Sample records for aerosols including sulfate

  1. Heterogeneous Production of Sulfate Aerosol over China.

    NASA Astrophysics Data System (ADS)

    Shao, J.; Alexander, B.; Chen, Q.; Zhang, L.; Wang, Y.; Xie, Z.; He, P.

    2017-12-01

    Sulfate is thought to be the main contributor to the growth of PM2.5 during the severe haze pollution over China, but most studies have shown that traditional gas- and aqueous-phase chemistry cannot explain the rapid sulfate production during haze events, suggesting a missing heterogeneous oxidation mechanism. In this work, we implement heterogeneous sulfate formation into a 3-D global chemical transport model (GEOS-Chem) to evaluate the different pathways for global and regional sulfate production, including SO2 oxidation by NO2, O3, H2O2, and TMI+O2. Heterogeneous sulfate production rates and the dominant heterogeneous sulfate formation mechanism depends on calculations of aerosol pH, which is in turn is dependent upon thermodynamic state assumptions. We evaluate the influence of aerosol pH and potential impacts of aerosol ionic strength on sulfate production rates and mechanisms in the model, and its implications for PM2.5 in Chinese haze events.

  2. Formation and deposition of volcanic sulfate aerosols on Mars

    NASA Technical Reports Server (NTRS)

    Settle, M.

    1979-01-01

    The paper considers the formation and deposition of volcanic sulfate aerosols on Mars. The rate limiting step in sulfate aerosol formation on Mars is the gas phase oxidation of SO2 by chemical reactions with O, OH, and HO2; submicron aerosol particles would circuit Mars and then be removed from the atmosphere by gravitational forces, globally dispersed, and deposited over a range of equatorial and mid-latitudes. Volcanic sulfate aerosols on Mars consist of liquid droplets and slurries containing sulfuric acid; aerosol deposition on a global or hemispheric scale could account for the similar concentrations of sulfur within surficial soils at the two Viking lander sites.

  3. Anthropogenic and Volcanic Contributions to the Tropospheric and Stratospheric Sulfate Aerosols

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2011-01-01

    We investigate anthropogenic and volcanic contributions to sulfate aerosol in the atmosphere through modeling and analysis of Aura data. We use a global model GOCART to simualte 502 and sulfate aerosol from 2000 to 2010 with the new anthropogenic and volcanic emission estimates to assess the origin of sulfate aerosols in the atmosphere. We will compare the model results with 502 data from OMI and MLS instrument on Aura, and aerosol vertical profiles from CALIPSO. Our goal is to understand the dec ada 1 trends of observed tropospheric and stratospheric aerosols.

  4. Changing transport processes in the stratosphere by radiative heating of sulfate aerosols

    NASA Astrophysics Data System (ADS)

    Niemeier, Ulrike; Schmidt, Hauke

    2017-12-01

    The injection of sulfur dioxide (SO2) into the stratosphere to form an artificial stratospheric aerosol layer is discussed as an option for solar radiation management. Sulfate aerosol scatters solar radiation and absorbs infrared radiation, which warms the stratospheric sulfur layer. Simulations with the general circulation model ECHAM5-HAM, including aerosol microphysics, show consequences of this warming, including changes of the quasi-biennial oscillation (QBO) in the tropics. The QBO slows down after an injection of 4 Tg(S) yr-1 and completely shuts down after an injection of 8 Tg(S) yr-1. Transport of species in the tropics and sub-tropics depends on the phase of the QBO. Consequently, the heated aerosol layer not only impacts the oscillation of the QBO but also the meridional transport of the sulfate aerosols. The stronger the injection, the stronger the heating and the simulated impact on the QBO and equatorial wind systems. With increasing injection rate the velocity of the equatorial jet streams increases, and the less sulfate is transported out of the tropics. This reduces the global distribution of sulfate and decreases the radiative forcing efficiency of the aerosol layer by 10 to 14 % compared to simulations with low vertical resolution and without generated QBO. Increasing the height of the injection increases the radiative forcing only for injection rates below 10 Tg(S) yr-1 (8-18 %), a much smaller value than the 50 % calculated previously. Stronger injection rates at higher levels even result in smaller forcing than the injections at lower levels.

  5. Pathways of sulfate enhancement by natural and anthropogenic mineral aerosols in China

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

    Huang, Xin; Song, Yu; Zhao, Chun

    2014-12-27

    China, the world’s largest consumer of coal, emits approximately 30 million tons of sulfur dioxide (SO₂) per year. SO₂ is subsequently oxidized to sulfate in the atmosphere. However, large gaps exist between model-predicted and measured sulfate levels in China. Long-term field observations and numerical simulations were integrated to investigate the effect of mineral aerosols on sulfate formation. We found that mineral aerosols contributed a nationwide average of approximately 22% to sulfate production in 2006. The increased sulfate concentration was approximately 2 μg m⁻³ in the entire China. In East China and the Sichuan Basin, the increments reached 6.3 μg m⁻³more » and 7.3 μg m⁻³, respectively. Mineral aerosols led to faster SO₂ oxidation through three pathways. First, more SO₂ was dissolved as cloud water alkalinity increased due to water-soluble mineral cations. Sulfate production was then enhanced through the aqueous-phase oxidation of S(IV) (dissolved sulfur in oxidation state +4). The contribution to the national sulfate production was 5%. Second, sulfate was enhanced through S(IV) catalyzed oxidation by transition metals. The contribution to the annual sulfate production was 8%, with 19% during the winter that decreased to 2% during the summer. Third, SO₂ reacts on the surface of mineral aerosols to produce sulfate. The contribution to the national average sulfate concentration was 9% with 16% during the winter and a negligible effect during the summer. The inclusion of mineral aerosols does resolve model discrepancies with sulfate observations in China, especially during the winter. These three pathways, which are not fully considered in most current chemistry-climate models, will significantly impact assessments regarding the effects of aerosol on climate change in China.« less

  6. Importance of including ammonium sulfate ((NH4)2SO4) aerosols for ice cloud parameterization in GCMs

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

    Bhattacharjee, P. S.; Sud, Yogesh C.; Liu, Xiaohong

    2010-02-22

    A common deficiency of many cloud-physics parameterizations including the NASA’s microphysics of clouds with aerosol- cloud interactions (hereafter called McRAS-AC) is that they simulate less (larger) than the observed ice cloud particle number (size). A single column model (SCM) of McRAS-AC and Global Circulation Model (GCM) physics together with an adiabatic parcel model (APM) for ice-cloud nucleation (IN) of aerosols were used to systematically examine the influence of ammonium sulfate ((NH4)2SO4) aerosols, not included in the present formulations of McRAS-AC. Specifically, the influence of (NH4)2SO4 aerosols on the optical properties of both liquid and ice clouds were analyzed. First anmore » (NH4)2SO4 parameterization was included in the APM to assess its effect vis-à-vis that of the other aerosols. Subsequently, several evaluation tests were conducted over the ARM-SGP and thirteen other locations (sorted into pristine and polluted conditions) distributed over marine and continental sites with the SCM. The statistics of the simulated cloud climatology were evaluated against the available ground and satellite data. The results showed that inclusion of (NH4)2SO4 in the SCM made a remarkable improvement in the simulated effective radius of ice clouds. However, the corresponding ice-cloud optical thickness increased more than is observed. This can be caused by lack of cloud advection and evaporation. We argue that this deficiency can be mitigated by adjusting the other tunable parameters of McRAS-AC such as precipitation efficiency. Inclusion of ice cloud particle splintering introduced through well- established empirical equations is found to further improve the results. Preliminary tests show that these changes make a substantial improvement in simulating the cloud optical properties in the GCM, particularly by simulating a far more realistic cloud distribution over the ITCZ.« less

  7. Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

    NASA Astrophysics Data System (ADS)

    Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

    2018-03-01

    Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

  8. Sulfate Formation on Mars by Volcanic Aerosols: A New Look

    NASA Astrophysics Data System (ADS)

    Blaney, D. L.

    1996-03-01

    Sulfur was measured at both Viking Lander sites in abundances of 5-9 wt % SO3. Because the sulfur was more concentrated in clumps which disintegrated and the general oxidized nature of the Martian soil, these measurements led to the assumption that a sulfate duricrust existed. Two types of models for sulfate formation have been proposed. One is a formation by upwardly migrating ground water. The other is the formation of sulfates by the precipitation of volcanic aerosols. Most investigators have tended to favor the ground water origin of sulfates on Mars. However, evidence assemble since Viking may point to a volcanic aerosol origin.

  9. The relative roles of sulfate aerosols and greenhouse gases in climate forcing

    NASA Technical Reports Server (NTRS)

    Kiehl, J. T.; Briegleb, B. P.

    1993-01-01

    Calculations of the effects of both natural and anthropogenic tropospheric sulfate aerosols indicate that the aerosol climate forcing is sufficiently large in a number of regions of the Northern Hemisphere to reduce significantly the positive forcing from increased greenhouse gases. Summer sulfate aerosol forcing in the Northern Hemisphere completely offsets the greenhouse forcing over the eastern United States and central Europe. Anthropogenic sulfate aerosols contribute a globally averaged annual forcing of -0.3 watt per square meter as compared with +2.1 watts per square meter for greenhouse gases. Sources of the difference in magnitude with the previous estimate of Charlson et al. (1992) are discussed.

  10. Total particle, sulfate, and acidic aerosol emissions from kerosene space heaters

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

    Leaderer, B.P.; Boone, P.M.; Hammond, S.K.

    1990-06-01

    Chamber studies were conducted on four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine particles ({<=} 2.5-{mu}m diameter), sulfate, and acidic aerosol indoors. Fine particle concentrations in homes in which the heaters are used may be increased in excess of 20 {mu}g/m{sup 3} over background levels. Sulfate and acidic aerosol levels in such homes could exceed average and peak outdoor concentrations. Maltuned heaters could produce exceptionally high levels of all air contaminantsmore » measured.« less

  11. Total particle, sulfate, and acidic aerosol emissions from kerosene space heaters

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

    Leaderer, B.P.; Boone, P.M.; Hammond, S.K.

    1990-01-01

    The article discusses chamber studies of four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine particles (= or < 2.5 micrometer diameter), sulfate, and acidic aerosol indoors. Fine particle concentrations in houses in which the heaters are used may be increased in excess of 20 micrograms/m3 over background levels. Sulfate and acidic aerosol levels in such houses could exceed average and peak outdoor concentrations. Maltuned heaters could produce exceptionally high levels ofmore » all air contaminants measured.« less

  12. The Polar Mesopause Sulfate Aerosol Layer

    NASA Astrophysics Data System (ADS)

    Mills, M. J.; Toon, O. B.; Thomas, G.; Solomon, S.

    2001-05-01

    Noctilucent ("night-luminous") clouds (NLC), or as seen from space, Polar Mesospheric Clouds (PMC), are typically 1 to 2 km thick and located at altitudes of 80 to 85 km, where the temperature is near 150K. NLC generally occur between 50 degrees latitude to the pole from May to August in the Northern Hemisphere, with occasional sightings at lower latitudes. An extraordinary low-latitude sighting occurred on June 21, 1999 at 41oN. Direct evidence that PMC are composed of water ice was recently reported from satellite observations made in the near infrared. The formation of ice clouds in the upper atmosphere has been studied extensively as a result of the role of Polar Stratospheric Clouds (PSC) in polar ozone depletion. There exists ample evidence that preexisting stratospheric liquid sulfate aerosol plays an important role in the formation of solid PSC particles. Until recent laboratory measurements showed otherwise, however, it was believed that photolysis of sulfuric acid in the upper stratosphere would prevent the formation of such aerosol in the mesosphere. We present here calculations from a microphysical atmospheric model which point to sulfate from volcanic and non-volcanic sources alike as the origin of nuclei on which PMC and NLC form. Current theories have relied on meteor 'smoke' particles arising from meteor ablation and recondensation to explain the nucleation of NLC/PMC ice particles. Our calculated sizes and concentrations of high latitude summer mesosphere sulfate aerosol particles are comparable to or exceed those expected of the meteor source. The model shows that large volcanic eruptions will add significantly to this particle population, several years following the injection. The record of the number of NLC sightings in response to large volcanic eruptions is contradictory. However, microphysical models show that injections of particles may result in positive, negative or neutral response in the visual brightness of NLC, depending on sulfur

  13. Global microphysical simulation of stratospheric sulfate aerosol after the Mt. Pinatubo eruption

    NASA Astrophysics Data System (ADS)

    Sekiya, T.; Sudo, K.

    2014-12-01

    An explosive volcanic eruption can inject a large amount of SO2 into the stratosphere, which is oxidized to form sulfate aerosol. Such aerosol has an impact on the Earth's radiative budget by enhancing back-scattering of the solar radiation. Changes in the size distribution of the aerosol were observed after large volcanic eruptions. Representing the changes in size distribution is important for climate simulation, because the changes affect climate responses to large volcanic eruptions. This study newly developed an aerosol microphysics module and investigated changes in stratospheric sulfate aerosol after the Mt. Pinatubo eruption in the framework of a chemistry-aerosol coupled climate model MIROC-CHASER/SPRINTARS. The module represents aerosol size distribution with three lognormal modes (nucleation, Aitken, and accumulation modes) and includes nucleation, condensation growth/evaporation, and coagulation processes. As a model evaluation, we tested reproducibility of the impacts of the Mt. Pinatubo eruption. We carried out a simulation, in which 20 Mt of SO2 and 100 Mt of volcanic ash were injected respectively into 25 km and 16—22 km altitudes over Mt. Pinatubo (120.4°E, 15.1°N) on June 15th 1991. We compared the model results with space-borne and balloon-borne observations. Although our model overestimated a near-global mean (60°N—60°S) of stratospheric aerosol optical depth (SAOD) observed by SAGE II instrument until one year after the eruption, it reproduced the observed SAOD in the subsequent period. The model well captured the observed increase of effective radius at 20 km altitude in the northern midlatitudes. In addition, we analyzed the pathway of volcanic sulfur from SO2 to sulfate aerosol. The most amount of the volcanic sulfur was converted from SO2 to accumulation mode aerosol by 100 days after the eruption. The conversion into the accumulation mode aerosol is attributable to coagulation until the first 14 days and to condensation growth

  14. Spectral signatures of polar stratospheric clouds and sulfate aerosol

    NASA Technical Reports Server (NTRS)

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

    1994-01-01

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

  15. Global source attribution of sulfate aerosol and its radiative forcing

    NASA Astrophysics Data System (ADS)

    Yang, Y.; Wang, H.; Smith, S.; Easter, R. C.; Ma, P. L.; Qian, Y.; Li, C.; Yu, H.; Rasch, P. J.

    2017-12-01

    Sulfate is an important aerosol that poses health risks and influences climate. Due to long-range atmospheric transport, local sulfate pollution could result from intercontinental influences, making domestic efforts of improving air quality inefficient. Accurate understanding of source attribution of sulfate and its radiative forcing is important for both regional air quality improvement and global climate mitigation. In this study, for the first time, a sulfur source-tagging capability is implemented in the Community Atmosphere Model (CAM5) to quantify the global source-receptor relationships of sulfate and its direct and indirect radiative forcing (DRF and IRF). Near-surface sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate is primarily attributed to non-local sources from long-range transport. The export of SO2 and sulfate from Europe contributes 20% of sulfate concentrations over North Africa, Russia and Central Asia. Sources from the Middle East account for 20% of sulfate over North Africa, Southern Africa and Central Asia in winter and autumn, and 20% over South Asia in spring. East Asia accounts for about 50% of sulfate over Southeast Asia in winter and autumn, 15% over Russia in summer, and 10% over North America in spring. South Asia contributes to 25% of sulfate over Southeast Asia in spring. Lifetime of aerosols, together with regional export, is found to determine regional air quality. The simulated global total sulfate DRF is -0.42 W m-2, with 75% contributed by anthropogenic sulfate and 25% contributed by natural sulfate. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes the most to the total DRF. East Asia has the largest contribution of 20-30% over the Northern Hemisphere mid- and high-latitudes. A 20% perturbation of sulfate and its precursor emissions gives a sulfate IRF of -0.44 W m-2. DMS has the

  16. Analysis of reversibility and reaction products of glyoxal uptake onto ammonium sulfate aerosol

    NASA Astrophysics Data System (ADS)

    Galloway, M. M.; Chhabra, P. S.; Chan, A. W.; Surratt, J. D.; Kwan, A. J.; Wennberg, P. O.; Flagan, R. C.; Seinfeld, J. H.; Keutsch, F. N.

    2009-04-01

    Glyoxal, the smallest alpha-dicarbonyl, is an oxidation product of both biogenic and anthropogenic volatile organic compounds (Fu et al. JGR 113, D15303, 2008). Despite its low molecular weight, its role in secondary organic aerosol (SOA) formation has gained interest and a recent study suggested that it accounts for more than 15% of SOA in Mexico City (Volkamer et al. GRL 34, L19807, 2007). Despite numerous previous studies, questions remain regarding the processes controlling glyoxal uptake onto aerosol, including the role of acid catalysis, degree of reversibility, and identity of aerosol phase reaction products. We present results of chamber aerosol studies (Galloway et al. ACPD 8, 20799, 2008) and laboratory studies of bulk samples aimed at improving the understanding of these processes, in particular formation of oligomers and organosulfates of glyoxal, as well as the formation of imidazoles (carbon-nitrogen containing heterocyclic aromatic compounds) under dark and irradiated conditions. The relevance of these classes of reaction products extends beyond glyoxal, as evidence of oligomers and organosulfates other than those of glyoxal have been found in ambient aerosol (Surratt et al. JPCA 112, 8345, 2008; Denkenberger et al. Environ. Sci. Technol. 41, 5439, 2007). Experiments in which a chamber air mass was diluted after equilibration of glyoxal uptake onto ammonium sulfate seed aerosol (relative humidity 60% and glyoxal mixing ratios of 25-200 ppbv) shows that under these conditions uptake is reversible. The most important condensed phase products are hydrated oligomers of glyoxal, which are also formed reversibly under these conditions. Our studies show that organosulfates were not formed under dark conditions for neutral or acidified aerosol; similarly, Minerath et al. have recently shown that formation of a different class of organosulfates (alkyl sulfates) also proceeds very slowly even under acidic conditions (Environ. Sci. Technol. 42, 4410, 2008). The

  17. Geo-Engineering Climate Change with Sulfate Aerosol

    NASA Astrophysics Data System (ADS)

    Rasch, P. J.; Crutzen, P. J.

    2006-12-01

    We explore the impact of injecting a precursor of sulfate aerosols into the middle atmosphere where they would act to increase the planetary albedo and thus counter some of the effects of greenhouse gase forcing. We use an atmospheric general circulation model (CAM, the Community Atmosphere Model) coupled to a slab ocean model for this study. Only physical effects are examined, that is we ignore the biogeochemical and chemical implications of changes to greenhouse gases and aerosols, and do not explore the important ethical, legal, and moral issues that are associated with deliberate geo-engineering efforts. The simulations suggest that the sulfate aerosol produced from the SO2 source in the stratosphere is sufficient to counterbalance most of the warming associated with the greenhouse gas forcing. Surface temperatures return to within a few tenths of a degree(K) of present day levels. Sea ice and precipitation distributions are also much closer to their present day values. The polar region surface temperatures remain 1-3 degrees warm in the winter hemisphere than present day values. This study is very preliminary. Only a subset of the relevant effects have been explored. The effect of such an injection of aerosols on middle atmospheric chemistry, and the effect on cirrus clouds are obvious missing components that merit scrutiny. There are probably others that should be considered. The injection of such aerosols cannot help in ameliorating the effects of CO2 changes on ocean PH, or other effects on the biogeochemistry of the earth system.

  18. Intercomparison of Models Representing Direct Shortwave Radiative Forcing by Sulfate Aerosols

    NASA Technical Reports Server (NTRS)

    Boucher, O.; Schwartz, S. E.; Ackerman, T. P.; Anderson, T. L.; Bergstrom, B.; Bonnel, B.; Dahlback, A.; Fouquart, Y.; Chylek, P.; Fu, Q.; hide

    2000-01-01

    The importance of aerosols as agents of climate change has recently been highlighted. However, the magnitude of aerosol forcing by scattering of shortwave radiation (direct forcing) is still very uncertain even for the relatively well characterized sulfate aerosol. A potential source of uncertainty is in the model representation of aerosol optical properties and aerosol influences on radiative transfer in the atmosphere. Although radiative transfer methods and codes have been compared in the past, these comparisons have not focused on aerosol forcing (change in net radiative flux at the top of the atmosphere). Here we report results of a project involving 12 groups using 15 models to examine radiative forcing by sulfate aerosol for a wide range of values of particle radius, aerosol optical depth, surface albedo, and solar zenith angle. Among the models that were employed were high and low spectral resolution models incorporating a variety of radiative transfer approximations as well as a line-by-line model. The normalized forcings (forcing per sulfate column burden) obtained with the several radiative transfer models were examined, and the discrepancies were characterized. All models simulate forcings of comparable amplitude and exhibit a similar dependence on input parameters. As expected for a non-light-absorbing aerosol, forcings were negative (cooling influence) except at high surface albedo combined with small solar zenith angle. The relative standard deviation of the zenith-angle-averaged normalized broadband forcing for 15 models-was 8% for particle radius near the maximum in this forcing (approx. 0.2 microns) and at low surface albedo. Somewhat greater model-to-model discrepancies were exhibited at specific solar zenith angles. Still greater discrepancies were exhibited at small particle radii and much greater discrepancies were exhibited at high surface albedos, at which the forcing changes sign; in these situations, however, the normalized forcing is

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

    EPA Science Inventory

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

  20. Antarctic polar stratospheric aerosols: The roles of nitrates, chlorides and sulfates

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Snetsinger, K. G.; Goodman, J. K.; Ferry, G. V.; Oberbeck, V. R.; Verma, S.; Fong, W.

    1988-01-01

    Nitric and hydrochloric acids have been postulated to condense in the winter polar stratosphere to become an important component of polar stratospheric clouds. One implication is that the removal of NO(y) from the gas phase by this mechanism allows high Cl(x) concentrations to react with O3, because the formation of ClNO3 is inhibited. Contributions of NO3 and Cl to the stratospheric aerosol were determined during the 1987 Airborne Antarctic Ozone Experiment by testing for the presence of nitrates and chlorides in the condensed phase. Aerosol particles were collected on four 500 micron diameter gold wires, each pretreated differently to give results that were specific to certain physical and chemical aerosol properties. One wire was carbon-coated for concentration and size analyses by scanning electron microscopy; X-ray energy dispersive analyses permitted the detection of S and Cl in individual particles. Three more wires were coated with Nitron, barium chloride and silver nitrate, respectively, to detect nitrate, sulfate and chloride in aerosol particles. All three ions, viz., sulfates, nitrates and chlorides were detected in the Antarctic stratospheric aerosol. In terms of number concentrations, the aerosol was dominated by sulfates, followed by chlorides and nitrates. An inverse linear regression can be established between nitrate concentrations and ozone mixing ratio, and between temperature and nitrates.

  1. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

    PubMed Central

    Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; He, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang

    2016-01-01

    Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m−3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. PMID:28028539

  2. 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.

  3. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

    NASA Astrophysics Data System (ADS)

    Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; Wang, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang

    2017-04-01

    Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to 300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. Reference: Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Science Advances, 2, 10.1126/sciadv.1601530, 2016.

  4. Reactive Nitrogen Chemistry in Aerosol Water as a Source of Sulfate during Haze Events in China

    NASA Astrophysics Data System (ADS)

    Su, H.; Zheng, G.; Wei, C.; Mu, Q.; Zheng, B.; Wang, Z.; Zhang, Q.; Gao, M.; He, K.; Carmichael, G. R.; Poeschl, U.; Cheng, Y.

    2017-12-01

    Fine particle pollution associated with winter haze threatens the health of over 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations up to 300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models relying on sulfate production mechanisms that require photochemical oxidants, cannot predict these high levels due to the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content leading to faster sulfate production and more severe haze pollution. Reference: Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Science Advances, 2, 10.1126/sciadv.1601530, 2016.

  5. Acidic sulfate aerosols: characterization and exposure.

    PubMed Central

    Lioy, P J; Waldman, J M

    1989-01-01

    Exposures to acidic aerosol in the atmosphere are calculated from data reported in the scientific literature. The majority of date was not derived from studies necessarily designed to examine human exposures. Most of the studies were designed to investigate the characteristics of the atmosphere. However, the measurements were useful in defining two potential exposure situations: regional stagnation and transport conditions and local plume impacts. Levels of acidic aerosol in excess of 20 to 40 micrograms/m3 (as H2SO4) have been observed for time durations ranging from 1 to 12 hr. These were associated with high, but not necessarily the highest, atmospheric SO4(2)- levels. Exposures of 100 to 900 micrograms/m3/hr were calculated for the acid events that were monitored. In contrast, earlier London studies indicated that apparent acidity in excess of 100 micrograms/m3 (as H2SO4) was present in the atmosphere, and exposures less than 2000 micrograms/m3/hr were possible. Our present knowledge about the frequency, magnitude, and duration of acidic sulfate aerosol events and episodes is insufficient. Efforts must be made to gather more data, but these should be done in such a way that evaluation of human exposure is the focus of the research. In addition, further data are required on the mechanisms of formation of H2SO4 and on what factors can be used to predict acidic sulfate episodes. PMID:2651103

  6. Comparison of normal and asthmatic subjects' responses to sulfate pollutant aerosols

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

    Utell, M.J.; Morrow, P.E.; Hyde, R.W.

    Epidemiological studies support an association between elevated levels of sulfates and acute respiratory disease. To determine if these pollutants produce airway hyperreactivity, 16 normal and 17 asthmatic subjects inhaled a control NaCl aerosol and the following sulfates: ammonium sulfate, sodium bisulfate, ammonium bisulfate, and sulfuric acid. A Lovelace generator produced particles with an average MMAD of approx. 1.0 ..mu..m (sigma/sub g/ approx. = 2.0) and concentrations of 0.1 and 1.0 mg/m/sup 3/. By double-blind randomization, all subjects breathed these aerosols for a 16-minute period. To determine if sulfate inhalation caused increased reactivity to a known bronchoconstrictor, all subjects inhaled carbacholmore » following each 16-minute exposure. Before, during, and after exposure, pulmonary function studies were performed. When compared to NaCl, sulfate (1 mg/m/sup 3/) produced significant reductions in airway conductance and flow rates in asthmatics. The two most sensitive asthmatics demonstrated changes even at 0.1 mg/m/sup 3/ sulfate. To a far more significant degree, the bronchoconstrictor action of carbachol was potentiated by sulfates more or less in relation to their acidity in normals and asthmatics.« less

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

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

  8. Satellite observations and EMAC model calculations of sulfate aerosols from Kilauea: a study of aerosol formation, processing, and loss

    NASA Astrophysics Data System (ADS)

    Penning de Vries, Marloes; Beirle, Steffen; Brühl, Christoph; Dörner, Steffen; Pozzer, Andrea; Wagner, Thomas

    2016-04-01

    The currently most active volcano on Earth is Mount Kilauea on Hawaii, as it has been in a state of continuous eruption since 1983. The opening of a new vent in March 2008 caused half a year of strongly increased SO2 emissions, which in turn led to the formation of a sulfate plume with an extent of at least two thousand kilometers. The plume could be clearly identified from satellite measurements from March to November, 2008. The steady trade winds in the region and the lack of interfering sources allowed us to determine the life time of SO2 from Kilauea using only satellite-based measurements (no a priori or model information). The current investigation focuses on sulfate aerosols: their formation, processing and subsequent loss. Using space-based aerosol measurements by MODIS, we study the evolution of aerosol optical depth, which first increases as a function of distance from the volcano due to aerosol formation from SO2 oxidation, and subsequently decreases as aerosols are deposited to the surface. The outcome is compared to results from calculations using the EMAC (ECHAM/MESSy Atmospheric Chemistry) model to test the state of understanding of the sulfate aerosol life cycle. For this comparison, a particular focus is on the role of clouds and wet removal processes.

  9. [Tracing Sources of Sulfate Aerosol in Nanjing Northern Suburb Using Sulfur and Oxygen Isotopes].

    PubMed

    Wei, Ying; Guo, Zhao-bing; Ge, Xin; Zhu, Sheng-nan; Jiang, Wen-juan; Shi, Lei; Chen, Shu

    2015-04-01

    Abstract: To trace the sources of sulfate contributing to atmospheric aerosol, PM2.5 samples for isotopic analysis were collected in Nanjing northern suburb during January 2014. The sulfur and oxygen isotopic compositions of sulfate from these samples were determined by EA-IRMS. Source identification and apportionment were carried out using stable isotopic and chemical evidences, combined with absolute principal component analysis (APCA) method. The Δ34S values of aerosol sulfate ranged from 2.7 per thousand to 6.4 per thousand, with an average of 5.0 per thousand ± 0.9 per thousand, while the Δ18O values ranged from 10.6 per thousand to 16.1 per thousand, with an average of 12.5 per thousand ± 1.37 per thousand. In conjunction with air mass trajectories, the results suggested that aerosol sulfates were controlled by a dominance of local anthropogenic sulfate, followed by the contributions of long-distance transported sulfate. There was a minor effect of some other low-Δ34S valued sulfates, which might be expected from biogenic sources. Absolute principal component analysis results showed that the contributions of anthropogenic sulfate and long-distance transported sulfate were 46.74% and 31.54%, respectively.

  10. The Sectional Stratospheric Sulfate Aerosol module (S3A-v1) within the LMDZ general circulation model: description and evaluation against stratospheric aerosol observations

    NASA Astrophysics Data System (ADS)

    Kleinschmitt, Christoph; Boucher, Olivier; Bekki, Slimane; Lott, François; Platt, Ulrich

    2017-09-01

    Stratospheric aerosols play an important role in the climate system by affecting the Earth's radiative budget as well as atmospheric chemistry, and the capabilities to simulate them interactively within global models are continuously improving. It is important to represent accurately both aerosol microphysical and atmospheric dynamical processes because together they affect the size distribution and the residence time of the aerosol particles in the stratosphere. The newly developed LMDZ-S3A model presented in this article uses a sectional approach for sulfate particles in the stratosphere and includes the relevant microphysical processes. It allows full interaction between aerosol radiative effects (e.g. radiative heating) and atmospheric dynamics, including e.g. an internally generated quasi-biennial oscillation (QBO) in the stratosphere. Sulfur chemistry is semi-prescribed via climatological lifetimes. LMDZ-S3A reasonably reproduces aerosol observations in periods of low (background) and high (volcanic) stratospheric sulfate loading, but tends to overestimate the number of small particles and to underestimate the number of large particles. Thus, it may serve as a tool to study the climate impacts of volcanic eruptions, as well as the deliberate anthropogenic injection of aerosols into the stratosphere, which has been proposed as a method of geoengineering to abate global warming.

  11. MIPAS observations of volcanic sulfate aerosol and sulfur dioxide in the stratosphere

    NASA Astrophysics Data System (ADS)

    Günther, Annika; Höpfner, Michael; Sinnhuber, Björn-Martin; Griessbach, Sabine; Deshler, Terry; von Clarmann, Thomas; Stiller, Gabriele

    2018-01-01

    Volcanic eruptions can increase the stratospheric sulfur loading by orders of magnitude above the background level and are the most important source of variability in stratospheric sulfur. We present a set of vertical profiles of sulfate aerosol volume densities and derived liquid-phase H2SO4 (sulfuric acid) mole fractions for 2005-2012, retrieved from infrared limb emission measurements performed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board of the Environmental Satellite (Envisat). Relative to balloon-borne in situ measurements of aerosol at Laramie, Wyoming, the MIPAS aerosol data have a positive bias that has been corrected, based on the observed differences to the in situ data. We investigate the production of stratospheric sulfate aerosol from volcanically emitted SO2 for two case studies: the eruptions of Kasatochi in 2008 and Sarychev in 2009, which both occurred in the Northern Hemisphere midlatitudes during boreal summer. With the help of chemical transport model (CTM) simulations for the two volcanic eruptions we show that the MIPAS sulfate aerosol and SO2 data are qualitatively and quantitatively consistent with each other. Further, we demonstrate that the lifetime of SO2 is explained well by its oxidation by hydroxyl radicals (OH). While the sedimentation of sulfate aerosol plays a role, we find that the long-term decay of stratospheric sulfur after these volcanic eruptions in midlatitudes is mainly controlled by transport via the Brewer-Dobson circulation. Sulfur emitted by the two midlatitude volcanoes resides mostly north of 30° N at altitudes of ˜ 10-16 km, while at higher altitudes ( ˜ 18-22 km) part of the volcanic sulfur is transported towards the Equator where it is lifted into the stratospheric overworld and can further be transported into both hemispheres.

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

    PubMed

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

    2013-01-01

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

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

    PubMed Central

    2013-01-01

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

  14. A Sulfate Aerosol Trigger for the Sturtian Neoproterozoic Snowball Event

    NASA Astrophysics Data System (ADS)

    Wordsworth, R. D.; Macdonald, F. A.

    2017-12-01

    Despite the dominance of the carbon cycle in determining the evolution of Earth's climate in general, certain events defy easy explanation via atmospheric CO2 changes alone. Here we discuss the particular role that transient planetary albedo changes via sulfate aerosol formation can play in major climate transitions. Specifically, we propose that SO2 outgassing associated with the eruption of the Franklin Large Igneous Province (LIP) led to the first Neoproterozoic Snowball event, the Sturtian, 716 Ma. We summarize U/Pb zircon and baddeleyite dating indicating the synchronicity of the Franklin eruptions and the onset of the Sturtian, and paleomagnetic data indicating that the Franklin erupted close to the equator. We then discuss in detail the modeling we have performed of eruption rate, the plume height achieved during basaltic fissure volcanism, the chemistry and microphysics of sulfate aerosol formation, and the dependence of aerosol longwave and shortwave radiative effects on atmospheric loading, particle size and surface albedo. We discuss the critical importance of the latitude of eruption, the tropopause height, and ocean dynamics in determining the strength and sign of aerosol radiative forcing. We finish by comparing the Franklin event with other LIP emplacement events in Earth history and make suggestions for future modeling.

  15. Using stable isotopes to trace sources and formation processes of sulfate aerosols from Beijing, China

    PubMed Central

    Han, Xiaokun; Guo, Qingjun; Liu, Congqiang; Fu, Pingqing; Strauss, Harald; Yang, Junxing; Hu, Jian; Wei, Lianfang; Ren, Hong; Peters, Marc; Wei, Rongfei; Tian, Liyan

    2016-01-01

    Particulate pollution from anthropogenic and natural sources is a severe problem in China. Sulfur and oxygen isotopes of aerosol sulfate (δ34Ssulfate and δ18Osulfate) and water-soluble ions in aerosols collected from 2012 to 2014 in Beijing are being utilized to identify their sources and assess seasonal trends. The mean δ34S value of aerosol sulfate is similar to that of coal from North China, indicating that coal combustion is a significant contributor to atmospheric sulfate. The δ34Ssulfate and δ18Osulfate values are positively correlated and display an obvious seasonality (high in winter and low in summer). Although an influence of meteorological conditions to this seasonality in isotopic composition cannot be ruled out, the isotopic evidence suggests that the observed seasonality reflects temporal variations in the two main contributions to Beijing aerosol sulfate, notably biogenic sulfur emissions in the summer and the increasing coal consumption in winter. Our results clearly reveal that a reduction in the use of fossil fuels and the application of desulfurization technology will be important for effectively reducing sulfur emissions to the Beijing atmosphere. PMID:27435991

  16. Sulfur isotope measurements of submicrometer sulfate aerosol particles over the Pacific Ocean

    NASA Technical Reports Server (NTRS)

    Calhoun, Julie A.; Charlson, Robert J.; Bates, Timothy S.

    1991-01-01

    Stable isotopes were used to analyze the submicron-size sulfate aerosol particles in the atmosphere over the Pacific Ocean, together with the air-mass back trajectories, in order to test the hypothesis of Charlson et al. (1987) who suggested that, over the remote ocean areas, the primary source of atmospheric nonseasalt (NSS) sulfate is marine emissions of dimethylsulfide (DMS). The observed results of isotopic fractionation between the seawater sulfate and NSS sulfate fractions was found to be consistent with the isotopic fractionation predicted for the transformation of the seawater sulfate to the atmospheric NSS sulfate via a DMS path way, supporting the hypothesis of Charlson et al.

  17. Weathering of Olivine during Interaction of Sulfate Aerosols with Mars Soil under Current Climate Conditions

    NASA Astrophysics Data System (ADS)

    Niles, P. B.; Golden, D. C.; Michalski, J. R.; Ming, D. W.

    2017-12-01

    Sulfur concentrations in the Mars soils are elevated above 1 wt% in nearly every location visited by landed spacecraft. This observation was first made by the Viking landers, and has been confirmed by subsequent missions. The wide distribution of sulfur in martian soils has been attributed to volcanic degassing, formation of sulfate aerosols, and later incorporation into martian soils during gravitational sedimentation. However, later discoveries of more concentrated sulfur bearing sediments by the Opportunity rover has led some to believe that sulfates may instead be a product of evaporation and aeolian redistribution. One question that has not been addressed is whether the modern surface conditions are too cold for weathering of volcanic materials by sulfate aerosols. We suggest here that mixtures of atmospheric aerosols, ice, and dust have the potential for creating small films of cryo-concentrated acidic solutions that may represent an important unexamined environment for understanding weathering processes on Mars. Laboratory experiments were conducted to simulate weathering of olivine under Mars-like conditions. The weathering rates measured in this study suggest that fine grained olivine on Mars would weather into sulfate minerals in short time periods if they are exposed to H2SO4 aerosols at temperatures at or above -40°C. In this system, the strength of the acidic solution is maximized through eutectic freezing in an environment where the silicate minerals are extremely fine grained and have high surface areas. This provides an ideal environment for olivine weathering despite the very low temperatures. The likelihood of substantial sulfur-rich volcanism on Mars and creation of abundant sulfate aerosols suggests that this process would have been important during formation of martian soils and sediments. Future work modeling sulfur release rates during volcanic eruptions and aerosol distribution over the surface will help understand how well this process

  18. Characterizing the influence of anthropogenic emissions and transport variability on sulfate aerosol concentrations at Mauna Loa Observatory

    NASA Astrophysics Data System (ADS)

    Potter, Lauren E.

    Sulfate aerosol in the atmosphere has substantial impacts on human health and environmental quality. Most notably, atmospheric sulfate has the potential to modify the earth's climate system through both direct and indirect radiative forcing mechanisms (Meehl et al., 2007). Emissions of sulfur dioxide, the primary precursor of sulfate aerosol, are now globally dominated by anthropogenic sources as a result of widespread fossil fuel combustion. Economic development in Asian countries since 1990 has contributed considerably to atmospheric sulfur loading, particularly China, which currently emits approximately 1/3 of global anthropogenic SO2 (Klimont et al., 2013). Observational and modeling studies have confirmed that anthropogenic pollutants from Asian sources can be transported long distances with important implications for future air quality and global climate change. Located in the remote Pacific Ocean (19.54°N, 155.58°W) at an elevation of 3.4 kilometers above sea level, Mauna Loa Observatory (MLO) is an ideal measurement site for ground-based, free tropospheric observations and is well situated to experience influence from springtime Asian outflow. This study makes use of a 14-year data set of aerosol ionic composition, obtained at MLO by the University of Hawaii at Manoa. Daily filter samples of total aerosol concentrations were made during nighttime downslope (free-tropospheric) transport conditions, from 1995 to 2008, and were analyzed for aerosol-phase concentrations of the following species: nitrate (NO3-), sulfate (SO42-), methanesulfonate (MSA), chloride (Cl-), oxalate, sodium (Na+), ammonium (NH 4+), potassium (K+), magnesium (Mg 2+), and calcium (Ca2+). An understanding of the factors controlling seasonal and interannual variations in aerosol speciation and concentrations at this site is complicated by the relatively short lifetimes of aerosols, compared with greenhouse gases which have also been sampled over long time periods at MLO. Aerosol filter

  19. Arctic climate response to geoengineering with stratospheric sulfate aerosols

    NASA Astrophysics Data System (ADS)

    McCusker, K. E.; Battisti, D. S.; Bitz, C. M.

    2010-12-01

    Recent warming and record summer sea-ice area minimums have spurred expressions of concern for arctic ecosystems, permafrost, and polar bear populations, among other things. Geoengineering by stratospheric sulfate aerosol injections to deliberately cancel the anthropogenic temperature rise has been put forth as a possible solution to restoring Arctic (and global) climate to modern conditions. However, climate is particularly sensitive in the northern high latitudes, responding easily to radiative forcing changes. To that end, we explore the extent to which tropical injections of stratospheric sulfate aerosol can accomplish regional cancellation in the Arctic. We use the Community Climate System Model version 3 global climate model to execute simulations with combinations of doubled CO2 and imposed stratospheric sulfate burdens to investigate the effects on high latitude climate. We further explore the sensitivity of the polar climate to ocean dynamics by running a suite of simulations with and without ocean dynamics, transiently and to equilibrium respectively. We find that, although annual, global mean temperature cancellation is accomplished, there is over-cooling on land in Arctic summer, but residual warming in Arctic winter, which is largely due to atmospheric circulation changes. Furthermore, the spatial extent of these features and their concurrent impacts on sea-ice properties are modified by the inclusion of ocean dynamical feedbacks.

  20. Sulfate Aerosol Control of Tropical Atlantic Climate over the Twentieth Century

    NASA Technical Reports Server (NTRS)

    Chang, C.-Y.; Chiang, J. C. H.; Wehner, M. F.; Friedman, A. R.; Ruedy, R.

    2011-01-01

    The tropical Atlantic interhemispheric gradient in sea surface temperature significantly influences the rainfall climate of the tropical Atlantic sector, including droughts over West Africa and Northeast Brazil. This gradient exhibits a secular trend from the beginning of the twentieth century until the 1980s, with stronger warming in the south relative to the north. This trend behavior is on top of a multi-decadal variation associated with the Atlantic multi-decadal oscillation. A similar long-term forced trend is found in a multimodel ensemble of forced twentieth-century climate simulations. Through examining the distribution of the trend slopes in the multimodel twentieth-century and preindustrial models, the authors conclude that the observed trend in the gradient is unlikely to arise purely from natural variations; this study suggests that at least half the observed trend is a forced response to twentieth-century climate forcings. Further analysis using twentieth-century single-forcing runs indicates that sulfate aerosol forcing is the predominant cause of the multimodel trend. The authors conclude that anthropogenic sulfate aerosol emissions, originating predominantly from the Northern Hemisphere, may have significantly altered the tropical Atlantic rainfall climate over the twentieth century

  1. Aerosol pH buffering in the southeastern US: Fine particles remain highly acidic despite large reductions in sulfate

    NASA Astrophysics Data System (ADS)

    Weber, R. J.; Guo, H.; Russell, A. G.; Nenes, A.

    2015-12-01

    pH is a critical aerosol property that impacts many atmospheric processes, including biogenic secondary organic aerosol formation, gas-particle phase partitioning, and mineral dust or redox metal mobilization. Particle pH has also been linked to adverse health effects. Using a comprehensive data set from the Southern Oxidant and Aerosol Study (SOAS) as the basis for thermodynamic modeling, we have shown that particles are currently highly acidic in the southeastern US, with pH between 0 and 2. Sulfate and ammonium are the main acid-base components that determine particle pH in this region, however they have different sources and their concentrations are changing. Over 15 years of network data show that sulfur dioxide emission reductions have resulted in a roughly 70 percent decrease in sulfate, whereas ammonia emissions, mainly link to agricultural activities, have been largely steady, as have gas phase ammonia concentrations. This has led to the view that particles are becoming more neutralized. However, sensitivity analysis, based on thermodynamic modeling, to changing sulfate concentrations indicates that particles have remained highly acidic over the past decade, despite the large reductions in sulfate. Furthermore, anticipated continued reductions of sulfate and relatively constant ammonia emissions into the future will not significantly change particle pH until sulfate drops to clean continental background levels. The result reshapes our expectation of future particle pH and implies that atmospheric processes and adverse health effects linked to particle acidity will remain unchanged for some time into the future.

  2. Sulfate and MSA Aerosol Dynamics in the Marine Boundary Layer

    DTIC Science & Technology

    1997-09-30

    Kilauea Volcano as they move out over the Pacific Ocean, to understand what happens to marine and continental aerosols when they mix. This dataset will...SULFATE AND MSA AEROSOL DYNAMICS IN THE MARINE BOUNDARY LAYER P.I. - Barry J. Huebert Department of Oceanography University of Hawaii 1000 Pope Rd...6. AUTHOR(S) 5d. PROJECT NUMBER 5e. TASK NUMBER 5f. WORK UNIT NUMBER 7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) University of Hawaii

  3. Impacts of East Asian Sulfate Aerosols on Local and Remote Climate

    NASA Astrophysics Data System (ADS)

    Bartlett, R. E.; Bollasina, M. A.

    2017-12-01

    Anthropogenic aerosols exert significant climate forcing, which increases with emissions following trends of growing population and industry. Globally, aerosols cause a net cooling, counteracting greenhouse gas warming; however, regional impacts vary since emissions are spatially and temporally heterogeneous. While European and North American emissions have decreased in recent decades, Asian, particularly East Asian, emissions continued to rise into the 21st century. In addition to links between Asian anthropogenic aerosols and significant local climate impacts - for example, changes to the Asian monsoon system - studies have also shown influences on remote climate. Sulfate aerosols are particularly important for East Asia, remaining at constant levels higher than column burdens of other aerosol species. If a concerted effort - as laid out by government policies aiming to improve air quality - is made, the effects of anthropogenic aerosols (due to their short atmospheric lifetime) could be quickly reversed. Thus, it is vital to understand the climate impact aerosols have had up to now to aid in determining what will happen in the future. We use transient climate modelling experiments with the Community Earth System Model to investigate the impacts of East Asian sulfate aerosols in the present day compared to 1950 (i.e. before rapid industrialisation in this region), focusing on dynamical mechanisms leading to the occurrence of such impacts, and how their influence can spread to remote regions. We find, in addition to significant monsoon impacts, noticeable shifts in large-scale circulation features such as the ITCZ and the Pacific Walker cell. Through diabatic heating responses, changes to upper-level atmospheric dynamics are evident, leading to downstream effects on surface climate - for example, surface cooling over Europe. Understanding of these impacts is vital when considering how the good intentions of air quality improvement might inadvertently have

  4. Sulfate Aerosols Promote Lung Cancer Metastasis by Epigenetically Regulating the Epithelial-to-Mesenchymal Transition (EMT).

    PubMed

    Yun, Yang; Gao, Rui; Yue, Huifeng; Guo, Lin; Li, Guangke; Sang, Nan

    2017-10-03

    Secondary inorganic aerosols (SIA), particularly sulfate aerosols, are central particulate matter (PM) constituents of severe haze formation in China and exert profound impacts on human health; however, our understanding of the mechanisms by which sulfate aerosols cause malignancy in lung carcinogenesis remains incomplete. Here, we show that exposure to secondary inorganic aerosols induced the invasion and migration of lung epithelial cells, and that (NH 4 ) 2 SO 4 exerted the most serious effects in vitro and promoted lung tumor metastasis in vivo. This action was associated with alterations of phenotype markers in the epithelial-to-mesenchymal transition (EMT), such as the up-regulation of fibronectin (Fn1) and the down-regulation of E-cadherin (E-cad). Hypoxia-inducible factor 1α (HIF-1α)-Snail signaling, regulated by the generation of reactive oxygen species (ROS), was involved in the (NH 4 ) 2 SO 4 -induced EMT, and the potent antioxidant N-acetylcysteine (NAC) inhibited the activation of HIF-1α-Snail and blocked the EMT, cell invasion, and migration in response to (NH 4 ) 2 SO 4 . Additionally, CpG hypermethylation in the E-cad promoter regions partly contributed to the (NH 4 ) 2 SO 4 -regulated E-cad repression, and the DNA methyltransferase inhibitor 5-aza-2'-deoxycytidine (5-Aza) restored the (NH 4 ) 2 SO 4 -induced down-regulation of E-cad. Our findings reveal a potential mechanistic basis for exploring the association between sulfate aerosol exposure and increased malignancy during lung carcinogenesis, and suggest new approaches for the treatment, improvement, and prevention of lung cancer resulting from sulfate aerosol exposure in severe haze-fog.

  5. Tales of volcanoes and El-Nino southern oscillations with the oxygen isotope anomaly of sulfate aerosol.

    PubMed

    Shaheen, Robina; Abauanza, Mariana; Jackson, Teresa L; McCabe, Justin; Savarino, Joel; Thiemens, Mark H

    2013-10-29

    The ability of sulfate aerosols to reflect solar radiation and simultaneously act as cloud condensation nuclei renders them central players in the global climate system. The oxidation of S(IV) compounds and their transport as stable S(VI) in the Earth's system are intricately linked to planetary scale processes, and precise characterization of the overall process requires a detailed understanding of the linkage between climate dynamics and the chemistry leading to the product sulfate. This paper reports a high-resolution, 22-y (1980-2002) record of the oxygen-triple isotopic composition of sulfate (SO4) aerosols retrieved from a snow pit at the South Pole. Observed variation in the O-isotopic anomaly of SO4 aerosol is linked to the ozone variation in the tropical upper troposphere/lower stratosphere via the Ozone El-Niño Southern Oscillations (ENSO) Index (OEI). Higher (17)O values (3.3‰, 4.5‰, and 4.2‰) were observed during the three largest ENSO events of the past 2 decades. Volcanic events inject significant quantities of SO4 aerosol into the stratosphere, which are known to affect ENSO strength by modulating stratospheric ozone levels (OEI = 6 and (17)O = 3.3‰, OEI = 11 and (17)O = 4.5‰) and normal oxidative pathways. Our high-resolution data indicated that (17)O of sulfate aerosols can record extreme phases of naturally occurring climate cycles, such as ENSOs, which couple variations in the ozone levels in the atmosphere and the hydrosphere via temperature driven changes in relative humidity levels. A longer term, higher resolution oxygen-triple isotope analysis of sulfate aerosols from ice cores, encompassing more ENSO periods, is required to reconstruct paleo-ENSO events and paleotropical ozone variations.

  6. Black Carbon and Sulfate Aerosols in the Arctic: Long-term Trends, Radiative Impacts, and Source Attributions

    NASA Astrophysics Data System (ADS)

    Wang, H.; Zhang, R.; Yang, Y.; Smith, S.; Rasch, P. J.

    2017-12-01

    The Arctic has warmed dramatically in recent decades. As one of the important short-lived climate forcers, aerosols affect the Arctic radiative budget directly by interfering radiation and indirectly by modifying clouds. Light-absorbing particles (e.g., black carbon) in snow/ice can reduce the surface albedo. The direct radiative impact of aerosols on the Arctic climate can be either warming or cooling, depending on their composition and location, which can further alter the poleward heat transport. Anthropogenic emissions, especially, BC and SO2, have changed drastically in low/mid-latitude source regions in the past few decades. Arctic surface observations at some locations show that BC and sulfate aerosols had a decreasing trend in the recent decades. In order to understand the impact of long-term emission changes on aerosols and their radiative effects, we use the Community Earth System Model (CESM) equipped with an explicit BC and sulfur source-tagging technique to quantify the source-receptor relationships and decadal trends of Arctic sulfate and BC and to identify variations in their atmospheric transport pathways from lower latitudes. The simulation was conducted for 36 years (1979-2014) with prescribed sea surface temperatures and sea ice concentrations. To minimize potential biases in modeled large-scale circulations, wind fields in the simulation are nudged toward an atmospheric reanalysis dataset, while atmospheric constituents including water vapor, clouds, and aerosols are allowed to evolve according to the model physics. Both anthropogenic and open fire emissions came from the newly released CMIP6 datasets, which show strong regional trends in BC and SO2 emissions during the simulation time period. Results show that emissions from East Asia and South Asia together have the largest contributions to Arctic sulfate and BC concentrations in the upper troposphere, which have an increasing trend. The strong decrease in emissions from Europe, Russia and

  7. Temperature dependence of the formation of sulfate aerosols in the stratosphere

    NASA Technical Reports Server (NTRS)

    Yue, G. K.; Deepak, A.

    1982-01-01

    Classical nucleation theory is used in calculations of the temperature dependence of the characteristics and nucleation rates of sulfate aerosols in the binary H2SO4-H2O vapor mixture, in order to assess the influence of temperature on the formation of sulfate aerosols in the stratosphere, and to explore the possibility of new particle formation through homogeneous nucleation processes at regions where temperature is as low as -75 C, rather than the often-assumed -50 or -55 C. Calculation results indicate that the number of particles formed at a lower temperature is larger by several orders of magnitude than at higher temperatures, when water and sulfuric acid vapor concentrations are kept constant, and that large quantities of ultrafine particles which cannot be detected by conventional methods may exist at low-temperature stratospheric regions.

  8. Evaluation of Sulfate and Organic Aerosol in the Global UTLS: Budget and Size Distribution

    NASA Astrophysics Data System (ADS)

    Yu, P.; Froyd, K. D.; Murphy, D. M.; Jimenez, J. L.; Campuzano Jost, P.; Williamson, C.; Kupc, A.; Brock, C. A.; Liu, S.; Gao, R. S.; Thornberry, T. D.; Portmann, R. W.; Jensen, E. J.; Toon, O. B.; Rosenlof, K. H.

    2017-12-01

    Stratospheric sulfate and organic aerosols account for 20% of the total direct aerosol radiative forcing since 1850 [Yu et al., 2016]. Limited in-situ measurements on aerosol composition have been made in the upper troposphere and lower stratosphere (UTLS), mostly in the Northern Hemispheric mid-latitudes and tropics [Froyd et al., 2009; Murphy et al., 2014; Liao et al., 2015]. Based on those measurements and recent modeling studies [Yu et al., 2015a, 2015b, 2016], organic material commonly contributes half of the aerosol mass in the UTLS in the North Hemisphere. We summarize the global UTLS aerosol mass, size distribution and composition using in-situ measurements over the past 15 years including NASA SEAC4RS in 2013 [Liao et al., 2015; Yu et al., 2015a; Toon et al., 2016], NASA ATom in 2016 and 2017, NASA AVE in 2004 and 2006 [Froyd et al., 2009] and a balloon-borne campaign from Kunming in 2015 [Yu et al., 2017]. The most recent aerosol measurements on sulfate, organics, and their size distributions from the NASA ATom deployments provide a global view of upper tropospheric aerosol composition over remote regions (i.e. the Pacific and Atlantic oceans) in both hemispheres. These in-situ measurements are compared with a sectional aerosol model coupled with the NCAR Community Earth System Model (CESM-CARMA). The comparisons and simulations demonstrate the importance of UTLS aerosols on aerosol-radiation-climate interactions, and highlight the need for a better understanding on the UTLS aerosols' budget, sources, seasonal cycle, transport pathways and linkage to climate change. References:Froyd et al. (2009), Atmospheric Chemistry and Physics, 9(13), 4363-4385. Liao et al. (2016), J. Geophys. Res. Atmos., 120, 2990-3005. Murphy et al. (2014), Q.J.R. Meteorol. Soc., 140: 1269-1278 Toon, O. B. et al. (2016) , J. Geophys. Res. Atmos., 121, 4967-5009 Yu, P. et al. (2015a), J. Adv. Model. Earth Syst., 7, 865-914 Yu, P. et al. (2015b), Geophys. Res. Lett., 42, 2540-2546 Yu

  9. Global Distribution of Solid Ammonium Sulfate Aerosols and their Climate Impact Acting as Ice Nuclei

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Penner, J.

    2017-12-01

    Laboratory experiments show that liquid ammonium sulfate particles effloresce when RHw is below 34% to become solid and dissolve when RHw is above 79%. Solid ammonium sulfate aerosols can act as heterogeneous ice nuclei particles (INPs) to form ice particles in deposition mode when the relative humidity over ice is above 120%. In this study we used the coupled IMPACT/CAM5 model to track the efflorescence and deliquescence processes of ammonium sulfate. Results show that about 20% of the total simulated pure sulfate aerosol mass is in the solid state and is mainly distributed in the northern hemisphere (NH) from 50 hPa to 200 hPa. When these solid ammonium sulfate aerosols are allowed to act as ice nuclei particles, they act to increase the ice water path in the NH and reduce ice water path in the tropics. The addition of these particles leads to a positive net radiative effect at the TOA ranging from 0.5-0.9 W/m2 depending on the amounts of other ice nuclei particles (e.g., dust, soot) used in the ice nucleation process. The short-term climate feedback shows that the ITCZ shifts northwards and precipitation increases in the NH. There is also an average warming of 0.05-0.1 K near the surface (at 2 meter) in the NH which is most obvious in the Arctic region.

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

    EPA Science Inventory

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

  11. 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.

  12. Tales of volcanoes and El-Niño southern oscillations with the oxygen isotope anomaly of sulfate aerosol

    PubMed Central

    Shaheen, Robina; Abauanza, Mariana; Jackson, Teresa L.; McCabe, Justin; Savarino, Joel; Thiemens, Mark H.

    2013-01-01

    The ability of sulfate aerosols to reflect solar radiation and simultaneously act as cloud condensation nuclei renders them central players in the global climate system. The oxidation of S(IV) compounds and their transport as stable S(VI) in the Earth’s system are intricately linked to planetary scale processes, and precise characterization of the overall process requires a detailed understanding of the linkage between climate dynamics and the chemistry leading to the product sulfate. This paper reports a high-resolution, 22-y (1980–2002) record of the oxygen-triple isotopic composition of sulfate (SO4) aerosols retrieved from a snow pit at the South Pole. Observed variation in the O-isotopic anomaly of SO4 aerosol is linked to the ozone variation in the tropical upper troposphere/lower stratosphere via the Ozone El-Niño Southern Oscillations (ENSO) Index (OEI). Higher ∆17O values (3.3‰, 4.5‰, and 4.2‰) were observed during the three largest ENSO events of the past 2 decades. Volcanic events inject significant quantities of SO4 aerosol into the stratosphere, which are known to affect ENSO strength by modulating stratospheric ozone levels (OEI = 6 and ∆17O = 3.3‰, OEI = 11 and ∆17O = 4.5‰) and normal oxidative pathways. Our high-resolution data indicated that ∆17O of sulfate aerosols can record extreme phases of naturally occurring climate cycles, such as ENSOs, which couple variations in the ozone levels in the atmosphere and the hydrosphere via temperature driven changes in relative humidity levels. A longer term, higher resolution oxygen-triple isotope analysis of sulfate aerosols from ice cores, encompassing more ENSO periods, is required to reconstruct paleo-ENSO events and paleotropical ozone variations. PMID:23447567

  13. The paleo-ocean characteristics of the Taklimakan dust aerosol: high sulfate from primary sources and implication for climate modeling

    NASA Astrophysics Data System (ADS)

    Huang, K.; Zhuang, G.; Fu, J. S.; Dong, X.

    2017-12-01

    Multi-year monitoring of dust aerosol from the Taklimakan Desert has been conducted at one site in the hinterland of the desert, Tazhong and another site at the southern edge of the desert, Hotan. Compared to the other two important desert source regions of China, i.e. Gobi and Loess Plateau, the Taklimakan Desert is characterized of high calcium with a Ca/Al elemental ratio of around 1.50. The unique feature of the Taklimakan dust aerosol is its abundant sulfate. For instance, the mean concentration of sulfate over Tazhong reached as high as 34.7 and 48.8 ug/m3 during the spring of 2007 and 2008, respectively. During the dust storm events, the daily concentration of sulfate frequently exceeded 100 ug/m3. Sulfate showed strong correlations with the primary aerosol species such as Ca2+, Mg2+, Na+, Cl-, Al, Fe, Ti, etc. but weakly correlated with the secondary aerosol species such as NO3- and NH4+. The mass ratio of sulfate in the total suspended particles showed a relatively stable percentage of around 2.5% regardless of the intensity of the dust events. In addition, individual particle analysis using the scanning electron microscope (SEM) technique found that gypsum (CaSO4) particles could account for 11.1% of total number of particles as well as abundant Na2SO4 and NaCl particles. All the evidences above suggested the high sulfate observed in the Taklimakan Desert were largely attributed to primary sources but not formed via the traditional gas-to-particle formation pathway. As the Taklimakan Desert was speculated to be ocean 5-7 million years, the dried sea salts from the paleo-ocean should be the major source of the dust aerosol. Also, the dried salt lakes in the northwestern China may contribute to the high sulfate. Based on two different methods, the contribution of primary sources to sulfate over the Taklimakan Desert is estimated to be around 43% - 82%. This study implied that the cooling effect of the Taklimakan dust aerosol could be underestimated if the

  14. Heterogenous uptake of gaseous N(sub 2)O(sub 5) by sulfate aerosols

    NASA Technical Reports Server (NTRS)

    Leu, M. -T.; Kane, S. M.; Caloz, F.

    2001-01-01

    The heterogeneous uptake of gaseous N sub 2 O sub 5 by ammonium sulfate, ammonium bisulfate, and sulfuric acid aerosols as a function of relative humididty has been investigated at room temperature and atmsopheric pressure.

  15. Importance of Anthropogenic Aerosols for Climate Prediction: a Study on East Asian Sulfate Aerosols

    NASA Astrophysics Data System (ADS)

    Bartlett, R. E.; Bollasina, M. A.

