Science.gov

Sample records for aerosol precursor emissions

  1. Effect of bark beetle infestation on secondary organic aerosol precursor emissions.

    PubMed

    Amin, Hardik; Atkins, P Tyson; Russo, Rachel S; Brown, Aaron W; Sive, Barkley; Hallar, A Gannet; Huff Hartz, Kara E

    2012-06-01

    Bark beetles are a potentially destructive force in forest ecosystems; however, it is not known how insect attacks affect the atmosphere. The emissions of volatile organic compounds (VOCs) were sampled i.) from bark beetle infested and healthy lodgepole pine (Pinus contorta var. latifolia) trees and ii.) from sites with and without active mountain pine beetle infestation. The emissions from the trunk and the canopy were collected via sorbent traps. After collection, the sorbent traps were extracted with hexane, and the extracts were separated and detected using gas chromatography/mass spectroscopy. Canister samples were also collected and analyzed by a multicolumn gas chromatographic system. The samples from bark beetle infested lodgepole pine trees suggest a 5- to 20-fold enhancement in total VOCs emissions. Furthermore, increases in the β-phellandrene emissions correlated with bark beetle infestation. A shift in the type and the quantity of VOC emissions can be used to identify bark beetle infestation but, more importantly, can lead to increases in secondary organic aerosol from these forests as potent SOA precursors are produced. PMID:22545866

  2. Projected response of East Asian summer monsoon system to future reductions in emissions of anthropogenic aerosols and their precursors

    NASA Astrophysics Data System (ADS)

    Wang, Zhili; Zhang, Hua; Zhang, Xiaoye

    2016-09-01

    The response of the East Asian summer monsoon (EASM) system to reductions in emissions of anthropogenic aerosols and their precursors at the end of the twenty-first century projected by Representative Concentration Pathway 4.5 is studied using an aerosol-climate model with aerosol direct, semi-direct, and indirect effects included. Our results show that the global annual mean aerosol effective radiative forcing at the top of the atmosphere (TOA) is +1.45 W m-2 from 2000 to 2100. The summer mean net all-sky shortwave fluxes averaged over the East Asian monsoon region (EAMR) at the TOA and surface increased by +3.9 and +4.0 W m-2, respectively, due to the reductions of aerosols in 2100 relative to 2000. Changes in radiations affect local thermodynamic and dynamic processes and the hydrological cycle. The summer mean surface temperature and pressure averaged over the EAMR are shown to increase by 1.7 K and decreased by 0.3 hPa, respectively, due to the reduced aerosols. The magnitudes of these changes are larger over land than ocean, causing a marked increase in the contrast of land-sea surface temperature and pressure in the EAMR, thus strengthening the EASM. The summer mean southwest and south winds at 850 hPa are enhanced over eastern and southern China and the surrounding oceans, and the East Asian subtropical jet shifted northward due to the decreases of aerosols. These factors also indicate enhanced EASM circulation, which in turn causes a 10 % increase in summer mean precipitation averaged over the EAMR.

  3. Plant and Soil Emissions of Amines and Amino Acids: A Source of Secondary Aerosol Precursors

    NASA Astrophysics Data System (ADS)

    Jackson, M. L.; Doskey, P. V.; Pypker, T. G.

    2011-12-01

    Ammonia (NH3) is the most abundant alkaline gas in the atmosphere and forms secondary aerosol by neutralizing sulfuric and nitric acids that are released during combustion of fossil fuels. Ammonia is primarily emitted by cropping and livestock operations. However, C2 and C3 amines (pKb 3.3-3.4), which are stronger bases than NH3 (pKb 4.7) have been observed in nuclei mode aerosol that is the precursor to secondary aerosol. Mixtures of amines and amino acids have been identified in diverse environments in aerosol, fog water, cloud water, the soluble fraction of precipitation, and in dew. Glycine (pKb 4.2), serine (pKb 4.8) and alanine (pKb 3.7 and 4.1 for the D and L forms, respectively) are typically the most abundant species. The only reported values of gas-phase glycine, serine and alanine were in marine air and ranged from 6-14 pptv. The origin of atmospheric amines and amino acids has not been fully identified, although sources are likely similar to NH3. Nitrate assimilation in plants forms glycine, serine, and L-alanine, while D-alanine is present in bacterial cell walls. Glycine is converted to serine during C3 plant photorespiration, producing CO2 and NH3. Bacteria metabolize glycine and alanine to methylamine and ethylamine via decarboxylation. Likely sources of amino acids are plants and bacteria, thus concentrations near continental sources are likely greater than those measured in marine air. The overall goal of the research is to examine seasonal variations and relationships between the exchange of CO2, NH3, amines, and amino acids with a corn/soybean rotation in the Midwest Corn Belt. The study presents gaseous profiles of organic amine compounds from various species of vegetation using a mist chamber trapping technique and analysis of the derivatized species by high pressure liquid chromatography with fluorescence detection. Amino acid and amine profiles were obtained for red oak (Quercus rubra), sugar maple (Acer saccharinum), white pine (Pinus

  4. Design of Aerosol Coating Reactors: Precursor Injection

    PubMed Central

    Buesser, Beat; Pratsinis, Sotiris E.

    2013-01-01

    Particles are coated with thin shells to facilitate their processing and incorporation into liquid or solid matrixes without altering core particle properties (coloristic, magnetic, etc.). Here, computational fluid and particle dynamics are combined to investigate the geometry of an aerosol reactor for continuous coating of freshly-made titanium dioxide core nanoparticles with nanothin silica shells by injection of hexamethyldisiloxane (HMDSO) vapor downstream of TiO2 particle formation. The focus is on the influence of HMDSO vapor jet number and direction in terms of azimuth and inclination jet angles on process temperature and coated particle characteristics (shell thickness and fraction of uncoated particles). Rapid and homogeneous mixing of core particle aerosol and coating precursor vapor facilitates synthesis of core-shell nanoparticles with uniform shell thickness and high coating efficiency (minimal uncoated core and free coating particles). PMID:23658471

  5. Atmospheric science: marine aerosols and iodine emissions.

    PubMed

    McFiggans, Gordon

    2005-02-10

    O'Dowd et al. describe the formation of marine aerosols from biogenic iodine and the growth of these aerosols into cloud-condensation nuclei (CCN). Based on chamber and modelling results, the authors suggest that biogenic organic iodine compounds emitted from macroalgae may be responsible for coastal particle bursts and that production of these compounds in the open ocean could increase CCN there too. It has since been shown that coastal particles are more likely to be produced from the photooxidation of molecular iodine. Moreover, I contend that open-ocean particle production and cloud enhancement do not result from emissions of organic iodine at atmospheric levels. For iodine particles to affect cloud properties over the remote ocean, an additional source of iodine is necessary as organic precursors cannot be responsible.

  6. Atmospheric science: marine aerosols and iodine emissions.

    PubMed

    McFiggans, Gordon

    2005-02-10

    O'Dowd et al. describe the formation of marine aerosols from biogenic iodine and the growth of these aerosols into cloud-condensation nuclei (CCN). Based on chamber and modelling results, the authors suggest that biogenic organic iodine compounds emitted from macroalgae may be responsible for coastal particle bursts and that production of these compounds in the open ocean could increase CCN there too. It has since been shown that coastal particles are more likely to be produced from the photooxidation of molecular iodine. Moreover, I contend that open-ocean particle production and cloud enhancement do not result from emissions of organic iodine at atmospheric levels. For iodine particles to affect cloud properties over the remote ocean, an additional source of iodine is necessary as organic precursors cannot be responsible. PMID:15703706

  7. Identification of significant precursor gases of secondary organic aerosols from residential wood combustion

    PubMed Central

    Bruns, Emily A.; El Haddad, Imad; Slowik, Jay G.; Kilic, Dogushan; Klein, Felix; Baltensperger, Urs; Prévôt, André S. H.

    2016-01-01

    Organic gases undergoing conversion to form secondary organic aerosol (SOA) during atmospheric aging are largely unidentified, particularly in regions influenced by anthropogenic emissions. SOA dominates the atmospheric organic aerosol burden and this knowledge gap contributes to uncertainties in aerosol effects on climate and human health. Here we characterize primary and aged emissions from residential wood combustion using high resolution mass spectrometry to identify SOA precursors. We determine that SOA precursors traditionally included in models account for only ~3–27% of the observed SOA, whereas for the first time we explain ~84–116% of the SOA by inclusion of non-traditional precursors. Although hundreds of organic gases are emitted during wood combustion, SOA is dominated by the aging products of only 22 compounds. In some cases, oxidation products of phenol, naphthalene and benzene alone comprise up to ~80% of the observed SOA. Identifying the main precursors responsible for SOA formation enables improved model parameterizations and SOA mitigation strategies in regions impacted by residential wood combustion, more productive targets for ambient monitoring programs and future laboratories studies, and links between direct emissions and SOA impacts on climate and health in these regions. PMID:27312480

  8. Identification of significant precursor gases of secondary organic aerosols from residential wood combustion.

    PubMed

    Bruns, Emily A; El Haddad, Imad; Slowik, Jay G; Kilic, Dogushan; Klein, Felix; Baltensperger, Urs; Prévôt, André S H

    2016-01-01

    Organic gases undergoing conversion to form secondary organic aerosol (SOA) during atmospheric aging are largely unidentified, particularly in regions influenced by anthropogenic emissions. SOA dominates the atmospheric organic aerosol burden and this knowledge gap contributes to uncertainties in aerosol effects on climate and human health. Here we characterize primary and aged emissions from residential wood combustion using high resolution mass spectrometry to identify SOA precursors. We determine that SOA precursors traditionally included in models account for only ~3-27% of the observed SOA, whereas for the first time we explain ~84-116% of the SOA by inclusion of non-traditional precursors. Although hundreds of organic gases are emitted during wood combustion, SOA is dominated by the aging products of only 22 compounds. In some cases, oxidation products of phenol, naphthalene and benzene alone comprise up to ~80% of the observed SOA. Identifying the main precursors responsible for SOA formation enables improved model parameterizations and SOA mitigation strategies in regions impacted by residential wood combustion, more productive targets for ambient monitoring programs and future laboratories studies, and links between direct emissions and SOA impacts on climate and health in these regions. PMID:27312480

  9. Identification of significant precursor gases of secondary organic aerosols from residential wood combustion

    NASA Astrophysics Data System (ADS)

    Bruns, Emily A.; El Haddad, Imad; Slowik, Jay G.; Kilic, Dogushan; Klein, Felix; Baltensperger, Urs; Prévôt, André S. H.

    2016-06-01

    Organic gases undergoing conversion to form secondary organic aerosol (SOA) during atmospheric aging are largely unidentified, particularly in regions influenced by anthropogenic emissions. SOA dominates the atmospheric organic aerosol burden and this knowledge gap contributes to uncertainties in aerosol effects on climate and human health. Here we characterize primary and aged emissions from residential wood combustion using high resolution mass spectrometry to identify SOA precursors. We determine that SOA precursors traditionally included in models account for only ~3–27% of the observed SOA, whereas for the first time we explain ~84–116% of the SOA by inclusion of non-traditional precursors. Although hundreds of organic gases are emitted during wood combustion, SOA is dominated by the aging products of only 22 compounds. In some cases, oxidation products of phenol, naphthalene and benzene alone comprise up to ~80% of the observed SOA. Identifying the main precursors responsible for SOA formation enables improved model parameterizations and SOA mitigation strategies in regions impacted by residential wood combustion, more productive targets for ambient monitoring programs and future laboratories studies, and links between direct emissions and SOA impacts on climate and health in these regions.

  10. Secondary aerosol production from agricultural gas precursors

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Studies of air quality indicate that agricultural emissions may impact particulate mass concentrations through both primary and secondary processes. Increasing evidence from both laboratory and field work suggests that not only does ammonia produce secondary particulate matter, but some volatile org...

  11. Can scooter emissions dominate urban organic aerosol?

    NASA Astrophysics Data System (ADS)

    El Haddad, Imad; Platt, Stephen; Huang, Ru-Jin; Zardini, Alessandro; Clairotte, Micheal; Pieber, Simone; Pfaffenberger, Lisa; Fuller, Steve; Hellebust, Stig; Temime-Roussel, Brice; Slowik, Jay; Chirico, Roberto; Kalberer, Markus; Marchand, Nicolas; Dommen, Josef; Astorga, Covadonga; Baltensperger, Urs; Prevot, Andre

    2014-05-01

    In urban areas, where the health impact of pollutants increases due to higher population density, traffic is a major source of ambient organic aerosol (OA). A significant fraction of OA from traffic is secondary, produced via the reaction of exhaust volatile organic compounds (VOCs) with atmospheric oxidants. Secondary OA (SOA) has not been systematically assessed for different vehicles and driving conditions and thus its relative importance compared to directly emitted, primary OA (POA) is unknown, hindering the design of effective vehicle emissions regulations. 2-stroke (2S) scooters are inexpensive and convenient and as such a popular means of transportation globally, particularly in Asia. European regulations for scooters are less stringent than for other vehicles and thus primary particulate emissions and SOA precursor VOCs from 2S engines are estimated to be much higher. Assessing the effects of scooters on public health requires consideration of both POA, and SOA production. Here, we quantify POA emission factors and potential SOA EFs from 2S scooters, and the effect of using aromatic free fuel instead of standard gasoline thereon. During the tests, Euro 1 and Euro 2 2S scooters were run in idle or simulated low power conditions. Emissions from a Euro 2 2S scooter were also sampled during regulatory driving cycles on a chassis dynamometer. Vehicle exhaust was introduced into smog chambers, where POA emission and SOA production were quantified using a high-resolution time-of-flight aerosol mass spectrometer. A high resolution proton transfer time-of-flight mass spectrometer was used to investigate volatile organic compounds and a suite of instruments was utilized to quantify CO, CO2, O3, NOX and total hydrocarbons. We show that the oxidation of VOCs in the exhaust emissions of 2S scooters produce significant SOA, exceeding by up to an order of magnitude POA emissions. By monitoring the decay of VOC precursors, we show that SOA formation from 2S scooter

  12. COS in the stratosphere. [sulfuric acid aerosol precursor

    NASA Technical Reports Server (NTRS)

    Inn, E. C. Y.; Vedder, J. F.; Tyson, B. J.; Ohara, D.

    1979-01-01

    Carbonyl sulfide (COS) has been detected in the stratosphere, and mixing ratio measurements are reported for altitudes of 15.2 to 31.2 km. A large volume, cryogenic sampling system mounted on board a U-2 aircraft has been used for lower stratosphere measurements and a balloon platform for measurement at 31.2 km. These observations and measurements strongly support the concept that stratospheric COS is an important precursor in the formation of sulfuric acid aerosols.

  13. Titan Aerosol Analogs from Aromatic Precursors: Comparisons to Cassini CIRS Observations in the Thermal Infrared

    NASA Technical Reports Server (NTRS)

    Trainer, Melissa G.; Sebree, Joshua A.; Anderson, Carrie M.; Loeffler, Mark J.

    2012-01-01

    Since Cassini's arrival at Titan, ppm levels of benzene (C6H6) as well as large positive ions, which may be polycyclic aromatic hydrocarbons (PAHs). have been detected in the atmosphere. Aromatic molecules. photolytically active in the ultraviolet, may be important in the formation of the organic aerosol comprising the Titan haze layer even when present at low mixing ratios. Yet there have not been laboratory simulations exploring the impact of these molecules as precursors to Titan's organic aerosol. Observations of Titan by the Cassini Composite Infrared Spectrometer (CIRS) in the far-infrared (far-IR) between 560 and 20/cm (approx. 18 to 500 microns) and in the mid-infrared (mid-IR) between 1500 and 600/cm (approx. 7 to 17 microns) have been used to infer the vertical variations of Titan's aerosol from the surface to an altitude of 300 km in the far-IR and between 150 and 350 km in the mid-IR. Titan's aerosol has several observed emission features which cannot be reproduced using currently available optical constants from laboratory-generated Titan aerosol analogs, including a broad far-IR feature centered approximately at 140/cm (71 microns).

  14. Sensitivity of the climate response to regional aerosol emissions

    NASA Astrophysics Data System (ADS)

    Kasoar, Matthew; Voulgarakis, Apostolos; Shindell, Drew; Lamarque, Jean-Francois; Shawki, Dilshad

    2015-04-01

    Short-lived emissions like aerosols and their precursors have inhomogeneous distributions in the atmosphere. As a result, aerosol radiative forcing of the climate is highly uneven, and depends on both the location of emission as well as circulation patterns. Unlike well-mixed greenhouse gases such as CO2, the climate response to aerosol forcing may therefore be very dependent on the source region, and so understanding how the sensitivity of the climate varies with emission and forcing location has implications for the design of policy regarding short-lived climate forcers, as well as for understanding the coupling between radiative forcing and climate response. Using the UK Met Office's HadGEM3 composition-climate model, we have performed a series of experiments to investigate the climate response to aerosol species from different key anthropogenic emission regions, in particular East Asia, South Asia, the USA, and the whole northern mid-latitude band. Recent results from these simulations will be presented, focusing in particular on the patterns of climate forcing due to Asian anthropogenic emissions, and the resulting responses in surface temperature and precipitation. Large-scale circulation changes, driven by regional temperature gradients, are found to play an important role in explaining the observed climate responses, which can be substantial even in in parts of the world far from the location of the forcing. The correct magnitude of aerosol forcing remains, however, one of the greatest uncertainties in our current understanding of anthropogenic influences on climate. Aerosol radiative forcing varies considerably between different composition-climate models, and to explore the implications of this for climate responses we use the GISS Model-E2 and NCAR CESM1 models in addition to HadGEM3. These reveal a remarkable variation in the simulated climate response as a result of differences in the radiative forcing from identical perturbations to regional sulphate

  15. "APEC Blue": Secondary Aerosol Reductions from Emission Controls in Beijing.

    PubMed

    Sun, Yele; Wang, Zifa; Wild, Oliver; Xu, Weiqi; Chen, Chen; Fu, Pingqing; Du, Wei; Zhou, Libo; Zhang, Qi; Han, Tingting; Wang, Qingqing; Pan, Xiaole; Zheng, Haitao; Li, Jie; Guo, Xiaofeng; Liu, Jianguo; Worsnop, Douglas R

    2016-01-01

    China implemented strict emission control measures in Beijing and surrounding regions to ensure good air quality during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. We conducted synchronous aerosol particle measurements with two aerosol mass spectrometers at different heights on a meteorological tower in urban Beijing to investigate the variations in particulate composition, sources and size distributions in response to emission controls. Our results show consistently large reductions in secondary inorganic aerosol (SIA) of 61-67% and 51-57%, and in secondary organic aerosol (SOA) of 55% and 37%, at 260 m and ground level, respectively, during the APEC summit. These changes were mainly caused by large reductions in accumulation mode particles and by suppression of the growth of SIA and SOA by a factor of 2-3, which led to blue sky days during APEC commonly referred to as "APEC Blue". We propose a conceptual framework for the evolution of primary and secondary species and highlight the importance of regional atmospheric transport in the formation of severe pollution episodes in Beijing. Our results indicate that reducing the precursors of secondary aerosol over regional scales is crucial and effective in suppressing the formation of secondary particulates and mitigating PM pollution. PMID:26891104

  16. Aerosol Formation In The Free Troposphere: Aircraft and Laboratory Measurements of Ionic and Gaseous Aerosol Precursors

    NASA Astrophysics Data System (ADS)

    Arnold, F.

    Aerosol formation seems to be very efficient in the upper troposphere (UT) as in- dicated by the frequent presence of numerous very small and therefore very young aerosol particles. Aersosol formation proceeds via nucleation of supersaturated low volatility trace gases (LVG) involving either a homogeneous (HONU) or an ion- induced (INU) mechanism. LVG experience rapid removal by condenstation on prefer- ably pre-existing aerosol particles and therefore LVG must be formed locally in the UT by photochemical conversion of precursor gases. A prominent example is gaseous sulfuric acid which is formed from SO2. This SO2 originates at least in the northern hemisphere mostly from fossil fuel combustion at ground-level and to some part origi- nates also from jet aircraft cruising in the UT. Other conceivable LVG's are low volatil- ity organic compounds. After formation by nucleation new particles may experience condensational growth involving LVG. Alternatively new particles may experience scavenging by attachment to pre-existing larger particles. The LVG-concentration has a strong influence on the growth-rate of new particles and thereby on the possibil- ity for growth to the size of a cloud condensation nucleus. Unfortunately present knowledge on free tropospheric LVG is rather poor. Here will be reported free tropo- spheric aircraft-based measurements of ionic and gaseous aerosol-precursors. These include both measurements in the "background" FT as well as measurements in ex- haust plumes of jet aircraft cruising in the UT. Furthermore accompanying new labo- ratory investigations of INU and measurements behind aircraft jet engines at ground- level will also be adressed.

  17. Measurements of Biogenic and Anthropogenic Ozone and Aerosol Precursors during the SENEX (Southeast Nexus) Campaign 2013

    NASA Astrophysics Data System (ADS)

    Warneke, C.; Trainer, M.; De Gouw, J. A.

    2013-12-01

    Natural emissions of ozone and aerosol precursor gases such as isoprene and monoterpenes are the highest in the southeast of the U.S. and rival those found in tropical forests. In addition, anthropogenic emissions are significant in the Southeast and photochemistry is rapid. The southeast U.S. has not warmed like other parts of the U.S. in response to global climate change, and the temperature anomaly has been suggested to be related to aerosols derived from a combination of anthropogenic and biogenic precursors. The NOAA SENEX aircraft campaign took place in June-July 2013 in the southeast U.S. as part of the Southeast Atmosphere Study (SAS). The NOAA WP-3 aircraft conducted 20 research flights between May 27 and July 10, 2013 based out of Smyrna, TN. To investigate the combination of anthropogenic and biogenic emissions several flights were designed to follow the emissions of cities and power plants as they are transported over forested regions in the Southeast. For example, over-flights of Atlanta, Birmingham and Nashville were performed and the plumes were followed to the forested areas with high isoprene and monoterpene emissions. The same was done for several power plants such as EC Gaston, Scherer and Johnsonville. In the anthropogenic plumes, effects such as the modulation of the isoprene chemistry by high NOx and particle formation and growth were investigated. The same strategy was used for three nighttime flights over Atlanta, Birmingham and the New Madrid and White Bluff power plants. Flights over and downwind of St Lois and Indianapolis were used as a contrast in areas with smaller biogenic emissions. Other anthropogenic emissions sources that were investigated during SENEX included bio refineries, paper mills, coalmines, poultry and pork farming. Also biomass burning emissions were observed during one daytime and one nighttime flight. Another focus of the SENEX campaign was to determine the emissions of natural gas and oil production from the

  18. Dynamic model evaluation for secondary inorganic aerosol and its precursors over Europe between 1990 and 2009

    NASA Astrophysics Data System (ADS)

    Banzhaf, S.; Schaap, M.; Kranenburg, R.; Manders, A. M. M.; Segers, A. J.; Visschedijk, A. J. H.; Denier van der Gon, H. A. C.; Kuenen, J. J. P.; van Meijgaard, E.; van Ulft, L. H.; Cofala, J.; Builtjes, P. J. H.

    2015-04-01

    In this study we present a dynamic model evaluation of chemistry transport model LOTOS-EUROS (LOng Term Ozone Simulation - EURopean Operational Smog) to analyse the ability of the model to reproduce observed non-linear responses to emission changes and interannual variability of secondary inorganic aerosol (SIA) and its precursors over Europe from 1990 to 2009. The 20 year simulation was performed using a consistent set of meteorological data provided by RACMO2 (Regional Atmospheric Climate MOdel). Observations at European rural background sites have been used as a reference for the model evaluation. To ensure the consistency of the used observational data, stringent selection criteria were applied, including a comprehensive visual screening to remove suspicious data from the analysis. The LOTOS-EUROS model was able to capture a large part of the seasonal and interannual variability of SIA and its precursors' concentrations. The dynamic evaluation has shown that the model is able to simulate the declining trends observed for all considered sulfur and nitrogen components following the implementation of emission abatement strategies for SIA precursors over Europe. Both the observations and the model show the largest part of the decline in the 1990s, while smaller concentration changes and an increasing number of non-significant trends are observed and modelled between 2000 and 2009. Furthermore, the results confirm former studies showing that the observed trends in sulfate and total nitrate concentrations from 1990 to 2009 are lower than the trends in precursor emissions and precursor concentrations. The model captured well these non-linear responses to the emission changes. Using the LOTOS-EUROS source apportionment module, trends in the formation efficiency of SIA have been quantified for four European regions. The exercise has revealed a 20-50% more efficient sulfate formation in 2009 compared to 1990 and an up to 20% more efficient nitrate formation per unit

  19. Far-IR Absorption Features of Titan Aerosol Analogs Produced from Aromatic Precursors

    NASA Astrophysics Data System (ADS)

    Sebree, Joshua; Trainer, M. G.; Anderson, C. M.; Loeffler, M. J.

    2012-10-01

    The arrival of the Cassini spacecraft in orbit around Saturn has led to the discovery of benzene (C6H6) at ppm levels, as well as large positive ions in Titan’s atmosphere, tentatively identified as polycyclic aromatic hydrocarbons (PAHs).[1] The presence of aromatic molecules, which are photolytically active in the ultraviolet, may be an important part of the formation of aerosol particles in Titan’s haze layers, even at these low concentrations. To date, there have been no laboratory experiments in the literature exploring this area of study. The analysis of data from the Composite Infrared Spectrometer (CIRS) on-board Cassini has recently uncovered a broad emission feature centered at 140 cm-1 in the far-IR that is unique to the aerosol layers of Titan’s atmosphere.[2] Current optical constants from laboratory-generated aerosol analogs have been unable to reproduce this feature.[3,4] From the broadness of this feature, we speculate that the emission is a blended composite of low-energy vibrations of large molecules such as PAHs and their nitrogen containing counterparts, polycyclic aromatic nitrogen heterocycles (PANHs). We hypothesize that the inclusion of trace amounts of aromatic precursors will aid in the production of these large structures in the laboratory-generated aerosols. In this study, we perform UV irradiation of several aromatic precursors, both with and without nitrogen heteroatoms, to understand their influence on the observable characteristics of the aerosol. Measured optical and chemical properties will be compared to those formed from CH4/N2 mixtures [5,6] as well as to those from Cassini observations. [1] Waite, J. H., et al. (2007) Science 316 870-875. [2] Anderson, C.M, et al. (2011) Icarus 212 762-778. [3] Khare, B.N., et al. (1984) Icarus 60 127-137. [4] Imanaka, H., et al. (2012) Icarus 218 247-261. [5] Trainer, M.G., et al. (2006) PNAS 103 18035-18042. [6] Trainer, M.G., et al. (2012) Astrobiology 12 315-326.

  20. Secondary organic aerosol origin in an urban environment: influence of biogenic and fuel combustion precursors.

    PubMed

    Minguillón, M C; Pérez, N; Marchand, N; Bertrand, A; Temime-Roussel, B; Agrios, K; Szidat, S; van Drooge, B; Sylvestre, A; Alastuey, A; Reche, C; Ripoll, A; Marco, E; Grimalt, J O; Querol, X

    2016-07-18

    Source contributions of organic aerosol (OA) are still not fully understood, especially in terms of quantitative distinction between secondary OA formed from anthropogenic precursors vs. that formed from natural precursors. In order to investigate the OA origin, a field campaign was carried out in Barcelona in summer 2013, including two periods characterized by low and high traffic conditions. Volatile organic compound (VOC) concentrations were higher during the second period, especially aromatic hydrocarbons related to traffic emissions, which showed a marked daily cycle peaking during traffic rush hours, similarly to black carbon (BC) concentrations. Biogenic VOC (BVOC) concentrations showed only minor changes from the low to the high traffic period, and their intra-day variability was related to temperature and solar radiation cycles, although a decrease was observed for monoterpenes during the day. The organic carbon (OC) concentrations increased from the first to the second period, and the fraction of non-fossil OC as determined by (14)C analysis increased from 43% to 54% of the total OC. The combination of (14)C analysis and Aerosol Chemical Speciation Monitor (ACSM) OA source apportionment showed that the fossil OC was mainly secondary (>70%) except for the last sample, when the fossil secondary OC only represented 51% of the total fossil OC. The fraction of non-fossil secondary OC increased from 37% of total secondary OC for the first sample to 60% for the last sample. This enhanced formation of non-fossil secondary OA (SOA) could be attributed to the reaction of BVOC precursors with NOx emitted from road traffic (or from its nocturnal derivative nitrate that enhances night-time semi-volatile oxygenated OA (SV-OOA)), since NO2 concentrations increased from 19 to 42 μg m(-3) from the first to the last sample. PMID:27119273

  1. Simulating the Contributions from Aircraft Emissions to Organic Aerosols Using the Volatility Basis Set

    NASA Astrophysics Data System (ADS)

    Woody, M. C.; Arunachalam, S.; Binkowski, F.; West, J.; Jathar, S.; Robinson, A. L.

    2012-12-01

    Regional air quality studies aimed at quantifying the impacts of aviation emissions to PM2.5 have generally predicted relatively low contributions from organic aerosols. However, recent sampling and smog chamber experiments have suggested that organic aerosols comprise a significant fraction of total PM2.5 formed from aircraft emissions. In this study, the results of aircraft-specific sampling and smog chamber experiments are incorporated into a regional chemical transport model with the volatility basis set and used to predict organic aerosol contributions from aircraft emissions. Contributions of aircraft emissions to primary organic aerosols (POA), secondary organic aerosols (SOA) formed from traditional precursors (e.g. aromatics and long-chain alkanes), and non-traditional SOA formed from unidentified precursors previously unaccounted for in air quality models are modeled using the volatility basis set approach in CMAQ v4.7.1. The model includes oxidation reactions of traditional SOA (both biogenic and anthropogenic) and non-traditional SOA precursors (specific to aircraft emissions) with OH to produce products of lower volatility. Non-traditional SOA yields and precursor emission estimates for idle and non-idle aircraft activities are based on sampling and smog chamber experiments. This model predicts the organic aerosol and total PM2.5 concentrations formed from aircraft emissions due to landing and takeoff activities at the Hartsfield-Jackson International Airport in Atlanta during January and July, 2002. Overall model results are compared against monitoring data in the region to determine the impacts of using the volatility basis set on CMAQ model performance.

  2. Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

    NASA Astrophysics Data System (ADS)

    Jathar, Shantanu Hemant

    -only model suggested that differences in the volatility of the precursors were able to explain most of the variability observed in the SOA formation. For aircraft exhaust, the previous methods to simulate SOA formation from SVOC and IVOC performed poorly. A more physically-realistic modeling framework was developed, which was then used to show that SOA formation from aircraft exhaust was (a) higher for petroleum-based than synthetically derived jet fuel and (b) higher at lower engine loads and vice versa. All of the SOA data from combustion emissions experiments were used to determine source-specific parameterizations to model SOA formation from SVOC, IVOC and other unspeciated emissions. The new parameterizations were used to investigate their influence on the OA budget in the United States. Combustion sources were estimated to emit about 2.61 Tg yr-1 of SVOC, 1VOC and other unspeciated emissions (sixth of the total anthropogenic organic emissions), which are predicted to double SOA production from combustion sources in the United States. The contribution of SVOC and IVOC emissions to global SOA formation was assessed using a global climate model. Simulations were performed using a modified version of GISS GCM 11'. The modified model predicted that SVOC and IVOC contributed to half of the OA mass in the atmosphere. Their inclusion improved OA model-measurement comparisons for absolute concentrations, POA-SOA split and volatility (gas-particle partitioning) globally suggesting that atmospheric models need to incorporate SOA formation from SVOC and IVOC if they are to reasonably predict the abundance and properties of aerosols. This thesis demonstrates that SVOC/IVOC and possibly other unspeciated organics emitted by combustion sources are very important precursors of SOA and potentially large contributors to the atmospheric aerosol mass. Models used for research and policy applications need to represent them to improve model-predictions of aerosols on climate and health

  3. Future Projections of Aerosol Optical Depth, Radiative Forcing, and Climate Response Due to Declining Aerosol Emissions in the Representative Concentration Pathways

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Mauzerall, D. L.; Horowitz, L. W.; Naik, V.

    2014-12-01

    It is widely expected that global emissions of atmospheric aerosols and their precursors will decrease strongly throughout the remainder of the 21st century, due to emission reduction policies enacted based on human health concerns. However, the resulting decrease in atmospheric aerosol burden will have unintended climate consequences. Since aerosols generally exert a net cooling influence on the climate, their removal will lead to an unmasking of global warming as well as other changes to the climate system. Aerosol and precursor global emissions decrease by as much as 80% by the year 2100, according to projections in four Representative Concentration Pathway (RCP) scenarios. We use the Geophysical Fluid Dynamics Laboratory Climate Model version 3 (GFDL CM3) to simulate future climate over the 21st century with and without aerosol emission changes projected by the RCPs in order to isolate the radiative forcing and climate response due to the aerosol reductions. We find that up to 1 W m-2 of radiative forcing may be unmasked globally by 2100 due to reductions in aerosol and precursor emissions, leading to average global temperature increases up to 1 K and global precipitation rate increases up to 0.09 mm d-1 (3%). Regionally and locally, climate impacts are much larger, as RCP8.5 projects a 2.1 K warming over China, Japan, and Korea due to reduced aerosol emissions. Our results highlight the importance of crafting emissions control policies with both climate and air pollution benefits in mind. The expected unmasking of additional global warming from aerosol reductions highlights the importance of robust greenhouse gas mitigation policies and may require more aggressive policies than anticipated.

  4. Is benzene a precursor for secondary organic aerosol?

    PubMed

    Martín-Reviejo, Montserrat; Wirtz, Klaus

    2005-02-15

    It is currently assumed that benzene contributes only negligibly to secondary organic aerosol formation in the atmosphere. Our understanding of the capacity of benzene to generate secondary aerosols is based on the work of Izumi and Fukuyama (Atmos. Environ. 1990, 24A, 1433) in which two photosmog experiments with benzene in the presence of NOx were performed and no particle formation was observed. In contrast to the observations of Izumi and Fukuyama, experiments performed in the EUPHORE large outdoor simulation chamber have clearly shown aerosol formation during the photochemical oxidation of benzene in various NOx regimes. The maximum aerosol yields of 8-25% on a mass basis are comparable to yields obtained during the photochemical oxidation of other aromatic compounds under similar conditions. In addition, a density of 1.35+/-0.04 g/cm3 for the secondary organic aerosol from the benzene photochemical oxidation in the presence of NOx has been determined through the simultaneous measurement of aerosol volume and aerosol mass using two independent measurement techniques. Comparing the results in the present work with previous findings underscores the strong influence that the NOx content in the system has on aerosol formation during the photochemical oxidation of aromatic hydrocarbons and the importance of performing experiments with NOx concentrations relevant to the atmosphere.

  5. The impact of residential combustion emissions on atmospheric aerosol, human health and climate

    NASA Astrophysics Data System (ADS)

    Butt, E. W.; Rap, A.; Schmidt, A.; Reddington, C.; Scott, C.; Pringle, K.; Woodhouse, M.; Spracklen, D. V.

