volatility-resolved Measurements of the Chemical Composition of Arctic Aerosol Particles

NASA Astrophysics Data System (ADS)

Ehn, M.; Kroll, J.; Coffman, D.; Quinn, P.; Bates, T.; Williams, E.; Kulmala, M.; Worsnop, D.

2008-12-01

Here we describe measurements of the chemical composition of submicron particles in the Arctic marine boundary layer, taken on board the R/V Knorr during the IPY-ICEALOT mission (March-April 2008). Measurements were made with an Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) for the measurement of the non-refractory fraction of the aerosol, in particular allowing for the determination of the oxygen/carbon (O/C) ratio of the particulate organics and the unambiguous identification of trace inorganic species. Sampling alternated between ambient air and air sent through a thermodenuder (TD), continually scanned between 50 and 250C in order to remove aerosol components by volatility. The mass spectra of particulate matter in the Arctic (including Arctic haze) were dominated by sulfur-containing peaks and the CO2+ ion (at m/z 44), indicating the main non-refractory components of the aerosol are acidic sulfate and highly oxygenated organics. Thermodenuder measurements allow for the clear speciation of sulfate compounds by volatility, as well as the comparison of the degree of atmospheric aging of the organics to measurements taken elsewhere (including at terrestrial sites). AMS measurements will be compared to results from a hygroscopicity tandem differential mobility analyzer (HTDMA), also downstream of the thermodenuder, as well as from semicontinuous (PILS) and offline (filter) measurements of particle composition.

Balloon-Borne Measurements of Total Reactive Nitrogen, Nitric Acid, and Aerosol in the Cold Arctic Stratosphere

NASA Technical Reports Server (NTRS)

Kondo, Y.; Aimedieu, P.; Matthews, W. A.; Fahey, D. W.; Murcray, D. G.; Hofmann, D. J.; Johnston, P. V.; Iwasaka, Y.; Iwata, A.; Sheldon, W. R.

1990-01-01

Total reactive nitrogen (NO(Y)) between 15 and 29 km was measured for the first time on board a balloon within the Arctic cold vortex. Observations of HNO3, aerosol, and ozone were made by instruments on the same balloon gondola which was launched from Esrange, Sweden (68 deg N, 20 deg E) on January 23, 1989. The NO(y) mixing ratio was observed to increase very rapidly from 6 ppbv at 18 km altitude to a maximum of 21 ppbv at 21 km, forming a sharp layer with a thickness of about 2 km. A minimum in the NO(y) mixing ratio of 5 ppbv was found at 27 km. The measured HNO3 profile shows broad similarities to that of NO(y). This observation, together with the observed very low column amount of NO2, shows that NO(x) had been almost totally converted to HNO3, and that NO(y) was composed mainly of HNO3. The enhanced aerosol concentration between 19 and 22 km suggests that the maximum abundance of HNO3 trapped in the form of nitric acid trihydrate (NAT) was about 6 ppbv at 21 km. The sampled air parcels were highly supersaturated with respect to NAT. Although extensive denitrification throughout the stratosphere did not prevail, an indication of denitrification was found at altitudes of 27 and 22 km, and between 18 and 15 km.

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

Hygroscopic behavior of atmospheric aerosols containing nitrate salts and water-soluble organic acids

NASA Astrophysics Data System (ADS)

Jing, Bo; Wang, Zhen; Tan, Fang; Guo, Yucong; Tong, Shengrui; Wang, Weigang; Zhang, Yunhong; Ge, Maofa

2018-04-01

While nitrate salts have critical impacts on environmental effects of atmospheric aerosols, the effects of coexisting species on hygroscopicity of nitrate salts remain uncertain. The hygroscopic behaviors of nitrate salt aerosols (NH4NO3, NaNO3, Ca(NO3)2) and their internal mixtures with water-soluble organic acids were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA). The nitrate salt / organic acid mixed aerosols exhibit varying phase behavior and hygroscopic growth depending upon the type of components in the particles. Whereas pure nitrate salt particles show continuous water uptake with increasing relative humidity (RH), the deliquescence transition is still observed for ammonium nitrate particles internally mixed with organic acids such as oxalic acid and succinic acid with a high deliquescence point. The hygroscopicity of submicron aerosols containing sodium nitrate and an organic acid is also characterized by continuous growth, indicating that sodium nitrate tends to exist in a liquid-like state under dry conditions. It is observed that in contrast to the pure components, the water uptake is hindered at low and moderate RH for calcium nitrate particles containing malonic acid or phthalic acid, suggesting the potential effects of mass transfer limitation in highly viscous mixed systems. Our findings improve fundamental understanding of the phase behavior and water uptake of nitrate-salt-containing aerosols in the atmospheric environment.

Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities.

PubMed

Van Wyngarden, A L; Pérez-Montaño, S; Bui, J V H; Li, E S W; Nelson, T E; Ha, K T; Leong, L; Iraci, L T

Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H 2 SO 4 ) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and 1 H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal

Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities

PubMed Central

Van Wyngarden, A. L.; Pérez-Montaño, S.; Bui, J. V. H.; Li, E. S. W.; Nelson, T. E.; Ha, K. T.; Leong, L.; Iraci, L. T.

2016-01-01

Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40–80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H2SO4) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance–Fourier transform infrared (ATR-FTIR) and 1H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal and

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

DOE PAGES

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

2015-09-25

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

Laboratory study of the effect of oxalic acid on the cloud condensation nuclei activity of mineral dust aerosol

NASA Astrophysics Data System (ADS)

Gierlus, Kelly M.; Laskina, Olga; Abernathy, Tricia L.; Grassian, Vicki H.

2012-01-01

Dicarboxylic acids, which make up a significant portion of the atmospheric organic aerosol, are emitted directly through biomass burning as well as produced through the oxidation of volatile organic compounds. Oxalic acid, the most abundant of the dicarboxylic acids, has been shown by recent field studies to be present in mineral dust aerosol particles. The presence of these internally mixed organic compounds can alter the water absorption and cloud condensation nuclei (CCN) abilities of mineral particles in the Earth's atmosphere. The University of Iowa's Multi-Analysis Aerosol Reactor System ( MAARS) was used to measure the CCN activity of internally mixed particles that were generated from a mixture of either calcite or polystyrene latex spheres (PSLs) in an aqueous solution of oxalic acid. Although PSL is not a mineral dust component, it is used here as a non-reactive, insoluble particle. CCN measurements indicate that the internally mixed oxalate/calcite particles showed nearly identical CCN activity compared to the original calcite particles whereas oxalic acid/PSL internally mixed particles showed much greater CCN activity compared to PSL particles alone. This difference is due to the reaction of calcite with oxalic acid, which produces a relatively insoluble calcium oxalate coating on the particle surface and not a soluble coating as it does on the PSL particle. Our results suggest that atmospheric processing of mineral dust aerosol through heterogeneous processes will likely depend on the mineralogy and the specific chemistry involved. Increase in the CCN activity by incorporation of oxalic acid are only expected for unreactive insoluble dust particles that form a soluble coating.

Aerosol measurements in the winter/spring Antarctic stratosphere. I - Correlative measurements with ozone. II - Impact on polar stratospheric cloud theories

NASA Technical Reports Server (NTRS)

Hofmann, D. J.; Rosen, J. M.; Harder, J. W.

1988-01-01

Aerosol measurements collected from August 25-November 3, 1986 at McMurdo Station using balloon-borne optical particle counters are examined in order to study the relationship between aerosol and ozone distribution and the formation of polar stratospheric clouds (PSCs). Ozone, aerosol, and condensation nuclei profiles, and pressure, temperature, and humidity measurements are analyzed. It is observed that the height of the stratospheric sulfate layer decreases over the period of measurement suggesting that upwelling in the votex is not important in the zone depletion process. Three theories on PSC formation are described, and the effects of the aerosol measurements on the theories are considered. The three theories are: (1) the original theory of water vapor pressure over a solution of H2SO4 of Steele et al. (1983) and Hamill and Mc Master (1984); (2) the nitric acid theory of PSCs of Toon et al. (1986) and Hamill et al. (1986); and (3) the quasi-cirrus cloud theory of Heymsfield (1986).

Solubility of HOBr in Acidic Solution and Implications for Liberation of Halogens Via Aerosol Processing

NASA Technical Reports Server (NTRS)

Iraci, Laura T.; Michelsen, R. R.; Rammer, T. A.; Ashbourn, S. F. M.

2004-01-01

Halogen species are known to catalytically destroy ozone in several regions of the atmosphere. In addition to direct catalytic losses, bromine compounds can indirectly enhance ozone loss through coupling to other radical families. Hypobromous acid (HOBr) is a key species in the linkage of BrOx to ClOx and HOx. The aqueous- phase coupling reaction HOBr + HCI (right arrow) BrCl + H2O may provide a pathway for chlorine activation on sulfate aerosols at temperatures warmer than those required for polar stratospheric cloud formation. We have measured t h e solubility of HOBr in 45 - 70 wt% sulfuric acid solutions. Over the temperature range 201 - 252 K, HOBr is quite soluble in sulfuric acid, H* = 10(exp 4) - 10(exp 7) mol dm(exp -3) atm(exp -1). The expected inverse dependence of H* on temperature was observed, but only a weak dependence on acidity was found. The solubility of HOBr is comparable to that of HBr, indicating that equilibrium concentrations of HOBr could equal or exceed those of HBr in upper tropospheric and lower stratospheric aerosols. Despite the high solubility of HOBr, aerosol volumes are not large enough to sequester a significant fraction of inorganic bromine from the gas phase. Our measurements of HOBr uptake in aqueous sulfuric acid in the presence of other brominated gases show the evolution of gaseous products including Br2O and Br2.

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

New particle formation in the sulfuric acid-dimethylamine-water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

NASA Astrophysics Data System (ADS)

Kürten, Andreas; Li, Chenxi; Bianchi, Federico; Curtius, Joachim; Dias, António; Donahue, Neil M.; Duplissy, Jonathan; Flagan, Richard C.; Hakala, Jani; Jokinen, Tuija; Kirkby, Jasper; Kulmala, Markku; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Onnela, Antti; Rissanen, Matti P.; Simon, Mario; Sipilä, Mikko; Stozhkov, Yuri; Tröstl, Jasmin; Ye, Penglin; McMurry, Peter H.

2018-01-01

A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (˜ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107 cm-3, and dimethylamine mixing ratio of ˜ 40 pptv, i.e., 1 × 109 cm-3).

Aircraft measurement of dicarboxylic acids in the free tropospheric aerosols over the western to central North Pacific

NASA Astrophysics Data System (ADS)

Narukawa, M.; Kawamura, K.; Okada, K.; Zaizen, Y.; Makino, Y.

2003-07-01

Aircraft observation of aerosols was conducted in February 2000, for spatial and vertical distributions of dicarboxylic acids in the free troposphere over the western to central North Pacific. Oxalic, malonic, adipic and azelaic acids were detected in the aerosol samples as the major species. Concentrations of these diacids decreased exponentially with an increase in altitude. They were higher in the western North Pacific (130°E) and decrease eastward. Local flights conducted over Naha (Okinawa), Iwo-jima and Saipan showed that diacid concentrations decreased from the lower to upper troposphere. In the atmosphere over Saipan, where the air is not strongly affected from polluted East Asia, diacid concentrations were almost below the detection limit. Vertical profiles of diacids over Naha and Iwo-jima would be typical over the western North Pacific during winter, suggesting that diacids were significantly injected to the free troposphere from East Asia. Backward air mass trajectories also suggested that the diacids in the free troposphere over the North Pacific are strongly affected by the outflow from East Asia. Diacids, which were produced by both primary emission and secondary photochemical processes in polluted air of East Asia, could alter the physico-chemical properties of aerosols in the free troposphere over the western North Pacific.

Water soluble dicarboxylic acids and related compounds in Antarctic aerosols

NASA Astrophysics Data System (ADS)

Kawamura, Kimitaka; SeméRé, Richard; Imai, Yoshie; Fujii, Yoshiyuki; Hayashi, Masahiko

1996-08-01

Antarctic aerosols collected at Syowa Station were studied for water soluble organic compounds by employing a water extraction and dibutyl ester derivatization and using a capillary gas chromatography (GC) and GC/mass spectrometry (GC/MS). Total carbon and nitrogen were also determined. A homologous series of α,ω-dicarboxylic acids (C2-C11), ω-oxocarboxylic acids (C2-C9), and α-dicarbonyls (C2-C3) were detected, as well as pyruvic acid and aromatic (phthalic) diacid. Succinic (C4) or oxalic (C2) acid was found to be the dominant diacid species, followed by azelaic (C9), adipic (C6), or malonic (C3) acid. Concentration range of the total diacids was 5.9-88 ng m-3, with an average of 29 ng m-3. Highest concentrations were observed in the summer sample with a predominance of succinic acid (61.5 ng m-3), which comprised approximately 70% of the total diacids and accounted for 3.5% of total aerosol carbon (1020 ng m-3). The succinic acid (C4) is likely produced by photooxidation of 4-oxocarboxylic acids, which are present in the atmosphere as intermediates of the photooxidation of unsaturated fatty acids. These results indicate that the Antarctic organic aerosols originate from marine-derived lipids and are transformed largely by photochemical oxidations. ω-Oxocarboxylic acids (C2-C9, 0.36-3.0 ng m-3) also showed the highest concentration in the summer sample, again suggesting a secondary production in the atmosphere of the Antarctic and in the Southern Ocean.

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).

Identification of keto- and hydroxy-dicarboxylic acids in remote marine aerosols from the western North Pacific: GC and GC/TOF-MS measurements

NASA Astrophysics Data System (ADS)

Vani, D.; Kawamura, K.; Tachibana, E.; Boreddy, S. K. R.

2015-12-01

Dicarboxylic acids (diacids) are dominant components of organic aerosols in the atmosphere. They contribute significantly to the total aerosol mass and have a serious impacts on global climate changes. However, studies on keto- and hydroxy-diacids in marine aerosols are limited. Compare to diacids, keto- and hydroxy-diacids are more hygroscopic due to the additional polar groups (OH and CO) and, hence, acts as cloud condensation nuclei (CCN). Molecular characterization of these compounds provides insight into organic aerosols sources and transformation pathways. We collected marine aerosols from remote Chichijima Island in the western North Pacific from December 2010 to November 2011 and studied for water-soluble keto- and hydroxy-diacids. Carboxyl groups were derivatized to dibutyl esters with 14% boron trifluoride/n-butanol, whereas hydroxyl groups were derivatized to trimethylsilyl ethers using N,O-Bis (trimethylsilyl) trifluoroacetamide (BSTFA). After two-step derivatization, samples were injected to GC, GC/MS and GC/TOF-MS. In the GC chromatogram, we detected several new peaks after BSTFA derivatization of dibutyl ester fraction. Based on mass spectral interpretation, we found these peaks as homologues series of hydroxy-diacids and keto-diacids. Some of these hydroxy-diacids have been individually reported in literature in the laboratory photo-oxidation experiments and forest environments samples. But, there are no evidences to prove their sources and formation mechanism in the atmosphere. Here, we report for the first time homologous series of hydroxy-diacids (hC3di-hC6di) and keto-diacid (oxaloacetic acid, enol and keto forms) in remote marine atmosphere. Molecular distributions of hydroxy-diacids generally showed the predominance of malic acid followed by tartronic acid. Both hydroxy- and keto-diacids show significant positive correlation with oxalic acid and SO42-, suggesting that they are generated in the atmosphere and play an important role in the

Measurements of Gas-phase H2so4, Oh, So2 and Aerosol Size Distribution On Mount Zugspitze At The Schneefernerhaus: Estimation of Sources and Sinks of Sulfuric Acid

NASA Astrophysics Data System (ADS)

Uecker, J.; Hanke, M.; Kamm, S.; Umann, B.; Arnold, F.; Poeschl, U.; Niessner, R.

Gas-phase sulfuric acid and OH have been measured by the novel MPI-K ULTRA- CIMS (ultra-trace gas detection by CIMS technique) at the Schneefernerhaus( 2750 m asl; below the summit of Mount Zugspitze, Germany) in October 2001. These mea- surements were accompanied by measurements of SO2 with another MPI-K CIMS instrument and aerosol size distribution measurements by DMPS (differential mobil- ity particle sizer) operated by the Institut fuer Wasserchemie (Technische Universitaet Muenchen). In that way a data set was obtained which allows investigating major sources and sinks of sulfuric acid under relative clean conditions. H2SO4 and espe- cially OH concentrations are relatively well correlated to solar flux. Noon maximum concentrations of OH and H2SO4 of 6.5·106 and 2·106 cm-3, respectively, were ob- served. The average SO2 concentrations were below 20 ppt. The aerosol size distribu- tion was obtained in 39 size ranges from 10 to 1056 nm. Typical aerosol concentrations are in the range of 400 to 1800 cm-3 during the discussed period of time. An estima- tion of the production rate of H2SO4 was inferred building on the reaction of SO2 and OH, while the loss rate was calculated by considering the condensation of H2SO4 on aerosol particles (Fuchs and Sutugin approach). Results of the measurements and calculations will be discussed.

Atmospheric acidity measurements on allegheny mountain and the origins of ambient acidity in the Northeastern United States

NASA Astrophysics Data System (ADS)

Pierson, William R.; Brachaczek, Wanda W.; Gorse, Robert A.; Japar, Steven M.; Norbeck, Joseph M.; Keeler, Gerald J.

Atmospheric acidity as HNO 3(g), SO 2(g), and aerosol H + was measured on Allegheny Mountain and Laurel Hill in southwest Pennsylvania in August 1983. The aerosol H + appeared to represent the net after H 2SO 4 reaction with NH 3(g). The resulting H +/SO 42- ratio depended on SO 42- concentration, approaching that of H 2SO 4 at the highest SO 42- concentrations. The atmosphere was acidic; the average concentrations of HNO 3 (78 nmole m -3) and aerosol H + (205 nmole m -3), NH 4+ (172 nmole m -3) and SO 42- (201 nmole m -3), and the dearth of NH 3(< 15 nmolem -3), show that the proton acidity (HNO 3, H 2SO 4) of the air exceeded the acid-neutralizing capacity of the air by a factor of > 2, with one 10-h period averaging 263 and 844 nmolem -3 for HNO 3 and aerosol H +, respectively. SO 2 added another 900 nmole m -3 (average) of potential H + acidity. HNO 3 and aerosol H + episodes were concurrent, on 7-8 day cycles, unrelated to SO 2 which existed more in short-lived bursts of apparently more local origin. NOx was sporadic like SO 2. Laurel and Allegheny, separated by 35.5 km, were essentially identical in aerosol SO 42-, and in aerosol H +, less so in HNO 3 and especially less so in SO 2; apparently, chemistry involving HNO 3 and aerosol H + or SO 42- was slow compared to inter-site transport times (1-2 h). From growth of bscat and decline of SO 2 during one instance of inter-site transport, daytime rate coefficients for SO 2 oxidation and SO 2 dry deposition were inferred to have been, respectively, ~ 0.05 and ⩽ 0.1 h -1. HNO 3 declined at night. Aerosol H + and SO 42- showed no significant diurnal variation, and O 3 showed very little; these observations, together with high PAN/NO x ratios, indicate that regional transport rather than local chemistry is governing. The O 3 concentration (average 56 ppb or 2178 nmolem -3) connotes an oxidizing atmosphere conducive to acid formation. Highest atmospheric acidity was associated with (1) slow westerly winds

Stable carbon isotopic compositions of total carbon, dicarboxylic acids and glyoxylic acid in the tropical Indian aerosols: Implications for sources and photochemical processing of organic aerosols

NASA Astrophysics Data System (ADS)

Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.; Tachibana, Eri

2011-09-01

The tropical Indian aerosols (PM10) collected on day- and nighttime bases in winter and summer, 2007 from Chennai (13.04°N; 80.17°E) were studied for stable carbon isotopic compositions (δ13C) of total carbon (TC), individual dicarboxylic acids (C2-C9) and glyoxylic acid (ωC2). δ13C values of TC ranged from -23.9‰ to -25.9‰ (-25.0 ± 0.6‰; n = 49). Oxalic (C2) (-17.1 ± 2.5‰), malonic (C3) (-20.8 ± 1.8‰), succinic (C4) (-22.5 ± 1.5‰) and adipic (C6) (-20.6 ± 4.1‰) acids and ωC2 acid (-22.4 ± 5.5‰) were found to be more enriched with 13C compared to TC. In contrast, suberic (C8) (-29.4 ± 1.8‰), phthalic (Ph) (-30.1 ± 3.5‰) and azelaic (C9) (-28.4 ± 5.8‰) acids showed smaller δ13C values than TC. Based on comparisons of δ13C values of TC in Chennai aerosols to those (-24.7 ± 2.2‰) found in unburned cow-dung samples collected from Chennai and isotopic signatures of the particles emitted from point sources, we found that biofuel/biomass burning are the major sources of carbonaceous aerosols in South and Southeast Asia. The decrease in δ13C values of C9 diacid by about 5‰ from winter to summer suggests that tropical plant emissions also significantly contribute to organic aerosol in this region. Significant increase in δ13C values from C4 to C2 diacids in Chennai aerosols could be attributed for their photochemical processing in the tropical atmosphere during long-range transport from source regions.

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.

Hygroscopic Behavior of Multicomponent Aerosols Involving NaCl and Dicarboxylic Acids.

PubMed

Peng, Chao; Jing, Bo; Guo, Yu-Cong; Zhang, Yun-Hong; Ge, Mao-Fa

2016-02-25

Atmospheric aerosols are usually complex mixtures of inorganic and organic compounds. The hygroscopicity of mixed particles is closely related to their chemical composition and interactions between components, which is still poorly understood. In this study, the hygroscopic properties of submicron particles composed of NaCl and dicarboxylic acids including oxalic acid (OA), malonic acid (MA), and succinic acid (SA) with various mass ratios are investigated with a hygroscopicity tandem differential mobility analyzer (HTDMA) system. Both the Zdanovskii-Stokes-Robinson (ZSR) method and extended aerosol inorganics model (E-AIM) are applied to predict the water uptake behaviors of sodium chloride/dicarboxylic acid mixtures. For NaCl/OA mixed particles, the measured growth factors were significantly lower than predictions from the model methods, indicating a change in particle composition caused by chloride depletion. The hygroscopic growth of NaCl/MA particles was well described by E-AIM, and that of NaCl/SA particles was dependent upon mixing ratio. Compared with model predictions, it was determined that water uptake of the NaCl/OA mixture could be enhanced and could be closer to the predictions by addition of levoglucosan or malonic acid, which retained water even at low relative humidity (RH), leading to inhibition of HCl evaporation during dehydration. These results demonstrate that the coexisting hygroscopic species have a strong influence on the phase state of particles, thus affecting chemical interactions between inorganic and organic compounds as well as the overall hygroscopicity of mixed particles.

Dimers in α-pinene secondary organic aerosol: effect of hydroxyl radical, ozone, relative humidity and aerosol acidity

NASA Astrophysics Data System (ADS)

Kristensen, K.; Cui, T.; Zhang, H.; Gold, A.; Glasius, M.; Surratt, J. D.

2014-04-01

The formation of secondary organic aerosol (SOA) from both ozonolysis and hydroxyl radical (OH)-initiated oxidation of α-pinene under conditions of high nitric oxide (NO) concentrations with varying relative humidity (RH) and aerosol acidity was investigated in the University of North Carolina dual outdoor smog chamber facility. SOA formation from ozonolysis of α-pinene was enhanced relative to that from OH-initiated oxidation in the presence of initially high-NO conditions. However, no effect of RH on SOA mass was evident. Ozone (O3)-initiated oxidation of α-pinene in the presence of ammonium sulfate (AS) seed coated with organic aerosol from OH-initiated oxidation of α-pinene showed reduced nucleation compared to ozonolysis in the presence of pure AS seed aerosol. The chemical composition of α-pinene SOA was investigated by ultra-performance liquid chromatography/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-Q-TOFMS), with a focus on the formation of carboxylic acids and high-molecular weight dimers. A total of eight carboxylic acids and four dimers were identified, constituting between 8 and 12% of the total α-pinene SOA mass. OH-initiated oxidation of α-pinene in the presence of nitrogen oxides (NOx) resulted in the formation of highly oxidized carboxylic acids, such as 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA) and diaterpenylic acid acetate (DTAA). The formation of dimers was observed only in SOA produced from the ozonolysis of α-pinene in the absence of NOx, with increased concentrations by a factor of two at higher RH (50-90%) relative to lower RH (30-50%). The increased formation of dimers correlates with an observed increase in new particle formation at higher RH due to nucleation. Increased aerosol acidity was found to have a negligible effect on the formation of the dimers. SOA mass yield did not influence the chemical composition of SOA formed from α-pinene ozonolysis with respect to

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.

Effects of Precursor Concentration and Acidic Sulfate in Aqueous Glyoxal−OH Radical Oxidation and Implications for Secondary Organic Aerosol

PubMed Central

2009-01-01

Previous experiments demonstrated that aqueous OH radical oxidation of glyoxal yields low-volatility compounds. When this chemistry takes place in clouds and fogs, followed by droplet evaporation (or if it occurs in aerosol water), the products are expected to remain partially in the particle phase, forming secondary organic aerosol (SOA). Acidic sulfate exists ubiquitously in atmospheric water and has been shown to enhance SOA formation through aerosol phase reactions. In this work, we investigate how starting concentrations of glyoxal (30−3000 μM) and the presence of acidic sulfate (0−840 μM) affect product formation in the aqueous reaction between glyoxal and OH radical. The oxalic acid yield decreased with increasing precursor concentrations, and the presence of sulfuric acid did not alter oxalic acid concentrations significantly. A dilute aqueous chemistry model successfully reproduced oxalic acid concentrations, when the experiment was performed at cloud-relevant concentrations (glyoxal <300 μM), but predictions deviated from measurements at increasing concentrations. Results elucidate similarities and differences in aqueous glyoxal chemistry in clouds and in wet aerosols. They validate for the first time the accuracy of model predictions at cloud-relevant concentrations. These results suggest that cloud processing of glyoxal could be an important source of SOA. PMID:19924930

Ambient aerosols remain highly acidic despite dramatic sulfate reductions

NASA Astrophysics Data System (ADS)

Nenes, Athanasios; Weber, Rodney; Guo, Hongyu; Russell, Armistead

2016-04-01

The pH of fine particles has many vital environmental impacts. By affecting aerosol concentrations, chemical composition and toxicity, particle pH is linked to regional air quality and climate, and adverse effects on human health. Sulfate is often the main acid component that drives pH of fine particles (i.e., PM2.5) and is neutralized to varying degrees by gas phase ammonia. Sulfate levels have decreased by approximately 70% over the Southeastern United States in the last fifteen years, but measured ammonia levels have been fairly steady implying the aerosol may becoming more neutral. Using a chemically comprehensive data set, combined with a thermodynamic analysis, we show that PM2.5 in the Southeastern U.S. is highly acidic (pH between 0 and 2), and that pH has remained relatively unchanged throughout the past decade and a half of decreasing sulfate. Even with further sulfate reductions, pH buffering by gas-particle partitioning of ammonia is expected to continue until sulfate drops to near background levels, indicating that fine particle pH will remain near current levels into the future. These results are non-intuitive and reshape expectations of how sulfur emission reductions impact air quality in the Southeastern U.S. and possibly other regions across the globe.

Measurements and Modeling of Aerosol Absorption and Single Scattering Albedo at Ambient Relative Hum

NASA Technical Reports Server (NTRS)

Redemann, J.; Russell, P. B.; Hamill, P.

2000-01-01

Uncertainties in the aerosol single scattering albedo have been identified to be an important source of errors in current large-scale model estimates of the direct aerosol radiative forcing of climate. A number of investigators have obtained estimates of the single scattering albedo from a variety of remote sensing and in situ measurements during aerosol field experiments. During the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX, 1996) for example, estimates of the aerosol single scattering albedo were obtained (1) as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from independently measured aerosol properties; (2) from estimates of the aerosol complex index of refraction derived using a combination of airborne sunphotometer, lidar backscatter and in situ size distribution measurements; and (3) from airborne measurements of aerosol scattering and absorption using nephelometers and absorption photometers. In this paper, we briefly compare the results of the latter two methods for two TARFOX case studies, since those techniques provide height-resolved information about the aerosol single scattering albedo. Estimates of the aerosol single scattering albedo from nephelometer and absorption photometer measurements require knowledge of the scattering and absorption humidification (i.e., the increase in these properties in response to an increase in ambient relative humidity), since both measurements are usually carried out at a relative humidity different from the ambient atmosphere. In principle, the scattering humidification factor can be measured, but there is currently no technique widely available to measure the absorption of an aerosol sample as a function of relative humidity. Frequently, for lack of better knowledge, the absorption humidification is assumed to be unity (meaning that there is no change in aerosol absorption due to an increase in ambient relative humidity). This

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

Apparatus for rapid measurement of aerosol bulk chemical composition

DOEpatents

Lee, Yin-Nan E.; Weber, Rodney J.