    2017-12-01

    Climate prediction is vital to ensure that we are able to adapt to our changing climate. Understandably, the main focus for such prediction is greenhouse gas forcing, as this will be the main anthropogenic driver of long-term global climate change; however, other forcings could still be important. Atmospheric aerosols represent one such forcing, especially in regions with high present-day aerosol loading such as Asia; yet, uncertainty in their future emissions are under-sampled by commonly used climate forcing projections, such as the Representative Concentration Pathways (RCPs). Globally, anthropogenic aerosols exert a net cooling, but their effects show large variation at regional scales. Studies have shown that aerosols impact locally upon temperature, precipitation and hydroclimate, and also upon larger scale atmospheric circulation (for example, the Asian monsoon) with implications for climate remote from aerosol sources. We investigate how future climate could evolve differently given the same greenhouse gas forcing pathway but differing aerosol emissions. Specifically, we use climate modelling experiments (using HadGEM2-ES) of two scenarios based upon RCP2.6 greenhouse gas forcing but with large differences in sulfur dioxide emissions over East Asia. Results show that increased sulfate aerosols (associated with increased sulfur dioxide) lead to large regional cooling through aerosol-radiation and aerosol-cloud interactions. Focussing on dynamical mechanisms, we explore the consequences of this cooling for the Asian summer and winter monsoons. In addition to local temperature and precipitation changes, we find significant changes to large scale atmospheric circulation. Wave-like responses to upper-level atmospheric changes propagate across the northern hemisphere with far-reaching effects on surface climate, for example, cooling over Europe. Within the tropics, we find alterations to zonal circulation (notably, shifts in the Pacific Walker cell) and monsoon

  16. Radiative and Chemical Response to Interactive Stratospheric Sulfate Aerosols in Fully Coupled CESM1(WACCM): Stratospheric Aerosols in CESM1(WACCM)

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

    Mills, Michael J.; Richter, Jadwiga H.; Tilmes, Simone

    We present a new version of the Community Earth System Model, version 1 (CESM1) with the Whole Atmosphere Community Climate Model (WACCM) featuring numerous improvements that are unique among earth system models. Improved horizontal resolution, dynamics, and chemistry now provide the development of an internally generated quasi-biennial oscillation, and significant improvements to temperatures and ozone throughout the stratosphere. The prognostic treatment of stratospheric sulfate aerosols is shown to represent well the evolution of stratospheric aerosol optical depth and perturbations to solar and longwave radiation following volcanic eruptions. We identify the inclusion of interactive OH chemistry as crucial to the studymore » of aerosol formation following large inputs of SO2 to the stratosphere. We show that depletion of OH levels within the dense SO2 cloud in the first weeks following the June 1991 eruption of Mt. Pinatubo significantly prolonged the e-folding decay time for SO2 oxidation to 47 days. Previous observational and model studies showing a 30-day decay time have not accounted for the large initial losses of SO2 on ash and ice in the first 7-9 days following the eruption, and have not correctly accounted for OH depletion. The completeness of the chemistry, dynamics, and aerosol microphysics in WACCM uniquely qualify it for studies of stratospheric sulfate aerosol geoengineering.« less

  17. Direct comparison of the hygroscopic properties of ammonium sulfate and sodium chloride aerosol at relative humidities approaching saturation.

    PubMed

    Walker, Jim S; Wills, Jon B; Reid, Jonathan P; Wang, Liangyu; Topping, David O; Butler, Jason R; Zhang, Yun-Hong

    2010-12-09

    Holographic optical tweezers are used to make comparative measurements of the hygroscopic properties of single component aqueous aerosol containing sodium chloride and ammonium sulfate over a range of relative humidity from 84% to 96%. The change in RH over the course of the experiment is monitored precisely using a sodium chloride probe droplet with accuracy better than ±0.09%. The measurements are used to assess the accuracy of thermodynamic treatments of the relationship between water activity and solute mass fraction with particular attention focused on the dilute solute limit approaching saturation vapor pressure. The consistency of the frequently used Clegg-Brimblecombe-Wexler (CBW) treatment for predicting the hygroscopic properties of sodium chloride and ammonium sulfate aerosol is confirmed. Measurements of the equilibrium size of ammonium sulfate aerosol are found to agree with predictions to within an uncertainty of ±0.2%. Given the accuracy of treating equilibrium composition, the inconsistencies highlighted in recent calibration measurements of critical supersaturations of sodium chloride and ammonium sulfate aerosol cannot be attributed to uncertainties associated with the thermodynamic predictions and must have an alternative origin. It is concluded that the CBW treatment can allow the critical supersaturation to be estimated for sodium chloride and ammonium sulfate aerosol with an accuracy of better than ±0.002% in RH. This corresponds to an uncertainty of ≤1% in the critical supersaturation for typical supersaturations of 0.2% and above. This supports the view that these systems can be used to accurately calibrate instruments that measure cloud condensation nuclei concentrations at selected supersaturations. These measurements represent the first study in which the equilibrium properties of two particles of chemically distinct composition have been compared simultaneously and directly alongside each other in the same environment.

  18. Interactive coupling of regional climate and sulfate aerosol models over eastern Asia

    NASA Astrophysics Data System (ADS)

    Qian, Yun; Giorgi, Filippo

    1999-03-01

    The NCAR regional climate model (RegCM) is interactively coupled to a simple radiatively active sulfate aerosol model over eastern Asia. Both direct and indirect aerosol effects are represented. The coupled model system is tested for two simulation periods, November 1994 and July 1995, with aerosol sources representative of present-day anthropogenic sulfur emissions. The model sensitivity to the intensity of the aerosol source is also studied. The main conclusions from our work are as follows: (1) The aerosol distribution and cycling processes show substantial regional spatial variability, and temporal variability varying on a range of scales, from the diurnal scale of boundary layer and cumulus cloud evolution to the 3-10 day scale of synoptic scale events and the interseasonal scale of general circulation features; (2) both direct and indirect aerosol forcings have regional effects on surface climate; (3) the regional climate response to the aerosol forcing is highly nonlinear, especially during the summer, due to the interactions with cloud and precipitation processes; (4) in our simulations the role of the aerosol indirect effects is dominant over that of direct effects; (5) aerosol-induced feedback processes can affect the aerosol burdens at the subregional scale. This work constitutes the first step in a long term research project aimed at coupling a hierarchy of chemistry/aerosol models to the RegCM over the eastern Asia region.

  19. Endotracheal aerosolization of atropine sulfate protects against soman-induced acute respiratory toxicity in guinea pigs.

    PubMed

    Perkins, Michael W; Pierre, Zdenka; Rezk, Peter; Song, Jian; Marshall, Seema; Oguntayo, Samuel; Morthole, Venee; Sciuto, Alfred M; Doctor, Bhupendra P; Nambiar, Madhusoodana P

    2011-03-01

    The efficacy of endotracheal aerosolization of atropine sulfate for protection against soman (GD)-induced respiratory toxicity was investigated using microinstillation technique in guinea pigs. GD (841 mg/m(3), 1.3 LCt(50) or 1121 mg/m(3), 1.7 LCt(50)) was aerosolized endotracheally to anesthetized male guinea pigs that were treated with atropine sulfate (5.0 mg/kg) 30 s postexposure by endotracheal microinstillation. Animals exposed to 841 mg/m(3) and 1121 mg/m(3)GD resulted in 31 and 13% while treatment with atropine sulfate resulted in 100 and 50% survival, respectively. Cholinergic symptoms and increased body weight loss were reduced in atropine-treated animals compared to GD controls. Diminished pulse rate and blood O(2) saturation in GD-exposed animals returned to normal levels after atropine treatment. Increased cell death, total cell count and protein in the bronchoalveolar fluid (BALF) in GD-exposed animals returned to normal levels following atropine treatment. GD exposure increased glutathione and superoxide dismutase levels in BALF and that were reduced in animals treated with atropine. Respiratory parameters measured by whole-body barometric plethysmography revealed that treatment with atropine sulfate resulted in normalization of respiratory frequency, tidal volume, time of expiration, time of inspiration, end expiratory pause, pseudo lung resistance (Penh) and pause at 4 and 24 h post 841 mg/m(3) GD exposure. Lung histopathology showed that atropine treatment reduced bronchial epithelial subepithelial inflammation and multifocal alveolar septal edema. These results suggest that endotracheal aerosolization of atropine sulfate protects against respiratory toxicity and lung injury induced by microinstillation inhalation exposure to lethal doses of GD.

  20. Radiative and Chemical Response to Interactive Stratospheric Sulfate Aerosols in Fully Coupled CESM1(WACCM)

    NASA Astrophysics Data System (ADS)

    Mills, Michael J.; Richter, Jadwiga H.; Tilmes, Simone; Kravitz, Ben; MacMartin, Douglas G.; Glanville, Anne A.; Tribbia, Joseph J.; Lamarque, Jean-François; Vitt, Francis; Schmidt, Anja; Gettelman, Andrew; Hannay, Cecile; Bacmeister, Julio T.; Kinnison, Douglas E.

    2017-12-01

    We present new insights into the evolution and interactions of stratospheric aerosol using an updated version of the Whole Atmosphere Community Climate Model (WACCM). Improved horizontal resolution, dynamics, and chemistry now produce an internally generated quasi-biennial oscillation and significant improvements to stratospheric temperatures and ozone compared to observations. We present a validation of WACCM column ozone and climate calculations against observations. The prognostic treatment of stratospheric sulfate aerosols accurately represents the evolution of stratospheric aerosol optical depth and perturbations to solar and longwave radiation following the June 1991 eruption of Mount Pinatubo. We confirm the inclusion of interactive OH chemistry as an important factor in the formation and initial distribution of aerosol following large inputs of sulfur dioxide (SO2) to the stratosphere. We calculate that depletion of OH levels within the dense SO2 cloud in the first weeks following the Pinatubo eruption significantly prolonged the average initial e-folding decay time for SO2 oxidation to 47 days. Previous observational and model studies showing a 30 day decay time have not accounted for the large (30-55%) losses of SO2 on ash and ice within 7-9 days posteruption and have not correctly accounted for OH depletion. We examine the variability of aerosol evolution in free-running climate simulations due to meteorology, with comparison to simulations nudged with specified dynamics. We assess calculated impacts of volcanic aerosols on ozone loss with comparisons to observations. The completeness of the chemistry, dynamics, and aerosol microphysics in WACCM qualify it for studies of stratospheric sulfate aerosol geoengineering.

  1. Arrival of Sulfate Aerosols from Iceland's Laki Eruption (1783-1784 AD) to the Greenland Ice Sheet: A Critical Ice Core Dating Tool

    NASA Astrophysics Data System (ADS)

    Wei, L.; Mosley-Thompson, E.

    2006-12-01

    The Laki (Iceland) volcanic event was a basaltic flood lava eruption lasting from June 8, 1783 to February 7, 1784. The timing of the arrival of the sulfate aerosols and volcanic fragments to the Greenland Ice Sheet (GIS) remains uncertain, but is important to confirm as the highly conductive sulfate layer has been consistently used as a time stratigraphic marker (1783 AD) in ice cores collected across Greenland. However, in the GISP2 ice core a few glass shards were found within the annual layer lying just below that containing the sulfate aerosols from Laki suggesting that the ash arrived first, in 1783, while the aerosols arrived the following year [Fiacco et al., 1994]. Additional published ice core results have neither confirmed nor refuted this observation. We have taken advantage of the accurately dated, high temporal resolution ice cores collected by PARCA (Program for Arctic Regional Climate Assessment) to (1) determine more precisely the timing of the arrival of Laki's sulfate aerosols and (2) assess the spatial variability of the excess sulfate contributed by Laki to the GIS. Our results indicate that the sulfate emitted from the Laki eruption most likely arrived on the GIS in the late summer or early fall of 1783 AD. This is also supported by contemporary weather logs and official reports of the appearance of Laki haze [Thordarson and Self, 2003]. The flux of Laki sulfate varies significantly over the GIS, largely as a function of the regional annual accumulation rate. Laki sulfate aerosols also arrived as a single pulse in most of the PARCA cores, suggesting that only a small fraction of the gases emitted from Laki reached the stratosphere. References: Fiacco, R.J.,et al., Atmospheric aerosol loading and transport due to the 1783-84 Laki eruption in Iceland, interpreted from ash particles and acidity in the GISP2 ice core, Quat. Res., 42, 231-240, 1994. Thordarson, T, and S. Self, Atmospheric and environmental effects of the 1783-1784 Laki eruption: A

  2. Investigating the influence of volcanic sulfate aerosol on cloud properties Along A-Train tracks

    NASA Astrophysics Data System (ADS)

    Mace, G. G.

    2017-12-01

    Marine boundary layer (MBL) clouds are central actors in the climate system given their extensive coverage on the Earth's surface, their 1-way influence on the radiative balance (cooling), and their intimate coupling between air motions, anthropogenic and natural aerosol sources, and processes within the upper ocean mixed layer. Knowledge of how MBL shallow cumulus clouds respond to changes in aerosol is central to understanding how MBL clouds modulate the climate system. A frequent approach to investigating how sulfate aerosol influences MBL clouds has been to examine sulfate plumes extending downstream of active island volcanoes. This approach is challenging due to modification of the air motions in the plumes downstream of islands and due to the tendency of most researchers to examine only level-2 retrievals ignoring the actual data collected by sensors such as MODIS. Past studies have concluded that sulfate aerosols have large effects consistent with the 1st aerosol indirect effect (AIE). We reason that if such effects are as large as suggested in level-2 retrievals then evidence should also be present in the raw MODIS reflectance data as well as other data sources. In this paper we will build on our recently published work where we tested that hypothesis from data collected near Mount Kilauea during a 3-year period. Separating data into aerosol optical depth (A) quartiles, we found little support for a large 1st AIE response. We did find an unambiguous increase in sub 1km-scale cloud fraction with A. This increase in sub 1 km cloud fraction was entirely consistent with increased reflectance with increasing A that is used, via the level 2 retrievals, to argue for a large AIE response of MBL clouds. While the 1-km pixels became unambiguously brighter, that brightening was due to increased sub 1 km cloud fraction and not necessarily due to changes in pixel-level cloud microphysics. We also found that MBL cloud top heights increase as do surface wind speeds as

  3. Physiochemical properties of alkylaminium sulfates: hygroscopicity, thermostability, and density.

    PubMed

    Qiu, Chong; Zhang, Renyi

    2012-04-17

    Although heterogeneous interaction of amines has been recently shown to play an important role in the formation and growth of atmospheric aerosols, little information is available on the physicochemical properties of aminium sulfates. In this study, the hygroscopicity, thermostability, and density of alkylaminium sulfates (AASs) have been measured by an integrated aerosol analytical system including a tandem differential mobility analyzer and an aerosol particle mass analyzer. AAS aerosols exhibit monotonic size growth at increasing RH without a well-defined deliquescence point. Mixing of ammonium sulfate (AS) with AASs lowers the deliquescence point corresponding to AS. Particles with AASs show comparable or higher thermostability than that of AS. The density of AASs is determined to be 1.2-1.5 g cm(-3), and an empirical model is developed to predict the density of AASs on the basis of the mole ratio of alkyl carbons to total sulfate. Our results reveal that the heterogeneous uptake of amines on sulfate particles may considerably alter the aerosol properties. In particular, the displacement reaction of alkylamines with ammonium sulfate aerosols leads to a transition from the crystalline to an amorphorous phase and an improved water uptake, considerably enhancing their direct and indirect climate forcing.

  4. Radiative and Chemical Response to Interactive Stratospheric Sulfate Aerosols in Fully Coupled CESM1(WACCM)

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

    Mills, Mike; Richter, Jadwiga; Tilmes, S.

    2017-11-06

    We present a new version of the Community Earth System Model, version 1 (CESM1) with the Whole Atmosphere Community Climate Model (WACCM) featuring numerous improvements that are unique among earth system models. Improved horizontal resolution, dynamics, and chemistry now provide the development of an internally generated quasi-biennial oscillation, and significant improvements to temperatures and ozone throughout the stratosphere. The prognostic treatment of stratospheric sulfate aerosols is shown to represent well the evolution of stratospheric aerosol optical depth and perturbations to solar and longwave radiation following volcanic eruptions. We identify the inclusion of interactive OH chemistry as crucial to the studymore » of aerosol formation following large inputs of SO2 to the stratosphere. We show that depletion of OH levels within the dense SO2 cloud in the first weeks following the June 1991 eruption of Mt. Pinatubo significantly prolonged the e-folding decay time for SO2 oxidation to 47 days. Previous observational and model studies showing a 30-day decay time have not accounted for the large initial losses of SO2 on ash and ice in the first 7-9 days following the eruption, and have not correctly accounted for OH depletion. The completeness of the chemistry, dynamics, and aerosol microphysics in WACCM uniquely qualify it for studies of stratospheric sulfate aerosol geoengineering.« less

  5. Absorption and scattering properties of organic carbon vs. sulfate dominant aerosols at Gosan climate observatory in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Lim, S.; Lee, M.; Kim, S.-W.; Yoon, S.-C.; Lee, G.; Lee, Y.

    2013-12-01

    Carbonaceous and soluble ionic species of PM1.0 and PM10 were measured along with the absorption and scattering properties and aerosol number size distributions at Gosan climate observatory (GCO) from January to September 2008. The daily averaged equivalent black carbon (EBC) measured as aerosol absorption exhibited two types of spectral dependence with a distinct maximum (peak) at either 370 nm or 880 nm, by which two subsets were extracted and classified into the respective groups (370 nm and 880 nm). The 370 nm group was distinguished by high organic carbon (OC) concentrations relative to elemental carbon (EC) and sulfate, but sulfate was predominant for the 880 nm group. The PM1.0 OC of the 370 nm group was mainly composed of refractory and pyrolized components that correlated well with PM1.0 EC1, referred to as char EC, which suggests biofuel and biomass combustion as the source of these OC fractions, particularly during winter. The scanning electron microscope (SEM) images and the number size distributions implied that aerosols of the 370 nm group were externally mixed upon transport in fast-moving air masses that passed through the Beijing area in about one day. In contrast, the aerosols of the 880 nm group were characterized by high sulfate concentrations, and seemed to be internally mixed during slow transport over the Yellow Sea region over approximately two to four days. The absorption and scattering coefficients of the 880 nm group were noticeably higher compared to those of the 370 nm group. The average absorption ångström exponent (AAE) was estimated to be 1.29 and 1.0 for the 370 nm and 880 nm groups, respectively, in the range 370-950 nm. These results demonstrated that the optical properties of aerosols were intimately linked to chemical composition and mixing state, characteristics determined both by source and atmospheric aging processes. In OC dominant aerosols, absorption was enhanced in the UV region, which was possibly due to refractory and

  6. Absorption and scattering properties of organic carbon versus sulfate dominant aerosols at Gosan climate observatory in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Lim, S.; Lee, M.; Kim, S.-W.; Yoon, S.-C.; Lee, G.; Lee, Y. J.

    2014-08-01

    Carbonaceous and soluble ionic species of PM1.0 and PM10 were measured along with the absorption and scattering properties and aerosol number size distributions at Gosan Climate Observatory (GCO) from January to September 2008. The daily averaged equivalent black carbon (EBC) measured as aerosol absorption exhibited two types of spectral dependence with a distinct maximum (peak) at either 370 nm or 880 nm, by which two subsets were extracted and classified into the respective groups (370 and 880 nm). The 370 nm group was distinguished by high organic carbon (OC) concentrations relative to elemental carbon (EC) and sulfate, but sulfate was predominant for the 880 nm group. The PM1.0 OC of the 370 nm group was mainly composed of refractory and pyrolized components that correlated well with PM1.0 EC1, referred to as char EC, which suggests biofuel and biomass combustion as the source of these OC fractions, particularly during winter. The scanning electron microscope (SEM) images and the number size distributions implied that aerosols of the 370 nm group were externally mixed upon transport in fast-moving air masses that passed through the Beijing area in about one day. In contrast, the aerosols of the 880 nm group were characterized by high sulfate concentrations, and seemed to be internally mixed during slow transport over the Yellow Sea region over approximately 2 to 4 days. The absorption and scattering coefficients of the 880 nm group were noticeably higher compared to those of the 370 nm group. The average absorption ångström exponent (AAE) was estimated to be 1.29 and 1.0 for the 370 and 880 nm groups, respectively, in the range 370-950 nm. These results demonstrated that the optical properties of aerosols were intimately linked to chemical composition and mixing state, characteristics determined both by source and atmospheric aging processes. In OC dominant aerosols, absorption was enhanced in the UV region, which was possibly due to refractory and pyrolized

  7. Effects of ammonium sulfate aerosols on vegetation—II. Mode of entry and responses of vegetation

    NASA Astrophysics Data System (ADS)

    Gmur, Nicholas F.; Evans, Lance S.; Cunningham, Elizabeth A.

    These experiments were designed to provide information on the rates of aerosol deposition, mode of entry, and effects of deposition of submicrometer ammonium sulfate aerosols on foliage of Phaseolus vulgaris L. A deposition velocity of 3.2 × 10 3cms-1 was constant during 3-week exposures of plants to aerosol concentrations of 26mg m -3 (i.e. about two orders of magnitude above ambient episode concentrations). Mean deposition rate on foliage was 4.1 × 10 -11 μg cm -2s -1. Visible injury symptoms included leaf chlorosis, necrosis and loss of turgor. Chlorosis was most frequent near leaf margins causing epinasty and near major veins. Internal injury occurred initially in spongy mesophyll cells. Eventually abaxial epidermal and palisade parenchyma cells were injured. These results suggest that submicrometer aerosols enter abaxial stomata and affect more internal cells before affecting leaf surface cells. Exposure to aerosols decreased both abaxial and adaxial leaf resistances markedly. Although visible injury to foliage occurred, no changes in dry mass of roots and shoots or leaf area occurred. These results suggest that for the plant developmental stage studied, while leaf resistances decreased and cellular injury occurred in foliage, these factors were not significantly related to plant growth and development.

  8. Evaluations of tropospheric aerosol properties simulated by the community earth system model with a sectional aerosol microphysics scheme

    PubMed Central

    Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.

    2015-01-01

    Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data. PMID:27668039

  9. Assessment of the first indirect radiative effect of ammonium-sulfate-nitrate aerosols in East Asia

    NASA Astrophysics Data System (ADS)

    Han, Xiao; Zhang, Meigen; Skorokhod, Andrei

    2017-11-01

    A physically based cloud nucleation parameterization was introduced into an optical properties/radiative transfer module incorporated with the off-line air quality modeling system Regional Atmospheric Modeling System (RAMS)-Models-3 Community Multi Scale Air Quality (CMAQ) to investigate the distribution features of the first indirect radiative effects of sulfate, nitrate, and ammonium-sulfate-nitrate (ASN) over East Asia for the years of 2005, 2010, and 2013. The relationship between aerosol particles and cloud droplet number concentration could be properly described by this parameterization because the simulated cloud fraction and cloud liquid water path were generally reliable compared with Moderate Resolution Imaging Spectroradiometer (MODIS) retrieved data. Simulation results showed that the strong effect of indirect forcing was mainly concentrated in Southeast China, the East China Sea, the Yellow Sea, and the Sea of Japan. The highest indirect radiative forcing of ASN reached -3.47 W m-2 over Southeast China and was obviously larger than the global mean of the indirect forcing of all anthropogenic aerosols. In addition, sulfate provided about half of the contribution to the ASN indirect forcing effect. However, the effect caused by nitrate was weak because the mass burden of nitrate was very low during summer, whereas the cloud fraction was the highest. The analysis indicated that even though the interannual variation of indirect forcing magnitude generally followed the trend of aerosol mass burden from 2005 to 2013, the cloud fraction was an important factor that determined the distribution pattern of indirect forcing. The heaviest aerosol loading in North China did not cause a strong radiative effect because of the low cloud fraction over this region.

  10. Simulation of nitrate, sulfate, and ammonium aerosols over the United States

    NASA Astrophysics Data System (ADS)

    Walker, J. M.; Philip, S.; Martin, R. V.; Seinfeld, J. H.

    2012-11-01

    Atmospheric concentrations of inorganic gases and aerosols (nitrate, sulfate, and ammonium) are simulated for 2009 over the United States using the chemical transport model GEOS-Chem. Predicted aerosol concentrations are compared with surface-level measurement data from the Interagency Monitoring of Protected Visual Environments (IMPROVE), the Clean Air Status and Trends Network (CASTNET), and the California Air Resources Board (CARB). Sulfate predictions nationwide are in reasonably good agreement with observations, while nitrate and ammonium are over-predicted in the East and Midwest, but under-predicted in California, where observed concentrations are the highest in the country. Over-prediction of nitrate in the East and Midwest is consistent with results of recent studies, which suggest that nighttime nitric acid formation by heterogeneous hydrolysis of N2O5 is over-predicted based on current values of the N2O5 uptake coefficient, γ, onto aerosols. After reducing the value of γ by a factor of 10, predicted nitrate levels in the US Midwest and East still remain higher than those measured, and over-prediction of nitrate in this region remains unexplained. Comparison of model predictions with satellite measurements of ammonia from the Tropospheric Emissions Spectrometer (TES) indicates that ammonia emissions in GEOS-Chem are underestimated in California and that the nationwide seasonality applied to ammonia emissions in GEOS-Chem does not represent California very well, particularly underestimating winter emissions. An ammonia sensitivity study indicates that GEOS-Chem simulation of nitrate is ammonia-limited in southern California and much of the state, suggesting that an underestimate of ammonia emissions is likely the main cause for the under-prediction of nitrate aerosol in many areas of California. An approximate doubling of ammonia emissions is needed to reproduce observed nitrate concentrations in southern California and in other ammonia sensitive areas

  11. 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).

  12. Optical constants of ammonium sulfate in the infrared. [stratospheric aerosol refractive and absorption indices

    NASA Technical Reports Server (NTRS)

    Downing, H. D.; Pinkley, L. W.; Sethna, P. P.; Williams, D.

    1977-01-01

    The infrared spectral reflectance at near normal incidence has been measured for 3.2 M, 2.4 M, and 1.6 M solutions of ammonium sulfate, an aerosol abundant in the stratosphere and also present in the troposphere. Kramers-Kronig analysis was used to determine values of the refractive and absorption indices from the measured spectral reflectance. A synthetic spectrum of crystalline ammonium sulfate was obtained by extrapolation of the absorption index obtained for the solution to the absorber number densities of the NH4 and SO4 ions characteristic of the crystal.

  13. Crystallization pathways of sulfate-nitrate-ammonium aerosol particles.

    PubMed

    Schlenker, Julie C; Martin, Scot T

    2005-11-10

    Crystallization experiments are conducted for aerosol particles composed of aqueous mixtures of (NH(4))(2)SO(4)(aq) and NH(4)NO(3)(aq), (NH(4))(2)SO(4)(aq) and NH(4)HSO(4)(aq), and NH(4)NO(3)(aq) and NH(4)HSO(4)(aq). Depending on the aqueous composition, crystals of (NH(4))(2)SO(4)(s), (NH(4))(3)H(SO(4))(2)(s), NH(4)HSO(4)(s), NH(4)NO(3)(s), 2NH(4)NO(3) x (NH(4))(2)SO(4)(s), and 3NH(4)NO(3) x (NH(4))(2)SO(4)(s) are formed. Although particles of NH(4)NO(3)(aq) and NH(4)HSO(4)(aq) do not crystallize even at 1% relative humidity, additions of 0.05 mol fraction SO(4)(2-)(aq) or NO(3)(-)(aq) ions promote crystallization, respectively. 2NH(4)NO(3) x (NH(4))(2)SO(4)(s) and (NH(4))(3)H(SO(4))(2)(s) appear to serve as good heterogeneous nuclei for NH(4)NO(3)(s) and NH(4)HSO(4)(s), respectively. 2NH(4)NO(3) x (NH(4))(2)SO(4)(s) crystallizes over a greater range of aqueous compositions than 3NH(4)NO(3) x (NH(4))(2)SO(4)(s). An infrared aerosol spectrum is provided for each solid based upon a linear decomposition analysis of the recorded spectra. Small nonzero residuals occur in the analysis because aerosol spectra depend on particle morphology, which changes slightly across the range of compositions studied. In addition, several of the mixed compositions crystallize with residual aqueous water of up to 5% particle mass. We attribute this water content to enclosed water pockets. The results provide further insights into the nonlinear crystallization pathways of sulfate-nitrate-ammonium aerosol particles.

  14. Aerosolized delivery of oxime MMB-4 in combination with atropine sulfate protects against soman exposure in guinea pigs.

    PubMed

    Perkins, Michael W; Pierre, Zdenka; Sabnekar, Praveena; Sciuto, Alfred M; Song, Jian; Soojhawon, Iswarduth; Oguntayo, Samuel; Doctor, Bhupendra P; Nambiar, Madhusoodana P

    2012-08-01

    We evaluated the efficacy of aerosolized acetylcholinesterase (AChE) reactivator oxime MMB-4 in combination with the anticholinergic atropine sulfate for protection against respiratory toxicity and lung injury following microinstillation inhalation exposure to nerve agent soman (GD) in guinea pigs. Anesthetized animals were exposed to GD (841 mg/m(3), 1.2 LCt(50)) and treated with endotracheally aerosolized MMB-4 (50 µmol/kg) plus atropine sulfate (0.25 mg/kg) at 30 sec post-exposure. Treatment with MMB-4 plus atropine increased survival to 100% compared to 38% in animals exposed to GD. Decreases in the pulse rate and blood O(2) saturation following exposure to GD returned to normal levels in the treatment group. The body-weight loss and lung edema was significantly reduced in the treatment group. Similarly, bronchoalveolar cell death was significantly reduced in the treatment group while GD-induced increase in total cell count was decreased consistently but was not significant. GD-induced increase in bronchoalveolar protein was diminished after treatment with MMB-4 plus atropine. Bronchoalveolar lavage AChE and BChE activity were significantly increased in animals treated with MMB-4 plus atropine at 24 h. Lung and diaphragm tissue also showed a significant increase in AChE activity in the treatment group. Treatment with MMB-4 plus atropine sulfate normalized various respiratory dynamics parameters including respiratory frequency, tidal volume, peak inspiratory and expiratory flow, time of inspiration and expiration, enhanced pause and pause post-exposure to GD. Collectively, these results suggest that aerosolization of MMB-4 plus atropine increased survival, decreased respiratory toxicity and lung injury following GD inhalation exposure.

  15. pH of Aerosols in a Polluted Atmosphere: Source Contributions to Highly Acidic Aerosol.

    PubMed

    Shi, Guoliang; Xu, Jiao; Peng, Xing; Xiao, Zhimei; Chen, Kui; Tian, Yingze; Guan, Xinbei; Feng, Yinchang; Yu, Haofei; Nenes, Athanasios; Russell, Armistead G

    2017-04-18

    Acidity (pH) plays a key role in the physical and chemical behavior of PM 2.5 . However, understanding of how specific PM sources impact aerosol pH is rarely considered. Performing source apportionment of PM 2.5 allows a unique link of sources pH of aerosol from the polluted city. Hourly water-soluble (WS) ions of PM 2.5 were measured online from December 25th, 2014 to June 19th, 2015 in a northern city in China. Five sources were resolved including secondary nitrate (41%), secondary sulfate (26%), coal combustion (14%), mineral dust (11%), and vehicle exhaust (9%). The influence of source contributions to pH was estimated by ISORROPIA-II. The lowest aerosol pH levels were found at low WS-ion levels and then increased with increasing total ion levels, until high ion levels occur, at which point the aerosol becomes more acidic as both sulfate and nitrate increase. Ammonium levels increased nearly linearly with sulfate and nitrate until approximately 20 μg m -3 , supporting that the ammonium in the aerosol was more limited by thermodynamics than source limitations, and aerosol pH responded more to the contributions of sources such as dust than levels of sulfate. Commonly used pH indicator ratios were not indicative of the pH estimated using the thermodynamic model.

  16. Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

    NASA Technical Reports Server (NTRS)

    Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Dickerson, R. R.; Thompson, A. M.; Slutsker, I.; Li, Z.; Tripathi, S. N.; Singh, R. P.; hide

    2010-01-01

    Aerosols are generated in the atmosphere through anthropogenic and natural mechanisms. These sources have signatures in the aerosol optical and microphysical properties that can be used to identify the aerosol type/mixture. Spectral aerosol absorption information (absorption Angstrom exponent; AAE) used in conjunction with the particle size parameterization (extinction Angstrom exponent; EAE) can only identify the dominant absorbing aerosol type in the sample volume (e.g., black carbon vs. iron oxides in dust). This AAE/EAE relationship can be expanded to also identify non-absorbing aerosol types/mixtures by applying an absorption weighting. This new relationship provides improved aerosol type distinction when the magnitude of absorption is not equal (e.g, black carbon vs. sulfates). The Aerosol Robotic Network (AERONET) data provide spectral aerosol optical depth and single scattering albedo - key parameters used to determine EAE and AAE. The proposed aerosol type/mixture relationship is demonstrated using the long-term data archive acquired at AERONET sites within various source regions. The preliminary analysis has found that dust, sulfate, organic carbon, and black carbon aerosol types/mixtures can be determined from this AAE/EAE relationship when applying the absorption weighting for each available wavelength (Le., 440, 675, 870nm). Large, non-spherical dust particles absorb in the shorter wavelengths and the application of 440nm wavelength absorption weighting produced the best particle type definition. Sulfate particles scatter light efficiently and organic carbon particles are small near the source and aggregate over time to form larger less absorbing particles. Both sulfates and organic carbon showed generally better definition using the 870nm wavelength absorption weighting. Black carbon generation results from varying combustion rates from a number of sources including industrial processes and biomass burning. Cases with primarily black carbon showed

  17. 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

  18. An aerosol climatology for a rapidly growing arid region (southern Arizona): Major aerosol species and remotely sensed aerosol properties

    NASA Astrophysics Data System (ADS)

    Sorooshian, Armin; Wonaschütz, Anna; Jarjour, Elias G.; Hashimoto, Bryce I.; Schichtel, Bret A.; Betterton, Eric A.

    2011-10-01

    This study reports a comprehensive characterization of atmospheric aerosol particle properties in relation to meteorological and back trajectory data in the southern Arizona region, which includes two of the fastest growing metropolitan areas in the United States (Phoenix and Tucson). Multiple data sets (MODIS, AERONET, OMI/TOMS, MISR, GOCART, ground-based aerosol measurements) are used to examine monthly trends in aerosol composition, aerosol optical depth (AOD), and aerosol size. Fine soil, sulfate, and organics dominate PM2.5 mass in the region. Dust strongly influences the region between March and July owing to the dry and hot meteorological conditions and back trajectory patterns. Because monsoon precipitation begins typically in July, dust levels decrease, while AOD, sulfate, and organic aerosol reach their maximum levels because of summertime photochemistry and monsoon moisture. Evidence points to biogenic volatile organic compounds being a significant source of secondary organic aerosol in this region. Biomass burning also is shown to be a major contributor to the carbonaceous aerosol budget in the region, leading to enhanced organic and elemental carbon levels aloft at a sky-island site north of Tucson (Mt. Lemmon). Phoenix exhibits different monthly trends for aerosol components in comparison with the other sites owing to the strong influence of fossil carbon and anthropogenic dust. Trend analyses between 1988 and 2009 indicate that the strongest statistically significant trends are reductions in sulfate, elemental carbon, and organic carbon, and increases in fine soil during the spring (March-May) at select sites. These results can be explained by population growth, land-use changes, and improved source controls.

  19. 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.

  20. Model intra-comparison of transboundary sulfate loadings over springtime east Asia

    NASA Astrophysics Data System (ADS)

    Goto, D.; Ohara, T.; Nakajima, T.; Takemura, T.; Kajino, M.; Dai, T.; Matsui, H.; Takami, A.; Hatakeyama, S.; Aoki, K.; Sugimoto, N.; Shimizu, A.

    2013-12-01

    Over east Asia, a spatial gradient of sulfate aerosols from source to outflow regions has not fully evaluated by simulations. In the present study, we executed a global aerosol-transport model (SPRINTARS) during April 2006 to investigate the spatial gradient of sulfate aerosols using multiple measurements including surface mass concentration, aerosol optical thickness, and vertical profiles of extinction coefficients for spherical particles. We also performed sensitivity experiments to estimate possible uncertainties of sulfate mass loadings caused by macrophysical processes; emission inventory, dynamic core, and spatial resolution. Among the experiments, although a difference in the surface sulfate mass concentrations over east Asia was large, none of the simulations in the present study as well as regional models reproduced the spatial gradient of the surface sulfate from the source over China to the outflow regions in Japan. The sensitivity of different macrophysical factors to the surface sulfate differs from that to sulfate loadings in the column especially in the marine boundary layers (MBL). Therefore, to properly simulate the transboundary air pollution over east Asia is required to use multiple measurements in both the source and outflow regions especially in the MBL during the polluted days.

  1. Aerosol Modeling for the Global Model Initiative

    NASA Technical Reports Server (NTRS)

    Weisenstein, Debra K.; Ko, Malcolm K. W.

    2001-01-01

    The goal of this project is to develop an aerosol module to be used within the framework of the Global Modeling Initiative (GMI). The model development work will be preformed jointly by the University of Michigan and AER, using existing aerosol models at the two institutions as starting points. The GMI aerosol model will be tested, evaluated against observations, and then applied to assessment of the effects of aircraft sulfur emissions as needed by the NASA Subsonic Assessment in 2001. The work includes the following tasks: 1. Implementation of the sulfur cycle within GMI, including sources, sinks, and aqueous conversion of sulfur. Aerosol modules will be added as they are developed and the GMI schedule permits. 2. Addition of aerosol types other than sulfate particles, including dust, soot, organic carbon, and black carbon. 3. Development of new and more efficient parameterizations for treating sulfate aerosol nucleation, condensation, and coagulation among different particle sizes and types.

  2. Effects of sulfate aerosols upon cardiopulmonary function in squirrel monkeys (final report). (Second year final report: effects of nitrate and /or sulfate aerosols upon cardiopulmonary function)

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

    Greenberg, H.L.; Avol, E.L.; Bailey, R.M.

    1977-06-24

    Squirrel monkeys were exposed to nominal concentrations of 2.5 mg/cu m of the following generated aerosols: zinc ammonium sulfate at both low (40%) and high (85%) nominal relative humidities, histamine diphosphate at low relative humidity, and ammonium bisulfate at low relative humidity. There were few statistically significant changes in oscillatory resistance, however, several trends toward increased resistance were present. Additional studies were performed using two different aerosol nebulizers to produce histamine diphosphate particles in two distinct size distributions, an order of magnitude different in size. These results, supported by data collected during sulfur dioxide exposures of squirrel monkeys, are usedmore » to discuss the suitability of Saimiri sciureus as a sensitive indicator species and oscillatory resistance as a valuable measurement of proximal airway changes. Development of the esophageal balloon technique as a means of measuring compliance and resistance in the unanesthetized squirrel monkey is discussed.« less

  3. Hygroscopicity of organic surrogate compounds from biomass burning and their effect on the efflorescence of ammonium sulfate in mixed aerosol particles

    NASA Astrophysics Data System (ADS)

    Lei, Ting; Zuend, Andreas; Cheng, Yafang; Su, Hang; Wang, Weigang; Ge, Maofa

    2018-01-01

    relatively good agreement between models and observed growth factors, as well as ERH of AS in the mixed system. The use of the ZSR relation leads to good agreement with measured diameter growth factors of aerosol particles containing humic acid and ammonium sulfate. Lastly, two distinct mixtures of organic surrogate compounds, including levoglucosan, 4-hydroxybenzoic acid, and humic acid, were used to represent the average water-soluble organic carbon (WSOC) fractions observed during the wet and dry seasons in the central Amazon Basin. A comparison of the organic fraction's hygroscopicity parameter for the simple mixtures, e.g., κ ≈ 0.12 to 0.15 for the wet-season mixture in the 90 to 40 % RH range, shows good agreement with field data for the wet season in the Amazon Basin (WSOC κ ≈ 0.14±0.06 at 90 % RH). This suggests that laboratory-generated mixtures containing organic surrogate compounds and ammonium sulfate can be used to mimic, in a simplified manner, the chemical composition of ambient aerosols from the Amazon Basin for the purpose of RH-dependent hygroscopicity studies.

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

    NASA Astrophysics Data System (ADS)

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

    2015-11-01

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

  5. First Simulations of Designing Stratospheric Sulfate Aerosol Geoengineering to Meet Multiple Simultaneous Climate Objectives

    NASA Astrophysics Data System (ADS)

    Kravitz, Ben; MacMartin, Douglas G.; Mills, Michael J.; Richter, Jadwiga H.; Tilmes, Simone; Lamarque, Jean-Francois; Tribbia, Joseph J.; Vitt, Francis

    2017-12-01

    We describe the first simulations of stratospheric sulfate aerosol geoengineering using multiple injection locations to meet multiple simultaneous surface temperature objectives. Simulations were performed using CESM1(WACCM), a coupled atmosphere-ocean general circulation model with fully interactive stratospheric chemistry, dynamics (including an internally generated quasi-biennial oscillation), and a sophisticated treatment of sulfate aerosol formation, microphysical growth, and deposition. The objectives are defined as maintaining three temperature features at their 2020 levels against a background of the RCP8.5 scenario over the period 2020-2099. These objectives are met using a feedback mechanism in which the rate of sulfur dioxide injection at each of the four locations is adjusted independently every year of simulation. Even in the presence of uncertainties, nonlinearities, and variability, the objectives are met, predominantly by SO2 injection at 30°N and 30°S. By the last year of simulation, the feedback algorithm calls for a total injection rate of 51 Tg SO2 per year. The injections are not in the tropics, which results in a greater degree of linearity of the surface climate response with injection amount than has been found in many previous studies using injection at the equator. Because the objectives are defined in terms of annual mean temperature, the required geongineering results in "overcooling" during summer and "undercooling" during winter. The hydrological cycle is also suppressed as compared to the reference values corresponding to the year 2020. The demonstration we describe in this study is an important step toward understanding what geoengineering can do and what it cannot do.

  6. Study of pH Stability of R-Salbutamol Sulfate Aerosol Solution and Its Antiasthmatic Effects in Guinea Pigs.

    PubMed

    Liu, Qing; Li, Qingrui; Han, Ting; Hu, Tingting; Zhang, Xuemei; Hu, Junhua; Hu, Hui; Tan, Wen

    2017-09-01

    Currently, all commercial available nebulized salbutamol in China is in its racemic form. It is known that only R-salbutamol (eutomer) has therapeutic effects, while S-salbutamol (distomer) may exacerbate asthma after chronic use. Therefore, it is an unmet clinical need to develop R-salbutamol as a nebulized product that is more convenient for young and old patients. In our study, a stable aerosol solution of R-salbutamol sulfate was established, and its antiasthmatic effects were confirmed. The decomposition rate and racemization effect of the R-salbutamol sulfate solution were evaluated over a pH range from 1 to 10 (except pH=7, 8) at 60°C. The aerodynamic particle size of the R-salbutamol sulfate solution and commercial RS-salbutamol sulfate solution were both tested in vitro by Next-Generation Impactor (NGI) in 5°C. Laser diffractometer was used to characterize the droplet-size distribution (DSD) of both solutions. We next conducted an in vivo animal study to document the antiasthmatic effect of R-salbutamol aerosol sulfate solution and determine the relationship to RS-salbutamol. The results showed that the R-salbutamol sulfate solution was more stable at pH 6. In vitro comparison studies indicated that there was no distribution difference between R-salbutamol sulfate solution and the commercial RS-salbutamol solution. The animal results showed that R-salbutamol was more potent than RS-salbutamol against the same dose of histamine challenge. Unlike commercial RS-salbutamol, which was acidified to a pH of 3.5 to extend bench life but may cause bronchoconstriction in asthmatic patients, the neutralized R-salbutamol solution was more suitable for clinic use.

  7. Secondary organic aerosol formation during evaporation of droplets containing atmospheric aldehydes, amines, and ammonium sulfate.

    PubMed

    Galloway, Melissa M; Powelson, Michelle H; Sedehi, Nahzaneen; Wood, Stephanie E; Millage, Katherine D; Kononenko, Julia A; Rynaski, Alec D; De Haan, David O

    2014-12-16

    Reactions of carbonyl compounds in cloudwater produce organic aerosol mass through in-cloud oxidation and during postcloud evaporation. In this work, postcloud evaporation was simulated in laboratory experiments on evaporating droplets that contain mixtures of common atmospheric aldehydes with ammonium sulfate (AS), methylamine, or glycine. Aerosol diameters were measured during monodisperse droplet drying experiments and during polydisperse droplet equilibration experiments at 75% relative humidity, and condensed-phase mass was measured in bulk thermogravimetric experiments. The evaporation of water from a droplet was found to trigger aldehyde reactions that increased residual particle volumes by a similar extent in room-temperature experiments, regardless of whether AS, methylamine, or glycine was present. The production of organic aerosol volume was highest from droplets containing glyoxal, followed by similar production from methylglyoxal or hydroxyacetone. Significant organic aerosol production was observed for glycolaldehyde, acetaldehyde, and formaldehyde only at elevated temperatures in thermogravimetric experiments. In many experiments, the amount of aerosol produced was greater than the sum of all solutes plus nonvolatile solvent impurities, indicating the additional presence of trapped water, likely caused by increasing aerosol-phase viscosity due to oligomer formation.

  8. Simulated responses of terrestrial aridity to black carbon and sulfate aerosols

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

    Lin, L.; Gettelman, A.; Xu, Y.

    Aridity index (AI), defined as the ratio of precipitation to potential evapotranspiration (PET), is a measure of the dryness of terrestrial climate. Global climate models generally project future decreases of AI (drying) associated with global warming scenarios driven by increasing greenhouse gas and declining aerosols. Given their different effects in the climate system, scattering and absorbing aerosols may affect AI differently. In this work, we explore the terrestrial aridity responses to anthropogenic black carbon (BC) and sulfate (SO 4) aerosols with Community Earth System Model simulations. Positive BC radiative forcing decreases precipitation averaged over global land at a rate ofmore » 0.9%/°C of global mean surface temperature increase (moderate drying), while BC radiative forcing increases PET by 1.0%/°C (also drying). BC leads to a global decrease of 1.9%/°C in AI (drying). SO 4 forcing is negative and causes precipitation a decrease at a rate of 6.7%/°C cooling (strong drying). PET also decreases in response to SO 4 aerosol cooling by 6.3%/°C cooling (contributing to moistening). Thus, SO 4 cooling leads to a small decrease in AI (drying) by 0.4%/°C cooling. Despite the opposite effects on global mean temperature, BC and SO 4 both contribute to the twentieth century drying (AI decrease). Sensitivity test indicates that surface temperature and surface available energy changes dominate BC- and SO 4-induced PET changes.« less

  9. Simulated responses of terrestrial aridity to black carbon and sulfate aerosols

    NASA Astrophysics Data System (ADS)

    Lin, L.; Gettelman, A.; Xu, Y.; Fu, Q.

    2016-01-01

    Aridity index (AI), defined as the ratio of precipitation to potential evapotranspiration (PET), is a measure of the dryness of terrestrial climate. Global climate models generally project future decreases of AI (drying) associated with global warming scenarios driven by increasing greenhouse gas and declining aerosols. Given their different effects in the climate system, scattering and absorbing aerosols may affect AI differently. Here we explore the terrestrial aridity responses to anthropogenic black carbon (BC) and sulfate (SO4) aerosols with Community Earth System Model simulations. Positive BC radiative forcing decreases precipitation averaged over global land at a rate of 0.9%/°C of global mean surface temperature increase (moderate drying), while BC radiative forcing increases PET by 1.0%/°C (also drying). BC leads to a global decrease of 1.9%/°C in AI (drying). SO4 forcing is negative and causes precipitation a decrease at a rate of 6.7%/°C cooling (strong drying). PET also decreases in response to SO4 aerosol cooling by 6.3%/°C cooling (contributing to moistening). Thus, SO4 cooling leads to a small decrease in AI (drying) by 0.4%/°C cooling. Despite the opposite effects on global mean temperature, BC and SO4 both contribute to the twentieth century drying (AI decrease). Sensitivity test indicates that surface temperature and surface available energy changes dominate BC- and SO4-induced PET changes.

  10. Simulated responses of terrestrial aridity to black carbon and sulfate aerosols

    DOE PAGES

    Lin, L.; Gettelman, A.; Xu, Y.; ...

    2016-01-27

    Aridity index (AI), defined as the ratio of precipitation to potential evapotranspiration (PET), is a measure of the dryness of terrestrial climate. Global climate models generally project future decreases of AI (drying) associated with global warming scenarios driven by increasing greenhouse gas and declining aerosols. Given their different effects in the climate system, scattering and absorbing aerosols may affect AI differently. In this work, we explore the terrestrial aridity responses to anthropogenic black carbon (BC) and sulfate (SO 4) aerosols with Community Earth System Model simulations. Positive BC radiative forcing decreases precipitation averaged over global land at a rate ofmore » 0.9%/°C of global mean surface temperature increase (moderate drying), while BC radiative forcing increases PET by 1.0%/°C (also drying). BC leads to a global decrease of 1.9%/°C in AI (drying). SO 4 forcing is negative and causes precipitation a decrease at a rate of 6.7%/°C cooling (strong drying). PET also decreases in response to SO 4 aerosol cooling by 6.3%/°C cooling (contributing to moistening). Thus, SO 4 cooling leads to a small decrease in AI (drying) by 0.4%/°C cooling. Despite the opposite effects on global mean temperature, BC and SO 4 both contribute to the twentieth century drying (AI decrease). Sensitivity test indicates that surface temperature and surface available energy changes dominate BC- and SO 4-induced PET changes.« less

  11. Multiple stable oxygen isotopic studies of atmospheric sulfate: A new quantitative way to understand sulfate formation processes in the atmosphere

    NASA Astrophysics Data System (ADS)

    Lee, Charles Chi-Woo

    2000-11-01

    Sulfate is an important trace species in the Earth's atmosphere because of its roles in numerous atmospheric processes. In addition to its inherent light-scattering properties, sulfate can serve as cloud condensation nucleus (CCN), affecting cloud formation as well as microphysical properties of clouds. Consequently, atmospheric sulfate species influence the global radiative energy balance. Sulfate is known to increase acidity of rainwater with negative consequences in both natural and urban environments. In addition, aerosol sulfate (<=2.5 μm) is respirable and poses a threat to human health as a potential carrier of toxic pollutants through the respiratory tract. Despite intense investigative effort, uncertainty regarding the relative significance of gas and aqueous phase oxidation pathways still remains. Acquisition of such information is important because the lifetime and transport of S(IV) species and sulfate aerosols are influenced by the oxidative pathways. In addition, sulfate formation processes affect the aerosol size distribution, which ultimately influences radiative properties of atmospheric aerosols. Therefore, the budgetary information of the sulfur cycle, as well as the radiative effects of sulfate on global climate variation, can be attained from better quantitative understanding of in situ sulfate formation processes in the atmosphere. Multiple stable oxygen isotopic studies of atmospheric sulfate are presented as a new tool to better comprehend the atmospheric sulfate formation processes. Coupled with isotopic studies, 35S radioactivity measurements have been utilized to assess contribution of sulfate from high altitude air masses. Atmospheric sulfate (aerosols and rainwater) samples have been collected from diverse environments. Laboratory experiments of gas and aqueous phase S(IV) oxidation by various oxidants, as well as biomass burning experiments, have also been conducted. The main isotopic results from these studies are as follows: (1

  12. What is the "Clim-Likely" aerosol product?

    Atmospheric Science Data Center

    2014-12-08

    ... identifying a range of components and mixtures for the MISR Standard Aerosol Retrieval Algorithm climatology, and as one standard against ... retrieval results. Six component aerosols included in the model were medium and coarse mode mineral dust, sulfate, sea salt, black ...

  13. Anthropogenic Sulfate, Clouds, and Climate Forcing

    NASA Technical Reports Server (NTRS)

    Ghan, Steven J.

    1997-01-01

    This research work is a joint effort between research groups at the Battelle Pacific Northwest Laboratory, Virginia Tech University, Georgia Institute of Technology, Brookhaven National Laboratory, and Texas A&M University. It has been jointly sponsored by the National Aeronautics and Space Administration, the U.S. Department of Energy, and the U.S. Environmental Protection Agency. In this research, a detailed tropospheric aerosol-chemistry model that predicts oxidant concentrations as well as concentrations of sulfur dioxide and sulfate aerosols has been coupled to a general circulation model that distinguishes between cloud water mass and cloud droplet number. The coupled model system has been first validated and then used to estimate the radiative impact of anthropogenic sulfur emissions. Both the direct radiative impact of the aerosols and their indirect impact through their influence on cloud droplet number are represented by distinguishing between sulfuric acid vapor and fresh and aged sulfate aerosols, and by parameterizing cloud droplet nucleation in terms of vertical velocity and the number concentration of aged sulfur aerosols. Natural sulfate aerosols, dust, and carbonaceous and nitrate aerosols and their influence on the radiative impact of anthropogenic sulfate aerosols, through competition as cloud condensation nuclei, will also be simulated. Parallel simulations with and without anthropogenic sulfur emissions are performed for a global domain. The objectives of the research are: To couple a state-of-the-art tropospheric aerosol-chemistry model with a global climate model. To use field and satellite measurements to evaluate the treatment of tropospheric chemistry and aerosol physics in the coupled model. To use the coupled model to simulate the radiative (and ultimately climatic) impacts of anthropogenic sulfur emissions.

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

    PubMed Central

    2009-01-01

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

  15. Modeling the global distribution of the oxygen isotopic composition of sulfate aerosols: Importance of transition metal catalyzed S(IV) oxidation chemistry

    NASA Astrophysics Data System (ADS)

    Alexander, B.; Park, R. J.

    2006-12-01

    The oxygen isotopic composition of sulfate aerosols (Δ17O ~ δ&&17O 0.5*δ18O) reflects the relative importance of different photochemical oxidation pathways in the atmosphere. Simulated isotopic variability in a global chemical transport model (GEOS-Chem) shows good agreement with observations in oceanic [Alexander et al., 2005] and some continental sites. However, a large discrepancy exists between modeled and measured isotopic composition in the high northern latitudes, reflecting an incomplete understanding of the sulfur budget in this region. Recent oxygen isotope measurements of sulfate aerosols collected at Alert, Canada suggest that transition metal catalyzed oxidation of SO2 by O2 in the aqueous-phase is significant during winter [Mc Cabe et al.,2006]. Global chemistry models ignore this oxidation pathway because it is believed to be important only regionally, and because of the large uncertainties in atmospheric metal concentrations and oxidation states. We have incorporated Fe(III) and Mn(II) catalyzed oxidation of S(IV) (S(IV) = SO2·H2O + HSO3- + SO32-) by O2 into the GEOS-Chem model using the McCabe et al. [2006] isotope measurements as a constraint. We will examine the importance of this oxidation pathway for the sulfur budget in the Arctic, and on the global scale. Preliminary results suggest that, during winter, up to 75% of aerosol sulfate at Alert forms via the metal catalysis pathway. The addition of this chemical pathway decreases the SO2 burden in the Arctic (north of 60°N) by 40% due to an increase in the oxidation rate. The comparison of large-scale sulfate aerosol models study (COSAM) showed that on average, models over-predict SO2 mixing ratios by factors of 2 or more [Barrie et al., 2001]. This "missing" S(IV) oxidation pathway can partially explain this discrepancy.

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

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

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

    2013-10-25

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

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

    PubMed

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

    2016-05-15

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

  18. Balloon profiles of stratospheric NO2 and HNO3 for testing the heterogeneous hydrolysis of N2O5 on sulfate aerosols

    NASA Technical Reports Server (NTRS)

    Webster, C. R.; May, R. D.; Allen, M.; Jaegle, L.; Mccormick, M. P.

    1994-01-01

    Simultaneous in situ measurements of stratospheric NO2, HNO3, HCl, and CH4 from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS) tunable diode laser spectrometer. Although the measurements of NO2, HNO3, and NO2/HNO3 agree well with gas-phase model calculations near 34 km where Stratospheric Aerosol and Gas Experiment (SAGE) 2 data show little sulfate aerosol, this is not true at the lower altitudes where SAGE 2 shows high aerosol loadings. At 24 km the BLISS NO2 and HNO3 measurements are 70% lower and 50% higher, respectively, than the gas phase model predictions, with a measured NO2/HNO3 ratio 5 times smaller. When the heterogeneous hydrolysis of N2O5 and ClONO2 on sulfate aerosol of surface area densities matching the SAGE 2 measurements is added to the model, good agreement with the BLISS measurements is found over the whole altitude range.

  19. DYNAMICS OF AUTOMOTIVE SULFATE EMISSIONS

    EPA Science Inventory

    A preliminary assessment of the potential environmental impact of automotive sulfuric acid (or sulfate) aerosol has been made by analyzing the aerosol dynamics. This analysis leads to the prediction of ambient automotive sulfuric acid aerosol concentrations over and around a larg...

  20. Optical constants of concentrated aqueous ammonium sulfate.

    NASA Technical Reports Server (NTRS)

    Remsberg, E. E.

    1973-01-01

    Using experimental data obtained from applying spectroscopy to a 39-wt-% aqueous ammonium sulfate solution, it is shown that, even though specific aerosol optical constants appear quite accurate, spectral variations may exist as functions of material composition or concentration or both. Prudent users of optical constant data must then include liberal data error estimates when performing calculations or in interpreting spectroscopic surveys of collected aerosol material.

  1. Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

    NASA Astrophysics Data System (ADS)

    Adachi, K.; Buseck, P. R.

    2008-05-01

    Soot particles are major aerosol constituents that result from emissions of burning of fossil fuel and biomass. Because they both absorb sunlight and contribute to cloud formation, they are an influence on climate on local, regional, and global scales. It is therefore important to evaluate their optical and hygroscopic properties and those effects on the radiation budget. Those properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using transmission electron microscopy, we measured ~8000 particles (25 samples) with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC) and adjacent areas. More than 50% of the particles consist of internally mixed soot, organic matter, and sulfate. Imaging combined with chemical analysis of individual particles show that many are coated, consist of aggregates, or both. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetime. Our results suggest that a mixture of materials from multiple sources such as vehicles, power plants, and biomass burning occurs in individual particles, thereby increasing their complexity. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate than uncoated soot particles. Moreover, soot occurs in more than 60% of all particles in the MC plumes, suggesting its important role in the formation of secondary aerosol particles.

  2. Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements

    NASA Technical Reports Server (NTRS)

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

    2011-01-01

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

  3. Agglomerated novel spray-dried lactose-leucine tailored as a carrier to enhance the aerosolization performance of salbutamol sulfate from DPI formulations.

    PubMed

    Molina, Carlos; Kaialy, Waseem; Chen, Qiao; Commandeur, Daniel; Nokhodchi, Ali

    2017-12-19

    Spray-drying allows to modify the physicochemical/mechanical properties of particles along with their morphology. In the present study, L -leucine with varying concentrations (0.1, 0.5, 1, 5, and 10% w/v) were incorporated into lactose monohydrate solution for spray-drying to enhance the aerosolization performance of dry powder inhalers containing spray-dried lactose-leucine and salbutamol sulfate. The prepared spray-dried lactose-leucine carriers were analyzed using laser diffraction (particle size), differential scanning calorimetry (thermal behavior), scanning electron microscopy (morphology), powder X-ray diffraction (crystallinity), Fourier transform infrared spectroscopy (interaction at molecular level), and in vitro aerosolization performance (deposition). The results showed that the efficacy of salbutamol sulfate's aerosolization performance was, in part, due to the introduction of L -leucine in the carrier, prior to being spray-dried, accounting for an increase in the fine particle fraction (FPF) of salbutamol sulfate from spray-dried lactose-leucine (0.5% leucine) in comparison to all other carriers. It was shown that all of the spray-dried carriers were spherical in their morphology with some agglomerates and contained a mixture of amorphous, α-lactose, and β-lactose. It was also interesting to note that spray-dried lactose-leucine particles were agglomerated during the spray-drying process to make coarse particles (volume mean diameter of 79 to 87 μm) suitable as a carrier in DPI formulations.

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

    NASA Astrophysics Data System (ADS)

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

    2007-12-01

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

  5. Antarctic aerosols - A review

    NASA Astrophysics Data System (ADS)

    Shaw, Glenn E.

    1988-02-01

    Tropospheric aerosols with the diameter range of half a micron reside in the atmosphere for tens of days and teleconnect Antarctica with other regions by transport that reaches planetary scales of distances; thus, the aerosol on the Antarctic ice represents 'memory modules' of events that took place at regions separated from Antarctica by tens of thousands of kilometers. In terms of aerosol mass, the aerosol species include insoluble crustal products (less than 5 percent), transported sea-salt residues (highly variable but averaging about 10 percent), Ni-rich meteoric material, and anomalously enriched material with an unknown origin. Most (70-90 percent by mass) of the aerosol over the Antarctic ice shield, however, is the 'natural acid sulfate aerosol', apparently deriving from biological processes taking place in the surrounding oceans.

  6. Small volcanic eruptions and the stratospheric sulfate aerosol burden

    NASA Astrophysics Data System (ADS)

    Pyle, David M.

    2012-09-01

    Understanding of volcanic activity and its impacts on the atmosphere has evolved in discrete steps, associated with defining eruptions. The eruption of Krakatau, Indonesia, in August 1883 was the first whose global reach was recorded through observations of atmospheric phenomena around the world (Symons 1888). The rapid equatorial spread of Krakatau's ash cloud revealed new details of atmospheric circulation, while the vivid twilights and other optical phenomena were soon causally linked to the effects of particles and gases released from the volcano (e.g. Stothers 1996, Schroder 1999, Hamilton 2012). Later, eruptions of Agung, Bali (1963), El Chichón, Mexico (1982) and Pinatubo, Philippines (1991) led to a fuller understanding of how volcanic SO2 is transformed to a long-lived stratospheric sulfate aerosol, and its consequences (e.g. Meinel and Meinel 1967, Rampino and Self 1982, Hoffman and Rosen 1983, Bekki and Pyle 1994, McCormick et al 1995). While our ability to track the dispersal of volcanic emissions has been transformed since Pinatubo, with the launch of fleets of Earth-observing satellites (e.g. NASA's A-Train; ESA's MetOp) and burgeoning networks of ground-based remote-sensing instruments (e.g. lidar and sun-photometers; infrasound and lightning detection systems), there have been relatively few significant eruptions. Thus, there have been limited opportunities to test emerging hypotheses including, for example, the vexed question of the role of 'smaller' explosive eruptions in perturbations of the atmosphere—those that may just be large enough to reach the stratosphere (of size 'VEI 3', Newhall and Self 1982, Pyle 2000). Geological evidence, from ice-cores and historical eruptions, suggests that small explosive volcanic eruptions with the potential to transport material into the stratosphere should be frequent (5-10 per decade), and responsible for a significant proportion of the long-term time-averaged flux of volcanic sulfur into the stratosphere

  7. Interactions of aerosols (ammonium sulfate, ammonium nitrate and ammonium chloride) and of gases (HCl, HNO 3) with fogwater

    NASA Astrophysics Data System (ADS)

    Ruprecht, Heidi; Sigg, Laura

    The concentrations of aerosols (NH 4NO 3, (NH 4) 2SO 4 and NH 4Cl) and of gases (HCl (g), HNO 3(g), NH 3(g) were determined by denuder methods under different conditions (in the absence of fog, before, during and after fog events). At this site situated in an urban region, high concentrations of the gaseous strong acids HCl (g) and HNO 3(g) are observed. NH 4Cl and NH 4NO 3 aerosols represent a major fraction of the Cl - and NO 3- aerosols (<2.4 μm)collected by denuders. During a fog event, very high concentrations of SO 42- were found in small aerosols, which are attributed to the aqueous phase oxidation of SO 2 under the influence of high pH due to the presence of NH 3. Differences in SO 42- concentrations measured in aerosols (<2.4 μm) and in fog droplets were probably due to mass-transport limitations of the SO 2 oxidation. Ammonium sulfate aerosols represent in some cases a significant fraction of the total S present (SO 2(g) + SO 42-. Soluble aerosols and gases contribute to the composition of fogwater and are released again after fog dissipation.