    2015-12-01

    Combustion of fuels in the residential sector for cooking and heating, results in the emission of aerosol and aerosol precursors that effect air quality, human health and climate. Residential emissions are dominated by the combustion of solid fuels which are the primary energy source for nearly half the world's population. Despite this importance, residential emissions are poorly quantified, as are their impacts on air quality and climate. We used a global aerosol microphysics model to simulate the impact of residential emissions on atmospheric aerosol in the year 2000, and evaluated simulated concentrations against surface observations of aerosol mass and number. Residential emissions make the largest contributions to surface particulate matter (PM2.5) concentrations in East Asia, South Asia and Eastern Europe, matching regions of greatest emissions. We used concentration response functions to estimate a global annual excess adult (> 30 years of age) premature mortality due to residential emissions of between 113, 300 and 827, 000 when uncertainties in both residential emissions and health effects of PM2.5 were accounted for. Premature mortality was greatest in Asia, with China and India accounting for 50% of simulated global excess mortality. Using an offline radiative transfer model, we show that residential emissions exerted a global annual mean direct radiative effect of between -66 mW m-2 and +21 mW m-2, accounting for uncertainties in emissions flux and assumed ratio of carbonaceous and sulphur emissions. Residential emissions exerted a negative global annual mean first aerosol indirect effect of between -52 mW m-2 and -16 mW m-2, which was found to be sensitive to the assumed size distribution of carbonaceous emissions. Our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

  6. Marine aerosol formation from biogenic iodine emissions.

    PubMed

    O'Dowd, Colin D; Jimenez, Jose L; Bahreini, Roya; Flagan, Richard C; Seinfeld, John H; Hämeri, Kaarle; Pirjola, Liisa; Kulmala, Markku; Jennings, S Gerard; Hoffmann, Thorsten

    2002-06-01

    The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing.

  7. Marine aerosol formation from biogenic iodine emissions.

    PubMed

    O'Dowd, Colin D; Jimenez, Jose L; Bahreini, Roya; Flagan, Richard C; Seinfeld, John H; Hämeri, Kaarle; Pirjola, Liisa; Kulmala, Markku; Jennings, S Gerard; Hoffmann, Thorsten

    2002-06-01

    The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing. PMID:12050661

  8. Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor.

    PubMed

    Tkacik, Daniel S; Lambe, Andrew T; Jathar, Shantanu; Li, Xiang; Presto, Albert A; Zhao, Yunliang; Blake, Donald; Meinardi, Simone; Jayne, John T; Croteau, Philip L; Robinson, Allen L

    2014-10-01

    Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

  9. Secondary Aerosol: Precursors and Formation Mechanisms. Technical Report on Grant

    SciTech Connect

    Weinstein-Lloyd, Judith B

    2009-05-04

    This project focused on studying trace gases that participate in chemical reactions that form atmospheric aerosols. Ammonium sulfate is a major constituent of these tiny particles, and one important pathway to sulfate formation is oxidation of dissolved sulfur dioxide by hydrogen peroxide in cloud, fog and rainwater. Sulfate aerosols influence the number and size of cloud droplets, and since these factors determine cloud radiative properties, sulfate aerosols also influence climate. Peroxide measurements, in conjunction with those of other gaseous species, can used to distinguish the contribution of in-cloud reaction to new sulfate aerosol formation from gas-phase nucleation reactions. This will lead to more reliable global climate models. We constructed and tested a new 4-channel fluorescence detector for airborne detection of peroxides. We integrated the instrument on the G-1 in January, 2006 and took a test flight in anticipation of the MAX-Mex field program, where we planned to fly under pressurized conditions for the first time. We participated in the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) - Megacity Aerosol EXperiment Mexico City (MAX-Mex) field measurement campaign. Peroxide instrumentation was deployed on the DOE G-1 research aircraft based in Veracruz, and at the surface site at Tecamac University.

  10. The impact of residential combustion emissions on atmospheric aerosol, human health and climate

    NASA Astrophysics Data System (ADS)

    Butt, E. W.; Rap, A.; Schmidt, A.; Scott, C. E.; Pringle, K. J.; Reddington, C. L.; Richards, N. A. D.; Woodhouse, M. T.; Ramirez-Villegas, J.; Yang, H.; Vakkari, V.; Stone, E. A.; Rupakheti, M.; Praveen, P. S.; van Zyl, P. G.; Beukes, J. P.; Josipovic, M.; Mitchell, E. J. S.; Sallu, S. M.; Forster, P. M.; Spracklen, D. V.

    2015-07-01

    Combustion of fuels in the residential sector for cooking and heating, results in the emission of aerosol and aerosol precursors impacting air quality, human health and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the uncertainties in the impact of residential fuel combustion on atmospheric aerosol. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia and Eastern Europe. We use a concentration response function to estimate the health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (> 30 years of age) premature mortality of 308 000 (113 300-497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000-827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect of between -66 and +21 mW m-2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between -52 and -16 mW m-2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential

  11. Aerosol emission in a road tunnel

    NASA Astrophysics Data System (ADS)

    Weingartner, E.; Keller, C.; Stahel, W. A.; Burtscher, H.; Baltensperger, U.

    Continuous measurements of aerosol emissions were performed within the scope of emission measurements in the Gubrist tunnel, a 3250 m long freeway tunnel near Zürich, Switzerland, from 20 September to 26 September 1993. The particles in the respirable size range ( d < 3 μm) were found to be mainly tail pipe emissions with very small amount of tire wear and road dust. The calculated PM 3 emission factor for diesel engines was about 310 mg km -1, where the main part (63%) of the diesel vehicles were heavy-duty vehicles. Thirty-one percent of the PM 3 emissions from diesel vehicles were black carbon and 0.86% particle bound PAR Due to the high fraction emitted by diesel engines the contribution of gasoline engines could not be evaluated by the statistical model. During their residence time in the tunnel the particles undergo significant changes, resulting in a more compact structure. It is concluded that this is mainly due to adsorption of volatile material from the gas phase to the particle surface.

  12. Secondary organic aerosol formation from gasoline passenger vehicle emissions investigated in a smog chamber

    NASA Astrophysics Data System (ADS)

    Nordin, E. Z.; Eriksson, A. C.; Roldin, P.; Nilsson, P. T.; Carlsson, J. E.; Kajos, M. K.; Hellén, H.; Wittbom, C.; Rissler, J.; Löndahl, J.; Swietlicki, E.; Svenningsson, B.; Bohgard, M.; Kulmala, M.; Hallquist, M.; Pagels, J.

    2012-12-01

    Gasoline vehicles have elevated emissions of volatile organic compounds during cold starts and idling and have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA formation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from one Euro II, one Euro III and one Euro IV passenger vehicles were investigated using photo-oxidation experiments in a 6 m3 smog chamber. The experiments were carried out at atmospherically relevant organic aerosol mass concentrations. The characterization methods included a high resolution aerosol mass spectrometer and a proton transfer mass spectrometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the organic aerosol mass spectra downwind urban areas. After 4 h aging the formed SOA was 1-2 orders of magnitude higher than the Primary OA emissions. The SOA mass spectrum from a relevant mixture of traditional light aromatic precursors gave f43 (mass fraction at m/z = 4 3) approximately two times higher than to the gasoline SOA. However O : C and H : C ratios were similar for the two cases. Classical C6-C9 light aromatic precursors were responsible for up to 60% of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher order aromatic compounds such as C10, C11 light aromatics, naphthalene and methyl-naphthalenes.

  13. Secondary organic aerosol formation from idling gasoline passenger vehicle emissions investigated in a smog chamber

    NASA Astrophysics Data System (ADS)

    Nordin, E. Z.; Eriksson, A. C.; Roldin, P.; Nilsson, P. T.; Carlsson, J. E.; Kajos, M. K.; Hellén, H.; Wittbom, C.; Rissler, J.; Löndahl, J.; Swietlicki, E.; Svenningsson, B.; Bohgard, M.; Kulmala, M.; Hallquist, M.; Pagels, J. H.

    2013-06-01

    Gasoline vehicles have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA formation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from three passenger vehicles (EURO2-EURO4) were investigated with photo-oxidation experiments in a 6 m3 smog chamber. The experiments were carried out down to atmospherically relevant organic aerosol mass concentrations. The characterization instruments included a high-resolution aerosol mass spectrometer and a proton transfer mass spectrometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the organic aerosol mass spectra downwind of urban areas. After a cumulative OH exposure of ~5 × 106 cm-3 h, the formed SOA was 1-2 orders of magnitude higher than the primary OA emissions. The SOA mass spectrum from a relevant mixture of traditional light aromatic precursors gave f43 (mass fraction at m/z = 43), approximately two times higher than to the gasoline SOA. However O : C and H : C ratios were similar for the two cases. Classical C6-C9 light aromatic precursors were responsible for up to 60% of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher-order aromatic compounds such as C10 and C11 light aromatics, naphthalene and methyl-naphthalenes. We conclude that approaches using only light aromatic precursors give an incomplete picture of the magnitude of SOA formation and the SOA composition from gasoline exhaust.

  14. Quantifying the effect of organic aerosol aging and intermediate-volatility emissions on regional-scale aerosol pollution in China

    NASA Astrophysics Data System (ADS)

    Zhao, Bin; Wang, Shuxiao; Donahue, Neil M.; Jathar, Shantanu H.; Huang, Xiaofeng; Wu, Wenjing; Hao, Jiming; Robinson, Allen L.

    2016-06-01

    Secondary organic aerosol (SOA) is one of the least understood constituents of fine particles; current widely-used models cannot predict its loadings or oxidation state. Recent laboratory experiments demonstrated the importance of several new processes, including aging of SOA from traditional precursors, aging of primary organic aerosol (POA), and photo-oxidation of intermediate volatility organic compounds (IVOCs). However, evaluating the effect of these processes in the real atmosphere is challenging. Most models used in previous studies are over-simplified and some key reaction trajectories are not captured, and model parameters are usually phenomenological and lack experimental constraints. Here we comprehensively assess the effect of organic aerosol (OA) aging and intermediate-volatility emissions on regional-scale OA pollution with a state-of-the-art model framework and experimentally constrained parameters. We find that OA aging and intermediate-volatility emissions together increase OA and SOA concentrations in Eastern China by about 40% and a factor of 10, respectively, thereby improving model-measurement agreement significantly. POA and IVOCs both constitute over 40% of OA concentrations, and IVOCs constitute over half of SOA concentrations; this differs significantly from previous apportionment of SOA sources. This study facilitates an improved estimate of aerosol-induced climate and health impacts, and implies a shift from current fine-particle control policies.

  15. Quantifying the effect of organic aerosol aging and intermediate-volatility emissions on regional-scale aerosol pollution in China.

    PubMed

    Zhao, Bin; Wang, Shuxiao; Donahue, Neil M; Jathar, Shantanu H; Huang, Xiaofeng; Wu, Wenjing; Hao, Jiming; Robinson, Allen L

    2016-01-01

    Secondary organic aerosol (SOA) is one of the least understood constituents of fine particles; current widely-used models cannot predict its loadings or oxidation state. Recent laboratory experiments demonstrated the importance of several new processes, including aging of SOA from traditional precursors, aging of primary organic aerosol (POA), and photo-oxidation of intermediate volatility organic compounds (IVOCs). However, evaluating the effect of these processes in the real atmosphere is challenging. Most models used in previous studies are over-simplified and some key reaction trajectories are not captured, and model parameters are usually phenomenological and lack experimental constraints. Here we comprehensively assess the effect of organic aerosol (OA) aging and intermediate-volatility emissions on regional-scale OA pollution with a state-of-the-art model framework and experimentally constrained parameters. We find that OA aging and intermediate-volatility emissions together increase OA and SOA concentrations in Eastern China by about 40% and a factor of 10, respectively, thereby improving model-measurement agreement significantly. POA and IVOCs both constitute over 40% of OA concentrations, and IVOCs constitute over half of SOA concentrations; this differs significantly from previous apportionment of SOA sources. This study facilitates an improved estimate of aerosol-induced climate and health impacts, and implies a shift from current fine-particle control policies. PMID:27350423

  16. Quantifying the effect of organic aerosol aging and intermediate-volatility emissions on regional-scale aerosol pollution in China

    PubMed Central

    Zhao, Bin; Wang, Shuxiao; Donahue, Neil M.; Jathar, Shantanu H.; Huang, Xiaofeng; Wu, Wenjing; Hao, Jiming; Robinson, Allen L.

    2016-01-01

    Secondary organic aerosol (SOA) is one of the least understood constituents of fine particles; current widely-used models cannot predict its loadings or oxidation state. Recent laboratory experiments demonstrated the importance of several new processes, including aging of SOA from traditional precursors, aging of primary organic aerosol (POA), and photo-oxidation of intermediate volatility organic compounds (IVOCs). However, evaluating the effect of these processes in the real atmosphere is challenging. Most models used in previous studies are over-simplified and some key reaction trajectories are not captured, and model parameters are usually phenomenological and lack experimental constraints. Here we comprehensively assess the effect of organic aerosol (OA) aging and intermediate-volatility emissions on regional-scale OA pollution with a state-of-the-art model framework and experimentally constrained parameters. We find that OA aging and intermediate-volatility emissions together increase OA and SOA concentrations in Eastern China by about 40% and a factor of 10, respectively, thereby improving model-measurement agreement significantly. POA and IVOCs both constitute over 40% of OA concentrations, and IVOCs constitute over half of SOA concentrations; this differs significantly from previous apportionment of SOA sources. This study facilitates an improved estimate of aerosol-induced climate and health impacts, and implies a shift from current fine-particle control policies. PMID:27350423

  17. Spectroscopic studies of homogeneous precursors to atmospheric acids and aerosols

    SciTech Connect

    Leopold, K.R.; Canagaratna, M.; Phillips, J.A.; Goodfriend, H.

    1996-10-01

    A detailed understanding of the nucleation and growth of atmospheric particulates is benefitted by precise knowledge of the structure and energetics of small molecular aggregates. We present the results of microwave spectroscopic characterization of three binary clusters which are potential precursors in such processes: H{sub 2}O-SO{sub 3}, H{sub 3}N-SO{sub 3}, and H{sub 2}O-HNO{sub 3}. In addition to providing detailed structural information, we describe the nature of the bonding in these systems. For the SO{sub 3} complexes, the intermolecular interaction is weaker than a chemical bond, but stronger than a van der Waals bond. We discuss how this feature of these systems renders their structure and energetics unusually sensitive to the presence of additional binding partners, and infer that an accurate molecular-level description of cluster growth will need to account for this effect. The results are compared with published high level ab initio calculations for all three systems.

  18. The "Parade Blue": effects of short-term emission control on aerosol chemistry.

    PubMed

    Li, Haiyan; Zhang, Qiang; Duan, Fengkui; Zheng, Bo; He, Kebin

    2016-07-18

    The strict control on emissions implemented in Beijing, China, during the 2015 China Victory Day Parade (V-day Parade) to commemorate the 70(th) Anniversary of Victory in World War II, provided a good opportunity to investigate the relationship between emission sources and aerosol chemistry in a heavily polluted megacity. From August 11 to September 3, 2015, an Aerosol Chemical Speciation Monitor was deployed in urban Beijing, together with other collocated instruments, for the real-time measurement of submicron aerosol characteristics. The average PM1 mass concentration was 11.3 (±6.7) μg m(-3) during the V-day Parade, 63.5% lower than that before the V-day Parade. Differently to the relatively smaller decrease of organics (53%), secondary inorganic aerosols (sulfate, nitrate and ammonium) showed significant reductions of 65-78% during the V-day Parade. According to the positive matrix factorization results, primary organic aerosol (POA) from traffic and cooking emissions decreased by 41.5% during the parade, whereas secondary organic aerosol (SOA) presented a much greater reduction (59%). The net effectiveness of emission control measures was investigated further under comparable weather conditions before and during the parade. By excluding the effects of meteorological parameters, the total PM1 mass was reduced by 52-57% because of the emission controls. Although the mass concentrations of aerosol species were reduced substantially, the PM1 bulk composition was similar before and during the control period as a consequence of synergetic control of various precursors. The emission restrictions also suppressed the secondary formation processes of sulfate and nitrate, indicated by the substantially reduced SOR and NOR (molar ratios of sulfate or nitrate to the sums of the sulfate and SO2 or nitrate and NO2) during the event. The study also explored the influence of emission controls on the evolution of organic aerosol using the mass ratios of SOA/POA and oxygen

  19. The impact of residential combustion emissions on atmospheric aerosol, human health, and climate

    NASA Astrophysics Data System (ADS)

    Butt, E. W.; Rap, A.; Schmidt, A.; Scott, C. E.; Pringle, K. J.; Reddington, C. L.; Richards, N. A. D.; Woodhouse, M. T.; Ramirez-Villegas, J.; Yang, H.; Vakkari, V.; Stone, E. A.; Rupakheti, M.; Praveen, P. S.; van Zyl, P. G.; Beukes, J. P.; Josipovic, M.; Mitchell, E. J. S.; Sallu, S. M.; Forster, P. M.; Spracklen, D. V.

    2016-01-01

    Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (> 30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300-497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000-827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between -66 and +21 mW m-2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between -52 and -16 mW m-2, which is sensitive to the assumed size distribution of carbonaceous emissions

  20. Unique airborne measurements at the tropopause of Fukushima Xe-133, aerosol, and aerosol precursors indicate aerosol formation via homogeneous and cosmic ray induced nucleation

    NASA Astrophysics Data System (ADS)

    Schlager, Hans; Arnold, Frank; Aufmhoff, Heinfried; Minikin, Andreas; Baumann, Robert; Simgen, Hardy; Lindemann, Stefan; Rauch, Ludwig; Kaether, Frank; Pirjola, Liisa; Schumann, Ulrich

    2014-05-01

    We report unique airborne measurements, at the tropopause, of the Fukushima radio nuclide Xe-133, aerosol particles (size, shape, number concentration, volatility), aerosol precursor gases (particularly SO2, HNO3, H2O). Our measurements and accompanying model simulations indicate homogeneous and cosmic ray induced aerosol formation at the tropopause. Using an extremely sensitive detection method, we managed to detect Fukushima Xe-133, an ideal transport tracer, at and even above the tropopause. To our knowledge, these airborne Xe-133 measurements are the only of their kind. Our investigations represent a striking example how a pioneering measurement of a Fukshima radio nuclide, employing an extremely sensitive method, can lead to new insights into an important atmospheric process. After the Fukushima accidential Xe-133 release (mostly during 11-15 March 2011), we have conducted two aircraft missions, which took place over Central Europe, on 23 March and 11 April 2011. In the air masses, encountered by the research aircraft on 23 March, we have detected Fukushima Xe-133 by an extremely sensitive method, at and even above the tropopause. Besides increased concentrations of Xe-133, we have detected also increased concentrations of the gases SO2, HNO3, and H2O. The Xe-133 data and accompanying transport model simulations indicate that a West-Pacific Warm Conveyor Belt (WCB) lifted East-Asian planetary boundary layer air to and even above the tropopause, followed by relatively fast quasi-horizontal advection to Europe. Along with Xe-133, anthropogenic SO2, NOx (mostly released from East-Asian ground-level combustion sources), and warer vapour were also lifted by the WCB. After the lift, SO2 and NOx experienced efficient solar UV-radiation driven conversion to the important aerosol precursors gases H2SO4 and HNO3. Our investigations indicate that, increased concentrations of the gases SO2, HNO3, and H2O promoted homogeneous and cosmic ray induced aerosol formation at and

  1. “APEC Blue”: Secondary Aerosol Reductions from Emission Controls in Beijing

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Wang, Zifa; Wild, Oliver; Xu, Weiqi; Chen, Chen; Fu, Pingqing; Du, Wei; Zhou, Libo; Zhang, Qi; Han, Tingting; Wang, Qingqing; Pan, Xiaole; Zheng, Haitao; Li, Jie; Guo, Xiaofeng; Liu, Jianguo; Worsnop, Douglas R.

    2016-02-01

    China implemented strict emission control measures in Beijing and surrounding regions to ensure good air quality during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. We conducted synchronous aerosol particle measurements with two aerosol mass spectrometers at different heights on a meteorological tower in urban Beijing to investigate the variations in particulate composition, sources and size distributions in response to emission controls. Our results show consistently large reductions in secondary inorganic aerosol (SIA) of 61–67% and 51–57%, and in secondary organic aerosol (SOA) of 55% and 37%, at 260 m and ground level, respectively, during the APEC summit. These changes were mainly caused by large reductions in accumulation mode particles and by suppression of the growth of SIA and SOA by a factor of 2–3, which led to blue sky days during APEC commonly referred to as “APEC Blue”. We propose a conceptual framework for the evolution of primary and secondary species and highlight the importance of regional atmospheric transport in the formation of severe pollution episodes in Beijing. Our results indicate that reducing the precursors of secondary aerosol over regional scales is crucial and effective in suppressing the formation of secondary particulates and mitigating PM pollution.

  2. “APEC Blue”: Secondary Aerosol Reductions from Emission Controls in Beijing

    PubMed Central

    Sun, Yele; Wang, Zifa; Wild, Oliver; Xu, Weiqi; Chen, Chen; Fu, Pingqing; Du, Wei; Zhou, Libo; Zhang, Qi; Han, Tingting; Wang, Qingqing; Pan, Xiaole; Zheng, Haitao; Li, Jie; Guo, Xiaofeng; Liu, Jianguo; Worsnop, Douglas R.

    2016-01-01

    China implemented strict emission control measures in Beijing and surrounding regions to ensure good air quality during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. We conducted synchronous aerosol particle measurements with two aerosol mass spectrometers at different heights on a meteorological tower in urban Beijing to investigate the variations in particulate composition, sources and size distributions in response to emission controls. Our results show consistently large reductions in secondary inorganic aerosol (SIA) of 61–67% and 51–57%, and in secondary organic aerosol (SOA) of 55% and 37%, at 260 m and ground level, respectively, during the APEC summit. These changes were mainly caused by large reductions in accumulation mode particles and by suppression of the growth of SIA and SOA by a factor of 2–3, which led to blue sky days during APEC commonly referred to as “APEC Blue”. We propose a conceptual framework for the evolution of primary and secondary species and highlight the importance of regional atmospheric transport in the formation of severe pollution episodes in Beijing. Our results indicate that reducing the precursors of secondary aerosol over regional scales is crucial and effective in suppressing the formation of secondary particulates and mitigating PM pollution. PMID:26891104

  3. The impact of residential combustion emission on Arctic aerosol concentrations

    NASA Astrophysics Data System (ADS)

    Eckhardt, Sabine; Stohl, Andreas; Olivie, Dirk J. L.; Grini, Alf

    2016-04-01

    Arctic haze is a seasonal phenomenon with high concentrations of accumulation-mode aerosols occurring in the Arctic in winter and early spring. It has been challenging to reproduced this cylce and concentration levels with atmospheric transport and climate models. However, simulations have been improving recently and it has been shown, that a better scavenging parametrization as well as more realistic emissions are important to obtain better results. In this study we focus on the emission from residential heating, which depend on air temperature, as heating demand is higher on cold days. Varying this emission shows a clear effect on modeled Arctic concentrations. Arctic-mean and annual-mean concentrations of black carbon from Arctic domestic combustion emissions due to heating requirements, are nearly 70% higher when accounting for diurnal emission variability relative to constant emissions (Stohl et al., 2013). Emissions are high when ambient temperatures are low and cold air is transported to the Arctic. In order to capture this systematic effect, we created an interactive emission module for NorESM, a climate model, using the heating degree-day concept. Domestic combustion emissions of BC and other species are scaled interactively with the modeled ambient air temperatures, while securing that levels of annual total emissions from emission scenarios are reproduced. We compare the modeled aerosol concentration in the Arctic to observations and show the level of improvements achieved by using varying emission.

  4. Characterization of selenium in ambient aerosols and primary emission sources.

    PubMed

    De Santiago, Arlette; Longo, Amelia F; Ingall, Ellery D; Diaz, Julia M; King, Laura E; Lai, Barry; Weber, Rodney J; Russell, Armistead G; Oakes, Michelle

    2014-08-19

    Atmospheric selenium (Se) in aerosols was investigated using X-ray absorption near-edge structure (XANES) spectroscopy and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the oxidation state and elemental associations of Se in common primary emission sources and ambient aerosols collected from the greater Atlanta area. In the majority of ambient aerosol and primary emission source samples, the spectroscopic patterns as well as the absence of elemental correlations suggest Se is in an elemental, organic, or oxide form. XRF microscopy revealed numerous Se-rich particles, or hotspots, accounting on average for ∼16% of the total Se in ambient aerosols. Hotspots contained primarily Se(0)/Se(-II). However, larger, bulk spectroscopic characterizations revealed Se(IV) as the dominant oxidation state in ambient aerosol, followed by Se(0)/Se(-II) and Se(VI). Se(IV) was the only observed oxidation state in gasoline, diesel, and coal fly ash, while biomass burning contained a combination of Se(0)/Se(-II) and Se(IV). Although the majority of Se in aerosols was in the most toxic form, the Se concentration is well below the California Environmental Protection Agency chronic exposure limit (∼20000 ng/m(3)). PMID:25075640

  5. Top-Down Inversion of Aerosol Emissions through Adjoint Integration of Satellite Radiance and GEOS-Chem Chemical Transport Model

    NASA Astrophysics Data System (ADS)

    Xu, X.; Wang, J.; Henze, D. K.; Qu, W.; Kopacz, M.

    2012-12-01

    The knowledge of aerosol emissions from both natural and anthropogenic sources are needed to study the impacts of tropospheric aerosol on atmospheric composition, climate, and human health, but large uncertainties persist in quantifying the aerosol sources with the current bottom-up methods. This study presents a new top-down approach that spatially constrains the amount of aerosol emissions from satellite (MODIS) observed reflectance with the adjoint of a chemistry transport model (GEOS-Chem). We apply this technique with a one-month case study (April 2008) over the East Asia. The bottom-up estimated sulfate-nitrate-ammonium precursors, such as sulfur dioxide (SO2), ammonia (NH3), and nitrogen oxides (NOx), all from INTEX-B 2006 inventory, emissions of black carbon (BC), organic carbon (OC) from Bond-2007 inventory, and mineral dust simulated from DEAD dust mobilization scheme, are spatially optimized from the GEOS-Chem model and its adjoint constrained by the aerosol optical depth (AOD) that are derived from MODIS reflectance with the GEOS-Chem aerosol single scattering properties. The adjoint inverse modeling for the study period yields notable decreases in anthropogenic aerosol emissions over China: 436 Gg (33.5%) for SO2, 378 Gg (34.5%) for NH3, 319 (18.8%) for NOx, 10 Gg (9.1%) for BC, and 30 Gg (15.0%) for OC. The total amount of the mineral dust emission is reduced by 56.4% from the DEAD mobilization module which simulates dust production of 19020 Gg. Sub-regional adjustments are significant and directions of changes are spatially different. The model simulation with optimized aerosol emissions shows much better agreement with independent observations from sun-spectrophotometer observed AOD from AERONET, MISR (Multi-angle Imaging SpectroRadiometer) AOD, OMI (Ozone Monitoring Instrument) NO2 and SO2 columns, and surface aerosol concentrations measured over both anthropogenic pollution and dust source regions. Assuming the used bottom-up anthropogenic

  6. Spectroscopic Study of Methylglyoxal and its Hydrates : a Gaseous Precursor of Secondary Organic Aerosols.

    NASA Astrophysics Data System (ADS)

    Bteich, Sabath; Goubet, Manuel; Margulès, L.; Motiyenko, R. A.; Huet, T. R.

    2016-06-01

    Secondary organic aerosols (SOA) have a significant effect on climate change. They are mainly produced in the atmosphere by oxidation of gaseous precursors. Fu et al. have suggested trans-methylglyoxal (MG) as a possible precursor of SOA in the cloud for its presence in large quantities in the atmosphere. The characterization of SOAs precursors by laboratory spectroscopy allows providing elements for the understanding of the process of formation of these aerosols. For this purpose, we completed the existing pure rotational spectrum of MG in the 12-40 GHz range by new records in a supersonic jet in the 4-20 GHz range (FTMW) and at room temperature in the 150-500 GHz range (mm/submm-wave spectrometer). The analysis was made with the support of quantum chemistry calculations (MP2/CBS and B98/CBS using the Gaussian 09 software). The adjustment of the spectroscopic parameters, taking into account the internal rotation related to the presence of a methyl group, was performed using the RAM36 code. The spectra have been reproduced at the experimental precision up to maximal values of J and K_a equal to 85 and 35, respectively. The data obtained for the isolated molecule, both experimentally and theoretically, will allow the study of its hydrated complexes and, by comparison, will give access to (micro-) hydration properties. For this purpose, two stable complexes predicted by theoretical calculations will be studied. T.- M. Fu et al., J. Geophys. Res., 113, (2008). C.E. Dyltick-Brenzinger and A. Bauder, Chem. Phys. 30, 147 (1978).

  7. Secondary organic aerosol formation from road vehicle emissions

    NASA Astrophysics Data System (ADS)

    Pieber, Simone M.; Platt, Stephen M.; El Haddad, Imad; Zardini, Alessandro A.; Suarez-Bertoa, Ricardo; Slowik, Jay G.; Huang, Ru-Jin; Hellebust, Stig; Temime-Roussel, Brice; Marchand, Nicolas; Drinovec, Luca; Mocnik, Grisa; Baltensperger, Urs; Astorga, Covadogna; Prévôt, André S. H.

    2014-05-01

    Organic aerosol particles (OA) are a major fraction of the submicron particulate matter. OA consists of directly emitted primary (POA) and secondary OA (SOA). SOA is formed in-situ in the atmosphere via the reaction of volatile organic precursors. The partitioning of SOA species depends not only on the exposure to oxidants, but for instance also on temperature, relative humidity (RH), and the absorptive mass chemical composition (presence of inorganics) and concentration. Vehicle exhaust is a known source of POA and likely contributes to SOA formation in urban areas [1;2]. This has recently been estimated by (i) analyzing ambient data from urban areas combined with fuel consumption data [3], (ii) by examining the chemical composition of raw fuels [4], or (iii) smog chamber studies [5, 6]. Contradictory and thus somewhat controversial results in the relative quantity of SOA from diesel vs. gasoline vehicle exhaust were observed. In order to elucidate the impact of variable ambient conditions on the potential SOA formation of vehicle exhaust, and its relation to the emitted gas phase species, we studied SOA formed from the exhaust of passenger cars and trucks as a function of fuel and engine type (gasoline, diesel) at different temperatures (T 22 vs. -7oC) and RH (40 vs. 90%), as well as with different levels of inorganic salt concentrations. The exhaust was sampled at the tailpipe during regulatory driving cycles on chassis dynamometers, diluted (200 - 400x) and introduced into the PSI mobile smog chamber [6], where the emissions were subjected to simulated atmospheric ageing. Particle phase instruments (HR-ToF-AMS, aethalometers, CPC, SMPS) and gas phase instruments (PTR-TOF-MS, CO, CO2, CH4, THC, NH3 and other gases) were used online during the experiments. We found that gasoline emissions, because of cold starts, were generally larger than diesel, especially during cold temperatures driving cycles. Gasoline vehicles also showed the highest SOA formation

  8. A simple parameterization of aerosol emissions in RAMS

    NASA Astrophysics Data System (ADS)

    Letcher, Theodore

    Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical

  9. Measurement of gas and aerosol agricultural emissions

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Studies of air quality indicate that agricultural emissions may impact particulate mass concentrations through both primary and secondary processes. Agriculture impacts can include primary dust emission, on-facility combustion from vehicles or seasonal field burning, and gaseous emissions from waste...

  10. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Zhao, Y.

    2015-12-01

    To better understand the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations in China, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal and spatial distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols. The national OC emissions are estimated to have increased 29% from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37% (from 1356 to 1857 Gg). Updated emission factors based on the most recent local field measurements, particularly for biofuel stoves, lead to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while SOC/OC ratios are found in southern cities, due to the joint effects of primary emissions and meteorology. Higher OC/EC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, smaller SOC/OC is found for cold seasons, particularly at rural and remote sites, attributed partly to weaker atmospheric oxidation and SOC formation in winter. Enhanced SOC formation from oxidization and anthropogenic activities like biomass combustion is judged to have crucial effects on severe haze events characterized by high particle concentrations. Several observational studies indicate an increasing trend in ambient OC/EC (but not in OC or EC individually) from 2000 to 2010, confirming increased atmospheric oxidation of OC across the country. Combining the results of

  11. TOWARD AN EMPIRICAL THEORY OF PULSAR EMISSION. X. ON THE PRECURSOR AND POSTCURSOR EMISSION

    SciTech Connect

    Basu, Rahul; Mitra, Dipanjan; Rankin, Joanna M.

    2015-01-10

    Precursors and postcursors (PPCs) are rare emission components, which appear beyond the main pulse emission, in some cases far away from it, and are detected in a handful of pulsar. In this paper we attempt to characterize the PPC emission in relation to the pulsar main pulse geometry. In our analysis we find that PPC components have properties very different from that of outer conal emission. The separation of the PPC components from the main pulse center remains constant with frequency. In addition the beam opening angles corresponding to the separation of PPC components from the pulsar center are much larger than the largest encountered in conal emission. Pulsar radio emission is believed to originate within the magnetic polar flux tubes due to the growth of instabilities in the outflowing relativistic plasma. Observationally, there is strong evidence that the main pulse emission originates at altitudes of about 50 neutron star radii for a canonical pulsar. Currently, the most plausible radio emission model that can explain main pulse emission is the coherent curvature radiation mechanism, wherein relativistic charged solitons are formed in a non-stationary electron-positron-pair plasma. The wider beam opening angles of PPC require the emission to emanate from larger altitudes as compared to the main pulse, if both these components originate by the same emission mechanism. We explore this possibility and find that this emission mechanism is probably inapplicable at the height of the PPC emission. We propose that the PPC emission represents a new type of radiation from pulsars with a mechanism different from that of the main pulse.

  12. Isoprene Epoxydiols as Precursors to Secondary Organic Aerosol Formation: Acid-Catalyzed Reactive Uptake Studies with Authentic Compounds

    PubMed Central

    Lin, Ying-Hsuan; Zhang, Zhenfa; Docherty, Kenneth S.; Zhang, Haofei; Budisulistiorini, Sri Hapsari; Rubitschun, Caitlin L.; Shaw, Stephanie L.; Knipping, Eladio M.; Edgerton, Eric S.; Kleindienst, Tadeusz E.; Gold, Avram; Surratt, Jason D.