2003-01-01

An apparatus and method for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution are provided. The apparatus includes a modified particle size magnifier for producing activated aerosol particles and a collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical methods. The method provided for on-line measurement of chemical composition of aerosol particles includes exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

Apparatus for rapid measurement of aerosol bulk chemical composition

DOEpatents

Lee, Yin-Nan E.; Weber, Rodney J.; Orsini, Douglas

2006-04-18

An apparatus for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution is provided. The apparatus includes an enhanced particle size magnifier for producing activated aerosol particles and an enhanced collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical means. Methods for on-line measurement of chemical composition of aerosol particles are also provided, the method including exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; and flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

Uptake of Alkylamines on Dicarboxylic Acids Relevant to Secondary Organic Aerosol Formation

NASA Astrophysics Data System (ADS)

Marrero-Ortiz, W.; Secrest, J.; Zhang, R.

2017-12-01

Aerosols play a critical role in climate directly by scattering and absorbing solar radiation, and indirectly by functioning as cloud condensation nuclei (CCN); both represent the largest uncertainties in climate predictions. New particle formation contributes significantly to CCN production; however, the mechanisms related to particle nucleation and growth processes are not well understood. Organic acids are atmospherically abundant, and their neutralization by low molecular weight amines may result in the formation of stable low volatility aminium salt products contributing to the growth of secondary organic aerosols and even the alteration of the aerosol properties. The acid-base neutralization of particle phase succinic acid and tartaric acid by low molecular weight aliphatic amines, i.e. methylamine, dimethylamine, and trimethylamine, has been investigated by employing a low-pressure fast flow reactor at 298K with an ion drift - chemical ionization mass spectrometer (ID-CIMS). The heterogeneous uptake is time dependent and influenced by organic acids functionality, alkylamines basicity, and steric effect. The implications of our results to atmospheric nanoparticle growth will be discussed.

Vacuum FTIR observation on hygroscopic properties and phase transition of malonic acid aerosols

NASA Astrophysics Data System (ADS)

Shao, Xu; Zhang, Yun; Pang, Shu-Feng; Zhang, Yun-Hong

2017-02-01

A novel approach based on a combination of a pulse relative humidity (RH) controlling system and a rapid scan vacuum FTIR spectrometer was utilized to investigate the hygroscopic property and phase transition of malonic acid (MA) aerosols. By using this approach, both water vapor amount around the aerosols and water content within aerosols with sub-second time resolution were obtained. Based on the features of FTIR absorbing bands, it can be known that the evolution of hydrogen-bonding structures of malonic acid aerosols took place from (H2O)n-MA to MA-MA accompanying with phase transition in the dehumidifying process. And in present paper, the stepwise efflorescence of MA aerosols and nucleation rates at different RHs are first reported. Our observation has shown that the efflorescence of MA started at ∼17% RH and the nucleation rates increased with decreasing RH.

FTIR studies of low temperature sulfuric acid aerosols

NASA Technical Reports Server (NTRS)

Anthony, S. E.; Tisdale, R. T.; Disselkamp, R. S.; Tolbert, M. A.; Wilson, J. C.

1995-01-01

Sub-micrometer sized sulfuric acid H2SO4 particles were generated using a constant output atomizer source. The particles were then exposed to water vapor before being injected into a low temperature cell. Multipass transmission Fourier Transformation Infrared (FTIR) spectroscopy was used to determine the phase and composition of the aerosols as a function of time for periods of up to five hours. Binary H2SO4H2O aerosols with compositions from 35 to 95 wt % H2SO4 remained liquid for over 3 hours at room temperatures ranging from 189-240 K. These results suggest that it is very difficut to freeze SSAs via homogeneous nucleation. Attempts to form aerosols more dilute than 35 wt % H2SO4 resulted in ice formation.

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.;

Applications of broadband cavity enhanced spectroscopy for measurements of trace gases and aerosols

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A. R.; Brock, C. A.; Brown, S. S.; Dube, W. P.; Flores, J. M.; Langford, A. O.; Min, K. E.; Rudich, Y.; Stutz, J.; Wagner, N.; Young, C.; Zarzana, K. J.

2015-12-01

Broadband cavity enhanced spectroscopy (BBCES) uses a broadband light source, optical cavity, and multichannel detector to measure light extinction with high sensitivity. This method differs from cavity ringdown spectroscopy, because it uses an inexpensive, incoherent light source and allows optical extinction to be determined simultaneously across a broad wavelength region.Spectral fitting methods can be used to retrieve multiple absorbers across the observed wavelength region. We have successfully used this method to measure glyoxal (CHOCHO), nitrous acid (HONO), and nitrogen dioxide (NO2) from ground-based and aircraft-based sampling platforms. The detection limit (2-sigma) in 5 s for retrievals of CHOCHO, HONO and NO2 is 32, 250 and 80 parts per trillion (pptv).Alternatively, gas-phase absorbers can be chemically removed to allow the accurate determination of aerosol extinction. In the laboratory, we have used the aerosol extinction measurements to determine scattering and absorption as a function of wavelength. We have deployed a ground-based field instrument to measure aerosol extinction, with a detection limit of approximately 0.2 Mm-1 in 1 min.BBCES methods are most widely used in the near-ultraviolet and visible spectral region. Recently, we have demonstrated measurements at 315-350 nm for formaldehyde (CH2O) and NO2. Extending the technique further into the ultraviolet spectral region will allow important additional measurements of trace gas species and aerosol extinction.

HCl in rocket exhaust clouds - Atmospheric dispersion, acid aerosol characteristics, and acid rain deposition

NASA Technical Reports Server (NTRS)

Pellett, G. L.; Sebacher, D. I.; Bendura, R. J.; Wornom, D. E.

1983-01-01

Both measurements and model calculations of the temporal dispersion of peak HCl (g + aq) concentration in Titan III exhaust clouds are found to be well characterized by one-term power-law decay expressions. The respective coefficients and decay exponents, however, are found to vary widely with meteorology. The HCl (g), HCl (g + aq), dewpoint, and temperature-pressure-altitude data for Titan III exhaust clouds are consistent with accurately calculated HCl/H2O vapor-liquid compositions for a model quasi-equilibrated flat surface aqueous aerosol. Some cloud evolution characteristics are also defined. Rapid and extensive condensation of aqueous acid clearly occurs during the first three min of cloud rise. Condensation is found to be intensified by the initial entrainment of relatively moist ambient air from lower levels, that is, from levels below eventual cloud stabilization. It is pointed out that if subsequent dilution air at stabilization altitude is significantly drier, a state of maximum condensation soon occurs, followed by an aerosol evaporation phase.

Carbonaceous aerosol characterization in the Amazon basin, Brazil: novel dicarboxylic acids and related compounds

NASA Astrophysics Data System (ADS)

Kubátová, Alena; Vermeylen, Reinhilde; Claeys, Magda; Cafmeyer, Jan; Maenhaut, Willy; Roberts, Greg; Artaxo, Paulo

High-resolution capillary gas chromatography (GC) and GC/mass spectrometry (MS) were employed for the quantitative determination of dichloromethane-extractable organic compounds in total and size-fractionated aerosol samples which were collected in the Amazon basin, Brazil, during the wet season, as part of the LBA-CLAIRE-98 experiment. Special emphasis was placed on the characterization and identification of several novel unknown dicarboxylic acids and related oxidative degradation products. This class of acidic products was enriched in the fine size fraction, suggesting that they were secondary organic aerosol products formed by gas-to-particle conversion. Some of the unknowns contributed more to the class of dicarboxylic acids than the major known compound, nonadioic acid (azelaic acid). The same unknowns were also observed in urban aerosol samples collected on hot summer days in Gent, Belgium. For the characterization and structure elucidation of the unknowns, various types of derivatizations and fractionation by solid-phase extraction were employed in combination with GC/MS. Four unknowns were identified. The most abundant were two derivatives of glutaric acid, 3-isopropyl pentanedioic acid and 3-acetyl pentanedioic acid. The other two identified unknowns were another oxo homologue, 3-acetyl hexanedioic acid, and, interestingly, 3-carboxy heptanedioic acid. To our knowledge, the occurrence of these four compounds in atmospheric aerosols has not yet been reported. The biogenic precursors of the novel identified compounds could not be pinpointed, but most likely include monoterpenes and fatty acids.

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.

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%.

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

NASA Astrophysics Data System (ADS)

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

2011-11-01

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

Laboratory photochemical processing of aqueous aerosols: formation and degradation of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls

NASA Astrophysics Data System (ADS)

Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Swaminathan, T.

2015-01-01

To better understand the photochemical processing of dicarboxylic acids and related polar compounds, we conducted batch UV irradiation experiments on two types of aerosol samples collected from India, which represent anthropogenic (AA) and biogenic aerosols (BA), for time periods of 0.5 to 120 h. The irradiated samples were analyzed for molecular compositions of diacids, oxoacids and α-dicarbonyls. The results show that photochemical degradation of oxalic (C2) and malonic (C3) and other C8-C12 diacids overwhelmed their production in aqueous aerosols whereas succinic acid (C4) and C5-C7 diacids showed a significant increase (ca. 10 times) during the course of irradiation experiments. The photochemical formation of oxoacids and α-dicarbonyls overwhelmed their degradation during the early stages of experiment, except for ω-oxooctanoic acid (ωC8) that showed a similar pattern to that of C4. We also found a gradual decrease in the relative abundance of C2 to total diacids and an increase in the relative abundance of C4 during prolonged experiment. Based on the changes in concentrations and mass ratios of selected species with the irradiation time, we hypothesize that iron-catalyzed photolysis of C2 and C3 diacids dominates their concentrations in Fe-rich atmospheric waters, whereas photochemical formation of C4 diacid (via ωC8) is enhanced with photochemical processing of aqueous aerosols in the atmosphere. This study demonstrates that the ambient aerosols contain abundant precursors that produce diacids, oxoacids and α-dicarbonyls, although some species such as oxalic acid decompose extensively during an early stage of photochemical processing.

Laboratory photochemical processing of aqueous aerosols: formation and degradation of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls

NASA Astrophysics Data System (ADS)

Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Swaminathan, T.

2015-07-01

To better understand the photochemical processing of dicarboxylic acids and related polar compounds, we conducted batch UV irradiation experiments on two types of aerosol samples collected from India, which represent anthropogenic (AA) and biogenic (BA) aerosols, for time periods of 0.5 to 120 h. The irradiated samples were analyzed for molecular compositions of diacids, oxoacids and α-dicarbonyls. The results show that photochemical degradation of oxalic (C2), malonic (C3) and other C8-C12 diacids overwhelmed their production in aqueous aerosols, whereas succinic acid (C4) and C5-C7 diacids showed a significant increase (ca. 10 times) during the course of irradiation experiments. The photochemical formation of oxoacids and α-dicarbonyls overwhelmed their degradation during the early stages of experiment except for ω-oxooctanoic acid (ωC8), which showed a similar pattern to that of C4. We also found a gradual decrease in the relative abundance of C2 to total diacids and an increase in the relative abundance of C4 during prolonged experiment. Based on the changes in concentrations and mass ratios of selected species with the irradiation time, we hypothesize that iron-catalyzed photolysis of C2 and C3 diacids controls their concentrations in Fe-rich atmospheric waters, whereas photochemical formation of C4 diacid (via ωC8) is enhanced with photochemical processing of aqueous aerosols in the atmosphere. This study demonstrates that the ambient aerosols contain abundant precursors that produce diacids, oxoacids and α-dicarbonyls, although some species such as oxalic acid decompose extensively during an early stage of photochemical processing.

Aerosol-Forming Reactions of Glyoxal, Methylglyoxal and Amino Acids in Clouds

NASA Astrophysics Data System (ADS)

de Haan, D. O.; Smith, K. W.; Stroik, D. R.; Corrigan, A. L.; Lee, F. E.; Phan, J. T.; Conley, A. C.

2008-12-01

Glyoxal and methylglyoxal are two common aldehydes present in fog and cloud water. Amino acids are present in clouds at similar concentrations. Here we present bulk and aerosol mass spectroscopic data demonstrating that irreversible reactions between glyoxal and amino acids, triggered by droplet evaporation, produce N-derivatized imidazole compounds along with deeply colored Maillard reaction products. These reactions can occur in the dark and in the absence of oxidants. Reactions between methylglyoxal and amino acids produce analogous methylated products plus oligomers with masses up to m/z = 1000. These reactions, which go to completion on the 10-min-timescale of cloud processing, could be significant sources of secondary organic aerosol and humic-like substances (HULIS or brown carbon).

Dimer esters in α-pinene secondary organic aerosol: effect of hydroxyl radical, ozone, relative humidity and aerosol acidity

NASA Astrophysics Data System (ADS)

Kristensen, K.; Cui, T.; Zhang, H.; Gold, A.; Glasius, M.; Surratt, J. D.

2013-12-01

The formation of secondary organic aerosol (SOA) from both ozonolysis and hydroxyl radical (OH)-initiated oxidation of α-pinene under conditions of high nitric oxide (NO) concentrations with varying relative humidity (RH) and aerosol acidity was investigated in the University of North Carolina dual outdoor smog chamber facility. SOA formation from ozonolysis of α-pinene was enhanced relative to that from OH-initiated oxidation in the presence of initially high NO conditions. However, no effect of RH on SOA mass was evident. Ozone (O3)-initiated oxidation of α-pinene in the presence of ammonium sulfate (AS) seed coated with organic aerosol from OH-initiated oxidation of α-pinene showed reduced nucleation compared to ozonolysis in the presence of pure AS seed aerosol. The chemical composition of α-pinene SOA was investigated by ultra-performance liquid chromatography/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-Q-TOFMS), with a focus on the formation of carboxylic acids and high-molecular weight dimer esters. A total of eight carboxylic acids and four dimer esters were identified, constituting between 8 and 12% of the total α-pinene SOA mass. OH-initiated oxidation of α-pinene in the presence of nitrogen oxides (NOx) resulted in the formation of highly oxidized carboxylic acids, such as 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA) and diaterpenylic acid acetate (DTAA). The formation of dimer esters was observed only in SOA produced from the ozonolysis of α-pinene in the absence of NOx, with increased concentrations by a~factor of two at higher RH (50-90%) relative to lower RH (30-50%). The increased formation of dimer esters correlates with an observed increase in new particle formation at higher RH due to nucleation. Increased aerosol acidity was found to have a negligible effect on the formation of the dimer esters. SOA mass yield did not influence the chemical composition of SOA formed from �

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

On the Link Between Ocean Biota Emissions, Aerosol, and Maritime Clouds: Airborne, Ground, and Satellite Measurements Off the Coast of California

DTIC Science & Technology

2009-10-14

sulfate. DEA is likely produced via the reaction of the gaseous amine and acidic sulfates. Subsaturated aerosol hygroscopicity data indicate 14 that the...D., and A. Wiedensohler (1998). NaCl aerosol particle hygroscopicity dependence on mixing with organic compounds, J. Atmos. Chem., 31, 321–346...M. N., and C. K. Chan (2001). The hygroscopic properties of dicarboxylic and multifunctional acids : measurements and UNIFAC

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.

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

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...

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

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.

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.

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.

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.

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

PubMed

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

2017-03-07

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

Aerosol Fragmentation Driven by Coupling of Acid-Base and Free-Radical Chemistry in the Heterogeneous Oxidation of Aqueous Citric Acid by OH Radicals.

PubMed

Liu, Matthew J; Wiegel, Aaron A; Wilson, Kevin R; Houle, Frances A

2017-08-10

A key uncertainty in the heterogeneous oxidation of carboxylic acids by hydroxyl radicals (OH) in aqueous-phase aerosol is how the free-radical reaction pathways might be altered by acid-base chemistry. In particular, if acid-base reactions occur concurrently with acyloxy radical formation and unimolecular decomposition of alkoxy radicals, there is a possibility that differences in reaction pathways impact the partitioning of organic carbon between the gas and aqueous phases. To examine these questions, a kinetic model is developed for the OH-initiated oxidation of citric acid aerosol at high relative humidity. The reaction scheme, containing both free-radical and acid-base elementary reaction steps with physically validated rate coefficients, accurately predicts the experimentally observed molecular composition, particle size, and average elemental composition of the aerosol upon oxidation. The difference between the two reaction channels centers on the reactivity of carboxylic acid groups. Free-radical reactions mainly add functional groups to the carbon skeleton of neutral citric acid, because carboxylic acid moieties deactivate the unimolecular fragmentation of alkoxy radicals. In contrast, the conjugate carboxylate groups originating from acid-base equilibria activate both acyloxy radical formation and carbon-carbon bond scission of alkoxy radicals, leading to the formation of low molecular weight, highly oxidized products such as oxalic and mesoxalic acid. Subsequent hydration of carbonyl groups in the oxidized products increases the aerosol hygroscopicity and accelerates the substantial water uptake and volume growth that accompany oxidation. These results frame the oxidative lifecycle of atmospheric aerosol: it is governed by feedbacks between reactions that first increase the particle oxidation state, then eventually promote water uptake and acid-base chemistry. When coupled to free-radical reactions, acid-base channels lead to formation of low molecular

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

An advanced LC-MS (Q-TOF) technique for the detection of amino acids in atmospheric aerosols

EPA Science Inventory

Methodology for detection of native (underivitized) amino acids in atmospheric aerosols has been developed. This article describes the use of LC-MS (Q-TOF) and microwave-assisted gas phase hydrolysis for detection of free and combined amino acids in aerosols collected in a Southe...

Backscatter laser depolarization studies of simulated stratospheric aerosols - Crystallized sulfuric acid droplets

NASA Technical Reports Server (NTRS)

Sassen, Kenneth; Zhao, Hongjie; Yu, Bing-Kun

1989-01-01

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystalization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

Backscatter laser depolarization studies of simulated stratospheric aerosols: Crystallized sulfuric acid droplets

NASA Technical Reports Server (NTRS)

Sassen, Kenneth; Zhao, Hongjie; Yu, Bing-Kun

1988-01-01

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystallization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

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.

Measurements of aerosol chemical composition in boreal forest summer conditions

NASA Astrophysics Data System (ADS)

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

2012-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

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

Aerosol in the Pacific troposphere

NASA Technical Reports Server (NTRS)

Clarke, Antony D.

1989-01-01

The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.

Water-soluble organic carbon, dicarboxylic acids, ketoacids, and α-dicarbonyls in the tropical Indian aerosols

NASA Astrophysics Data System (ADS)

Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.

2010-06-01

Tropical aerosol (PM10) samples (n = 49) collected from southeast coast of India were studied for water-soluble dicarboxylic acids (C2-C12), ketocarboxylic acids (C2-C9), and α-dicarbonyls (glyoxal and methylglyoxal), together with analyses of total carbon (TC) and water-soluble organic carbon (WSOC). Their distributions were characterized by a predominance of oxalic acid followed by terephthalic (t-Ph), malonic, and succinic acids. Total concentrations of diacids (227-1030 ng m-3), ketoacids (16-105 ng m-3), and dicarbonyls (4-23 ng m-3) are comparative to those from other Asian megacities such as Tokyo and Hong Kong. t-Ph acid was found as the second most abundant diacid in the Chennai aerosols. This feature has not been reported previously in atmospheric aerosols. t-Ph acid is most likely derived from the field burning of plastics. Water-soluble diacids were found to contribute 0.4%-3% of TC and 4%-11% of WSOC. Based on molecular distributions and backward air mass trajectories, we found that diacids and related compounds in coastal South Indian aerosols are influenced by South Asian and Indian Ocean monsoons. Organic aerosols are also suggested to be significantly transported long distances from North India and the Middle East in early winter and from Southeast Asia in late winter, but some originate from photochemical reactions over the Bay of Bengal. In contrast, the Arabian Sea, Indian Ocean, and South Indian continent are suggested as major source regions in summer. We also found daytime maxima of most diacids, except for C9 and t-Ph acids, which showed nighttime maxima in summer. Emissions from marine and terrestrial plants, combined with land/sea breezes and in situ photochemical oxidation, are suggested especially in summer as an important factor that controls the composition of water-soluble organic aerosols over the southeast coast of India. Regional emissions from anthropogenic sources are also important in megacity Chennai, but their influence is

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

Source and reaction pathways of dicarboxylic acids, ketoacids and dicarbonyls in arctic aerosols: One year of observations

NASA Astrophysics Data System (ADS)

Kawamura, Kimitaka; Kasukabe, Hideki; Barrie, Leonard A.

Normal saturated (C 2C 11) and unsaturated (C 4C 5, C 8) dicarboxylic acids were measured in arctic aerosol samples collected weekly at Alert, Canada in 1987-1988. In all seasons, oxalic (C 2) acid was usually the dominant diacid species (1.8-70 ng m -3, av. 14 ± 12 ng m -3) followed by malonic (C 3; 0.05-19 ng m -3, av. 2.5 ± 3.3 ng m -3) and succinic (C 4; 0.51-18 ng m -3, av. 3.8 ± 3.5 ng m -3) acids. The total concentrations of dicarboxylic acids showed a seasonal variation (4.3-97 ng m -3, av. 25 ± 20 ng m -3),with two maxima in September to October and in March to April. The autumn peak is characterized by high concentrations of oxalic acid and azelaic (C 9) acids, which were probably caused by enhanced contributions from anthropogenic and biogenic sources, respectively, followed by photochemical reactions. This is consistent with higher concentrations of n-alkanes from terrestrial plant waxes and of soil-derived aluminum in the autumn aerosol samples. On the other hand, during "Arctic Sunrise" in March to April, oxalic, malonic and succinic acids as well as some other (C 5C 6) diacids were 5 to 20 times more abundant than in the preceding dark winter months, suggesting that diacids are produced in situ by secondary photochemical oxidation of organic pollutants carried to the Arctic. ω-Oxocarboxylic acids (C 2C 5, C 9), pyruvic acid and α-dicarbonyls (methylglyoxal and glyoxal) were also detected in the arctic aerosols. Their concentration also showed spring maxima; however, they were observed a few weeks earlier than the spring peak of diacids. The ω-oxoacids are likely intermediates to the production of α,ω-dicarboxylic acids at the polar sunrise.

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.

Water-soluble dicarboxylic acids and ketocarboxylic acids in the aerosols collected during ACE-Asia/C-130 aircraft campaign 2001

NASA Astrophysics Data System (ADS)

Kawamura, K.; Mochida, M.; Uemoto, N.; Bertram, T.; Huebert, B.

2001-12-01

During the ACE-Asia campaign with C-130 aircraft, aerosol samples were collected over the western North Pacific, East China Sea, and Japan Sea, as well as over Japanese Islands and Korean Peninsula in 8 April to 3 May 2001. The filter samples (N=15) were extracted with organic-free pure water to separate water-soluble dicarboxylic acids and related compounds. The extracts were reacted with 14% BF3 in n-butanol and the dibutyl esters and other derivatives were determined using a capillary GC and GC/MS. The results showed that 14 species of diacids (C2-C11) and 4 species of ketoacids (C2-C4) were detected in the aerosols over the East Asia. Total concentrations of the diacids were 113-500 (av. 330) ng/m3 whereas those of ketoacids were 43-260 (av. 103) ng/m3. The concentrations are equivalent to or more abundant than those reported for the urban Tokyo atmosphere in this season on the ground level. All the samples showed that oxalic acid (C2) is the most abundant diacid, which accounted for 58-83% of total diacids. These values are greater than that (ca. 50%) reported in the urban air near the ground, suggesting that oxalic acid is preferentially produced and/or longer diacids are selectively decomposed in the upper troposphere. Malonic (C3) acid is the second most abundant species followed by succinic (C4) acid. Longer diacids are less abundant, but azelaic (C9) acid is generally more abundant than C6-C8 diacids. Glyoxylic acid (C2) is the most abundant ketoacid followed by pyruvic acid. However, C3 and C4 omega-oxoacids were found as minor species. Although oxalic acid is the dominant component in the aerosols, few samples showed the predominance of glyoxylic acid over oxalic acid. This feature has not been reported for the urban aerosols collected near the ground level. We will discuss a potential photochemical production of water-soluble organic acids in the upper troposphere over the eastern ridge of the Asian continent.

Aerosol Composition and Variability in Baltimore Measured during DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Thornhill, K. L.; Winstead, E. L.; Diskin, G. S.; Chatfield, R. B.; Natraj, V.; Anderson, B. E.

2012-12-01

In order to relate satellite-based measurements of aerosols to ground-level air quality, the correlation between aerosol optical properties (wavelength-dependent scattering and absorption measured by satellites) and mass measurements of aerosol loading (i.e. 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, hygroscopicity, and mass scattering and absorption efficiencies) and to the surrounding atmosphere (such as temperature, relative humidity and altitude). The DISCOVER-AQ (Deriving Information on Surface conditions from COlumn and VERtically resolved observations relevant to Air Quality) project was designed to provide a unique dataset for determining variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Extensive in-situ profiling of the lower atmosphere in the Baltimore-Washington D.C. region was performed during fourteen flights during July 2011. Identical flight plans and profile locations throughout the campaign provide meaningful statistics for analysis. Measured aerosol mass was composed primarily of ammonium sulfate (campaign average of 36%) and water-soluble organics (58%). A distinct difference in composition was related to aerosol loading with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 60%). This composition shift causes a change in the water-uptake potential (hygroscopicity) of the aerosols with higher relative organic composition decreasing water-uptake. On average, sulfate mass increased during the day due to increased photochemistry, while organics decreased. Analysis of the linkage between aerosol loading and optical properties was also performed. The absorption by black carbon was dependent on the amount of organic coating with an increase in mass absorption efficiency from 7.5 m2/g for bare soot to 16 m2/g at an

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.

Longitudinal distributions of dicarboxylic acids, ω-oxoacids, pyruvic acid, α-dicarbonyls, and fatty acids in the marine aerosols from the central Pacific including equatorial upwelling

NASA Astrophysics Data System (ADS)

Hoque, Mir Md. Mozammal; Kawamura, Kimitaka

2016-03-01

Remote marine aerosol samples (total suspended particles) were collected during a cruise in the central Pacific from Japan to Mexico (1°59'N-35°N and 171°54'E-90°58'W). The aerosol samples were analyzed for dicarboxylic acids (C2-C11), ω-oxoacids, pyruvic acid, α-dicarbonyls, and fatty acids as well as organic and elemental carbon, water-soluble organic carbon, and total nitrogen (WSTN). During the study, diacids were the most abundant compound class followed by fatty acids, ω-oxoacids, and α-dicarbonyls. Molecular compositions of diacids showed a predominance of oxalic (C2) acid followed by malonic (C3) and succinic (C4) acids. Oxalic acid comprises 74% of total diacids. This result suggests that photochemical production of oxalic acid is significant over the central Pacific. Spatial distributions of diacids, ω-oxoacids, pyruvic acid, α-dicarbonyls, and fatty acids together with total carbon and WSTN showed higher abundances in the eastern equatorial Pacific where the upwelling of high-nutrient waters followed by high biological productivity is common, indicating that their in situ production is important in the warmer central Pacific through photochemical oxidation from their gaseous and particulate precursors. This study demonstrates that there is a strong linkage in biogeochemical cycles of carbon in the sea-air interface via ocean upwelling, phytoplankton productivity, sea-to-air emissions of organic matter, and formation of secondary organic aerosols in the eastern equatorial Pacific.

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.

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.

Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

NASA Technical Reports Server (NTRS)

Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

2004-01-01

During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic

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.

On the prolonged lifetime of the El Chichon sulfuric acid aerosol cloud

NASA Technical Reports Server (NTRS)

Hofmann, D. J.; Rosen, J. M.

1987-01-01

The observed decay of the aerosol mixing ratio following the eruption of El Chichon appears to have been 20-30 percent slower than that following the eruption of Fuego in 1974, even though the sulfuric acid droplets were observed to grow to considerably larger sizes after El Chichon. This suggests the possible presence of a condensation nuclei and sulfuric acid vapor source and continued growth phenomena occurring well after the El Chichon eruption. It is proposed that the source of these nuclei and the associated vapor may be derived from annual evaporation and condensation of aerosol in the high polar regions during stratospheric warming events, with subsequent spreading to lower latitudes.

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

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.

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.

