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

NASA Astrophysics Data System (ADS)

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

2015-04-01

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

Volatility Properties of Internally- and Externally-Mixed Ambient Aerosols at an Anthropogenically-influenced Forest Site in Southeastern USA

NASA Astrophysics Data System (ADS)

Khlystov, A.; Subramanian, R.

2015-12-01

Secondary organic aerosol (SOA) from biogenic sources has a significant contribution to ambient aerosol loadings in Southeastern USA and thus contributes to adverse health effects of air pollution and influences regional and global climate. Volatility properties of biogenic SOA determine its concentration, reactivity, and lifetime, but are still largely unknown. As part of a larger study to assess the effect of biogenic SOA on aerosol optical properties, a set of instruments, including scanning mobility sizers (SMPS), single particle soot photometer (SP2), and a thermodenuder, was deployed during June 2015 at a Duke Forest site near Chapel Hill, NC. The site is characterized by a significant contribution of both biogenic and urban (mostly traffic) sources. Measurements of changes in aerosol volume and optical size upon heating in the thermodenuder at different temperatures are used to derive volatility properties of the ambient aerosol. A limited set of experiments was carried out using the tandem differential mobility analysis (TDMA) approach to investigate whether the ambient aerosol at the Duke Forest site is internally mixed with respect to its volatility properties. In this presentation we will discuss equilibrium and kinetic aspects of aerosol volatility observed during this study and implications of external vs. internal mixing for derivation of bulk volatility properties of ambient aerosol.

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

NASA Astrophysics Data System (ADS)

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

2017-10-01

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

The application of an improved gas and aerosol collector for ambient air pollutants in China

NASA Astrophysics Data System (ADS)

Dong, Huabin; Zeng, Limin; Zhang, Yuanhang; Hu, Min; Wu, Yusheng

2016-04-01

An improved Gas and Aerosol Collector (GAC) equipped with a newly designed aerosol collector and a set of dull-polished wet annular denuder (WAD) was developed by Peking University based on a Steam Jet Aerosol Collector (SJAC) sampler. Combined with Ion Chromatography (IC) the new sampler performed well in laboratory tests with high collection efficiencies for SO2 (above 98 %) and particulate sulfate (as high as 99.5 %). An inter-comparison between the GAC-IC system and the filter-pack method was performed and the results indicated that the GAC-IC system could supply reliable particulate sulfate, nitrate, chloride, and ammonium data in field measurement with a much wider range of ambient concentrations. From 2008 to 2015, dozens of big field campaigns (rural and coastal sites) were executed in different parts of China, the GAC-IC system took the chance having its field measurement performance checked repeatedly and provided high quality data in ambient conditions either under high loadings of pollutants or background area. Its measurements were highly correlated with data by other commercial instruments such as the SO2 analyzer, the HONO analyzer, a filter sampler, Aerosol Mass Spectrometer (AMS), etc. over a wide range of concentrations and proved particularly useful in future intensive campaigns or long-term monitoring stations to study various environmental issues such as secondary aerosol and haze formation. During these years of applications of GAC-IC in those field campaigns, we found some problems of several instruments running under field environment and some interesting results could also be drew from the large amount of data measured in near 20 provinces of China. Detail results will be demonstrated on the poster afterwards.

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

ISS Ambient Air Quality: Updated Inventory of Known Aerosol Sources

NASA Technical Reports Server (NTRS)

Meyer, Marit

2014-01-01

Spacecraft cabin air quality is of fundamental importance to crew health, with concerns encompassing both gaseous contaminants and particulate matter. Little opportunity exists for direct measurement of aerosol concentrations on the International Space Station (ISS), however, an aerosol source model was developed for the purpose of filtration and ventilation systems design. This model has successfully been applied, however, since the initial effort, an increase in the number of crewmembers from 3 to 6 and new processes on board the ISS necessitate an updated aerosol inventory to accurately reflect the current ambient aerosol conditions. Results from recent analyses of dust samples from ISS, combined with a literature review provide new predicted aerosol emission rates in terms of size-segregated mass and number concentration. Some new aerosol sources have been considered and added to the existing array of materials. The goal of this work is to provide updated filtration model inputs which can verify that the current ISS filtration system is adequate and filter lifetime targets are met. This inventory of aerosol sources is applicable to other spacecraft, and becomes more important as NASA considers future long term exploration missions, which will preclude the opportunity for resupply of filtration products.

An intercomparison study of analytical methods used for quantification of levoglucosan in ambient aerosol filter samples

NASA Astrophysics Data System (ADS)

Yttri, K. E.; Schnelle-Kreiss, J.; Maenhaut, W.; Alves, C.; Bossi, R.; Bjerke, A.; Claeys, M.; Dye, C.; Evtyugina, M.; García-Gacio, D.; Gülcin, A.; Hillamo, R.; Hoffer, A.; Hyder, M.; Iinuma, Y.; Jaffrezo, J.-L.; Kasper-Giebl, A.; Kiss, G.; López-Mahia, P. L.; Pio, C.; Piot, C.; Ramirez-Santa-Cruz, C.; Sciare, J.; Teinilä, K.; Vermeylen, R.; Vicente, A.; Zimmermann, R.

2014-07-01

The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wild fire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for biomass burning particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied High-Performance Anion-Exchange Chromatography (HPAEC), four used High-Performance Liquid Chromatography (HPLC) or Ultra-Performance Liquid Chromatography (UPLC), and six resorted to Gas Chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from -63 to 23%; however, for 62% of the laboratories the mean PE was within ±10%, and for 85% the mean PE was within ±20%. For mannosan, the corresponding range was -60 to 69%, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e., for 33% of

An intercomparison study of analytical methods used for quantification of levoglucosan in ambient aerosol filter samples

NASA Astrophysics Data System (ADS)

Yttri, K. E.; Schnelle-Kreis, J.; Maenhaut, W.; Abbaszade, G.; Alves, C.; Bjerke, A.; Bonnier, N.; Bossi, R.; Claeys, M.; Dye, C.; Evtyugina, M.; García-Gacio, D.; Hillamo, R.; Hoffer, A.; Hyder, M.; Iinuma, Y.; Jaffrezo, J.-L.; Kasper-Giebl, A.; Kiss, G.; López-Mahia, P. L.; Pio, C.; Piot, C.; Ramirez-Santa-Cruz, C.; Sciare, J.; Teinilä, K.; Vermeylen, R.; Vicente, A.; Zimmermann, R.

2015-01-01

The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning (BB) aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wildfire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for BB particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied high-performance anion-exchange chromatography (HPAEC), four used high-performance liquid chromatography (HPLC) or ultra-performance liquid chromatography (UPLC) and six resorted to gas chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from -63 to 20%; however, for 62% of the laboratories the mean PE was within ±10%, and for 85% the mean PE was within ±20%. For mannosan, the corresponding range was -60 to 69%, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e. for 33% of the

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

First Quantification of Imidazoles in Ambient Aerosol Particles: Potential Photosensitizers, Brown Carbon Constituents, and Hazardous Components.

PubMed

Teich, Monique; van Pinxteren, Dominik; Kecorius, Simonas; Wang, Zhibin; Herrmann, Hartmut

2016-02-02

Imidazoles are widely discussed in recent literature. They have been studied as a secondary product of the reaction of dicarbonyls with nitrogen containing compounds in a number of laboratory studies, potentially acting as photosensitizers triggering secondary organic aerosol growth and are forming constituents of light absorbing brown carbon. Despite the knowledge from laboratory studies, no quantitative information about imidazoles in ambient aerosol particles is available. Within the present study, five imidazoles (1-butylimidazole, 1-ethylimidazole, 2-ethylimidazole, imidazol-2-carboxaldehyde, and 4(5)-methylimidazole) were successfully identified and quantified for the first time in ambient aerosol samples from different environments in Europe and China. Their concentrations range between 0.2 and 14 ng/m(3). 4(5)-Methylimidazole was found to be the most abundant imidazole. The occurrence of imidazoles seems to be favored at sites with strong biomass burning influence or connected to more polluted air masses. No connection was found between aerosol particle pH and imidazole concentration. Our work corroborates the laboratory studies by showing that imidazoles are present in ambient aerosol samples in measurable amounts. Moreover, it further motivates to explore the potential photosensitizing properties of small alkyl-substituted imidazoles.

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.

BIOGENIC CONTRIBUTION TO PM-2.5 AMBIENT AEROSOL FROM RADIOCARBON MEASUREMENTS

EPA Science Inventory

Knowledge of the relative contributions of biogenic versus anthropogenic sources to ambient aerosol is of great interest in the formulation of strategies to achieve nationally mandated air quality standards. Radiocarbon (Carbon-14) measurements provide a means to quantify the ...

Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations.

PubMed

Mohr, Claudia; Huffman, Alex; Cubison, Michael J; Aiken, Allison C; Docherty, Kenneth S; Kimmel, Joel R; Ulbrich, Ingrid M; Hannigan, Michael; Jimenez, Jose L

2009-04-01

Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS). High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning emissions contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to those from ambient hydrocarbon-like OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from these sources is unlikelyto be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/zs that may be useful for differentiating some of these sources. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, whereas motor vehicle emissions have very low signal at this m/z.

RADIOCARBON MEASUREMENTS ON PM 2.5 AMBIENT AEROSOL FROM NASHVILLE, TN

EPA Science Inventory

Radiocarbon (Carbon-14) 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...

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.;

ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED AMBIENT AEROSOLS FOR DIFFERENT DOSE METRICS

EPA Science Inventory

ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED AMBIENT AEROSOLS FOR DIFFERENT DOSE METRICS.
Chong S. Kim, SC. Hu**, PA Jaques*, US EPA, National Health and Environmental Effects Research Laboratory, Research Triangle Park, NC 27711; **IIT Research Institute, Chicago, IL; *South...

Inhalation Exposure and Lung Dose Analysis of Multi-mode Complex Ambient Aerosols

EPA Science Inventory

Rationale: Ambient aerosols are complex mixture of particles with different size, shape and chemical composition. Although they are known to cause health hazard, it is not fully understood about causal mechanisms and specific attributes of particles causing the effects. Internal ...

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.

Profiling quinones in ambient air samples collected from the Athabasca region (Canada).

PubMed

Wnorowski, Andrzej; Charland, Jean-Pierre

2017-12-01

This paper presents new findings on polycyclic aromatic hydrocarbon oxidation products-quinones that were collected in ambient air samples in the proximity of oil sands exploration. Quinones were characterized for their diurnal concentration variability, phase partitioning, and molecular size distribution. Gas-phase (GP) and particle-phase (PM) ambient air samples were collected separately in the summer; a lower quinone content was observed in the PM samples from continuous 24-h sampling than from combined 12-h sampling (day and night). The daytime/nocturnal samples demonstrated that nighttime conditions led to lower concentrations and some quinones not being detected. The highest quinone levels were associated with wind directions originating from oil sands exploration sites. The statistical correlation with primary pollutants directly emitted from oil sands industrial activities indicated that the bulk of the detected quinones did not originate directly from primary emission sources and that quinone formation paralleled a reduction in primary source NO x levels. This suggests a secondary chemical transformation of primary pollutants as the origin of the determined quinones. Measurements of 19 quinones included five that have not previously been reported in ambient air or in Standard Reference Material 1649a/1649b and seven that have not been previously measured in ambient air in the underivatized form. This is the first paper to report on quinone characterization in secondary organic aerosols originating from oil sands activities, to distinguish chrysenequinone and anthraquinone positional isomers in ambient air, and to report the requirement of daylight conditions for benzo[a]pyrenequinone and naphthacenequinone to be present in ambient air. Crown Copyright © 2017. Published by Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2010-12-01

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

Quantifying compositional impacts of ambient aerosol on cloud droplet formation

NASA Astrophysics Data System (ADS)

Lance, Sara

It has been historically assumed that most of the uncertainty associated with the aerosol indirect effect on climate can be attributed to the unpredictability of updrafts. In Chapter 1, we analyze the sensitivity of cloud droplet number density, to realistic variations in aerosol chemical properties and to variable updraft velocities using a 1-dimensional cloud parcel model in three important environmental cases (continental, polluted and remote marine). The results suggest that aerosol chemical variability may be as important to the aerosol indirect effect as the effect of unresolved cloud dynamics, especially in polluted environments. We next used a continuous flow streamwise thermal gradient Cloud Condensation Nuclei counter (CCNc) to study the water-uptake properties of the ambient aerosol, by exposing an aerosol sample to a controlled water vapor supersaturation and counting the resulting number of droplets. In Chapter 2, we modeled and experimentally characterized the heat transfer properties and droplet growth within the CCNc. Chapter 3 describes results from the MIRAGE field campaign, in which the CCNc and a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) were deployed at a ground-based site during March, 2006. Size-resolved CCN activation spectra and growth factor distributions of the ambient aerosol in Mexico City were obtained, and an analytical technique was developed to quantify a probability distribution of solute volume fractions for the CCN in addition to the aerosol mixing-state. The CCN were shown to be much less CCN active than ammonium sulfate, with water uptake properties more consistent with low molecular weight organic compounds. The pollution outflow from Mexico City was shown to have CCN with an even lower fraction of soluble material. "Chemical Closure" was attained for the CCN, by comparing the inferred solute volume fraction with that from direct chemical measurements. A clear diurnal pattern was observed for the CCN solute

On the link between hygroscopicity, volatility, and oxidation state of ambient and water-soluble aerosol in the Southeastern United States

NASA Astrophysics Data System (ADS)

Cerully, K. M.; Bougiatioti, A.; Hite, J. R., Jr.; Guo, H.; Xu, L.; Ng, N. L.; Weber, R.; Nenes, A.

2014-12-01

The formation of secondary organic aerosol (SOA) combined with the partitioning of semi-volatile organic components can impact numerous aerosol properties including cloud condensation nuclei (CCN) activity, hygroscopicity and volatility. During the summer 2013 Southern Oxidant and Aerosol Study (SOAS) field campaign in a rural site in the Southeastern United States, a suite of instruments including a CCN counter, a thermodenuder (TD) and a high resolution time-of-flight aerosol mass spectrometer (AMS) were used to measure CCN activity, aerosol volatility, composition and oxidation state. Particles were either sampled directly from ambient or through a Particle Into Liquid Sampler (PILS), allowing the investigation of the water-soluble aerosol component. Ambient aerosol exhibited size-dependent composition with larger particles being more hygroscopic. The hygroscopicity of thermally-denuded aerosol was similar between ambient and PILS-generated aerosol and showed limited dependence on volatilization. Results of AMS 3-factor Positive Matrix Factorization (PMF) analysis for the PILS-generated aerosol showed that the most hygroscopic components are most likely the most and the least volatile features of the aerosol. No clear relationship was found between organic hygroscopicity and oxygen-to-carbon ratio; in fact, Isoprene organic aerosol (Isoprene-OA) was found to be the most hygroscopic factor, while at the same time being the least oxidized and likely most volatile of all PMF factors. Considering the diurnal variation of each PMF factor and its associated hygroscopicity, Isoprene-OA and More Oxidized - Oxidized Oxygenated Organic Aerosol (MO-OOA) are the prime contributors to hygroscopicity and covary with Less Oxidized - Oxidized Oxygenated Organic Aerosol (LO-OOA) in a way that induces the observed diurnal invariance in total organic hygroscopicity. Biomass Burning Organic Aerosol (BBOA) contributed little to aerosol hygroscopicity, which is expected since there

Hygroscopic Characteristics of Organic Laden Ambient Aerosols in Yosemite National Park

NASA Astrophysics Data System (ADS)

Malm, W. C.; Day, D. E.; Kreidenweis, S. M.; Collett, J. L.; Carrico, C. M.; Lee, T.; Bench, G.; Carrillo, J.

2003-12-01

Water absorption by inorganic compounds can be modeled with some degree of certainty; however, water uptake by ambient organic aerosols remains speculative. To improve the understanding of organic hygroscopicity, an aerosol characterization study was conducted at Yosemite National Park, California, starting in July and ending in the first week of September 2002. High time resolution measurement (15-minute time increments) of PM2.5 ionic species (Cl-, SO42-, NO3-, Na+, NH4+, K+, Mg2+, and Ca2+) were measured using PILS (Particle-Into-Liquid-System)/IC (Ion Chromatography). Commercially available annular denuders and a PM2.5 cyclone (URG) were used upstream of the PILS/IC to remove particles greater than 2.5 μm and acidic and basic gases. A dual wavelength aethalometer and an R&P particulate carbon monitor were used to measure carbon on a semi-continuous basis while a DRUM sampler allowed for semi-continuous estimates of concentrations of elements associated with crustal material. Standard IMPROVE type samplers were used to measure 24-hr integrated samples of these same aerosols. Two nephelometers operated in tandem, one dry and the other with a controlled humidity environment, were used to measure f(RH) = bscat(RH)/bscat,dry, where bscat(RH) is the scattering coefficient measured at some relative humidity and bscat,dry is the scattering coefficient measured at RH <10%. The aerosol composition was highly variable in time, with a strong diurnal cycle. Organic carbon mass was observed to be, on the average, 70% of the fine mass with days where its contribution was well over 95% of the mass. Measurements of carbon isotopes revealed the fraction of carbon from biogenic sources to range from approximately 73 to 95%. Water soluble potassium was highly correlated with carbon mass, suggesting the influence of wood smoke. The ionic fraction of the aerosol consisted primarily of ammonium sulfate and in most cases nitrate was in the form of sodium nitrate. Fine soil mass was

Collection of Aerosolized Human Cytokines Using Teflon® Filters

PubMed Central

McKenzie, Jennifer H.; McDevitt, James J.; Fabian, M. Patricia; Hwang, Grace M.; Milton, Donald K.

2012-01-01

Background Collection of exhaled breath samples for the analysis of inflammatory biomarkers is an important area of research aimed at improving our ability to diagnose, treat and understand the mechanisms of chronic pulmonary disease. Current collection methods based on condensation of water vapor from exhaled breath yield biomarker levels at or near the detection limits of immunoassays contributing to problems with reproducibility and validity of biomarker measurements. In this study, we compare the collection efficiency of two aerosol-to-liquid sampling devices to a filter-based collection method for recovery of dilute laboratory generated aerosols of human cytokines so as to identify potential alternatives to exhaled breath condensate collection. Methodology/Principal Findings Two aerosol-to-liquid sampling devices, the SKC® Biosampler and Omni 3000™, as well as Teflon® filters were used to collect aerosols of human cytokines generated using a HEART nebulizer and single-pass aerosol chamber setup in order to compare the collection efficiencies of these sampling methods. Additionally, methods for the use of Teflon® filters to collect and measure cytokines recovered from aerosols were developed and evaluated through use of a high-sensitivity multiplex immunoassay. Our results show successful collection of cytokines from pg/m3 aerosol concentrations using Teflon® filters and measurement of cytokine levels in the sub-picogram/mL concentration range using a multiplex immunoassay with sampling times less than 30 minutes. Significant degradation of cytokines was observed due to storage of cytokines in concentrated filter extract solutions as compared to storage of dry filters. Conclusions Use of filter collection methods resulted in significantly higher efficiency of collection than the two aerosol-to-liquid samplers evaluated in our study. The results of this study provide the foundation for a potential new technique to evaluate biomarkers of inflammation in

Photoacoustic optical properties at UV, VIS, and near IR wavelengths for laboratory generated and winter time ambient urban aerosols

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

Gyawali, Madhu S.; Arnott, W. Patrick; Zaveri, Rahul A.

2012-03-08

We present the laboratory and ambient photoacoustic (PA) measurement of aerosol light absorption coefficients at ultraviolet wavelength (i.e., 355 nm) and compare with measurements at 405, 532, 870, and 1047 nm. Simultaneous measurements of aerosol light scattering coefficients were achieved by the integrating reciprocal nephelometer within the PA's acoustic resonator. Absorption and scattering measurements were carried out for various laboratory generated aerosols, including salt, incense, and kerosene soot to evaluate the instrument calibration and gain insight on the spectral dependence of aerosol light absorption and scattering. Ambient measurements were obtained in Reno, Nevada, between 18 December 2009 and 18 Januarymore » 2010. The measurement period included days with and without strong ground level temperature inversions, corresponding to highly polluted (freshly emitted aerosols) and relatively clean (aged aerosols) conditions. Particulate matter (PM) concentrations were measured and analyzed with other tracers of traffic emissions. The temperature inversion episodes caused very high concentration of PM{sub 2.5} and PM{sub 10} (particulate matter with aerodynamic diameters less than 2.5 {mu}m and 10 {mu}m, respectively) and gaseous pollutants: carbon monoxide (CO), nitric oxide (NO), and nitrogen dioxide (NO{sub 2}). The diurnal change of absorption and scattering coefficients during the polluted (inversion) days increased approximately by a factor of two for all wavelengths compared to the clean days. The spectral variation in aerosol absorption coefficients indicated a significant amount of absorbing aerosol from traffic emissions and residential wood burning. The analysis of single scattering albedo (SSA), Angstrom exponent of absorption (AEA), and Angstrom exponent of scattering (AES) for clean and polluted days provides evidences that the aerosol aging and coating process is suppressed by strong temperature inversion under cloudy conditions. In

Photoacoustic Optical Properties at UV, VIS, and near IR Wavelengths for Laboratory Generated and Winter Time Ambient Urban Aerosols

NASA Technical Reports Server (NTRS)

Gyawali, M.; Arnott, W. P.; Zaveri, R. A.; Song, C.; Moosmuller, H.; Liu, L.; Mishchenko, M. I.; Chen, L.-W.A.; Green, M. C.; Watson, J. G.;

ANALYSIS OF RESPIRATORY DESPOSITION DOSE OF INHALED AMBIENT AEROSOLS FOR DIFFERENT SIZE FRACTIONS

EPA Science Inventory

ANALYSIS OF RESPIRATORY DEPOSITION DOSE OF INHALED AMBIENT AEROSOLS FOR DIFFERENT SIZE FRACTIONS. Chong S. Kim, SC. Hu**, PA Jaques*, US EPA, National Health and Environmental Effects Research Laboratory, Research Triangle Park, NC 27711; **IIT Research Institute, Chicago, IL; *S...

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

Individual aerosol particles in ambient and updraft conditions below convective cloud bases in the Oman mountain region

NASA Astrophysics Data System (ADS)

Semeniuk, T. A.; Bruintjes, R. T.; Salazar, V.; Breed, D. W.; Jensen, T. L.; Buseck, P. R.

2014-03-01

An airborne study of cloud microphysics provided an opportunity to collect aerosol particles in ambient and updraft conditions of natural convection systems for transmission electron microscopy (TEM). Particles were collected simultaneously on lacey carbon and calcium-coated carbon (Ca-C) TEM grids, providing information on particle morphology and chemistry and a unique record of the particle's physical state on impact. In total, 22 particle categories were identified, including single, coated, aggregate, and droplet types. The fine fraction comprised up to 90% mixed cation sulfate (MCS) droplets, while the coarse fraction comprised up to 80% mineral-containing aggregates. Insoluble (dry), partially soluble (wet), and fully soluble particles (droplets) were recorded on Ca-C grids. Dry particles were typically silicate grains; wet particles were mineral aggregates with chloride, nitrate, or sulfate components; and droplets were mainly aqueous NaCl and MCS. Higher numbers of droplets were present in updrafts (80% relative humidity (RH)) compared with ambient conditions (60% RH), and almost all particles activated at cloud base (100% RH). Greatest changes in size and shape were observed in NaCl-containing aggregates (>0.3 µm diameter) along updraft trajectories. Their abundance was associated with high numbers of cloud condensation nuclei (CCN) and cloud droplets, as well as large droplet sizes in updrafts. Thus, compositional dependence was observed in activation behavior recorded for coarse and fine fractions. Soluble salts from local pollution and natural sources clearly affected aerosol-cloud interactions, enhancing the spectrum of particles forming CCN and by forming giant CCN from aggregates, thus, making cloud seeding with hygroscopic flares ineffective in this region.

Dependence of Aerosol Light Absorption and Single-Scattering Albedo On Ambient Relative Humidity for Sulfate Aerosols with Black Carbon Cores

NASA Technical Reports Server (NTRS)

Redemann, Jens; Russell, Philip B.; Hamill, Patrick

2001-01-01

Atmospheric aerosols frequently contain hygroscopic sulfate species and black carbon (soot) inclusions. In this paper we report results of a modeling study to determine the change in aerosol absorption due to increases in ambient relative humidity (RH), for three common sulfate species, assuming that the soot mass fraction is present as a single concentric core within each particle. Because of the lack of detailed knowledge about various input parameters to models describing internally mixed aerosol particle optics, we focus on results that were aimed at determining the maximum effect that particle humidification may have on aerosol light absorption. In the wavelength range from 450 to 750 nm, maximum absorption humidification factors (ratio of wet to 'dry=30% RH' absorption) for single aerosol particles are found to be as large as 1.75 when the RH changes from 30 to 99.5%. Upon lesser humidification from 30 to 80% RH, absorption humidification for single particles is only as much as 1.2, even for the most favorable combination of initial ('dry') soot mass fraction and particle size. Integrated over monomodal lognormal particle size distributions, maximum absorption humidification factors range between 1.07 and 1.15 for humidification from 30 to 80% and between 1.1 and 1.35 for humidification from 30 to 95% RH for all species considered. The largest humidification factors at a wavelength of 450 nm are obtained for 'dry' particle size distributions that peak at a radius of 0.05 microns, while the absorption humidification factors at 700 nm are largest for 'dry' size distributions that are dominated by particles in the radius range of 0.06 to 0.08 microns. Single-scattering albedo estimates at ambient conditions are often based on absorption measurements at low RH (approx. 30%) and the assumption that aerosol absorption does not change upon humidification (i.e., absorption humidification equal to unity). Our modeling study suggests that this assumption alone can

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.

Chemical Imaging of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

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

O'Brien, Rachel; Wang, Bingbing; Laskin, Alexander

2015-09-28

A new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission x-ray microscopy/near edge x-ray absorption fine structure (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on June 27th and 28th during the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierramore » Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. Both microscopy imaging techniques showed more changes over these two days in the mixing state at the T0 site than at the T1 site. The STXM data showed evidence of changes in the mixing state associated with a build-up of organic matter confirmed by collocated measurements and the largest impact on the mixing state was due to an increase in soot dominant particles during this build-up. The CCSEM/EDX analysis showed the presence of two types of particle populations; the first was dominated by aged sea salt particles and had a higher mixing state index (indicating a more homogeneous population), the second was dominated by carbonaceous particles and had a lower mixing state index.« less

Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

DOE PAGES

O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; ...

2015-08-26

In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near themore » Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.« less

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.

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)

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

Hu, Weiwei; Palm, Brett B.; Day, Douglas A.

Isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA) can contribute substantially to organic aerosol (OA) concentrations in forested areas under low NO conditions, hence significantly influencing the regional and global OA budgets, accounting, for example, for 16–36 % of the submicron OA in the southeastern United States (SE US) summer. Particle evaporation measurements from a thermodenuder show that the volatility of ambient IEPOX-SOA is lower than that of bulk OA and also much lower than that of known monomer IEPOX-SOA tracer species, indicating that IEPOX-SOA likely exists mostly as oligomers in the aerosol phase. The OH aging process of ambient IEPOX-SOA was investigatedmore » with an oxidation flow reactor (OFR). New IEPOX-SOA formation in the reactor was negligible, as the OFR does not accelerate processes such as aerosol uptake and reactions that do not scale with OH. Simulation results indicate that adding ~100 µg m -3 of pure H 2SO 4 to the ambient air allows IEPOX-SOA to be efficiently formed in the reactor. The heterogeneous reaction rate coefficient of ambient IEPOX-SOA with OH radical ( k OH) was estimated as 4.0 ± 2.0 ×10 -13 cm 3 molec -1 s -1, which is equivalent to more than a 2-week lifetime. A similar k OH was found for measurements of OH oxidation of ambient Amazon forest air in an OFR. At higher OH exposures in the reactor (> 1 × 10 12 molec cm -3 s), the mass loss of IEPOX-SOA due to heterogeneous reaction was mainly due to revolatilization of fragmented reaction products. We report, for the first time, OH reactive uptake coefficients ( γ OH = 0.59±0.33 in SE US and γ OH = 0.68±0.38 in Amazon) for SOA under ambient conditions. A relative humidity dependence of k OH and γ OH was observed, consistent with surface-area-limited OH uptake. No decrease of k OH was observed as OH concentrations increased. These observations of physicochemical properties of IEPOX-SOA can help to constrain OA impact on air quality and climate.« less

Photoacoustic optical properties at UV, VIS, and near IR wavelengths for laboratory generated and winter time ambient urban aerosols

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Zaveri, R. A.; Song, C.; Moosmüller, H.; Liu, L.; Mishchenko, M. I.; Chen, L.-W. A.; Green, M. C.; Watson, J. G.; Chow, J. C.

2011-09-01

We present the first laboratory and ambient photoacoustic (PA) measurement of aerosol light absorption coefficients at ultraviolet (UV) wavelength (i.e. 355 nm) and compare with measurements at 405, 532, 870, and 1047 nm. Simultaneous measurements of aerosol light scattering coefficients were achieved by the integrating reciprocal nephelometer within the PA';s acoustic resonator. Absorption and scattering measurements were carried out for various laboratory-generated aerosols, including salt, incense, and kerosene soot to evaluate the instrument calibration and gain insight on the spectral dependence of aerosol light absorption and scattering. Exact T-matrix method calculations were used to model the absorption and scattering characteristics of fractal-like agglomerates of different compactness and varying number of monomers. With these calculations, we attempted to estimate the number of monomers and fractal dimension of laboratory generated kerosene soot. Ambient measurements were obtained in Reno, Nevada, between 18 December 2009, and 18 January 2010. The measurement period included days with and without strong ground level temperature inversions, corresponding to highly polluted (freshly emitted aerosols) and relatively clean (aged aerosols) conditions. Particulate matter (PM) concentrations were measured and analyzed with other tracers of traffic emissions. The temperature inversion episodes caused very high concentration of PM2.5 and PM10 (particulate matter with aerodynamic diameters less than 2.5 μm and 10 μm, respectively) and gaseous pollutants: carbon monoxide (CO), nitric oxide (NO), and nitrogen dioxide (NO2). The diurnal change of absorption and scattering coefficients during the polluted (inversion) days increased approximately by a factor of two for all wavelengths compared to the clean days. The spectral variation in aerosol absorption coefficients indicated a significant amount of absorbing aerosol from traffic emissions and residential wood

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

DOE PAGES

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

2018-02-20

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

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

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

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

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

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

NASA Astrophysics Data System (ADS)

Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A.; Campuzano-Jost, Pedro; Hu, Weiwei; Seco, Roger; Sjostedt, Steven J.; Park, Jeong-Hoo; Guenther, Alex B.; Kim, Saewung; Brito, Joel; Wurm, Florian; Artaxo, Paulo; Thalman, Ryan; Wang, Jian; Yee, Lindsay D.; Wernis, Rebecca; Isaacman-VanWertz, Gabriel; Goldstein, Allen H.; Liu, Yingjun; Springston, Stephen R.; Souza, Rodrigo; Newburn, Matt K.; Lizabeth Alexander, M.; Martin, Scot T.; Jimenez, Jose L.

2018-01-01

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m-3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ˜ 1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10-50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign

Effects of post-sampling conditions on ambient carbon aerosol filter measurements

NASA Astrophysics Data System (ADS)

Dillner, Ann M.; Phuah, Chin H.; Turner, Jay R.

2009-12-01

Ambient carbonaceous material collected on quartz filters is prone to measurement artifacts due to material gained or lost during post-sampling field latency, shipping, and storage. In seventeen sampling events over a one year period, ambient PM 2.5 aerosols were collected on quartz filters (without denuders) and subjected to various filter treatments to assess the potential for and extent of artifacts. The filter treatments simulated post-sampling environments that filters may be exposed to and included: storage at 40 °C for up to 96 h, storage at -16 °C for 48 h, and storage at room temperature (˜21 °C) for 48 h. Carbon mass on the filters was measured using a thermal-optical method. The total carbon (TC), total organic carbon (TOC) and total elemental carbon (TEC) as well as carbon thermal fraction masses were obtained. Statistical analyses were performed to identify significant differences in carbon fraction concentrations between filters analyzed immediately after sampling and after being subjected to treatment. TOC and TC concentrations decreased by on average 15 ± 5% and 10 ± 4%, respectively, for filters maintained at 40 °C for 96 h but did not change for filters stored at room temperature or frozen for 48 h. TEC did not change for any of the filter treatments. The mass concentration for the organic carbon thermal fraction that evolves at the lowest temperature step (OC1) decreased with increasing storage time at 40 °C with average losses of 70 ± 7% after 96 h. Therefore, OC1 is not a stable measurement due to post-sampling conditions that may be encountered. This work demonstrates that TOC and TC can have substantial measurement artifacts on filters subjected to field latency and other non-temperature controlled post-sampling handling, compared to the carbon loadings on the filter at the end of the sampling period.

Laboratory and field based evaluation of chromatography related performance of the Monitor for Aerosols and Gases in Ambient Air (MARGA)

EPA Science Inventory

The Monitor for AeRosols and GAses in ambient air (MARGA) is an on-line ion-chromatography-based instrument designed for speciation of the inorganic gas and aerosol ammonium-nitrate-sulfate system. Previous work to characterize the performance of the MARGA has been primarily base...

Chemical characteristics of ambient aerosols contributed by cooking process at Noorpur village near Delhi (India)

NASA Astrophysics Data System (ADS)

Singh, Sudha; Kumar, Bablu; Gupta, Gyan Prakash; Kulshrestha, U. C.

2013-05-01

Combustion of fuels such as wood, crop residue and dung cakes etc. is one of the major sources of air pollution in developing countries. These fuels are still used commonly for cooking purpose in rural India. This study investigates the chemical composition of the ambient aerosols during cooking hours at a village called Noorpur (28.470 N, 77.030 E) which lies near Delhi city. Aerosol sampling was carried out during August 2011-May 2012 by using handy sampler (Envirotech model APM 821) installed at the terrace of a building (˜6m). The samples were collected on 8 hourly basis using Teflon filters. The water extract of these filters was analyzed for major anions (F-, Cl-, NO3-, SO42-) and major cations (Na+, NH4+, K+, Ca2+ Mg2+) by ion chromatography (Metrohm 883 Basic IC Plus). Results highlighted that cooking process contributed significant amount of SO42- and K+ṡ. Biomass burning is considered as a potential source of K+ in air. The high concentration of SO42- might be due to oxidation of SO2 contributed by the combustion of dung cakes. Further, the detailed results will be discussed during the conference.

Variability of Ambient Aerosol in the Mexico City Metropolian Area

NASA Astrophysics Data System (ADS)

Onasch, T. B.; Worsnop, D. R.; Canagaratna, M.; Jayne, J. T.; Herndon, S.; Mortimer, P.; Kolb, C. E.; Rogers, T.; Knighton, B.; Dunlea, E.; Marr, L.; de Foy, B.; Molina, M.; Molina, L.; Salcedo, D.; Dzepina, K.; Jimenez, J. L.

2004-12-01

The spatial and temporal variations of the ambient aerosol in the Mexico City Metropolitan area was characterized during the springs of 2002 and 2003 using a mobile laboratory equipped with gas and particulate measurement instrumentation. The laboratory was operated at various fixed sites locations in and at the edge of the metropolitan area (Xalostoc, Merced, Cenica, Pedregal, and Santa Ana). Size-resolved aerosol mass and chemical composition was measured with an aerosol mass spectrometer and selected trace gas species (low mass organic compounds, NO, NO2, NOy, O3, SO2, CH2O, NH3, CO2) were measured using a proton transfer reaction mass spectrometer and various optical systems. The aerosol was predominantly organic in composition with lesser amounts of ammonium nitrate, sulfate, and chloride. The organic component was composed of mixed primary and secondary organic compounds. The mass loading and chemical composition of the aerosol was influenced by local and regional air pollution sources and the meteorology in Mexico City. Most urban sites were influenced by a strong diurnal particulate mass trend indicative of primary organic emissions from traffic during early morning and subsequently oxidized/processed organics and ammonium nitrate particles starting in the mid-morning (~9 AM) and continuing throughout the day. Morning traffic-related primary organic emissions were strongest at La Merced (center of Mexico City, located near a busy food market), more subdued at other fixed sites further from the city center, and varied depending upon the day of week and holiday schedules. Particle-bound polycyclic aromatic hydrocarbons were observed within Mexico City fixed sites and were correlated with traffic organic PM emissions. Oxidized organic and ammonium nitrate events occurred during mid-morning at all city sites and were well correlated with gas phase photochemical activity. The daily ammonium nitrate aerosol event occurred later at sites near the city limits

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)

DOE PAGES

Hu, Weiwei; Palm, Brett B.; Day, Douglas A.; ...

2016-09-19

Isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA) can contribute substantially to organic aerosol (OA) concentrations in forested areas under low NO conditions, hence significantly influencing the regional and global OA budgets, accounting, for example, for 16–36 % of the submicron OA in the southeastern United States (SE US) summer. Particle evaporation measurements from a thermodenuder show that the volatility of ambient IEPOX-SOA is lower than that of bulk OA and also much lower than that of known monomer IEPOX-SOA tracer species, indicating that IEPOX-SOA likely exists mostly as oligomers in the aerosol phase. The OH aging process of ambient IEPOX-SOA was investigated withmore » an oxidation flow reactor (OFR). New IEPOX-SOA formation in the reactor was negligible, as the OFR does not accelerate processes such as aerosol uptake and reactions that do not scale with OH. Simulation results indicate that adding  ∼  100 µg m −3 of pure H 2SO 4 to the ambient air allows IEPOX-SOA to be efficiently formed in the reactor. The heterogeneous reaction rate coefficient of ambient IEPOX-SOA with OH radical ( k OH) was estimated as 4.0 ± 2.0  ×  10 −13 cm 3 molec −1 s −1, which is equivalent to more than a 2-week lifetime. A similar k OH was found for measurements of OH oxidation of ambient Amazon forest air in an OFR. At higher OH exposures in the reactor (>  1  ×  10 12 molec cm −3 s), the mass loss of IEPOX-SOA due to heterogeneous reaction was mainly due to revolatilization of fragmented reaction products. We report, for the first time, OH reactive uptake coefficients ( γ OH =  0.59 ± 0.33 in SE US and γ OH =  0.68 ± 0.38 in Amazon) for SOA under ambient conditions. A relative humidity dependence of k OH and γ OH was observed, consistent with surface-area-limited OH uptake. No decrease of k OH was observed as OH concentrations increased. These observations of

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)

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

Hu, Weiwei; Palm, Brett B.; Day, Douglas A.

Isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA) can contribute substantially to organic aerosol (OA) concentrations in forested areas under low NO conditions, hence significantly influencing the regional and global OA budgets, accounting, for example, for 16–36 % of the submicron OA in the southeastern United States (SE US) summer. Particle evaporation measurements from a thermodenuder show that the volatility of ambient IEPOX-SOA is lower than that of bulk OA and also much lower than that of known monomer IEPOX-SOA tracer species, indicating that IEPOX-SOA likely exists mostly as oligomers in the aerosol phase. The OH aging process of ambient IEPOX-SOA was investigated withmore » an oxidation flow reactor (OFR). New IEPOX-SOA formation in the reactor was negligible, as the OFR does not accelerate processes such as aerosol uptake and reactions that do not scale with OH. Simulation results indicate that adding  ∼  100 µg m −3 of pure H 2SO 4 to the ambient air allows IEPOX-SOA to be efficiently formed in the reactor. The heterogeneous reaction rate coefficient of ambient IEPOX-SOA with OH radical ( k OH) was estimated as 4.0 ± 2.0  ×  10 −13 cm 3 molec −1 s −1, which is equivalent to more than a 2-week lifetime. A similar k OH was found for measurements of OH oxidation of ambient Amazon forest air in an OFR. At higher OH exposures in the reactor (>  1  ×  10 12 molec cm −3 s), the mass loss of IEPOX-SOA due to heterogeneous reaction was mainly due to revolatilization of fragmented reaction products. We report, for the first time, OH reactive uptake coefficients ( γ OH =  0.59 ± 0.33 in SE US and γ OH =  0.68 ± 0.38 in Amazon) for SOA under ambient conditions. A relative humidity dependence of k OH and γ OH was observed, consistent with surface-area-limited OH uptake. No decrease of k OH was observed as OH concentrations increased. These observations of

The source identification of ambient aerosols in Beijing, China by multivariate analysis coupled with {sup 14}C tracer

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

Xiaoyan Tang; Min Shao; Yuanhang Zhang

1996-12-31

Ambient aerosol is one of most important pollutants in China. This paper showed the results of aerosol sources of Beijing area revealed by combination of multivariate analysis models and 14C tracer measured on Accelerator Mass Spectrometry (AMS). The results indicated that the mass concentration of particulate (<100 (M)) didn`t increase rapidly, compared with economic development in Beijing city. The multivariate analysis showed that the predominant source was soil dust which contributed more than 50% to atmospheric particles. However, it would be a risk to conclude that the aerosol pollution from anthropogenic sources was less important in Beijing city based onmore » above phenomenon. Due to lack of reliable tracers, it was very hard to distinguish coal burning from soil source. Thus, it was suspected that the soil source above might be the mixture of soil dust and coal burning. The 14C measurement showed that carbonaceous species of aerosol had quite different emission sources. For carbonaceous aerosols in Beijing, the contribution from fossil fuel to ambient particles was nearly 2/3, as the man-made activities ( coal-burning, etc.) increased, the fossil part would contribute more to atmospheric carbonaceous particles. For example, in downtown Beijing at space-heating seasons, the fossil fuel even contributed more than 95% to carbonaceous particles, which would be potential harmful to population. By using multivariate analysis together with 14C data, two important sources of aerosols in Beijing (soil and coal) combustion were more reliably distinguished, which was critical important for the assessment of aerosol problem in China.« less

Aqueous photooxidation of ambient Po Valley Italy air samples: Insights into secondary organic aerosol formation

NASA Astrophysics Data System (ADS)

Kirkland, J. R.; Lim, Y. B.; Sullivan, A. P.; Decesari, S.; Facchini, C.; Collett, J. L.; Keutsch, F. N.; Turpin, B. J.

2012-12-01

In this work, we conducted aqueous photooxidation experiments with ambient samples in order to develop insights concerning the formation of secondary organic aerosol through gas followed by aqueous chemistry (SOAaq). Water-soluble organics (e.g., glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone) are formed through gas phase oxidation of alkene and aromatic emissions of anthropogenic and biogenic origin. Their further oxidation in clouds, fogs and wet aerosols can form lower volatility products (e.g., oligomers, organic acids) that remain in the particle phase after water evaporation, thus producing SOA. The aqueous OH radical oxidation of several individual potentially important precursors has been studied in the laboratory. In this work, we used a mist-chamber apparatus to collect atmospheric mixtures of water-soluble gases from the ambient air at San Pietro Capofiume, Italy during the PEGASOS field campaign. We measured the concentration dynamics after addition of OH radicals, in order to develop new insights regarding formation of SOA through aqueous chemistry. Specifically, batch aqueous reactions were conducted with 33 ml mist-chamber samples (TOC ~ 50-100μM) and OH radicals (~10-12M) in a new low-volume aqueous reaction vessel. OH radicals were formed in-situ, continuously by H2O2 photolysis. Products were analyzed by ion chromatography (IC), electrospray ionization mass spectrometry (ESI-MS +/-), and ESI-MS with IC pre-separation (IC/ESI-MS-). Reproducible formation of pyruvate and oxalate were observed both by IC and ESI-MS. These compounds are known to form from aldehyde oxidation in the aqueous phase. New insights regarding the aqueous chemistry of these "more atmospherically-realistic" experiments will be discussed.

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

DOE PAGES

Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A.; ...

2018-01-17

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O 3, over ranges from hours to days (O 3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to asmore » much as 10 μg m -3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O 3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air, and confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ~ 1.0, and then decreased as O : C increased further. Some possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. And while measured ambient precursors were sufficient to explain the amount of SOA formed from O 3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

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

Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A.

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O 3, over ranges from hours to days (O 3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to asmore » much as 10 μg m -3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O 3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air, and confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ~ 1.0, and then decreased as O : C increased further. Some possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. And while measured ambient precursors were sufficient to explain the amount of SOA formed from O 3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

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

Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A.

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O 3, over ranges from hours to days (O 3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to asmore » much as 10 µg m −3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O 3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ∼ 1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O 3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the

Investigating Source Contributions of Size-Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

NASA Astrophysics Data System (ADS)

Li, Jianghanyang; Michalski, Greg; Davy, Perry; Harvey, Mike; Katzman, Tanya; Wilkins, Benjamin

2018-04-01

Marine sulfate aerosols in the Southern Ocean are critical to the global radiation balance, yet the sources of sulfate and their seasonal variations are unclear. We separately sampled marine and ambient aerosols at Baring Head, New Zealand for 1 year using two collectors and evaluated the sources of sulfate in coarse (1-10 μm) and fine (0.05-1 μm) aerosols using sulfur isotopes (δ34S). In both collectors, sea-salt sulfate (SO42-SS) mainly existed in coarse aerosols and nonsea-salt sulfate (SO42-NSS) dominated the sulfate in fine aerosols, although some summer SO42-NSS appeared in coarse particles due to aerosol coagulation. SO42-NSS in the marine aerosols was mainly (88-100%) from marine biogenic dimethylsulfide (DMS) emission, while the SO42-NSS in the ambient aerosols was a combination of DMS (73-79%) and SO2 emissions from shipping activities ( 21-27%). The seasonal variations of SO42-NSS concentrations inferred from the δ34S values in both collectors were mainly controlled by the DMS flux.

Secondary Organic Aerosol Formation in the Captive Aerosol Growth and Evolution (CAGE) Chambers during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, AL

NASA Astrophysics Data System (ADS)

Leong, Y.; Karakurt Cevik, B.; Hernandez, C.; Griffin, R. J.; Taylor, N.; Matus, J.; Collins, D. R.

2013-12-01

reversibility and the sensitivity of SOA reactions to oxidant or NOx enhancement and aerosol liquid water content. Available ambient trace gas concentrations include VOCs, NOx, SO2, ozone, peroxyaxyl nitrates, and ammonia. Chamber data will also be compared to ambient aerosol measurements collected by the instruments mentioned above as well as those from other research groups.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

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.

Improved Large-Volume Sampler for the Collection of Bacterial Cells from Aerosol

PubMed Central

White, L. A.; Hadley, D. J.; Davids, D. E.; Naylor, R.

1975-01-01

A modified large-volume sampler was demonstrated to be an efficient device for the collection of mono-disperse aerosols of rhodamine B and poly-disperse aerosols of bacterial cells. Absolute efficiency for collection of rhodamine B varied from 100% with 5-μm particles to about 70% with 0.5-μm particles. The sampler concentrated the particles from 950 liters of air into a flow of between 1 and 2 ml of collecting fluid per min. Spores of Bacillus subtilis var. niger were collected at an efficiency of about 82% compared to the collection in the standard AGI-30 sampler. In the most desirable collecting fluids tested, aerosolized cells of Serratia marcescens, Escherichia coli, and Aerobacter aerogenes were collected at comparative efficiencies of approximately 90, 80, and 90%, respectively. The modified sampler has practical application in the study of aerosol transmission of respiratory pathogens. Images PMID:803820

Physical and Chemical Properties of Individual Marine Aerosols Collected over the Arctic Ocean

NASA Astrophysics Data System (ADS)

Yoshizue, M.; Taketani, F.; Adachi, K.; Iwamoto, Y.; Mori, T.; Miura, K.