    2011-01-01

    Isoprene epoxydiols (IEPOX), formed from the photooxidation of isoprene under low-NOx conditions, have recently been proposed as precursors of secondary organic aerosol (SOA) on the basis of mass spectrometric evidence. In the present study, IEPOX isomers were synthesized in high purity (> 99%) to investigate their potential to form SOA via reactive uptake in a series of controlled dark chamber studies followed by reaction product analyses. IEPOX-derived SOA was substantially observed only in the presence of acidic aerosols, with conservative lower-bound yields of 4.7–6.4% for β-IEPOX and 3.4–5.5% for δ-IEPOX, providing direct evidence for IEPOX isomers as precursors to isoprene SOA. These chamber studies demonstrate that IEPOX uptake explains the formation of known isoprene SOA tracers found in ambient aerosols, including 2-methyltetrols, C5-alkene triols, dimers, and IEPOX-derived organosulfates. Additionally, we show reactive uptake on the acidified sulfate aerosols supports a previously unreported acid-catalyzed intramolecular rearrangement of IEPOX to cis- and trans-3-methyltetrahydrofuran-3,4-diols (3-MeTHF-3,4-diols) in the particle phase. Analysis of these novel tracer compounds by aerosol mass spectrometry (AMS) suggests that they contribute to a unique factor resolved from positive matrix factorization (PMF) of AMS organic aerosol spectra collected from low-NOx, isoprene-dominated regions influenced by the presence of acidic aerosols. PMID:22103348

  13. Land cover maps, BVOC emissions, and SOA burden in a global aerosol-climate model

    NASA Astrophysics Data System (ADS)

    Stanelle, Tanja; Henrot, Alexandra; Bey, Isaelle

    2015-04-01

    It has been reported that different land cover representations influence the emission of biogenic volatile organic compounds (BVOC) (e.g. Guenther et al., 2006). But the land cover forcing used in model simulations is quite uncertain (e.g. Jung et al., 2006). As a consequence the simulated emission of BVOCs depends on the applied land cover map. To test the sensitivity of global and regional estimates of BVOC emissions on the applied land cover map we applied 3 different land cover maps into our global aerosol-climate model ECHAM6-HAM2.2. We found a high sensitivity for tropical regions. BVOCs are a very prominent precursor for the production of Secondary Organic Aerosols (SOA). Therefore the sensitivity of BVOC emissions on land cover maps impacts the SOA burden in the atmosphere. With our model system we are able to quantify that impact. References: Guenther et al. (2006), Estimates of global terrestrial isoprene emissions using MEGAN, Atmos. Chem. Phys., 6, 3181-3210, doi:10.5194/acp-6-3181-2006. Jung et al. (2006), Exploiting synergies of global land cover products for carbon cycle modeling, Rem. Sens. Environm., 101, 534-553, doi:10.1016/j.rse.2006.01.020.

  14. Lagrangian aerosol and ozone precursor forecasts utilizing NASA Aura OMI NO2 and NOAA GOES-GASP AOD Observations

    NASA Astrophysics Data System (ADS)

    Pierce, R. B.; Szykman, J.; Kondragunta, S.; Al-Saadi, J.; Hertherington, G.; Majewski, M.; Kittaka, C.

    2008-05-01

    Over the past decade, the remote sensing of trace gases and aerosols from space has dramatically improved. The emergence and application of these measurements adds a new dimension to air quality management and forecasting by enabling consistent observations of pollutants over large spatial domains. Current instruments aboard NASA and European Space Agency satellites can provide derived measurements of trace gases and aerosols relating directly to most of the EPA's criteria pollutants: ozone, NO2, SO2, CO, and particulate matter (PM10 and PM2.5). Al-Saadi et. al., (2005) provided one of the first demonstrations on the use of AOD as a forecast tool for PM2.5 through IDEA, Infusing satellite Data into Environmental air quality Applications, a joint project between NASA, EPA, and NOAA. We have developed a new approach for forecasting aerosol and ozone precursor levels that utilizes Reverse Domain Filling [Sutton, 1994] techniques and measurements of NO2 from the Ozone Monitoring Instrument (OMI) onboard the NASA Aura satellite and aerosol optical depth (AOD) from NOAA's operational geostationary satellite retrievals [Knapp et al., 2002 and Prados et al. 2007]. Using the LaRC trajectory model [Pierce and Fairlie, 1993], 72-hr back-trajectories are initialized on a uniform grid (0.25° x 0.25°) at the surface over the Midwestern US. Coincidences between the back-trajectories and previous OMI NO2 and GOES AOD observations are identified and used to map the satellite observations back onto the uniform grid at the forecast time. The resulting RDF mapped NO2 forecast is valid at 21Z on the next day. This talk will present a case study for May 2007 over the Western Great Lakes Region. We present a comparison of the RDF forecast to an RDF forecast based on hourly NO2 and SO2 emissions used for CAMx Air Quality Model along with a comparison to in-situ concentrations of PM2.5 and O3. Disclaimer: Although this work was reviewed by the U.S. Environmental Protection Agency

  15. Enhancement of aerosol responses to changes in emissions over East Asia by gas-oxidant-aerosol coupling and detailed aerosol processes

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.

    2016-06-01

    We quantify the responses of aerosols to changes in emissions (sulfur dioxide, black carbon (BC), primary organic aerosol, nitrogen oxides (NOx), and volatile organic compounds) over East Asia by using simulations including gas-oxidant-aerosol coupling, organic aerosol (OA) formation, and BC aging processes. The responses of aerosols to NOx emissions are complex and are dramatically changed by simulating gas-phase chemistry and aerosol processes online. Reduction of NOx emissions by 50% causes a 30-40% reduction of oxidant (hydroxyl radical and ozone) concentrations and slows the formation of sulfate and OA by 20-30%. Because the response of OA to changes in NOx emissions is sensitive to the treatment of emission and oxidation of semivolatile and intermediate volatility organic compounds, reduction of the uncertainty in these processes is necessary to evaluate gas-oxidant-aerosol coupling accurately. Our simulations also show that the sensitivity of aerosols to changes in emissions is enhanced by 50-100% when OA formation and BC aging processes are resolved in the model. Sensitivity simulations show that the increase of NOx emissions from 1850 to 2000 explains 70% (40%) of the enhancement of aerosol mass concentrations (direct radiative effects) over East Asia during that period through enhancement of oxidant concentrations and that this estimation is sensitive to the representation of OA formation and BC aging processes. Our results demonstrate the importance of simultaneous simulation of gas-oxidant-aerosol coupling and detailed aerosol processes. The impact of NOx emissions on aerosol formation will be a key to formulating effective emission reduction strategies such as BC mitigation and aerosol reduction policies in East Asia.

  16. Emissions of biogenic volatile organic compounds and subsequent formation of secondary organic aerosols in a Larix kaempferi forest

    NASA Astrophysics Data System (ADS)

    Mochizuki, T.; Miyazaki, Y.; Ono, K.; Wada, R.; Takahashi, Y.; Saigusa, N.; Kawamura, K.; Tani, A.

    2015-04-01

    We conducted simultaneous measurements of concentrations and above-canopy fluxes of isoprene and α-pinene, along with their oxidation products in aerosols in a Larix kaempferi (Japanese larch) forest in summer 2012. Vertical profiles of isoprene showed the maximum concentration near the forest floor with a peak around noon, whereas oxidation products of isoprene, i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), showed higher concentrations near the canopy level of the forest. The vertical profile suggests large emissions of isoprene near the forest floor, likely due to Dryopteris crassirhizoma (a fern species), and the subsequent reaction within the canopy. The concentrations of α-pinene also showed highest values near the forest floor with maximums in the early morning and late afternoon. The vertical profiles of α-pinene suggest its large emissions from soil and litter in addition to emissions from L. kaempferi leaves at the forest site. Isoprene and its oxidation products in aerosols exhibited similar diurnal variations within the forest canopy, providing evidence for secondary organic aerosol (SOA) formation via oxidation of isoprene most likely emitted from the forest floor. Although high abundance of α-pinene was observed in the morning, its oxidation products in aerosols showed peaks in daytime, due to a time lag between the emission and atmospheric reactions of α-pinene to form SOA. Positive matrix factorization (PMF) analysis indicated that anthropogenic influence is the most important factor contributing to the elevated concentrations of molecular oxidation products of isoprene- (> 64%) and α-pinene-derived SOA (> 57%). The combination of the measured fluxes and vertical profiles of biogenic volatile organic compounds (BVOCs) suggests that the inflow of anthropogenic precursors/aerosols likely enhanced the formation of both isoprene- and α-pinene-SOA within the forest canopy even when the BVOC flux was relatively low. This study highlights

  17. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-08-01

    China is experiencing severe carbonaceous aerosol pollution driven mainly by large emissions resulting from intensive use of solid fuels. To gain a better understanding of the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations at the national scale, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal, spatial, and size distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols, and propose possible improvements in emission estimation for the future. The national OC emissions are estimated to have increased 29 % from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37 % (from 1356 to 1857 Gg). The residential, industrial, and transportation sectors contributed an estimated 74-78, 17-21, and 4-6 % of the total emissions of OC, respectively, and 49-55, 30-34, and 14-18 % of EC. Updated emission factors (EFs) based on the most recent local field measurements, particularly for biofuel stoves, led to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while higher OC / EC ratios are found in southern sites, due to the joint effects of primary emissions and meteorology. Higher OC / EC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, higher concentrations of OC, EC, and SOC are observed in colder seasons, while SOC / OC is reduced, particularly at rural and remote sites

  18. Gas phase emissions from cooking processes and their secondary aerosol production potential

    NASA Astrophysics Data System (ADS)

    Klein, Felix; Platt, Stephen; Bruns, Emily; Termime-roussel, Brice; Detournay, Anais; Mohr, Claudia; Crippa, Monica; Slowik, Jay; Marchand, Nicolas; Baltensperger, Urs; Prevot, Andre; El Haddad, Imad

    2014-05-01

    Long before the industrial evolution and the era of fossil fuels, high concentrations of aerosol particles were alluded to in heavily populated areas, including ancient Rome and medieval London. Recent radiocarbon measurements (14C) conducted in modern megacities came as a surprise: carbonaceous aerosol (mainly organic aerosol, OA), a predominant fraction of particulate matter (PM), remains overwhelmingly non-fossil despite extensive fossil fuel combustion. Such particles are directly emitted (primary OA, POA) or formed in-situ in the atmosphere (secondary OA, SOA) via photochemical reactions of volatile organic compounds (VOCs). Urban levels of non-fossil OA greatly exceed the levels measured in pristine environments strongly impacted by biogenic emissions, suggesting a contribution from unidentified anthropogenic non-fossil sources to urban OA. Positive matrix factorization (PMF) techniques applied to ambient aerosol mass spectrometer (AMS, Aerodyne) data identify primary cooking emissions (COA) as one of the main sources of primary non-fossil OA in major cities like London (Allan et al., 2010), New York (Sun et al., 2011) and Beijing (Huang et al., 2010). Cooking processes can also emit VOCs that can act as SOA precursors, potentially explaining in part the high levels of oxygenated OA (OOA) identified by the AMS in urban areas. However, at present, the chemical nature of these VOCs and their secondary aerosol production potential (SAPP) remain virtually unknown. The approach adopted here involves laboratory quantification of PM and VOC emission factors from the main primary COA emitting processes and their SAPP. Primary emissions from deep-fat frying, vegetable boiling, vegetable frying and meat cooking for different oils, meats and vegetables were analysed under controlled conditions after ~100 times dilution. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a high resolution proton transfer time-of-flight mass spectrometer (PTR

  19. Epoxide as a precursor to secondary organic aerosol formation from isoprene photooxidation in the presence of nitrogen oxides.

    PubMed

    Lin, Ying-Hsuan; Zhang, Haofei; Pye, Havala O T; Zhang, Zhenfa; Marth, Wendy J; Park, Sarah; Arashiro, Maiko; Cui, Tianqu; Budisulistiorini, Sri Hapsari; Sexton, Kenneth G; Vizuete, William; Xie, Ying; Luecken, Deborah J; Piletic, Ivan R; Edney, Edward O; Bartolotti, Libero J; Gold, Avram; Surratt, Jason D

    2013-04-23

    Isoprene is a substantial contributor to the global secondary organic aerosol (SOA) burden, with implications for public health and the climate system. The mechanism by which isoprene-derived SOA is formed and the influence of environmental conditions, however, remain unclear. We present evidence from controlled smog chamber experiments and field measurements that in the presence of high levels of nitrogen oxides (NO(x) = NO + NO2) typical of urban atmospheres, 2-methyloxirane-2-carboxylic acid (methacrylic acid epoxide, MAE) is a precursor to known isoprene-derived SOA tracers, and ultimately to SOA. We propose that MAE arises from decomposition of the OH adduct of methacryloylperoxynitrate (MPAN). This hypothesis is supported by the similarity of SOA constituents derived from MAE to those from photooxidation of isoprene, methacrolein, and MPAN under high-NOx conditions. Strong support is further derived from computational chemistry calculations and Community Multiscale Air Quality model simulations, yielding predictions consistent with field observations. Field measurements taken in Chapel Hill, North Carolina, considered along with the modeling results indicate the atmospheric significance and relevance of MAE chemistry across the United States, especially in urban areas heavily impacted by isoprene emissions. Identification of MAE implies a major role of atmospheric epoxides in forming SOA from isoprene photooxidation. Updating current atmospheric modeling frameworks with MAE chemistry could improve the way that SOA has been attributed to isoprene based on ambient tracer measurements, and lead to SOA parameterizations that better capture the dependency of yield on NO(x). PMID:23553832

  20. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-10-01

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.

  1. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

    PubMed Central

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-01-01

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks. PMID:27733773

  2. Evaluation of the operational Aerosol Layer Height retrieval algorithm for Sentinel-5 Precursor: application to O2 A band observations from GOME-2A

    NASA Astrophysics Data System (ADS)

    Sanders, A. F. J.; de Haan, J. F.; Sneep, M.; Apituley, A.; Stammes, P.; Vieitez, M. O.; Tilstra, L. G.; Tuinder, O. N. E.; Koning, C. E.; Veefkind, J. P.

    2015-06-01

    An algorithm setup for the operational Aerosol Layer Height product for TROPOMI on the Sentinel-5 Precursor mission is described and discussed, applied to GOME-2A data, and evaluated with lidar measurements. The algorithm makes a spectral fit of reflectance at the O2 A band in the near-infrared and the fit window runs from 758 to 770 nm. The aerosol profile is parameterized by a scattering layer with constant aerosol volume extinction coefficient and aerosol single scattering albedo and with a fixed pressure thickness. The algorithm's target parameter is the height of this layer. In this paper, we apply the algorithm to observations from GOME-2A in a number of systematic and extensive case studies and we compare retrieved aerosol layer heights with lidar measurements. Aerosol scenes cover various aerosol types, both elevated and boundary layer aerosols, and land and sea surfaces. The aerosol optical thicknesses for these scenes are relatively moderate. Retrieval experiments with GOME-2A spectra are used to investigate various sensitivities, in which particular attention is given to the role of the surface albedo. From retrieval simulations with the single-layer model, we learn that the surface albedo should be a fit parameter when retrieving aerosol layer height from the O2 A band. Current uncertainties in surface albedo climatologies cause biases and non-convergences when the surface albedo is fixed in the retrieval. Biases disappear and convergence improves when the surface albedo is fitted, while precision of retrieved aerosol layer pressure is still largely within requirement levels. Moreover, we show that fitting the surface albedo helps to ameliorate biases in retrieved aerosol layer height when the assumed aerosol model is inaccurate. Subsequent retrievals with GOME-2A spectra confirm that convergence is better when the surface albedo is retrieved simultaneously with aerosol parameters. However, retrieved aerosol layer pressures are systematically low (i

  3. Evaluation of the operational Aerosol Layer Height retrieval algorithm for Sentinel-5 Precursor: application to O2 A band observations from GOME-2A

    NASA Astrophysics Data System (ADS)

    Sanders, A. F. J.; de Haan, J. F.; Sneep, M.; Apituley, A.; Stammes, P.; Vieitez, M. O.; Tilstra, L. G.; Tuinder, O. N. E.; Koning, C. E.; Veefkind, J. P.

    2015-11-01

    An algorithm setup for the operational Aerosol Layer Height product for TROPOMI on the Sentinel-5 Precursor mission is described and discussed, applied to GOME-2A data, and evaluated with lidar measurements. The algorithm makes a spectral fit of reflectance at the O2 A band in the near-infrared and the fit window runs from 758 to 770 nm. The aerosol profile is parameterised by a scattering layer with constant aerosol volume extinction coefficient and aerosol single scattering albedo and with a fixed pressure thickness. The algorithm's target parameter is the height of this layer. In this paper, we apply the algorithm to observations from GOME-2A in a number of systematic and extensive case studies, and we compare retrieved aerosol layer heights with lidar measurements. Aerosol scenes cover various aerosol types, both elevated and boundary layer aerosols, and land and sea surfaces. The aerosol optical thicknesses for these scenes are relatively moderate. Retrieval experiments with GOME-2A spectra are used to investigate various sensitivities, in which particular attention is given to the role of the surface albedo. From retrieval simulations with the single-layer model, we learn that the surface albedo should be a fit parameter when retrieving aerosol layer height from the O2 A band. Current uncertainties in surface albedo climatologies cause biases and non-convergences when the surface albedo is fixed in the retrieval. Biases disappear and convergence improves when the surface albedo is fitted, while precision of retrieved aerosol layer pressure is still largely within requirement levels. Moreover, we show that fitting the surface albedo helps to ameliorate biases in retrieved aerosol layer height when the assumed aerosol model is inaccurate. Subsequent retrievals with GOME-2A spectra confirm that convergence is better when the surface albedo is retrieved simultaneously with aerosol parameters. However, retrieved aerosol layer pressures are systematically low (i

  4. Emission of sunscreen salicylic esters from desert vegetation and their contribution to aerosol formation

    NASA Astrophysics Data System (ADS)

    Matsunaga, S. N.; Guenther, A. B.; Potosnak, M. J.; Apel, E. C.

    2008-12-01

    Biogenic volatile organic compounds (BVOC) produced by plants are known to have an important role in atmospheric chemistry. However, our knowledge of the range of BVOCs produced by different plant processes is still expanding, and there remain poorly understood categories of BVOCs. In this study, emissions of a novel class of BVOC emissions were investigated in a desert region. Our study considered 8 species of common desert plants: blackbrush (Coleogyne ramosissima), desert willow (Chilopsis linearis), mesquite (Prosopis glandulosa), mondel pine (Pinus eldarica), pinyon pine (Pinus monophylla), cottonwood (Populus deltoides), saguaro cactus (Carnegiea gigantea) and yucca (Yucca baccata). The measurements focused on BVOCs with relatively high molecular weight (>C15) and/or an oxygenated functional group. Significantly high emission rates of two salicylic esters were found for blackbrush, desert willow and mesquite with emission rates of 3.1, 1.0 and 4.8μgC dwg-1 h-1, respectively (dwg; dry weight of the leaves in gram). The salicylic esters were identified as 2-ethylhexenyl salicylate (2-EHS) and 3,3,5-trimethylcyclohexenyl salicylate (homosalate) and are known as effective ultraviolet (UV) absorbers. We propose that the plants derive a protective benefit against UV radiation from the salicylic esters and that the emission process is driven by the physical evaporation of the salicylic esters due to the high ambient temperatures. In addition, the salicylic esters are predicted to be an effective precursor of secondary organic aerosol (SOA) because they probably produce oxidation products that can condense onto the aerosol phase. We estimated the contribution of the sunscreen esters themselves and their oxidation products on the SOA formation for the Las Vegas area using a BVOC emission model. The contribution was estimated to reach 50% of the biogenic terpenoid emission in the landscapes dominated by desert willow and mesquite and 13% in the Las Vegas area. The

  5. Science verification of operational aerosol and cloud products for TROPOMI on Sentinel-5 precursor

    NASA Astrophysics Data System (ADS)

    Lelli, Luca; Gimeno-Garcia, Sebastian; Sanders, Abram; Sneep, Maarten; Rozanov, Vladimir V.; Kokhanvosky, Alexander A.; Loyola, Diego; Burrows, John P.

    2016-04-01

    With the approaching launch of the Sentinel-5 precursor (S-5P) satellite, scheduled by mid 2016, one preparatory task of the L2 working group (composed by the Institute of Environmental Physics IUP Bremen, the Royal Netherlands Meteorological Institute KNMI De Bilt, and the German Aerospace Center DLR Oberpfaffenhofen) has been the assessment of biases among aerosol and cloud products, that are going to be inferred by the respective algorithms from measurements of the platform's payload TROPOspheric Monitoring Instrument (TROPOMI). The instrument will measure terrestrial radiance with varying moderate spectral resolutions from the ultraviolet throughout the shortwave infrared. Specifically, all the operational and verification algorithms involved in this comparison exploit the sensitivity of molecular oxygen absorption (the A-band, 755-775 nm, with a resolution of 0.54 nm) to changes in optical and geometrical parameters of tropospheric scattering layers. Therefore, aerosol layer height (ALH) and thickness (AOT), cloud top height (CTH), thickness (COT) and albedo (CA) are the targeted properties. First, the verification of these properties has been accomplished upon synchronisation of the respective forward radiative transfer models for a variety of atmospheric scenarios. Then, biases against independent techniques have been evaluated with real measurements of selected GOME-2 orbits. Global seasonal bias assessment has been carried out for CTH, CA and COT, whereas the verification of ALH and AOT is based on the analysis of the ash plume emitted by the icelandic volcanic eruption Eyjafjallajökull in May 2010 and selected dust scenes off the Saharan west coast sensed by SCIAMACHY in year 2009.

  6. Secondary organic aerosol formation exceeds primary particulate matter emissions for light-duty gasoline vehicles

    NASA Astrophysics Data System (ADS)

    Gordon, T. D.; Presto, A. A.; May, A. A.; Nguyen, N. T.; Lipsky, E. M.; Donahue, N. M.; Gutierrez, A.; Zhang, M.; Maddox, C.; Rieger, P.; Chattopadhyay, S.; Maldonado, H.; Maricq, M. M.; Robinson, A. L.

    2013-09-01

    The effects of photochemical aging on emissions from 15 light-duty gasoline vehicles were investigated using a smog chamber to probe the critical link between the tailpipe and ambient atmosphere. The vehicles were recruited from the California in-use fleet; they represent a wide range of model years (1987 to 2011), vehicle types and emission control technologies. Each vehicle was tested on a chassis dynamometer using the unified cycle. Dilute emissions were sampled into a portable smog chamber and then photochemically aged under urban-like conditions. For every vehicle, substantial secondary organic aerosol (SOA) formation occurred during cold-start tests, with the emissions from some vehicles generating as much as 6 times the amount of SOA as primary particulate matter after three hours of oxidation inside the chamber at typical atmospheric oxidant levels. Therefore, the contribution of light duty gasoline vehicle exhaust to ambient PM levels is likely dominated by secondary PM production (SOA and nitrate). Emissions from hot-start tests formed about a factor of 3-7 less SOA than cold-start tests. Therefore, catalyst warm-up appears to be an important factor in controlling SOA precursor emissions. The mass of SOA generated by photo-oxidizing exhaust from newer (LEV1 and LEV2) vehicles was only modestly lower (38%) than that formed from exhaust emitted by older (pre-LEV) vehicles, despite much larger reductions in non-methane organic gas emissions. These data suggest that a complex and non-linear relationship exists between organic gas emissions and SOA formation, which is not surprising since SOA precursors are only one component of the exhaust. Except for the oldest (pre-LEV) vehicles, the SOA production could not be fully explained by the measured oxidation of speciated (traditional) SOA precursors. Over the time scale of these experiments, the mixture of organic vapors emitted by newer vehicles appear to be more efficient (higher yielding) in producing SOA than

  7. Secondary organic aerosol formation exceeds primary particulate matter emissions for light-duty gasoline vehicles

    NASA Astrophysics Data System (ADS)

    Gordon, T. D.; Presto, A. A.; May, A. A.; Nguyen, N. T.; Lipsky, E. M.; Donahue, N. M.; Gutierrez, A.; Zhang, M.; Maddox, C.; Rieger, P.; Chattopadhyay, S.; Maldonado, H.; Maricq, M. M.; Robinson, A. L.

    2014-05-01

    The effects of photochemical aging on emissions from 15 light-duty gasoline vehicles were investigated using a smog chamber to probe the critical link between the tailpipe and ambient atmosphere. The vehicles were recruited from the California in-use fleet; they represent a wide range of model years (1987 to 2011), vehicle types and emission control technologies. Each vehicle was tested on a chassis dynamometer using the unified cycle. Dilute emissions were sampled into a portable smog chamber and then photochemically aged under urban-like conditions. For every vehicle, substantial secondary organic aerosol (SOA) formation occurred during cold-start tests, with the emissions from some vehicles generating as much as 6 times the amount of SOA as primary particulate matter (PM) after 3 h of oxidation inside the chamber at typical atmospheric oxidant levels (and 5 times the amount of SOA as primary PM after 5 × 106 molecules cm-3 h of OH exposure). Therefore, the contribution of light-duty gasoline vehicle exhaust to ambient PM levels is likely dominated by secondary PM production (SOA and nitrate). Emissions from hot-start tests formed about a factor of 3-7 less SOA than cold-start tests. Therefore, catalyst warm-up appears to be an important factor in controlling SOA precursor emissions. The mass of SOA generated by photooxidizing exhaust from newer (LEV2) vehicles was a factor of 3 lower than that formed from exhaust emitted by older (pre-LEV) vehicles, despite much larger reductions (a factor of 11-15) in nonmethane organic gas emissions. These data suggest that a complex and nonlinear relationship exists between organic gas emissions and SOA formation, which is not surprising since SOA precursors are only one component of the exhaust. Except for the oldest (pre-LEV) vehicles, the SOA production could not be fully explained by the measured oxidation of speciated (traditional) SOA precursors. Over the timescale of these experiments, the mixture of organic vapors

  8. Inorganic aerosols responses to emission changes in Yangtze River Delta, China

    SciTech Connect

    Dong, Xinyi; Li, Juan; Fu, Joshua S.; Gao, Yang; Huang, Kan; Zhuang, Guoshun

    2014-05-15

    China announced the Chinese National Ambient Air Quality standards (CH-NAAQS) on Feb. 29th, 2012, and PM2.5 is for the very first time included in the standards as a criteria pollutant. In order to probe into PM2.5 pollution over Yangtze River Delta, which is one of the major urban clusters hosting more than 80 million people in China, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Both simulation and observation demonstrated that, inorganic aerosols have substantial contributions to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3-) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3-concentration throughout the year. We also found that in winter NO3- was even increased under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4+) and sulfate (SO42-), while other seasons showed decrease response of NO3-. Sensitivity responses of NO3- under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3- formation was actually VOC sensitive due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols.

  9. Inorganic aerosols responses to emission changes in Yangtze River Delta, China.

    PubMed

    Dong, Xinyi; Li, Juan; Fu, Joshua S; Gao, Yang; Huang, Kan; Zhuang, Guoshun

    2014-05-15

    The new Chinese National Ambient Air Quality standards (CH-NAAQS) published on Feb. 29th, 2012 listed PM2.5 as criteria pollutant for the very first time. In order to probe into PM2.5 pollution over Yangtze River Delta, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Total PM2.5 concentration over YRD was found to have strong seasonal variation with higher values in winter months (up to 89.9 μg/m(3) in January) and lower values in summer months (down to 28.8 μg/m(3) in July). Inorganic aerosols were found to have substantial contribution to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3(-)) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3(-) concentration throughout the year. In winter, NO3(-) was found to increase under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4(+)) and sulfate (SO4(2-)), while other seasons showed decrease response of NO3(-). Sensitivity responses of NO3(-) under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3(-) formation was actually more sensitive to VOC than NOx due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols.

  10. Inorganic aerosols responses to emission changes in Yangtze River Delta, China.

    PubMed

    Dong, Xinyi; Li, Juan; Fu, Joshua S; Gao, Yang; Huang, Kan; Zhuang, Guoshun

    2014-05-15

    The new Chinese National Ambient Air Quality standards (CH-NAAQS) published on Feb. 29th, 2012 listed PM2.5 as criteria pollutant for the very first time. In order to probe into PM2.5 pollution over Yangtze River Delta, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Total PM2.5 concentration over YRD was found to have strong seasonal variation with higher values in winter months (up to 89.9 μg/m(3) in January) and lower values in summer months (down to 28.8 μg/m(3) in July). Inorganic aerosols were found to have substantial contribution to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3(-)) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3(-) concentration throughout the year. In winter, NO3(-) was found to increase under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4(+)) and sulfate (SO4(2-)), while other seasons showed decrease response of NO3(-). Sensitivity responses of NO3(-) under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3(-) formation was actually more sensitive to VOC than NOx due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols. PMID:24631615

  11. Radio Emissions Precursors of Impulsive Phase of Solar Flares Recorded by CALLISTO-BR

    NASA Astrophysics Data System (ADS)

    Fernandes, Francisco; Cunha-Silva, Rafael; Galdino, Marcela; Sodré, Zuleika

    2016-07-01

    A solar flare consists in an eruptive process and involves a sudden release of energy generated by processes carried on from instabilities in the magnetic configuration at solar atmosphere, generating emissions at different wavelengths. Usually, the pre-flare phase presents an increasing of soft X-ray, ultraviolet and radio emissions. In this work, we present a survey of solar radio emission recorded in metric wavelengths (45 - 250 MHz) by CALLISTO-BR spectrograph, belong to the e-Callisto network, associated with pre-flare phase of solar X-rays flares. A sample of 281 radio emissions was analyzed, and 120 were identified as precursor emissions of X-rays flares. The main results of the statistics can be summarized as: (a) 55% of the precursor radio emissions start less than 60 minutes before the beginning of the associated X-ray flare and about 20% start less than 20 minutes before the X-ray emission; (b) 27% of flares with precursor emissions are classified as B class, 61% of C class, and less than 22% of M class. No precursors radio emissions were associated with X class flare; (c) about 42% of radio precursor emissions are of type III bursts and 33% have complex morphology, as drifting pulsating structures. Analysis of global emission trends recorded during the precursor phase of the C4.8 flare of February 15, 2011 (14:32-14:51 UT) is also presented. The occurrence of radio emission during the pre-impulsive phase of a solar flare suggests the presence of plasma turbulence in the active region, since during the impulsive phase, when the energy is released, occur the heating of the plasma and increasing of soft X-ray emission as identified in the event analyzed. The results are presented and discussed.

  12. Effects of Bark Beetle Infestation on Secondary Organic Aerosol Precursors in the Western United States

    NASA Astrophysics Data System (ADS)

    Huff Hartz, K. E.; Amin, H.; Dodson, C.; Atkins, P. T.; Hallar, G.

    2009-12-01

    Bark beetles are a potentially destructive force in forest ecosytems; however, it is not known how insect attacks affect the atmosphere. Other insects, such as the weevil (Strophosoma melanogrammum) attacks on spruce trees in Denmark, have a significant local effect on monoterpene emissions. In fact, a single weevil induced a three-fold increase in monoterpene emission, and the response lasted for several weeks. Mountain pine bark beetles (Dendroctonus ponderosae) have infested the forests in the vicinity of Storm Peak Laboratory near Steamboat Springs, Colorado. Emissions were sampled from the headspace of bark at the trunk and from the tree branches in the canopy from bark beetle infested and healthy lodgepole pine (Pinus contorta var. latifolia) and Engelmann spruce (Picea engelmannii) trees. The emissions were collected onto scent traps, containing 110 mg of Porapak Q sorbent, using PAS-500 micro air samplers set to a 0.4 mL/min flow rate for two hours. After collection, the scent traps were spiked with a recovery standard, perdeutrated decane, and extracted with 1.5 mL hexanes (in three portions). The analytes in the extracts were separated and detected using gas chromatography/mass spectroscopy. The analytes were identified and quantified using calibration curves from authentic standards, and when authentic standards were not available, the NIST mass spectra library and Adams retention time indices were used. The samples from lodgepole pine trees suggest an enhancement in the 3-carene, beta-phellandrene, and estragole (methyl chavicol) emissions upon bark beetle infestation. The samples from the Engelmann spruce trees suggest an enhancement in the 1,4-cineole, p-cymene, and beta-phellandrene emissions upon bark beetle infestation. A shift in the type and the quantity of VOC emissions due to bark beetle infestation may lead increases in SOA from these forests, since potent SOA precursors are produced.

  13. Experiment to Characterize Aircraft Volatile Aerosol and Trace-Species Emissions (EXCAVATE)

    NASA Technical Reports Server (NTRS)

    Anderson, B. E.; Branham, H.-S.; Hudgins, C. H.; Plant, J. V.; Ballenthin, J. O.; Miller, T. M.; Viggiano, A. A.; Blake, D. R.; Boudries, H.; Canagaratna, M.

    2005-01-01

    The Experiment to Characterize Aircraft Volatile and Trace Species Emissions (EXCAVATE) was conducted at Langley Research Center (LaRC) in January 2002 and focused upon assaying the production of aerosols and aerosol precursors by a modern commercial aircraft, the Langley B757, during ground-based operation. Remaining uncertainty in the postcombustion fate of jet fuel sulfur contaminants, the need for data to test new theories of particle formation and growth within engine exhaust plumes, and the need for observations to develop air quality models for predicting pollution levels in airport terminal areas were the primary factors motivating the experiment. NASA's Atmospheric Effects of Aviation Project (AEAP) and the Ultra Effect Engine Technology (UEET) Program sponsored the experiment which had the specific objectives of determining ion densities; the fraction of fuel S converted from S(IV) to S(VI); the concentration and speciation of volatile aerosols and black carbon; and gas-phase concentrations of long-chain hydrocarbon and PAH species, all as functions of engine power, fuel composition, and plume age.

  14. Precursor gases of aerosols in the Mount St. Helens eruption plumes at stratospheric altitudes

    NASA Technical Reports Server (NTRS)

    Inn, E. C. Y.; Vedder, J. F.; Condon, E. P.; Ohara, D.

    1982-01-01

    Nineteen stratospheric samples from the eruption plumes of Mount St. Helens were collected in five flight experiments. The plume samples were collected at various altitudes from 13.1 to 20.7 km by using the Ames cryogenic sampling system on board the NASA U-2 aircraft. The enriched, cryogenically collected samples were analyzed by chromatography. The concentrations of aerosols precursor gases (OCS, SO2, and CS2), CH3Cl, N2O, CF2Cl2, and CFCl3 were measured by gas chromatography. Large enhancement of the mixing ratio of SO2 and moderate enhancement of CS2 and OCS were found in the plume samples compared with similar measurement under pre-volcanic conditions. A fast decay rate of the SO2 mixing ratio in the plume was observed. Measurement of Cl(-), SO2(2-), and NO3(-) by ion chromatography was also carried out on water solutions prepared from the plume samples. The results obtained with this technique imply large mixing ratios of HCl, (NO + NO2 + HNO3), and SO2, in which these constituents are the respective sources of the anions. Measurement of the Rn222 concentration in the plume was made. Other stratospheric constituents in the plume samples, such as H2O, CO2, CH4, and CO, were also observed.