Cloud forming potential of oligomers relevant to secondary organic aerosols

NASA Astrophysics Data System (ADS)

Xu, Wen; Guo, Song; Gomez-Hernandez, Mario; Zamora, Misti L.; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Zhang, Annie L.; Collins, Don R.; Zhang, Renyi

2014-09-01

The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity are measured for surrogates that mimic atmospherically relevant oligomers, including glyoxal trimer dihydrate, methyl glyoxal trimer dihydrate, sucrose, methyl glyoxal mixtures with sulfuric acid and glycolic acid, and 2,4-hexandienal mixtures with sulfuric acid and glycolic acid. For the single-component aerosols, the measured HGF ranges from 1.3 to 1.4 at a relative humidity of 90%, and the hygroscopicity parameter (κ) is in the range of 0.06 to 0.19 on the basis of the measured CCN activity and 0.13 to 0.22 on the basis of the measured HGF, compared to the calculated values of 0.08 to 0.16. Large differences exist in the κ values derived using the measured HGF and CCN data for the multi-component aerosols. Our results reveal that, in contrast to the oxidation process, oligomerization decreases particle hygroscopicity and CCN activity and provides guidance for analyzing the organic species in ambient aerosols.

Stratospheric aerosol acidity, density, and refractive index deduced from SAGE 2 and NMC temperature data

NASA Technical Reports Server (NTRS)

Yue, G. K.; Poole, L. R.; Wang, P.-H.; Chiou, E. W.

1994-01-01

Water vapor concentrations obtained by the Stratospheric Aerosol and Gas Experiment 2 (SAGE 2) and collocated temperatures provided by the National Meteorological Center (NMC) from 1986 to 1990 are used to deduce seasonally and zonally averaged acidity, density, and refractive index of stratospheric aerosols. It is found that the weight percentage of sulfuric acid in the aerosols increases from about 60 just above the tropopause to about 86 at 35 km. The density increases from about 1.55 to 1.85 g/cu cm between the same altitude limits. Some seasonal variations of composition and density are evident at high latitudes. The refractive indices at 1.02, 0.694, and 0.532 micrometers increase, respectively, from about 1.425, 1.430, and 1.435 just above the tropopause to about 1.445, 1.455, and 1.458 at altitudes above 27 km, depending on the season and latitude. The aerosol properties presented can be used in models to study the effectiveness of heterogeneous chemistry, the mass loading of stratospheric aerosols, and the extinction and backscatter of aerosols at different wavelengths. Computed aerosol surface areas, rate coefficients for the heterogeneous reaction ClONO2 + H2O yields HOCl + HNO3 and aerosol mass concentrations before and after the Pinatubo eruption in June 1991 are shown as sample applications.

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.

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

Identification of aerosol composition from multi-wavelength lidar measurements

NASA Technical Reports Server (NTRS)

Wood, S. A.

1984-01-01

This paper seeks to develop the potential of lidar for the identification of the chemical composition of atmospheric aerosols. Available numerical computations suggest that aerosols can be identified by the wavelength dependence of aerosol optical properties. Since lidar can derive the volume backscatter coefficient as a function of wavelength, a multi-wavelength lidar system may be able to provide valuable information on the composition of aerosols. This research theoretically investigates the volume backscatter coefficients for the aerosol classes, sea-salts, and sulfates, as a function of wavelength. The results show that these aerosol compositions can be characterized and identified by their backscatter wavelength dependence. A method to utilize multi-wavelength lidar measurements to discriminate between compositionally different thin aerosol layers is discussed.

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.

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

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.

Health effects of acid aerosols formed by atmospheric mixtures.

PubMed Central

Kleinman, M T; Phalen, R F; Mautz, W J; Mannix, R C; McClure, T R; Crocker, T T

1989-01-01

Under ambient conditions, sulfur and nitrogen oxides can react with photochemical products and airborne particles to form acidic vapors and aerosols. Inhalation toxicological studies were conducted, exposing laboratory animals, at rest and during exercise, to multicomponent atmospheric mixtures under conditions favorable to the formation of acidic reaction products. Effects of acid and ozone mixtures on early and late clearance of insoluble radioactive particles in the lungs of rats appeared to be dominated by the oxidant component (i.e., the mixture did cause effects that were significantly different from those of ozone alone). Histopathological evaluations showed that sulfuric acid particles alone did not cause inflammatory responses in centriacinar units of rat lung parenchyma (expressed in terms of percent lesion area) but did cause significant damage (cell killing followed by a wave of cell replication) in nasal respiratory epithelium, as measured by uptake of tritiated thymidine in the DNA of replicating cells. Mixtures of ozone and nitrogen dioxide, which form nitric acid, caused significant inflammatory responses in lung parenchyma (in excess of effects seen in rats exposed to ozone alone), but did not damage nasal epithelium. Mixtures containing acidic sulfate particles, ozone, and nitrogen dioxide damaged both lung parenchyma and nasal epithelia. In rats exposed at rest, the response of the lung appeared to be dominated by the oxidant gas-phase components, while responses in the nose were dominated by the acidic particles. In rats exposed at exercise, however, mixtures of ozone and sulfuric acid particles significantly (2.5-fold) elevated the degree of lung lesion formation over that seen in rats exposed to ozone alone under an identical exercise protocol. PMID:2707193

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.

Spatio-temporal distributions of dicarboxylic acids, ω-oxocarboxylic acids, pyruvic acid, α-dicarbonyls and fatty acids in the marine aerosols from the North and South Pacific

NASA Astrophysics Data System (ADS)

Hoque, Mir Md. Mozammal; Kawamura, Kimitaka; Uematsu, Mitsuo

2017-03-01

Aerosol samples (TSP) were collected during a cruise in the North (3°05‧N-34°02‧N) and South (6°59‧S-25°46‧S) Pacific to investigate the spatio-temporal distributions of water-soluble dicarboxylic acids and related compounds. The molecular distributions of diacids were characterized by the predominance of oxalic (C2) acid followed by malonic (C3) and then succinic (C4) acid. However, we found a predominance of C4 over C3 in the aerosol sample that was collected in the western North Pacific Rim with a heavy influence from continental air masses. Atmospheric abundances of short chain diacids (C2-C4) are 2-3 times higher in the North Pacific than in the South Pacific. During the cruise, abundances of C2 in the western North Pacific are 5 times higher than those in the rest of the samples collected. Moreover, the aerosol samples collected in the western North Pacific demonstrated that glyoxylic (ωC2) acid and methylglyoxal (MeGly) were dominant together with C2. We found a strong correlation between C2 and ωC2 (r = 0.87) and C2 and MeGly (r = 0.97) in the western North Pacific aerosols but the correlations are significantly weak in the samples from the central North Pacific and Southern Ocean. Diacids were found to account for 1.6 to 14% of organic carbon with higher values in the western North Pacific. These results, together with 7-day backward air mass trajectories, indicate that ωC2 and MeGly are both originated from the photochemical oxidation of continent-derived organic precursors including isoprene, which can serve as precursors for the production of C2 during long-range atmospheric transport.

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.

The boiling point of stratospheric aerosols.

NASA Technical Reports Server (NTRS)

Rosen, J. M.

1971-01-01

A photoelectric particle counter was used for the measurement of aerosol boiling points. The operational principle involves raising the temperature of the aerosol by vigorously heating a portion of the intake tube. At or above the boiling point, the particles disintegrate rather quickly, and a noticeable effect on the size distribution and concentration is observed. Stratospheric aerosols appear to have the same volatility as a solution of 75% sulfuric acid. Chemical analysis of the aerosols indicates that there are other substances present, but that the sulfate radical is apparently the major constituent.

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.

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.

Atmospheric measurements of pyruvic and formic acid

NASA Technical Reports Server (NTRS)

Andreae, Meinrat O.; Li, Shao-Meng; Talbot, Robert W.

1987-01-01

Pyruvic acid, a product of the atmospheric oxidation of cresols and probably of isoprene, has been determined together with formic acid in atmospheric aerosols and rain as well as in the vapor phase. Both acids are present predominantly as vapor; only about 10-20 percent of the total atmospheric pyruvate and 1-2 percent of the total formate are in the particulate phase. The concentrations of pyruvic and formic acid are highly correlated, with typical formic-to-pyruvic ratios of 10-30 in the gas phase, 20-30 in rain, and 2-10 in aerosols. The gas-phase and rain ratios are comparable to those predicted to result from isoprene oxidation. Pyruvic acid levels were similar in the eastern United States (during summer) and the Amazon Basin, suggesting that natural processes, particularly the photochemical oxidation of isoprene, could account for most of the pyruvic acid present in the atmosphere.

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

Molecular distributions and isotopic compositions of marine aerosols over the western North Atlantic: Dicarboxylic acids, ketoacids, α-dicarbonyls (glyoxal and methylglyoxal), fatty acids, sugars, and SOA tracers

NASA Astrophysics Data System (ADS)

Kawamura, K.; Ono, K.; Tachibana, E.; Quinn, P.; Bates, T. S.

2013-12-01

Marine aerosols were collected over the western North Atlantic from off the coast of Boston to Bermuda during the WACS (Western Atlantic Climate Study) cruise of R/V Ronald H. Brown in August 2012 using a high volume air sampler and pre-combusted quartz fiber filters. Aerosol filter samples (n=5) were analyzed for OC/EC, major inorganic ions, low molecular weight dicarboxylic acids and various secondary organic aerosol (SOA) tracers using carbon analyzer, ion chromatograph, GC/FID and GC/MS, respectively. Homologous series (C2-C12) of dicarboxylic acids (31-335 ng m-3) were detected with a predominance of oxalic acid. Total carbon and nitrogen and their stable isotope ratios were determined as well as stable carbon isotopic compositions of individual diacids using IRMS. Diacids were found to be the most abundant compound class followed by monoterpene-SOA tracers > isoprene-SOA tracers > sugar compounds > ketoacids > fatty alcohols > fatty acids > α-dicarbonyls > aromatic acids > n-alkanes. The concentrations of these compounds were higher in the coastal site and decreased in the open ocean. However, diacids stayed relatively high even in the remote ocean. Interestingly, contributions of oxalic acid to total aerosol carbon increased from the coast (2.3%) to the remote ocean (5.6%) during long-range atmospheric transport. Stable carbon isotopic composition of oxalic acid increased from the coast (-17.5‰) to open ocean (-12.4‰), suggesting that photochemical aging of organic aerosols occurred during the atmospheric transport over the ocean. Stable carbon isotope ratios of bulk aerosol carbon also increased from the coast near Boston to the open ocean near Bermuda.

Application of FIGAERO (Filter Inlet for Gases and AEROsol) coupled to a high resolution time of flight chemical ionization mass spectrometer to field and chamber organic aerosol: Implications for carboxylic acid formation and gas-particle partitioning from monoterpene oxidation

NASA Astrophysics Data System (ADS)

Lopez-Hilfiker, F.; Mohr, C.; Ehn, M.; Rubach, F.; Mentel, T. F.; Kleist, E.; Wildt, J.; Thornton, J. A.

2013-12-01

We present measurements of a large suite of gas and particle phase carboxylic acid containing compounds made with a Filter Inlet for Gas and AEROsol (FIGAERO) coupled to a high resolution time of flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. A prototype operated with acetate negative ion proton transfer chemistry was deployed on the Julich Plant Atmosphere Chamber to study a-pinene oxidation, and a modified version was deployed at the SMEAR II forest station in Hyytiälä, Finland and SOAS, in Brent Alabama. We focus here on results from JPAC and Hyytiälä, where we utilized the same ionization method most selective towards carboxylic acids. In all locations, 100's of organic acid compounds were observed in the gas and particles and many of the same composition acids detected in the gas-phase were detected in the particles upon temperature programmed thermal desorption. Particulate organics detected by FIGAERO are highly correlated with organic aerosol mass measured by an AMS, providing additional volatility and molecular level information about collected aerosol. The fraction of a given compound measured in the particle phase follows expected trends with elemental composition, but many compounds would not be well described by an absorptive partitioning model assuming unity activity coefficients. Moreover the detailed structure in the thermal desorption signals reveals a contribution from thermal decomposition of large molecular weight organics and or oligomers with implications for partitioning measurements and model validation

Stable carbon isotope ratios of low molecular weight dicarboxylic acids, ketoacids and glyoxal in marine aerosols from the western North Pacific: Long-term trends in Chichijima Island

NASA Astrophysics Data System (ADS)

Kawamura, K.; Tachibana, E.

2012-12-01

Dicarboxylic acids such as oxalic, malonic and succinic acids are the most abundant water-soluble organic compound class in aerosols. To better understand the source and photochemical processes of water-soluble organic aerosols in the remote marine aerosols, we measured stable carbon isotopic composition (δ13C) of dicarboxylic acids and related compounds using a GC/IR/MS technique. The aerosol samples were collected in 2001-2011 at a remote island, Chichijima (27°04'E; 142°13'N) in the western North Pacific. Here we present decadal variations of the isotopic composition of dicarboxylic acids (C2-C9), ketoacids (C2-C8) and glyoxal in summertime aerosols (June, July and August). The molecular distributions of diacids were characterized by the predominance of oxalic (C2) acid followed by malonic (C3) and succinic (C4) acids. Oxalic acid showed higher δ13C values than other species ranging from -18‰ to -2‰ with no clear decadal trend. In contrast, C3 and C4 diacids showed δ13C values of -24 to -5‰ and -40 to -12‰ with a decadal decline. Glyoxal (-60 to -10‰) and ωC7 acid (-34 to -12‰) also showed lower values toward 2011. However, azelaic acid (C9) (-32 to -24‰) stayed relatively constant throughout the observation period. We will discuss the detailed isotopic compositions of these organic species in terms of the photochemical aging and processing in the western North Pacific and the changes in the sources and source regions.

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%.

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 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.

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

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...

Atmospheric oxalic acid and related secondary organic aerosols in Qinghai Lake, a continental background site in Tibet Plateau

NASA Astrophysics Data System (ADS)

Meng, Jingjing; Wang, Gehui; Li, Jianjun; Cheng, Chunlei; Cao, Junji

2013-11-01

Summertime PM2.5 aerosols collected from Qinghai Lake (3200 m a.s.l.), a remote continental site in the northeastern part of Tibetan Plateau, were analyzed for dicarboxylic acids (C2-C11), ketocarboxylic acids and α-dicarbonyals. Oxalic acid (C2) is the dominant dicarboxylic acid in the samples, followed by malonic, succinic and azelaic acids. Total dicarboxylic acids (231 ± 119 ng m-3), ketocarboxylic acids (8.4 ± 4.3 ng m-3), and α-dicarbonyls (2.7 ± 2.1 ng m-3) at the Tibetan background site are 2-5 times less than those detected in lowland areas such as 14 Chinese megacities. Compared to those in other urban and marine areas enhancements in relative abundances of C2/total diacids and diacids-C/WSOC of the PM2.5 samples suggest that organic aerosols in the region are more oxidized due to strong solar radiation. Molecular compositions and air mass trajectories demonstrate that the above secondary organic aerosols in the Qinghai Lake atmosphere are largely derived from long-range transport. Ratios of oxalic acid, glyoxal and methylglyoxal to levoglucosan in PM2.5 aerosols emitted from household burning of yak dung, a major energy source for Tibetan in the region, are 30-400 times lower than those in the ambient air, which further indicates that primary emission from biomass burning is a negligible source of atmospheric oxalic acid and α-dicarbonyls at this background site.

Thermal decomposition in thermal desorption instruments: importance of thermogram measurements for analysis of secondary organic aerosol

NASA Astrophysics Data System (ADS)

Stark, H.; Yatavelli, R. L. N.; Thompson, S.; Kang, H.; Krechmer, J. E.; Kimmel, J.; Palm, B. B.; Hu, W.; Hayes, P.; Day, D. A.; Campuzano Jost, P.; Ye, P.; Canagaratna, M. R.; Jayne, J. T.; Worsnop, D. R.; Jimenez, J. L.

2017-12-01

Understanding the chemical composition of secondary organic aerosol (SOA) is crucial for explaining sources and fate of this important aerosol class in tropospheric chemistry. Further, determining SOA volatility is key in predicting its atmospheric lifetime and fate, due to partitioning from and to the gas phase. We present three analysis approaches to determine SOA volatility distributions from two field campaigns in areas with strong biogenic emissions, a Ponderosa pine forest in Colorado, USA, from the BEACHON-RoMBAS campaign, and a mixed forest in Alabama, USA, from the SOAS campaign. We used a high-resolution-time-of-flight chemical ionization mass spectrometer (CIMS) for both campaigns, equipped with a micro-orifice volatilization impactor (MOVI) inlet for BEACHON and a filter inlet for gases and aerosols (FIGAERO) for SOAS. These inlets allow near simultaneous analysis of particle and gas-phase species by the CIMS. While gas-phase species are directly measured without heating, particles undergo thermal desorption prior to analysis. Volatility distributions can be estimated in three ways: (1) analysis of the thermograms (signal vs. temperature); (2) via partitioning theory using the gas- and particle-phase measurements; (3) from measured chemical formulas via a group contribution model. Comparison of the SOA volatility distributions from the three methods shows large discrepancies for both campaigns. Results from the thermogram method are the most consistent of the methods when compared with independent AMS-thermal denuder measurements. The volatility distributions estimated from partitioning measurements are very narrow, likely due to signal-to-noise limits in the measurements. The discrepancy between the formula and the thermogram methods indicates large-scale thermal decomposition of the SOA species. We will also show results of citric acid thermal decomposition, where, in addition to the mass spectra, measurements of CO, CO2 and H2O were made, showing

Aqueous aerosol SOA formation: impact on aerosol physical properties.

PubMed

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

2013-01-01

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

TOTAL PARTICLE, SULFATE, AND ACIDIC AEROSOL EMISSIONS FROM KEROSENE SPACE HEATERS

EPA Science Inventory

Chamber studies were conducted on four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine part...

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

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

Breaks induced in the deoxyribonucleic acid of aerosolized Escherichia coli by ozonized cyclohexene.

PubMed Central

De Mik, G; De Groot, I

1978-01-01

The inactivation of aerosolized Escherichia coli by ozone, cyclohexene, and ozonized cyclohexene was studied. The parameters for damage were loss of reproduction and introduction of breaks in the deoxyribonucleic acid (DNA). Aerosolization of E. coli in clean air at 80 percent relative humidity or in air containing either ozone or cyclohexene hardly affected survival; however, some breaks per DNA molecule were induced, as shown by sucrose gradient sedimentation of the DNA. Aerosolization of E. coli in air containing ozonized cyclohexene at 80 percent relative humidity decreased the survival by a factor of 10(3) or more after 1 h of exposure and induced many breaks in the DNA. PMID:341811

Distributions of low molecular weight dicarboxylic acids, ketoacids and α-dicarbonyls in the marine aerosols collected over the Arctic Ocean during late summer

NASA Astrophysics Data System (ADS)

Kawamura, K.; Ono, K.; Tachibana, E.; Charriére, B.; Sempéré, R.

2012-11-01

Oxalic and other small dicarboxylic acids have been reported as important water-soluble organic constituents of atmospheric aerosols from different environments. Their molecular distributions are generally characterized by the predominance of oxalic acid (C2) followed by malonic (C3) and/or succinic (C4) acids. In this study, we collected marine aerosols from the Arctic Ocean during late summer in 2009 when sea ice was retreating. The marine aerosols were analyzed for the molecular distributions of dicarboxylic acids as well as ketocarboxylic acids and α-dicarbonyls to better understand the source of water-soluble organics and their photochemical processes in the high Arctic marine atmosphere. We found that diacids are more abundant than ketoacids and α-dicarbonyls, but their concentrations are generally low (< 30 ng m-3), except for one sample (up to 70 ng m-3) that was collected near the mouth of Mackenzie River during clear sky condition. Although the molecular compositions of diacids are in general characterized by the predominance of oxalic acid, a depletion of C2 was found in two samples in which C4 became the most abundant. Similar depletion of oxalic acid has previously been reported in the Arctic aerosols collected at Alert after polar sunrise and in the summer aerosols from the coast of Antarctica. Because the marine aerosols that showed a depletion of C2 were collected under the overcast and/or foggy conditions, we suggest that a photochemical decomposition of oxalic acid may have occurred in aqueous phase of aerosols over the Arctic Ocean via the photo dissociation of oxalate-Fe (III) complex. We also determined stable carbon isotopic compositions (δ13C) of bulk aerosol carbon and individual diacids. The δ13C of bulk aerosols showed -26.5‰ (range: -29.7 to -24.7‰, suggesting that marine aerosol carbon is derived from both terrestrial and marine organic materials. In contrast, oxalic acid showed much larger δ13C values (average: -20.9‰, range

Distributions of low molecular weight dicarboxylic acids, ketoacids and α-dicarbonyls in the marine aerosols collected over the Arctic Ocean during late summer

NASA Astrophysics Data System (ADS)

Kawamura, K.; Ono, K.; Tachibana, E.; Charriére, B.; Sempéré, R.

2012-08-01

Oxalic and other small dicarboxylic acids have been reported as important water-soluble organic constituents of atmospheric aerosols from different environments. Their molecular distributions are generally characterized by the predominance of oxalic acid (C2) followed by malonic (C3) and/or succinic (C4) acids. In this study, we collected marine aerosols from the Arctic Ocean during late summer in 2009 when sea ice is retreated. The marine aerosols were analyzed for the molecular distributions of dicarboxylic acids as well as ketocarboxylic acids and α-dicarbonyls to better understand the source of water-soluble organics and their photochemical processes in the high Arctic marine atmosphere. We found that diacids are more abundant than ketoacids and α-dicarbonyls, but their concentrations are generally low (< 30 ng m-3), except for one sample (up to 70 ng m-3) that was collected near the mouth of Mackenzie River during clear sky condition. Although the molecular compositions of diacids are in general characterized by the predominance of oxalic acid, a depletion of C2 was found in two samples in which C4 became the most abundant. Similar depletion of oxalic acid has previously been reported in the Arctic aerosols collected at Alert after polar sunrise and in the summer aerosols from the coastal Antarctica. Because the marine aerosols that showed a depletion of C2 were observed under the overcast and/or foggy conditions, we suggest that a photochemical decomposition of oxalic acid may have occurred in aqueous phase of aerosols over the Arctic Ocean via the photo dissociation of oxalate-Fe (III) complex. We also determined stable carbon isotopic compositions (δ13C) of bulk aerosol carbon and individual diacids. The δ13C of bulk aerosols showed -26.5‰ (range: -29.7‰ to -24.7‰), suggesting that marine aerosol carbon is derived from both terrestrial and marine organic materials. In contrast, oxalic acid showed much larger δ13C values (average: -20.9‰, range

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.

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

NASA Astrophysics Data System (ADS)

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

2014-08-01

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

The 2005 catastrophic acid crater lake drainage, lahar, and acidic aerosol formation at Mount Chiginagak volcano, Alaska, USA: Field observations and preliminary water and vegetation chemistry results

NASA Astrophysics Data System (ADS)

Schaefer, Janet R.; Scott, William E.; Evans, William C.; Jorgenson, Janet; McGimsey, Robert G.; Wang, Bronwen

2008-07-01

A mass of snow and ice 400-m-wide and 105-m-thick began melting in the summit crater of Mount Chiginagak volcano sometime between November 2004 and early May 2005, presumably owing to increased heat flux from the hydrothermal system, or possibly from magma intrusion and degassing. In early May 2005, an estimated 3.8 × 106 m3 of sulfurous, clay-rich debris and acidic water, with an accompanying acidic aerosol component, exited the crater through a tunnel at the base of a glacier that breaches the south crater rim. Over 27 km downstream, the acidic waters of the flood inundated an important salmon spawning drainage, acidifying Mother Goose Lake from surface to depth (approximately 0.5 km3 in volume at a pH of 2.9 to 3.1), killing all aquatic life, and preventing the annual salmon run. Over 2 months later, crater lake water sampled 8 km downstream of the outlet after considerable dilution from glacial meltwater was a weak sulfuric acid solution (pH = 3.2, SO4 = 504 mg/L, Cl = 53.6 mg/L, and F = 7.92 mg/L). The acid flood waters caused severe vegetation damage, including plant death and leaf kill along the flood path. The crater lake drainage was accompanied by an ambioructic flow of acidic aerosols that followed the flood path, contributing to defoliation and necrotic leaf damage to vegetation in a 29 km2 area along and above affected streams, in areas to heights of over 150 m above stream level. Moss species killed in the event contained high levels of sulfur, indicating extremely elevated atmospheric sulfur content. The most abundant airborne phytotoxic constituent was likely sulfuric acid aerosols that were generated during the catastrophic partial crater lake drainage event. Two mechanisms of acidic aerosol formation are proposed: (1) generation of aerosol mist through turbulent flow of acidic water and (2) catastrophic gas exsolution. This previously undocumented phenomenon of simultaneous vegetation-damaging acidic aerosols accompanying drainage of an acidic

The 2005 catastrophic acid crater lake drainage, lahar, and acidic aerosol formation at Mount Chiginagak volcano, Alaska, USA: Field observations and preliminary water and vegetation chemistry results

USGS Publications Warehouse

Schaefer, J.R.; Scott, W.E.; Evans, William C.; Jorgenson, J.; McGimsey, R.G.; Wang, B.

2008-01-01

A mass of snow and ice 400-m-wide and 105-m-thick began melting in the summit crater of Mount Chiginagak volcano sometime between November 2004 and early May 2005, presumably owing to increased heat flux from the hydrothermal system, or possibly from magma intrusion and degassing. In early May 2005, an estimated 3.8??106 m3 of sulfurous, clay-rich debris and acidic water, with an accompanying acidic aerosol component, exited the crater through a tunnel at the base of a glacier that breaches the south crater rim. Over 27 km downstream, the acidic waters of the flood inundated an important salmon spawning drainage, acidifying Mother Goose Lake from surface to depth (approximately 0.5 km3 in volume at a pH of 2.9 to 3.1), killing all aquatic life, and preventing the annual salmon run. Over 2 months later, crater lake water sampled 8 km downstream of the outlet after considerable dilution from glacial meltwater was a weak sulfuric acid solution (pH = 3.2, SO4 = 504 mg/L, Cl = 53.6 mg/L, and F = 7.92 mg/L). The acid flood waters caused severe vegetation damage, including plant death and leaf kill along the flood path. The crater lake drainage was accompanied by an ambioructic flow of acidic aerosols that followed the flood path, contributing to defoliation and necrotic leaf damage to vegetation in a 29 km2 area along and above affected streams, in areas to heights of over 150 m above stream level. Moss species killed in the event contained high levels of sulfur, indicating extremely elevated atmospheric sulfurcontent. The most abundant airborne phytotoxic constituent was likely sulfuric acid aerosols that were generated during the catastrophic partial crater lake drainage event. Two mechanisms of acidic aerosol formation are proposed: (1) generation of aerosol mist through turbulent flow of acidic water and (2) catastrophic gas exsolution. This previously undocumented phenomenon of simultaneous vegetationdamaging acidic aerosols accompanying drainage of an acidic crater

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.

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

PubMed

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

2018-06-01

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

pH Variance in Aerosols Undergoing Liquid-Liquid Phase Separation

NASA Astrophysics Data System (ADS)

Eddingsaas, N. C.; Dallemagne, M.; Huang, X.

2014-12-01

The water content of aerosols is largely governed by relative humidity (RH). As the relative humidity decreases, and thus the water content of aerosols, a number of processes occur including the shrinking of aerosols, the increase in concentration of components, and potentially the formation of liquid liquid phase separation (llps) due to the salting out of inorganic salts. The most ubiquitous salt in atmospheric aerosols is ammonium sulfate which results in many aerosols to be at least mildly acidic. However, during llps, the pH of the different phases is not necessarily the same. Many reactions that take place within atmospheric aerosols are acid catalyzed so a better understanding of the pH of the individual phases as well as the interface between the phases is important to understanding aerosol processing and aging. Through the use of pH sensitive dyes and confocal microscopy we have directly measured the pH of micron sized model aerosols during high RH where the aerosols are in a single phase, at intermediate while the aerosols are in llps, and low RH where the aerosols consist of one liquid phase and one solid phase. We will discuss the variation in RH during these different phase states in the presence and absence of excess sulfuric acid. We will also discuss how this variation in pH affects aging of aerosols.

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

NASA Astrophysics Data System (ADS)

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

2014-02-01

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

Aerosol generation and measurement of multi-wall carbon nanotubes

NASA Astrophysics Data System (ADS)

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

2009-01-01

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

Measurement of the Vertical Distribution of Aerosol by Globally Distributed MP Lidar Network Sites

NASA Technical Reports Server (NTRS)

Spinhirne, James; Welton, Judd; Campbell, James; Starr, David OC. (Technical Monitor)

2001-01-01

The global distribution of aerosol has an important influence on climate through the scattering and absorption of shortwave radiation and through modification of cloud optical properties. Current satellite and other data already provide a great amount of information on aerosol distribution. However there are critical parameters that can only be obtained by active optical profiling. For aerosol, no passive technique can adequately resolve the height profile of aerosol. The aerosol height distribution is required for any model for aerosol transport and the height resolved radiative heating/cooling effect of aerosol. The Geoscience Laser Altimeter System (GLAS) is an orbital lidar to be launched by 2002. GLAS will provide global measurements of the height distribution of aerosol. The sampling will be limited by nadir only coverage. There is a need for local sites to address sampling, and accuracy factors. 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 profiling of all significant cloud and aerosol to the limit of signal attenuation from compact, eye safe instruments. There are currently six sites in operation and over a dozen planned. At all sites there are a complement of passive aerosol and radiation measurements supporting the lidar data. Four of the installations are at Atmospheric Radiation Measurement program sites. The aerosol measurements, retrievals and data products from the network sites will be discussed. The current and planned application of data to supplement satellite aerosol measurements is covered.