2017-12-01

Atmospheric aerosol particles including black carbon (BC) play an important role in Arctic climate effect through absorbing and scattering solar radiation. However, quantitative understanding of atmospheric aerosol's behavior in Arctic region is limited. In this study, we characterized the mixing states and chemical compositions of marine aerosol particles collected over the Arctic Ocean on the basis of an individual particle analysis using a transmission electron microscope (TEM) and an energy dispersive X-ray spectrometer. Observations and TEM samplings were conducted on-board the R/V Mirai from 22 August to 5 October 2016 in a round trip to the Arctic Ocean from a port of Hachinohe (40.52°N, 141.51°E), Japan. Samplings of atmospheric aerosol particles were carried out on the flying deck (18 m a.s.l.) of R/V Mirai using a low volume cascade impactor with a volumetric flow of 1 L/min. The sampling times ranged from 40 to 70 min. To monitor ambient BC mass concentrations, we also used an online instrument of single particle soot photometer (SP2). In >70°N, we captured relatively high BC mass concentration events on 7 and 16 September 2016 at 71.70°N, 155.10°W and 72.48°N, 155.42°W, respectively. Within clean condition samples on 11 and 14 September 2016, the number fractions of sulfur-rich (S-rich) and carbon-rich (C-rich) particles were, respectively, less than 40% and 15% in the analyzed particles (n=423). On the other hand, in the sample collected at 7 September, the number fractions of S- and C-rich particles were more than 70% and about 5% (n=299), respectively, suggesting that the air mass had been affected by anthropogenic substances. In a sample collected at 16 September, the number fractions of S- and C-rich particles were about 15% and 40% (n=88), respectively. The backward trajectory analyses indicated that the air masses came from Siberian coastal area through the East Siberian Sea, suggesting that the events might be influenced by long

Efficiency of aerosol collection on wires exposed in the stratosphere

NASA Technical Reports Server (NTRS)

Lem, H. Y.; Farlow, N. H.

1979-01-01

The theory of inertial impaction is briefly presented. Stratospheric aerosol research experiments were performed duplicating Wong et al. experiments. The use of the curve of inertial parameters vs particle collection efficiency, derived from Wong et al., was found to be justified. The results show that stratospheric aerosol particles of all sizes are collectible by wire impaction technique. Curves and tables are presented and used to correct particle counts for collection efficiencies less than 100%.

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

Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US

DOE PAGES

Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.; ...

2016-09-09

During the summer 2013 Southern Aerosol and Oxidant Study (SOAS) field campaign in a rural site in the southeastern United States, the effect of hygroscopicity and composition on the phase state of atmospheric aerosol particles dominated by the organic fraction was studied. The analysis is based on hygroscopicity measurements by a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA), physical phase state investigations by an Aerosol Bounce Instrument (ABI) and composition measurements using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). To study the effect of atmospheric aging on these properties, an OH-radical oxidation flow reactor (OFR) was used to simulate longer atmosphericmore » aging times of up to 3 weeks. Hygroscopicity and bounce behavior of the particles had a clear relationship showing higher bounce at elevated relative humidity (RH) values for less hygroscopic particles, which agrees well with earlier laboratory studies. Additional OH oxidation of the aerosol particles in the OFR increased the O:C and the hygroscopicity resulting in liquefying of the particles at lower RH values. At the highest OH exposures, the inorganic fraction starts to dominate the bounce process due to production of inorganics and concurrent loss of organics in the OFR. Our results indicate that at typical ambient RH and temperature, organic-dominated particles stay mostly liquid in the atmospheric conditions in the southeastern US, but they often turn semisolid when dried below ~50 % RH in the sampling inlets. Furthermore, while the liquid phase state suggests solution behavior and equilibrium partitioning for the SOA particles in ambient air, the possible phase change in the drying process highlights the importance of thoroughly considered sampling techniques of SOA particles.« less

Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US

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

Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.

During the summer 2013 Southern Aerosol and Oxidant Study (SOAS) field campaign in a rural site in the southeastern United States, the effect of hygroscopicity and composition on the phase state of atmospheric aerosol particles dominated by the organic fraction was studied. The analysis is based on hygroscopicity measurements by a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA), physical phase state investigations by an Aerosol Bounce Instrument (ABI) and composition measurements using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). To study the effect of atmospheric aging on these properties, an OH-radical oxidation flow reactor (OFR) was used to simulate longer atmosphericmore » aging times of up to 3 weeks. Hygroscopicity and bounce behavior of the particles had a clear relationship showing higher bounce at elevated relative humidity (RH) values for less hygroscopic particles, which agrees well with earlier laboratory studies. Additional OH oxidation of the aerosol particles in the OFR increased the O:C and the hygroscopicity resulting in liquefying of the particles at lower RH values. At the highest OH exposures, the inorganic fraction starts to dominate the bounce process due to production of inorganics and concurrent loss of organics in the OFR. Our results indicate that at typical ambient RH and temperature, organic-dominated particles stay mostly liquid in the atmospheric conditions in the southeastern US, but they often turn semisolid when dried below ~50 % RH in the sampling inlets. Furthermore, while the liquid phase state suggests solution behavior and equilibrium partitioning for the SOA particles in ambient air, the possible phase change in the drying process highlights the importance of thoroughly considered sampling techniques of SOA particles.« less

Utilisation of Rep-PCR to track microbes in aerosols collected adjacent to their source, a saline lake in Victoria, Australia.

PubMed

Munday, Chris I; O'Loingsigh, Tadhg; Tapper, Nigel J; De Deckker, Patrick; Allison, Gwen E

2013-04-15

Dust storms are a major source of aerosolized bacteria, especially in the drought conditions experienced in Australia in the decade to 2009. The major aims of this project were to identify the culturable bacteria in environmental samples and to genetically fingerprint all isolates using repetitive element PCR (Rep-PCR) to investigate the possibility of tracking isolates from their source into the atmosphere. Four field trips were conducted to a dry lake in western Victoria, Australia to sample aerosols and sediments. Aerosols were collected at heights up to 150 m using vacuum pumps with filters attached to a tethered helium balloon, while corresponding sediments were collected in sterile polypropylene tubes. Isolates were cultivated on Tryptic Soy Agar, R2 Agar and Marine Agar, and grown in dark conditions at ambient temperature. By sequencing the 16S rRNA gene of 270 isolates, fifteen different bacterial families were identified, with both the aerosols and sediments dominated by the Bacillaceae family. Four sets of Rep-PCR primers were tested, with the ERIC and (GTG)5 primers proving to be the most suitable for fingerprinting the cultured taxa. Rep-PCR revealed very high strain diversity in the samples collected, however some strains were still able to be tracked from sediments up to 150 m in height. This shows the potential of Rep-PCR, however very large reference databases would be required for the technique to be more useful. Copyright © 2013 Elsevier B.V. All rights reserved.

Chemical characterization of ambient aerosol collected during the southwest monsoon and intermonsoon seasons over the Arabian Sea: Labile-Fe(II) and other trace metals

NASA Astrophysics Data System (ADS)

Siefert, Ronald L.; Johansen, Anne M.; Hoffmann, Michael R.

1999-02-01

Atmospheric deposition of iron (Fe) to certain regions of the oceans is an important nutrient source of Fe to the biota, and the ability of the biota to uptake Fe is dependent on the speciation of the Fe. Therefore understanding the speciation of Fe in the atmosphere is critical to understanding the role of Fe as a nutrient source in surface ocean waters. Labile ferrous iron (Fe(II)) concentrations as well as total concentrations for Fe and other important trace metals, cations, and anions were determined over the Arabian Sea for two nonconsecutive months during 1995. Ambient aerosol samples were collected during the Indian Ocean intermonsoon and southwest monsoon seasons over the Arabian Sea. Sampling took place aboard the German research vessel Meteor in the months of May (leg M32/3; intermonsoon) and July/August (leg M32/5; southwest monsoon). Both cruise tracks followed the 65th east meridian, traveling for 30 days each (from north to south during leg M32/3 and from south to north during leg M32/5). A high-volume dichotomous virtual impactor with an aerodynamic cutoff size of 3 μm was used to collect the fine and coarse aerosol fractions for metal analysis. A low volume collector was used to collect aerosol samples for anion and cation analysis. The analysis for labile-Fe(II) was done immediately after sample collection to minimize any possible Fe redox reactions which might occur during sample storage. The analytical procedure involved filter extraction in a formate/formic acid buffered solution at pH 4.2 followed by colorimetric quantification of soluble Fe(II). Metals, anions, and cations were analyzed after the cruise. Total atmospheric aqueous-labile-Fe(II) concentrations during the intermonsoon were between 4.75 and <0.4 ng m-3, of which most (>80%) was present in the fine fraction (<3.0 μm). During the southwest monsoon, atmospheric aqueous-labile-Fe(II) concentrations were consistently below the detection limit (<0.34 to <0.089 ng m-3, depending on

The ambient aerosol characterization during the prescribed bushfire season in Brisbane 2013.

PubMed

Milic, A; Miljevic, B; Alroe, J; Mallet, M; Canonaco, F; Prevot, A S H; Ristovski, Z D

2016-08-01

Prescribed burnings are conducted in Queensland each year from August until November aiming to decrease the impact of bushfire hazards and maintain the health of vegetation. This study reports chemical characteristics of the ambient aerosol, with a focus on source apportionment of the organic aerosol (OA) fraction, during the prescribed biomass burning (BB) season in Brisbane 2013. All measurements were conducted within the International Laboratory for Air Quality and Health (ILAQH) located in Brisbane's Central Business District. Chemical composition, degree of ageing and the influence of BB emission on the air quality of central Brisbane were characterized using a compact Time of Flight Aerosol Mass Spectrometer (cToF-AMS). AMS loadings were dominated by OA (64%), followed by, sulfate (17%), ammonium (14%) and nitrates (5%). Source apportionment was applied on the AMS OA mass spectra via the multilinear engine solver (ME-2) implementation within the recently developed Source Finder (SoFi) interface. Six factors were extracted including hydrocarbon-like OA (HOA), cooking-related OA (COA), biomass burning OA (BBOA), low-volatility oxygenated OA (LV-OOA), semivolatile oxygenated OA (SV-OOA), and nitrogen-enriched OA (NOA). The aerosol fraction that was attributed to BB factor was 9%, on average over the sampling period. The high proportion of oxygenated OA (72%), typically representing aged emissions, could possess a fraction of oxygenated species transfored from BB components on their way to the sampling site. Copyright © 2016 Elsevier B.V. All rights reserved.

High-Resolution Electrospray Ionization Mass Spectrometry Analysis of Water- Soluble Organic Aerosols Collected with a Particle into Liquid Sampler

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

Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia

2010-10-01

This work demonstrates the utility of a particle-into-liquid sampler (PILS) a technique traditionally used for identification of inorganic ions present in ambient or laboratory aerosols for the analysis of water soluble organic aerosol (OA) using high resolution electrospray ionization mass spectrometry (HR ESI-MS). Secondary organic aerosol (SOA) was produced from 0.5 ppm mixing ratios of limonene and ozone in a 5 m3 Teflon chamber. SOA was collected simultaneously using a traditional filter sampler and a PILS. The filter samples were later extracted with either water or acetonitrile, while the aqueous PILS samples were analyzed directly. In terms of peak intensities,more » types of detectable compounds, average O:C ratios, and organic mass to organic carbon ratios, the resulting high resolution mass spectra were essentially identical for the PILS and filter based samples. SOA compounds extracted from both filter/acetonitrile extraction and PILS/water extraction accounted for >95% of the total ion current in ESI mass spectra. This similarity was attributed to high solubility of limonene SOA in water. In contrast, significant differences in detected ions and peak abundances were observed for pine needle biomass burning organic aerosol (BBOA) collected with PILS and filter sampling. The water soluble fraction of BBOA is considerably smaller than for SOA, and a number of unique peaks were detectable only by the filter/acetonitrile method. The combination of PILS collection with HR-ESI-MS analysis offers a new approach for molecular analysis of the water-soluble organic fraction in biogenic SOA, aged photochemical smog, and BBOA.« less

Determinants of the Associations between Ambient Concentrations and Personal Exposures to Ambient PM2.5, NO2, and O3 during DEARS

EPA Science Inventory

In this analysis, ambient concentrations and personal exposures to PM2.5, O3, and NO2, air exchange rates, meteorological parameters, and questionnaire survey responses collected during the Detroit Exposure and Aerosol Research Study (DEARS) are used: 1) to evaluate different met...

A continuous sampler with background suppression for monitoring alpha-emitting aerosol particles.

PubMed

McFarland, A R; Rodgers, J C; Ortiz, C A; Moore, M E

1992-05-01

A continuous air monitor has been developed that includes provisions for improving the detection of alpha-emitting aerosol particles in the presence of radon/thoron progeny that are unattached to ambient aerosol particles. Wind tunnel tests show that 80% of 10-microns aerodynamic equivalent diameter particles penetrate the flow system from the ambient air to the collection filter when the flow rate is 57 L min-1 (2 cfm) and the wind speed is 1 m s-1. Uniformity of aerosol collection on the filter, as characterized by the coefficient of variation of the areal density deposits, is less than 15% for 10-microns aerodynamic-equivalent-diameter aerosol particles. Tests with unattached radon daughters in a flow-through chamber showed that approximately 99% of the 218Po was removed by an inlet screen that is designed to collect radon daughters that are in the size range of molecular clusters. The inlet screen offers the opportunity to improve the signal-to-noise ratio of energy spectra in the regions of interest (subranges of the energy spectrum) of transuranic elements and thereby enhance the performance of background compensation algorithms.

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

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

Recent Rainfall and Aerosol Chemistry From Bermuda

NASA Astrophysics Data System (ADS)

Landing, W. M.; Shelley, R.; Kadko, D. C.

2014-12-01

This project was devoted to testing the use of Be-7 as a tracer for quantifying trace element fluxes from the atmosphere to the oceans. Rainfall and aerosol samples were collected between June 15, 2011 and July 27, 2013 at the Bermuda Institute of Ocean Sciences (BIOS) located near the eastern end of the island of Bermuda. Collectors were situated near ground level, clear of surrounding vegetation, at a meteorological monitoring station in front of the BIOS laboratory, about 10 m above sea level. This is a Bermuda Air Quality Program site used for ambient air quality monitoring. To quantify the atmospheric deposition of Be-7, plastic buckets were deployed for collection of fallout over ~3 week periods. Wet deposition was collected for trace element analysis using a specially modified "GEOTRACES" N-CON automated wet deposition collector. Aerosol samples were collected with a Tisch TE-5170V-BL high volume aerosol sampler, modified to collect 12 replicate samples on acid-washed 47mm diameter Whatman-41 filters, using procedures identical to those used for the US GEOTRACES aerosol program (Morton et al., 2013). Aerosol and rainfall samples were analyzed for total Na, Mg, Al, P, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Rb, Sr, Zr, Cd, Sb, Ba, La, Ce, Nd, Pb, Th, and U using ICPMS. Confirming earlier data from Bermuda, strong seasonality in rainfall and aerosol loading and chemistry was observed, particularly for aerosol and rainfall Fe concentrations when Saharan dust arrives in July/August with SE trajectories.

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Reactions and mass spectra of complex particles using Aerosol CIMS

NASA Astrophysics Data System (ADS)

Hearn, John D.; Smith, Geoffrey D.

2006-12-01

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

Chromatography related performance of the Monitor for Aerosols and Gases in Ambient Air (MARGA): laboratory and field based evaluation

EPA Science Inventory

Evaluation of the semi-continuous Monitor for Aerosols and Gases in Ambient Air (MARGA, Metrohm Applikon B.V.) was conducted with an emphasis on examination of accuracy and precision associated with processing of chromatograms. Using laboratory standards and atmospheric measureme...

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

NASA Technical Reports Server (NTRS)

Mazurek, Monica A.; Cofer, Wesley R., III; Levine, Joel S.

1991-01-01

During the boreal forest burn studied, the ambient concentrations for the particle carbon smoke aerosol are highest for the full-fire burn conditions and vary significantly throughout the burn. Collection strategies must accordingly define ranges in the smoke aerosol concentrations produced. While the highest elemental C concentrations are observed during full-fire conditions, the great majority of smoke aerosol particles are in the form of organic C particles irrespective of fire temperature. The formation of organic C light-scattering particles was a significant process in the burn studied.

Aerosol collection of the (Bladewerx Corporation) breathing zone monitor and portable workplace monitor.

PubMed

Moore, Murray E; Kennedy, Trevor J; Dimmerling, Paul J

2007-11-01

The Radiation Protection Group at the Los Alamos National Laboratory has a wind tunnel capable of measuring the aerosol collection efficiencies of air sampling devices. In the fall of 2005, the group received an internal Los Alamos request to perform aerosol collection efficiency tests on two air samplers manufactured by the Bladewerx Corporation (Rio Rancho, NM). This paper presents the results from tests performed in the wind tunnel facility at a test velocity of 0.5 m s. The SabreAlert (Portable Workplace Monitor) and the SabreBZM (Breathing Zone Monitor) are both designed to detect and measure the presence of alpha emitting isotopes in atmospheres. The SabreAlert was operated at two test air flow rates of 6 and 45 liters per minute (LPM), and the SabreBZM was operated at two test air flow rates of 3 and 19 LPM. The aerosol collection efficiencies of both samplers were evaluated with oleic acid (monodisperse) liquid droplet aerosols tagged with sodium fluorescein tracer. These test aerosols varied in size from about 2.3 to 17.2 microns (aerodynamic equivalent diameter). The SabreAlert was roughly 100% efficient in aerosol collection at a flow rate of 6 LPM, and had an aerodynamic cutpoint diameter of 11.3 microns at the 45 LPM flow rate. The SabreBZM had an aerodynamic cutpoint diameter of 6.7 microns at the 3 LPM flow rate, but the SabreBZM aerosol collection efficiency never exceeded 13.6% at the 19 LPM test flow rate condition.

Characterization of ambient aerosol at a remote site and twin cities of Pakistan

NASA Astrophysics Data System (ADS)

Ghauri, B.; Lodhi, A.

The pollution controls have significantly decreased pollutant concentrations in the industrialized nations in the west while the concentrations are expected to grow in developing countries. In this study the concentrations of major ions i.e SO4 2 -, NO3 -, NO2 -, Cl- , NH4 + and trace metals i.e. Al, V, Cr, Mn, Cu, As, Se, Cd, Sb, Ba, Ti and Pb were determined in aerosols at a remote site of Northern Pakistan in July 1996. Later in May 1998, a comparative study of aerosols in two size fractions (bulk &PM10) at 14 sites enabled to understand the anomalous distribution of several constituents present in the ambient air of the twin cities, Islamabad / Rawalpindi 90 km from South East of earlier site. The suspended particulate matter concentrations (bulk and PM10) were 475 ug/m3, 175 ug/m3 respectively. For urban areas Pb, Cd, Zn and Ni are obviously contributed by steel and other allied industries besides vehicle's contribution of lead and cadmium. In Northern area concentrations of Al, K, Ca, and Fe exceeded 1000 ng/m3. The SO2 concentrations varied from 0.03 to 1.2 ppb. Mean SO4 2- and NO3 - concentrations were 5.2 ug/m3 and 3.6 ug/m3 respectively. Concentrations of Se, Ti, Pb, Cd, Sb, Zn and As in all aerosol samples were highly enriched relative to average crustal abundances indicating significant anthropogenic contributions. As the dominant flow pattern from the Arabian Sea through India (monsoon air pattern) this may transport pollution derived aerosol and moisture from distant sources in China or India. Key word index: Aerosol, trace metals , enrichment, anions, air pollution, Islamabad/Rawalpindi, remote site.

The MODIS Aerosol Algorithm: Critical Evaluation and Plans for Collection 6

NASA Technical Reports Server (NTRS)

Remer, Lorraine

2010-01-01

For ten years the MODIS aerosol algorithm has been applied to measured MODIS radiances to produce a continuous set of aerosol products, over land and ocean. The MODIS aerosol products are widely used by the scientific and applied science communities for variety of purposes that span operational air quality forecasting in estimates o[ clear-sky direct radiative effects over ocean and aerosol-cloud interactions. The products undergo continual evaluation, including self-consistency checks and comparisons with highly accurate ground-based instruments. The result of these evaluation exercises is a quantitative understanding of the strengths and weaknesses of the retrieval, where and when the products are accurate and the situations where and when accuracy degrades. We intend 10 present results of the most recent critical evaluations including the first comparison of the over ocean products against the shipboard aerosol optical depth measurements of the Marine Aerosol Network (MAN), the demonstration of the lack of sensitivity to size parameter in the over land products and identification of residual problems and regional issues. While the current data set is undergoing evaluation, we are preparing for the next data processing, labeled Collection 6. Collection 6 will include transparent Quality Flags, a 3 km aerosol product and the 500m resolution cloud mask used within the aerosol n:bicvu|. These new products and adjustments to algorithm assumptions should provide users with more options and greater control, as they adapt the product for their own purposes.

Radiative absorption enhancement from coatings on black carbon aerosols.

PubMed

Cui, Xinjuan; Wang, Xinfeng; Yang, Lingxiao; Chen, Bing; Chen, Jianmin; Andersson, August; Gustafsson, Örjan

2016-05-01

The radiative absorption enhancement of ambient black carbon (BC), by light-refractive coatings of atmospheric aerosols, constitutes a large uncertainty in estimates of climate forcing. The direct measurements of radiative absorption enhancement require the experimentally-removing the coating materials in ambient BC-containing aerosols, which remains a challenge. Here, the absorption enhancement of the BC core by non-absorbing aerosol coatings was quantified using a two-step removal of both inorganic and organic matter coatings of ambient aerosols. The mass absorption cross-section (MAC) of decoated/pure atmospheric BC aerosols of 4.4±0.8m(2)g(-1) was enhanced to 9.6±1.8m(2)g(-1) at 678-nm wavelength for ambiently-coated BC aerosols at a rural Northern China site. The enhancement of MAC (EMAC) rises from 1.4±0.3 in fresh combustion emissions to ~3 for aged ambient China aerosols. The three-week high-intensity campaign observed an average EMAC of 2.25±0.55, and sulfates were primary drivers of the enhanced BC absorption. Copyright © 2016 Elsevier B.V. All rights reserved.

Real-time characterization of particle-bound polycyclic aromatic hydrocarbons in ambient aerosols and from motor-vehicle exhaust

NASA Astrophysics Data System (ADS)

Polidori, A.; Hu, S.; Biswas, S.; Delfino, R. J.; Sioutas, C.

2007-12-01

A photo-electric aerosol sensor, a diffusion charger, an Aethalometer, and a continuous particle counter were used along with other real-time instruments to characterize the particle-bound polycyclic aromatic hydrocarbon (p-PAH) content, and the physical/chemical characteristics of aerosols collected a) in Wilmington (CA) near the Los Angeles port and close to 2 major freeways, and b) at a dynamometer testing facility in downtown Los Angeles (CA), where 3 diesel trucks were tested. In Wilmington, the p-PAH, surface area, particle number, and "black" carbon concentrations were 4-8 times higher at 09:00-11:00 a.m. than between 17:00 and 18:00 p.m., suggesting that during rush hour traffic people living in that area are exposed to a higher number of diesel combustion particles enriched in p-PAH coatings. Dynamometer tests revealed that the p-PAH emissions from the "baseline" truck (no catalytic converted) were up to 200 times higher than those from the 2 vehicles equipped with advanced emission control technologies, and increased when the truck was accelerating. In Wilmington, integrated filter samples were collected and analyzed to determine the concentrations of the most abundant p-PAHs. A correlation between the total p-PAH concentration (μg/m3) and the measured photo-electric aerosol sensor signal (fA) was also established. Estimated ambient p-PAH concentrations (Average = 0.64 ng/m3; Standard deviation = 0.46 ng/m3) were in good agreement with those reported in previous studies conducted in Los Angeles during a similar time period. Finally, we calculated the approximate theoretical lifetime (70 years per 24-h/day) lung-cancer risk in the Wilmington area due to inhalation of multi-component p-PAHs and "black" carbon. Our results indicate that the lung-cancer risk is highest during rush hour traffic and lowest in the afternoon, and that the genotoxic risk of the considered p-PAHs does not seem to contribute to a significant part of the total lung-cancer risk

Real-time characterization of particle-bound polycyclic aromatic hydrocarbons in ambient aerosols and from motor-vehicle exhaust

NASA Astrophysics Data System (ADS)

Polidori, A.; Hu, S.; Biswas, S.; Delfino, R. J.; Sioutas, C.

2008-03-01

A photo-electric aerosol sensor, a diffusion charger, an Aethalometer, and a continuous particle counter were used along with other real-time instruments to characterize the particle-bound polycyclic aromatic hydrocarbon (p-PAH) content, and the physical/chemical characteristics of aerosols collected a) in Wilmington (CA) near the Los Angeles port and close to 2 major freeways, and b) at a dynamometer testing facility in downtown Los Angeles (CA), where 3 diesel trucks were tested. In Wilmington, the p-PAH, surface area, particle number, and "black" carbon concentrations were 4-8 times higher at 09:00-11:00 a.m. than between 17:00 and 18:00 p.m., suggesting that during rush hour traffic people living in that area are exposed to a higher number of diesel combustion particles enriched in p-PAH coatings. Dynamometer tests revealed that the p-PAH emissions from the "baseline" truck (no catalytic converter) were up to 200 times higher than those from the 2 vehicles equipped with advanced emission control technologies, and increased when the truck was accelerating. In Wilmington, integrated filter samples were collected and analyzed to determine the concentrations of the most abundant p-PAHs. A correlation between the total p-PAH concentration (μg/m3) and the measured photo-electric aerosol sensor signal (fA) was also established. Estimated ambient p-PAH concentrations (Average=0.64 ng/m3; Standard deviation=0.46 ng/m3 were in good agreement with those reported in previous studies conducted in Los Angeles during a similar time period. Finally, we calculated the approximate theoretical lifetime (70 years per 24-h/day) lung-cancer risk in the Wilmington area due to inhalation of multi-component p-PAHs and "black" carbon. Our results indicate that the lung-cancer risk is highest during rush hour traffic and lowest in the afternoon, and that the genotoxic risk of the considered p-PAHs does not seem to contribute to a significant part of the total lung-cancer risk

Linking Aerosol Optical Properties Between Laboratory, Field, and Model Studies

NASA Astrophysics Data System (ADS)

Murphy, S. M.; Pokhrel, R. P.; Foster, K. A.; Brown, H.; Liu, X.

2017-12-01

The optical properties of aerosol emissions from biomass burning have a significant impact on the Earth's radiative balance. Based on measurements made during the Fourth Fire Lab in Missoula Experiment, our group published a series of parameterizations that related optical properties (single scattering albedo and absorption due to brown carbon at multiple wavelengths) to the elemental to total carbon ratio of aerosols emitted from biomass burning. In this presentation, the ability of these parameterizations to simulate the optical properties of ambient aerosol is assessed using observations collected in 2017 from our mobile laboratory chasing wildfires in the Western United States. The ambient data includes measurements of multi-wavelength absorption, scattering, and extinction, size distribution, chemical composition, and volatility. In addition to testing the laboratory parameterizations, this combination of measurements allows us to assess the ability of core-shell Mie Theory to replicate observations and to assess the impact of brown carbon and mixing state on optical properties. Finally, both laboratory and ambient data are compared to the optical properties generated by a prominent climate model (Community Earth System Model (CESM) coupled with the Community Atmosphere Model (CAM 5)). The discrepancies between lab observations, ambient observations and model output will be discussed.

Local emission of primary air pollutants and its contribution to wet deposition and concentrations of aerosols and gases in ambient air in Japan

NASA Astrophysics Data System (ADS)

Aikawa, Masahide; Hiraki, Takatoshi; Tomoyose, Nobutaka; Ohizumi, Tsuyoshi; Noguchi, Izumi; Murano, Kentaro; Mukai, Hitoshi

2013-11-01

We studied wet deposition by precipitation and the concentrations of aerosols and gases in ambient air in relation to the primary air pollutants discharged from domestic areas. The concentrations of aerosols and gases were influenced by nearby emissions except for non-sea-salt SO, which is transported long distances. The area facing the Sea of Japan showed much larger wet deposition than other areas, although the domestic emissions of the primary air pollutants there were small and showed a peak in wet deposition from October to March, as distinct from April to September in other areas. We performed the correlation analyses between wet deposition of each component and the product of the concentrations of corresponding aerosols and gases in ambient air and the two-thirds power of the precipitation. From the results, following scavenging processes were suggested. • Sulfate and ammonium were scavenged in precipitation as particulate matter such as (NH4)2SO4 and NH4HSO4. • Nitrate was scavenged mainly in precipitation through gaseous HNO3. • Ammonium was complementarily scavenged in precipitation through aerosols such as (NH4)2SO4 and NH4HSO4 and through gaseous NH3.

Ambient Tropospheric Particles

EPA Science Inventory

Atmospheric particulate matter (PM) is a complex mixture of solid and liquid particles suspended in ambient air (also known as the atmospheric aerosol). Ambient PM arises from a wide-range of sources and/or processes, and consists of particles of different shapes, sizes, and com...

An automated baseline correction protocol for infrared spectra of atmospheric aerosols collected on polytetrafluoroethylene (Teflon) filters

NASA Astrophysics Data System (ADS)

Kuzmiakova, Adele; Dillner, Ann M.; Takahama, Satoshi

2016-06-01

A growing body of research on statistical applications for characterization of atmospheric aerosol Fourier transform infrared (FT-IR) samples collected on polytetrafluoroethylene (PTFE) filters (e.g., Russell et al., 2011; Ruthenburg et al., 2014) and a rising interest in analyzing FT-IR samples collected by air quality monitoring networks call for an automated PTFE baseline correction solution. The existing polynomial technique (Takahama et al., 2013) is not scalable to a project with a large number of aerosol samples because it contains many parameters and requires expert intervention. Therefore, the question of how to develop an automated method for baseline correcting hundreds to thousands of ambient aerosol spectra given the variability in both environmental mixture composition and PTFE baselines remains. This study approaches the question by detailing the statistical protocol, which allows for the precise definition of analyte and background subregions, applies nonparametric smoothing splines to reproduce sample-specific PTFE variations, and integrates performance metrics from atmospheric aerosol and blank samples alike in the smoothing parameter selection. Referencing 794 atmospheric aerosol samples from seven Interagency Monitoring of PROtected Visual Environment (IMPROVE) sites collected during 2011, we start by identifying key FT-IR signal characteristics, such as non-negative absorbance or analyte segment transformation, to capture sample-specific transitions between background and analyte. While referring to qualitative properties of PTFE background, the goal of smoothing splines interpolation is to learn the baseline structure in the background region to predict the baseline structure in the analyte region. We then validate the model by comparing smoothing splines baseline-corrected spectra with uncorrected and polynomial baseline (PB)-corrected equivalents via three statistical applications: (1) clustering analysis, (2) functional group quantification

Validation of MODIS Dust Aerosol Retrieval and Development Ambient Dust Phase Function using PRIDE Data

NASA Technical Reports Server (NTRS)

Remer, Lorraine A.; Lau, William (Technical Monitor)

2002-01-01

The PRIDE data set of MODIS aerosol retrievals co-located with sunphotometer measurements provides the basis of MODIS validation in a dust environment. The sunphotometer measurements include AERONET automatic instruments, land-based Microtops instruments, ship-board Microtops instruments and the AATS-6 aboard the Navajo aircraft. Analysis of these data indicate that the MODIS retrieval is within pre-launch estimates of uncertainty within the spectral range of 600-900 nm. However, the MODIS algorithm consistently retrieves smaller particles than reality thus leading to incorrect spectral response outside of the 600-900 nm range and improper size information. Further analysis of MODIS retrievals in other dust environments shows the inconsistencies are due to nonspherical effects in the phase function. These data are used to develop an ambient phase function for dust aerosol to be used for remote sensing purposes.

76 FR 60020 - Agency Information Collection Activities: Proposed Collection; Comment Request; Ambient Air...

Federal Register 2010, 2011, 2012, 2013, 2014

2011-09-28

... ENVIRONMENTAL PROTECTION AGENCY [EPA-HQ-OAR-2002-0091, FRL-9472-8] Agency Information Collection Activities: Proposed Collection; Comment Request; Ambient Air Quality Surveillance AGENCY: Environmental... . Fax: (202) 566-1741. Mail: Environmental Protection Agency, EPA Docket Center (EPA/DC), Air and...

Chemical characterization of ambient aerosol collected during the southwest monsoon and intermonsoon seasons over the Arabian Sea: Anions and cations

NASA Astrophysics Data System (ADS)

Johansen, Anne M.; Siefert, Ronald L.; Hoffmann, Michael R.

1999-11-01

Ambient aerosol samples were collected over the northern Indian Ocean during two 1 month-long research cruises (German R/V Meteor) that took place during the intermonsoon (May) and SW monsoon (July/August) of 1995. A high volume and two small volume collectors were used to collect samples, which were subsequently analyzed for ferrous iron, 32 elements, and anions and cations. The present paper focuses on the bulk aerosol material, the ions, while utilizing some of the trace metal data that were presented in more detail in our previous paper [Siefert et al., 1999]. Data are analyzed and interpreted with the aid of principal component and multiple linear regression analyses. Intermonsoon samples were strongly influenced by continental material, both of crustal and anthropogenic origin. The crustal component (24.5±13% of the total suspended particulate mass (TSP), 6.0±4.4 μg m-3) contained 3.2% gypsum (CaSO4). While more than half of the TSP (21.2±9.6 μg m-3) during the SW monsoon was sea-salt-derived due to the strong winds prevailing during this season, only 1.7±1.1% (0.7±0.4 μg m-3) was found to be of crustal origin. Sulfate (SO42-) sources were determined and quantified with linear regression analyses utilizing specific tracers for the independent variables. Lead (Pb) was found to be a more reliable surrogate for anthropogenic SO42- compared to nitrate (NO3-) during the relatively polluted intermonsoon. Soluble calcium (Ca2+) served as the tracer for gypsum, and methane sulfonate (MSA) served as the tracer for biogenically derived SO42- during both seasons. On the basis of this analysis, 75% of the non-sea-salt sulfate (NSS-SO42-) (0.8±0.2 μg m-3, representing ˜2.4% of TSP) was found to be of biogenic origin during the SW monsoon with the remaining 25% of anthropogenic origin. During the intermonsoon, NSS-SO42- accounted for 2.1±1.2 μg m-3 (˜9.2% of TSP) and had a composition that was 65% anthropogenic, 21% biogenic, and 14% gypsum-derived. Linear

NASA's Aerosol Sampling Experiment Summary

NASA Technical Reports Server (NTRS)

Meyer, Marit E.

2016-01-01

In a spacecraft cabin environment, the size range of indoor aerosols is much larger and they persist longer than on Earth because they are not removed by gravitational settling. A previous aerosol experiment in 1991 documented that over 90 of the mass concentration of particles in the NASA Space Shuttle air were between 10 m and 100 m based on measurements with a multi-stage virtual impactor and a nephelometer (Liu et al. 1991). While the now-retired Space Shuttle had short duration missions (less than two weeks), the International Space Station (ISS) has been continually inhabited by astronauts for over a decade. High concentrations of inhalable particles on ISS are potentially responsible for crew complaints of respiratory and eye irritation and comments about 'dusty' air. Air filtration is the current control strategy for airborne particles on the ISS, and filtration modeling, performed for engineering and design validation of the air revitalization system in ISS, predicted that PM requirements would be met. However, aerosol monitoring has never been performed on the ISS to verify PM levels. A flight experiment is in preparation which will provide data on particulate matter in ISS ambient air. Particles will be collected with a thermophoretic sampler as well as with passive samplers which will extend the particle size range of sampling. Samples will be returned to Earth for chemical and microscopic analyses, providing the first aerosol data for ISS ambient air.

Oxidative potential of ambient fine aerosol over a semi-urban site in the Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Patel, Anil; Rastogi, Neeraj

2018-02-01

Indo-Gangetic Plain (IGP) receives emissions from variety of pollutant sources such as post-harvest crop residue burning, vehicles, industries, power plants, and bio-fuel burning. Several studies have documented physical, chemical and optical properties of aerosol over the IGP; however, their oxidative potential (OP) has not yet documented. Present study reports the OP (measured through dithiothreitol (DTT) assay) of soluble particulate matter smaller than 2.5 μm aerodynamic diameter (PM2.5) over Patiala (30.3°N, 76.4°E, 249 m amsl), a semi-urban site located in the IGP, during winter 2014. Volume-normalized OP (range: 1.3-7.2 nmol DTT min-1 m-3, average: 3.8 ± 1.4, 1σ) is found to be ∼3 to 20 times higher, and mass-normalized OP (range: 13-50 pmol DTT min-1 μg-1, average: 27 ± 8, 1σ) is found to be similar or higher than those documented in literature. Further, observed OP is found to depend more on PM2.5 composition rather than mass concentration. Mass fractions of organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon (WSOC) correlate positively whereas that of secondary inorganic aerosol (SIA, sum of the concentrations of SO42-, NO3- and NH4+) correlate negatively with OP μg-1 at considerable significance level (p < 0.05). Negative correlation of SIA with OP μg-1 has been assessed in laboratory experiment and attributed to their DTT inactive nature. It is suggested to use WSOC/SIA ratio as a measure of DTT activity of secondary particles over the study region. Further, biomass burning derived species are observed to be more DTT active than those derived from fossil fuel burning. It was also observed that the slope of OP μg-1 and WSOC/SIA ratio linear relationship enhances significantly in samples collected during days following foggy nights in comparison to that in samples collected during non-foggy period, which may be due to the production of redox-active species by fog processing. Such studies have implications in assessing

Ergosterol, arabitol and manitol as tracers for biological aerosols

NASA Astrophysics Data System (ADS)

Rudich, Y.; Burshtein, N.; Lang-Yona, N.

2010-12-01

Airborne fungi can cause a wide array of adverse responses in humans depending on the type and quantity present. Since dose and human response is highly individual, the sensitivity of a person exposed is also an important consideration. The abundance of bioaerosols in the ambient air and their health impacts depend on the season and on the environmental conditions. In order to quantify and identify fungi bioaerosols’ contribution to atmospheric aerosols and the impact to public health, it has been suggested to use chemicals that are typical of bioaerosols as biomarkers in chemical analysis of collected aerosols. An often used biomarker for determining the fungal biomass is ergosterol. Recently, Bauer et al. (2008) found that mannitol and arabitol concentrations are correlated with the fungal spore counts in atmospheric PM10. In this study, ergosterol, arabitol and mannitol were quantified in ambient aerosols collected in the Eastern Mediterranean region for 12 months in order to understand their annual and seasonal behavior and to test whether arabitol and mannitol are good predictors of fungi. Finally, correlations between ergosterol abundances with inorganic ions, humidity, temperature, and synoptic data in order to identify dominant sources of fungal spores were also studied. We will report on the measurements and the observed correlations between the different tracers.

Laboratory and field based evaluations of chromatography related performance of the Monitor for AeRosols and GAses in ambient Air (MARGA)

EPA Science Inventory

The semi-continuous Monitor for AeRosols and Gases in Ambient air (MARGA) was evaluated using laboratory and field data with a focus on chromatography. The performance and accuracy assessment revealed various errors and uncertainties resulting from mis-identification and mis-int...

Laboratory and field based evaluation of chromatography related performance of the Monitor for AeRosols and Gases in ambient Air (MARGA)

EPA Science Inventory

The semi-continuous Monitor for AeRosols and Gases in Ambient air (MARGA) was evaluated using laboratory and field data with a focus on chromatography. The performance and accuracy assessment revealed various errors and uncertainties resulting from mis-identification and mis-int...

Study on the surfactants present in atmospheric aerosols collected in the Okinawa Japan

NASA Astrophysics Data System (ADS)

Kamegawa, A.; Kasaba, T.; Shimabukuro, W.; Arakaki, T.

2017-12-01

The main constituent of atmospheric aerosols is organic substances, which occupy 20 to 70% of the mass. Organic matters in the aerosols contain organic acids, protein and humic acid, which behave similar to surfactants. Since surfactants contain both hydrophobic and hydrophilic functional groups in the molecule, they can play important roles in cloud formation and can affect climate change, but detailed mechanisms and magnitude are not well understood. In addition, surfactants can cause asthma, allergy, dry eye and so on. In this study, our aim is to characterize surfactants in the aerosols collected in different seasons in Okinawa, Japan. Atmospheric aerosols were collected at Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS) during Sep. 2013 and July 2014. Surfactants in the environment are comprised of artificially synthesized compounds and naturally derived organics so we only differentiate them into anionic and cationic surfactants. Colorimetric methods were used to determine the concentrations of anionic surfactants as methylene blue active substance (MBAS). Cationic surfactants were also measured by colorimetric method as disulfine blue active substance (DBAS) and showed always below detection limit. Thus, we only discuss anionic surfactants measured as MBAS. Water soluble organic carbon (WSOC) and metal concentrations were also measured for the same aerosol samples. Concentrations of MBAS in the studied samples were 2-3 times higher in spring, fall and winter than those collected in summer. MBAS concentration in the aerosols showed strong correlation with sulfate ion and WSOC, and slightly weaker correlation with nss-sulfate ion. Among the metals, only sodium ion showed a relatively strong correlation with MBAS concentrations. It is suggested that the anionic surfactants in the studied aerosols are mainly derived from marine sources.

AEROSOL CHEMICAL CHARACTERISTION ON BOARD THE DOE G1 AIRCRAFT USING A PARTICLE INTO LIQUID SAMPLER DURING THE TEXAQS 2000 EXPERIMENT.

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

LEE,Y.N.; SONG,Z.; LIU,Y.

2001-01-13

Knowledge of aerosol chemical composition is key to understanding a number of properties of ambient aerosol particles including sources, size/number distribution, chemical evolution, optical properties and human health effects. Although filter based techniques have been widely used to determine aerosol chemical constituents, they generally cannot provide sufficiently fast time resolution needed to investigate sources and chemical evolution that effect aerosol chemical, size and number changes. In order to gain an ability to describe and predict the life cycles of ambient aerosols as a basis for ambient air quality control, fast and sensitive determination of the aerosol chemical composition must bemore » made available. To help to achieve this goal, we deployed a newly developed technique, referred to as PILS (particle-into-liquid-sampler), on the DOE G1 aircraft during the 2000 Texas Air Quality Study (TexAQS 2000) to characterize the major ionic species of aerosol particles with aerodynamic size smaller than 2.5 {micro}m (PM 2.5). The results obtained are examined in the context of other simultaneously collected data for insights into the measurement capability of the PILS system.« less

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

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

ß-CARYOPHYLLINIC ACID: AN ATMOSPHERIC TRACER FOR ß-CARYOPHYLLENE SECONDARY ORGANIC AEROSOL

EPA Science Inventory

The chemical compositions of ambient PM_2.5 samples, collected in Research Triangle Park, North Carolina, USA, and a sample of secondary organic aerosol, formed by irradiating a mixture of the sesquiterpene, ß-caryophyllene, and oxides of nitrogen in a smog chamber, wer...

Novel measurement technologies for ambient and combustion source aerosols

EPA Science Inventory

Thie presentaiton examines the chemical properties of atmospheric and combustion source aerosols. It describes the aerosol chemical fractions and the specific chemical constituents in these aerosols. The presentation will cover (i) the limitatins and benefits of hyphenated chroma...

Ambient Observations of the Soot Aging Process during the SHARP Intensive Field Campaign

NASA Astrophysics Data System (ADS)

Reed, C.; Collins, D. R.; Khalizov, A. F.; Zheng, J.; Zhang, R.

2009-12-01

Soot aerosols affect climate both directly through absorption of solar radiation and indirectly by potentially serving as cloud condensation nuclei. Among the sources of uncertainty surrounding the effects of soot aerosol on the environment is the lack of scientific insight into the soot aging process, in which soot particles develop a coating of secondary species such as sulfates, ammonium, nitrate, and organics. Such processes may alter the behavior of soot by modifying particle morphology over time leading to changes in chemical, physical and scattering properties of the aerosol. However, it is often difficult to quantify such processes in the ambient environment due to the complex composition and spatial and temporal variability of the atmospheric aerosol. In order to better understand the effects of the environment on soot particles, it is desirable to study the processes responsible for their transformation in the ambient air without influence from variability in source region and history prior to sampling. To achieve this, the overall soot aging process in the ambient environment was physically isolated utilizing environmental chambers. Chamber measurements were conducted on the Moody Tower at the University of Houston using The Ambient Aerosol Chamber for Evolution Studies (AACES) during the SHARP campaign. AACES is a roughly cubical chamber constructed of a rigid acrylic outer shell, which transmits UV radiation both in the UV-B and UV-A ranges. FEP Teflon lines the inside of the chamber on all sides and the top, while expanded-PTFE (ePTFE) Teflon is used on the bottom of the chamber. The fibrous structure of the ePTFE acts as a barrier to particulates, while allowing gas molecules to move virtually unimpeded from the surrounding air into the chamber, creating an environment inside the chamber that is initially free of particles and continuously mimics the local ambient air. In order to study the effects of the soot aging process, a non-premixed propane

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

NASA Astrophysics Data System (ADS)

Dzepina, K.; Mazzoleni, C.; Fialho, P.; China, S.; Zhang, B.; Owen, R. C.; Helmig, D.; Hueber, J.; Kumar, S.; Perlinger, J. A.; Kramer, L. J.; Dziobak, M. P.; Ampadu, M. T.; Olsen, S.; Wuebbles, D. J.; Mazzoleni, L. R.

2015-05-01

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m-3. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100-1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests

Estimate of biogenic VOC emissions in Japan and their effects on photochemical formation of ambient ozone and secondary organic aerosol

NASA Astrophysics Data System (ADS)

Chatani, Satoru; Matsunaga, Sou N.; Nakatsuka, Seiji

2015-11-01

A new gridded database has been developed to estimate the amount of isoprene, monoterpene, and sesquiterpene emitted from all the broadleaf and coniferous trees in Japan with the Model of Emissions of Gases and Aerosols from Nature (MEGAN). This database reflects the vegetation specific to Japan more accurately than existing ones. It estimates much lower isoprene emitted from other vegetation than trees, and higher sesquiterpene emissions mainly emitted from Cryptomeria japonica, which is the most abundant plant type in Japan. Changes in biogenic emissions result in the decrease in ambient ozone and increase in organic aerosol simulated by the air quality simulation over the Tokyo Metropolitan Area in Japan. Although newly estimated biogenic emissions contribute to a better model performance on overestimated ozone and underestimated organic aerosol, they are not a single solution to solve problems associated with the air quality simulation.

Comparison of two derivatization methods for the analysis of short chain fatty acids in the ambient aerosol using GC-MS

NASA Astrophysics Data System (ADS)

Kim, G.; Jeon, S.