  8. An evaluation of possible mechanisms for conversion of sulfur dioxide to sulfuric acid and sulfate aerosols in the troposphere

    Treesearch

    Jack G. Calvert

    1976-01-01

    The mechanisms and rates of conversion of sulfur dioxide to sulfur trioxide, sulfuric acid, and other "sulfate" aerosol precursors are considered in view of current knowledge related to atmospheric reactions and chemical kinetics. Several heterogeneous pathways exist for SO2 oxidation promoted on solid catalyst particles and in aqueous...

  9. Upper-atmosphere Aerosols: Properties and Natural Cycles

    NASA Technical Reports Server (NTRS)

    Turco, Richard P.

    1992-01-01

    The middle atmosphere is rich in its variety of particulate matter, which ranges from meteorite debris, to sulfate aerosols, to polar stratospheric ice clouds. Volcanic eruptions strongly perturb the stratospheric sulfate (Junge) layer. High-altitude 'noctilucent' ice clouds condense at the summer mesopause. The properties of these particles, including their composition, sizes, and geographical distribution, are discussed, and their global effects, including chemical, radiative, and climatic roles, are reviewed. Polar stratospheric clouds (PSCs) are composed of water and nitric acid in the form of micron-sized ice crystals. These particles catalyze reactions of chlorine compounds that 'activate' otherwise inert chlorine reservoirs, leading to severe ozone depletions in the southern polar stratosphere during austral spring. PSCs also modify the composition of the polar stratosphere through complex physiocochemical processes, including dehydration and denitrification, and the conversion of reactive nitrogen oxides into nitric acid. If water vapor and nitric acid concentrations are enhanced by high-altitude aircraft activity, the frequency, geographical range, and duration of PSCs might increase accordingly, thus enhancing the destruction of the ozone layer (which would be naturally limited in geographical extent by the same factors that confine the ozone hole to high latitudes in winter). The stratospheric sulfate aerosol layer reflects solar radiation and increases the planetary albedo, thereby cooling the surface and possibly altering the climate. Major volcanic eruptions, which increase the sulfate aerosol burden by a factor of 100 or more, may cause significant global climate anomalies. Sulfate aerosols might also be capable of activating stratospheric chlorine reservoirs on a global scale (unlike PCSs, which represent a localized polar winter phenomenon), although existing evidence suggests relatively minor perturbations in chlorine chemistry. Nevertheless, if

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

    NASA Astrophysics Data System (ADS)

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

    2017-12-01

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

  11. Climate forcing by anthropogenic aerosols

    NASA Technical Reports Server (NTRS)

    Charlson, R. J.; Schwartz, S. E.; Hales, J. M.; Cess, R. D.; Coakley, J. A., Jr.; Hansen, J. E.; Hofmann, D. J.

    1992-01-01

    Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol, in particular, has imposed a major perturbation to this forcing. Both the direct scattering of short-wavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

  12. Climate forcing by anthropogenic aerosols.

    PubMed

    Charlson, R J; Schwartz, S E; Hales, J M; Cess, R D; Coakley, J A; Hansen, J E; Hofmann, D J

    1992-01-24

    Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol in particular has imposed a major perturbation to this forcing. Both the direct scattering of shortwavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

  13. A Study of the Relationship Between Anthropogenic Sulfate and Cloud Drop Nucleation

    NASA Technical Reports Server (NTRS)

    Chuang, Catherine C.; Penner, Joyce E.

    1994-01-01

    The characteristics of the cloud drop size distribution near cloud base are initially determined by the aerosol particles that serve as CCN and by the local updraft velocity. Chemical reactions of the emitted gaseous sulfur compounds due to human activities will alter, through gas-to-particle conversion, the aerosol size distribution, total number, and its chemical composition. Recently, Boucher and Rodhe and Jones et.al have each developed parameterizations relating cloud drop concentration to sulfate mass or aerosol number concentration, respectively, and used them to develop estimates of the indirect forcing by anthropogenic sulfate aerosols. THese parameterizations made use of measure relationships in continental and maritime clouds. However, these relationships are inherently noisy, yielding more than a factor of 2 variation in cloud drop concentration for a given aerosol number (or for a given sulfate mass) concentration. The large spatial and temporal variabilities in the concentration, chemical characteristics, and size distribution of aerosols have made it difficult to develop such a parameterization from data. In this paper, our focus is to develop a means for relating the predicted anthropogenic sulfate mass to cloud drop number concentration over the range of expected conditions associated with continental and marine aerosol. We start with an assumed pre-existing particle size distribution and develop an approximation of the altered distribution after addition of anthropogenic sulfate. We thereby develop a conservative estimate of the possible change in cloud drop number concentration due to anthropogenic sulfate.

  14. First Simulations of Designing Stratospheric Sulfate Aerosol Geoengineering to Meet Multiple Simultaneous Climate Objectives: DESIGNING STRATOSPHERIC GEOENGINEERING

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

    Kravitz, Ben; MacMartin, Douglas G.; Mills, Michael J.

    We describe the first simulations of stratospheric sulfate aerosol geoengineering using multiple injection locations to meet multiple simultaneous surface temperature objectives. Simulations were performed using CESM1(WACCM), a coupled atmosphere-ocean general circulation model with fully interactive stratospheric chemistry, dynamics (including an internally generated quasi-biennial oscillation), and a sophisticated treatment of sulfate aerosol formation, microphysical growth, and deposition. The objectives are defined as maintaining three temperature features at their 2020 levels against a background of the RCP8.5 scenario over the period 2020-2099. These objectives are met using a feedback mechanism in which the rate of sulfur dioxide injection at each of themore » four locations is adjusted independently every year of simulation. Even in the presence of uncertainties, nonlinearities, and variability, the objectives are met, predominantly by SO2 injection at 30°N and 30°S. By the last year of simulation, the feedback algorithm calls for a total injection rate of 51 Tg SO2 per year. The injections are not in the tropics, which results in a greater degree of linearity of the surface climate response with injection amount than has been found in many previous studies using injection at the equator. Because the objectives are defined in terms of annual mean temperature, the required geeongineering results in "overcooling" during summer and "undercooling" during winter. The hydrological cycle is also suppressed as compared to the reference values corresponding to the year 2020. The demonstration we describe in this study is an important step toward understanding what geoengineering can do and what it cannot do.« less

  15. Aerosol simulation including chemical and nuclear reactions

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

    Marwil, E.S.; Lemmon, E.C.

    1985-01-01

    The numerical simulation of aerosol transport, including the effects of chemical and nuclear reactions presents a challenging dynamic accounting problem. Particles of different sizes agglomerate and settle out due to various mechanisms, such as diffusion, diffusiophoresis, thermophoresis, gravitational settling, turbulent acceleration, and centrifugal acceleration. Particles also change size, due to the condensation and evaporation of materials on the particle. Heterogeneous chemical reactions occur at the interface between a particle and the suspending medium, or a surface and the gas in the aerosol. Homogeneous chemical reactions occur within the aersol suspending medium, within a particle, and on a surface. These reactionsmore » may include a phase change. Nuclear reactions occur in all locations. These spontaneous transmutations from one element form to another occur at greatly varying rates and may result in phase or chemical changes which complicate the accounting process. This paper presents an approach for inclusion of these effects on the transport of aerosols. The accounting system is very complex and results in a large set of stiff ordinary differential equations (ODEs). The techniques for numerical solution of these ODEs require special attention to achieve their solution in an efficient and affordable manner. 4 refs.« less

  16. Atmospheric oxidation of isoprene and 1,3-butadiene: influence of aerosol acidity and relative humidity on secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Lewandowski, M.; Jaoui, M.; Offenberg, J. H.; Krug, J. D.; Kleindienst, T. E.

    2014-11-01

    The effects of acidic seed aerosols on the formation of secondary organic aerosol (SOA) have been examined in a number of previous studies, several of which have observed strong linear correlations between the aerosol acidity (measured as nmol H+ per m3 air sample volume) and the percent change of secondary organic carbon (SOC). The measurements have used several precursor compounds representative of different classes of biogenic hydrocarbons including isoprene, monoterpenes, and sesquiterpenes. To date, isoprene has displayed the most pronounced increase in SOC, although few measurements have been conducted with anthropogenic hydrocarbons. In the present study, we examine several aspects of the effect of aerosol acidity on the secondary organic carbon formation from the photooxidation of 1,3-butadiene, as well as extending the previous analysis of isoprene. The photooxidation products measured in the absence and presence of acidic sulfate aerosols were generated either through photochemical oxidation of SO2 or by nebulizing mixtures of ammonium sulfate and sulfuric acid into a 14.5 m3 smog chamber system. The results showed that, like isoprene and β-caryophyllene, 1,3-butadiene SOC yields linearly correlate with increasing acidic sulfate aerosol. The observed acid sensitivity of 0.11% SOC increase per nmol m-3 increase in H+ was approximately a factor of three less than that measured for isoprene. The results also showed that the aerosol yield decreased with increasing humidity for both isoprene and 1,3-butadiene, although to different degrees. Increasing the absolute humidity from 2 to 12 g m-3 reduced the 1,3-butadiene yield by 45% and the isoprene yield by 85%.

  17. Atmospheric oxidation of isoprene and 1,3-butadiene: influence of aerosol acidity and relative humidity on secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Lewandowski, M.; Jaoui, M.; Offenberg, J. H.; Krug, J. D.; Kleindienst, T. E.

    2015-04-01

    The effects of acidic seed aerosols on the formation of secondary organic aerosol (SOA) have been examined in a number of previous studies, several of which have observed strong linear correlations between the aerosol acidity (measured as nmol H+ m-3 air sample volume) and the percent change in secondary organic carbon (SOC). The measurements have used several precursor compounds representative of different classes of biogenic hydrocarbons including isoprene, monoterpenes, and sesquiterpenes. To date, isoprene has displayed the most pronounced increase in SOC, although few measurements have been conducted with anthropogenic hydrocarbons. In the present study, we examine several aspects of the effect of aerosol acidity on the secondary organic carbon formation from the photooxidation of 1,3-butadiene, and extend the previous analysis of isoprene. The photooxidation products measured in the absence and presence of acidic sulfate aerosols were generated either through photochemical oxidation of SO2 or by nebulizing mixtures of ammonium sulfate and sulfuric acid into a 14.5 m3 smog chamber system. The results showed that, like isoprene and β-caryophyllene, 1,3-butadiene SOC yields linearly correlate with increasing acidic sulfate aerosol. The observed acid sensitivity of 0.11% SOC increase per nmol m-3 increase in H+ was approximately a factor of 3 less than that measured for isoprene. The results also showed that the aerosol yield decreased with increasing humidity for both isoprene and 1,3-butadiene, although to different degrees. Increasing the absolute humidity from 2 to 12 g m-3 reduced the 1,3-butadiene yield by 45% and the isoprene yield by 85%.

  18. Easy Volcanic Aerosol

    NASA Astrophysics Data System (ADS)

    Toohey, Matthew; Stevens, Bjorn; Schmidt, Hauke; Timmreck, Claudia

    2016-04-01

    Radiative forcing by stratospheric sulfate aerosol of volcanic origin is one of the strongest drivers of natural climate variability. Transient model simulations attempting to match observed climate variability, such as the CMIP historical simulations, rely on volcanic forcing reconstructions based on observations of a small sample of recent eruptions and coarse proxy data for eruptions before the satellite era. Volcanic forcing data sets used in CMIP5 were provided either in terms of optical properties, or in terms of sulfate aerosol mass, leading to significant inter-model spread in the actual volcanic radiative forcing produced by models and in their resulting climate responses. It remains therefore unclear to what degree inter-model spread in response to volcanic forcing represents model differences or variations in the forcing. In order to isolate model differences, Easy Volcanic Aerosol (EVA) provides an analytic representation of volcanic stratospheric aerosol forcing, based on available observations and aerosol model results, prescribing the aerosol's radiative properties and primary modes of spatial and temporal variability. In contrast to regriddings of observational data, EVA allows for the production of physically consistent forcing for historic and hypothetical eruptions of varying magnitude, source latitude, and season. Within CMIP6, EVA will be used to reconstruct volcanic forcing over the past 2000 years for use in the Paleo-Modeling Intercomparison Project (PMIP), and will provide forcing sets for VolMIP experiments aiming to quantify model uncertainty in the response to volcanic forcing. Here, the functional form of EVA will be introduced, along with illustrative examples including the EVA-based reconstruction of volcanic forcing over the historical period, and that of the 1815 Tambora eruption.

  19. Simulated responses of terrestrial aridity to black carbon and sulfate aerosols: LIN: SIMULATED RESPONSES ARIDITY

    DOE PAGES

    Lin, L.; Gettelman, A.; Xu, Y.; ...

    2016-01-27

    Aridity index (AI), defined as the ratio of precipitation to potential evapotranspiration (PET), is a measure of the dryness of terrestrial climate. Global climate models generally project future decreases of AI (drying) associated with global warming scenarios driven by increasing greenhouse gas and declining aerosols. Given their different effects in the climate system, scattering and absorbing aerosols may affect AI differently. Here we explore the terrestrial aridity responses to anthropogenic black carbon (BC) and sulfate (SO4) aerosols with Community Earth System Model simulations. Positive BC radiative forcing decreases precipitation averaged over global land at a rate of 0.9%/°C of globalmore » mean surface temperature increase (moderate drying), while BC radiative forcing increases PET by 1.0%/°C (also drying). BC leads to a global decrease of 1.9%/°C in AI (drying). SO4 forcing is negative and causes precipitation a decrease at a rate of 6.7%/°C cooling (strong drying). PET also decreases in response to SO4 aerosol cooling by 6.3%/°C cooling (contributing to moistening). Thus, SO4 cooling leads to a small decrease in AI (drying) by 0.4%/°C cooling. Despite the opposite effects on global mean temperature, BC and SO4 both contribute to the twentieth century drying (AI decrease). Sensitivity test indicates that surface temperature and surface available energy changes dominate BC- and SO4-induced PET changes.« less

  20. Glacier evolution in high-mountain Asia under stratospheric sulfate aerosol injection geoengineering

    NASA Astrophysics Data System (ADS)

    Zhao, Liyun; Yang, Yi; Cheng, Wei; Ji, Duoying; Moore, John C.

    2017-06-01

    Geoengineering by stratospheric sulfate aerosol injection may help preserve mountain glaciers by reducing summer temperatures. We examine this hypothesis for the glaciers in high-mountain Asia using a glacier mass balance model driven by climate simulations from the Geoengineering Model Intercomparison Project (GeoMIP). The G3 and G4 schemes specify use of stratospheric sulfate aerosols to reduce the radiative forcing under the Representative Concentration Pathway (RCP) 4.5 scenario for the 50 years between 2020 and 2069, and for a further 20 years after termination of geoengineering. We estimate and compare glacier volume loss for every glacier in the region using a glacier model based on surface mass balance parameterization under climate projections from three Earth system models under G3, five models under G4, and six models under RCP4.5 and RCP8.5. The ensemble projections suggest that glacier shrinkage over the period 2010-2069 is equivalent to sea-level rise of 9.0 ± 1.6 mm (G3), 9.8 ± 4.3 mm (G4), 15.5 ± 2.3 mm (RCP4.5), and 18.5 ± 1.7 mm (RCP8.5). Although G3 keeps the average temperature from increasing in the geoengineering period, G3 only slows glacier shrinkage by about 50 % relative to losses from RCP8.5. Approximately 72 % of glaciated area remains at 2069 under G3, as compared with about 30 % for RCP8.5. The widely reported reduction in mean precipitation expected for solar geoengineering is unlikely to be as important as the temperature-driven shift from solid to liquid precipitation for forcing Himalayan glacier change. The termination of geoengineering at 2069 under G3 leads to temperature rise of about 1.3 °C over the period 2070-2089 relative to the period 2050-2069 and corresponding increase in annual mean glacier volume loss rate from 0.17 to 1.1 % yr-1, which is higher than the 0.66 % yr-1 under RCP8.5 during 2070-2089.

  1. CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

    EPA Science Inventory

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

  2. Role of interfacial water in the heterogeneous uptake of glyoxal by mixed glycine and ammonium sulfate aerosols.

    PubMed

    Trainic, Miri; Riziq, Ali Abo; Lavi, Avi; Rudich, Yinon

    2012-06-21

    This study focuses on the heterogeneous reactions of gas phase glyoxal with aerosols of glycine, the most abundant amino acid in atmospheric aerosols, as well as with a mixture of glycine and ammonium sulfate (AS) at a molar ratio of 1:100 (glycine-AS 1:100). Aerosols were exposed to varying relative humidity (RH) conditions in the presence of gas phase glyoxal for ∼1 h, followed by drying and efflorescence. The changes in size, chemical composition, and optical properties were consequently measured. The reactions occur over a wide range of relative humidities, from ∼30% up to 90% RH, covering values that are substantially lower as well as above the deliquescence point of the investigated aerosols. The product aerosols exhibit a trend of increasing growth in size, in optical extinction cross sections, and in extinction efficiencies (at λ = 355 nm) with decreasing seed aerosol size, and with decreasing RH values from 90% to ∼50%. For glycine-AS 1:100 particles, the ratio of the geometric cross section of the product aerosol to the original seed aerosol reached a value of ∼3, the optical extinction cross section ratio was up to ∼25, and the Q(ext) ratio was up to ∼8, exceeding those of both AS and glycine separately, suggesting a synergistic effect. Aerosol mass spectrometer analyses show that the main products of all the studied reactions are glyoxal oligomers (light scattering compounds), with a minor contribution from imidazoles (absorbing compounds at λ = 355 nm). These findings imply that the changes in the optical properties are likely due to enhanced scattering by the reaction products. The fraction of absorbing substances in the reacted aerosol increases with increasing RH, suggesting that the absorption component may become more substantial after longer reaction times, possibly in cloud or fog droplets. The results suggest that these reactions are possibly important in low RH regions, plausibly due to the reaction occurring in a few interfacial

  3. Composition of individual aerosol particles above the Israelian Mediterranean coast during the summer time

    NASA Astrophysics Data System (ADS)

    Ganor, E.; Levin, Z.; Van Grieken, R.

    Aerosol particles were collected aboard a ship in Haifa Bay and Tel Aviv, Israel, during the summer time. The aerosol particles (6170) were analyzed as individual particles and classified according to their chemical composition, size, number concentration per cubic centimeter and morphology. Most of the aerosol particles could be classified into four groups. The first contains gypsum from the sea and from industrial sources brought in by land breezes. A second group is characterized by continental aluminosilicate and quartz. A third group consists of sea salt mixed with sulfate particles. The fourth group is characterized by an abundance of sulfate particles, some of which are ammonium sulfate brought by the land breezes. The particles were identified as marine and mineral aerosols which originated in Eastern Europe and the Mediterranean sea, while local aerosols brought by land breeze characterized by phosphate, fly ash and soil particles originated in the Haifa industrial zone. In addition, the aerosols were analyzed for sulfates and nitrates. Aerosols of sea and land breezes differed as follows: (1) Sulfate and nitrate concentrations in the aerosols were 5-10 times higher during land breeze than during sea breeze, and the total content of suspended particles was, respectively, 6-12 times higher. (2) Particle size spectra during land breeze were broader than during sea breeze and their concentrations were about 20 times greater. Analyses of individual particles by electron microscopy revealed that during the sea breeze the aerosols contained calcium sulfate, sodium sulfate and sulfuric acid. The sulfuric acid, of pH 2.5, is due to the long-range transport as previously reported ( Ganor et al., 1993) while the other sulfates are from the sea. This explains the high concentration of sulfates in the atmospheric sea breeze above the Israelian Mediterranean coast during the summertime.

  4. Isotopic constraints on heterogeneous sulfate production in Beijing haze

    NASA Astrophysics Data System (ADS)

    He, Pengzhen; Alexander, Becky; Geng, Lei; Chi, Xiyuan; Fan, Shidong; Zhan, Haicong; Kang, Hui; Zheng, Guangjie; Cheng, Yafang; Su, Hang; Liu, Cheng; Xie, Zhouqing

    2018-04-01

    Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter) in Beijing is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. Here we present observations of the oxygen-17 excess of PM2.5 sulfate (Δ17O(SO42-)) collected in Beijing haze from October 2014 to January 2015 to constrain possible sulfate formation pathways. Throughout the sampling campaign, the 12-hourly averaged PM2.5 concentrations ranged from 16 to 323 µg m-3 with a mean of (141 ± 88 (1σ)) µg m-3, with SO42- representing 8-25 % of PM2.5 mass. The observed Δ17O(SO42-) varied from 0.1 to 1.6 ‰ with a mean of (0.9 ± 0.3) ‰. Δ17O(SO42-) increased with PM2.5 levels in October 2014 while the opposite trend was observed from November 2014 to January 2015. Our estimate suggested that in-cloud reactions dominated sulfate production on polluted days (PDs, PM2.5 ≥ 75 µg m-3) of Case II in October 2014 due to the relatively high cloud liquid water content, with a fractional contribution of up to 68 %. During PDs of Cases I and III-V, heterogeneous sulfate production (Phet) was estimated to contribute 41-54 % to total sulfate formation with a mean of (48 ± 5) %. For the specific mechanisms of heterogeneous oxidation of SO2, chemical reaction kinetics calculations suggested S(IV) ( = SO2 ⚫ H2O + HSO3- + SO32-) oxidation by H2O2 in aerosol water accounted for 5-13 % of Phet. The relative importance of heterogeneous sulfate production by other mechanisms was constrained by our observed Δ17O(SO42-). Heterogeneous sulfate production via S(IV) oxidation by O3 was estimated to contribute 21-22 % of Phet on average. Heterogeneous sulfate production pathways that result in zero-Δ17O(SO42-), such as S(IV) oxidation by NO2 in aerosol water and/or by O2 via a radical chain mechanism, contributed the remaining 66-73 % of Phet. The assumption about the thermodynamic state of aerosols

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

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

  6. Synergistic reaction between SO2 and NO2 on mineral oxides: a potential formation pathway of sulfate aerosol.

    PubMed

    Liu, Chang; Ma, Qingxin; Liu, Yongchun; Ma, Jinzhu; He, Hong

    2012-02-07

    Sulfate is one of the most important aerosols in the atmosphere. A new sulfate formation pathway via synergistic reactions between SO(2) and NO(2) on mineral oxides was proposed. The heterogeneous reactions of SO(2) and NO(2) on CaO, α-Fe(2)O(3), ZnO, MgO, α-Al(2)O(3), TiO(2), and SiO(2) were investigated by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in situ DRIFTS) at ambient temperature. Formation of sulfate from adsorbed SO(2) was promoted by the coexisting NO(2), while surface N(2)O(4) was observed as the crucial oxidant for the oxidation of surface sulfite. This process was significantly promoted by the presence of O(2). The synergistic effect between SO(2) and NO(2) was not observed on other mineral particles (such as CaCO(3) and CaSO(4)) probably due to the lack of the surface reactive oxygen sites. The synergistic reaction between SO(2) and NO(2) on mineral oxides resulted in the formation of internal mixtures of sulfate, nitrate, and mineral oxides. The change of mixture state will affect the physicochemical properties of atmospheric particles and therefore further influence their environmental and climate effects.

  7. Multi-model comparison of the volcanic sulfate deposition from the 1815 eruption of Mt. Tambora

    NASA Astrophysics Data System (ADS)

    Marshall, Lauren; Schmidt, Anja; Toohey, Matthew; Carslaw, Ken S.; Mann, Graham W.; Sigl, Michael; Khodri, Myriam; Timmreck, Claudia; Zanchettin, Davide; Ball, William T.; Bekki, Slimane; Brooke, James S. A.; Dhomse, Sandip; Johnson, Colin; Lamarque, Jean-Francois; LeGrande, Allegra N.; Mills, Michael J.; Niemeier, Ulrike; Pope, James O.; Poulain, Virginie; Robock, Alan; Rozanov, Eugene; Stenke, Andrea; Sukhodolov, Timofei; Tilmes, Simone; Tsigaridis, Kostas; Tummon, Fiona

    2018-02-01

    The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 year without a summer, and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic sulfate signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), five state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora) and volcanic (with Tambora) sulfate deposition to polar regions and compare to ice core records. The models simulate overall similar patterns of background sulfate deposition, although there are differences in regional details and magnitude. However, the volcanic sulfate deposition varies considerably between the models with differences in timing, spatial pattern and magnitude. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kg km-2 and on Greenland from 31 to 194 kg km-2, as compared to the mean ice-core-derived estimates of roughly 50 kg km-2 for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results suggest that deriving relationships between sulfate deposited on ice sheets and atmospheric sulfate burdens from model simulations may be associated with greater uncertainties than previously thought.

  8. Reactivity of stratospheric aerosols to small amounts of ammonia in the laboratory environment

    NASA Technical Reports Server (NTRS)

    Hayes, D.; Snetsinger, K.; Ferry, G.; Oberbeck, V.; Farlow, N.

    1980-01-01

    Trace ammonia in laboratory air reacts easily with sulfuric acid aerosol samples to form crystalline ammonium sulfate. Argon atmospheres, however, protect sampling surfaces from ammonia contamination. It is found that atmospheric aerosols treated in this way contain only sulfuric acid. After an hour exposed to laboratory air, these same samples convert to ammonium sulfate. Aerosol particles have been collected, using argon control, to determine if the absence of crystalline sulfate is common. But so far there is no evidence that aerosols are neutralized by ammonia in the stratosphere.

  9. Is there an aerosol signature of aqueous processing?

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Sorooshian, A.

    2017-12-01

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

  10. Tropospheric Trace Gas Interactions with Aerosols

    NASA Technical Reports Server (NTRS)

    Penner, Joyce E.; Maddrea, George L., Jr. (Technical Monitor)

    2002-01-01

    Tropospheric aerosols are of considerable environmental importance. They modify the radiative budget of Earth by scattering and absorbing radiation, and by providing nuclei for cloud formation. Additionally, they provide surfaces for heterogeneous and multiphase reactions that affect tropospheric chemistry. For example, Dentener and Crutzen (1993) showed that reactions of N2O5 and NO3 with sulfate aerosols may significantly alter the tropospheric concentrations of NO(x), O3, and OH by converting NOx to HNO3 which is rapidly removed by precipitation. Zhang et al. (1994) assumed these same reactions would occur on dust aerosols and showed that dust outbreaks may reduce NO(x) levels by up to 50%. Dentener et al. (1996) studied the possible effect of reactions on dust on sulfate, nitrate, and O3 concentration. Heterogeneous and multiphase reactions on aerosols may also perturb the sulfur cycle the chlorine cycle and the bromine cycle. Because these reactions can release free chlorine and free bromine they might lead to the destruction of ozone in the marine boundary layer that may be important to include in models of tropospheric chemistry. The goal of our proposed work is to examine the role of heterogeneous and multiphase reactions in the tropospheric cycles of reactive nitrogen and sulfur.

  11. Towards a Global Aerosol Climatology: Preliminary Trends in Tropospheric Aerosol Amounts and Corresponding Impact on Radiative Forcing between 1950 and 1990

    NASA Technical Reports Server (NTRS)

    Tegen, Ina; Koch, Dorothy; Lacis, Andrew A.; Sato, Makiko

    1999-01-01

    A global aerosol climatology is needed in the study of decadal temperature change due to natural and anthropogenic forcing of global climate change. A preliminary aerosol climatology has been developed from global transport models for a mixture of sulfate and carbonaceous aerosols from fossil fuel burning, including also contributions from other major aerosol types such as soil dust and sea salt. The aerosol distributions change for the period of 1950 to 1990 due to changes in emissions of SO2 and carbon particles from fossil fuel burning. The optical thickness of fossil fuel derived aerosols increased by nearly a factor of 3 during this period, with particularly strong increase in eastern Asia over the whole time period. In countries where environmental laws came into effect since the early 1980s (e.g. US and western Europe), emissions and consequently aerosol optical thicknesses did not increase considerably after 1980, resulting in a shift in the global distribution pattern over this period. In addition to the optical thickness, aerosol single scattering albedos may have changed during this period due to different trends in absorbing black carbon and reflecting sulfate aerosols. However, due to the uncertainties in the emission trends, this change cannot be determined with any confidence. Radiative forcing of this aerosol distribution is calculated for several scenarios, resulting in a wide range of uncertainties for top-of-atmosphere (TOA) forcings. Uncertainties in the contribution of the strongly absorbing black carbon aerosol leads to a range in TOA forcings of ca. -0.5 to + 0.1 Wm (exp. -2), while the change in aerosol distributions between 1950 to 1990 leads to a change of -0.1 to -0.3 Wm (exp. -2), for fossil fuel derived aerosol with a "moderate" contribution of black carbon aerosol.

  12. Olivine Weathering aud Sulfate Formation Under Cryogenic Conditions

    NASA Technical Reports Server (NTRS)

    Niles, Paul B.; Golden, D. C.; Michalski, J.

    2013-01-01

    High resolution photography and spectroscopy of the martian surface (MOC, HiRISE) from orbit has revolutionized our view of Mars with one of the most important discoveries being wide-spread layered sedimentary deposits associated with sulfate minerals across the low to mid latitude regions of Mars. The mechanism for sulfate formation on Mars has been frequently attributed to playa-like evaporative environments under prolonged warm conditions. An alternate view of the ancient martian climate contends that prolonged warm temperatures were never present and that the atmosphere and climate has been similar to modern conditions throughout most of its history. This view has had a difficult time explaining the sedimentary history of Mars and in particular the presence of sulfate minerals which seemingly need more water. We suggest here that mixtures of atmospheric aerosols, ice, and dust have the potential for creating small films of cryo-concentrated acidic solutions that may represent an important unexamined environment for understanding weathering processes on Mars. This study seeks to test whether sulfate formation may be possible at temperatures well below 0degC in water limited environments removing the need for prolonged warm periods to form sulfates on early Mars. To test this idea we performed laboratory experiments to simulate weathering of mafic minerals under Mars-like conditions. The weathering rates measured in this study suggest that fine grained olivine on Mars would weather into sulfate minerals in short time periods if they are exposed to H2SO4 aerosols at temperatures at or above -40degC. In this system, the strength of the acidic solution is maximized through eutectic freezing in an environment where the silicate minerals are extremely fine grained and have high surface areas. This provides an ideal environment despite the very low temperatures. On Mars the presence of large deposits of mixed ice and dust is undisputed. The presence of substantial

  13. Direct radiative effect by multicomponent aerosol over China

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

    Huang, Xin; Song, Yu; Zhao, Chun

    The direct radiative effect (DRE) of multiple aerosol species (sulfate, nitrate, ammonium, black carbon (BC), organic carbon (OC), and mineral aerosol) and their spatiotemporal variations over China were investigated using a fully coupled meteorology–chemistry model (WRF-Chem) for the entire year of 2006. We made modifications to improve model performance, including updating land surface parameters, improving the calculation of transition metal-catalyzed oxidation of SO 2, and adding in heterogeneous reactions between mineral aerosol and acid gases. The modified model well reproduced the magnitude, seasonal pattern, and spatial distribution of the measured meteorological conditions, concentrations of PM 10 and its components, andmore » aerosol optical depth (AOD). A diagnostic iteration method was used to estimate the overall DRE of aerosols and contributions from different components. At the land surface, all kinds of aerosol species reduced the incident net radiation flux with a total DRE of 10.2 W m -2 over China. Aerosols significantly warm the atmosphere with the national mean DRE of +10.8 W m -2. BC was the leading radiative-heating component (+8.7 W m -2), followed by mineral aerosol (+1.1 W m -2). At the top of the atmosphere (TOA), BC introduced the largest radiative perturbation (+4.5 W m -2), followed by sulfate (-1.4 W m -2). The overall perturbation of aerosols on radiation transfer is quite small over China, demonstrating the counterbalancing effect between scattering and adsorbing aerosols. Aerosol DRE at the TOA had distinct seasonality, generally with a summer maximum and winter minimum, mainly determined by mass loadings, hygroscopic growth, and incident radiation flux.« less

  14. 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.

  15. Aerosol Remote Sensing from AERONET, the Ground-Based Satellite

    NASA Technical Reports Server (NTRS)

    Holben, Brent N.

    2012-01-01

    Atmospheric particles including mineral dust, biomass burning smoke, pollution from carbonaceous aerosols and sulfates, sea salt, impact air quality and climate. The Aerosol Robotic Network (AERONET) program, established in the early 1990s, is a federation of ground-based remote sensing aerosol networks of Sun/sky radiometers distributed around the world, which provides a long-term, continuous and readily accessible public domain database of aerosol optical (e.g., aerosol optical depth) and microphysical (e.g., aerosol volume size distribution) properties for aerosol characterization, validation of satellite retrievals, and synergism with Earth science databases. Climatological aerosol properties will be presented at key worldwide locations exhibiting discrete dominant aerosol types. Further, AERONET's temporary mesoscale network campaign (e.g., UAE2, TIGERZ, DRAGON-USA.) results that attempt to quantify spatial and temporal variability of aerosol properties, establish validation of ground-based aerosol retrievals using aircraft profile measurements, and measure aerosol properties on compatible spatial scales with satellite retrievals and aerosol transport models allowing for more robust validation will be discussed.

  16. Photochemical organonitrate formation in wet aerosols

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  17. Linkages Between Ozone-depleting Substances, Tropospheric Oxidation and Aerosols

    NASA Technical Reports Server (NTRS)

    Voulgarakis, A.; Shindell, D. T.; Faluvegi, G.

    2013-01-01

    Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (-22.6mW/sq. m for CFCs and -6.7mW/sq. m for N2O) and sulfate aerosols (-3.0mW/sq. m for CFCs and +6.5mW/sq. m for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

  18. 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.

  19. Effect of the eruption of El Chichon stratospheric aerosol size and composition

    NASA Technical Reports Server (NTRS)

    Oberbeck, V. R.; Danielsen, E. F.; Snetsinger, K. G.; Ferry, G. V.; Fong, W.; Hayes, D. M.

    1983-01-01

    Dominant effects of the El Chichon eruption on stratospheric aerosols at 19.8 to 20.7 km are: (1) vapor depositional growth of the small-aerosol (background) mode; (2) development of a large-particle mode by sedimentation from the highest altitudes in the cloud; (3) a change in the large-particle mode from sulfate-coated silicates to sulfate aerosols, some with silicate cores; (4) a 100-fold increase in sulfate mass in the large particle mode. Terminal velocities of large silicate particles, maximum r = 2.3 micron, sampled 1 month after eruption, and calibrated with the aid of lidar data, indicate initial injection to 26 to 27 km. Smaller velocities of sulfate aerosols, median r = 0.5 micron, are compatible with major growth in 2 to 3 months at 27 to 28 km. Aerosol settling accounts for the descent of the main lidar return to 26.5 km in August and to 20 to 21 km in December.

  20. Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

    NASA Astrophysics Data System (ADS)

    Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Shrivastava, Manish; Thomas, Jennie L.

    2017-10-01

    In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain-Fritsch + Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

  1. A Global Data Assimilation System for Atmospheric Aerosol

    NASA Technical Reports Server (NTRS)

    daSilva, Arlindo

    1999-01-01

    We will give an overview of an aerosol data assimilation system which combines advances in remote sensing of atmospheric aerosols, aerosol modeling and data assimilation methodology to produce high spatial and temporal resolution 3D aerosol fields. Initially, the Goddard Aerosol Assimilation System (GAAS) will assimilate TOMS, AVHRR and AERONET observations; later we will include MODIS and MISR. This data assimilation capability will allows us to integrate complementing aerosol observations from these platforms, enabling the development of an assimilated aerosol climatology as well as a global aerosol forecasting system in support of field campaigns. Furthermore, this system provides an interactive retrieval framework for each aerosol observing satellites, in particular TOMS and AVHRR. The Goddard Aerosol Assimilation System (GAAS) takes advantage of recent advances in constituent data assimilation at DAO, including flow dependent parameterizations of error covariances and the proper consideration of model bias. For its prognostic transport model, GAAS will utilize the Goddard Ozone, Chemistry, Aerosol, Radiation and Transport (GOCART) model developed at NASA/GSFC Codes 916 and 910.3. GOCART includes the Lin-Rood flux-form, semi-Langrangian transport model with parameterized aerosol chemistry and physical processes for absorbing (dust and black carbon) and non-absorbing aerosols (sulfate and organic carbon). Observations and model fields are combined using a constituent version of DAO's Physical-space Statistical Analysis System (PSAS), including its adaptive quality control system. In this talk we describe the main components of this assimilation system and present preliminary results obtained by assimilating TOMS data.

  2. A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

    NASA Astrophysics Data System (ADS)

    Sareen, N.; McNeill, V. F.

    2011-12-01

    In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

  3. Easy Volcanic Aerosol (EVA v1.0): an idealized forcing generator for climate simulations

    NASA Astrophysics Data System (ADS)

    Toohey, Matthew; Stevens, Bjorn; Schmidt, Hauke; Timmreck, Claudia

    2016-11-01

    Stratospheric sulfate aerosols from volcanic eruptions have a significant impact on the Earth's climate. To include the effects of volcanic eruptions in climate model simulations, the Easy Volcanic Aerosol (EVA) forcing generator provides stratospheric aerosol optical properties as a function of time, latitude, height, and wavelength for a given input list of volcanic eruption attributes. EVA is based on a parameterized three-box model of stratospheric transport and simple scaling relationships used to derive mid-visible (550 nm) aerosol optical depth and aerosol effective radius from stratospheric sulfate mass. Precalculated look-up tables computed from Mie theory are used to produce wavelength-dependent aerosol extinction, single scattering albedo, and scattering asymmetry factor values. The structural form of EVA and the tuning of its parameters are chosen to produce best agreement with the satellite-based reconstruction of stratospheric aerosol properties following the 1991 Pinatubo eruption, and with prior millennial-timescale forcing reconstructions, including the 1815 eruption of Tambora. EVA can be used to produce volcanic forcing for climate models which is based on recent observations and physical understanding but internally self-consistent over any timescale of choice. In addition, EVA is constructed so as to allow for easy modification of different aspects of aerosol properties, in order to be used in model experiments to help advance understanding of what aspects of the volcanic aerosol are important for the climate system.

  4. Transported acid aerosols measured in southern Ontario

    NASA Astrophysics Data System (ADS)

    Keeler, Gerald J.; Spengler, John D.; Koutrakis, Petros; Allen, George A.; Raizenne, Mark; Stern, Bonnie

    During the period 29 June 1986-9 August 1986, a field health study assessing the acute health effects of air pollutants on children was conducted at a summer girls' camp on the northern shore of Lake Erie in SW Ontario. Continuous air pollution measurements of SO 2, O 3, NO x, particulate sulfates, light scattering, and meteorological measurements including temperature, dew point, and wind speed and direction were made. Twelve-hour integrated samples of size fractioned particles were also obtained using dichotomous samplers and Harvard impactors equipped with an ammonia denuder for subsequent hydrogen ion determination. Particulate samples were analyzed for trace elements by X-ray fluorescence and Neutron Activation, and for organic and elemental carbon by a thermal/optical technique. The measured aerosol was periodically very acidic with observed 12-h averaged H + concentrations in the range < 10-560 nmoles m -3. The aerosol H + appeared to represent the net strong acidity after H 2SO 4 reaction with NH 3(g). Average daytime concentrations were higher than night-time for aerosol H +, sulfate, fine mass and ozone. Prolonged episodes of atmospheric acidity, sulfate, and ozone were associated with air masses arriving at the measurement site from the west and from the southwest over Lake Erie. Sulfate concentrations measured at the lakeshore camp were more than twice those measured at inland sites during extreme pollution episodes. The concentration gradient observed with onshore flow was potentially due to enhanced deposition near the lakeshore caused by discontinuities in the meteorological fields in this region.

  5. Lidar determination of the composition of atmosphere aerosols

    NASA Technical Reports Server (NTRS)

    Wright, M. L.

    1980-01-01

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

  6. Persistent sulfate formation from London Fog to Chinese haze

    PubMed Central

    Wang, Gehui; Zhang, Renyi; Gomez, Mario E.; Yang, Lingxiao; Levy Zamora, Misti; Hu, Min; Lin, Yun; Peng, Jianfei; Guo, Song; Meng, Jingjing; Li, Jianjun; Cheng, Chunlei; Hu, Tafeng; Ren, Yanqin; Wang, Yuesi; Gao, Jian; Cao, Junji; An, Zhisheng; Zhou, Weijian; Li, Guohui; Wang, Jiayuan; Tian, Pengfei; Marrero-Ortiz, Wilmarie; Secrest, Jeremiah; Du, Zhuofei; Zheng, Jing; Shang, Dongjie; Zeng, Limin; Shao, Min; Wang, Weigang; Huang, Yao; Wang, Yuan; Zhu, Yujiao; Li, Yixin; Hu, Jiaxi; Pan, Bowen; Cai, Li; Cheng, Yuting; Ji, Yuemeng; Zhang, Fang; Rosenfeld, Daniel; Liss, Peter S.; Duce, Robert A.; Kolb, Charles E.; Molina, Mario J.

    2016-01-01

    Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO2 by NO2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH3 neutralization or under cloud conditions. Under polluted environments, this SO2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH3 and NO2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world. PMID:27849598

  7. Investigating hygroscopic behavior and phase separation of organic/inorganic mixed phase aerosol particles with FTIR spectroscopy

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Cziczo, D. J.

    2013-12-01

    Atmospheric aerosol particles can be composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have very well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. For example, the deliquescence relative humidity of pure ammonium sulfate is about 80% and its efflorescence point is about 35%. This behavior of ammonium sulfate is important to atmospheric chemistry because some reactions, such as the hydrolysis of nitrogen pentoxide, occur on aqueous but not crystalline surfaces. Deliquescence and efflorescence of simple inorganic salt particles have been investigated by a variety of methods, such as IR spectroscopy, tandem mobility analysis and electrodynamic balance. Field measurements have shown that atmospheric aerosol are not typically a single inorganic salt, instead they often contain organic as well as inorganic species. Mixed inorganic/organic aerosol particles, while abundant in the atmosphere, have not been studied as extensively. Many recent studies have focused on microscopy techniques that require deposition of the aerosol on a glass slide, possibly changing its surface properties. This project investigates the deliquescence and efflorescence points, phase separation and ability to exchange gas-phase components of mixed organic and inorganic aerosol using a flow tube coupled with FTIR spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O:C ratios, including glycerol, 1,2,6-hexanetriol, 1,4-butanediol and 1,5-pentanediol have been investigated. This project aims to study gas-phase exchange in these aerosol systems to determine if exchange is impacted when phase separation occurs.

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

    PubMed

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

    2013-03-19

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

  9. Sensitivity of high-spectral resolution and broadband thermal infrared nadir instruments to the chemical and microphysical properties of secondary sulfate aerosols in the upper-troposphere/lower-stratosphere

    NASA Astrophysics Data System (ADS)

    Sellitto, Pasquale; Legras, Bernard

    2016-04-01

    The observation of upper-tropospheric/lower-stratospheric (UTLS) secondary sulfate aerosols (SSA) and their chemical and microphysical properties from satellite nadir observations (with better spatial resolution than limb observations) is a fundamental tool to better understand their formation and evolution processes and then to estimate their impact on UTLS chemistry, and on regional and global radiative balance. Thermal infrared (TIR) observations are sensitive to the chemical composition of the aerosols due to the strong spectral variations of the imaginary part of the refractive index in this band and, correspondingly, of the absorption, as a function of the composition Then, these observations are, in principle, well adapted to detect and characterize UTLS SSA. Unfortunately, the exploitation of nadir TIR observations for sulfate aerosol layer monitoring is today very limited. Here we present a study aimed at the evaluation of the sensitivity of TIR satellite nadir observations to the chemical composition and the size distribution of idealised UTLS SSA layers. The sulfate aerosol particles are assumed as binary systems of sulfuric acid/water solution droplets, with varying sulphuric acid mixing ratios. The extinction properties of the SSA, for different sulfuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indices taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. High-spectral resolution pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealised aerosol layers, at typical UTLS conditions, on

  10. The optical constants of several atmospheric aerosol species - Ammonium sulfate, aluminum oxide, and sodium chloride

    NASA Technical Reports Server (NTRS)

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

    1976-01-01

    An investigation is conducted of problems which are related to a use of measured optical constants in the simulation of the optical constants of real atmospheric aerosols. The techniques of measuring optical constants are discussed, taking into account transmission measurements through homogeneous and inhomogeneous materials, the immersion of a material in a liquid of a known refractive index, the consideration of the minimum deviation angle of prism measurement, the interference of multiply reflected light, reflectivity measurements, and aspects of mathematical analysis. Graphs show the real and the imaginary part of the refractive index as a function of wavelength for aluminum oxide, NaCl, and ammonium sulfate. Tables are provided for the dispersion parameters and the optical constants.

  11. Balloon profiles of stratospheric NO[sub 2] and HNO[sub 3] for testing the heterogeneous hydrolysis of N[sub 2]O[sub 5] on sulfate aerosols

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

    Webster, C.R.; May, R.D.; Allen, M.

    1994-01-01

    Simultaneous in situ measurements of stratospheric NO[sub 2], HNO[sub 3], HCl, and CH[sub 4] from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS) tunable diode laser spectrometer. Although the measurements of NO[sub 2], HNO[sub 3], and NO[sub 2]/HNO[sub 3] agree well with gas-phase model calculations near 34 km where SAGE II data show little sulfate aerosol, this is not true at the lower altitudes where SAGE II shows high aerosol loadings. At 24 km the BLISS NO[sub 2] and HNO[sub 3] measurements are 70% lower, and 50% higher, respectively,more » than the gas phase model predictions, with a measured NO[sub 2]/HNO[sub 3] ratio 5 times smaller. When the heterogeneous hydrolysis of N[sub 2]O[sub 5] and ClONO[sub 2] on sulfate aerosol of surface area densities matching the SAGE II measurements is added to the model, good agreement with the BLISS measurements is found over the whole altitude range. 24 refs., 4 figs., 1 tab.« less

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

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

  13. Global direct radiative forcing by process-parameterized aerosol optical properties

    NASA Astrophysics Data System (ADS)

    KirkevâG, Alf; Iversen, Trond

    2002-10-01

    A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

  14. Vertical Profiles of Aerosol Volume from High Spectral Resolution Infrared Transmission Measurements: Results

    NASA Technical Reports Server (NTRS)

    Eldering, Annmarie; Kahn, Brian H.; Mills, Franklin P.; Irion, Fredrick W.; Steele, Helen M.; Gunson, Michael R.

    2004-01-01

    The high-resolution infrared absorption spectra of the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment are utilized to derive vertical profiles of sulfate aerosol volume density and extinction coefficient. Following the eruption of Mt. Pinatubo in June 1991, the ATMOS spectra obtained on three Space Shuttle missions (1992, 1993, and 1994) provide a unique opportunity to study the global stratospheric sulfate aerosol layer shortly after a major volcanic eruption and periodically during the decay phase. Synthetic sulfate aerosol spectra are fit to the observed spectra, and a global fitting inversion routine is used to derive vertical profiles of sulfate aerosol volume density. Vertical profiles of sulfate aerosol volume density for the three missions over portions of the globe are presented, with the peak in aerosol volume density occurring from as low as 10 km (polar latitudes) to as high as 20 km (subtropical latitudes). Derived aerosol volume density is as high as 2-3.5 (mu)m(exp 3) per cubic centimeter +/-10% in 1992, decreasing to 0.2-0.5 (mu)m(exp 3) per cubic centimeter +/-20% in 1994, in agreement with other experiments. Vertical extinction profiles derived from ATMOS are compared with profiles from Improved Stratospheric And Mesospheric Sounder (ISAMS) and Cryogenic Limb Array Etalon Spectrometer (CLAES) that coincide in space and time and show good general agreement. The uncertainty of the ATMOS vertical profiles is similar to CLAES and consistently smaller than ISAMS at similar altitudes.

  15. A New WRF-Chem Treatment for Studying Regional Scale Impacts of Cloud-Aerosol Interactions in Parameterized Cumuli

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

    Berg, Larry K.; Shrivastava, ManishKumar B.; Easter, Richard C.

    A new treatment of cloud-aerosol interactions within parameterized shallow and deep convection has been implemented in WRF-Chem that can be used to better understand the aerosol lifecycle over regional to synoptic scales. The modifications to the model to represent cloud-aerosol interactions include treatment of the cloud dropletnumber mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. Thesechanges have beenmore » implemented in both the WRF-Chem chemistry packages as well as the Kain-Fritsch cumulus parameterization that has been modified to better represent shallow convective clouds. Preliminary testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS) as well as a high-resolution simulation that does not include parameterized convection. The simulation results are used to investigate the impact of cloud-aerosol interactions on the regional scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column integrated BC can be as large as -50% when cloud-aerosol interactions are considered (due largely to wet removal), or as large as +35% for sulfate in non-precipitating conditions due to the sulfate production in the parameterized clouds. The modifications to WRF-Chem version 3.2.1 are found to account for changes in the cloud drop number concentration (CDNC) and changes in the chemical composition of cloud-drop residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to WRF-Chem version 3.5, and it is anticipated

  16. Modelled and observed changes in aerosols and surface solar radiation over Europe between 1960 and 2009

    NASA Astrophysics Data System (ADS)

    Turnock, S. T.; Spracklen, D. V.; Carslaw, K. S.; Mann, G. W.; Woodhouse, M. T.; Forster, P. M.; Haywood, J.; Johnson, C. E.; Dalvi, M.; Bellouin, N.; Sanchez-Lorenzo, A.

    2015-08-01

    Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry-climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry-climate model for the period 1960-2009 against extensive ground-based observations of sulfate aerosol mass (1978-2009), total suspended particle matter (SPM, 1978-1998), PM10 (1997-2009), aerosol optical depth (AOD, 2000-2009), aerosol size distributions (2008-2009) and surface solar radiation (SSR, 1960-2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = -0.4), SPM (NMBF = -0.9), PM10 (NMBF = -0.2), aerosol number concentrations (N30 NMBF = -0.85; N50 NMBF = -0.65; and N100 NMBF = -0.96) and AOD (NMBF = -0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of -68 % (-78 %), SPM of -42 % (-20 %), PM10 of -9 % (-8 %) and AOD of -11 % (-14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990-2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m-2 during the period 1970-2009 in response to changes in anthropogenic emissions and aerosol concentrations.

  17. Acidity of fine sulfate particles at Great Smokey Mountains National Park

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

    Day, D.; Malm, W.C.; Kreidenweis, S.

    1995-12-31

    The acidity of ambient particles is of interest from the perspectives of human health, visibility, and ecology. This paper reports on the acidity of fine (< 2.5{mu}m) particles measured during August 1994 at Look Rock observation tower in Great Smokey Mountains National Park. This site is located at latitude 35{degrees} 37 feet 56 inches, longitude 83{degrees} 56 feet 32 inches, and at an elevation of 808m above sea level. All samples were collected using the IMPROVE (Interagency Monitoring of Protected Visual Environments) sampler. The sampling periods included: (1) 4-hour samples collected three times daily with starting times of 8:00 AM,more » 12:00 noon, and 4:00 PM; (2) 12-hour samples collected twice daily with starting times of 8:00 AM and 8:00 PM (all times reported are eastern daylight savings time). The IMPROVE sampler, collecting 4-hour samples, employed a citric acid/glycerol coated annular denuder to remove ammonia gas while the 12-hour sampler did not use a citric acid denuder. The intensive monitoring effort, conducted during August 1994, showed that: (1) the fine aerosol mass is generally dominated by sulfate and its associated water; (2) there was no statistically significant difference in average sulfate concentration between the 12-hour samples nor was there a statistically significant difference in average sulfate concentration between the 4-hour samples; (3) the aerosol is highly acidic, ranging from almost pure sulfuric acid to pure ammonium bisulfate, with an average molar ammonium ion to sulfate ratio of about 0.75 which suggests the ambient sulfate aerosol was a mixture of ammonium bisulfate and sulfuric acid; and (4) there was no statistically significant diurnal variation in particle acidity nor was there a statistically significant difference in particle acidity between the 4 hour samples.« less

  18. Understanding hygroscopic growth and phase transformation of aerosols using single particle Raman spectroscopy in an electrodynamic balance.

    PubMed

    Lee, Alex K Y; Ling, T Y; Chan, Chak K

    2008-01-01

    Hygroscopic growth is one of the most fundamental properties of atmospheric aerosols. By absorbing or evaporating water, an aerosol particle changes its size, morphology, phase, chemical composition and reactivity and other parameters such as its refractive index. These changes affect the fate and the environmental impacts of atmospheric aerosols, including global climate change. The ElectroDynamic Balance (EDB) has been widely accepted as a unique tool for measuring hygroscopic properties and for investigating phase transformation of aerosols via single particle levitation. Coupled with Raman spectroscopy, an EDB/Raman system is a powerful tool that can be used to investigate both physical and chemical changes associated with the hygroscopic properties of individually levitated particles under controlled environments. In this paper, we report the use of an EDB/Raman system to investigate (1) contact ion pairs formation in supersaturated magnesium sulfate solutions; (2) phase transformation in ammonium nitrate/ammonium sulfate mixed particles; (3) hygroscopicity of organically coated inorganic aerosols; and (4) heterogeneous reactions altering the hygroscopicity of organic aerosols.

  19. 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

  20. The Life Cycle of Stratospheric Aerosol Particles

    NASA Technical Reports Server (NTRS)

    Hamill, Patrick; Jensen, Eric J.; Russell, P. B.; Bauman, Jill J.

    1997-01-01

    This paper describes the life cycle of the background (nonvolcanic) stratospheric sulfate aerosol. The authors assume the particles are formed by homogeneous nucleation near the tropical tropopause and are carried aloft into the stratosphere. The particles remain in the Tropics for most of their life, and during this period of time a size distribution is developed by a combination of coagulation, growth by heteromolecular condensation, and mixing with air parcels containing preexisting sulfate particles. The aerosol eventually migrates to higher latitudes and descends across isentropic surfaces to the lower stratosphere. The aerosol is removed from the stratosphere primarily at mid- and high latitudes through various processes, mainly by isentropic transport across the tropopause from the stratosphere into the troposphere.

  1. Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

    DOE PAGES

    Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.; ...

    2017-01-01

    In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain–Fritsch +more » Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.« less

  2. Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

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

    Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.

    In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain–Fritsch +more » Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.« less

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

    DOE PAGES

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

    2015-04-10

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

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

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

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

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

  5. 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 order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type, such as composition, size and hygroscopicity, and to the surrounding atmosphere, such as temperature, relative humidity (RH) and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in-situ atmospheric profiling in the Baltimore, MD-Washington, DC region was performed during fourteen flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 49 %) due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of ammonium sulfate increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity causing an increase in the water content of the aerosol. Conversely, low aerosol loading days had lower ammonium sulfate and higher black carbon contributions causing lower single scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km decreasing to 35 ng m-3

  6. Fine Iron Aerosols Are Internally Mixed with Nitrate in the Urban European Atmosphere.

    PubMed

    Dall'Osto, Manuel; Beddows, D C S; Harrison, Roy M; Onat, Burcu

    2016-04-19

    Atmospheric iron aerosol is a bioavailable essential nutrient playing a role in oceanic productivity. Using aerosol time-of-flight mass spectrometry (ATOFMS), the particle size (0.3-1.5 μm), chemical composition and mixing state of Fe-containing particles collected at two European urban sites (London and Barcelona) were characterized. Out of the six particle types accounting for the entire Fe-aerosol population, that arising from long-range transport (LRT) of fine Fe-containing particles (Fe-LRT, 54-82% across the two sites) was predominant. This particle type was found to be internally mixed with nitrate and not with sulfate, and likely mostly associated with urban traffic activities. This is in profound contrast with previous studies carried out in Asia, where the majority of iron-containing particles are mixed with sulfate and are of coal combustion origin. Other minor fine iron aerosol sources included mineral dust (8-11%), traffic brake wear material (1-17%), shipping/oil (1-6%), biomass combustion (4-13%) and vegetative debris (1-3%). Overall, relative to anthropogenic Asian Fe-sulfate dust, anthropogenic European dust internally mixed with additional key nutrients such as nitrate is likely to play a different role in ocean global biogeochemical cycles.

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

    NASA Astrophysics Data System (ADS)

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

    2016-12-01

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

  8. 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...

  9. Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere.

    PubMed

    Shaheen, Robina; Abaunza, Mariana M; Jackson, Teresa L; McCabe, Justin; Savarino, Joël; Thiemens, Mark H

    2014-08-19

    Sulfur-isotopic anomalies have been used to trace the evolution of oxygen in the Precambrian atmosphere and to document past volcanic eruptions. High-precision sulfur quadruple isotope measurements of sulfate aerosols extracted from a snow pit at the South Pole (1984-2001) showed the highest S-isotopic anomalies (Δ(33)S = +1.66‰ and Δ(36)S = +2‰) in a nonvolcanic (1998-1999) period, similar in magnitude to Pinatubo and Agung, the largest volcanic eruptions of the 20th century. The highest isotopic anomaly may be produced from a combination of different stratospheric sources (sulfur dioxide and carbonyl sulfide) via SOx photochemistry, including photoexcitation and photodissociation. The source of anomaly is linked to super El Niño Southern Oscillation (ENSO) (1997-1998)-induced changes in troposphere-stratosphere chemistry and dynamics. The data possess recurring negative S-isotope anomalies (Δ(36)S = -0.6 ± 0.2‰) in nonvolcanic and non-ENSO years, thus requiring a second source that may be tropospheric. The generation of nonvolcanic S-isotopic anomalies in an oxidizing atmosphere has implications for interpreting Archean sulfur deposits used to determine the redox state of the paleoatmosphere.

  10. Multidecadal trends in aerosol radiative forcing over the Arctic: Contribution of changes in anthropogenic aerosol to Arctic warming since 1980

    NASA Astrophysics Data System (ADS)

    Breider, Thomas J.; Mickley, Loretta J.; Jacob, Daniel J.; Ge, Cui; Wang, Jun; Payer Sulprizio, Melissa; Croft, Betty; Ridley, David A.; McConnell, Joseph R.; Sharma, Sangeeta; Husain, Liaquat; Dutkiewicz, Vincent A.; Eleftheriadis, Konstantinos; Skov, Henrik; Hopke, Phillip K.

    2017-03-01

    Arctic observations show large decreases in the concentrations of sulfate and black carbon (BC) aerosols since the early 1980s. These near-term climate-forcing pollutants perturb the radiative balance of the atmosphere and may have played an important role in recent Arctic warming. We use the GEOS-Chem global chemical transport model to construct a 3-D representation of Arctic aerosols that is generally consistent with observations and their trends from 1980 to 2010. Observations at Arctic surface sites show significant decreases in sulfate and BC mass concentrations of 2-3% per year. We find that anthropogenic aerosols yield a negative forcing over the Arctic, with an average 2005-2010 Arctic shortwave radiative forcing (RF) of -0.19 ± 0.05 W m-2 at the top of atmosphere (TOA). Anthropogenic sulfate in our study yields more strongly negative forcings over the Arctic troposphere in spring (-1.17 ± 0.10 W m-2) than previously reported. From 1980 to 2010, TOA negative RF by Arctic aerosol declined, from -0.67 ± 0.06 W m-2 to -0.19 ± 0.05 W m-2, yielding a net TOA RF of +0.48 ± 0.06 W m-2. The net positive RF is due almost entirely to decreases in anthropogenic sulfate loading over the Arctic. We estimate that 1980-2010 trends in aerosol-radiation interactions over the Arctic and Northern Hemisphere midlatitudes have contributed a net warming at the Arctic surface of +0.27 ± 0.04 K, roughly one quarter of the observed warming. Our study does not consider BC emissions from gas flaring nor the regional climate response to aerosol-cloud interactions or BC deposition on snow.

  11. Online and offline mass spectrometric study of the impact of oxidation and ageing on glyoxal chemistry and uptake onto ammonium sulfate aerosols.

    PubMed

    Hamilton, Jacqueline F; Baeza-Romero, M Teresa; Finessi, Emanuela; Rickard, Andrew R; Healy, Robert M; Peppe, Salvatore; Adams, Thomas J; Daniels, Mark J S; Ball, Stephen M; Goodall, Iain C A; Monks, Paul S; Borrás, Esther; Muñoz, Amalia

    2013-01-01

    Recent laboratory and modelling studies have shown that reactive uptake of low molecular weight alpha-dicarbonyls such as glyoxal (GLY) by aerosols is a potentially significant source of secondary organic aerosol (SOA). However, previous studies disagree in the magnitude of the uptake of GLY, the mechanism involved and the physicochemical factors affecting particle formation. In this study, the chemistry of GLY with ammonium sulfate (AS) in both bulk laboratory solutions and in aerosol particles is investigated. For the first time, Aerosol Time of Flight Mass Spectrometry (ATOFMS), a single particle technique, is used together with offline (ESI-MS and LC-MS2) mass spectrometric techniques to investigate the change in composition of bulk solutions of GLY and AS resulting from aqueous photooxidation by OH and from ageing of the solutions in the dark. The mass spectral ions obtained in these laboratory studies were used as tracers of GLY uptake and chemistry in AS seed particles in a series of experiments carried out under dark and natural irradiated conditions at the outdoor European Photo-reactor (EUPHORE). Glyoxal oligomers formed were not detected by the ATOFMS, perhaps due to inefficient absorption at the laser wavelength. However, the presence of organic nitrogen compounds, formed by reaction of GLY with ammonia was confirmed, resulting in an increase in the absorption efficiency of the aerosol, and this increased the number of particles successfully ionised by the ATOFMS. A number of light absorbing organic nitrogen species, including 1H-imidazole, 1H-imidazole-2-carboxaldehyde, 2,2'-bis-imidazole and a glyoxal substituted 2,2'-bisimidazole, previously identified in aqueous laboratory solutions, were also identified in chamber aerosol and formed on atmospherically relevant timescales. An additional compound, predicted to be 1,2,5-oxadiazole, had an enhanced formation rate when the chamber was open and is predicted to be formed via a light activated pathway

  12. Uptake of Organic Vapors by Sulfate Aerosols: Physical and Chemical Processes

    NASA Technical Reports Server (NTRS)

    Michelsen, R. R.; Ashbourn, S. F. M.; Iraci, L.T.; Staton, S. J. R.

    2003-01-01

    While it is known that upper tropospheric sulfate particles contain a significant amount of organic matter, both the source of the organic fraction and its form in solution are unknown. These studies explore how the chemical characteristics of the molecules and surfaces in question affect heterogeneous interactions. The solubilities of acetaldehyde [CH3CHO] and ethanol [CH3CH20H] in cold, aqueous sulfuric acid solutions have been measured by Knudsen cell studies. Henry's law solubility coefficients range from 10(exp 2) to 10(exp 5) M/atm for acetaldehyde, and from 10(exp 4) to 10(exp 9) M/atm for ethanol under upper tropospheric conditions (210-240 K, 40-80 wt. % H2S04). The multiple solvation pathways (protonation, enolization, etc.) available to these compounds in acidic aqueous environments will be discussed. Preliminary results from the interaction of acetaldehyde with solutions of formaldehyde in sulfuric acid will be presented as well. The physical and chemical processes that affect organic uptake by aqueous aerosols will be explored, with the aim of evaluating organic species not yet studied in low temperature aqueous sulfuric acid.