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

Field Studies Measuring the aerosolization of Endotoxin ...

EPA Pesticide Factsheets

Endotoxin is a component of the cell walls of Gram-negative bacteria and is known to be present in biosolids. Endotoxins have been shown to be a potent stimulator of the innate immune response causing airway irritation and shortness of breath. Class B biosolids are routinely applied to agricultural lands in the US to enhance soil properties and can be used as an alternative to chemical fertilizers. This study investigated the aerosolized endotoxin produced during the land application of Class B biosolids from various wastewater treatment plants on agricultural land and a concrete surface at two sites in Colorado, USA. Aerosolized endotoxin was captured using HiVol sampler fitted with glass fiber filter, polycarbonate filter cassette (both open and closed), and BioSampler impinger air samplers. Endotoxins were also measured in the bulk biosolids to allow for correlating bulk biosolids concentrations with aerosol emission rates. Endotoxin concentrations in biosolids, impinger solutions, and filter extracts were determined using the kinetic Limulus amebocyte lysate assay. Aerosolized endotoxin concentration was detected from all sites with levels ranging from 0.5 to 642 EU/m3. The four types of sampling apparatus were compared and the HiVol and open-faced cassette samplers used produced higher TWA measurements (EU/m3) than the impinger and closed cassette samplers. Ambient wind speed at the sites was found to be the variable best describing the results wit

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

PubMed

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

2018-02-01

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

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.

Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer

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

Wang, Yang; Pinterich, Tamara; Wang, Jian

We present rapid measurement of submicron particle size distributions enables the characterization of aerosols with fast changing properties, and is often necessary for measurements onboard mobile platforms (e.g., research aircraft). Aerosol mobility size distribution is commonly measured by a scanning mobility particle sizer (SMPS), which relies on voltage scanning or stepping to classify particles of different sizes, and may take up to several minutes to obtain a complete size spectrum of aerosol particles. The recently developed fast integrated mobility spectrometer (FIMS) with enhanced dynamic size range classifies and detects particles from 10 to ~600 nm simultaneously, allowing submicron aerosol mobilitymore » size distributions to be captured at a time resolution of 1 second. In this study, we present a detailed data inversion routine for deriving aerosol size distribution from FIMS measurements. The inversion routine takes into consideration the FIMS transfer function, particle penetration efficiency in the FIMS, and multiple charging of aerosols. The accuracy of the FIMS measurement is demonstrated by comparing parallel FIMS and SMPS measurements of stable aerosols with a wide range of size spectrum shapes, including ambient aerosols and aerosols classified by a differential mobility analyzer (DMA). The FIMS and SMPS-derived size distributions show excellent agreements for all aerosols tested. In addition, total number concentrations of ambient aerosols were integrated from 1 Hz FIMS size distributions, and compared with those directly measured by a condensation particle counter (CPC) operated in parallel. Finally, the integrated and measured total particle concentrations agree well within 5%.« less

Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer

DOE PAGES

Wang, Yang; Pinterich, Tamara; Wang, Jian

2018-03-30

We present rapid measurement of submicron particle size distributions enables the characterization of aerosols with fast changing properties, and is often necessary for measurements onboard mobile platforms (e.g., research aircraft). Aerosol mobility size distribution is commonly measured by a scanning mobility particle sizer (SMPS), which relies on voltage scanning or stepping to classify particles of different sizes, and may take up to several minutes to obtain a complete size spectrum of aerosol particles. The recently developed fast integrated mobility spectrometer (FIMS) with enhanced dynamic size range classifies and detects particles from 10 to ~600 nm simultaneously, allowing submicron aerosol mobilitymore » size distributions to be captured at a time resolution of 1 second. In this study, we present a detailed data inversion routine for deriving aerosol size distribution from FIMS measurements. The inversion routine takes into consideration the FIMS transfer function, particle penetration efficiency in the FIMS, and multiple charging of aerosols. The accuracy of the FIMS measurement is demonstrated by comparing parallel FIMS and SMPS measurements of stable aerosols with a wide range of size spectrum shapes, including ambient aerosols and aerosols classified by a differential mobility analyzer (DMA). The FIMS and SMPS-derived size distributions show excellent agreements for all aerosols tested. In addition, total number concentrations of ambient aerosols were integrated from 1 Hz FIMS size distributions, and compared with those directly measured by a condensation particle counter (CPC) operated in parallel. Finally, the integrated and measured total particle concentrations agree well within 5%.« less

New Measurements of Aerosol Vertical Structure from Space Using the NASA Geoscience Laser Altimeter System (GLAS): Applications for Aerosol Transport Models

NASA Technical Reports Server (NTRS)

Welton, Ellsworth J.; Ginoux, Paul; Colarco, Peter; Chin, Mian; Spinhirne, James D.; Palm, Steven P.; Hlavka, Dennis; Hart, William

2003-01-01

In the past, satellite measurements of aerosols have only been possible using passive sensors. Analysis of passive satellite data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth s climate. However, direct measurement of aerosol vertical distribution has not been possible using only the passive data. Knowledge of aerosol vertical distribution is important to correctly assess the impact of aerosol absorption, for certain atmospheric correction procedures, and to help constrain height profiles in aerosol transport models. On January 12,2003 NASA launched the first satellite-based lidar, the Geoscience Laser Altimeter System (GLAS), onboard the ICESat spacecraft. GLAS is both an altimeter and an atmospheric lidar, and obtains direct measurements of aerosol and cloud heights. Here we show an overview of GLAS, provide an update of its current status, and discuss how GUS data will be useful for modeling efforts. In particular, a strategy of using GLAS to characterize the height profile of dust plumes over source regions will be presented, along with initial results. Such information can be used to validate and improve output from aerosol transport models. Aerosol height profile comparisons between GLAS and transport models will be shown for regions downwind of aerosol sources. We will also discuss the feasibility of assimilating GLAS profiles into the models in order to improve their output,

New Measurements of Aerosol Vertical Structure from Space using the NASA Geoscience Laser Altimeter System (GLAS): Applications for Aerosol Transport Models

NASA Technical Reports Server (NTRS)

Welton, E. J.; Spinhime, J.; Palm, S.; Hlavka, D.; Hart, W.; Ginoux, P.; Chin, M.; Colarco, P.

2004-01-01

In the past, satellite measurements of aerosols have only been possible using passive sensors. Analysis of passive satellite data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth,s climate. However, direct measurement of aerosol vertical distribution has not been possible using only the passive data. Knowledge of aerosol vertical distribution is important to correctly assess the impact of aerosol absorption, for certain atmospheric correction procedures, and to help constrain height profiles in aerosol transport models. On January 12,2003 NASA launched the first satellite-based lidar, the Geoscience Laser Altimeter System (GLAS), onboard the ICESat spacecraft. GLAS is both an altimeter and an atmospheric lidar, and obtains direct measurements of aerosol and cloud heights. Here we show an overview of GLAS, provide an update of its current status, and discuss how GLAS data will be useful for modeling efforts. In particular, a strategy of using GLAS to characterize the height profile of dust plumes over source regions will be presented, along with initial results. Such information can be used to validate and improve output from aerosol transport models. Aerosol height profile comparisons between GLAS and transport models will be shown for regions downwind of aerosol sources. We will also discuss the feasibility of assimilating GLAS profiles into the models in order to improve their output.

Measuring Aerosol Optical Properties with the Ozone Monitoring Instrument (OMI)

NASA Technical Reports Server (NTRS)

Veefkind, J. P.; Torres, O.; Syniuk, A.; Decae, R.; deLeeuw, G.

2003-01-01

The Ozone Monitoring Instrument (OMI) is the Dutch-Finnish contribution to the NASA EOS-Aura mission scheduled for launch in January 2004. OM1 is an imaging spectrometer that will measure the back-scattered Solar radiance between 270 an 500 nm. With its relatively high spatial resolution (13x24 sq km at nadir) and daily global coverage. OM1 will make a major contribution to our understanding of atmospheric chemistry and to climate research. OM1 will provide data continuity with the TOMS instruments. One of the pleasant surprises of the TOMS data record was its information on aerosol properties. First, only the absorbing aerosol index, which is sensitive to elevated lay- ers of aerosols such as desert dust and smoke aerosols, was derived. Recently these methods were further improved to yield aerosol optical thickness and single scattering albedo over land and ocean for 19 years of TOMS data (1979-1992,1997-2002), making it one of the longest and most valuable time series for aerosols presently available. Such long time series are essential to quantify the effect of aerosols on the Earth& climate. The OM1 instrument is better suited to measure aerosols than the TOMS instruments because of the smaller footprint, and better spectral coverage. The better capabilities of OMI will enable us to provide an improved aerosol product, but the knowledge will also be used for further analysis of the aerosol record from TOMS. The OM1 aerosol product that is currently being developed for OM1 combines the TOMS experience and the multi-spectral techniques that are used in the visible and near infrared. The challenge for this new product is to provide aerosol optical thickness and single scattering albedo from the near ultraviolet to the visible (330-500 nm) over land and ocean. In this presentation the methods for deriving the OM1 aerosol product will be presented. Part of these methods developed for OM1 can already be applied to TOMS data and results of such analysis will be shown.

Aerosol deposition in the human respiratory tract

NASA Astrophysics Data System (ADS)

Winchester, John W.; Jones, Donald L.; Mu-tian, Bi

1984-04-01

Rising sulfur dioxide emissions from increased coal combustion present risks, not only of acid rain, but also to health by inhalation of the SO 2 and acid to the lung. We are investigating human inhalation of ppm SO 2 concentrations mixed with aerosol of submicrometer aqueous salt droplets to determine the effects on lung function and body chemistry. Unlike some investigators, we emphasize ammonium sulfate and trace element aerosol composition which simulates ambient air; aerosol pH, relative humidity, and temperature control to reveal gas-particle reaction mechanisms; and dose estimates from length of exposure, SO 2 concentration, and a direct measurement of respiratory deposition of aerosol as a function of particle size by cascade impactor sampling and elemental analysis by PIXE. Exposures, at rest or during exercise, are in a walk-in chamber at body temperature and high humidity to simulate Florida's summer climate. Lung function measurement by spirometry is carried out immediately after exposure. The results are significant in relating air quality to athletic performance and to public health in the southeastern United States.

Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide

NASA Astrophysics Data System (ADS)

Konovalov, Igor B.; Beekmann, Matthias; Berezin, Evgeny V.; Formenti, Paola; Andreae, Meinrat O.

2017-04-01

Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there is substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes under different environmental conditions and at various temporal scales hinders development of their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol photochemical age (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but that is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from MODIS and IASI measurements, respectively, are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with spatial average PM2. 5 concentration exceeding 100 µg m-3). For such plumes, the ER is found to increase almost 2-fold on the scale of ˜ 10 h of daytime aerosol

Diurnal variations of total carbon, dicarboxylic acids, ketoacids and α-dicarbonyls in aerosols in the northern vicinity of Beijing

NASA Astrophysics Data System (ADS)

He, N.; Kawamura, K.; Okuzawa, K.; Kanaya, Y.; Wang, Z. F.

2013-06-01

Aerosol samples (TSP, n=58) were collected on day- and night-time basis at Mangshan in the north of Beijing, China in autumn 2007 to better understand the status of air quality and the influence of urban pollutants in the northern vicinity of Beijing. The samples were analyzed for aerosol mass, total carbon (TC), low molecular weight α, ω-dicarboxylic acids (C2-C12), ketoacids (ωC2-ωC9, pyruvic acid), α-dicarbonyls (glyoxal and methylglyoxal), as well as aromatic (phthalic, iso- and tere-phthalic) diacids. Aerosol mass and TC concentrations are higher in daytime than in nighttime. TC/aerosol mass ratios in this study are lower than those reported in megacities in East Asia, but higher than those reported in marine aerosols. Molecular distributions of diacids demonstrated that oxalic (C2) acid was the most abundant species, comprising 38-77% of total diacids, followed by succinic (C4) and malonic (C3) acids. For most compounds, the concentrations were higher in daytime than nighttime, indicating that diacids are produced in daytime by photochemical oxidation of organic precursors emitted from anthropogenic sources in Beijing during the transport to Mangshan area by the northward wind. However, we found that C2 concentrations are higher in nighttime than in daytime. A positive correlation of C2 to glyoxylic acid (ωC2) was obtained at night when relative humidity increased up to 100%, suggesting that aqueous phase production of C2 occurs in nighttime via the oxidation of ωC2. Depletion of C2 by photolysis of Fe-oxalato complexes might be another reason for the lower concentrations of C2 in daytime samples. High phthalic acid/C4 ratios in the aerosol samples suggest that automobile combustion and coal burning products are important sources, which are subjected to photochemical oxidation during the atmospheric transport of urban aerosols from Beijing. In contrast, higher concentrations of methylglyoxal in nighttime than daytime may suggest that isoprene emitted

Three optical methods for remotely measuring aerosol size distributions.

NASA Technical Reports Server (NTRS)

Reagan, J. A.; Herman, B. M.

1971-01-01

Three optical probing methods for remotely measuring atmospheric aerosol size distributions are discussed and contrasted. The particular detection methods which are considered make use of monostatic lidar (laser radar), bistatic lidar, and solar radiometer sensing techniques. The theory of each of these measurement techniques is discussed briefly, and the necessary constraints which must be applied to obtain aerosol size distribution information from such measurements are pointed out. Theoretical and/or experimental results are also presented which demonstrate the utility of the three proposed probing methods.

The Aerosol Models in MODTRAN: Incorporating Selected Measurements From Northern Australia

DTIC Science & Technology

2005-12-01

biomass burning smoke aerosol is modelled assuming the particles are spherical and Mie scattering theory is used to calculate the extinction and...and therefore internally mixed aerosol particles are hygroscopic . Shettle and Fenn model the growth in the size of aerosol particles and changes in...by Sutherland and Khanna [21] was to obtain measurements of the optical properties of organic -based aerosols produced by burning vegetation.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles.

PubMed

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-04-22

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30-500 nm, number concentration in range of 5 × 10²-10⁷ /cm³. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles.

Spatial variation of stratospheric aerosol acidity and model refractive index - Implications of recent results

NASA Technical Reports Server (NTRS)

Russell, P. B.; Hamill, P.

1984-01-01

Recent experimental results indicate that little or no solid ammonium sulfate is present in background stratospheric aerosols. Other results allow straightforward calculation of sulfuric acid/water droplet properties (acidity, specific gravity, refractive index) as functions of stratospheric temperature and humidity. These results are combined with a variety of latitudinal and seasonal temperature and humidity profiles to obtain corresponding profiles of droplet properties. These profiles are used to update a previous model of stratospheric aerosol refractive index. The new model retains the simplifying approximation of vertically constant refractive index in the inner stratosphere, but has sulfuric acid/water refractive index values that significantly exceed the previously used room temperature values. Mean conversion ratios (e.g., extinction-to-number, backscatter-to-volume) obtained using Mie scattering calculations with the new refractive indices are very similar to those obtained for the old indices, because the effects of deleting ammonium sulfate and increasing acid indices tend to cancel each other.

Spectral signatures of polar stratospheric clouds and sulfate aerosol

NASA Technical Reports Server (NTRS)

Massie, S. T.; Bailey, P. L.; Gille, J. C.; Lee, E. C.; Mergenthaler, J. L.; Roche, A. E.; Kumer, J. B.; Fishbein, E. F.; Waters, J. W.; Lahoz, W. A.

1994-01-01

Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite (UARS) are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605/cm (10.8, 8.0, and 6.2 micrometers) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheriodal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculations and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles.

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.

The impact of marine surface organic enrichment on the measured hygroscopicity parameter of laboratory generated sea-spray aerosols

NASA Astrophysics Data System (ADS)

Schill, S.; Novak, G.; Zimmermann, K.; Bertram, T. H.

2014-12-01

The ocean serves as a major source for atmospheric aerosol particles, yet the chemicophysical properties of sea spray aerosol to date are not well characterized. Understanding the transfer of organic compounds, present in the sea surface microlayer (SSML), to sea-spray particles and their resulting impact on cloud formation is important for predicting aerosol impact on climate in remote marine environments. Here, we present a series of laboratory experiments designed to probe the fractionation of select organic molecules during wave breaking. We use a representative set of organic mimics (e.g. sterols, sugars, lipids, proteins, fatty acids) to test a recent physically based model of organic enrichment in sea-spray aerosol [Burrows et al., 2014] that is based on Langmuir absorption equilibria. Experiments were conducted in the UCSD Marine Aerosol Reference Tank (MART) permitting accurate representation of wave breaking processes in the laboratory. We report kappa values for the resulting sea-spray aerosols and compare them to a predictions made using Kappa-Köhler Theory driven by a linear combination of the pure component kappa values. Hygroscopicity determinations made using the model systems are discussed within the context of measurements of CCN activity made using natural, coastal water.

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

Vertically resolved aerosol properties by multi wavelengths lidar measurements

NASA Astrophysics Data System (ADS)

Perrone, M. R.; De Tomasi, F.; Gobbi, G. P.

2013-07-01

A new approach is introduced to characterize the dependence on altitude of the aerosol fine mode radius (Rf) and of the fine mode contribution (η) to the aerosol optical thickness (AOT) by three-wavelength lidar measurements. The introduced approach is based on the graphical method of Gobbi et al. (2007), which was applied to AERONET spectral extinction observations and relies on the combined analysis of the Ångstrom exponent (å) and its spectral curvature Δå. Lidar measurements at 355, 532 and 1064 nm were used in this study to retrieve the vertical profiles of å and Δå and to determine the dependence on altitude of Rf and η (532 nm) from the å-Δå combined analysis. Lidar measurements were performed at the Mathematics and Physics Department of Universita' del Salento, in south eastern Italy. Aerosol from continental Europe, the Atlantic, northern Africa, and the Mediterranean Sea are often advected over south eastern Italy and as a consequence, mixed advection patterns leading to aerosol properties varying with altitude are dominant. The proposed approach was applied to eleven measurement days to demonstrate its feasibility in different aerosol load conditions. The selected-days were characterized by AOTs spanning the 0.23-0.67, 0.15-0.41, and 0.04-0.25 range at 355, 532, and 1064 nm, respectively. Lidar ratios varied within the 28-80, 30-70, and 30-55 sr range at 355, 532, and 1064 nm, respectively, for the high variability of the aerosol optical and microphysical properties. å(355 nm, 1064 nm) values retrieved from lidar measurements ranged between 0.12 and 2.5 with mean value ±1 standard deviation equal to 1.4 ± 0.5. Δå varied within the -0.10-0.87 range with mean value equal to 0.1 ± 0.4. Rf and η (532 nm) values spanning the 0.02-0.30 μm and the 0.30-0.99 range, respectively were associated to the å-Δå data points. Rf and η values showed no dependence on the altitude. 72% of the data points were in the Δå-å space delimited by the �

Measurement of phase function of aerosol at different altitudes by CCD Lidar

NASA Astrophysics Data System (ADS)

Sun, Peiyu; Yuan, Ke'e.; Yang, Jie; Hu, Shunxing

2018-02-01

The aerosols near the ground are closely related to human health and climate change, the study on which has important significance. As we all know, the aerosol is inhomogeneous at different altitudes, of which the phase function is also different. In order to simplify the retrieval algorithm, it is usually assumed that the aerosol is uniform at different altitudes, which will bring measurement error. In this work, an experimental approach is demonstrated to measure the scattering phase function of atmospheric aerosol particles at different heights by CCD lidar system, which could solve the problem of the traditional CCD lidar system in assumption of phase function. The phase functions obtained by the new experimental approach are used to retrieve the aerosol extinction coefficient profiles. By comparison of the aerosol extinction coefficient retrieved by Mie-scattering aerosol lidar and CCD lidar at night, the reliability of new experimental approach is verified.

Retrieval of Aerosol Parameters from Continuous H24 Lidar-Ceilometer Measurements

NASA Astrophysics Data System (ADS)

Dionisi, D.; Barnaba, F.; Costabile, F.; Di Liberto, L.; Gobbi, G. P.; Wille, H.

2016-06-01

Ceilometer technology is increasingly applied to the monitoring and the characterization of tropospheric aerosols. In this work, a method to estimate some key aerosol parameters (extinction coefficient, surface area concentration and volume concentration) from ceilometer measurements is presented. A numerical model has been set up to derive a mean functional relationships between backscatter and the above mentioned parameters based on a large set of simulated aerosol optical properties. A good agreement was found between the modeled backscatter and extinction coefficients and the ones measured by the EARLINET Raman lidars. The developed methodology has then been applied to the measurements acquired by a prototype Polarization Lidar-Ceilometer (PLC). This PLC instrument was developed within the EC- LIFE+ project "DIAPASON" as an upgrade of the commercial, single-channel Jenoptik CHM15k system. The PLC run continuously (h24) close to Rome (Italy) for a whole year (2013-2014). Retrievals of the aerosol backscatter coefficient at 1064 nm and of the relevant aerosol properties were performed using the proposed methodology. This information, coupled to some key aerosol type identification made possible by the depolarization channel, allowed a year-round characterization of the aerosol field at this site. Examples are given to show how this technology coupled to appropriate data inversion methods is potentially useful in the operational monitoring of parameters of air quality and meteorological interest.

LC-MS-MS-TOF analysis of oxygenated organic compounds in ambient aerosol

NASA Astrophysics Data System (ADS)

Roempp, A.; Moortgat, G.

2003-04-01

Ambient aerosol samples were taken at different sites across Europe. The fine mode aerosol was collected on quartz filters at flow rates of 160 L/min and 500 L/min. These samples were analyzed for organic acids (C>4) by an HPLC system coupled to a hybrid mass spectrometer. The mass spectrometer consists of a quadrupole mass analyzer, a quadrupole collision cell and a time-of-flight mass analyzer (TOF). Analytes were identified by standards when available or MS-MS experiments and exact mass measurements utilizing the high mass resolution of the TOF instrument. Monoterpenes (alpha-pinene, beta-pinene, sabinene, limonene, 3-carene) were ozonolyzed in the laboratory and compared with field samples. Besides the commonly measured organic acids (pinic, pinonic and norpinic acid) sabinic, caric and caronic acid were identified for the first time in ambient aerosol. In addition, nearly all samples showed significant concentrations of newly identified keto dicarboxylic acids (C9 - C12). Laboratory experiments were used to investigate the formation mechanisms of these compounds. By comparing laboratory measurements of wood combustion and field samples from the Eastern Mediterranean region, nitrocatechol was identified as a possible tracer for biomass burning. The data obtained is used to determine the role of biogenic sources in secondary organic aerosol formation.

Vertically resolved aerosol properties by multi-wavelength lidar measurements

NASA Astrophysics Data System (ADS)

Perrone, M. R.; De Tomasi, F.; Gobbi, G. P.

2014-02-01

An approach based on the graphical method of Gobbi and co-authors (2007) is introduced to estimate the dependence on altitude of the aerosol fine mode radius (Rf) and of the fine mode contribution (η) to the aerosol optical thickness (AOT) from three-wavelength lidar measurements. The graphical method of Gobbi and co-authors (2007) was applied to AERONET (AErosol RObotic NETwork) spectral extinction observations and relies on the combined analysis of the Ångstrom exponent (å) and its spectral curvature Δå. Lidar measurements at 355, 532 and 1064 nm were used in this study to retrieve the vertical profiles of å and Δå and to estimate the dependence on altitude of Rf and η(532 nm) from the å-Δå combined analysis. Lidar measurements were performed at the Department of Mathematics and Physics of the Universita' del Salento, in south-eastern Italy. Aerosol from continental Europe, the Atlantic, northern Africa, and the Mediterranean Sea are often advected over south-eastern Italy and as a consequence, mixed advection patterns leading to aerosol properties varying with altitude are dominant. The proposed approach was applied to ten measurement days to demonstrate its feasibility in different aerosol load conditions. The selected days were characterized by AOTs spanning the 0.26-0.67, 0.15-0.39, and 0.04-0.27 range at 355, 532, and 1064 nm, respectively. Mean lidar ratios varied within the 31-83, 32-84, and 11-47 sr range at 355, 532, and 1064 nm, respectively, for the high variability of the aerosol optical and microphysical properties. å values calculated from lidar extinction profiles at 355 and 1064 nm ranged between 0.1 and 2.5 with a mean value ± 1 standard deviation equal to 1.3 ± 0.7. Δå varied within the -0.1-1 range with mean value equal to 0.25 ± 0.43. Rf and η(532 nm) values spanning the 0.05-0.3 μm and the 0.3-0.99 range, respectively, were associated with the å-Δå data points. Rf and η values showed no dependence on the altitude. 60

Airborne Lidar Measurements of Aerosol Optical Properties During SAFARI-2000

NASA Technical Reports Server (NTRS)

McGill, M. J.; Hlavka, D. L.; Hart, W. D.; Welton, E. J.; Campbell, J. R.; Starr, David OC. (Technical Monitor)

2002-01-01

The Cloud Physics Lidar (CPL) operated onboard the NASA ER-2 high altitude aircraft during the SAFARI-2000 field campaign. The CPL provided high spatial resolution measurements of aerosol optical properties at both 1064 nm and 532 nm. We present here results of planetary boundary layer (PBL) aerosol optical depth analysis and profiles of aerosol extinction. Variation of optical depth and extinction are examined as a function of regional location. The wide-scale aerosol mapping obtained by the CPL is a unique data set that will aid in future studies of aerosol transport. Comparisons between the airborne CPL and ground-based MicroPulse Lidar Network (MPL-Net) sites are shown to have good agreement.

Preparation of amino acid nanoparticles at varying saturation conditions in an aerosol flow reactor

NASA Astrophysics Data System (ADS)

Raula, Janne; Lehtimäki, Matti; Karppinen, Maarit; Antopolsky, Maxim; Jiang, Hua; Rahikkala, Antti; Kauppinen, Esko I.

2012-07-01

Nanoparticle formation of five amino acids, glycine, l-proline, l-valine, l-phenylalanine, and l-leucine was studied. The aim was to explore factors determining nanoparticle formation and crystallinity. The amino acid nanoparticles have been prepared at different saturation conditions in the aerosol reactor. In a condensed state, the particles were formed by droplet drying. The raise in temperature induced the sublimation of amino acids from the aerosol particles. The amino acid vapor was condensed by physical vapor deposition in a rapid cooling process. The diffusion coefficients and nucleation rates of amino acids have been calculated to understand particle formation. Upon the vapor deposition, amino acids formed crystalline nanoparticles except in the case l-phenylalanine according to X-ray diffraction. The crystal polymorph of glycine in the nanoparticles depended on the applied reactor temperature. The preference of crystallographic orientation varied in both the particle formations from condensed and vapor phase. l-Valine, l-phenylalanine, and l-leucine formed leafy-looking particles. These results could be utilized in the fabrication of nano-sized asperities on drug particle surfaces to reduce forces between particles and accordingly increase particle dispersion in dry powder inhalers.

The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

NASA Astrophysics Data System (ADS)

Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

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.

A SURVEY OF SULFATE, NITRATE, AND ACID AEROSOL EMISSIONS AND THEIR CONTROL

EPA Science Inventory

The report gives results of an evaluation of the effects of fuel and combustion modifications on the formation of primary acid aerosols (used broadly to include all sulfates, nitrates, chlorides, and fluorides in all their forms) and their significance as combustion-generated pol...

Quantifying Above-Cloud Aerosols through Integrating Multi-Sensor Measurements from A-Train Satellites

NASA Technical Reports Server (NTRS)

Zhang, Yan

2012-01-01

Quantifying above-cloud aerosols can help improve the assessment of aerosol intercontinental transport and climate impacts. Large-scale measurements of aerosol above low-level clouds had been generally unexplored until very recently when CALIPSO lidar started to acquire aerosol and cloud profiles in June 2006. Despite CALIPSO s unique capability of measuring above-cloud aerosol optical depth (AOD), such observations are substantially limited in spatial coverage because of the lidar s near-zero swath. We developed an approach that integrates measurements from A-Train satellite sensors (including CALIPSO lidar, OMI, and MODIS) to extend CALIPSO above-cloud AOD observations to substantially larger areas. We first examine relationships between collocated CALIPSO above-cloud AOD and OMI absorbing aerosol index (AI, a qualitative measure of AOD for elevated dust and smoke aerosol) as a function of MODIS cloud optical depth (COD) by using 8-month data in the Saharan dust outflow and southwest African smoke outflow regions. The analysis shows that for a given cloud albedo, above-cloud AOD correlates positively with AI in a linear manner. We then apply the derived relationships with MODIS COD and OMI AI measurements to derive above-cloud AOD over the whole outflow regions. In this talk, we will present spatial and day-to-day variations of the above-cloud AOD and the estimated direct radiative forcing by the above-cloud aerosols.