  15. Soot aggregate restructuring due to coatings of secondary organic aerosol derived from aromatic precursors.

    PubMed

    Schnitzler, Elijah G; Dutt, Ashneil; Charbonneau, André M; Olfert, Jason S; Jäger, Wolfgang

    2014-12-16

    Restructuring of monodisperse soot aggregates due to coatings of secondary organic aerosol (SOA) derived from hydroxyl radical-initiated oxidation of toluene, p-xylene, ethylbenzene, and benzene was investigated in a series of photo-oxidation (smog) chamber experiments. Soot aggregates were generated by combustion of ethylene using a McKenna burner, treated by denuding, size-selected by a differential mobility analyzer, and injected into a smog chamber, where they were exposed to low vapor pressure products of aromatic hydrocarbon oxidation, which formed SOA coatings. Aggregate restructuring began once a threshold coating mass was reached, and the degree of the subsequent restructuring increased with mass growth factor. Although significantly compacted, fully processed aggregates were not spherical, with a mass-mobility exponent of 2.78, so additional SOA was required to fill indentations between collapsed branches of the restructured aggregates before the dynamic shape factor of coated particles approached 1. Trends in diameter growth factor, effective density, and dynamic shape factor with increasing mass growth factor indicate distinct stages in soot aggregate processing by SOA coatings. The final degree and coating mass dependence of soot restructuring were found to be the same for SOA coatings from all four aromatic precursors, indicating that the surface tensions of the SOA coatings are similar. PMID:25390075

  16. Aerosol assisted chemical vapour deposition of Cu-ZnO composite from single source precursors.

    PubMed

    Shahid, Muhammad; Mazhar, Muhammad; Hamid, Mazhar; O'Brien, Paul; Malik, Mohammad A; Helliwell, Madeleine; Raftery, James

    2009-07-28

    Two heterobimetallic precursors [Zn(TFA)3(micro-OH)Cu3(dmae)3Cl].THF (1) and [Zn(TFA)4Cu3(dmae)4] (2) [dmae=N,N-dimethylaminoethanolate and TFA=trifluoroacetate], have been synthesized and characterized by their melting points, elemental analysis, FT-IR spectroscopy, mass spectrometry, TGA and single crystal X-ray diffraction methods. Both complexes were used to deposit thin films of Cu-ZnO composite on glass substrates by aerosol assisted chemical vapor deposition (AACVD) method. The films were characterized by "scotch tape" test for adhesion, thickness measurement as a function of temperature, EDX for composition, SEM for surface morphology and XRD for crystalline phases. Thin film deposition studies at 250, 325, 400, 475 degrees C indicated the increase in thickness with temperature reaching a maximum at 400 degrees C and then decreasing. EDX and PXRD results showed the uniform distribution of cubic metallic copper and hexagonal zinc oxide phases which make them useful for nanocatalysis on structured surfaces. PMID:19587992

  17. Soot aggregate restructuring due to coatings of secondary organic aerosol derived from aromatic precursors.

    PubMed

    Schnitzler, Elijah G; Dutt, Ashneil; Charbonneau, André M; Olfert, Jason S; Jäger, Wolfgang

    2014-12-16

    Restructuring of monodisperse soot aggregates due to coatings of secondary organic aerosol (SOA) derived from hydroxyl radical-initiated oxidation of toluene, p-xylene, ethylbenzene, and benzene was investigated in a series of photo-oxidation (smog) chamber experiments. Soot aggregates were generated by combustion of ethylene using a McKenna burner, treated by denuding, size-selected by a differential mobility analyzer, and injected into a smog chamber, where they were exposed to low vapor pressure products of aromatic hydrocarbon oxidation, which formed SOA coatings. Aggregate restructuring began once a threshold coating mass was reached, and the degree of the subsequent restructuring increased with mass growth factor. Although significantly compacted, fully processed aggregates were not spherical, with a mass-mobility exponent of 2.78, so additional SOA was required to fill indentations between collapsed branches of the restructured aggregates before the dynamic shape factor of coated particles approached 1. Trends in diameter growth factor, effective density, and dynamic shape factor with increasing mass growth factor indicate distinct stages in soot aggregate processing by SOA coatings. The final degree and coating mass dependence of soot restructuring were found to be the same for SOA coatings from all four aromatic precursors, indicating that the surface tensions of the SOA coatings are similar.

  18. Carbon and Aerosol Emissions from Biomass Fires in Mexico

    NASA Astrophysics Data System (ADS)

    Hao, W. M.; Flores Garnica, G.; Baker, S. P.; Urbanski, S. P.

    2009-12-01

    Biomass burning is an important source of many atmospheric greenhouse gases and photochemically reactive trace gases. There are limited data available on the spatial and temporal extent of biomass fires and associated trace gas and aerosol emissions in Mexico. Biomass burning is a unique source of these gases and aerosols, in comparison to industrial and biogenic sources, because the locations of fires vary considerably both daily and seasonally and depend on human activities and meteorological conditions. In Mexico, the fire season starts in January and about two-thirds of the fires occur in April and May. The amount of trace gases and aerosols emitted by fires spatially and temporally is a major uncertainty in quantifying the impact of fire emissions on regional atmospheric chemical composition. To quantify emissions, it is necessary to know the type of vegetation, the burned area, the amount of biomass burned, and the emission factor of each compound for each ecosystem. In this study biomass burning experiments were conducted in Mexico to measure trace gas emissions from 24 experimental fires and wildfires in semiarid, temperate, and tropical ecosystems from 2005 to 2007. A range of representative vegetation types were selected for ground-based experimental burns to characterize fire emissions from representative Mexico fuels. A third of the country was surveyed each year, beginning in the north. The fire experiments in the first year were conducted in Chihuahua, Nuevo Leon, and Tamaulipas states in pine forest, oak forest, grass, and chaparral. The second-year fire experiments were conducted on pine forest, oak forest, shrub, agricultural, grass, and herbaceous fuels in Jalisco, Puebla, and Oaxaca states in central Mexico. The third-year experiments were conducted in pine-oak forests of Chiapas, coastal grass, and low subtropical forest on the Yucatan peninsula. FASS (Fire Atmosphere Sampling System) towers were deployed for the experimental fires. Each FASS

  19. Chemical composition of emissions from urban sources of fine organic aerosol

    SciTech Connect

    Hildemann, L.M.; Markowski, G.R.; Cass, G.R. )

    1991-04-01

    A dilution source sampling system was used to collect primary fine aerosol emissions from important sources of urban organic aerosol, including a boiler burning No. 2 fuel oil, a home fireplace, a fleet of catalyst-equipped and noncatalyst automobiles, heavy-duty diesel trucks, natural gas home appliances, and meat cooking operations. Alternative dilution sampling techniques were used to collect emissions from cigarette smoking and a roofing tar pot, and grab sample techniques were employed to characterize paved road dust, brake lining wear, and vegetative detritus. Organic aerosol constituted the majority of the fine aerosol mass emitted from many of the sources tested. Fine primary organic aerosol emissions within the heavily urbanized western portion of the Los Angeles Basin were determined to total 29.8 metric ton/day. Over 40% of these organic aerosol emissions are from anthropogenic pollution sources that are expected to emit contemporary (nonfossil) aerosol carbon, in good agreement with the available ambient monitoring data.

  20. Formation of brown carbon via reactions of ammonia with secondary organic aerosols from biogenic and anthropogenic precursors

    NASA Astrophysics Data System (ADS)

    Updyke, Katelyn M.; Nguyen, Tran B.; Nizkorodov, Sergey A.

    2012-12-01

    Filter samples of secondary organic aerosols (SOA) generated from the ozone (O3)- and hydroxyl radical (OH)-initiated oxidation of various biogenic (isoprene, α-pinene, limonene, α-cedrene, α-humulene, farnesene, pine leaf essential oils, cedar leaf essential oils) and anthropogenic (tetradecane, 1,3,5-trimethylbenzene, naphthalene) precursors were exposed to humid air containing approximately 100 ppb of gaseous ammonia (NH3). Reactions of SOA compounds with NH3 resulted in production of light-absorbing "brown carbon" compounds, with the extent of browning ranging from no observable change (isoprene SOA) to visible change in color (limonene SOA). The aqueous phase reactions with dissolved ammonium (NH4+) salts, such as ammonium sulfate, were equally efficient in producing brown carbon. Wavelength-dependent mass absorption coefficients (MAC) of the aged SOA were quantified by extracting known amounts of SOA material in methanol and recording its UV/Vis absorption spectra. For a given precursor, the OH-generated SOA had systematically lower MAC compared to the O3-generated SOA. The highest MAC values, for brown carbon from SOA resulting from O3 oxidation of limonene and sesquiterpenes, were comparable to MAC values for biomass burning particles but considerably smaller than MAC values for black carbon aerosols. The NH3/NH4+ + SOA brown carbon aerosol may contribute to aerosol optical density in regions with elevated concentrations of NH3 or ammonium sulfate and high photochemical activity.

  1. Secondary Organic Aerosol Formation from Ultra-Low Super Ultra-Low and Partial Zero Emission Vehicle Exhaust

    NASA Astrophysics Data System (ADS)

    Robinson, A. L.; Zhao, Y.; Lambe, A. T.; Saleh, R.; Saliba, G.; Maldonado, H.; Sardar, S.; Frodin, B.; Drozd, G.; Goldstein, A. H.; Kroll, J. H.; Cross, E. S.; Franklin, J. P.

    2015-12-01

    Secondary organic aerosol (SOA) is the dominant component of organic aerosol in many urban areas during the summertime. On-road light duty gasoline vehicles (LDGV) have been indicated as a major source of SOA precursors. Emissions of the SOA-forming non methane hydrocarbons (NMHCs) from on-road LDGV have been substantially reduced along with more stringent emission standards, leading to reduced potential for SOA formation. However, recent smog chamber measurements reported that the reductions in SOA formation were less than those in NMHC emissions, indicating that newer, low emitting vehicles may emit a more efficient of SOA precursors. Vehicles that meet the ultra-low, super ultra-low and partial zero emission standards have substantially lower NMHC emissions than vehicles tested in past studies. To better understand the effects of more stringent emission controls on the SOA formation, we conducted experiments 13 vehicles recruited from the Southern California vehicle fleet (five ultra-low emission vehicles, four super ultra-low emission vehicles and four partial zero emission vehicles) at the California Air Resources Board Haagen-Smit Laboratory. In addition, we investigated several vehicles compliant with older emission standards have also been investigated here to bridge the previous studies. Dilute vehicle exhaust were photo-oxidized in a smog chamber with the VOC-to-NOx ratio adjusted to simulate the photochemistry in urban air. Application of literature data from single-ring aromatic compounds cannot explain the observed SOA during chamber experiments. The average ratios between estimated and measured SOA for vehicles under different emission standards ranged from 0.04 to 0.71. Comprehensive measurements of SOA precursor emissions were made, including NMHCs, intermediate volatility and semi-volatile organic compounds. This study presents results of SOA production from these low emitting vehicles and compares the results with recently published data. This

  2. Emissions of Black Carbon Aerosols from Alaskan Boreal Forest Wildfires

    NASA Astrophysics Data System (ADS)

    Mouteva, G.; Fahrni, S. M.; Rogers, B. M.; Wiggins, E. B.; Santos, G.; Czimczik, C. I.; Randerson, J. T.

    2014-12-01

    Boreal wildfires are a major source of carbonaceous aerosols. Emissions from wildfires in Alaska represent ~ 33% of all open biomass combustion emissions of black carbon (BC) in the United States. BC contributes to atmospheric warming and accelerates melting of ice and snow. With fire frequency and burned area projected to increase in boreal regions, BC has the potential to become an important positive feedback to climate change. Quantifying the emissions, constraining the sources and better understanding the transportation patterns of BC to the polar regions are therefore critical for constraining the strength of this feedback. We present results from direct measurements of BC from wildfires in Alaska during the summer of 2013 collected as a part of NASA's Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) campaign. Fine aerosol particulate matter (PM2.5) was collected at two locations: Caribou-Poker Creek Research Watershed and Delta Junction Agricultural and Forestry Experimental Site. Using a Sunset OCEC analyzer, we separated BC from organic carbon aerosols, measured concentrations and analyzed the radiocarbon (14C) content with accelerator mass spectrometry. We also analyzed the total carbon (C) and nitrogen (N) elemental and stable isotope composition of the bulk PM2.5 with EA-IRMS. We compared the temporal dynamics of BC concentrations and isotopic composition with active fire/thermal anomaly information from MODIS. Our results show that boreal forest fire emissions in interior Alaska increased BC concentrations by up to an order of magnitude above background levels. The mean Δ14C value of fire-emitted BC was 120‰ with a range of +99‰ to +149‰ after correcting for contributions from background BC. This range was in good agreement with measurements of the depth of burn in soil organic carbon layers from interior wildland fires, and Δ14C profiles. High fire periods also corresponded to elevated C:N ratios. The δ15N of the aerosols was

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  4. Marine Primary and Secondary Aerosol emissions related to seawater biogeochemistry

    NASA Astrophysics Data System (ADS)

    Sellegri, Karine; D'Anna, Barbara; Marchand, Nicolas; Charriere, Bruno; Sempere, Richard; Mas, Sebastien; Schwier, Allison; Rose, Clémence; Pey, Jorge; Langley Dewitt, Helen; Même, Aurélie; R'mili, Badr; George, Christian; Delmont, Anne

    2014-05-01

    Marine aerosol contributes significantly to the global aerosol load and consequently has an important impact on both the Earth's albedo and climate. Different factors influence the way they are produced from the sea water and transferred to the atmosphere. The sea state (whitecap coverage) and sea temperature influence the size and concentration of primarily produced particles but also biogeochemical characteristics of the sea water may influence both the physical and chemical fluxes. In order to study marine emissions, one approach is to use semicontrolled environments such as mesocosms. Within the SAM project (Sources of marine Aerosol in the Mediterranean), we characterize the primary Sea Salt Aerosol (SSA) and Secondary aerosol formation by nucleation during mesocosms experiments performed in May 2013 at the Oceanographic and Marine Station STARESO in western Corsica. We followed both water and air characteristics of three mesocosms containing an immerged part filled with 3,3 m3 of sea water and an emerged part filled with filtered natural air. Mesocosms were equipped with a pack of optical and physicochemical sensors and received different treatments: one of these mesocosms was left unchanged as control and the two others were enriched by addition of nitrates and phosphates respecting Redfield ratio (N:P = 16) in order to create different levels of phytoplanctonic activities. The set of sensors in each mesocosm was allowed to monitor the water temperature, conductivity, pH, incident light, fluorescence of chlorophyll a, and dissolved oxygen concentration. The mesocosms waters were daily sampled for chemical and biological (dissolved organic matter (i.e. DOC and CDOM), particulate matter and related polar compounds, transparent polysaccharides and nutrients concentration) and biological (chlorophyll a, virus, bacteria, phytoplankton and zooplankton concentrations) analyses. Secondary new particle formation was followed on-line in the emerged parts of the

  5. 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

  6. Real-Time Observations of Secondary Aerosol Formation and Aging from Different Emission Sources and Environments

    NASA Astrophysics Data System (ADS)

    Ortega, A. M.; Palm, B. B.; Hayes, P. L.; Day, D. A.; Cubison, M.; Brune, W. H.; Hu, W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Rappenglueck, B.; Bon, D.; Graus, M.; Warneke, C.; Gilman, J.; Kuster, W.; De Gouw, J. A.; Jimenez, J. L.

    2013-12-01

    To investigate atmospheric processing of direct urban and wildfire emissions, we deployed a photochemical flow reactor (Potential Aerosol Mass, PAM) with submicron aerosol size and chemical composition measurements during FLAME-3, a biomass-burning study at USDA Fire Sciences Laboratory in Missoula, MT, and CalNex, a field study investigating the nexus of air quality and climate change at a receptor site in the LA-Basin at Pasadena, CA. The reactor produces OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent aging of ~2 weeks in 5 minutes of processing. The OH exposure (OHexp) was stepped every 20 min in both field studies. Results show the value of this approach as a tool for in-situ evaluation of changes in OA concentration and composition due to photochemical processing. In FLAME-3, the average OA enhancement factor was 1.42 × 0.36 of the initial POA. Reactive VOCs, such as toluene, monoterpenes, and acetaldehyde, decreased with increased OHexp; however, formic acid, acetone, and some unidentified OVOCs increased after significant exposure. Net SOA formation in the photochemical reactor increased with OHexp, typically peaking around 3 days of equivalent atmospheric photochemical age (OHexp ~3.9e11 molecules cm-3 s), then leveling off at higher exposures. Unlike other studies, no decrease in OA is observed at high exposure, likely due to lower max OHexp in this study due to very high OH reactivity. The amount of additional OA mass added from aging is positively correlated with initial POA concentration, but not with the total VOC concentration or the concentration of known SOA precursors. The mass of SOA formed often exceeded the mass of the known VOC precursors, indicating the likely importance of primary semivolatile/intermediate volatility species, and possibly of unidentified VOCs as SOA precursors in biomass burning smoke. Results from CalNex show enhancement of OA and inorganic aerosol from gas-phase precursors

  7. Acceleration of acoustical emission precursors preceding failure in sheared granular material

    NASA Astrophysics Data System (ADS)

    Johnson, P. A.; Kaproth, B. M.; Scuderi, M.; Ferdowsi, B.; Griffa, M.; Carmeliet, J.; Guyer, R. A.; Le Bas, P.; Trugman, D.; Ben Naim, E.; Daub, E. G.; Marone, C.

    2013-12-01

    Earthquake precursor observations are becoming progressively more widespread as instrumentation improves, in particular for interplate earthquakes (e.g., Bouchon et al., Nature Geoscience, 2013). One question regarding precursor behavior is whether or not they are due to a triggering cascade where one precursor triggers the next, or if they are independent events resulting from slow slip. We investigate this topic in order to characterize the physics of precursors, by applying laboratory experiments of sheared granular media in a bi-axial configuration. We sheared layers of glass beads under applied normal loads of 2-8 MPa, shearing rates of 5-10 μm/s at room temperature and humidity. We show that above ~ 3 MPa load, precursors are manifest by an exponential increase in time of the acoustic emission (AE), with an additional acceleration of event rate leading to the primary stick-slip failure event. The recorded AE are clearly correlated with small drops in shear stress during slow slip prior to the main stick-slip failure. Event precursors take place where the material is still modestly dilating, yet while the macroscopic frictional strength is no longer increasing. The precursors are of order 100x smaller in recorded strain amplitude than the stick-slip events. We are currently working on statistical methods to determine whether or not the precursors are triggered cascades. [reference: Bouchon et al., (2013) Nature Geoscience 6, 299-302 doi:10.1038/ngeo1770].

  8. Anomalous radon emission as precursor of medium to strong earthquakes

    NASA Astrophysics Data System (ADS)

    Zoran, Maria

    2016-03-01

    Anomalous radon (Rn222) emissions enhanced by forthcoming earthquakes is considered to be a precursory phenomenon related to an increased geotectonic activity in seismic areas. Rock microfracturing in the Earth's crust preceding a seismic rupture may cause local surface deformation fields, rock dislocations, charged particle generation and motion, electrical conductivity changes, radon and other gases emission, fluid diffusion, electrokinetic, piezomagnetic and piezoelectric effects as well as climate fluctuations. Space-time anomalies of radon gas emitted in underground water, soil and near the ground air weeks to days in the epicentral areas can be associated with the strain stress changes that occurred before the occurrence of medium and strong earthquakes. This paper aims to investigate temporal variations of radon concentration levels in air near or in the ground by the use of solid state nuclear track detectors (SSNTD) CR-39 and LR-115 in relation with some important seismic events recorded in Vrancea region, Romania.

  9. Emissions of biogenic volatile organic compounds and subsequent formation of secondary organic aerosols in a Larix kaempferi forest

    NASA Astrophysics Data System (ADS)

    Mochizuki, T.; Miyazaki, Y.; Ono, K.; Wada, R.; Takahashi, Y.; Saigusa, N.; Kawamura, K.; Tani, A.

    2015-10-01

    We conducted simultaneous measurements of concentrations and above-canopy fluxes of isoprene and α-pinene, along with their oxidation products in aerosols in a Larix kaempferi (Japanese larch) forest in summer 2012. Vertical profiles of isoprene showed the maximum concentration near the forest floor with a peak around noon, whereas oxidation products of isoprene, i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), showed higher concentrations near the canopy level of the forest. The vertical profile suggests large emissions of isoprene near the forest floor, likely due to Dryopteris crassirhizoma (a fern species), and the subsequent reaction within the canopy. The concentrations of α-pinene also showed highest values near the forest floor, with maximums in the early morning and late afternoon. The vertical profiles of α-pinene suggest its large emissions from soil and litter in addition to emissions from L. kaempferi leaves at the forest site. Isoprene and its oxidation products in aerosols exhibited similar diurnal variations within the forest canopy, providing evidence of secondary organic aerosol (SOA) formation via oxidation of isoprene most likely emitted from the forest floor. Although high abundance of α-pinene was observed in the morning, its oxidation products in aerosols showed peaks in daytime, due to a time lag between the emission and atmospheric reactions of α-pinene to form SOA. Positive matrix factorization (PMF) analysis indicated that anthropogenic influence is the most important factor contributing to the elevated concentrations of molecular oxidation products of isoprene- (> 64 %) and α-pinene-derived SOA (> 57 %). The combination of the measured fluxes and vertical profiles of biogenic volatile organic compounds (BVOCs) suggests that the inflow of anthropogenic precursors/aerosols likely enhanced the formation of both isoprene SOA and α-pinene SOA within the forest canopy even when the BVOC flux was relatively low. This study

  10. Effects of precursor concentration and acidic sulfate in aqueous glyoxal-OH radical oxidation and implications for secondary organic aerosol.

    PubMed

    Tan, Yi; Perri, Mark J; Seitzinger, Sybil P; Turpin, Barbara J

    2009-11-01

    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 microM) and the presence of acidic sulfate (0-840 microM) 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 microM), 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

  11. Effects of precursor concentration and acidic sulfate in aqueous glyoxal-OH radical oxidation and implications for secondary organic aerosol.

    PubMed

    Tan, Yi; Perri, Mark J; Seitzinger, Sybil P; Turpin, Barbara J

    2009-11-01

    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 microM) and the presence of acidic sulfate (0-840 microM) 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 microM), 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.

  12. High-time resolved measurements of biogenic and anthropogenic secondary organic aerosol precursors and products in urban air

    NASA Astrophysics Data System (ADS)

    Flores, Rosa M.; Doskey, Paul V.

    2016-04-01

    Volatile organic compounds (VOCs), which are present in the atmosphere entirely in the gas phase are directly emitted by biogenic (~1089 Tg yr-1) and anthropogenic sources (~185 Tg yr-1). However, the sources and molecular speciation of intermediate VOCs (IVOCs), which are for the most part also present almost entirely in the gas phase, are not well characterized. The VOCs and IVOCs participate in reactions that form ozone and semivolatile OC (SVOC) that partition into the aerosol phase. Formation and evolution of secondary organic aerosol (SOA) are part of a complex dynamic process that depends on the molecular speciation and concentration of VOCs, IVOCs, primary organic aerosol (POA), and the level of oxidants (NO3, OH, O3). The current lack of understanding of OA properties and their impact on radiative forcing, ecosystems, and human health is partly due to limitations of models to predict SOA production on local, regional, and global scales. More accurate forecasting of SOA production requires high-temporal resolution measurement and molecular characterization of SOA precursors and products. For the subject study, the IVOCs and aerosol-phase organic matter were collected using the high-volume sampling technique and were analyzed by multidimensional gas chromatography with time-of-flight mass spectrometry (GCxGC-ToFMS). The IVOCs included terpenes, terpenoids, n-alkanes, branched alkanes, isoprenoids, alkylbenzenes, cycloalkylbenzenes, PAH, alkyl PAH, and an unresolved complex mixture (UCM). Diurnal variations of OA species containing multiple oxygenated functionalities and selected SOA tracers of isorprene, α-pinene, toluene, cyclohexene, and n-dodecane oxidation were also quantified. The data for SOA precursor and oxidation products presented here will be useful for evaluating the ability of molecular-specific SOA models to forecast SOA production in and downwind of urban areas.

  13. Ammonia emissions in Europe, part II: How ammonia emission abatement strategies affect secondary aerosols

    NASA Astrophysics Data System (ADS)

    Backes, Anna M.; Aulinger, Armin; Bieser, Johannes; Matthias, Volker; Quante, Markus

    2016-02-01

    In central Europe, ammonium sulphate and ammonium nitrate make up a large fraction of fine particles which pose a threat to human health. Most studies on air pollution through particulate matter investigate the influence of emission reductions of sulphur- and nitrogen oxides on aerosol concentration. Here, we focus on the influence of ammonia (NH3) emissions. Emission scenarios have been created on the basis of the improved ammonia emission parameterization implemented in the SMOKE for Europe and CMAQ model systems described in part I of this study. This includes emissions based on future European legislation (the National Emission Ceilings) as well as a dynamic evaluation of the influence of different agricultural sectors (e.g. animal husbandry) on particle formation. The study compares the concentrations of NH3, NH4+, NO3 -, sulphur compounds and the total concentration of particles in winter and summer for a political-, technical- and behavioural scenario. It was found that a reduction of ammonia emissions by 50% lead to a 24% reduction of the total PM2.5 concentrations in northwest Europe. The observed reduction was mainly driven by reduced formation of ammonium nitrate. Moreover, emission reductions during winter had a larger impact than during the rest of the year. This leads to the conclusion that a reduction of the ammonia emissions from the agricultural sector related to animal husbandry could be more efficient than the reduction from other sectors due to its larger share in winter ammonia emissions.

  14. Uncertainties in global aerosols and climate effects due to biofuel emissions

    NASA Astrophysics Data System (ADS)

    Kodros, J. K.; Scott, C. E.; Farina, S. C.; Lee, Y. H.; L'Orange, C.; Volckens, J.; Pierce, J. R.

    2015-08-01

    Aerosol emissions from biofuel combustion impact both health and climate; however, while reducing emissions through improvements to combustion technologies will improve health, the net effect on climate is largely unconstrained. In this study, we examine sensitivities in global aerosol concentration, direct radiative climate effect, and cloud-albedo aerosol indirect climate effect to uncertainties in biofuel emission factors, optical mixing state, and model nucleation and background secondary organic aerosol (SOA). We use the Goddard Earth Observing System global chemical-transport model (GEOS-Chem) with TwO Moment Aerosol Sectional (TOMAS) microphysics. The emission factors include amount, composition, size, and hygroscopicity, as well as optical mixing-state properties. We also evaluate emissions from domestic coal use, which is not biofuel but is also frequently emitted from homes. We estimate the direct radiative effect assuming different mixing states (homogeneous, core-shell, and external) with and without absorptive organic aerosol (brown carbon). We find the global-mean direct radiative effect of biofuel emissions ranges from -0.02 to +0.06 W m-2 across all simulation/mixing-state combinations with regional effects in source regions ranging from -0.2 to +0.8 W m-2. The global-mean cloud-albedo aerosol indirect effect (AIE) ranges from +0.01 to -0.02 W m-2 with regional effects in source regions ranging from -1.0 to -0.05 W m-2. The direct radiative effect is strongly dependent on uncertainties in emissions mass, composition, emissions aerosol size distributions, and assumed optical mixing state, while the indirect effect is dependent on the emissions mass, emissions aerosol size distribution, and the choice of model nucleation and secondary organic aerosol schemes. The sign and magnitude of these effects have a strong regional dependence. We conclude that the climate effects of biofuel aerosols are largely unconstrained, and the overall sign of the aerosol

  15. Emission of sunscreen salicylic esters from desert vegetation and their contribution to aerosol formation

    NASA Astrophysics Data System (ADS)

    Matsunaga, S. N.; Guenther, A. B.; Potosnak, M. J.; Apel, E. C.

    2008-07-01

    Biogenic volatile organic compounds (BVOC) produced by plants are known to have an important role in atmospheric chemistry. However, our knowledge of the range of BVOCs produced by different plant processes is still expanding, and there remain poorly understood categories of BVOCs. In this study, emissions of a novel class of BVOC emissions were investigated in a desert region. Our study considered 8 species of common desert plants: blackbrush (Coleogyne ramosissima), desert willow (Chilopsis linearis), mesquite (Prosopis glandulosa), mondel pine (Pinus eldarica), pinyon pine (Pinus monophylla), cottonwood (Populus deltoides), saguaro cactus (Carnegiea gigantea) and yucca (Yucca baccata). The measurements focused on BVOCs with relatively high molecular weight (>C15) and/or an oxygenated functional group. Significantly high emission rates of two salicylic esters were found for blackbrush, desert willow and mesquite with emission rates of 1.4, 2.1 and 0.46 μgC dwg-1 h-1, respectively. The salicylic esters were identified as 2-ethylhexenyl salicylate (2-EHS) and 3,3,5-trimethylcyclohexenyl salicylate (homosalate) and are known as effective ultraviolet (UV) absorbers. We propose that the plants derive a protective benefit against UV radiation from the salicylic esters and that the emission process is driven by the physical evaporation of the salicylic esters due to the high ambient temperatures. In addition, the salicylic esters are predicted to be an effective precursor of secondary organic aerosol (SOA) because of their low vapor pressure due to a high number of carbon atoms (15 or 16) and the presence of three oxygen atoms. We estimated the contribution of the sunscreen esters themselves and their oxidation products on the SOA formation for the Las Vegas region using a BVOC emission model. The contribution was estimated to reach 90% of the biogenic SOA in the landscapes dominated by desert willow and mesquite and 25% in Las Vegas area.

  16. Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

    NASA Astrophysics Data System (ADS)

    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.; Fisher, J. A.; Travis, K.; Yu, K.; Hanisco, T. F.; Wolfe, G. M.; Arkinson, H. L.; Pye, H. O. T.; Froyd, K. D.; Liao, J.; McNeill, V. F.

    2016-02-01

    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 (γ) 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 on aerosol acidity and volume). The US Environmental Protection Agency (EPA) projects 2013-2025 decreases in anthropogenic emissions of

  17. Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign.

    PubMed

    Collier, Sonya; Zhou, Shan; Onasch, Timothy B; Jaffe, Daniel A; Kleinman, Lawrence; Sedlacek, Arthur J; Briggs, Nicole L; Hee, Jonathan; Fortner, Edward; Shilling, John E; Worsnop, Douglas; Yokelson, Robert J; Parworth, Caroline; Ge, Xinlei; Xu, Jianzhong; Butterfield, Zachary; Chand, Duli; Dubey, Manvendra K; Pekour, Mikhail S; Springston, Stephen; Zhang, Qi

    2016-08-16

    Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (∼2700 m a.s.l.) as well as near their sources using an aircraft. The regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), an index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (∼1 h old) and emissions sampled after atmospheric transport (6-45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. These results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate.

  18. Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign.

    PubMed

    Collier, Sonya; Zhou, Shan; Onasch, Timothy B; Jaffe, Daniel A; Kleinman, Lawrence; Sedlacek, Arthur J; Briggs, Nicole L; Hee, Jonathan; Fortner, Edward; Shilling, John E; Worsnop, Douglas; Yokelson, Robert J; Parworth, Caroline; Ge, Xinlei; Xu, Jianzhong; Butterfield, Zachary; Chand, Duli; Dubey, Manvendra K; Pekour, Mikhail S; Springston, Stephen; Zhang, Qi

    2016-08-16

    Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (∼2700 m a.s.l.) as well as near their sources using an aircraft. The regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), an index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (∼1 h old) and emissions sampled after atmospheric transport (6-45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. These results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate. PMID:27398804

  19. Measurement of elemental concentration of aerosols using spark emission spectroscopy†

    PubMed Central

    Diwakar, Prasoon K.

    2015-01-01

    A coaxial microelectrode system has been used to collect and analyse the elemental composition of aerosol particles in near real-time using spark emission spectroscopy. The technique involves focused electrostatic deposition of charged aerosol particles onto the flat tip of a microelectrode, followed by introduction of spark discharge. A pulsed spark discharge was generated across the electrodes with input energy ranging from 50 to 300 mJ per pulse, resulting in the formation of controlled pulsed plasma. The particulate matter on the cathode tip is ablated and atomized by the spark plasma, resulting in atomic emissions which are subsequently recorded using a broadband optical spectrometer for element identification and quantification. The plasma characteristics were found to be very consistent and reproducible even after several thousands of spark discharges using the same electrode system. The spark plasma was characterized by measuring the excitation temperature (~7000 to 10 000 K), electron density (~1016 cm−3), and evolution of spectral responses as a function of time. The system was calibrated using particles containing Pb, Si, Na and Cr. Absolute mass detection limits in the range 11 pg to 1.75 ng were obtained. Repeatability of spectral measurements varied from 2 to 15%. The technique offers key advantages over similar microplasma-based techniques such as laser-induced breakdown spectroscopy, as: (i) it does not require any laser beam optics and eliminates any need for beam alignment, (ii) pulse energy from dc power supply in SIBS system can be much higher compared to that from laser source of the same physical size, and (iii) it is quite conducive to compact, field-portable instrumentation. PMID:26491209

  20. Changes in future air quality, deposition, and aerosol-cloud interactions under future climate and emission scenarios

    NASA Astrophysics Data System (ADS)

    Glotfelty, Timothy; Zhang, Yang; Karamchandani, Prakash; Streets, David G.

    2016-08-01

    The prospect of global climate change will have wide scale impacts, such as ecological stress and human health hazards. One aspect of concern is future changes in air quality that will result from changes in both meteorological forcing and air pollutant emissions. In this study, the GU-WRF/Chem model is employed to simulate the impact of changing climate and emissions following the IPCC AR4 SRES A1B scenario. An average of 4 future years (2020, 2030, 2040, and 2050) is compared against an average of 2 current years (2001 and 2010). Under this scenario, by the Mid-21st century global air quality is projected to degrade with a global average increase of 2.5 ppb in the maximum 8-hr O3 level and of 0.3 μg m-3 in 24-hr average PM2.5. However, PM2.5 changes are more regional due to regional variations in primary aerosol emissions and emissions of gaseous precursor for secondary PM2.5. Increasing NOx emissions in this scenario combines with a wetter climate elevating levels of OH, HO2, H2O2, and the nitrate radical and increasing the atmosphere's near surface oxidation state. This differs from findings under the RCP scenarios that experience declines in OH from reduced NOx emissions, stratospheric recovery of O3, and increases in CH4 and VOCs. Increasing NOx and O3 levels enhances the nitrogen and O3 deposition, indicating potentially enhanced crop damage and ecosystem stress under this scenario. The enhanced global aerosol level results in enhancements in aerosol optical depth, cloud droplet number concentration, and cloud optical thickness. This leads to dimming at the Earth's surface with a global average reduction in shortwave radiation of 1.2 W m-2. This enhanced dimming leads to a more moderate warming trend and different trends in radiation than those found in NCAR's CCSM simulation, which does not include the advanced chemistry and aerosol treatment of GU-WRF/Chem and cannot simulate the impacts of changing climate and emissions with the same level of detailed

  1. Dust aerosol emission over the Sahara during summertime from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) observations

    NASA Astrophysics Data System (ADS)

    Todd, Martin C.; Cavazos-Guerra, Carolina

    2016-03-01

    Dust aerosols are an important component of the climate system and a challenge to incorporate into weather and climate models. Information on the location and magnitude of dust emission remains a key information gap to inform model development. Inadequate surface observations ensure that satellite data remain the primary source of this information over extensive and remote desert regions. Here, we develop estimates of the relative magnitude of active dust emission over the Sahara desert based on data from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). Utilising the unique vertical profile of aerosol characteristics provided by CALIOP our algorithm identifies emission from aerosol extinction and lidar backscatter in the near surface layers. From the long-term CALIOP archive of day and night-time orbits over 2006-13 we construct coarse resolution maps of a new dust emission index (DEI) for the Sahara desert during the peak summer dust season (June to September). The spatial structure of DEI indicates highest emission over a broad zone focused on the border regions of Southern Algeria, Northern Mali and northwest Niger, displaced substantially (∼7°) to the east of the mean maximum in satellite-derived aerosol optical depth. In this region night-time emission exceeds that during the day. The DEI maps substantially corroborate recently derived dust source frequency count maps based on back-tracking plumes in high temporal resolution SEVIRI imagery. As such, a convergence of evidence from multiple satellite data sources using independent methods provides an increasingly robust picture of Saharan dust emission sources. Various caveats are considered. As such, quantitative estimates of dust emission may require a synergistic combined multi-sensor analysis.