2016-12-01

Fatty acids are one of the important compound classes in the polar organic fraction of ambient aerosols. Among them, short chain fatty acids play a significant role in the atmospheric transformation processes. For short-chain acids, the bottleneck of analysis has been the difficulty of sample preparation due to the high solubility and volatility. To overcome this problem, derivatization of polar organic fraction is widely used with silylation reagents to increase the resolution and sensitivity. Two different derivatization procedures; (1) using the tertbutyldimethylsilyl (TBDMS) derivatization and (2) the headspace-solid phase microextraction (HS-SPME) with in-fiber derivatization are compared using gas chromatography-mass spectrometry (GC-MS). At the second method, simultaneous derivatization and extraction were performed by a poly acrylate (PA) coated fiber doped with pyrenyldiazomethane (PDAM). We investigated the chromatographic property and relative sensitivities of each individual short chain acids according to two different derivatization procedures. For the method validation, the linearity, recovery and method detection limit (MDL) were compared. Also, two derivatization methods were applied to the ambient aerosol samples and evaluated with respect to the effectiveness.

SOURCE APPORTIONMENT OF PHOENIX PM2.5 AEROSOL WITH THE UNMIX RECEPTOR MODEL

EPA Science Inventory

The multivariate receptor model Unmix has been used to analyze a 3-yr PM2.5 ambient aerosol data set collected in Phoenix, AZ, beginning in 1995. The analysis generated source profiles and overall percentage source contribution estimates (SCE) for five source categories: ga...

A thermal desorption mass spectrometer for freshly nucleated secondary aerosol particles

NASA Astrophysics Data System (ADS)

Held, A.; Gonser, S. G.

2012-04-01

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

Geochemical, Sulfur Isotopic Characteristics and Source Contributions of Size-Aggregated Aerosols Collected in Baring Head, New Zealand.

NASA Astrophysics Data System (ADS)

Li, J.; Michalski, G. M.; Davy, P.; Harvey, M.; Wilkins, B. P.; Katzman, T. L.

2017-12-01

Sulfate aerosols are critical to the climate, human health, and the hydrological cycle in the atmosphere, yet the sources of sulfate in aerosols are not completely understood. In this work, we evaluated the sources of sulfate in size-aggregated aerosols from the Southern Pacific Ocean and the land of New Zealand using geochemical and isotopic analyses. Aerosols were collected at Baring Head, New Zealand between 6/30/15 to 8/4/16 using two collectors, one only collects Southern Pacific Ocean derived aerosols (open-ocean collector), the other collects aerosols from both the ocean and the land (all-direction collector). Each collector is equipped with two filters to sample size-aggregated aerosols (fine aerosols: <0.5 um and coarse aerosols: 0.5-10 um). Our results show that fine and coarse aerosols show distinctive sulfate sources: sulfate in fine aerosols is a mixture of sea-salt sulfate ( 30%) and Non-Sea-Salt sulfate (NSS-SO42-, 70%), while coarse aerosols are dominated by sea-salt sulfate. However, some NSS-SO42- was also observed in coarse aerosols collected in summer, suggesting the presence of accumulation mode NSS-SO42- aerosols, which is possibly due to high summer biogenic DMS flux. The sources of sulfur in NSS-SO42- could be further determined by their d34S values. DMS emission is likely the sole sulfur source in the open-ocean collector as it shows constant DMS-like d34S signatures (15-18‰) throughout the year. Meanwhile, the d34S of NSS-SO42- in the all-direction collector display a seasonal trend: summer time d34S values are higher and DMS-like (15-18‰), indicating DMS emission is the dominant sulfur source; winter time d34S values are lower ( 6-12‰), therefore the sulfur is likely sourced from both DMS emission and terrestrial S input with low d34S values, such as volcanic activities, fossil fuel and wood burning.

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

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

Dzepina, K.; Mazzoleni, C.; Fialho, P.

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3. On average, organic aerosol components represent the largest mass fraction of the totalmore » measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

DOE PAGES

Dzepina, K.; Mazzoleni, C.; Fialho, P.; ...

2015-05-05

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3. On average, organic aerosol components represent the largest mass fraction of the totalmore » measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species

Organic Components and Elemental Carbon in Soils and Ambient Particles near Phoenix, AZ

NASA Astrophysics Data System (ADS)

Fraser, M. P.; Jia, Y.; Clements, A.

2008-12-01

In the desert southwest, fugitive dust emissions contribute significantly to ambient aerosol concentrations. Wind erosion from the arid land is a primary contributor to ambient particulate matter (PM) concentrations but, in regions including Central Arizona, desert lands have been converted for agriculture use and thus agriculture processes constitute another contributor. As the metropolitan Phoenix region expands into these agricultural lands, urban sources and construction also contributes to the ambient PM load. In an effort to identify and access relative contribution of these and other major PM sources in the region, a series of ambient PM samples and soil samples were collected near Higley, AZ, a suburb of Phoenix which has seen rapid urbanization onto agricultural lands between January and May 2008. The soil samples collected were resuspended and samples of resuspended dust were collected to represent particles smaller than 2.5 microns and 10 microns in aerodynamic diameter (PM2.5 and PM10 respectively). The size segregated soil and ambient PM samples were analyzed for bulk mass, elemental and organic carbon content, and a number of specific compounds including ions, metals, alkanes, organic acids, polycyclic aromatic hydrocarbons, and saccharides. The saccharide contribution to soil organic carbon has been studied to elucidate key factors in the soil carbon balance and markers have been developed for tracing fungal metabolites, plant growth and budding and organic matter decay. Using organic markers, the contribution of various sources to PM10 and PM2.5 levels have been determined by positive matrix factorization (PMF) of the ambient aerosol marker concentrations quantified from PM samples. Subsequently, samples of local soil from native and agricultural fields and local roadways wers size- segregated and analyzed in an effort to create a source profile for the dust in the area. A chemical mass balance model has been used to compare with the PMF results

The Collection 6 'dark-target' MODIS Aerosol Products

NASA Technical Reports Server (NTRS)

Levy, Robert C.; Mattoo, Shana; Munchak, Leigh A.; Kleidman, Richard G.; Patadia, Falguni; Gupta, Pawan; Remer, Lorraine

2013-01-01

Aerosol retrieval algorithms are applied to Moderate resolution Imaging Spectroradiometer (MODIS) sensors on both Terra and Aqua, creating two streams of decade-plus aerosol information. Products of aerosol optical depth (AOD) and aerosol size are used for many applications, but the primary concern is that these global products are comprehensive and consistent enough for use in climate studies. One of our major customers is the international modeling comparison study known as AEROCOM, which relies on the MODIS data as a benchmark. In order to keep up with the needs of AEROCOM and other MODIS data users, while utilizing new science and tools, we have improved the algorithms and products. The code, and the associated products, will be known as Collection 6 (C6). While not a major overhaul from the previous Collection 5 (C5) version, there are enough changes that there are significant impacts to the products and their interpretation. In its entirety, the C6 algorithm is comprised of three sub-algorithms for retrieving aerosol properties over different surfaces: These include the dark-target DT algorithms to retrieve over (1) ocean and (2) vegetated-dark-soiled land, plus the (3) Deep Blue (DB) algorithm, originally developed to retrieve over desert-arid land. Focusing on the two DT algorithms, we have updated assumptions for central wavelengths, Rayleigh optical depths and gas (H2O, O3, CO2, etc.) absorption corrections, while relaxing the solar zenith angle limit (up to 84) to increase pole-ward coverage. For DT-land, we have updated the cloud mask to allow heavy smoke retrievals, fine-tuned the assignments for aerosol type as function of season location, corrected bugs in the Quality Assurance (QA) logic, and added diagnostic parameters such as topographic altitude. For DT-ocean, improvements include a revised cloud mask for thin-cirrus detection, inclusion of wind speed dependence in the retrieval, updates to logic of QA Confidence flag (QAC) assignment, and

Light-Absorbing Brown Carbon Aerosol Constituents from Combustion of Indonesian Peat and Biomass.

PubMed

Budisulistiorini, Sri Hapsari; Riva, Matthieu; Williams, Michael; Chen, Jing; Itoh, Masayuki; Surratt, Jason D; Kuwata, Mikinori

2017-04-18

Light-absorbing brown carbon (BrC) constituents of organic aerosol (OA) have been shown to significantly absorb ultraviolet (UV) and visible light and thus impact radiative forcing. However, molecular identification of the BrC constituents is still limited. In this study, we characterize BrC constituents at the molecular level in (i) aerosols emitted by combustion of peat, fern/leaf, and charcoal from Indonesia and (ii) ambient aerosols collected in Singapore during the 2015 haze episode. Aerosols were analyzed using ultra performance liquid chromatography instrument interfaced to a diode array detector and electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer operated in the negative ion mode. In the laboratory-generated aerosols, we identified 41 compounds that can potentially absorb near-UV and visible wavelengths, such as oxygenated-conjugated compounds, nitroaromatics, and S-containing compounds. The sum of BrC constituents in peat, fern/leaf, and charcoal burning aerosols are 16%, 35%, and 28% of the OA mass, respectively, giving an average contribution of 24%. On average, the BrC constituents account for 0.4% of the ambient OA mass; however, large uncertainties in mass closure remain because of the lack of authentic standards. This study highlights the potential of light-absorbing BrC OA constituents from peat, fern/leaf, and charcoal burning and their importance in the atmosphere.

78 FR 12052 - Agency Information Collection Activities: Proposed Collection; Comment Request; Ambient Air...

Federal Register 2010, 2011, 2012, 2013, 2014

2013-02-21

... pollution control agencies, and tribal entities which collect and report ambient air quality data for the..., documenting episodes and initiating episode controls, air quality trends assessment, and air pollution.... Although the state and local air pollution control agencies and tribal entities are responsible for the...

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

Sampling Indoor Aerosols on the International Space Station

NASA Technical Reports Server (NTRS)

Meyer, Marit E.

2016-01-01

In a spacecraft cabin environment, the size range of indoor aerosols is much larger and they persist longer than on Earth because they are not removed by gravitational settling. A previous aerosol experiment in 1991 documented that over 90 of the mass concentration of particles in the NASA Space Shuttle air were between 10 m and 100 m based on measurements with a multi-stage virtual impactor and a nephelometer (Liu et al. 1991). While the now-retired Space Shuttle had short duration missions (less than two weeks), the International Space Station (ISS) has been continually inhabited by astronauts for over a decade. High concentrations of inhalable particles on ISS are potentially responsible for crew complaints of respiratory and eye irritation and comments about 'dusty' air. Air filtration is the current control strategy for airborne particles on the ISS, and filtration modeling, performed for engineering and design validation of the air revitalization system in ISS, predicted that PM requirements would be met. However, aerosol monitoring has never been performed on the ISS to verify PM levels. A flight experiment is in preparation which will provide data on particulate matter in ISS ambient air. Particles will be collected with a thermophoretic sampler as well as with passive samplers which will extend the particle size range of sampling. Samples will be returned to Earth for chemical and microscopic analyses, providing the first aerosol data for ISS ambient air.

Chemical characteristics of ambient aerosols contributed by cooking process at Noorpur village near New Delhi

NASA Astrophysics Data System (ADS)

Singh, Sudha

Generally, industrial and transport sectors are considered as major contributors of air pollution but recently, biomass burning is also reported as a major source of atmospheric aerosols (1, 2) especially in the developing world where solid fuels such as dung cake, wood and crop residues are used in traditional cooking which are responsible for poor air quality, respiratory problems and radiative forcing etc .In India, most of the research has been focused on emission estimates from biomass burning and cooking. No effort has been made to understand the chemistry and sources of fine aerosols in rural areas during cooking hours. This study fills this knowledge gap and strengthens our understanding about abundance of various chemical constituents of atmospheric aerosols emitted during cooking hours.Aerosol samples were collected from village called Noorpur (28.470 N, 77.030 E) which lies near Delhi city. Sampling was carried out during August 2011-May 2012 by using handy sampler (Envirotech model APM 821) installed at the terrace of a building (~6m). The aerosol samples were collected on 8 hourly basis at a flow rate of 1 LPM. Water extracts of these filters were analyzed for major anions (F-, Cl-, NO3-, SO42-) and major cations (Na+, NH4+, K+, Ca2+ Mg2+) by ion chromatography (Metrohm 883 Basic IC Plus). During cooking period, the concentration of the major ions followed the order of Ca2+> SO42-> NO3-> Cl-> K+> NH4+> Mg2+> Na2+> F-. Among anion SO42 (5 µg/m3) showed highest value and in case of cations Ca2+ (7.32µg/m3) has highest value.

Chemical characterization of individual particles and residuals of cloud droplets and ice crystals collected on board research aircraft in the ISDAC 2008 study

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Brooks, S. D.; Moffet, R. C.; Glen, A.; Laskin, A.; Gilles, M. K.; Liu, P.; MacDonald, A. M.; Strapp, J. W.; McFarquhar, G. M.

2013-06-01

Ambient particles and the dry residuals of mixed-phase cloud droplets and ice crystals were collected during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) near Barrow, Alaska, in spring of 2008. The collected particles were analyzed using Computer Controlled Scanning Electron Microscopy with Energy Dispersive X-ray analysis and Scanning Transmission X-ray Microscopy coupled with Near Edge X-ray Absorption Fine Structure spectroscopy to identify physico-chemical properties that differentiate cloud-nucleating particles from the total aerosol population. A wide range of individually mixed components was identified in the ambient particles and residuals including organic carbon compounds, inorganics, carbonates, and black carbon. Our results show that cloud droplet residuals differ from the ambient particles in both size and composition, suggesting that both properties may impact the cloud-nucleating ability of aerosols in mixed-phase clouds. The percentage of residual particles which contained carbonates (47%) was almost four times higher than those in ambient samples. Residual populations were also enhanced in sea salt and black carbon and reduced in organic compounds relative to the ambient particles. Further, our measurements suggest that chemical processing of aerosols may improve their cloud-nucleating ability. Comparison of results for various time periods within ISDAC suggests that the number and composition of cloud-nucleating particles over Alaska can be influenced by episodic events bringing aerosols from both the local vicinity and as far away as Siberia.

Source characterization of ambient fine aerosol in Singapore during a haze episode in 2015

NASA Astrophysics Data System (ADS)

Hapsari Budisulistiorini, Sri; Riva, Matthieu; Williams, Michael; Miyakawa, Takuma; Komazaki, Yuichi; Chen, Jing; Surratt, Jason; Kuwata, Mikinori

2017-04-01

Recurring transboundary haze from Indonesia peatland fires in the previous decades has significantly elevated particulate matter (PM) concentration in Southeast Asia, particularly during the 2015 El Niño event. Previous studies have investigated chemical composition of particles emitted during haze episodes; however, they were limited to time-integrated samples and the number of identified compounds. Low time-resolution measurement results in co-variance of PM sources; therefore, higher time-resolution measurement is important in PM source apportionment. Between October 10-31, 2015, Aerodyne Time-of-Flight Aerosol Chemical Speciation Monitor (ToF-ACSM) was deployed for real-time chemical characterization of ambient submicron PM (NR-PM1) in Singapore. Simultaneously, PM2.5 filter samples were collected for molecular-level organic aerosol (OA) constituents, organic carbon (OC), elemental carbon (EC) and water-soluble OC (WSOC) analyses. OA constituents were quantified by gas chromatography interfaced to electron ionization mass spectrometry (GC/EI-MS) and ultra-performance liquid chromatography interfaced to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer operated in the negative ion mode (UPLC/(-)ESI-HR-Q-TOFMS). OA and SO42- are dominant components of the haze particles, accounting for ˜77% and ˜12% of the total NR-PM1 mass, respectively. OC/EC ratio of 4.8 might indicate formation of secondary OA (SOA) and aerosols from biomass burning, including those from peat burning. OA fraction from ToF-ACSM measurements was analyzed for source apportionment using a bilinear model through multi-linear engine algorithm (ME-2) in graphical user interface SoFi (Source Finder). Five OA factors were identified: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), peat burning OA (PBOA), low-volatility oxygenated OA (LV-OOA), and semi-volatile oxygenated OA (SV-OOA). The HOA factor shows a distinct diurnal profile peaking in the morning and

Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol.

PubMed

Vaden, Timothy D; Imre, Dan; Beránek, Josef; Shrivastava, Manish; Zelenyuk, Alla

2011-02-08

Field measurements of secondary organic aerosol (SOA) find significantly higher mass loads than predicted by models, sparking intense effort focused on finding additional SOA sources but leaving the fundamental assumptions used by models unchallenged. Current air-quality models use absorptive partitioning theory assuming SOA particles are liquid droplets, forming instantaneous reversible equilibrium with gas phase. Further, they ignore the effects of adsorption of spectator organic species during SOA formation on SOA properties and fate. Using accurate and highly sensitive experimental approach for studying evaporation kinetics of size-selected single SOA particles, we characterized room-temperature evaporation kinetics of laboratory-generated α-pinene SOA and ambient atmospheric SOA. We found that even when gas phase organics are removed, it takes ∼24 h for pure α-pinene SOA particles to evaporate 75% of their mass, which is in sharp contrast to the ∼10 min time scale predicted by current kinetic models. Adsorption of "spectator" organic vapors during SOA formation, and aging of these coated SOA particles, dramatically reduced the evaporation rate, and in some cases nearly stopped it. Ambient SOA was found to exhibit evaporation behavior very similar to that of laboratory-generated coated and aged SOA. For all cases studied in this work, SOA evaporation behavior is nearly size-independent and does not follow the evaporation kinetics of liquid droplets, in sharp contrast with model assumptions. The findings about SOA phase, evaporation rates, and the importance of spectator gases and aging all indicate that there is need to reformulate the way SOA formation and evaporation are treated by models.

Development of a double-layered ceramic filter for aerosol filtration at high-temperatures: the filter collection efficiency.

PubMed

de Freitas, Normanda L; Gonçalves, José A S; Innocentini, Murilo D M; Coury, José R

2006-08-25

The performance of double-layered ceramic filters for aerosol filtration at high temperatures was evaluated in this work. The filtering structure was composed of two layers: a thin granular membrane deposited on a reticulate ceramic support of high porosity. The goal was to minimize the high pressure drop inherent of granular structures, without decreasing their high collection efficiency for small particles. The reticulate support was developed using the technique of ceramic replication of polyurethane foam substrates of 45 and 75 pores per inch (ppi). The filtering membrane was prepared by depositing a thin layer of granular alumina-clay paste on one face of the support. Filters had their permeability and fractional collection efficiency analyzed for filtration of an airborne suspension of phosphatic rock in temperatures ranging from ambient to 700 degrees C. Results revealed that collection efficiency decreased with gas temperature and was enhanced with filtration time. Also, the support layer influenced the collection efficiency: the 75 ppi support was more effective than the 45 ppi. Particle collection efficiency dropped considerably for particles below 2 microm in diameter. The maximum collection occurred for particle diameters of approximately 3 microm, and decreased again for diameters between 4 and 8 microm. Such trend was successfully represented by the proposed correlation, which is based on the classical mechanisms acting on particle collection. Inertial impaction seems to be the predominant collection mechanism, with particle bouncing/re-entrainment acting as detachment mechanisms.

ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED PARTICLES FOR DIFFERENT DOSE METRICS: COMPARISON OF NUMBER, SURFACE AREA AND MASS DOSE OF TYPICAL AMBIENT BI-MODAL AEROSOLS

EPA Science Inventory

ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED PARTICLES FOR DIFFERENT DOSE METRICS: COMPARISON OF NUMBER, SURFACE AREA AND MASS DOSE OF TYPICAL AMBIENT BI-MODAL AEROSOLS.
Chong S. Kim, SC. Hu*, PA Jaques*, US EPA, National Health and Environmental Effects Research Laboratory, ...

Aerosol from Organic Nitrogen in the Southeast United States

EPA Science Inventory

Biogenic volatile organic compounds (BVOCs) contribute significantly to organic aerosol in the southeastern United States. During the Southern Oxidant and Aerosol Study (SOAS), a portion of ambient organic aerosol was attributed to isoprene oxidation and organic nitrogen from BVO...

PIXE Analysis of Aerosol and Soil Samples Collected in the Adirondack Mountains

NASA Astrophysics Data System (ADS)

Yoskowitz, Joshua; Ali, Salina; Nadareski, Benjamin; Labrake, Scott; Vineyard, Michael

2014-09-01

We have performed an elemental analysis of aerosol and soil samples collected at Piseco Lake in Upstate New York using proton induced X-ray emission spectroscopy (PIXE). This work is part of a systematic study of airborne pollution in the Adirondack Mountains. Of particular interest is the sulfur content that can contribute to acid rain, a well-documented problem in the Adirondacks. We used a nine-stage cascade impactor to collect the aerosol samples near Piseco Lake and distribute the particulate matter onto Kapton foils by particle size. The soil samples were also collected at Piseco Lake and pressed into cylindrical pellets for experimentation. PIXE analysis of the aerosol and soil samples were performed with 2.2-MeV proton beams from the 1.1-MV Pelletron accelerator in the Union College Ion-Beam Analysis Laboratory. There are higher concentrations of sulfur at smaller particle sizes (0.25-1 μm), suggesting that it could be suspended in the air for days and originate from sources very far away. Other elements with significant concentrations peak at larger particle sizes (1-4 μm) and are found in the soil samples, suggesting that these elements could originate in the soil. The PIXE analysis will be described and the resulting data will be presented.

Role of ammonium ion and transition metals in the formation of secondary organic aerosol and metallo-organic complex within fog processed ambient deliquescent submicron particles collected in central part of Indo-Gangetic Plain.

PubMed

Singh, Dharmendra Kumar; Gupta, Tarun

2017-08-01

In this study we observed the role of ammonium ion (NH 4 + ) and transition metals (Fe, Mn, Cr, and Cu) present in ambient submicron particles in stabilizing and enhancing the yield of water soluble organic carbon (WSOC). A good correlation of WSOC with transition metals and NH 4 + was found (R 2  = 0.87 and 0.71), respectively within foggy episode collected ambient PM 1 (particles having aerodynamic diameter ≤1.0 μm) suggesting plausibleness of alternate oxidation (primarily various carbonyls into their respective organic acids, esters and other derivatives.) and aging mechanisms. Molar concentration of ammonium ion was observed to be exceeded over and above to require in neutralizing the sulphate and nitrate which further hints its role in the neutralization, stabilization and enhancement of subset of WSOC such as water soluble organic acids. Transition metals were further apportioned using enrichment factor analysis. The source of Fe, Mn, and Cr was found to be crustal and Cu was tagged to anthropogenic origin. This study also described the plausible role of significant predictors (Fe and Cu) in the secondary organic aerosol (SOA) formation through effect of Fenton chemistry. Mass-to-charge ratio of identified oxalic acid from our published recent field study (carried out from same sampling location) was used for understanding the possible metallo-organic complex with Fe supports the substantial role of Fe in SOA formation in the deliquescent submicron particles facilitated by aqueous-phase chemistry. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2011-07-01

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

Using Satellite Aerosol Retrievals to Monitor Surface Particulate Air Quality

NASA Technical Reports Server (NTRS)

Levy, Robert C.; Remer, Lorraine A.; Kahn, Ralph A.; Chu, D. Allen; Mattoo, Shana; Holben, Brent N.; Schafer, Joel S.

2011-01-01

The MODIS and MISR aerosol products were designed nearly two decades ago for the purpose of climate applications. Since launch of Terra in 1999, these two sensors have provided global, quantitative information about column-integrated aerosol properties, including aerosol optical depth (AOD) and relative aerosol type parameters (such as Angstrom exponent). Although primarily designed for climate, the air quality (AQ) community quickly recognized that passive satellite products could be used for particulate air quality monitoring and forecasting. However, AOD and particulate matter (PM) concentrations have different units, and represent aerosol conditions in different layers of the atmosphere. Also, due to low visible contrast over brighter surface conditions, satellite-derived aerosol retrievals tend to have larger uncertainty in urban or populated regions. Nonetheless, the AQ community has made significant progress in relating column-integrated AOD at ambient relative humidity (RH) to surface PM concentrations at dried RH. Knowledge of aerosol optical and microphysical properties, ambient meteorological conditions, and especially vertical profile, are critical for physically relating AOD and PM. To make urban-scale maps of PM, we also must account for spatial variability. Since surface PM may vary on a finer spatial scale than the resolution of standard MODIS (10 km) and MISR (17km) products, we test higher-resolution versions of MODIS (3km) and MISR (1km research mode) retrievals. The recent (July 2011) DISCOVER-AQ campaign in the mid-Atlantic offers a comprehensive network of sun photometers (DRAGON) and other data that we use for validating the higher resolution satellite data. In the future, we expect that the wealth of aircraft and ground-based measurements, collected during DISCOVER-AQ, will help us quantitatively link remote sensed and ground-based measurements in the urban region.

Stable carbon and nitrogen isotopic compositions of ambient aerosols collected from Okinawa Island in the western North Pacific Rim, an outflow region of Asian dusts and pollutants

NASA Astrophysics Data System (ADS)

Kunwar, Bhagawati; Kawamura, Kimitaka; Zhu, Chunmao

2016-04-01

Stable carbon (δ13C) and nitrogen (δ15N) isotope ratios were measured for total carbon (TC) and nitrogen (TN), respectively, in aerosol (TSP) samples collected at Cape Hedo, Okinawa, an outflow region of Asian pollutants, during 2009-2010. The averaged δ13C and δ15N ratios are -22.2‰ and +12.5‰, respectively. The δ13C values are similar in both spring (-22.5‰) and winter (-22.5‰), suggesting the similar sources and/or source regions. We found that δ13C from Okinawa aerosols are ca. 2‰ higher than those reported from Chinese megacities probably due to photochemical aging of organic aerosols. A strong correlation (r = 0.81) was found between nss-Ca and TSP, suggesting that springtime aerosols are influenced from Asian dusts. However, carbonates in the Asian dusts were titrated with acidic species such as sulfuric acid and oxalic acid during atmospheric transport although two samples suggested the presence of remaining carbonate. No correlations were found between δ13C and tracer compounds (levoglucosan, elemental carbon, oxalic acid, and Na+). During winter and spring, coal burning is significant source in China. Based on isotopic mass balance, contribution of coal burning origin particles to total aerosol carbon was estimated as ca. 97% in winter, which is probably associated with the high emissions in China. Contribution of NO3- to TN was on average 45% whereas that of NH4+ was 18%. These results suggest that vehicular exhaust is an important source of TN in Okinawa aerosols. Concentration of water-soluble organic nitrogen (WSON) is higher in summer, suggesting that WSON is more emitted from the ocean in warmer season whereas inorganic nitrogen is more emitted in winter and spring from pollution sources in the Asian continent.

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

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

Cappa, Christopher D; Atkinson, Dean B

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

Heterogeneous reaction of peroxyacetic acid and hydrogen peroxide on ambient aerosol particles under dry and humid conditions: kinetics, mechanism and implications

NASA Astrophysics Data System (ADS)

Wu, Q. Q.; Huang, L. B.; Liang, H.; Zhao, Y.; Huang, D.; Chen, Z. M.

2015-06-01

Hydrogen peroxide (H2O2) and organic peroxides play important roles in the cycle of oxidants and the formation of secondary aerosols in the atmosphere. Recent field observations have suggested that the budget of peroxyacetic acid (PAA, CH3C(O)OOH) is potentially related to the aerosol phase processes, especially to secondary aerosol formation. Here, we present the first laboratory measurements of the uptake coefficient of gaseous PAA and H2O2 onto ambient fine particulate matter (PM2.5) as a function of relative humidity (RH) at 298 K. The results show that the PM2.5, which was collected in an urban area, can take up PAA and H2O2 at the uptake coefficient (γ) of 10-4, and both γPAA and γH2O2 increase with increasing RH. The value of γPAA at 90 % RH is 5.4 ± 1.9 times that at 3 % RH, whereas γH2O2 at 90 % RH is 2.4 ± 0.5 times that at 3 % RH, which suggests that PAA is more sensitive to the RH variation than H2O2 is. Considering the larger Henry's law constant of H2O2 than that of PAA, the smaller RH sensitivity of the H2O2 uptake coefficient suggests that the enhanced uptake of peroxide compounds on PM2.5 under humid conditions is dominated by chemical processes rather than dissolution. Considering that mineral dust is one of the main components of PM2.5 in Beijing, we also determined the uptake coefficients of gaseous PAA and H2O2 on authentic Asian Dust storm (ADS) and Arizona Test Dust (ATD) particles. Compared to ambient PM2.5, ADS shows a similar γ value and RH dependence in its uptake coefficient for PAA and H2O2, while ATD gives a negative dependence on RH. The present study indicates that, in addition to the mineral dust in PM2.5, other components (e.g., soluble inorganic salts) are also important to the uptake of peroxide compounds. When the heterogeneous reaction of PAA on PM2.5 is considered, its atmospheric lifetime is estimated to be 3.0 h on haze days and 7.1 h on non-haze days, values that are in good agreement with the field observations.

Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol

PubMed Central

Vaden, Timothy D.; Imre, Dan; Beránek, Josef; Shrivastava, Manish; Zelenyuk, Alla

2011-01-01

Field measurements of secondary organic aerosol (SOA) find significantly higher mass loads than predicted by models, sparking intense effort focused on finding additional SOA sources but leaving the fundamental assumptions used by models unchallenged. Current air-quality models use absorptive partitioning theory assuming SOA particles are liquid droplets, forming instantaneous reversible equilibrium with gas phase. Further, they ignore the effects of adsorption of spectator organic species during SOA formation on SOA properties and fate. Using accurate and highly sensitive experimental approach for studying evaporation kinetics of size-selected single SOA particles, we characterized room-temperature evaporation kinetics of laboratory-generated α-pinene SOA and ambient atmospheric SOA. We found that even when gas phase organics are removed, it takes ∼24 h for pure α-pinene SOA particles to evaporate 75% of their mass, which is in sharp contrast to the ∼10 min time scale predicted by current kinetic models. Adsorption of “spectator” organic vapors during SOA formation, and aging of these coated SOA particles, dramatically reduced the evaporation rate, and in some cases nearly stopped it. Ambient SOA was found to exhibit evaporation behavior very similar to that of laboratory-generated coated and aged SOA. For all cases studied in this work, SOA evaporation behavior is nearly size-independent and does not follow the evaporation kinetics of liquid droplets, in sharp contrast with model assumptions. The findings about SOA phase, evaporation rates, and the importance of spectator gases and aging all indicate that there is need to reformulate the way SOA formation and evaporation are treated by models. PMID:21262848

Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes

NASA Astrophysics Data System (ADS)

Bian, Qijing; Jathar, Shantanu H.; Kodros, John K.; Barsanti, Kelley C.; Hatch, Lindsay E.; May, Andrew A.; Kreidenweis, Sonia M.; Pierce, Jeffrey R.

2017-04-01

Secondary organic aerosol (SOA) has been shown to form in biomass-burning emissions in laboratory and field studies. However, there is significant variability among studies in mass enhancement, which could be due to differences in fuels, fire conditions, dilution, and/or limitations of laboratory experiments and observations. This study focuses on understanding processes affecting biomass-burning SOA formation in laboratory smog-chamber experiments and in ambient plumes. Vapor wall losses have been demonstrated to be an important factor that can suppress SOA formation in laboratory studies of traditional SOA precursors; however, impacts of vapor wall losses on biomass-burning SOA have not yet been investigated. We use an aerosol-microphysical model that includes representations of volatility and oxidation chemistry to estimate the influence of vapor wall loss on SOA formation observed in the FLAME III smog-chamber studies. Our simulations with base-case assumptions for chemistry and wall loss predict a mean OA mass enhancement (the ratio of final to initial OA mass, corrected for particle-phase wall losses) of 1.8 across all experiments when vapor wall losses are modeled, roughly matching the mean observed enhancement during FLAME III. The mean OA enhancement increases to over 3 when vapor wall losses are turned off, implying that vapor wall losses reduce the apparent SOA formation. We find that this decrease in the apparent SOA formation due to vapor wall losses is robust across the ranges of uncertainties in the key model assumptions for wall-loss and mass-transfer coefficients and chemical mechanisms.We then apply similar assumptions regarding SOA formation chemistry and physics to smoke emitted into the atmosphere. In ambient plumes, the plume dilution rate impacts the organic partitioning between the gas and particle phases, which may impact the potential for SOA to form as well as the rate of SOA formation. We add Gaussian dispersion to our aerosol

Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes

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

Bian, Qijing; Jathar, Shantanu H.; Kodros, John K.

Secondary organic aerosol (SOA) has been shown to form in biomass-burning emissions in laboratory and field studies. However, there is significant variability among studies in mass enhancement, which could be due to differences in fuels, fire conditions, dilution, and/or limitations of laboratory experiments and observations. This study focuses on understanding processes affecting biomass-burning SOA formation in laboratory smog-chamber experiments and in ambient plumes. Vapor wall losses have been demonstrated to be an important factor that can suppress SOA formation in laboratory studies of traditional SOA precursors; however, impacts of vapor wall losses on biomass-burning SOA have not yet been investigated.more » We use an aerosol-microphysical model that includes representations of volatility and oxidation chemistry to estimate the influence of vapor wall loss on SOA formation observed in the FLAME III smog-chamber studies. Our simulations with base-case assumptions for chemistry and wall loss predict a mean OA mass enhancement (the ratio of final to initial OA mass, corrected for particle-phase wall losses) of 1.8 across all experiments when vapor wall losses are modeled, roughly matching the mean observed enhancement during FLAME III. The mean OA enhancement increases to over 3 when vapor wall losses are turned off, implying that vapor wall losses reduce the apparent SOA formation. We find that this decrease in the apparent SOA formation due to vapor wall losses is robust across the ranges of uncertainties in the key model assumptions for wall-loss and mass-transfer coefficients and chemical mechanisms. We then apply similar assumptions regarding SOA formation chemistry and physics to smoke emitted into the atmosphere. In ambient plumes, the plume dilution rate impacts the organic partitioning between the gas and particle phases, which may impact the potential for SOA to form as well as the rate of SOA formation. We add Gaussian dispersion to our aerosol

Secondary organic aerosol formation in biomass-burning plumes: theoretical analysis of lab studies and ambient plumes

DOE PAGES

Bian, Qijing; Jathar, Shantanu H.; Kodros, John K.; ...

2017-04-28

Secondary organic aerosol (SOA) has been shown to form in biomass-burning emissions in laboratory and field studies. However, there is significant variability among studies in mass enhancement, which could be due to differences in fuels, fire conditions, dilution, and/or limitations of laboratory experiments and observations. This study focuses on understanding processes affecting biomass-burning SOA formation in laboratory smog-chamber experiments and in ambient plumes. Vapor wall losses have been demonstrated to be an important factor that can suppress SOA formation in laboratory studies of traditional SOA precursors; however, impacts of vapor wall losses on biomass-burning SOA have not yet been investigated.more » We use an aerosol-microphysical model that includes representations of volatility and oxidation chemistry to estimate the influence of vapor wall loss on SOA formation observed in the FLAME III smog-chamber studies. Our simulations with base-case assumptions for chemistry and wall loss predict a mean OA mass enhancement (the ratio of final to initial OA mass, corrected for particle-phase wall losses) of 1.8 across all experiments when vapor wall losses are modeled, roughly matching the mean observed enhancement during FLAME III. The mean OA enhancement increases to over 3 when vapor wall losses are turned off, implying that vapor wall losses reduce the apparent SOA formation. We find that this decrease in the apparent SOA formation due to vapor wall losses is robust across the ranges of uncertainties in the key model assumptions for wall-loss and mass-transfer coefficients and chemical mechanisms. We then apply similar assumptions regarding SOA formation chemistry and physics to smoke emitted into the atmosphere. In ambient plumes, the plume dilution rate impacts the organic partitioning between the gas and particle phases, which may impact the potential for SOA to form as well as the rate of SOA formation. We add Gaussian dispersion to our aerosol

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

DOE PAGES

Ortega, Amber M.; Hayes, Patrick L.; Peng, Zhe; ...

2016-06-15

Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient andmore » reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days–6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and O x, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive ( τ OH ~ 0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ~ –0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OS C ~ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

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

Ortega, Amber M.; Hayes, Patrick L.; Peng, Zhe

Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient andmore » reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days–6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and O x, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive ( τ OH ~ 0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ~ –0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OS C ~ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and

What Aerosol Water do Organic Compounds See?

EPA Science Inventory

Large amounts of aerosol water are associated with inorganic salts such as ammonium sulfate with generally smaller but important contributions from hydrophilic organics. Ambient aerosols can be externally or internally mixed in addition to containing one or multiple phases. The d...

Biological aerosol background characterization

NASA Astrophysics Data System (ADS)

Blatny, Janet; Fountain, Augustus W., III

2011-05-01

To provide useful information during military operations, or as part of other security situations, a biological aerosol detector has to respond within seconds or minutes to an attack by virulent biological agents, and with low false alarms. Within this time frame, measuring virulence of a known microorganism is extremely difficult, especially if the microorganism is of unknown antigenic or nucleic acid properties. Measuring "live" characteristics of an organism directly is not generally an option, yet only viable organisms are potentially infectious. Fluorescence based instruments have been designed to optically determine if aerosol particles have viability characteristics. Still, such commercially available biological aerosol detection equipment needs to be improved for their use in military and civil applications. Air has an endogenous population of microorganisms that may interfere with alarm software technologies. To design robust algorithms, a comprehensive knowledge of the airborne biological background content is essential. For this reason, there is a need to study ambient live bacterial populations in as many locations as possible. Doing so will permit collection of data to define diverse biological characteristics that in turn can be used to fine tune alarm algorithms. To avoid false alarms, improving software technologies for biological detectors is a crucial feature requiring considerations of various parameters that can be applied to suppress alarm triggers. This NATO Task Group will aim for developing reference methods for monitoring biological aerosol characteristics to improve alarm algorithms for biological detection. Additionally, they will focus on developing reference standard methodology for monitoring biological aerosol characteristics to reduce false alarm rates.

Organic carbon content of marine aerosols collected on Bermuda

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

Hoffman, E.J.; Duce, R.A.

1974-01-01

The concentration of total organic carbon in marine aerosols collected from a 20-m tower on the Southwest Coast of Bermuda ranged from 0.15 to 0.47 microgram/M/sup 3/ STP under onshore wind conditions. The mass of the organic carbon ranged from 1 to 19% of the mass of sea salt in the particles in Bermuda, and the percentage decreased with increasing salt content.

A COMPARATIVE ASSESSMENT OF BOISE, IDAHO, AMBIENT AIR FINE PARTICLE SAMPLES USING THE PLATE AND MICROSUSPENSION SALMONELLA MUTAGENICITY ASSAYS

EPA Science Inventory

The primary objective of this study is to characterize the genotoxic potential of the ambient air aerosols collected within an air shed impacted primarily by wood smoke and automotive emissions. The study also examines the relative merits of a microsuspension assay and the standa...

Heterogeneous reaction of peroxyacetic acid and hydrogen peroxide on ambient aerosol particles under dry and humid conditions: kinetics, mechanism and implications

NASA Astrophysics Data System (ADS)

Wu, Q. Q.; Huang, L. B.; Liang, H.; Zhao, Y.; Huang, D.; Chen, Z. M.

2015-02-01

Hydrogen peroxide (H2O2) and organic peroxides play important roles in the cycle of oxidants and the formation of secondary aerosols in the atmosphere. Recent field observations suggest that peroxyacetic acid (PAA, CH3C(O)OOH) is one of the most important organic peroxides in the atmosphere, whose budget is potentially related to the aerosols. Here we present the first laboratory measurements of the uptake coefficient of gaseous PAA and H2O2 onto the ambient fine particulate matter (PM2.5) as a function of relative humidity (RH) at 298 K. The results show that the PM2.5, which was collected in an urban area, can take up PAA and H2O2 at the uptake coefficient (γ) of 10-4, and both γPAA and γH2O2 increase with increasing RH. However, γPAA is more sensitive to the RH variation than is γH2O2, which indicates that the enhanced uptake of peroxide compounds on PM2.5 under humid conditions is dominated by chemical processes rather than dissolution. Considering that mineral dust is one of the main components of PM2.5, we also determined the uptake coefficients of gaseous PAA and H2O2 on authentic Asian Dust Storm (ADS) and Arizona Test Dust (ATD) particles. Compared to ambient PM2.5, ADS shows a similar γ value and RH dependence in its uptake coefficient for PAA and H2O2, while ATD gives a negative dependence on RH. The present study indicates that in addition to the mineral dust in PM2.5, other components (e.g., inorganic soluble salts) are also important to the uptake of peroxide compounds. When the heterogeneous reaction of PAA on PM2.5 is considered, its atmospheric lifetime is estimated to be 3.3 h on haze days and 7.6 h on non-haze days, values which agree well with the field observed result.

Long-term trends in California mobile source emissions and ambient concentrations of black carbon and organic aerosol.

PubMed

McDonald, Brian C; Goldstein, Allen H; Harley, Robert A

2015-04-21

A fuel-based approach is used to assess long-term trends (1970-2010) in mobile source emissions of black carbon (BC) and organic aerosol (OA, including both primary emissions and secondary formation). The main focus of this analysis is the Los Angeles Basin, where a long record of measurements is available to infer trends in ambient concentrations of BC and organic carbon (OC), with OC used here as a proxy for OA. Mobile source emissions and ambient concentrations have decreased similarly, reflecting the importance of on- and off-road engines as sources of BC and OA in urban areas. In 1970, the on-road sector accounted for ∼90% of total mobile source emissions of BC and OA (primary + secondary). Over time, as on-road engine emissions have been controlled, the relative importance of off-road sources has grown. By 2010, off-road engines were estimated to account for 37 ± 20% and 45 ± 16% of total mobile source contributions to BC and OA, respectively, in the Los Angeles area. This study highlights both the success of efforts to control on-road emission sources, and the importance of considering off-road engine and other VOC source contributions when assessing long-term emission and ambient air quality trends.

Modeling aerosol water uptake in the arctic based on the κ-Kohler theory

NASA Astrophysics Data System (ADS)

Rastak, N.; Ekman, A.; Silvergren, S.; Zieger, P.; Wideqvist, U.; Ström, J.; Svenningsson, B.; Tunved, P.; Riipinen, I.

2013-05-01

Water uptake or hygroscopicity is one of the most fundamental properties of atmospheric aerosols. Aerosol particles containing soluble materials can grow in size by absorbing water in ambient atmosphere. This property is measured by a parameter known as growth factor (GF), which is defined as the ratio of the wet diameter to the dry diameter. Hygroscopicity controls the size of an aerosol particle and therefore its optical properties in the atmosphere. Hygroscopic growth depends on the dry size of the particle, its chemical composition and the relative humidity in the ambient air (Fitzgerald, 1975; Pilinis et al., 1995). One of the typical problems in aerosol studies is the lack of measurements of aerosol size distributions and optical properties in ambient conditions. The gap between dry measurements and the real humid atmosphere is filled in this study by utilizing a hygroscopic model which calculates the hygroscopic growth of aerosol particles at Mt Zeppelin station, Ny Ålesund, Svalbard during 2008.

Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor

NASA Astrophysics Data System (ADS)

Palm, Brett B.; Campuzano-Jost, Pedro; Day, Douglas A.; Ortega, Amber M.; Fry, Juliane L.; Brown, Steven S.; Zarzana, Kyle J.; Dube, William; Wagner, Nicholas L.; Draper, Danielle C.; Kaser, Lisa; Jud, Werner; Karl, Thomas; Hansel, Armin; Gutiérrez-Montes, Cándido; Jimenez, Jose L.

2017-04-01

Ambient pine forest air was oxidized by OH, O3, or NO3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen - Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O3 and NO3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20-30 min, in order to determine how the availability of SOA precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O3 or NO3 oxidation. This is likely because O3 and NO3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O3 and NO3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O3 and NO3 oxidation produced SOA with elemental O : C and H : C

Secondary organic aerosol formation from in situ OH, O 3, and NO 3 oxidation of ambient forest air in an oxidation flow reactor

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

Palm, Brett B.; Campuzano-Jost, Pedro; Day, Douglas A.

Ambient pine forest air was oxidized by OH, O 3, or NO 3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio–hydro–atmosphere interactions of Energy, Aerosols, Carbon, H 2O, Organics and Nitrogen – Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O 3 and NO 3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20–30 min, in order to determine how the availability of SOAmore » precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O 3 or NO 3 oxidation. This is likely because O 3 and NO 3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O 3 and NO 3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O 3 and NO 3 oxidation produced SOA with

Secondary organic aerosol formation from in situ OH, O 3, and NO 3 oxidation of ambient forest air in an oxidation flow reactor

DOE PAGES

Palm, Brett B.; Campuzano-Jost, Pedro; Day, Douglas A.; ...

2017-04-25

Ambient pine forest air was oxidized by OH, O 3, or NO 3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio–hydro–atmosphere interactions of Energy, Aerosols, Carbon, H 2O, Organics and Nitrogen – Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O 3 and NO 3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20–30 min, in order to determine how the availability of SOAmore » precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O 3 or NO 3 oxidation. This is likely because O 3 and NO 3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O 3 and NO 3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O 3 and NO 3 oxidation produced SOA with

Microfluidic Air Sampler for Highly Efficient Bacterial Aerosol Collection and Identification.

PubMed

Bian, Xiaojun; Lan, Ying; Wang, Bing; Zhang, Yu Shrike; Liu, Baohong; Yang, Pengyuan; Zhang, Weijia; Qiao, Liang

2016-12-06

The early warning capability of the presence of biological aerosol threats is an urgent demand in ensuing civilian and military safety. Efficient and rapid air sample collection in relevant indoor or outdoor environment is a key step for subsequent analysis of airborne microorganisms. Herein, we report a portable battery-powered sampler that is capable of highly efficient bioaerosol collection. The essential module of the sampler is a polydimethylsiloxane (PDMS) microfluidic chip, which consisted of a 3-loop double-spiral microchannel featuring embedded herringbone and sawtooth wave-shaped structures. Vibrio parahemolyticus (V. parahemolyticus) as a model microorganism, was initially employed to validate the bioaerosol collection performance of the device. Results showed that the sampling efficacy reached as high as >99.9%. The microfluidic sampler showed greatly improved capturing efficiency compared with traditional plate sedimentation methods. The high performance of our device was attributed to the horizontal inertial centrifugal force and the vertical turbulence applied to airflow during sampling. The centrifugation field and turbulence were generated by the specially designed herringbone structures when air circulated in the double-spiral microchannel. The sawtooth wave-shaped microstructure created larger specific surface area for accommodating more aerosols. Furthermore, a mixture of bacterial aerosols formed by V. parahemolyticus, Listeria monocytogenes, and Escherichia coli was extracted by the microfluidic sampler. Subsequent integration with mass spectrometry conveniently identified the multiple bacterial species captured by the sampler. Our developed stand-alone and cable-free sampler shows clear advantages comparing with conventional strategies, including portability, easy-to-use, and low cost, indicating great potential in future field applications.

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

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

On the Evaporation Kinetics and Phase of Laboratory and Ambient Secondary Organic Aerosol

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Vaden, T.; Imre, D. G.; Beránek, J.; Shrivastava, M.