Importance of Unimolecular HO 2 Elimination in the Heterogeneous OH Reaction of Highly Oxygenated Tartaric Acid Aerosol

DOE PAGES

Cheng, Chiu Tung; Chan, Man Nin; Wilson, Kevin R.

2016-07-09

Oxygenated organic molecules are abundant in atmospheric aerosols and are transformed by oxidation reactions near the aerosol surface by gas-phase oxidants such as hydroxyl (OH) radicals. To gain better insights into how the structure of an organic molecule, particularly in the presence of hydroxyl groups, controls the heterogeneous reaction mechanisms of oxygenated organic compounds, this paper investigates the OH-radical initiated oxidation of aqueous tartaric acid (C 4H 6O 6) droplets using an aerosol flow tube reactor. The molecular composition of the aerosols before and after reaction is characterized by a soft atmospheric pressure ionization source (Direct Analysis in Real Time)more » coupled with a high-resolution mass spectrometer. The aerosol mass spectra reveal that four major reaction products are formed: a single C 4 functionalization product (C 4H 4O 6) and three C 3 fragmentation products (C 3H 4O 4, C 3H 2O 4, and C 3H 2O 5). The C 4 functionalization product does not appear to originate from peroxy radical self-reactions but instead forms via an α-hydroxylperoxy radical produced by a hydrogen atom abstraction by OH at the tertiary carbon site. The proximity of a hydroxyl group to peroxy group enhances the unimolecular HO 2 elimination from the α-hydroxylperoxy intermediate. This alcohol-to-ketone conversion yields 2-hydroxy-3-oxosuccinic acid (C 4H 4O 6), the major reaction product. While in general, C–C bond scission reactions are expected to dominate the chemistry of organic compounds with high average carbon oxidation states (OS C), our results show that molecular structure can play a larger role in the heterogeneous transformation of tartaric acid (OS C = 1.5). Finally, these results are also compared with two structurally related dicarboxylic acids (succinic acid and 2,3-dimethylsuccinic acid) to elucidate how the identity and location of functional groups (methyl and hydroxyl groups) alter heterogeneous reaction mechanisms.« less

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

NASA Astrophysics Data System (ADS)

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

2002-12-01

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

Satellite Remote Sensing: Aerosol Measurements

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.

2013-01-01

Aerosols are solid or liquid particles suspended in the air, and those observed by satellite remote sensing are typically between about 0.05 and 10 microns in size. (Note that in traditional aerosol science, the term "aerosol" refers to both the particles and the medium in which they reside, whereas for remote sensing, the term commonly refers to the particles only. In this article, we adopt the remote-sensing definition.) They originate from a great diversity of sources, such as wildfires, volcanoes, soils and desert sands, breaking waves, natural biological activity, agricultural burning, cement production, and fossil fuel combustion. They typically remain in the atmosphere from several days to a week or more, and some travel great distances before returning to Earth's surface via gravitational settling or washout by precipitation. Many aerosol sources exhibit strong seasonal variability, and most experience inter-annual fluctuations. As such, the frequent, global coverage that space-based aerosol remote-sensing instruments can provide is making increasingly important contributions to regional and larger-scale aerosol studies.

Vertical Profiles of Cloud Condensation Nuclei, Condensation Nuclei, Optical Aerosol, Aerosol Optical Properties, and Aerosol Volatility Measured from Balloons

NASA Technical Reports Server (NTRS)

Deshler, T.; Snider, J. R.; Vali, G.

1998-01-01

Under the support of this grant a balloon-borne gondola containing a variety of aerosol instruments was developed and flown from Laramie, Wyoming, (41 deg N, 105 deg W) and from Lauder, New Zealand (45 deg S, 170 deg E). The gondola includes instruments to measure the concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), optically detectable aerosol (OA.) (r greater than or equal to 0.15 - 2.0 microns), and optical scattering properties using a nephelometer (lambda = 530 microns). All instruments sampled from a common inlet which was heated to 40 C on ascent and to 160 C on descent. Flights with the CN counter, OA counter, and nephelometer began in July 1994. The CCN counter was added in November 1994, and the engineering problems were solved by June 1995. Since then the flights have included all four instruments, and were completed in January 1998. Altogether there were 20 flights from Laramie, approximately 5 per year, and 2 from Lauder. Of these there were one or more engineering problems on 6 of the flights from Laramie, hence the data are somewhat limited on those 6 flights, while a complete data set was obtained from the other 14 flights. Good CCN data are available from 12 of the Laramie flights. The two flights from Lauder in January 1998 were successful for all measurements. The results from these flights, and the development of the balloon-bome CCN counter have formed the basis for five conference presentations. The heated and unheated CN and OA measurements have been used to estimate the mass fraction of the aerosol volatile, while comparisons of the nephelometer measurements were used to estimate the light scattering, associated with the volatile aerosol. These estimates were calculated for 0.5 km averages of the ascent and descent data between 2.5 km and the tropopause, near 11.5 km.

Particle size distribution of the stratospheric aerosol from SCIAMACHY limb measurements

NASA Astrophysics Data System (ADS)

Rozanov, Alexei; Malinina, Elizaveta; Bovensmann, Heinrich; Burrows, John

2017-04-01

A crucial role of the stratospheric aerosols for the radiative budget of the Earth's atmosphere and the consequences for the climate change are widely recognized. A reliable knowledge on physical and optical properties of the stratospheric aerosols as well as on their vertical and spatial distributing is a key issue to assure a proper initialization and running conditions for climate models. On a global scale this information can only be gained from space borne measurements. While a series of past, present and future instruments provide extensive date sets of such aerosol characteristics as extinction coefficient or backscattering ratio, information on a size distribution of the stratospheric aerosols is sparse. One of the important sources on vertically and spatially resolved information on the particle size distribution of stratospheric aerosols is provided by space borne measurements of the scattered solar light in limb viewing geometry performed in visible, near-infrared and short-wave infrared spectral ranges. SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) instrument operated on the European satellite Envisat from 2002 to 2102 was capable of providing spectral information needed to retrieve parameters of aerosol particle size distributions. In this presentation we discuss the retrieval method, present first validation results with SAGE II data and analyze first data sets of stratospheric aerosol particle size distribution parameters obtained from SCIAMACHY limb measurements. The research work was performed in the framework of ROMIC (Role of the middle atmosphere in climate) project.

Sources and formation processes of water-soluble dicarboxylic acids, ω-oxocarboxylic acids, α-dicarbonyls, and major ions in summer aerosols from eastern central India

NASA Astrophysics Data System (ADS)

Deshmukh, Dhananjay K.; Kawamura, Kimitaka; Deb, Manas K.; Boreddy, Suresh K. R.

2017-03-01

The sources and formation processes of dicarboxylic acids are still under investigation. Size-segregated aerosol (nine-size) samples collected in the urban site (Raipur: 21.2°N and 82.3°E) in eastern central India during summer of 2013 were measured for water-soluble diacids (C2-C12), ω-oxoacids (ωC2-ωC9), α-dicarbonyls (C2-C3), and inorganic ions to better understand their sources and formation processes. Diacids showed the predominance of oxalic acid (C2), whereas ω-oxoacids showed the predominance of glyoxylic acid (ωC2), and glyoxal (Gly) was a major α-dicarbonyl in all the sizes. Diacids, ω-oxoacids, and α-dicarbonyls as well as SO42

Protection of hydrophobic amino acids against moisture-induced deterioration in the aerosolization performance of highly hygroscopic spray-dried powders.

PubMed

Yu, Jiaqi; Chan, Hak-Kim; Gengenbach, Thomas; Denman, John A

2017-10-01

Inhalable particles containing amorphous form of drugs or excipients may absorb atmospheric moisture, causing powder aggregation and recrystallization, adversely affecting powder dispersion and lung deposition. The present study aims to explore hydrophobic amino acids for protection against moisture in spray-dried amorphous powders, using disodium cromoglycate (DSCG) as a model drug. DSCG powders were produced by co-spray drying with isoleucine (Ile), valine (Val) and methionine (Met) in various concentrations (10, 20 and 40%w/w). Particle size distribution and morphology were measured by laser diffraction and scanning electron microscopy (SEM). Physiochemical properties of the powders were characterized by X-ray powder diffraction (XRPD), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA) and dynamic vapor sorption (DVS). Particle surface chemistry was analyzed by X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). In vitro aerosolization performance was evaluated by a next generation impactor (NGI) after the powders were stored at 60% or 75% relative humidity (RH) for one month and three months. Ile, Val and Met significantly reduced the deleterious effect of moisture on aerosol performance, depending on the amount of amino acids in the formulation. Formulations containing 10% or 20% of Ile, Val and Met showed notable deterioration in aerosol performance, with fine particle fraction (FPF) reduced by 6-15% after one-month storage at both 60% and 75% RH. However, 40% Ile was able to maintain the aerosol performance of DSCG stored at 75% RH for one month, while the FPF dropped by 7.5% after three months of storage. In contrast, 40% Val or Met were able to maintain the aerosol performance at 60% RH storage but not at 75% RH. At 40%w/w ratio, these formulations had particle surface coverage of 94.5% (molar percent) of Ile, 87.1% of Val and 84.6% of Met, respectively, which may explain their

Evaluating Secondary Inorganic Aerosols in Three Dimensions

NASA Technical Reports Server (NTRS)

Mezuman, Keren; Bauer, Susanne E.; Tsigaridis, Kostas

2016-01-01

The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the three-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e., sulfate, ammonium, and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000 to 2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model. Heterogeneous reactions on dust surfaces are an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3/NH4(+) partitioning which affects the HNO3/NO3(-) partitioning.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles

PubMed Central

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-01-01

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30–500 nm, number concentration in range of 5 × 102–5 × 107 /cm3. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles. PMID:28441740

A review of dicarboxylic acids and related compounds in atmospheric aerosols: Molecular distributions, sources and transformation

NASA Astrophysics Data System (ADS)

Kawamura, Kimitaka; Bikkina, Srinivas

2016-03-01

This review aims to update our understanding on molecular distributions of water-soluble dicarboxylic acids and related compounds in atmospheric aerosols with a focus on their geographical variability, size distribution, sources and formation pathways. In general, molecular distributions of diacids in aerosols from the continental sites and over the open ocean waters are often characterized by the predominance of oxalic acid (C2) followed by malonic acid (C3) and/or succinic acid (C4), while those sampled over the polar regions often follow the order of C4 ≥ C2 and C3. The most abundant and ubiquitous diacid is oxalic acid, which is principally formed via atmospheric oxidation of its higher homologues of long chain diacids and other pollution-derived organic precursors (e.g., olefins and aromatic hydrocarbons). However, its occurrence in marine aerosols is mainly due to the transport from continental outflows (e.g., East Asian outflow during winter/spring to the North Pacific) and/or governed by photochemical/aqueous phase oxidation of biogenic unsaturated fatty acids (e.g., oleic acid) and isoprene emitted from the productive open ocean waters. The long-range atmospheric transport of pollutants from mid latitudes to the Arctic in dark winter facilitates to accumulate the reactants prior to their intense photochemical oxidation during springtime polar sunrise. Furthermore, the relative abundances of C2 in total diacid mass showed similar temporal trends with downward solar irradiation and ambient temperatures, suggesting the significance of atmospheric photochemical oxidation processing. Compound-specific isotopic analyses of oxalic acid showed the highest δ13C among diacids whereas azelaic acid showed the lowest value, corroborating the significance of atmospheric aging of oxalic acid. On the other hand, other diacids gave intermediate values between these two diacids, suggesting that aging of oxalic acid is associated with 13C enrichment.

Characterization of aerosol scattering and spectral absorption by unique methods: a polar/imaging nephelometer and spectral reflectance measurements of aerosol samples collected on filters

NASA Astrophysics Data System (ADS)

Dolgos, Gergely; Martins, J. Vanderlei; Remer, Lorraine A.; Correia, Alexandre L.; Tabacniks, Manfredo; Lima, Adriana R.

2010-02-01

Characterization of aerosol scattering and absorption properties is essential to accurate radiative transfer calculations in the atmosphere. Applications of this work include remote sensing of aerosols, corrections for aerosol distortions in satellite imagery of the surface, global climate models, and atmospheric beam propagation. Here we demonstrate successful instrument development at the Laboratory for Aerosols, Clouds and Optics at UMBC that better characterizes aerosol scattering phase matrix using an imaging polar nephelometer (LACO-I-Neph) and enables measurement of spectral aerosol absorption from 200 nm to 2500 nm. The LACO-I-Neph measures the scattering phase function from 1.5° to 178.5° scattering angle with sufficient sensitivity to match theoretical expectations of Rayleigh scattering of various gases. Previous measurements either lack a sufficiently wide range of measured scattering angles or their sensitivity is too low and therefore the required sample amount is prohibitively high for in situ measurements. The LACO-I-Neph also returns expected characterization of the linear polarization signal of Rayleigh scattering. Previous work demonstrated the ability of measuring spectral absorption of aerosol particles using a reflectance technique characterization of aerosol samples collected on Nuclepore filters. This first generation methodology yielded absorption measurements from 350 nm to 2500 nm. Here we demonstrate the possibility of extending this wavelength range into the deep UV, to 200 nm. This extended UV region holds much promise in identifying and characterizing aerosol types and species. The second generation, deep UV, procedure requires careful choice of filter substrates. Here the choice of substrates is explored and preliminary results are provided.

SAGE Aerosol Measurements. Volume 2: 1 January - 31 December 1980

NASA Technical Reports Server (NTRS)

Mccormick, M. P.

1986-01-01

The stratospheric Aerosol and Gas Experiment (SAGE) satellite system, launched on February 18, 1979, provides profiles of aerosol extinction at wavelengths of 1.00 and 0.45 micron, ozone concentration, and nitrogen dioxide concentration. Data taken during sunset events in the form of zonal averages and seasonal averages of the aerosol extinction at 1.00 and 0.45 micron, ratios of the aerosol extinction to the molecular extinction at 1.00 micron, and ratios of the aerosol extinction at 0.45 micron to the aerosol extinction at 1.00 micron are presented. The averages for l980 are shown in tables and in profile and contour plots (as a function of altitude and latitude). In addition, temperature data provided by the National Oceanic and Atmospheric Administration (NOAA) for the time and location of each SAGE measurement are averaged and shown in a similar format.

Characterization of particulate products for aging of ethylbenzene secondary organic aerosol in the presence of ammonium sulfate seed aerosol.

PubMed

Huang, Mingqiang; Zhang, Jiahui; Cai, Shunyou; Liao, Yingmin; Zhao, Weixiong; Hu, Changjin; Gu, Xuejun; Fang, Li; Zhang, Weijun

2016-09-01

Aging of secondary organic aerosol (SOA) particles formed from OH- initiated oxidation of ethylbenzene in the presence of high mass (100-300μg/m(3)) concentrations of (NH4)2SO4 seed aerosol was investigated in a home-made smog chamber in this study. The chemical composition of aged ethylbenzene SOA particles was measured using an aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with a Fuzzy C-Means (FCM) clustering algorithm. Experimental results showed that nitrophenol, ethyl-nitrophenol, 2,4-dinitrophenol, methyl glyoxylic acid, 5-ethyl-6-oxo-2,4-hexadienoic acid, 2-ethyl-2,4-hexadiendioic acid, 2,3-dihydroxy-5-ethyl-6-oxo-4-hexenoic acid, 1H-imidazole, hydrated N-glyoxal substituted 1H-imidazole, hydrated glyoxal dimer substituted imidazole, 1H-imidazole-2-carbaldehyde, N-glyoxal substituted hydrated 1H-imidazole-2-carbaldehyde and high-molecular-weight (HMW) components were the predominant products in the aged particles. Compared to the previous aromatic SOA aging studies, imidazole compounds, which can absorb solar radiation effectively, were newly detected in aged ethylbenzene SOA in the presence of high concentrations of (NH4)2SO4 seed aerosol. These findings provide new information for discussing aromatic SOA aging mechanisms. Copyright © 2016. Published by Elsevier B.V.

Coherent Uncertainty Analysis of Aerosol Measurements from Multiple Satellite Sensors

NASA Technical Reports Server (NTRS)

Petrenko, M.; Ichoku, C.

2013-01-01

Aerosol retrievals from multiple spaceborne sensors, including MODIS (on Terra and Aqua), MISR, OMI, POLDER, CALIOP, and SeaWiFS altogether, a total of 11 different aerosol products were comparatively analyzed using data collocated with ground-based aerosol observations from the Aerosol Robotic Network (AERONET) stations within the Multi-sensor Aerosol Products Sampling System (MAPSS, http://giovanni.gsfc.nasa.gov/mapss/ and http://giovanni.gsfc.nasa.gov/aerostat/). The analysis was performed by comparing quality-screened satellite aerosol optical depth or thickness (AOD or AOT) retrievals during 2006-2010 to available collocated AERONET measurements globally, regionally, and seasonally, and deriving a number of statistical measures of accuracy. We used a robust statistical approach to detect and remove possible outliers in the collocated data that can bias the results of the analysis. Overall, the proportion of outliers in each of the quality-screened AOD products was within 12%. Squared correlation coefficient (R2) values of the satellite AOD retrievals relative to AERONET exceeded 0.6, with R2 for most of the products exceeding 0.7 over land and 0.8 over ocean. Root mean square error (RMSE) values for most of the AOD products were within 0.15 over land and 0.09 over ocean. We have been able to generate global maps showing regions where the different products present advantages over the others, as well as the relative performance of each product over different landcover types. It was observed that while MODIS, MISR, and SeaWiFS provide accurate retrievals over most of the landcover types, multi-angle capabilities make MISR the only sensor to retrieve reliable AOD over barren and snow / ice surfaces. Likewise, active sensing enables CALIOP to retrieve aerosol properties over bright-surface shrublands more accurately than the other sensors, while POLDER, which is the only one of the sensors capable of measuring polarized aerosols, outperforms other sensors in

Size distribution of ions in atmospheric aerosols

NASA Astrophysics Data System (ADS)

Krivácsy, Z.; Molnár, Á.

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

Direct Aerosol Radiative Forcing: Calculations and Measurements from the Tropospheric

NASA Technical Reports Server (NTRS)

Russell, P. B.; Hignett, P.; Stowe, L. L.; Livingston, J. M.; Kinne, S.; Wong, J.; Chan, K. Roland (Technical Monitor)

1997-01-01

Radiative forcing is defined as the change in the net (downwelling minus upwelling) radiative flux at a given level in the atmosphere. This net flux is the radiative power density available to drive climatic processes in the earth-atmosphere system below that level. Recent research shows that radiative forcing by aerosol particles is a major source of uncertainty in climate predictions. To reduce those uncertainties, TARFOX was designed to determine direct (cloud-free) radiative forcing by the aerosols in one of the world's major industrial pollution plumes--that flowing from the east coast of the US over the Atlantic Ocean. TARFOX measured a variety of aerosol radiative effects (including direct forcing) while simultaneously measuring the chemical, physical, and optical properties of the aerosol particles causing those effects. The resulting data sets permit a wide variety of tests of the consistency, or closure, among the measurements and the models that link them. Because climate predictions use the same or similar model components, closure tests help to assess and reduce prediction uncertainties. In this work we use the TARFOX-determined aerosol, gas, and surface properties to compute radiative forcing for a variety of aerosol episodes, with inadvisable optical depths ranging from 0.07 to 0.6. We calculate forcing by several techniques with varying degrees of sophistication, in part to test the range of applicability of simplified techniques--which are often the only ones feasible in climate predictions by general circulation models (GCMs). We then compare computed forcing to that determined from: (1) Upwelling and downwelling fluxes (0.3-0.7 mm and 0.7-3.0 mm) measured by radiometers on the UK MRF C-130. and (2) Daily average cloud-free absorbed solar and emitted thermal radiative flux at the top of the atmosphere derived from the AVHRR radiometer on the NOAA- 14 satellite. The calculations and measurements all yield aerosol direct radiative forcing in the

Orbiting lidar simulations. I - Aerosol and cloud measurements by an independent-wavelength technique

NASA Technical Reports Server (NTRS)

Russell, P. B.; Morley, B. M.; Livingston, J. M.; Grams, G. W.; Patterson, E. M.

1982-01-01

Aerosol and cloud measurements have been simulated for a Space Shuttle lidar. Expected errors - in signal, transmission, density, and calibration - are calculated algebraically and checked by simulating measurements and retrievals using random-number generators. By day, vertical structure is retrieved for tenuous clouds, Saharan aerosols, and boundary layer aerosols (at 0.53 and 1.06 micron) as well as strong volcanic stratospheric aerosols (at 0.53 micron). By night, all these constituents are retrieved plus upper tropospheric and stratospheric aerosols (at 1.06 micron), mesospheric aerosols (at 0.53 micron), and noctilucent clouds (at 1.06 and 0.53 micron). The vertical resolution was 0.1-0.5 km in the troposphere, 0.5-2.0 km above, except 0.25-1.0 km in the mesospheric cloud and aerosol layers; horizontal resolution was 100-2000 km.

Airborne measurements of multi-wavelength aerosol optical depth and cloud-transmitted radiances in the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES)

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Johnson, R. R.; LeBlanc, S. E.; Chang, C. S.; Redemann, J.

2016-12-01

We report on our recent airborne measurements of multi-wavelength aerosol optical depth and cloud-transmitted radiances over the North Atlantic. We ran the Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) in November 2015 and the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) in May and June 2016, both aboard the NASA C-130 aircraft. These sunphotometers provide measurements of overlying cirrus and aerosol optical depths of up to about 0.5 and constrain ecosystem and aerosol retrievals from the accompanying nadir-viewing remote sensing instruments. In addition, 4STAR measures hyperspectral transmitted light, which enables the retrieval of cloud optical depth, effective radius, and thermodynamic phase from below cloud. Our measurements contribute to the science objectives of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES), an interdisciplinary investigation resolving key processes controlling marine ecosystems and aerosols that are essential to our understanding of Earth system function and future change.

Infrared Emission from Gas-Aerosol Reactions

DTIC Science & Technology

1982-09-01

Gaseous Amonia Infrared (IR) "Gas-aerosol Reactions Sulfuric Acid- amonia IR Luminescence Exothermic Reactions Octanoic Acid- amonia IR Laser Acid-base...of radiation observed from the reactions of chloro- sulfuric acid aerosol with gaseous amonia and water. Other systems which were screened including

Interpretation of DIAL Measurements of Lower Stratospheric Ozone in Regions with Pinatubo Aerosols

NASA Technical Reports Server (NTRS)

Grant, William B.; Browell, Edward V.; Fenn, Marta A.; Butler, Carolyn F.; Brackett, Vincent G.; Veiga, Robert E.; Mayor, Shane D.; Fishman, Jack; Nganga, D.; Minga, A.

1992-01-01

The influence of volcanic aerosols on stratospheric ozone is a topic of current interest, especially with the June 15, 1991 eruption of Mt. Pinatubo in the Philippines. Lidar has been used in the past to provide aerosol profiles which could be compared with ozone profiles measured using ozonesondes to look for coincidences between volcanic aerosols and ozone decreases. The differential absorption lidar (DIAL) technique has the advantages of being able to measure ozone and aerosol profiles simultaneously as well as being able to cover large geographical regions rapidly. While there are problems associated with correcting the ozone profiles for the presence of aerosols, the corrections can be made reliably when the wavelengths are closely spaced and the Bernoulli method is applied. The DIAL measurements considered in this paper are those obtained in the tropical stratosphere in January 1992 during the Airborne Arctic Stratospheric Expedition (AASE-II). The determination of ozone profiles in the presence of Pinatubo aerosols is discussed in a companion paper.

Remote sensing of aerosols over land surfaces from POLDER-ADEOS-1 polarized measurements

NASA Astrophysics Data System (ADS)

Deuzé, J. L.; BréOn, F. M.; Devaux, C.; Goloub, P.; Herman, M.; Lafrance, B.; Maignan, F.; Marchand, A.; Nadal, F.; Perry, G.; Tanré, D.

2001-03-01

The polarization measurements achieved by the POLDER instrument on ADEOS-1 are used for the remote sensing of aerosols over land surfaces. The key advantage of using polarized observations is their ability to systematically correct for the ground contribution, whereas the classical approach using natural light fails. The estimation of land surface polarizing properties from POLDER has been examined in a previous paper. Here we consider how the optical thickness δ0 and Ångstrom exponent α of aerosols are derived from the polarized light backscattered by the particles. The inversion scheme is detailed, and illustrative results are presented. Maps of the retrieved optical thickness allow for detection of large aerosol features, and in the case of small aerosols, the δ0 and α retrievals are consistent with correlative ground-based measurements. However, because polarized light stems mainly from small particles, the results are biased for aerosol distributions containing coarser modes of particles. To overcome this limitation, an aerosol index defined as the product AI = δ0α is proposed. Theoretical analysis and comparison with ground-based measurements suggest that AI is approximately the same when using δ0, and α is related to the entire aerosol size distribution or derived from the polarized light originating from the small polarizing particles alone. This invariance is specially assessed by testing the continuity of AI across coastlines, given the unbiased properties of aerosol retrieval over ocean. Although reducing the information concerning the aerosols, this single parameter allows a link between the POLDER aerosol surveys over land and ocean. POLDER aerosol index global maps enable the monitoring of major aerosol sources over continental areas.

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

NASA Technical Reports Server (NTRS)

Ricci, K.; Strawa, A. W.; Provencal, R.; Castaneda, R.; Bucholtz, A.; Schmid, B.

2004-01-01

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 with an estimated precision of 0.1/Mm for 1550 nm light and 0.2/Mm 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 from 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.

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

NASA Astrophysics Data System (ADS)

Ricci, K.; Strawa, A. W.; Provencal, R.; Castaneda, R.; Bucholtz, A.; Schmid, B.

2003-12-01

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 Mm-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 from a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS14 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.

Spectral Aerosol Extinction (SpEx): A New Instrument for In situ Ambient Aerosol Extinction Measurements Across the UV/Visible Wavelength Range

NASA Technical Reports Server (NTRS)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Corr, C. A.; Dibb, J. E.; Greenslade, M. E.; Martin, R. F.; Moore, R. H.; Scheuer, E.; Shook, M. A.;

Measurements of HNO3, SO2 High Resolution Aerosol SO4 (sup 2-), and Selected Aerosol Species Aboard the NASA DC-8 Aircraft: During the Transport and Chemical Evolution Over the Pacific Airborne Mission (TRACE-P)

NASA Technical Reports Server (NTRS)

Talbot, Robert W.; Dibb, Jack E.

2004-01-01

The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.

The Measurement of Aerosol Optical Properties Using Continuous Wave Cavity Ring-Down Techniques

NASA Technical Reports Server (NTRS)

Strawa, A. W.; Owano, T.; Castaneda, R.; Baer, D. S.; Paldus, B. A.; Gore, Warren J. (Technical Monitor)

2002-01-01

Large uncertainties in the effects that aerosols have on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This abstract describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5/Mm). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

Raman lidar measurements of aerosol extinction and backscattering: 2. Derivation of aerosol real refractive index, single-scattering albedo, and humidification factor using Raman lidar and aircraft size distribution measurements

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Melfi, S. H.; Whiteman, D. N.; Evans, K. D.; Poellot, M.; Kaufman, Y. J.

1998-08-01

Aerosol backscattering and extinction profiles measured 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 during two nights in April 1994 are discussed. These profiles are shown to be consistent with the simultaneous aerosol size distribution measurements made by a PCASP (Passive Cavity Aerosol Spectrometer Probe) optical particle counter flown on the University of North Dakota Citation aircraft. We describe a technique which uses both lidar and PCASP measurements to derive the dependence of particle size on relative humidity, the aerosol real refractive index n, and estimate the effective single-scattering albedo ω0. Values of n ranged between 1.4-1.5 (dry) and 1.37-1.47 (wet); ω0 varied between 0.7 and 1.0. The single-scattering albedo derived from this technique is sensitive to the manner in which absorbing particles are represented in the aerosol mixture; representing the absorbing particles as an internal mixture rather than the external mixture assumed here results in generally higher values of ω0. The lidar measurements indicate that the change in particle size with relative humidity as measured by the PCASP can be represented in the form discussed by Hanel [1976] with the exponent γ = 0.3 ± 0.05. The variations in aerosol optical and physical characteristics captured in the lidar and aircraft size distribution measurements are discussed in the context of the meteorological conditions observed during the experiment.