  2. Response of aerosol composition to different emission scenarios in Beijing, China.

    PubMed

    Zhang, Yingjie; Sun, Yele; Du, Wei; Wang, Qingqing; Chen, Chen; Han, Tingting; Lin, Jian; Zhao, Jian; Xu, Weiqi; Gao, Jian; Li, Jie; Fu, Pingqing; Wang, Zifa; Han, Yongxiang

    2016-11-15

    Understanding the response of aerosol chemistry to different emission scenarios is of great importance for air pollution mitigating strategies in megacities. Here we investigate the variations in air pollutants under three different emission scenarios, i.e., heating season, spring festival holiday and non-heating season using aerosol composition and gaseous measurements from 2 February to 1 April 2015 along with source apportionment and FLEXPART analysis in Beijing. Our results showed substantially different aerosol composition among three emission scenarios that is primarily caused by different emission sources. All aerosol and gas species showed ubiquitously higher concentrations in heating season than non-heating season with the largest enhancement for fossil OA (FOA) and chloride. On average, the particulate matter (PM) level in winter heating season can be enhanced by 70% due to coal combustion emissions. In contrast, cooking aerosols and traffic related species showed significant reductions as a response of reduced anthropogenic activities during the spring festival holiday, sulfate and secondary organic aerosol (SOA) however even increased due to enhanced aqueous-phase production. Such compensating effects resulted in small changes in PM levels for haze episodes during the holiday period despite reduced anthropogenic emissions. Our results have significant implications that local emission controls during winter severe pollution episodes can reduce primary aerosols substantially, but the mitigating effects can be significantly suppressed by enhanced secondary formation under stagnant meteorological conditions. PMID:27425439

  3. Transient Climate Impacts for Scenarios of Aerosol Emissions from Asia: A Story of Coal versus Gas

    NASA Astrophysics Data System (ADS)

    Grandey, B. S.; Cheng, H.; Wang, C.

    2014-12-01

    Projections of anthropogenic aerosol emissions are uncertain. In Asia, it is possible that emissions may increase if business continues as usual, with economic growth driving an increase in coal burning. But it is also possible that emissions may decrease rapidly due to the widespread adoption of cleaner technology or a shift towards non-coal fuels, such as natural gas. In this study, the transient climate impacts of three aerosol emissions scenarios are investigated: an RCP4.5 (Representative Concentration Pathway 4.5) control; a scenario with reduced Asian anthropogenic aerosol emissions; and a scenario with enhanced Asian anthropogenic aerosol emissions. A coupled atmosphere-ocean configuration of CESM (Community Earth System Model), including CAM5 (Community Atmosphere Model version 5), is used. Enhanced Asian aerosol emissions are found to delay global mean warming by one decade at the end of the century. Aerosol-induced suppression of the East Asian and South Asian summer monsoon precipitation occurs. The enhanced Asian aerosol emissions also remotely impact precipitation in other parts of the world: over the Sahel, West African monsoon precipitation is suppressed; and over Australia, austral summer monsoon precipitation is enhanced. These remote impacts on precipitation are associated with a southward shift of the ITCZ. The aerosol-induced sea surface temperature (SST) response appears to play an important role in the precipitation changes over South Asia and Australia, but not over East Asia. These results indicate that energy production in Asia, through the consequent aerosol emissions and associated radiative effects, might significantly influence future climate both locally and globally.

  4. Secondary organic aerosol formation from photo-oxidation of unburned fuel: experimental results and implications for aerosol formation from combustion emissions.

    PubMed

    Jathar, Shantanu H; Miracolo, Marissa A; Tkacik, Daniel S; Donahue, Neil M; Adams, Peter J; Robinson, Allen L

    2013-11-19

    We conducted photo-oxidation experiments in a smog chamber to investigate secondary organic aerosol (SOA) formation from eleven different unburned fuels: commercial gasoline, three types of jet fuel, and seven different diesel fuels. The goals were to investigate the influence of fuel composition on SOA formation and to compare SOA production from unburned fuel to that from diluted exhaust. The trends in SOA production were largely consistent with differences in carbon number and molecular structure of the fuel, i.e., fuels with higher carbon numbers and/or more aromatics formed more SOA than fuels with lower carbon numbers and/or substituted alkanes. However, SOA production from different diesel fuels did not depend strongly on aromatic content, highlighting the important contribution of large alkanes to SOA formation from mixtures of high carbon number (lower volatility) precursors. In comparison to diesels, SOA production from higher volatility fuels such as gasoline appeared to be more sensitive to aromatic content. On the basis of a comparison of SOA mass yields (SOA mass formed per mass of fuel reacted) and SOA composition (as measured by an aerosol mass spectrometer) from unburned fuels and diluted exhaust, unburned fuels may be reasonable surrogates for emissions from uncontrolled engines but not for emissions from engines with after treatment devices such as catalytic converters. PMID:24144104

  5. Secondary organic aerosol formation from photo-oxidation of unburned fuel: experimental results and implications for aerosol formation from combustion emissions.

    PubMed

    Jathar, Shantanu H; Miracolo, Marissa A; Tkacik, Daniel S; Donahue, Neil M; Adams, Peter J; Robinson, Allen L

    2013-11-19

    We conducted photo-oxidation experiments in a smog chamber to investigate secondary organic aerosol (SOA) formation from eleven different unburned fuels: commercial gasoline, three types of jet fuel, and seven different diesel fuels. The goals were to investigate the influence of fuel composition on SOA formation and to compare SOA production from unburned fuel to that from diluted exhaust. The trends in SOA production were largely consistent with differences in carbon number and molecular structure of the fuel, i.e., fuels with higher carbon numbers and/or more aromatics formed more SOA than fuels with lower carbon numbers and/or substituted alkanes. However, SOA production from different diesel fuels did not depend strongly on aromatic content, highlighting the important contribution of large alkanes to SOA formation from mixtures of high carbon number (lower volatility) precursors. In comparison to diesels, SOA production from higher volatility fuels such as gasoline appeared to be more sensitive to aromatic content. On the basis of a comparison of SOA mass yields (SOA mass formed per mass of fuel reacted) and SOA composition (as measured by an aerosol mass spectrometer) from unburned fuels and diluted exhaust, unburned fuels may be reasonable surrogates for emissions from uncontrolled engines but not for emissions from engines with after treatment devices such as catalytic converters.

  6. Measurement of the emission rate of an aerosol source--comparison of aerosol and gas transport coefficients.

    PubMed

    Bémer, D; Callé, S; Godinot, S; Régnier, R; Dessagne, J M

    2000-12-01

    A measuring method of the emission rate of an atmospheric pollutant source, based on the use of a tracer gas (helium) and developed in the case of a gaseous source, was tested for an aerosol source. The influence of both particle sedimentation and wall depositions was studied. The transport coefficients of the tracer gas and of alumina particles of various particle sizes (MMAD from 8 to 36 microns) were measured on a vertical axis close to the source, in a 71 m3 room swept by a piston flow. The measurements clearly demonstrated the predominant influence of sedimentation in the case of particles with aerodynamic diameters greater than 10 microns. Particle wall deposition was determined by measuring the gas and particle concentration decay in the ventilated room. To do this, a new tracing method using a fluorescent aerosol was developed. The measured aerosol deposition rates are much higher than those calculated from the formula of Corner for a cubical volume. Aerosol sedimentation and wall deposition are two phenomena limiting the use of a tracer gas to measure the aerosol emission rate. The chemical substances and materials used in work premises are likely to be released into the atmosphere and lead to the formation of pollutants. These emissions stem from either physical or chemical processes (evaporation of a solvent) or from mechanical processes (dispersion of oil droplets at the source of mists).

  7. [The research on remote sensing dust aerosol by using split window emissivity].

    PubMed

    Xu, Hui; Yu, Tao; Gu, Xing-Fa; Cheng, Tian-Hai; Xie, Dong-Hai; Liu, Qian

    2013-05-01

    Dust aerosol can cause the change in the land surface emissivity in split window by radiative forcing (RF). Firstly, the present paper explained from the microscopic point of view the extinction properties of dust aerosols in the 11 and 12 microm channels, and their influence on the land surface emissivity. Secondly, on April 29, 2011, in the northern region of Inner Mongolia a strong sandstorm outbroke, and based on the analysis of the changes in land surface emissivity, this paper proposed a dust identification method by using the variation of emissivity. At last, the dust identification result was evaluated by the dust monitoring product provided by the National Satellite Meteorological Center. The result shows that under the assumption that the 12 microm emissivity equals to 1, using 11 microm relative emissivity could identify dust cover region effectively, and the 11 microm relative emissivity to a certain extent represented the intensity information of dust aerosol.

  8. [The research on remote sensing dust aerosol by using split window emissivity].

    PubMed

    Xu, Hui; Yu, Tao; Gu, Xing-Fa; Cheng, Tian-Hai; Xie, Dong-Hai; Liu, Qian

    2013-05-01

    Dust aerosol can cause the change in the land surface emissivity in split window by radiative forcing (RF). Firstly, the present paper explained from the microscopic point of view the extinction properties of dust aerosols in the 11 and 12 microm channels, and their influence on the land surface emissivity. Secondly, on April 29, 2011, in the northern region of Inner Mongolia a strong sandstorm outbroke, and based on the analysis of the changes in land surface emissivity, this paper proposed a dust identification method by using the variation of emissivity. At last, the dust identification result was evaluated by the dust monitoring product provided by the National Satellite Meteorological Center. The result shows that under the assumption that the 12 microm emissivity equals to 1, using 11 microm relative emissivity could identify dust cover region effectively, and the 11 microm relative emissivity to a certain extent represented the intensity information of dust aerosol. PMID:23905316

  9. Urban stress-induced biogenic VOC emissions impact secondary aerosol formation in Beijing

    NASA Astrophysics Data System (ADS)

    Ghirardo, A.; Xie, J.; Zheng, X.; Wang, Y.; Grote, R.; Block, K.; Wildt, J.; Mentel, T.; Kiendler-Scharr, A.; Hallquist, M.; Butterbach-Bahl, K.; Schnitzler, J.-P.

    2015-08-01

    Trees can significantly impact the urban air chemistry by the uptake and emission of reactive biogenic volatile organic compounds (BVOCs), which are involved in ozone and particle formation. Here we present the emission potentials of "constitutive" (cBVOCs) and "stress-induced" BVOCs (sBVOCs) from the dominant broadleaf woody plant species in the megacity of Beijing. Based on an inventory of BVOC emissions and the tree census, we assessed the potential impact of BVOCs on secondary particulate matter formation in 2005 and 2010, i.e., before and after realizing the large tree-planting program for the 2008 Olympic Games. We found that sBVOCs, such as fatty acid derivatives, benzenoids and sesquiterpenes, constituted a significant fraction (∼ 15 %) of the total annual BVOC emissions, and we estimated that the overall annual BVOC budget may have doubled from ∼ 3.6 × 109 g C year-1 in 2005 to ∼ 7.1 × 109 g C year-1 in 2010 due to the increase in urban greens, while at the same time, the emission of anthropogenic VOCs (AVOCs) could be lowered by 24 %. Based on our BVOC emission assessment, we estimated the biological impact on SOA mass formation in Beijing. Compared to AVOCs, the contribution of biogenic precursors (2-5 %) for secondary particulate matter in Beijing was low. However, sBVOCs can significantly contribute (∼ 40 %) to the formation of total secondary organic aerosol (SOA) from biogenic sources; apparently, their annual emission increased from 1.05 μg m-3 in 2005 to 2.05 μg m-3 in 2010. This study demonstrates that biogenic and, in particular, sBVOC emissions contribute to SOA formation in megacities. However, the main problems regarding air quality in Beijing still originate from anthropogenic activities. Nevertheless, the present survey suggests that in urban plantation programs, the selection of plant species with low cBVOC and sBVOC emission potentials have some possible beneficial effects on urban air quality.

  10. Aerosol-assisted delivery of precursors for chemical vapour deposition: expanding the scope of CVD for materials fabrication.

    PubMed

    Marchand, Peter; Hassan, Iman A; Parkin, Ivan P; Carmalt, Claire J

    2013-07-14

    The production of thin films of materials has become the attention of a great deal of research throughout academia and industry worldwide owing to the array of applications which utilise them, including electronic devices, gas sensors, solar cells, window coatings and catalytic systems. Whilst a number of deposition techniques are in common use, chemical vapour deposition (CVD) is an attractive process for the production of a wide range of materials due to the control it offers over film composition, coverage and uniformity, even on large scales. Conventional CVD processes can be limited, however, by the need for suitably volatile precursors. Aerosol-assisted (AA)CVD is a solution-based process which relies on the solubility of the precursor, rather than its volatility and thus vastly extends the range of potentially applicable precursors. In addition, AACVD offers extra means to control film morphology and concurrently the properties of the deposited materials. In this perspective we discuss the AACVD process, the influence of deposition conditions on film characteristics and a number of materials and applications to which AACVD has been found beneficial. PMID:23629474

  11. Potential sensitivity of photosynthesis and isoprene emission to direct radiative effects of atmospheric aerosol pollution

    NASA Astrophysics Data System (ADS)

    Strada, S.; Unger, N.

    2015-09-01

    A global Earth system model is applied to quantify the impacts of direct anthropogenic aerosol effective radiative forcing on gross primary productivity (GPP) and isoprene emission. The impacts of different pollution aerosol sources (all anthropogenic, biomass burning and non-biomass burning) are investigated by performing sensitivity experiments. On the global scale, our results show that land carbon fluxes (GPP and isoprene emission) are not sensitive to pollution aerosols, even under a global decline in surface solar radiation (direct + diffuse) by ~ 9 %. At the regional scale, plant productivity (GPP) and isoprene emission show a robust but opposite sensitivity to pollution aerosols, in regions where complex canopies dominate. In eastern North America and Europe, anthropogenic pollution aerosols (mainly from non-biomass burning sources) enhance GPP by +8-12 % on an annual average, with a stronger increase during the growing season (> 12 %). In the Amazon basin and central Africa, biomass burning aerosols increase GPP by +2-5 % on an annual average, with a peak in the Amazon basin during the dry-fire season (+5-8 %). In Europe and China, anthropogenic pollution aerosols drive a decrease in isoprene emission of -2 to -12 % on the annual average. Anthropogenic aerosols affect land carbon fluxes via different mechanisms and we suggest that the dominant mechanism varies across regions: (1) light scattering dominates in the eastern US; (2) cooling in the Amazon basin; and (3) reduction in direct radiation in Europe and China.

  12. Potential emission flux to aerosol pollutants over Bengal Gangetic plain through combined trajectory clustering and aerosol source fields analysis

    NASA Astrophysics Data System (ADS)

    Kumar, D. Bharath; Verma, S.

    2016-09-01

    A hybrid source-receptor analysis was carried out to evaluate the potential emission flux to winter monsoon (WinMon) aerosols over Bengal Gangetic plain urban (Kolkata, Kol) and semi-urban atmospheres (Kharagpur, Kgp). This was done through application of fuzzy c-mean clustering to back-trajectory data combined with emission flux and residence time weighted aerosols analysis. WinMon mean aerosol optical depth (AOD) and angstrom exponent (AE) at Kol (AOD: 0.77; AE: 1.17) were respectively slightly higher than and nearly equal to that at Kgp (AOD: 0.71; AE: 1.18). Out of six source region clusters over Indian subcontinent and two over Indian oceanic region, the cluster mean AOD was the highest when associated with the mean path of air mass originating from the Bay of Bengal and the Arabian sea clusters at Kol and that from the Indo-Gangetic plain (IGP) cluster at Kgp. Spatial distribution of weighted AOD fields showed the highest potential source of aerosols over the IGP, primarily over upper IGP (e.g. Punjab, Haryana), lower IGP (e.g. Uttarpradesh) and eastern region (e.g. west Bengal, Bihar, northeast India) clusters. The emission flux contribution potential (EFCP) of fossil fuel (FF) emissions at surface (SL) of Kol/Kgp, elevated layer (EL) of Kol, and of biomass burning (BB) emissions at SL of Kol were primarily from upper, lower, upper/lower IGP clusters respectively. The EFCP of FF/BB emissions at Kgp-EL/SL, and that of BB at EL of Kol/Kgp were mainly from eastern region and Africa (AFR) clusters respectively. Though the AFR cluster was constituted of significantly high emission flux source potential of dust emissions, the EFCP of dust from northwest India (NWI) was comparable to that from AFR at Kol SL/EL.

  13. Effects of temperature on the formation of secondary organic aerosol from amine precursors

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Aerosol formation is directly influenced by meteorological properties such as temperature and relative humidity. Temperature, for example, directly affects the gas-to-particle partitioning of amine salts and semi-volatile organic amine products. These salts are formed in areas with high agricultur...

  14. Sensitivity of ozone to precursor emissions in urban Beijing with a Monte Carlo scheme

    NASA Astrophysics Data System (ADS)

    Tang, Xiao; Wang, Zifa; Zhu, Jiang; Gbaguidi, Alex E.; Wu, Qizhong; Li, Jie; Zhu, Tong

    2010-10-01

    In order to understand the formation mechanisms of high surface ozone and identify the main contributor sources in Beijing, this study investigates the sensitivity of surface ozone to NO, NO 2 and nine types of NMVOC emissions during a photochemical smog episode. Monte Carlo sensitivity analysis scheme with fifty simulations is established based on the Nested Air Quality Prediction Model System (NAQPMS). At every simulation, each of the eleven precursor emissions is perturbed with a distinct set of perturbations. The sensitivities of ozone to emissions are identified by multiple linear regressions. The stability of sensitivity results is validated by two experiments with standard deviations of log-normal perturbations set as 30% and 50% respectively. The sensitivity results suggest that the current high surface ozone is strongly stimulated by NMVOC emissions. Among NMVOC emissions, formaldehyde, ethylene and olefins emissions present the greatest impacts on ozone. On the other hand, NOx emissions have a strong inhibitory effect on ozone formation, even after 50% NOx emission reduction. This indicates that the current ozone formation in Beijing is under NOx-saturated conditions. A transition of ozone formation is observed from NOx-saturated to NOx-limited sensitivity behavior with a 75% reduction of NOx emissions. This study gives the implication that abatement of the four NMVOC types mentioned above could be efficient on reducing the high levels of surface ozone in central urban Beijing, while inadequate abatement in NOx emissions probably induces reverse effects.

  15. Satellite Characterization of Fire Emissions of Aerosols and Gases Relevant to Air-Quality Modeling

    NASA Astrophysics Data System (ADS)

    Ichoku, C. M.; Ellison, L.; Yue, Y.; Wang, J.

    2015-12-01

    Because of the transient and widespread nature of wildfires and other types of open biomass burning, satellite remote sensing has become an indispensable technique for characterizing their smoke emissions for modeling applications, especially at regional to global scales. Fire radiative energy (FRE), whose instantaneous rate of release or fire radiative power (FRP) is measurable from space, has been found to be proportional to both the biomass consumption and emission of aerosol particulate matter. We have leveraged this relationship to generate a global, gridded smoke-aerosol emission coefficients (Ce) dataset based on FRP and aerosol optical thickness (AOT) measurements from the MODIS sensors aboard the Terra and Aqua satellites. Ce is a simple coefficient to convert FRE to smoke aerosol emissions, in the same manner as traditional emission factors are used to convert burned biomass to emissions. The first version of this Fire Energetics and Emissions Research (FEER.v1) global gridded Ce product at 1°x1° resolution is available at http://feer.gsfc.nasa.gov/. Based on published emission ratios, the FEER.v1 Ce product for total smoke aerosol has also been used to generate similar products for specific fire-emitted aerosols and gases, including those that are regulated as 'criteria pollutants' under the US Environmental Protection Agency's National Ambient Air Quality Standards (NAAQS), such as particulate matter (PM) and carbon monoxide (CO). These gridded Ce products were used in conjunction with satellite measurements of FRP to derive emissions of several smoke constituents, which were applied to WRF-Chem fully coupled meteorology-chemistry-aerosol model simulations, with promising results. In this presentation, we analyze WRF-Chem simulations of surface-level concentrations of various pollutants based on FEER.v1 emission products to illustrate their value for air-quality modeling, particularly in parts of Africa and southeast Asia where ground-based air

  16. Importing ozone precursors and aerosols to the North American free troposphere: An analysis of peroxyacetyl nitrate and aerosol observations at Mount Bachelor

    NASA Astrophysics Data System (ADS)

    Fischer, Emily V.

    Exposure to aerosols and ozone poses a health threat to a large portion of the U.S. population. Domestic sources and a global background burden both contribute to ambient concentrations, and East Asia is currently a fast growing air pollution source. This dissertation presents results from two projects, and in each case observations from the Mount Bachelor Observatory (MBO, 43.980 N, 121.69° W; 2.7 km amsl) play a central role in the analysis. The first component of this dissertation presents an analysis of the first multi-year springtime measurements of peroxyacetyl nitrate (PAN) in the free troposphere over the Pacific Northwest. The measurements were made by gas chromatography with electron capture detector during spring 2008, 2009, and 2010. Springtime mean PAN mixing ratios at MBO varied from 100 pptv to 152 pptv. The observed relationship between PAN and 03 in a descending Asian air mass was used to derive an ozone production efficiency of 51-73 mol mol-1. I combined the observed variability in PAN and ozone at MBO with a range of trends to determine the observational requirements for trend detection. If springtime PAN mixing ratios increase at a rate of 4% per year due to rising Asian emissions, we would detect a trend with 13 years of measurements. If the corresponding trend in ozone is 1% per year, the trend in ozone will be detected on approximately the same timescale. The second component of this dissertation addresses the physical evolution of Asian aerosols and their impact on U.S. air quality. I showed that approximately 50% of the interannual variability in springtime average PM2.5 in remote areas of the U.S. Pacific Northwest can be explained by changes in Asian dust emissions. Next I identified 7 plumes of Asian origin within observations of sub --microm aerosol scattering and absorption from MBO. The average sub-microm scattering Angstrom exponent for the plumes was significantly larger than the same parameter observed closer to Asia, suggesting

  17. Effects of aerosol emission pathways on future warming and human health

    NASA Astrophysics Data System (ADS)

    Partanen, Antti-Ilari; Matthews, Damon

    2016-04-01

    The peak global temperature is largely determined by cumulative emissions of long-lived greenhouse gases. However, anthropogenic emissions include also so-called short-lived climate forcers (SLCFs), which include aerosol particles and methane. Previous studies with simple models indicate that the timing of SLCF emission reductions has only a small effect on the rate of global warming and even less of an effect on global peak temperatures. However, these simple model analyses do not capture the spatial dynamics of aerosol-climate interactions, nor do they consider the additional effects of aerosol emissions on human health. There is therefore merit in assessing how the timing of aerosol emission reductions affects global temperature and premature mortality caused by elevated aerosol concentrations, using more comprehensive climate models. Here, we used an aerosol-climate model ECHAM-HAMMOZ to simulate the direct and indirect radiative forcing resulting from aerosol emissions. We simulated Representative Concentration Pathway (RCP) scenarios, and we also designed idealized low and high aerosol emission pathways based on RCP4.5 scenario (LOW and HIGH, respectively). From these simulations, we calculated the Effective Radiative Forcing (ERF) from aerosol emissions between 1850 and 2100, as well as aerosol concentrations used to estimate the premature mortality caused by particulate pollution. We then use the University of Victoria Earth System Climate Model to simulate the spatial and temporal pattern of climate response to these aerosol-forcing scenarios, in combination with prescribed emissions of both short and long-lived greenhouse gases according to the RCP4.5 scenario. In the RCP scenarios, global mean ERF declined during the 21st century from -1.3 W m-2 to -0.4 W m-2 (RCP8.5) and -0.2 W m-2 (RCP2.6). In the sensitivity scenarios, the forcing at the end of the 21st century was -1.6 W m-2 (HIGH) and practically zero (LOW). The difference in global mean temperature

  18. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

    EPA Science Inventory

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles,...

  19. Assessment of ozone and PM-10 precursor emissions from the dairy industry

    SciTech Connect

    Schmidt, C.E.; Ungvarsky, J.; Winegar, E.

    1997-12-31

    Many new regulations have resulted in the need to assess and better understand a variety of industries with air emission sources that have not been studied in the past. The dairy industry is one such industry with area air emission sources that are now being studied for evaluation and ranking with the intent to control air emissions that exceed regulatory acceptance standards, especially for ozone precursors. The area sources at a dairy include facility processes such as dry feed lot, flushed lanes, settling ponds, liquid waste storage, waste windrows, cow washing area, milk parlor, dry cow area birthing area, feed storage, and livestock waste fertilizer usage areas. Given that these processes are area sources and dynamic and highly variable, assessment requires proper selection of measurement technology and innovative applications. Direct assessment flux chamber technology was used to assess the air emissions from dairies located in northern California. All process were screened and evaluated for testing, and all significant air emission sources were studied. A variety of compounds were studied in order to satisfy program objectives, including: volatile organic compounds, semi-volatile organic compounds, amine, ammonia, reduced sulfur compounds, aldehydes, ketones, and fixed gases. Analytical development work extending applicability of methods, such as EPA TO-14 for semi-volatile compounds, assessing total content was also conducted. This paper presents a summary of the assessment approach used to gain a better understanding of air emissions from livestock waste at California dairies. Data are presented as emission factors (per surface area and per head) and as emissions from various size dairies. These data were used to evaluate ozone and PM-10 precursor emissions from the dairy industry.

  20. Secondary Organic Aerosol from On- and Off-Road Combustion Emissions: Scientific and Policy Perspectives

    NASA Astrophysics Data System (ADS)

    Gordon, Timothy D.

    Combustion emissions from on-road sources such as light duty gasoline vehicles (LDGV), medium duty diesel vehicles (MDDV) and heavy duty diesel vehicles (HDDV) as well as small off-road engines (SORE) such those used in lawn and garden equipment are a major source of fine particulate matter (PM) pollution in the ambient atmosphere. Existing regulations have restricted direct PM emissions, especially for on-road sources; however, recent studies suggest that organic PM formed from the photo-oxidation of gaseous precursor emissions—so-called secondary organic aerosol (SOA)—contributes at least as much to the overall PM burden as PM "emitted from the tailpipe." A major limitation of many of these studies is that they attempt to induce from the behavior of simple emission surrogates (e.g., vaporized whole fuel) the behavior of actual combustion emissions from real world sources. This research investigates combustion emissions directly. The primary gas- and particle-phase emissions, SOA production and SOA yields from a range of different on-road and off-road combustion sources were characterized. LDGV, MDDV and HDDV were driven on chassis dynamometers over realistic, urban driving cycles. Off-road sources, including 2- and 4-stroke lawn and garden equipment and a diesel transportation refrigeration unit were tested using engine dynamometers operated over certification cycles. For nearly all gasoline engines (LDGV and SOREs), photo-oxidizing dilute combustion emissions for 3 hours produced at least as much SOA as the directly emitted primary PM. SOA increased net PM production for LDGV by a factor of 1-10, depending on the vehicle emission standard. SOA yields were found to increase with newer vehicles, which have lower primary emissions. SOA for diesel vehicles, while still large on an absolute basis, was a smaller fraction of the primary PM emissions (between 10-30%), due to the very high elemental carbon (EC) emissions from vehicles without diesel particulate

  1. Aerosol synthesis of nano and micro-scale zero valent metal particles from oxide precursors

    SciTech Connect

    Phillips, Jonathan; Luhrs, Claudia; Lesman, Zayd; Soliman, Haytham; Zea, Hugo

    2010-01-01

    In this work a novel aerosol method, derived form the batch Reduction/Expansion Synthesis (RES) method, for production of nano / micro-scale metal particles from oxides and hydroxides is presented. In the Aerosol-RES (A-RES) method, an aerosol, consisting of a physical mixture of urea and metal oxide or hydroxides, is passed through a heated oven (1000 C) with a residence time of the order of 1 second, producing pure (zero valent) metal particles. It appears that the process is flexible regarding metal or alloy identity, allows control of particle size and can be readily scaled to very large throughput. Current work is focused on creating nanoparticles of metal and metal alloy using this method. Although this is primarily a report on observations, some key elements of the chemistry are clear. In particular, the reducing species produced by urea decomposition are the primary agents responsible for reduction of oxides and hydroxides to metal. It is also likely that the rapid expansion that takes place when solid/liquid urea decomposes to form gas species influences the final morphology of the particles.

  2. Laboratory studies of oxidation of primary emissions: Oxidation of organic molecular markers and secondary organic aerosol production

    NASA Astrophysics Data System (ADS)

    Weitkamp, Emily A.

    vehicle markers. Aerosol composition is a key influence on reaction rate constants, perhaps more significant than external influences. Alkenoic acid concentrations in the meat grease particles appear to influence cholesterol oxidation rates. Also, the reaction rate constants for new motor oil were faster than those of the more viscous used motor oil. The measured reaction rate constants were used to oxidize source profiles that were subsequently run in the Chemical Mass Balance (CMB) model. Oxidizing the molecular markers in the meat-cooking profile led to unrealistically high meat-cooking aerosol contributions to the total organic carbon (OC), often more than 100%. This suggests that there is either unaccounted for sources of meat-cooking molecular markers in the ambient samples, or there is some property of atmospheric aerosols that significantly inhibits reaction that was not captured in this study. Oxidation of motor vehicle profiles led to both higher estimates of total vehicle OC and a quadrupling of gasoline OC, while the diesel contribution changed very little. The increase in gasoline OC changes gasoline vehicle emissions from a relatively minor source to a major one. Thus, oxidation of molecular markers can have a significant impact on receptor model predictions. The second objective was to investigate SOA formation from the photo-oxidation of whole diesel exhaust. Diluted exhaust from a diesel engine was photo-oxidized in a smog chamber to investigate SOA production. Photochemical oxidation rapidly produced significant SOA, almost doubling the organic aerosol contribution of primary emissions after several hours of processing. Less than 10% of the SOA mass could be explained using a SOA model and the measured oxidation of known precursors, such as light aromatics. However, the ultimate yield of SOA is uncertain because it is sensitive to treatment of particle and vapor losses to the chamber walls. Aerosol Mass Spectrometer (AMS) mass spectra reveal that the

  3. Airborne Observations of Aerosol Emissions from F-16 Aircraft

    NASA Technical Reports Server (NTRS)

    Anderson, B. E.; Cofer, W. R.; McDougal, D. S.

    1999-01-01

    We presented results from the SASS Near-Field Interactions Flight (SNIF-III) Experiment which was conducted during May and June 1997 in collaboration with the Vermont and New Jersey Air National Guard Units. The project objectives were to quantify the fraction of fuel sulfur converted to S(VI) species by jet engines and to gain a better understanding of particle formation and growth processes within aircraft wakes. Size and volatility segregated aerosol measurements along with sulfur species measurements were recorded in the exhaust of F-16 aircraft equipped with F-100 engines burning fuels with a range of fuel S concentrations at different altitudes and engine power settings. A total of 10 missions were flown in which F-16 exhaust plumes were sampled by an instrumented T-39 Sabreliner aircraft. On six of the flights, measurements were obtained behind the same two aircraft, one burning standard JP-8 fuel and the other either approximately 28 ppm or 1100 ppm S fuel or an equal mixture of the two (approximately 560 ppm S). A pair of flights was conducted for each fuel mixture, one at 30,000 ft altitude and the other starting at 35,000 ft and climbing to higher altitudes if contrail conditions were not encountered at the initial flight level. In each flight, the F-16s were operated at two power settings, approx. 80% and full military power. Exhaust emissions were sampled behind both aircraft at each flight level, power setting, and fuel S concentration at an initial aircraft separation of 30 m, gradually widening to about 3 km. Analyses of the aerosol data in the cases where fuel S was varied suggest results were consistent with observations from project SUCCESS, i.e., a significant fraction of the fuel S was oxidized to form S(VI) species and volatile particle emission indices (EIs) in comparably aged plumes exhibited a nonlinear dependence upon the fuel S concentration. For the high sulfur fuel, volatile particle EIs in 10-second-old-plumes were 2 to 3 x 10 (exp 17

  4. Future Arctic temperature change resulting from a range of aerosol emissions scenarios

    NASA Astrophysics Data System (ADS)

    Wobus, Cameron; Flanner, Mark; Sarofim, Marcus C.; Moura, Maria Cecilia P.; Smith, Steven J.

    2016-06-01

    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 from 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 SO2 emissions from the energy sector. Thus, long-term climate mitigation strategies that are focused on reducing carbon dioxide (CO2) emissions from the energy sector could generate short-term, aerosol-induced Arctic warming. 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 CO2 mitigation -- could potentially avoid some amount of short-term Arctic warming.

  5. CuInS2 Films Deposited by Aerosol-Assisted Chemical Vapor Deposition Using Ternary Single-Source Precursors

    NASA Technical Reports Server (NTRS)

    Jin, Michael; Banger, Kal; Harris, Jerry; Hepp, Aloysius

    2003-01-01

    Polycrystalline CuInS2 films were deposited by aerosol-assisted chemical vapor deposition using both solid and liquid ternary single-source precursors (SSPs) which were prepared in-house. Films with either (112) or (204/220) preferred orientation, had a chalcopyrite structure, and (112)-oriented films contained more copper than (204/220)-oriented films. The preferred orientation of the film is likely related to the decomposition and reaction kinetics associated with the molecular structure of the precursors at the substrate. Interestingly, the (204/220)-oriented films were always In-rich and were accompanied by a secondary phase. From the results of post-growth annealing, etching experiments, and Raman spectroscopic data, the secondary phase was identified as an In-rich compound. On the contrary, (112)-oriented films were always obtained with a minimal amount of the secondary phase, and had a maximum grain size of about 0.5 micron. Electrical and optical properties of all the films grown were characterized. They all showed p-type conduction with an electrical resistivity between 0.1 and 30 Omega-cm, and an optical band gap of approximately 1.46 eV +/- 0.02, as deposited. The material properties of deposited films revealed this methodology of using SSPs for fabricating chalcopyrite-based solar cells to be highly promising.

  6. CuInS2 Films Deposited by Aerosol-Assisted Chemical Vapor Deposition Using Ternary Single-Source Precursors

    NASA Technical Reports Server (NTRS)

    Jin, Michael H.-C.; Banger, Kulbinder K.; Harris, Jerry D.; Hepp, Aloysius F.