2010-12-01

Field measurements of secondary organic aerosol (SOA) find significantly higher mass loads than predicted by models, sparking intense effort that is focused on finding additional SOA sources, but leaves many of the fundamental assumptions that are used by models unchallenged. Current air-quality models use absorptive partitioning theory assuming SOA particles are liquid droplets that form instantaneous reversible equilibrium with gas phase. Further, they ignore the effects of adsorption of spectator organic species during SOA formation on SOA properties and fate. Using an accurate and highly sensitive experimental approach for studying evaporation kinetics of size-selected single SOA particles, we characterized room-temperature evaporation kinetics of laboratory generated α-pinene SOA and ambient atmospheric SOA. The experimental setup was first tested by measuring the evaporation kinetics of single component organic particles of known vapor pressure. We show that, as expected for liquid droplets, smaller particles evaporate faster, and that these data yield the correct vapor pressure. We then study the evaporation kinetics of α-pinene SOA and find that evaporation proceeds in two stages: a fast stage, during which 50% of the particle volume evaporates in ~100 minutes, followed by a slower stage, when additional 25% evaporate in 1400 minutes, which is in sharp contrast to the ~10 minutes timescale predicted by current kinetic models. α-pinene SOA formed in the presence of “spectator” hydrophobic organic vapors like dioctyl phthalate, dioctyl sebacate, pyrene, or their mixture, were shown to adsorb noticeable amounts of these organics, forming what we term here ‘coated’ SOA particles. We show that these adsorbed coatings reduce evaporation rates of SOA particles. Moreover, aging of coated SOA particles dramatically reduces evaporation rates, and in some cases nearly stops it. For example, aging of SOA with adsorbed pyrene reduces evaporation rate to the

Processing of aerosol particles within the Habshan pollution plume

NASA Astrophysics Data System (ADS)

Semeniuk, T. A.; Bruintjes, R.; Salazar, V.; Breed, D.; Jensen, T.; Buseck, P. R.

2015-03-01

The Habshan industrial site in the United Arab Emirates produces a regional-scale pollution plume associated with oil and gas processing, discharging high loadings of sulfates and chlorides into the atmosphere, which interact with the ambient aerosol population. Aerosol particles and trace gas chemistry at this site were studied on two flights in the summer of 2002. Measurements were collected along vertical plume profiles to show changes associated with atmospheric processing of particle and gas components. Close to the outlet stack, particle concentrations were over 10,000 cm-3, dropping to <2000 cm-3 in more dilute plume around 1500 m above the stack. Particles collected close to the stack and within the dilute plume were individually measured for size, morphology, composition, and mixing state using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy. Close to the stack, most coarse particles consisted of mineral dust and NaCl crystals from burning oil brines, while sulfate droplets dominated the fine mode. In more dilute plume, at least 1500 m above the stack, the particle spectrum was more diverse, with a significant increase in internally mixed particle types. Dilute plume samples consisted of coarse NaCl/silicate aggregates or NaCl-rich droplets, often with a sulfate component, while fine-fraction particles were of mixed cation sulfates, also internally mixed with nanospherical soot or silicates. Thus, both chloride and sulfate components of the pollution plume rapidly reacted with ambient mineral dust to form coated and aggregate particles, enhancing particle size, hygroscopicity, and reactivity of the coarse mode. The fine-fraction sulfate-bearing particles formed in the plume contribute to regional transport of sulfates, while coarse sulfate-bearing fractions locally reduced the SO2 loading through sedimentation. The chloride- and sulfate-bearing internally mixed particles formed in the plume markedly changed the

Collection of Viable Aerosolized Influenza Virus and Other Respiratory Viruses in a Student Health Care Center through Water-Based Condensation Growth

PubMed Central

Pan, Maohua; Bonny, Tania S.; Loeb, Julia; Jiang, Xiao; Eiguren-Fernandez, Arantzazu; Hering, Susanne; Fan, Z. Hugh; Wu, Chang-Yu

2017-01-01

ABSTRACT The dynamics and significance of aerosol transmission of respiratory viruses are still controversial, for the major reasons that virus aerosols are inefficiently collected by commonly used air samplers and that the collected viruses are inactivated by the collection method. Without knowledge of virus viability, infection risk analyses lack accuracy. This pilot study was performed to (i) determine whether infectious (viable) respiratory viruses in aerosols could be collected from air in a real world environment by the viable virus aerosol sampler (VIVAS), (ii) compare and contrast the efficacy of the standard bioaerosol sampler, the BioSampler, with that of the VIVAS for the collection of airborne viruses in a real world environment, and (iii) gain insights for the use of the VIVAS for respiratory virus sampling. The VIVAS operates via a water vapor condensation process to enlarge aerosolized virus particles to facilitate their capture. A variety of viable human respiratory viruses, including influenza A H1N1 and H3N2 viruses and influenza B viruses, were collected by the VIVAS located at least 2 m from seated patients, during a late-onset 2016 influenza virus outbreak. Whereas the BioSampler when operated following our optimized parameters also collected virus aerosols, it was nevertheless overall less successful based on a lower frequency of virus isolation in most cases. This side-by-side comparison highlights some limitations of past studies based on impingement-based sampling, which may have generated false-negative results due to either poor collection efficiency and/or virus inactivation due to the collection process. IMPORTANCE The significance of virus aerosols in the natural transmission of respiratory diseases has been a contentious issue, primarily because it is difficult to collect or sample virus aerosols using currently available air sampling devices. We tested a new air sampler based on water vapor condensation for efficient sampling of

Evidence and quantitation of aromatic organosulfates in ambient aerosols in Lahore, Pakistan

NASA Astrophysics Data System (ADS)

Kundu, S.; Quraishi, T. A.; Yu, G.; Suarez, C.; Keutsch, F. N.; Stone, E. A.

2013-05-01

Organosulfates are important components of atmospheric organic aerosols, yet their structures, abundances, sources and formation processes are not adequately understood. This study presents the identification and quantitation of benzyl sulfate in atmospheric aerosols, which is the first confirmed atmospheric organosulfate with aromatic carbon backbone. Benzyl sulfate was identified and quantified in fine particulate matter (PM2.5) collected in Lahore, Pakistan, during 2007-2008. An authentic standard of benzyl sulfate was synthesized, standardized, and identified in atmospheric aerosols with quadrupole time-of-flight (Q-ToF) mass spectrometry (MS). Benzyl sulfate was quantified in aerosol samples using ultra performance liquid chromatography (UPLC) coupled to negative electrospray ionization triple quadrupole (TQ) MS. The highest benzyl sulfate concentrations were recorded in November and January 2007 (0.50 ± 0.11 ng m-3) whereas the lowest concentration was observed in July (0.05 ± 0.02 ng m-3). To evaluate matrix effects, benzyl sulfate concentrations were determined using external calibration and the method of standard addition; comparable concentrations were detected by the two methods, which ruled out significant matrix effects in benzyl sulfate quantitation. Three additional organosulfates with m/z 187, 201 and 215 were qualitatively identified as aromatic organosulfates with additional methyl substituents by high-resolution mass measurements and tandem MS. The observed aromatic organosulfates form a homologous series analogous to toluene, xylene, and trimethylbenzene, which are abundant anthropogenic volatile organic compounds (VOC), suggesting that aromatic organosulfates may be formed by secondary reactions. However, stronger statistical correlations of benzyl sulfate with combustion tracers (EC and levoglucosan) than with secondary tracers (SO42- and α-pinene-derived nitrooxy organosulfates) suggest that aromatic organosulfates may be emitted from the

Influence of Humidity on the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

NASA Technical Reports Server (NTRS)

Gasso, B. S.; Hegg, D. A.; Covert, D. S.; Collins, D.; Noone, K.; Oestroem, E.; Schmid, B.; Russell, P. B.; Livingston, J. M.; Durkee, P. A.;

Influence of Humidity On the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

NASA Technical Reports Server (NTRS)

Gasso, S.; Hegg, D. A.; Covert, D. S.; Collins, D.; Noone, K. J.; Oestroem, E.; Schmid, B.; Russell, P. B.; Livingston, J. M.; Durkee, P. A.

2000-01-01

Aerosol scattering coefficients (sigma(sub sp)) have been measured over the ocean at different relative humidities (RH) as a function of altitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions, absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of sigma(sub sp) as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands of the EOS (Earth Observing System) AM-1 (Terra) detectors, MODIS (Moderate Resolution Imaging Spectroradiometer) and MISR (Multi-angle Imaging Spectroradiometer). The UWPH measured sigma(sub sp) at two RHs, one below and the other above ambient conditions. Ambient sigma(sub sp) was obtained by interpolation of these two measurements. The data were stratified in terms of three types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., two- or one-day old polluted aerosols advected from Europe). An empirical relation for the dependence of sigma(sub sp) on RH, defined by sigma(sub sp)(RH) = k.(1 - RH/100)(sup gamma), was used with the hygroscopic exponent gamma derived from the data. The following gamma values were obtained for the 3 aerosol types: gamma(dust) = 0.23 +/- 0.05, gamma(clean marine) = 0.69 +/- 0.06 and gamma(polluted marine) = 0.57 +/- 0.06. Based on the measured gammas, the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each

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

Apportionment of Primary and Secondary Organic Aerosols in Southern California During the 2005 Study of Organic Aerosols in Riverside (SOAR-1)

EPA Science Inventory

Ambient sampling was conducted in Riverside, California during the 2005 Study of Organic Aerosols in Riverside to characterize the composition and sources of organic aerosol using a variety of state-of-the-art instrumentation and source apportionment techniques.

Size-resolved characterization of the polysaccharidic and proteinaceous components of sea spray aerosol

NASA Astrophysics Data System (ADS)

Aller, Josephine Y.; Radway, JoAnn C.; Kilthau, Wendy P.; Bothe, Dylan W.; Wilson, Theodore W.; Vaillancourt, Robert D.; Quinn, Patricia K.; Coffman, Derek J.; Murray, Benjamin J.; Knopf, Daniel A.

2017-04-01

Dissolved organic polymers released by phytoplankton and bacteria abiologically self-assemble in surface ocean waters into nano-to micro-sized gels containing polysaccharides, proteins, lipids and other components. These gels concentrate in the sea surface microlayer (SML), where they can potentially contribute to sea spray aerosol (SSA). Sea spray is a major source of atmospheric aerosol mass over much of the earth's surface, and knowledge of its properties (including the amount and nature of the organic content), size distributions and fluxes are fundamental for determining its role in atmospheric chemistry and climate. Using a cascade impactor, we collected size-fractionated aerosol particles from ambient air and from freshly generated Sea Sweep SSA in the western North Atlantic Ocean together with biological and chemical characterization of subsurface and SML waters. Spectrophotometric methods were applied to quantify the polysaccharide-containing transparent exopolymer (TEP) and protein-containing Coomassie stainable material (CSM) in these particles and waters. This study demonstrates that both TEP and CSM in surface ocean waters are aerosolized with sea spray with the greatest total TEP associated with particles <180 nm in diameter and >5 000 nm. The higher concentrations of TEP and CSM in particles >5 000 nm most likely reflects collection of microorganism cells and/or fragments. The greater concentration of CSM in larger size particles may also reflect greater stability of proteinaceous gels compared to polysaccharide-rich gels in surface waters and the SML. Both TEP and CSM were measured in the ambient marine air sample with concentrations of 2.1 ± 0.16 μg xanthan gum equivalents (XG eq.) m-3 and 14 ± 1.0 μg bovine serum albumin equivalents (BSA eq.) m-3. TEP in Sea Sweep SSA averaged 4.7 ± 3.1 μg XG eq. m-3 and CSM 8.6 ± 7.3 μg BSA eq. m-3. This work shows the transport of marine biogenic material across the air-sea interface through primary

Aerosol Inlet Characterization Experiment Report

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

Bullard, Robert L.; Kuang, Chongai; Uin, Janek

2017-05-01

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility Aerosol Observation System inlet stack was characterized for particle penetration efficiency from 10 nm to 20 μm in diameter using duplicate scanning mobility particle sizers (10 nm-450 nm), ultra-high-sensitivity aerosol spectrometers (60 nm-μm), and aerodynamic particle sizers (0.5 μm-20 μm). Results show good model-measurement agreement and unit transmission efficiency of aerosols from 10 nm to 4 μm in diameter. Large uncertainties in the measured transmission efficiency exist above 4 μm due to low ambient aerosol signal in that size range.

Weekday/weekend differences in ambient aerosol level and chemical characteristics of water-soluble components in the city centre

NASA Astrophysics Data System (ADS)

Khoder, M. I.; Hassan, S. K.

Weekday and weekend ambient aerosol samples were collected from the city centre of Cairo, namely "Ramsis" during the summer season of the year 2006, and have been analyzed for water-soluble ionic species. The average concentrations of the total suspended particulate matter (TSP) and their water-soluble components were higher during weekdays than on weekends, indicating that the decreased traffic density on weekends leads to a decrease in the levels of the TSP and their water-soluble ionic species. The average concentrations of the TSP were 454 μg m -3 on weekdays and 298 μg m -3 on weekends. The weekday/weekend concentration ratios were 1.52 for TSP, 1.27 for SO 42-, 1.64 for Cl -, 1.54 for NO 3-, 1.17 for NH 4+, 1.67 for Ca 2+, 1.83 for Na +, 1.75 for K + and 1.73 for Mg 2+. City centre of Cairo has high levels of the TSP and their water-soluble ionic species compared with many polluted cities in the world. Among all of the measured water-soluble components, SO 42- was the most abundant species followed by Ca 2+ on weekdays and weekends. The average mass ratios of NO 3-/SO 42- in the TSP were 0.41 on weekdays and 0.34 on weekends, suggesting that the stationary source emissions were more predominant. The NH 4+/SO 42- molar ratios and its relation with the concentrations of TSP and Ca 2+ during the weekdays and weekends indicate that the chemical form of sulfate and ammonium in aerosol particles varies with TSP and Ca 2+ levels. At high TSP and Ca 2+ levels, and NH 4+/SO 42- molar ratios less than one, SO 42- in aerosol particles may be present as CaSO 4 and (NH 4) 2SO 4·CaSO 4·2H 2O, whereas it is expected to be present as (NH 4) 2SO 4, (NH 4) 2SO 4·CaSO 4·2H 2O and CaSO 4 at low levels of TSP and Ca 2+, and NH 4+/SO 42- molar ratios between 1 and 2. The mean pH values of the TSP were 7.65 on weekdays and 6.97 on weekends, indicating that aerosol particles brought a large amount of crustal species, and might alleviate the tendency of acidification. The

Long-Range Transport of Perchlorate Observed in the Atmospheric Aerosols Collected at Okinawa Island, Japan

NASA Astrophysics Data System (ADS)

Handa, D.; Okada, K.; Kuroki, Y.; Nakama, Y.; Nakajima, H.; Arakaki, T.; Tanahara, A.; Oomori, T.; Miyagi, T.; Kadena, H.; Ishizaki, T.; Nakama, F.

2007-12-01

The study of perchlorate has become quite active in the U.S. in the last several years. Perchlorate has been recognized as a new environmental pollutant and it attracted much attention quickly in the world. The health concern about perchlorate stems from the fact that it displaces iodide in the thyroid gland, while iodine-containing thyroid hormones are essential for proper neural development from the fetal stage through the first years of life. In this study, we determined the concentrations of perchlorate ion present in the atmospheric aerosols collected in Okinawa Island, Japan. We then examined the relationships between the perchlorate concentrations and the environmental parameters and the climatic conditions peculiar to Okinawa. Bulk aerosol samples were collected on quartz filters by using a high volume air sampler at Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS). Each sampling duration was one week. The quartz filters with aerosols were stirred with Milli-Q pure water for three hours before perchlorate ion was extracted. The extracted perchlorate ion concentrations were determined by ion chromatography (ICS-2000, DIONEX). The mean perchlorate concentration for the samples collected at CHAAMS was 1.83 ng/m3, and the minimum was 0.18 ng/m3. The samples collected during November 21-27, 2005, January 23-30, 2006 and April 24-01, 2006 had highest perchlorate concentrations. For these three samples, we performed back trajectory analysis, and found that the air mass for the three samples arrived from the Asian continent. A relatively strong correlation (r2 = 0.55) was found between perchlorate and nss-sulfate concentrations for the CHAAMS samples. Furthermore, we analyzed perchlorate in the soils and the fertilizers used for sugar cane farming around the CHAAMS area. The Milli-Q extract of the soil and the fertilizers did not contain any detectable levels of perchlorate ions. Therefore, it was suggested that perchlorate found in the atmospheric

Kinetics of heterogeneous reactions of HO2 radical at ambient concentration levels with (NH4)2SO4 and NaCl aerosol particles.

PubMed

Taketani, Fumikazu; Kanaya, Yugo; Akimoto, Hajime

2008-03-20

The HO2 uptake coefficient (gamma) for inorganic submicrometer wet and dry aerosol particles ((NH4)2SO4 and NaCl) under ambient conditions (760 Torr and 296 +/- 2 K) was measured using an aerosol flow tube (AFT) coupled with a chemical conversion/laser-induced fluorescence (CC/LIF) technique. The CC/LIF technique enabled experiments to be performed at almost the same HO2 radical concentration as that in the atmosphere. HO2 radicals were injected into the AFT through a vertically movable Pyrex tube. Injector position-dependent profiles of LIF intensity were measured as a function of aerosol concentration. Measured gamma values for dry aerosols of (NH4)2SO4 were 0.04 +/- 0.02 and 0.05 +/- 0.02 at 20% and 45% relative humidity (RH), respectively, while those of NaCl were <0.01 and 0.02 +/- 0.01 at 20% and 53% RH, respectively. For wet (NH4)2SO4 aerosols, measured gamma values were 0.11 +/- 0.03, 0.15 +/- 0.03, 0.17 +/- 0.04, and 0.19 +/- 0.04, at 45%, 55%, 65%, and 75% RH, respectively, whereas for wet NaCl aerosols the values were 0.11 +/- 0.03, 0.09 +/- 0.02, and 0.10 +/- 0.02 for 53%, 63%, and 75% RH, respectively. Wet (NH4)2SO4 and NaCl aerosols doped with CuSO4 showed gamma values of 0.53 +/- 0.12 and 0.65 +/- 0.17, respectively. These results suggest that compositions, RH, and phase for aerosol particles are significant to HO2 uptake. Potential HO2 loss processes and their atmospheric contributions are discussed.

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

NASA Astrophysics Data System (ADS)

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

2013-07-01

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

Validation and Uncertainty Estimates for MODIS Collection 6 "Deep Blue" Aerosol Data

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Hsu, N. C.; Bettenhausen, C.; Jeong, M.-J.

2013-01-01

The "Deep Blue" aerosol optical depth (AOD) retrieval algorithm was introduced in Collection 5 of the Moderate Resolution Imaging Spectroradiometer (MODIS) product suite, and complemented the existing "Dark Target" land and ocean algorithms by retrieving AOD over bright arid land surfaces, such as deserts. The forthcoming Collection 6 of MODIS products will include a "second generation" Deep Blue algorithm, expanding coverage to all cloud-free and snow-free land surfaces. The Deep Blue dataset will also provide an estimate of the absolute uncertainty on AOD at 550 nm for each retrieval. This study describes the validation of Deep Blue Collection 6 AOD at 550 nm (Tau(sub M)) from MODIS Aqua against Aerosol Robotic Network (AERONET) data from 60 sites to quantify these uncertainties. The highest quality (denoted quality assurance flag value 3) data are shown to have an absolute uncertainty of approximately (0.086+0.56Tau(sub M))/AMF, where AMF is the geometric air mass factor. For a typical AMF of 2.8, this is approximately 0.03+0.20Tau(sub M), comparable in quality to other satellite AOD datasets. Regional variability of retrieval performance and comparisons against Collection 5 results are also discussed.

Chromatography related performance of the Monitor for AeRosols and GAses in ambient air (MARGA): laboratory and field-based evaluation

NASA Astrophysics Data System (ADS)

Chen, Xi; Walker, John T.; Geron, Chris

2017-10-01

Evaluation of the semi-continuous Monitor for AeRosols and GAses in ambient air (MARGA, Metrohm Applikon B.V.) was conducted with an emphasis on examination of accuracy and precision associated with processing of chromatograms. Using laboratory standards and atmospheric measurements, analytical accuracy, precision and method detection limits derived using the commercial MARGA software were compared to an alternative chromatography procedure consisting of a custom Java script to reformat raw MARGA conductivity data and Chromeleon (Thermo Scientific Dionex) software for peak integration. Our analysis revealed issues with accuracy and precision resulting from misidentification and misintegration of chromatograph peaks by the MARGA automated software as well as a systematic bias at low concentrations for anions. Reprocessing and calibration of raw MARGA data using the alternative chromatography method lowered method detection limits and reduced variability (precision) between parallel sampler boxes. Instrument performance was further evaluated during a 1-month intensive field campaign in the fall of 2014, including analysis of diurnal patterns of gaseous and particulate water-soluble species (NH3, SO2, HNO3, NH4+, SO42- and NO3-), gas-to-particle partitioning and particle neutralization state. At ambient concentrations below ˜ 1 µg m-3, concentrations determined using the MARGA software are biased +30 and +10 % for NO3- and SO42-, respectively, compared to concentrations determined using the alternative chromatography procedure. Differences between the two methods increase at lower concentrations. We demonstrate that positively biased NO3- and SO42- measurements result in overestimation of aerosol acidity and introduce nontrivial errors to ion balances of inorganic aerosol. Though the source of the bias is uncertain, it is not corrected by the MARGA online single-point internal LiBr standard. Our results show that calibration and verification of instrument accuracy

Collection of Viable Aerosolized Influenza Virus and Other Respiratory Viruses in a Student Health Care Center through Water-Based Condensation Growth.

PubMed

Pan, Maohua; Bonny, Tania S; Loeb, Julia; Jiang, Xiao; Lednicky, John A; Eiguren-Fernandez, Arantzazu; Hering, Susanne; Fan, Z Hugh; Wu, Chang-Yu

2017-01-01

The dynamics and significance of aerosol transmission of respiratory viruses are still controversial, for the major reasons that virus aerosols are inefficiently collected by commonly used air samplers and that the collected viruses are inactivated by the collection method. Without knowledge of virus viability, infection risk analyses lack accuracy. This pilot study was performed to (i) determine whether infectious (viable) respiratory viruses in aerosols could be collected from air in a real world environment by the vi able v irus a erosol s ampler (VIVAS), (ii) compare and contrast the efficacy of the standard bioaerosol sampler, the BioSampler, with that of the VIVAS for the collection of airborne viruses in a real world environment, and (iii) gain insights for the use of the VIVAS for respiratory virus sampling. The VIVAS operates via a water vapor condensation process to enlarge aerosolized virus particles to facilitate their capture. A variety of viable human respiratory viruses, including influenza A H1N1 and H3N2 viruses and influenza B viruses, were collected by the VIVAS located at least 2 m from seated patients, during a late-onset 2016 influenza virus outbreak. Whereas the BioSampler when operated following our optimized parameters also collected virus aerosols, it was nevertheless overall less successful based on a lower frequency of virus isolation in most cases. This side-by-side comparison highlights some limitations of past studies based on impingement-based sampling, which may have generated false-negative results due to either poor collection efficiency and/or virus inactivation due to the collection process. IMPORTANCE The significance of virus aerosols in the natural transmission of respiratory diseases has been a contentious issue, primarily because it is difficult to collect or sample virus aerosols using currently available air sampling devices. We tested a new air sampler based on water vapor condensation for efficient sampling of viable

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

Analyses of biomass burning contribution to aerosol in Zhengzhou during wheat harvest season in 2015

NASA Astrophysics Data System (ADS)

Chen, Hongyang; Yin, Shasha; Li, Xiao; Wang, Jia; Zhang, Ruiqin

2018-07-01

Ambient PM2.5 samples were collected in suburban area of Zhengzhou, China to investigate the impact of straw open burning on local aerosol during wheat harvest season in 2015. Secondary formation and accumulation processes were found under unfavorable meteorological conditions through the chemical composition analysis in PM2.5. And spatial and temporal variation of the agricultural activities were observed through MODIS fire spots data combined with back trajectory analysis. Results showed elevated levoglucosan was affected directly during biomass burning episodes and transportation periods. In order to estimate the contribution, levoglucosan/K+ combined with levoglucosan/mannosan were analyzed to identify biomass burning sources. And the results showed that levoglucosan were emitted from straw burning mixing with softwood combustion during the study period, emphasizing that wood combustion for households was non-negligible which consists part of the levoglucosan background in Zhengzhou aerosol. Based on emission factors (levoglucosan/OC or levoglucosan/PM2.5) summarized by laboratory simulation experiments, the study period was divided into 7 depending on the former characteristics to estimate the contribution of biomass burning to aerosol, and the average contributions of biomass burning emission to OC and PM2.5 were 46% and 13% relatively, indicating biomass burning have a significant impact on ambient aerosol levels during harvest season.

Field test of a new instrument to measure UV/Vis (300-700 nm) ambient aerosol extinction spectra in Colorado during DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Dibb, J. E.; Greenslade, M. E.; Martin, R.; Scheuer, E. M.; Shook, M.; Thornhill, K. L., II; Troop, D.; Winstead, E.; Ziemba, L. D.

2014-12-01

An optical instrument has been developed to investigate aerosol extinction spectra in the ambient atmosphere. Based on a White-type cell design and using a differential optical approach, aerosol extinction spectra over the 300-700 nm ultraviolet and visible (UV/Vis) wavelength range are obtained. Laboratory tests conducted at NASA Langley Research Center (NASA LaRC) in March 2014 showed good agreement with Cavity Attenuated Phase Shift (CAPS PMex, Aerodyne Research) extinction measurements (at 450, 530, and 630 nm) for a variety of aerosols, e.g., scatterers such as polystyrene latex spheres and ammonium sulfate; absorbers such as dust (including pigmented minerals), smoke (generated in a miniCAST burning propane) and laboratory smoke analogs (e.g., fullerene soot and aquadag). The instrument was field tested in Colorado in July and August 2014 aboard the NASA mobile laboratory at various ground sites during the DISCOVER-AQ (Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality) field campaign. A description of the instrument, results from the laboratory tests, and summer field data will be presented. The instrument provides a new tool for probing in situ aerosol optical properties that may help inform remote sensing approaches well into the UV range.

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

DOE PAGES

Palm, Brett B.; Campuzano-Jost, Pedro; Ortega, Amber M.; ...

2016-03-08

An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H 2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowedmore » for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m –3 when LVOC fate corrected) compared to daytime (average 0.9 µg m –3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+ p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (>10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

NASA Astrophysics Data System (ADS)

Palm, Brett B.; Campuzano-Jost, Pedro; Ortega, Amber M.; Day, Douglas A.; Kaser, Lisa; Jud, Werner; Karl, Thomas; Hansel, Armin; Hunter, James F.; Cross, Eben S.; Kroll, Jesse H.; Peng, Zhe; Brune, William H.; Jimenez, Jose L.

2016-03-01

An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen-Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m-3 when LVOC fate corrected) compared to daytime (average 0.9 µg m-3 when LVOC fate corrected), with maximum formation observed at 0.4-1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic

Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air

NASA Astrophysics Data System (ADS)

Palm, Brett Brian

Secondary organic aerosols (SOA) in the atmosphere play an important role in air quality, human health, and climate. However, the sources, formation pathways, and fate of SOA are poorly constrained. In this dissertation, I present development and application of the oxidation flow reactor (OFR) technique for studying SOA formation from OH, O3, and NO3 oxidation of ambient air. With a several-minute residence time and a portable design with no inlet, OFRs are particularly well-suited for this purpose. I first introduce the OFR concept, and discuss several advances I have made in performing and interpreting OFR experiments. This includes estimating oxidant exposures, modeling the fate of low-volatility gases in the OFR (wall loss, condensation, and oxidation), and comparing SOA yields of single precursors in the OFR with yields measured in environmental chambers. When these experimental details are carefully considered, SOA formation in an OFR can be more reliably compared with ambient SOA formation processes. I then present an overview of what OFR measurements have taught us about SOA formation in the atmosphere. I provide a comparison of SOA formation from OH, O3, and NO3 oxidation of ambient air in a wide variety of environments, from rural forests to urban air. In a rural forest, the SOA formation correlated with biogenic precursors (e.g., monoterpenes). In urban air, it correlated instead with reactive anthropogenic tracers (e.g., trimethylbenzene). In mixed-source regions, the SOA formation did not correlate well with any single precursor, but could be predicted by multilinear regression from several precursors. Despite these correlations, the concentrations of speciated ambient VOCs could only explain approximately 10-50% of the total SOA formed from OH oxidation. In contrast, ambient VOCs could explain all of the SOA formation observed from O3 and NO3 oxidation. Evidence suggests that lower-volatility gases (semivolatile and intermediate-volatility organic

A CAM (continuous air monitor) sampler for collecting and assessing alpha-emitting aerosol particles

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

McFarland, A.R.; Bethel, E.L.; Ortiz, C.A.

1991-07-01

A new continuous air monitor (CAM) sampler for assessing alpha-emitting transuranic aerosol particles has been developed. The system has been designed to permit collection of particles that can potentially penetrate into the thoracic region of the human respiratory system. Wind tunnel testing of the sampler has been used to characterize the penetration of aerosol to the collection filter. Results show that greater than or equal to 50% of 10-micrograms aerodynamic equivalent diameter (AED) particles are collected by the filter at wind speeds of 0.3 to 2 m s-1 and at sampling flow rates of 28 to 113 L min-1 (1more » to 4 cfm). The deposition of 10-microns AED particles takes place primarily in the center of the filter, where the counting efficiency of the detector is highest.« less

Daily and hourly chemical impact of springtime transboundary aerosols on Japanese air quality

NASA Astrophysics Data System (ADS)

Moreno, T.; Kojima, T.; Amato, F.; Lucarelli, F.; de la Rosa, J.; Calzolai, G.; Nava, S.; Chiari, M.; Alastuey, A.; Querol, X.; Gibbons, W.

2013-02-01

The regular eastward drift of transboundary aerosol intrusions from the Asian mainland into the NW Pacific region has a pervasive impact on air quality in Japan, especially during springtime. Analysis of 24-h filter samples with Inductively Coupled Plasma Atomic Emission Spectroscopy (ICP-AES) and Mass Spectrometry (ICP-MS), and hourly Streaker with Particle Induced X-ray Emission (PIXE) samples collected continuously for six weeks reveal the chemistry of successive waves of natural mineral desert dust ("Kosa") and metalliferous sulphatic pollutants arriving in western Japan during spring 2011. The main aerosol sources recognised by Positive Matrix Factorization (PMF) analysis of Streaker data are mineral dust and fresh sea salt (both mostly in the coarser fraction PM2.5-10), As-bearing sulphatic aerosol (PM0.1-2.5), metalliferous sodic particulate matter (PM) interpreted as aged, industrially contaminated marine aerosol, and ZnCu-bearing aerosols. Whereas mineral dust arrivals are typically highly transient, peaking over a few hours, sulphatic intrusions build up and decline more slowly, and are accompanied by notable rises in ambient concentrations of metallic trace elements such as Pb, As, Zn, Sn and Cd. The magnitude of the loss in regional air quality due to the spread and persistence of pollution from mainland Asia is especially clear when cleansing oceanic air advects westward across Japan, removing the continental influence and reducing concentrations of the undesirable metalliferous pollutants by over 90%. Our new chemical database, especially the Streaker data, demonstrates the rapidly changing complexity of ambient air inhaled during these transboundary events, and implicates Chinese coal combustion as the main source of the anthropogenic aerosol component.

Raman microscopy of size-segregated aerosol particles, collected at the Sonnblick Observatory in Austria

NASA Astrophysics Data System (ADS)

Ofner, Johannes; Kasper-Giebl, Anneliese; Kistler, Magdalena; Matzl, Julia; Schauer, Gerhard; Hitzenberger, Regina; Lohninger, Johann; Lendl, Bernhard

2014-05-01

Size classified aerosol samples were collected using low pressure impactors in July 2013 at the high alpine background site Sonnnblick. The Sonnblick Observatory is located in the Austrian Alps, at the summit of Sonnblick 3100 m asl. Sampling was performed in parallel on the platform of the Observatory and after the aerosol inlet. The inlet is constructed as a whole air inlet and is operated at an overall sampling flow of 137 lpm and heated to 30 °C. Size cuts of the eight stage low pressure impactors were from 0.1 to 12.8 µm a.d.. Alumina foils were used as sample substrates for the impactor stages. In addition to the size classified aerosol sampling overall aerosol mass (Sharp Monitor 5030, Thermo Scientific) and number concentrations (TSI, CPC 3022a; TCC-3, Klotz) were determined. A Horiba LabRam 800HR Raman microscope was used for vibrational mapping of an area of about 100 µm x 100 µm of the alumina foils at a resolution of about 0.5 µm. The Raman microscope is equipped with a laser with an excitation wavelength of 532 nm and a grating with 300 gr/mm. Both optical images and the related chemical images were combined and a chemometric investigation of the combined images was done using the software package Imagelab (Epina Software Labs). Based on the well-known environment, a basic assignment of Raman signals of single particles is possible at a sufficient certainty. Main aerosol constituents e.g. like sulfates, black carbon and mineral particles could be identified. First results of the chemical imaging of size-segregated aerosol, collected at the Sonnblick Observatory, will be discussed with respect to standardized long-term measurements at the sampling station. Further, advantages and disadvantages of chemical imaging with subsequent chemometric investigation of the single images will be discussed and compared to the established methods of aerosol analysis. The chemometric analysis of the dataset is focused on mixing and variation of single compounds at

PIXE Analysis of Atmospheric Aerosol Samples Collected in the Adirondack Mountains

NASA Astrophysics Data System (ADS)

Yoskowitz, Josh; Ali, Salina; Nadareski, Benjamin; Safiq, Alexandrea; Smith, Jeremy; Labrake, Scott; Vineyard, Michael

2013-10-01

We have performed an elemental analysis of atmospheric aerosol samples collected at Piseco Lake in Upstate New York using proton induced x-ray emission spectroscopy (PIXE). This work is part of a systematic study of airborne pollution in the Adirondack Mountains. Of particular interest is the sulfur content that can contribute to acid rain, a well-documented problem in the Adirondacks. We used a nine-stage cascade impactor to collect the samples and distribute the particulate matter onto Kapton foils by particle size. The PIXE experiments were performed with 2.2-MeV proton beams from the 1.1-MV pelletron accelerator in the Union College Ion-Beam Analysis Laboratory. X-Ray energy spectra were measured with a silicon drift detector and analyzed with GUPIX software to determine the elemental concentrations of the aerosols. A broad range of elements from silicon to zinc were detected with significant sulfur concentrations measured for particulate matter between 0.25 and 0.5 μm in size. The PIXE analysis will be described and preliminary results will be presented.

Aerosol sampling system for collection of Capstone depleted uranium particles in a high-energy environment.

PubMed

Holmes, Thomas D; Guilmette, Raymond A; Cheng, Yung Sung; Parkhurst, Mary Ann; Hoover, Mark D

2009-03-01

The Capstone Depleted Uranium (DU) Aerosol Study was undertaken to obtain aerosol samples resulting from a large-caliber DU penetrator striking an Abrams or Bradley test vehicle. The sampling strategy was designed to (1) optimize the performance of the samplers and maintain their integrity in the extreme environment created during perforation of an armored vehicle by a DU penetrator, (2) collect aerosols as a function of time post perforation, and (3) obtain size-classified samples for analysis of chemical composition, particle morphology, and solubility in lung fluid. This paper describes the experimental setup and sampling methodologies used to achieve these objectives. Custom-designed arrays of sampling heads were secured to the inside of the target in locations approximating the breathing zones of the crew locations in the test vehicles. Each array was designed to support nine filter cassettes and nine cascade impactors mounted with quick-disconnect fittings. Shielding and sampler placement strategies were used to minimize sampler loss caused by the penetrator impact and the resulting fragments of eroded penetrator and perforated armor. A cyclone train was used to collect larger quantities of DU aerosol for measurement of chemical composition and solubility. A moving filter sample was used to obtain semicontinuous samples for DU concentration determination. Control for the air samplers was provided by five remotely located valve control and pressure monitoring units located inside and around the test vehicle. These units were connected to a computer interface chassis and controlled using a customized LabVIEW engineering computer control program. The aerosol sampling arrays and control systems for the Capstone study provided the needed aerosol samples for physicochemical analysis, and the resultant data were used for risk assessment of exposure to DU aerosol.

Aerosol Sampling System for Collection of Capstone Depleted Uranium Particles in a High-Energy Environment

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

Holmes, Thomas D.; Guilmette, Raymond A.; Cheng, Yung-Sung

2009-03-01

The Capstone Depleted Uranium Aerosol Study was undertaken to obtain aerosol samples resulting from a kinetic-energy cartridge with a large-caliber depleted uranium (DU) penetrator striking an Abrams or Bradley test vehicle. The sampling strategy was designed to (1) optimize the performance of the samplers and maintain their integrity in the extreme environment created during perforation of an armored vehicle by a DU penetrator, (2) collect aerosols as a function of time post-impact, and (3) obtain size-classified samples for analysis of chemical composition, particle morphology, and solubility in lung fluid. This paper describes the experimental setup and sampling methodologies used tomore » achieve these objectives. Custom-designed arrays of sampling heads were secured to the inside of the target in locations approximating the breathing zones of the vehicle commander, loader, gunner, and driver. Each array was designed to support nine filter cassettes and nine cascade impactors mounted with quick-disconnect fittings. Shielding and sampler placement strategies were used to minimize sampler loss caused by the penetrator impact and the resulting fragments of eroded penetrator and perforated armor. A cyclone train was used to collect larger quantities of DU aerosol for chemical composition and solubility. A moving filter sample was used to obtain semicontinuous samples for depleted uranium concentration determination. Control for the air samplers was provided by five remotely located valve control and pressure monitoring units located inside and around the test vehicle. These units were connected to a computer interface chassis and controlled using a customized LabVIEW engineering computer control program. The aerosol sampling arrays and control systems for the Capstone study provided the needed aerosol samples for physicochemical analysis, and the resultant data were used for risk assessment of exposure to DU aerosol.« less

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

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

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

2006-03-16

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

Aerosol Lidar and MODIS Satellite Comparisons for Future Aerosol Loading Forecast

NASA Technical Reports Server (NTRS)

DeYoung, Russell; Szykman, James; Severance, Kurt; Chu, D. Allen; Rosen, Rebecca; Al-Saadi, Jassim

2006-01-01

Knowledge of the concentration and distribution of atmospheric aerosols using both airborne lidar and satellite instruments is a field of active research. An aircraft based aerosol lidar has been used to study the distribution of atmospheric aerosols in the California Central Valley and eastern US coast. Concurrently, satellite aerosol retrievals, from the MODIS (Moderate Resolution Imaging Spectroradiometer) instrument aboard the Terra and Aqua satellites, were take over the Central Valley. The MODIS Level 2 aerosol data product provides retrieved ambient aerosol optical properties (e.g., optical depth (AOD) and size distribution) globally over ocean and land at a spatial resolution of 10 km. The Central Valley topography was overlaid with MODIS AOD (5x5 sq km resolution) and the aerosol scattering vertical profiles from a lidar flight. Backward air parcel trajectories for the lidar data show that air from the Pacific and northern part of the Central Valley converge confining the aerosols to the lower valley region and below the mixed layer. Below an altitude of 1 km, the lidar aerosol and MODIS AOD exhibit good agreement. Both data sets indicate a high presence of aerosols near Bakersfield and the Tehachapi Mountains. These and other results to be presented indicate that the majority of the aerosols are below the mixed layer such that the MODIS AOD should correspond well with surface measurements. Lidar measurements will help interpret satellite AOD retrievals so that one day they can be used on a routine basis for prediction of boundary layer aerosol pollution events.

Characterization of the inorganic aerosol in Barcelona site during DAURE 2009 field campaigns

NASA Astrophysics Data System (ADS)

Plaza, Javier; Gómez-Moreno, Francisco J.; Aránzazu Revuelta, M.; Coz, Esther; Moreno, Natalia; Pujadas, Manuel; Artíñano, Begoña.

2010-05-01

Inorganic compounds account for a significant mass of the ambient aerosol. However this contribution varies with time and aerosol size fraction, depending on the influence of source emissions and ambient conditions, which can be relevant in the formation processes of secondary species. Time series of particulate nitrate, 10 m time resolution, have been obtained during the February-March and July 2009 DAURE (Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean) field campaigns in the urban area of Barcelona by means of an R&P8400N monitor. Meteorological conditions during these periods were relevant for the photochemical formation and accumulation of secondary species. Ambient concentrations were higher in winter, specially coinciding with development of atmospheric stagnant episodes that enhanced the accumulation of pollutants including particulate nitrate that reached concentrations of 25 µgm-3 in some occasions, day or night, under these conditions. High humidity periods favored in occasions the formation of nitrates at submicronic scale. Variations in wind direction resulted in transport of particulate nitrate from near emission areas. Size segregated aerosol was sampled during the winter campaign with a micro-orifice uniform deposit impactor (MOUDI) using eleven size stages with aluminum substrates and a quartz fiber backup filter. Samples were collected twice per day for day/night periods. The first sampling period tried to collect secondary aerosol as it started after the early morning emission period. The second sample collected the night aerosol and the emission period. Soluble ions (sulfate, nitrate, ammonium and calcium) were later analyzed by IC. The nitrate mass was concentrated in two modes, the accumulation one around 0.75 µm and the coarse one around 3.90 µm. The sulfate and ammonium masses were concentrated in the accumulation mode, around 0.50 µm, although a small peak close to 5 µm

Particle size distribution of the radon progeny and ambient aerosols in the Underground Tourist Route "Liczyrzepa" Mine in Kowary Adit

NASA Astrophysics Data System (ADS)

Wołoszczuk, Katarzyna; Skubacz, Krystian

2018-01-01

Central Laboratory for Radiological Protection, in cooperation with Central Mining Institute performed measurements of radon concentration in air, potential alpha energy concentration (PAEC), particle size distribution of the radon progeny and ambient aerosols in the Underground Tourist-Educational Route "Liczyrzepa" Mine in Kowary Adit. A research study was developed to investigate the appropriate dose conversion factors for short-lived radon progeny. The particle size distribution of radon progeny was determined using Radon Progeny Particle Size Spectrometer (RPPSS). The device allows to receive the distribution of PAEC in the particle size range from 0.6 nm to 2494 nm, based on their activity measured on 8 stages composed of impaction plates or diffusion screens. The measurements of the ambient airborne particle size distribution were performed in the range from a few nanometres to about 20 micrometres using Aerodynamic Particle Sizer (APS) spectrometer and the Scanning Mobility Particle Sizer Spectrometer (SMPS).

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

NASA Technical Reports Server (NTRS)

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

2012-01-01

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

Aerosol Particle Interfacial Thermodynamics and Phase Partitioning Measurements Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Dutcher, Cari; Metcalf, Andrew

2015-03-01

Secondary organic aerosol particles are nearly ubiquitous in the atmosphere and yet there remain 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. Interfacial properties affect the ambient aerosol morphology, or internal structure of the particle, which in turn can affect the way a particle interacts with an environment of condensable clusters and organic vapors. To improve our ability to accurately predict ambient aerosol morphology, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Unfortunately, many techniques employed to measure interfacial properties do so in bulk solutions or in the presence of a ternary (e.g. solid) phase. 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 or interfacial tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred.

Predicting ambient aerosol thermal-optical reflectance (TOR) measurements from infrared spectra: organic carbon

NASA Astrophysics Data System (ADS)

Dillner, A. M.; Takahama, S.

2015-03-01

Organic carbon (OC) can constitute 50% or more of the mass of atmospheric particulate matter. Typically, organic carbon is measured from a quartz fiber filter that has been exposed to a volume of ambient air and analyzed using thermal methods such as thermal-optical reflectance (TOR). Here, methods are presented that show the feasibility of using Fourier transform infrared (FT-IR) absorbance spectra from polytetrafluoroethylene (PTFE or Teflon) filters to accurately predict TOR OC. This work marks an initial step in proposing a method that can reduce the operating costs of large air quality monitoring networks with an inexpensive, non-destructive analysis technique using routinely collected PTFE filter samples which, in addition to OC concentrations, can concurrently provide information regarding the composition of organic aerosol. This feasibility study suggests that the minimum detection limit and errors (or uncertainty) of FT-IR predictions are on par with TOR OC such that evaluation of long-term trends and epidemiological studies would not be significantly impacted. To develop and test the method, FT-IR absorbance spectra are obtained from 794 samples from seven Interagency Monitoring of PROtected Visual Environment (IMPROVE) sites collected during 2011. Partial least-squares regression is used to calibrate sample FT-IR absorbance spectra to TOR OC. The FTIR spectra are divided into calibration and test sets by sampling site and date. The calibration produces precise and accurate TOR OC predictions of the test set samples by FT-IR as indicated by high coefficient of variation (R2; 0.96), low bias (0.02 μg m-3, the nominal IMPROVE sample volume is 32.8 m3), low error (0.08 μg m-3) and low normalized error (11%). These performance metrics can be achieved with various degrees of spectral pretreatment (e.g., including or excluding substrate contributions to the absorbances) and are comparable in precision to collocated TOR measurements. FT-IR spectra are also

Characterization of Secondary Organic Aerosol Precursors Using Two-Dimensional Gas-Chromatography

NASA Astrophysics Data System (ADS)

Roskamp, M.; Lou, W.; Pankow, J. F.; Harley, P. C.; Turnipseed, A.; Barsanti, K. C.