Satellite measurements of aerosol mass and transport

NASA Technical Reports Server (NTRS)

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

1984-01-01

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

Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

NASA Technical Reports Server (NTRS)

Wang, Jian; Collins, Don; Covert, David; Elleman, Robert; Ferrare, Richard A.; Gasparini, Roberto; Jonsson, Haflidi; Ogren, John; Sheridan, Patrick; Tsay, Si-Chee

2006-01-01

Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

Seasonal measurements of organic acid fluxes over a ponderosa pine forest

NASA Astrophysics Data System (ADS)

Fulgham, S. R.; Brophy, P.; Link, M.; Ortega, J. V.; Farmer, D.

2016-12-01

The biosphere acts as both a source and a sink of oxidized organic compounds. Ignoring dry deposition leads to overestimation of secondary organic aerosols by aerosol models, while ignoring emission sources underestimates the budget of organic acids. Developing parameterizations for oxidized organic dry deposition and emission requires observational constraints. Although biosphere parameters are impacted by seasonal variability, most reactive, trace-gas exchange measurements are made for only short periods of time in the main growing season. Here we make fast (5 - 10 Hz) and sensitive (e.g. 0.73 ppt mean limit of detection for formic acid with 10 s averaging) eddy covariance measurements of gas-phase organic acids and other oxidized organic species with a high resolution Time-of-Flight Chemical Ionization Mass Spectrometer with acetate and iodide reagent ions. Measurements were made in 4 - 6 week campaigns over five seasons from summer 2015 to fall 2016 as part of the Seasonal Particles in Forests Flux studY (SPIFFY) at the Manitou Experimental Forest Observatory near Woodland Park, Colorado. Permeation tubes were used for online calibration of carboxylic acids including formic (C1), propionic (C3), butyric (C4), methacrylic (CH2C(CH3)COOH), valeric (C5), and heptanoic (C7) acids. Average daytime mixing ratios for formic acid were 100 ± 100 ppt in winter and 1500 ± 1000 ppt in summer 2016. Upward fluxes of formic acid were observed throughout the experiment, daytime averages and standard deviations ranging from 1900 ± 1000 ppt cm s-1 in winter to 170 ± 130 ppt cm s-1 in spring. Propionic (22 ± 22 ppt cm s-1), butyric (17 ± 16 ppt cm s-1), and methacrylic (3.5 ± 6.1 ppt cm s-1) acids exhibit a mix of upward, near-zero, and downward fluxes. Fluxes were exponentially correlated to temperature, suggesting an ecosystem-scale source of these acids. We also measure exchange velocities of a broad suite of other oxidized organic compounds (31.99 m/z to 311.523 m/z in

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

Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

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

Kleinman L. I.; Daum, P. H.; Lee, Y.-N.

2012-01-04

During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate. Pollutant layers in the free troposphere (FT) can be a result of emissionsmore » to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a boundary layer (BL) contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (D{sub p} > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25 % of aerosol with D{sub p} > 100 nm are interstitial (not activated). A direct comparison of pre-cloud and in-cloud aerosol yields a higher estimate. Artifacts in the measurement of interstitial aerosol due to droplet shatter and evaporation are discussed. Within each of 102 constant altitude cloud transects, CDNC and interstitial aerosol were anti-correlated. An examination of one cloud as a case study shows that the

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

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

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

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

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

DOE PAGES

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

2017-10-30

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

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

PubMed

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

2017-10-01

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

Citizen-Enabled Aerosol Measurements for Satellites (CEAMS): A Network for High-Resolution Measurements of PM2.5 and Aerosol Optical Depth

NASA Astrophysics Data System (ADS)

Pierce, J. R.; Volckens, J.; Ford, B.; Jathar, S.; Long, M.; Quinn, C.; Van Zyl, L.; Wendt, E.

2017-12-01

Atmospheric particulate matter with diameter smaller than 2.5 μm (PM2.5) is a pollutant that contributes to the development of human disease. Satellite-derived estimates of surface-level PM2.5 concentrations have the potential to contribute greatly to our understanding of how particulate matter affects health globally. However, these satellite-derived PM2.5 estimates are often uncertain due to a lack of information about the ratio of surface PM2.5 to aerosol optical depth (AOD), which is the primary aerosol retrieval made by satellite instruments. While modelling and statistical analyses have improved estimates of PM2.5:AOD, large uncertainties remain in situations of high PM2.5 exposure (such as urban areas and in wildfire-smoke plumes) where the health impacts of PM2.5 may be the greatest. Surface monitoring networks for co-incident PM2.5 and AOD measurements are extremely rare, even in the North America. To provide constraints for the PM2.5:AOD relationship, we have developed a relatively low-cost (<$1000) monitor for citizen use that provides sun-photometer AOD measurements and filter-based PM2.5 measurements. The instrument is solar-powered, lightweight (< 1kg), and operated wirelessly via smartphone application (iOS and Android). Sun photometry is performed across 4 discrete wavelengths that match those reported by the Aerosol Robotic Network (AERONET). Aerosol concentration is reported using both time-integrated filter mass (analyzed in an academic laboratory and reported as a 24-48hr average) and a continuous PM sensor within the instrument. Citizen scientists use the device to report daily AOD and PM2.5 measurements made in their backyards to a central server for data display and download. In this presentation, we provide an overview of (1) AOD and PM2.5 measurement calibration; (2) citizen recruiting and training efforts; and (3) results from our pilot citizen-science measurement campaign.

The ambient organic aerosol soluble in water: Measurements, chemical characterization, and an investigation of sources

NASA Astrophysics Data System (ADS)

Sullivan, Amy P.

hydrophobic fraction. By coupling a PILS with this technique, on-line measurements of WSOC, hydrophilic WSOC, and hydrophobic WSOC are possible. Urban measurements from St. Louis and Atlanta, on a carbon mass basis, show an increase in the mean WSOC fraction from winter (51%) to summer (61%), due to increases in the hydrophilic WSOC to OC ratio from 0.25 to 0.35. During a summer Atlanta PM event, WSOC to OC was 0.75, driven largely by increases in the hydrophilic WSOC fraction. The results are consistent with the view that in the summer there are increased amounts of oxygenated polar compounds, that are mainly hydrophilic and possibly from SOA production. These compounds can account for an even larger fraction of OC during stagnation events. The XAD-8 resin can also be used in the first step of a two-step off-line method to isolate chemical fractions of ambient organic aerosol based on acid, neutral, and basic functional groups. The second step is a newly developed method involving size-exclusion chromatography (SEC) to separate the hydrophilic WSOC and recovered hydrophobic WSOC compounds by organic functional group. Calibrations show that hydrophilic WSOC separates into short-chain aliphatic acids, neutrals (e.g. saccharides, polyols, and short-chain carbonyls), and organic bases. The recovered hydrophobic compounds are separated into acids (e.g., aromatic) and neutrals (e.g., phenols). Comparisons are made between XAD-8/SEC results from urban Atlanta summer and winter, and biomass burning samples. During the summer in Atlanta, approximately 20% of the OC (on a carbon mass basis) is due to hydrophilic aliphatic acids and recovered hydrophobic acids. The hydrophilic aliphatic acids are additionally the largest isolated fraction of Atlanta summer WSOC (29% microg C/microg C), suggesting aliphatic acids of less than C4 or C5 are the dominant SOA product, and are also correlated with the recovered hydrophobic acids (R2 = 0.74), elemental carbon (R2 = 0.64), CO (R2 = 0.73), and

Retrieving the Vertical Structure of the Effective Aerosol Complex Index of Refraction from a Combination of Aerosol in Situ and Remote Sensing Measurements During TARFOX

NASA Technical Reports Server (NTRS)

Redemann, J.; Turco, R. P.; Liou, K. N.; Russell, P. B.; Bergstrom, R. W.; Schmid, B.; Livingston, J. M.; Hobbs, P. V.; Hartley, W. S.; Ismail, S.;

A study of the sea-salt chemistry using size-segregated aerosol measurements at coastal Antarctic station Neumayer

NASA Astrophysics Data System (ADS)

Teinilä, K.; Frey, A.; Hillamo, R.; Tülp, H. C.; Weller, R.

2014-10-01

Aerosol chemical and physical properties were measured in 2010 at Neumayer research station, Antarctica. Samples for chemical analysis (ion chromatography) were collected using a Teflon/Nylon filter combination (TNy) sampler, and with a multi stage low pressure impactor (SDI). Particle number concentration was measured continuously with a Grimm OPC optical particle counter. Total particle number concentration varied largely throughout the year, and the highest number concentrations for particles larger than 0.3 μm were observed simultaneously with the highest sea salt concentrations. About 50% of the sea salt aerosol mass was found in the submicron size range. Below 0.2 μm of particle aerodynamic diameter the contribution of sea salt aerosols was negligible. Further analysis showed that sea salt aerosols had undergone physico-chemical processes, either during the transportation, or during their formation. High degree of chloride depletion was observed during austral summer, when the presence of acidic gases exhibit their characteristic seasonal maximum. Apart from chloride depletion, excess chloride relating to sodium was also detected in one SDI sample, indicating actually a sodium depletion by mirabilite formation on freshly formed sea ice areas. Analysis of selected episodes showed that the concentration of sea salt particles, their modal structure, and their chemical composition is connected with their source areas, their formation mechanisms, and local transport history.

Directions for combustion engine aerosol measurement in the 21st century.

PubMed

Maricq, M Matti; Maldonado, Hector

2010-10-01

The Coordinating Research Council convened two Real-Time PM Measurement Workshops in December 2008 and March 2009 to take an intensive look at the current status and future directions of combustion aerosol measurement. The purpose was to examine the implications of parallel rapid developments over the past decade in ambient aerosol science, engine aftertreatment technology, and aerosol measurement methodology, which provide benefits and challenges to the stakeholders in air quality management. The workshops were organized into sessions targeting key issues in ambient and source combustion particulate matter (PM). These include (1) metrics to characterize and quantify PM, (2) the need to reconcile ambient and source measurements, (3) the role of atmospheric transformations on modeling emissions and exposures, (4) the impact of sampling conditions on PM measurement, and (5) the potential benefits of novel PM instrumentation. This paper distills the material presented by subject experts and the insights derived from the in-depth discussions that formed the core of each session. The paper's objectives are to identify areas of consensus that allow wider practical application of the past decade's advances in combustion aerosol measurement to improve emissions and air quality modeling, develop emissions reduction strategies, and to recommend directions for progress on issues in which uncertainties remain.

Airborne Sunphotometer Measurements of Aerosol Optical Depth and Water Vapor in ACE-Asia and Their Comparisons to Correlative Measurements

NASA Technical Reports Server (NTRS)

Schmid, B.; Redemann, J.; Livingston, J.; Russell, P.; Hegg, D.; Wang, J.; Kahn, R.; Hsu, C.; Masonis, S.; Murayama, T.;

Aerosol typing - key information from aerosol studies

NASA Astrophysics Data System (ADS)

Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

2016-04-01

Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

The Measurement of Aerosol Optical Properties using Continuous Wave Cavity Ring-Down Techniques

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Castaneda, Rene; Owano, Thomas; Baer, Douglas S.; Paldus, Barbara A.; Gore, Warren J. (Technical Monitor)

2002-01-01

Large uncertainties in the effects that aerosols have on climate require improved in situ measurements of extinction coefficient and single-scattering albedo. This paper describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5 M/m). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

Combining Airborne and Lidar Measurements for Attribution of Aerosol Layers

NASA Astrophysics Data System (ADS)

Nikandrova, A.; Väänänen, R.; Tabakova, K.; Kerminen, V. M.; O'Connor, E.

2016-12-01

The aim of this work was to identify discrete aerosol layers and diagnose their origin, investigate the strength of mixing within the free-troposphere and with the boundary layer (BL), and understand the impact that mixing has on local and long-range transport of aerosol. For these purposes we combined airborne in-situ aerosol measurements with data obtained by a High Spectral Resolution Lidar (HSRL). The HSRL was deployed in Hyytiälä, Southern Finland, from January to September 2014 as a part of the US DoE ARM (Atmospheric Radiation Measurement) Mobile Facility during the BAECC (Biogenic Aerosols - Effects on Cloud and Climate) Campaign. Two airborne campaigns took place in April and August 2014 during the BAECC campaign. The vertical profile of backscatter coefficient from the HSRL was used to diagnose the location and depth of significant aerosol layers in the atmosphere. Frequently, in addition to the BL, one or two tropospheric layers were identified. In-situ measurements of the aerosol size distribution in these layers were obtained from a Scanning Mobility Particle Sizer (SMPS) and Optical Particle Sizer (OPS), that were installed on board the aircraft; these measurements were combined to cover sizes ranging from 10 nm to 10 µm. As expected, the highest number concentration of aerosol particles at all size ranges was found predominantly in the BL. Many upper layers had size distributions with a similar shape to that in the BL but with overall lower concentrations attributed to dilution of particles into a large volume of air. Hence, these layers were likely of very similar origin to the air in the BL and presumably were the result of lofted residual layers. Intervening layers however, could contain markedly different distribution shapes, which could be attributed to both different air mass origins, and different ambient relative humidity. Potential for mixing between two discreet elevated layers was often seen as a thin interface layer, which exhibited a

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

Retrieving the Vertical Structure of the Effective Aerosol Complex Index of Refraction from a Combination of Aerosol in Situ and Remote Sensing Measurements During TARFOX

NASA Technical Reports Server (NTRS)

Redemann, J.; Turco, R. P.; Liou, K. N.; Russell, P. B.; Bergstrom, R. W.; Schmid, B.; Livingston, J. M.; Hobbs, P. V.; Hartley, W. S.; Ismail, S.

2000-01-01

The largest uncertainty in estimates of the effects of atmospheric aerosols on climate stems from uncertainties in the determination of their microphysical properties, including the aerosol complex index of refraction, which in turn determines their optical properties. A novel technique is used to estimate the aerosol complex index of refraction in distinct vertical layers from a combination of aerosol in situ size distribution and remote sensing measurements during the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX). In particular, aerosol backscatter measurements using the NASA Langley LASE (Lidar Atmospheric Sensing Experiment) instrument and in situ aerosol size distribution data are utilized to derive vertical profiles of the 'effective' aerosol complex index of refraction at 815 nm (i.e., the refractive index that would provide the same backscatter signal in a forward calculation on the basis of the measured in situ particle size distributions for homogeneous, spherical aerosols). A sensitivity study shows that this method yields small errors in the retrieved aerosol refractive indices, provided the errors in the lidar derived aerosol backscatter are less than 30% and random in nature. Absolute errors in the estimated aerosol refractive indices are generally less than 0.04 for the real part and can be as much as 0.042 for the imaginary part in the case of a 30% error in the lidar-derived aerosol backscatter. The measurements of aerosol optical depth from the NASA Ames Airborne Tracking Sunphotometer (AATS-6) are successfully incorporated into the new technique and help constrain the retrieved aerosol refractive indices. An application of the technique to two TARFOX case studies yields the occurrence of vertical layers of distinct aerosol refractive indices. Values of the estimated complex aerosol refractive index range from 1.33 to 1.45 for the real part and 0.001 to 0.008 for the imaginary part. The methodology devised in this study

Chemical evolution of multicomponent aerosol particles during evaporation

NASA Astrophysics Data System (ADS)

Zardini, Alessandro; Riipinen, Ilona; Pagels, Joakim; Eriksson, Axel; Worsnop, Douglas; Switieckli, Erik; Kulmala, Markku; Bilde, Merete

2010-05-01

Atmospheric aerosol particles have an important but not well quantified effect on climate and human health. Despite the efforts made in the last decades, the formation and evolution of aerosol particles in the atmosphere is still not fully understood. The uncertainty is partly due to the complex chemical composition of the particles which comprise inorganic and organic compounds. Many organics (like dicarboxylic acids) can be present both in the gas and in the condensed phase due to their low vapor pressure. Clearly, an understanding of this partition is crucial to address any other issue in atmospheric physics and chemistry. Moreover, many organics are water soluble, and their influence on the properties of aqueous solution droplets is still poorly characterized. The solid and sub-cooled liquid state vapor pressures of some organic compounds have been previously determined by measuring the evaporation rate of single-compound crystals [1-3] or binary aqueous droplets [4-6]. In this work, we deploy the HTDMA technique (Hygroscopicity Tandem Differential Mobility Analyzer) coupled with a 3.5m laminar flow-tube and an Aerosol Mass Spectrometer (AMS) for determining the chemical evolution during evaporation of ternary droplets made of one dicarboxylic acid (succinic acid, commonly found in atmospheric samples) and one inorganic compound (sodium chloride or ammonium sulfate) in different mixing ratios, in equilibrium with water vapor at a fixed relative humidity. In addition, we investigate the evaporation of multicomponent droplets and crystals made of three organic species (dicarboxylic acids and sugars), of which one or two are semi-volatile. 1. Bilde M. and Pandis, S.N.: Evaporation Rates and Vapor Pressures of Individual Aerosol Species Formed in the Atmospheric Oxidation of alpha- and beta-Pinene. Environmental Science and Technology, 35, 2001. 2. Bilde M., et al.: Even-Odd Alternation of Evaporation Rates and Vapor Pressures of C3-C9 Dicarboxylic Acid Aerosols

Impact of Tropospheric Aerosol Absorption on Ozone Retrieval from buv Measurements

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.

1998-01-01

The impact of tropospheric aerosols on the retrieval of column ozone amounts using spaceborne measurements of backscattered ultraviolet radiation is examined. Using radiative transfer calculations, we show that uv-absorbing desert dust may introduce errors as large as 10% in ozone column amount, depending on the aerosol layer height and optical depth. Smaller errors are produced by carbonaceous aerosols that result from biomass burning. Though the error is produced by complex interactions between ozone absorption (both stratospheric and tropospheric), aerosol scattering, and aerosol absorption, a surprisingly simple correction procedure reduces the error to about 1%, for a variety of aerosols and for a wide range of aerosol loading. Comparison of the corrected TOMS data with operational data indicates that though the zonal mean total ozone derived from TOMS are not significantly affected by these errors, localized affects in the tropics can be large enough to seriously affect the studies of tropospheric ozone that are currently undergoing using the TOMS data.

Intercomparison of in situ and remote sensing aerosol measurements in the lowermost stratosphere during varying volcanic influence

NASA Astrophysics Data System (ADS)

Sandvik, Oscar S.; Martinsson, Bengt G.; Friberg, Johan; Hermann, Markus; van Velthoven, Peter J. F.; Zahn, Andreas

2017-04-01

In this study two aerosol measurement platforms have been compared. Aerosol optical depth (AOD) per meter in the lowermost stratosphere was obtained with the "In-service Aircraft for a Global Observing System - Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container" (IAGOS-CARIBIC) platform and with the "Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation" (CALIPSO) satellite. The in situ measurements were taken from the IAGOS-CARIBIC platform, where sampling of aerosol and trace gases was undertaken in the altitude range 9 - 12 km from a passenger aircraft, usually on four intercontinental flights a month (Brenninkmeijer et al., 2007). Here we use impactor samples that were analyzed for elemental concentrations with Particle-Induced X-ray Emission (PIXE) and Particle Elastic Scattering Analysis (PESA) (Nguyen et al., 2006; Martinsson et al., 2014). The comparison was based on the sulfurous aerosol, which is the main component of the aerosol in the stratosphere. From the amount of sulfur, the AOD per meter could be estimated, assuming standard stratospheric aerosol composition (75% sulfuric acid and 25% water) and stratospheric background particle size distribution (Jäger and Deshler, 2002). The CALIPSO measurements were taken with a polarization-sensitive lidar with a high vertical resolution, of 30 m at most, using laser wavelengths of 532 nm and 1064 nm. In this study level 1b data was used to calculate AOD per meter. Clouds were removed based on depolarization ratio (Vernier et al., 2009). The results from the two measurement platforms were compared with each other for time periods after the volcanic eruptions of Sarychev (2009) and Nabro (2011) as well as the period from autumn 2013 to early spring of 2014 which had small volcanic influence. The measurements in this study were taken between 40°N and 75°N. Vertical profiles of AOD per meter were created for data above the tropopause. In this study the

RADIOCARBON MEASUREMENTS ON PM-2.5 AMBIENT AEROSOL

EPA Science Inventory

Radiocarbon (14C) measurements provide an estimate of the fraction of carbon in a sample that is biogenic. The methodology has been extensively used in past wintertime studies to quantify the contribution of wood smoke to ambient aerosol. In summertime such measurements can p...

Hygroscopic Measurements of Aerosol Particles in Colorado during the Discover AQ Campaign 2014

NASA Astrophysics Data System (ADS)

Orozco, D.; Delgado, R.; Espinosa, R.; Martins, J. V.; Hoff, R. M.

2014-12-01

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 and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground observations with other optical aerosol measurements such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. In the summer of 2014, the DISCOVER-AQ campaign was held in Colorado, where systematic and concurrent observations of column- integrated surface, and vertically-resolved distributions of aerosols and trace gases relevant to air quality and their evolution during the day were observed. Aerosol optical properties were measured in the UMBC trailer at the city of Golden using a TSI-3563 nephelometer and an in-situ Polarized Imaging Nephelometer (PI-NEPH) designed and built by the LACO group at UMBC. The PI-NEPH measures aerosol phase matrix components in high angular range between 2 and 178 degrees scattering angle at three wavelengths (λ=473, 532 and 671nm). The two measured elements of the phase matrix, intensity (P11) and linear polarization (P12) provide extensive characterization of the scattering properties of the studied aerosol. The scattering coefficient, P11 and P12 were measured under different humidity conditions to obtain the enhancement factor f(RH) and the dependence of P11 and P12 to RH using a humidifier dryer system covering a RH range from 20 to 90%. The ratio between scattering coefficients at high and low humidity in Golden Colorado showed relatively low hygroscopic growth in the aerosol particles f(RH=80%) was 1.27±0.19 for the first three weeks of sampling. According to speciated measurements performed at the UMBC trailer, the predominance of dust and organic aerosols over more hygroscopic nitrate and sulfate in the

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.

Measurements of Intensive Aerosol Optical Properties During TexAQS II

NASA Astrophysics Data System (ADS)

Atkinson, D. B.; Radney, J. G.; Wright, M. E.

2007-12-01

Time-resolved measurements of the bulk extensive aerosol optical properties - particle extinction coefficient (bext) and particle scattering coefficient (bscat) - and particle number concentrations were made as part of the six-week TRAMP experiment during the TexAQS II (2006) study. These measurements were done at a nominal surface site (the roof of an 18 story building) on the University of Houston campus near downtown Houston, Texas. Our ground-based tandem cavity ring-down transmissometer/nephelometer instrument (CRDT/N) provided the aerosol optical property measurements. A commercial Condensation Particle Counter (TSI 3007) was used to measure the number concentrations during part of the study period. The optical data was used to construct the intensive aerosol optical properties single scattering albedo ω0 at 532 nm and the Angstrom exponent for extinction between 532 nm and 1064 nm. Recent validation studies of size- selected laboratory generated aerosols are presented to illustrate the soundness of this approach using our instrument. The Angstrom exponent is compared to values from other instruments operating in the area and is found to be a characteristic of the regional air mass under some conditions. Size distributions measured during the study were used to create a new empirical adjustment to scattering measured by the Radiance Research nephelometer, resulting in improved results for particle absorption coefficient and single scattering albedo. The study average value of ω0(532 nm) = 0.78 is lower than expected from comparable field studies and even lower values are experienced during the study. Possible causes of this discrepancy are examined and the utility of using the current version of the CRDT/N instrument to measure the key radiative property ω0 is assessed. Observed episodes of rapid increases in particle number concentration with little corresponding growth in the optical properties can presumably be used to signal the occurrence of particle

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.

Seasonal variations of low molecular weight hydroxy-dicarboxylic acids and oxaloacetic acid in remote marine aerosols from Chichijima Island in the western North Pacific (December 2010-November 2011)

NASA Astrophysics Data System (ADS)

Gowda, Divyavani; Kawamura, Kimitaka

2018-05-01

Concentrations of homologous hydroxy-dicarboxylic acids (diacids) (hC3-hC6) and keto-diacid (oxaloacetic acid) were measured in the atmospheric aerosols collected at Chichijima Island (27.04° N, 142.13° E) in the western North Pacific from December 2010 to November 2011. The monthly averaged concentrations of hydroxy-diacids and oxaloacetic acid were significantly higher in spring followed by winter and autumn. Molecular distributions of hydroxy-diacids demonstrated that malic acid was the most abundant species in all four seasons, followed by tartronic acid in winter and spring and 3- and 2-hydroxyglutaric acids in summer and autumn. Hydroxy-diacids and keto-diacid maximized in spring and winter when air masses originated from the Asian continent with westerly winds. The concentrations of total hydroxy-diacids and oxaloacetic acid ranged from 0.1 to 27.3 ng m-3 and <0.005 to 2 ng m-3, respectively. The enhanced concentrations of diacids and their intermediates in winter and spring are associated with a long-range atmospheric transport of pollutants from East Asia to remote Chichijima Island followed by photochemical processing of organic aerosols. Seasonal molecular distribution of hydroxy-diacids and oxaloacetic acid was found to be dependent on the source strengths and plausible photochemical processing to form smaller diacids. Moderate to strong correlations among hydroxy-diacids, oxaloacetic acid and low molecular weight (LMW) diacids suggest that hydroxy-diacids and oxaloacetic acid are the intermediates in the photochemical oxidation of LMW diacid. Hence, photochemical formation of the most abundant LMW diacids, i.e., oxalic acid, could be produced from hydroxy- and keto-diacid as intermediates.

Laboratory studies of stratospheric aerosol chemistry

NASA Technical Reports Server (NTRS)

Molina, Mario J.

1996-01-01

In this report we summarize the results of the two sets of projects funded by the NASA grant NAG2-632, namely investigations of various thermodynamic and nucleation properties of the aqueous acid system which makes up stratospheric aerosols, and measurements of reaction probabilities directly on ice aerosols with sizes corresponding to those of polar stratospheric cloud particles. The results of these investigations are of importance for the assessment of the potential stratospheric effects of future fleets of supersonic aircraft. In particular, the results permit to better estimate the effects of increased amounts of water vapor and nitric acid (which forms from nitrogen oxides) on polar stratospheric clouds and on the chemistry induced by these clouds.

Laser radar measurements of the aerosol content of the atmosphere

NASA Technical Reports Server (NTRS)

Grams, G. W.

1969-01-01

A summary of the results of laser radar observations of atmospheric aerosols is presented along with a description of the laser radar system devised during the study and of the data handling techniques utilized for the analysis of the data of the temporal and spatial distribution of atmospheric aerosols. Current research conducted by the group is directed toward the analysis of the frequency spectrum of laser radar echoes to obtain absolute measurements of the dust content of the atmosphere by resolving the molecular and aerosol contributions to the laser radar echoes.

Chemical characteristics of size-resolved atmospheric aerosols in Iasi, north-eastern Romania: nitrogen-containing inorganic compounds control aerosol chemistry in the area

NASA Astrophysics Data System (ADS)

Giorgiana Galon-Negru, Alina; Iulian Olariu, Romeo; Arsene, Cecilia

2018-04-01

This study assesses the effects of particle size and season on the content of the major inorganic and organic aerosol ionic components in the Iasi urban area, north-eastern Romania. Continuous measurements were carried out over 2016 using a cascade Dekati low-pressure impactor (DLPI) performing aerosol size classification in 13 specific fractions over the 0.0276-9.94 µm size range. Fine-particulate Cl-, NO3-, NH4+, and K+ exhibited clear minima during the warm season and clear maxima over the cold season, mainly due to trends in emission sources, changes in the mixing layer depth and specific meteorological conditions. Fine-particulate SO42- did not show much variation with respect to seasons. Particulate NH4+ and NO3- ions were identified as critical parameters controlling aerosol chemistry in the area, and their measured concentrations in fine-mode (PM2.5) aerosols were found to be in reasonable good agreement with modelled values for winter but not for summer. The likely reason is that NH4NO3 aerosols are lost due to volatility over the warm season. We found that NH4+ in PM2.5 is primarily associated with SO42- and NO3- but not with Cl-. Actually, indirect ISORROPIA-II estimations showed that the atmosphere in the Iasi area might be ammonia rich during both the cold and warm seasons, enabling enough NH3 to be present to neutralize H2SO4, HNO3, and HCl acidic components and to generate fine-particulate ammonium salts, in the form of (NH4)2SO4, NH4NO3, and NH4Cl. ISORROPIA-II runs allowed us to estimate that over the warm season ˜ 35 % of the total analysed samples had very strongly acidic pH (0-3), a fraction that rose to ˜ 43 % over the cold season. Moreover, while in the cold season the acidity is mainly accounted for by inorganic acids, in the warm ones there is an important contribution by other compounds, possibly organic. Indeed, changes in aerosol acidity would most likely impact the gas-particle partitioning of semi-volatile organic acids. Overall, we

Hydrolysis of glyoxal in water-restricted environments: formation of organic aerosol precursors through formic acid catalysis.