    2004-01-01

    Polycrystalline CuInS2 films were deposited by aerosol-assisted chemical vapor deposition using both solid and liquid ternary single-source precursors (SSPs) prepared in-house. Films with either (112) or (204/220) preferred orientation were obtained, and compositional analysis showed that (112)-oriented films contained more copper than (204/220)-oriented films. Using X-ray diffraction, the signature of chalcopyrite structure was often confirmed for (112)-oriented films. The preferred orientation of the film is likely related to the decomposition and reaction kinetics associated with the molecular structure of the precursors at the substrate. Interestingly, the (204/220)-oriented films were always accompanied by a secondary phase, which was identified as an unknown In-rich compound from the results of post-growth annealing, etching experiments, and Raman spectroscopic data. By increasing Cu to In ratio in the film, (112)-oriented films were obtained with a maximum grain size of about 0.5 micrometers, and their X-ray diffractions did not show any observable signature of the In secondary phase. Electrical and optical properties of all the films grown were characterized. They all showed p-type conduction with an electrical resistivity between 0.1 omega cm and 30 omega cm, and an optical band gap of 1.46eV +/- 0.02, as deposited. The material properties of deposited films revealed this methodology of using SSPs for fabricating chalcopyrite-based solar cells to be highly promising.

  7. The influence of ozone precursor emissions from four world regions on tropospheric composition and radiative climate forcing

    NASA Astrophysics Data System (ADS)

    Fry, Meridith M.; Naik, Vaishali; West, J. Jason; Schwarzkopf, M. Daniel; Fiore, Arlene M.; Collins, William J.; Dentener, Frank J.; Shindell, Drew T.; Atherton, Cyndi; Bergmann, Daniel; Duncan, Bryan N.; Hess, Peter; MacKenzie, Ian A.; Marmer, Elina; Schultz, Martin G.; Szopa, Sophie; Wild, Oliver; Zeng, Guang

    2012-04-01

    Ozone (O3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO42-). We examine changes in the tropospheric composition of O3, CH4, SO42- and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean ± 1 standard deviation) across multiple CTMs. We evaluate steady state O3responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 ± 0.6 to 1.7 ± 2 mWm-2/Tg N yr-1), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 ± 2 mWm-2 for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 ± 0.2 to -0.7 ± 0.2 mWm-2/Tg C yr-1) and CO emissions (-0.13 ± 0.02 to -0.15 ± 0.02 mWm-2/Tg CO yr-1). Including the effect of O3 on CO2 uptake by vegetation likely makes these net RFs more negative by -1.9 to -5.2 mWm-2/Tg N yr-1, -0.2 to -0.7 mWm-2/Tg C yr-1, and -0.02 to -0.05 mWm-2/Tg CO yr-1. Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO42-, regionally to hemispherically by O3, and globally by CH4. Global annual average SO42- responses to oxidant changes range from 0.4 ± 2.6 to -1.9 ± 1.3 Gg for NOxreductions, 0.1 ± 1.2 to -0.9 ± 0.8 Gg for NMVOC reductions, and -0.09 ± 0.5 to -0.9 ± 0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP100) are calculated for the global CH

  8. Global volcanic aerosol properties derived from emissions, 1990-2015, using CESM1(WACCM)

    NASA Astrophysics Data System (ADS)

    Mills, Michael; Schmidt, Anja; Easter, Richard; Solomon, Susan; Kinnison, Douglas; Ghan, Steven; Neely, Ryan; Marsh, Daniel; Conley, Andrew; Bardeen, Charles; Gettelman, Andrew

    2016-04-01

    Accurate representation of global stratospheric aerosols from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-losses that may be linked to volcanic activity. Attribution of climate variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the rate of global average temperature increases. We have compiled a database of volcanic SO2 emissions and plume altitudes for eruptions from 1990 to 2015, and developed a new prognostic capability for simulating stratospheric sulfate aerosols in the Community Earth System Model (CESM). We combined these with other non-volcanic emissions of sulfur sources to reconstruct global aerosol properties from 1990 to 2015. Our calculations show remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of stratospheric aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD calculations represent a clear improvement over available satellite-based analyses, which generally 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 calculations greatly improve on that provided for the Chemistry-Climate Model Initiative, which misses about 60% of the SAD measured in situ on average during both volcanically active and volcanically quiescent periods. The stark differences in SAOD and SAD compared to other data sets will have significant effects on calculations of the radiative forcing of climate and global stratospheric chemistry over the period 2005-2015. In light of these results, the impact of volcanic aerosols in reducing the rate of global average temperature increases since the year 2000 should be revisited. We have made our calculated aerosol properties from January 1990 to

  9. Potential sensitivity of photosynthesis and isoprene emission to direct radiative effects of atmospheric aerosol pollution

    NASA Astrophysics Data System (ADS)

    Strada, Susanna; Unger, Nadine

    2016-04-01

    A global Earth system model is applied to quantify the impacts of direct anthropogenic aerosol effective radiative forcing on gross primary productivity (GPP) and isoprene emission. The impacts of different pollution aerosol sources (anthropogenic, biomass burning, and non-biomass burning) are investigated by performing sensitivity experiments. The model framework includes all known light and meteorological responses of photosynthesis, but uses fixed canopy structures and phenology. On a global scale, our results show that global land carbon fluxes (GPP and isoprene emission) are not sensitive to pollution aerosols, even under a global decline in surface solar radiation (direct + diffuse) by ˜ 9 %. At a regional scale, GPP and isoprene emission show a robust but opposite sensitivity to pollution aerosols in regions where forested canopies dominate. In eastern North America and Eurasia, anthropogenic pollution aerosols (mainly from non-biomass burning sources) enhance GPP by +5-8 % on an annual average. In the northwestern Amazon Basin and central Africa, biomass burning aerosols increase GPP by +2-5 % on an annual average, with a peak in the northwestern Amazon Basin during the dry-fire season (+5-8 %). The prevailing mechanism varies across regions: light scattering dominates in eastern North America, while a reduction in direct radiation dominates in Europe and China. Aerosol-induced GPP productivity increases in the Amazon and central Africa include an additional positive feedback from reduced canopy temperatures in response to increases in canopy conductance. In Eurasia and northeastern China, anthropogenic pollution aerosols drive a decrease in isoprene emission of -2 to -12 % on an annual average. Future research needs to incorporate the indirect effects of aerosols and possible feedbacks from dynamic carbon allocation and phenology.

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

    SciTech Connect

    Gao, Yi; Liu, Xiaohong; Zhao, Chun; Zhang, Meigen

    2011-12-12

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

  11. The ISA-MIP Historical Eruption SO2 Emissions Assessment (HErSEA): an intercomparison for interactive stratospheric aerosol models

    NASA Astrophysics Data System (ADS)

    Mann, Graham; Dhomse, Sandip; Sheng, Jianxiong; Mills, Mike

    2016-04-01

    Major historical volcanic eruptions have injected huge amounts of sulphur dioxide into the stratosphere with observations showing an enhancement of the stratospheric aerosol layer for several years (ASAP, 2006). Such long-lasting increases in stratospheric aerosol loading cool the Earth's surface by scattering incoming solar radiation and warm the stratosphere via absorption of near infra-red solar and long-wave terrestrial radiation with complex effects on climate (e.g. Robock, 2000). Two recent modelling studies of Mount Pinatubo (Dhomse et al., 2014; Sheng et al. 2015) have highlighted that observations suggest the sulphur loading of the volcanically enhanced stratospheric aerosol may have been considerably lower than suggested by measurements of the injected SO2. This poster describes a new model intercomparison activity "ISA-MIP" for interactive stratospheric aerosol models within the framework of the SPARC initiative on Stratospheric Sulphur and its Role in Climate (SSiRC). The new "Historical Eruption SO2 emissions Assessment" (HErSEA) will intercompare model simulations of the three largest volcanic perturbations to the stratosphere in the last 50 years, 1963 Mt Agung, 1982 El Chichon and 1991 Mt Pinatubo. The aim is to assess how effectively the emitted SO2 translates into perturbations to stratospheric aerosol properties and simulated radiative forcings in different composition-climate models with interactive stratospheric aerosol (ISA). Each modelling group will run a mini-ensemble of transient AMIP-type runs for the 3 eruptions with a control no-eruption run followed by upper and lower bound injection amount estimates and 3 different injection height settings for two shallow (e.g. 19-21km amd 23-25km) and one deep (e.g. 19-25km) injection. First order analysis will intercompare stratospheric aerosol metrics such as 2D-monthly AOD(550nm, 1020nm) and timeseries of tropical and NH/SH mid-visible extinction at three different models levels (15, 20 and 25km

  12. Inverse relationship between the degree of oxidation of OOA (oxygenated organic aerosol) and the oxidant OX (O3 +NO2) due to biogenic emissions

    NASA Astrophysics Data System (ADS)

    Canonaco, F.; Slowik, J. G.; Baltensperger, U.; Prévôt, A. S. H.

    2014-11-01

    Aerosol chemical speciation monitor (ACSM) measurements were performed in Zurich, Switzerland for 13 months (February 2011 through February 2012). Many previous studies using this or related instruments have utilized the fraction of organic mass measured at m/z 44 (f44), which is typically dominated by the CO2+ ion and related to oxygenation, as an indicator of atmospheric aging. The current study demonstrates that during summer afternoons, when photochemical processes are most vigorous as indicated by high oxidant OX (O3+NO2), f44 for ambient SOA is not higher but is rather similar or lower than on days with low OX. This is likely due to the formation of semi-volatile oxygenated aerosol produced from biogenic precursor gases, whose emissions increase with ambient temperature. An additional observation is that in winter often higher f44 values in SOA are reached compared to summer. A possible cause could be aqueous processes associated with enhanced relative humidities and cloud cover in winter. The main changes in f44 for the summer case are discussed in the f44f43 space frequently used to interpret ACSM and aerosol mass spectrometer (AMS) data. In addition, source apportionment analyses conducted on winter and summer data using positive matrix factorization (PMF) yield semi-volatile oxygenated organic aerosol (SV-OOA) factors that retain source-related chemical information. Winter SV-OOA is highly influenced by biomass burning, whereas summer SV-OOA is to a high degree produced from biogenic precursor gases.

  13. Implications of the Temporal Resolution of Fire Emissions on Direct and Indirect Aerosol Effects

    NASA Astrophysics Data System (ADS)

    Darmenov, A.; Barahona, D.; Kim, K. M.; da Silva, A.; Colarco, P. R.; Govindaraju, R.

    2014-12-01

    Biomass burning is an important source of particulates and trace gases and a major element of the terrestrial carbon cycle. Well constrained emissions from open vegetation fires in both time and space are needed to model direct and indirect effect of biomass burning aerosols, homogeneous and heterogeneous chemistry in the atmosphere and perform credible integrated earth system analysis, climate and air pollution studies. However representing fires in regional and global numerical models is challenging because of the subgrid scales at which fire processes operate. An example of apparent discrepancy in scales is the use of monthly- or seasonal-mean fire emissions which given the stochastic nature of fires means that at certain spatial scales the temporal behavior of emissions becomes influenced by individual fire events and becomes more variable. The present study aims at investigating the impact of monthly-mean fire emissions on direct and indirect aerosol effects. Key element of our work is the use of fire radiative power (FRP) based emissions and a global fully interactive cloud-aerosol-radiation modeling system. We used the Goddard Earth Observing System Model, Version 5 (GEOS-5) with two moment cloud microphysics and explicit cloud droplet activation and ice nucleation. GEOS-5 is coupled with an online version of the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. Biomass burning emissions used in this study are from the Quick Fire Emission Dataset (QFED) available daily at up to 0.1 degrees horizontal resolution. We performed experiments with daily-mean and monthly-mean QFED emissions at two degree horizontal resolutions and report differences in aerosol burden and radiative forcing, for example we found that regional differences of clear-sky aerosol direct radiative effect at the surface and at the top of the atmosphere in MAM and JJA can be as high as 4 Wm-2 and 3 Wm-2, respectively.

  14. Ground and Airborne Aerosol Composition Measurements of California Coastal Chaparral Smoke Emissions

    NASA Astrophysics Data System (ADS)

    Craven, J. S.; Sorooshian, A.; Hersey, S. P.; Metcalf, A. R.; Schilling-Fahnestock, K.; Newman, S.; Akagi, S. K.; Taylor, J.; McMeeking, G.; Coe, H.; Tang, P.; Cocker, D. R., III; Yokelson, R. J.; Flagan, R. C.; Seinfeld, J.

    2014-12-01

    Wildfire smoke has large local to global pollution impacts. We present aerosol composition data from two fires in southern California. We measured organic aerosol (OA) of nascent and aged (4 h) smoke from the Williams Fire during the 2009 airborne San Luis Obispo Biomass Burning Campaign (SLOBB). The net ΔOA/ΔCO2 decreased by ~20%; however, positive matrix factorization (PMF) analysis of the organic mass spectra supports two factors that enable the OA emissions to be separated into fresh and oxidized OA. The Δfresh BBOA/ΔCO2 had a steeper decline than the ΔOA/ΔCO2 consistent with outgassing of semi-voltile organic compounds (SVOCs) due to dilution, whereas the Δoxidized BBOA/ΔCO2 increased from its initial value, consist with formation of secondary organic aerosol (SOA). We compare these fresh and oxidized mass spectral signatures, along with chaparral smoke samples measured in the Missoula Fire Lab, to ground-based aerosol measurements made during the Station Fire that occurred one month earlier than the Williams Fire during the Pasadena Aerosol Characterization Observatory Campaign (PACO). Night and daytime aerosol smoke emissions were sampled for one week during the Station Fire. Daytime organic aerosol smoke emissions exhibited larger variability both in mass concentration and composition than nighttime smoke emissions. Both levoglucosan and potassium, known biomass burning tracers, were measured and had distinct time series, supporting diversity in the flaming vs. smoldering initial burning conditions. Similar to the Williams Fire, PMF of the Station Fire mass spectra also reveal two biomass burning factors, one that is less oxidized and correlates strongly with levoglucosan measurements and one that is heavily oxidized and correlates in time with the potassium signal. These two campaigns have allowed us to probe fresh and oxidized smoke in both night and daytime conditions, and PMF results have revealed that at least two emission factors are useful to

  15. An estimate of the emission rate of primary fine aerosols from urban vegetation

    SciTech Connect

    Hildemann, L.M.; Rogge, W.F.; Cass, G.R.

    1995-12-31

    Analyses of ambient organic aerosol samples have shown a distribution of higher molecular weight n-alkanes that is characteristic of vegetation waxes. This suggests that plant waxes and other vegetative detritus may contribute significantly to airborne concentrations of particulate matter. However, to date no estimate has been made of the relative strength of vegetation as a source of primary aerosol emissions. In the present study, the n-alkanes present in the fine atmospheric aerosol of Los Angeles are utilized to deduce an upperbound estimate of the amount of fine vegetative detritus aerosol present. First the major known sources of fine organic aerosol in the Los Angeles area are characterized for n-alkanes via GC/MS. Then air quality modeling procedures are utilized to predict the n-alkane concentrations present in Los Angeles ambient air due to these major sources. By comparing these model predictions to actual ambient samples, the n-alkane mass in the ambient air that is not, accounted for by the known major source emissions can be determined. From this data, it is estimated that, at most, 0.2-1.0 micrograms per cubic meter of the fine aerosol in Los Angeles air could originate from primary vegetative detritus emissions - this corresponds to 1-3% of the total fine aerosol mass present in this urban atmosphere. The air quality model is also used to provide a first, upperbound estimate of the source emission strength of primary fine particulate emissions from urban vegetation. It is estimated that the vegetation present in every square kilometer of land within the heavily urbanized region of Los Angeles emits, at most, 300-900 grams of fine particulate matter per day. This upperbound estimate corresponds to a source emission strength for fine urban vegetative detritus of 1-4 grams per day per metric ton of leaf mass in Los Angeles.

  16. Kudzu (Pueraria montana) Invasion Doubles Emissions of Nitric Oxide, a Precursor to Tropospheric Ozone.

    NASA Astrophysics Data System (ADS)

    Hickman, J. E.; Wu, S.; Mickley, L. J.; Lerdau, M. T.

    2008-12-01

    Nitrogen-fixing plants can increase rates of nitrogen (N) cycling in soils, fluxes of the greenhouse gas nitrous oxide (N2O), and fluxes of the ozone precursor nitric oxide (NO). Invasion by the nitrogen-fixing legume kudzu (Pueraria montana) across millions of hectares in the southeastern United States could be contributing to increased ozone concentrations. Ozone formation in the Southeast is broadly limited by atmospheric NO concentrations, so perturbations to the N cycle by kudzu have the potential to increase ozone concentrations in the region. At three sites in Madison County, Georgia, kudzu invasion increased rates of net N mineralization by up to an order of magnitude and rates of net nitrification and soil pools of NO3- and NO2- by up to 500%. Emissions of NO from soils invaded by kudzu averaged 2.81 ng NO-N cm-2 h-1, significantly higher than emissions from soil dominated by native vegetation, which averaged 1.24 ng NO-N cm-2 h-1. Emissions of N2O display a trend towards increasing under kudzu invasion, but N2O emissions at these sites were three orders of magnitude smaller than emissions of NO. Atmospheric chemical modeling suggests that these higher NO emissions could increase ozone concentrations in the region by up to 2 ppb. We propose that kudzu invasion in the southeastern United States represents a novel threat to air quality and could increase the frequency with which federal ozone standards are exceeded.

  17. Primary gas- and particle-phase emissions and secondary organic aerosol production from gasoline and diesel off-road engines.

    PubMed

    Gordon, Timothy D; Tkacik, Daniel S; Presto, Albert A; Zhang, Mang; Jathar, Shantanu H; Nguyen, Ngoc T; Massetti, John; Truong, Tin; Cicero-Fernandez, Pablo; Maddox, Christine; Rieger, Paul; Chattopadhyay, Sulekha; Maldonado, Hector; Maricq, M Matti; Robinson, Allen L

    2013-12-17

    Dilution and smog chamber experiments were performed to characterize the primary emissions and secondary organic aerosol (SOA) formation from gasoline and diesel small off-road engines (SOREs). These engines are high emitters of primary gas- and particle-phase pollutants relative to their fuel consumption. Two- and 4-stroke gasoline SOREs emit much more (up to 3 orders of magnitude more) nonmethane organic gases (NMOGs), primary PM and organic carbon than newer on-road gasoline vehicles (per kg of fuel burned). The primary emissions from a diesel transportation refrigeration unit were similar to those of older, uncontrolled diesel engines used in on-road vehicles (e.g., premodel year 2007 heavy-duty diesel trucks). Two-strokes emitted the largest fractional (and absolute) amount of SOA precursors compared to diesel and 4-stroke gasoline SOREs; however, 35-80% of the NMOG emissions from the engines could not be speciated using traditional gas chromatography or high-performance liquid chromatography. After 3 h of photo-oxidation in a smog chamber, dilute emissions from both 2- and 4-stroke gasoline SOREs produced large amounts of semivolatile SOA. The effective SOA yield (defined as the ratio of SOA mass to estimated mass of reacted precursors) was 2-4% for 2- and 4-stroke SOREs, which is comparable to yields from dilute exhaust from older passenger cars and unburned gasoline. This suggests that much of the SOA production was due to unburned fuel and/or lubrication oil. The total PM contribution of different mobile source categories to the ambient PM burden was calculated by combining primary emission, SOA production and fuel consumption data. Relative to their fuel consumption, SOREs are disproportionately high total PM sources; however, the vastly greater fuel consumption of on-road vehicles renders them (on-road vehicles) the dominant mobile source of ambient PM in the Los Angeles area.

  18. Infrared limb emission measurements of aerosol in the troposphere and stratosphere

    NASA Astrophysics Data System (ADS)

    Griessbach, Sabine; Hoffmann, Lars; Spang, Reinhold; von Hobe, Marc; Müller, Rolf; Riese, Martin

    2016-09-01

    Altitude-resolved aerosol detection in the upper troposphere and lower stratosphere (UTLS) is a challenging task for remote sensing instruments. Infrared limb emission measurements provide vertically resolved global measurements at day- and nighttime in the UTLS. For high-spectral-resolution infrared limb instruments we present here a new method to detect aerosol and separate between ice and non-ice particles. The method is based on an improved aerosol-cloud index that identifies infrared limb emission spectra affected by non-ice aerosol or ice clouds. For the discrimination between non-ice aerosol and ice clouds we employed brightness temperature difference correlations. The discrimination thresholds for this method were derived from radiative transfer simulations (including scattering) and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS)/Envisat measurements obtained in 2011. We demonstrate the value of this approach for observations of volcanic ash and sulfate aerosol originating from the Grímsvötn (Iceland, 64° N), Puyehue-Cordón Caulle (Chile, 40° S), and Nabro (Eritrea, 13° N) eruptions in May and June 2011 by comparing the MIPAS volcanic aerosol detections with Atmospheric Infrared Sounder (AIRS) volcanic ash and SO2 measurements.

  19. Emissions and Secondary Organic Aerosol Production from Semivolatile and Intermediate Volatility Organic Compounds

    NASA Astrophysics Data System (ADS)

    Robinson, A. L.; Presto, A. A.; Miracolo, M. A.; Donahue, N. M.; Kroll, J. H.; Worsnop, D. R.

    2008-12-01

    Organic aerosols are a highly-dynamic system dominated by both variable gas-particle partitioning and chemical evolution. Important classes of organics include semivolatile and intermediate volatility organic compounds (SVOC and IVOC, respectively). SVOCs are compounds that exist in both the gas and particle phases at typical atmospheric conditions while IVOC are low-volatility vapors that exist exclusively in the gas phase. Both classes have saturation concentrations that are orders of magnitude lower than volatile organic compounds (VOC) that are the traditional subjects of atmosphere chemistry, such as monoterpenes, alkyl benzenes, etc. The SVOC and IVOC are poorly represented for in current atmospheric chemistry models. Source testing indicates that SVOC and IVOC emissions from biomass combustion, diesel engines and other sources exceed the primary organic aerosol emissions; thus the oxidation of these vapors could serve as a significant source of organic aerosol in the atmosphere. The formation of secondary organic aerosol (SOA) from the reactions between OH radicals and SVOCs and IVOCs was investigated in the Carnegie Mellon University smog chamber. Experiments were conducted with n-alkanes and emission surrogates (diesel fuel and lubricating oil). SVOC oxidation produces oxidized organic aerosol but little new organic aerosol mass. This behavior can be explained by the coupled effects of partitioning and aging. Oxidation of SVOC vapors creates low volatility species that partition into the condensed phase; this oxidation also reduces the SVOC vapor concentration which, in turn, requires particle-phase SVOC to evaporate to maintain phase equilibrium. In contrast, oxidation of IVOC results in sustained production of SOA consistent with a reaction with relatively slow kinetics and high mass yield. Aerosol Mass Spectrometer data indicates that the SOA formed from IVOC has a mass spectrum that is quite similar to the oxygenated organic aerosol factor observed in

  20. Simulating secondary organic aerosol from missing diesel-related intermediate-volatility organic compound emissions during the Clean Air for London (ClearfLo) campaign

    NASA Astrophysics Data System (ADS)

    Ots, Riinu; Young, Dominique E.; Vieno, Massimo; Xu, Lu; Dunmore, Rachel E.; Allan, James D.; Coe, Hugh; Williams, Leah R.; Herndon, Scott C.; Ng, Nga L.; Hamilton, Jacqueline F.; Bergström, Robert; Di Marco, Chiara; Nemitz, Eiko; Mackenzie, Ian A.; Kuenen, Jeroen J. P.; Green, David C.; Reis, Stefan; Heal, Mathew R.

    2016-05-01

    We present high-resolution (5 km × 5 km) atmospheric chemical transport model (ACTM) simulations of the impact of newly estimated traffic-related emissions on secondary organic aerosol (SOA) formation over the UK for 2012. Our simulations include additional diesel-related intermediate-volatility organic compound (IVOC) emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo) campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA) as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA) components derived from aerosol mass spectrometer (AMS) measurements also made during the ClearfLo campaign at three sites in the London area. According to the model simulations, diesel-related IVOCs can explain on average ˜ 30 % of the annual SOA in and around London. Furthermore, the 90th percentile of modelled daily SOA concentrations for the whole year is 3.8 µg m-3, constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories) is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.

  1. Impact of Manaus City on the Amazon Green Ocean atmosphere: ozone production, precursor sensitivity and aerosol load

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Ganzeveld, L.; Thielmann, A.; Dindorf, T.; Schebeske, G.; Welling, M.; Sciare, J.; Roberts, G.; Meixner, F. X.; Kesselmeier, J.; Lelieveld, J.; Kolle, O.; Ciccioli, P.; Lloyd, J.; Trentmann, J.; Artaxo, P.; Andreae, M. O.

    2010-05-01

    As a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001) field campaign in the heart of the Amazon Basin, we analyzed the temporal and spatial dynamics of the urban plume of Manaus City during the wet-to-dry season transition period in July 2001. During the flights, we performed vertical stacks of crosswind transects in the urban outflow downwind of Manaus City, measuring a comprehensive set of trace constituents including O3, NO, NO2, CO, VOC, CO2, and H2O. Aerosol loads were characterized by total aerosol number concentration (CN) and cloud condensation nuclei (CCN) concentrations, and light scattering properties. Measurements over pristine rainforest areas during the campaign showed low levels of pollution from biomass burning or industrial emissions, representative of wet season background conditions. The urban plume of Manaus City was found to be joined by plumes from power plants south of the city, all showing evidence of very strong photochemical ozone formation. One episode is discussed in detail, where a threefold increase in ozone mixing ratios in the atmospheric boundary layer occurred within a 100 km travel distance downwind of Manaus. Observation-based estimates of the ozone production rates in the plume reached 15 ppb h-1. Within the plume core, aerosol concentrations were strongly enhanced, with ΔCN/ΔCO ratios about one order of magnitude higher than observed in Amazon biomass burning plumes. ΔCN/ΔCO ratios tended to decrease with increasing transport time, indicative of a significant reduction in particle number by coagulation, and without substantial new particle nucleation occurring within the time/space observed. While in the background atmosphere a large fraction of the total particle number served as CCN (about 60-80% at 0.6% supersaturation), the CCN/CN ratios within the plume indicated that only a small fraction (16 ± 12%) of the plume particles were

  2. Impact of Manaus City on the Amazon Green Ocean atmosphere: ozone production, precursor sensitivity and aerosol load

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Ganzeveld, L.; Thielmann, A.; Dindorf, T.; Schebeske, G.; Welling, M.; Sciare, J.; Roberts, G.; Meixner, F. X.; Kesselmeier, J.; Lelieveld, J.; Kolle, O.; Ciccioli, P.; Lloyd, J.; Trentmann, J.; Artaxo, P.; Andreae, M. O.

    2010-10-01

    As a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001) field campaign in the heart of the Amazon Basin, we analyzed the temporal and spatial dynamics of the urban plume of Manaus City during the wet-to-dry season transition period in July 2001. During the flights, we performed vertical stacks of crosswind transects in the urban outflow downwind of Manaus City, measuring a comprehensive set of trace constituents including O3, NO, NO2, CO, VOC, CO2, and H2O. Aerosol loads were characterized by concentrations of total aerosol number (CN) and cloud condensation nuclei (CCN), and by light scattering properties. Measurements over pristine rainforest areas during the campaign showed low levels of pollution from biomass burning or industrial emissions, representative of wet season background conditions. The urban plume of Manaus City was found to be joined by plumes from power plants south of the city, all showing evidence of very strong photochemical ozone formation. One episode is discussed in detail, where a threefold increase in ozone mixing ratios within the atmospheric boundary layer occurred within a 100 km travel distance downwind of Manaus. Observation-based estimates of the ozone production rates in the plume reached 15 ppb h-1. Within the plume core, aerosol concentrations were strongly enhanced, with ΔCN/ΔCO ratios about one order of magnitude higher than observed in Amazon biomass burning plumes. ΔCN/ΔCO ratios tended to decrease with increasing transport time, indicative of a significant reduction in particle number by coagulation, and without substantial new particle nucleation occurring within the time/space observed. While in the background atmosphere a large fraction of the total particle number served as CCN (about 60-80% at 0.6% supersaturation), the CCN/CN ratios within the plume indicated that only a small fraction (16±12%) of the plume particles were CCN

  3. MODELING THE EFFECT OF CHLORINE EMISSIONS ON ATMOSPHERIC OZONE AND SECONDARY ORGANIC AEROSOL CONCENTRATIONS ACROSS THE UNITED STATES

    EPA Science Inventory

    This paper presents the modeled effects of natural and anthropogenic chlorine emissions on the atmospheric concentrations of ozone and secondary organic aerosol across the United States. The model calculations include anthropogenic molecular chlorine emissions, anthropogenic hypo...

  4. The Influence of Anthropogenic Sources on Fluxes of Secondary Organic Aerosol Precursors From a Deciduous Forest in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Saylor, R. D.; Stein, A. F.

    2012-12-01

    The dynamic, bi-directional exchange of trace chemical species between forests and the atmosphere has important impacts on both the forest ecosystem and atmospheric composition, with potentially profound consequences on air quality, climate and global ecosystem functioning. Forests are a dominant source of biogenic volatile organic compound (BVOC) emissions into the earth's atmosphere and thus play an important role in the formation of secondary organic aerosol (SOA). To arrive at a better scientific understanding of the complex chemical and physical processes of forest-atmosphere exchange and provide a platform for robust analysis of field measurements of these processes, a process-level, multiphase model of the atmospheric chemistry and physics of forest canopies is being developed. This model, the Atmospheric Chemistry and Canopy Exchange Simulation System (ACCESS) is being used to investigate various aspects of forest-atmosphere exchange and chemistry including gas, aqueous and aerosol phases. ACCESS currently includes processes accounting for the emission of BVOCs from the canopy, turbulent vertical transport within and above the canopy and throughout the height of the planetary boundary layer, detailed chemical reactions, mixing with the background atmosphere and bi-directional exchange between the atmosphere and the canopy and the forest floor. The Walker Branch Watershed (WBW) is a dedicated ecosystem research area on the U. S. Department of Energy's Oak Ridge Reservation in eastern Tennessee. The 97.5 ha watershed has been the site of long-term ecosystem and atmospheric research activities since the mid-1960's. A flux tower located within the watershed (35°57'30"N, 84°17'15"W; 365 m above mean sea level) and 10 km southwest of Oak Ridge, Tennessee, has served as a focal point for previous atmospheric turbulence and chemical flux measurements and the canopy morphology of the forest surrounding the flux tower has been extensively documented. The forest is

  5. Interannual variability of tropospheric trace gases and aerosols: The role of biomass burning emissions

    NASA Astrophysics Data System (ADS)

    Voulgarakis, Apostolos; Marlier, Miriam E.; Faluvegi, Greg; Shindell, Drew T.; Tsigaridis, Kostas; Mangeon, Stéphane

    2015-07-01

    Fires are responsible for a range of gaseous and aerosol emissions. However, their influence on the interannual variability of atmospheric trace gases and aerosols has not been systematically investigated from a global perspective. We examine biomass burning emissions as a driver of interannual variability of large-scale abundances of short-lived constituents such as carbon monoxide (CO), hydroxyl radicals (OH), ozone, and aerosols using the Goddard Institute for Space Studies ModelE composition-climate model and a range of observations, with an emphasis on satellite information. Our model captures the observed variability of the constituents examined in most cases, but with substantial underestimates in boreal regions. The strongest interannual variability on a global scale is found for carbon monoxide (~10% for its global annual burden), while the lowest is found for tropospheric ozone (~1% for its global annual burden). Regionally, aerosol optical depth shows the largest variability which exceeds 50%. Areas of strong variability of both aerosols and CO include the tropical land regions (especially Equatorial Asia and South America) and northern high latitudes, while even regions in the northern midlatitudes experience substantial interannual variability of aerosols. Ozone variability peaks over equatorial Asia in boreal autumn, partly due to varying biomass burning emissions, and over the western and central Pacific in the rest of the year, mainly due to meteorological fluctuations. We find that biomass burning emissions are almost entirely responsible for global CO interannual variability, and similarly important for OH variability. The same is true for global and regional aerosol variability, especially when not taking into account dust and sea-salt particles. We show that important implications can arise from such interannual influences for regional climate and air quality.

  6. Aerosol-assisted chemical vapor deposition of tungsten oxide films and nanorods from oxo tungsten(VI) fluoroalkoxide precursors.

    PubMed

    Kim, Hankook; Bonsu, Richard O; O'Donohue, Christopher; Korotkov, Roman Y; McElwee-White, Lisa; Anderson, Timothy J

    2015-02-01

    Aerosol-assisted chemical vapor deposition (AACVD) of WOx was demonstrated using the oxo tungsten(VI) fluoroalkoxide single-source precursors, WO[OCCH3(CF3)2]4 and WO[OC(CH3)2CF3]4. Substoichiometric amorphous tungsten oxide thin films were grown on indium tin oxide (ITO) substrates in nitrogen at low deposition temperature (100-250 °C). At growth temperatures above 300 °C, the W18O49 monoclinic crystalline phase was observed. The surface morphology and roughness, visible light transmittance, electrical conductivity, and work function of the tungsten oxide materials are reported. The solvent and carrier gas minimally affected surface morphology and composition at low deposition temperature; however, material crystallinity varied with solvent choice at higher temperatures. The work function of the tungsten oxide thin films grown between 150 and 250 °C was determined to be in the range 5.0 to 5.7 eV, according to ultraviolet photoelectron spectroscopy (UPS). PMID:25569472

  7. Tris(phosphino)borato silver(I) complexes as precursors for metallic silver aerosol-assisted chemical vapor deposition.

    PubMed

    McCain, Matthew N; Schneider, Sven; Salata, Michael R; Marks, Tobin J

    2008-04-01

    A series of light- and air-stable tris(phosphino)borato silver(I) complexes has been synthesized, structurally and spectroscopically characterized, and implemented in the growth of low resistivity metallic silver thin films by aerosol-assisted chemical vapor deposition (AACVD). Of the four complexes in the series, [RB(CH2PR'2) 3]AgPEt3 (R = Ph (1, 3), (n)Bu (2, 4); R' = Ph (1, 2), (i)Pr (3, 4), complexes 1 and 2 have been characterized by single-crystal X-ray diffraction. Complex 2 represents a significant improvement over previously available nonfluorinated Ag precursors, owing to ease of handling and efficient film deposition characteristics. Thermogravimetric analysis (TGA) shows that the thermolytic properties of these complexes can be significantly modified by altering the ligand structure. Polycrystalline cubic-phase Ag thin films were grown on glass, MgO(100), and 52100 steel substrates. Ag films of thicknesses 3 microm, grown at rates of 14-18 nm/min, exhibit low levels of extraneous element contamination by X-ray photoelectron spectroscopy (XPS). Atomic force microscopy (AFM) and scanning electron microscopy (SEM) indicate that film growth proceeds primarily via an island growth (Volmer-Weber) mechanism. PMID:18293915

  8. Lung physiology and aerosol deposition imaged with positron emission tomography.

    PubMed

    Venegas, Jose; Winkler, Tilo; Harris, R Scott

    2013-02-01

    Physiological conditions and pathophysiological changes in the lungs may affect many applications in aerosol medicine and pulmonary drug delivery. In the diseased lung, spatial heterogeneity in function and structure may cause substantial changes in aerosol transport and local deposition among different lung regions. Non-uniform aerosol deposition affects airway or tissue pharmacological dosing, which could reduce the therapeutic effectiveness of inhalation therapy. This review article presents examples of pulmonary imaging using PET and PET-CT in lung physiology with an emphasis on their implications for aerosol medicine. Measurements of regional ventilation, perfusion, and ventilation/perfusion ratio, by imaging local kinetics of intravenously injected Nitrogen-13 in saline solution, and of pulmonary inflammation, by assessing the regional uptake of the radiotracer (18)F-FDG, are presented. These examples demonstrate that it is possible to access both preexisting conditions, such as heterogeneity of ventilation, perfusion, and/or inflammatory stimuli, which may affect inhalation therapy, and the functional effects of inhaled medications or inflammatory agents on lung regional function. The imaging techniques described could be efficient tools to evaluate quantitatively and noninvasively these processes in vivo. Furthermore, it can be expected that imaging of respiratory structure and function will yield sensitive biomarkers of disease, which will help and speed drug discovery, and the evaluation of novel inhalation therapies.