2012-12-01

The oxidation of volatile organic compounds (VOCs) plays a role in both regional and global air quality. However, field and laboratory research indicate that the body of knowledge around the identities, quantities and oxidation processes of these compounds in the ambient atmosphere is still incomplete (e.g., Goldstein & Galbally, 2007; Robinson et al., 2009). VOCs emitted to the atmosphere largely are of biogenic origin (Guenther et al., 2006), and many studies of ambient secondary organic aerosol (SOA) suggest that SOA is largely of biogenic origin (albeit closely connected to anthropogenic activities, e.g., de Gouw and Jimenez, 2009). Accurate modeling of SOA levels and properties will require a more complete understanding of biogenic VOCs (BOCs) and their atmospheric oxidation products. For example, satellite measurements indicate that biogenic VOC emissions are two to three times greater than levels currently included in models (Heald et al., 2010). Two-dimensional gas chromatography (GC×GC) is a powerful analytical technique that shows much promise in advancing the state-of-knowledge regarding BVOCs and their role in SOA formation. In this work, samples were collected during BEACHON-RoMBAS (Bio-hydro-atmosphere Interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study) in July and August of 2011. The field site was a Ponderosa Pine forest near Woodland, CO, inside the Manitou Experimental Forest, which is operated by the US Forest Service. The area is characteristic of the central Rocky Mountains and trace gas monitoring indicates that little anthropogenic pollution is transported from the nearby urban areas (Kim et al. 2010 and references therein). Ambient and enclosure samples were collected on ATD (adsorption/thermal desorption) cartridges and analyzed for BVOCs using two-dimensional gas chromatography (GC×GC) with time of flight mass spectrometry (TOFMS) and flame ionized detection (FID). Measurements of

Inorganic ions in ambient fine particles over a National Park in central India: Seasonality, dependencies between SO42-, NO3-, and NH4+, and neutralization of aerosol acidity

NASA Astrophysics Data System (ADS)

Kumar, Samresh; Sunder Raman, Ramya

2016-10-01

Twelve hour integrated ambient fine particles (PM2.5) were collected over an Van Vihar National Park (VVNP), in Bhopal, Central India. Samples were collected on filter substrates every-other-day for two years (2012 and 2013). In addition to PM2.5 mass concentration, water soluble inorganic ions (WSIIs) were also measured. Further, on-site meteorological parameters including temperature, wind speed, wind direction, relative humidity, rainfall and atmospheric pressure were recorded. During 2012, the average PM2.5 concentration was 40 ± 31 μgm-3 while during 2013 it was 48 ± 50 μgm-3. Further, in about 20% of the samples the 12 h integrated fine PM mass exceeded the daily (24 h) average standards (60 μgm-3). This observation suggests that the PM2.5 mass concentration at the study site is likely to be in violation of the National Ambient Air Quality Standard (NAAQS), India. During the study period the sum of three major ions (SO42-, NO3-, and NH4+) accounted for 19.4% of PM2.5 mass on average. Air parcel back trajectory ensembles revealed that emissions from thermal power plants were likely to be the main regional source of particulate SO42- and NO3- measured over VVNP. Further, local traffic activities appeared to have no significant impact on the concentrations of PM2.5 and its WSIIs constituents, as revealed by a day-of-the-week analysis. PM2.5 mass, SO42-, NO3-, and NH4+ showed a pronounced seasonal trend with winter (Jan, Feb) and post-monsoon (Oct, Nov, Dec) highs and pre-monsoon (Mar, Apr, May) and monsoon (Jun, Jul, Aug, Sep) lows, during both 2012 and 2013. Further, when the sum of SO42- and NO3- constituted greater than 90% of water soluble inorganic anions by mass, they were linearly dependent on one another and moderately anti-correlated (r2 = 0.60). The molar ratios of NH4+ and non-sea salt SO42- were examined to understand the aerosol neutralization mechanisms and particulate NO3- formation. An assessment of these ratios and subsequent analyses

Chemical characteristics of size-resolved aerosols in winter in Beijing.

PubMed

Sun, Kang; Qu, Yu; Wu, Qiong; Han, Tingting; Gu, Jianwei; Zhao, Jingjing; Sun, Yele; Jiang, Qi; Gao, Ziqi; Hu, Min; Zhang, Yuanhang; Lu, Keding; Nordmann, Stephan; Cheng, Yafang; Hou, Li; Ge, Hui; Furuuchi, Masami; Hata, Mitsuhiko; Liu, Xingang

2014-08-01

Size-resolved aerosols were continuously collected by a Nano Sampler for 13 days at an urban site in Beijing during winter 2012 to measure the chemical composition of ambient aerosol particles. Data collected by the Nano Sampler and an ACSM (Aerodyne Aerosol Chemical Speciation Monitor) were compared. Between the data sets, similar trends and strong correlations were observed, demonstrating the validity of the Nano Sampler. PM₁₀ and PM₂.₅ concentrations during the measurement were 150.5 ± 96.0 μg/m³ (mean ± standard variation) and 106.9 ± 71.6 μg/m³, respectively. The PM₂.₅/PM₁₀ ratio was 0.70 ± 0.10, indicating that PM₂.₅ dominated PM₁₀. The aerosol size distributions showed that three size bins of 0.5-1, 1-2.5 and 2.5-10 μm contributed 21.8%, 23.3% and 26.0% to the total mass concentration (TMC), respectively. OM (organic matter) and SIA (secondary ionic aerosol, mainly SO₄(2-), NO₃(-) and NH₄(+)) were major components of PM₂.₅. Secondary compounds (SIA and secondary organic carbon) accounted for half of TMC (about 49.8%) in PM₂.₅, and suggested that secondary aerosols significantly contributed to the serious particulate matter pollution observed in winter. Coal burning, biomass combustion, vehicle emissions and SIA were found to be the main sources of PM₂.₅. Mass concentrations of water-soluble ions and undetected materials, as well as their fractions in TMC, strikingly increased with deteriorating particle pollution conditions, while OM and EC (elemental carbon) exhibited different variations, with mass concentrations slightly increasing but fractions in TMC decreasing. Copyright © 2014. Published by Elsevier B.V.

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

Remote Sensing of Aerosol and Non-Aerosol Absorption

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Dubovik, O.; Holben, B. N.; Remer, L. A.; Tanre, D.; Lau, William K. M. (Technical Monitor)

2001-01-01

Remote sensing of aerosol from the new satellite instruments (e.g. MODIS from Terra) and ground based radiometers (e.g. the AERONET) provides the opportunity to measure the absorption characteristics of the ambient undisturbed aerosol in the entire atmospheric column. For example Landsat and AERONET data are used to measure spectral absorption of sunlight by dust from West Africa. Both Application of the Landsat and AERONET data demonstrate that Saharan dust absorption of solar radiation is several times smaller than the current international standards. This is due to difficulties of measuring dust absorption in situ, and due to the often contamination of dust properties by the presence of air pollution or smoke. We use the remotely sensed aerosol absorption properties described by the spectral sin le scattering albedo, together with statistics of the monthly optical thickness for the fine and coarse aerosol derived from the MODIS data. The result is an estimate of the flux of solar radiation absorbed by the aerosol layer in different regions around the globe where aerosol is prevalent. If this aerosol forcing through absorption is not included in global circulation models, it may be interpreted as anomalous absorption in these regions. In a preliminary exercise we also use the absorption measurements by AERONET, to derive the non-aerosol absorption of the atmosphere in cloud free conditions. The results are obtained for the atmospheric windows: 0.44 microns, 0.66 microns, 0.86 microns and 1.05 microns. In all the locations over the land and ocean that were tested no anomalous absorption in these wavelengths, was found within absorption optical thickness of +/- 0.005.

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.

Submicron aerosol organic functional groups, ions, and water content at the Centreville SEARCH site (Alabama), during SOAS campaign

NASA Astrophysics Data System (ADS)

Ruggeri, G.; Ergin, G.; Modini, R. L.; Takahama, S.

2013-12-01

The SOAS campaign was conducted from June 1 to July 15 of 2013 in order to understand the relationship between biogenic and anthropogenic emissions in the South East US1,2. In this study, the organic and inorganic composition of submicron aerosol in the Centreville SEARCH site was measured by Fourier Transform Infrared Spectroscopy (FTIR) and the Ambient Ion Monitor (AIM; URG Corporation), whereas the aerosol water content was measured with a Dry Ambient Aerosol Size Spectrometer (DAASS)3. Organic functional group analysis was performed on PM1 aerosol selected by cyclone and collected on teflon filters with a time resolution of 4-12 hours, using one inlet heated to 50 °C and the other operated either at ambient temperature or 70 °C 4. The AIM measured both condensed and gas phase composition with a time resolution of 1 hour, providing partitioning behavior of inorganic species such as NH3/NH4+, HNO3/NO3-. These measurements collectively permit calculation of pure-component vapor pressures of candidate organic compounds and activity coefficients of interacting components in the condensed phase, using models such as SIMPOL.15, E-AIM6, and AIOMFAC7. From these results, the water content of the aerosol is predicted, and a comparison between modeled and measured partitioning of inorganic compounds and water vapor are discussed, in addition to organic aerosol volatility prediction based on functional group analysis. [1]- Goldstein, A.H., et al., Biogenic carbon and anthropogenic pollutants combine to form a cooling haze over the southeastern United States. Proceedings of the National Academy of Sciences of the United States of America, 2009. 106(22), 8835-8840. [2]- Carlton, A.G., Turpin, B.J., 2013. Particle partitioning potential of organic compounds is highest in the Eastern US and driven by anthropogenic water. Atmospheric Chemistry and Physics Discussions 13, 12743-12770. [3]- Khlystov, A., Stanier, C.O., Takahama, S., Pandis, S.N., 2005. Water content of ambient

Aerosol-Assisted Solid Debris Collection for the National Ignition Facility

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

Nelson, S L; Shaughnessy, D A; Moody, K J

2010-05-21

The National Ignition Facility (NIF) has been completed and has made its first shots on-target. While upcoming experiments will be focused on achieving ignition, a variety of subsequent experiments are planned for the facility, including measurement of cross sections, astrophysical measurements, and investigation of hydrodynamic instability in the target capsule. In order to successfully execute several of these planned experiments, the ability to collect solid debris following a NIF capsule shot will be required. The ability to collect and analyze solid debris generated in a shot at the National Ignition Facility (NIF) will greatly expand the number of nuclear reactionsmore » studied for diagnostic purposes. Currently, reactions are limited to only those producing noble gases for cryogenic collection and counting with the Radchem Apparatus for Gas Sampling (RAGS). The radchem solid collection diagnostic has already been identified by NIF to be valuable for the determination and understanding of mix generated in the target capsule's ablation. LLNL is currently developing this solid debris collection capability at NIF, and is in the stage of testing credible designs. Some of these designs explore the use of x-ray generated aerosols to assist in collection of solid debris. However, the variety of harsh experimental conditions this solid collection device will encounter in NIF are challenging to replicate. Experiments performed by Gary Grim et al. at Sandia National Laboratory's RHEPP1 facility have shown that ablation causes a cloud of material removed from an exposed surface to move normal to and away from the surface. This ablation is certain to be a concern in the NIF target chamber from the prompt x-rays, gamma rays, etc. generated in the shot. The cloud of ablated material could interfere with the collection of the desired reaction debris by slowing down the debris so that the kinetic energy is too low to allow implantation, or by stopping the debris from

Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Hansen, Kristen J.

An integrated sampling and supercritical fluid extraction (SFE) cell has been designed for whole-sample analysis of organic compounds on tropospheric aerosol particles. The low-volume extraction cell has been interfaced with a sampling manifold for aerosol particle collection in the field. After sample collection, the entire SFE cell was coupled to a gas chromatograph; after on-line extraction, the cryogenically -focused sample was separated and the volatile compounds detected with either a mass spectrometer or a flame ionization detector. A 20-minute extraction at 450 atm and 90 ^circC with pure supercritical CO _2 is sufficient for quantitative extraction of most volatile compounds in aerosol particle samples. A comparison between SFE and thermal desorption, the traditional whole-sample technique for analyses of this type, was performed using ambient aerosol particle samples, as well as samples containing known amounts of standard analytes. The results of these studies indicate that SFE of atmospheric aerosol particles provides quantitative measurement of several classes of organic compounds. SFE provides information that is complementary to that gained by the thermal desorption analysis. The results also indicate that SFE with CO _2 can be validated as an alternative to thermal desorption for quantitative recovery of several organic compounds. In 1989, the organic constituents of atmospheric aerosol particles collected at Niwot Ridge, Colorado, along with various physical and meteorological data, were measured during a collaborative field study. Temporal changes in the composition of samples collected during summertime at the rural site were studied. Thermal desorption-GC/FID was used to quantify selected compounds in samples collected during the field study. The statistical analysis of the 1989 Niwot Ridge data set is presented in this work. Principal component analysis was performed on thirty-one variables selected from the data set in order to ascertain

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Organics, Meteoritic Material, and other Elements in High Altitude Aerosols

NASA Technical Reports Server (NTRS)

Mahoney, M.; Murphy, D. M.; Thomson, D. S.

1998-01-01

Recent in situ measurements of the chemical composition of single aerosol particles at altitudes up to 19 km have revealed a number of surprising features about ambient particles. Upper tropospheric aerosols in the study region often contained more organic material than sulfate.

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

NASA Astrophysics Data System (ADS)

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

2016-01-01

3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed-layer aerosol extinction. Aerosol loading (dry extinction) was found to be the predominant source, accounting for 88 % on average of the measured spatial variability in ambient extinction, with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite-modeling assimilation products that are able to capture these components of the aerosol optical depth (AOD)-PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day to day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015), who determined that the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.

VERSATILE AEROSOL CONCENTRATION ENRICHMENT SYSTEM (VACES) FOR SIMULTANEOUS IN-VIVO AND IN-VITRO EVALUATION OF TOXIC EFFECTS OF ULTRAFINE, FINE, AND COARSE AMBIENT PARTICLES. PART II. FIELD EVALUATION. (R826232)

EPA Science Inventory

Abstract

This study presents results from a field evaluation of a mobile versatile aerosol concentration enrichment system (VACES), designed to enhance the ambient concentrations of ultrafine (less than 0.18 Aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing in Guangzhou during the 2006 Pearl River Delta campaign.

PubMed

Jung, Jinsang; Lee, Hanlim; Kim, Young J; Liu, Xingang; Zhang, Yuanhang; Gu, Jianwei; Fan, Shaojia

2009-08-01

Optical and chemical aerosol measurements were obtained from 2 to 31 July 2006 at an urban site in the metropolitan area of Guangzhou (China) as part of the Program of Regional Integrated Experiment of Air Quality over Pearl River Delta (PRIDE-PRD2006) to investigate aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing. During the PRIDE-PRD2006 campaign, the average contributions of ammonium sulfate, organic mass by carbon (OMC), elemental carbon (EC), and sea salt (SS) to total PM(2.5) mass were measured to be 36.5%, 5.7%, 27.1%, 7.8%, and 3.7%, respectively. Compared with the clean marine period, (NH(4))(2)SO(4), NH(4)NO(3), and OMC were all greatly enhanced (by up to 430%) during local haze periods via the accumulation of a secondary aerosol component. The OMC dominance increased when high levels of biomass burning influenced the measurement site while (NH(4))(2)SO(4) and OMC did when both biomass burning and industrial emissions influenced it. The effect of aerosol water content on the total light-extinction coefficient was estimated to be 34.2%, of which 25.8% was due to aerosol water in (NH(4))(2)SO(4), 5.1% that in NH(4)NO(3), and 3.3% that in SS. The average mass-scattering efficiency (MSE) of PM(10) particles was determined to be 2.2+/-0.6 and 4.6+/-1.7m(2)g(-1) under dry (RH<40%) and ambient conditions, respectively. The average single-scattering albedo (SSA) was 0.80+/-0.08 and 0.90+/-0.04 under dry and ambient conditions, respectively. Not only are the extinction and scattering coefficients greatly enhanced by aerosol water content, but MSE and SSA are also highly sensitive. It can be concluded that sulfate and carbonaceous aerosol, as well as aerosol water content, play important roles in the processes that determine visibility impairment and radiative forcing in the ambient atmosphere of the Guangzhou urban area.

Combustion Organic Aerosol as Cloud Condensation Nuclei in Ship Tracks.

NASA Astrophysics Data System (ADS)

Russell, Lynn M.; Noone, Kevin J.; Ferek, Ronald J.; Pockalny, Robert A.; Flagan, Richard C.; Seinfeld, John H.

2000-08-01

Polycyclic aromatic hydrocarbons (PAHs) have been sampled in marine stratiform clouds to identify the contribution of anthropogenic combustion emissions in activation of aerosol to cloud droplets. The Monterey Area Ship Track experiment provided an opportunity to acquire data on the role of organic compounds in ambient clouds and in ship tracks identified in satellite images. Identification of PAHs in cloud droplet residual samples indicates that several PAHs are present in cloud condensation nuclei in anthropogenically influenced air and do result in activated droplets in cloud. These results establish the presence of combustion products, such as PAHs, in submicrometer aerosols in anthropogenically influenced marine air, with enhanced concentrations in air polluted by ship effluent. The presence of PAHs in droplet residuals in anthropogenically influenced air masses indicates that some fraction of those combustion products is present in the cloud condensation nuclei that activate in cloud. Although a sufficient mass of droplet residuals was not collected to establish a similar role for organics from measurements in satellite-identified ship tracks, the available evidence from the fraction of organics present in the interstitial aerosol is consistent with part of the organic fraction partitioning to the droplet population. In addition, the probability that a compound will be found in cloud droplets rather than in the unactivated aerosol and the compound's water solubility are compared. The PAHs studied are only weakly soluble in water, but most of the sparse data collected support more soluble compounds having a higher probability of activation.

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

NASA Astrophysics Data System (ADS)

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

2013-05-01

Ambient wintertime background urban aerosol in Cork city, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the ca. 1 350 000 single particles characterized by an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally mixed to different proportions with elemental carbon (EC), sulphate and nitrate, while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS) and was also found to comprise organic aerosol as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix, and a five-factor solution was found to describe the variance in the data well. Specifically, "hydrocarbon-like" organic aerosol (HOA) comprised 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA) comprised 18%, "biomass burning" organic aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "peat and coal" organic aerosol (PCOA) comprised 21%, and finally a species type characterized by primary {m/z} peaks at 41 and 55, similar to previously reported "cooking" organic aerosol (COA), but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosol mass and non-refractory total PM1, respectively).

Sugars in Antarctic aerosol

NASA Astrophysics Data System (ADS)

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

2015-10-01

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

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

NASA Astrophysics Data System (ADS)

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

2012-11-01

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

FRACTIONAL AEROSOL FILTRATION EFFICIENCY OF IN-DUCT VENTILATION AIR CLEANERS

EPA Science Inventory

The filtration efficiency of ventilation air cleaners is highly particle-size dependent over the 0.01 to 3 μm diameter size range. Current standardized test methods, which determine only overall efficiencies for ambient aerosol or other test aerosols, provide data of limited util...

The impact of changing surface ocean conditions on the dissolution of aerosol iron

NASA Astrophysics Data System (ADS)

Fishwick, Matthew P.; Sedwick, Peter N.; Lohan, Maeve C.; Worsfold, Paul J.; Buck, Kristen N.; Church, Thomas M.; Ussher, Simon J.

2014-11-01

The proportion of aerosol iron (Fe) that dissolves in seawater varies greatly and is dependent on aerosol composition and the physicochemical conditions of seawater, which may change depending on location or be altered by global environmental change. Aerosol and surface seawater samples were collected in the Sargasso Sea and used to investigate the impact of these changing conditions on aerosol Fe dissolution in seawater. Our data show that seawater temperature, pH, and oxygen concentration, within the range of current and projected future values, had no significant effect on the dissolution of aerosol Fe. However, the source and composition of aerosols had the most significant effect on the aerosol Fe solubility, with the most anthropogenically influenced samples having the highest fractional solubility (up to 3.2%). The impact of ocean warming and acidification on aerosol Fe dissolution is therefore unlikely to be as important as changes in land usage and fossil fuel combustion. Our experimental results also reveal important changes in the size distribution of soluble aerosol Fe in solution, depending on the chemical conditions of seawater. Under typical conditions, the majority (77-100%) of Fe released from aerosols into ambient seawater existed in the colloidal (0.02-0.4 µm) size fraction. However, in the presence of a sufficient concentration of strong Fe-binding organic ligands (10 nM) most of the aerosol-derived colloidal Fe was converted to soluble Fe (<0.02 µm). This finding highlights the potential importance of organic ligands in retaining aerosol Fe in a biologically available form in the surface ocean.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores: OPTICAL AND CHEMICAL PROPERTIES OF BROWN CARBON AEROSOLS

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

Bluvshtein, Nir; Lin, Peng; Flores, J. Michel

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders ofmore » magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.« less

On the Implications of aerosol liquid water and phase separation for modeled organic aerosol mass

EPA Science Inventory

Current chemical transport models assume that organic aerosol (OA)-forming compounds partition mostly to a water-poor, organic-rich phase in accordance with their vapor pressures. However, in the southeast United States, a significant fraction of ambient organic compounds are wat...

Elucidating the Chemical Complexity of Organic Aerosol Constituents Measured During the Southeastern Oxidant and Aerosol Study (SOAS)

NASA Astrophysics Data System (ADS)

Yee, L.; Isaacman, G. A.; Spielman, S. R.; Worton, D. R.; Zhang, H.; Kreisberg, N. M.; Wilson, K. R.; Hering, S. V.; Goldstein, A. H.

2013-12-01

Thousands of volatile organic compounds are uniquely created in the atmosphere, many of which undergo chemical transformations that result in more highly-oxidized and often lower vapor pressure species. These species can contribute to secondary organic aerosol, a complex mixture of organic compounds that is still not chemically well-resolved. Organic aerosol collected on filters taken during the Southeastern Oxidant and Aerosol Study (SOAS) constitute hundreds of unique chemical compounds. Some of these include known anthropogenic and biogenic tracers characterized using standardized analytical techniques (e.g. GC-MS, UPLC, LC-MS), but the majority of the chemical diversity has yet to be explored. By employing analytical techniques involving sample derivatization and comprehensive two-dimensional gas chromatography (GC x GC) with high-resolution-time-of-flight mass spectrometry (HR-ToF-MS), we elucidate the chemical complexity of the organic aerosol matrix along the volatility and polarity grids. Further, by utilizing both electron impact (EI) and novel soft vacuum ultraviolet (VUV) ionization mass spectrometry, a greater fraction of the organic mass is fully speciated. The GC x GC-HR-ToF-MS with EI/VUV technique efficiently provides an unprecedented level of speciation for complex ambient samples. We present an extensive chemical characterization and quantification of organic species that goes beyond typical atmospheric tracers in the SOAS samples. We further demonstrate that complex organic mixtures can be chemically deconvoluted by elucidation of chemical formulae, volatility, functionality, and polarity. These parameters provide insight into the sources (anthropogenic vs. biogenic), chemical processes (oxidation pathways), and environmental factors (temperature, humidity), controlling organic aerosol growth in the Southeastern United States.

A study of the physical, chemical, and optical properties of ambient aerosol particles in Southeast Asia during hazy and nonhazy days

NASA Astrophysics Data System (ADS)

See, S. W.; Balasubramanian, R.; Wang, W.

2006-05-01

Many Southeast Asian countries have been constantly plagued by recurring smoke haze episodes as a result of traditional slash-and-burn practices in agricultural areas to clear crop lands or uncontrolled forest fires. However, our current knowledge on the physiochemical and optical properties of ambient aerosols associated with regional haze phenomenon is still fairly limited. Therefore a comprehensive field study was carried out in Singapore from March 2001 to March 2002 under varying weather conditions to gain a better understanding of the characteristics. The physical (size distribution of mass and number concentrations), chemical (mass concentrations of chemical components: 14 ions, 24 metals, elemental carbon (EC) and organic carbon (OC)), and optical (light absorption (bap) and scattering (bsp) by particles) characteristics of ambient aerosol particles were investigated. The results are reported separately for clear and hazy days by categorizing the days as clear or hazy on the basis of visibility data. It was observed that the average concentrations of PM2.5 and most chemical components increased approximately by a factor of 2 on hazy days. Backward air trajectories together with the hot spot distributions in the region indicated that the degradation in Singapore's air quality on hazy days was attributable to large-scale forest fires in Sumatra. This visibility degradation was quantitatively measured on the basis of the light absorption and scattering by particles. As expected, scattering rather than absorption controlled atmospheric visibility, and PM2.5 particles present on hazy days were more efficient at scattering light than those found on clear days.

Near real time vapor detection and enhancement using aerosol adsorption

DOEpatents

Novick, Vincent J.; Johnson, Stanley A.

1999-01-01

A vapor sample detection method where the vapor sample contains vapor and ambient air and surrounding natural background particles. The vapor sample detection method includes the steps of generating a supply of aerosol that have a particular effective median particle size, mixing the aerosol with the vapor sample forming aerosol and adsorbed vapor suspended in an air stream, impacting the suspended aerosol and adsorbed vapor upon a reflecting element, alternatively directing infrared light to the impacted aerosol and adsorbed vapor, detecting and analyzing the alternatively directed infrared light in essentially real time using a spectrometer and a microcomputer and identifying the vapor sample.

VERSATILE AEROSOL CONCENTRATION ENRICHMENT SYSTEM (VACES) FOR SIMULTANEOUS IN VIVO AND IN VITRO EVALUATION OF TOXIC EFFECTS OF ULTRAFINE, FINE AND COARSE AMBIENT PARTICLES. PART II: FIELD EVALUATION. (R827352C001)

EPA Science Inventory

This study presents results from a field evaluation of a mobile versatile aerosol concentration enrichment system (VACES), designed to enhance the ambient concentrations of ultrafine (less than 0.18 Molecular Characterization of Organosulfates in Urban Aerosols during the Spring Festival by FT-ICR Mass Spectrometry

NASA Astrophysics Data System (ADS)

Xie, Q.; Fu, P.

2017-12-01

Aerosol particles collected at daytime and nighttime in Beijing during the spring festival, including the episodes of various gradient level pollution and short-term pollution raised by fireworks, were analyzed using 15T Fourier transform ion cyclotron resonance mass spectrometry (FT-ICRMS). Organosulfates (OSs), tracers for secondary organic aerosol formation, were identified through accurate mass measurements. Both the total number and the arbitrary abundance of OSs were consistent with the total OC concentrations of the aerosol samples. Nitrooxy-organosulfates were more abundant in the nighttime than those in the daytime due to high NOX concentrations at night. Although all subgroups OSs increased with the deterioration of air quality, especially for the relative abundance of aromatic OSs with high double bond equivalents, the percentage contributions of aliphatic OSs with low degree of unsaturation decreased. It was worth to note that aliphatic OSs with a wide range in carbon-chain length of C6-40 were identified in this study. The candidates for their potential precursors were alkanes and fatty acids. Moreover, a large number of aromatic OSs, about two thirds of OSs, were detected. The rapid formation of these compounds in New Year's Eve with plentiful aromatics from firework burning suggests that they may be derived from PAHs. The high carbon and oxygen contents of OSs may indicate the presence of dimmers, even polymers. Our results support the important contribution of anthropogenic precursors to OSs in ambient aerosols on the basis of aromatic and aliphatic OSs, which may have a significant impact on the hygroscopic properties of ambient aerosol particles.

Aerosol composition and source apportionment in Santiago de Chile

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (2Aerosol mass (PM 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3. Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An

Primary to secondary organic aerosol: evolution of organic emissions from mobile combustion sources

NASA Astrophysics Data System (ADS)

Presto, A. A.; Gordon, T. D.; Robinson, A. L.

2014-05-01

A series of smog chamber experiments were conducted to investigate the transformation of primary organic aerosol (POA) and formation of secondary organic aerosol (SOA) during the photooxidation of dilute exhaust from a fleet of gasoline and diesel motor vehicles and two gas-turbine engines. In experiments where POA was present in the chamber at the onset of photooxidation, positive matrix factorization (PMF) was used to determine separate POA and SOA factors from aerosol mass spectrometer data. A 2-factor solution, with one POA factor and one SOA factor, was sufficient to describe the organic aerosol for gasoline vehicles, diesel vehicles, and one of the gas-turbine engines. Experiments with the second gas-turbine engine required a 3-factor PMF solution with a POA factor and two SOA factors. Results from the PMF analysis were compared to the residual method for determining SOA and POA mass concentrations. The residual method apportioned a larger fraction of the organic aerosol mass as POA because it assumes that all mass at m / z 57 is associated with POA. The POA mass spectrum for the gasoline and diesel vehicles exhibited high abundances of the CnH2n+1 series of ions (m / z 43, 57, etc.) and was similar to the mass spectra of the hydrocarbon-like organic aerosol factor determined from ambient data sets with one exception, a diesel vehicle equipped with a diesel oxidation catalyst. POA mass spectra for the gas-turbine engines are enriched in the CnH2n-1 series of ions (m / z 41, 55, etc.), consistent with the composition of the lubricating oil used in these engines. The SOA formed from the three sources exhibits high abundances of m / z 44 and 43, indicative of mild oxidation. The SOA mass spectra are consistent with less-oxidized ambient SV-OOA (semivolatile oxygenated organic aerosols) and fall within the triangular region of f44 versus f43 defined by ambient measurements. However there is poor absolute agreement between the experimentally derived SOA mass

A method for the direct measurement of surface tension of collected atmospherically relevant aerosol particles using atomic force microscopy

NASA Astrophysics Data System (ADS)

Hritz, Andrew D.; Raymond, Timothy M.; Dutcher, Dabrina D.

2016-08-01

Accurate estimates of particle surface tension are required for models concerning atmospheric aerosol nucleation and activation. However, it is difficult to collect the volumes of atmospheric aerosol required by typical instruments that measure surface tension, such as goniometers or Wilhelmy plates. In this work, a method that measures, ex situ, the surface tension of collected liquid nanoparticles using atomic force microscopy is presented. A film of particles is collected via impaction and is probed using nanoneedle tips with the atomic force microscope. This micro-Wilhelmy method allows for direct measurements of the surface tension of small amounts of sample. This method was verified using liquids, whose surface tensions were known. Particles of ozone oxidized α-pinene, a well-characterized system, were then produced, collected, and analyzed using this method to demonstrate its applicability for liquid aerosol samples. It was determined that oxidized α-pinene particles formed in dry conditions have a surface tension similar to that of pure α-pinene, and oxidized α-pinene particles formed in more humid conditions have a surface tension that is significantly higher.

Vertical Profiles of Aerosol Optical Properties Over Central Illinois and Comparison with Surface and Satellite Measurements

NASA Technical Reports Server (NTRS)

Sheridan P. J.; Andrews, E.; Ogren, J A.; Tackett, J. L.; Winker, D. M.

2012-01-01

Between June 2006 and September 2009, an instrumented light aircraft measured over 400 vertical profiles of aerosol and trace gas properties over eastern and central Illinois. The primary objectives of this program were to (1) measure the in situ aerosol properties and determine their vertical and temporal variability and (2) relate these aircraft measurements to concurrent surface and satellite measurements. Underflights of the CALIPSO satellite show reasonable agreement in a majority of retrieved profiles between aircraft-measured extinction at 532 nm (adjusted to ambient relative humidity) and CALIPSO-retrieved extinction, and suggest that routine aircraft profiling programs can be used to better understand and validate satellite retrieval algorithms. CALIPSO tended to overestimate the aerosol extinction at this location in some boundary layer flight segments when scattered or broken clouds were present, which could be related to problems with CALIPSO cloud screening methods. The in situ aircraft-collected aerosol data suggest extinction thresholds for the likelihood of aerosol layers being detected by the CALIOP lidar. These statistical data offer guidance as to the likelihood of CALIPSO's ability to retrieve aerosol extinction at various locations around the globe.

Identification of amines in wintertime ambient particulate material using high resolution aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Bottenus, Courtney L. H.; Massoli, Paola; Sueper, Donna; Canagaratna, Manjula R.; VanderSchelden, Graham; Jobson, B. Thomas; VanReken, Timothy M.

2018-05-01

Significant amounts of amines were detected in fine particulate matter (PM) during ambient wintertime conditions in Yakima, WA, using a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Positive matrix factorization (PMF) of the organic aerosol (OA) signal resulted in a six-factor solution that included two previously unreported amine OA factors. The contributions of the amine factors were strongly episodic, but the concentration of the combined amine factors was as high as 10-15 μg m-3 (2-min average) during those episodes. In one occasion, the Amine-II component was 45% of total OA signal. The Amine-I factor was dominated by spectral peaks at m/z 86 (C5H12N+) and m/z 100 (C6H14N+), while the Amine-II factor was dominated by spectral peaks at m/z 58 (C3H8N+ and C2H6N2+) and m/z 72 (C4H10N+ and C3H8N2+). The ions dominating each amine factor showed distinct time traces, suggesting different sources or formation processes. Investigation into the chemistry of the amine factors suggests a correlation with inorganic anions for Amine-I, but no evidence that the Amine-II was being neutralized by the same inorganic ions. We also excluded the presence of organonitrates (ON) in the OA. The presence of C2H4O2+ at m/z 60 (a levoglucosan fragment) in the Amine-I spectrum suggests some influence of biomass burning emissions (more specifically residential wood combustion) in this PMF factor, but wind direction suggested that the most likely sources of these amines were agricultural activities and feedlots to the S-SW of the site.

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.

CHARACTERIZATION OF AMBIENT PM2.5 AEROSOL AT A SOUTHEASTERN US SITE: FOURIER TRANSFORM INFRARED ANALYSIS OR PARTICLE PHASE

EPA Science Inventory

During a field study in the summer of 2000 in the Research Triangle Park (RTP), aerosol samples were collected using a five stage cascade impactor and subsequently analyzed using Fourier Transform Infrared Spectroscopy (FTIR). The impaction surfaces were stainless steel disks....

Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study

NASA Astrophysics Data System (ADS)

Rattanavaraha, Weruka; Chu, Kevin; Hapsari Budisulistiorini, Sri; Riva, Matthieu; Lin, Ying-Hsuan; Edgerton, Eric S.; Baumann, Karsten; Shaw, Stephanie L.; Guo, Hongyu; King, Laura; Weber, Rodney J.; Neff, Miranda E.; Stone, Elizabeth A.; Offenberg, John H.; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.

2016-04-01

In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA) that contributes to fine particulate matter (PM2.5). Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2), oxides of nitrogen (NOx), and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH)-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM), ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS). Sample extracts were analyzed by gas chromatography-electron ionization-mass spectrometry (GC/EI-MS) with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH) network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM) ( ˜ 7 to ˜ 20 %). Isoprene-derived SOA tracers correlated with sulfate (SO42-) (r2 = 0.34, n = 117) but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML)-derived SOA tracers with nitrate radical production (P[NO3]) (r2 = 0.57, n = 40) were observed during nighttime, suggesting a potential role of the NO3 radical in

Shipborne measurements of aerosol number size distribution and hygroscopicity over the North Pacific Ocean

NASA Astrophysics Data System (ADS)

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

2016-12-01

We report aerosol number size distribution and hygroscopicity data collected over the Pacific Ocean near the Hawaii Ocean Timeseries (HOT) Station ALOHA (centered near 22°N, 158°W). From June 25 to July 3, 2016 our hygroscopicity tandem differential mobility analyzer (HTDMA)/scanning mobility particle sizer (SMPS) system was deployed onboard of NOAA Ship Hi'ialakai that participated in mooring operations associated with the Woods Hole Oceanographic Institution WHOTS project. The ambient aerosol data was collected during the ship's planned operations. The inlet was located at the bow of the ship and the air samples were drawn (using 3/8 inch stainless steel tubing) inside a dry, air-conditioned lab. The region north of Oahu was very clean, with total particle number approximately 200 cm-3, occasionally dropping below 100 cm-3. We compare our particle number size distribution and hygroscopicity data with previously reported estimates. Our measurements contribute to process-level understanding of the role of sea spray aerosol in marine boundary layer cloud condensation nuclei (CCN) budget and provide crucial information to the community interested in studying and projecting climate change using Earth System Models.

The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

PubMed

Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

2015-06-24

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

Single-particle characterization of urban aerosol particles collected in three Korean cites using low-Z electron probe X-ray microanalysis.

PubMed

Ro, Chul-Un; Kim, HyeKyeong; Oh, Keun-Young; Yea, Sun Kyung; Lee, Chong Bum; Jang, Meongdo; Van Grieken, René

2002-11-15

A recently developed single-particle analytical technique, called low-Z electron probe X-ray microanalysis (low-Z EPMA), was applied to characterize urban aerosol particles collected in three cities of Korea (Seoul, CheongJu, and ChunCheon) on single days in the winter of 1999. In this study, it is clearly demonstrated that the low-Z EPMA technique can provide detailed and quantitative information on the chemical composition of particles in the urban atmosphere. The collected aerosol particles were analyzed and classified on the basis of their chemical species. Various types of particles were identified, such as soil-derived, carbonaceous, marine-originated, and anthropogenic particles. In the sample collected in Seoul, carbonaceous, aluminosilicates, silicon dioxide, and calcium carbonate aerosol particles were abundantly encountered. In the CheongJu and ChunCheon samples, carbonaceous, aluminosilicates, reacted sea salts, and ammonium sulfate aerosol particles were often seen. However, in the CheongJu sample, ammonium sulfate particles were the most abundant in the fine fraction. Also, calcium sulfate and nitrate particles were significantly observed. In the ChunCheon sample, organic particles were the most abundant in the fine fraction. Also, sodium nitrate particles were seen at high levels. The ChunCheon sample seemed to be strongly influenced by sea-salt aerosols originating from the Yellow Sea, which is located about 115 km away from the city.

Near real time vapor detection and enhancement using aerosol adsorption

DOEpatents

Novick, V.J.; Johnson, S.A.

1999-08-03

A vapor sample detection method is described where the vapor sample contains vapor and ambient air and surrounding natural background particles. The vapor sample detection method includes the steps of generating a supply of aerosol that have a particular effective median particle size, mixing the aerosol with the vapor sample forming aerosol and adsorbed vapor suspended in an air stream, impacting the suspended aerosol and adsorbed vapor upon a reflecting element, alternatively directing infrared light to the impacted aerosol and adsorbed vapor, detecting and analyzing the alternatively directed infrared light in essentially real time using a spectrometer and a microcomputer and identifying the vapor sample. 13 figs.

Trends in aerosol abundances and distributions

NASA Technical Reports Server (NTRS)

Turco, R. P.; Mccormick, M. P.; Clancy, R. T.; Curran, R.; Deluisi, J.; Hamill, P.; Kent, G.; Rosen, J. M.; Toon, O. B.; Yue, G.

1989-01-01

The properties of aerosols that reside in the upper atmosphere are described. Special emphasis is given to the influence these aerosols have on ozone observation systems, mainly through radiative effects, and on ambient ozone concentrations, mainly through chemical effects. It has long been appreciated that stratospheric particles can interfere with the remote sensing of ozone distribution. The mechanism and magnitude of this interference are evaluated. Separate sections deal with the optical properties of upper atmospheric aerosols, long-term trends in stratospheric aerosols, perturbations of the stratospheric aerosol layer by volcanic eruptions, and estimates of the impacts that such particles have on remotely measured ozone concentrations. Another section is devoted to a discussion of the polar stratospheric clouds (PSC's). These unique clouds, recently discovered by satellite observation, are now thought to be intimately connected with the Antarctic ozone hole. Accordingly, interest in PSC's has grown considerably in recent years. This chapter describes what we know about the morphology, physical chemistry, and microphysics of PSC's.

VERSATILE AEROSOL CONCENTRATION ENRICHMENT SYSTEM (VACES) FOR SIMULTANEOUS IN VIVO AND IN VITRO EVALUATION OF TOXIC EFFECTS OF ULTRAFINE, FINE AND COARSE AMBIENT PARTICLES. PART I: DEVELOPMENT AND LABORATORY CHARACTERIZATION. (R827352C001)

EPA Science Inventory

This study presents the development and bench-testing of a versatile aerosol concentration enrichment system (VACES) capable of simultaneously concentrating ambient particles of the coarse, fine and ultrafine size fractions for conducting in vivo and in vitro studies. The VACE...

Online measurements of ambient fluorescent aerosol particles by WIBS at a polluted regional site in the North China Plain: potential impact of burning activities

NASA Astrophysics Data System (ADS)

Su, H.; Wang, Z.; Cheng, Y.; Xie, Z.; Kecorius, S.; McMeeking, G. R.; Yu, X.; Pöhlker, C.; Zhang, M.; Wiedensohler, A.; Kuhn, U.; Poeschl, U.; Huffman, J. A.

2015-12-01

Online measurements of ambient fluorescent aerosol particles by WIBS at a polluted regional site in the North China Plain: potential impact of burning activities Zhibin Wang1, Xiawei Yu1,3, Simonas Kecorius2, Zhouqing Xie3, Gavin McMeeking4, Christopher Pöhlker1, Minghui, Zhang1, Alfred Wiedensohler2, Uwe Kuhn1, Yafang Cheng1, Ulrich Pöschl1, Hang Su1,*1Multiphase Chemistry and Biogeochemistry Departments, Max Planck Institute for Chemistry, Mainz 55128, Germany2Leibniz-Institute for Tropospheric Research, Leipzig 04318, Germany3School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China4Droplet Measurement Technologies, Boulder 80301, USA ABSTRACTBioaerosols are the main subset of super-micron particles, and significantly influence the evolution of cloud and precipitation, as well as the public health. Currently, the detection of ambient biological materials in real-time is mainly based on the presence of fluorophores in the particles. In this study, we present the wideband integrated bioaerosol spectrometer (WIBS) measurement results to characterize the fluorescent aerosol particles (FAP) at a polluted regional site (Xianghe, 39.80 °N, 116.96 °E) in the North China Plain. We observed substantially much higher number concentration of FAP as compared with those of previous studies in clean environments. We found the good agreement between the FAP number fraction in coarse mode particles (> 1 mm) and BC mass fraction in fine particles (< 1 mm), possibly indicating a majority of the observed FAP is to a certain extent related to the anthropogenic burning activities nearby. This interference and uncertainty should be especially noticed when performing fluorescence measurements in the polluted area, where the certain non-biological compounds (such as SOA, PAH and soot) may significantly lead to a positive fluorescence measurement artifacts and an overestimation of actual fluorescent biological aerosol particles. We also

Exposure and effect assessment of aerosolized red tide toxins (brevetoxins) and asthma.

PubMed

Fleming, Lora E; Bean, Judy A; Kirkpatrick, Barbara; Cheng, Yung Sung; Pierce, Richard; Naar, Jerome; Nierenberg, Kate; Backer, Lorraine C; Wanner, Adam; Reich, Andrew; Zhou, Yue; Watkins, Sharon; Henry, Mike; Zaias, Julia; Abraham, William M; Benson, Janet; Cassedy, Amy; Hollenbeck, Julie; Kirkpatrick, Gary; Clarke, Tainya; Baden, Daniel G

2009-07-01

In previous studies we demonstrated statistically significant changes in reported symptoms for lifeguards, general beach goers, and persons with asthma, as well as statistically significant changes in pulmonary function tests (PFTs) in asthmatics, after exposure to brevetoxins in Florida red tide (Karenia brevis bloom) aerosols. In this study we explored the use of different methods of intensive ambient and personal air monitoring to characterize these exposures to predict self-reported health effects in our asthmatic study population. We evaluated health effects in 87 subjects with asthma before and after 1 hr of exposure to Florida red tide aerosols and assessed for aerosolized brevetoxin exposure using personal and ambient samplers. After only 1 hr of exposure to Florida red tide aerosols containing brevetoxin concentrations > 57 ng/m(3), asthmatics had statistically significant increases in self-reported respiratory symptoms and total symptom scores. However, we did not see the expected corresponding changes in PFT results. Significant increases in self-reported symptoms were also observed for those not using asthma medication and those living >/= 1 mile from the coast. These results provide additional evidence of health effects in asthmatics from ambient exposure to aerosols containing very low concentrations of brevetoxins, possibly at the lower threshold for inducing a biologic response (i.e., toxicity). Consistent with the literature describing self-reported symptoms as an accurate measure of asthmatic distress, our results suggest that self-reported symptoms are a valuable measure of the extent of health effects from exposure to aerosolized brevetoxins in asthmatic populations.

Aerosols attenuating the solar radiation collected by solar tower plants: The horizontal pathway at surface level

NASA Astrophysics Data System (ADS)

Elias, Thierry; Ramon, Didier; Dubus, Laurent; Bourdil, Charles; Cuevas-Agulló, Emilio; Zaidouni, Taoufik; Formenti, Paola

2016-05-01

Aerosols attenuate the solar radiation collected by solar tower plants (STP), along two pathways: 1) the atmospheric column pathway, between the top of the atmosphere and the heliostats, resulting in Direct Normal Irradiance (DNI) changes; 2) the grazing pathway close to surface level, between the heliostats and the optical receiver. The attenuation along the surface-level grazing pathway has been less studied than the aerosol impact on changes of DNI, while it becomes significant in STP of 100 MW or more. Indeed aerosols mostly lay within the surface atmospheric layer, called the boundary layer, and the attenuation increases with the distance covered by the solar radiation in the boundary layer. In STP of 100 MW or more, the distance between the heliostats and the optical receiver becomes large enough to produce a significant attenuation by aerosols. We used measured aerosol optical thickness and computed boundary layer height to estimate the attenuation of the solar radiation at surface level at Ouarzazate (Morocco). High variabilities in aerosol amount and in vertical layering generated a significant magnitude in the annual cycle and significant inter-annual changes. Indeed the annual mean of the attenuation caused by aerosols over a 1-km heliostat-receiver distance was 3.7% in 2013, and 5.4% in 2014 because of a longest desert dust season. The monthly minimum attenuation of less than 3% was observed in winter and the maximum of more than 7% was observed in summer.

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

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

Mazurek, M.A.; Cofer, W.R. III; Levine, J.S.

1990-10-01

The identity and ambient mass concentrations of radiatively important carbonaceous aerosols were measured for a boreal forest prescribed burn conducted in northern Ontario, CAN in August 1989. Nonsize-segregated airborne particles were collected for smoldering-fire and full-fire conditions using a helicopter sampling platform. Total carbon (TC), organic carbon (OC) and elemental carbon (EC) were measured. Smoke plume mass concentrations of the OC and EC particles were greatest for full-fire conditions and had ranges of 1.560 to 2.160 mg/m{sup {minus}1} (OC) and 0.120 to 0.160 mg/m{sup {minus}3} (EC) with OC:EC ratios of 10 to 18, respectively. Smoldering fire conditions showed smoke plumemore » OC and EC levels of 0.570--1.030 mg/m{sup {minus}3} (OC) and 0.006--0.050 mg/m{sup {minus}3} (EC) and much higher ratios of OC:EC (21 to 95). These aerosol data indicate the formation of EC particles is greatest during full-fire combustion of boreal forest material relative to smoldering combustion. However, EC particles comprise a minor fraction of the particulate carbon smoke aerosols for both full-fire and smoldering conditions; the major component of carbonaceous smoke aerosols emitted during the prescribed burn is OC. Overall, the OC and EC in-plume smoke aerosol data show nonuniform production of these particles during various stages of the prescribed burn, and major differences in the type of carbonaceous aerosol that is generated (OC versus EC).« less

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.