PubMed

Hazra, Montu K; Francisco, Joseph S; Sinha, Amitabha

2014-06-12

The hydrolysis of glyoxal involving one to three water molecules and also in the presence of a water molecule and formic acid has been investigated. Our results show that glyoxal-diol is the major product of the hydrolysis and that formic acid, through its ability to facilitate intermolecular hydrogen atom transfer, is considerably more efficient than water as a catalyst in the hydrolysis process. Additionally, once the glyoxal-diol is formed, the barrier for further hydrolysis to form the glyoxal-tetrol is effectively reduced to zero in the presence of a single water and formic acid molecule. There are two important implications arising from these findings. First, the results suggest that under the catalytic influence of formic acid, glyoxal hydrolysis can impact the growth of atmospheric aerosols. As a result of enhanced hydrogen bonding, mediated through their polar OH functional groups, the diol and tetrol products are expected to have significantly lower vapor pressure than the parent glyoxal molecule; hence they can more readily partition into the particle phase and contribute to the growth of secondary organic aerosols. In addition, our findings provide insight into how glyoxal-diol and glyoxal-tetrol might be formed under atmospheric conditions associated with water-restricted environments and strongly suggest that the formation of these precursors for secondary organic aerosol growth is not likely restricted solely to the bulk aqueous phase as is currently assumed.

Aerosol Fragmentation Driven by Coupling of Acid–Base and Free-Radical Chemistry in the Heterogeneous Oxidation of Aqueous Citric Acid by OH Radicals

DOE PAGES

Liu, Matthew J.; Wiegel, Aaron A.; Wilson, Kevin R.; ...

2017-07-14

A key uncertainty in the heterogeneous oxidation of carboxylic acids by hydroxyl radicals (OH) in aqueous-phase aerosol is how the free-radical reaction pathways might be altered by acid-base chemistry. In particular, if acid-base reactions occur concurrently with acyloxy radical formation and unimolecular decomposition of alkoxy radicals, there is a possibility that differences in reaction pathways impact the partitioning of organic carbon between the gas and aqueous phases. To examine these questions, a kinetic model is developed for the OH-initiated oxidation of citric acid aerosol at high relative humidity. The reaction scheme, containing both free-radical and acid-base elementary reaction steps withmore » physically validated rate coefficients, accurately predicts the experimentally observed molecular composition, particle size, and average elemental composition of the aerosol upon oxidation. The difference between the two reaction channels centers on the reactivity of carboxylic acid groups. Free-radical reactions mainly add functional groups to the carbon skeleton of neutral citric acid, because carboxylic acid moieties deactivate the unimolecular fragmentation of alkoxy radicals. In contrast, the conjugate carboxylate groups originating from acid-base equilibria activate both acyloxy radical formation and carbon-carbon bond scission of alkoxy radicals, leading to the formation of low molecular weight, highly oxidized products such as oxalic and mesoxalic acid. Subsequent hydration of carbonyl groups in the oxidized products increases the aerosol hygroscopicity and accelerates the substantial water uptake and volume growth that accompany oxidation. These results frame the oxidative lifecycle of atmospheric aerosol: it is governed by feedbacks between reactions that first increase the particle oxidation state, then eventually promote water uptake and acid-base chemistry. When coupled to free-radical reactions, acid-base channels lead to formation of low

Aerosol Fragmentation Driven by Coupling of Acid–Base and Free-Radical Chemistry in the Heterogeneous Oxidation of Aqueous Citric Acid by OH Radicals

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

Liu, Matthew J.; Wiegel, Aaron A.; Wilson, Kevin R.

A key uncertainty in the heterogeneous oxidation of carboxylic acids by hydroxyl radicals (OH) in aqueous-phase aerosol is how the free-radical reaction pathways might be altered by acid-base chemistry. In particular, if acid-base reactions occur concurrently with acyloxy radical formation and unimolecular decomposition of alkoxy radicals, there is a possibility that differences in reaction pathways impact the partitioning of organic carbon between the gas and aqueous phases. To examine these questions, a kinetic model is developed for the OH-initiated oxidation of citric acid aerosol at high relative humidity. The reaction scheme, containing both free-radical and acid-base elementary reaction steps withmore » physically validated rate coefficients, accurately predicts the experimentally observed molecular composition, particle size, and average elemental composition of the aerosol upon oxidation. The difference between the two reaction channels centers on the reactivity of carboxylic acid groups. Free-radical reactions mainly add functional groups to the carbon skeleton of neutral citric acid, because carboxylic acid moieties deactivate the unimolecular fragmentation of alkoxy radicals. In contrast, the conjugate carboxylate groups originating from acid-base equilibria activate both acyloxy radical formation and carbon-carbon bond scission of alkoxy radicals, leading to the formation of low molecular weight, highly oxidized products such as oxalic and mesoxalic acid. Subsequent hydration of carbonyl groups in the oxidized products increases the aerosol hygroscopicity and accelerates the substantial water uptake and volume growth that accompany oxidation. These results frame the oxidative lifecycle of atmospheric aerosol: it is governed by feedbacks between reactions that first increase the particle oxidation state, then eventually promote water uptake and acid-base chemistry. When coupled to free-radical reactions, acid-base channels lead to formation of low

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

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

Physical properties of the stratospheric aerosols

NASA Technical Reports Server (NTRS)

Toon, O. B.; Pollack, J. B.

1973-01-01

A comparison of the equilibrium vapor pressure over nitric acid solutions with observed water and nitric acid partial pressures in the stratosphere implies that nitric acid cannot be present as an aerosol particle in the lower stratosphere. A similar comparison for sulfuric acid solutions indicates that sulfuric acid aerosol particles are 75% H2SO4 by weight in water, in good agreement with direct observations. The freezing curve of H2SO4 solutions requires that the H2SO4 aerosol particles be solid or supercooled. The equilibrium vapor pressure of H2SO4 in the stratosphere is of the order of 20 picotorr. At stratospheric temperatures, ammonium sulfate is in a ferroelectric phase. As a result, polar molecules may form a surface coating on these aerosols, which may be a fertile ground for further chemical reaction.

Passive remote sensing of aerosol layer height using near-UV multiangle polarization measurements

NASA Astrophysics Data System (ADS)

Wu, Lianghai; Hasekamp, Otto; van Diedenhoven, Bastiaan; Cairns, Brian; Yorks, John E.; Chowdhary, Jacek

2016-08-01

We demonstrate that multiangle polarization measurements in the near-UV and blue part of the spectrum are very well suited for passive remote sensing of aerosol layer height. For this purpose we use simulated measurements with different setups (different wavelength ranges, with and without polarization, different polarimetric accuracies) as well as airborne measurements from the Research Scanning Polarimeter (RSP) obtained over the continental USA. We find good agreement of the retrieved aerosol layer height from RSP with measurements from the Cloud Physics Lidar showing a mean absolute difference of less than 1 km. Furthermore, we found that the information on aerosol layer height is provided for large part by the multiangle polarization measurements with high accuracy rather than the multiangle intensity measurements. The information on aerosol layer height is significantly decreased when the shortest RSP wavelength (410 nm) is excluded from the retrieval and is virtually absent when 550 nm is used as shortest wavelength.

Secondary Organic Aerosol Formation from 2-Methyl-3-Buten-2-ol Photooxidation: Evidence of Acid-Catalyzed Reactive Uptake of Epoxides

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

Zhang, Haofei; Zhang, Zhenfa; Cui, Tianqu

2014-04-08

Secondary organic aerosol (SOA) formation from 2-methyl-3-buten-2-ol (MBO) photooxidation has recently been observed in both field and laboratory studies. Similar to isoprene, MBO-derived SOA increases with elevated aerosol acidity in the absence of nitric oxide; therefore, an epoxide intermediate, (3,3-dimethyloxiran-2-yl)methanol (MBO epoxide) was synthesized and tentatively proposed here to explain this enhancement. In the present study, the potential of the synthetic MBO epoxide to form SOA via reactive uptake was systematically examined. SOA was observed only in the presence of acidic aerosols. Major SOA constituents, 2,3-dihydroxyisopentanol (DHIP) and MBO-derived organosulfate isomers, were chemically characterized in both laboratory-generated SOA and inmore » ambient fine aerosols collected from the BEACHON-RoMBAS field campaign during summer 2011, where MBO emissions are substantial. Our results support epoxides as potential products of MBO photooxidation leading to formation of atmospheric SOA and suggest that reactive uptake of epoxides may generally explain acid enhancement of SOA observed from other biogenic hydrocarbons.« less

Quantification of uncertainty in aerosol optical thickness retrieval arising from aerosol microphysical model and other sources, applied to Ozone Monitoring Instrument (OMI) measurements

NASA Astrophysics Data System (ADS)

Määttä, A.; Laine, M.; Tamminen, J.; Veefkind, J. P.

2014-05-01

Satellite instruments are nowadays successfully utilised for measuring atmospheric aerosol in many applications as well as in research. Therefore, there is a growing need for rigorous error characterisation of the measurements. Here, we introduce a methodology for quantifying the uncertainty in the retrieval of aerosol optical thickness (AOT). In particular, we concentrate on two aspects: uncertainty due to aerosol microphysical model selection and uncertainty due to imperfect forward modelling. We apply the introduced methodology for aerosol optical thickness retrieval of the Ozone Monitoring Instrument (OMI) on board NASA's Earth Observing System (EOS) Aura satellite, launched in 2004. We apply statistical methodologies that improve the uncertainty estimates of the aerosol optical thickness retrieval by propagating aerosol microphysical model selection and forward model error more realistically. For the microphysical model selection problem, we utilise Bayesian model selection and model averaging methods. Gaussian processes are utilised to characterise the smooth systematic discrepancies between the measured and modelled reflectances (i.e. residuals). The spectral correlation is composed empirically by exploring a set of residuals. The operational OMI multi-wavelength aerosol retrieval algorithm OMAERO is used for cloud-free, over-land pixels of the OMI instrument with the additional Bayesian model selection and model discrepancy techniques introduced here. The method and improved uncertainty characterisation is demonstrated by several examples with different aerosol properties: weakly absorbing aerosols, forest fires over Greece and Russia, and Sahara desert dust. The statistical methodology presented is general; it is not restricted to this particular satellite retrieval application.

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

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

Jefferson, A.; Hageman, D.; Morrow, H.

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol hygroscopic growth. Annual average sub 10 um fRH values (the ratio of aerosol scattering at 85%/40% RH) were 1.75 and 1.87 for the gamma and kappa fit algorithms, respectively. The study found higher growth rates in the winter and spring seasons that correlated with high aerosol nitrate mass fraction. FRH, exhibited strong, but differing correlations with the scattering Ångström exponent and backscatter fraction, two opticalmore » size-dependent parameters. The aerosol organic fraction had a strong influence, with fRH decreasing with increases in the organic mass fraction and absorption Ångström exponent and increasing with the aerosol single scatter albedo. Uncertainty analysis if the fit algorithms revealed high uncertainty at low scattering coefficients and slight increases in uncertainty at high RH and fit parameters values.« less

Aerosol and gamma background measurements at Basic Environmental Observatory Moussala

NASA Astrophysics Data System (ADS)

Angelov, Christo; Arsov, Todor; Penev, Ilia; Nikolova, Nina; Kalapov, Ivo; Georgiev, Stefan

2016-03-01

Trans boundary and local pollution, global climate changes and cosmic rays are the main areas of research performed at the regional Global Atmospheric Watch (GAW) station Moussala BEO (2925 m a.s.l., 42°10'45'' N, 23°35'07'' E). Real time measurements and observations are performed in the field of atmospheric chemistry and physics. Complex information about the aerosol is obtained by using a threewavelength integrating Nephelometer for measuring the scattering and backscattering coefficients, a continuous light absorption photometer and a scanning mobile particle sizer. The system for measuring radioactivity and heavy metals in aerosols allows us to monitor a large scale radioactive aerosol transport. The measurements of the gamma background and the gamma-rays spectrum in the air near Moussala peak are carried out in real time. The HYSPLIT back trajectory model is used to determine the origin of the data registered. DREAM code calculations [2] are used to forecast the air mass trajectory. The information obtained combined with a full set of corresponding meteorological parameters is transmitted via a high frequency radio telecommunication system to the Internet.

Evaluating aerosol influence on cloud models using in-situ measurements during the INUPIAQ campaign

NASA Astrophysics Data System (ADS)

Farrington, R.; Connolly, P.; Choularton, T.; Bower, K.; Lloyd, G.; Flynn, M.; Crosier, J.; Field, P.

2014-12-01

At temperatures between -35°C and 0°C, the presence of insoluble aerosols acting as ice nuclei (IN) initiate the nucleation of ice under atmospheric conditions. Previous field and laboratory campaigns have suggested that mineral dust present in the atmosphere act as IN at temperatures around -20°C (e.g. Sassen et al. 2003), however the cause of ice nucleation at temperatures of around -5°C is less certain. Coupled with the limited representation of aerosol and cloud processes in large-scale weather and climate models, the need for improved in-situ measurements of aerosol properties and cloud micro-physical processes to drive the improvement of aerosol-clouds processes in models is evident. As part of the Ice NUcleation Process Investigation and Quantification (INUPIAQ) project, two field campaigns were conducted in early 2013 and early 2014. Both campaigns included measurements of cloud micro-physical properties at the summit of Jungfraujoch in Switzerland (3580m asl). Using data from the 2013 campaign and modelling simulations from the Weather Research and Forecasting model (WRF), an upwind site, located at Schilthorn (2970m asl), was determined for measuring aerosol properties out of cloud during the 2014 campaign. Further measurements of the cloud and aerosols properties were taken remotely using a doppler LiDAR located at Kleine Scheidegg (2061m asl). The aim of this project is to determine whether detailed aerosol information is important to determining cloud and precipitation properties downwind. To this end WRF was run using the aerosol number concentrations and size distributions measured at the Schilthorn site to compare modelled ice number concentrations with measurements taken at Jungfraujoch using state of the science cloud ice probes, including the Three-View Cloud Particle Imager (3V-CPI) and the Cloud Aerosol Spectrometer with Depolarization (CAS-DPOL), with the results of the comparison presented and discussed at this meeting. References

Eddy Covariance Measurements of the Sea-Spray Aerosol Flu

NASA Astrophysics Data System (ADS)

Brooks, I. M.; Norris, S. J.; Yelland, M. J.; Pascal, R. W.; Prytherch, J.

2015-12-01

Historically, almost all estimates of the sea-spray aerosol source flux have been inferred through various indirect methods. Direct estimates via eddy covariance have been attempted by only a handful of studies, most of which measured only the total number flux, or achieved rather coarse size segregation. Applying eddy covariance to the measurement of sea-spray fluxes is challenging: most instrumentation must be located in a laboratory space requiring long sample lines to an inlet collocated with a sonic anemometer; however, larger particles are easily lost to the walls of the sample line. Marine particle concentrations are generally low, requiring a high sample volume to achieve adequate statistics. The highly hygroscopic nature of sea salt means particles change size rapidly with fluctuations in relative humidity; this introduces an apparent bias in flux measurements if particles are sized at ambient humidity. The Compact Lightweight Aerosol Spectrometer Probe (CLASP) was developed specifically to make high rate measurements of aerosol size distributions for use in eddy covariance measurements, and the instrument and data processing and analysis techniques have been refined over the course of several projects. Here we will review some of the issues and limitations related to making eddy covariance measurements of the sea spray source flux over the open ocean, summarise some key results from the last decade, and present new results from a 3-year long ship-based measurement campaign as part of the WAGES project. Finally we will consider requirements for future progress.

Aerosol-chamber study of the α-pinene/O 3 reaction: influence of particle acidity on aerosol yields and products

NASA Astrophysics Data System (ADS)

Iinuma, Yoshiteru; Böge, Olaf; Gnauk, Thomas; Herrmann, Hartmut

α-Pinene ozonolysis was carried out in the presence of ammonium sulfate or sulfuric acid seed particles in a 9 m 3 Teflon chamber at the mixing ratios of 100 ppbv for α-pinene and about 70 ppbv for ozone. The evolution of size distribution was measured by means of a differential mobility particle sizer (DMPS). The resulting secondary organic aerosol (SOA) was sampled by a denuder/quartz fiber filter combination for the determination of the total organic carbon concentration (TOC) in the particle phase, using a thermographic method and by a denuder/PTFE filter combination for the analysis of individual chemical species in the particle phase using capillary electrophoresis-electrospray ionization-mass spectrometry (CE-ESI-MS). cis-Pinic acid ( m/ z 185) and another species tentatively identified at m/ z 171 and 199 were the major particle phase species for both seed particles although the product yields were different, indicating the influence of seed particle acidity. A thermographic method for the determination of TOC showed an increase of particle phase organics by 40% for the experiments with higher acidity. CE-ESI-MS analysis showed a large increase in the concentration of compounds with Mw>300 from the experiments with sulfuric acid seed particles. These results suggest that the seed particle acidity enhances the yield of SOA and plays an important role in the formation of larger molecules in the particle phase. Our results from direct particle phase chemical analysis suggest for the first time that condensation of smaller organics takes place by polymerization or aldol condensation following the formation of aldehydes, such as pinonaldehyde from the terpene ozonolysis.

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.

Long term measurements of the estimated hygroscopic enhancement of aerosol optical properties

NASA Astrophysics Data System (ADS)

Hervo, Maxime; Sellegri, Karine; Pichon, Jean Marc; Roger, Jean Claude; Laj, Paolo

2015-04-01

Water vapour has a major impact on aerosol optical properties, thus on the Radiative Forcing for aerosol-radiation interaction (RFari). However there is few studies measuring this impact over a large period. Optical properties of aerosols were measured at the GAW Puy de Dôme station (1465m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the dry optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the planetary boundary layer height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type and the season. At 90% humidity, the scattering factor enhancement (fsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH= 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type. To our knowledge, these results are one of the first presenting the impact of water vapour on the aerosol optical properties for a long period, and the first for a site at the border between the planetary boundary layer

Aerosol Daytime Variations over North and South America Derived from Multiyear AERONET Measurements

NASA Technical Reports Server (NTRS)

Zhang, Yan; Yu, Hongbin; Eck, Tom F.; Smirnov, Alexander; Chin, Mian; Remer, Lorraine A.; Bian, Huisheng; Tan, Qian; Levy, Roberrt; Holben, Brent N.

2012-01-01

This study analyzes the daytime variation of aerosol with seasonal distinction by using multi-year measurements from 54 of the Aerosol Robotic Network (AERONET) sites over North America, South America, and islands in surrounding oceans. The analysis shows a wide range of daily variability of aerosol optical depth (AOO) and Angstrom exponent depending on location and season. Possible reasons for daytime variations are given. The largest AOO daytime variation range at 440 nm, up to 75%, occurs in Mexico City, with maximum AOO in the afternoon. Large AOO daily variations are also observed in the polluted mid-Atlantic U.S. and U.S. West Coast with maximum AOO occurring in the afternoon in the mid-Atlantic U.S., but in the morning in the West Coast. In South American sites during the biomass burning season (August to October), maximum AOO generally occurs in the afternoon. But the daytime variation becomes smaller when sites are influenced more by long-range transported smoke than by local burning. Islands show minimum AOO in the morning and maximum AOO in the afternoon. The diverse patterns of aerosol daytime variation suggest that geostationary satellite measurements would be invaluable for characterizing aerosol temporal variations on regional and continental scales. In particular, simultaneous measurements of aerosols and aerosol precursors from a geostationary satellite would greatly aid in understanding the evolution of aerosol as determined by emissions, chemical transformations, and transport processes.

[Determination of the error of aerosol extinction coefficient measured by DOAS].

PubMed

Si, Fu-qi; Liu, Jian-guo; Xie, Pin-hua; Zhang, Yu-jun; Wang, Mian; Liu, Wen-qing; Hiroaki, Kuze; Liu, Cheng; Nobuo, Takeuchi

2006-10-01

The method of defining the error of aerosol extinction coefficient measured by differential optical absorption spectroscopy (DOAS) is described. Some factors which could bring errors to result, such as variation of source, integral time, atmospheric turbulence, calibration of system parameter, displacement of system, and back scattering of particles, are analyzed. The error of aerosol extinction coefficient, 0.03 km(-1), is determined by theoretical analysis and practical measurement.

Dicarboxylic acids, oxoacids, benzoic acid, α-dicarbonyls, WSOC, OC, and ions in spring aerosols from Okinawa Island in the western North Pacific Rim: size distributions and formation processes

NASA Astrophysics Data System (ADS)

Deshmukh, D. K.; Kawamura, K.; Lazaar, M.; Kunwar, B.; Boreddy, S. K. R.

2015-09-01

Size-segregated aerosols (9-stages from < 0.43 to > 11.3 μm in diameter) were collected at Cape Hedo, Okinawa in spring 2008 and analyzed for water-soluble diacids (C2-C12), ω-oxoacids (ωC2-ωC9), pyruvic acid, benzoic acid and α-dicarbonyls (C2-C3) as well as water-soluble organic carbon (WSOC), organic carbon (OC) and major ions. In all the size-segregated aerosols, oxalic acid (C2) was found as the most abundant species followed by malonic and succinic acids whereas glyoxylic acid (ωC2) was the dominant oxoacid and glyoxal (Gly) was more abundant than methylglyoxal. Diacids (C2-C5), ωC2 and Gly as well as WSOC and OC peaked at 0.65-1.1 μm in fine mode whereas azelaic (C9) and 9-oxononanoic (ωC9) acids peaked at 3.3-4.7 μm in coarse mode. Sulfate and ammonium are enriched in fine mode whereas sodium and chloride are in coarse mode. These results imply that water-soluble species in the marine aerosols could act as cloud condensation nuclei (CCN) to develop the cloud cover over the western North Pacific Rim. The organic species are likely produced by a combination of gas-phase photooxidation, and aerosol-phase or in-cloud processing during long-range transport. The coarse mode peaks of malonic and succinic acids were obtained in the samples with marine air masses, suggesting that they may be associated with the reaction on sea salt particles. Bimodal size distributions of longer-chain diacid (C9) and oxoacid (ωC9) with a major peak in the coarse mode suggest their production by photooxidation of biogenic unsaturated fatty acids via heterogeneous reactions on sea salt particles.

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

NASA Astrophysics Data System (ADS)

Malinina, Elizaveta; Rozanov, Alexei; Rozanov, Vladimir; Liebing, Patricia; Bovensmann, Heinrich; Burrows, John P.

2018-04-01

aerosols in the Earth's atmosphere is of a great importance in the scientific community. While tropospheric aerosol influences the radiative balance of the troposphere and affects human health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N-20° S) for 10 years (2002-2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size

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.

Epoxide pathways improve model predictions of isoprene markers and reveal key role of acidity in aerosol formation.

PubMed

Pye, Havala O T; Pinder, Robert W; Piletic, Ivan R; Xie, Ying; Capps, Shannon L; Lin, Ying-Hsuan; Surratt, Jason D; Zhang, Zhenfa; Gold, Avram; Luecken, Deborah J; Hutzell, William T; Jaoui, Mohammed; Offenberg, John H; Kleindienst, Tadeusz E; Lewandowski, Michael; Edney, Edward O

2013-10-01

Isoprene significantly contributes to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, the Community Multiscale Air Quality model is updated to predict isoprene aerosol from epoxides produced under both high- and low-NOx conditions. The new aqueous aerosol pathways allow for explicit predictions of two key isoprene-derived species, 2-methyltetrols and 2-methylglyceric acid, that are more consistent with observations than estimates based on semivolatile partitioning. The new mechanism represents a significant source of organic carbon in the lower 2 km of the atmosphere and captures the abundance of 2-methyltetrols relative to organosulfates during the simulation period. For the parametrization considered here, a 25% reduction in SOx emissions effectively reduces isoprene aerosol, while a similar reduction in NOx leads to small increases in isoprene aerosol.

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.

Lidar measurements of wildfire smoke aerosols in the atmosphere above Sofia, Bulgaria

NASA Astrophysics Data System (ADS)

Peshev, Zahary Y.; Deleva, Atanaska D.; Dreischuh, Tanja N.; Stoyanov, Dimitar V.

2016-01-01

Presented are results of lidar measurements and characterization of wildfire caused smoke aerosols observed in the atmosphere above the city of Sofia, Bulgaria, related to two local wildfires raging in forest areas near the city. A lidar systems based on a frequency-doubled Nd:YAG laser operated at 532 nm and 1064 nm is used in the smoke aerosol observations. It belongs to the Sofia LIDAR Station (at Laser Radars Laboratory, Institute of Electronics, Bulgarian Academy of Sciences), being a part of the European Aerosol Lidar Network. Optical, dynamical, microphysical, and geometrical properties and parameters of the observed smoke aerosol particles and layers are displayed and analyzed, such as: range/height-resolved profiles of the aerosol backscatter coefficient; integral aerosol backscattering; sets of colormaps displaying time series of the height distribution of the aerosol density; topologic, geometric, and volumetric properties of the smoke aerosol layers; time-averaged height profiles of backscatter-related Ångström exponent (BAE). Obtained results of retrieving and profiling smoke aerosols are commented in their relations to available meteorological and air-mass-transport forecasting and modelling data.

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

Sun and aureole spectrometer for airborne measurements to derive aerosol optical properties.

PubMed

Asseng, Hagen; Ruhtz, Thomas; Fischer, Jürgen

2004-04-01

We have designed an airborne spectrometer system for the simultaneous measurement of the direct Sun irradiance and aureole radiance. The instrument is based on diffraction grating spectrometers with linear image sensors. It is robust, lightweight, compact, and reliable, characteristics that are important for airborne applications. The multispectral radiation measurements are used to derive optical properties of tropospheric aerosols. We extract the altitude dependence of the aerosol volume scattering function and of the aerosol optical depth by using flight patterns with descents and ascents ranging from the surface level to the top of the boundary layer. The extinction coefficient and the product of single scattering albedo and phase function of separate layers can be derived from the airborne measurements.

Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Kazil, J.; Stier, P.; Zhang, K.; Quaas, J.; Kinne, S.; O'Donnell, D.; Rast, S.; Esch, M.; Ferrachat, S.; Lohmann, U.; Feichter, J.

2010-05-01

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative budget. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative budget over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local

Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Kazil, J.; Stier, P.; Zhang, K.; Quaas, J.; Kinne, S.; O'Donnell, D.; Rast, S.; Esch, M.; Ferrachat, S.; Lohmann, U.; Feichter, J.

2010-11-01

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative forcing. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative forcing over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local

Measuring the influence of aerosols and albedo on sky polarization.

PubMed

Kreuter, A; Emde, C; Blumthaler, M

2010-11-01

All-sky distributions of the polarized radiance are measured using an automated fish-eye camera system with a rotating polarizer. For a large range of aerosol and surface albedo situations, the influence on the degree of polarization and sky radiance is investigated. The range of aerosol optical depth and albedo is 0.05-0.5 and 0.1-0.75, respectively. For this range of parameters, a reduction of the degree of polarization from about 0.7 to 0.4 was observed. The analysis is done for 90° scattering angle in the principal plane under clear sky conditions for a broadband channel of 450 ± 25 nm and solar zenith angles between 55° and 60°. Radiative transfer calculations considering three different aerosol mixtures are performed and and agree with the measurements within the statistical error.

In situ acidity and pH of size-fractionated aerosols during a recent smoke-haze episode in Southeast Asia.

PubMed

Behera, Sailesh N; Cheng, Jinping; Balasubramanian, Rajasekhar

2015-10-01

The characterization of aerosol acidity has received increased attention in recent years due to its influence on atmospheric visibility, climate change and human health. Distribution of water soluble inorganic (WSI) ions in 12 different size fractions of aerosols was investigated under two different atmospheric conditions (smoke-haze and non-haze periods) in 2012 using the Micro-Orifice Uniform Deposit Impactor (MOUDI) and nano-MOUDI for the first time in Singapore. To estimate the in situ acidity ([H(+)]Ins) and in situ aerosol pH (pHIS), the Aerosol Inorganic Model version-IV under deliquescent mode of airborne particles was used at prevailing ambient temperature and relative humidity. The study revealed an increase in the levels of airborne particulate matter (PM) mass and concentrations of WSI ions for all size fractions during the smoke-haze period, which was caused by the trans-boundary transport of biomass burning-impacted air masses from Indonesia. A bimodal distribution was observed for concentrations of SO4(2-), NO3(-), Cl(-), K(+) and Na(+), whereas concentrations of NH4(+), Ca(2+) and Mg(2+) showed a single mode distribution. The concentration of WSI ions in PM1.8 during the smoke-haze period increased by 3.8 (for SO4(2-)) to 10.5 (for K(+)) times more than those observed during the non-haze period. The pHIS were observed to be lower during the smoke-haze period than that during the non-haze period for all size fractions of PM, indicating that atmospheric aerosols were more acidic due to the influence of biomass burning emissions. The particles in the accumulation mode were more acidic than those in the coarse mode.