  9. Urban emission hot spots as sources for remote aerosol deposition

    NASA Astrophysics Data System (ADS)

    Kunkel, D.; Lawrence, M. G.; Tost, H.; Kerkweg, A.; Jöckel, P.; Borrmann, S.

    2012-01-01

    Large point sources such as major population centers (MPCs) emit pollutants which can be deposited nearby or transported over long distances before deposition. We have used tracer simulations of aerosols emitted from MPCs worldwide to assess the fractions which are deposited at various distances away from their source location. Considering only source location, prevailing meteorology, and the aerosol size and solubility, we show that fine aerosol particles have a high potential to pollute remote regions. About half of the emitted mass of aerosol tracers with an ambient diameter ≤1.0 μm is typically deposited in regions more than 1000 km away from the source. Furthermore, using the Köppen-Geiger climate classification to categorize the sources into various climate classes we find substantial differences in the deposition potential between these classes. Tracers originating in arid regions show the largest remote deposition potentials, with values more than doubled compared to the smallest potentials from tracers in tropical regions. Seasonal changes in atmospheric conditions lead to variations in the remote deposition potentials. On average the remote deposition potentials in summer correspond to about 70-80% of the values in winter, with a large spread among the climate classes. For tracers from tropical regions the summer remote deposition values are only about 31% of the winter values, while they are about 95% for tracers from arid regions.

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

    NASA Astrophysics Data System (ADS)

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

    2014-10-01

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

  11. Top-Down Smoke Aerosol Emission Estimation Using Satellite Fire Radiative Power Measurements

    NASA Astrophysics Data System (ADS)

    Ichoku, C. M.; Ellison, L.

    2013-05-01

    Biomass burning (BB) occurs seasonally in different vegetated parts of the world, devastating the landscapes, consuming large amounts of biomass fuel, generating intense heat energy, and emitting corresponding amounts of smoke plumes that comprise different species of aerosols and trace gases, many of which have adverse effects on human health, air quality, and environmental processes. Accurate estimates of these emissions are required as model inputs to evaluate and forecast smoke plume transport and impacts on air quality, human health, clouds, weather, radiation, and climate. Emissions estimates have long been based on bottom-up approaches that are not only complex, but also fraught with uncertainties. Fortunately, a series of recent studies have revealed that both the rate of biomass consumption and the rate of emission of aerosol particulate matter (PM) by open biomass burning are directly proportional to the fire radiative power (FRP) or rate of release of fire radiative energy (FRE) that is measurable from satellite. We have leveraged this relationship to generate a global gridded FRE-based emission coefficients (Ce) of particulate matter using measurements of FRP and aerosol optical depth (AOD) from the Moderate-resolution Imaging Spectro-radiometer (MODIS) twin sensors onboard the Terra and Aqua satellites. Ce is a simple coefficient to convert FRP (or FRE) to smoke aerosol emissions, in the same manner as emission factors are used to convert burned biomass to emissions. In this presentation, we will discuss the characteristics of the Ce product, including its uncertainties, strengths and limitations. We will also demonstrate the simplicity and utility of using the gridded Ce product and satellite measurements of FRP to derive emissions, and present some comparisons of these emission products against other emissions inventories.

  12. Basic biogenic aerosol precursors: Agricultural source attribution of volatile amines revised

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Sintermann, J.; Spirig, C.; Jocher, M.; Ammann, C.; Neftel, A.

    2011-08-01

    Despite recent evidence on an important role of volatile amines in the nucleation of particulate matter, very scarce information is available on their atmospheric abundance and source distribution. Previous measurements in animal housings had identified livestock husbandry as the main amine source, with trimethylamine (TMA) being the key component. This has led to the assumption that the agricultural sources for amines are similar as for ammonia, emitted throughout the cascade of animal excretion, storage and application in the field. In this study, we present the first micrometeorological flux measurements as well as dynamic enclosure experiments showing that the amine source strength from stored slurry is negligible, implying significant consequences for the global amine emission inventory. In the case of cattle, amine production is attributed to the animal's rumination activity and exhalation is suggested to be an important emission pathway, similar to the greenhouse gas methane. Fodder like hay and silage also emits volatile amines, potentially assigning these alkaloid compounds a key function in enhancing particle formation in remote areas.

  13. Characterizing the impact of urban emissions on regional aerosol particles: airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouche, N.; Pichon, J.-M.; Bourianne, T.; Gomes, L.; Prevot, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2014-02-01

    The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation

  14. Impact on aerosol emissions in China and India on local and global climate

    NASA Astrophysics Data System (ADS)

    Kühn, Thomas; Partanen, Antti-Ilari; Henriksson, Svante V.; Bergman, Tommi; Laakso, Anton; Kokkola, Harri; Romakkaniemi, Sami; Laaksonen, Ari

    2013-04-01

    Existing surface temperature records show warming in the beginning of last century, followed by cooling starting from 1940 and again strong heating from 1975 until recent years. This behaviour has been attributed to increase in the greenhouse gas and aerosol emission as well as to natural variability of climate. Making a difference between these is crucial as climate predictions and international policy related to emission reductions are based on the models that are mainly evaluated against the historical temperature records. While in Europe and North America the aerosol emissions have decreased since the late 1970s, the emissions in China and India have started to increase dramatically at about the same time and have only recently started to stagnate due to new regulations in China. Here we use emission scenarios from the years 1996 through 2010 to assess the effect that these emissions have on local aerosol properties and climate as well as on the global climate. We use the aerosol-climate model ECHAM5-HAM [Roeckner2003, Roeckner2004] to simulate the local aerosol properties in China and India in the years 1996 through 2010, and their impact on local as well as global climate. For anthropogenic aerosol greenhouse gas emissions we use the ACCMIP-MACCity Aerocom emissions (Aerocom 2) [Lamarque2010] in combination with the emissions for China and India after Lu et. al [Lu2011] for the mentioned period of time. To assess the effect of anthropogenic aerosol emissions on earth's climate is assessed using the ECHAM-HAM model coupled to a mixed layer ocean on a T42L19 grid. The model is run with fixed yearly emissions for several emission scenarios (e.g. for the years 1996 and 2010), with data derived from 100-year averages. Additionally we run a number of transient simulations (i.e. with varying yearly emissions) from 1996 to 2010 in the attempt to extract a climate trend for the given period. References [Roeckner2003] Roeckner, E., Bäuml, R., Bonaventura, L., Brokopf

  15. Biomass burning emissions over northern Australia constrained by aerosol measurements: I—Modelling the distribution of hourly emissions

    NASA Astrophysics Data System (ADS)

    Meyer, C. P. (Mick); Luhar, Ashok K.; Mitchell, Ross M.

    Emissions of aerosol from biomass burning in northern Australia are globally significant, yet existing estimates of their magnitude are essentially unconstrained by observation. This two-part series (see Part II by Luhar et al. [2008. Biomass burning emissions over northern Australia constrained by aerosol measurements: II—Model validation, and impacts on air quality and radiative forcing. Atmospheric Environment, submitted for publication] seeks to address this by first formulating a scheme to determine the emissions from the Top End region of the Northern Territory during the 2004 burning season at a high temporal and spatial resolution (1 h, 1 km). The emissions are then validated using a meteorological and transport model called TAPM coupled with a variety of field measurements. The high resolution not only enables validation against various meteorological and aerosol data sets, but also allows prediction of local air quality events. Essential inputs to the emission calculations are satellite-based measurements of fire scars, yielding burnt areas, and hotspots, providing timing information on daily basis. It is shown that hotspots without associated fire scars must be taken into account in order to produce credible aerosol fields. Prediction of emissions at hourly time resolution is enabled by assigning a diurnal variation based on a McArthur fire danger meter. The total carbon emission for the 2004 season is computed to be 67.6 Tg, in remarkable agreement with the bulk estimate of 64.3 Tg derived for the Australian National Greenhouse Gas Inventory, and comparable to the figure of 57.0 Tg determined from the Global Fire Emissions Database (GFEDv2). The total PM 2.5 (particulate matter with an aerodynamic diameter of 2.5 μm or less) emission is computed to be 0.67 Tg. The transport modelling shows that emissions leaving the study region are largely advected to the west over the Timor Sea towards the Indonesian archipelago from April to September, shifting to

  16. Constraining Predicted Secondary Organic Aerosol Formation and Processing Using Real-Time Observations of Aging Urban Emissions in an Oxidation Flow Reactor

    NASA Astrophysics Data System (ADS)

    Ortega, A. M.; Palm, B. B.; Hayes, P. L.; Day, D. A.; Cubison, M.; Brune, W. H.; Hu, W.; Graus, M.; Warneke, C.; Gilman, J.; De Gouw, J. A.; Jimenez, J. L.

    2014-12-01

    To investigate atmospheric processing of urban emissions, we deployed an oxidation flow reactor with measurements of size-resolved chemical composition of submicron aerosol during CalNex-LA, a field study investigating air quality and climate change at a receptor site in the Los Angeles Basin. The reactor produces OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent atmospheric aging of hours to ~2 weeks in 5 minutes of processing. The OH exposure (OHexp) was stepped every 20 min to survey the effects of a range of oxidation exposures on gases and aerosols. This approach is a valuable tool for in-situ evaluation of changes in organic aerosol (OA) concentration and composition due to photochemical processing over a range of ambient atmospheric conditions and composition. Combined with collocated gas-phase measurements of volatile organic compounds, this novel approach enables the comparison of measured SOA to predicted SOA formation from a prescribed set of precursors. Results from CalNex-LA show enhancements of OA and inorganic aerosol from gas-phase precursors. The OA mass enhancement from aging was highest at night and correlated with trimethylbenzene, indicating the importance of relatively short-lived VOC (OH lifetime of ~12 hrs or less) as SOA precursors in the LA Basin. Maximum net SOA production is observed between 3-6 days of aging and decreases at higher exposures. Aging in the reactor shows similar behavior to atmospheric processing; the elemental composition of ambient and reactor measurements follow similar slopes when plotted in a Van Krevelen diagram. Additionally, for air processed in the reactor, oxygen-to-carbon ratios (O/C) of aerosol extended over a larger range compared to ambient aerosol observed in the LA Basin. While reactor aging always increases O/C, often beyond maximum observed ambient levels, a transition from net OA production to destruction occurs at intermediate OHexp, suggesting a transition

  17. Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

    NASA Astrophysics Data System (ADS)

    Lacey, Forrest; Henze, Daven

    2015-11-01

    Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the

  18. Profile and Morphology of Fungal Aerosols Characterized by Field Emission Scanning Electron Microscopy (FESEM)

    PubMed Central

    Afanou, Komlavi Anani; Straumfors, Anne; Skogstad, Asbjørn; Skaar, Ida; Hjeljord, Linda; Skare, Øivind; Green, Brett James; Tronsmo, Arne; Eduard, Wijnand

    2016-01-01

    Fungal aerosols consist of spores and fragments with diverse array of morphologies; however, the size, shape, and origin of the constituents require further characterization. In this study, we characterize the profile of aerosols generated from Aspergillus fumigatus, A. versicolor, and Penicillium chrysogenum grown for 8 weeks on gypsum boards. Fungal particles were aerosolized at 12 and 20 L min−1 using the Fungal Spore Source Strength Tester (FSSST) and the Stami particle generator (SPG). Collected particles were analyzed with field emission scanning electron microscopy (FESEM). We observed spore particle fraction consisting of single spores and spore aggregates in four size categories, and a fragment fraction that contained submicronic fragments and three size categories of larger fragments. Single spores dominated the aerosols from A. fumigatus (median: 53%), while the submicronic fragment fraction was the highest in the aerosols collected from A. versicolor (median: 34%) and P. chrysogenum (median: 31%). Morphological characteristics showed near spherical particles that were only single spores, oblong particles that comprise some spore aggregates and fragments (<3.5 μm), and fiber-like particles that regroup chained spore aggregates and fragments (>3.5 μm). Further, the near spherical particles dominated the aerosols from A. fumigatus (median: 53%), while oblong particles were dominant in the aerosols from A. versicolor (68%) and P. chrysogenum (55%). Fiber-like particles represented 21% and 24% of the aerosols from A. versicolor and P. chrysogenum, respectively. This study shows that fungal particles of various size, shape, and origin are aerosolized, and supports the need to include a broader range of particle types in fungal exposure assessment. PMID:26855468

  19. Ozone precursor levels and responses to emissions reductions: Analysis of regional oxidant model results

    NASA Astrophysics Data System (ADS)

    Milford, Jana B.; Gao, Dongfen; Zafirakou, Antigoni; Pierce, Thomas E.

    An analysis of results from the Regional Oxidant Modeling for Northeast Transport (ROMNET) study ( U.S. EPA, 1991, EPA-450/4-91-002a) has investigated the chemical conditions under which air quality was predicted to improve with reductions in ROG and/or NO ξ emissions, or with changes in the composition of ROG emissions. The ROMNET simulations used emissions projected to the year 2005, with meteorological conditions from July 1988. Predicted concentrations of PAN, HNO 3, H 2O 2 and HCHO are shown along with O 3 for the 2005 base case, allowing limited comparisons to be made with field observations and results from other modeling studies. Predicted secondary pollutant concentrations indicate an unusual degree of photochemical activity over much of the model domain, directionally consistent with the extreme nature of the July 1988 episode. Reducing NO ξ emissions was predicted to reduce O 3 in grid cells in which reactive nitrogen (NO y) concentrations were below about 25 ppb, but to be counterproductive for some cells with higher NO y. The New York City area where NO ξ control was predicted to be counterproductive was characterized by very high NO ξ to NO y ratios. Ozone was relatively insensitive to ROG controls in grid cells with NO y concentrations below 5-10 ppb. Comparison of unweighted ROG concentrations with concentrations weighted by HO rate constants (i.e. reactivity) showed that the latter varied less across locations. Predicted spatial gradients of NO y were generally sharper than those of reactivity-weighted ROG, supporting a dominant role for variations in NO y in controlling the sensitivity of ozone to its precursors. Reductions in reactivity-weighted ROG achieved with composition changes were similar to reductions achieved with ROG emissions cuts, explaining the similar response of ozone to these two control strategies.

  20. Use of MODIS-Derived Fire Radiative Energy to Estimate Smoke Aerosol Emissions over Different Ecosystems

    NASA Technical Reports Server (NTRS)

    Ichoku, Charles; Kaufman, Yoram J.

    2003-01-01

    Biomass burning is the main source of smoke aerosols and certain trace gases in the atmosphere. However, estimates of the rates of biomass consumption and emission of aerosols and trace gases from fires have not attained adequate reliability thus far. Traditional methods for deriving emission rates employ the use of emission factors e(sub x), (in g of species x per kg of biomass burned), which are difficult to measure from satellites. In this era of environmental monitoring from space, fire characterization was not a major consideration in the design of the early satellite-borne remote sensing instruments, such as AVHRR. Therefore, although they are able to provide fire location information, they were not adequately sensitive to variations in fire strength or size, because their thermal bands used for fire detection saturated at the lower end of fire radiative temperature range. As such, hitherto, satellite-based emission estimates employ proxy techniques using satellite derived fire pixel counts (which do not express the fire strength or rate of biomass consumption) or burned areas (which can only be obtained after the fire is over). The MODIS sensor, recently launched into orbit aboard EOS Terra (1999) and Aqua (2002) satellites, have a much higher saturation level and can, not only detect the fire locations 4 times daily, but also measures the at-satellite fire radiative energy (which is a measure of the fire strength) based on its 4 micron channel temperature. Also, MODIS measures the optical thickness of smoke and other aerosols. Preliminary analysis shows appreciable correlation between the MODIS-derived rates of emission of fire radiative energy and smoke over different regions across the globe. These relationships hold great promise for deriving emission coefficients, which can be used for estimating smoke aerosol emissions from MODIS active fire products. This procedure has the potential to provide more accurate emission estimates in near real

  1. AGRICULTURAL AMMONIA EMISSIONS AND AMMONIUM CONCENTRATIONS ASSOCIATED WITH AEROSOLS AND PRECIPITATION IN THE SOUTHEAST UNITED STATES

    EPA Science Inventory

    Temporal and spatial variations in ammonia (NH3) emissions and ammonium (NH4+) concentrations associated with aerosols and volume-weighted NH4+ concentration in precipitation are investigated over the period 1990-1998 in the southeast United States (Alabama, Florida, Georgia, Ken...

  2. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model

    EPA Science Inventory

    Sea spray aerosols (SSA) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. In this study, the Community Multiscale Air Quality (CMAQ) model is updated to enhance fine mode SSA emissions,...

  3. Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

    NASA Astrophysics Data System (ADS)

    Mentel, Th. F.; Kleist, E.; Andres, S.; Dal Maso, M.; Hohaus, T.; Kiendler-Scharr, A.; Rudich, Y.; Springer, M.; Tillmann, R.; Uerlings, R.; Wahner, A.; Wildt, J.

    2013-09-01

    Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Biogenic secondary organic aerosols (BSOAs) comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOCs) emitted by vegetation are the source of BSOAs. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed BSOAs, and possibly their climatic effects. This raises questions of whether stress-induced changes in BSOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on BSOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical BSOA formation for plants infested by aphids in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify BSOA formation and yield. Stress-induced emissions of sesquiterpenes, methyl salicylate, and C17-BVOCs increase BSOA yields. Mixtures including these compounds exhibit BSOA yields between 17 and 33%, significantly higher than mixtures containing mainly monoterpenes (4-6% yield). Green leaf volatiles suppress SOA formation, presumably by scavenging OH, similar to isoprene. By classifying emission types, stressors and BSOA formation potential, we discuss possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate-vegetation feedback mechanisms.

  4. Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouch, N.; Pichon, J.-M.; Prévôt, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2013-09-01

    The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA

  5. Analysis of aerosol emission and hazard evaluation of electrical discharge machining (EDM) process.

    PubMed

    Jose, Mathew; Sivapirakasam, S P; Surianarayanan, M

    2010-01-01

    The safety and environmental aspects of a manufacturing process are important due to increased environmental regulations and life quality. In this paper, the concentration of aerosols in the breathing zone of the operator of Electrical Discharge Machining (EDM), a commonly used non traditional manufacturing process is presented. The pattern of aerosol emissions from this process with varying process parameters such as peak current, pulse duration, dielectric flushing pressure and the level of dielectric was evaluated. Further, the HAZOP technique was employed to identify the inherent safety aspects and fire risk of the EDM process under different working conditions. The analysis of aerosol exposure showed that the concentration of aerosol was increased with increase in the peak current, pulse duration and dielectric level and was decreased with increase in the flushing pressure. It was also found that at higher values of peak current (7A) and pulse duration (520 micros), the concentration of aerosols at breathing zone of the operator was above the permissible exposure limit value for respirable particulates (5 mg/m(3)). HAZOP study of the EDM process showed that this process is vulnerable to fire and explosion hazards. A detailed discussion on preventing the fire and explosion hazard is presented in this paper. The emission and risk of fire of the EDM process can be minimized by selecting proper process parameters and employing appropriate control strategy.

  6. The chemical and microphysical properties of secondary organic aerosols from Holm Oak emissions

    NASA Astrophysics Data System (ADS)

    Lang-Yona, N.; Rudich, Y.; Mentel, Th. F.; Buchholz, A.; Kiendler-Scharr, A.; Kleist, E.; Spindler, C.; Tillmann, R.; Wildt, J.

    2010-02-01

    The Mediterranean region is expected to experience substantial climatic change in the next 50 years. But, possible effects of climate change on biogenic volatile organic compound (VOC) emissions as well as on the formation of secondary organic aerosols (SOA) produced from these VOC are yet unexplored. To address such issues, the effects of temperature and light intensity on the VOC emissions of Mediterranean Holm Oak have been studied in the Jülich plant aerosol atmosphere chamber, as well as the optical and microphysical properties of the resulting SOA. Monoterpenes dominated the VOC emissions from Holm Oak (97.5%) and temperature increase enhanced the emission strength under variation of the emission pattern. The amount of SOA increased linearly with the emission strength with a fractional mass yield of 5.7±1%, independent of the detailed emission pattern. The particles were highly scattering with no absorption abilities. Their average hygroscopic growth factor was 1.13±0.03 at 90% RH with a critical diameter of droplet activation of 100±4 nm at a supersaturation of 0.4%. All microphysical properties did not depend on the detailed emission pattern, in accordance with an invariant O/C ratio (0.57(+0.03/-0.1)) of the SOA observed by high resolution aerosol mass spectrometry. The increase of Holm oak emissions with temperature (≈20% per degree) was stronger than e.g. for Boreal tree species (≈10% per degree). Increasing mean temperature in Mediterranean areas therefore may have a stronger impact on VOC emissions and SOA formation than in areas with Boreal forests.

  7. Ozone sensitivity to its precursor emissions in northeastern Mexico for a summer air pollution episode.

    PubMed

    Sierra, A; Vanoye, A Y; Mendoza, A

    2013-10-01

    A summer episode was modeled to address the expected response of ambient air O3 to hypothetical emission control scenarios in northeastern Mexico, and in particular in the Monterrey Metropolitan Area (MMA). This region is of interest because the MMA holds one of the worst air quality problems in the country and levels of air pollutants in the rest of northeastern Mexico are starting to be a concern. The MM5-SMOKE-CMAQ platform was used to conduct the numerical experiments. Twenty-four control scenarios were evaluated, combining the level of emission controls of O3 precursors (NO(x) and volatile organic compounds [VOCs]) from 0% to 50%. For the MMA, VOC-only controls result in the best option to reduce O3 concentrations, though the benefit is limited to the urban core. This same strategy results in negligible benefits for the rest of northeastern Mexico. NO(x) controls result in an increase in O3 concentration within the MMA of up to 20 ppbv and a decrease at downwind locations of up to 11 ppbv, with respect to the base-case scenario. Indicator ratios were also used to probe for NO(x)-sensitive and VOC-sensitive areas. Locations with an important influence of NO(x) point sources (i.e., Monclova and Nava/Acuña) are quite sensitive to changes in NO(x) emissions. Border cities in the Rio Bravo/Grande Valley tend to be marginally NO(x)-sensitive. Overall, the MMA seems to be dominated by a VOC-sensitive regime, while the rest of the region would tend to have a NO(x)-sensitive response. The results obtained serve to expand the current knowledge on the chemical regimes that dominate this region (VOC- or NO(x)-sensitive), and thus could help guide public policies related to emission regional control strategies. PMID:24282975

  8. Secondary organic aerosol formation from gasoline vehicle emissions in a new mobile environmental reaction chamber

    NASA Astrophysics Data System (ADS)

    Platt, S. M.; El Haddad, I.; Zardini, A. A.; Clairotte, M.; Astorga, C.; Wolf, R.; Slowik, J. G.; Temime-Roussel, B.; Marchand, N.; Ježek, I.; Drinovec, L.; Močnik, G.; Möhler, O.; Richter, R.; Barmet, P.; Bianchi, F.; Baltensperger, U.; Prévôt, A. S. H.

    2012-10-01

    We present a new mobile environmental reaction chamber for the simulation of the atmospheric aging of aerosols from different emissions sources without limitation from the instruments or facilities available at any single site. The chamber can be mounted on a trailer for transport to host facilities or for mobile measurements. Photochemistry is simulated using a set of 40 UV lights (total power 4 KW). Characterisation of the emission spectrum of these lights shows that atmospheric photochemistry can be accurately simulated over a range of temperatures from -7-25 °C. A photolysis rate of NO2, JNO2, of (8.0 ± 0.7) × 10-3 molecules cm-3 s-1 was determined at 25 °C. Further, we present the first application of the mobile chamber and demonstrate its utility by quantifying primary organic aerosol (POA) emission and secondary organic aerosol (SOA) production from a Euro 5 light duty gasoline vehicle. Exhaust emissions were sampled during the New European Driving Cycle (NEDC), the standard driving cycle for European regulatory purposes, and injected into the chamber. The relative concentrations of oxides of nitrogen (NOx) and total hydrocarbon (THC) during the aging of emissions inside the chamber were controlled using an injection system developed as a part of the new mobile chamber set up. Total OA (POA + SOA) emission factors of (370 ± 18) × 10-3 g kg-1 fuel, or (14.6 ± 0.8) × 10-3 g km-1, after aging, were calculated from concentrations measured inside the smog chamber during two experiments. The average SOA/POA ratio for the two experiments was 15.1, a much larger increase than has previously been seen for diesel vehicles, where smog chamber studies have found SOA/POA ratios of 1.3-1.7. Due to this SOA formation, carbonaceous particulate matter (PM) emissions from a gasoline vehicle may approach those of a diesel vehicle of the same class. Furthermore, with the advent of emission controls requiring the use of diesel particle filters, gasoline vehicle emissions

  9. Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

    NASA Astrophysics Data System (ADS)

    Mentel, Th. F.; Kleist, E.; Andres, S.; Maso, M. D.; Hohaus, T.; Kiendler-Scharr, A.; Rudich, Y.; Springer, M.; Tillmann, R.; Uerlings, R.; Wahner, A.; Wildt, J.

    2013-03-01

    Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Secondary organic aerosols (SOA) comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOC) emitted by vegetation are a major source of SOA. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed SOA, and possibly their climatic effects. This raises questions whether stress-induced changes in SOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on SOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical SOA formation for infested plants in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify SOA formation. While sesquiterpenes, methyl salicylate, and C17-BVOC increase SOA yield, green leaf volatiles suppress SOA formation. By classifying emission types, stressors and SOA formation potential, we propose possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate-vegetation feedback mechanisms.

  10. Optical properties of aerosol emissions from biomass burning in the tropics, BASE-A

    NASA Technical Reports Server (NTRS)

    Holben, Brent N.; Kaufman, Yoram J.; Setzer, Alberto W.; Tanre, Didre D.; Ward, Darold E.

    1991-01-01

    Ground-based and airborne measurements of biomass-burning smoke particle optical properties, obtained with a view to aerosol-absorption properties, are presented as a function of time and atmospheric height. The wavelength dependence of the optical thickness can be explained by a log-normal size distribution, with particles' effective radius varying between 0.1 and 0.2 microns. The strong correlation noted between aerosol particle profile and CO profile indicates that smoke particulates constitute a good tracer for emission trace gases from tropical biomass burning.

  11. Gas-particle partitioning of primary organic aerosol emissions: 3. Biomass burning

    NASA Astrophysics Data System (ADS)

    May, Andrew A.; Levin, Ezra J. T.; Hennigan, Christopher J.; Riipinen, Ilona; Lee, Taehyoung; Collett, Jeffrey L.; Jimenez, Jose L.; Kreidenweis, Sonia M.; Robinson, Allen L.

    2013-10-01

    organic aerosol concentrations depend in part on the gas-particle partitioning of primary organic aerosol (POA) emissions. Consequently, heating and dilution were used to investigate the volatility of biomass-burning smoke particles from combustion of common North American trees/shrubs/grasses during the third Fire Lab at Missoula Experiment. Fifty to eighty percent of the mass of biomass-burning POA evaporated when isothermally diluted from plume- (~1000 µg m-3) to ambient-like concentrations (~10 µg m-3), while roughly 80% of the POA evaporated upon heating to 100°C in a thermodenuder with a residence time of ~14 sec. Therefore, the majority of the POA emissions were semivolatile. Thermodenuder measurements performed at three different residence times indicated that there were not substantial mass transfer limitations to evaporation (i.e., the mass accommodation coefficient appears to be between 0.1 and 1). An evaporation kinetics model was used to derive volatility distributions and enthalpies of vaporization from the thermodenuder data. A single volatility distribution can be used to represent the measured gas-particle partitioning from the entire set of experiments, including different fuels, organic aerosol concentrations, and thermodenuder residence times. This distribution, derived from the thermodenuder measurements, also predicts the dilution-driven changes in gas-particle partitioning. This volatility distribution and associated emission factors for each fuel studied can be used to update emission inventories and to simulate the gas-particle partitioning of biomass-burning POA emissions in chemical transport models.

  12. The chemical and microphysical properties of secondary organic aerosols from Holm Oak emissions

    NASA Astrophysics Data System (ADS)

    Lang-Yona, N.; Rudich, Y.; Mentel, Th. F.; Bohne, A.; Buchholz, A.; Kiendler-Scharr, A.; Kleist, E.; Spindler, C.; Tillmann, R.; Wildt, J.

    2010-08-01

    The Mediterranean region is expected to experience substantial climatic change in the next 50 years. But, possible effects of climate change on biogenic volatile organic compound (VOC) emissions as well as on the formation of secondary organic aerosols (SOA) produced from these VOC are yet unexplored. To address such issues, the effects of temperature on the VOC emissions of Mediterranean Holm Oak and small Mediterranean stand of Wild Pistacio, Aleppo Pine, and Palestine Oak have been studied in the Jülich plant aerosol atmosphere chamber. For Holm Oak the optical and microphysical properties of the resulting SOA were investigated. Monoterpenes dominated the VOC emissions from Holm Oak (97.5%) and Mediterranean stand (97%). Higher temperatures enhanced the overall VOC emission but with different ratios of the emitted species. The amount of SOA increased linearly with the emission strength with a fractional mass yield of 6.0±0.6%, independent of the detailed emission pattern. The investigated particles were highly scattering with no absorption abilities. Their average hygroscopic growth factor of 1.13±0.03 at 90% RH with a critical diameter of droplet activation was 100±4 nm at a supersaturation of 0.4%. All microphysical properties did not depend on the detailed emission pattern, in accordance with an invariant O/C ratio (0.57(+0.03/-0.1)) of the SOA observed by high resolution aerosol mass spectrometry. The increase of Holm oak emissions with temperature (≈20% per degree) was stronger than e.g. for Boreal tree species (≈10% per degree). The SOA yield for Mediterranean trees determined here is similar as for Boreal trees. Increasing mean temperature in Mediterranean areas could thus have a stronger impact on BVOC emissions and SOA formation than in areas with Boreal forests.

  13. The Influence of Ozone Precursor Emissions from Four World Regions on Tropospheric Composition and Radiative Climate Forcing

    NASA Technical Reports Server (NTRS)

    Fry, Meridith; Naik, Vaishali; West, J. Jason; Schwarzkopf, M. Daniel; Fiore, Arlene M.; Collins, William J.; Dentener, Frank J.; Shindell, Drew T.; Atherton, Cyndi; Bergmann, Daniel; Duncan, Bryan N.; Hess, Peter; MacKenzie, Ian A.; Marmer, Elina; Schultz, Martin G.; Szopa, Sophie; Wild, Oliver; Zeng, Guang

    2012-01-01

    Ozone (O3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO4 (sup 2-)). We examine changes in the tropospheric composition of O3, CH4, SO4 (sup 2-) and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean plus or minus 1 standard deviation) across multiple CTMs. We evaluate steady state O3 responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 plus or minus 0.6 to 1.7 2 mWm(sup -2)/Tg N yr(sup -1), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 plus or minus 2 mWm(sup -2) for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 plus or minus 0.2 to 0.7 plus or minus 0.2 mWm(sup -2)/Tg C yr(sup -1) and CO emissions (-0.13 plus or minus 0.02 to -0.15 plus or minus 0.02 mWm(sup-2)/Tg CO yr(sup-1). Including the effect of O3 on CO2 uptake by vegetation likely makes these net RFs more negative by -1.9 to- 5.2 mWm(sup -2)/Tg N yr(sup -1), -0.2 to -0.7 mWm(sup -2)/Tg C yr(sup -1), and -0.02 to -0.05 mWm(sup -2)/ Tg CO yr(sup -1). Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO4 (sup -2), regionally to hemispherically by O3, and globally by CH4. Global annual average SO4 2 responses to oxidant changes range from 0.4 plus or minus 2.6 to -1.9 plus or minus 1.3 Gg for NOx reductions, 0.1 plus or minus 1.2 to -0.9 plus

  14. Modeling Trends in Tropospheric Aerosol Burden & Its Radiative Effects

    EPA Science Inventory

    Large changes in emissions of aerosol precursors have occurred across the southeast U.S., North America, as well as the northern hemisphere. The spatial heterogeneity and contrasting trends in the aerosol burden is resulting in differing effects on regional radiative balance. Mul...

  15. Airborne studies of emissions from savanna fires in southern Africa. 1. Aerosol emissions measured with a laser optical particle counter

    NASA Astrophysics Data System (ADS)

    Le Canut, P.; Andreae, M. O.; Harris, G. W.; Wienhold, F. G.; Zenker, T.