Characteristics of regional aerosols: Southern Arizona and eastern Pacific Ocean

NASA Astrophysics Data System (ADS)

Prabhakar, Gouri

Atmospheric aerosols impact the quality of our life in many direct and indirect ways. Inhalation of aerosols can have harmful effects on human health. Aerosols also have climatic impacts by absorbing or scattering solar radiation, or more indirectly through their interactions with clouds. Despite a better understanding of several relevant aerosol properties and processes in the past years, they remain the largest uncertainty in the estimate of global radiative forcing. The uncertainties arise because although aerosols are ubiquitous in the Earth's atmosphere they are highly variable in space, time and their physicochemical properties. This makes in-situ measurements of aerosols vital in our effort towards reducing uncertainties in the estimate of global radiative forcing due to aerosols. This study is an effort to characterize atmospheric aerosols at a regional scale, in southern Arizona and eastern Pacific Ocean, based on ground and airborne observations of aerosols. Metals and metalloids in particles with aerodynamic diameter (Dp) smaller than 2.5 μm are found to be ubiquitous in southern Arizona. The major sources of the elements considered in the study are identified to be crustal dust, smelting/mining activities and fuel combustion. The spatial and temporal variability in the mass concentrations of these elements depend both on the source strength and meteorological conditions. Aircraft measurements of aerosol and cloud properties collected during various field campaigns over the eastern Pacific Ocean are used to study the sources of nitrate in stratocumulus cloud water and the relevant processes. The major sources of nitrate in cloud water in the region are emissions from ships and wildfires. Different pathways for nitrate to enter cloud water and the role of meteorology in these processes are examined. Observations of microphysical properties of ambient aerosols in ship plumes are examined. The study shows that there is an enhancement in the number

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Ice nucleation properties of atmospheric aerosol particles collected during a field campaign in Cyprus

NASA Astrophysics Data System (ADS)

Yordanova, Petya; Maier, Stefanie; Lang-Yona, Naama; Tamm, Alexandra; Meusel, Hannah; Pöschl, Ulrich; Weber, Bettina; Fröhlich-Nowoisky, Janine

2017-04-01

Atmospheric aerosol particles, including desert and soil dust as well as marine aerosols, are well known to act as ice nuclei (IN) and thus have been investigated in numerous ice nucleation studies. Based on their cloud condensation nuclei potential and their impacts on radiative properties of clouds (via scattering and absorption of solar radiation), aerosol particles may significantly affect the cloud and precipitation development. Atmospheric aerosols of the Eastern Mediterranean have been described to be dominated by desert dust, but only little is known on their composition and ice nucleating properties. In this study we investigated the ice nucleating ability of total suspended particles (TSP), collected at the remote site Agia Marina Xyliatou on Cyprus during a field campaign in April 2016. Airborne TSP samples containing air masses of various types such as African (Saharan) and Arabian dust and European and Middle Eastern pollution were collected on glass fiber filters at 24 h intervals. Sampling was performed ˜5 m above ground level and ˜521 m above sea level. During the sampling period, two major dust storms (PM 10max 118 μg/m3 and 66 μg/m3) and a rain event (rainfall amount: 3.4 mm) were documented. Chemical and physical characterizations of the particles were analyzed experimentally through filtration, thermal, chemical and enzyme treatments. Immersion freezing experiments were performed at relatively high subzero temperatures (-1 to -15˚ C) using the mono ice nucleation array. Preliminary results indicate that highest IN particle numbers (INPs) occurred during the second dust storm event with lower particle concentrations. Treatments at 60˚ C lead to a gradual IN deactivation, indicating the presence of biological INPs, which were observed to be larger than 300 kDa. Additional results originating from this study will be shown. Acknowledgement: This work was funded by the DFG Ice Nuclei Research Unit (INUIT).

Hygroscopic and Chemical Properties of Aerosols collected near a Copper Smelter: Implications for Public and Environmental Health

PubMed Central

Sorooshian, Armin; Csavina, Janae; Shingler, Taylor; Dey, Stephen; Brechtel, Fred J.; Sáez, A. Eduardo; Betterton, Eric A.

2012-01-01

Particulate matter emissions near active copper smelters and mine tailings in the southwestern United States pose a potential threat to nearby environments owing to toxic species that can be inhaled and deposited in various regions of the body depending on the composition and size of the particles, which are linked by particle hygroscopic properties. This study reports the first simultaneous measurements of size-resolved chemical and hygroscopic properties of particles next to an active copper smelter and mine tailings by the towns of Hayden and Winkelman in southern Arizona. Size-resolved particulate matter samples collected near an active copper smelter were examined with inductively coupled plasma mass spectrometry, ion chromatography, and a humidified tandem differential mobility analyzer. Aerosol particles collected at the measurement site are enriched in metals and metalloids (e.g. arsenic, lead, and cadmium) and water-uptake measurements of aqueous extracts of collected samples indicate that the particle diameter range of particles most enriched with these species (0.18–0.55 µm) overlaps with the most hygroscopic mode at a relative humidity of 90% (0.10–0.32 µm). These measurements have implications for public health, microphysical effects of aerosols, and regional impacts owing to the transport and deposition of contaminated aerosol particles. PMID:22852879

Ambient in-situ immersion freezing measurements - findings from the ZAMBIS 2014 field campaign for three ice nucleation techniques

NASA Astrophysics Data System (ADS)

Kohn, Monika; Atkinson, James D.; Lohmann, Ulrike; Kanji, Zamin A.

2015-04-01

well as a droplet freezing method on aerosol particles either collected in a suspension or on PM10-filters to obtain atmospheric IN concentrations based on the measured ambient aerosol. Investigation of physical properties (number and size distribution) and chemical composition as well as the meteorological conditions provide supplementary information that help to understand the nature of particles and air masses that contribute to immersion freezing. Acknowledgements We thank Hannes Wydler and Hansjörg Frei from ETH Zurich for their technical support. Furthermore, the authors want thank Franz Conen from the University of Basel for sharing equipment and training in the drop freezing experiment. References [1] Chou et al. (2011), Atmos. Chem. Phys., 11, 4725-4738. [2] Nicolet et al. (2010), Atmos. Chem. Phys., 10, 313-325. [3] Conen et al. (2012), Atmos. Meas. Tech., 5, 321-327. [4] Stopelli et al. (2014), Atmos. Meas. Tech., 7, 129-134.

Characterization of fresh and aged organic aerosol emissions from meat charbroiling

NASA Astrophysics Data System (ADS)

Kaltsonoudis, Christos; Kostenidou, Evangelia; Louvaris, Evangelos; Psichoudaki, Magda; Tsiligiannis, Epameinondas; Florou, Kalliopi; Liangou, Aikaterini; Pandis, Spyros N.

2017-06-01

Cooking emissions can be a significant source of fine particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. Greek souvlakia with pork were cooked using a commercial charbroiler and a fraction of the emissions were introduced into a smog chamber where after a characterization phase they were exposed to UV illumination and oxidants. The particulate and gas phases were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a proton-transfer-reaction mass spectrometer (PTR-MS) correspondingly. More than 99 % of the aerosol emitted was composed of organic compounds, while black carbon (BC) contributed 0.3 % and the inorganic species less than 0.5 % of the total aerosol mass. The initial O : C ratio was approximately 0.09 and increased up to 0.30 after a few hours of chemical aging (exposures of 1010 molecules cm-3 s for OH and 100 ppb h for ozone). The initial and aged AMS spectra differed considerably (θ = 27°). Ambient measurements were also conducted during Fat Thursday in Patras, Greece, when traditionally meat is charbroiled everywhere in the city. Positive matrix factorization (PMF) revealed that cooking organic aerosol (COA) reached up to 85 % of the total OA from 10:00 to 12:00 LST that day. The ambient COA factor in two major Greek cities had a mass spectrum during spring and summer similar to the aged meat charbroiling emissions. In contrast, the ambient COA factor during winter resembled strongly the fresh laboratory meat charbroiling emissions.

Radiative Effects of Aerosols

NASA Technical Reports Server (NTRS)

Valero, Francisco P. J.

1996-01-01

During the Atlantic Stratocumulus Transition Experiment (ASTEX) in June 1992, two descents in cloud-free regions allowed comparison of the change in aerosol optical depth as determined by an onboard total-direct-diffuse radiometer (TDDR) to the change calculated from measured size-resolved aerosol microphysics and chemistry. Both profiles included a pollution haze from Europe but the second also included the effect of a Saharan dust layer above the haze. The separate contributions of supermicrometer (coarse) and submicrometer (fine) aerosol were determined and thermal analysis of the pollution haze indicated that the fine aerosol was composed primarily of a sulfate/water mixture with a refractory soot-like core. The soot core increased the calculated extinction by about 10% in the most polluted drier layer relative to a pure sulfate aerosol but had significantly less effect at higher humidities. A 3 km descent through a boundary layer air mass dominated by pollutant aerosol with relative humidities (RH) 10-77% yielded a close agreement between the measured and calculated aerosol optical depths (550 nm) of 0.160 (+/- 0.07) and 0. 157 (+/- 0.034) respectively. During descent the aerosol mass scattering coefficient per unit sulfate mass varied from about 5 to 16 m(exp 2)/g and primarily dependent upon ambient RH. However, the total scattering coefficient per total fine mass was far less variable at about 4+/- 0.7 m(exp 2)/g. A subsequent descent through a Saharan dust layer located above the pollution aerosol layer revealed that both layers contributed similarly to aerosol optical depth. The scattering per unit mass of the coarse aged dust was estimated at 1.1 +/- 0.2 m(exp 2)/g. The large difference (50%) in measured and calculated optical depth for the dust layer exceeded measurements.

Organosulfates as tracers for secondary organic aerosol (SOA) formation from 2-methyl-3-buten-2-ol (MBO) in the atmosphere.

PubMed

Zhang, Haofei; Worton, David R; Lewandowski, Michael; Ortega, John; Rubitschun, Caitlin L; Park, Jeong-Hoo; Kristensen, Kasper; Campuzano-Jost, Pedro; Day, Douglas A; Jimenez, Jose L; Jaoui, Mohammed; Offenberg, John H; Kleindienst, Tadeusz E; Gilman, Jessica; Kuster, William C; de Gouw, Joost; Park, Changhyoun; Schade, Gunnar W; Frossard, Amanda A; Russell, Lynn; Kaser, Lisa; Jud, Werner; Hansel, Armin; Cappellin, Luca; Karl, Thomas; Glasius, Marianne; Guenther, Alex; Goldstein, Allen H; Seinfeld, John H; Gold, Avram; Kamens, Richard M; Surratt, Jason D

2012-09-04

2-Methyl-3-buten-2-ol (MBO) is an important biogenic volatile organic compound (BVOC) emitted by pine trees and a potential precursor of atmospheric secondary organic aerosol (SOA) in forested regions. In the present study, hydroxyl radical (OH)-initiated oxidation of MBO was examined in smog chambers under varied initial nitric oxide (NO) and aerosol acidity levels. Results indicate measurable SOA from MBO under low-NO conditions. Moreover, increasing aerosol acidity was found to enhance MBO SOA. Chemical characterization of laboratory-generated MBO SOA reveals that an organosulfate species (C(5)H(12)O(6)S, MW 200) formed and was substantially enhanced with elevated aerosol acidity. Ambient fine aerosol (PM(2.5)) samples collected from the BEARPEX campaign during 2007 and 2009, as well as from the BEACHON-RoMBAS campaign during 2011, were also analyzed. The MBO-derived organosulfate characterized from laboratory-generated aerosol was observed in PM(2.5) collected from these campaigns, demonstrating that it is a molecular tracer for MBO-initiated SOA in the atmosphere. Furthermore, mass concentrations of the MBO-derived organosulfate are well correlated with MBO mixing ratio, temperature, and acidity in the field campaigns. Importantly, this compound accounted for an average of 0.25% and as high as 1% of the total organic aerosol mass during BEARPEX 2009. An epoxide intermediate generated under low-NO conditions is tentatively proposed to produce MBO SOA.

Analysis of Marine Aerosol Polysaccharides by Pyrolysis Time-of-Flight Mass Spectrometry

NASA Astrophysics Data System (ADS)

Lawler, M. J.; Grieman, M. M.; Sengur, I.; Saltzman, E. S.

2017-12-01

The relationship between surface ocean biological productivity and marine cloud formation and properties has been explored for decades, but the impacts of marine biogenic emissions on cloudiness and climate remain highly uncertain. This is in part due to the challenge of directly linking biogenic materials in the surface ocean with cloud-forming aerosol. It has been shown that polysaccharide gel-forming materials, also known as transparent exopolymers, may be mechanically ejected from the sea surface during air bubble bursting (Leck and Bigg, 2005). Existing analysis methods for such aerosols require considerable sample mass and sample preparation. As part of the multi-year seasonal North Atlantic Aerosols and Marine Ecosystems Study (NAAMES), ambient submicron marine aerosol was collected in November 2015 and May 2016 from the R/V Atlantis at using a Particle into Liquid Sampler (PILS). These samples of roughly 15 minute time resolution were frozen and returned to UC Irvine for analysis. A new technique has been developed to attempt to quantify polysaccharide material in these ambient samples. A small subsample (1- 5 µL) is taken from the PILS vial samples and allowed to dry on a Pt ribbon filament in the chemical ionization source region of a time-of-flight mass spectrometer. The sample then undergoes a two-step heating process, in which volatilizable molecules are first desorbed and then non-volatilizable large molecules such as polysaccharides are pyrolyzed. These desorbed molecules and decomposition products are ionized using either O2- or H3O+ reagent ion and are directly sampled into the mass spectrometer. The resulting spectra can then be compared to standards of known polysaccharide materials for quantification and potentially structural and/or compositional information.

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

Single-particle characterization of indoor aerosol particles collected at an underground shopping area in Seoul, Korea.

PubMed

Maskey, Shila; Kang, TaeHee; Jung, Hae-Jin; Ro, Chul-Un

2011-02-01

In this study, single-particle characterization of aerosol particles collected at an underground shopping area was performed for the first time. A quantitative single-particle analytical technique, low-Z particle electron probe X-ray microanalysis, was used to characterize a total of 7900 individual particles for eight sets of aerosol samples collected at an underground shopping area in Seoul, Korea. Based on secondary electron images and X-ray spectral data of individual particles, fourteen particle types were identified, in which primary soil-derived particles were the most abundant, followed by carbonaceous, Fe-containing, secondary soil-derived, and secondary sea-salt particles. Carbonaceous particles exist in three types: organic carbon, carbon-rich, and CNO-rich. A significant number of textile particles with chemical composition C, N, and O were encountered in some of the aerosol samples, which were from the textile shops and/or from clothes of passersby. Primary soil-derived particles showed seasonal variation, with peak values in spring samples, reflecting higher air exchange between indoor and outdoor environments in the spring. Secondary soil-derived, secondary sea-salt, and ammonium sulfate particles were frequently encountered in winter samples. Fe-containing particles, contributed from a nearby subway station, were in the range of about 19% relative abundances for all samples. In underground shopping areas, particulate matters can be a considerable health hazard to the workers, shoppers, passersby, and shop-keepers as they spend their considerable time in this closed microenvironment. However, no study on the characteristics of indoor aerosols in an underground shopping area has been reported to our knowledge. This work provides detailed information on characteristics of underground shopping area aerosols on a single particle level. © 2010 John Wiley & Sons A/S.

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

Traffic emission factors of ultrafine particles: effects from ambient air.

PubMed

Janhäll, Sara; Molnar, Peter; Hallquist, Mattias

2012-09-01

Ultrafine particles have a significant detrimental effect on both human health and climate. In order to abate this problem, it is necessary to identify the sources of ultrafine particles. A parameterisation method is presented for estimating the levels of traffic-emitted ultrafine particles in terms of variables describing the ambient conditions. The method is versatile and could easily be applied to similar datasets in other environments. The data used were collected during a four-week period in February 2005, in Gothenburg, as part of the Göte-2005 campaign. The specific variables tested were temperature (T), relative humidity (RH), carbon monoxide concentration (CO), and the concentration of particles up to 10 μm diameter (PM(10)); all indicators are of importance for aerosol processes such as coagulation and gas-particle partitioning. These variables were selected because of their direct effect on aerosol processes (T and RH) or as proxies for aerosol surface area (CO and PM(10)) and because of their availability in local monitoring programmes, increasing the usability of the parameterization. Emission factors are presented for 10-100 nm particles (ultrafine particles; EF(ufp)), for 10-40 nm particles (EF(10-40)), and for 40-100 nm particles (EF(40-100)). For EF(40-100) no effect of ambient conditions was found. The emission factor equations are calculated based on an emission factor for NO(x) of 1 g km(-1), thus the particle emission factors are easily expressed in units of particles per gram of NO(x) emitted. For 10-100 nm particles the emission factor is EF(ufp) = 1.8 × 10(15) × (1 - 0.095 × CO - 3.2 × 10(-3) × T) particles km(-1). Alternative equations for the EFs in terms of T and PM(10) concentration are also presented.

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

PubMed

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

2015-07-15

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

Light-absorbing oligomer formation in secondary organic aerosol from reactive uptake of isoprene epoxydiols.

PubMed

Lin, Ying-Hsuan; Budisulistiorini, Sri Hapsari; Chu, Kevin; Siejack, Richard A; Zhang, Haofei; Riva, Matthieu; Zhang, Zhenfa; Gold, Avram; Kautzman, Kathryn E; Surratt, Jason D

2014-10-21

Secondary organic aerosol (SOA) produced from reactive uptake and multiphase chemistry of isoprene epoxydiols (IEPOX) has been found to contribute substantially (upward of 33%) to the fine organic aerosol mass over the Southeastern U.S. Brown carbon (BrC) in rural areas of this region has been linked to secondary sources in the summer when the influence of biomass burning is low. We demonstrate the formation of light-absorbing (290 < λ < 700 nm) SOA constituents from reactive uptake of trans-β-IEPOX onto preexisting sulfate aerosols as a potential source of secondary BrC. IEPOX-derived BrC generated in controlled chamber experiments under dry, acidic conditions has an average mass absorption coefficient of ∼ 300 cm(2) g(-1). Chemical analyses of SOA constituents using UV-visible spectroscopy and high-resolution mass spectrometry indicate the presence of highly unsaturated oligomeric species with molecular weights separated by mass units of 100 (C5H8O2) and 82 (C5H6O) coincident with the observations of enhanced light absorption, suggesting such oligomers as chromophores, and potentially explaining one source of humic-like substances (HULIS) ubiquitously present in atmospheric aerosol. Similar light-absorbing oligomers were identified in fine aerosol collected in the rural Southeastern U.S., supporting their atmospheric relevance and revealing a previously unrecognized source of oligomers derived from isoprene that contributes to ambient fine aerosol mass.

Organosulfate Formation in Biogenic Secondary Organic Aerosol

EPA Science Inventory

Organosulfates of isoprene, α-pinene, and β-pinene have recently been identified in both laboratory-generated and ambient secondary organic aerosol (SOA). In this study, the mechanism and ubiquity of organosulfate formation in biogenic SOA is investigated by a comprehensive seri...

How well can we Measure the Vertical Profile of Tropospheric Aerosol Extinction?

NASA Technical Reports Server (NTRS)

Schmid, Beat; Ferrare, R.; Flynn, C.; Elleman, R.; Covert, D.; Strawa, A.; Welton, E.; Turner, D.; Jonsson, H.; Redemann, J.

2005-01-01

The recent Department of Energy Atmospheric Radiation Measurement (ARM) Aerosol Intensive Operations Period (MOP, May 2003) yielded one of the best measurement sets obtained to-date to assess our ability to measure the vertical profile of ambient aerosol extinction sigma(sub ep)(lambda) in the lower troposphere. During one month, a heavily instrumented aircraft with well characterized aerosol sampling ability carrying well proven and new aerosol instrumentation, devoted most of the 60 available flight hours to flying vertical profiles over the heavily instrumented ARM Southern Great Plains (SGP) Climate Research Facility (CRF). This allowed us to compare vertical extinction profiles obtained from 6 different instuments: airborne Sun photometer (AATS-14), airborne nephelometer/absorption photometer, airborne cavity ring-down system, ground-based Raman lidar and 2 ground-based elastic backscatter lidars. We find the in-situ measured sigma(sub ep)(lambda) to be lower than the AATS-14 derived values. Bias differences are 0.002 - 0.004 K/m equivalent to 12-17% in the visible, or 45% in the near-infrared. On the other hand, we find that with respect to AATS-14, the lidar sigma(sub ep)(lambda) are higher. An unnoticed loss of sensitivity of the Raman lidar had occurred leading up to AIOP and we expect better agreement from the recently restored system looking at the collective results from 6 field campaigns conducted since 1996, airborne in situ measurements of sigma(sub ep)(lambda) tend to be biased slightly low (17% at visible wavelengths) when compared to airborne Sun photometer sigma(sub ep)(lambda). On the other hand, sigma(sub ep)(lambda) values derived from lidars tend to have no or positive biases. From the bias differences we conclude that the typical systematic error associated with measuring the tropospheric vertical profile of the ambient aerosol extinction with current state of-the art instrumentation is 15-20% at visible wavelengths and potentially larger in

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

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem. Revision

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

Mazurek, M.A.; Cofer, W.R. III; Levine, J.S.

1990-10-01

The identity and ambient mass concentrations of radiatively important carbonaceous aerosols were measured for a boreal forest prescribed burn conducted in northern Ontario, CAN in August 1989. Nonsize-segregated airborne particles were collected for smoldering-fire and full-fire conditions using a helicopter sampling platform. Total carbon (TC), organic carbon (OC) and elemental carbon (EC) were measured. Smoke plume mass concentrations of the OC and EC particles were greatest for full-fire conditions and had ranges of 1.560 to 2.160 mg/m{sup {minus}1} (OC) and 0.120 to 0.160 mg/m{sup {minus}3} (EC) with OC:EC ratios of 10 to 18, respectively. Smoldering fire conditions showed smoke plumemore » OC and EC levels of 0.570--1.030 mg/m{sup {minus}3} (OC) and 0.006--0.050 mg/m{sup {minus}3} (EC) and much higher ratios of OC:EC (21 to 95). These aerosol data indicate the formation of EC particles is greatest during full-fire combustion of boreal forest material relative to smoldering combustion. However, EC particles comprise a minor fraction of the particulate carbon smoke aerosols for both full-fire and smoldering conditions; the major component of carbonaceous smoke aerosols emitted during the prescribed burn is OC. Overall, the OC and EC in-plume smoke aerosol data show nonuniform production of these particles during various stages of the prescribed burn, and major differences in the type of carbonaceous aerosol that is generated (OC versus EC).« less

Comparing the mechanism of water condensation and evaporation in glassy aerosol.

PubMed

Bones, David L; Reid, Jonathan P; Lienhard, Daniel M; Krieger, Ulrich K

2012-07-17

Atmospheric models generally assume that aerosol particles are in equilibrium with the surrounding gas phase. However, recent observations that secondary organic aerosols can exist in a glassy state have highlighted the need to more fully understand the kinetic limitations that may control water partitioning in ambient particles. Here, we explore the influence of slow water diffusion in the condensed aerosol phase on the rates of both condensation and evaporation, demonstrating that significant inhibition in mass transfer occurs for ultraviscous aerosol, not just for glassy aerosol. Using coarse mode (3-4 um radius) ternary sucrose/sodium chloride/aqueous droplets as a proxy for multicomponent ambient aerosol, we demonstrate that the timescale for particle equilibration correlates with bulk viscosity and can be ≫10(3) s. Extrapolation of these timescales to particle sizes in the accumulation mode (e.g., approximately 100 nm) by applying the Stokes-Einstein equation suggests that the kinetic limitations imposed on mass transfer of water by slow bulk phase diffusion must be more fully investigated for atmospheric aerosol. Measurements have been made on particles covering a range in dynamic viscosity from < 0.1 to > 10(13) Pa s. We also retrieve the radial inhomogeneities apparent in particle composition during condensation and evaporation and contrast the dynamics of slow dissolution of a viscous core into a labile shell during condensation with the slow percolation of water during evaporation through a more homogeneous viscous particle bulk.

Empirical model for conveniently predicting total and regional lung deposition of inhaled aerosols

EPA Science Inventory

Accurate estimate of a dose of inhaled aerosols is a key factor for estimating potential health risks to exposure to ambient pollutant particulate matter on the one hand, and the therapeutic efficacy of inhaled drug aerosols on the other hand. Particle deposition in the lung is d...

Analysis of Atmospheric Aerosols Collected in an Urban Area in Upstate NY Using Proton Induced X-ray Emission (PIXE) Spectroscopy

NASA Astrophysics Data System (ADS)

Smith, Jeremy; Ali, Salina; Nadareski, Benjamin; Safiq, Alexandrea; Yoskowitz, Joshua; Labrake, Scott; Vineyard, Michael

2013-10-01

We examined atmospheric aerosol samples collected in Schenectady NY for evidence of pollution. We collected aerosol samples using a nine stage cascade impactor which distributes the particulate matter by aerodynamic size onto 7.5 μm Kapton foils. We then used a 1MV electrostatic Pelletron accelerator to produce a 2.2 MeV proton beam to hit the impacted foils. X-ray intensity versus energy spectra were collected using an Amptek x-ray detector where the x-rays are produced from the proton beam interacting with the sample. This is called PIXE. The elemental composition and concentrations of the elements present in the aerosol samples were determined using a software package called GUPIX. We have found elements ranging from Al to Pb and in particular have found significant amounts of Pb and Br on some of our impacted foils, with a Br/Pb ratio of 0.6 +/- 0.2 which agrees with previous studies. This result suggests the presence of leaded aviation fuel perhaps due to the proximity of the collection site to a small airport with a significant amount of general aviation traffic. Union College.

Improving correlations between MODIS aerosol optical thickness and ground-based PM 2.5 observations through 3D spatial analyses

NASA Astrophysics Data System (ADS)

Hutchison, Keith D.; Faruqui, Shazia J.; Smith, Solar

The Center for Space Research (CSR) continues to focus on developing methods to improve correlations between satellite-based aerosol optical thickness (AOT) values and ground-based, air pollution observations made at continuous ambient monitoring sites (CAMS) operated by the Texas commission on environmental quality (TCEQ). Strong correlations and improved understanding of the relationships between satellite and ground observations are needed to formulate reliable real-time predictions of air quality using data accessed from the moderate resolution imaging spectroradiometer (MODIS) at the CSR direct-broadcast ground station. In this paper, improvements in these correlations are demonstrated first as a result of the evolution in the MODIS retrieval algorithms. Further improvement is then shown using procedures that compensate for differences in horizontal spatial scales between the nominal 10-km MODIS AOT products and CAMS point measurements. Finally, airborne light detection and ranging (lidar) observations, collected during the Texas Air Quality Study of 2000, are used to examine aerosol profile concentrations, which may vary greatly between aerosol classes as a result of the sources, chemical composition, and meteorological conditions that govern transport processes. Further improvement in correlations is demonstrated with this limited dataset using insights into aerosol profile information inferred from the vertical motion vectors in a trajectory-based forecast model. Analyses are ongoing to verify these procedures on a variety of aerosol classes using data collected by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite (Calipso) lidar.

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

EPA Science Inventory

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

Ambient Aerosols in the Southern Hemisphere on Ascension Island during the LASIC Campaign: Biomass Burning Season versus Near Pristine Background Conditions

NASA Astrophysics Data System (ADS)

Aiken, A. C.; Springston, S. R.; Watson, T. B.; Sedlacek, A. J., III; Zuidema, P.; Adebiyi, A. A.; Uin, J.; Kuang, C.; Flynn, C. J.

2017-12-01

Ascension Island is located 8 degrees South of the Equator and 15 degrees West Longitude in the middle of the South Atlantic Ocean, at least 1000 miles from any major shoreline and closest to the continent of Africa. While low Southern Hemisphere background aerosol and trace gas measurements are observed most of the year, that picture changes during the South African Biomass Burning (BB) season. BB emissions are a large source of carbon to the atmosphere via particles and gas phase species and with a potential rise in drought and extreme events in the future, these numbers are expected to increase. From approximately June-October every year, the plume of South African BB emissions, the largest BB source in the world, are advected West and are known to impact both the boundary layer and free troposphere at Ascension Island (Zuidema et al., 2016). During the U.S. DOE ARM field campaign, Layered Atlantic Smoke Interactions with Clouds (LASIC), aerosol and trace gas measurements were collected continuously from June 2016 through October 2017 over a 1.5 year period. Two BB seasons are contrasted with the near pristine background conditions during the campaign from the ARM Aerosol Mobile Facility 1 (AMF1) and Mobile Aerosol Observing System (MAOS). Numerous direct in situ aerosol and trace gas measurements are presented, e.g. black carbon (BC), carbon monoxide (CO), PM1 and PM10 aerosol absorption and scattering, submicron non-refractory chemical composition (Organics, Sulfate, Nitrate, Ammonium, Chloride), etc. Aerosol and trace gas signatures are investigated along with backtrajectories to identify sources. Carbonaceous aerosols emitted with gas-phase CO are used to determine particulate emission ratios along with intrinsic and extrinsic aerosol properties. BC mass concentrations reach 1 µg m-3 during multiday plumes and exceed 25% of the total aerosol submicron mass concentration. Organic Aerosol (OA) to BC Ratios of 2.4 in the plume are much higher than previously

A re-assessment of aerosol size distributions from Masaya volcano (Nicaragua)

NASA Astrophysics Data System (ADS)

Martin, R. S.; Ilyinskaya, E.; Sawyer, G. M.; Tsanev, V. I.; Oppenheimer, C.

2011-01-01

Cascade impactors were used to sample volcanic aerosol from Masaya (Nicaragua) in 2007, 2009 and 2010. Differences were found in the size distributions of volcanic aerosol between these recent campaigns and with a campaign in 2001: (1) SO 42- showed modes in both the fine (<1 μm; with low Na +/K +) and coarse (>1 μm; with high Na +/K +) fractions in all of the recent campaigns despite being unimodal in 2001 (<1 μm); (2) The modal diameters for SO 42- roughly doubled in 2009, compared to 2007 or 2010; (3) total Cl - was depleted in volcanic aerosol compared to background aerosol in all the more recent campaigns but was enriched in 2001. Other aspects of the volcanic aerosol appear to be persistent, such as a fine SO 42--H +-Na +-K + mode, which was the most abundant mode in all campaigns, and a coarse Cl --F --Mg 2+-Ca 2+ mode of lower abundance. Water uptake and speciation in the aerosol were investigated using the equilibrium model, ISORROPIA II. Results show that the coarse SO 42--rich mode deliquesces at lower relative humidity (40% RH) than the fine SO 42--rich mode (50% RH) due to increased Na +/K + in the former. The aerosol was predicted to be dry at ambient relative humidity in 2009 and dominated by NaHSO 4, KHSO 4, CaSO 4 and MgSO 4. In contrast, model results predict a liquid aerosol at ambient relative humidity in 2010. These results indicate that aerosol emissions from a volcano can vary in ionic composition and even more so in physical speciation (i.e., salts or solutions). These observations are set against a near-constant magmatic gas composition at Masaya, which highlights the significance of atmospheric and dynamic factors in the formation of volcanic aerosols.

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

NASA Astrophysics Data System (ADS)

Carrico, Christian M.; Gomez, Samantha L.; Dubey, Manvendra K.; Aiken, Allison C.

2018-04-01

Pyrotechnics (fireworks) displays are common for many cultures worldwide, with Independence Day celebrations occurring annually on July 4th as the most notable in the U.S. Given an episodic nature, fireworks aerosol properties are poorly characterized. Here we report observations of optical properties of fresh smoke emissions from Independence Day fireworks smoke sampled at Los Alamos National Laboratory, New Mexico U.S.A. on 4-5 July 2016. Aerosol optical properties were measured with a photoacoustic extinctiometer (PAX, DMT, Inc., Model 870 nm) at low RH < 30% and a humidity controlled nephelometry system (Ecotech, Inc., 450 nm Aurora). 'Dry' light scattering coefficient (σsp) increased from background < 15 Mm-1 reaching 120 Mm-1 (450 nm) as a 2-min event peak, while the absorption coefficient increased from background of 0.5-4.4 Mm-1 (870 nm). The event peak occurred at 00:35 on 5 July 2016, ∼3 h after local fireworks events, and decreased to background by 04:00 on 5 July 2016, showing well mixed aerosol properties. A notable result is that the aerosol hygroscopic response, as characterized by the ratio of wet to dry light scattering or f(RH = 85%), declined to 1.02 at the peak fireworks influence from a background ∼1.7. Strong wavelength dependence of light scattering with Ångström exponent ∼2.2 throughout the event showed a size distribution dominated by sub-micrometer particles. Likewise, single scattering albedo at 870 nm remained constant throughout the event with ω = 0.86 ± 0.03, indicating light absorbing carbon, though not dominant, was mixed with organic carbon. Subsequent laboratory testing with ground-level sparklers showed that pyrotechnics smoke can generate a strong hygroscopic response, however. As confirmed with chemical analysis, the chemistry of the fireworks was key to defining the hygroscopic response. Sparkler smoke was dominated by salt species such as hygroscopic potassium chloride while it lacked the black powder explosives in

Carbonaceous aerosol over a Pinus taeda forest in Central North Carolina, USA

EPA Science Inventory

Organic aerosol is the least understood component of ambient fine particulate matter (PM2.5). Presented in this study are organic and elemental carbon (OC and EC) within ambient PM2.5 over a three-year period at a forested site in the North Carolina Piedmon. EC exhibited signifi...

Long-term observation of water-soluble chemical components in the bulk atmospheric aerosols collected at Okinawa, Japan

NASA Astrophysics Data System (ADS)

Handa, Daishi; Somada, Yuka; Ijyu, Moriaki; Azechi, Sotaro; Nakaema, Fumiya; Arakaki, Takemitsu; Tanahara, Akira

2010-05-01

The economic development and population growth in recent Asia spread air pollution. Emission rate of air pollutants from Asia, in particular oxides of nitrogen, surpassed those from North America and Europe and should continue to exceed them for decades. The study of the long-range transported air pollution from Asian continent has gained a special attention in Japan because of increase in photochemical oxidants in relatively remote islands. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location in Asia is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. Bulk aerosol samples were collected on quartz filters by using a high volume air sampler. Sampling duration was one week for each sample. We determined the concentrations of water-soluble anions, cations and dissolved organic carbon (DOC) in the bulk aerosols collected at the Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS) using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. We will report water-soluble chemical components data of anions, cations and DOC in bulk atmospheric aerosols collected at CHAAMS during August, 2005 to April, 2010. Seasonal variation of water-soluble chemical components showed that the concentrations were relatively low in summer, higher in fall and winter, and the highest in spring. When air mass came from Asian Continent, the concentrations of water-soluble chemical components were much higher compared to the other directions. In addition, we calculated background concentration of water-soluble chemical components at Okinawa

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

Atmospheric oxidation of 1,3-butadiene: characterization of gas and aerosol reaction products and implications for PM2.5

NASA Astrophysics Data System (ADS)

Jaoui, M.; Lewandowski, M.; Docherty, K.; Offenberg, J. H.; Kleindienst, T. E.

2014-12-01

Secondary organic aerosol (SOA) was generated by irradiating 1,3-butadiene (13BD) in the presence of H2O2 or NOx. Experiments were conducted in a smog chamber operated in either flow or batch mode. A filter/denuder sampling system was used for simultaneously collecting gas- and particle-phase products. The chemical composition of the gas phase and SOA was analyzed using derivative-based methods (BSTFA, BSTFA + PFBHA, or DNPH) followed by gas chromatography-mass spectrometry (GC-MS) or high-performance liquid chromatography (HPLC) analysis of the derivative compounds. The analysis showed the occurrence of more than 60 oxygenated organic compounds in the gas and particle phases, of which 31 organic monomers were tentatively identified. The major identified products include glyceric acid, d-threitol, erythritol, d-threonic acid, meso-threonic acid, erythrose, malic acid, tartaric acid, and carbonyls including glycolaldehyde, glyoxal, acrolein, malonaldehyde, glyceraldehyde, and peroxyacryloyl nitrate (APAN). Some of these were detected in ambient PM2.5 samples, and could potentially serve as organic markers of 13BD. Furthermore, a series of oligoesters were detected and found to be produced through chemical reactions occurring in the aerosol phase between compounds bearing alcoholic groups and compounds bearing acidic groups. SOA was analyzed for organic mass to organic carbon (OM /OC) ratio, effective enthalpy of vaporization (Δ Hvapeff), and aerosol yield. The average OM /OC ratio and SOA density were 2.7 ± 0.09 and 1.2 ± 0.05, respectively. The average Δ Hvapeff was -26.08 ± 1.46 kJ mol-1, a value lower than that of isoprene SOA. The average laboratory SOA yield measured in this study at aerosol mass concentrations between 22.5 and 140.2 μg m-3 was 0.025 ± 0.011, a value consistent with the literature (0.021-0.178). While the focus of this study has been examination of the particle-phase measurements, the gas-phase photooxidation products have also been

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

DOE PAGES

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

2016-11-25

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

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

NASA Astrophysics Data System (ADS)

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

2016-11-01

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

Elemental composition of ambient aerosols measured with high temporal resolution using an online XRF spectrometer

NASA Astrophysics Data System (ADS)

Furger, Markus; Cruz Minguillón, María; Yadav, Varun; Slowik, Jay G.; Hüglin, Christoph; Fröhlich, Roman; Petterson, Krag; Baltensperger, Urs; Prévôt, André S. H.

2017-06-01

The Xact 625 Ambient Metals Monitor was tested during a 3-week field campaign at the rural, traffic-influenced site Härkingen in Switzerland during the summer of 2015. The field campaign encompassed the Swiss National Day fireworks event, providing increased concentrations and unique chemical signatures compared to non-fireworks (or background) periods. The objective was to evaluate the data quality by intercomparison with other independent measurements and test its applicability for aerosol source quantification. The Xact was configured to measure 24 elements in PM10 with 1 h time resolution. Data quality was evaluated for 10 24 h averages of Xact data by intercomparison with 24 h PM10 filter data analysed with ICP-OES for major elements, ICP-MS for trace elements, and gold amalgamation atomic absorption spectrometry for Hg. Ten elements (S, K, Ca, Ti, Mn, Fe, Cu, Zn, Ba, Pb) showed excellent correlation between the compared methods, with r2 values ≥ 0.95. However, the slopes of the regressions between Xact 625 and ICP data varied from 0.97 to 1.8 (average 1.28) and thus indicated generally higher Xact elemental concentrations than ICP for these elements. Possible reasons for these differences are discussed, but further investigations are needed. For the remaining elements no conclusions could be drawn about their quantification for various reasons, mainly detection limit issues. An indirect intercomparison of hourly values was performed for the fireworks peak, which brought good agreement of total masses when the Xact data were corrected with the regressions from the 24 h value intercomparison. The results demonstrate that multi-metal characterization at high-time-resolution capability of Xact is a valuable and practical tool for ambient monitoring.

Ultrafine particles are not major carriers of carcinogenic PAHs and their genotoxicity in size-segregated aerosols.

PubMed

Topinka, Jan; Milcova, Alena; Schmuczerova, Jana; Krouzek, Jiri; Hovorka, Jan

2013-06-14

Some studies suggest that genotoxic effects of combustion-related aerosols are induced by carcinogenic polycyclic aromatic hydrocarbons (c-PAHs) and their derivatives, which are part of the organic fraction of the particulate matter (PM) in ambient air. The proportion of the organic fraction in PM is known to vary with particle size. The ultrafine fraction is hypothesized to be the most important carrier of c-PAHs, since it possesses the highest specific surface area of PM. To test this hypothesis, the distribution of c-PAHs in organic extracts (EOMs) was compared for four size fractions of ambient-air aerosols: coarse (1aerosol particles and ultrafine particles (dae<0.17). High-volume aerosol samples were collected consecutively in four localities that differed in the level of environmental pollution. The genotoxicity of EOMs was measured by analysis of DNA adducts induced in an a cellular assay consisting of calf thymus DNA with/without rat liver microsomal S9 fraction coupled with (32)P-postlabelling. The upper accumulation fraction was the major size fraction in all four localities, forming 37-46% of the total PM mass. Per m(3) of sampled air, this fraction also bound the largest amount of c-PAHs. Correspondingly, the upper accumulation fraction induced the highest DNA-adduct levels. Per PM mass itself, the lower accumulation fraction is seen to be the most efficient in binding DNA-reactive organic compounds. Interestingly, the results suggest that the fraction of ultrafine particles of various ambient-air samples is neither a major carrier of c-PAHs, nor a major inducer of their genotoxicity, which is an important finding that is relevant to the toxicity and health effects of ultrafine particles, which are so extensively discussed these days. Copyright © 2013. Published by Elsevier B.V.

Secondary Organic Aerosol Formation and Aging in a Flow Reactor in the Forested Southeast US during SOAS

NASA Astrophysics Data System (ADS)

Hu, W.; Palm, B. B.; Hacker, L.; Campuzano Jost, P.; Day, D. A.; de Sá, S. S.; Ayres, B. R.; Draper, D.; Fry, J.; Ortega, A. M.; Kiendler-Scharr, A.; Pajunoja, A.; Virtanen, A.; Krechmer, J.; Canagaratna, M. R.; Thompson, S.; Yatavelli, R. L. N.; Stark, H.; Worsnop, D. R.; Martin, S. T.; Farmer, D.; Brown, S. S.; Jimenez, J. L.

2015-12-01

A major field campaign (Southern Oxidant and Aerosol Study, SOAS) was conducted in summer 2013 in a forested area in Centreville Supersite, AL (SEARCH network) in the southeast U.S. To investigate secondary organic aerosol (SOA) formation from biogenic volatile organic compounds (BVOCs), 3 oxidation flow reactors (OFR) were used to expose ambient air to oxidants and their output was analyzed by state-of-the-art gas and aerosol instruments including a High-Resolution Aerosol Mass Spectrometer (HR-AMS), a HR Proton-Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOFMS), and Two HR-TOF Chemical Ionization Mass Spectrometers (HRToF-CIMS). Ambient air was exposed 24/7 to variable concentrations of each of the 3 main atmospheric oxidants (OH, NO3 radicals and O3) to investigate the oxidation of BVOCs (including isoprene derived epoxydiols, IEPOX) and SOA formation and aging. Effective OH exposures up to 1×1013 molec cm-3 s were achieved, equivalent to over a month of aging in the atmosphere. Multiple oxidation products from isoprene and monoterpenes including small gas-phase acids were observed in OH OFR. High SOA formation of up to 12 μg m-3 above ambient concentrations of 5 μg m-3 was observed under intermediate OH exposures, while very high OH exposures led to destruction of ~30% of ambient OA, indicating shifting contributions of functionalization vs. fragmentation, consistent with results from urban and terpene-dominated environments. The highest SOA enhancements were 3-4 times higher than ambient OA. More SOA is typically formed during nighttime when terpenes are higher and photochemistry is absent, and less during daytime when isoprene is higher, although the IEPOX pathway is suppressed in the OFR. SOA is also observed after exposure of ambient air to O3 or NO3, although the amounts and oxidation levels were lower than for OH. Formation of organic nitrates in the NO3 reaction will also be discussed.A major field campaign (Southern Oxidant and Aerosol

Dissolution of aerosol particles collected from nuclear facility plutonium production process

DOE PAGES

Xu, Ning; Martinez, Alexander; Schappert, Michael Francis; ...

2015-08-14

Here, a simple, robust analytical chemistry method has been developed to dissolve plutonium containing particles in a complex matrix. The aerosol particles collected on Marple cascade impactor substrates were shown to be dissolved completely with an acid mixture of 12 M HNO 3 and 0.1 M HF. A pressurized closed vessel acid digestion technique was utilized to heat the samples at 130 °C for 16 h to facilitate the digestion. The dissolution efficiency for plutonium particles was 99 %. The resulting particle digestate solution was suitable for trace elemental analysis and isotope composition determination, as well as radiochemistry measurements.

Effects of aerosol species on atmospheric visibility in Kaohsiung City, Taiwan

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

Chang-Gai Lee; Chung-Shin Yuan; Jui-Cheng Chang

2005-07-01

Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During the study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition ofmore » Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 {mu}m, corresponding with the wavelength region of visible light, which accounted for {approximately} 72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH{sub 4}){sup 2}SO{sub 4}, NH{sub 4}NO{sub 3}, total carbon, and fine particulate matter (PM2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein. 35 refs., 10 figs., 4 tabs.« less

Aerosol Optical Properties of Smoke from the Las Conchas Wildfire, Los Alamos, NM

NASA Astrophysics Data System (ADS)

Gorkowski, K.; Dubey, M. K.; Flowers, B. A.; Aiken, A. C.; Klein, B. Z.; Mazzoleni, C.; Sharma, N.; China`, S.

2011-12-01

The Las Conchas wildfire in Northern New Mexico started on June, 26 2011 and spread rapidly, eventually burning an area of 634 km2 (245 mi2). Due to the close proximity to the fire, the Los Alamos National Laboratory (LANL) was shut down and the town evacuated for several days. Immediately after LANL reopened (7/6/2011) the Earth and Environmental Sciences Division (EES-14) attained unique measurements of the smoke by sampling the ambient air. Three Integrated Photoacoustic/Nephelometer Spectrometers (DMT Inc.) were set up to measure aerosol light absorption and scattering coefficients. A University of Northwest Switzerland thermodenuder was used to remove compounds that are volatile at temperatures up to 200C. The aerosol's optical properties were measured before and after denuding the sample at 405nm (blue), 532nm (green), 781nm (red), and for non-denuded particles also at 375nm (ultraviolet). The aerosol size distributions were measured after the denuder with a Laser Aerosol Spectrometer (LAS, TSI Inc.) and black carbon was measured with a Single Particle Soot Photometer (SP2, DMT Inc.). Additionally, ambient measurements of Total Particulate Matter (PM2.5 and PM10) were collected continuously at the LANL air monitoring stations. These measurements are used in conjunction with numerical simulations to determine the bulk optical properties of the aerosol. Aerosols in wildfire smoke are composed of organic and black carbon (soot) particles that are formed during wood combustion and pyrolysis. The optical properties of the smoke particles are complex and lead to large uncertainties in assessing the global climate. During the measurement period, the Las Conchas fire provided very high particle concentrations (up to 200 μg/m3) that were exploited to investigate their optical properties. By heating the particles to temperatures ranging from 75 to 200C in the denuder, volatile organics were removed and the optical properties of the remaining particles were measured

Biogenic-Anthropogenic Interactions in Secondary Organic Aerosol Formation and Health Effects of Atmospheric Organic Aerosol

NASA Astrophysics Data System (ADS)

Ye, Jianhuai

Secondary organic aerosol (SOA) formed from oxidation of volatile organic compounds (VOCs), comprises a major fraction of atmospheric submicron particulate matter, which is crucial for global climate change and human health. While biogenic VOCs are naturally emitted and cannot be directly controlled, field measurements and satellite observations have shown that biogenic SOA (BSOA) formation correlates well with anthropogenic pollutants and may be anthropogenically controlled. In this work, the formation of the "anthropogenically controllable BSOA" was examined. BSOA from alpha-pinene ozonolysis was investigated in the presence of laboratory-generated or ambient organic aerosol such as Toronto ambient particles. It is shown that SOA was not equally miscible with all organic species. Aerosol mixing thermodynamics in the atmosphere is composition dependent. Based on laboratory observations, an empirical framework using bulk elemental ratios was developed to predict atmospheric organic miscibility and SOA yield enhancements. Besides organic aerosol, interactions between BSOA formation and SO2 was also examined. Synergistic effects were observed between BSOA formation and SO2 oxidation through Criegee and peroxide chemistry under atmospherically relevant RH conditions. In addition to the physicochemical properties of SOA, health impacts of SOA were examined. An atmospheric simulation reactor (ASR) was developed to investigate the health effects of air pollutants by permitting controlled chronic in vivo exposure of mice to combine particulate and gaseous pollutants at 'real-life' concentrations. Results show that daily exposure to SOA from naphthalene photooxidation led to increased airway hyperresponsiveness (AHR) to methacholine in a dose-dependent manner. Multi-pollutant exposures with ozone and/or NO2 in conjunction with a sub-toxic concentration of SOA resulted in additive effects on AHR to methacholine. Inflammatory cell recruitment to the airways was not observed

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

DOE PAGES

Carrico, Christian M.; Gomez, Samantha Laray; Dubey, Manvendra Krishna; ...