  13. Impact of dimethylsulfide chemistry on sulfate over the Northern Hemisphere

    EPA Science Inventory

    Sulfate aerosol forms from the gas- and aqueous-phase oxidation of sulfur dioxide and is an important component of atmospheric aerosols. Dimethylsulfide (DMS) present in sea-water can be emitted into the atmosphere which can then react with atmospheric oxidants to produce sulfur ...

  14. Development of a new corona discharge based ion source for high resolution time-of-flight chemical ionization mass spectrometer to measure gaseous H2SO4 and aerosol sulfate

    NASA Astrophysics Data System (ADS)

    Zheng, Jun; Yang, Dongsen; Ma, Yan; Chen, Mindong; Cheng, Jin; Li, Shizheng; Wang, Ming

    2015-10-01

    A new corona discharge (CD) based ion source was developed for a commercial high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS) (Aerodyne Research Inc.) to measure both gaseous sulfuric acid (H2SO4) and aerosol sulfate after thermal desorption. Nitrate core ions (NO3-) were used as reagent ions and were generated by a negative discharge in zero air followed by addition of excess nitrogen dioxide (NO2) to convert primary ions and hydroxyl radicals (OH) into NO3- ions and nitric acid (HNO3). The CD-HRToF-CIMS showed no detectable interference from hundreds parts per billion by volume (ppbv) of sulfur dioxide (SO2). Unlike the atmospheric pressure ionization (API) ToF-CIMS, the CD ion source was integrated onto the ion-molecule reaction (IMR) chamber and which made it possible to measure aerosol sulfate by coupling to a filter inlet for gases and aerosols (FIGAERO). Moreover, compared with a quadrupole-based mass spectrometer, the desired HSO4- signal was detected by its exact mass of m/z 96.960, which was well resolved from the potential interferences of HCO3-ṡ(H2O)2 (m/z 97.014) and O-ṡH2OṡHNO3 (m/z 97.002). In this work, using laboratory-generated standards the CD-HRToF-CIMS was demonstrated to be able to detect as low as 3.1 × 105 molecules cm-3 gaseous H2SO4 and 0.5 μg m-3 ammonium sulfate based on 10-s integration time and two times of the baseline noise. The CD ion source had the advantages of low cost and a simple but robust structure. Since the system was non-radioactive and did not require corrosive HNO3 gas, it can be readily field deployed. The CD-HRToF-CIMS can be a powerful tool for both field and laboratory studies of aerosol formation mechanism and the chemical processes that were critical to understand the evolution of aerosols in the atmosphere.

  15. Analysis of Anions in Ambient Aerosols by Microchip Capillary Electrophoresis

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

    Liu, Yan; MacDonald, David A.; Yu, Xiao-Ying

    2006-10-01

    We describe a microchip capillary electrophoresis method for the analysis of nitrate and sulfate in ambient aerosols. Investigating the chemical composition of ambient aerosol particles is essential for understanding their sources and effects. Significant progress has been made towards developing mass spectrometry-based instrumentation for rapid qualitative analysis of aerosols. Alternative methods for rapid quantification of selected high abundance compounds are needed to augment the capacity for widespread routine analysis. Such methods could provide much higher temporal and spatial resolution than can be achieved currently. Inorganic anions comprise a large percentage of particulate mass with nitrate and sulfate among the mostmore » abundant species. While ion chromatography has proven very useful for analyzing extracts of time-integrated ambient aerosol samples collected on filters and for semi-continuous, on-line particle composition measurements, there is a growing need for development of new compact, inexpensive approaches to routine on-line aerosol ion analysis for deployment in spatially dense, atmospheric measurement networks. Microchip capillary electrophoresis provides the necessary speed and portability to address this need. In this report, on-column contact conductivity detection is used with hydrodynamic injection to create a simple microchip instrument for analysis of nitrate and sulfate. On-column contact conductivity detection was achieved using a Pd decoupler placed upstream from the working electrodes. Microchips containing two Au or Pd working electrodes showed a good linear range (5-500 µM) and low limits-of-detection for sulfate and nitrate with Au providing the lowest detection limits (1 µM) for both ions. The completed microchip system was used to analyze ambient aerosol filter samples. Nitrate and sulfate concentrations measured by the microchip matched the concentrations measured by ion chromatography.« less

  16. AOD Distributions and Trends of Major Aerosol Species over a Selection of the World's Most Populated Cities Based on the 1st Version of NASA's MERRA Aerosol Reanalysis

    NASA Technical Reports Server (NTRS)

    Provencal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

    2017-01-01

    NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to

  17. AOD distributions and trends of major aerosol species over a selection of the world's most populated cities based on the 1st Version of NASA's MERRA Aerosol Reanalysis.

    PubMed

    Provençal, Simon; Kishcha, Pavel; da Silva, Arlindo M; Elhacham, Emily; Alpert, Pinhas

    2017-06-01

    NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to

  18. Seasonal variations in the physico-chemical characteristics of aerosols in North Taiwan

    NASA Astrophysics Data System (ADS)

    Chou, Charles

    2014-05-01

    From 2007 to 2012, this study investigated the mass concentration and chemical composition of ambient aerosols (i.e. PM10, PM2.5, and PMc = PM10-PM2.5) at Cape Fuguei, Yangminshan, and NTU (National Taiwan University) stations in northern Taiwan. It was found that the concentration and composition of aerosols exhibited significant seasonal variations but without an inter-annual trend during the study period. Moderate correlations (R2 = 0.4-0.6) were observed among the aerosol concentrations at the respective stations, indicating that the aerosol concentrations were dominated by factors on regional scales. During the seasons of northeasterly winter monsoons, long range transport of dust and particulate air pollutants from the Asia Continent had negatively impacted the atmospheric environment in this area. On the other hand, as a highly developed urban area, Taipei has substantial local emissions of air pollutants that should have transported to the surrounding areas of Taipei basin and caused deterioration of air quality and visibility in Cape Fuguei and Yangminshan. The results indicated that the major components of aerosols in Taipei include sulfate, sea salts, dust, and organic matters. In addition, contributions from nitrate, ammonium, and elemental carbon were also significant. In terms of mass concentration, most of the sea salts and dust particles existed in the coarse mode of aerosols, whereas sulfate and EC were confined within PM2.5. This suggests that the dust and sea salts particles were externally mixed with EC and sulfate in the aerosols over Taipei area. Further, it was found that nitrate were closely associated with sea salts in aerosols, suggesting the reaction between nitric acid and sea salt particles. Different seasonality was observed for sea salt and dust: sea salts peaked in fall and dust reached the maximal level in springtime, implying their sources were regulated by independent seasonal factors. Particulate pollutants (i.e. sulfate, nitrate

  19. Sulfate Aerosol in the Arctic: Source Attribution and Radiative Forcing

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

    Yang, Yang; Wang, Hailong; Smith, Steven J.

    Source attributions of Arctic sulfate and its direct radiative effect for 2010–2014 are quantified in this study using the Community Earth System Model (CESM) equipped with an explicit sulfur source-tagging technique. Regions that have high emissions and/or are near/within the Arctic present relatively large contributions to Arctic sulfate burden, with the largest contribution from sources in East Asia (27%). East Asia and South Asia together have the largest contributions to Arctic sulfate concentrations at 9–12 km, whereas sources within or near the Arctic account largely below 2 km. For remote sources with strong emissions, their contributions to Arctic sulfate burdenmore » are primarily driven by meteorology, while contributions of sources within or near the Arctic are dominated by their emission strength. The sulfate direct radiative effect (DRE) is –0.080 W m-2 at the Arctic surface, offsetting the net warming effect from the combination of in-snow heating and DRE cooling from black carbon. East Asia, Arctic local and Russia/Belarus/Ukraine sources contribute –0.017, –0.016 and –0.014 W m-2, respectively, to Arctic sulfate DRE. A 20% reduction in anthropogenic SO2 emissions leads to a net increase of +0.013 W m-2 forcing at the Arctic surface. These results indicate that a joint reduction in BC emissions could prevent possible Arctic warming from future reductions in SO2 emissions. Sulfate DRE efficiency calculations suggest that short transport pathways together with meteorology favoring long sulfate lifetimes make certain sources more efficient in influencing the Arctic sulfate DRE.« less

  20. Two-Column Aerosol Project (TCAP) Field Campaign Report

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

    Berg, Larry K

    This study included the deployment of the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Mobile Facility (AMF), ARM Mobile Aerosol Observing System (MAOS) and the ARM Aerial Facility (AAF). The study was a collaborative effort involving scientists from DOE national laboratories, NOAA, NASA, and universities. The AAF and MAOS were deployed for two approximately month-long Intensive Operational Periods (IOPs) conducted in June 2012 and February 2013. Seasonal differences in the aerosol chemical and optical properties observed using the AMF, AAF, and MAOS are presented in this report. The total mass loading of aerosol is found tomore » be much greater in the summer than in the winter, with the difference associated with greater amounts of organic aerosol. The mass fraction of organic aerosol is much reduced in the winter, when sulfate is the dominant aerosol type. Surprisingly, very little sea-salt aerosol was observed in the summer. In contrast, much more sea salt aerosol was observed in the winter. The mass loading of black carbon is nearly the same in both seasons. These differences lead to a relative increase in the aerosol light absorption in the winter and an associated decrease in observed single-scattering albedo. Measurements of aerosol mixing state were made using a single-particle mass spectrometer, which showed that the majority of the summertime aerosol consisted of organic compounds mixed with various amounts of sulfate. A number of other findings are also summarized in the report, including: impact of aerosol layers aloft on the column aerosol optical depth; documentation of the aerosol properties at the AMF; differences in the aerosol properties associated with both columns, which are not systematic but reflect the complicated meteorological and chemical processes that impact aerosol as it is advected away from North America; and new instruments and data-processing techniques for measuring both

  1. Production of Highly Charged Pharmaceutical Aerosols Using a New Aerosol Induction Charger

    PubMed Central

    Golshahi, Laleh; Longest, P. Worth; Holbrook, Landon; Snead, Jessica; Hindle, Michael

    2015-01-01

    Purpose Properly charged particles can be used for effective lung targeting of pharmaceutical aerosols. The objective of this study was to characterize the performance of a new induction charger that operates with a mesh nebulizer for the production of highly charged submicrometer aerosols to bypass the mouth-throat and deliver clinically relevant doses of medications to the lungs. Methods Variables of interest included combinations of model drug (i.e. albuterol sulfate) and charging excipient (NaCl) as well as strength of the charging field (1–5 kV/cm). Aerosol charge and size were measured using a modified electrical low pressure impactor system combined with high performance liquid chromatography. Results At the approximate mass median aerodynamic diameter (MMAD) of the aerosol (~ 0.4 μm), the induction charge on the particles was an order of magnitude above the field and diffusion charge limit. The nebulization rate was 439.3 ± 42.9 μl/min, which with a 0.1 % w/v solution delivered 419.5 ± 34.2 μg of medication per minute. A new correlation was developed to predict particle charge produced by the induction charger. Conclusions The combination of the aerosol induction charger and predictive correlations will allow for the practical generation and control of charged submicrometer aerosols for targeting deposition within the lungs. PMID:25823649

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

    NASA Astrophysics Data System (ADS)

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

    2016-01-01

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

  3. Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Lohmann, U.; Hoose, C.

    2009-11-01

    Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m-2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

  4. Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Lohmann, U.; Hoose, C.

    2009-07-01

    Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m-2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

  5. Reducing the Uncertainties in Direct Aerosol Radiative Forcing

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.

    2011-01-01

    Airborne particles, which include desert and soil dust, wildfire smoke, sea salt, volcanic ash, black carbon, natural and anthropogenic sulfate, nitrate, and organic aerosol, affect Earth's climate, in part by reflecting and absorbing sunlight. This paper reviews current status, and evaluates future prospects for reducing the uncertainty aerosols contribute to the energy budget of Earth, which at present represents a leading factor limiting the quality of climate predictions. Information from satellites is critical for this work, because they provide frequent, global coverage of the diverse and variable atmospheric aerosol load. Both aerosol amount and type must be determined. Satellites are very close to measuring aerosol amount at the level-of-accuracy needed, but aerosol type, especially how bright the airborne particles are, cannot be constrained adequately by current techniques. However, satellite instruments can map out aerosol air mass type, which is a qualitative classification rather than a quantitative measurement, and targeted suborbital measurements can provide the required particle property detail. So combining satellite and suborbital measurements, and then using this combination to constrain climate models, will produce a major advance in climate prediction.

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

    NASA Astrophysics Data System (ADS)

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

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

  7. Microphysical processes affecting stratospheric aerosol particles

    NASA Technical Reports Server (NTRS)

    Hamill, P.; Toon, O. B.; Kiang, C. S.

    1977-01-01

    Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

  8. Aerosol Composition and Variability in Baltimore Measured during DISCOVER-AQ

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

    In order to relate satellite-based measurements of aerosols to ground-level air quality, the correlation between aerosol optical properties (wavelength-dependent scattering and absorption measured by satellites) and mass measurements of aerosol loading (i.e. PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type (such as composition, size, hygroscopicity, and mass scattering and absorption efficiencies) and to the surrounding atmosphere (such as temperature, relative humidity and altitude). The DISCOVER-AQ (Deriving Information on Surface conditions from COlumn and VERtically resolved observations relevant to Air Quality) project was designed to provide a unique dataset for determining variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Extensive in-situ profiling of the lower atmosphere in the Baltimore-Washington D.C. region was performed during fourteen flights during July 2011. Identical flight plans and profile locations throughout the campaign provide meaningful statistics for analysis. Measured aerosol mass was composed primarily of ammonium sulfate (campaign average of 36%) and water-soluble organics (58%). A distinct difference in composition was related to aerosol loading with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 60%). This composition shift causes a change in the water-uptake potential (hygroscopicity) of the aerosols with higher relative organic composition decreasing water-uptake. On average, sulfate mass increased during the day due to increased photochemistry, while organics decreased. Analysis of the linkage between aerosol loading and optical properties was also performed. The absorption by black carbon was dependent on the amount of organic coating with an increase in mass absorption efficiency from 7.5 m2/g for bare soot to 16 m2/g at an

  9. [Composition and source of atmosphere aerosol water soluble ions over the East China Sea in winter].

    PubMed

    He, Yu-Hui; Yang, Gui-Peng; Zhang, Hong-Hai

    2011-08-01

    With the ion chromatographic method, the water-soluble ion concentrations of Cl(-), NO3(-), SO4(2-) , CH3SO3(-) (MSA), Na+, K+, NH4+, Mg2+ and Ca2+ in the atmospheric aerosol over the East China Sea in winter 2009 was determined and the sources of these ions was investigated through correlation analysis by SPSS (statistical package for social sciences) software. The results indicated that the concentrations of secondary ions in aerosol were the highest (non-sea-salt sulfates nss-SO4(2-), NO3(-), NH4+), accounting for 78.4% of total determining ions. The calculation results of equivalent concentration of anions and cations showed that the acid ions of aerosol were neutralized inadequately. The stoichiometry of NH4+ in different compounds showed that NH4HSO4 was the main binding form of NH4+ and SO4(2-) in the aerosol. The concentration of methanesulfonic acid (MSA) was low, and the average value was (0.0088 +/- 0.0037) microg x m(-3). According to calculation, the contribution of sea-salt sulfates was 4.5% to total sulfates, and that of biogenous sulfates was 1.4% to non-sea-salt sulfate (nss-SO4(2-)), showing that human input was the main source of sulfates in aerosol over the East China Sea. In addition, nss-SO4(2-)/NO3(-) in the aerosol was 1.08, reflecting that China's energy structure adjustment played an important role in recent years.

  10. Impacts of aerosol-cloud interactions on past and future changes in tropospheric composition

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

    Unger, N.; Menon, S.; Shindell, D. T.

    2009-02-02

    The development of effective emissions control policies that are beneficial to both climate and air quality requires a detailed understanding of all the feedbacks in the atmospheric composition and climate system. We perform sensitivity studies with a global atmospheric composition-climate model to assess the impact of aerosols on tropospheric chemistry through their modification on clouds, aerosol-cloud interactions (ACI). The model includes coupling between both tropospheric gas-phase and aerosol chemistry and aerosols and liquid-phase clouds. We investigate past impacts from preindustrial (PI) to present day (PD) and future impacts from PD to 2050 (for the moderate IPCC A1B scenario) that embracemore » a wide spectrum of precursor emission changes and consequential ACI. The aerosol indirect effect (AIE) is estimated to be -2.0 Wm{sup -2} for PD-PI and -0.6 Wm{sup -2} for 2050-PD, at the high end of current estimates. Inclusion of ACI substantially impacts changes in global mean methane lifetime across both time periods, enhancing the past and future increases by 10% and 30%, respectively. In regions where pollution emissions increase, inclusion of ACI leads to 20% enhancements in in-cloud sulfate production and {approx}10% enhancements in sulfate wet deposition that is displaced away from the immediate source regions. The enhanced in-cloud sulfate formation leads to larger increases in surface sulfate across polluted regions ({approx}10-30%). Nitric acid wet deposition is dampened by 15-20% across the industrialized regions due to ACI allowing additional re-release of reactive nitrogen that contributes to 1-2 ppbv increases in surface ozone in outflow regions. Our model findings indicate that ACI must be considered in studies of methane trends and projections of future changes to particulate matter air quality.« less

  11. 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.

  12. The boiling point of stratospheric aerosols.

    NASA Technical Reports Server (NTRS)

    Rosen, J. M.

    1971-01-01

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

  13. AOD distributions and trends of major aerosol species over a selection of the world’s most populated cities based on the 1st Version of NASA’s MERRA Aerosol Reanalysis

    PubMed Central

    Provençal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

    2018-01-01

    NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003–2015) and over a selection of 200 of the world’s most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don’t tend

  14. Aerosol Absorption in the Atmosphere: Perspectives from Global Model, Ground-Based Measurements, and Field Observations

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Dubovik, Oleg; Holben, Brent; Torres, Omar; Anderson, Tad; Quinn, Patricia; Ginoux, Paul

    2004-01-01

    Aerosol absorption in the atmosphere poses a major uncertainty in assessing the aerosol climate effects. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, and our limited knowledge of aerosol mixing state and optical properties. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt. We compare the model calculated total aerosol optical thickness, extinction, and absorption with those quantities from the ground-based sun photometer measurements from AERONET, satellite retrievals from the TOMS instrument, and field observations from ACE-Asia. We will examine the most sensitive factors in determining the aerosol absorption. and the consequences of assessing the aerosol radiative forcing and atmospheric heating associated with those factors.

  15. Aerosol Absorption in the Atmosphere: Perspectives from Global Model, Ground-Based Measurements, and Field Observations

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Dubovik, Oleg; Holben, Brent; Anderson, Tad; Quinn, Patricia; Duncan, Bryan; Ginoux, Paul

    2003-01-01

    Aerosol absorption in the atmosphere poses a major uncertainty in assessing the aerosol climate effects. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, and our limited knowledge of aerosol mixing state and optical properties. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt. We compare the model calculated total aerosol optical thickness, extinction, and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia. We will examine what are the most sensitive factors in determining the aerosol absorption, and the consequences of assessing the aerosol radiative forcing and atmospheric heating associated with those factors.

  16. Aerosol Absorption in the Atmosphere: Perspectives from Global Model, Ground-Based Measurements, and Field Observations

    NASA Technical Reports Server (NTRS)

    Chin, Main; Dubovik, Oleg; Holben, Brent; Anderson, Tad; Quinn, Patricia; Duncan, Bryan; Ginoux, Paul

    2004-01-01

    Aerosol absorption in the atmosphere poses a major uncertainty in assessing the aerosol climate effects. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, and our limited knowledge of aerosol mixing state and optical properties. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt. We compare the model calculated total aerosol optical thickness, extinction, and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia. We will examine the most sensitive factors in determining the aerosol absorption, and the consequences of assessing the aerosol radiative forcing and atmospheric heating associated with those factors.

  17. Formation of aqueous-phase sulfate during the haze period in China: Kinetics and atmospheric implications

    NASA Astrophysics Data System (ADS)

    Zhang, Haijie; Chen, Shilu; Zhong, Jie; Zhang, Shaowen; Zhang, Yunhong; Zhang, Xiuhui; Li, Zesheng; Zeng, Xiao Cheng

    2018-03-01

    Sulfate is one of the most important components in the aerosol due to its key role in air pollution and global climate change. Recent work has suggested that reactive nitrogen chemistry in aqueous water can explain the missing source of sulfate in the aqueous water. Herein, we have mapped out the energy profile of the oxidization process of SO2 leading from NO2 and two feasible three-step mechanisms have been proposed. For the oxidation of HOSO2- and HSO3- by the dissolved NO2 in weakly acidic and neutral aerosol (pH ≤ 7), the main contribution to the missing sulfate production comes from the oxidation of HOSO2-. The whole process is a self-sustaining process. For the oxidation of SO32- in alkaline aerosol (pH > 7), the third step - decomposition step of H2O or hydrolysis of SO3 step which are two parallel processes are the rate-limiting steps. The present results are of avail to better understand the missing source of sulfate in the aerosol and hence may lead to better science-based solutions for resolving the severe haze problems in China.

  18. Efflorescence relative humidity for ammonium sulfate particles.

    PubMed

    Gao, Yonggang; Chen, Shing Bor; Yu, Liya E

    2006-06-22

    The classical homogeneous nucleation theory was employed to calculate the efflorescence relative humidity (ERH) of airborne ammonium sulfate particles with a wide size range (8 nm to 17 microm) at room temperature. The theoretical predictions are in good agreement with the experimentally measured values. When the ammonium sulfate particle is decreased in size, the ERH first decreases, reaches a minimum around 30% for particle diameter equal to about 30 nm, and then increases. It is for the first time that the Kelvin effect is theoretically verified to substantially affect the ERH of ammonium sulfate particles smaller than 30 nm, while the aerosol size is the dominant factor affecting the efflorescent behavior of ammonium sulfate particles larger than 50 nm.

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

    NASA Astrophysics Data System (ADS)

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

    2017-10-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

  1. Impacts of Four SO2 Oxidation Pathways on Wintertime Sulfate Concentrations

    NASA Astrophysics Data System (ADS)

    Sarwar, G.; Fahey, K.; Zhang, Y.; Kang, D.; Mathur, R.; Xing, J.; Wei, C.; Cheng, Y.

    2017-12-01

    Air quality models tend to under-estimate winter-time sulfate concentrations compared to observed data. Such under-estimations are particularly acute in China where very high concentrations of sulfate have been measured. Sulfate is produced by oxidation of sulfur dioxide (SO2) in gas-phase by hydroxyl radical and in aqueous-phase by hydrogen peroxide, ozone, etc. and most air quality models employ such typical reactions. Several additional SO2 oxidation pathways have recently been proposed. Heterogeneous reaction on dust has been suggested to be an important sink for SO2. Oxidation of SO2 on fine particles in presence of nitrogen dioxide (NO2) and ammonia (NH3) at high relative humidity has been implicated for sulfate formation in Chinese haze and London fog. Reactive nitrogen chemistry in aerosol water has also been suggested to produce winter-time sulfate in China. Specifically, high aerosol water can trap SO2 which can be subsequently oxidized by NO2 to form sulfate. Aqueous-phase (in-cloud) oxidation of SO2 by NO2 can also produce sulfate. Here, we use the hemispheric Community Multiscale Air Quality (CMAQ) modeling system to examine the potential impacts of these SO2 oxidation pathways on sulfate formation. We use anthropogenic emissions from the Emissions Database for Global Atmospheric Research and biogenic emissions from Global Emissions InitiAtive. We performed simulations without and with these SO2 oxidation pathways for October-December of 2014 using meteorological fields obtained from the Weather Research and Forecasting model. The standard CMAQ model contains one gas-phase chemical reaction and five aqueous-phase chemical reactions for SO2 oxidation. We implement four additional SO2 oxidation pathways into the CMAQ model. Our preliminary results suggest that the dust chemistry enhances mean sulfate over parts of China and Middle-East, the in-cloud SO2 oxidation by NO2 enhances sulfate over parts of western Europe, oxidation of SO2 by NO2 and NH3 on

  2. Summer aerosol particle mixing in different climate and source regions of the United Arab Emirates (UAE)

    NASA Astrophysics Data System (ADS)

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

    2005-12-01

    The high aerosol loadings over the UAE reflect local to regional natural and anthropogenic pollution sources. To understand the impact of the high levels of pollution on both local and global climate systems, aerosol characterization flights in summer 2002 were used to sample major source areas, and to provide information on the interaction of aerosol particles within different geographic regions of the UAE. Atmospheric information and aerosol samples were collected from the marine/oil-industry region, NW coastal industries and cities, Oman Mountain Range, and NE coastal region. Aerosol samples were collected with multi-stage impactors and were analysed later using transmission electron microscopy. All samples are dominated by mineral grains or mineral aggregates in the coarse-mode fraction, and ammonium sulfate droplets in the fine-mode fraction. Differences in the types of mineral grains (different regional desert sources), inorganic salt and soot fractions, and types of internally mixed particles occur between regions. Oil-related industry sites have an abundance of coated and internally mixed particles, including sulfate-coated mineral grains, and mineral aggregates with chloride and sulfate. Cities have slightly elevated soot fractions, and typically have metal oxides. The NE coastal area is characterized by high soot fractions (local shipping) and mixed volatile droplets (regional Asian pollution). Particle populations within the convection zone over the Oman Mountain Range comprise an external mixture of particles from NW and NE sources, with many deliquesced particles. Both land-sea breezes in the NW regions and convection systems in the mountains mix aerosol particles from different local and regional sources, resulting in the formation of abundant internally mixed particles. The interaction between desert dust and anthropogenic pollution, and in particular the formation of mineral aggregates with chloride and sulfate, enhances the coarse-mode fraction and

  3. Some considerations on the washout of sulfate from stack plumes

    Treesearch

    Leonard K. Peters

    1976-01-01

    A theoretical analysis of the contribution to rainwater sulfate concentration by precipitation scavenging of gaseous SO2 and sulfate containing aerosols is presented. Aspects, such as the proper choice of mean raindrop diameter, are discussed in detail, and guidelines for their use are explored. Sample calculations are provided in which emissions...

  4. Isotopic mass independent signature of black crusts: a proxy for atmospheric aerosols formation in the Paris area (France).

    NASA Astrophysics Data System (ADS)

    Genot, Isabelle; Martin, Erwan; Yang, David Au; De Rafelis, Marc; Cartigny, Pierre; Wing, Boswell; Le Gendre, Erwann; Bekki, Slimane

    2016-04-01

    In view of the negative forcing of the sulfate aerosols on climate, a more accurate understanding of the formation of these particles is crucial. Indeed, despite the knowledge of their effects, uncertainties remain regarding the formation of sulfate aerosols, particularly the oxidation processes of S-bearing gases. Since the discovery of oxygen and sulfur mass independent fractionation (O- and S-MIF) processes on Earth, the sulfate isotopic composition became essential to investigate the atmospheric composition evolution and its consequences on the climate and the biosphere. Large amount of S-bearing compounds (SO2 mainly) is released into the atmosphere by anthropogenic and natural sources. Their oxidation in the atmosphere generates sulfate aerosols, H2SO4, which precipitate on the earth surface mainly as acid rain. One consequence of this precipitation is the formation of black crust on buildings made of carbonate stones. Indeed the chemical alteration of CaCO3 by H2SO4 leads to gypsum (CaSO4·2H2O) concretions on building walls. Associated to other particles, gypsum forms black-crusts. Therefore, black crusts acts as 'sulfate aerosol traps', meaning that their isotopic composition reveals the composition and thus the source and formation processes of sulfate aerosols in the atmosphere in a specific region. In this study we collected 37 black crusts on a 300km NW-SE profile centered on Paris (France). In our samples, sulfate represent 40wt.% and other particles 60wt.% of the black crusts. After sulfate extraction from each samples we measured their O- and S-isotopes composition. Variations of about 10‰ in δ18O and δ34S are observed and both O-MIF (Δ17O from 0 to 1.4‰) and S-MIF (Δ33S from 0 to -0.3‰) compositions have been measured. In regards to these compositions we can discuss the source and formation (oxidation pathways) of the sulfate aerosols in troposphere above the Paris region that covers urban, rural and coastal environments. Furthermore

  5. Aerosol Properties Observed in the Subtropical North Pacific Boundary Layer

    NASA Astrophysics Data System (ADS)

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

    2017-09-01

    The impact of anthropogenic aerosol on climate forcing remains uncertain largely due to inadequate representation of natural aerosols in climate models. The marine boundary layer (MBL) might serve as a model location to study natural aerosol processes. Yet source and sink mechanisms controlling the MBL aerosol number, size distribution, chemical composition, and hygroscopic properties remain poorly constrained. Here aerosol size distribution and water uptake measurements were made aboard the R/V Hi'ialakai from 27 June to 3 July 2016 in the subtropical North Pacific Ocean. Size distributions were predominantly bimodal with an average integrated number concentration of 197 ± 98 cm-3. Hygroscopic growth factors were measured using the tandem differential mobility analyzer technique for dry 48, 96, and 144 nm particles. Mode kappa values for these were 0.57 ± 0.12, 0.51 ± 0.09, and 0.52 ± 0.08, respectively. To better understand remote MBL aerosol sources, a new algorithm was developed which decomposes hygroscopicity distributions into three classes: carbon-containing particles, sulfate-like particles, and sodium-containing particles. Results from this algorithm showed low and steady sodium-containing particle concentrations while the sulfate-like and carbon-containing particle concentrations varied during the cruise. According to the classification scheme, carbon-containing particles contributed at least 3-7%, sulfate-like particles contributed at most 77-88% and sodium-containing particles at least contributed 9-16% to the total aerosol number concentration. Size distribution and hygroscopicity data, in conjunction with air mass back trajectory analysis, suggested that the aerosol budget in the subtropical North Pacific MBL may be controlled by aerosol entrainment from the free troposphere.

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

    NASA Astrophysics Data System (ADS)

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

    2012-07-01

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

  7. Online Simulations and Forecasts of the Global Aerosol Distribution in the NASA GEOS-5 Model

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2006-01-01

    We present an analysis of simulations of the global aerosol system in the NASA GEOS-5 transport, radiation, and chemistry model. The model includes representations of all major tropospheric aerosol species, including dust, sea salt, black carbon, particulate organic matter, and sulfates. The aerosols are run online for the period 2000 through 2005 in a simulation driven by assimilated meteorology from the NASA Goddard Data Assimilation System. Aerosol surface mass concentrations are compared with existing long-term surface measurement networks. Aerosol optical thickness is compared with ground-based AERONET sun photometry and space-based retrievals from MODIS, MISR, and OMI. Particular emphasis is placed here on consistent sampling of model and satellite aerosol optical thickness to account for diurnal variations in aerosol optical properties. Additionally, we illustrate the use of this system for providing chemical weather forecasts in support of various NASA and community field missions.

  8. 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

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

    NASA Technical Reports Server (NTRS)

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

    1994-01-01

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

  10. On the Complex Coupling Between the Production of Ozone and Secondary Organic Aerosol in Polluted Urban Regions

    NASA Astrophysics Data System (ADS)

    Stewart, D. R.; Stockwell, W. R.; Morris, V. R.; Fitzgerald, R. M.

    2016-12-01

    The major photochemical processes that produce ozone and aerosols are coupled together strongly in the polluted urban atmosphere. Aerosols are either directly emitted or formed through the same kind of chemistry that leads to the production of ozone. The aerosols produced through atmospheric chemistry are known as secondary aerosols and they may be composed of inorganic (nitrates, sulfates) or organic compounds. Wind blown dust and soot are two examples of primary aerosols. The component of secondary inorganic aerosols includes compounds such as ammonium nitrate, ammonium bisulfate and ammonium sulfate. Secondary organic aerosols are a very important component of PM with strong implications for health. The formation of secondary organic aerosol is linked with ozone photochemistry through the reactions of volatile organic compounds (VOC). The oxidation of VOC produces radicals that convert nitric oxide to nitrogen dioxide that photolyze to produce ozone. Larger VOC (those with more carbon atoms) undergo a number of oxidation cycles that add oxygen atoms to large organic molecules. The vapor pressure of many of these highly oxidized compounds is sufficiently low that they condense to produce secondary organic aerosols. The Community Multi-scale Air Quality model (CMAQ) and other chemical simulations have been made to quantify the relationship between varying emissions of VOC and NOx and the production of inorganic and secondary organic aerosols. The results from this analysis will be presented.

  11. Hygroscopic and phase separation properties of ammonium sulfate/organic/water ternary solutions

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Proud, S. R.; Seppalainen, S. S.; Cziczo, D. J.

    2015-03-01

    Atmospheric aerosol particles are often partially or completely composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. Deliquescence and efflorescence of simple inorganic salt particles have been investigated by a variety of methods, such as IR spectroscopy, tandem mobility analysis and electrodynamic balance. Field measurements have shown that atmospheric aerosols are not typically pure inorganic salt, instead they often also contain organic species. There is ample evidence from laboratory studies that suggests that mixed particles exist in a phase-separated state, with an aqueous inorganic core and organic shell. Although phase separation has not been measured in situ, there is no reason it would not also take place in the atmosphere. Many recent studies have focused on microscopy techniques that require deposition of the aerosol on a glass slide, possibly changing its surface properties. Here, we investigate the deliquescence and efflorescence points, phase separation and ability to exchange gas-phase components of mixed organic and inorganic aerosol using a flow tube coupled with FTIR spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O : C ratios, including 1,4-butanediol, glycerol, 1,2,6-hexanetriol, 1,2-hexanediol, and 1,5-pentanediol have been investigated. Those constituents correspond to materials found in the atmosphere in great abundance, and therefore, particles prepared in this study should mimic atmospheric mixed phase aerosol particles. The results of this study tend to be in agreement with previous microscopy experiments, with several key differences, which possibly reveal a size-dependent effect on phase separation in organic/inorganic aerosol particles.

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

    NASA Technical Reports Server (NTRS)

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

    2006-01-01

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

  13. Aerosols at the Poles: An Aerocom Phase II Multi-Model Evaluation

    NASA Technical Reports Server (NTRS)

    Sand, Maria; Bauer, Susanne E.; Samset, Bjorn H.; Balkanski, Yves; Bellouin, Nicolas; Berntsen, Terje K.; Bian, Huisheng; Chin, Mian; Diehl, Thomas; Easter, Richard; hide

    2017-01-01

    Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes. The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (seasalt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60 degrees N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70 degrees S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (-0.12 W m(exp. -2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments

  14. Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

    NASA Astrophysics Data System (ADS)

    Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

    2018-04-01

    In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude. The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires. In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and

  15. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

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

    Berg, L. K.; Shrivastava, M.; Easter, R. C.

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it

  16. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    DOE PAGES

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; ...

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it

  17. Chemical compositions of sulfate and chloride salts over the last termination reconstructed from the Dome Fuji ice core, inland Antarctica

    NASA Astrophysics Data System (ADS)

    Oyabu, Ikumi; Iizuka, Yoshinori; Uemura, Ryu; Miyake, Takayuki; Hirabayashi, Motohiro; Motoyama, Hideaki; Sakurai, Toshimitsu; Suzuki, Toshitaka; Hondoh, Takeo

    2014-12-01

    The flux and chemical composition of aerosols impact the climate. Antarctic ice cores preserve the record of past atmospheric aerosols, providing useful information about past atmospheric environments. However, few studies have directly measured the chemical composition of aerosol particles preserved in ice cores. Here we present the chemical compositions of sulfate and chloride salts from aerosol particles in the Dome Fuji ice core. The analysis method involves ice sublimation, and the period covers the last termination, 25.0-11.0 thousand years before present (kyr B.P.), with a 350 year resolution. The major components of the soluble particles are CaSO4, Na2SO4, and NaCl. The dominant sulfate salt changes at 16.8 kyr B.P. from CaSO4, a glacial type, to Na2SO4, an interglacial type. The sulfate salt flux (CaSO4 plus Na2SO4) inversely correlates with δ18O in Dome Fuji over millennial timescales. This correlation is consistent with the idea that sulfate salt aerosols contributed to the last deglacial warming of inland Antarctica by reducing the aerosol indirect effect. Between 16.3 and 11.0 kyr B.P., the presence of NaCl suggests that winter atmospheric aerosols are preserved. A high NaCl/Na2SO4 fraction between 12.3 and 11.0 kyr B.P. indicates that the contribution from the transport of winter atmospheric aerosols increased during this period.

  18. Review of sulfur dioxide to sulfate aerosol chemistry at Kīlauea Volcano, Hawai'i

    NASA Astrophysics Data System (ADS)

    Pattantyus, Andre K.; Businger, Steven; Howell, Steven G.

    2018-07-01

    Sulfur dioxide emissions from the Kīlauea Volcano on the island of Hawai'i and the subsequent formation of sulfate aerosols have caused a public health hazard across the state of Hawai'i since the volcano began erupting continuously in 1983. The University of Hawai'i at Mānoa began to forecast the trajectory and dispersion of emissions in 2010 to help mitigate the hazards to public health. In this paper a comprehensive review of potential conversion reactions is presented with the goal of more accurately representing the sulfur dioxide chemistry in the dispersion model. Atmospheric sulfur dioxide chemistry and major process responsible for sulfate formation are well documented in urban and industrial settings. The atmosphere in the vicinity of Kīlauea Volcano on the island of Hawai'i differs from that in previous investigations by virtue of being far removed from both urban and industrial settings in a remote, tropical marine atmosphere. Additionally, the combination of the high rate of sulfur dioxide emissions and trace gases and metals from Kīlauea Volcano creates a unique circumstance that requires a new look at potential conversion pathways to determine the dominant reactions. The theoretical analysis suggests that the dominant reaction in clear air will be between sulfur dioxide and the hydroxyl radical (0.01-5% h-1) and the dominant reaction in cloudy air involves hydrogen peroxide (3-50% s-1). Moreover, given the high SO2 emissions from the Halema'uma'u Crater vent, the oxidation of sulfur dioxide by these reactants is limited by their rate of production.

  19. An in-depth investigation of the life cycle of sulfate from the Kilauea volcano using satellite observations and EMAC model calculations

    NASA Astrophysics Data System (ADS)

    Penning de Vries, Marloes; Beirle, Steffen; Brühl, Christoph; Hörmann, Christoph; Wagner, Thomas

    2015-04-01

    The Kilauea volcano (Hawaii), currently perhaps the most active volcano on Earth, has been continuously erupting since the beginning of 1983. A pronounced degassing phase in March-November 2008 caused the formation of an extensive SO2 plume, which in turn led to the formation of sulfate aerosols. The steady trade winds and lack of interfering sources previously allowed us to determine the life time of SO2 using only satellite-based measurements (no a priori or model information). The current investigation is focused on improving our understanding of the processes contributing to sulfate aerosol formation, processing, and loss. We use space-based aerosol measurements by MODIS, MISR, and CALIOP to characterize the aerosols (amount, size, altitude) and study the evolution of aerosol optical depth as a function of distance from the volcano to determine formation and loss rates. The outcome is compared to results from calculations using the EMAC (ECHAM/MESSy Atmospheric Chemistry) model to test the state of understanding of the sulfate aerosol life cycle.

  20. A new approach to modeling aerosol effects on East Asian climate: Parametric uncertainties associated with emissions, cloud microphysics, and their interactions: AEROSOL EFFECTS ON EAST ASIAN CLIMATE

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

    Yan, Huiping; Qian, Yun; Zhao, Chun

    2015-09-09

    In this study, we adopt a parametric sensitivity analysis framework that integrates the quasi-Monte Carlo parameter sampling approach and a surrogate model to examine aerosol effects on the East Asian Monsoon climate simulated in the Community Atmosphere Model (CAM5). A total number of 256 CAM5 simulations are conducted to quantify the model responses to the uncertain parameters associated with cloud microphysics parameterizations and aerosol (e.g., sulfate, black carbon (BC), and dust) emission factors and their interactions. Results show that the interaction terms among parameters are important for quantifying the sensitivity of fields of interest, especially precipitation, to the parameters. Themore » relative importance of cloud-microphysics parameters and emission factors (strength) depends on evaluation metrics or the model fields we focused on, and the presence of uncertainty in cloud microphysics imposes an additional challenge in quantifying the impact of aerosols on cloud and climate. Due to their different optical and microphysical properties and spatial distributions, sulfate, BC, and dust aerosols have very different impacts on East Asian Monsoon through aerosol-cloud-radiation interactions. The climatic effects of aerosol do not always have a monotonic response to the change of emission factors. The spatial patterns of both sign and magnitude of aerosol-induced changes in radiative fluxes, cloud, and precipitation could be different, depending on the aerosol types, when parameters are sampled in different ranges of values. We also identify the different cloud microphysical parameters that show the most significant impact on climatic effect induced by sulfate, BC and dust, respectively, in East Asia.« less

  1. Hygroscopic and phase separation properties of ammonium sulfate/organics/water ternary solutions

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Proud, S. R.; Seppalainen, S. S.; Cziczo, D. J.

    2015-08-01

    Atmospheric aerosol particles are often partially or completely composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. Field measurements have shown that atmospheric aerosols are not typically pure inorganic salt, instead, they often also contain organic species. There is ample evidence from laboratory studies that suggests that mixed particles exist in a phase-separated state, with an aqueous inorganic core and organic shell. Although phase separation has not been measured in situ, there is no reason it would not also take place in the atmosphere. Here, we investigate the deliquescence and efflorescence points, phase separation and ability to exchange gas-phase components of mixed organic and inorganic aerosol using a flow tube coupled with FTIR (Fourier transform infrared) spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O : C ratios, including 1,4-butanediol, glycerol, 1,2,6-hexanetriol, 1,2-hexanediol, and 1,5-pentanediol have been investigated. Those constituents correspond to materials found in the atmosphere in great abundance and, therefore, particles prepared in this study should mimic atmospheric mixed-phase aerosol particles. Some results of this study tend to be in agreement with previous microscopy experiments, but others, such as phase separation properties of 1,2,6-hexanetriol, do not agree with previous work. Because the particles studied in this experiment are of a smaller size than those used in microscopy studies, the discrepancies found could be a size-related effect.

  2. Evaluating Ammonium, Nitrate and Sulfate Aerosols in 3-Dimensions

    NASA Technical Reports Server (NTRS)

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

    2015-01-01

    The effect aerosols have on climate and air quality is a func-on of their chemical composi-on, concentra-on and spa-al distribu-on. These parameters are controlled by emissions, heterogeneous and homogeneous chemistry, where thermodynamics plays a key role, transport, which includes stratospheric-­- tropospheric exchange, and deposi-onal sinks. In this work we demonstrate the effect of some of these processes on the SO4-NH4­-NO3 system using the GISS ModelE2 Global Circula-on Model (GCM).

  3. WRF-Chem simulations of aerosols and anthropogenic aerosol radiative forcing in East Asia

    NASA Astrophysics Data System (ADS)

    Gao, Yi; Zhao, Chun; Liu, Xiaohong; Zhang, Meigen; Leung, L. Ruby

    2014-08-01

    This study aims to provide a first comprehensive evaluation of WRF-Chem for modeling aerosols and anthropogenic aerosol radiative forcing (RF, including direct, semi-direct and indirect forcing) over East Asia. Several numerical experiments were conducted from November 2007 to December 2008. Comparison between model results and observations shows that the model can generally reproduce the observed spatial distributions of aerosol concentration, aerosol optical depth (AOD) and single scattering albedo (SSA) from measurements at many sites, including the relatively higher aerosol concentration and AOD over East China and the relatively lower AOD over Southeast Asia, Korea, and Japan. The model also depicts the seasonal variation and transport of pollutions over East Asia. Particulate matter of 10 μm or less in the aerodynamic diameter (PM10), black carbon (BC), sulfate (SO42-), nitrate (NO3-) and ammonium (NH4+) concentrations are higher in spring than other seasons in Japan, which indicates the possible influence of pollutant transport from polluted area of East Asia. The model underestimates SO42- and organic carbon (OC) concentrations over mainland China by about a factor of 2, while overestimates NO3- concentration in autumn along the Yangtze River. The model captures the dust events at the Zhangye site in the semi-arid region of China. AOD is high over Southwest and Central China in winter and spring and over North China in winter, spring and summer while is low over South China in summer due to monsoon precipitation. SSA is lowest in winter and highest in summer. Anthropogenic aerosol RF is estimated to range from -5 to -20 W m-2 over land and -20 to -40 W m-2 over adjacent oceans at the top of atmosphere (TOA), 5-30 W m-2 in the atmosphere (ATM) and -15 to -40 W m-2 at the bottom (BOT). The warming effect of anthropogenic aerosol in ATM results from BC aerosol while the negative aerosol RF at TOA is caused by scattering aerosols such as SO42-, NO3- and NH4

  4. Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

    NASA Astrophysics Data System (ADS)

    Kaul, D. S.; Gupta, T.; Tripathi, S. N.

    2012-06-01

    An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

  5. Evolution of Asian aerosols during transpacific transport in INTEX-B

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

    Dunlea, E. J.; DeCarlo, Peter; Aiken, Allison

    2009-10-01

    Measurements of aerosol composition were made with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) on board the NSF/NCAR C-130 aircraft as part of the Intercontinental Chemical Transport Experiment Phase B 5 (INTEX-B) field campaign over the Eastern Pacific Ocean. The HR-ToF-AMS measurements of non-refractory submicron aerosol mass are shown to compare well with other aerosol instrumentation in the INTEX-B field study. Two case studies are described for pollution layers transported across the Pacific from the Asian continent, intercepted 3–4 days and 7–10 days downwind of Asia, respectively. Aerosol chemistry is shown to 10 be a robust tracer formore » air masses originating in Asia, specifically the presence of sulfate dominated aerosol is a distinguishing feature of Asian pollution layers that have been transported to the Eastern Pacific. We examine the time scales of processing for sulfate and organic aerosol in the atmosphere and show that our observations confirm a conceptual model for transpacific transport from Asia proposed by Brock et al. (2004). 15 Our observations of both sulfate and organic aerosol in aged Asian pollution layers are consistent with fast formation near the Asian continent, followed by washout during lofting and subsequent transformation during transport across the Pacific. Our observations are the first atmospheric measurements to indicate that although secondary organic aerosol (SOA) formation from pollution happens on the timescale of one day, 20 the oxidation of organic aerosol continues at longer timescales in the atmosphere. Comparisons with chemical transport models of data from the entire campaign reveal an under-prediction of SOA mass in the MOZART model, but much smaller discrepancies with the GEOS-Chem model than found in previous studies over the Western Pacific. No evidence is found to support a previous hypothesis for significant secondary 25 organic aerosol formation in the free

  6. DEPOSITION OF SULFATE ACID AEROSOLS IN THE DEVELOPING HUMAN LUNG

    EPA Science Inventory

    Computations of aerosol deposition as affected by (i) aerosol hygroscopicity, (ii) human age, and (iii) respiratory intensity are accomplished using a validated mathematical model. he interactive effects are very complicated but systematic. ew general observations can be made; ra...

  7. 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

  8. Increases to Biogenic Secondary Organic Aerosols from SO2 and NOx in the Southeastern US

    NASA Astrophysics Data System (ADS)

    Russell, L. M.; Liu, J.; Ruggeri, G.; Takahama, S.; Claflin, M. S.; Ziemann, P. J.; Lee, A.; Murphy, B.; Pye, H. O. T.; Ng, N. L.; McKinney, K. A.; Surratt, J. D.

    2017-12-01

    During the 2013 Southern Oxidant and Aerosol Study, Fourier Transform Infrared Spectroscopy (FTIR) and Aerosol Mass Spectrometer (AMS) measurements of submicron mass were collected at Look Rock, Tennessee, and Centreville, Alabama. The low NOx, low wind, little rain, and increased daytime isoprene emissions led to multi-day stagnation events at Look Rock that provided clear evidence of particle-phase sulfate enhancing biogenic secondary organic aerosol (bSOA) by selective uptake. Organic mass (OM) sources were apportioned as 42% "vehicle-related" and 54% bSOA, with the latter including "sulfate-related bSOA" that correlated to sulfate (r=0.72) and "nitrate-related bSOA" that correlated to nitrate (r=0.65). Single-particle mass spectra showed three composition types that corresponded to the mass-based factors with spectra cosine similarity of 0.93 and time series correlations of r>0.4. The vehicle-related OM with m/z 44 was correlated to black carbon, "sulfate-related bSOA" was on particles with high sulfate, and "nitrate-related bSOA" was on all particles. The similarity of the m/z spectra (cosine similarity=0.97) and the time series correlation (r=0.80) of the "sulfate-related bSOA" to the sulfate-containing single-particle type provide evidence for particle composition contributing to selective uptake of isoprene oxidation products onto particles that contain sulfate from power plants. Since Look Rock had much less NOx than Centreville, comparing the bSOA at the two sites provides an evaluation of the role of NOx for bSOA. CO and submicron sulfate and OM concentrations were 15-60 % higher at Centreville than at Look Rock but their time series had moderate correlations of r= 0.51, 0.54, and 0.47, respectively. However, NOx had no correlation (r=0.08) between the two sites. OM correlated with the higher NOx levels at Centreville but with O3 at Look Rock. OM sources identified by Positive Matrix Factorization had three very similar factors at both sites from FTIR

  9. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Dubovik, Oleg; Holben, Brent; Kaufman, Yoram; chu, Allen; Anderson, Tad; Quinn, Patricia

    2003-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  10. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies Among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Chu, Allen; Levy, Robert; Remer, Lorraine; Kaufman, Yoram; Dubovik, Oleg; Holben, Brent; Eck, Tom; Anderson, Tad; Quinn, Patricia

    2004-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, .biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERON" at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  11. Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate

    DOE PAGES

    Kwong, Kai Chung; Chim, Man Mei; Davies, James F.; ...

    2018-02-27

    Organosulfates are important organosulfur compounds present in atmospheric particles. While the abundance, composition, and formation mechanisms of organosulfates have been extensively investigated, it remains unclear how they transform and evolve throughout their atmospheric lifetime. To acquire a fundamental understanding of how organosulfates chemically transform in the atmosphere, this study investigates the heterogeneous OH radical-initiated oxidation of sodium methyl sulfate (CH 3SO 4Na) droplets, the smallest organosulfate detected in atmospheric particles, using an aerosol flow tube reactor at a high relative humidity (RH) of 85%. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (direct analysis in real time,more » DART) coupled with a high-resolution mass spectrometer showed that neither functionalization nor fragmentation products are detected. Instead, the ion signal intensity of the bisulfate ion (HSO 4 -) has been found to increase significantly after OH oxidation. We postulate that sodium methyl sulfate tends to fragment into a formaldehyde (CH 2O) and a sulfate radical anion (SO 4 .-) upon OH oxidation. The formaldehyde is likely partitioned back to the gas phase due to its high volatility. The sulfate radical anion, similar to OH radical, can abstract a hydrogen atom from neighboring sodium methyl sulfate to form the bisulfate ion, contributing to the secondary chemistry. Kinetic measurements show that the heterogeneous OH reaction rate constant, k, is (3.79 ± 0.19) × 10 -13cm 3molecule -1s -1 with an effective OH uptake coefficient, γ eff, of 0.17 ± 0.03. While about 40% of sodium methyl sulfate is being oxidized at the maximum OH exposure (1.27 × 10 12molecule cm -3s), only a 3% decrease in particle diameter is observed. This can be attributed to a small fraction of particle mass lost via the formation and volatilization of formaldehyde. Overall, we firstly demonstrate that the heterogeneous OH oxidation of an

  12. Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate

    NASA Astrophysics Data System (ADS)

    Chung Kwong, Kai; Chim, Man Mei; Davies, James F.; Wilson, Kevin R.; Nin Chan, Man

    2018-02-01

    Organosulfates are important organosulfur compounds present in atmospheric particles. While the abundance, composition, and formation mechanisms of organosulfates have been extensively investigated, it remains unclear how they transform and evolve throughout their atmospheric lifetime. To acquire a fundamental understanding of how organosulfates chemically transform in the atmosphere, this work investigates the heterogeneous OH radical-initiated oxidation of sodium methyl sulfate (CH3SO4Na) droplets, the smallest organosulfate detected in atmospheric particles, using an aerosol flow tube reactor at a high relative humidity (RH) of 85 %. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (direct analysis in real time, DART) coupled with a high-resolution mass spectrometer showed that neither functionalization nor fragmentation products are detected. Instead, the ion signal intensity of the bisulfate ion (HSO4-) has been found to increase significantly after OH oxidation. We postulate that sodium methyl sulfate tends to fragment into a formaldehyde (CH2O) and a sulfate radical anion (SO4 ṡ -) upon OH oxidation. The formaldehyde is likely partitioned back to the gas phase due to its high volatility. The sulfate radical anion, similar to OH radical, can abstract a hydrogen atom from neighboring sodium methyl sulfate to form the bisulfate ion, contributing to the secondary chemistry. Kinetic measurements show that the heterogeneous OH reaction rate constant, k, is (3.79 ± 0.19) × 10-13 cm3 molecule-1 s-1 with an effective OH uptake coefficient, γeff, of 0.17 ± 0.03. While about 40 % of sodium methyl sulfate is being oxidized at the maximum OH exposure (1.27 × 1012 molecule cm-3 s), only a 3 % decrease in particle diameter is observed. This can be attributed to a small fraction of particle mass lost via the formation and volatilization of formaldehyde. Overall, we firstly demonstrate that the heterogeneous OH oxidation of an

  13. Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate

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

    Kwong, Kai Chung; Chim, Man Mei; Davies, James F.

    Organosulfates are important organosulfur compounds present in atmospheric particles. While the abundance, composition, and formation mechanisms of organosulfates have been extensively investigated, it remains unclear how they transform and evolve throughout their atmospheric lifetime. To acquire a fundamental understanding of how organosulfates chemically transform in the atmosphere, this study investigates the heterogeneous OH radical-initiated oxidation of sodium methyl sulfate (CH 3SO 4Na) droplets, the smallest organosulfate detected in atmospheric particles, using an aerosol flow tube reactor at a high relative humidity (RH) of 85%. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (direct analysis in real time,more » DART) coupled with a high-resolution mass spectrometer showed that neither functionalization nor fragmentation products are detected. Instead, the ion signal intensity of the bisulfate ion (HSO 4 -) has been found to increase significantly after OH oxidation. We postulate that sodium methyl sulfate tends to fragment into a formaldehyde (CH 2O) and a sulfate radical anion (SO 4 .-) upon OH oxidation. The formaldehyde is likely partitioned back to the gas phase due to its high volatility. The sulfate radical anion, similar to OH radical, can abstract a hydrogen atom from neighboring sodium methyl sulfate to form the bisulfate ion, contributing to the secondary chemistry. Kinetic measurements show that the heterogeneous OH reaction rate constant, k, is (3.79 ± 0.19) × 10 -13cm 3molecule -1s -1 with an effective OH uptake coefficient, γ eff, of 0.17 ± 0.03. While about 40% of sodium methyl sulfate is being oxidized at the maximum OH exposure (1.27 × 10 12molecule cm -3s), only a 3% decrease in particle diameter is observed. This can be attributed to a small fraction of particle mass lost via the formation and volatilization of formaldehyde. Overall, we firstly demonstrate that the heterogeneous OH oxidation of an

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

    NASA Astrophysics Data System (ADS)

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

    2002-12-01

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

  15. Aerosols at the poles: an AeroCom Phase II multi-model evaluation

    DOE PAGES

    Sand, Maria; Samset, Bjorn H.; Balkanski, Yves; ...

    2017-10-13

    Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document themore » geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes. The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (-0.12 W m -2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of

  16. Aerosols at the poles: an AeroCom Phase II multi-model evaluation

    NASA Astrophysics Data System (ADS)

    Sand, Maria; Samset, Bjørn H.; Balkanski, Yves; Bauer, Susanne; Bellouin, Nicolas; Berntsen, Terje K.; Bian, Huisheng; Chin, Mian; Diehl, Thomas; Easter, Richard; Ghan, Steven J.; Iversen, Trond; Kirkevåg, Alf; Lamarque, Jean-François; Lin, Guangxing; Liu, Xiaohong; Luo, Gan; Myhre, Gunnar; van Noije, Twan; Penner, Joyce E.; Schulz, Michael; Seland, Øyvind; Skeie, Ragnhild B.; Stier, Philip; Takemura, Toshihiko; Tsigaridis, Kostas; Yu, Fangqun; Zhang, Kai; Zhang, Hua

    2017-10-01

    Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes.The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (-0.12 W m-2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of the Aero

  17. Aerosols at the poles: an AeroCom Phase II multi-model evaluation

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

    Sand, Maria; Samset, Bjorn H.; Balkanski, Yves

    Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document themore » geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes. The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (-0.12 W m -2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of

  18. 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.

  19. 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.

  20. Semi-Continuous Measurements of Aerosol Chemical Composition During the Summer 2002 Yosemite National Park Special Study

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

    Collette, J; Lee, T; Heath, J

    2003-02-16

    Semi-continuous measurements of fine particle composition were made over a period of several weeks in summer 2002 in Yosemite National Park, California. These included measurement of aerosol ionic composition (by PILS- Particle-Into-Liquid System) and aerosol carbon (by dual wavelength aethalometer and an R&P particulate carbon monitor). The data reveal that aerosol composition at the site is highly :variable in time, with a strong diurnal cycle. Interestingly, however, different diurnal cycles were sometimes observed for different chemical constituents of the particles. Organic carbon was observed to dominate fine particle mass, with some periods apparently associated with influx of smoke from wildfiresmore » in the western U.S. Measurements of fine particle carbon isotopes revealed the fraction of carbon from biogenic sources to range from approximately 73 to 95%. The ionic fraction of the aerosol was usually dominated by ammoniated sulfate. During most periods, PM{sub 2.5} nitrate was found primarily in sea salt particles from which chloride had been displaced. Strong variations in the extent of ammonia neutralization of sulfate were also observed. The ability to observe rapid changes in aerosol composition using these semi-continuous aerosol composition measurements is helpful for understanding the dynamic chemical composition of fine particles responsible for regional haze.« less

  1. An evaluation of simulated particulate sulfate over East Asia through global model intercomparison

    NASA Astrophysics Data System (ADS)

    Goto, Daisuke; Nakajima, Teruyuki; Dai, Tie; Takemura, Toshihiko; Kajino, Mizuo; Matsui, Hitoshi; Takami, Akinori; Hatakeyama, Shiro; Sugimoto, Nobuo; Shimizu, Atsushi; Ohara, Toshimasa

    2015-06-01

    Sulfate aerosols simulated by an aerosol module coupled to the Nonhydrostatic Icosahedral Atmospheric Model (NICAM) at a spatial resolution (220 km) widely used by global climate models were evaluated by a comparison with in situ observations and the same aerosol module coupled to the Model for Interdisciplinary Research on Climate (MIROC) over East Asia for January, April, July, and October 2006. The results indicated that a horizontal gradient of sulfate from the source over China to the outflow over Korea-Japan was present in both the simulations and the observations. At the observation sites, the correlation coefficients of the sulfate concentrations between the simulations and the observations were high (NICAM: 0.49-0.89, MIROC: 0.61-0.77), whereas the simulated sulfate concentrations were lower than those obtained by the observation with the normalized mean bias of NICAM being -68 to -54% (all), -77 to -63% (source), and -67 to -30% (outflow) and that of MIROC being -61 to -28% (all), -77 to -63% (source), and -60 to +2% (outflow). Both NICAM and MIROC strongly underpredict surface SO2 over China source regions and Korea-Japan outflow regions, but the MIROC SO2 is much higher than NICAM SO2 over both regions. These differences between the models were mainly explained by differences in the sulfate formation within clouds and the dry deposition of SO2. These results indicated that the uncertainty of the meteorological and cloud fields as well as the vertical transport patterns between the different host climate models has a substantial impact on the simulated sulfate distribution.

  2. The NASA-AMES Research Center Stratospheric Aerosol Model. 1. Physical Processes and Computational Analogs

    NASA Technical Reports Server (NTRS)

    Turco, R. P.; Hamill, P.; Toon, O. B.; Whitten, R. C.; Kiang, C. S.

    1979-01-01

    A time-dependent one-dimensional model of the stratospheric sulfate aerosol layer is presented. In constructing the model, a wide range of basic physical and chemical processes are incorporated in order to avoid predetermining or biasing the model predictions. The simulation, which extends from the surface to an altitude of 58 km, includes the troposphere as a source of gases and condensation nuclei and as a sink for aerosol droplets. The size distribution of aerosol particles is resolved into 25 categories with particle radii increasing geometrically from 0.01 to 2.56 microns such that particle volume doubles between categories.

  3. Anthropogenic and Volcanic Contributions to the Decadal Variations of Aerosols in the Upper Troposphere and Lower Stratosphere

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Diehl, Thomas; Bian, Huisheng; Aquila, Valentina; Colarco, Peter R.; Tan, Qian; Burrows, John P.; Krotov, Nickolay A.; Vernier, Jean P.; Lu, Zifeng; hide

    2014-01-01

    We investigated the anthropogenic and volcanic contributions to sulfate aerosol in the stratosphere through modeling and analysis of satellite data. We use a global model GOCART to simulate SO2 and sulfate aerosol in the period of 2000 to 2010, during which numerous volcanic eruptions occurred although nothing like the magnitudes of El Chichon or Pinatubo. We compared the model results with the column SO2 data from OMI and stratospheric SO2 data from MLS instrument on Aura satellite and the aerosol vertical profiles from the SCIAMACHY instrument on Envisat and the CALIOP instrument on CALIPSO satellites. Finally, we assessed the relative contributions of volcanic aerosols vs. anthropogenic aerosols to the observed decadal stratospheric aerosol trends.

  4. Aerosols in the Atmosphere: Sources, Transport, and Multi-decadal Trends

    NASA Technical Reports Server (NTRS)

    Chin, M.; Diehl, T.; Bian, H.; Kucsera, T.

    2016-01-01

    We present our recent studies with global modeling and analysis of atmospheric aerosols. We have used the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and satellite and in situ data to investigate (1) long-term variations of aerosols over polluted and dust source regions and downwind ocean areas in the past three decades and the cause of the changes and (2) anthropogenic and volcanic contributions to the sulfate aerosol in the upper tropospherelower stratosphere.

  5. 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.

  6. Space-borne Observations of Aerosols

    NASA Astrophysics Data System (ADS)

    Kaufman, Y. J.; Tanre, D.; Coakley, J. A.; Fraser, R. S.