Comparative Optical Measurements of Airspeed and Aerosols on a DC-8 Aircraft

NASA Technical Reports Server (NTRS)

Bogue, Rodney; McGann, Rick; Wagener, Thomas; Abbiss, John; Smart, Anthony

1997-01-01

NASA Dryden supported a cooperative flight test program on the NASA DC-8 aircraft in November 1993. This program evaluated optical airspeed and aerosol measurement techniques. Three brassboard optical systems were tested. Two were laser Doppler systems designed to measure free-stream-referenced airspeed. The third system was designed to characterize the natural aerosol statistics and airspeed. These systems relied on optical backscatter from natural aerosols for operation. The DC-8 aircraft carried instrumentation that provided real-time flight situation information and reference data on the aerosol environment. This test is believed to be the first to include multiple optical airspeed systems on the same carrier aircraft, so performance could be directly compared. During 23 hr of flight, a broad range of atmospheric conditions was encountered, including aerosol-rich layers, visible clouds, and unusually clean (aerosol-poor) regions. Substantial amounts of data were obtained. Important insights regarding the use of laser-based systems of this type in an aircraft environment were gained. This paper describes the sensors used and flight operations conducted to support the experiments. The paper also briefly describes the general results of the experiments.

Aerosol and precipitation chemistry measurements in a remote site in Central Amazonia: the role of biogenic contribution

NASA Astrophysics Data System (ADS)

Pauliquevis, T.; Lara, L. L.; Antunes, M. L.; Artaxo, P.

2012-06-01

ones observed in other remote sites in tropical forests. The volume-weighted mean (VWM) pH was 4.90. The most important contribution to acidity was from weak organic acids. The organic acidity was predominantly associated with the presence of acetic acid instead of formic acid, which is more often observed in pristine tropical areas. Wet deposition rates for major species did not differ significantly between dry and wet season, except for NH4+, citrate and acetate, which had smaller deposition rates during dry season. While biomass burning emissions were clearly identified in the aerosol component, it did not present a clear signature in rainwater. The biogenic component and the long-range transport of sea salt were observed both in aerosols and rainwater composition. The results shown here indicate that in Central Amazonia it is still possible to observe quite pristine atmospheric conditions, relatively free of anthropogenic influences.

Outdoor chamber measurements of biological aerosols with a passive FTIR spectrometer

NASA Astrophysics Data System (ADS)

D'Amico, Francis M.; Emge, Darren K.; Roelant, Geoffrey J.

2004-02-01

Outdoor measurements of dry bacillus subtilis (BG) spores were conducted with a passive Fourier transform infrared (FTIR) spectrometer using two types of chambers. One was a large open-ended cell, and the other was a canyon of similar dimensions. The canyon exposes the aerosol plume to downwelling sky radiance, while the open-ended cell does not. The goal of the experiments was to develop a suitable test methodology for evaluation of passive standoff detectors for open-air aerosol measurements. Dry BG aerosol particles were dispersed with a blower through an opening in the side of the chamber to create a pseudo-stationary plume, wind conditions permitting. Numerous trials were performed with the FTIR spectrometer positioned to view mountain, sky and mixed mountain-sky backgrounds. This paper will discuss the results of the FTIR measurements for BG and Kaolin dust releases.

Investigation of aerosol effects on shallow marine convection - Lidar measurements during NARVAL-I and NARVAL-II

NASA Astrophysics Data System (ADS)

Groß, Silke; Wirth, Martin; Gutleben, Manuel; Ewald, Florian; Kiemle, Christoph; Kölling, Tobias; Mayer, Bernhard

2017-04-01

Clouds and aerosols have a large impact on the Earth's radiation budget by scattering and absorption of solar and terrestrial radiation. Furthermore aerosols can modify cloud properties and distribution. Up to now no sufficient understanding in aerosol-cloud interaction and in climate feedback of clouds is achieved. Especially shallow marine convection in the trade wind regions show large uncertainties in climate feedback. Thus a better understanding of these shallow marine convective clouds and how aerosols affect these clouds, e.g. by changing the cloud properties and distribution, is highly demanded. During NARVAL-I (Next-generation airborne remote-sensing for validation studies) and NARVAL-II a set of active and passive remote sensing instruments, i.e. a cloud radar, an aerosol and water vapor lidar system, microwave radiometer, a hyper spectral imager (NARVAL-II only) and radiation measurements, were installed on the German research aircraft HALO. Measurements were performed out of Barbados over the tropical North-Atlantic region in December 2013 and August 2016 to study shallow trade wind convection as well as its environment in the dry and wet season. While no or only few aerosol layers were observed above the marine boundary layer during the dry season in December 2013, part of the measurement area was influenced by high aerosol load caused by long-range transport of Saharan dust during the NARVAL-II measurements in August 2016. Measurement flights during NARVAL-II were conducted the way that we could probed aerosol influenced regions as well as areas with low aerosol load. Thus the measurements during both campaigns provide the opportunity to investigate if and how the transported aerosol layers change the distribution and formation of the shallow marine convection by altering their properties and environment. In our presentation we will focus on the lidar measurements performed during NARVAL-I and NARVAL-II. We will give an overview of the measurements

Reactive Heterogeneous Chemistry on Organic Aerosols: Two Case Studies

NASA Astrophysics Data System (ADS)

Abbatt, J.; Braban, C.; Broekhuizen, K.; Thornberry, T.; Thornton, J.

2003-12-01

Two sets of laboratory studies will be discussed to illustrate the impact that heterogeneous chemistry involving tropospheric organic aerosols may have on both the gas-phase composition of the atmosphere and the chemical nature of the particles themselves. In the first case, the reactive uptake coefficient for the hydrolysis of dinitrogen pentoxide (N2O5) on organic aerosols has been measured in an entrained aerosol flow tube coupled to a Chemical-Ionization Mass Spectrometer (CIMS). The general observation is that the reaction on aqueous malonic acid aerosols behaves in an analogous manner to that on aqueous inorganic salts, i.e. the uptake coefficient shows a linear dependence on the particle water content up to 50% relative humidity (RH), at which point the effect saturates. In addition, there is evidence for the kinetics being dependent on both the size of the particles and the levels of dissolved nitrate. By contrast, the N2O5 hydrolysis kinetics on solid azelaic acid particles are too slow to be atmospherically significant, even at 85% RH. In the second case, the kinetics and product yields from the oxidation of liquid oleic acid by ozone have been studied in considerable detail, with emphasis on the quantification of gas-phase products (nonanal) by CIMS and water-soluble species by HPLC/Electrospray-Ionization Mass Spectrometry (azelaic acid, nonanoic acid). The atmospheric importance of these results will be discussed, in particular with respect to the role of organic aerosol oxidation as a source of cloud condensation nuclei.

Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft

NASA Technical Reports Server (NTRS)

Pueschel , R. F.; Gore, Waren J. Y. (Technical Monitor)

1997-01-01

Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

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

Jefferson, A.; Hageman, D.; Morrow, H.

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol water uptake. Annual average sub-10 μm fRH values (the ratio of aerosol scattering at 85%/40% relative humidity (RH)) were 1.78 and 1.99 for the gamma and kappa fit algorithms, respectively. Our study found higher growth rates in the winter and spring seasons that correlated with a high aerosol nitrate mass fraction. fRH exhibited strong, but differing, correlations with the scattering Ångström exponent and backscatter fraction,more » two optical size-dependent parameters. The aerosol organic mass fraction had a strong influence on fRH. Increases in the organic mass fraction and absorption Ångström exponent coincided with a decrease in fRH. Similarly, fRH declined with decreases in the aerosol single scatter albedo. The uncertainty analysis of the fit algorithms revealed high uncertainty at low scattering coefficients and increased uncertainty at high RH and fit parameters values.« less

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

DOE PAGES

Jefferson, A.; Hageman, D.; Morrow, H.; ...

2017-09-11

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol water uptake. Annual average sub-10 μm fRH values (the ratio of aerosol scattering at 85%/40% relative humidity (RH)) were 1.78 and 1.99 for the gamma and kappa fit algorithms, respectively. Our study found higher growth rates in the winter and spring seasons that correlated with a high aerosol nitrate mass fraction. fRH exhibited strong, but differing, correlations with the scattering Ångström exponent and backscatter fraction,more » two optical size-dependent parameters. The aerosol organic mass fraction had a strong influence on fRH. Increases in the organic mass fraction and absorption Ångström exponent coincided with a decrease in fRH. Similarly, fRH declined with decreases in the aerosol single scatter albedo. The uncertainty analysis of the fit algorithms revealed high uncertainty at low scattering coefficients and increased uncertainty at high RH and fit parameters values.« less

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.

Maritime Infrared Propagation: Particle Size Distribution Measurements Using a Helicopter-Borne Aerosol Counter.

DTIC Science & Technology

1981-09-01

COUNTER by R. R. Allan S. Craig SUMMARY -Particle size distribution measurements were made on nine successive days in late August 1980 using a PMS FSSP-100...aerosol counter flown on a Wessex Mk 5 helicopter. In all, 14 flights were made giving data at two heights, 30 and 100 ft above the sea surface...aerosol content over deep water. It was a specific recommendation of TTCP-JAG9 that airborne aerosol measurements should be made in conjunction with al

Photochemical organonitrate formation in wet aerosols

NASA Astrophysics Data System (ADS)

Lim, Yong Bin; Kim, Hwajin; Kim, Jin Young; Turpin, Barbara J.

2016-10-01

Water is the most abundant component of atmospheric fine aerosol. However, despite rapid progress, multiphase chemistry involving wet aerosols is still poorly understood. In this work, we report results from smog chamber photooxidation of glyoxal- and OH-containing ammonium sulfate or sulfuric acid particles in the presence of NOx and O3 at high and low relative humidity. Particles were analyzed using ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). During the 3 h irradiation, OH oxidation products of glyoxal that are also produced in dilute aqueous solutions (e.g., oxalic acids and tartaric acids) were formed in both ammonium sulfate (AS) aerosols and sulfuric acid (SA) aerosols. However, the major products were organonitrogens (CHNO), organosulfates (CHOS), and organonitrogen sulfates (CHNOS). These were also the dominant products formed in the dark chamber, indicating non-radical formation. In the humid chamber (> 70 % relative humidity, RH), two main products for both AS and SA aerosols were organonitrates, which appeared at m / z- 147 and 226. They were formed in the aqueous phase via non-radical reactions of glyoxal and nitric acid, and their formation was enhanced by photochemistry because of the photochemical formation of nitric acid via reactions of peroxy radicals, NOx and OH during the irradiation.

Aerosol Retrieval from Multiangle Multispectral Photopolarimetric Measurements: Importance of Spectral Range and Angular Resolution

NASA Technical Reports Server (NTRS)

Wu, L.; Hasekamp, O.; Van Diedenhoven, B.; Cairns, B.

2015-01-01

We investigated the importance of spectral range and angular resolution for aerosol retrieval from multiangle photopolarimetric measurements over land. For this purpose, we use an extensive set of simulated measurements for different spectral ranges and angular resolutions and subsets of real measurements of the airborne Research Scanning Polarimeter (RSP) carried out during the PODEX and SEAC4RS campaigns over the continental USA. Aerosol retrievals performed from RSP measurements show good agreement with ground-based AERONET measurements for aerosol optical depth (AOD), single scattering albedo (SSA) and refractive index. Furthermore, we found that inclusion of shortwave infrared bands (1590 and/or 2250 nm) significantly improves the retrieval of AOD, SSA and coarse mode microphysical properties. However, accuracies of the retrieved aerosol properties do not improve significantly when more than five viewing angles are used in the retrieval.

Ultra-Low Background Measurements Of Decayed Aerosol Filters

NASA Astrophysics Data System (ADS)

Miley, H.

2009-04-01

To experimentally evaluate the opportunity to apply ultra-low background measurement methods to samples collected, for instance, by the Comprehensive Test Ban Treaty International Monitoring System (IMS), aerosol samples collected on filter media were measured using HPGe spectrometers of varying low-background technology approaches. In this way, realistic estimates of the impact of low-background methodology can be assessed on the Minimum Detectable Activities obtained in systems such as the IMS. The current measurement requirement of stations in the IMS is 30 microBq per cubic meter of air for 140Ba, or about 106 fissions per daily sample. Importantly, this is for a fresh aerosol filter. Decay varying form 3 days to one week reduce the intrinsic background from radon daughters in the sample. Computational estimates of the improvement factor for these decayed filters for underground-based HPGe in clean shielding materials are orders of magnitude less, even when the decay of the isotopes of interest is included.

Direct Measurement of pH in Individual Particles via Raman Microspectroscopy and Variation in Acidity with Relative Humidity.

PubMed

Rindelaub, Joel D; Craig, Rebecca L; Nandy, Lucy; Bondy, Amy L; Dutcher, Cari S; Shepson, Paul B; Ault, Andrew P

2016-02-18

Atmospheric aerosol acidity is an important characteristic of aqueous particles, which has been linked to the formation of secondary organic aerosol by catalyzing reactions of oxidized organic compounds that have partitioned to the particle phase. However, aerosol acidity is difficult to measure and traditionally estimated using indirect methods or assumptions based on composition. Ongoing disagreements between experiments and thermodynamic models of particle acidity necessitate improved fundamental understanding of pH and ion behavior in high ionic strength atmospheric particles. Herein, Raman microspectroscopy was used to determine the pH of individual particles (H2SO4+MgSO4) based on sulfate and bisulfate concentrations determined from νs(SO4(2-)) and νs(HSO4(-)), the acid dissociation constant, and activity coefficients from extended Debye-Hückel calculations. Shifts in pH and peak positions of νs(SO4(2-)) and νs(HSO4(-)) were observed as a function of relative humidity. These results indicate the potential for direct spectroscopic determination of pH in individual particles and the need to improve fundamental understanding of ion behavior in atmospheric particles.

ACE-Asia Aerosol Optical Depth and Water Vapor Measured by Airborne Sunphotometers and Related to Other Measurements and Calculations

NASA Technical Reports Server (NTRS)

Livingston, John M.; Russell, P. B.; Schmid, B.; Redemann, J.; Eilers, J. A.; Ramirez, S. A.; Kahn, R.; Hegg, D.; Pilewskie, P.; Anderson, T.;

Airborne Sun Photometer Measurements of Aerosol Optical Depth during SOLVE II: Comparison with SAGE III and POAM III Measurements

NASA Technical Reports Server (NTRS)

Russell, P.; Livingston, J.; Schmid, B.; Eilers, J.; Kolyer, R.; Redemann, J.; Yee, J.-H.; Trepte, C.; Thomason, L.; Zawodny, J.

2003-01-01

The 14-channel NASA Ames Airborne Tracking Sunphotometer (AATS-14) was operated aboard the NASA DC-8 during the Second SAGE III Ozone Loss and Validation Experiment (SOLVE II) and obtained successful measurements during the sunlit segments of eight science flights. These included six flights out of Kiruna, Sweden, one flight out of NASA Dryden Flight Research Center (DFRC), and the Kiruna-DFRC return transit flight. Values of spectral aerosol optical depth (AOD), columnar ozone and columnar water vapor have been derived from the AATS-14 measurements. In this paper, we focus on AATS-14 AOD data. In particular, we compare AATS-14 AOD spectra with temporally and spatially near-coincident measurements by the Stratospheric Aerosol and Gas Experiment III (SAGE III) and the Polar Ozone and Aerosol Measurement III (POAM III) satellite sensors. We examine the effect on retrieved AOD of uncertainties in relative optical airmass (the ratio of AOD along the instrument-to-sun slant path to that along the vertical path) at large solar zenith angles. Airmass uncertainties result fiom uncertainties in requisite assumed vertical profiles of aerosol extinction due to inhomogeneity along the viewing path or simply to lack of available data. We also compare AATS-14 slant path solar transmission measurements with coincident measurements acquired from the DC-8 by the NASA Langley Research Center Gas and Aerosol Measurement Sensor (GAMS).

MGS TES Measurements of Dust and Ice Aerosol Behaviors

NASA Astrophysics Data System (ADS)

Clancy, R. T.; Wolff, M. J.; Christensen, P. R.

2000-10-01

The Thermal Emission Spectrometer (TES, Christensen et al., Science, v279, 1692-1697, 1998) on board the Mars Global Surveyor obtains simultaneous solar band and thermal IR spectral emission-phase-function (EPF) observations with global spatial coverage and continuous seasonal sampling. These measurements allow the first comprehensive study of the coupled visible scattering and thermal IR absorption properties of Mars atmospheric aerosols, a fundamental requirement towards defining opacities, particle sizes, and particle shapes for separable dust and water ice aerosol components. Furthermore, TES limb sounding at solar band and IR wavelengths may be analyzed in the context of these EPF column determinations to constrain the distinctive vertical profile behaviors of dust and ice clouds. We present initial radiative transfer analyses of TES visible and IR EPFs, which indicate surprisingly complex dust and ice aerosol behaviors over all latitudes and seasons. Distinctive backscattering peaks of variable intensity are observed for several types of water ice clouds, along with evidence for ice-coated dust aerosols. We will present a broad spatial and temporal sampling of solar band and spectral IR results for Mars atmospheric ice and dust aerosols observed over the 1998-2000 period. This research is supported by the MGS Participating Scientist and MED Science Data Analysis programs.

Development of a Photo-fragmentation Laser Induced Fluorescence Instrument for the Measurement of Nitrous Acid

NASA Astrophysics Data System (ADS)

Boustead, G.; Blitz, M. A.; Heard, D. E.; Ingham, T.; Stone, D. J.; Whalley, L.

2017-12-01

The hydroxyl radical (OH) is the primary oxidant in the atmosphere with its concentration determining the lifetime of many species and its reaction with volatile organic compounds (VOCs) leading to the production of secondary organic aerosols (SOA) and tropospheric ozone. Nitrous acid (HONO) is an important source of OH as it builds up overnight and is photolysed to form OH in the morning. HONO is also present during the day, with several hundred pptv observed in urban environments. Atmospheric models currently under predict the concentration of HONO observed during the day, indicating a missing source. Heterogeneous reactions on ground and aerosol surfaces are now recognised as potentially important HONO sources. To identify and quantify some of these missing heterogeneous sources, a photo-fragmentation laser induced fluorescence (PF-LIF) instrument has been developed to provide a fast and sensitive measurement of HONO. The PF-LIF instrument detects the OH fragment at 308 nm after the photolysis of HONO at 355 nm. This instrument is coupled to an aerosol flow tube and can be used to measure HONO production from aerosols under illuminated conditions. We will present an overview of the instrument and its development as well as preliminary results including the production of HONO from illuminated TiO2 aerosols.

Measuring the influence of aerosols and albedo on sky polarization

PubMed Central

Kreuter, A.; Emde, C.; Blumthaler, M.

2010-01-01

All-sky distributions of the polarized radiance are measured using an automated fish-eye camera system with a rotating polarizer. For a large range of aerosol and surface albedo situations, the influence on the degree of polarization and sky radiance is investigated. The range of aerosol optical depth and albedo is 0.05–0.5 and 0.1–0.75, respectively. For this range of parameters, a reduction of the degree of polarization from about 0.7 to 0.4 was observed. The analysis is done for 90° scattering angle in the principal plane under clear sky conditions for a broadband channel of 450 ± 25 nm and solar zenith angles between 55° and 60°. Radiative transfer calculations considering three different aerosol mixtures are performed and and agree with the measurements within the statistical error. PMID:24068851

SAM II aerosol profile measurements, Poker Flat, Alaska; July 16-19, 1979

NASA Technical Reports Server (NTRS)

Mccormick, M. P.; Chu, W. P.; Mcmaster, L. R.; Grams, G. W.; Herman, B. M.; Pepin, T. J.; Russell, P. B.; Swissler, T. J.

1981-01-01

SAM II satellite measurements during the July 1979 Poker Flat mission, yielded an aerosol extinction coefficient of 0.0004/km at 1.0 micron wavelength, in the region of the stratospheric aerosol mixing ratio peak (12-16 km). The stratospheric aerosol optical depth for these data, calculated from the tropopause through 30 km, is approximately 0.001. These results are consistent with the average 1979 summertime values found throughout the Arctic.

Estimation of Aerosol Direct Radiative Effects from Satellite and In Situ Measurements

NASA Technical Reports Server (NTRS)

Bergstrom, Robert W.; Russell, Philip B.; Schmid, Beat; Redemann, Jens; McIntosh, Dawn

2000-01-01

Ames researchers have combined measurements from satellite, aircraft, and the surface to estimate the effect of airborne particles (aerosols) on the solar radiation over the North Atlantic region. These aerosols (which come from both natural and pollution sources) can reflect solar radiation, causing a cooling effect that opposes the warming caused by carbon dioxide. Recently, increased attention has been paid to aerosol effects to better understand the Earth climate system.

Biomass Burning Aerosol Absorption Measurements with MODIS Using the Critical Reflectance Method

NASA Technical Reports Server (NTRS)

Zhu, Li; Martins, Vanderlei J.; Remer, Lorraine A.

2010-01-01

This research uses the critical reflectance technique, a space-based remote sensing method, to measure the spatial distribution of aerosol absorption properties over land. Choosing two regions dominated by biomass burning aerosols, a series of sensitivity studies were undertaken to analyze the potential limitations of this method for the type of aerosol to be encountered in the selected study areas, and to show that the retrieved results are relatively insensitive to uncertainties in the assumptions used in the retrieval of smoke aerosol. The critical reflectance technique is then applied to Moderate Resolution Imaging Spectrometer (MODIS) data to retrieve the spectral aerosol single scattering albedo (SSA) in South African and South American 35 biomass burning events. The retrieved results were validated with collocated Aerosol Robotic Network (AERONET) retrievals. One standard deviation of mean MODIS retrievals match AERONET products to within 0.03, the magnitude of the AERONET uncertainty. The overlap of the two retrievals increases to 88%, allowing for measurement variance in the MODIS retrievals as well. The ensemble average of MODIS-derived SSA for the Amazon forest station is 0.92 at 670 nm, and 0.84-0.89 for the southern African savanna stations. The critical reflectance technique allows evaluation of the spatial variability of SSA, and shows that SSA in South America exhibits higher spatial variation than in South Africa. The accuracy of the retrieved aerosol SSA from MODIS data indicates that this product can help to better understand 44 how aerosols affect the regional and global climate.

Inactivation of Encephalomyocarditis Virus in Aerosols: Fate of Virus Protein and Ribonucleic Acid

PubMed Central

De Jong, J. C.; Harmsen, M.; Trouwborst, T.; Winkler, K. C.

1974-01-01

After aerosolization at relative humidities of 50% or lower, encephalomyocarditis virus is rapidly inactivated. In this process the protein coat of the virion is damaged. This appears as a loss of hemagglutination activity and loss of affinity for hemagglutination inhibiting antibodies. The ribonucleic acid of the virus retains its infectivity but it becomes susceptible to ribonuclease. It sediments in sucrose gradients when centrifuged at high speed with the same velocity as free infectious ribonucleic acid extracted with phenol from intact encephalomyocarditis virus. PMID:4358862

Multiwavelength Comparison of Modeled and Measured Remote Tropospheric Aerosol Backscatter Over Pacific Ocean

NASA Technical Reports Server (NTRS)

Cutten, D. R.; Pueschel, R. F.; Srivastava, V.; Clarke, A. D.; Rothermel, J.; Spinhirne, J. D.; Menzies, R. T.

1996-01-01

Aerosol concentrations and size distributions in the middle and upper troposphere over the remote Pacific Ocean were measured with a forward scattering spectrometer probe (FSSP) on the NASA DC-8 aircraft during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. The FSSP size channels were recalibrated based on refractive index estimates from flight-level aerosol volatility measurements with a collocated laser optical particle counter (LOPC). The recalibrated FSSP size distributions were averaged over 100-s intervals, fitted with lo-normal distributions and used to calculate aerosol backscatter coefficients at selected wavelengths. The FSSP-derived backscatter estimates were averaged over 300-s intervals to reduce large random fluctuations. The smoothed FSSP aerosol backscatter coefficients were then compared with LOPC-derived backscatter values and with backscatter measured at or near flight level from four lidar systems operating at 0.53, 1.06, 9.11, 9.25, and 10.59 micrometers. Agreement between FSSP-derived and lidar-measured backscatter was generally best at flight level in homogeneous aerosol fields and at high backscatter values. FSSP data often underestimated low backscatter values especially at the longer wavelengths due to poor counting statistics for larger particles (greater than 0.8 micrometers diameter) that usually dominate aerosol backscatter at these wavelengths. FSSP data also underestimated backscatter at shorter wavelengths when particles smaller than the FSSP lower cutoff diameter (0.35 micrometers) made significant contributions to the total backscatter.

Aerosol Profile Measurements from the NASA Langley Research Center Airborne High Spectral Resolution Lidar

NASA Technical Reports Server (NTRS)

Obland, Michael D.; Hostetler, Chris A.; Ferrare, Richard A.; Hair, John W.; Roers, Raymond R.; Burton, Sharon P.; Cook, Anthony L.; Harper, David B.

2008-01-01

Since achieving first light in December of 2005, the NASA Langley Research Center (LaRC) Airborne High Spectral Resolution Lidar (HSRL) has been involved in seven field campaigns, accumulating over 450 hours of science data across more than 120 flights. Data from the instrument have been used in a variety of studies including validation and comparison with the Cloud- Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite mission, aerosol property retrievals combining passive and active instrument measurements, aerosol type identification, aerosol-cloud interactions, and cloud top and planetary boundary layer (PBL) height determinations. Measurements and lessons learned from the HSRL are leading towards next-generation HSRL instrument designs that will enable even further studies of aerosol intensive and extensive parameters and the effects of aerosols on the climate system. This paper will highlight several of the areas in which the NASA Airborne HSRL is making contributions to climate science.

Apparatus having reduced background for measuring radiation activity in aerosol particles

DOEpatents

Rodgers, John C.; McFarland, Andrew R.; Oritz, Carlos A.; Marlow, William H.

1992-01-01

Apparatus having reduced background for measuring radiation activity in aerosol particles. A continuous air monitoring sampler is described for use in detecting the presence of alpha-emitting aerosol particles. An inlet fractionating screen has been demonstrated to remove about 95% of freshly formed radon progeny from the aerosol sample, and approximately 33% of partially aged progeny. Addition of an electrical condenser and a modified dichotomous virtual impactor are expected to produce considerable improvement in these numbers, the goal being to enrich the transuranic (TRU) fraction of the aerosols. This offers the possibility of improving the signal-to-noise ratio for the detected alpha-particle energy spectrum in the region of interest for detecting TRU materials associated with aerosols, thereby enhancing the performance of background-compensation algorithms for improving the quality of alarm signals intended to warn personnel of potentially harmful quantities of TRU materials in the ambient air.

Ground-based aerosol measurements during CHARMEX/ADRIMED campaign at Granada station

NASA Astrophysics Data System (ADS)

Granados-Muñoz, Maria Jose; Bravo-Aranda, Juan Antonio; Navas-Guzman, Francisco; Guerro-Rascado, Juan Luis; Titos, Gloria; Lyamani, Hassan; Valenzuela, Antonio; Cazorla, Alberto; Olmo, Francisco Jose; Mallet, Marc; Alados-Arboledas, Lucas

2015-04-01

In the framework of ChArMEx/ADRIMED (Chemistry-Aerosol Mediterranean Experiment, http://charmex.lsce.ipsl.fr/; Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) projects, a field experiment based on in situ and remote sensing measurements from surface and airborne platforms was performed. The ADRIMED project aimed to capture the high complexity of the Mediterranean region by using an integrated approach based on intensive experimental field campaign and spaceborne observations, radiative transfer calculations and climate modelling with Regional Climate Models better adapted than global circulation models. For this purpose, measurements were performed at different surface super-sites (including Granada station) over the Occidental Mediterranean region during summer 2013 for creating an updated database of the physical, chemical, optical properties and the vertical distribution of the major "Mediterranean aerosols". Namely, measurements at Granada station were performed on 16 and 17 July 2013, in coincidence with the overpasses of the ATR aircraft over the station. The instrumentation used for the campaign includes both remote sensing instruments (a multiwavelength Raman lidar and a sun photometer) and in-situ measurements (a nephelometer, a Multi-Angle Absorption Photometer (MAAP), an Aerodynamic particle sizer (APS), a high volume sampler of PM10 and an aethalometer). During the measurement period a mineral dust event was detected, with similar dust load on both days. According to in-situ measurements, the event reached the surface level on 16 of June. Vertically resolved lidar measurements indicated presence of mineral dust layers up to 5 km asl both on 16 and 17 June 2013. Temporal evolution analysis indicated that on 17 June the dust layer decoupled from the boundary layer and disappeared around 14:00 UTC. In addition, lidar and sun-photometer data were used to retrieve volume concentration profiles by means of LIRIC (Lidar

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