2018-01-31

Pyrotechnics (fireworks) displays are common for many cultures worldwide, with Independence Day celebrations occurring annually on July 4th as the most notable in the U.S. Given an episodic nature, fireworks aerosol properties are poorly characterized. Here we report observations of optical properties of fresh smoke emissions from Independence Day fireworks smoke sampled at Los Alamos National Laboratory, New Mexico U.S.A. on 4–5 July 2016. Aerosol optical properties were measured with a photoacoustic extinctiometer (PAX, DMT, Inc., Model 870 nm) at low RH < 30% and a humidity controlled nephelometry system (Ecotech, Inc., 450 nm Aurora). ‘Dry’ light scattering coefficient (σsp)more » increased from background < 15 Mm –1 reaching 120 Mm –1 (450 nm) as a 2-min event peak, while the absorption coefficient increased from background of 0.5–4.4 Mm –1 (870 nm). The event peak occurred at 00:35 on 5 July 2016, ~3 h after local fireworks events, and decreased to background by 04:00 on 5 July 2016, showing well mixed aerosol properties. A notable result is that the aerosol hygroscopic response, as characterized by the ratio of wet to dry light scattering or f(RH = 85%), declined to 1.02 at the peak fireworks influence from a background ~1.7. Strong wavelength dependence of light scattering with Ångström exponent ~2.2 throughout the event showed a size distribution dominated by sub-micrometer particles. Likewise, single scattering albedo at 870 nm remained constant throughout the event with ω = 0.86 ± 0.03, indicating light absorbing carbon, though not dominant, was mixed with organic carbon. Subsequent laboratory testing with ground-level sparklers showed that pyrotechnics smoke can generate a strong hygroscopic response, however. As confirmed with chemical analysis, the chemistry of the fireworks was key to defining the hygroscopic response. As a result, sparkler smoke was dominated by salt species such as hygroscopic potassium chloride while it lacked

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

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

Carrico, Christian M.; Gomez, Samantha Laray; Dubey, Manvendra Krishna

Pyrotechnics (fireworks) displays are common for many cultures worldwide, with Independence Day celebrations occurring annually on July 4th as the most notable in the U.S. Given an episodic nature, fireworks aerosol properties are poorly characterized. Here we report observations of optical properties of fresh smoke emissions from Independence Day fireworks smoke sampled at Los Alamos National Laboratory, New Mexico U.S.A. on 4–5 July 2016. Aerosol optical properties were measured with a photoacoustic extinctiometer (PAX, DMT, Inc., Model 870 nm) at low RH < 30% and a humidity controlled nephelometry system (Ecotech, Inc., 450 nm Aurora). ‘Dry’ light scattering coefficient (σsp)more » increased from background < 15 Mm –1 reaching 120 Mm –1 (450 nm) as a 2-min event peak, while the absorption coefficient increased from background of 0.5–4.4 Mm –1 (870 nm). The event peak occurred at 00:35 on 5 July 2016, ~3 h after local fireworks events, and decreased to background by 04:00 on 5 July 2016, showing well mixed aerosol properties. A notable result is that the aerosol hygroscopic response, as characterized by the ratio of wet to dry light scattering or f(RH = 85%), declined to 1.02 at the peak fireworks influence from a background ~1.7. Strong wavelength dependence of light scattering with Ångström exponent ~2.2 throughout the event showed a size distribution dominated by sub-micrometer particles. Likewise, single scattering albedo at 870 nm remained constant throughout the event with ω = 0.86 ± 0.03, indicating light absorbing carbon, though not dominant, was mixed with organic carbon. Subsequent laboratory testing with ground-level sparklers showed that pyrotechnics smoke can generate a strong hygroscopic response, however. As confirmed with chemical analysis, the chemistry of the fireworks was key to defining the hygroscopic response. As a result, sparkler smoke was dominated by salt species such as hygroscopic potassium chloride while it lacked

Monitoring biological aerosols using UV fluorescence

NASA Astrophysics Data System (ADS)

Eversole, Jay D.; Roselle, Dominick; Seaver, Mark E.

1999-01-01

An apparatus has been designed and constructed to continuously monitor the number density, size, and fluorescent emission of ambient aerosol particles. The application of fluorescence to biological particles suspended in the atmosphere requires laser excitation in the UV spectral region. In this study, a Nd:YAG laser is quadrupled to provide a 266 nm wavelength to excite emission from single micrometer-sized particles in air. Fluorescent emission is used to continuously identify aerosol particles of biological origin. For calibration, biological samples of Bacillus subtilis spores and vegetative cells, Esherichia coli, Bacillus thuringiensis and Erwinia herbicola vegetative cells were prepared as suspensions in water and nebulized to produce aerosols. Detection of single aerosol particles, provides elastic scattering response as well as fluorescent emission in two spectral bands simultaneously. Our efforts have focuses on empirical characterization of the emission and scattering characteristics of various bacterial samples to determine the feasibility of optical discrimination between different cell types. Preliminary spectroscopic evidence suggest that different samples can be distinguished as separate bio-aerosol groups. In addition to controlled sample results, we will also discuss the most recent result on the effectiveness of detection outdoor releases and variations in environmental backgrounds.

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

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

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

2009-03-01

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

Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

PubMed

Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

Evaluating Organic Aerosol Model Performance: Impact of two Embedded Assumptions

NASA Astrophysics Data System (ADS)

Jiang, W.; Giroux, E.; Roth, H.; Yin, D.

2004-05-01

Organic aerosols are important due to their abundance in the polluted lower atmosphere and their impact on human health and vegetation. However, modeling organic aerosols is a very challenging task because of the complexity of aerosol composition, structure, and formation processes. Assumptions and their associated uncertainties in both models and measurement data make model performance evaluation a truly demanding job. Although some assumptions are obvious, others are hidden and embedded, and can significantly impact modeling results, possibly even changing conclusions about model performance. This paper focuses on analyzing the impact of two embedded assumptions on evaluation of organic aerosol model performance. One assumption is about the enthalpy of vaporization widely used in various secondary organic aerosol (SOA) algorithms. The other is about the conversion factor used to obtain ambient organic aerosol concentrations from measured organic carbon. These two assumptions reflect uncertainties in the model and in the ambient measurement data, respectively. For illustration purposes, various choices of the assumed values are implemented in the evaluation process for an air quality model based on CMAQ (the Community Multiscale Air Quality Model). Model simulations are conducted for the Lower Fraser Valley covering Southwest British Columbia, Canada, and Northwest Washington, United States, for a historical pollution episode in 1993. To understand the impact of the assumed enthalpy of vaporization on modeling results, its impact on instantaneous organic aerosol yields (IAY) through partitioning coefficients is analysed first. The analysis shows that utilizing different enthalpy of vaporization values causes changes in the shapes of IAY curves and in the response of SOA formation capability of reactive organic gases to temperature variations. These changes are then carried into the air quality model and cause substantial changes in the organic aerosol modeling

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

Liquid-liquid phase separation in aerosol particles: Imaging at the Nanometer Scale

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

O'Brien, Rachel; Wang, Bingbing; Kelly, Stephen T.

2015-04-21

Atmospheric aerosols can undergo phase transitions including liquid-liquid phase separation (LLPS) while responding to changes in the ambient relative humidity (RH). Here, we report results of chemical imaging experiments using environmental scanning electron microscopy (ESEM) and scanning transmission x-ray microscopy (STXM) to investigate the LLPS of micron sized particles undergoing a full hydration-dehydration cycle. Internally mixed particles composed of ammonium sulfate (AS) and either: limonene secondary organic carbon (LSOC), a, 4-dihydroxy-3-methoxybenzeneaceticacid (HMMA), or polyethylene glycol (PEG-400) were studied. Events of LLPS with apparent core-shell particle morphology were observed for all samples with both techniques. Chemical imaging with STXM showed thatmore » both LSOC/AS and HMMA/AS particles were never homogeneously mixed for all measured RH’s above the deliquescence point and that the majority of the organic component was located in the shell. The shell composition was estimated as 65:35 organic: inorganic in LSOC/AS and as 50:50 organic: inorganic for HMMA/AS. PEG-400/AS particles showed fully homogeneous mixtures at high RH and phase separated below 89-92% RH with an estimated 50:50% organic to inorganic mix in the shell. These two chemical imaging techniques are well suited for in-situ analysis of the hygroscopic behavior, phase separation, and surface composition of collected ambient aerosol particles.« less

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

NASA Astrophysics Data System (ADS)

Sullivan, Amy P.

This thesis characterizes the ambient fine organic carbon (OC) aerosol and investigates its sources through the development and deployment of new analytical measurement techniques. Recognizing that OC is highly chemically complex, the approach was to develop methods capable of quantitatively measuring a large chemical fraction of the aerosol instead of specific chemical speciation. The focus is on organic compounds that are soluble in water (WSOC) since little is known about its chemical nature. The results from this thesis show that WSOC has mainly two sources: biomass burning and secondary organic aerosol (SOA). In urban areas, WSOC increases with plume age, and tracks other photochemically produced compounds. Chemical analysis of WSOC suggests that in urban Atlanta, the SOA is mainly small-chain aliphatic compounds indirectly linked to vehicle emissions. A method was first developed for quantitative on-line measurements of WSOC by extending the application of the Particle-into-Liquid Sampler (PILS) from inorganic to organic aerosol measurements. In this approach a PILS captures ambient particles into a flow of purified water, which is then forced through a liquid filter and the carbonaceous content quantified on-line by a Total Organic Carbon (TOC) analyzer. An instrument was first developed for ground-based measurements and then modified for airborne deployment. Ground-based measurements at the St. Louis - Midwest Supersite during the summer of 2003 showed that the fraction of OC that is water-soluble can have a highly diurnal pattern with WSOC to OC ratios reaching 0.80 during the day and lows of 0.40 during the night. During extended periods under stagnation pollution events, this pattern was well correlated with ozone concentrations. The results are consistent with formation of SOA. Airborne PILS-TOC measurements from the NOAA WP-3D during the New England Air Quality Study/Intercontinental Transport and Chemical Transformation (NEAQS/ITCT) 2004 program

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA Technical Reports Server (NTRS)

Ackerman, A.; Jensen, E.; Stevens, D.; Wang, D.; Heymsfield, A.; Miloshevich, L.; Twohy, C.; Poellot, M.; VanReken, T.; Fridland, Ann

2003-01-01

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores

NASA Astrophysics Data System (ADS)

Bluvshtein, Nir; Lin, Peng; Flores, J. Michel; Segev, Lior; Mazar, Yinon; Tas, Eran; Snider, Graydon; Weagle, Crystal; Brown, Steven S.; Laskin, Alexander; Rudich, Yinon

2017-05-01

The radiative effects of biomass-burning aerosols on regional and global scales can be substantial. Accurate modeling of the radiative effects of smoke aerosols requires wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass-burning aerosols from 300 to 650 nm wavelengths during a regional nighttime bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about 2 orders of magnitude, changing the single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and slightly aged biomass-burning aerosols. In addition, PM2.5 filter samples were collected for detailed offline chemical analysis of the water-soluble organics that contribute to light absorption. Nitroaromatics were identified as major organic species responsible for the increased absorption at 400 to 500 nm. Typical chromophores include 4-nitrocatechol, 4-nitrophenol, nitrosyringol, and nitroguaiacol; oxidation-nitration products of methoxyphenols; and known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosols from biomass burning in absorption of solar radiation and in effective radiative forcing.

PIXE Analysis of Indoor Aerosols

NASA Astrophysics Data System (ADS)

Johnson, Christopher; Turley, Colin; Moore, Robert; Battaglia, Maria; Labrake, Scott; Vineyard, Michael

2011-10-01

We have performed a proton-induced X-ray emission (PIXE) analysis of aerosol samples collected in academic buildings at Union College to investigate the air quality in these buildings and the effectiveness of their air filtration systems. This is also the commissioning experiment for a new scattering chamber in the Union College Ion-Beam Analysis Laboratory. The aerosol samples were collected on Kapton foils using a nine-stage cascade impactor that separates particles according to their aerodynamic size. The foils were bombarded with beams of 2.2-MeV protons from the Union College 1.1-MV Pelletron Accelerator and the X-ray products were detected with an Amptek silicon drift detector. After subtracting the contribution from the Kapton foils, the X-ray energy spectra of the aerosol samples were analyzed using GUPIX software to determine the elemental concentrations of the samples. We will describe the collection of the aerosol samples, discuss the PIXE analysis, and present the results.

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

PubMed

Mikuska, Pavel; Vecera, Zbynek

2005-09-01

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

Identifying precursors and aqueous organic aerosol formation pathways during the SOAS campaign

NASA Astrophysics Data System (ADS)

Sareen, Neha; Carlton, Annmarie G.; Surratt, Jason D.; Gold, Avram; Lee, Ben; Lopez-Hilfiker, Felipe D.; Mohr, Claudia; Thornton, Joel A.; Zhang, Zhenfa; Lim, Yong B.; Turpin, Barbara J.

2016-11-01

Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized, low-volatility organic aerosol and, in some cases, light-absorbing (brown) carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, and health. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented, forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols), leading to the formation of secondary organic aerosol (SOAAQ). Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify additional precursors and products that may be atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere into water at Brent, Alabama, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Hydroxyl (OH⚫) radical oxidation experiments were conducted with the aqueous mixtures collected from SOAS to better understand the formation of SOA through gas-phase followed by aqueous-phase chemistry. Total aqueous-phase organic carbon concentrations for these mixtures ranged from 92 to 179 µM-C, relevant for cloud and fog waters. Aqueous OH-reactive compounds were primarily observed as odd ions in the positive ion mode by electrospray ionization mass spectrometry (ESI-MS). Ultra high-resolution Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) spectra and tandem MS (MS-MS) fragmentation of these ions were consistent with the presence of carbonyls and tetrols. Products were observed in the negative ion mode and included pyruvate and oxalate, which were confirmed by ion chromatography. Pyruvate and oxalate have been found in the particle phase in many locations (as salts and complexes). Thus

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.

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

Fluorescent biological aerosol particles measured with the Waveband Integrated Bioaerosol Sensor WIBS-4: laboratory tests combined with a one year field study

NASA Astrophysics Data System (ADS)

Toprak, E.; Schnaiter, M.

2013-01-01

In this paper bioaerosol measurements conducted with the Waveband Integrated Bioaerosol Sensor mark 4 (WIBS-4) are presented. The measurements comprise aerosol chamber characterization experiments and a one-year ambient measurement period at a semi-rural site in South Western Germany. This study aims to investigate the sensitivity of WIBS-4 to biological and non-biological aerosols and detection of biological particles in the ambient aerosol. Several types of biological and non-biological aerosol samples, including fungal spores, bacteria, mineral dust, ammonium sulphate, combustion soot, and fluorescent polystyrene spheres, were analyzed by WIBS-4 in the laboratory. The results confirm the sensitivity of the ultraviolet light-induced fluorescence (UV-LIF) method to biological fluorophores and show the good discrimination capabilities of the two excitation wavelengths/detection wavebands method applied in WIBS-4. However, a weak cross-sensitivity to non-biological fluorescent interferers remains and is discussed in this paper. All the laboratory studies have been undertaken in order to prepare WIBS-4 for ambient aerosol measurements. According to the one-year ambient aerosol study, number concentration of fluorescent biological aerosol particles (FBAP) show strong seasonal and diurnal variability. The highest number concentration of FBAP was measured during the summer term and decreased towards the winter period when colder and drier conditions prevail. Diurnal FBAP concentrations start to increase after sunset and reach maximum values during the late night and early morning hours. On the other hand, the total aerosol number concentration was almost always higher during daytime than during nighttime and a sharp decrease after sunset was observed. There was no correlation observed between the FBAP concentration and the meteorological parameters temperature, precipitation, wind direction and wind speed. However, a clear correlation was identified between the FBAP

Seasonal variation of water-soluble chemical components in the bulk atmospheric aerosols collected at Okinawa Island, Japan

NASA Astrophysics Data System (ADS)

Handa, D.; Nakajima, H.; Nakaema, F.; Arakaki, T.; Tanahara, A.

2008-12-01

The economic development and population growth in recent Asia spread air pollution. Emission rate of air pollutants from Asia, in particular oxides of nitrogen, surpassed those from North America and Europe and should continue to exceed them for decades. The study of the air pollution transported from Asian continent has gained a special attention in Japan. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location is ideal in observing East Asian atmospheric aerosols because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. In 2005, Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS) was established by the National Institute for Environmental Studies (NIES) at the northern tip of Okinawa Island, Japan to monitor the air quality of Asia. Bulk aerosol samples were collected on quartz filters by using a high volume air sampler. Sampling duration was one week for each sample. We determined the concentrations of water-soluble anions, cations and dissolved organic carbon in the bulk aerosols collected at the CHAAMS, using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. Seasonal variation of water-soluble chemical components showed that the concentrations were relatively low in summer, higher in fall and winter, and the highest in spring. When air mass came from Asian Continent, the concentrations of water-soluble chemical components were much higher compared to the other directions.

Use of RNA amplification and electrophoresis for studying virus aerosol collection efficiency and their comparison with plaque assays.

PubMed

Jiang, Xiao; Pan, Maohua; Hering, Susanne V; Lednicky, John A; Wu, Chang-Yu; Fan, Z Hugh

2016-10-01

The spread of virus-induced infectious diseases through airborne routes of transmission is a global concern for economic and medical reasons. To study virus transmission, it is essential to have an effective aerosol collector such as the growth tube collector (GTC) system that utilizes water-based condensation for collecting virus-containing aerosols. In this work, we characterized the GTC system using bacteriophage MS2 as a surrogate for a small RNA virus. We investigated using RNA extraction and reverse transcription- polymerase chain reaction (RT-PCR) to study the total virus collection efficiency of the GTC system. Plaque assays were also used to enumerate viable viruses collected by the GTC system compared to that by a commercially available apparatus, the SKC® Biosampler. The plaque assay counts were used to enumerate viable viruses whereas RT-PCR provides a total virus count, including those viruses inactivated during collection. The effects of relative humidity (RH) and other conditions on collection efficiency were also investigated. Our results suggest that the GTC has a collection efficiency for viable viruses between 0.24 and 1.8% and a total virus collection efficiency between 18.3 and 79.0%, which is 1-2 orders of magnitude higher than that of the SKC® Biosampler. Moreover, higher RH significantly increases both the viable and total collection efficiency of the GTC, while its effect on the collection efficiency of the SKC® Biosampler is not significant. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

PubMed

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

2010-04-01

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

Aerosol composition and sources in the Central Arctic Ocean during ASCOS

NASA Astrophysics Data System (ADS)

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

2011-05-01

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

Aerosol Chemistry of Furfural and Sugars

NASA Astrophysics Data System (ADS)

Srithawirat, T.; Brimblecombe, P.

2008-12-01

Furfural and sugars (as levoglucosan equivalent) are derived from biomass burning and contribute to aerosol composition. This study examined the potential of furfural and levoglucosan to be tracers of biomass burning. Furfural is likely to be oxidized quickly so comparison with levoglucosan may give a sense of the age of the aerosols in forest fire smoke. However, few furfural emissions are available for biomass combustion. Furfural and sugars were determined in coarse aerosols (>2.4μm aerodynamic diameter) and fine aerosols (<2.4μm aerodynamic diameter) collected in 24 hour periods during different seasons in the United Kingdom and PM10 collected from Thailand and Malaysia including haze episodes. Also total suspended particulate matter (TSP) samples were collected from Taiwan. Furfural and sugars dominated in fine fractions, especially in the UK autumn. Sugars were found at 5.96-18.37 nmol m-3 in fine mode and 1.36-5.75 nmol m-3 in coarse mode aerosols in the UK. Furfural was found at 0.18-0.91 nmol m-3 and 0.05-0.51 nmol m-3 respectively in the same aerosols. Sugars were a dominant contributor to aerosol derived from biomass burning. Sugars and furfural were about 10 and 20 times higher during haze episodes in Malaysia. Laboratory experimental simulation suggested furfural is more rapid destroyed by UV and sunlight than levoglucosan.

The colors of biomass burning aerosols in the atmosphere.

PubMed

Liu, Chao; Chung, Chul Eddy; Zhang, Feng; Yin, Yan

2016-06-16

Biomass burning aerosols mainly consist of black carbon (BC) and organic aerosols (OAs), and some of OAs are brown carbon (BrC). This study simulates the colors of BrC, BC and their mixture with scattering OAs in the ambient atmosphere by using a combination of light scattering simulations, a two-stream radiative transfer model and a RGB (Red, Green, Blue) color model. We find that both BCs and tar balls (a class of BrC) appear brownish at small particle sizes and blackish at large sizes. This is because the aerosol absorption Ångström exponent (AAE) largely controls the color and larger particles give smaller AAE values. At realistic size distributions, BCs look more blackish than tar balls, but still exhibit some brown color. However, when the absorptance of aerosol layer at green wavelength becomes larger than approximately 0.8, all biomass burning aerosols look blackish. The colors for mixture of purely scattering and absorptive carbonaceous aerosol layers in the atmosphere are also investigated. We suggest that the brownishness of biomass burning aerosols indicates the amount of BC/BrC as well as the ratio of BC to BrC.

Apparatus for sampling and characterizing aerosols

DOEpatents

Dunn, Patrick F.; Herceg, Joseph E.; Klocksieben, Robert H.

1986-01-01

Apparatus for sampling and characterizing aerosols having a wide particle size range at relatively low velocities may comprise a chamber having an inlet and an outlet, the chamber including: a plurality of vertically stacked, successive particle collection stages; each collection stage includes a separator plate and a channel guide mounted transverse to the separator plate, defining a labyrinthine flow path across the collection stage. An opening in each separator plate provides a path for the aerosols from one collection stage to the next. Mounted within each collection stage are one or more particle collection frames.

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

DOE PAGES

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

2011-02-01

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

Source and long-term behavior of transuranic aerosols in the WIPP environment.

PubMed

Thakur, P; Lemons, B G

2016-10-01

Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2013-05-01

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

Gas/Particle Partitioning of Organic Acids and Organic Aerosols in a Ponderosa Pine Forest in Colorado during BEACHON-RoMBAS 2011

NASA Astrophysics Data System (ADS)

Jimenez, J. L.; Yatavelli, L.; Stark, H.; Hayes, P. L.; Campuzano-Jost, P.; Thompson, S.; Kimmel, J. R.; Day, D. A.; Cubison, M. J.; Thornton, J. A.; Jayne, J.; Worsnop, D. R.

2012-12-01

The Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study (BEACHON-RoMBAS) took place at Manitou Forest, CO, during July-Aug. 2011. Gas and particle-phase organic acids were analyzed in real time using a micro-orifice volatilization impactor chemical ionization high-resolution time-of-flight mass spectrometer (MOVI-HRToF-CIMS; Yatavelli et al., AS&T 2012; Yatavelli & Thornton, AS&T 2010) with acetate as the reagent ion. During the gas sampling phase (when the MOVI was at room temperature) aerosol was collected on the MOVI impactor, and was subsequently thermally desorbed over 10 min. under nitrogen, allowing the collection of temperature-programmed thermal desorption (TPTD) mass spectra of particle-phase species. The high resolution of the instrument allows the determination of the elemental composition of most detected ions. Positive Matrix Factorization (PMF) is shown to be very useful to quantify the CIMS backgrounds during the different phases of operation. Two methods were used to estimate the volatility of the detected species. First, the fraction of each species in the particle phase (Fp) vs carbon number was found to approximately follow partitioning theory, both for the alkanoic acids and also for the total acid signal, after accounting for the effect of the oxidation state on vapor pressure. Fp was found to respond on timescales of ~1 h to changes in ambient temperature, indicating that diffusion limitations to evaporation are not major for the aerosol at this site. Preliminary results suggest that Fp depends more strongly on vapor pressure and temperature than on RH, suggesting preferential partitioning for the organic phase rather than the water phase. Secondly, the volatility of individual or groups of acids can be quantified based on the TPTD signal based on calibration with multiple acids of known vapor pressure at concentrations similar to ambient, analogous to the methods of

Measurement of aerosol chemical, physical and radiative properties in the Yangtze delta region of China

NASA Astrophysics Data System (ADS)

Xu, Jin; Bergin, M. H.; Yu, X.; Liu, G.; Zhao, J.; Carrico, C. M.; Baumann, K.

In order to understand the possible influence of aerosols on the environment in the agricultural Yangtze delta region of China, a one-month field sampling campaign was carried out during November 1999 in Linan, China. Measurements included the aerosol light scattering coefficient at 530 nm, σsp, measured at both dry relative humidity (RH<40%) and under ambient conditions (sample RH=63±19%), and the absorption coefficient at 565 nm, σap, for aerosol particles having diameters <2.5 μm (PM 2.5). At the same time, daily filter samples of PM 2.5 as well as aerosol particles having diameters <10 μm (PM 10) were collected and analyzed for mass, major ion, organic compound (OC), and elemental carbon (EC) concentrations in order to determine which anthropogenic chemical species were primarily responsible for aerosol light extinction. The aerosol loading in the rural Yangtze delta region was comparable to highly polluted urban areas, with mean and standard deviation (S.D.) values for σsp, σap and PM 2.5 of 353 Mm -1 (202 Mm -1), 23 Mm -1 (14 Mm -1) and 90 μg m -3 (47 μg m -3), respectively. A clear diurnal pattern was observed in σsp and σap with minimum values occurring in the middle of the day, most likely associated with the maximum midday mixing height. The ratio of the change in light scattering coefficient at ambient RH to that at controlled RH (RH<40%), Fσsp (RH), indicates that condensed water typically contributed ˜40% to the light scattering budget in this region. The mass scattering efficiency of the dry aerosol, E scat_2.5, and mass absorption efficiency of EC, E abs_2.5, have mean and S.D. values of 4.0 m 2 g -1 (0.4 m 2 g -1) and 8.6 m 2 g -1 (7.0 m 2 g -1), respectively. PM 2.5 concentrations in Linan and two other locations in the Yangtze delta, Sheshan and Changshu (which have monthly mean values ranging from ˜80 to 110 μg m -3), are all significantly higher than the proposed 24-h average US PM 2.5 NAAQS of 65 μg m -3. Organic compounds are

Size selective isocyanate aerosols personal air sampling using porous plastic foams

NASA Astrophysics Data System (ADS)

Khanh Huynh, Cong; Duc, Trinh Vu

2009-02-01

As part of a European project (SMT4-CT96-2137), various European institutions specialized in occupational hygiene (BGIA, HSL, IOM, INRS, IST, Ambiente e Lavoro) have established a program of scientific collaboration to develop one or more prototypes of European personal samplers for the collection of simultaneous three dust fractions: inhalable, thoracic and respirable. These samplers based on existing sampling heads (IOM, GSP and cassettes) use Polyurethane Plastic Foam (PUF) according to their porosity to support sampling and separator size of the particles. In this study, the authors present an original application of size selective personal air sampling using chemical impregnated PUF to perform isocyanate aerosols capturing and derivatizing in industrial spray-painting shops.

2-Hydroxyterpenylic acid: An oxygenated marker compound for a-pinene secondary organic aerosol in ambient fine aerosol

EPA Science Inventory

An oxygenated MW 188 compound is commonly observed in substantial abundance in atmospheric aerosol samples and was proposed in previous studies as an α-pinene-related marker compound that is associated with aging processes. Owing to difficulties in producing this compound in suff...

Light Absorption of Brown Carbon Aerosol in the Pearl River Delta Region of China

NASA Astrophysics Data System (ADS)

Huang, X.

2015-12-01

X.F. Huang, J.F. Yuan, L.M. Cao, J. Cui, C.N. Huang, Z.J. Lan and L.Y. He Key Laboratory for Urban Habitat Environmental Science and Technology, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen 518055, ChinaCorresponding author. Tel.: +86 755 26032532; fax: +86 755 26035332. E-mail address: huangxf@pku.edu.cn (X. F. Huang). Abstract: The strong spectral dependence of light absorption of brown carbon (BrC) aerosol has been recognized in recent decades. The Absorption Angstrom Exponent (AAE) of ambient aerosol was widely used in previous studies to attribute light absorption of brown carbon at shorter wavelengths, with a theoretical assumption that the AAE of black carbon (BC) aerosol equals to unit. In this study, the AAE method was improved by statistical extrapolation based on ambient measurements in the polluted seasons in typical urban and rural areas in the Pearl River Delta (PRD) region of China. A three-wavelength photoacoustic soot spectrometer (PASS-3) and an aerosol mass spectrometer (AMS) were used to explore the relationship between the ambient measured AAE and the ratio of organic aerosol to BC aerosol, in order to extract the more realistic AAE by pure BC aerosol, which were found to be 0.86, 0.82 and 1.02 at 405nm and 0.70, 0.71, and 0.86 at 532nm in the campaigns of urban-winter, urban-fall, and rural-fall, respectively. Roadway tunnel experiment results further supported the effectiveness of the obtained AAE for pure BC aerosol. In addition, biomass burning experiments proved higher spectral dependence of more-BrC environment and further verified the reliability of the instruments' response. Then, the average light absorption contribution of BrC aerosol was calculated to be 11.7, 6.3 and 12.1% (with total relative uncertainty of 7.5, 6.9 and 10.0%) at 405nm and 10.0, 4.1 and 5.5% (with total relative uncertainty of 6.5, 8.6 and 15.4%) at 532nm of the three campaigns, respectively. These results indicate that the

Impact of Transpacific Aerosol on Air Quality over the United States: A Perspective from Aerosol-Cloud-Radiation Interactions

NASA Technical Reports Server (NTRS)

Tao, Zhining; Yu, Hongbin; Chin, Mian

2015-01-01

Observations have well established that aerosols from various sources in Asia, Europe, and Africa can travel across the Pacific and reach the contiguous United States (U.S.) at least on episodic bases throughout a year, with a maximum import in spring. The imported aerosol not only can serve as an additional source to regional air pollution (e.g., direct input), but also can influence regional air quality through the aerosol-cloud-radiation (ACR) interactions that change local and regional meteorology. This study assessed impacts of the transpacific aerosol on air quality, focusing on surface ozone and PM2.5, over the U.S. using the NASA Unified Weather Research Forecast model. Based on the results of 3- month (April to June of 2010) simulations, the impact of direct input (as an additional source) of transpacific aerosol caused an increase of surface PM2.5 concentration by approximately 1.5 micro-g/cu m over the west coast and about 0.5 micro-g/cu m over the east coast of the U.S. By influencing key meteorological processes through the ACR interactions, the transpacific aerosol exerted a significant effect on both surface PM2.5 (+/-6 micro-g/cu m3) and ozone (+/-12 ppbv) over the central and eastern U.S. This suggests that the transpacific transport of aerosol could either improve or deteriorate local air quality and complicate local effort toward the compliance with the U.S. National Ambient Air Quality Standards.

The Hygroscopicity Parameter of Marine Organics in Sea Spray Aerosols

NASA Astrophysics Data System (ADS)

Boyer, M.; Chang, R. Y. W.

2015-12-01

The effects of aerosols on climate are poorly understood, specifically with respect to their influence on cloud properties. Since oceans cover >70% of Earth's surface, sea spray aerosols (SSA), which act efficiently as cloud condensation nuclei (CCN), may have important implications on Earth's radiation budget. Surface active organic species readily accumulate in the sea surface microlayer (SML), located at the ocean-atmosphere interface, and transfer onto nascent SSA. While it is understood that SSA are commonly enriched with organics, the resulting effect of the organic content on CCN activation remains unresolved. The hygroscopicity parameter, kappa (k), allows for the cloud nucleating properties of individual components to be predicted in particles of mixed composition; however, most studies typically infer k from ambient measurements without assessing the contribution of the individual components to the overall k. In this study, a method for quantifying the cloud nucleating properties of the organic species in surface seawater using k-Kohler theory is proposed. Ambient SML and bulk water samples will be collected and atomized to generate particles such that the overall k can be inferred from CCN measurements. The inorganic and organic components will be quantified, and the organic component will be separated so that the hygroscopicity of only the organic constituents can be determined. By comparing the inferred k values for the samples before and after removal of the inorganic component, the hygroscopicity of the organic constituents alone can be calculated, providing insight on the effect of organic species on CCN activation in SSA.

Stable Carbon Fractionation In Size Segregated Aerosol Particles Produced By Controlled Biomass Burning

NASA Astrophysics Data System (ADS)

Masalaite, Agne; Garbaras, Andrius; Garbariene, Inga; Ceburnis, Darius; Martuzevicius, Dainius; Puida, Egidijus; Kvietkus, Kestutis; Remeikis, Vidmantas

2014-05-01

Biomass burning is the largest source of primary fine fraction carbonaceous particles and the second largest source of trace gases in the global atmosphere with a strong effect not only on the regional scale but also in areas distant from the source . Many studies have often assumed no significant carbon isotope fractionation occurring between black carbon and the original vegetation during combustion. However, other studies suggested that stable carbon isotope ratios of char or BC may not reliably reflect carbon isotopic signatures of the source vegetation. Overall, the apparently conflicting results throughout the literature regarding the observed fractionation suggest that combustion conditions may be responsible for the observed effects. The purpose of the present study was to gather more quantitative information on carbonaceous aerosols produced in controlled biomass burning, thereby having a potential impact on interpreting ambient atmospheric observations. Seven different biomass fuel types were burned under controlled conditions to determine the effect of the biomass type on the emitted particulate matter mass and stable carbon isotope composition of bulk and size segregated particles. Size segregated aerosol particles were collected using the total suspended particle (TSP) sampler and a micro-orifice uniform deposit impactor (MOUDI). The results demonstrated that particle emissions were dominated by the submicron particles in all biomass types. However, significant differences in emissions of submicron particles and their dominant sizes were found between different biomass fuels. The largest negative fractionation was obtained for the wood pellet fuel type while the largest positive isotopic fractionation was observed during the buckwheat shells combustion. The carbon isotope composition of MOUDI samples compared very well with isotope composition of TSP samples indicating consistency of the results. The measurements of the stable carbon isotope ratio in

Diurnal Evolution of Aerosol Optical Properties and Morphology at Pico Tres Padres: A Phenomenological Analysis

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; Chakrabarty, R.; Dubey, M. K.; Moosmuller, H.; Chylek, P.; Onasch, T. B.; Herndon, S.; Zavala, M.; Kolb, C.

2007-05-01

Aerosol optical properties affect planetary radiative balance and therefore climate. The optical properties are related to chemical composition, size distribution, and morphology, which also have implications for human health and environmental degradation. During the MILAGRO field campaign, we measured ensemble aerosol absorption and angle-integrated scattering in Mexico City. These measurements were performed using the Los Alamos aerosol photoacoustic instrument with an integrated nephelometer (LAPA) operating at 781 nm. The LAPA was mounted on-board the Aerodyne Inc. mobile laboratory, which hosted a wide variety of gaseous and aerosol instruments. During the campaign, the Aerodyne mobile laboratory was moved to different sites, capturing the influence of spatial and temporal parameters including location, aging, elevation, and sources on ambient air pollution. The LAPA operated almost continuously between the 3rd and the 28th of March 2006. During the same period we collected ambient aerosols on more than 100 Nuclepore filters for scanning electron microscopy (SEM) analysis. Filter samples were collected during specific pollution events and different times of the day. Subsequently, SEM images of selected filters were taken to study particle morphology. The elemental composition of a few individual particles was also qualitatively assessed by energy dispersive X-ray spectroscopy. Between March 7th and 19th the laboratory was sampling air close to the top of the Pico Tres Padres, a ~3000 m high mountain on the north side of the Mexico City. Daily changes of aerosol loading and pollutant concentrations followed the expected diurnal variations of the boundary layer height. Here we report a preliminary analysis of aerosol absorption, scattering, and morphology at Pico Tres Padres for three specific days (9th, 11th and 12th of March 2006). The single scattering albedo (ratio of scattering to total extinction) during these three days showed a characteristic drop in the

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.

Global Survey of Submicron Aerosol Acidity (pH)

NASA Astrophysics Data System (ADS)

Nault, B.; Day, D. A.; Campuzano Jost, P.; Hu, W.; Schroder, J. C.; Bian, H.; Chin, M.; Clegg, S. L.; Colarco, P. R.; Dibb, J. E.; Kim, M. J.; Kodros, J.; Marais, E. A.; Pierce, J. R.; Scheuer, E. M.; Wennberg, P. O.; Jimenez, J. L.

2017-12-01

Aerosol acidity (H+, often expressed as "pH" defined in various ways) is an important property that influences uptake and partitioning of gases, and homogeneous and surface aqueous reactions of key inorganic and organic compounds. As there is currently no rapid method to measure ambient aerosol acidity, a thermodynamic model, constrained by both inorganic aerosol species (e.g., NH4, NO3, SO4, Cl) and at least one inorganic gas (HNO3, NH3, or HCl), are currently understood to lead to the most reliable estimates of aerosol acidity. In this study, we calculated submicron (less than PM1) aerosol pH from the NASA ATom, "pole-to-pole," flights that covers both the Pacific and Atlantic ocean basins. The E-AIM thermodynamic model was used with measurements by an Aerodyne high-resolution time-of-flight aerosol-mass-spectrometer (HR-ToF-AMS) of inorganic aerosol species, along with inorganic gas measurements from other mass spectrometers and ion chromatography. We compare the results with those for the NASA KORUS-AQ, SEAC4RS, DC3, and ARCTAS campaigns, as well as several ground-based campaigns and recently-published studies. This provides an opportunity to compare the aerosol acidity in urban, rural, and remote regions, by season, and between the boundary layer and free troposphere. In addition, we compare the submicron aerosol acidity from these various localities with results from global models, such as GEOS-Chem, in order to investigate the ability of the global models to simulate aerosol acidity, and the processes it affects, such as nitrate, ammonium, and MSA partitioning.

Burning of olive tree branches: a major organic aerosol source in the Mediterranean

NASA Astrophysics Data System (ADS)

Kostenidou, E.; Kaltsonoudis, C.; Tsiflikiotou, M.; Louvaris, E.; Russell, L. M.; Pandis, S. N.

2013-09-01

Aerosol produced during the burning of olive tree branches was characterized with both direct source sampling (using a mobile smog chamber) and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8-10% black carbon (BC), 5% potassium, 3-4% sulfate, 2-3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA) consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O : C) ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034-0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O : C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs) such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF) was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%), HOA (hydrocarbon-like organic aerosol, 11.3%) and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.9 g kg-1. Assuming that half of the olive tree branches pruned is burned in Greece, 2300 ± 600 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in Mediterranean countries.

Burning of olive tree branches: a major organic aerosol source in the Mediterranean

NASA Astrophysics Data System (ADS)

Kostenidou, E.; Kaltsonoudis, C.; Tsiflikiotou, M.; Louvaris, E.; Russell, L. M.; Pandis, S. N.

2013-03-01

Aerosol produced during the burning of olive tree branches was characterized with both direct source-sampling (using a mobile smog chamber) and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8-10% black carbon (BC), 5% potassium, 3-4% sulfate, 2-3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA) consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O:C) ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034-0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O:C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs) such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF) was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%), HOA (hydrocarbon-like organic aerosol, 11.3%) and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.2 g kg-1. Assuming that half of the olive tree branches pruned is burned in Greece 2280 ± 140 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in the Mediterranean countries.

DEVELOPMENT OF A TAMPER RESISTANT/INDICATING AEROSOL COLLECTION SYSTEM FOR ENVIRONMENTAL SAMPLING AT BULK HANDLING FACILITIES

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

Sexton, L.

2012-06-06

Environmental sampling has become a key component of International Atomic Energy Agency (IAEA) safeguards approaches since its approval for use in 1996. Environmental sampling supports the IAEA's mission of drawing conclusions concerning the absence of undeclared nuclear material or nuclear activities in a Nation State. Swipe sampling is the most commonly used method for the collection of environmental samples from bulk handling facilities. However, augmenting swipe samples with an air monitoring system, which could continuously draw samples from the environment of bulk handling facilities, could improve the possibility of the detection of undeclared activities. Continuous sampling offers the opportunity tomore » collect airborne materials before they settle onto surfaces which can be decontaminated, taken into existing duct work, filtered by plant ventilation, or escape via alternate pathways (i.e. drains, doors). Researchers at the Savannah River National Laboratory and Oak Ridge National Laboratory have been working to further develop an aerosol collection technology that could be installed at IAEA safeguarded bulk handling facilities. The addition of this technology may reduce the number of IAEA inspector visits required to effectively collect samples. The principal sample collection device is a patented Aerosol Contaminant Extractor (ACE) which utilizes electrostatic precipitation principles to deposit particulates onto selected substrates. Recent work has focused on comparing traditional swipe sampling to samples collected via an ACE system, and incorporating tamper resistant and tamper indicating (TRI) technologies into the ACE system. Development of a TRI-ACE system would allow collection of samples at uranium/plutonium bulk handling facilities in a manner that ensures sample integrity and could be an important addition to the international nuclear safeguards inspector's toolkit. This work was supported by the Next Generation Safeguards Initiative (NGSI

Atmospheric oxidation of 1,3-butadiene: characterization of gas and aerosol reaction products and implication for PM2.5

NASA Astrophysics Data System (ADS)

Jaoui, M.; Lewandowski, M.; Docherty, K.; Offenberg, J. H.; Kleindienst, T. E.

2014-06-01

Secondary organic aerosol (SOA) was generated by irradiating 1,3-butadiene (13BD) in the presence of H2O2 or NOx. Experiments were conducted in a smog chamber operated in either flow or batch mode. A filter/denuder sampling system was used for simultaneously collecting gas- and particle-phase products. The chemical composition of the gas phase and SOA was analyzed using derivative-based methods (BSTFA, BSTFA + PFBHA, or DNPH) followed by gas chromatography-mass spectrometry (GC-MS) or high-performance liquid chromatography (HPLC) analysis of the derivative compounds. The analysis showed the occurrence of more than 60 oxygenated organic compounds in the gas and particle phases, of which 31 organic monomers were tentatively identified. The major identified products include glyceric acid, d-threitol, erythritol, d-threonic acid, meso-threonic acid, erythrose, malic acid, tartaric acid, and carbonyls including glycolaldehyde, glyoxal, acrolein, malonaldehyde, glyceraldehyde, and peroxyacryloyl nitrate (APAN). Some of these were detected in ambient PM2.5 samples and could potentially serve as organic markers of 1,3-butadiene (13BD). Furthermore, a series of oligoesters were detected and found to be produced from esterification reactions among compounds bearing alcoholic groups and compounds bearing acidic groups. Time profiles are provided for selected compounds. SOA was analyzed for organic mass to organic carbon (OM / OC) ratio, effective enthalpy of vaporization (ΔHvapeff), and aerosol yield. The average OM / OC ratio and SOA density were 2.7 ± 0.09 and 1.2 ± 0.05, respectively. The average ΔHvapeff was 26.1 ± 1.5 kJ mol-1, a value lower than that of isoprene SOA. The average laboratory SOA yield measured in this study at aerosol mass concentrations between 22.5 and 140.2 μg m-3 was 0.025 ± 0.011, a value consistent with the literature (0.021-0.178). While the focus of this study has been examination of the particle-phase measurements, the gas

Indian aerosols: present status.

PubMed

Mitra, A P; Sharma, C

2002-12-01

This article presents the status of aerosols in India based on the research activities undertaken during last few decades in this region. Programs, like International Geophysical Year (IGY), Monsoon Experiment (MONEX), Indian Middle Atmospheric Program (IMAP) and recently conducted Indian Ocean Experiment (INDOEX), have thrown new lights on the role of aerosols in global change. INDOEX has proved that the effects of aerosols are no longer confined to the local levels but extend at regional as well as global scales due to occurrence of long range transportation of aerosols from source regions along with wind trajectories. The loading of aerosols in the atmosphere is on rising due to energy intensive activities for developmental processes and other anthropogenic activities. One of the significant observation of INDOEX is the presence of high concentrations of carbonaceous aerosols in the near persistent winter time haze layer over tropical Indian Ocean which have probably been emitted from the burning of fossil-fuels and biofuels in the source region. These have significant bearing on the radiative forcing in the region and, therefore, have potential to alter monsoon and hydrological cycles. In general, the SPM concentrations have been found to be on higher sides in ambient atmosphere in many Indian cities but the NOx concentrations have been found to be on lower side. Even in the haze layer over Indian Ocean and surrounding areas, the NOx concentrations have been reported to be low which is not conducive of O3 formation in the haze/smog layer. The acid rain problem does not seem to exist at the moment in India because of the presence of neutralizing soil dust in the atmosphere. But the high particulate concentrations in most of the cities' atmosphere in India are of concern as it can cause deteriorated health conditions.

Fluorescent biological aerosol particles (FBAPs) measured with the Waveband Integrated Bioaerosol Sensor WIBS-4: laboratory tests combined with a one year field study

NASA Astrophysics Data System (ADS)

Toprak, E.; Schnaiter, M.

2012-07-01

In this paper bioaerosol measurements conducted with the Waveband Integrated Bioaerosol Sensor mark 4 (WIBS-4) are presented. The measurements comprise aerosol chamber characterization experiments and a one-year ambient measurement period at a semi-rural site in South Western Germany. This study aims to investigate the sensitivity of WIBS-4 to biological and non-biological aerosols, performance of WIBS-4 for discrimination of several types of aerosols, and the detection and identification of biological particles in the ambient aerosol. Several types of biological and non-biological aerosol samples including spores, bacteria, pollen, mineral dust, ammonium sulphate, combustion soot, and fluorescent polystyrene spheres were analysed by WIBS-4 in the laboratory. The results confirm the sensitivity of the Ultra Violet Light Induced Fluorescence (UV-LIF) method to biological fluorophores and show the good discrimination capabilities of the two wavelengths excitation/two wavebands detection method applied in WIBS-4. However, a weak cross-sensitivity to non-biological fluorescent interferers remains and is discussed in this paper. All the laboratory studies have been undertaken in order to prepare WIBS-4 for ambient aerosol measurements. According to the one year ambient aerosol study, number concentration of fluorescent biological aerosol particles (FBAP) show strong seasonal and diurnal variability. The highest number concentration of FBAP was measured during the summer term and it decreases towards the winter period when colder and drier conditions are prevailing. Diurnal FBAP concentrations start to increase after sunset and reach maximum values during the late night and early morning hours. On the other hand the total aerosol number concentration was always higher during day time than during night time and a sharp decrease after sunset was observed. There was no correlation observed between the FBAP concentration and the meteorological parameters temperature

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

NASA Astrophysics Data System (ADS)

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

2017-08-01

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

Chemical characterization of secondary organic aerosol constituents from isoprene ozonolysis in the presence of acidic aerosol

NASA Astrophysics Data System (ADS)

Riva, Matthieu; Budisulistiorini, Sri Hapsari; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.

2016-04-01

Isoprene is the most abundant non-methane hydrocarbon emitted into Earth's atmosphere and is predominantly derived from terrestrial vegetation. Prior studies have focused largely on the hydroxyl (OH) radical-initiated oxidation of isoprene and have demonstrated that highly oxidized compounds, such as isoprene-derived epoxides, enhance the formation of secondary organic aerosol (SOA) through heterogeneous (multiphase) reactions on acidified sulfate aerosol. However, studies on the impact of acidified sulfate aerosol on SOA formation from isoprene ozonolysis are lacking and the current work systematically examines this reaction. SOA was generated in an indoor smog chamber from isoprene ozonolysis under dark conditions in the presence of non-acidified or acidified sulfate seed aerosol. The effect of OH radicals on SOA chemical composition was investigated using diethyl ether as an OH radical scavenger. Aerosols were collected and chemically characterized by ultra performance liquid chromatography/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) and gas chromatography/electron impact ionization-mass spectrometry (GC/EI-MS). Analysis revealed the formation of highly oxidized compounds, including organosulfates (OSs) and 2-methylterols, which were significantly enhanced in the presence of acidified sulfate seed aerosol. OSs identified in the chamber experiments were also observed and quantified in summertime fine aerosol collected from two rural locations in the southeastern United States during the 2013 Southern Oxidant and Aerosol Study (SOAS).