    2005-12-01

    As early as 1963, photographs of the twilight horizon from the Vostok-6 spaceship were used by G. V. Rozenberg and V. V. Nikolaeva-Tereshkova to derive profiles of stratospheric aerosols. The launch of the ATS III satellite in 1967 sparked interest in using satellites to observe aerosol emission, transport, and their effects on climate, precipitation and health. The first use of autonomous satellites in aerosol research appears to be by Toby Carlson and Joe Prospero who tracked dust from the Sahara to the Americas in the early `70s using ATS III images. The launch of the calibrated Landsat instrument in 1972 allowed Bob Fraser to perform quantitative analyses of dust column concentrations for individual scenes. GOES launched in 1975 provided hourly data that allowed Walter Lyons and J.C. Dooley in the late 70's to report on the transport of sulfate air pollution which was later followed by estimates of the export of sulfate aerosol from the US to the Atlantic Ocean. With the launch of SAGE in 1979, Pat McCormick and co-workers began long term observations of statospheric aerosols. The launch of TIROS(N) and the AVHRR in 1979 marked the start of concerted efforts by Larry Stowe and his colleagues to produce operationally an aerosol product over oceans from the NOAA polar orbiting satellite. With the launch of the Earth Radiation Budget Experiment scanners in the late 1980's, Sundar Christopher and his colleagues began linking AVHRR-derived aerosol burdens to their effects on the Earth's radiation budget. A remarkable aspect of this early work is that instruments like the AVHRR, Landsat, and GOES imager were not originally designed to perform quantitative estimates of aerosol properties. In fact, corrections for the effects of aerosols in determining ocean reflectances implemented primarily through the work of Howard Gordon, facilitated much improved pictures of chlorophyll in the upper oceans than had been hoped for from CZCS data collected in the late 70's. This

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

    NASA Astrophysics Data System (ADS)

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

    2014-08-01

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

  8. Development of an Operational Multi-sensor and Multi-channel Aerosol Assimilation Package

    DTIC Science & Technology

    2011-08-18

    2010, EGU General Assembly 2010. Shi, Y., J. Zhang, J. S. Reid, E. Hyer, Evaluation of MISR Aerosol Optical Depth Product for Aerosol Data...empirical correction procedures for generating data-assimilation-friendly over-water MODIS aerosol products. This study has been published (Shi et al...type as large r\\ values are generally related to fine mode aerosols, such as sulfate and smoke aerosols, and small r\\ values typically indicate sea

  9. Global source attribution of sulfate concentration and direct and indirect radiative forcing

    NASA Astrophysics Data System (ADS)

    Yang, Yang; Wang, Hailong; Smith, Steven J.; Easter, Richard; Ma, Po-Lun; Qian, Yun; Yu, Hongbin; Li, Can; Rasch, Philip J.

    2017-07-01

    The global source-receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF) from 16 regions/sectors for years 2010-2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggesting that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is -0.42 W m-2, with -0.31 W m-2 contributed by anthropogenic sulfate and -0.11 W m-2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17-84 % to the total DRF. East Asia has the largest contribution of 20-30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of -0.44 W m-2. DMS has the largest contribution, explaining -0.23 W m-2 of the global sulfate incremental IRF. Incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.

  10. Photophoretic levitation of engineered aerosols for geoengineering

    PubMed Central

    Keith, David W.

    2010-01-01

    Aerosols could be injected into the upper atmosphere to engineer the climate by scattering incident sunlight so as to produce a cooling tendency that may mitigate the risks posed by the accumulation of greenhouse gases. Analysis of climate engineering has focused on sulfate aerosols. Here I examine the possibility that engineered nanoparticles could exploit photophoretic forces, enabling more control over particle distribution and lifetime than is possible with sulfates, perhaps allowing climate engineering to be accomplished with fewer side effects. The use of electrostatic or magnetic materials enables a class of photophoretic forces not found in nature. Photophoretic levitation could loft particles above the stratosphere, reducing their capacity to interfere with ozone chemistry; and, by increasing particle lifetimes, it would reduce the need for continual replenishment of the aerosol. Moreover, particles might be engineered to drift poleward enabling albedo modification to be tailored to counter polar warming while minimizing the impact on equatorial climates. PMID:20823254

  11. Photophoretic levitation of engineered aerosols for geoengineering.

    PubMed

    Keith, David W

    2010-09-21

    Aerosols could be injected into the upper atmosphere to engineer the climate by scattering incident sunlight so as to produce a cooling tendency that may mitigate the risks posed by the accumulation of greenhouse gases. Analysis of climate engineering has focused on sulfate aerosols. Here I examine the possibility that engineered nanoparticles could exploit photophoretic forces, enabling more control over particle distribution and lifetime than is possible with sulfates, perhaps allowing climate engineering to be accomplished with fewer side effects. The use of electrostatic or magnetic materials enables a class of photophoretic forces not found in nature. Photophoretic levitation could loft particles above the stratosphere, reducing their capacity to interfere with ozone chemistry; and, by increasing particle lifetimes, it would reduce the need for continual replenishment of the aerosol. Moreover, particles might be engineered to drift poleward enabling albedo modification to be tailored to counter polar warming while minimizing the impact on equatorial climates.

  12. Factors Affecting Aerosol Radiative Forcing

    NASA Astrophysics Data System (ADS)

    Wang, Jingxu; Lin, Jintai; Ni, Ruijing

    2016-04-01

    Rapid industrial and economic growth has meant a large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RF of aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissions per unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size. South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions, its aerosol RF is alleviated by its lowest chemical efficiency. The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is lowered by a small per capita GDP. Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The

  13. Factors Affecting Aerosol Radiative Forcing

    NASA Astrophysics Data System (ADS)

    Wang, J.; Lin, J.; Ni, R.

    2016-12-01

    Rapid industrial and economic growth has meant large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RFof aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissionsper unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size.South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions,its aerosol RF is alleviated by its lowest chemical efficiency.The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is loweredbyasmall per capita GDP.Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The resulting

  14. Condensed nitrate, sulfate, and chloride in Antarctic stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Snetsinger, K. G.; Toon, O. B.; Ferry, G. V.; Oberbeck, V. R.; Starr, W. L.; Chan, K. R.; Goodman, J. K.

    1989-01-01

    The 1987 Airborne Antarctic Ozone Experiment, in which the NO3, Cl, and SO4 contents of stratospheric aerosols were estimated, is discussed. The aerosol size and chemical composition measurements were carried out on samples collected during August 17 to September 4, 1987. The data indicate that condensed nitrate is found below a threshold temperature of 193.6 + or - 3.0 K, which is generally found at latitudes exceeding 64 deg S. A negative correlation exists between condensed nitrate and ozone correlation.

  15. Overview of ACE-Asia Spring 2001 Investigations on Aerosol Radiative Effects and Related Aerosol Properties

    NASA Technical Reports Server (NTRS)

    Russell, Philip B.; Valero, F. P. J.; Flatau, P. J.; Bergin, M.; Holben, B.; Nakajima, T.; Pilewskie, P.; Bergstrom, R.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    depth gradient, with AOD(500 nm) extremes from 0.1 to 1.1. On the Pacific transit from Honolulu to Hachijo AOD(500 nm) averaged 0.2, including increases to 0.4 after several storms, suggesting the strong impact of wind-generated seasalt. The AOD maximum, found in the Sea of Japan, was influenced by dust and anthropogenic sources. (4) In Beijing, single scattering albedo retrieved from AERONET sun-sky radiometry yielded midvisible SSA=0.88 with strong wavelength dependence, suggesting a significant black carbon component. SSA retrieved during dust episodes was approx. 0.90 and variable but wavelength neutral reflecting the presence of urban haze with the dust. Downwind at Anmyon Island SSA was considerably higher, approx. 0.94, but wavelength neutral for dust episodes and spectrally dependent during non dust periods. (5) Satellite retrievals show major aerosol features moving from Asia over the Pacific; however, determining seasonal-average aerosol effects is hampered by sampling frequency and large-scale cloud systems that obscure key parts of aerosol patterns. Preliminary calculations using, satellite-retrieved AOD fields and initial ACE-Asia aerosol properties (including sulfates, soot, and dust) yield clear-sky aerosol radiative effects in the seasonal-average ACE-Asia plume exceeding those of manmade greenhouse gases. Quantifying all-sky direct aerosol radiative effects is complicated by the need to define the height of absorbing aerosols with respect to cloud decks.

  16. pH Variance in Aerosols Undergoing Liquid-Liquid Phase Separation

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  17. Development of an Operational Multi-sensor and Multi-channel Aerosol Assimilation Package Using NAAPS and NAVDAS

    DTIC Science & Technology

    2010-09-30

    5593-1, 2010, EGU General Assembly 2010. Shi, Y., J. Zhang, J. S. Reid, E. Hyer, Evaluation of MISR Aerosol Optical Depth Product for Aerosol Data...a surrogate for aerosol type, as large η values are generally related to fine mode aerosols, such as sulfate and smoke aerosols, and small η values

  18. Observations and Modeling of the Green Ocean Amazon 2014/15: Transmission Electron Microscopy Analysis of Aerosol Particles Field Campaign Report

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

    Buseck, Peter

    2016-03-01

    During two Intensive Operational Periods (IOP), we collected samples at 3-hour intervals for transmission electron microscopy analysis. The resulting transmission electron microscopy images and compositions were analyzed for the samples of interest. Further analysis will be done especially for the plume of interest. We found solid spherical organic particles from rebounded samples collected with Professor Scot Martin’s group (Harvard University). Approximately 30% of the rebounded particles at 95% relative humidity were spherical organic particles. Their sources and formation process are not known, but such spherical particles could be solid and will have heterogeneous chemical reactions. We observed many organic particlesmore » that are internally mixed with inorganic elements such as potassium and nitrogen. They are either homogeneously mixed or have inorganic cores with organic aerosol coatings. Samples collected from the Manaus, Brazil, pollution plume included many nano-size soot particles mixed with organic material and sulfate. Aerosol particles from clean periods included organic aerosol particles, sulfate, sea salt, dust, and primary biogenic aerosol particles. There was more dust, primary biogenic aerosol, and tar balls in samples taken during IOP1 than those taken during IOP2. Many dust particles were found between March 2 and 3.« less

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

    NASA Astrophysics Data System (ADS)

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

    2010-06-01

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

  20. Global source attribution of sulfate concentration and direct and indirect radiative forcing

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

    Yang, Yang; Wang, Hailong; Smith, Steven J.

    The global source–receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF) from 16 regions/sectors for years 2010–2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO 2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggestingmore » that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is –0.42 W m –2, with –0.31 W m –2 contributed by anthropogenic sulfate and –0.11 W m –2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17–84 % to the total DRF. East Asia has the largest contribution of 20–30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of –0.44 W m –2. DMS has the largest contribution, explaining –0.23 W m –2 of the global sulfate incremental IRF. Here, incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.« less

  1. Global source attribution of sulfate concentration and direct and indirect radiative forcing

    DOE PAGES

    Yang, Yang; Wang, Hailong; Smith, Steven J.; ...

    2017-07-25

    The global source–receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF) from 16 regions/sectors for years 2010–2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO 2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggestingmore » that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is –0.42 W m –2, with –0.31 W m –2 contributed by anthropogenic sulfate and –0.11 W m –2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17–84 % to the total DRF. East Asia has the largest contribution of 20–30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of –0.44 W m –2. DMS has the largest contribution, explaining –0.23 W m –2 of the global sulfate incremental IRF. Here, incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.« less

  2. 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

  3. Asthmatic responses to airborne acid aerosols

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

    Ostro, B.D.; Lipsett, M.J.; Wiener, M.B.

    1991-06-01

    Controlled exposure studies suggest that asthmatics may be more sensitive to the respiratory effects of acidic aerosols than individuals without asthma. This study investigates whether acidic aerosols and other air pollutants are associated with respiratory symptoms in free-living asthmatics. Daily concentrations of hydrogen ion (H+), nitric acid, fine particulates, sulfates and nitrates were obtained during an intensive air monitoring effort in Denver, Colorado, in the winter of 1987-88. A panel of 207 asthmatics recorded respiratory symptoms, frequency of medication use, and related information in daily diaries. We used a multiple regression time-series model to analyze which air pollutants, if any,more » were associated with health outcomes reported by study participants. Airborne H+ was found to be significantly associated with several indicators of asthma status, including moderate or severe cough and shortness of breath. Cough was also associated with fine particulates, and shortness of breath with sulfates. Incorporating the participants' time spent outside and exercise intensity into the daily measure of exposure strengthened the association between these pollutants and asthmatic symptoms. Nitric acid and nitrates were not significantly associated with any respiratory symptom analyzed. In this population of asthmatics, several outdoor air pollutants, particularly airborne acidity, were associated with daily respiratory symptoms.« less

  4. Organic Aerosols as Cloud Condensation Nuclei

    NASA Astrophysics Data System (ADS)

    Hudson, J. G.

    2002-05-01

    The large organic component of the atmospheric aerosol contributes to both natural and anthropogenic cloud condensation nuclei (CCN). Moreover, some organic substances may reduce droplet surface tension (Facchini et al. 1999), while others may be partially soluble (Laaksonen et al. 1998), and others may inhibit water condensation. The interaction of organics with water need to be understood in order to better understand the indirect aerosol effect. Therefore, laboratory CCN spectral measurements of organic aerosols are presented. These are measurements of the critical supersaturation (Sc), the supersaturation needed to produce an activated cloud droplet, as a function of the size of the organic particles. Substances include sodium lauryl (dodecyl) sulfate, oxalic, adipic, pinonic, hexadecanedioic, glutaric, stearic, succinic, phthalic, and benzoic acids. These size-Sc relationships are compared with theoretical and measured size-Sc relationships of common inorganic compounds (e.g., NaCl, KI, ammonium and calcium sulfate). Unlike most inorganics some organics display variations in solubility per unit mass as a function of particle size. Those showing relatively greater solubility at smaller sizes may be attributable to surface tension reduction, which is greater for less water dilution, as is the case for smaller particles, which are less diluted at the critical sizes. This was the case for sodium dodecyl sulfate, which does reduce surface tension. Relatively greater solubility for larger particles may be caused by greater dissolution at the higher dilutions that occur with larger particles; this is partial solubility. Measurements are also presented of internal mixtures of various organic and inorganic substances. These measurements were done with two CCN spectrometers (Hudson 1989) operating simultaneously. These two instruments usually displayed similar results in spite of the fact that they have different flow rates and supersaturation profiles. The degree of

  5. Aerosol in the Pacific troposphere

    NASA Technical Reports Server (NTRS)

    Clarke, Antony D.

    1989-01-01

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

  6. Global Impacts of Gas-Phase Chemistry-Aerosol Interactions on Direct Radiative Forcing by Anthropogenic Aerosols and Ozone

    NASA Technical Reports Server (NTRS)

    Liao, Hong; Seinfeld, John H.

    2005-01-01

    We present here a first global modeling study on the influence of gas-phase chemistry/aerosol interactions on estimates of anthropogenic forcing by tropospheric O3 and aerosols. Concentrations of gas-phase species and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols in the preindustrial, present-day, and year 2100 (IPCC SRES A2) atmospheres are simulated online in the Goddard Institute for Space Studies general circulation model II' (GISS GCM II'). With fully coupled chemistry and aerosols, the preindustrial, presentday, and year 2100 global burdens of tropospheric ozone are predicted to be 190, 319, and 519 Tg, respectively. The burdens of sulfate, nitrate, black carbon, and organic carbon are predicted respectively to be 0.32. 0.18, 0.01, 0.33 Tg in preindustrial time, 1.40, 0.48, 0.23, 1.60 Tg in presentday, and 1.37, 1.97, 0.54, 3.31 Tg in year 2100. Anthropogenic O3 is predicted to have a globally and annually averaged present-day forcing of +0.22 W m(sup -2) and year 2100 forcing of +0.57 W m(sup -2) at the top of the atmosphere (TOA). Net anthropogenic TOA forcing by internally mixed sulfate, nitrate, organic carbon, and black carbon aerosols is estimated to be virtually zero in the present-day and +0.34 W m(sup -2) in year 2100, whereas it is predicted to be -0.39 W m(sup -2) in present-day and -0.61 W m(sup -2) in year 2100 if the aerosols are externally mixed. Heterogeneous reactions are shown to be important in affecting anthropogenic forcing. When reactions of N2O5, NO3, NO2, and HO2 on aerosols are accounted for, TOA anthropogenic O3 forcing is less by 20-45% in present-day and by 20-32% in year 2100 at mid to high latitudes in the Northern Hemisphere, as compared with values predicted in the absence of heterogeneous gas aerosol reactions. Mineral dust uptake of HNO3 and O3 is shown to have practically no influence on anthropogenic O3 forcing. Heterogeneous reactions of N2Os

  7. Identification of aerosol composition from multi-wavelength lidar measurements

    NASA Technical Reports Server (NTRS)

    Wood, S. A.

    1984-01-01

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

  8. SECONDARY ORGANIC AEROSOL FORMATION FROM THE OXIDATION OF AROMATIC HYDROCARBONS IN THE PRESENCE OF DRY SUBMICRON AMMONIUM SULFATE AEROSOL

    EPA Science Inventory

    A laboratory study was conducted to examine formation of secondary organic aerosols. A smog chamber system was developed for studying gas-aerosol interactions in a dynamic flow reactor. These experiments were conducted to investigate the fate of gas and aerosol phase compounds ...

  9. Aromatic organosulfates in atmospheric aerosols: synthesis, characterization, and abundance.

    PubMed

    Staudt, Sean; Kundu, Shuvashish; Lehmler, Hans-Joachim; He, Xianran; Cui, Tianqu; Lin, Ying-Hsuan; Kristensen, Kasper; Glasius, Marianne; Zhang, Xiaolu; Weber, Rodney J; Surratt, Jason D; Stone1, Elizabeth A

    2014-09-01

    Aromatic organosulfates are identified and quantified in fine particulate matter (PM 2.5 ) from Lahore, Pakistan, Godavari, Nepal, and Pasadena, California. To support detection and quantification, authentic standards of phenyl sulfate, benzyl sulfate, 3-and 4-methylphenyl sulfate and 2-, 3-, and 4-methylbenzyl sulfate were synthesized. Authentic standards and aerosol samples were analyzed by ultra-performance liquid chromatography (UPLC) coupled to negative electrospray ionization (ESI) quadrupole time-of-flight (ToF) mass spectrometry. Benzyl sulfate was present in all three locations at concentrations ranging from 4 - 90 pg m -3 . Phenyl sulfate, methylphenyl sulfates and methylbenzyl sulfates were observed intermittently with abundances of 4 pg m -3 , 2-31 pg m -3 , 109 pg m -3 , respectively. Characteristic fragment ions of aromatic organosulfates include the sulfite radical ( • SO 3 - , m/z 80) and the sulfate radical ( • SO 4 - , m/z 96). Instrumental response factors of phenyl and benzyl sulfates varied by a factor of 4.3, indicating that structurally-similar organosulfates may have significantly different instrumental responses and highlighting the need to develop authentic standards for absolute quantitation organosulfates. In an effort to better understand the sources of aromatic organosulfates to the atmosphere, chamber experiments with the precursor toluene were conducted under conditions that form biogenic organosulfates. Aromatic organosulfates were not detected in the chamber samples, suggesting that they form through different pathways, have different precursors (e.g. naphthalene or methylnaphthalene), or are emitted from primary sources.

  10. Aromatic organosulfates in atmospheric aerosols: Synthesis, characterization, and abundance

    NASA Astrophysics Data System (ADS)

    Staudt, Sean; Kundu, Shuvashish; Lehmler, Hans-Joachim; He, Xianran; Cui, Tianqu; Lin, Ying-Hsuan; Kristensen, Kasper; Glasius, Marianne; Zhang, Xiaolu; Weber, Rodney J.; Surratt, Jason D.; Stone, Elizabeth A.

    2014-09-01

    Aromatic organosulfates are identified and quantified in fine particulate matter (PM2.5) from Lahore, Pakistan, Godavari, Nepal, and Pasadena, California. To support detection and quantification, authentic standards of phenyl sulfate, benzyl sulfate, 3- and 4-methylphenyl sulfate and 2-, 3-, and 4-methylbenzyl sulfate were synthesized. Authentic standards and aerosol samples were analyzed by ultra-performance liquid chromatography (UPLC) coupled to negative electrospray ionization (ESI) quadrupole time-of-flight (ToF) mass spectrometry. Benzyl sulfate was present in all three locations at concentrations ranging from 4 to 90 pg m-3. Phenyl sulfate, methylphenyl sulfates and methylbenzyl sulfates were observed intermittently with abundances of 4 pg m-3, 2-31 pg m-3, 109 pg m-3, respectively. Characteristic fragment ions of aromatic organosulfates include the sulfite radical (rad SO3-, m/z 80) and the sulfate radical (rad SO4-, m/z 96). Instrumental response factors of phenyl and benzyl sulfates varied by a factor of 4.3, indicating that structurally-similar organosulfates have significantly different instrumental responses and highlighting the need to develop authentic standards for absolute quantitation organosulfates. In an effort to better understand the sources of aromatic organosulfates to the atmosphere, chamber experiments with the precursor toluene were conducted under conditions that form biogenic organosulfates. Aromatic organosulfates were not detected in the chamber samples, suggesting that they form through different pathways, have different precursors (e.g. naphthalene or methylnaphthalene), or are emitted from primary sources.

  11. ARM-Led Improvements Aerosols in Climate and Climate Models

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

    Ghan, Steven J.; Penner, Joyce E.

    2016-07-25

    The DOE ARM program has played a foundational role in efforts to quantify aerosol effects on climate, beginning with the early back-of-the-envelope estimates of direct radiative forcing by anthropogenic sulfate and biomass burning aerosol (Penner et al., 1994). In this chapter we review the role that ARM has played in subsequent detailed estimates based on physically-based representations of aerosols in climate models. The focus is on quantifying the direct and indirect effects of anthropogenic aerosol on the planetary energy balance. Only recently have other DOE programs applied the aerosol modeling capability to simulate the climate response to the radiative forcing.

  12. Size distribution of ions in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Krivácsy, Z.; Molnár, Á.

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

  13. Trace Gas/Aerosol Interactions and GMI Modeling Support

    NASA Technical Reports Server (NTRS)

    Penner, Joyce E.; Liu, Xiaohong; Das, Bigyani; Bergmann, Dan; Rodriquez, Jose M.; Strahan, Susan; Wang, Minghuai; Feng, Yan

    2005-01-01

    Current global aerosol models use different physical and chemical schemes and parameters, different meteorological fields, and often different emission sources. Since the physical and chemical parameterization schemes are often tuned to obtain results that are consistent with observations, it is difficult to assess the true uncertainty due to meteorology alone. Under the framework of the NASA global modeling initiative (GMI), the differences and uncertainties in aerosol simulations (for sulfate, organic carbon, black carbon, dust and sea salt) solely due to different meteorological fields are analyzed and quantified. Three meteorological datasets available from the NASA DAO GCM, the GISS-II' GCM, and the NASA finite volume GCM (FVGCM) are used to drive the same aerosol model. The global sulfate and mineral dust burdens with FVGCM fields are 40% and 20% less than those with DAO and GISS fields, respectively due to its heavier rainfall. Meanwhile, the sea salt burden predicted with FVGCM fields is 56% and 43% higher than those with DAO and GISS, respectively, due to its stronger convection especially over the Southern Hemispheric Ocean. Sulfate concentrations at the surface in the Northern Hemisphere extratropics and in the middle to upper troposphere differ by more than a factor of 3 between the three meteorological datasets. The agreement between model calculated and observed aerosol concentrations in the industrial regions (e.g., North America and Europe) is quite similar for all three meteorological datasets. Away from the source regions, however, the comparisons with observations differ greatly for DAO, FVGCM and GISS, and the performance of the model using different datasets varies largely depending on sites and species. Global annual average aerosol optical depth at 550 nm is 0.120-0.131 for the three meteorological datasets.

  14. Field and Laboratory Studies of Atmospheric Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Coggon, Matthew Mitchell

    these conditions to all measurements conducted during E-PEACE demonstrated that a large fraction of cloud droplet (72%) and dry aerosol mass (12%) sampled in the California coastal study region was heavily or moderately influenced by ship emissions. Another study investigated the chemical and physical evolution of a controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed of oxidized organic compounds contributed nearly an order of magnitude more cloud condensation nuclei (CCN) than less oxidized particles formed under cloudy conditions. The processing time necessary for particles to become CCN active was short ( 4 hr). Laboratory chamber experiments were also conducted to evaluate particle-phase processes influencing aerosol phase and composition. In one study, ammonium sulfate seed was coated with a layer of secondary organic aerosol (SOA) from toluene oxidation followed by a layer of SOA from α-pinene oxidation. The system exhibited different evaporative properties than ammonium sulfate seed initially coated with α-pinene SOA followed by a layer of toluene SOA. This behavior is consistent with a shell-and-core model and suggests limited mixing among different SOA types. Another study investigated the reactive uptake of isoprene epoxy diols (IEPOX) onto non-acidified aerosol. It was demonstrated that particle acidity has limited influence on organic aerosol formation onto ammonium sulfate seed, and that the chemical system is limited by the availability of nucleophiles such as sulfate. Flow tube experiments were conducted to examine the role of iron in the reactive uptake and chemical oxidation of glycolaldehyde. Aerosol particles doped with iron and hydrogen peroxide were mixed with gas-phase glycolaldehyde and photochemically aged in a custom-built flow reactor. Compared to particles free of iron, iron-doped aerosols significantly enhanced the oxygen to carbon (O/C) ratio of accumulated organic mass. The primary

  15. Impacts of stratospheric sulfate geoengineering on tropospheric ozone

    NASA Astrophysics Data System (ADS)

    Xia, Lili; Nowack, Peer J.; Tilmes, Simone; Robock, Alan

    2017-10-01

    A range of solar radiation management (SRM) techniques has been proposed to counter anthropogenic climate change. Here, we examine the potential effects of stratospheric sulfate aerosols and solar insolation reduction on tropospheric ozone and ozone at Earth's surface. Ozone is a key air pollutant, which can produce respiratory diseases and crop damage. Using a version of the Community Earth System Model from the National Center for Atmospheric Research that includes comprehensive tropospheric and stratospheric chemistry, we model both stratospheric sulfur injection and solar irradiance reduction schemes, with the aim of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This allows us to compare the impacts of sulfate aerosols and solar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate injection decreases it. A fundamental difference between the two geoengineering schemes is the importance of heterogeneous reactions in the photochemical ozone balance with larger stratospheric sulfate abundance, resulting in increased ozone depletion in mid- and high latitudes. This reduces the net transport of stratospheric ozone into the troposphere and thus is a key driver of the overall decrease in surface ozone. At the same time, the change in stratospheric ozone alters the tropospheric photochemical environment due to enhanced ultraviolet radiation. A shared factor among both SRM scenarios is decreased chemical ozone loss due to reduced tropospheric humidity. Under insolation reduction, this is the dominant factor giving rise to the global surface ozone increase. Regionally, both surface ozone increases and decreases are found for both scenarios; that is, SRM would affect regions of the world differently in terms of air pollution. In conclusion

  16. Sensitivity of aerosol loading and properties to cloudiness

    NASA Astrophysics Data System (ADS)

    Iversen, T.; Seland, O.; Kirkevag, A.; Kristjansson, J. E.

    2005-12-01

    Clouds influence aerosols in various ways. Sulfate is swiftly produced in liquid phase provided there is both sulfur dioxide and oxidants available. Nucleation and Aitken mode aerosol particles efficiently grow in size by collision and coagulation with cloud droplets. When precipitation is formed, aerosol and precursor gases may be quickly removed bay rainout. The dynamics associated with clouds in some cases may swiftly mix aerosols deeply into the troposphere. In some cases Aitken-mode particles may be formed in cloud droplets by splitting agglomerates of particulate matter such as black carbon In this presentation we will discuss how global cloudiness may influence the burden, residence time, and spatial distribution of sulfate, black carbon and particulate organic matter. A similar physico-chemical scheme for there compounds has been implemented in three generations of the NCAR community climate model (CCM3, CAM2 and CAM3). The scheme is documented in the literature and is a part of the Aerocom-intercomparison. There are many differences between these models. With respect to aerosols, a major difference is that CAM3 has a considerably higher global cloud volume and more then twice the amount of cloud water than CAM2 and CCM3. Atmospheric simulations have been made with prescribed ocean temperatures. It is slightly surprising to discover that certain aspects of the aerosols are not particularly sensitive to these differences in cloud availability. This sensitivity will be compared to sensitivities with respect to processing in deep convective clouds.

  17. Evaluation of ultraviolet radiation, ozone and aerosol interactions in the troposphere using automatic differentiation. Final report

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

    Carmichael, G.R.; Potra, F.

    1998-10-06

    A major goal of this research was to quantify the interactions between UVR, ozone and aerosols. One method of quantification was to calculate sensitivity coefficients. A novel aspect of this work was the use of Automatic Differentiation software to calculate the sensitivities. The authors demonstrated the use of ADIFOR for the first time in a dimensional framework. Automatic Differentiation was used to calculate such quantities as: sensitivities of UV-B fluxes to changes in ozone and aerosols in the stratosphere and the troposphere; changes in ozone production/destruction rates to changes in UV-B flux; aerosol properties including loading, scattering properties (including relativemore » humidity effects), and composition (mineral dust, soot, and sulfate aerosol, etc.). The combined radiation/chemistry model offers an important test of the utility of Automatic Differentiation as a tool in atmospheric modeling.« less

  18. Photochemistry of Glyoxal in Wet Aerosols: Smog Chamber Study

    NASA Astrophysics Data System (ADS)

    Lim, Y. B.; Kim, H.; Turpin, B. J.

    2015-12-01

    Aqueous chemistry is an important pathway for the formation of secondary organic aerosol (SOA). Reaction vessel studies provide evidence that in the aqueous phase photooxidation of water soluble organic compounds (e.g., glyoxal, methylglyoxal) form multifunctional organic products and oligomers. In this work, we extend this bulk-phase chemistry to the condensed-phase chemistry that occurs in/on aerosols by conducting smog chamber experiments — photooxidation of ammonium sulfate and sulfuric acid aerosols containing glyoxal and hydrogen peroxide in the presence of NOx under dry/humid conditions. Particles were analyzed using ultra performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). In the irradiated chamber, photooxidation products of glyoxal as seen in reaction vessel experiments (e.g., oxalic acids and tartaric acids) were also formed in both ammonium sulfate aerosols and sulfuric acid aerosols at humid and even dry conditions. However, the major products were organosulfurs (CHOS), organonitrogens (CHON), and nitrooxy-organosulfates (CHONS), which were also dominantly formed in the dark chamber. These products were formed via non-radical reactions, which depend on acidity and humidity. However, the real-time profiles in the dark chamber and the irradiated chamber were very different, suggesting photochemistry substantially affects non-radical formation in the condensed phase.

  19. Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Wang, Xiaowei; Jing, Bo; Tan, Fang; Ma, Jiabi; Zhang, Yunhong; Ge, Maofa

    2017-10-01

    Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA) and mixed particles composed of ammonium sulfate (AS) and OA with different organic to inorganic molar ratios (OIRs) have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH), and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH) for mixed OA / AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH) of AS in mixed OA / AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA / AS droplets indicate the formation of ammonium hydrogen oxalate (NH4HC2O4) and ammonium hydrogen sulfate (NH4HSO4) from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA / AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH4)2SO4 into NH4HC2O4 with a high DRH. Although the hygroscopic growth of mixed OA / AS droplets is comparable to that of AS or OA at high RH during the dehydration process, Raman growth

  20. Vacuum FTIR Observation on the Dynamic Hygroscopicity of Aerosols under Pulsed Relative Humidity.

    PubMed

    Leng, Chun-Bo; Pang, Shu-Feng; Zhang, Yun; Cai, Chen; Liu, Yong; Zhang, Yun-Hong

    2015-08-04

    A novel approach based on a combination of a pulse RH controlling system and a rapid scan vacuum FTIR spectrometer (PRHCS-RSVFTIR) was utilized to investigate dynamic hygroscopicity of two atmospheric aerosols: ammonium sulfate ((NH4)2SO4) and magnesium sulfate (MgSO4). In this approach, rapid-scan infrared spectra of water vapor and aerosols were obtained to determine relative humidity (RH) in sample cell and hygroscopic property of aerosols with a subsecond time resolution. Heterogeneous nucleation rates of (NH4)2SO4 were, for the first time, measured under low RH conditions (<35% RH). In addition, studies of MgSO4 aerosols revealed that water mass transport may be limited by different processes depending on RH values (surface limited at 40% < RH < 52% and bulk phase limited at RH < 40%). Furthermore, we are also the first to report water diffusion constants in micron size MgSO4 aerosols at very low RH values. Our results have shown that the PRHCS-RSVFTIR is well-suited for determination of hygroscopicity of atmospheric aerosols and water transport and nucleation kinetics of liquid aerosols.

  1. Formation of light absorbing organo-nitrogen species from evaporation of droplets containing glyoxal and ammonium sulfate.

    PubMed

    Lee, Alex K Y; Zhao, Ran; Li, Richard; Liggio, John; Li, Shao-Meng; Abbatt, Jonathan P D

    2013-11-19

    In the atmosphere, volatile organic compounds such as glyoxal can partition into aqueous droplets containing significant levels of inorganic salts. Upon droplet evaporation, both the organics and inorganic ions become highly concentrated, accelerating reactions between them. To demonstrate this process, we investigated the formation of organo-nitrogen and light absorbing materials in evaporating droplets containing glyoxal and different ammonium salts including (NH4)2SO4, NH4NO3, and NH4Cl. Our results demonstrate that evaporating glyoxal-(NH4)2SO4 droplets produce light absorbing species on a time scale of seconds, which is orders of magnitude faster than observed in bulk solutions. Using aerosol mass spectrometry, we show that particle-phase organics with high N:C ratios were formed when ammonium salts were used, and that the presence of sulfate ions promoted this chemistry. Since sulfate can also significantly enhance the Henry's law partitioning of glyoxal, our results highlight the atmospheric importance of such inorganic-organic interactions in aqueous phase aerosol chemistry.

  2. Evaluating Secondary Inorganic Aerosols in Three Dimensions

    NASA Technical Reports Server (NTRS)

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

    2016-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2007-01-01

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

  4. Aerosol concentrations and composition in the North Pacific marine boundary layer

    NASA Astrophysics Data System (ADS)

    Choi, Yongjoo; Rhee, Tae Siek; Collett, Jeffrey L.; Park, Taehyun; Park, Seung-Myung; Seo, Beom-Keun; Park, Gyutae; Park, Keyhong; Lee, Taehyoung

    2017-12-01

    Ship-borne measurements of inorganic and organic aerosols, including methanesulfonic acid (MSA), were conducted over the Northern Pacific using a High Resolution Time of Flight Aerosol Mass Spectrometer (AMS). This study, conducted aboard the Korean ice breaker R/V Araon, was part of the SHIP-borne Pole-to-Pole Observations (SHIPPO) project. Based on air mass source region, the cruise track could be divided into five sections. Overall, the South Asia and Northern Japan ship transects showed higher aerosol concentrations due to continental pollution and biomass burning sources, respectively. In all five regions, the average mass concentrations of sulfate and organic aerosols (OA) were much higher than concentrations of nitrate and ammonium. Positive matrix factorization (PMF) analysis distinguished two organic aerosol factors as hydrocarbon-like and oxidized OA (HOA and OOA). HOA peaked in South Asia under the influence of anthropogenic pollution source areas, such as China and Korea, and generally decreased with increasing latitude across the full study region. OOA concentrations peaked in Northern Japan near the Tsugaru Strait and appear to reflect fine particle contributions from biomass burning. The mean HOA concentration in the clean marine area (Aleutian Island to Siberia) was 0.06 μg/m3 and comprised approximately 8% of the OA mass fraction. The highest MSA concentrations peaked in the Aleutian Islands at nearly 15 μg/m3, suggesting influence from higher dimethyl sulfide (DMS) emissions resulting from biological nutrient uptake during summer. The MSA/sulfate ratio, an indicator of the relative fine particle contributions of DMS and anthropogenic sources, revealed a sharp gradient as the ship approached the clean marine areas where the dominance of DMS increased. The patterns in OOA, HOA, and MSA concentrations found in this study provide a better understanding of the characteristics of inorganic and organic aerosols in the Northern Pacific Ocean.

  5. Simulating the Effects of Semivolatile Compounds on Cloud Processing of Aerosol

    NASA Astrophysics Data System (ADS)

    Kokkola, H.; Kudzotsa, I.; Tonttila, J.; Raatikainen, T.; Romakkaniemi, S.

    2017-12-01

    Aerosol removal processes largely dictate how well aerosol is transported in the atmosphere and thus the aerosol load over remote regions depends on how effectively aerosol is removed during its transport from the source regions. This means that in order to model the global distribution aerosol, both in vertical and horizontal, wet deposition processes have to be properly modelled. However, in large scale models, the description of wet removal and the vertical redistribution of aerosol by cloud processes is often extremely simplified.Here we present a novel aerosol-cloud model SALSA, where the aerosol properties are tracked through different cloud processes. These processes include: cloud droplet activation, precipitation formation, ice nucleation, melting, and evaporation. It is a sectional model that includes separate size sections for non-activated aerosol, cloud droplets, precipitation droplets, and ice crystals. The aerosol-cloud model was coupled to a large eddy model UCLALES which simulates the boundary-layer dynamics. In this study, the model has been applied in studying the wet removal as well as interactions between aerosol, clouds, and semi-volatile compounds, ammonia and nitric acid. These semi-volative compounds are special in the sense that they co-condense together with water during cloud activation and have been suggested to form droplets that can be considered cloud-droplet-like already in subsaturated conditions. In our model, we calculate the kinetic partitioning of ammonia and sulfate thus explicitly taking into account the effect of ammonia and nitric acid in the cloud formation. Our simulations indicate that especially in polluted conditions, these compounds significantly affect the properties of cloud droplets thus significantly affecting the lifecycle of different aerosol compounds.

  6. Aerosol analysis and forecast in the European Centre for Medium-Range Weather Forecasts Integrated Forecast System: 3. Evaluation by means of case studies

    NASA Astrophysics Data System (ADS)

    Mangold, A.; de Backer, H.; de Paepe, B.; Dewitte, S.; Chiapello, I.; Derimian, Y.; Kacenelenbogen, M.; LéOn, J.-F.; Huneeus, N.; Schulz, M.; Ceburnis, D.; O'Dowd, C.; Flentje, H.; Kinne, S.; Benedetti, A.; Morcrette, J.-J.; Boucher, O.

    2011-02-01

    A near real-time system for assimilation and forecasts of aerosols, greenhouse and trace gases, extending the ECMWF Integrated Forecasting System (IFS), has been developed in the framework of the Global and regional Earth-system Monitoring using Satellite and in-situ data (GEMS) project. The GEMS aerosol modeling system is novel as it is the first aerosol model fully coupled to a numerical weather prediction model with data assimilation. A reanalysis of the period 2003-2009 has been carried out with the same system. During its development phase, the aerosol system was first run for the time period January 2003 to December 2004 and included sea salt, desert dust, organic matter, black carbon, and sulfate aerosols. In the analysis, Moderate Resolution Imaging Spectroradiometer (MODIS) total aerosol optical depth (AOD) at 550 nm over ocean and land (except over bright surfaces) was assimilated. This work evaluates the performance of the aerosol system by means of case studies. The case studies include (1) the summer heat wave in Europe in August 2003, characterized by forest fire aerosol and conditions of high temperatures and stagnation, favoring photochemistry and secondary aerosol formation, (2) a large Saharan dust event in March 2004, and (3) periods of high and low sea salt aerosol production. During the heat wave period in 2003, the linear correlation coefficients between modeled and observed AOD (550 nm) and between modeled and observed PM2.5 mass concentrations are 0.82 and 0.71, respectively, for all investigated sites together. The AOD is slightly and the PM2.5 mass concentration is clearly overestimated by the aerosol model during this period. The simulated sulfate mass concentration is significantly correlated with observations but is distinctly overestimated. The horizontal and vertical locations of the main features of the aerosol distribution during the Saharan dust outbreak are generally well captured, as well as the timing of the AOD peaks. The

  7. Measurements of Hygroscopicity- and Size-Resolved Sea Spray Aerosol

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  8. Coupled Aerosol-Chemistry-Climate Twentieth-Century Transient Model Investigation: Trends in Short-Lived Species and Climate Responses

    NASA Technical Reports Server (NTRS)

    Koch, Dorothy; Bauer, Susanne E.; Del Genio, Anthony; Faluvegi, Greg; McConnell, Joseph R.; Menon, Surabi; Miller, Ronald L.; Rind, David; Ruedy, Reto; Schmidt, Gavin A.; hide

    2011-01-01

    The authors simulate transient twentieth-century climate in the Goddard Institute for Space Studies (GISS) GCM, with aerosol and ozone chemistry fully coupled to one another and to climate including a full dynamic ocean. Aerosols include sulfate, black carbon (BC), organic carbon, nitrate, sea salt, and dust. Direct and BC snow-albedo radiative effects are included. Model BC and sulfur trends agree fairly well with records from Greenland and European ice cores and with sulfur deposition in North America; however, the model underestimates the sulfur decline at the end of the century in Greenland. Global BC effects peak early in the century (1940s); afterward the BC effects decrease at high latitudes of the Northern Hemisphere but continue to increase at lower latitudes. The largest increase in aerosol optical depth occurs in the middle of the century (1940s-80s) when sulfate forcing peaks and causes global dimming. After this, aerosols decrease in eastern North America and northern Eurasia leading to regional positive forcing changes and brightening. These surface forcing changes have the correct trend but are too weak. Over the century, the net aerosol direct effect is -0.41 Watts per square meter, the BC-albedo effect is -0.02 Watts per square meter, and the net ozone forcing is +0.24 Watts per square meter. The model polar stratospheric ozone depletion develops, beginning in the 1970s. Concurrently, the sea salt load and negative radiative flux increase over the oceans around Antarctica. Net warming over the century is modeled fairly well; however, the model fails to capture the dynamics of the observedmidcentury cooling followed by the late century warming.Over the century, 20% of Arctic warming and snow ice cover loss is attributed to the BC albedo effect. However, the decrease in this effect at the end of the century contributes to Arctic cooling. To test the climate responses to sulfate and BC pollution, two experiments were branched from 1970 that removed

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

    NASA Astrophysics Data System (ADS)

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

    2018-05-01

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

  10. Prediction of health effects of cross-border atmospheric pollutants using an aerosol forecast model.

    PubMed

    Onishi, Kazunari; Sekiyama, Tsuyoshi Thomas; Nojima, Masanori; Kurosaki, Yasunori; Fujitani, Yusuke; Otani, Shinji; Maki, Takashi; Shinoda, Masato; Kurozawa, Youichi; Yamagata, Zentaro

    2018-08-01

    Health effects of cross-border air pollutants and Asian dust are of significant concern in Japan. Currently, models predicting the arrival of aerosols have not investigated the association between arrival predictions and health effects. We investigated the association between subjective health symptoms and unreleased aerosol data from the Model of Aerosol Species in the Global Atmosphere (MASINGAR) acquired from the Japan Meteorological Agency, with the objective of ascertaining if these data could be applied to predicting health effects. Subjective symptom scores were collected via self-administered questionnaires and, along with modeled surface aerosol concentration data, were used to conduct a risk evaluation using generalized estimating equations between October and November 2011. Altogether, 29 individuals provided 1670 responses. Spearman's correlation coefficients were determined for the relationship between the proportion of the participants reporting the maximum score of two or more for each symptom and the surface concentrations for each considered aerosol species calculated using MASINGAR; the coefficients showed significant intermediate correlations between surface sulfate aerosol concentration and respiratory, throat, and fever symptoms (R = 0.557, 0.454, and 0.470, respectively; p < 0.01). In the general estimation equation (logit link) analyses, a significant linear association of surface sulfate aerosol concentration, with an endpoint determined by reported respiratory symptom scores of two or more, was observed (P trend = 0.001, odds ratio [OR] of the highest quartile [Q4] vs. the lowest [Q1] = 5.31, 95% CI = 2.18 to 12.96), with adjustment for potential confounding. The surface sulfate aerosol concentration was also associated with throat and fever symptoms. In conclusion, our findings suggest that modeled data are potentially useful for predicting health risks of cross-border aerosol arrivals. Copyright © 2018 Elsevier Ltd

  11. The effect of formaldehyde and nitrogen-containing compounds on the size and volume of aerosol particles

    NASA Astrophysics Data System (ADS)

    Millage, K.; Galloway, M. M.; De Haan, D. O.

    2012-12-01

    Atmospheric aerosol can interact with clouds in many ways, often resulting in the redistribution or absorption of solar energy or changes in precipitation efficiency. Secondary organic aerosol (SOA) in particular has been linked to climate change and a reduction in the number and size of cloud particles. The reactions of nitrogen containing compounds (primary amines, amino acids and ammonium sulfate) with carbonyl compounds (such as formaldehyde and glycolaldehyde) are potential sources of SOA. Aerosol containing formaldehyde and nitrogen-containing compounds (glycine, methylamine, arginine, or ammonium sulfate) was generated from buffered solutions (pH 5.4) using a nebulizer. The aerosol was then equilibrated into a chamber containing humid air (82-84% RH), and particle sizes were measured using a SMPS system over a period of 1 hour in order to examine how the size and volume of the aerosol particles changed. Formaldehyde concentrations were varied over multiple experiments. Arginine displayed a trend of increasing relative particle size with increasing formaldehyde concentration. Ammonium sulfate and formaldehyde displayed a decrease in relative particle sizes from 0:1 to 2:1 ratios of formaldehyde to ammonium sulfate, but then an increase in relative particle sizes with increasing amounts of formaldehyde. Similarly, glycine and methylamine initially displayed decreasing relative particle sizes, until reaching a 1:1 ratio of each to formaldehyde at which point the relative particle sizes steadily increased. These effects were likely caused by the evaporation of first-generation imine products.

  12. 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.

  13. Characterization of distinct Arctic aerosol accumulation modes and their sources

    NASA Astrophysics Data System (ADS)

    Lange, R.; Dall'Osto, M.; Skov, H.; Nøjgaard, J. K.; Nielsen, I. E.; Beddows, D. C. S.; Simo, R.; Harrison, R. M.; Massling, A.

    2018-06-01

    In this work we use cluster analysis of long term particle size distribution data to expand an array of different shorter term atmospheric measurements, thereby gaining insights into longer term patterns and properties of Arctic aerosol. Measurements of aerosol number size distributions (9-915 nm) were conducted at Villum Research Station (VRS), Station Nord in North Greenland during a 5 year record (2012-2016). Alongside this, measurements of aerosol composition, meteorological parameters, gaseous compounds and cloud condensation nuclei (CCN) activity were performed during different shorter occasions. K-means clustering analysis of particle number size distributions on daily basis identified several clusters. Clusters of accumulation mode aerosols (main size modes > 100 nm) accounted for 56% of the total aerosol during the sampling period (89-91% during February-April, 1-3% during June-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking in February-April, with highest loadings of sulfate and black carbon concentrations. (2) Accumulation mode Bimodal aerosol shows two modes, at 38 nm and 150 nm, peaking in June-August, with the highest ratio of organics to sulfate concentrations. (3) Aged accumulation mode aerosol shows a single mode at 213 nm, peaking in September-October and is associated with cloudy and humid weather conditions during autumn. The three aerosol clusters were considered alongside CCN concentrations. We suggest that organic compounds, that are likely marine biogenic in nature, greatly influence the Bimodal cluster and contribute significantly to its CCN activity. This stresses the importance of better characterizing the marine ecosystem and the aerosol-mediated climate effects in the

  14. The influence of different black carbon and sulfate mixing methods on their optical and radiative properties

    NASA Astrophysics Data System (ADS)

    Zhang, Hua; Zhou, Chen; Wang, Zhili; Zhao, Shuyun; Li, Jiangnan

    2015-08-01

    Three different internal mixing methods (Core-Shell, Maxwell-Garnett, and Bruggeman) and one external mixing method are used to study the impact of mixing methods of black carbon (BC) with sulfate aerosol on their optical properties, radiative flux, and heating rate. The optical properties of a mixture of BC and sulfate aerosol particles are considered for three typical bands. The results show that mixing methods, the volume ratio of BC to sulfate, and relative humidity have a strong influence on the optical properties of mixed aerosols. Compared to internal mixing, external mixing underestimates the particle mass absorption coefficient by 20-70% and the particle mass scattering coefficient by up to 50%, whereas it overestimates the particle single scattering albedo by 20-50% in most cases. However, the asymmetry parameter is strongly sensitive to the equivalent particle radius, but is only weakly sensitive to the different mixing methods. Of the internal methods, there is less than 2% difference in all optical properties between the Maxwell-Garnett and Bruggeman methods in all bands; however, the differences between the Core-Shell and Maxwell-Garnett/Bruggeman methods are usually larger than 15% in the ultraviolet and visible bands. A sensitivity test is conducted with the Beijing Climate Center Radiation transfer model (BCC-RAD) using a simulated BC concentration that is typical of east-central China and a sulfate volume ratio of 75%. The results show that the internal mixing methods could reduce the radiative flux more effectively because they produce a higher absorption. The annual mean instantaneous radiative force due to BC-sulfate aerosol is about -3.18 W/m2 for the external method and -6.91 W/m2 for the internal methods at the surface, and -3.03/-1.56/-1.85 W/m2 for the external/Core-Shell/(Maxwell-Garnett/Bruggeman) methods, respectively, at the tropopause.

  15. The Impact of Geoengineering Aerosols on Stratospheric Temperature and Ozone

    NASA Technical Reports Server (NTRS)

    Heckendorn, P.; Weisenstein, D.; Fueglistaler, S.; Luo, B. P.; Rozanov, E.; Schraner, M.; Peter, T.; Thomason, L. W.

    2009-01-01

    Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model, to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H2O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will be significantly reduced.

  16. The Impact of Geoengineering Aerosols on Stratospheric Temperature and Ozone

    NASA Technical Reports Server (NTRS)

    Heckendorn, P.; Weisenstein, D.; Fueglistaler, S.; Luo, B. P.; Rozanov, E.; Schraner, M.; Thomason, L. W.; Peter, T.

    2011-01-01

    Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model. to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H2O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will he significantly reduced.

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

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

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

  18. Modern Day Re-analysis of Pinatubo SO2 Injection, Cloud dispersion and Stratospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Bhartia, P. K.; Krotkov, N. A.; Aquila, V.; Hughes, E. J.; Li, C.; Fisher, B. L.

    2016-12-01

    Cataclysmic June 15 1991 eruption of Mt. Pinatubo injected largest amount of SO2 in the lower stratosphere during the satellite era. The resulting volcanic clouds were tracked by the NASA's Nimbus 7 TOMS sensor that provided first estimates of total emissions of SO2 gas ( 15+/-3 Mt). Over time SO2 converted to long-lasting sulfate aerosols affecting radiation balance and composition of the stratosphere. Large numbers of articles and papers published in the past 25 years make this the most well-studied volcanic eruption. Still, several unresolved scientific issues remain: SO2 injection height, subsequent lofting of SO2 and aerosols in the stratosphere, how much sulfate aerosols were produced in the eruption (i.e., initial sulfate to SO2 ratio), and impact on stratospheric ozone. To answer these questions we have re-analyzed past satellite measurements using modern day tools, such as re-analyzed wind data from Goddard Modeling and Assimilation Office (GMAO), improved trajectory analysis tools, better radiative transfer model to process backscatter UV data from N7/TOMS and two NOAA SBUV/2s sensors, which provided measurements at shorter UV wavelengths that are sensitive to aerosols and SO2 in the mid stratosphere ( 25 km). We have also re-analyzed aerosol data from SAGE, AVHRR, and several instruments on the UARS satellite. These data provide strong support for recent assessment by modelers that the bulk of SO2 mass injected by the volcano was well below the 25 km altitude, contrary to earlier estimates. We also find convincing evidence that there was significant amount of sulfate aerosols embedded even in the day-old SO2 cloud. These results strongly support the hypothesis that SO2 gas self-lofted to 25 km as seeen by UARS MLS several weeks after the eruption and aerosols to 35 km, as seen by the SAGE sensor several months later.

  19. INTERCOMPARISON OF PERIODIC FINE PARTICLE SULFUR AND SULFATE CONCENTRATION RESULTS

    EPA Science Inventory

    A one-week study was conducted in August 1979 to evaluate the comparative ability of representative aerosol sampling systems to monitor fine particulate sulfur and sulfate concentrations periodically in situ. Participants in the study operated their samplers simultaneously in the...

  20. Aerosolization Characteristics of Dry Powder Inhaler Formulations for the Excipient Enhanced Growth (EEG) Application: Effect of Spray Drying Process Conditions on Aerosol Performance

    PubMed Central

    Son, Yoen-Ju; Longest, P. Worth; Hindle, Michael

    2013-01-01

    The aim of this study was to develop a spray dried submicrometer powder formulation suitable for the excipient enhanced growth (EEG) application. Combination particles were prepared using the Buchi Nano spray dryer B-90. A number of spray drying and formulation variables were investigated with the aims of producing dry powder formulations that were readily dispersed upon aerosolization and maximizing the fraction of submicrometer particles. Albuterol sulfate, mannitol, L-leucine, and poloxamer 188 were selected as a model drug, hygroscopic excipient, dispersibility enhancer and surfactant, respectively. Formulations were assessed by scanning electron microscopy and aerosol performance following aerosolization using an Aerolizer® dry powder inhaler (DPI). In vitro drug deposition was studied using a realistic mouth-throat (MT) model. Based on the in vitro aerosolization results, the best performing submicrometer powder formulation consisted of albuterol sulfate, mannitol, L-leucine and poloxamer 188 in a ratio of 30:48:20:2, containing 0.5% solids in a water:ethanol (80:20% v/v) solution which was spray dried at 70 °C. The submicrometer particle fraction (FPF1μm/ED) of this final formulation was 28.3% with more than 80% of the capsule contents being emitted during aerosolization. This formulation also showed 4.1% MT deposition. The developed combination formulation delivered a powder aerosol developed for the EEG application with high dispersion efficiency and low MT deposition from a convenient DPI device platform. PMID:23313343

  1. 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.

  2. Physical properties of the stratospheric aerosols

    NASA Technical Reports Server (NTRS)

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

    1973-01-01

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

  3. Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

    NASA Astrophysics Data System (ADS)

    Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

    2017-12-01

    The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

  4. 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

  5. Small molecules as tracers in atmospheric secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Yu, Ge

    Secondary organic aerosol (SOA), formed from in-air oxidation of volatile organic compounds, greatly affects human health and climate. Although substantial research has been devoted to SOA formation and evolution, the modeled and lab-generated SOA are still low in mass and degree of oxidation compared to ambient measurements. In order to compensate for these discrepancies, the aqueous processing pathway has been brought to attention. The atmospheric waters serve as aqueous reaction media for dissolved organics to undergo further oxidation, oligomerization, or other functionalization reactions, which decreases the vapor pressure while increasing the oxidation state of carbon atoms. Field evidence for aqueous processing requires the identification of tracer products such as organosulfates. We synthesized the standards for two organosulfates, glycolic acid sulfate and lactic acid sulfate, in order to measure their aerosol-state concentration from five distinct locations via filter samples. The water-extracted filter samples were analyzed by LC-MS. Lactic acid sulfate and glycolic acid sulfate were detected in urban locations in the United States, Mexico City, and Pakistan with varied concentrations, indicating their potential as tracers. We studied the aqueous processing reaction between glyoxal and nitrogen-containing species such as ammonium and amines exclusively by NMR spectrometry. The reaction products formic acid and several imidazoles along with the quantified kinetics were reported. The brown carbon generated from these reactions were quantified optically by UV-Vis spectroscopy. The organic-phase reaction between oxygen molecule and alkenes photosensitized by alpha-dicarbonyls were studied in the same manner. We observed the fast kinetics transferring alkenes to epoxides under simulated sunlight. Statistical estimations indicate a very effective conversion of aerosol-phase alkenes to epoxides, potentially forming organosulfates in a deliquescence event and

  6. Sulfate aerosols and polar stratospheric cloud formation

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

    Tolbert, M.A.

    Before the discovery of the Antarctic ozone hole, it was generally assumed that gas-phase chemical reactions controlled the abundance of stratospheric ozone. However, the massive springtime ozone losses over Antarctica first reported by Farman et al in 1985 could not be explained on the basis of gas-phase chemistry alone. In 1986, Solomon et al suggested that chemical reactions occurring on the surfaces of polar stratospheric clouds (PSCs) could be important for the observed ozone losses. Since that time, an explosion of laboratory, field, and theoretical research in heterogeneous atmospheric chemistry has occurred. Recent work has indicated that the most importantmore » heterogeneous reaction on PSCs is ClONO[sub 2] + HCl [yields] Cl[sub 2] + HNO[sub 3]. This reaction converts inert chlorine into photochemically active Cl[sub 2]. Photolysis of Cl[sub 2] then leads to chlorine radicals capable of destroying ozone through very efficient catalytic chain reactions. New observations during the second Airborne Arctic Stratospheric Expedition found stoichiometric loss of ClONO[sub 2] and HCl in air processed by PSCs in accordance with reaction 1. Attention is turning toward understanding what kinds of aerosols form in the stratospheric, their formation mechanism, surface area, and specific chemical reactivity. Some of the latest findings, which underline the importance of aerosols, were presented at a recent National Aeronautics and Space Administration workshop in Boulder, Colorado.« less

  7. Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming

    NASA Technical Reports Server (NTRS)

    Hofmann, David J.

    1993-01-01

    The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.

  8. Reactive intermediates revealed in secondary organic aerosol formation from isoprene

    PubMed Central

    Surratt, Jason D.; Chan, Arthur W. H.; Eddingsaas, Nathan C.; Chan, ManNin; Loza, Christine L.; Kwan, Alan J.; Hersey, Scott P.; Flagan, Richard C.; Wennberg, Paul O.; Seinfeld, John H.

    2010-01-01

    Isoprene is a significant source of atmospheric organic aerosol; however, the oxidation pathways that lead to secondary organic aerosol (SOA) have remained elusive. Here, we identify the role of two key reactive intermediates, epoxydiols of isoprene (IEPOX = β-IEPOX + δ-IEPOX) and methacryloylperoxynitrate (MPAN), which are formed during isoprene oxidation under low- and high-NOx conditions, respectively. Isoprene low-NOx SOA is enhanced in the presence of acidified sulfate seed aerosol (mass yield 28.6%) over that in the presence of neutral aerosol (mass yield 1.3%). Increased uptake of IEPOX by acid-catalyzed particle-phase reactions is shown to explain this enhancement. Under high-NOx conditions, isoprene SOA formation occurs through oxidation of its second-generation product, MPAN. The similarity of the composition of SOA formed from the photooxidation of MPAN to that formed from isoprene and methacrolein demonstrates the role of MPAN in the formation of isoprene high-NOx SOA. Reactions of IEPOX and MPAN in the presence of anthropogenic pollutants (i.e., acidic aerosol produced from the oxidation of SO2 and NO2, respectively) could be a substantial source of “missing urban SOA” not included in current atmospheric models. PMID:20080572

  9. Sulfates on Mars: TES Observations and Thermal Inertia Data

    NASA Astrophysics Data System (ADS)

    Cooper, C. D.; Mustard, J. F.

    2001-05-01

    The high resolution thermal emission spectra returned by the TES spectrometer on the MGS spacecraft have allowed the mapping of a variety of minerals and rock types by different sets of researchers. Recently, we have used a linear deconvolution approach to compare sulfate-palagonite soil mixtures created in the laboratory with Martian surface spectra. This approach showed that a number of areas on Mars have spectral properties that match those of sulfate-cemented soils (but neither loose powder mixtures of sulfates and soils nor sand-sized grains of disaggregated crusted soils). These features do not appear to be caused by atmospheric or instrumental effects and are thus believed to be related to surface composition and texture. The distribution and physical state of sulfate are important pieces of information for interpreting surface processes on Mars. A number of different mechanisms could have deposited sulfate in surface layers. Some of these include evaporation of standing bodies of water, aerosol deposition of volcanic gases, hydrothermal alteration from groundwater, and in situ interaction between the atmosphere and soil. The areas on Mars with cemented sulfate signatures are spread across a wide range of elevations and are generally large in spatial scale. Some of the areas are associated with volcanic regions, but many are in dark red plains that have previously been interpreted as duricrust deposits. Our current work compares the distribution of sulfate-cemented soils as mapped by the spectral deconvolution approach with thermal inertia maps produced from both Viking and MGS-TES. Duricrust regions, interpreted from intermediate thermal inertia values, are large regions thought to be sulfate-cemented soils similar to coherent, sulfate-rich materials seen at the Viking lander sites. Our observations of apparent regions of cemented sulfate are also large in spatial extent. This scale information is important for evaluating formation mechanisms for the

  10. Characteristics of aerosol acidity in Hong Kong

    NASA Astrophysics Data System (ADS)

    Pathak, Ravi Kant; Louie, Peter K. K.; Chan, Chak K.

    The ammonium-to-sulfate ratio ([NH 4+]/[SO 42-]) and the strong acidity have been generally used as parameters to describe the acidic nature of atmospheric aerosols. However, both parameters do not provide the in situ acidic characteristics of atmospheric aerosols, which are more relevant to the reactivity and the environmental impacts of the aerosols. In this study, the in situ free acid concentrations and the in situ pH of aerosols are investigated to understand the acidic characteristics of atmospheric aerosols in Hong Kong (HK). Over 182 datasets on 24 h Respirable Suspended Particles (RSP) samples collected in 2001 from seven air-quality-monitoring sites run by the Hong Kong Environmental Protection Department are analyzed. Simulations using the Aerosol Inorganic Model (AIM2) reveal that the in situ acidity, i.e., the free acid concentration ([H +] free), is only a minor fraction (˜23%) of the estimated strong acidity in the fine particles because of the presence of bisulfate ions. The acidity characteristics of fine particles are a function of mainly RH and ammonium to sulfate ratio. The in situ free acid concentration, the normalized water content ([H 2O] AIM2/[SO 42-]), and the dissociation of bisulfate to free acid in the aerosols decrease as the [NH 4+]/[SO 42-] ratio increases and the Relative Humidity (RH) decreases. The acidic fine mode particles have average molar [NH 4+]/[SO 42-] ratio of 1.42, strong acidity of 51 nmol m -3, in situ acidity of 11 nmol m -3, and in situ pH of 0.25 on average. Our findings suggest that even the more neutralized ([NH 4+]/[SO 42-] >1.5) particles, such as those found when HK is under the influence of continental air masses from the Chinese mainland, can have high in situ acidity and low pH when the RH is low. This study calls for more investigation of the acidity of aerosols in HK, incorporating the concepts of in situ acidity and pH.

  11. Elements including metals in the atomizer and aerosol of disposable electronic cigarettes and electronic hookahs.

    PubMed

    Williams, Monique; Bozhilov, Krassimir; Ghai, Sanjay; Talbot, Prue

    2017-01-01

    Our purpose was to quantify 36 inorganic chemical elements in aerosols from disposable electronic cigarettes (ECs) and electronic hookahs (EHs), examine the effect of puffing topography on elements in aerosols, and identify the source of the elements. Thirty-six inorganic chemical elements and their concentrations in EC/EH aerosols were determined using inductively coupled plasma optical emission spectroscopy, and their source was identified by analyzing disassembled atomizers using scanning electron microscopy and energy dispersive X-ray spectroscopy. Of 36 elements screened, 35 were detected in EC/EH aerosols, while only 15 were detected in conventional tobacco smoke. Some elements/metals were present in significantly higher concentrations in EC/EH aerosol than in cigarette smoke. Concentrations of particular elements/metals within EC/EH brands were sometimes variable. Aerosols generated at low and high air-flow rates produced the same pattern of elements, although the total element concentration decreased at the higher air flow rate. The relative amount of elements in the first and last 60 puffs was generally different. Silicon was the dominant element in aerosols from all EC/EH brands and in cigarette smoke. The elements appeared to come from the filament (nickel, chromium), thick wire (copper coated with silver), brass clamp (copper, zinc), solder joints (tin, lead), and wick and sheath (silicon, oxygen, calcium, magnesium, aluminum). Lead was identified in the solder and aerosol of two brands of EHs (up to 0.165 μg/10 puffs). These data show that EC/EH aerosols contain a mixture of elements, including heavy metals, with concentrations often significantly higher than in conventional cigarette smoke. While the health effects of inhaling mixtures of heated metals is currently not known, these data will be valuable in future risk assessments involving EC/EH elements/metals.

  12. Elements including metals in the atomizer and aerosol of disposable electronic cigarettes and electronic hookahs

    PubMed Central

    Williams, Monique; Bozhilov, Krassimir; Ghai, Sanjay; Talbot, Prue

    2017-01-01

    Objective Our purpose was to quantify 36 inorganic chemical elements in aerosols from disposable electronic cigarettes (ECs) and electronic hookahs (EHs), examine the effect of puffing topography on elements in aerosols, and identify the source of the elements. Methods Thirty-six inorganic chemical elements and their concentrations in EC/EH aerosols were determined using inductively coupled plasma optical emission spectroscopy, and their source was identified by analyzing disassembled atomizers using scanning electron microscopy and energy dispersive X-ray spectroscopy. Results Of 36 elements screened, 35 were detected in EC/EH aerosols, while only 15 were detected in conventional tobacco smoke. Some elements/metals were present in significantly higher concentrations in EC/EH aerosol than in cigarette smoke. Concentrations of particular elements/metals within EC/EH brands were sometimes variable. Aerosols generated at low and high air-flow rates produced the same pattern of elements, although the total element concentration decreased at the higher air flow rate. The relative amount of elements in the first and last 60 puffs was generally different. Silicon was the dominant element in aerosols from all EC/EH brands and in cigarette smoke. The elements appeared to come from the filament (nickel, chromium), thick wire (copper coated with silver), brass clamp (copper, zinc), solder joints (tin, lead), and wick and sheath (silicon, oxygen, calcium, magnesium, aluminum). Lead was identified in the solder and aerosol of two brands of EHs (up to 0.165 μg/10 puffs). Conclusion These data show that EC/EH aerosols contain a mixture of elements, including heavy metals, with concentrations often significantly higher than in conventional cigarette smoke. While the health effects of inhaling mixtures of heated metals is currently not known, these data will be valuable in future risk assessments involving EC/EH elements/metals. PMID:28414730

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  14. Characteristics of aerosol pollution during heavy haze events in Suzhou, China

    NASA Astrophysics Data System (ADS)

    Tian, M.; Wang, H. B.; Chen, Y.; Yang, F. M.; Zhang, X. H.; Zou, Q.; Zhang, R. Q.; Ma, Y. L.; He, K. B.

    2015-11-01

    A comprehensive measurement was carried out to analyze the heavy haze events in Suzhou in January 2013 when extremely severe haze pollution occurred in many cities in China especially in the East. Hourly concentrations of PM2.5, chemical composition (including water-soluble inorganic ions, OC, and EC), and gas-phase precursors were obtained via on-line monitoring system. Based on these data, detailed aerosol composition, light extinction and gas-phase precursors were analyzed to understand the characteristics of the haze events, moreover, the formation mechanism of nitrate and sulfate in PM2.5 and the regional sources deduced from trajectory and PSCF were discussed to explore the origin of the heavy aerosol pollution. The results showed that frequent haze events were occurred on January 2013 and the concentrations of PM2.5 often exceeded 150 μg m-3 during the haze occurrence, with a maximum concentration of 324 μg m-3 on 14 January 2013. Unfavorable weather conditions (high RH, and low rainfall, wind speed and atmospheric pressure), high concentration of secondary aerosol species (including SO42-, NO3-, NH4+, and SOC) and precursors were observed during the haze events. Additionally, OM, (NH4)2SO4, NH4NO3 were demonstrated to be the major contributors to the visibility impairment but the share differed from haze events. This study also found that the high concentration of sulfate might be explained by the heterogeneous reactions in the aqueous surface layer of pre-existing particles or in cloud processes while nitrate might be mainly formed through homogeneous gas-phase reactions. The results of trajectory clustering and the PSCF method manifested that aerosol pollutions in the studied areas were mainly affected by local activities and surrounding sources transported from nearby cities.

  15. Comparative thermodynamic studies of aqueous glutaric acid, ammonium sulfate and sodium chloride aerosol at high humidity.

    PubMed

    Hanford, Kate L; Mitchem, Laura; Reid, Jonathan P; Clegg, Simon L; Topping, David O; McFiggans, Gordon B

    2008-10-02

    Aerosol optical tweezers are used to simultaneously characterize and compare the hygroscopic properties of two aerosol droplets, one containing inorganic and organic solutes and the second, referred to as the control droplet, containing a single inorganic salt. The inorganic solute is either sodium chloride or ammonium sulfate and the organic component is glutaric acid. The time variation in the size of each droplet (3-7 microm in radius) is recorded with 1 s time resolution and with nanometre accuracy. The size of the control droplet is used to estimate the relative humidity with an accuracy of better than +/-0.09%. Thus, the Kohler curve of the multicomponent inorganic/organic droplet, which characterizes the variation in equilibrium droplet size with relative humidity, can be determined directly. The measurements presented here focus on high relative humidities, above 97%, in the limit of dilute solutes. The experimental data are compared with theoretical treatments that, while ignoring the interactions between the inorganic and organic components, are based upon accurate representations of the activity-concentration relationships of aqueous solutions of the individual salts. The organic component is treated by a parametrized fit to experimental data or by the UNIFAC model and the water activity of the equilibrium solution droplet is calculated using the approach suggested by Clegg, Seinfeld and Brimblecombe or the Zdanovskii-Stokes-Robinson approximation. It is shown that such an experimental strategy, comparing directly droplets of different composition, enables highly accurate measurements of the hygroscopic properties, allowing the theoretical treatments to be rigorously tested. Typical deviations of the experimental measurements from theoretical predictions are shown to be around 1% in equilibrium size, comparable to the variation between the theoretical frameworks considered.

  16. Online Simulations of Global Aerosol Distributions in the NASA GEOS-4 Model and Comparisons to Satellite and Ground-Based Aerosol Optical Depth

    NASA Technical Reports Server (NTRS)

    Colarco, Peter; daSilva, Arlindo; Chin, Mian; Diehl, Thomas

    2010-01-01

    We have implemented a module for tropospheric aerosols (GO CART) online in the NASA Goddard Earth Observing System version 4 model and simulated global aerosol distributions for the period 2000-2006. The new online system offers several advantages over the previous offline version, providing a platform for aerosol data assimilation, aerosol-chemistry-climate interaction studies, and short-range chemical weather forecasting and climate prediction. We introduce as well a methodology for sampling model output consistently with satellite aerosol optical thickness (AOT) retrievals to facilitate model-satellite comparison. Our results are similar to the offline GOCART model and to the models participating in the AeroCom intercomparison. The simulated AOT has similar seasonal and regional variability and magnitude to Aerosol Robotic Network (AERONET), Moderate Resolution Imaging Spectroradiometer, and Multiangle Imaging Spectroradiometer observations. The model AOT and Angstrom parameter are consistently low relative to AERONET in biomass-burning-dominated regions, where emissions appear to be underestimated, consistent with the results of the offline GOCART model. In contrast, the model AOT is biased high in sulfate-dominated regions of North America and Europe. Our model-satellite comparison methodology shows that diurnal variability in aerosol loading is unimportant compared to sampling the model where the satellite has cloud-free observations, particularly in sulfate-dominated regions. Simulated sea salt burden and optical thickness are high by a factor of 2-3 relative to other models, and agreement between model and satellite over-ocean AOT is improved by reducing the model sea salt burden by a factor of 2. The best agreement in both AOT magnitude and variability occurs immediately downwind of the Saharan dust plume.

  17. Global Studies of the Sulfur Cycle Including the Influence of DMS and Fossil Fuel Sulfur on Climate and Climate Change

    NASA Technical Reports Server (NTRS)

    Penner, Joyce E.

    1998-01-01

    The indirect effect of anthropogenic aerosols, wherein aerosol particles are thought to increase cloud droplet concentrations and cloud lifetime, is the most uncertain component of climate forcing over the past 100 years. Here, for the first time, we use a mechanistic treatment of droplet nucleation and a prognostic treatment of the number of cloud droplets to study the indirect aerosol effect from changes in carbonaceous and sulfate aerosols. Cloud droplet nucleation is parameterized as a function of total aerosol number concentration, updraft velocity and a shape parameter, which takes into account the mechanism, of sulfate aerosol formation, while cloud droplet number depends on the nucleation as well as on droplet sinks. Whereas previous treatments have predicted annual average indirect effects between -1 and -2 W/sq m, we obtain an indirect aerosol effect between -0.14 W/sq m and -0.42 W/sq m in the global mean.

  18. Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

    NASA Technical Reports Server (NTRS)

    Sheridan, Patrick J.

    1999-01-01

    Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  20. Sulfate and Pb-210 Simulated in a Global Model Using Assimilated Meteorological Fields

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Rood, Richard; Lin, S.-J.; Jacob, Daniel; Muller, Jean-Francois

    1999-01-01

    This report presents the results of distributions of tropospheric sulfate, Pb-210 and their precursors from a global 3-D model. This model is driven by assimilated meteorological fields generated by the Goddard Data Assimilation Office. Model results are compared with observations from surface sites and from multiplatform field campaigns of Pacific Exploratory Missions (PEM) and Advanced Composition Explorer (ACE). The model generally captures the seasonal variation of sulfate at the surface sites, and reproduces well the short-term in-situ observations. We will discuss the roles of various processes contributing to the sulfate levels in the troposphere, and the roles of sulfate aerosol in regional and global radiative forcing.

  1. Identification of secondary aerosol precursors emitted by an aircraft turbofan

    NASA Astrophysics Data System (ADS)

    Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

    2018-05-01

    Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

  2. Study of the chemical composition of atmospheric aerosol particles in Hungary: a review

    NASA Astrophysics Data System (ADS)

    Mészáros, E.

    The methods used in Hungarian laboratories to study the chemical composition of atmospheric aerosol particles over the last 30 years are reviewed. Individual particles were identified by topochemical techniques and morphological identification with an electron microscope. Bulk analyses were also carried out by applying wet chemical methods, and more recently by the PIXE procedure. The results gained are summarized in connection with the general development of atmospheric aerosol science during the last decades. These studies demonstrated that cloud condensation nuclei are water soluble Aitken sized particles which are composed of sulfates. Neutralized and acidic sulfate particles constitute the main class of fine aerosol particles under continental and oceanic background conditions. Coarse particles contain mostly sodium, silicon and aluminium. The formation and origin of particles in different size ranges are also discussed.

  3. Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model

    NASA Astrophysics Data System (ADS)

    Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.; Ridley, D. A.; Manktelow, P. T.; Chipperfield, M. P.; Pickering, S. J.; Johnson, C. E.

    2010-10-01

    A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.

  4. Dry deposition of sulfate to Quercus rubra and Liriodendron tulipifera foliage

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

    Vandenberg, J.J.

    1987-01-01

    Estimates were made of the rate of dry deposition to red oak (Quercus rubra) and tulip poplar (Liriodendron tulipifera) foliage. In the laboratory, radioactive ammonium sulfate aerosols were generated in an exposure chamber. These aerosols were dry deposited onto leaves that were sequentially washed to examine the efficacy of washing procedures in removal of surface deposits. Over 90% of dry deposited sulfate was removed after a 30 second wash duration. Laboratory procedures also estimated the magnitude of foliar sulfur that leached into leaf wash solutions. The majority of laboratory leaves demonstrated no leaching of sulfur from the internal pool. However,more » some leaves showed significant sulfur leaching. It was concluded that leaching of internal sulfur was highly leaf specific. This indicated that each leaf used in field experiments needed to be individually examined for leaching.« less

  5. Role of sucrose in the heterogeneous uptake of dimethylamine by ammonium sulfate aerosol particles

    NASA Astrophysics Data System (ADS)

    Chu, Y.; Chan, C. K.

    2016-12-01

    Alkyl amines are important alkaline gases besides ammonia in the atmosphere and widely detected in both gas and particle phases. Heterogeneous uptake by pre-existing particles containing acids as well as ammonium salts is one of the major pathways of alkyl amines partitioning into aerosols. Recently, phase state of ammonium salt particles has been revealed to largely affect the degree of alkyl amines uptake. Using an electrodynamic balance coupled with Raman spectroscopy, we extend the study by investigating the alkyl amine uptake by ammonium sulfate (AS) - sucrose mixed particles, since ambient aerosols usually consist of a mixed phase of organics and inorganics. Sucrose is a surrogate of hydrophilic viscous organics that can alter the phase of AS at low relative humidity (RH) and dimethylamine (DMA) is selected for its abundance amongst alkyl amine compounds. DMA uptake occurred effectively at not only 70% RH but also RH as low as 10%, significantly below the AS crystallization point. The net uptake coefficient decreased as RH decreased for fixed initial AS - sucrose particle compositions. Interestingly, it followed a first increasing then decreasing trend as sucrose molar fraction increased from 0 to 0.5, at RH below 30%. Sucrose, albeit inert to DMA vapor, indirectly affected the interaction between DMA and AS - sucrose particles. On one hand, it absorbed water at low RH and delayed the efflorescence of AS to promote DMA uptake. On the other hand, the particle became more viscous with higher sucrose concentration and exhibited an effective mass transport barrier. Hence, the uptake of alkyl amines may occur slowly once ammonium salts are mixed with viscous organics, such as those secondary organic materials formed via the oxidation of biogenic volatile organic compounds, in the particle phase. Acknowledgment This work is supported by Research Grants Council (RGC) of Hong Kong Special Administrative Region, China (GRF 16300214). The grant from Hong Kong RGC Ph

  6. Biogenic influence on the composition and growth of summertime Arctic aerosol

    NASA Astrophysics Data System (ADS)

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

    2016-12-01

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

  7. File Specification for the MERRA Aerosol Reanalysis (MERRAero): MODIS AOD Assimilation based on a MERRA Replay

    NASA Technical Reports Server (NTRS)

    Da Silva, A. M.; Randles, C. A.; Buchard, V.; Darmenov, A.; Colarco, P. R.; Govindaraju, R.

    2015-01-01

    This document describes the gridded output files produced by the Goddard Earth Observing System version 5 (GEOS-5) Goddard Aerosol Assimilation System (GAAS) from July 2002 through December 2014. The MERRA Aerosol Reanalysis (MERRAero) is produced with the hydrostatic version of the GEOS-5 Atmospheric Global Climate Model (AGCM). In addition to standard meteorological parameters (wind, temperature, moisture, surface pressure), this simulation includes 15 aerosol tracers (dust, sea-salt, sulfate, black and organic carbon), ozone, carbon monoxide and carbon dioxide. This model simulation is driven by prescribed sea-surface temperature and sea-ice, daily volcanic and biomass burning emissions, as well as high-resolution inventories of anthropogenic emission sources. Meteorology is replayed from the MERRA Reanalysis.

  8. Development of an inorganic and organic aerosol model (CHIMERE 2017β v1.0): seasonal and spatial evaluation over Europe

    NASA Astrophysics Data System (ADS)

    Couvidat, Florian; Bessagnet, Bertrand; Garcia-Vivanco, Marta; Real, Elsa; Menut, Laurent; Colette, Augustin

    2018-01-01

    A new aerosol module was developed and integrated in the air quality model CHIMERE. Developments include the use of the Model of Emissions and Gases and Aerosols from Nature (MEGAN) 2.1 for biogenic emissions, the implementation of the inorganic thermodynamic model ISORROPIA 2.1, revision of wet deposition processes and of the algorithms of condensation/evaporation and coagulation and the implementation of the secondary organic aerosol (SOA) mechanism H2O and the thermodynamic model SOAP. Concentrations of particles over Europe were simulated by the model for the year 2013. Model concentrations were compared to the European Monitoring and Evaluation Programme (EMEP) observations and other observations available in the EBAS database to evaluate the performance of the model. Performances were determined for several components of particles (sea salt, sulfate, ammonium, nitrate, organic aerosol) with a seasonal and regional analysis of results. The model gives satisfactory performance in general. For sea salt, the model succeeds in reproducing the seasonal evolution of concentrations for western and central Europe. For sulfate, except for an overestimation of sulfate in northern Europe, modeled concentrations are close to observations and the model succeeds in reproducing the seasonal evolution of concentrations. For organic aerosol, the model reproduces with satisfactory results concentrations for stations with strong modeled biogenic SOA concentrations. However, the model strongly overestimates ammonium nitrate concentrations during late autumn (possibly due to problems in the temporal evolution of emissions) and strongly underestimates summer organic aerosol concentrations over most of the stations (especially in the northern half of Europe). This underestimation could be due to a lack of anthropogenic SOA or biogenic emissions in northern Europe. A list of recommended tests and developments to improve the model is also given.

  9. Salting Constants of Small Organic Molecules in Aerosol-Relevant Salts and Application to Aerosol Formation in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Waxman, E.; Carlton, A. M. G.; Ziemann, P. J.; Volkamer, R. M.

    2014-12-01

    Secondary organic aerosol (SOA) formation from small water-soluble molecules such as glyoxal and methyl glyoxal is a topic of emerging interest. Results from recent field campaigns, e.g. Waxman et al. (2013, GRL) and Knote et al. (2014, ACP), show that these molecules can form significant SOA mass as a result of 'salting-in'. Salting-in happens when a molecule's solubility increases with salt concentration and salting-out is the reverse. Salting effects modify the solubility exponentially with increasing salt concentration, and thus the effective Henry's law constant can strongly modify partitioning, and multiphase chemical reaction rates in aerosol water. Moreover, the solubility in aerosol water cannot easily inferred based on the solubility in cloud water, as the salting effects could change the solubility by a factor of 104 or more. In this work, we have devised and applied a novel experimental setup to measure salting constants using an ion trap mass spectrometer. We focus on small, water soluble molecules like methyl glyoxal and similar compounds and measure salting constants for aerosol-relevant salts including ammonium sulfate, ammonium nitrate, and sodium chloride. The Setschenow salting-constant values are then used to parameterize the effects of salting in CMAQ. We present a series of sensitivity studies of the effects that inorganic aerosols have on the SOA formation from small soluble molecules in the southeastern United States.

  10. Photochemical aging of light-absorbing secondary organic aerosol material.

    PubMed

    Sareen, Neha; Moussa, Samar G; McNeill, V Faye

    2013-04-11

    Dark reactions of methylglyoxal with NH4(+) in aqueous aerosols yield light-absorbing and surface-active products that can influence the physical properties of the particles. Little is known about how the product mixture and its optical properties will change due to photolysis as well as oxidative aging by O3 and OH in the atmosphere. Here, we report the results of kinetics and product studies of the photochemical aging of aerosols formed by atomizing aqueous solutions of methylglyoxal and ammonium sulfate. Experiments were performed using aerosol flow tube reactors coupled with an aerosol chemical ionization mass spectrometer (Aerosol-CIMS) for monitoring gas- and particle-phase compositions. Particles were also impacted onto quartz windows in order to assess changes in their UV-visible absorption upon oxidation. Photooxidation of the aerosols leads to the formation of small, volatile organic acids including formic acid, acetic acid, and glyoxylic acid. The atmospheric lifetime of these species during the daytime is predicted to be on the order of minutes, with photolysis being an important mechanism of degradation. The lifetime with respect to O3 oxidation was observed to be on the order of hours. O3 oxidation also leads to a net increase in light absorption by the particles due to the formation of additional carbonyl compounds. Our results are consistent with field observations of high brown carbon absorption in the early morning.

  11. Observing the Impact of Calbuco Volcanic Aerosols on South Polar Ozone Depletion in 2015

    NASA Astrophysics Data System (ADS)

    Stone, Kane A.; Solomon, Susan; Kinnison, Doug E.; Pitts, Michael C.; Poole, Lamont R.; Mills, Michael J.; Schmidt, Anja; Neely, Ryan R.; Ivy, Diane; Schwartz, Michael J.; Vernier, Jean-Paul; Johnson, Bryan J.; Tully, Matthew B.; Klekociuk, Andrew R.; König-Langlo, Gert; Hagiya, Satoshi

    2017-11-01

    The Southern Hemisphere Antarctic stratosphere experienced two noteworthy events in 2015: a significant injection of sulfur from the Calbuco volcanic eruption in Chile in April and a record-large Antarctic ozone hole in October and November. Here we quantify Calbuco's influence on stratospheric ozone depletion in austral spring 2015 using observations and an Earth system model. We analyze ozonesondes, as well as data from the Microwave Limb Sounder. We employ the Community Earth System Model, version 1, with the Whole Atmosphere Community Climate Model (WACCM) in a specified dynamics setup, which includes calculations of volcanic effects. The Cloud-Aerosol Lidar with Orthogonal Polarization data indicate enhanced volcanic liquid sulfate 532 nm backscatter values as far poleward as 68°S during October and November (in broad agreement with WACCM). Comparison of the location of the enhanced aerosols to ozone data supports the view that aerosols played a major role in increasing the ozone hole size, especially at pressure levels between 150 and 100 hPa. Ozonesonde vertical ozone profiles from the sites of Syowa, South Pole, and Neumayer display the lowest individual October or November measurements at 150 hPa since the 1991 Mount Pinatubo eruption period, with Davis showing similarly low values, but no available 1990 data. The analysis suggests that under the cold conditions ideal for ozone depletion, stratospheric volcanic aerosol particles from the moderate-magnitude eruption of Calbuco in 2015 greatly enhanced austral ozone depletion, particularly at 55-68°S, where liquid binary sulfate aerosols have a large influence on ozone concentrations.

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

    NASA Technical Reports Server (NTRS)

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

    2001-01-01

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

  13. 21 CFR 700.14 - Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products.

    Code of Federal Regulations, 2011 CFR

    2011-04-01

    ... propellant of cosmetic aerosol products. 700.14 Section 700.14 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES (CONTINUED) COSMETICS GENERAL Requirements for Specific Cosmetic Products § 700.14 Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products...

  14. 21 CFR 700.14 - Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products.

    Code of Federal Regulations, 2013 CFR

    2013-04-01

    ... propellant of cosmetic aerosol products. 700.14 Section 700.14 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES (CONTINUED) COSMETICS GENERAL Requirements for Specific Cosmetic Products § 700.14 Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products...

  15. 21 CFR 700.14 - Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products.

    Code of Federal Regulations, 2012 CFR

    2012-04-01

    ... propellant of cosmetic aerosol products. 700.14 Section 700.14 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES (CONTINUED) COSMETICS GENERAL Requirements for Specific Cosmetic Products § 700.14 Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products...

  16. 21 CFR 700.14 - Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products.

    Code of Federal Regulations, 2014 CFR

    2014-04-01

    ... propellant of cosmetic aerosol products. 700.14 Section 700.14 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES (CONTINUED) COSMETICS GENERAL Requirements for Specific Cosmetic Products § 700.14 Use of vinyl chloride as an ingredient, including propellant of cosmetic aerosol products...

  17. Aqueous-Phase Mechanism for Secondary Organic Aerosol Formation from Isoprene: Application to the Southeast United States and Co-Benefit of SO2 Emission Controls

    NASA Technical Reports Server (NTRS)

    Marais, E. A.; Jacob, D. J.; Jimenez, J. L.; Campuzano-Jost, P.; Day, D. A.; Hu, W.; Krechmer, J.; Zhu, L.; Kim, P. S.; Miller, C. C.; hide

    2016-01-01

    Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA), but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (gamma) for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS) and ground-based (SOAS) observations over the Southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx = NO + NO2) over the Southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2) react significantly with both NO (high-NOx pathway) and HO2 (low-NOx pathway), leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA) and formaldehyde (a product of isoprene oxidation). Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58% of isoprene SOA) from the low-NOx pathway and glyoxal (28%) from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation), but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate 42 on aerosol acidity and volume). The US EPA projects 2013-2025 decreases in anthropogenic emissions of 34% for NOx (leading to 7

  18. Multiple sulfur-isotope signatures in Archean sulfates and their implications for the chemistry and dynamics of the early atmosphere

    PubMed Central

    Muller, Élodie; Philippot, Pascal; Rollion-Bard, Claire; Cartigny, Pierre

    2016-01-01

    Sulfur isotopic anomalies (∆33S and ∆36S) have been used to trace the redox evolution of the Precambrian atmosphere and to document the photochemistry and transport properties of the modern atmosphere. Recently, it was shown that modern sulfate aerosols formed in an oxidizing atmosphere can display important isotopic anomalies, thus questioning the significance of Archean sulfate deposits. Here, we performed in situ 4S-isotope measurements of 3.2- and 3.5-billion-year (Ga)-old sulfates. This in situ approach allows us to investigate the diversity of Archean sulfate texture and mineralogy with unprecedented resolution and from then on to deconvolute the ocean and atmosphere Archean sulfur cycle. A striking feature of our data is a bimodal distribution of δ34S values at ∼+5‰ and +9‰, which is matched by modern sulfate aerosols. The peak at +5‰ represents barite of different ages and host-rock lithology showing a wide range of ∆33S between −1.77‰ and +0.24‰. These barites are interpreted as primary volcanic emissions formed by SO2 photochemical processes with variable contribution of carbonyl sulfide (OCS) shielding in an evolving volcanic plume. The δ34S peak at +9‰ is associated with non–33S-anomalous barites displaying negative ∆36S values, which are best interpreted as volcanic sulfate aerosols formed from OCS photolysis. Our findings confirm the occurrence of a volcanic photochemical pathway specific to the early reduced atmosphere but identify variability within the Archean sulfate isotope record that suggests persistence throughout Earth history of photochemical reactions characteristic of the present-day stratosphere. PMID:27330111

  19. Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

    NASA Technical Reports Server (NTRS)

    da Silva, Arlindo

    2010-01-01

    A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

  20. Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols. Part 1; Aerosol Trends and Radiative Forcing

    NASA Technical Reports Server (NTRS)

    Leibensperger, E. M.; Mickley, L. J.; Jacob, D. J.; Chen, W.-T.; Seinfeld, J. H.; Nenes, A.; Adams, P. J.; Streets, D. G.; Kumar, N.; Rind, D.

    2012-01-01

    We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of -2.0Wm(exp-2 for direct forcing including contributions from sulfate (-2.0Wm-2), nitrate (-0.2Wm(exp-2), organic carbon (-0.2Wm(exp-2), and black carbon (+0.4Wm(exp-2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp-2) direct and 1.0Wm(exp-2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp-2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

  1. Oxidation of Gas-Phase SO2 on the Surfaces of Acidic Microdroplets: Implications for Sulfate and Sulfate Radical Anion Formation in the Atmospheric Liquid Phase.

    PubMed

    Hung, Hui-Ming; Hoffmann, Michael R

    2015-12-01

    The oxidation of SO2(g) on the interfacial layers of microdroplet surfaces was investigated using a spray-chamber reactor coupled to an electrospray ionization mass spectrometer. Four major ions, HSO3(-), SO3(•-), SO4(•-) and HSO4(-), were observed as the SO2(g)/N2(g) gas-mixture was passed through a suspended microdroplet flow, where the residence time in the dynamic reaction zone was limited to a few hundred microseconds. The relatively high signal intensities of SO3(•-), SO4(•-), and HSO4(-) compared to those of HSO3(-) as observed at pH < 3 without addition of oxidants other than oxygen suggests an efficient oxidation pathway via sulfite and sulfate radical anions on droplets possibly via the direct interfacial electron transfer from HSO3(-) to O2. The concentrations of HSO3(-) in the aqueous aerosol as a function of pH were controlled by the deprotonation of hydrated sulfur dioxide, SO2·H2O, which is also affected by the pH dependent uptake coefficient. When H2O2(g) was introduced into the spray chamber simultaneously with SO2(g), HSO3(-) is rapidly oxidized to form bisulfate in the pH range of 3 to 5. Conversion to sulfate was less at pH < 3 due to relatively low HSO3(-) concentration caused by the fast interfacial reactions. The rapid oxidation of SO2(g) on the acidic microdroplets was estimated as 1.5 × 10(6) [S(IV)] (M s(-1)) at pH ≤ 3. In the presence of acidic aerosols, this oxidation rate is approximately 2 orders of magnitude higher than the rate of oxidation with H2O2(g) at a typical atmospheric H2O2(g) concentration of 1 ppb. This finding highlights the relative importance of the acidic surfaces for SO2 oxidation in the atmosphere. Surface chemical reactions on aquated aerosol surfaces, as observed in this study, are overlooked in most atmospheric chemistry models. These reaction pathways may contribute to the rapid production of sulfate aerosols that is often observed in regions impacted by acidic haze aerosol such as Beijing and other

  2. Linking Remotely Sensed Aerosol Types to Their Chemical Composition

    NASA Technical Reports Server (NTRS)

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

    2016-01-01

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

  3. Linking remotely sensed aerosol types to their chemical composition

    NASA Astrophysics Data System (ADS)

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

    2016-12-01

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

  4. Correlation of plume opacity with particles and sulfates from boilers

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

    Lou, J.C.; Lee, M.; Chen, K.S.

    1997-07-01

    The effects of emission concentrations of particulate matters and sulfates on plume opacity are investigated by in situ measurements. The studies are conducted for three processes of two coal-fired plants and one oil-fired that are all equipped with electrostatic precipitators. Flue-gas sampling and analysis include the concentrations of particles and total water soluble sulfates, particle size distribution, and flue-gas composition; while in-stack and out-of-stack opacities are determined by a transmissometer and certified smoke inspectors, respectively. Experimental results show that plume opacity outside the stack linearly correlates well with the in-stack opacity. The mixing of hot flue gas with cold ambientmore » air would result in the condensation of hygroscopic sulfuric acid aerosols and an increase about 1.6% out of typical 15--25% measured opacity. An empirical equation similar to the Beer-Lambert-Bouger form is derived for predicting the plume opacity in terms of the stack diameter and the concentrations of particles and total water soluble sulfates. Good comparisons are achieved between predictions by the empirical equation and other available field data.« less

  5. Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

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

    Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen

    Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the ‘climate sensitivity’). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through a combinationmore » of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic

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

    NASA Technical Reports Server (NTRS)

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

    1994-01-01

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

  7. Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

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

    Saide, Pablo; Spak, S. N.; Carmichael, Gregory

    2012-03-30

    We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign averaged longitudinal gradients, and highlight differences in model simulations with (W) and without wet (NW) deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptualmore » model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, including the reliability required for policy analysis and geo-engineering applications.« less

  8. Assessment of Aerosol Distributions from GEOS-5 Using the CALIPSO Feature Mask

    NASA Technical Reports Server (NTRS)

    Welton, Ellsworth

    2010-01-01

    A-train sensors such as MODIS, MISR, and CALIPSO are used to determine aerosol properties, and in the process a means of estimating aerosol type (e.g. smoke vs. dust). Correct classification of aerosol type is important for climate assessment, air quality applications, and for comparisons and analysis with aerosol transport models. The Aerosols-Clouds-Ecosystems (ACE) satellite mission proposed in the NRC Decadal Survey describes a next generation aerosol and cloud suite similar to the current A-train, including a lidar. The future ACE lidar must be able to determine aerosol type effectively in conjunction with modeling activities to achieve ACE objectives. Here we examine the current capabilities of CALIPSO and the NASA Goddard Earth Observing System general circulation model and data assimilation system (GEOS-5), to place future ACE needs in context. The CALIPSO level 2 feature mask includes vertical profiles of aerosol layers classified by type. GEOS-5 provides global 3D aerosol mass for sulfate, sea salt, dust, and black and organic carbon. A GEOS aerosol scene classification algorithm has been developed to provide estimates of aerosol mixtures and extinction profiles along the CALIPSO orbit track. In previous work, initial comparisons between GEOS-5 derived aerosol mixtures and CALIPSO derived aerosol types were presented for July 2007. In general, the results showed that model and lidar derived aerosol types did not agree well in the boundary layer. Agreement was poor over Europe, where CALIPSO indicated the presence of dust and pollution mixtures yet GEOS-5 was dominated by pollution with little dust. Over the ocean in the tropics, the model appeared to contain less sea salt than detected by CALIPSO, yet at high latitudes the situation was reserved. Agreement between CALIPSO and GEOS-5, aerosol types improved above the boundary layer, primarily in dust and smoke dominated regions. At higher altitudes (> 5 km), the model contained aerosol layers not detected

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

    DTIC Science & Technology

    2009-10-14

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

  10. Optical extinction of highly porous aerosol following atmospheric freeze drying

    NASA Astrophysics Data System (ADS)

    Adler, Gabriela; Haspel, Carynelisa; Moise, Tamar; Rudich, Yinon

    2014-06-01

    Porous glassy particles are a potentially significant but unexplored component of atmospheric aerosol that can form by aerosol processing through the ice phase of high convective clouds. The optical properties of porous glassy aerosols formed from a freeze-dry cycle simulating freezing and sublimation of ice particles were measured using a cavity ring down aerosol spectrometer (CRD-AS) at 532 nm and 355 nm wavelength. The measured extinction efficiency was significantly reduced for porous organic and mixed organic-ammonium sulfate particles as compared to the extinction efficiency of the homogeneous aerosol of the same composition prior to the freeze-drying process. A number of theoretical approaches for modeling the optical extinction of porous aerosols were explored. These include effective medium approximations, extended effective medium approximations, multilayer concentric sphere models, Rayleigh-Debye-Gans theory, and the discrete dipole approximation. Though such approaches are commonly used to describe porous particles in astrophysical and atmospheric contexts, in the current study, these approaches predicted an even lower extinction than the measured one. Rather, the best representation of the measured extinction was obtained with an effective refractive index retrieved from a fit to Mie scattering theory assuming spherical particles with a fixed void content. The single-scattering albedo of the porous glassy aerosols was derived using this effective refractive index and was found to be lower than that of the corresponding homogeneous aerosol, indicating stronger relative absorption at the wavelengths measured. The reduced extinction and increased absorption may be of significance in assessing direct, indirect, and semidirect forcing in regions where porous aerosols are expected to be prevalent.

  11. IMPACT OF AEROSOL LIQUID WATER ON SECONDARY ORGANIC AEROSOL YIELDS OF IRRADIATED TOLUENE/PROPYLENE/NOX/(NH4)2SO4/AIR MIXUTRES

    EPA Science Inventory

    Laboratory experiments were conducted to assess whether the presence of liquid water on pre-existing submicron ammonium sulfate aerosols affects yields of condensible organic compounds. Toluene/propylene/NOX/air mixtures were irradiated in the presence of submicron ammonium su...

  12. Removal of sulfur dioxide and formation of sulfate aerosol in Tokyo

    NASA Astrophysics Data System (ADS)

    Miyakawa, T.; Takegawa, N.; Kondo, Y.

    2007-07-01

    Ground-based in situ measurements of sulfur dioxide (SO2) and submicron sulfate aerosol (SO42-) together with carbon monoxide (CO) were conducted at an urban site in Tokyo, Japan from spring 2003 to winter 2004. The observed concentrations of SO2 were affected dominantly by anthropogenic emissions (for example, manufacturing industries) in source areas, while small fraction of the data (<30%) was affected by large point sources of SO2 (power plant and volcano). Although emission sources of CO in Tokyo are different from those of SO2, the major emission sources of CO and SO2 are colocated, indicating that CO can be used as a tracer of anthropogenic SO2 emissions in Tokyo. The ratio of SO42- to total sulfur compounds (SOx = SO2 + SO42-) and the remaining fraction of SOx, which is derived as the ratio of the linear regression slope of the SOx-CO correlation, is used as measures for the formation of SO42- and removal of SOx, respectively. Using these parameters, the average formation efficiency of SO42- (i.e., amount of SO42- produced per SO2 emitted from emission sources) are estimated to be 0.18 and 0.03 in the summer and winter periods, respectively. A simple box model was developed to estimate the lifetime of SOx. The lifetime of SOx for the summer period (26 h) is estimated to be about two times longer than that for the winter period (14 h). The seasonal variations of the remaining fraction of SOx, estimated formation efficiency of SO42-, and lifetime of SOx are likely due to those of the boundary layer height and photochemical activity (i.e., hydroxyl radical). These results provide useful insights into the formation and removal processes of sulfur compounds exported from an urban area.

  13. Chemical composition of atmospheric aerosols resolved via positive matrix factorization

    NASA Astrophysics Data System (ADS)

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

    2017-04-01

    secondary aerosols via atmospheric physicochemical processes (e.g. condensation and evaporation of gases) and on the other hand the potential non-linear summation (Spracklen et al., 2011 2011) of anthropogenic and biogenic aerosol emissions. From the perspective of statistical analysis there is no definite reason why inorganics could not be included, as long as their uncertainties are estimated correctly and their influence is properly weighted in the factor model. For result validation, external, additional information available from most measurement sites, such as correlations with trace gas concentrations or size distribution derived, mode-specific mass loadings can be used instead of AMS inorganics. In recent analyses, nitrate compounds have already been added to PMF analyses and shown to interact with organic semi-volatile compounds (Hao et al., 2014). In this study we tested including all the default AMS chemical species, i.e. organics, sulfates, nitrates, ammonia and chlorides, in a PMF analysis, and present potential interpretations of the results with regard to aerosol sources and the chemical processes shaping the aerosol types. In addition to resolving organic-dominated aerosol classes, the results shed light on inorganic salt formation and may imply formation of organics salts. Canagaratna, M. et al. (2007). Mass Spectrom Rev., 26:185-222. Hao, L. et al. (2014). Atmos. Chem. Phys., 14, 13483-13495. Paatero, P. (1999). J Comput Graph Stat, 8: 854-888. Spracklen, D. et al (2011) Atmos. Chem. Phys., 11, 12109-12136.

  14. 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

  15. Upper tropospheric ice sensitivity to sulfate geoengineering

    NASA Astrophysics Data System (ADS)

    Visioni, Daniele; Pitari, Giovanni; Mancini, Eva

    2017-04-01

    In light of the Paris Agreement which aims to keep global warming under 2 °C in the next century and considering the emission scenarios produced by the IPCC for the same time span, it is likely that to remain below that threshold some kind of geoengineering technique will have to be deployed. Amongst the different methods, the injection of sulfur into the stratosphere has received much attention considering its effectiveness and affordability. Aside from the rather well established surface cooling sulfate geoengineering (SG) would produce, the investigation on possible side-effects of this method is still ongoing. For instance, some recent studies have investigated the effect SG would have on upper tropospheric cirrus clouds, expecially on the homogenous freezing mechanisms that produces the ice particles (Kuebbeler et al., 2012). The goal of the present study is to better understand the effect of thermal and dynamical anomalies caused by SG on the formation of ice crystals via homogeneous freezing by comparing a complete SG simulation with a RCP4.5 reference case and with a number of sensitivity studies where atmospheric temperature changes in the upper tropospheric region are specified in a schematic way as a function of the aerosol driven stratospheric warming and mid-lower tropospheric cooling. These changes in the temperature profile tend to increase atmospheric stabilization, thus decreasing updraft and with it the amount of water vapor available for homogeneous freezing in the upper troposphere. However, what still needs to be assessed is the interaction between this dynamical effect and the thermal effects of tropospheric cooling (which would increase ice nucleation rates) and stratospheric warming (which would probably extend to the uppermost troposphere via SG aerosol gravitational settling, thus reducing ice nucleation rates), in order to understand how they combine together. Changes in ice clouds coverage could be important for SG, because cirrus ice

  16. Broadband measurements of aerosol extinction in the ultraviolet spectral region

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  17. Broadband measurements of aerosol extinction in the ultraviolet spectral region

    NASA Astrophysics Data System (ADS)

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

    2013-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2017-02-01

    quality in Seoul during winter is influenced strongly by secondary aerosol formation, with sulfate, nitrate, ammonium, SV-OOA, and LV-OOA together accounting for 64 % of the PM1 mass during this study. However, aerosol sources and composition were found to be significantly different between clean and polluted periods. During stagnant periods with low wind speed (WS) and high relative humidity (RH), PM concentration was generally high (average ±1σ = 43.6 ± 12.4 µg m-3) with enhanced fractions of nitrate (27 %) and SV-OOA (8 %), which suggested a strong influence from local production of secondary aerosol. Low-PM loading periods (12.6 ± 7.1 µg m-3) tended to occur under higher-WS and lower-RH conditions and appeared to be more strongly influenced by regional air masses, as indicated by higher mass fractions of sulfate (12 %) and LV-OOA (20 %) in PM1. Overall, our results indicate that PM pollutants in urban Korea originate from complex emission sources and atmospheric processes and that their concentrations and composition are controlled by various factors, including meteorological conditions, local anthropogenic emissions, and upwind sources.

  19. A global modeling study on carbonaceous aerosol microphysical characteristics and radiative forcing

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

    2010-02-01

    Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Assuming that sulfates, nitrates and secondary organics form a coating around a black carbon core, rather than forming a uniformly mixed particle, changes the overall net aerosol radiative forcing from negative to positive. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Black carbon absorption is amplified by sulfate and nitrate coatings, but even more strongly by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative forcing when sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to climate benefits.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  1. Effect of nitrate and sulfate relative abundance in PM2.5 on liquid water content explored through half-hourly observations of inorganic soluble aerosols at a polluted receptor site

    NASA Astrophysics Data System (ADS)

    Xue, Jian; Griffith, Stephen M.; Yu, Xin; Lau, Alexis K. H.; Yu, Jian Zhen

    2014-12-01

    Liquid water content (LWC) is the amount of liquid water on aerosols. It contributes to visibility degradation, provides a surface for gas condensation, and acts as a medium for heterogeneous gas/particle reactions. In this study, 520 half-hourly measurements of ionic chemical composition in PM2.5 at a receptor site in Hong Kong are used to investigate the dependence of LWC on ionic chemical composition, particularly on the relative abundance of sulfate and nitrate. LWC was estimated using a thermodynamic model (AIM-III). Within this data set of PM2.5 ionic compositions, LWC was highly correlated with the multivariate combination of sulfate and nitrate concentrations and RH (R2 = 0.90). The empirical linear regression result indicates that LWC is more sensitive to nitrate mass than sulfate. During a nitrate episode, the highest LWC (80.6 ± 17.9 μg m-3) was observed and the level was 70% higher than that during a sulfate episode despite a similar ionic PM2.5 mass concentration. A series of sensitivity tests were conducted to study LWC change as a function of the relative nitrate and sulfate abundance, the trend of which is expected to shift to more nitrate in China as a result of SO2 reduction and increase in NOx emission. Starting from a base case that uses the average of measured PM2.5 ionic chemical composition (63% SO42-, 11% NO3-, 19% NH4+, and 7% other ions) and an ionic equivalence ratio, [NH4+]/(2[SO42-] + [NO3-]), set constant to 0.72, the results show LWC would increase by 204% at RH = 40% when 50% of the SO42- is replaced by NO3- mass concentration. This is largely due to inhibition of (NH4)3H(SO4)2 crystallization while PM2.5 ionic species persist in the aqueous phase. At RH = 90%, LWC would increase by 12% when 50% of the SO42- is replaced by NO3- mass concentration. The results of this study highlight the important implications to aerosol chemistry and visibility degradation associated with LWC as a result of a shift in PM2.5 ionic chemical

  2. Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

    NASA Astrophysics Data System (ADS)

    Schill, G. P.; Tolbert, M. A.

    2013-05-01

    Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescence, organic-sulfate particles are known to undergo another phase transition known as liquid-liquid phase separation. The ice nucleation properties of particles that have undergone liquid-liquid phase separation are unknown. Here, Raman microscopy coupled with an environmental cell was used to study the low temperature deliquescence, efflorescence, and liquid-liquid phase separation behavior of 2 : 1 mixtures of organic polyols (1,2,6-hexanetriol and 1 : 1 1,2,6-hexanetriol + 2,2,6,6-tetrakis(hydroxymethyl)cyclohexanol) and ammonium sulfate from 240-265 K. Further, the ice nucleation efficiency of these organic-sulfate systems after liquid-liquid phase separation and efflorescence was investigated from 210-235 K. Raman mapping and volume-geometry analysis indicate that these particles contain solid ammonium sulfate cores fully engulfed in organic shells. For the ice nucleation experiments, we find that if the organic coatings are liquid, water vapor diffuses through the shell and ice nucleates on the ammonium sulfate core. In this case, the coatings minimally affect the ice nucleation efficiency of ammonium sulfate. In contrast, if the coatings become semi-solid or glassy, ice instead nucleates on the organic shell. Consistent with recent findings that glasses can be efficient ice nuclei, the phase-separated particles are nearly as efficient at ice nucleation as pure crystalline ammonium sulfate.

  3. Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

    NASA Astrophysics Data System (ADS)

    Schill, G. P.; Tolbert, M. A.

    2012-12-01

    Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescence, organic-sulfate particles are known to undergo another phase transition known as liquid-liquid phase separation. The ice nucleation properties of particles that have undergone liquid-liquid phase separation are unknown. Here, Raman microscopy coupled with an environmental cell was used to study the low temperature deliquescence, efflorescence, and liquid-liquid phase separation behavior of 2:1 mixtures of organic polyols (1,2,6-hexanetriol, and 1:1 1,2,6-hexanetriol +2,2,6,6-tetrakis(hydroxymethyl)cycohexanol) and ammonium sulfate from 240-265 K. Further, the ice nucleation efficiency of these organic-sulfate systems after liquid-liquid phase separation and efflorescence was investigated from 210-235 K. Raman mapping and volume-geometry analysis indicates that these particles contain solid ammonium sulfate cores fully engulfed in organic shells. For the ice nucleation experiments, we find that if the organic coatings are liquid, water vapor diffuses through the shell and ice nucleates on the ammonium sulfate core. In this case, the coatings minimally affect the ice nucleation efficiency of ammonium sulfate. In contrast, if the coatings become semi-solid or glassy, ice instead nucleates on the organic shell. Consistent with recent findings that glasses can be efficient ice nuclei, the phase separated particles are nearly as efficient at ice nucleation as pure crystalline ammonium sulfate.

  4. Sulfur Geochemistry of a Lacustrine Record from Taiwan Reveals Enhanced Marine Aerosol Input during the Early Holocene

    PubMed Central

    Ding, Xiaodong; Li, Dawei; Zheng, Liwei; Bao, Hongyan; Chen, Huei-Fen; Kao, Shuh-Ji

    2016-01-01

    Lacustrine record of marine aerosol input has rarely been documented. Here, we present the sulfur geochemistry during the last deglaciation and early Holocene of a sediment core retrieved from the Dongyuan Lake in southern Taiwan. An unusually high sulfur peak accompanying pyrite presence is observed at 10.5 ka BP. Such high sulfur content in lacustrine record is unusual. The δ34S of sulfur varied from +9.5 to + 17.1‰ with two significant positive shifts at 10.5 and 9.4 ka BP. The sources of sulfur and potential processes involving the sulfur isotope variation including bacterial sulfate reduction, volcanic emissions, in-catchment sulfide oxidation and marine aerosol input are discussed. Enhanced marine aerosol input is the most likely explanation for such sulfur peaks and δ34S shifts. The positive δ34S shifts appeared concurrently with the maximum landslide events over Taiwan resulted from enhanced typhoon activities. The synchronicity among records suggests that increased typhoon activities promoted sea spray, and consequently enhanced the marine aerosol input with 34S-enriched sulfate. Our sulfur geochemistry data revealed sea spray history and marine influence onto terrestrial environment at coastal regions. Wider coverage of spatial-temporal lacustrine sulfur geochemistry record is needed to validate the applicability of sulfur proxy in paleoenvironmental research. PMID:27941864

  5. 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.

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

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

    Matsui, Hitoshi; Koike, Makoto; Kondo, Yutaka

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

  7. The Many Problems with Geoengineering Using Stratospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Robock, Alan

    2009-05-01

    In response to the global warming problem, there has been a recent renewed call for geoengineering ``solutions'' involving injecting particles into the stratosphere or blocking sunlight with satellites between the Sun and Earth. While volcanic eruptions have been suggested as innocuous examples of stratospheric aerosols cooling the planet, the volcano analog actually argues against geoengineering because of ozone depletion and regional hydrologic and temperature responses. In this talk, I consider the suggestion to create an artificial stratospheric aerosol layer. No systems to conduct geoengineering now exist, but a comparison of different proposed stratospheric injection schemes, airplanes, balloons, artillery, and a space elevator, shows that using airplanes would not be that expensive. We simulated the climate response to both tropical and Arctic stratospheric injection of sulfate aerosol precursors using a comprehensive atmosphere-ocean general circulation model, the National Aeronautics and Space Administration Goddard Institute for Space Studies ModelE. We simulated the injection of SO2 and the model converts it to sulfate aerosols, transports them and removes them through dry and wet deposition, and calculates the climate response to the radiative forcing from the aerosols. We conducted simulations of future climate with the Intergovernmental Panel on Climate Change A1B business-as-usual scenario both with and without geoengineering, and compare the results. We found that if there were a way to continuously inject SO2 into the lower stratosphere, it would produce global cooling. Acid deposition from the sulfate would not be enough to disturb most ecosystems. Tropical SO2 injection would produce sustained cooling over most of the world, with more cooling over continents. Arctic SO2 injection would not just cool the Arctic. But both tropical and Arctic SO2 injection would disrupt the Asian and African summer monsoons, reducing precipitation to the food supply

  8. Improving source identification of Atlanta aerosol using temperature resolved carbon fractions in positive matrix factorization

    NASA Astrophysics Data System (ADS)

    Kim, Eugene; Hopke, Philip K.; Edgerton, Eric S.

    Daily integrated PM 2.5 (particulate matter ⩽2.5 μm in aerodynamic diameter) composition data including eight individual carbon fractions collected at the Jefferson Street monitoring site in Atlanta were analyzed with positive matrix factorization (PMF). Particulate carbon was analyzed using the thermal optical reflectance method that divides carbon into four organic carbon (OC), pyrolized organic carbon (OP), and three elemental carbon (EC) fractions. A total of 529 samples and 28 variables were measured between August 1998 and August 2000. PMF identified 11 sources in this study: sulfate-rich secondary aerosol I (50%), on-road diesel emissions (11%), nitrate-rich secondary aerosol (9%), wood smoke (7%), gasoline vehicle (6%), sulfate-rich secondary aerosol II (6%), metal processing (3%), airborne soil (3%), railroad traffic (3%), cement kiln/carbon-rich (2%), and bus maintenance facility/highway traffic (2%). Differences from previous studies using only the traditional OC and EC data (J. Air Waste Manag. Assoc. 53(2003a)731; Atmos Environ. (2003b)) include four traffic-related combustion sources (gasoline vehicle, on-road diesel, railroad, and bus maintenance facility) containing carbon fractions whose abundances were different between the various sources. This study indicates that the temperature resolved fractional carbon data can be utilized to enhance source apportionment study, especially with respect to the separation of diesel emissions from gasoline vehicle sources. Conditional probability functions using surface wind data and identified source contributions aid the identifications of local point sources.

  9. Impact of North America on the aerosol composition in the North Atlantic free troposphere

    NASA Astrophysics Data System (ADS)

    García, M. Isabel; Rodríguez, Sergio; Alastuey, Andrés

    2017-06-01

    In the AEROATLAN project we study the composition of aerosols collected over ˜ 5 years at Izaña Observatory (located at ˜ 2400 m a.s.l. in Tenerife, the Canary Islands) under the prevailing westerly airflows typical of the North Atlantic free troposphere at subtropical latitudes and midlatitudes. Mass concentrations of sub-10 µm aerosols (PM10) carried by westerly winds to Izaña, after transatlantic transport, are typically within the range 1.2 and 4.2 µg m-3 (20th and 80th percentiles). The main contributors to background levels of aerosols (PM10 within the 1st-50th percentiles = 0.15-2.54 µg m-3) are North American dust (53 %), non-sea-salt sulfate (14 %) and organic matter (18 %). High PM10 events (75th-95th percentiles ≈ 4.0-9.0 µg m-3) are prompted by dust (56 %), organic matter (24 %) and non-sea-salt sulfate (9 %). These aerosol components experience a seasonal evolution explained by (i) their spatial distribution in North America and (ii) the seasonal shift of the North American outflow, which migrates from low latitudes in winter (˜ 32° N, January-March) to high latitudes in summer (˜ 52° N, August-September). The westerlies carry maximum loads of non-sea-salt sulfate, ammonium and organic matter in spring (March-May), of North American dust from midwinter to mid-spring (February-May) and of elemental carbon in summer (August-September). Our results suggest that a significant fraction of organic aerosols may be linked to sources other than combustion (e.g. biogenic); further studies are necessary for this topic. The present study suggests that long-term evolution of the aerosol composition in the North Atlantic free troposphere will be influenced by air quality policies and the use of soils (potential dust emitter) in North America.

  10. 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.

  11. Global Distribution of Dust, Smoke, Volcanic Ash, and Pollutant Aerosols Seen from Space

    NASA Technical Reports Server (NTRS)

    Herman, Jay R.; Hsu, Christina; Krotkov, Nickolay; Torres, Omar

    1998-01-01

    New technique for observing aerosols from space, using ultraviolet (UV) wavelengths, have been developed during the past three years. The chief benefit from observing aerosols in the UV is that they are easily visible over both land and water. While there is presently more than one satellite that can observe aerosols in the UV, only Total Ozone Mapping Spectrometer (TOMS) has a long-term record (since 1979) and adequate spatial resolutions (50 to 100 km) to observe the seasonal and interannual variations, and to locate some of the land sources of dust, smoke, volcanic ash and sulfate pollutants. The data has been assembled into daily images of the atmospheric aerosol loading in terms of optical depth and UV transmittance. For the major sources of aerosols, it is common for at least 50% of the total UV to be absorbed underneath aerosol plumes. This is particularly true for the spectacular smoke plumes originating from the recent Indonesian and Mexican fires, as well as under the huge African dust plumes. The sulfate pollutants are mostly present in the Northern Hemisphere and are associated with regions of high industrial activity. The location and seasonal dependence of these aerosol plumes over Europe and North America will be contrasted with the relatively clean Southern Hemisphere. Because of the success of this technique, it has formed the basis for a new generation of space-borne aerosol detection instruments. These new instruments combine the UV observations with the more traditional visible-wavelength data to obtain a more comprehensive characterization of aerosols that is possible with either UV or visible techniques by themselves.

  12. Nanoparticle agglomerates of fluticasone propionate in combination with albuterol sulfate as dry powder aerosols

    PubMed Central

    El-Gendy, Nashwa; Pornputtapitak, Warangkana; Berkland, Cory

    2015-01-01

    Particle engineering strategies remain at the forefront of aerosol research for localized treatment of lung diseases and represent an alternative for systemic drug therapy. With the hastily growing popularity and complexity of inhalation therapy, there is a rising demand for tailor-made inhalable drug particles capable of affording the most proficient delivery to the lungs and the most advantageous therapeutic outcomes. To address this formulation demand, nanoparticle agglomeration was used to develop aerosols of the asthma therapeutics, fluticasone or albuterol. In addition, a combination aerosol was formed by drying agglomerates of fluticasone nanoparticles in the presence of albuterol in solution. Powders of the single drug nanoparticle agglomerates or of the combined therapeutics possessed desirable aerodynamic properties for inhalation. Powders were efficiently aerosolized (~75% deposition determined by cascade impaction) with high fine particle fraction and rapid dissolution. Nanoparticle agglomeration offers a unique approach to obtain high performance aerosols from combinations of asthma therapeutics. PMID:21964203

  13. The single scattering properties of the aerosol particles as aggregated spheres

    NASA Astrophysics Data System (ADS)

    Wu, Y.; Gu, X.; Cheng, T.; Xie, D.; Yu, T.; Chen, H.; Guo, J.

    2012-08-01

    The light scattering and absorption properties of anthropogenic aerosol particles such as soot aggregates are complicated in the temporal and spatial distribution, which introduce uncertainty of radiative forcing on global climate change. In order to study the single scattering properties of anthorpogenic aerosol particles, the structures of these aerosols such as soot paticles and soot-containing mixtures with the sulfate or organic matter, are simulated using the parallel diffusion limited aggregation algorithm (DLA) based on the transmission electron microscope images (TEM). Then, the single scattering properties of randomly oriented aerosols, such as scattering matrix, single scattering albedo (SSA), and asymmetry parameter (AP), are computed using the superposition T-matrix method. The comparisons of the single scattering properties of these specific types of clusters with different morphological and chemical factors such as fractal parameters, aspect ratio, monomer radius, mixture mode and refractive index, indicate that these different impact factors can respectively generate the significant influences on the single scattering properties of these aerosols. The results show that aspect ratio of circumscribed shape has relatively small effect on single scattering properties, for both differences of SSA and AP are less than 0.1. However, mixture modes of soot clusters with larger sulfate particles have remarkably important effects on the scattering and absorption properties of aggregated spheres, and SSA of those soot-containing mixtures are increased in proportion to the ratio of larger weakly absorbing attachments. Therefore, these complex aerosols come from man made pollution cannot be neglected in the aerosol retrievals. The study of the single scattering properties on these kinds of aggregated spheres is important and helpful in remote sensing observations and atmospheric radiation balance computations.

  14. A TEST OF THERMODYNAMIC EQUILIBRIUM MODELS AND 3-D AIR QUALITY MODELS FOR PREDICTIONS OF AEROSOL NO3-

    EPA Science Inventory

    The inorganic species of sulfate, nitrate and ammonium constitute a major fraction of atmospheric aerosols. The behavior of nitrate is one of the most intriguing aspects of inorganic atmospheric aerosols because particulate nitrate concentrations depend not only on the amount of ...

  15. Toward Synchronous Evaluation of Source Apportionments for Atmospheric Concentration and Deposition of Sulfate Aerosol Over East Asia

    NASA Astrophysics Data System (ADS)

    Itahashi, S.

    2018-03-01

    Source apportionments for atmospheric concentration, dry deposition, and wet deposition of sulfate aerosol (SO42-) were synchronously evaluated over East Asia, a main source of anthropogenic sulfur dioxide (SO2) emissions. Estimating dry deposition was difficult owing to the difficulty of measuring deposition velocity directly; therefore, sensitivity simulations using two dry deposition schemes were conducted. Moreover, sensitivity simulations for different emission inventories, the largest uncertainty source in the air quality model, were also conducted. In total, four experimental settings were used. Model performance was verified for atmospheric concentration and wet deposition using a ground-based observation network in China, Korea, and Japan, and all four model settings captured the observations. The underestimation of wet deposition over China was improved by an adjusted approach that linearly scaled the modeled precipitation values to observations. The synchronous evaluation of source apportionments for atmospheric concentration and dry and wet deposition showed the dominant contribution of anthropogenic emissions from China to the atmospheric concentration and deposition in Japan. The contributions of emissions from volcanoes were more important for wet deposition than for atmospheric concentration. Differences in the dry deposition scheme and emission inventory did not substantially influence the relative ratio of source apportionments over Japan. Because the dry deposition was more attributed to local factors, the differences in dry deposition may be an important determinant of the source contributions from China to Japan. Verification of these findings, including the dry deposition velocity, is necessary for better understanding of the behavior of sulfur compound in East Asia.

  16. Year-round records of bulk and size-segregated aerosol composition in central Antarctica (Concordia site) - Part 1: Fractionation of sea-salt particles

    NASA Astrophysics Data System (ADS)

    Legrand, Michel; Preunkert, Susanne; Wolff, Eric; Weller, Rolf; Jourdain, Bruno; Wagenbach, Dietmar

    2017-11-01

    Multiple year-round records of bulk and size-segregated composition of aerosol were obtained at the inland site of Concordia located at Dome C in East Antarctica. In parallel, sampling of acidic gases on denuder tubes was carried out to quantify the concentrations of HCl and HNO3 present in the gas phase. These time series are used to examine aerosol present over central Antarctica in terms of chloride depletion relative to sodium with respect to freshly emitted sea-salt aerosol as well as depletion of sulfate relative to sodium with respect to the composition of seawater. A depletion of chloride relative to sodium is observed over most of the year, reaching a maximum of ˜ 20 ng m-3 in spring when there are still large sea-salt amounts and acidic components start to recover. The role of acidic sulfur aerosol and nitric acid in replacing chloride from sea-salt particles is here discussed. HCl is found to be around twice more abundant than the amount of chloride lost by sea-salt aerosol, suggesting that either HCl is more efficiently transported to Concordia than sea-salt aerosol or re-emission from the snow pack over the Antarctic plateau represents an additional significant HCl source. The size-segregated composition of aerosol collected in winter (from 2006 to 2011) indicates a mean sulfate to sodium ratio of sea-salt aerosol present over central Antarctica of 0.16 ± 0.05, suggesting that, on average, the sea-ice and open-ocean emissions equally contribute to sea-salt aerosol load of the inland Antarctic atmosphere. The temporal variability of the sulfate depletion relative to sodium was examined at the light of air mass backward trajectories, showing an overall decreasing trend of the ratio (i.e., a stronger sulfate depletion relative to sodium) when air masses arriving at Dome C had traveled a longer time over sea ice than over open ocean. The findings are shown to be useful to discuss sea-salt ice records extracted at deep drilling sites located inland

  17. Variations in the methanesulfonate to sulfate molar ratio in submicrometer marine aerosol particles over the south Pacific Ocean

    NASA Technical Reports Server (NTRS)

    Bates, Timothy S.; Calhoun, Julie A.; Quinn, Patricia K.