An online monitor of the oxidative capacity of aerosols (o-MOCA)

NASA Astrophysics Data System (ADS)

Eiguren-Fernandez, Arantzazu; Kreisberg, Nathan; Hering, Susanne

2017-02-01

The capacity of airborne particulate matter to generate reactive oxygen species (ROS) has been correlated with the generation of oxidative stress both in vitro and in vivo. The cellular damage from oxidative stress, and by implication with ROS, is associated with several common diseases, such as asthma and chronic obstructive pulmonary disease (COPD), and some neurological diseases. Yet currently available chemical and in vitro assays to determine the oxidative capacity of ambient particles require large samples, analyses are typically done offline, and the results are not immediate.Here we report the development of an online monitor of the oxidative capacity of aerosols (o-MOCA) to provide online, time-resolved assessment of the capacity of airborne particles to generate ROS. Our approach combines the Liquid Spot Sampler (LSS), which collects particles directly into small volumes of liquid, and a chemical module optimized for online measurement of the oxidative capacity of aerosol using the dithiothreitol (DTT) assay. The LSS uses a three-stage, laminar-flow water condensation approach to enable the collection of particles as small as 5 nm into liquid. The DTT assay has been improved to allow the online, time-resolved analysis of samples collected with the LSS but could be adapted to other collection methods or offline analysis of liquid extracts.The o-MOCA was optimized and its performance evaluated using the 9,10-phenanthraquinone (PQ) as a standard redox-active compound. Laboratory testing shows minimum interferences or carryover between consecutive samples, low blanks, and a reproducible, linear response between the DTT consumption rate (nmol min-1) and PQ concentration (µM). The calculated limit of detection for o-MOCA was 0.15 nmol min-1. The system was validated with a diesel exhaust particle (DEP) extract, previously characterized and used for the development, improvement, and validation of the standard DTT analysis. The DTT consumption rates (nmol min-1

A new direct thermal desorption-GC/MS method: Organic speciation of ambient particulate matter collected in Golden, BC

NASA Astrophysics Data System (ADS)

Ding, Luyi C.; Ke, Fu; Wang, Daniel K. W.; Dann, Tom; Austin, Claire C.

Particulate matter having an aerodynamic diameter less than 2.5 μm (PM2.5) is thought to be implicated in a number of medical conditions, including cancer, rheumatoid arthritis, heart attack, and aging. However, very little chemical speciation data is available for the organic fraction of ambient aerosols. A new direct thermal desorption-gas chromatography/mass spectrometry (TD-GC/MS) method was developed for the analysis of the organic fraction of PM2.5. Samples were collected in Golden, British Columbia, over a 15-month period. n-Alkanes constituted 33-98% by mass of the organic compounds identified. PAHs accounted for 1-65% and biomarkers (hopanes and steranes) 1-8% of the organic mass. Annual mean concentrations were: n-alkanes (0.07-1.55 ng m -3), 16 PAHs (0.02-1.83 ng m -3), and biomarkers (0.02-0.18 ng m -3). Daily levels of these organics were 4.89-74.38 ng m -3, 0.27-100.24 ng m -3, 0.14-4.39 ng m -3, respectively. Ratios of organic carbon to elemental carbon (OC/EC) and trends over time were similar to those observed for PM2.5. There was no clear seasonal variation in the distribution of petroleum biomarkers, but elevated levels of other organic species were observed during the winter. Strong correlations between PAHs and EC, and between petroleum biomarkers and EC, suggest a common emission source - most likely motor vehicles and space heating.

The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Slowik, J. G.; Shantz, N. C.; Vlasenko, A.; Liggio, J.; Sjostedt, S. J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-06-01

Cloud condensation nuclei (CCN) concentrations were measured at Egbert, a rural site in Ontario, Canada during the spring of 2007. The CCN concentrations were compared to values predicted from the aerosol chemical composition and size distribution using κ-Köhler theory, with the specific goal of this work being to determine the hygroscopic parameter (κ) of the oxygenated organic component of the aerosol, assuming that oxygenation drives the hygroscopicity for the entire organic fraction of the aerosol. The hygroscopicity of the oxygenated fraction of the organic component, as determined by an Aerodyne aerosol mass spectrometer (AMS), was characterised by two methods. First, positive matrix factorization (PMF) was used to separate oxygenated and unoxygenated organic aerosol factors. By assuming that the unoxygenated factor is completely non-hygroscopic and by varying κ of the oxygenated factor so that the predicted and measured CCN concentrations are internally consistent and in good agreement, κ of the oxygenated organic factor was found to be 0.22±0.04 for the suite of measurements made during this five-week campaign. In a second, equivalent approach, we continue to assume that the unoxygenated component of the aerosol, with a mole ratio of atomic oxygen to atomic carbon (O/C) ≈ 0, is completely non-hygroscopic, and we postulate a simple linear relationship between κorg and O/C. Under these assumptions, the κ of the entire organic component for bulk aerosols measured by the AMS can be parameterised as κorg=(0.29±0.05)·(O/C), for the range of O/C observed in this study (0.3 to 0.6). These results are averaged over our five-week study at one location using only the AMS for composition analysis. Empirically, our measurements are consistent with κorg generally increasing with increasing particle oxygenation, but high uncertainties preclude us from testing this hypothesis. Lastly, we examine select periods of different aerosol composition, corresponding

Measurement of the temperature dependent partitioning of semi-volatile organics onto aerosol near roadways

NASA Astrophysics Data System (ADS)

Wentzell, J. J.; Liggio, J.; Li, S.; Brook, J.; Staebler, R. M.; Evans, G. J.; Jeong, C.; Sheppard, A.; Lu, G.; Gordon, M.; Mihele, C.

2010-12-01

The volatility of the organic aerosol fraction has received a great deal of attention recently in light of new volatility-based modelling approaches and due to the inability of current models to fully account for secondary organic aerosol (SOA). In this regard, evaporation of primary organic aerosol species and their subsequent oxidation may contribute significantly to SOA downwind of sources. This implies that moderate ambient temperature fluctuations can significantly increase or decrease the aerosol bound fraction of semi-volatile and intermediate volatility (SVOC + IVOC) compounds. In order to examine the importance of these more volatile organic components, a temperature controlled inlet was developed with the ability to heat and cool the aerosol in 2 C increments to 15 C above or below ambient temperature. The inlet was coupled to an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and deployed on a mobile platform upwind and downwind of a major Southern Ontario highway as part of the Fast Evolution of Vehicle Emissions near Roadways (FEVER 2010) campaign. Preliminary results suggest that changes in temperature of 5-10 C can alter the partitioning of volatile organic aerosol components by up to 30%. Although the largest affect was observed 10-13 meters downwind of the vehicle emissions, a measurable affect was observed beyond 500 m and in aerosol upwind of the highway. These results suggest that a significant pool of semi-volatile organics exist, which can condense onto particles at slightly lower temperatures or evaporate to the gas phase and be further oxidized. The nature of these organic species at locations upwind and downwind of vehicle emissions will be discussed.

During air cool process aerosol absorption detection with photothermal interferometry

NASA Astrophysics Data System (ADS)

Li, Baosheng; Xu, Limei; Huang, Junling; Ma, Fei; Wang, Yicheng; Li, Zhengqiang

2014-11-01

This paper studies the basic principle of laser photothermal interferometry method of aerosol particles absorption coefficient. The photothermal interferometry method with higher accuracy and lower uncertainty can directly measure the absorption coefficient of atmospheric aerosols and not be affected by scattered light. With Jones matrix expression, the math expression of a special polarization interferometer is described. This paper using folded Jamin interferometer, which overcomes the influence of vibration on measuring system. Interference come from light polarization beam with two orthogonal and then combine to one beam, finally aerosol absorption induced refractive index changes can be gotten with four beam of phase orthogonal light. These kinds of styles really improve the stability of system and resolution of the system. Four-channel detections interact with interference fringes, to reduce the light intensity `zero drift' effect on the system. In the laboratory, this device typical aerosol absorption index, it shows that the result completely agrees with actual value. After heated by laser, cool process of air also show the process of aerosol absorption. This kind of instrument will be used to monitor ambient aerosol absorption and suspended particulate matter chemical component. Keywords: Aerosol absorption coefficient; Photothermal interferometry; Suspended particulate matter.

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.

PASSIVE AEROSOL SAMPLER FOR CHARACTERIZATION, AMBIENT CONCENTRATION, AND PARTICLE SIZE MEASUREMENT

EPA Science Inventory

This is an extended abstract of a presentation made at the Air and Waste Management Association's Symposium on Air Quality Measurement Methods and Technology, Durham, NC, May 9-11, 2006. The abstract describes the theory, design, and initial testing of a passive aerosol sampler f...

Intercontinental Transport of Aerosols: Implication for Regional Air Quality

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Ginoux, Paul

2006-01-01

Aerosol particles, also known as PM2.5 (particle diameter less than 2.5 microns) and PM10 (particle diameter less than 10 microns), is one of the key atmospheric components that determine ambient air quality. Current US air quality standards for PM10 (particles with diameter < 10 microns) and PM2.5 (particles with diameter 2.5 microns) are 50 pg/cu m and 15 pg/cu m, respectively. While local and regional emission sources are the main cause of air pollution problems, aerosols can be transported on a hemispheric or global scale. In this study, we use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to quantify contributions of long-range transport vs. local/regional pollution sources and from natural vs. anthropogenic sources to PM concentrations different regions. In particular, we estimate the hemispheric impact of anthropogenic sulfate aerosols and dust from major source areas on other regions in the world. The GOCART model results are compared with satellite remote sensing and ground-based network measurements of aerosol optical depth and concentrations.

Radiative transfer model for aerosols in infrared wavelengths for passive remote sensing applications.

PubMed

Ben-David, Avishai; Embury, Janon F; Davidson, Charles E

2006-09-10

A comprehensive analytical radiative transfer model for isothermal aerosols and vapors for passive infrared remote sensing applications (ground-based and airborne sensors) has been developed. The theoretical model illustrates the qualitative difference between an aerosol cloud and a chemical vapor cloud. The model is based on two and two/four stream approximations and includes thermal emission-absorption by the aerosols; scattering of diffused sky radiances incident from all sides on the aerosols (downwelling, upwelling, left, and right); and scattering of aerosol thermal emission. The model uses moderate resolution transmittance ambient atmospheric radiances as boundary conditions and provides analytical expressions for the information on the aerosol cloud that is contained in remote sensing measurements by using thermal contrasts between the aerosols and diffused sky radiances. Simulated measurements of a ground-based sensor viewing Bacillus subtilis var. niger bioaerosols and kaolin aerosols are given and discussed to illustrate the differences between a vapor-only model (i.e., only emission-absorption effects) and a complete model that adds aerosol scattering effects.

Chemical Characterization and Source Apportionment of Size Fractionated Atmospheric Aerosols, and, Evaluating Student Attitudes and Learning in Large Lecture General Chemistry Classes

NASA Astrophysics Data System (ADS)

Allen, Gregory Harold

Chemical speciation and source apportionment of size fractionated atmospheric aerosols were investigated using laser desorption time-of-flight mass spectrometry (LD TOF-MS) and source apportionment was carried out using carbon-14 accelerator mass spectrometry (14C AMS). Sample collection was carried out using the Davis Rotating-drum Unit for Monitoring impact analyzer in Davis, Colfax, and Yosemite, CA. Ambient atmospheric aerosols collected during the winter of 2010/11 and 2011/12 showed a significant difference in the types of compounds found in the small and large sized particles. The difference was due to the increase number of oxidized carbon species that were found in the small particles size ranges, but not in the large particles size ranges. Overall, the ambient atmospheric aerosols collected during the winter in Davis, CA had and average fraction modern of F14C = 0.753 +/- 0.006, indicating that the majority of the size fractionated particles originated from biogenic sources. Samples collected during the King Fire in Colfax, CA were used to determine the contribution of biomass burning (wildfire) aerosols. Factor analysis was used to reduce the ions found in the LD TOF-MS analysis of the King Fire samples. The final factor analysis generated a total of four factors that explained an overall 83% of the variance in the data set. Two of the factors correlated heavily with increased smoke events during the sample period. The increased smoke events produced a large number of highly oxidized organic aerosols (OOA2) and aromatic compounds that are indicative of biomass burning organic aerosols (WBOA). The signal intensities of the factors generated in the King Fire data were investigated in samples collected in Yosemite and Davis, CA to look at the impact of biomass burning on ambient atmospheric aerosols. In both comparison sample collections the OOA2 and WBOA factors both increased during biomass burning events located near the sampling sites. The correlation

Influence of metal-mediated aerosol-phase oxidation on secondary organic aerosol formation from the ozonolysis and OH-oxidation of α-pinene

PubMed Central

Chu, Biwu; Liggio, John; Liu, Yongchun; He, Hong; Takekawa, Hideto; Li, Shao-Meng; Hao, Jiming

2017-01-01

The organic component is the most abundant fraction of atmospheric submicron particles, while the formation mechanisms of secondary organic aerosol (SOA) are not fully understood. The effects of sulfate seed aerosols on SOA formation were investigated with a series of experiments carried out using a 9 m3 smog chamber. The presence of FeSO4 or Fe2(SO4)3 seed aerosols decreased SOA yields and increased oxidation levels in both ozonolysis and OH-oxidation of α-pinene compared to that in the presence of ZnSO4 or (NH4)2SO4. These findings were explained by metal-mediated aerosol-phase oxidation of organics: reactive radicals were generated on FeSO4 or Fe2(SO4)3 seed aerosols and reacted further with the organic mass. This effect would help to explain the high O/C ratios of organics in ambient particles that thus far cannot be reproduced in laboratory and model studies. In addition, the gap in the SOA yields between experiments with different seed aerosols was more significant in OH-oxidation experiments compared to ozonolysis experiments, while the gap in estimated O/C ratios was less obvious. This may have resulted from the different chemical compositions and oxidation levels of the SOA generated in the two systems, which affect the branching ratio of functionalization and fragmentation during aerosol oxidation. PMID:28059151

Influence of metal-mediated aerosol-phase oxidation on secondary organic aerosol formation from the ozonolysis and OH-oxidation of α-pinene.

PubMed

Chu, Biwu; Liggio, John; Liu, Yongchun; He, Hong; Takekawa, Hideto; Li, Shao-Meng; Hao, Jiming

2017-01-06

The organic component is the most abundant fraction of atmospheric submicron particles, while the formation mechanisms of secondary organic aerosol (SOA) are not fully understood. The effects of sulfate seed aerosols on SOA formation were investigated with a series of experiments carried out using a 9 m 3 smog chamber. The presence of FeSO 4 or Fe 2 (SO 4 ) 3 seed aerosols decreased SOA yields and increased oxidation levels in both ozonolysis and OH-oxidation of α-pinene compared to that in the presence of ZnSO 4 or (NH 4 ) 2 SO 4 . These findings were explained by metal-mediated aerosol-phase oxidation of organics: reactive radicals were generated on FeSO 4 or Fe 2 (SO 4 ) 3 seed aerosols and reacted further with the organic mass. This effect would help to explain the high O/C ratios of organics in ambient particles that thus far cannot be reproduced in laboratory and model studies. In addition, the gap in the SOA yields between experiments with different seed aerosols was more significant in OH-oxidation experiments compared to ozonolysis experiments, while the gap in estimated O/C ratios was less obvious. This may have resulted from the different chemical compositions and oxidation levels of the SOA generated in the two systems, which affect the branching ratio of functionalization and fragmentation during aerosol oxidation.

Impacts of Long-Range Transport of Metals from East Asia in Bulk Aerosols Collected at the Okinawa Archipelago, Japan

NASA Astrophysics Data System (ADS)

A, Sotaro; S, Yuka; I, Moriaki; N, Fumiya; H, Daishi; A, Takemitsu; T, Akira

2010-05-01

Economy of East Asia has been growing rapidly, and atmospheric aerosols discharged from this region have been transported to Japan. Okinawa island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km of south Korea. Its location in Asian is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air mass which has been affected by anthropogenic activities. Therefore, Okinawa region is suitable area for studying impacts of air pollutants from East Asia. We simultaneously collected bulk aerosol samples by using the same type of high volume air samplers at Cape Hedo Atmospheric Aerosol Monitoring Station (CHAAMS, Okinawa island), Kume island (ca. 160 km south-west of CHAAMS), and Minami-Daitou island (ca. 320 km south-east of CHAAMS). We determined the concentrations of acid-digested metals using atomic absorption spectrometer and inductively-coupled plasma mass spectrometry (ICP-MS). We report and discuss spatial and temporal distribution of metals in the bulk atmospheric aerosols collected at CHAAMS, Kume island and Minami-Daitou island during June, 2008 to June 2009. We also determined 'background' concentration of metals in Okinawa archipelago. We then compare each chemical component among CHAAMS, Kume island and Minami-Daitou island to elucidate the influence of the transport processes and distances from Asian continent on metal concentrations.

On the implications of aerosol liquid water and phase ...

EPA Pesticide Factsheets

Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were hig

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

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

2013-11-01

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

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

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

2013-07-01

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

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

PubMed

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

2014-09-15

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

Aerosol carbon isotope composition over Baltic Sea

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

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

NASA Technical Reports Server (NTRS)

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

1994-01-01

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

Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

NASA Astrophysics Data System (ADS)

Liu, Tengyu; Li, Zijun; Chan, ManNin; Chan, Chak K.

2017-06-01

Cooking emissions can potentially contribute to secondary organic aerosol (SOA) but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils) was investigated in a potential aerosol mass (PAM) chamber. Experiments were conducted at 19-20 °C and 65-70 % relative humidity (RH). The characterization instruments included a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS). The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm-3 s, was 1. 35 ± 0. 30 µg min-1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5) from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol) in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc) of SOA was -1.51 to -0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA) and semi-volatile oxygenated organic aerosol (SV-OOA), indicating that SOA in these experiments was lightly oxidized.

Indirect and Semi-Direct Aerosol Campaign: The Impact of Arctic Aerosols on Clouds

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

McFarquhar, Greg; Ghan, Steven J.; Verlinde, J.

2011-02-01

A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the arctic boundary layer in the vicinity of Barrow, Alaska was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) sponsored by the Department of Energy Atmospheric Radiation Measurement (ARM) and Atmospheric Science Programs. The primary aim of ISDAC was to examine indirect effects of aerosols on clouds that contain both liquid and ice water. The experiment utilized the ARM permanent observational facilities at the North Slope of Alaska (NSA) in Barrow. These include a cloud radar, a polarized micropulse lidar, and an atmosphericmore » emitted radiance interferometer as well as instruments specially deployed for ISDAC measuring aerosol, ice fog, precipitation and spectral shortwave radiation. The National Research Council of Canada Convair-580 flew 27 sorties during ISDAC, collecting data using an unprecedented 42 cloud and aerosol instruments for more than 100 hours on 12 different days. Data were obtained above, below and within single-layer stratus on 8 April and 26 April 2008. These data enable a process-oriented understanding of how aerosols affect the microphysical and radiative properties of arctic clouds influenced by different surface conditions. Observations acquired on a heavily polluted day, 19 April 2008, are enhancing this understanding. Data acquired in cirrus on transit flights between Fairbanks and Barrow are improving our understanding of the performance of cloud probes in ice. Ultimately the ISDAC data will be used to improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and to determine the extent to which long-term surface-based measurements can provide retrievals of aerosols, clouds, precipitation and radiative heating in the Arctic.« less

Comparative In Vitro Toxicity Profile of Electronic and Tobacco Cigarettes, Smokeless Tobacco and Nicotine Replacement Therapy Products: E-Liquids, Extracts and Collected Aerosols

PubMed Central

Misra, Manoj; Leverette, Robert D.; Cooper, Bethany T.; Bennett, Melanee B.; Brown, Steven E.

2014-01-01

The use of electronic cigarettes (e-cigs) continues to increase worldwide in parallel with accumulating information on their potential toxicity and safety. In this study, an in vitro battery of established assays was used to examine the cytotoxicity, mutagenicity, genotoxicity and inflammatory responses of certain commercial e-cigs and compared to tobacco burning cigarettes, smokeless tobacco (SLT) products and a nicotine replacement therapy (NRT) product. The toxicity evaluation was performed on e-liquids and pad-collected aerosols of e-cigs, pad-collected smoke condensates of tobacco cigarettes and extracts of SLT and NRT products. In all assays, exposures with e-cig liquids and collected aerosols, at the doses tested, showed no significant activity when compared to tobacco burning cigarettes. Results for the e-cigs, with and without nicotine in two evaluated flavor variants, were very similar in all assays, indicating that the presence of nicotine and flavors, at the levels tested, did not induce any cytotoxic, genotoxic or inflammatory effects. The present findings indicate that neither the e-cig liquids and collected aerosols, nor the extracts of the SLT and NRT products produce any meaningful toxic effects in four widely-applied in vitro test systems, in which the conventional cigarette smoke preparations, at comparable exposures, are markedly cytotoxic and genotoxic. PMID:25361047

Aerosol composition and variability in the Baltimore-Washington, DC region

NASA Astrophysics Data System (ADS)

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

2015-08-01

in the free troposphere (above 3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed layer aerosol. Aerosol loading was found to be the predominant source accounting for 88 % on average of the measured spatial variability in extinction with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first-order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite/modelling assimilation products that are able to capture these components of the AOD-PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day-to-day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015) that determined the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.

Mount Saint Helens aerosol evolution

NASA Technical Reports Server (NTRS)

Oberbeck, V. R.; Farlow, N. H.; Snetsinger, K. G.; Ferry, G. V.; Fong, W.; Hayes, D. M.

1982-01-01

Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mt. St. Helens. Analysis of samples shows that aerosol volume increased for 6 months due to gas-to-particle conversion and then decreased to background levels in the following 6 months.

Direct impact aerosol sampling by electrostatic precipitation

DOEpatents

Braden, Jason D.; Harter, Andrew G.; Stinson, Brad J.; Sullivan, Nicholas M.

2016-02-02

The present disclosure provides apparatuses for collecting aerosol samples by ionizing an air sample at different degrees. An air flow is generated through a cavity in which at least one corona wire is disposed and electrically charged to form a corona therearound. At least one grounded sample collection plate is provided downstream of the at least one corona wire so that aerosol ions generated within the corona are deposited on the at least one grounded sample collection plate. A plurality of aerosol samples ionized to different degrees can be generated. The at least one corona wire may be perpendicular to the direction of the flow, or may be parallel to the direction of the flow. The apparatus can include a serial connection of a plurality of stages such that each stage is capable of generating at least one aerosol sample, and the air flow passes through the plurality of stages serially.

Preliminary observations of organic gas-particle partitioning from biomass combustion smoke using an aerosol mass spectrometer

Treesearch

T. Lee; S. M. Kreidenweis; J. L. Collett; A. P. Sullivan; C. M. Carrico; J. L. Jimenez; M. Cubison; S. Saarikoski; D. R. Worsnop; T. B. Onasch; E. Fortner; W. C. Malm; E. Lincoln; Cyle Wold; WeiMin Hao

2010-01-01

Aerosols play important roles in adverse health effects, indirect and direct forcing of Earth’s climate, and visibility degradation. Biomass burning emissions from wild and prescribed fires can make a significant contribution to ambient aerosol mass in many locations and seasons. In order to better understand the chemical properties of particles produced by combustion...

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

NASA Astrophysics Data System (ADS)

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

2008-12-01

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

Inflammatory responses to secondary organic aerosols (SOA) generated from biogenic and anthropogenic precursors

NASA Astrophysics Data System (ADS)

Tuet, Wing Y.; Chen, Yunle; Fok, Shierly; Champion, Julie A.; Ng, Nga L.

2017-09-01

Cardiopulmonary health implications resulting from exposure to secondary organic aerosols (SOA), which comprise a significant fraction of ambient particulate matter (PM), have received increasing interest in recent years. In this study, alveolar macrophages were exposed to SOA generated from the photooxidation of biogenic and anthropogenic precursors (isoprene, α-pinene, β-caryophyllene, pentadecane, m-xylene, and naphthalene) under different formation conditions (RO2 + HO2 vs. RO2 + NO dominant, dry vs. humid). Various cellular responses were measured, including reactive oxygen and nitrogen species (ROS/RNS) production and secreted levels of cytokines, tumor necrosis factor-α (TNF-α) and interleukin-6 (IL-6). SOA precursor identity and formation condition affected all measured responses in a hydrocarbon-specific manner. With the exception of naphthalene SOA, cellular responses followed a trend where TNF-α levels reached a plateau with increasing IL-6 levels. ROS/RNS levels were consistent with relative levels of TNF-α and IL-6, due to their respective inflammatory and anti-inflammatory effects. Exposure to naphthalene SOA, whose aromatic-ring-containing products may trigger different cellular pathways, induced higher levels of TNF-α and ROS/RNS than suggested by the trend. Distinct cellular response patterns were identified for hydrocarbons whose photooxidation products shared similar chemical functionalities and structures, which suggests that the chemical structure (carbon chain length and functionalities) of photooxidation products may be important for determining cellular effects. A positive nonlinear correlation was also detected between ROS/RNS levels and previously measured DTT (dithiothreitol) activities for SOA samples. In the context of ambient samples collected during summer and winter in the greater Atlanta area, all laboratory-generated SOA produced similar or higher levels of ROS/RNS and DTT activities. These results suggest that the health

Design and testing of a shrouded probe for airborne aerosol sampling in a high velocity airstream

NASA Astrophysics Data System (ADS)

Cain, Stuart Arthur

1997-07-01

Tropospheric aerosols play an important role in many phenomena related to global climate and climate change and two important parameters, aerosol size distribution and concentration, have been the focus of a great deal of attention. To study these parameters it is necessary to obtain a representative sample of the ambient aerosol using an airborne aerosol sampling probe mounted on a suitably equipped aircraft. Recently, however, serious questions have been raised (Huebert et al., 1990; Baumgardner et al., 1991) concerning the current procedures and techniques used in airborne aerosol sampling. We believe that these questions can be answered by: (1) use of a shrouded aerosol sampling probe, (2) proper aerodynamic sampler design using numerical simulation techniques, (3) calculation of the sampler calibration curve to be used in determining free-stream aerosol properties from measurements made with the sampler and (4) wind tunnel tests to verify the design and investigate the performance of the sampler at small angles of attack (typical in airborne sampling applications due to wind gusts and aircraft fuel consumption). Our analysis is limited to the collection of insoluble particles representative of the global tropospheric 'background aerosol' (0.1-2.6 μm diameter) whose characteristics are least likely to be affected by the collection process. We begin with a survey of the most relevant problems associated with current airborne aerosol samplers and define the physical quantity that we wish to measure. This includes the derivation of a unique mathematical expression relating the free-stream aerosol size distribution to aerosol data obtained from the airborne measurements with the sampler. We follow with the presentation of the results of our application of Computational Fluid Dynamics (CFD) and Computational Particle Dynamics (CPD) to the design of a shrouded probe for airborne aerosol sampling of insoluble tropospheric particles in the size range 0.1 to 15 �

Experimental Characterization and Hygroscopicity Determination of Secondary Aerosol from D5 Cyclic Siloxane Oxidation

NASA Astrophysics Data System (ADS)

Stanier, C. O.; Janechek, N. J.; Bryngelson, N.; Marek, R. F.; Lersch, T.; Bunker, K.; Casuccio, G.; Brune, W. H.; Hornbuckle, K. C.

2017-12-01

Cyclic volatile methyl siloxanes are anthropogenic chemicals present in personal care products such as antiperspirants and lotions. These are volatile chemicals that are readily released into the atmosphere by product use. Due to their emission and relatively slow kinetics of their major transformation pathway, reaction with hydroxyl radicals (OH), these compounds are present in high concentrations in indoor environments and widespread in outdoor environments. Cyclic siloxane reaction with OH can lead to secondary organic aerosols, and due to the widespread prevalence of the parent compounds, may be an important source of ambient aerosols. Atmospheric aerosols have important influences to the climate by affecting the radiative balance and by serving as cloud condensation nuclei (CCN) which influence clouds. While the parent compounds have been well-studied, the oxidation products have received much less attention, with almost no ambient measurements or experimental physical property data. We report physical properties of aerosols generated by reacting the cyclic siloxane D5 with OH using a Potential Aerosol Mass (PAM) photochemical chamber. The particles were characterized by SMPS, imaging and elemental analysis using both Transmission Electron Microscopy and Scanning Transmission Electron Microscopy equipped with Energy Dispersive X-ray Spectroscopy systems (TEM-EDS and STEM-EDS), volatility measurements using Volatility Tandem Differential Mobility Analyzer (V-TDMA), and hygroscopicity measurements to determine CCN potential using a Droplet Measurement Technologies Cloud Condensation Nuclei Counter (DMT-CCN). Aerosol yield sensitivity to D5 and OH concentrations, residence time, and seed aerosols were analyzed. TEM-EDS and STEM-EDS analysis show spherical particle morphology with elemental composition consistent with aerosols derived from cyclic siloxane sources. Measured aerosol yields were 20-50% with typical aerosol concentrations 300,000 particles cm-3, up to

A Computational Study of Acid Catalyzed Aerosol Reactions of Atmospherically Relevant Epoxides

EPA Science Inventory

Epoxides are important intermediates of atmospheric isoprene oxidation. Their subsequent reactions in the particle phase lead to the production of organic compounds detected in ambient aerosols. We apply density functional theory to determine the important kinetic factors that ...

Spatial distribution and temporal variation of chemical species in the bulk atmospheric aerosols collected at the Okinawa archipelago, Japan

NASA Astrophysics Data System (ADS)

Handa, D.; Somada, Y.; Ijyu, M.; Azechi, S.; Nakaema, F.; Arakaki, T.; Tanahara, A.

2009-12-01

The economic development and population growth in recent Asia have been increasing air pollution. A computer simulation study showed that air pollutants emitted from Asian continent could spread quickly within northern hemisphere. We initiated a study to elucidate the special distribution and chemical characterization of atmospheric aerosols around Okinawa archipelago, Japan. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location in Asia is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. We simultaneously collected bulk aerosol samples by using the same types of high volume air samplers at Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS, Okinawa Island), Kume Island (ca. 160 km south-west of CHAAMS) and Minami-daitou Island (ca. 320 km south-east of CHAAMS). We determined the concentrations of water-soluble anions, cations and dissolved organic carbon (DOC) using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. We report and discuss spatial distribution and temporal variation of chemical species concentrations in bulk atmospheric aerosols collected during July, 2008 to July, 2009. We determine “background” concentration of chemical components in Okinawa archipelago. We then compare each chemical component among CHAAMS, Kume Island and Minami-daito Island to elucidate the influence of the long-range transport of chemical species from Asian continent.

Nanotechnology and pharmaceutical inhalation aerosols.

PubMed

Patel, A R; Vavia, P R

2007-02-01

Pharmaceutical inhalation aerosols have been playing a crucial role in the health and well being of millions of people throughout the world for many years. The technology's continual advancement, the ease of use and the more desirable pulmonary-rather-than-needle delivery for systemic drugs has increased the attraction for the pharmaceutical aerosol in recent years. But administration of drugs by the pulmonary route is technically challenging because oral deposition can be high, and variations in inhalation technique can affect the quantity of drug delivered to the lungs. Recent advances in nanotechnology, particularly drug delivery field have encouraged formulation scientists to expand their reach in solving tricky problems related to drug delivery. Moreover, application of nanotechnology to aerosol science has opened up a new category of pharmaceutical aerosols (collectively known as nanoenabled-aerosols) with added advantages and effectiveness. In this review, some of the latest approaches of nano-enabled aerosol drug delivery system (including nano-suspension, trojan particles, bioadhesive nanoparticles and smart particle aerosols) that can be employed successfully to overcome problems of conventional aerosol systems have been introduced.

Black and Brown Carbon in Biogenic Settings with Different Levels of Anthropogenic Influence, and The Effect of Semivolatile Compounds on Aerosol Optical Properties

NASA Astrophysics Data System (ADS)

Tasoglou, A.; Ramachandran, S.; Khlystov, A.; Saha, P.; Grieshop, A. P.; Pandis, S. N.

2015-12-01

Secondary organic aerosol (SOA) is a major contributor to the global aerosol burden. Black carbon (BC) is a significant climate warming agent, while light-absorbing organic carbon (brown carbon, BrC), also impacts the atmospheric radiative balance. The optical properties of ambient aerosols can be affected by biogenic SOA through the lensing effect (coating of BC cores by semivolatile SOA), and by the potential formation of BrC from biogenic sources influenced by anthropogenic sources. To evaluate these effects, measurements of ambient aerosol optical properties and BC concentrations were made in rural Centreville, AL (a remote site with little anthropogenic influence) in summer 2013 and at Duke Forest in Chapel Hill, NC (a site close to high density vehicular traffic and industrial sources), during summer 2015. Photoacoustic extinctiometers (PAX, 405 nm and 532 nm) measured particulate light absorption and a single particle soot photometer (SP2) measured BC mass at both locations. A seven-wavelength Aethalometer and a three-wavelength nephelometer were also deployed at Duke Forest. A third PAX (870 nm) was deployed at Centreville. For absorption and BC measurements, the sample was cycled between a dry line and a dry/thermally-denuded line. Hourly samples were collected with a steam jet aerosol collector (SJAC) for online (2013) and offline (2015) chemical composition analysis. BC concentrations were generally higher at Duke Forest compared to the rural Centreville site. The Aethalometer readings at Duke Forest show greater absorption at the shorter wavelengths (370 nm and 470 nm) than expected from the absorption at 880 nm coupled with an inverse wavelength dependence, suggesting the presence of brown carbon. This presentation will examine the evidence for brown carbon at the two sites, as well as the effect of non-BC coatings on BC light absorption (the lensing effect.)

Derivation of Aerosol Columnar Mass from MODIS Optical Depth

NASA Technical Reports Server (NTRS)

Gasso, Santiago; Hegg, Dean A.

2003-01-01

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

Long term atmospheric aerosol characterization in the Amazon Basin

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Gerab, Fábio; Yamasoe, Marcia A.

This chapter presents a characterization of atmospheric aerosols collected in different places in the Amazon Basin. Both the biogenic aerosol emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burns during the dry season were studied. The samples were collected during a three year period at three different locations in the Amazon (Cuiabá, Alta Floresta and Serra do Navio), using stacked filter units. Aerosol samples were also collected directly over fires of cerrado vegetation and tropical primary forest burns The samples were analyzed using several techniques for a number of elements. Gravimetric analyses were used to determine the total atmospheric aerosol concentration. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. Cerrado burning emissions were enriched compared to forest ones, specially for Cl, K and Zn. High atmospheric aerosol concentrations were observed in large amazonian areas due to emissions from man-made burns in the period from June to September. The emissions from burns dominate the fine fraction of the atmospheric aerosol with characteristic high contents of black carbon, S and K. Aerosols emitted in biomass burning process are correlated to the increase in the aerosol optical thickness of the atmosphere during the Amazonian dry season. The Serra do Navio aerosol is characterized by biogenic emissions with strong marine influence. The presence of trace elements characteristic of soil particulate associated with this marine contribution indicates the existence of aerosol transport from Africa to South America. Similar composition characteristics were observed in the biogenic emission aerosols from Serra do Navio and Alta Floresta.

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

PubMed

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

2001-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

PIXE investigation of aerosol composition over the Zambian Copperbelt

NASA Astrophysics Data System (ADS)

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

1999-04-01

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

Aerosol composition and sources in the central Arctic Ocean during ASCOS

NASA Astrophysics Data System (ADS)

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

2011-10-01

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

Observational Study and Parameterization of Aerosol-fog Interactions

NASA Astrophysics Data System (ADS)

Duan, J.; Guo, X.; Liu, Y.; Fang, C.; Su, Z.; Chen, Y.

2014-12-01

Studies have shown that human activities such as increased aerosols affect fog occurrence and properties significantly, and accurate numerical fog forecasting depends on, to a large extent, parameterization of fog microphysics and aerosol-fog interactions. Furthermore, fogs can be considered as clouds near the ground, and enjoy an advantage of permitting comprehensive long-term in-situ measurements that clouds do not. Knowledge learned from studying aerosol-fog interactions will provide useful insights into aerosol-cloud interactions. To serve the twofold objectives of understanding and improving parameterizations of aerosol-fog interactions and aerosol-cloud interactions, this study examines the data collected from fogs, with a focus but not limited to the data collected in Beijing, China. Data examined include aerosol particle size distributions measured by a Passive Cavity Aerosol Spectrometer Probe (PCASP-100X), fog droplet size distributions measured by a Fog Monitor (FM-120), Cloud Condensation Nuclei (CCN), liquid water path measured by radiometers and visibility sensors, along with meteorological variables measured by a Tethered Balloon Sounding System (XLS-Ⅱ) and Automatic Weather Station (AWS). The results will be compared with low-level clouds for similarities and differences between fogs and clouds.

CHARACTERIZATION OF INCIDENTAL CARBONACEOUS NANOPARTICLES IN AMBIENT AIR AND COMBUSTION EXHAUST

EPA Science Inventory

The most important result of this research is one of the most complete datasets to date on the presence of C60 in the aerosol phase in the natural environment. This study expects that C60 fullerenes will not be found at detectable levels in combustion exhaust, ambient carbo...

Capstone Depleted Uranium Aerosols: Generation and Characterization

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

Parkhurst, MaryAnn; Szrom, Fran; Guilmette, Ray

2004-10-19

In a study designed to provide an improved scientific basis for assessing possible health effects from inhaling depleted uranium (DU) aerosols, a series of DU penetrators was fired at an Abrams tank and a Bradley fighting vehicle. A robust sampling system was designed to collect aerosols in this difficult environment and continuously monitor the sampler flow rates. Aerosols collected were analyzed for uranium concentration and particle size distribution as a function of time. They were also analyzed for uranium oxide phases, particle morphology, and dissolution in vitro. The resulting data provide input useful in human health risk assessments.

The Influence of Aerosol Hygroscopicity on Retrieving the Aerosol Extincting Coefficient from MPL Data

NASA Astrophysics Data System (ADS)

Zhao, G.; Zhao, C.

2016-12-01

Micro-pulse Lidar (MPL) measurements have been widely used to profile the ambient aerosol extincting coefficient(). Lidar Ratio (LR) ,which highly depends on the particle number size distribution (PNSD) and aerosol hygroscopicity, is the most important factor to retrieve the profile. A constant AOD constrained LR is usually used in current algorithms, which would lead to large bias when the relative humidity (RH) in the mixed layer is high. In this research, the influences of PNSD, aerosol hygroscopicity and RH profiles on the vertical variation of LR were investigated based on the datasets from field measurements in the North China Plain (NCP). Results show that LR can have an enhancement factor of more than 120% when the RH reaches to 92%. A new algorithm of retrieving the profile is proposed based on the variation of LR due to aerosol hygroscopicity. The magnitude and vertical structures of retrieved using this method can be significantly different to that of the fiexed LR method. The relative difference can reach up to 40% when the RH in the mixed layer is higher than 90% . Sensitivity studies show that RH profile and PNSD affect most on the retrieved by fiexed LR method. In view of this, a scheme of LR enhancement factor by RH is proposed in the NCP. The relative differnce of the calculated between using this scheme and the new algorithm with the variable LR can be less than 10%.

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.

Characterization of an Aerosol Microconcentrator for Analysis Using Microscale Optical Spectroscopies

PubMed Central

Zheng, Lina; Kulkarni, Pramod; Zavvos, Konstantinos; Liang, Huayan; Birch, M. Eileen; Dionysiou, Dionysios D.

2017-01-01

Efficient microconcentration of aerosols to a substrate is essential for effectively coupling the collected particles to microscale optical spectroscopies such as laser-induced or spark microplasma, or micro-Raman or infrared spectroscopies. In this study, we present detailed characterization of a corona-based aerosol microconcentration technique developed previously (Diwakar and Kulkarni, 2012). The method involves two coaxial electrodes separated by a few millimeters, one held at a high electrical potential and the other grounded. The particles are collected on the collection (i.e., ground) electrode from a coaxial aerosol flow in a one-step charge-and-collect scheme using corona discharge and electrical precipitation between the two electrodes. Performance of the corona microconcentration method was determined experimentally by measuring collection efficiency, wall losses, and particle deposition density. An intrinsic spectroscopic sensitivity was experimentally determined for the aerosol microconcentrator. Using this sensitivity, we show that corona-based microconcentration is much superior to alternative methods, including filtration, focused impaction using aerodynamic lens, and spot collection using condensational growth. The method offers unique advantages for compact, hand-held aerosol analytical instrumentation. PMID:28626243

Sampling stratospheric aerosols with impactors

NASA Technical Reports Server (NTRS)

Oberbeck, Verne R.

1989-01-01

Derivation of statistically significant size distributions from impactor samples of rarefield stratospheric aerosols imposes difficult sampling constraints on collector design. It is shown that it is necessary to design impactors of different size for each range of aerosol size collected so as to obtain acceptable levels of uncertainty with a reasonable amount of data reduction.

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

High Volume Air Sampling for Viral Aerosols: A Comparative Approach

DTIC Science & Technology

2010-03-01

Solid Impaction Aerosol Collection (Verreault, 2008. Reproduced with Permission from American Society of Microbiology ) Liquid collection...Reproduced with Permission from American Society of Microbiology ) Filter aerosol collection is often more efficient than other sampling...collected using a crude filter consisting of a glass tube packed with dry cotton. Sample analysis was conducted by inoculating chicken embryos with

Influence of Jet Fuel Composition on Aircraft Engine Emissions: A Synthesis of Aerosol Emissions Data from the NASA APEX, AAFEX, and ACCESS Missions

NASA Astrophysics Data System (ADS)

Moore, R.; Shook, M.; Beyersdorf, A. J.; Corr, C.; Herndon, S. C.; Knighton, W. B.; Miake-Lye, R. C.; Thornhill, K. L., II; Winstead, E.; Yu, Z.; Ziemba, L. D.; Anderson, B. E.

2015-12-01

We statistically analyze the impact of jet fuel properties on aerosols emitted by the NASA McDonnell Douglas DC-8 CFM56-2-C1 engines burning fifteen different aviation fuels. Data were collected for this single engine type during four different, comprehensive ground tests conducted over the past decade, which allow us to clearly link changes in aerosol emissions to fuel compositional changes. It is found that the volatile aerosol fraction dominates the number and volume emissions indices (EIs) over all engine powers, which are driven by changes in fuel aromatic and sulfur content. Meanwhile, the naphthalenic content of the fuel determines the magnitude of the non-volatile number and volume EI as well as the black carbon mass EI. Linear regression coefficients are reported for each aerosol EI in terms of these properties, engine fuel flow rate, and ambient temperature, and show that reducing both fuel sulfur content and napththalenes to near-zero levels would result in roughly a ten-fold decrease in aerosol number emitted per kg of fuel burn. This work informs future efforts to model aircraft emissions changes as the aviation fleet gradually begins to transition toward low-aromatic, low-sulfur alternative jet fuels from bio-based or Fischer-Tropsch production pathways.

INTEGRATION OF SATELLITE-DERIVED AEROSOL DATA INTO THE AIR QUALITY APPLICATIONS

EPA Science Inventory

Historically, the only source of aerosol air quality data available on an ongoing and systematic basis at national levels was generated by ambient air monitoring networks put in place for the US EPA's Air Quality Programs. Over the past several years, the remote sensing of aeros...

Ambient measurement of fluorescent aerosol particles with a WIBS in the Yangtze River Delta of China: potential impacts of combustion-related aerosol particles

NASA Astrophysics Data System (ADS)

Yu, Xiawei; Wang, Zhibin; Zhang, Minghui; Kuhn, Uwe; Xie, Zhouqing; Cheng, Yafang; Pöschl, Ulrich; Su, Hang

2016-09-01

Fluorescence characteristics of aerosol particles in a polluted atmosphere were studied using a wideband integrated bioaerosol spectrometer (WIBS-4A) in Nanjing, Yangtze River Delta area of China. We observed strong diurnal and day-to-day variations of fluorescent aerosol particles (FAPs). The average number concentrations of FAPs (1-15 µm) detected in the three WIBS measurement channels (FL1: 0.6 cm-3, FL2: 3.4 cm-3, FL3: 2.1 cm-3) were much higher than those observed in forests and rural areas, suggesting that FAPs other than bioaerosols were detected. We found that the number fractions of FAPs were positively correlated with the black carbon mass fraction, especially for the FL1 channel, indicating a large contribution of combustion-related aerosols. To distinguish bioaerosols from combustion-related FAPs, we investigated two classification schemes for use with WIBS data. Our analysis suggests a strong size dependence for the fractional contributions of different types of FAPs. In the FL3 channel, combustion-related particles seem to dominate the 1-2 µm size range while bioaerosols dominate the 2-5 µm range. The number fractions of combustion-related particles and non-combustion-related particles to total aerosol particles were ˜ 11 and ˜ 5 %, respectively.

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

PubMed

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

2009-09-01

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

Secondary Inorganic Aerosols over an Urban Location in North-Western Himalayan Region: Seasonal Variation in Composition and Formation Process(es)

NASA Astrophysics Data System (ADS)

Kaushal, D.; Tandon, A.

2017-12-01

Oxidative photo-chemical transformation of precursor gases, mainly of anthropogenic origin, produces secondary aerosols. Secondary inorganic aerosols constitute a significant fraction of total aerosol load over urban locations especially high altitude in wet-temperate climatic set-up. Towns situated in North-Western Himalayan region (NWHR) with sizable population and attractive tourist destinations have been facing ever increasing problem of gaseous and particulate air pollution from exponential increase in vehicular traffic and other anthropogenic emissions. The present study has been planned to investigate the seasonal variations in atmospheric processes responsible for the formation of Secondary Inorganic Aerosols (SIA) and to estimate contribution of SIA to PM­10 load over an Urban location, Dharamshala, in Dhauladhar region of NWHR. Twenty four hourly PM10 aerosol samples were collected, on quartz micro fibre filters in Dharamshala (1350 amsl) on weekly basis for complete one year time-period (February 2015 - January 2016). These samples were analyzed for Water Soluble Inorganic Ions (WSII) using Ion-Chromatographic System. On annual basis, SO42- ions contributed maximum (52%) followed by NO3- (13%) and NH4+ (12%) to WSII. Based upon Principal Component Analysis (PCA), dominant sources contributing to PM10 associated WSII were identified as: Fossil-Fuel and Bio-mass burning, Vehicular (mainly diesel) emissions and gaseous emissions from the microbial degradation of dead bio-mass. Throughout the year, significantly high proportion of SO42- and considerable thermodynamic stability of (NH4)2SO2 at ambient temperatures, made it the major contributor to SIA over NH4NO3 and NH4Cl. On seasonal basis, maximum contribution of SIA to PM10 was observed in monsoon followed by the winter season. Low ambient temperature in winter season favoured formation of NH4NO3 with significant contribution to SIA. It could be concluded that observed variability in the composition and

Photochemical Aging of Organic Aerosols: A Laboratory Study