    1992-01-01

    Seawater concentrations of dimethylsulfide (DMS) and atmospheric concentrations of DMS, sulfur dioxide, methanesulfonate (MSA), and non-sea-salt (nss) sulfate were measured over the eastern Pacific Ocean between 105 deg and 110 deg W from 20 deg N to 60 deg S during February and March 1989. Although the samples collected in the Southern Hemisphere appear to be of marine origin, no significant correlation was found between the latitudinal distributions of DMS, SO2, MSA, and nss SO4(2-). However, an inverse correlation was found between atmospheric temperature and the MSA to nss SO4(2-) molar ratio in submicrometer aerosol particles with a decrease in temperature corresponding to an increase in the molar ratio. Although this trend is consistent with laboratory results indicating the favored production of MSA at lower temperatures, it is contrary to Southern Hemisphere baseline station data. This suggests either a decrease in the supply of DMS relative to nonmarine sources of nss SO4(2-) at the baseline stations in winter or additional mechanisms that affect the relative production of MSA and nss SO4(2-).

  18. A microphysical parameterization of aqSOA and sulfate formation in clouds

    NASA Astrophysics Data System (ADS)

    McVay, Renee; Ervens, Barbara

    2017-07-01

    Sulfate and secondary organic aerosol (cloud aqSOA) can be chemically formed in cloud water. Model implementation of these processes represents a computational burden due to the large number of microphysical and chemical parameters. Chemical mechanisms have been condensed by reducing the number of chemical parameters. Here an alternative is presented to reduce the number of microphysical parameters (number of cloud droplet size classes). In-cloud mass formation is surface and volume dependent due to surface-limited oxidant uptake and/or size-dependent pH. Box and parcel model simulations show that using the effective cloud droplet diameter (proportional to total volume-to-surface ratio) reproduces sulfate and aqSOA formation rates within ≤30% as compared to full droplet distributions; other single diameters lead to much greater deviations. This single-class approach reduces computing time significantly and can be included in models when total liquid water content and effective diameter are available.

  19. Substantial Seasonal Contribution of Observed Biogenic Sulfate Particles to Cloud Condensation Nuclei.

    PubMed

    Sanchez, Kevin J; Chen, Chia-Li; Russell, Lynn M; Betha, Raghu; Liu, Jun; Price, Derek J; Massoli, Paola; Ziemba, Luke D; Crosbie, Ewan C; Moore, Richard H; Müller, Markus; Schiller, Sven A; Wisthaler, Armin; Lee, Alex K Y; Quinn, Patricia K; Bates, Timothy S; Porter, Jack; Bell, Thomas G; Saltzman, Eric S; Vaillancourt, Robert D; Behrenfeld, Mike J

    2018-02-19

    Biogenic sources contribute to cloud condensation nuclei (CCN) in the clean marine atmosphere, but few measurements exist to constrain climate model simulations of their importance. The chemical composition of individual atmospheric aerosol particles showed two types of sulfate-containing particles in clean marine air masses in addition to mass-based Estimated Salt particles. Both types of sulfate particles lack combustion tracers and correlate, for some conditions, to atmospheric or seawater dimethyl sulfide (DMS) concentrations, which means their source was largely biogenic. The first type is identified as New Sulfate because their large sulfate mass fraction (63% sulfate) and association with entrainment conditions means they could have formed by nucleation in the free troposphere. The second type is Added Sulfate particles (38% sulfate), because they are preexisting particles onto which additional sulfate condensed. New Sulfate particles accounted for 31% (7 cm -3 ) and 33% (36 cm -3 ) CCN at 0.1% supersaturation in late-autumn and late-spring, respectively, whereas sea spray provided 55% (13 cm -3 ) in late-autumn but only 4% (4 cm -3 ) in late-spring. Our results show a clear seasonal difference in the marine CCN budget, which illustrates how important phytoplankton-produced DMS emissions are for CCN in the North Atlantic.

  20. Simultaneous quantification of cholesterol sulfate, androgen sulfates, and progestagen sulfates in human serum by LC-MS/MS.

    PubMed

    Sánchez-Guijo, Alberto; Oji, Vinzenz; Hartmann, Michaela F; Traupe, Heiko; Wudy, Stefan A

    2015-09-01

    Steroids are primarily present in human fluids in their sulfated forms. Profiling of these compounds is important from both diagnostic and physiological points of view. Here, we present a novel method for the quantification of 11 intact steroid sulfates in human serum by LC-MS/MS. The compounds analyzed in our method, some of which are quantified for the first time in blood, include cholesterol sulfate, pregnenolone sulfate, 17-hydroxy-pregnenolone sulfate, 16-α-hydroxy-dehydroepiandrosterone sulfate, dehydroepiandrosterone sulfate, androstenediol sulfate, androsterone sulfate, epiandrosterone sulfate, testosterone sulfate, epitestosterone sulfate, and dihydrotestosterone sulfate. The assay was conceived to quantify sulfated steroids in a broad range of concentrations, requiring only 300 μl of serum. The method has been validated and its performance was studied at three quality controls, selected for each compound according to its physiological concentration. The assay showed good linearity (R(2) > 0.99) and recovery for all the compounds, with limits of quantification ranging between 1 and 80 ng/ml. Averaged intra-day and between-day precisions (coefficient of variation) and accuracies (relative errors) were below 10%. The method has been successfully applied to study the sulfated steroidome in diseases such as steroid sulfatase deficiency, proving its diagnostic value. This is, to our best knowledge, the most comprehensive method available for the quantification of sulfated steroids in human blood. Copyright © 2015 by the American Society for Biochemistry and Molecular Biology, Inc.

  1. Speciation of the major inorganic salts in atmospheric aerosols of Beijing, China: Measurements and comparison with model

    NASA Astrophysics Data System (ADS)

    Tang, Xiong; Zhang, Xiaoshan; Ci, Zhijia; Guo, Jia; Wang, Jiaqi

    2016-05-01

    In the winter and summer of 2013-2014, we used a sampling system, which consists of annular denuder, back-up filter and thermal desorption set-up, to measure the speciation of major inorganic salts in aerosols and the associated trace gases in Beijing. This sampling system can separate volatile ammonium salts (NH4NO3 and NH4Cl) from non-volatile ammonium salts ((NH4)2SO4), as well as the non-volatile nitrate and chloride. The measurement data was used as input of a thermodynamic equilibrium model (ISORROPIA II) to investigate the gas-aerosol equilibrium characteristics. Results show that (NH4)2SO4, NH4NO3 and NH4Cl were the major inorganic salts in aerosols and mainly existed in the fine particles. The sulfate, nitrate and chloride associated with crustal ions were also important in Beijing where mineral dust concentrations were high. About 19% of sulfate in winter and 11% of sulfate in summer were associated with crustal ions and originated from heterogeneous reactions or direct emissions. The non-volatile nitrate contributed about 33% and 15% of nitrate in winter and summer, respectively. Theoretical thermodynamic equilibrium calculations for NH4NO3 and NH4Cl suggest that the gaseous precursors were sufficient to form stable volatile ammonium salts in winter, whereas the internal mixing with sulfate and crustal species were important for the formation of volatile ammonium salts in summer. The results of the thermodynamic equilibrium model reasonably agreed with the measurements of aerosols and gases, but large discrepancy existed in predicting the speciation of inorganic ammonium salts. This indicates that the assumption on crustal species in the model was important for obtaining better understanding on gas-aerosol partitioning and improving the model prediction.

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

    NASA Astrophysics Data System (ADS)

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

    2010-11-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2017-03-01

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

  4. Chemical characterization of organosulfates in secondary organic aerosol derived from the photooxidation of alkanes

    NASA Astrophysics Data System (ADS)

    Riva, Matthieu; Da Silva Barbosa, Thais; Lin, Ying-Hsuan; Stone, Elizabeth A.; Gold, Avram; Surratt, Jason D.

    2016-09-01

    We report the formation of aliphatic organosulfates (OSs) in secondary organic aerosol (SOA) from the photooxidation of C10-C12 alkanes. The results complement those from our laboratories reporting the formation of OSs and sulfonates from gas-phase oxidation of polycyclic aromatic hydrocarbons (PAHs). Both studies strongly support the formation of OSs from the gas-phase oxidation of anthropogenic precursors, as hypothesized on the basis of recent field studies in which aromatic and aliphatic OSs were detected in fine aerosol collected from several major urban locations. In this study, dodecane, cyclodecane and decalin, considered to be important SOA precursors in urban areas, were photochemically oxidized in an outdoor smog chamber in the presence of either non-acidified or acidified ammonium sulfate seed aerosol. Effects of acidity and relative humidity on OS formation were examined. Aerosols collected from all experiments were characterized by ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS). Most of the OSs identified could be explained by formation of gaseous epoxide precursors with subsequent acid-catalyzed reactive uptake onto sulfate aerosol and/or heterogeneous reactions of hydroperoxides. The OSs identified here were also observed and quantified in fine urban aerosol samples collected in Lahore, Pakistan, and Pasadena, CA, USA. Several OSs identified from the photooxidation of decalin and cyclodecane are isobars of known monoterpene organosulfates, and thus care must be taken in the analysis of alkane-derived organosulfates in urban aerosol.

  5. Sulfur deposition changes under sulfate geoengineering conditions: quasi-biennial oscillation effects on the transport and lifetime of stratospheric aerosols

    NASA Astrophysics Data System (ADS)

    Visioni, Daniele; Pitari, Giovanni; Tuccella, Paolo; Curci, Gabriele

    2018-02-01

    Sustained injection of sulfur dioxide (SO2) in the tropical lower stratosphere has been proposed as a climate engineering technique for the coming decades. Among several possible environmental side effects, the increase in sulfur deposition deserves additional investigation. In this study we present results from a composition-climate coupled model (University of L'Aquila Composition-Chemistry Model, ULAQ-CCM) and a chemistry-transport model (Goddard Earth Observing System Chemistry-Transport Model, GEOS-Chem), assuming a sustained lower-stratospheric equatorial injection of 8 Tg SO2 yr-1. Total S deposition is found to globally increase by 5.2 % when sulfate geoengineering is deployed, with a clear interhemispheric asymmetry (+3.8 and +10.3 % in the Northern Hemisphere (NH) and the Southern Hemisphere (SH), due to +2.2 and +1.8 Tg S yr-1, respectively). The two models show good consistency, both globally and on a regional scale under background and geoengineering conditions, except for S-deposition changes over Africa and the Arctic. The consistency exists with regard to time-averaged values but also with regard to monthly and interannual deposition changes. The latter is driven essentially by the variability in stratospheric large-scale transport associated with the quasi-biennial oscillation (QBO). Using an externally nudged QBO, it is shown how a zonal wind E shear favors aerosol confinement in the tropical pipe and a significant increase in their effective radius (+13 % with respect to W shear conditions). The net result is an increase in the downward cross-tropopause S flux over the tropics with dominant E shear conditions with respect to W shear periods (+0.61 Tg S yr-1, +42 %, mostly due to enhanced aerosol gravitational settling) and a decrease over the extratropics (-0.86 Tg S yr-1, -35 %, mostly due to decreased large-scale stratosphere-troposphere exchange of geoengineering sulfate). This translates into S-deposition changes that are significantly

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

    NASA Astrophysics Data System (ADS)

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

    2017-10-01

    Size-segregated aerosol particles were collected with a 10-stage Micro-Orifice Uniform Deposit Impactor (MOUDI) at an urban site in Shanghai, China for four non-consecutive months representing four seasons from 2015 to 2016. Chemical composition, including water-soluble ions as well as organic carbon (OC), elemental carbon (EC) and secondary organic carbon (SOC) of size-resolved (0.056-18 μm) atmospheric aerosols in four seasons and in different polluted cases were studied. The size distributions of sulfate, nitrate and ammonium (SNA) and carbonaceous aerosol (OC, EC and SOC) were discussed and the potential sources of PM1.8-associated secondary species (SO42-, NO3-, SNA and SOC) in different seasons were identified by potential source contribution function (PSCF) model. Results showed that atmospheric ultrafine and fine particle pollution in Shanghai were very serious during the study period. Most of the water-soluble ions tended to be enriched in fine particles, especially being abundant in the droplet mode in polluted cases. Compared with sulfate, size distributions of nitrate and ammonium presented more significant seasonal variations and showed distinctive characteristics in polluted days. Abundant nitrate was concentrated in fine particles in cold seasons (spring and winter), whereas it was enriched in coarse mode during summer and autumn. The droplet mode sulfate with high concentration did not result in the aggravation of air pollution, while the nucleation mode sulfate may have made a great contribution to the air pollution in urban Shanghai. It was also found that the formation of air pollution in urban Shanghai had a significant link with nitrate and ammonium, especially with nitrate and ammonium in condensation mode and droplet mode, and the contribution of sulfate to the pollution formation in Shanghai would somehow be surpassed by the increasing nitrate and ammonium. OC and EC concentrations from spring to winter were found to be 11.10, 7.10, 12

  7. Simultaneous quantification of cholesterol sulfate, androgen sulfates, and progestagen sulfates in human serum by LC-MS/MS[S

    PubMed Central

    Sánchez-Guijo, Alberto; Oji, Vinzenz; Hartmann, Michaela F.; Traupe, Heiko; Wudy, Stefan A.

    2015-01-01

    Steroids are primarily present in human fluids in their sulfated forms. Profiling of these compounds is important from both diagnostic and physiological points of view. Here, we present a novel method for the quantification of 11 intact steroid sulfates in human serum by LC-MS/MS. The compounds analyzed in our method, some of which are quantified for the first time in blood, include cholesterol sulfate, pregnenolone sulfate, 17-hydroxy-pregnenolone sulfate, 16-α-hydroxy-dehydroepiandrosterone sulfate, dehydroepiandrosterone sulfate, androstenediol sulfate, androsterone sulfate, epiandrosterone sulfate, testosterone sulfate, epitestosterone sulfate, and dihydrotestosterone sulfate. The assay was conceived to quantify sulfated steroids in a broad range of concentrations, requiring only 300 μl of serum. The method has been validated and its performance was studied at three quality controls, selected for each compound according to its physiological concentration. The assay showed good linearity (R2 > 0.99) and recovery for all the compounds, with limits of quantification ranging between 1 and 80 ng/ml. Averaged intra-day and between-day precisions (coefficient of variation) and accuracies (relative errors) were below 10%. The method has been successfully applied to study the sulfated steroidome in diseases such as steroid sulfatase deficiency, proving its diagnostic value. This is, to our best knowledge, the most comprehensive method available for the quantification of sulfated steroids in human blood. PMID:26239050

  8. OCS, stratospheric aerosols and climate

    NASA Technical Reports Server (NTRS)

    Turco, R. P.; Whitten, R. C.; Toon, O. B.; Pollack, J. B.; Hamill, P.

    1980-01-01

    The carbonyl sulfide budget in the atmosphere is examined, and the effects of stratospheric sulfate aerosol particles, formed in part from atmospheric carbonyl sulfate, on global climate are considered. From tropospheric measurements of carbon disulfide and the rate constant for the conversion of carbon disulfide to carbonyl sulfide, it is estimated that five Tg of carbonyl sulfide/year could be generated from carbon disulfide in the atmosphere. Direct sources of OCS include the refining and combustion of fossil fuels (1 Tg/year), natural and agricultural fires (0.2 to 0.3 Tg/year), and soils (0.5 Tg/year), yielding a total influx of from 1 to 10 Tg/year, up to 50% of which may be anthropogenic. Considerations of carbonyl sulfide sinks and concentrations indicate an atmospheric lifetime of one year, with OCS the major atmospheric sulfur compound. It is estimated that a ten-fold increase in atmospheric carbonyl sulfide would cause an optical depth perturbation comparable to that of a modest volcanic eruption, leading to an average global surface temperature decrease of 0.1 K, in addition to a possible greenhouse effect.

  9. Roles of production, consumption and trade in global and regional aerosol radiative forcing

    NASA Astrophysics Data System (ADS)

    Lin, J.; Tong, D.; Davis, S. J.; Ni, R.; Tan, X.; Pan, D.; Zhao, H.; Lu, Z.; Streets, D. G.; Feng, T.; Zhang, Q.; Yan, Y.; Hu, Y.; Li, J.; Liu, Z.; Jiang, X.; Geng, G.; He, K.; Huang, Y.; Guan, D.

    2016-12-01

    Anthropogenic aerosols exert strong radiative forcing on the climate system. Prevailing view regards aerosol radiative forcing as a result of emissions from regions' economic production, with China and other developing regions having the largest contributions to radiative forcing at present. However, economic production is driven by global demand for computation, and international trade allows for separation of regions consuming goods and services from regions where goods and related aerosol pollution are produced. It has recently been recognized that regions' consumption and trade have profoundly altered the spatial distribution of aerosol emissions and pollution. Building upon our previous work, this study quantifies for the first time the roles of trade and consumption in aerosol climate forcing attributed to different regions. We contrast the direct radiative forcing of aerosols related to regions' consumption of goods and services against the forcing due to emissions produced in each region. Aerosols assessed include black carbon, primary organic aerosol, and secondary inorganic aerosols including sulfate, nitrate and ammonium. We find that global aerosol radiative forcing due to emissions produced in East Asia is much stronger than the forcing related to goods and services ultimately consumed in that region because of its large net export of emissions-intensive goods. The opposite is true for net importers like Western Europe and North America: global radiative forcing related to consumption is much greater than the forcing due to emissions produced in these regions. Overall, trade is associated with a shift of radiative forcing from net importing to net exporting regions. Compared to greenhouse gases such as carbon dioxide, the short atmospheric lifetimes of aerosols cause large localized differences in radiative forcing. International efforts to reduce emissions in the exporting countries will help alleviate trade-related climate and health impacts of

  10. Initial Verification of GEOS-4 Aerosols Using CALIPSO and MODIS: Scene Classification

    NASA Technical Reports Server (NTRS)

    Welton, Ellsworth J.; Colarco, Peter R.; Hlavka, Dennis; Levy, Robert C.; Vaughan, Mark A.; daSilva, Arlindo

    2007-01-01

    A-train sensors such as MODIS and MISR provide column aerosol properties, and in the process a means of estimating aerosol type (e.g. smoke vs. dust). Correct classification of aerosol type is important because retrievals are often dependent upon selection of the right aerosol model. In addition, aerosol scene classification helps place the retrieved products in context for comparisons and analysis with aerosol transport models. The recent addition of CALIPSO to the A-train now provides a means of classifying aerosol distribution with altitude. CALIPSO level 1 products include profiles of attenuated backscatter at 532 and 1064 nm, and depolarization at 532 nm. Backscatter intensity, wavelength ratio, and depolarization provide information on the vertical profile of aerosol concentration, size, and shape. Thus similar estimates of aerosol type using MODIS or MISR are possible with CALIPSO, and the combination of data from all sensors provides a means of 3D aerosol scene classification. The NASA Goddard Earth Observing System general circulation model and data assimilation system (GEOS-4) provides global 3D aerosol mass for sulfate, sea salt, dust, and black and organic carbon. A GEOS-4 aerosol scene classification algorithm has been developed to provide estimates of aerosol mixtures along the flight track for NASA's Geoscience Laser Altimeter System (GLAS) satellite lidar. GLAS launched in 2003 and did not have the benefit of depolarization measurements or other sensors from the A-train. Aerosol typing from GLAS data alone was not possible, and the GEOS-4 aerosol classifier has been used to identify aerosol type and improve the retrieval of GLAS products. Here we compare 3D aerosol scene classification using CALIPSO and MODIS with the GEOS-4 aerosol classifier. Dust, smoke, and pollution examples will be discussed in the context of providing an initial verification of the 3D GEOS-4 aerosol products. Prior model verification has only been attempted with surface mass

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

    PubMed

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

    2016-09-01

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

  12. Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO2

    NASA Astrophysics Data System (ADS)

    Liu, T.; Wang, X.; Hu, Q.; Deng, W.; Zhang, Y.; Ding, X.; Fu, X.; Bernard, F.; Zhang, Z.; Lü, S.; He, Q.; Bi, X.; Chen, J.; Sun, Y.; Yu, J.; Peng, P.; Sheng, G.; Fu, J.

    2016-01-01

    Sulfur dioxide (SO2) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE) and SO2, a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA) and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sulfate was formed through the oxidation of SO2 in the presence of high concentration of SO2. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60-200 % in the presence of high concentration of SO2. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (R2 = 0.97) between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) (0.44 ± 0.02) and higher hydrogen-to-carbon (H : C) (1.40 ± 0.03) molar ratios for the GVE / SO2 mixture, with a significantly lower estimated average carbon oxidation state (OSc) of -0.51 ± 0.06 than -0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be a significant explanation for the lower SOA oxidation degree.

  13. Formation of secondary aerosols from gasoline vehicle exhausts when mixing with SO2

    NASA Astrophysics Data System (ADS)

    Liu, T.; Wang, X.; Hu, Q.; Deng, W.; Zhang, Y.; Ding, X.; Fu, X.; Bernard, F.; Zhang, Z.; Lü, S.; He, Q.; Bi, X.; Chen, J.; Sun, Y.; Yu, J.; Peng, P.; Sheng, G.; Fu, J.

    2015-09-01

    Sulfur dioxide (SO2) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhausts, is still poorly understood. Here we directly co-introduced gasoline vehicles exhausts (GVE) and SO2, a typical pollutant from coal burning, into a smog chamber to investigate the formation of secondary organic aerosols (SOA) and sulfate aerosols through photooxidation. In the presence of high concentration of SO2, new particle formation was enhanced while substantial sulfate was formed through the oxidation of SO2. The homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60-200 % in the presence of high concentration of SO2. This increase could largely be attributed to acid-catalyzed SOA formation, which was evidenced by the strong positive linear correlation (R2 = 0.97) between the SOA production factor and in-situ particle acidity calculated by AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) and higher hydrogen-to-carbon (H : C) molar ratios for the GVE/SO2 mixture, with a much lower estimated average carbon oxidation state (OSc) of -0.51 ± 0.06 than that of -0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be the major reason for the lower oxidation degree of SOA.

  14. 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.

  15. Secondary Organic Aerosol Formation from Glyoxal: photochemical versus dark uptake and reversible versus irreversible SOA formation

    NASA Astrophysics Data System (ADS)

    Waxman, E.; Slowik, J. G.; Kampf, C. J.; Timkovsky, J.; Noziere, B.; Praplan, A. P.; Pfaffenberger, L.; Holzinger, R.; Hoffmann, T.; Dommen, J.; Prevot, A. S.; Baltensperger, U.; Volkamer, R.

    2011-12-01

    Glyoxal forms secondary organic aerosol (SOA) by partitioning to the aerosol aqueous phase according to Henry's law. The subsequent processing by heterogeneous and multiphase reactions shifts the partitioning towards aerosols. Currently it is not well understood whether these reactions result in reversible or irreversible SOA formation, and what parameters influence the rate limiting step of multiphase processing. We conducted a series of simulation chamber experiments at PSI in April and May 2011 to investigate processing under dark conditions, UV and/or visible light irradiated conditions, and in the presence and absence of OH radicals. Experiments used ammonium sulfate or ammonium sulfate/fulvic acid mixtures as seed aerosols, and were conducted between 50% and 85% relative humidity at approximately constant RH over the course of any given experiment. Glyoxal was produced photochemically from acetylene, using HONO photolysis as the OH radical source. Gas-phase glyoxal was measured by the CU LED-Cavity Enhanced-DOAS. The Thermal-Desorption Proton-Transfer-Reaction Mass Spectrometer (TD-PTR-MS) and Ion Chromatography Mass Spectrometer (IC-MS) monitored both gas and aerosol-phase organic reaction products. Particle composition was monitored by High-Resolution Time-of-Flight Aerosol Mass Spectrometry (HR-ToF-AMS), and HPLC-ESI MS/MS and LC-MS analysis of filter samples.

  16. Secondary Organic Aerosol Formation from Glyoxal: photochemical versus dark uptake and reversible versus irreversible SOA formation

    NASA Astrophysics Data System (ADS)

    Waxman, E.; Slowik, J.; Kampf, C.; Timkovsky, J.; Noziere, B.; Praplan, A.; Pffafenberger, L.; Holzinger, R.; Hoffmann, T.; Dommen, J.; Prevot, A.; Baltensperger, U.; Volkamer, R.

    2012-04-01

    Glyoxal forms secondary organic aerosol (SOA) by partitioning to the aerosol aqueous phase according to Henry's law. The subsequent processing by heterogeneous and multiphase reactions shifts the partitioning towards aerosols. Currently it is not well understood whether these reactions result in reversible or irreversible SOA formation, and what parameters influence the rate limiting step of multiphase processing. We conducted a series of simulation chamber experiments at PSI in April and May 2011 to investigate processing under dark conditions, UV and/or visible light irradiated conditions, and in the presence and absence of OH radicals. Experiments used ammonium sulfate or ammonium sulfate/fulvic acid mixtures as seed aerosols, and were conducted between 50% and 85% relative humidity at approximately constant RH over the course of any given experiment. Glyoxal was produced photochemically from acetylene, using HONO photolysis as the OH radical source. Gas-phase glyoxal was measured by the CU LED-Cavity Enhanced-DOAS. The Thermal-Desorption Proton-Transfer-Reaction Mass Spectrometer (TD-PTR-MS) and Ion Chromatography Mass Spectrometer (IC-MS) monitored both gas and aerosol-phase organic reaction products. Particle composition was monitored by High-Resolution Time-of-Flight Aerosol Mass Spectrometry (HR-ToF-AMS), and HPLC-ESI MS/MS and LC-MS analysis of filter samples.

  17. Sources, seasonality, and trends of Southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

    NASA Astrophysics Data System (ADS)

    Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

    2015-07-01

    We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the Southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 km × 25 km resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the Southeast US. GEOS-Chem simulation of sulfate requires a missing oxidant, taken here to be stabilized Criegee intermediates, but which could alternatively reflect an unaccounted for heterogeneous process. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 20 % in the cloud convective layer at 1.5-3 km, and 20 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-])) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by organic aerosol. This would explain the long-term decline of ammonium aerosol in the Southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the Southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the Southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 21 %. The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from

  18. Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

    NASA Astrophysics Data System (ADS)

    Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

    2012-12-01

    Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle

  19. Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

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

    Saide P. E.; Springston S.; Spak, S. N.

    2012-03-29

    We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and three aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign-averaged longitudinal gradients, and highlight differences in model simulations with (W) and without (NW) wet deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptualmore » model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, especially in the activation parameterization, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions, and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, and may do so with the reliability required for policy analysis.« less

  20. A 4-D Climatology (1979-2009) of the Monthly Tropospheric Aerosol Optical Depth Distribution over the Mediterranean Region from a Comparative Evaluation and Blending of Remote Sensing and Model Products

    NASA Technical Reports Server (NTRS)

    Nabat, P.; Somot, S.; Mallet, M.; Chiapello, I; Morcrette, J. J.; Solomon, F.; Szopa, S.; Dulac, F; Collins, W.; Ghan, S.; hide

    2013-01-01

    Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multiyear database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, seasalt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDER and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth- Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level- 2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatio-temporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust

  1. Sources and Removal of Springtime Arctic Aerosol

    NASA Astrophysics Data System (ADS)

    Willis, M. D.; Burkart, J.; Bozem, H.; Kunkel, D.; Schulz, H.; Hanna, S.; Aliabadi, A. A.; Bertram, A. K.; Hoor, P. M.; Herber, A. B.; Leaitch, R.; Abbatt, J.

    2017-12-01

    The sources and removal mechanisms of pollution transported to Arctic regions are key factors in controlling the impact of short-lived climate forcing agents on Arctic climate. We lack a predictive understanding of pollution transport to Arctic regions largely due to poor understanding of removal mechanisms and aerosol chemical and physical processing both within the Arctic and during transport. We present vertically resolved observations of aerosol physical and chemical properties in High Arctic springtime. While much previous work has focused on characterizing episodic events of high pollutant concentrations transported to Arctic regions, here we focus on measurements made under conditions consistent with chronic Arctic Haze, which is more representative of the pollution seasonal maximum observed at long term monitoring stations. On six flights based at Alert and Eureka, Nunavut, Canada, we observe evidence for vertical variations in both aerosol sources and removal mechanisms. With support from model calculations, we show evidence for sources of partially neutralized aerosol with higher organic aerosol (OA) and black carbon content in the middle troposphere, compared to lower tropospheric aerosol with higher amounts of acidic sulfate. Further, we show evidence for aerosol depletion relative to carbon monoxide, both in the mid-to-upper troposphere and within the Arctic Boundary Layer (ABL). Dry deposition, with relatively low removal efficiency, was responsible for aerosol removal in the ABL while ice or liquid-phase scavenging was responsible for aerosol removal at higher altitudes during transport. Overall, we find that vertical variations in both regional and remote aerosol sources, and removal mechanisms, combine with long aerosol residence times to drive the properties of springtime Arctic aerosol.

  2. An Aerosol Physical Chemistry Model for the Upper Troposphere

    NASA Technical Reports Server (NTRS)

    Lin, Jin-Sheng

    2001-01-01

    This report is the final report for the Cooperative Agreement NCC2-1000. The tasks outlined in the various proposals are listed with a brief comment as to the research performed. The publications titles are: The effects of particle size and nitric acid uptake on the homogenous freezing of sulfate aerosols; Parameterization of an aerosol physical chemistry model (APCM) for the NH3/H2SO4/HNO3/H2O system at cold temperatures; and The onset, extent and duration of dehydration in the Southern Hemisphere polar vortex.

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

    NASA Astrophysics Data System (ADS)

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

    2010-05-01

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

  4. An interfacial mechanism for cloud droplet formation on organic aerosols

    DOE PAGES

    Ruehl, C. R.; Davies, J. F.; Wilson, K. R.

    2016-03-25

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depressionmore » by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.« less

  5. An interfacial mechanism for cloud droplet formation on organic aerosols

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

    Ruehl, C. R.; Davies, J. F.; Wilson, K. R.

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depressionmore » by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.« less

  6. Coupling of organic and inorganic aerosol systems and the effect on gas–particle partitioning in the southeastern US

    PubMed Central

    Pye, Havala O. T.; Zuend, Andreas; Fry, Juliane L.; Isaacman-VanWertz, Gabriel; Capps, Shannon L.; Appel, K. Wyat; Foroutan, Hosein; Xu, Lu; Ng, Nga L.; Goldstein, Allen H.

    2018-01-01

    Several models were used to describe the partitioning of ammonia, water, and organic compounds between the gas and particle phases for conditions in the southeastern US during summer 2013. Existing equilibrium models and frameworks were found to be sufficient, although additional improvements in terms of estimating pure-species vapor pressures are needed. Thermodynamic model predictions were consistent, to first order, with a molar ratio of ammonium to sulfate of approximately 1.6 to 1.8 (ratio of ammonium to 2× sulfate, RN/2S ≈ 0.8 to 0.9) with approximately 70% of total ammonia and ammonium (NHx) in the particle. Southeastern Aerosol Research and Characterization Network (SEARCH) gas and aerosol and Southern Oxidant and Aerosol Study (SOAS) Monitor for AeRosols and Gases in Ambient air (MARGA) aerosol measurements were consistent with these conditions. CMAQv5.2 regional chemical transport model predictions did not reflect these conditions due to a factor of 3 overestimate of the nonvolatile cations. In addition, gas-phase ammonia was overestimated in the CMAQ model leading to an even lower fraction of total ammonia in the particle. Chemical Speciation Network (CSN) and aerosol mass spectrometer (AMS) measurements indicated less ammonium per sulfate than SEARCH and MARGA measurements and were inconsistent with thermodynamic model predictions. Organic compounds were predicted to be present to some extent in the same phase as inorganic constituents, modifying their activity and resulting in a decrease in [H+]air (H+ in μgm−3 air), increase in ammonia partitioning to the gas phase, and increase in pH compared to complete organic vs. inorganic liquid–liquid phase separation. In addition, accounting for nonideal mixing modified the pH such that a fully interactive inorganic–organic system had a pH roughly 0.7 units higher than predicted using traditional methods (pH = 1.5 vs. 0.7). Particle-phase interactions of organic and inorganic compounds were found to

  7. Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US

    NASA Astrophysics Data System (ADS)

    Pye, Havala O. T.; Zuend, Andreas; Fry, Juliane L.; Isaacman-VanWertz, Gabriel; Capps, Shannon L.; Wyat Appel, K.; Foroutan, Hosein; Xu, Lu; Ng, Nga L.; Goldstein, Allen H.

    2018-01-01

    Several models were used to describe the partitioning of ammonia, water, and organic compounds between the gas and particle phases for conditions in the southeastern US during summer 2013. Existing equilibrium models and frameworks were found to be sufficient, although additional improvements in terms of estimating pure-species vapor pressures are needed. Thermodynamic model predictions were consistent, to first order, with a molar ratio of ammonium to sulfate of approximately 1.6 to 1.8 (ratio of ammonium to 2 × sulfate, RN/2S ≈ 0.8 to 0.9) with approximately 70 % of total ammonia and ammonium (NHx) in the particle. Southeastern Aerosol Research and Characterization Network (SEARCH) gas and aerosol and Southern Oxidant and Aerosol Study (SOAS) Monitor for AeRosols and Gases in Ambient air (MARGA) aerosol measurements were consistent with these conditions. CMAQv5.2 regional chemical transport model predictions did not reflect these conditions due to a factor of 3 overestimate of the nonvolatile cations. In addition, gas-phase ammonia was overestimated in the CMAQ model leading to an even lower fraction of total ammonia in the particle. Chemical Speciation Network (CSN) and aerosol mass spectrometer (AMS) measurements indicated less ammonium per sulfate than SEARCH and MARGA measurements and were inconsistent with thermodynamic model predictions. Organic compounds were predicted to be present to some extent in the same phase as inorganic constituents, modifying their activity and resulting in a decrease in [H+]air (H+ in µg m-3 air), increase in ammonia partitioning to the gas phase, and increase in pH compared to complete organic vs. inorganic liquid-liquid phase separation. In addition, accounting for nonideal mixing modified the pH such that a fully interactive inorganic-organic system had a pH roughly 0.7 units higher than predicted using traditional methods (pH = 1.5 vs. 0.7). Particle-phase interactions of organic and inorganic compounds were found to

  8. Modeling of 2008 Kasatochi Volcanic Sulfate Direct Radiative Forcing: Assimilation of OMI SO2 Plume Height Data and Comparison with MODIS and CALIOP Observations

    NASA Technical Reports Server (NTRS)

    Wang, J.; Park, S.; Zeng, J.; Ge, C.; Yang, K.; Carn, S.; Krotkov, N.; Omar, A. H.

    2013-01-01

    Volcanic SO2 column amount and injection height retrieved from the Ozone Monitoring Instrument (OMI) with the Extended Iterative Spectral Fitting (EISF) technique are used to initialize a global chemistry transport model (GEOS-Chem) to simulate the atmospheric transport and lifecycle of volcanic SO2 and sulfate aerosol from the 2008 Kasatochi eruption, and to subsequently estimate the direct shortwave, top-of-the-atmosphere radiative forcing of the volcanic sulfate aerosol. Analysis shows that the integrated use of OMI SO2 plume height in GEOS-Chem yields: (a) good agreement of the temporal evolution of 3-D volcanic sulfate distributions between model simulations and satellite observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarisation (CALIOP), and (b) an e-folding time for volcanic SO2 that is consistent with OMI measurements, reflecting SO2 oxidation in the upper troposphere and stratosphere is reliably represented in the model. However, a consistent (approx. 25 %) low bias is found in the GEOS-Chem simulated SO2 burden, and is likely due to a high (approx.20 %) bias of cloud liquid water amount (as compared to the MODIS cloud product) and the resultant stronger SO2 oxidation in the GEOS meteorological data during the first week after eruption when part of SO2 underwent aqueous-phase oxidation in clouds. Radiative transfer calculations show that the forcing by Kasatochi volcanic sulfate aerosol becomes negligible 6 months after the eruption, but its global average over the first month is -1.3W/sq m, with the majority of the forcing-influenced region located north of 20degN, and with daily peak values up to -2W/sq m on days 16-17. Sensitivity experiments show that every 2 km decrease of SO2 injection height in the GEOS-Chem simulations will result in a approx.25% decrease in volcanic sulfate forcing; similar sensitivity but opposite sign also holds for a 0.03 m increase of geometric radius of

  9. Characterization of the sources and processes of organic and inorganic aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2010-10-01

    Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during the summer 2009 Field Intensive Study at Queens College in New York City. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of total PM1 mass on average. The average mass size distribution of OA presents a small mode peaking at ~150 nm (Dva) in addition to an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of sulfate and OA both show pronounced peaks between 01:00-02:00 p.m. EST due to photochemical production. The average (±1σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012(±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62(±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified five OA components: a hydrocarbon-like OA (HOA), two types of oxygenated OA (OOA) including a low-volatility OOA (LV-OOA) and a semi-volatile OOA (SV-OOA), a cooking-emission related OA (COA), and a unique nitrogen-enriched OA (NOA). HOA appears to represent primary OA (POA) from urban traffic emissions. It comprises primarily of reduced species (H/C=1.83; O/C=0.06) and shows a mass spectral pattern very similar to those of POA from fossil fuel combustion, and correlates tightly with traffic emission tracers including elemental carbon and NOx. LV-OOA, which is highly oxidized (O/C=0.63) and correlates well with sulfate, appears to be representative for regional, aged secondary OA (SOA). SV-OOA, which is less oxidized (O/C=0.38) and correlates well with non-refractory chloride, likely represents less photo-chemically aged, semi-volatile SOA. COA shows a similar spectral pattern to the reference spectra of POA from cooking emissions and a distinct diurnal pattern

  10. LLNL Scientists Use NERSC to Advance Global Aerosol Simulations

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

    Bergmann, D J; Chuang, C; Rotman, D

    2004-10-13

    While ''greenhouse gases'' have been the focus of climate change research for a number of years, DOE's ''Aerosol Initiative'' is now examining how aerosols (small particles of approximately micron size) affect the climate on both a global and regional scale. Scientists in the Atmospheric Science Division at Lawrence Livermore National Laboratory (LLNL) are using NERSC's IBM supercomputer and LLNL's IMPACT (atmospheric chemistry) model to perform simulations showing the historic effects of sulfur aerosols at a finer spatial resolution than ever done before. Simulations were carried out for five decades, from the 1950s through the 1990s. The results clearly show themore » effects of the changing global pattern of sulfur emissions. Whereas in 1950 the United States emitted 41 percent of the world's sulfur aerosols, this figure had dropped to 15 percent by 1990, due to conservation and anti-pollution policies. By contrast, the fraction of total sulfur emissions of European origin has only dropped by a factor of 2 and the Asian emission fraction jumped six fold during the same time, from 7 percent in 1950 to 44 percent in 1990. Under a special allocation of computing time provided by the Office of Science INCITE (Innovative and Novel Computational Impact on Theory and Experiment) program, Dan Bergmann, working with a team of LLNL scientists including Cathy Chuang, Philip Cameron-Smith, and Bala Govindasamy, was able to carry out a large number of calculations during the past month, making the aerosol project one of the largest users of NERSC resources. The applications ran on 128 and 256 processors. The objective was to assess the effects of anthropogenic (man-made) sulfate aerosols. The IMPACT model calculates the rate at which SO{sub 2} (a gas emitted by industrial activity) is oxidized and forms particles known as sulfate aerosols. These particles have a short lifespan in the atmosphere, often washing out in about a week. This means that their effects on climate

  11. Aerosols and Aerosol-related haze forecasting in China Meteorological Adminstration

    NASA Astrophysics Data System (ADS)

    Zhou, Chunhong; Zhang, Xiaoye; Gong, Sunling; Liu, Hongli; Xue, Min

    2017-04-01

    CMA Unified Atmospheric Chemistry Environmental Forecasting System (CUACE) is a unified numerical chemical weather forecasting system with BC, OC, Sulfate, Nitrate, Ammonia, Dust and Sea-Salt aerosols and their sources, gas to particle processes, SOA, microphysics and transformation. With an open interface, CUACE has been online coupled to mesoscale model MM5 and the new NWP system GRAPES (Global/Regional Assimilation and Prediction Enhanced System)min CMA. With Chinese Emissions from Cao and Zhang(2012 and 2013), a forecasting system called CUACE/Haze-fog has been running in real time in CMA and issue 5-days PM10, O3 and Visibility forecasts. A comprehensive ACI scheme has also been developed in CUACE Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The results show that interactive aerosols with the WDM6 in CUACE obviously improve the clouds properties and the precipitation, showing 24% to 48% enhancements of TS scoring for 6-h precipitation .

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  13. 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.

  14. Global Radiative Forcing of Coupled Tropospheric Ozone and Aerosols in a Unified General Circulation Model

    NASA Technical Reports Server (NTRS)

    Liao, Hong; Seinfeld, John H.; Adams, Peter J.; Mickley, Loretta J.

    2008-01-01

    Global simulations of sea salt and mineral dust aerosols are integrated into a previously developed unified general circulation model (GCM), the Goddard Institute for Space Studies (GISS) GCM II', that simulates coupled tropospheric ozone-NOx-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. The fully coupled gas-aerosol unified GCM allows one to evaluate the extent to which global burdens, radiative forcing, and eventually climate feedbacks of ozone and aerosols are influenced by gas-aerosol chemical interactions. Estimated present-day global burdens of sea salt and mineral dust are 6.93 and 18.1 Tg with lifetimes of 0.4 and 3.9 days, respectively. The GCM is applied to estimate current top of atmosphere (TOA) and surface radiative forcing by tropospheric ozone and all natural and anthropogenic aerosol components. The global annual mean value of the radiative forcing by tropospheric ozone is estimated to be +0.53 W m(sup -2) at TOA and +0.07 W m(sup -2) at the Earth's surface. Global, annual average TOA and surface radiative forcing by all aerosols are estimated as -0.72 and -4.04 W m(sup -2), respectively. While the predicted highest aerosol cooling and heating at TOA are -10 and +12 W m(sup -2) respectively, surface forcing can reach values as high as -30 W m(sup -2), mainly caused by the absorption by black carbon, mineral dust, and OC. We also estimate the effects of chemistry-aerosol coupling on forcing estimates based on currently available understanding of heterogeneous reactions on aerosols. Through altering the burdens of sulfate, nitrate, and ozone, heterogeneous reactions are predicted to change the global mean TOA forcing of aerosols by 17% and influence global mean TOA forcing of tropospheric ozone by 15%.

  15. 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.

  16. Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

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

    Mills, Michael J.; Schmidt, Anja; Easter, Richard

    Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptionsmore » between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.« less

  17. Glyoxal in aqueous ammonium sulfate solutions: products, kinetics and hydration effects.

    PubMed

    Yu, Ge; Bayer, Amanda R; Galloway, Melissa M; Korshavn, Kyle J; Fry, Charles G; Keutsch, Frank N

    2011-08-01

    Reactions and interactions between glyoxal and salts in aqueous solution were studied. Glyoxal was found to react with ammonium to form imidazole, imidazole-2-carboxaldehyde, formic acid, N-glyoxal substituted imidazole, and minor products at very low concentrations. Overall reaction orders and rates for each major product were measured. Sulfate ions have a strong and specific interaction with glyoxal in aqueous solution, which shifts the hydration equilibria of glyoxal from the unhydrated carbonyl form to the hydrated form. This ion-specific effect contributes to the observed enhancement of the effective Henry's law coefficient for glyoxal in sulfate-containing solutions. The results of UV-vis absorption and NMR spectroscopy studies of solutions of glyoxal with ammonium, methylamine, and dimethylamine salts reveal that light absorbing compounds require the formation of nitrogen containing molecules. These findings have implications on the role of glyoxal in the atmosphere, both in models of the contribution of glyoxal to form secondary organic aerosol (SOA), the role of nitrogen containing species for aerosol optical properties and in predictions of the behavior of other carbonyls or dicarbonyls in the atmosphere.

  18. Chemical and cellular oxidant production induced by naphthalene secondary organic aerosol (SOA): effect of redox-active metals and photochemical aging.

    PubMed

    Tuet, Wing Y; Chen, Yunle; Fok, Shierly; Gao, Dong; Weber, Rodney J; Champion, Julie A; Ng, Nga L

    2017-11-09

    Exposure to air pollution is a leading global health risk. Secondary organic aerosol (SOA) constitute a large portion of ambient particulate matter (PM). In this study, the water-soluble oxidative potential (OP) determined by dithiothreitol (DTT) consumption and intracellular reactive oxygen and nitrogen species (ROS/RNS) production was measured for SOA generated from the photooxidation of naphthalene in the presence of iron sulfate and ammonium sulfate seed particles. The measured intrinsic OP varied for aerosol formed using different initial naphthalene concentrations, however, no trends were observed between OP and bulk aerosol composition or seed type. For all experiments, aerosol generated in the presence of iron-containing seed induced higher ROS/RNS production compared to that formed in the presence of inorganic seed. This effect was primarily attributed to differences in aerosol carbon oxidation state [Formula: see text]. In the presence of iron, radical concentrations are elevated via iron redox cycling, resulting in more oxidized species. An exponential trend was also observed between ROS/RNS and [Formula: see text] for all naphthalene SOA, regardless of seed type or aerosol formation condition. This may have important implications as aerosol have an atmospheric lifetime of a week, over which [Formula: see text] increases due to continued photochemical aging, potentially resulting in more toxic aerosol.

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

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

    DOE PAGES

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

    2015-02-10

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

  1. Aerosol Climate Effects: Local Radiative Forcing and Column Closure Experiments

    NASA Technical Reports Server (NTRS)

    Russell, P. B.; Bergstrom, Robert W.; Kinne, S. A.

    2000-01-01

    In an effort to reduce uncertainties in climate change predictions, experiments are being planned and conducted to measure anthropogenic aerosol properties and effects, including effects on radiative fields. The global average, direct anthropogenic aerosol effect on upwelling shortwave fluxes is estimated to be about +1/2 W/sq m, whereas errors in flux changes measured with airborne and spaceborne radiometers are 2 to 8 W/sq m or larger. This poses the question of whether flux changes expected in field experiments will be large enough to measure accurately. This paper obtains a new expression for the aerosol-induced change in upwelling flux, compares it to two-stream and adding-doubling (AD) results, and uses all three methods to estimate expected flux changes. The new expression accounts for the solar zenith angle dependences of aerosol transmission and reflection, as well as of surface albedo, all of which can have a strong effect in determining flux changes measured in field experiments. Despite its relative simplicity, the new expression gives results similar to previous two-stream results. Relative to AD results, it agrees within a few watts per square meter for the intermediate solar elevation angles where the flux changes peak (roughly 10 to 30 degrees), but it has negative errors for higher Sun and positive errors for lower Sun. All three techniques yield aerosol-induced changes in upwelling flux of +8 to +50 W/sq m for aerosol midvisible optical depths of 0.1 to 0.5. Because such aerosol optical depths occur frequently off the U.S. and European Atlantic coasts in summer, the flux changes they induce should be measurable by airborne, and possibly by spaceborne, radiometers, provided sufficient care is taken in experiment design (including measurements to separate aerosol radiative effects from those of absorbing gases). The expected flux changes are about 15 to 100 times larger than the global average flux change expected for the global average

  2. Composition and diurnal variability of the natural Amazonian aerosol

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

  3. Criteria pollutant and acid aerosol characterization study, Catano, Puerto Rico

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

    Edgerton, E.S.; Harlos, D.P.; Sune, J.M.

    1995-07-01

    The primary objective of the Catano Criteria Pollutant and Acid Aerosol Characterization Study (CPAACS) was to measure criteria pollutant concentrations and acid aerosol concentrations in and around the Ward of Catano, Puerto Rico, during the summer of 1994. Continuous air sampling for criteria pollutants was performed at three fixed stations and one moobile station that was deployed to four locations. Air samples for acid aerosol analyses and particulate matter measurements were collected at three sites. Semicontinuous sulfate analysis was performed at the primary site. Continuous measurements of wind speed, wind direction, temperature, and relative humidity were also made at eachmore » site. The study was conducted from June 1 through September 30, 1994.« less

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  5. Constraining the long-term climate reponse to stratospheric sulfate aerosols injection by the short-term volcanic climate response

    NASA Astrophysics Data System (ADS)

    Plazzotta, M.; Seferian, R.; Douville, H.; Kravitz, B.; Tilmes, S.; Tjiputra, J.

    2016-12-01

    Rising greenhouse gas emissions are leading to global warming and climate change, which will have multiple impacts on human society. Geoengineering methods like solar radiation management by stratospheric sulfate aerosols injection (SSA-SRM) aim at treating the symptoms of climate change by reducing the global temperature. Since a real-world testing cannot be implemented, Earth System Models (ESMs) are useful tools to assess the climate impacts of such geoengineering methods. However, coordinated simulations performed with the Geoengineering Model Intercomparison Project (GeoMIP) have shown that climate cooling in response to a continuous injection of 5Tg of SO2 per year under RCP45 future projection (the so-called G4 experiment) differs substantially between ESMs. Here, we employ a volcano analog approach to constrain the climate response in SSA-SRM geoengineering simulations across an ensemble of 10 ESMs. We identify an emergent relationship between the long-term cooling in responses to the mitigation of the clear-sky surface downwelling shortwave radiation (RSDSCS), and the short-term cooling related to the change in RSDSCS during the major tropical volcanic eruptions observed over the historical period (1850-2005). This relationship explains almost 80% of the multi-model spread. Combined with contemporary observations of the latest volcanic eruptions (satellite observations and model reanalyzes), this relationship provides a tight constraint on the climate impacts of SSA-SRM. We estimate that a continuous injection of SO2 aerosols into the stratosphere will reduce the global average temperature of continental land surface by 0.47 K per W m-2, impacting both hydrological and carbon cycles. Compared with the unconstrained ESMs ensemble (range from 0.32 to 0.92 K per W m-2 ), our estimate represents much higher confidence ways to assess the impacts of SSA-SRM on the climate while ruling the most extreme projections of the unconstrained ensemble extremely unlikely.

  6. Formation of aqueous-phase secondary organic aerosols from glycolaldehyde and ammonium sulfate/amines: A kinetic and mechanistic study

    NASA Astrophysics Data System (ADS)

    Yi, Yayi; Cao, Zhaoyu; Zhou, Xuehua; Xue, Likun; Wang, Wenxing

    2018-05-01

    Atmospheric particles are largely represented by secondary organic aerosols (SOAs) produced by either aqueous- or gas-phase reactions. Recently, the contribution of the former to SOA formation has been shown to substantially increase and even reach that of the latter, which necessitates in-depth mechanistic investigations. For a deeper understanding of aqueous-phase SOA generation, we herein studied the production of these aerosols in the dark from glycolaldehyde (GAld) and ammonium sulfate (AS)/amines (methylamine (MAm) and glycine (Gly)). UV-vis spectroscopy showed that reaction mixtures featured two main absorption bands (at 209-230 and 280-330 nm) that were attributed to the π-π* transitions of Schiff bases and the n-π* transitions of oligomers produced in the above reactions, respectively. Further studies revealed that irrespective of reactant concentration and pH, all the investigated reactions were well fitted by first-order kinetics and were accelerated by increasing AS/MAm concentrations and solution pH under acidic conditions. The reaction rate constants (determined from changes of absorption at 300 nm) followed the order of Gly (kI = 2.39 × 10-6 s-1) > MAm (kI = 1.19 × 10-6 s-1) > AS (kI = 8.33 × 10-7 s-1) at identical low AS/amine concentrations and were in the order of MAm (kI = 2.5 × 10-6 s-1) > AS (kI = 1.39 × 10-6 s-1) at high AS/MAm concentrations. The main reaction pathways corresponded to the aldol self-condensation of GAld and the nucleophilic attack of AS/amines on GAld followed by dehydration, which afforded imines as the major products. The stronger light absorption of (GAld + Gly) mixtures than that of (glyoxal/methylglyoxal + Gly) mixtures was ascribed to the increased amount of imine- and carbonyl group-containing products produced in the former case.

  7. Aerosols in Alaska

    NASA Astrophysics Data System (ADS)

    Shaw, G. E.; Quinn, P. K.

    2008-12-01

    We are measuring the latitudinal gradient and time variation of aerosol chemical composition across Alaska looking for drifts that might be attributable to alteration in sources and chemical signatures that might allow the identification of sources. Alaska is a very clean region in the sense that the state has a low population density with little polluting emission sources. However it "receives" anthropogenic chemical signals from areas upstream in the westerly's, such as from China, and impacts of Arctic Haze. The region also generates sometime copious amounts of aerosol from wildfire in its boreal forests and condensed compounds from gases emitted by its surrounding oceans. The time series of aerosol composition from this small network goes back about a decade and shows clearly the spring peaking of anthropogenic signal known as Arctic Haze. This signal peaks year after year in spring months at all stations, but is most concentrated at north most stations. On the other hand, a signal indicative of products from the ocean, mainly sulfate with large fractional amounts of MSA peaks, year after year, in the summer and is strongest at the lower latitudes. We have identified not only chemical signatures associated with wildfire smoke from wildfires in Alaska, but the changed signatures from wildfires in far away regions, from Mongolia for example.

  8. 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.

  9. Observations and regional modeling of aerosol optical properties, speciation and size distribution over Northern Africa and western Europe

    NASA Astrophysics Data System (ADS)

    Menut, Laurent; Siour, Guillaume; Mailler, Sylvain; Couvidat, Florian; Bessagnet, Bertrand

    2016-10-01

    The aerosol speciation and size distribution is modeled during the summer 2013 and over a large area encompassing Africa, Mediterranean and western Europe. The modeled aerosol is compared to available measurements such as the AERONET aerosol optical depth (AOD) and aerosol size distribution (ASD) and the EMEP network for surface concentrations of particulate matter PM2.5, PM10 and inorganic species (nitrate, sulfate and ammonium). The main goal of this study is to quantify the model ability to realistically model the speciation and size distribution of the aerosol. Results first showed that the long-range transport pathways are well reproduced and mainly constituted by mineral dust: spatial correlation is ≈ 0.9 for AOD and Ångström exponent, when temporal correlations show that the day-to-day variability is more difficult to reproduce. Over Europe, PM2.5 and PM10 have a mean temporal correlation of ≈ 0.4 but the lowest spatial correlation ( ≈ 0.25 and 0.62, respectively), showing that the fine particles are not well localized or transported. Being short-lived species, the uncertainties on meteorology and emissions induce these lowest scores. However, time series of PM2.5 with the speciation show a good agreement between model and measurements and are useful for discriminating the aerosol composition. Using a classification from the south (Africa) to the north (northern Europe), it is shown that mineral dust relative mass contribution decreases from 50 to 10 % when nitrate increases from 0 to 20 % and all other species, sulfate, sea salt, ammonium, elemental carbon, primary organic matter, are constant. The secondary organic aerosol contribution is between 10 and 20 % with a maximum at the latitude of the Mediterranean Sea (Spanish stations). For inorganic species, it is shown that nitrate, sulfate and ammonium have a mean temporal correlation of 0.25, 0.37 and 0.17, respectively. The spatial correlation is better (0.25, 0.5 and 0.87), showing that the mean

  10. An interfacial mechanism for cloud droplet formation on organic aerosols.

    PubMed

    Ruehl, Christopher R; Davies, James F; Wilson, Kevin R

    2016-03-25

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation. Copyright © 2016, American Association for the Advancement of Science.

  11. Intercomparison of near real time monitors of PM2.5 nitrate and sulfate at the U.S. Environmental Protection Agency Atlanta Supersite

    NASA Astrophysics Data System (ADS)

    Weber, R.; Orsini, D.; Duan, Y.; Baumann, K.; Kiang, C. S.; Chameides, W.; Lee, Y. N.; Brechtel, F.; Klotz, P.; Jongejan, P.; ten Brink, H.; Slanina, J.; Boring, C. B.; Genfa, Z.; Dasgupta, P.; Hering, S.; Stolzenburg, M.; Dutcher, D. D.; Edgerton, E.; Hartsell, B.; Solomon, P.; Tanner, R.

    2003-04-01

    Five new instruments for semicontinuous measurements of fine particle (PM2.5) nitrate and sulfate were deployed in the Atlanta Supersite Experiment during an intensive study in August 1999. The instruments measured bulk aerosol chemical composition at rates ranging from every 5 min to once per hour. The techniques included a filter sampling system with automated water extraction and online ion chromatographic (IC) analysis, two systems that directly collected particles into water for IC analysis, and two techniques that converted aerosol nitrate or sulfate either catalytically or by flash vaporization to gaseous products that were measured with gas analyzers. During the one-month study, 15-min integrated nitrate concentrations were low, ranging from about 0.1 to 3.5 μg m-3 with a mean value of 0.5 μg m-3. Ten-minute integrated sulfate concentrations varied between 0.3 and 40 μg m-3 with a mean of 14 μg m-3. By the end of the one-month study most instruments were in close agreement, with r-squared values between instrument pairs typically ranging from 0.7 to 0.94. Based on comparison between individual semicontinuous devices and 24-hour integrated filter measurements, most instruments were within 20-30% for nitrate (˜0.1-0.2 μg m-3) and 10-15% for sulfate (1-2 μg m-3). Within 95% confidence intervals, linear regression fits suggest that no biases existed between the semicontinuous techniques and the 24-hour integrated filter measurements of nitrate and sulfate;, however, for nitrate, the semicontinuous intercomparisons showed significantly less variability than intercomparisons amongst the 24-hour integrated filters.

  12. Evaluation of Observed and Modelled Aerosol Lifetimes Using Radioactive Tracers of Opportunity and an Ensemble of 19 Global Models

    NASA Technical Reports Server (NTRS)

    Kristiansen, N. I.; Stohl, A.; Olivie, D. J. L.; Croft, B.; Sovde, O. A.; Klein, H.; Christoudias, T.; Kunkel, D.; Leadbetter, S. J.; Lee, Y. H.; hide

    2016-01-01

    Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95

  13. Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols

    NASA Technical Reports Server (NTRS)

    Liao, Hong; Chen, Wei-Ting; Seinfeld, John H.

    2006-01-01

    A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2

  14. 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

  15. Spatial and Temporal Variations of Aerosols Around Beijing in the Summer 2006: Model Evaluation and Source Apportionment

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

    Matsui, Hitoshi; Koike, Makoto; Kondo, Yutaka

    Regional aerosol model calculations were made using the WRF-CMAQ and WRF-chem models to study spatial and temporal variations of aerosols around Beijing, China, in August and September 2006 when the CAREBEIJING-2006 campaign was conducted. Model calculations were compared with in-situ observations made at the urban site in Beijing and suburb site in Yufa, which is 50 km to the south of Beijing. In general, the two model calculations reproduced features of temporal variations of meteorological parameters and concentrations of elemental carbon (EC) and inorganic aerosols (sulfate, ammonium, and nitrate). Spatial distributions of aerosol optical depth (AOD) obtained by the MODISmore » satellite sensor are also generally well reproduced. Model calculations show that enhancements in inorganic aerosol concentrations simultaneously observed at the two sites 4 to 5 times during the one-month observation period were resulted by accumulation of pollutants under stagnated air condition. Because Beijing is located at the north border the high anthropogenic emission area (the Great North China Plain), northward motion of air under the influence of anti-cyclone system caused enhancements in fine aerosol concentrations at Beijing. Concentrations of primary aerosols, such as EC, are found to be generally controlled by emissions within 100 km around Beijing within previous 24 hours. On the other hand, emissions as far as 500 km within previous 3 days were found to affect concentrations of secondary aerosols, such as sulfate. Because of significant contributions of secondary aerosols in Beijing, regional emission controls are found to be necessary for improvement of air quality in Beijing.« less

  16. 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...

  17. Radiative Effects of Atmospheric Aerosols and Impacts on Solar Photovoltaic Electricity Generation

    NASA Astrophysics Data System (ADS)

    Lund, Cory Christopher

    Atmospheric aerosols, by scattering and absorbing radiation, perturbs the Earth's energy balance and reduces the amount of insolation reaching the surface. This dissertation first studies the radiative effects of aerosols by analyzing the internal mixing of various aerosol species. It then examines the aerosol impact on solar PV efficiency and the resulting influence on power systems, including both atmospheric aerosols and deposition of particulate matter (PM) on PV surfaces,. Chapter 2 studies the radiative effects of black carbon (BC), sulfate and organic carbon (OC) internal mixing using a simple radiative transfer model. I find that internal mixing may not result in a positive radiative forcing compared to external mixing, but blocks additional shortwave radiation from the surface, enhancing the surface dimming effect. Chapter 3 estimates the impact of atmospheric aerosol attenuation on solar PV resources in China using a PV performance model with satellite-derived long-term surface irradiance data. I find that, in Eastern China, annual average reductions of solar resources due to aerosols are more than 20%, with comparable impacts to clouds in winter. Improving air quality in China would increase efficiency of solar PV generation. As a positive feedback, increased PV efficiency and deployment would further reduce air pollutant emissions too. Chapter 4 further quantifies the total aerosol impact on PV efficiency globally, including both atmospheric aerosols and the deposition of PM on PV surfaces. I find that, if panels are uncleaned and soiling is only removed by precipitation, deposition of PM accounts for more than two-thirds of the total aerosol impact in most regions. Cleaning the panels, even every few months, would largely increase PV efficiency in resource-abundant regions. Chapter 5 takes a further step to evaluate the impact of PV generation reduction due to aerosols on a projected 2030 power system in China with 400GW of PV. I find that aerosols

  18. Sulfate Formation Enhanced by a Cocktail of High NOx, SO2, Particulate Matter, and Droplet pH during Haze-Fog Events in Megacities in China: An Observation-Based Modeling Investigation.

    PubMed

    Xue, Jian; Yuan, Zibing; Griffith, Stephen M; Yu, Xin; Lau, Alexis K H; Yu, Jian Zhen

    2016-07-19

    In recent years in a few Chinese megacities, fog events lasting one to a few days have been frequently associated with high levels of aerosol loading characterized by high sulfate (as high as 30 μg m(-3)), therefore termed as haze-fog events. The concomitant pollution characteristics include high gas-phase mixing ratios of SO2 (up to 71 ppbv) and NO2 (up to 69 ppbv), high aqueous phase pH (5-6), and smaller fog droplets (as low as 2 μm), resulting from intense emissions from fossil fuel combustion and construction activities supplying abundant Ca(2+). In this work, we use an observation-based model for secondary inorganic aerosols (OBM-SIA) to simulate sulfate formation pathways under conditions of haze-fog events encountered in Chinese megacities. The OBM analysis has identified, at a typical haze-fogwater pH of 5.6, the most important pathway to be oxidation of S(IV) by dissolved NO2, followed by the heterogeneous reaction of SO2 on the aerosol surface. The aqueous phase oxidation of S(IV) by H2O2 is a very minor formation pathway as a result of the high NOx conditions suppressing H2O2 formation. The model results indicate that the unique cocktail of high fogwater pH, high concentrations of NO2, SO2, and PM, and small fog droplets are capable of greatly enhancing sulfate formation. Such haze-fog conditions could lead to rapid sulfate production at night and subsequently high PM2.5 in the morning when the fog evaporates. Sulfate formation is simulated to be highly sensitive to fogwater pH, PM, and precursor gases NO2 and SO2. Such insights on major contributing factors imply that reduction of road dust and NOx emissions could lessen PM2.5 loadings in Chinese megacities during fog events.

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

    NASA Technical Reports Server (NTRS)

    2005-01-01

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

  20. Biochemical and aerosol characterization of ricin for use in non-clinical efficacy studies.

    PubMed

    Barnewall, Roy E; Riffle, Carol G; Jones, Randy L; Guistino, David J; Chou, Richard M; Anderson, Mike S; Vassar, Michelle L; Howland, Carrie A

    2017-12-01

    Ricin toxin may be used as a biological warfare agent and no medical countermeasures are currently available. Here, a well-characterized lot of ricin was aerosolized to determine the delivered dose for future pre-clinical efficacy studies.  Mouse intraperitoneal (IP) median lethal dose (LD 50 ) bioassay measured potency at 5.62 and 7.35 μg/kg on Days 0 and 365, respectively. Additional analyses included total protein, sodium dodecyl sulfate polyacrylamide gel electrophoresis, Western blotting, and rabbit reticulocyte lysate activity assay. The nebulizer aerosol produced consistent concentrations (2.5 × 10 3 , 5.0 × 10 3 , 1.0 × 10 4 , and 1.5 × 10 4  μg/mL) and spray factor values. The aerosol particle size distribution was of sufficient size to deposit in lung alveoli (1.12-1.43 μm). Ricinus communis Agglutinin II (RCA 60), prepared at 19 mg/mL in phosphate-buffered saline, pH 7.8, and stored at -70°C, maintained attributes for toxicity following 1-year storage and aerosolized consistently. © 2017 Wiley Periodicals, Inc.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  2. Aerosol Retrievals Using Channel 1 and 2 AVHRR Data

    NASA Technical Reports Server (NTRS)

    Mishchenko, Michael I.; Geogdzhayev, Igor V.; Cairns, Brian; Rossow, William B.

    1999-01-01

    The effect of tropospheric aerosols on global climate via the direct and indirect radiative forcings is one of the largest remaining uncertainties in climate change studies. Current assessments of the direct aerosol radiative effect mainly focus on sulfate aerosols. It has become clear, however, that other aerosol types like soil dust and smoke from biomass burning are also likely to be important climate forcing factors. The magnitude and even the sign of the climate forcing caused by these aerosol types is still unknown. General circulation models (GCMs) can be used to estimate the climatic effect of the direct radiative forcing by tropospheric and stratospheric aerosols. Aerosol optical properties are already parameterized in the Goddard Institute for Space Studies GCM. Once the global distribution of aerosol properties (optical thickness, size distribution, and chemical composition) is available, the calculation of the direct aerosol forcing is rather straighfforward. However, estimates of the indirect aerosol effect require additional knowledge of the physics and chemistry of aerosol-cloud interactions which are still poorly understood. One of the main objectives of the Global Aerosol Climatology Project, established in 1998 as a joint initiative of NASA's Radiation Science Program and GEWEX, is to infer the global distribution of aerosols, their properties, and their seasonal and interannual variations for the full period of available satellite data. This will be accomplished primarily through a systematic application of multichannel aerosol retrieval algorithms to existing satellite data and advanced 3-dimensional aerosol chemistry/transport models. In this paper we outline the methodology of analyzing channel 1 and 2 AVHRR radiance data over the oceans and describe preliminary retrieval results.

  3. 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.

  4. Quantifying organic aerosol single scattering albedo over tropical biomass burning regions using ground-based observation

    NASA Astrophysics Data System (ADS)

    Chu, J. E.

    2016-12-01

    Despite growing evidence of light-absorbing organic aerosols (OAs), OA light absorption has been poorly understood due to difficulties in aerosol light absorption measurements. In this study, we developed an empirical method to quantify OA single scattering albedo (SSA), the ratio of light scattering to extinction, using ground-based Aerosol Robotic Network (AERONET) observation. Our method includes partitioning fine-mode aerosol optical depth (fAOD) to individual aerosol's optical depth (AOD), separating black carbon and OA absorption aerosol optical depths, and finally binding OA SSA and sulfate+nitrate AOD. Our best estimate of OA SSA over tropical biomass burning region is 0.91 at 550nm with a range of 0.82-0.93. It implies the common OA SSA values of 0.96-1.0 in aerosol CTMs and GCMs significantly underrepresent OA light absorption. Model experiments with prescribed OA SSA showed that the enhanced absorption of solar radiation due to light absorbing OA yields global mean radiative forcing is +0.09 Wm-2 at the TOA, +0.21 Wm-2 at the atmosphere, and -0.12 Wm-2 at the surface. Compared to the previous assessment of OA radiative forcing reported in AeroCom II project, our result indicate that OA light absorption causes TOA radiative forcing by OA to change from negative (i.e., cooling effect) to positive (warming effect).

  5. Molecular characterization of polar organosulfates in secondary organic aerosol from the green leaf volatile 3-Z-hexenal

    NASA Astrophysics Data System (ADS)

    Safi Shalamzari, Mohammad; Kahnt, Ariane; Wang, Wu; Vermeylen, Reinhilde; Kleindienst, Tadeusz; Lewandovski, Michael; Maenhaut, Willy; Claeys, Magda

    2014-05-01

    Much information is available about secondary organic aerosol (SOA) formation from terpenes, including mono- and sesquiterpenes, and isoprene. However, information about SOA formation from green leaf volatiles (GLVs), an important class of biogenic volatile organic compounds, which are emitted when plants are wounded or attacked by insects, is very scarce. In the present study, we provide evidence that 3-Z-hexenal is a potential precursor for SOA through formation of organosulfates. Organosulfate formation from 3-Z-hexenal was studied by conducting smog chamber photooxidation experiments in the presence of NO and acidic ammonium seed aerosol, where OH radicals were generated from the NOx mediated photochemical chain reactions. The focus of the study was on the structural characterization of products, i.e., organosulfates (OSs) with a molecular weight (MW) of 226, which are also present in ambient fine aerosol from a forested site (K puszta, Hungary) at a substantial relative abundance that is comparable to that of the MW 216 isoprene-related OSs. Polar OSs are of climatic relevance because of their capacity to increase the hydrophilic properties of aerosols and as such their cloud-condensation nuclei effects. Two different liquid chromatography (LC) techniques were employed to separate the polar OSs: the first technique uses a reversed-phase trifunctionally bonded C18 stationary phase, whereas the second one is based on ion-pairing C18 LC using dibutylammonium acetate as ion-pairing reagent. With regard to mass spectrometry (MS) techniques, use was made of high-resolution MS to determine the accurate mass (measured mass, 225.00809; elemental composition, C6H9O7S) as well as linear ion trap MS to obtain detailed structural information. The MW 226 OSs were structurally characterized as sulfated derivatives of 3,4-dihydroxyhex-2-enoic acid with the sulfate group positioned at C-3 or C-4. The formation of these OSs is explained through photooxidation in the gas phase

  6. 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.

  7. Analysis and interpretation of lidar observations of the stratospheric aerosol

    NASA Technical Reports Server (NTRS)

    Hamill, P.; Swissler, T. J.; Osborn, M.; Mccormick, M. P.

    1980-01-01

    Data obtained with a 48 in. telescope lidar system are compared with results obtained using a one-dimensional stratospheric aerosol model to analyze various microphysical processes influencing the formation of this aerosol. Special attention is given to the following problems: (1) how lidar data can help determine the composition of the aerosol particles and (2) how the layer corresponds to temperature profile variations. The lidar record during the period 1974 to 1979 shows a considerable decrease of the peak value of the backscatter ratio. Seasonal variations in the aerosol layer and a gradual decrease in stratospheric loading are observed. The aerosol model simulates a background stratospheric aerosol layer, and it predicts stratospheric aerosol concentrations and compositions. Numerical experiments are carried out by using the model and by comparing the theoretical results with the experimentally obtained lidar record. Comparisons show that the backscatter profile is consistent with the composition when the particles are sulfuric acid and water; it is not consistent with an ammonium sulfate composition. It is shown that the backscatter ratio is not sensitive to the composition or stratospheric loading of condensation nuclei such as meteoritic debris.

  8. Quantifying the risks of solid aerosol geoengineering: the role of fundamental material properties

    NASA Astrophysics Data System (ADS)

    Dykema, J. A.; Keutsch, F. N.; Keith, D.

    2017-12-01

    Solid aerosols have been considered as an alternative to sulfate aerosols for solar geoengineering due to their optical and chemical properties, which lead to different and possibly more attractive risk profiles. Solid aerosols can achieve higher solar scattering efficiency due to their higher refractive index, and in some cases may also be less effective absorbers of thermal infrared radiation. The optical properties of solid aerosols are however sensitive functions of the detailed physical properties of solid materials in question. The relevant details include the exact crystalline structure of the aerosols, the physical size of the particles, and interactions with background stratospheric molecular and particulate constituents. In this work, we examine the impact of these detailed physical properties on the radiative properties of calcite (CaCO3) solid aerosols. We examine how crystal morphology, size, chemical reactions, and interaction with background stratospheric aerosol may alter the scattering and absorption properties of calcite aerosols for solar and thermal infrared radiation. For example, in small particles, crystal lattice vibrations associated with the particle surface may lead to substantially different infrared absorption properties than bulk materials. We examine the wavelength dependence of absorption by the particles, which may lead to altered patterns of stratospheric radiative heating and equilibrium temperatures. Such temperature changes can lead to dynamical changes, with consequences for both stratospheric composition and tropospheric climate. We identify important uncertainties in the current state of understanding, investigate risks associated with these uncertainties, and survey potential approaches to quantitatively improving our knowledge of the relevant material properties.

  9. VARIATION OF ELEMENT SPECIATION IN COAL COMBUSTION AEROSOLS WITH PARTICLE SIZE

    EPA Science Inventory

    The speciation of sulfur, iron and key trace elements (Cr, As, Se, Zn) in combustion ash aerosols has been examined as a function of size from experimental combustion units burning Utah and Illinois bituminous coals. Although predominantly present as sulfate, sulfur was also pre...

  10. Future Arctic temperature change resulting from a range of aerosol emissions scenarios

    DOE PAGES

    Wobus, Cameron; Flanner, Mark; Sarofim, Marcus C.; ...

    2016-05-17

    The Arctic temperature response to emissions of aerosols – specifically black carbon (BC), organic carbon (OC), and sulfate – depends on both the sector and the region where these emissions originate. Thus, the net Arctic temperature response to global aerosol emissions reductions will depend strongly on the blend of emissions sources being targeted. We use recently published equilibrium Arctic temperature response factors for BC, OC, and sulfate to estimate the range of present-day and future Arctic temperature changes from seven different aerosol emissions scenarios. Globally, Arctic temperature changes calculated from all of these emissions scenarios indicate that present-day emissions frommore » the domestic and transportation sectors generate the majority of present-day Arctic warming from BC. However, in all of these scenarios, this warming is more than offset by cooling resulting from SO 2 emissions from the energy sector. Thus, long-term climate mitigation strategies that are focused on reducing carbon dioxide (CO 2) emissions from the energy sector could generate short-term, aerosol-induced Arctic warming. As a result, a properly phased approach that targets BC-rich emissions from the transportation sector as well as the domestic sectors in key regions – while simultaneously working toward longer-term goals of CO 2 mitigation – could potentially avoid some amount of short-term Arctic warming.« less

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

  12. 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.

  13. Optical properties of aerosols at Grand Canyon National Park

    NASA Astrophysics Data System (ADS)

    Malm, William C.; Day, Derek E.

    Visibility in the United States is expected to improve over the next few decades because of reduced emissions, especially sulfur dioxide. In the eastern United States, sulfates make up about 60-70% of aerosol extinction, while in the inner mountain west that fraction is only about 30%. In the inner mountain west, carbon aerosols make up about 35% of extinction, while coarse mass contributes between 15 and 25% depending on how absorption is estimated. Although sulfur dioxide emissions are projected to decrease, carbon emissions due to prescribed fire activity will increase by factors of 5-10, and while optical properties of sulfates have been extensively studied, similar properties of carbon and coarse particles are less well understood. The inability to conclusively apportion about 50% of the extinction budget motivated a study to examine aerosol physio-chemical-optical properties at Grand Canyon, Arizona during the months of July and August. Coarse particle mass has usually been assumed to consist primarily of wind-blown dust, with a mass-scattering efficiency between about 0.4 and 0.6 m 2 g -1. Although there were episodes where crustal material made up most of the coarse mass, on the average, organics and crustal material mass were about equal. Furthermore, about one-half of the sampling periods had coarse-mass-scattering efficiencies greater than 0.6 m 2 g -1 and at times coarse-mass-scattering efficiencies were near 1.0 m 2 g -1. It was shown that absorption by coarse- and fine-particle absorption were about equal and that both fine organic and sulfate mass-scattering efficiencies were substantially less than the nominal values of 4.0 and 3.0 m 2 g -1 that have typically been used.

  14. Effect of Sulfate Aerosol Geoengineering on Tropical cyclones

    NASA Astrophysics Data System (ADS)

    Wang, Q.; Moore, J.; Ji, D.

    2017-12-01

    Variation in tropical cyclone (TC) number and intensity is driven in part by changes in the thermodynamics that can be defined by ocean and atmospheric variables. Genesis Potential Index (GPI) and ventilation index (VI) are combinations of potential intensity, vertical wind shear, relative humidity, midlevel entropy deficit, and absolute vorticity that quantify thermodynamic forcing of TC activity under changed climates, and can be calculated from climate model output. Here we use five CMIP5 models running the RCP45 experiment the Geoengineering Model Intercomparison Project (GeoMIP) stratospheric aerosol injection G4 experiment to calculate the two indices over the 2020 to 2069 period. Globally, GPI under G4 is lower than under RCP45, though both have a slight increasing trend. Spatial patterns in the relative effectiveness of geoengineering show reductions in TC in all models in the North Atlantic basin, and northern Indian Ocean in all except NorESM1-M. In the North Pacific, most models also show relative reductions under G4. VI generally coincide with the GPI patterns. Most models project Potential intensity and Relative Humidity to be the dominant variable to affect genesis potential. Changes in vertical wind shear and vorticity are small with scatter across different models and ocean basins. We find that tropopause temperature maybe as important as sea surface temperature in effecting TC genesis. Thus stratospheric aerosol geoengineering impacts on potential intensity and hence TC intensity are reasonably consistent, but probably underestimated by statistical forecasts of Tropical North Atlantic hurricane activity driven by sea surface temperatures alone. However the impacts of geoengineering on other ocean basins are more difficult to assess, and require more complete understanding of their driving parameters under present day climates. Furthermore, the possible effects of stratospheric injection on chemical reactions in the stratosphere, such as ozone, are

  15. Reconstruction of Aerosol Concentration and Composition from Glacier Ice Cores

    NASA Astrophysics Data System (ADS)

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

    2017-04-01

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

  16. Characterization of Individual Aerosol Particles Associated with Clouds (CRYSTAL-FACE)

    NASA Technical Reports Server (NTRS)

    Buseck, Peter R.

    2004-01-01

    The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from near the bottoms and tops of the deep convective systems that lead to the generation of tropical cirrus clouds and to provide insights into the particles that serve as CCN or IN. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to compare the compositions, concentrations, size distributions, shapes, surface coatings, and degrees of aggregation of individual particles from cloud bases and the anvils near the tropopause. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are abundant in in-cloud samples. Cirrus samples contain many H2SO4 droplets, but acidic sulfate particles are rare at the cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. The relatively high extent of ammoniation in the upper troposphere in-cloud samples appears to have resulted from vertical transport by strong convection. The morphology of H2SO4 droplets indicates that they had been at least yartiy ammoniated at the time of collection. They are internally mixed with organic materials, metal sulfates, and solid particles of various compositions. Ammoniation and internal mixing of result in freezing at higher temperature than in pure H2SO4 aerosols. K- and S-bearing organic particles and Si-Al-rich particles are common throughout. Sea salt and mineral dust were incorporated into the convective systems from the cloud bases and worked as ice nuclei while being vertically transported. The nonsulfate particles originated from the lower troposphere and were transported to the upper troposphere and lower stratosphere.

  17. The Influence of Aerosol Hygroscopicity on Precipitation Intensity During a Mesoscale Convective Event

    NASA Astrophysics Data System (ADS)

    Kawecki, Stacey; Steiner, Allison L.

    2018-01-01

    We examine how aerosol composition affects precipitation intensity using the Weather and Research Forecasting Model with Chemistry (version 3.6). By changing the prescribed default hygroscopicity values to updated values from laboratory studies, we test model assumptions about individual component hygroscopicity values of ammonium, sulfate, nitrate, and organic species. We compare a baseline simulation (BASE, using default hygroscopicity values) with four sensitivity simulations (SULF, increasing the sulfate hygroscopicity; ORG, decreasing organic hygroscopicity; SWITCH, using a concentration-dependent hygroscopicity value for ammonium; and ALL, including all three changes) to understand the role of aerosol composition on precipitation during a mesoscale convective system (MCS). Overall, the hygroscopicity changes influence the spatial patterns of precipitation and the intensity. Focusing on the maximum precipitation in the model domain downwind of an urban area, we find that changing the individual component hygroscopicities leads to bulk hygroscopicity changes, especially in the ORG simulation. Reducing bulk hygroscopicity (e.g., ORG simulation) initially causes fewer activated drops, weakened updrafts in the midtroposphere, and increased precipitation from larger hydrometeors. Increasing bulk hygroscopicity (e.g., SULF simulation) simulates more numerous and smaller cloud drops and increases precipitation. In the ALL simulation, a stronger cold pool and downdrafts lead to precipitation suppression later in the MCS evolution. In this downwind region, the combined changes in hygroscopicity (ALL) reduces the overprediction of intense events (>70 mm d-1) and better captures the range of moderate intensity (30-60 mm d-1) events. The results of this single MCS analysis suggest that aerosol composition can play an important role in simulating high-intensity precipitation events.

  18. 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

  19. 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.

  20. Updated aerosol module and its application to simulate secondary organic aerosols during IMPACT campaign May 2008

    NASA Astrophysics Data System (ADS)

    Li, Y. P.; Elbern, H.; Lu, K. D.; Friese, E.; Kiendler-Scharr, A.; Mentel, Th. F.; Wang, X. S.; Wahner, A.; Zhang, Y. H.

    2013-03-01

    The formation of Secondary organic aerosol (SOA) was simulated with the Secondary ORGanic Aerosol Model (SORGAM) by a classical gas-particle partitioning concept, using the two-product model approach, which is widely used in chemical transport models. In this study, we extensively updated SORGAM including three major modifications: firstly, we derived temperature dependence functions of the SOA yields for aromatics and biogenic VOCs, based on recent chamber studies within a sophisticated mathematic optimization framework; secondly, we implemented the SOA formation pathways from photo oxidation (OH initiated) of isoprene; thirdly, we implemented the SOA formation channel from NO3-initiated oxidation of reactive biogenic hydrocarbons (isoprene and monoterpenes). The temperature dependence functions of the SOA yields were validated against available chamber experiments. Moreover, the whole updated SORGAM module was validated against ambient SOA observations represented by the summed oxygenated organic aerosol (OOA) concentrations abstracted from Aerosol Mass Spectrometer (AMS) measurements at a rural site near Rotterdam, the Netherlands, performed during the IMPACT campaign in May 2008. In this case, we embedded both the original and the updated SORGAM module into the EURopean Air pollution and Dispersion-Inverse Model (EURAD-IM), which showed general good agreements with the observed meteorological parameters and several secondary products such as O3, sulfate and nitrate. With the updated SORGAM module, the EURAD-IM model also captured the observed SOA concentrations reasonably well especially those during nighttime. In contrast, the EURAD-IM model before update underestimated the observations by a factor of up to 5. The large improvements of the modeled SOA concentrations by updated SORGAM were attributed to the mentioned three modifications. Embedding the temperature dependence functions of the SOA yields, including the new pathways from isoprene photo oxidations

  1. Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony.

    PubMed

    Hinneburg, Detlef; Renner, Eberhard; Wolke, Ralf

    2009-01-01

    The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of 'free' sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium-sulfate-nitrate-water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10

  2. Lung-clearance mechanisms following inhalation of acid sulfates

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

    Wolff, R.K.; Muggenburg, B.A.; Silbaugh, S.A.

    1982-08-01

    These studies have indicated that acute exposures (1-6 hrs) to sulfuric acid at levels of 0.5 to 1.0 mg/m/sup 3/ can produce impairments in mucous clearance. The impairments can last for up to a week following a 1 hr exposure. These effects and studies by others suggest that high sulfate levels in polluted conditions may be one factor in observed increases of hospital visits for respiratory problems. Long term exposures to elevated levels of sulfates resulting in decreases of clearance could also be an initiating factor in producing chronic obstructive pulmonary disease (COPD). These studies have also shown that itmore » is the larger size fraction (0.6 to 1.0 ..mu..m) of sulfuric acid mist in the urban aerosol which is predominantly responsible for at least the acute effects.« less

  3. Fog and Cloud Induced Aerosol Modification Observed by AERONET

    NASA Technical Reports Server (NTRS)

    Eck, T. F.; Holben, B. N.; Reid, J. S.; Giles, D. M.; Rivas, M. A.; Singh, R. P.; Tripathi, S. N.; Bruegge, C. J.; Platnick, S. E.; Arnold, G. T.; hide

    2011-01-01

    Large fine mode (sub-micron radius) dominated aerosols in size distributions retrieved from AERONET have been observed after fog or low-altitude cloud dissipation events. These column-integrated size distributions have been obtained at several sites in many regions of the world, typically after evaporation of low altitude cloud such as stratocumulus or fog. Retrievals with cloud processed aerosol are sometimes bimodal in the accumulation mode with the larger size mode often approx.0.4 - 0.5 microns radius (volume distribution); the smaller mode typically approx.0.12 to aprrox.0.20 microns may be interstitial aerosol that were not modified by incorporation in droplets and/or aerosol that are less hygroscopic in nature. Bimodal accumulation mode size distributions have often been observed from in situ measurements of aerosols that have interacted with clouds, and AERONET size distribution retrievals made after dissipation of cloud or fog are in good agreement with particle sizes measured by in situ techniques for cloud-processed aerosols. Aerosols of this type and large size range (in lower concentrations) may also be formed by cloud processing in partly cloudy conditions and may contribute to the shoulder of larger size particles in the accumulation mode retrievals, especially in regions where sulfate and other soluble aerosol are a significant component of the total aerosol composition. Observed trends of increasing aerosol optical depth (AOD) as fine mode radius increased suggests higher AOD in the near cloud environment and therefore greater aerosol direct radiative forcing than typically obtained from remote sensing, due to bias towards sampling at low cloud fraction.

  4. Vertically uniform formation pathways of tropospheric sulfate aerosols in East China detected from triple stable oxygen and radiogenic sulfur isotopes

    NASA Astrophysics Data System (ADS)

    Lin, Mang; Biglari, Saman; Zhang, Zhisheng; Crocker, Daniel; Tao, Jun; Su, Binbin; Liu, Lanzhong; Thiemens, Mark H.

    2017-05-01

    Sulfate aerosols (SO42-) in the continental outflow from East China significantly alter the atmospheric sulfur budget across the Pacific Rim, but its formation pathways, especially in the free troposphere (FT), remain poorly understood. Here we analyze stable oxygen (δ17O and δ18O) and radiogenic sulfur (35S) isotopes in SO42- collected at a mountain site in East China to investigate SO42- formation pathways at varying altitudes. We find that Δ17O (=δ17O-0.52 × δ18O) in SO42- is not correlated with 35S (a direct measure of high-altitude air masses). This pattern notably differs from the currently known 35S-Δ17O relation. The result implies that the formation pathway of tropospheric SO42- in East China is vertically uniform, likely due to large emissions and active convection in this region. Our measurements provide unambiguous isotopic constraints for reducing uncertainties in modeling SO42- in the FT over East China, which greatly affects regional climate but current models fail to accurately estimate.

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

    NASA Astrophysics Data System (ADS)

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

    2003-10-01

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

  6. Evolution of Pinatubo aerosol near 19 km altitude over western North America

    NASA Technical Reports Server (NTRS)

    Goodman, Jindra; Snetsinger, K. G.; Pueschel, R. F.; Ferry, G. V.; Verma, S.

    1994-01-01

    Stratospheric aerosols, collected near 19 km altitude on wire impactors over western North America from August 20, 1991 to May 11, 1993, show strong influence of the June 1991 Mt. Pinatubo eruption. Lognormal size distributions are bimodal; each of the mode radii increases and reaches maximum value at about 15 months after eruption. The second (large particle) mode becomes well developed then, and about 40% of the droplets are larger than 0.4 micron radius. The eruption of Mt. Spurr (Alaska) may also have contributed to this. Sulfate mass loading decays exponentially (e-folding 216 days), similar to El Chichon. Silicates are present in samples only immediately after eruption. Two years after eruption, sulfate mass loading is about 0.4 micrograms/cu m, about an order of magnitude higher than background pre-volcanic values. Aerosol size distributions are still bimodal with a very well-defined large droplet mode.

  7. Impacts of Stratospheric Sulfate Geoengineering on PM2.5

    NASA Astrophysics Data System (ADS)

    Robock, A.; Xia, L.; Tilmes, S.; Mills, M. J.; Richter, J.; Kravitz, B.; MacMartin, D.

    2017-12-01

    Particulate matter (PM) includes sulfate, nitrate, organic carbon, elemental carbon, soil dust, and sea salt. The first four components are mostly present near the ground as fine particulate matter with a diameter less than 2.5 µm (PM2.5), and these are of the most concern for human health. PM is efficiently scavenged by precipitation, which is its main atmospheric sink. Here we examine the impact of stratospheric climate engineering on this important pollutant and health risk, taking advantage of two sets of climate model simulations conducted at the National Center for Atmospheric Research. We use the full tropospheric and stratospheric chemistry version of the Community Earth System Model - Community Atmospheric Model 4 (CESM CAM4-chem) with a horizontal resolution of 0.9° x 1.25° lat-lon to simulate a stratospheric sulfate injection climate intervention of 8 Tg SO2 yr-1 combined with an RCP6.0 global warming forcing, the G4 Specified Stratospheric Aerosol (G4SSA) scenario. We also analyze the output from a 20-member ensemble of Community Earth System Model, version 1 with the Whole Atmosphere Community Climate Model as its atmospheric component (CESM1(WACCM)) simulations, also at 0.9° x 1.25° lat-lon resolution, with sulfur dioxide injection at 15°N, 15°S, 30°N, and 30°S varying in time to balance RCP8.5 forcing. While the CESM CAM4-chem model has full tropospheric and stratospheric chemistry, CESM1(WACCM) has an internally generated quasi-biennial oscillation and a comprehensive tropospheric and stratospheric sulfate aerosol treatment, but only stratospheric chemistry. For G4SSA, there are a global temperature reduction of 0.8 K and global averaged precipitation decrease of 3% relative to RCP6.0. The global averaged surface PM2.5 reduces about 1% compared with RCP6.0, mainly over Eurasian and East Asian regions in Northern Hemisphere winter. The PM2.5 concentration change is a combination of effects from tropospheric chemistry and precipitation

  8. A 4-D Climatology (1979-2009) of the Monthly Tropospheric Aerosol Optical Depth Distribution over the Mediterranean Region from a Comparative Evaluation and Blending of Remote Sensing and Model Products

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

    Nabat, P.; Somot, S.; Mallet, M.

    Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multiyear database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, seasalt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDERmore » and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth- Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level- 2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatiotemporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust

  9. Evidence for surface nucleation: efflorescence of ammonium sulfate and coated ammonium sulfate aerosol particles

    NASA Astrophysics Data System (ADS)

    Ciobanu, V. Gabriela; Marcolli, Claudia; Krieger, Ulrich K.; Zuend, Andreas; Peter, Thomas

    2010-05-01

    Aerosol particles are ubiquitous in the atmosphere and can undergo different phase transitions, such as deliquescence and efflorescence. Using optical microscopy, we investigated the efflorescence of ammonium sulfate (AS) in supersaturated AS and 1:1 and 8:1 (by weight) poly(ethylene glycol)-400 (PEG-400)/AS particles, which were deposited as droplets with diameters in the 16 - 35 μm range on a hydrophobically coated slide. The PEG-400/AS particles that are exposed to decreasing relative humidity (RH) exhibit a liquid-liquid phase separation below 90 % RH with the PEG-400 phase surrounding the aqueous AS inner phase (Marcolli and Krieger, 2006; Ciobanu et al., 2009). Pure AS particles effloresced in the RH range from 36.3 to 43.7 % RH, in agreement with literature data (31 - 48 % RH). In contrast, 1:1 PEG-400/AS particles with diameters of the AS phase from 7.2 - 19.2 μm effloresced between 26.8 - 33.9 % RH and 8:1 PEG-400/AS particles with diameters of the AS phase from 1.8 - 7.3 μm between 24.3 - 29.3 % RH. Such low efflorescence relative humidity (ERH) values have never been reached before for AS particles of this size range. We show that neither a potential inhibition of water evaporation via anomalously slow diffusion through the PEG coating, nor the presence of low amounts of PEG-400 in the AS phase, nor different timescales between various experimental techniques could possibly explain the low AS ERH values of PEG-400/AS particles in our setup. High-speed photography of the efflorescence process allowed to monitor the proceeding of the AS crystallization fronts within the particles with millisecond time resolution. The nucleation locations were deduced based on the initial crystals growth locations. Statistical analysis of 31 and 19 efflorescence events for pure AS and 1:1 PEG-400/AS particles, respectively, identified the air/droplet/substrate contact line and the air/droplet interface as preferred nucleation locations in the case of pure AS particles

  10. 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

  11. Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models

    DOE PAGES

    Kristiansen, N. I.; Stohl, A.; Olivie, D. J. L.; ...

    2016-03-17

    Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 ( 137Cs) and xenon-133 ( 133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to theirmore » available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τ e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days

  12. Comparison of heterogeneous photolytic reduction of Hg(II) in the coal fly ashes and synthetic aerosols

    NASA Astrophysics Data System (ADS)

    Tong, Yindong; Eichhorst, Terry; Olson, Michael R.; Rutter, Andrew P.; Shafer, Martin M.; Wang, Xuejun; Schauer, James J.

    2014-03-01

    In this study, we examined the heterogeneous reduction of Hg(II) on the coal fly ash samples and synthetic aerosols under different light conditions in a controlled laboratory reactor. Three types of coal fly ashes were studied: a high carbon fly ash from a stoker boiler, a low carbon/low sulfate fly ash from a pulverized coal combustor burning low sulfur coal, and a high sulfate fly ash from a pulverized coal combustor burning high sulfur coal. The rate of Hg(II) reduction on the three diverse fly ash samples was found to be relatively fast with an average half-life of 1.6 h under clear sky atmospheric conditions (under the irradiance of 1000 W/m2). The reduction rate in the low sulfate/low carbon fly ash was approximately 1.5 times faster than with the other coal fly ash samples. Synthetic aerosols made of carbon black and levoglucosan produced Hg(II) reduction rates similar to coal fly ashes. However, aerosols composed of adipic acid resulted in reduction rates that were 3-5 times faster. The sensitivity of adipic acid reduction to light source wavelength was found to be greater than for the coal fly ash and other synthetic aerosols. Aerosols made from the water extracts of coal fly ash samples produced reduction rates equal to or slightly higher than with the native fly ash suggesting that the soluble components of fly ash play a significant role in the reduction mechanism. The measured reduction rates are likely important in the chemical processing of mercury in power plant plumes and potentially in the atmosphere and should be considered for incorporation in atmospheric transport models that are used to understand the fate of atmospheric mercury.

  13. Do differences in future sulfate emission pathways matter for near-term climate? A case study for the Asian monsoon

    NASA Astrophysics Data System (ADS)

    Bartlett, Rachel E.; Bollasina, Massimo A.; Booth, Ben B. B.; Dunstone, Nick J.; Marenco, Franco; Messori, Gabriele; Bernie, Dan J.

    2018-03-01

    Anthropogenic aerosols could dominate over greenhouse gases in driving near-term hydroclimate change, especially in regions with high present-day aerosol loading such as Asia. Uncertainties in near-future aerosol emissions represent a potentially large, yet unexplored, source of ambiguity in climate projections for the coming decades. We investigated the near-term sensitivity of the Asian summer monsoon to aerosols by means of transient modelling experiments using HadGEM2-ES under two existing climate change mitigation scenarios selected to have similar greenhouse gas forcing, but to span a wide range of plausible global sulfur dioxide emissions. Increased sulfate aerosols, predominantly from East Asian sources, lead to large regional dimming through aerosol-radiation and aerosol-cloud interactions. This results in surface cooling and anomalous anticyclonic flow over land, while abating the western Pacific subtropical high. The East Asian monsoon circulation weakens and precipitation stagnates over Indochina, resembling the observed southern-flood-northern-drought pattern over China. Large-scale circulation adjustments drive suppression of the South Asian monsoon and a westward extension of the Maritime Continent convective region. Remote impacts across the Northern Hemisphere are also generated, including a northwestward shift of West African monsoon rainfall induced by the westward displacement of the Indian Ocean Walker cell, and temperature anomalies in northern midlatitudes linked to propagation of Rossby waves from East Asia. These results indicate that aerosol emissions are a key source of uncertainty in near-term projection of regional and global climate; a careful examination of the uncertainties associated with aerosol pathways in future climate assessments must be highly prioritised.

  14. Host model uncertainties in aerosol radiative forcing estimates: results from the AeroCom prescribed intercomparison study

    NASA Astrophysics Data System (ADS)

    Stier, P.; Schutgens, N. A. J.; Bian, H.; Boucher, O.; Chin, M.; Ghan, S.; Huneeus, N.; Kinne, S.; Lin, G.; Myhre, G.; Penner, J. E.; Randles, C.; Samset, B.; Schulz, M.; Yu, H.; Zhou, C.

    2012-09-01

    Simulated multi-model "diversity" in aerosol direct radiative forcing estimates is often perceived as measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated "host-model uncertainties" are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in nine participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is -4.51 W m-2 and the inter-model standard deviation is 0.70 W m-2, corresponding to a relative standard deviation of 15%. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.26 W m-2, and the standard deviation increases to 1.21 W m-2, corresponding to a significant relative standard deviation of 96%. However, the top-of-atmosphere forcing variability owing to absorption is low, with relative standard deviations of 9% clear-sky and 12% all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the AeroCom Direct Effect experiment, demonstrates that host model uncertainties could explain about half of the overall sulfate forcing diversity of 0.13 W m-2 in the AeroCom Direct Radiative Effect experiment. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host

  15. Host model uncertainties in aerosol radiative forcing estimates: results from the AeroCom Prescribed intercomparison study

    NASA Astrophysics Data System (ADS)

    Stier, P.; Schutgens, N. A. J.; Bellouin, N.; Bian, H.; Boucher, O.; Chin, M.; Ghan, S.; Huneeus, N.; Kinne, S.; Lin, G.; Ma, X.; Myhre, G.; Penner, J. E.; Randles, C. A.; Samset, B.; Schulz, M.; Takemura, T.; Yu, F.; Yu, H.; Zhou, C.

    2013-03-01

    Simulated multi-model "diversity" in aerosol direct radiative forcing estimates is often perceived as a measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated "host-model uncertainties" are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in twelve participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is -4.47 Wm-2 and the inter-model standard deviation is 0.55 Wm-2, corresponding to a relative standard deviation of 12%. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.04 Wm-2, and the standard deviation increases to 1.01 W-2, corresponding to a significant relative standard deviation of 97%. However, the top-of-atmosphere forcing variability owing to absorption (subtracting the scattering case from the case with scattering and absorption) is low, with absolute (relative) standard deviations of 0.45 Wm-2 (8%) clear-sky and 0.62 Wm-2 (11%) all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the AeroCom Direct Effect experiment demonstrates that host model uncertainties could explain about 36% of the overall sulfate forcing diversity of 0.11 Wm-2 in the AeroCom Direct Radiative Effect experiment. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus

  16. Sensitivity of Methane Lifetime and Transport to Sulfate Geoengineering

    NASA Astrophysics Data System (ADS)

    Aquila, V.; Pitari, G.; Tilmes, S.; Cionni, I.; de Luca, N.; Di Genova, G.; Iachetti, D.

    2014-12-01

    Sulfate geoengineering, made by sustained injection of SO2 in the tropical lower stratosphere, may impact the abundance of tropospheric methane through several photochemical mechanisms affecting the tropospheric OH abundance and hence the methane lifetime. Changes of the stratospheric Brewer-Dobson circulation also play a role in the upper tropospheric CH4 transport. Three mechanisms lead to lower OH concentrations and a longer CH4 lifetime: (a) solar radiation scattering increases the planetary albedo and cools the surface, with a tropospheric water vapor decrease as a response to this cooling. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extra-tropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-upper troposphere, thus reducing the amount of NOx and tropospheric O3 production. On the other hand, the tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rates perturbation are strongly latitude dependent, producing a significant change of the pole-to-equator temperature gradient and mean zonal wind distribution, with a net increase of tropical upwelling. A stronger meridional component of the Brewer-Dobson circulation increases the extra-tropical stratosphere to troposphere transport of CH4 poorer air, resulting in less CH4 transported in the UTLS. The net effect on tropospheric OH may be positive or negative depending on the net result of different superimposed species perturbations in the UTLS, i.e. CH4 (negative), NOy and O3 (positive). Three climate-chemistry coupled models are used here to explore the above radiative, chemical and dynamical mechanisms affecting the methane lifetime (ULAQ

  17. Quantifying the Aerosol Semi-Direct Effect in the NASA GEOS-5 AGCM

    NASA Technical Reports Server (NTRS)

    Randles, Cynthia A.; Colarco, Peter R.; daSilva, Arlindo

    2011-01-01

    Aerosols such as black carbon, dust, and some organic carbon species both scatter and absorb incoming solar radiation. This direct aerosol radiative forcing (DARF) redistributes solar energy both by cooling the surface and warming the atmosphere. As a result, these aerosols affect atmospheric stability and cloud cover (the semi-direct effect, or SDE). Furthermore, in regions with persistent high loadings of absorbing aerosols (e.g. Asia), regional circulation patterns may be altered, potentially resulting in changes in precipitation patterns. Here we investigate aerosol-climate coupling using the NASA Goddard Earth Observing System model version 5 (GEOS-5) atmospheric general circulation model (AGCM), in which we have implemented an online version of the Goddard Chemistry, Aerosol, Radiation and Transport (GOCART) model. GOCART includes representations of the sources, sinks, and chemical transformation of externally mixed dust, sea salt, sulfate, and carbonaceous aerosols. We examine a series of free-running ensemble climate simulations of the present-day period (2000-2009) forced by observed sea surface temperatures to determine the impact of aerosols on the model climate. The SDE and response of each simulation is determined by differencing with respect to the control simulation (no aerosol forcing). In a free-running model, any estimate of the SDE includes changes in clouds due both to atmospheric heating from aerosols and changes in circulation. To try and quantify the SDE without these circulation changes we then examine the DARF and SDE in GEOS-5 with prescribed meteorological analyses introduced by the MERRA analysis. By doing so, we are able to examine changes in model clouds that occur on shorter scales (six hours). In the GEOS-5 data assimilation system (DAS), the analysis is defined as the best estimate of the atmospheric state at any given time, and it is determined by optimally combining a first-guess short-term GCM forecast with all available

  18. Comparison of secondary organic aerosol formation from toluene on initially wet and dry ammonium sulfate particles at moderate relative humidity

    NASA Astrophysics Data System (ADS)

    Liu, Tengyu; Huang, Dan Dan; Li, Zijun; Liu, Qianyun; Chan, ManNin; Chan, Chak K.

    2018-04-01

    The formation of secondary organic aerosol (SOA) has been widely studied in the presence of dry seed particles at low relative humidity (RH). At higher RH, initially dry seed particles can exist as wet particles due to water uptake by the seeds as well as the SOA. Here, we investigated the formation of SOA from the photooxidation of toluene using an oxidation flow reactor in the absence of NOx under a range of OH exposures on initially wet or dry ammonium sulfate (AS) seed particles at an RH of 68 %. The ratio of the SOA yield on wet AS seeds to that on dry AS seeds, the relative SOA yield, decreased from 1.31 ± 0.02 at an OH exposure of 4.66 × 1010 molecules cm-3 s to 1.01 ± 0.01 at an OH exposure of 5.28 × 1011 molecules cm-3 s. This decrease may be due to the early deliquescence of initially dry AS seeds after being coated by highly oxidized toluene-derived SOA. SOA formation lowered the deliquescence RH of AS and resulted in the uptake of water by both AS and SOA. Hence the initially dry AS seeds contained aerosol liquid water (ALW) soon after SOA formed, and the SOA yield and ALW approached those of the initially wet AS seeds as OH exposure and ALW increased, especially at high OH exposure. However, a higher oxidation state of the SOA on initially wet AS seeds than that on dry AS seeds was observed at all levels of OH exposure. The difference in mass fractions of m / z 29, 43 and 44 of SOA mass spectra, obtained using an aerosol mass spectrometer (AMS), indicated that SOA formed on initially wet seeds may be enriched in earlier-generation products containing carbonyl functional groups at low OH exposures and later-generation products containing acidic functional groups at high exposures. Our results suggest that inorganic dry seeds become at least partially deliquesced particles during SOA formation and hence that ALW is inevitably involved in the SOA formation at moderate RH. More laboratory experiments conducted with a wide variety of SOA

  19. Simulation of Aerosols and Chemistry with a Unified Global Model

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2004-01-01

    This project is to continue the development of the global simulation capabilities of tropospheric and stratospheric chemistry and aerosols in a unified global model. This is a part of our overall investigation of aerosol-chemistry-climate interaction. In the past year, we have enabled the tropospheric chemistry simulations based on the GEOS-CHEM model, and added stratospheric chemical reactions into the GEOS-CHEM such that a globally unified troposphere-stratosphere chemistry and transport can be simulated consistently without any simplifications. The tropospheric chemical mechanism in the GEOS-CHEM includes 80 species and 150 reactions. 24 tracers are transported, including O3, NOx, total nitrogen (NOy), H2O2, CO, and several types of hydrocarbon. The chemical solver used in the GEOS-CHEM model is a highly accurate sparse-matrix vectorized Gear solver (SMVGEAR). The stratospheric chemical mechanism includes an additional approximately 100 reactions and photolysis processes. Because of the large number of total chemical reactions and photolysis processes and very different photochemical regimes involved in the unified simulation, the model demands significant computer resources that are currently not practical. Therefore, several improvements will be taken, such as massive parallelization, code optimization, or selecting a faster solver. We have also continued aerosol simulation (including sulfate, dust, black carbon, organic carbon, and sea-salt) in the global model to cover most of year 2002. These results have been made available to many groups worldwide and accessible from the website http://code916.gsfc.nasa.gov/People/Chin/aot.html.

  20. A 3-D Model Study of Aerosol Composition and Radiative Forcing in the Asian-Pacific Region

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Torres, Omar; Zhao, Xuepeng; Einaudi, Franco (Technical Monitor)

    2000-01-01

    The Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model will be used in analyzing the aerosol data in the ACE-Asia program. Our objectives are (1) to understand the physical, chemical, and optical properties of aerosol and the processes that control these properties over the Asian-Pacific region, (2) to determine the aerosol radiative forcing over the Asian-Pacific region, and (3) to investigate the interaction between aerosol and tropospheric chemistry. We will present the GOCART aerosol simulations of sulfate, dust, carbonaceous, and sea salt concentrations, their optical thicknesses, and their radiative effects. We will also show the comparisons of model results with data taken from previous field campaigns, ground-based sun photometer measurements, and satellite observations. Finally, we will present our plan for the ACE-Asia study.

  1. Tailoring Meridional and Seasonal Radiative Forcing by Sulfate Aerosol Solar Geoengineering

    NASA Astrophysics Data System (ADS)

    Dai, Z.; Weisenstein, D. K.; Keith, D. W.

    2018-01-01

    We study the possibility of designing solar radiation management schemes to achieve a desired meridional radiative forcing (RF) profile using a two-dimensional chemistry-transport-aerosol model. Varying SO2 or H2SO4 injection latitude, altitude, and season, we compute RF response functions for a broad range of possible injection schemes, finding that linear combinations of these injection cases can roughly achieve RF profiles that have been proposed to accomplish various climate objectives. Globally averaged RF normalized by the sulfur injection rate (the radiative efficacy) is largest for injections at high altitudes, near the equator, and using emission of H2SO4 vapor into an aircraft wake to produce accumulation-mode particles. There is a trade-off between radiative efficacy and control as temporal and spatial control is best achieved with injections at lower altitudes and higher latitudes. These results may inform studies using more realistic models that couple aerosol microphysics, chemistry, and stratospheric dynamics.

  2. Photochemical Formation of Sulfur-Containing Aerosols

    NASA Astrophysics Data System (ADS)

    Kroll, Jay A.; Vaida, Veronica

    2017-06-01

    In order to understand planetary climate systems, modeling the properties of atmospheric aerosols is vital. Aerosol formation plays an important role in planetary climates and is tied to feedback loops that can either warm or cool a planet. Sulfur compounds are known to play an important role in new particle aerosol formation and have been observed in a number of planetary atmospheres throughout our solar system. Our current understanding of sulfur chemistry explains much of what we observe in Earth's atmosphere; however, several discrepancies arise when comparing observations of the Venusian atmosphere with model predictions. This suggests that there are still problems in our fundamental understanding of sulfur chemistry. This is concerning given recent renewed interest in sulfate injections in the stratosphere for solar radiation management geo-engineering schemes. We investigate the role of sunlight as a potential driver of the formation of sulfur-containing aerosols. I will present recent work investigating the generation of large quantities of aerosol from the irradiation of mixtures of SO_2 with water and organic species, using a solar simulator that mimics the light that is available in the Earth's troposphere and the Venusian middle atmosphere. I will present on recent work done in our lab suggesting the formation of sulfurous acid, H_2SO_3, and describe experimental work that supports this proposed mechanism. Additionally I will present on new work showing the highly reactive nature of electronically excited SO_2 with saturated alkane species. The implications of this photochemically induced sulfur aerosol formation in the atmosphere of Earth and other planetary atmospheres will be discussed.

  3. Ozone Depletion at Mid-Latitudes: Coupling of Volcanic Aerosols and Temperature Variability to Anthropogenic Chlorine

    NASA Technical Reports Server (NTRS)

    Solomon, S.; Portmann, R. W.; Garcia, R. R.; Randel, W.; Wu, F.; Nagatani, R.; Gleason, J.; Thomason, L.; Poole, L. R.; McCormick, M. P.

    1998-01-01

    Satellite observations of total ozone at 40-60 deg N are presented from a variety of instruments over the time period 1979-1997. These reveal record low values in 1992-3 (after Pinatubo) followed by partial but incomplete recovery. The largest post-Pinatubo reductions and longer-term trends occur in spring, providing a critical test for chemical theories of ozone depletion. The observations are shown to be consistent with current understanding of the chemistry of ozone depletion when changes in reactive chlorine and stratospheric aerosol abundances are considered along with estimates of wave-driven fluctuations in stratospheric temperatures derived from global temperature analyses. Temperature fluctuations are shown to make significant contributions to model calculated northern mid-latitude ozone depletion due to heterogeneous chlorine activation on liquid sulfate aerosols at temperatures near 200-210 K (depending upon water vapor pressure), particularly after major volcanic eruptions. Future mid-latitude ozone recovery will hence depend not only on chlorine recovery but also on temperature trends and/or variability, volcanic activity, and any trends in stratospheric sulfate aerosol.

  4. Metal and silicate particles including nanoparticles are present in electronic cigarette cartomizer fluid and aerosol.

    PubMed

    Williams, Monique; Villarreal, Amanda; Bozhilov, Krassimir; Lin, Sabrina; Talbot, Prue

    2013-01-01

    Electronic cigarettes (EC) deliver aerosol by heating fluid containing nicotine. Cartomizer EC combine the fluid chamber and heating element in a single unit. Because EC do not burn tobacco, they may be safer than conventional cigarettes. Their use is rapidly increasing worldwide with little prior testing of their aerosol. We tested the hypothesis that EC aerosol contains metals derived from various components in EC. Cartomizer contents and aerosols were analyzed using light and electron microscopy, cytotoxicity testing, x-ray microanalysis, particle counting, and inductively coupled plasma optical emission spectrometry. The filament, a nickel-chromium wire, was coupled to a thicker copper wire coated with silver. The silver coating was sometimes missing. Four tin solder joints attached the wires to each other and coupled the copper/silver wire to the air tube and mouthpiece. All cartomizers had evidence of use before packaging (burn spots on the fibers and electrophoretic movement of fluid in the fibers). Fibers in two cartomizers had green deposits that contained copper. Centrifugation of the fibers produced large pellets containing tin. Tin particles and tin whiskers were identified in cartridge fluid and outer fibers. Cartomizer fluid with tin particles was cytotoxic in assays using human pulmonary fibroblasts. The aerosol contained particles >1 µm comprised of tin, silver, iron, nickel, aluminum, and silicate and nanoparticles (<100 nm) of tin, chromium and nickel. The concentrations of nine of eleven elements in EC aerosol were higher than or equal to the corresponding concentrations in conventional cigarette smoke. Many of the elements identified in EC aerosol are known to cause respiratory distress and disease. The presence of metal and silicate particles in cartomizer aerosol demonstrates the need for improved quality control in EC design and manufacture and studies on how EC aerosol impacts the health of users and bystanders.

  5. Investigating the influences of SO2 and NH3 levels on isoprene-derived secondary organic aerosol formation using conditional sampling approaches

    NASA Astrophysics Data System (ADS)

    Lin, Y.-H.; Knipping, E. M.; Edgerton, E. S.; Shaw, S. L.; Surratt, J. D.

    2013-08-01

    Filter-based PM2.5 samples were chemically analyzed to investigate secondary organic aerosol (SOA) formation from isoprene in a rural atmosphere of the southeastern US influenced by both anthropogenic sulfur dioxide (SO2) and ammonia (NH3) emissions. Daytime PM2.5 samples were collected during summer 2010 using conditional sampling approaches based on pre-defined high and low SO2 or NH3 thresholds. Known molecular-level tracers for isoprene SOA formation, including 2-methylglyceric acid, 3-methyltetrahydrofuran-3,4-diols, 2-methyltetrols, C5-alkene triols, dimers, and organosulfate derivatives, were identified and quantified by gas chromatography coupled to electron ionization mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-Q-TOFMS). Mass concentrations of six isoprene low-NOx SOA tracers contributed to 12-19% of total organic matter (OM) in PM2.5 samples collected during the sampling period, indicating the importance of the hydroxyl radical (OH)-initiated oxidation (so-called photooxidation) of isoprene under low-NOx conditions that lead to SOA formation through reactive uptake of gaseous isoprene epoxydiols (IEPOX) in this region. The contribution of the IEPOX-derived SOA tracers to total organic matter was enhanced by 1.4% (p = 0.012) under high-SO2 sampling scenarios, although only weak associations between aerosol acidity and mass of IEPOX SOA tracers were observed. This suggests that IEPOX-derived SOA formation might be modulated by other factors simultaneously, rather than only aerosol acidity. No clear associations between isoprene SOA formation and high or low NH3 conditional samples were found. Positive correlations between sulfate aerosol loadings and IEPOX-derived SOA tracers for samples collected under all conditions indicates that sulfate aerosol could be a surrogate for surface accommodation in the uptake of IEPOX onto

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  8. Aerosol analysis with the Coastal Zone Color Scanner: a simple method for including multiple scattering effects.

    PubMed

    Gordon, H R; Castaño, D J

    1989-04-01

    For measurement of aerosols over the ocean, the total radiance L(t) backscattered from the top of a stratified atmosphere which contains both stratospheric and tropospheric aerosols of various types has been computed. A similar computation is carried out for an aerosol-free atmosphere yielding the Rayleigh scattered radiance L(r). The difference L(t) - L(r) is shown to be linearly related to the radiance L(as), which the aerosol would produce in the single scattering approximation. This greatly simplifies the application of aerosol models to aerosol analysis by satellite since adding to, or in some way changing, the aerosol model requires no additional multiple scattering computations. In fact, the only multiple computations required for aerosol analysis are those for determining L(r), which can be performed once and for all. The computations are explicitly applied to Band 4 of the CZCS, which, because of its high radiometric sensitivity and excellent calibration, is ideal for studying aerosols over the ocean. Specifically, the constant A in the relationship L(as) = A(-1)(L(t) - L(r)) is given as a function of position along the scan for four typical orbital-solar position scenarios. The computations show that L(as) can be retrieved from L(t) - L(r) with an average error of no more than 5-7% except at the very edges of the scan.

  9. Impact of organic coating on growth of ammonium sulfate particles: light extinction measurements relevant for the direct effect

    NASA Astrophysics Data System (ADS)

    Robinson, C. B.; Zarzana, K. J.; Hasenkopf, C. A.; Tolbert, M. A.

    2012-12-01

    Light extinction by particles is strongly dependent on chemical composition, particle size, and water uptake. Relative humidity affects extinction by causing changes in refractive index and particle size due to hygroscopic growth. The ability of particles to take up water depends on their composition and structure. In both laboratory and field studies, inorganic salts completely covered by an organic coating have been observed. The impact of this coating on water uptake is uncertain, and a systematic study that examines water uptake as a function of relative humidity is highly desirable. These data are critical to evaluate the aerosol direct effect on climate, which is one of the most uncertain aspects of future climate change. In this study, we probe the connection between aerosol composition, size and light extinction directly by measuring fRHext, the ratio of the extinction coefficient for humidified particles to the extinction coefficient for dry particles. Particles were composed of 1,2,6-hexanetriol and ammonium sulfate, a system that forms organic coatings around the inorganic core. A cavity ring-down aerosol extinction spectrometer at 532 nm is used to measure the optical growth factor as a function of relative humidity. The fRHext values for a range of %RH for pure ammonium sulfate, pure 1,2,6-hexanetriol, and ammonium sulfate particles with 1,2,6-hexanetriol coatings were measured. The coated particles are created using a method of liquid-liquid separation, where the particles are exposed to water vapor creating a RH% above their deliquescence RH%. The particles are then dried with a Nafion dryer to a RH% that is below the point where liquid-liquid phase separation is observed, but above the efflorescence RH%. Pure 1,2,6-hexanetriol takes up little water over the observed RH range of 45-65%, and therefore fRHext ~ 1. With pure ammonium sulfate for the same RH% range, the fRHext varied from 1.5 - 2, depending on the RH% and the particle size. For the

  10. FTIR Analysis of Functional Groups in Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Shokri, S. M.; McKenzie, G.; Dransfield, T. J.

    2012-12-01

    Secondary organic aerosols (SOA) are suspensions of particulate matter composed of compounds formed from chemical reactions of organic species in the atmosphere. Atmospheric particulate matter can have impacts on climate, the environment and human health. Standardized techniques to analyze the characteristics and composition of complex secondary organic aerosols are necessary to further investigate the formation of SOA and provide a better understanding of the reaction pathways of organic species in the atmosphere. While Aerosol Mass Spectrometry (AMS) can provide detailed information about the elemental composition of a sample, it reveals little about the chemical moieties which make up the particles. This work probes aerosol particles deposited on Teflon filters using FTIR, based on the protocols of Russell, et al. (Journal of Geophysical Research - Atmospheres, 114, 2009) and the spectral fitting algorithm of Takahama, et al (submitted, 2012). To validate the necessary calibration curves for the analysis of complex samples, primary aerosols of key compounds (e.g., citric acid, ammonium sulfate, sodium benzoate) were generated, and the accumulated masses of the aerosol samples were related to their IR absorption intensity. These validated calibration curves were then used to classify and quantify functional groups in SOA samples generated in chamber studies by MIT's Kroll group. The fitting algorithm currently quantifies the following functionalities: alcohols, alkanes, alkenes, amines, aromatics, carbonyls and carboxylic acids.

  11. Experimental Evidence for Weathering and Martian Sulfate Formation Under Extremely Cold Weather-Limited Environments

    NASA Technical Reports Server (NTRS)

    Niles, Paul B.; Golden, D. C.; Michalski, J.

    2013-01-01

    High resolution photography and spectroscopy of the martian surface (MOC, HiRISE) from orbit has revolutionized our view of Mars with one of the most important discoveries being wide-spread layered sedimentary deposits associated with sulfate minerals across the low to mid latitude regions of Mars [1, 2]. The mechanism for sulfate formation on Mars has been frequently attributed to playa-like evaporative environments under prolonged warm conditions [3]. However, there are several problems with the presence of prolonged surface temperatures on Mars above 273 K during the Noachian including the faint young Sun [4] and the presence of suitable greenhouse gases [5]. The geomorphic evidence for early warm conditions may instead be explained by periodic episodes of warming rather than long term prolonged warm temperatures [6]. An alternate view of the ancient martian climate contends that prolonged warm temperatures were never present and that the atmosphere and climate has been similar to modern conditions throughout most of its history [6]. This view is more consistent with the climate models, but has had a difficult time explaining the sedimentary history of Mars and in particular the presence of sulfate minerals. We suggest here that mixtures of atmospheric aerosols, ice, and dust have the potential for creating small films of cryo-concentrated acidic solutions that may represent an important unexamined environment for understanding weathering processes on Mars [7, 8]. This study seeks to test whether sulfate formation may be possible at temperatures well below 0 C in water limited environments removing the need for prolonged warm periods to form sulfates on early Mars.

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

    NASA Astrophysics Data System (ADS)

    Kim, H.; Zhang, Q.

    2016-12-01

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

  13. North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Roberts, G.; Mauger, G.; Hadley, O.; Ramanathan, V.

    2006-07-01

    Measurements of aerosol and cloud properties in the Eastern Pacific Ocean were taken during an airborne experiment on the University of Wyoming's King Air during April 2004 as part of the Cloud Indirect Forcing Experiment (CIFEX). We observed a wide variety of aerosols, including those of long-range transport from Asia, clean marine boundary layer, and North American emissions. These aerosols, classified by their size distribution and history, were found in stratified layers between 500 to 7500 m above sea level and thicknesses from 100 to 3000 m. A comparison of the aerosol size distributions to measurements of cloud condensation nuclei (CCN) provides insight to the CCN activity of the different aerosol types. The overall ratio of measured to predicted CCN concentration (NCCN) is 0.56 ± 0.41 with a relationship of NCCN,measured = NCCN,predicted0.846±0.002 for 23 research flights and 1884 comparisons. Such a relationship does not accurately describe a CCN closure; however, it is consistent with our measurements that high CCN concentrations are more influenced by anthropogenic sources, which are less CCN active. While other CCN closures have obtained results closer to the expected 1:1 relationship, the different aerosol types (and presumably differences in aerosol chemistry) are responsible for the discrepancy. The measured NCCN at 0.3% supersaturation (Sc) ranged from 20 cm-3 (pristine) to 350 cm-3 (anthropogenic) with an average of 106 ± 54 cm-3 over the experiment. The inferred supersaturation in the clouds sampled during this experiment is ˜0.3%. CCN concentrations of cloud-processed aerosol were well predicted using an ammonium sulfate approximation for Sc ≤ 0.4%. Predicted NCCN for other aerosol types (i.e., Asian and North American aerosols) were high compared to measured values indicating a less CCN active aerosol. This study highlights the importance of chemical effects on CCN measurements and introduces a CCN activation index as a method of

  14. 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

  15. Mechanism and Kinetics of the Formation and Transport of Aerosol Particles in the Lower Stratosphere

    NASA Astrophysics Data System (ADS)

    Aloyan, A. E.; Ermakov, A. N.; Arutyunyan, V. O.

    2018-03-01

    Field and laboratory observation data on aerosol particles in the lower stratosphere are considered. The microphysics of their formation, mechanisms of heterogeneous chemical reactions involving reservoir gases (e.g., HCl, ClONO2, etc.) and their kinetic characteristics are analyzed. A new model of global transport of gaseous and aerosol admixtures in the lower stratosphere is described. The preliminary results from a numerical simulation of the formation of sulfate particles of the Junge layer and particles of polar stratospheric clouds (PSCs, types Ia, Ib, and II) are presented, and their effect on the gas and aerosol composition is analyzed.

  16. Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

    NASA Astrophysics Data System (ADS)

    Russell, L. M.

    2017-12-01

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

  17. Natural Aerosols Explain Seasonal and Spatial Patterns of Southern Ocean Cloud Albedo

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

    McCoy, Daniel; Burrows, Susannah M.; Wood, R.

    2015-07-17

    Small particles called aerosols act as nucleation sites for cloud drop formation, affecting clouds and cloud properties – ultimately influencing the cloud dynamics, lifetime, water path and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations not only affect cloud properties themselves, but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. Here, it is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more thanmore » half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd over regions of high biological activity is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35-45°S) and by organic matter in sea spray aerosol at higher latitudes (45-55°S). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m-2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.« less

  18. Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo

    PubMed Central

    McCoy, Daniel T.; Burrows, Susannah M.; Wood, Robert; Grosvenor, Daniel P.; Elliott, Scott M.; Ma, Po-Lun; Rasch, Phillip J.; Hartmann, Dennis L.

    2015-01-01

    Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties—ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in Nd is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35o to 45oS) and by organic matter in sea spray aerosol at higher latitudes (45o to 55oS). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m–2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere. PMID:26601216

  19. Primary and secondary aerosols in Beijing in winter: sources, variations and processes

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

    2016-07-01

    Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size

  20. The Characteristics of Long-range Transboundary Inorganic Secondary Aerosols in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Kim, Y. J.; Carmichael, G. R.; Woo, J. H.; Qiang, Z.

    2014-12-01

    Recurrent particle matter episodes greatly influence air quality in Northeast Asia. According to many studies, a major reason is long-range transport of air pollutant. Large amount of emission of chemical compounds aggravate air pollution in the region. Emitted air pollutants mainly come from industrialized regions along the East China coast. It can be transported over downwind region by the prevailing westerlies. The long-rang transported fine particle certainly attributes to air quality in downwind region, but there are many unknowns on the quantity, transport pattern, and secondary aerosol production mechanism despite the fact with many studies have been performed. Major contributors of PM2.5 are inorganic secondary aerosols, sulfate, nitrate and ammonium, in Korea. Especially high relative contributions of inorganic secondary aerosols appear for westerly wind cases. The main pathway of production of inorganic secondary aerosols is produced by converting from SO2 and NOx during the long-range transport but the contribution varies dramatically depending on season and wind pattern. Sulfate is consistently the primary contributor of PM2.5 still now but we should more concern nitrate because that NOx emissions of China is increasing steeply since 2000 by leading powerplant, industry, and transport, despite downward trend of SO2. In order to better understand regional air quality modeling of the long-range transport, international study, MICS-Asia phase III, has been initiated with many researchers. We will present chemical characteristics of PM2.5 long-range transport during westerly wind cases focused on secondary aerosol, tracking their transport pattern, and production pathway. Results using CMAQ with the modeling domain covering Northeast and Southeast China, Korea, and Japan with 15km resolution will be discussed.