    1996-10-01

    During the SAFARI-92 experiment (Southern Africa Fire Atmosphere Research Initiative, September-October 1992), we flew an instrumented DC-3 aircraft through plumes from fires in various southern African savanna ecosystems. Some fires had been managed purposely for scientific study (e.g., those in Kruger National Park, South Africa), while the others were "fires of opportunity" which are abundant during the burning season in southern Africa. We obtained the aerosol (0.1-3.0 μm diameter) number and mass emission ratios relative to carbon monoxide and carbon dioxide from 21 individual fires. The average particle number emission ratio ΔN/ΔCO (Δ: concentrations in plume minus background concentrations) varied between 14 ± 2 cm-3 ppb-1 for grasslands and 23 ± 7 cm-3 ppb-1 for savannas. An exceptionally high value of 43 ± 4 cm-3 ppb-1 was measured for a sugarcane fire. Similarly, the mass emission ratio ΔM/ΔCO varied from 36 ± 6 ng m-3 ppb-1 to 83 ± 45 ng m-3 ppb-1, respectively, with again an exceptionally high value of 124 ± 14 ng m-3 ppb-1 for the sugarcane fire. The number and mass emission ratios relative to CO depended strongly upon the fire intensity. Whereas the emission ratios varied greatly from one fire to the other, the aerosol number and volume distributions as a function of particle size were very consistent. The average background aerosol size distribution was characterized by three mass modes (0.2-0.4 μm, ≈1.0 μm, and ≈2.0 μm diameter). On the other hand, the aerosol size distribution in the smoke plumes showed only two mass modes, one centered in the interval 0.2-0.3 μm and the other above 2 μm diameter. From our mean emission factor (4 ± 1 g kg-1 dm) we estimate that savanna fires release some 11-18 Tg aerosol particles in the size range 0.1-3.0 μm annually, a somewhat lower amount than emitted from tropical forest fires. Worldwide, savanna fires emit some 3-8 × 1027 particles (in the same size range) annually, which is expected

  16. Cardiac and pulmonary oxidative stress in rats exposed to realistic emissions of source aerosols

    PubMed Central

    Lemos, Miriam; Diaz, Edgar A.; Gupta, Tarun; Kang, Choong-Min; Ruiz, Pablo; Coull, Brent A.; Godleski, John J.; Gonzalez-Flecha, Beatriz

    2013-01-01

    In vivo chemiluminescence (CL) is a measure of reactive oxygen species in tissues. CL was used to assess pulmonary and cardiac responses to inhaled aerosols derived from aged emissions of three coal-fired power plants in the USA. Sprague–Dawley rats were exposed to either filtered air or: (1) primary emissions (P); (2) ozone oxidized emissions (PO); (3) oxidized emissions + secondary organic aerosol (SOA) (POS); (4) neutralized oxidized emissions + SOA (PONS); and (5) control scenarios: oxidized emissions + SOA in the absence of primary particles (OS), oxidized emissions alone (O), and SOA alone (S). Immediately after 6 hours of exposure, CL in the lung and heart was measured. Tissues were also assayed for thiobarbituric acid reactive substances (TBARS). Exposure to P or PO aerosols led to no changes compared to filtered air in lung or heart CL at any individual plant or when all data were combined. POS caused significant increases in lung CL and TBARS at only one plant, and not in combined data from all plants; PONS resulted in increased lung CL only when data from all plants were combined. Heart CL was also significantly increased with exposure to POS only when data from all plants were combined. PONS increased heart CL significantly in one plant with TBARS accumulation, but not in combined data. Exposure to O, OS, and S had no CL effects. Univariate analyses of individual measured components of the exposure atmospheres did not identify any component associated with increased CL. These data suggest that coal-fired power plant emissions combined with other atmospheric constituents produce limited pulmonary and cardiac oxidative stress. PMID:21913821

  17. Airborne Measurements of Aerosol Emissions From the Alberta Oil Sands Complex

    NASA Astrophysics Data System (ADS)

    Howell, S. G.; Clarke, A. D.; McNaughton, C. S.; Freitag, S.

    2012-12-01

    The Alberta oil sands contain a vast reservoir of fossil hydrocarbons. The extremely viscous bitumen requires significant energy to extract and upgrade to make a fluid product suitable for pipelines and further refinement. The mining and upgrading process constitute a large industrial complex in an otherwise sparsely populated area of Canada. During the ARCTAS project in June/July 2008, while studying forest fire plumes, the NASA DC-8 and P-3B flew through the plume a total of 5 times. Once was a coordinated visit by both aircraft; the other 3 were fortuitous passes downwind. One study has been published about gas emissions from the complex. Here we concentrate on aerosol emissions and aging. As previously reported, there appear to be at least 2 types of plumes produced. One is an industrial-type plume with vast numbers of ultrafine particles, SO2, sulfate, black carbon (BC), CO, and NO2. The other, probably from the mining, has more organic aerosol and BC together with dust-like aerosols at 3 μm and a 1 μm mode of unknown origin. The DC-8 crossed the plume about 10 km downwind of the industrial site, giving time for the boundary layer to mix and enabling a very crude flux calculation suggesting that sulfate and organic aerosols were each produced at about 500 g/s (estimated errors are a factor of 2, chiefly due to concerns about vertical mixing). Since this was a single flight during a project dedicated to other purposes and operating conditions and weather may change fluxes considerably, this may not be a typical flux. As the plume progresses downwind, the ultrafine particles grow to sizes effective as cloud condensation nucei (CCN), SO2 is converted to sulfate, and organic aerosol is produced. During fair weather in the summer, as was the case during these flights, cloud convection pumps aerosol above the mixed layer. While the aerosol plume is difficult to detect from space, NO2 is measured by the OMI instrument an the Aura satellite and the oil sands plume

  18. Sulfur-rich geothermal emissions elevate acid aerosol levels in metropolitan Taipei.

    PubMed

    Lin, Chih-Hung; Mao, I-Fang; Tsai, Pei-Hsien; Chuang, Hsin-Yi; Chen, Yi-Ju; Chen, Mei-Lien

    2010-08-01

    Several studies have demonstrated that millions of people globally are potentially exposed to volcanic gases. Hydrogen sulfide is a typical gas in volcanic and geothermal areas. The gas is toxic at high concentrations that predominantly affects the nervous, cardiovascular, and respiratory systems. The WHO air quality guideline for hydrogen sulfide is 150 microg m(-3) (105 ppb). The northwest part of Taipei is surrounded by sulfur-rich geothermal and hot springs. Active fumaroles and bubbling springs around the geothermal area emit acidic gases. In combination with automobile emissions, the pollution of acid aerosols is characteristic of the metropolis. This study considered sulfur-rich geothermal, suburban and downtown locations of this metropolis to evaluate geothermally emitted acid aerosol and H(2)S pollution. Acid aerosols were collected using a honeycomb denuder filter pack sampling system (HDS), and then analyzed by ion chromatography (IC). Results indicated that long-term geothermal emissions, automobile emissions and photochemical reactions have led to significant variations in air pollution among regions of metropolitan Taipei. The highest H(2)S concentration was 1705 ppb in the geothermal area with low traffic density and the mean concentration was 404.06 ppb, which was higher than WHO guideline and might cause eye irritation. The SO(2) concentrations were relatively low (mean concentration was 3.9 ppb) in this area. It may partially result from the chemical reduction reaction in the geothermal emission, which converted the SO(2) gas into SO(4)(2-) and H(2)S. Consequently, very high sulfate concentrations (mean concentration higher than 25.0 microg m(-3)) were also observed in the area. The geothermal areas also emitted relatively high levels of aerosol acidity, Cl(-), F(-), PO(4)(3-), and N-containing aerosols. As a result, concentrations of HNO(3), NO(2)(-), PO(4)(3-), and SO(4)(2-) in metropolitan Taipei are significantly higher than those in other

  19. Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

    PubMed Central

    Massoli, Paola; Paglione, Marco; Giulianelli, Lara; Carbone, Claudio; Rinaldi, Matteo; Decesari, Stefano; Sandrini, Silvia; Costabile, Francesca; Gobbi, Gian Paolo; Pietrogrande, Maria Chiara; Visentin, Marco; Scotto, Fabiana; Fuzzi, Sandro; Facchini, Maria Cristina

    2016-01-01

    The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase. Aqueous SOA (aqSOA) formation is observed both in fog water and in wet aerosol. The aqSOA from biomass burning contributes to the “brown” carbon (BrC) budget and exhibits light absorption wavelength dependence close to the upper bound of the values observed in laboratory experiments for fresh and processed biomass-burning emissions. We estimate that the aqSOA from residential wood combustion can account for up to 0.1–0.5 Tg of organic aerosol (OA) per y in Europe, equivalent to 4–20% of the total OA emissions. Our findings highlight the importance of aqSOA from anthropogenic emissions on air quality and climate. PMID:27551086

  20. Direct observation of aqueous secondary organic aerosol from biomass-burning emissions.

    PubMed

    Gilardoni, Stefania; Massoli, Paola; Paglione, Marco; Giulianelli, Lara; Carbone, Claudio; Rinaldi, Matteo; Decesari, Stefano; Sandrini, Silvia; Costabile, Francesca; Gobbi, Gian Paolo; Pietrogrande, Maria Chiara; Visentin, Marco; Scotto, Fabiana; Fuzzi, Sandro; Facchini, Maria Cristina

    2016-09-01

    The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase. Aqueous SOA (aqSOA) formation is observed both in fog water and in wet aerosol. The aqSOA from biomass burning contributes to the "brown" carbon (BrC) budget and exhibits light absorption wavelength dependence close to the upper bound of the values observed in laboratory experiments for fresh and processed biomass-burning emissions. We estimate that the aqSOA from residential wood combustion can account for up to 0.1-0.5 Tg of organic aerosol (OA) per y in Europe, equivalent to 4-20% of the total OA emissions. Our findings highlight the importance of aqSOA from anthropogenic emissions on air quality and climate. PMID:27551086

  1. Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

    NASA Astrophysics Data System (ADS)

    Gilardoni, Stefania; Massoli, Paola; Paglione, Marco; Giulianelli, Lara; Carbone, Claudio; Rinaldi, Matteo; Decesari, Stefano; Sandrini, Silvia; Costabile, Francesca; Gobbi, Gian Paolo; Chiara Pietrogrande, Maria; Visentin, Marco; Scotto, Fabiana; Fuzzi, Sandro; Facchini, Maria Cristina

    2016-09-01

    The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase. Aqueous SOA (aqSOA) formation is observed both in fog water and in wet aerosol. The aqSOA from biomass burning contributes to the “brown” carbon (BrC) budget and exhibits light absorption wavelength dependence close to the upper bound of the values observed in laboratory experiments for fresh and processed biomass-burning emissions. We estimate that the aqSOA from residential wood combustion can account for up to 0.1-0.5 Tg of organic aerosol (OA) per y in Europe, equivalent to 4-20% of the total OA emissions. Our findings highlight the importance of aqSOA from anthropogenic emissions on air quality and climate.

  2. Global top-down smoke aerosol emissions estimation using satellite fire radiative power measurements

    NASA Astrophysics Data System (ADS)

    Ichoku, C.; Ellison, L.

    2013-10-01

    Biomass burning occurs seasonally in most vegetated parts of the world, consuming large amounts of biomass fuel, generating intense heat energy, and emitting corresponding amounts of smoke plumes that comprise different species of aerosols and trace gases. Accurate estimates of these emissions are required as model inputs to evaluate and forecast smoke plume transport and impacts on air quality, human health, clouds, weather, radiation, and climate. Emissions estimates have long been based on bottom-up approaches that are not only complex, but also fraught with compounding uncertainties. Fortunately, a series of recent studies have revealed that both the rate of biomass consumption and the rate of emission of aerosol particulate matter (PM) by open biomass burning are directly proportional to the rate of release of fire radiative energy (FRE), which is fire radiative power (FRP) that is measurable from satellite. This direct relationship enables the determination of coefficients of emission (Ce), which can be used to convert FRP or FRE to smoke aerosol emissions in the same manner as emission factors (EFs) are used to convert burned biomass to emissions. We have leveraged this relationship to generate the first global 1° × 1° gridded Ce product for smoke aerosol or total particulate matter (TPM) emissions using coincident measurements of FRP and aerosol optical thickness (AOT) from the Moderate-resolution Imaging Spectro-radiometer (MODIS) sensors aboard the Terra and Aqua satellites. This new Fire Energetics and Emissions Research version 1.0 (FEER.v1) Ce product has now been released to the community and can be obtained from http://feer.gsfc.nasa.gov/, along with the corresponding 1-to-1 mapping of their quality assurance (QA) flags that will enable the Ce values to be filtered by quality for use in various applications. The regional averages of Ce values for different ecosystem types were found to be in

  3. Aerosol emissions and dimming/brightening in Europe: Sensitivity studies with ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Folini, D.; Wild, M.

    2011-11-01

    Observational data indicate a decrease of surface solar radiation (SSR) in Europe from about 1950 to the mid-1980s, followed by a renewed increase. Changing aerosol emissions have been suggested as a likely cause for this observed dimming and brightening. To quantify this hypothesis, we performed ensembles of transient sensitivity experiments with the global climate model ECHAM5-HAM, which includes interactive treatment of aerosols. The simulations cover the period 1950-2005 and use transient aerosol emissions (National Institute of Environmental Science, Japan) and prescribed sea surface temperatures (SSTs) from the Hadley Centre. The simulated clear-sky dimming and brightening can be attributed to changing aerosol emissions from fossil fuel combustion. Ensemble means of modeled SSR trends are in agreement with observed values. Dimming ceases too early in the model, around 1970. Potential causes are discussed. Brightening sets in at about the right time. Regional differences of modeled SSR are substantial, with clear-sky dimming trends ranging from -6.1 (eastern Europe) to -0.4 W m-2 decade-1 (British Isles) and brightening trends ranging from +1.3 to +6.3 W m-2 decade-1 (Scandinavia and eastern Europe). All-sky conditions show similar trends in the ensemble mean, but the spread among ensemble members is considerable, emphasizing the importance of clouds. Surface temperatures are found to depend mostly on the prescribed SSTs, with an additional aerosol component in some regions like eastern Europe. For precipitation, internal variability is too large to allow for any firm conclusions.

  4. Simulating aerosols over Arabian Peninsula with CHIMERE: Sensitivity to soil, surface parameters and anthropogenic emission inventories

    NASA Astrophysics Data System (ADS)

    Beegum, S. Naseema; Gherboudj, Imen; Chaouch, Naira; Couvidat, Florian; Menut, Laurent; Ghedira, Hosni

    2016-03-01

    A three dimensional chemistry transport model, CHIMERE, was used to simulate the aerosol optical depths (AOD) over the Arabian Peninsula desert with an offline coupling of Weather Research and Forecasting (WRF) model. The simulations were undertaken with: (i) different horizontal and vertical configurations, (ii) new datasets derived for soil/surface properties, and (iii) EDGAR-HTAP anthropogenic emissions inventories. The model performance evaluations were assessed: (i) qualitatively using MODIS (Moderate-Resolution Imaging Spectroradiometer) deep blue (DB) AOD data for the two local dust events of August 6th and 23rd (2013), and (ii) quantitatively using AERONET (Aerosol Robotic Network) AOD observations, CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) aerosol extinction profiles, and AOD simulations from various forecast models. The model results were observed to be highly sensitive to erodibility and aerodynamic surface roughness length. The use of new datasets on soil erodibility, derived from the MODIS reflectance, and aerodynamic surface roughness length (z0), derived from the ERA-Interim datasets, significantly improved the simulation results. Simulations with the global EDGAR-HTAP anthropogenic emission inventories brought the simulated AOD values closer to the observations. Performance testing of the adapted model for the Arabian Peninsula domain with improved datasets showed good agreement between AERONET AOD measurements and CHIMERE simulations, where the correlation coefficient (R) is 0.6. Higher values of the correlation coefficients and slopes were observed for the dusty periods compared to the non-dusty periods.

  5. Thin films of tin(II) sulphide (SnS) by aerosol-assisted chemical vapour deposition (AACVD) using tin(II) dithiocarbamates as single-source precursors

    NASA Astrophysics Data System (ADS)

    Kevin, Punarja; Lewis, David J.; Raftery, James; Azad Malik, M.; O'Brien, Paul

    2015-04-01

    The synthesis of the asymmetric dithiocarbamates of tin(II) with the formula [Sn(S2CNRR')2] (where R=Et, R'=n-Bu (1); R=Me, R'=n-Bu (2); R=R'=Et (3)) and their use for the deposition of SnS thin films by aerosol-assisted chemical vapour deposition (AACVD) is described. The effects of temperature and the concentration of the precursors on deposition were investigated. The stoichiometry of SnS was best at higher concentrations of precursors (250 mM) and at 450 °C. The direct electronic band gap of the SnS produced by this method was estimated from optical absorbance measurements as 1.2 eV. The composition of films was confirmed by powder X-ray diffraction (p-XRD) and energy dispersive analysis of X-rays (EDAX) spectroscopy.

  6. Aerosol emissions from biochar-amended agricultural soils

    NASA Astrophysics Data System (ADS)

    Ravi, S.; Sharratt, B. S.; Li, J. J.; Olshvevski, S.; Meng, Z.; Zhang, J.

    2015-12-01

    Agricultural production is a major contributor to anthropogenic greenhouse gas emissions and associated global warming. In this regard, novel carbon sequestration strategies such as large-scale biochar application may provide sustainable pathways to increase the terrestrial storage of carbon in agricultural areas. Biochar has a long residence time in the soil and hence understanding the soil properties affected by biochar addition needs to be investigated to identify the tradeoffs and synergies of large-scale biochar application. Even though several studies have investigated the impacts of biochar application on a variety of soil properties, very few studies have investigated the impacts on soil erosion, in particular wind (aeolian) erosion and subsequent particulate emissions. Using a combination of wind tunnel studies and laboratory experiments, we investigated the dust emission potential of biochar-amended agricultural soils. We amended biochar (unsieved or sieved to appropriate particle size; application rates ranging from 1 - 5 % of the soil by weight) to three soil types (sand, sandy loam, and silt loam) and estimated the changes in threshold shear velocity for wind erosion and dust emission potential in comparison to control soils. Our experiments demonstrate that emissions of fine biochar particles may result from two mechanisms (a) very fine biochar particles (suspension size) that are entrained into the air stream when the wind velocity exceeds the threshold, and (b) production of fine biochar particles originating from the abrasion by quartz grains. The results indicate that biochar application significantly increased particulate emissions and more interestingly, the rate of increase was found to be higher in the intermediate range of biochar application. As fine biochar particles effectively adsorb/trap contaminants and pathogens from the soil, the preferential erosion of fine biochar particles by wind may lead to concentration of contaminants in the

  7. Emissions and Characteristics of Ice Nucleating Particles Associated with Laboratory Generated Nascent Sea Spray Aerosol

    NASA Astrophysics Data System (ADS)

    McCluskey, C. S.; Hill, T. C. J.; Beall, C.; Sultana, C. M.; Moore, K.; Cornwell, G.; Lee, C.; Al-Mashat, H.; Laskina, O.; Trueblood, J.; Grassian, V. H.; Prather, K. A.; Kreidenweis, S. M.; DeMott, P. J.

    2015-12-01

    Accurate emission rates and activity spectra of atmospheric ice nucleating particles (INPs) are required for proper representation of aerosol-cloud interactions in atmospheric modeling studies. However, few investigations have quantified or characterized oceanic INP emissions. In conjunction with the Center for Aerosol Impacts on the Climate and the Environment, we have directly measured changes in INP emissions and properties of INPs from nascent sea spray aerosol (SSA) through the evolution of phytoplankton blooms. Multiple offline and online instruments were used to monitor aerosol chemistry and size, and bulk water characteristics during two phytoplankton bloom experiments. Two methods were utilized to monitor the number concentrations of INPs from 0 to -34 °C: The online CSU continuous flow diffusion chamber (CFDC) and collections processed offline using the CSU ice spectrometer. Single particle analyses were performed on ice crystal residuals downstream of the CFDC, presumed to be INPs, via scanning transmission electron microscopy (STEM) and Raman microspectroscopy. Preliminary results indicate that laboratory-generated nascent SSA corresponds to number concentrations of INPs that are generally consistent with open ocean regions, based on current knowledge. STEM analyses revealed that the sizes of ice crystal residuals that were associated with nascent SSA ranged from 0.3 to 2.5 μm. Raman microspectroscopy analysis of 1 μm sized residuals found a variety of INP identities, including long chain organics, diatom fragments and polysaccharides. Our data suggest that biological processes play a significant role in ocean INP emissions by generating the species and compounds that were identified during these studies.

  8. The Chemical and Microphysical Properties of Secondary Organic Aerosols from Holm Oak Emissions

    NASA Astrophysics Data System (ADS)

    Lang-Yona, Naama; Rudich, Yinon; Thomas, Mentel; Angela, Buchholz; Astrid, Kiendler-Scharr; Einhard, Kleist; Christian, Spindler; Ralf, Tillmann; Jürgen, Wildt

    2010-05-01

    Plant-emitted volatile organic compounds (VOC) undergo atmospheric oxidation, which leads to the formation of secondary organic aerosols (SOA). Large uncertainties exist about possible climatic effects on SOA formation from biogenic sources. Therefore it is important to investigate the impact of environmental conditions on the plants' emissions, on the formation of biogenic SOA, and on SOA properties in order to understand possible climatic impacts. The Mediterranean region is expected to experience substantial climatic change in the next 50 years and the possible effects on biogenic emissions are yet unexplored. To address such issues, the effects of temperature and light intensity on Mediterranean Holm Oak VOC emissions, as well as on microphysical properties and chemical composition of the resulting SOA have been studied in the Jülich plant aerosol atmosphere chamber. We studied SOA formation from Holm Oak under conditions possibly simulating future climate warming. Monoterpenes dominate the VOC emissions from Holm Oak (97.5%) and temperature increase enhanced the emission strength and changed the emission pattern. Enhanced emissions lead to linearly enhanced SOA formation with a fractional mass yield of SOA (5.7±1%) independent of the detailed emission pattern. The particles are highly scattering with no absorption abilities. Their average hygroscopic growth factor was 1.13±0.03 at 90% RH with a critical diameter of droplet activation was 100±4 nm at a supersaturation of 0.4%. All microphysical properties were not dependent on the detailed emission pattern, in accordance with an invariant O/C ratio (0.57(+0.03/-0.1)) of the SOA as derived from high resolution aerosol mass spectrometry. The temperature increase for the plants essentially led to stronger VOC emissions with the SOA mass being linearly related to the VOC concentrations. However, the increase of Holm oak emissions with temperature (≈ 20 % per degree) was stronger than for Boreal tree species

  9. A Multimodel Assessment of the Influence of Regional Anthropogenic Emission Reductions on Aerosol Direct Radiative Forcing and the Role of Intercontinental Transport

    NASA Technical Reports Server (NTRS)

    Yu, Hongbin; Chin, Mian; West, Jason; Atherton, Cynthia S.; Bellouin, Nicolas; Bergmann, Dan; Bey, Isabelle; Bian, Huisheng; Diehl, Thomas; Forberth, Gerd; Hess, Peter; Schulz, Michael; Shindell, Drew; Takemura, Toshihiko; Tan, Qian

    2013-01-01

    In this study, we assess changes of aerosol optical depth (AOD) and direct radiative forcing (DRF) in response to the reduction of anthropogenic emissions in four major pollution regions in the Northern Hemisphere by using results from nine global models in the framework of the Hemispheric Transport of Air Pollution (HTAP). DRF at top of atmosphere (TOA) and surface is estimated based on AOD results from the HTAP models and AOD-normalized DRF (NDRF) from a chemical transport model. The multimodel results show that, on average, a 20% reduction of anthropogenic emissions in North America, Europe, East Asia, and South Asia lowers the global mean AOD (all-sky TOA DRF) by 9.2% (9.0%), 3.5% (3.0%), and 9.4% (10.0%) for sulfate, particulate organic matter (POM), and black carbon (BC), respectively. Global annual average TOA all-sky forcing efficiency relative to particle or gaseous precursor emissions from the four regions (expressed as multimodel mean +/- one standard deviation) is -3.5 +/-0.8, -4.0 +/- 1.7, and 29.5+/-18.1mW / sq m per Tg for sulfate (relative to SO2), POM, and BC, respectively. The impacts of the regional emission reductions on AOD and DRF extend well beyond the source regions because of intercontinental transport (ICT). On an annual basis, ICT accounts for 11 +/- 5% to 31 +/- 9% of AOD and DRF in a receptor region at continental or subcontinental scale, with domestic emissions accounting for the remainder, depending on regions and species. For sulfate AOD, the largest ICT contribution of 31 +/- 9% occurs in South Asia, which is dominated by the emissions from Europe. For BC AOD, the largest ICT contribution of 28 +/- 18% occurs in North America, which is dominated by the emissions from East Asia. The large spreads among models highlight the need to improve aerosol processes in models, and evaluate and constrain models with observations.

  10. The Use of Combined MODIS and MISR AOD to Constrain Biomass Burning Aerosol Emissions in the GOCART Model

    NASA Astrophysics Data System (ADS)

    Petrenko, M. M.; Kahn, R. A.; Chin, M.

    2013-05-01

    Aerosol models rely heavily on external emission inventories to simulate location and strength of biomass burning (BB) sources. These inventories, however, use different methods and assumptions to estimate aerosol emissions, and consequently their estimates differ, often by a factor of up to 8 globally and even more regionally. We have previously introduced a method of using snapshots of MODIS-measured aerosol optical depth (AOD) to constrain BB emissions in the GOCART model (M. M. Petrenko et al., 2012, JGR). This work builds up on the developed method and aims to (1) address some of the previously discussed method limitations, and (2) apply previously suggested corrections to the BB emissions used in the GOCART model. For example, we increased the number of studied smoke cases, and use MODIS AOD in combination with MISR AOD, which is expected to improve the satellite AOD we use as a reference. We apply previously developed quantitative relationship to correct the emission estimates and assess the performance of the corrected emissions in the model. We expect this method for correcting BB aerosol emissions to be useful to aerosol modelers as well as developers of emission inventories.

  11. Vegetation fires in the himalayan region - Aerosol load, black carbon emissions and smoke plume heights

    NASA Astrophysics Data System (ADS)

    Vadrevu, Krishna Prasad; Ellicott, Evan; Giglio, Louis; Badarinath, K. V. S.; Vermote, Eric; Justice, Chris; Lau, William K. M.

    2012-02-01

    In this study, we investigate the potential of multi-satellite datasets for quantifying the biomass burning emissions from the Himalayan region. A variety of satellite products were used for characterizing fire events including active fire counts, burnt areas, aerosol optical depth (AOD) variations, aerosol index and smoke plume heights. Results from the MODerate-resolution Imaging Spectroradiometer (MODIS) fire product suggest March-June as the major fire season with the peak during the April. An average of 3908 fire counts per year were recorded with sixty four percent of the fires occurring in the low elevation areas in the Himalayan Region. We estimate average burnt areas of 1129 sq. km, with the black carbon emissions of 431 Mg, per year. The mean AOD (2005-2010) was 0.287 ± 0.105 (one sigma) with peak values in May. Correlation analysis between the fire counts and AOD resulted in a Pearson correlation coefficient of 0.553; the correlation between the FRP and AOD is relatively weaker ( r = 0.499). Planetary boundary layer height retrieved from the Modern Era Retrospective-Analysis For Research And Applications (MERRA) product suggests typical PBL height of 1000-1200 m during the April-May peak biomass burning season. Cloud-Aerosol Lidar Orthogonal Polarisation (CALIOP) retrievals show the extent of smoke plume heights beyond the planetary boundary layer during the peak biomass burning month of April. However, comparison of fires in the Himalayan region with other regions and comparisons to aerosol index data from the Ozone Monitoring Instrument (OMI) suggest smoke plumes reaching less than 3 km. Our results on fires and smoke plume height relationships provide valuable information for addressing aerosol transport in the region.

  12. Radiative forcing and climate metrics for ozone precursor emissions: the impact of multi-model averaging

    NASA Astrophysics Data System (ADS)

    MacIntosh, C. R.; Shine, K. P.; Collins, W. J.

    2014-10-01

    Multi-model ensembles are frequently used to assess understanding of the response of ozone and methane lifetime to changes in emissions of ozone precursors such as NOx, VOC and CO. When these ozone changes are used to calculate radiative forcing (RF) (and climate metrics such as the global warming potential (GWP) and global temperature potential (GTP)) there is a methodological choice, determined partly by the available computing resources, as to whether the mean ozone (and methane lifetime) changes are input to the radiation code, or whether each model's ozone and methane changes are used as input, with the average RF computed from the individual model RFs. We use data from the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model ensemble to assess the impact of this choice for emission changes in 4 regions (East Asia, Europe, North America and South Asia). We conclude that using the multi-model mean ozone and methane responses is accurate for calculating the mean RF, with differences up to 0.6% for CO, 0.7% for VOC and 2% for NOx. Differences of up to 60% for NOx 7% for VOC and 3% for CO are introduced into the 20 year GWP as a result of the exponential decay terms, with similar values for the 20 years GTP. However, estimates of the SD calculated from the ensemble-mean input fields (where the SD at each point on the model grid is added to or subtracted from the mean field) are almost always substantially larger in RF, GWP and GTP metrics than the true SD, and can be larger than the model range for short-lived ozone RF, and for the 20 and 100 year GWP and 100 year GTP. We find that the effect is generally most marked for the case of NOx emissions, where the net effect is a smaller residual of terms of opposing signs. For example, the SD for the 20 year GWP is two to three times larger using the ensemble-mean fields than using the individual models to calculate the RF. Hence, while the average of multi-model fields

  13. Light absorbing organic aerosols (brown carbon) over the tropical Indian Ocean: impact of biomass burning emissions

    NASA Astrophysics Data System (ADS)

    Srinivas, Bikkina; Sarin, M. M.

    2013-12-01

    The first field measurements of light absorbing water-soluble organic carbon (WSOC), referred as brown carbon (BrC), have been made in the marine atmospheric boundary layer (MABL) during the continental outflow to the Bay of Bengal (BoB) and the Arabian Sea (ARS). The absorption signal measured at 365 nm in aqueous extracts of aerosols shows a systematic linear increase with WSOC concentration, suggesting a significant contribution from BrC to the absorption properties of organic aerosols. The mass absorption coefficient (babs) of BrC shows an inverse hyperbolic relation with wavelength (from ˜300 to 700 nm), providing an estimate of the Angstrom exponent (αP, range: 3-19 Av: 9 ± 3). The mass absorption efficiency of brown carbon (σabs-BrC) in the MABL varies from 0.17 to 0.72 m2 g-1 (Av: 0.45 ± 0.14 m2 g-1). The αP and σabs-BrC over the BoB are quite similar to that studied from a sampling site in the Indo-Gangetic Plain (IGP), suggesting the dominant impact of organic aerosols associated with the continental outflow. A comparison of the mass absorption efficiency of BrC and elemental carbon (EC) brings to focus the significant role of light absorbing organic aerosols (from biomass burning emissions) in atmospheric radiative forcing over oceanic regions located downwind of the pollution sources.

  14. Final Report, The Influence of Organic-Aerosol Emissions and Aging on Regional and Global Aerosol Size Distributions and the CCN Number Budget

    SciTech Connect

    Donahue, Neil M.

    2015-12-23

    We conducted laboratory experiments and analyzed data on aging of organic aerosol and analysis of field data on volatility and CCN activity. With supplemental ASR funding we participated in the FLAME-IV campaign in Missoula MT in the Fall of 2012, deploying a two-chamber photochemical aging system to enable experimental exploration of photochemical aging of biomass burning emissions. Results from that campaign will lead to numerous publications, including demonstration of photochemical production of Brown Carbon (BrC) from secondary organic aerosol associated with biomass burning emissions as well as extensive characterization of the effect of photochemical aging on the overall concentrations of biomass burning organic aerosol. Excluding publications arising from the FLAME-IV campaign, project research resulted in 8 papers: [11, 5, 3, 10, 12, 4, 8, 7], including on in Nature Geoscience addressing the role of organic compounds in nanoparticle growth [11

  15. Detailed Chemical Characterization of Unresolved Complex Mixtures (UCM) inAtmospheric Organics: Insights into Emission Sources, Atmospheric Processing andSecondary Organic Aerosol Formation

    EPA Science Inventory

    Recent studies suggest that semivolatile organic compounds (SVOCs) are important precursors to secondary organic aerosol (SOA) in urban atmospheres. However, knowledge of the chemical composition of SVOCs is limited by current analytical techniques, which are typically unable to...

  16. Investigation of aviation emission impacts on global tropospheric chemistry and climate using a size-resolved aerosol-chemistry model

    NASA Astrophysics Data System (ADS)

    Kapadia, Zarashpe; Spracklen, Dominick; Arnold, Stephen; Borman, Duncan; Mann, Graham; Pringle, Kirsty; Monks, Sarah; Reddington, Carly; Rap, Alexandru; Scott, Catherine

    2014-05-01

    Aviation is responsible for 3% of global anthropogenic CO2 emissions, but 2-14% of anthropogenic induced climate warming due to contributions from short lived climate forcers. The global civil aviation fleet is projected to double by 2026 in relation to a 2006 baseline and so will play a substantial role in future climate change. Uncertainty in the net impact of aviation on climate is largely due to uncertainty in the impacts of aviation emissions on ozone and aerosol. To study the impact of aviation emissions we use the GLOMAP-mode global aerosol microphysics model coupled to the 3-D chemical transport model TOMCAT. GLOMAP-mode has been extended to include treatment of nitrate aerosol. We include a full suite of non-CO2 aviation emissions (including NOX, SO2, HCs, BC and OC) in the model. We combined the simulated changes in ozone and aerosol with a 3D radiative transfer model to quantify the radiative effect due to aviation non-CO2 emissions. We find that aviation emissions increase O3 concentrations by up to 5.3% in the upper troposphere (UT), broadly matching previous studies. Black carbon (BC) and organic carbon (OC) concentrations increase by 26.5% and 14.6% respectively in the UT, whereas nitrate aerosol is reduced in some regions due to co-emission of NOX and SO2 In the UT, aviation emissions increase both total aerosol number as well as the concentration of particles greater than 70 nm diameter (N70). Entrainment of these particles into the free troposphere results in aviation emissions also increasing N70 in the boundary layer, causing a cooling through the first aerosol indirect effect. We explore differences in these responses compared with those simulated when using the recommended aviation emissions from CMIP5 (5th Climate Model Intercomparison Project), which only include NOX and BC emissions. Our results suggest that aviation emissions of SO2 and HCs neglected by CMIP5 produce important effects on ozone, aerosol number, and N70. We suggest CMIP5

  17. Mutagenicity assessment of aerosols in emissions from domestic combustion processes.

    PubMed

    Canha, Nuno; Lopes, Isabel; Vicente, Estela Domingos; Vicente, Ana M; Bandowe, Benjamin A Musa; Almeida, Susana Marta; Alves, Célia A

    2016-06-01

    Domestic biofuel combustion is one of the major sources of regional and local air pollution, mainly regarding particulate matter and organic compounds, during winter periods. Mutagenic and carcinogenic activity potentials of the ambient particulate matter have been associated with the fraction of polycyclic aromatic hydrocarbons (PAH) and their oxygenated (OPAH) and nitrogenated (NPAH) derivatives. This study aimed at assessing the mutagenicity potential of the fraction of this polycyclic aromatic compound in particles (PM10) from domestic combustion by using the Ames assays with Salmonella typhimurium TA98 and TA100. Seven biofuels, including four types of pellets and three agro-fuels (olive pit, almond shell and shell of pine nuts), were tested in an automatic pellet stove, and two types of wood (Pinus pinaster, maritime pine, and Eucalyptus globulus, eucalypt) were burned in a traditional wood stove. For this latter appliance, two combustion phases-devolatilisation and flaming/smouldering-were characterised separately. A direct-acting mutagenic effect for the devolatilisation phase of pine combustion and for both phases of eucalypt combustion was found. Almond shell revealed a weak direct-acting mutagenic effect, while one type of pellets, made of recycled wastes, and pine (devolatilisation) presented a cytotoxic effect towards strain TA100. Compared to the manually fired appliance, the automatic pellet stove promoted lower polyaromatic mutagenic emissions. For this device, only two of the studied biofuels presented a weak mutagenic or cytotoxic potential. PMID:26893179

  18. Mutagenicity assessment of aerosols in emissions from domestic combustion processes.

    PubMed

    Canha, Nuno; Lopes, Isabel; Vicente, Estela Domingos; Vicente, Ana M; Bandowe, Benjamin A Musa; Almeida, Susana Marta; Alves, Célia A

    2016-06-01

    Domestic biofuel combustion is one of the major sources of regional and local air pollution, mainly regarding particulate matter and organic compounds, during winter periods. Mutagenic and carcinogenic activity potentials of the ambient particulate matter have been associated with the fraction of polycyclic aromatic hydrocarbons (PAH) and their oxygenated (OPAH) and nitrogenated (NPAH) derivatives. This study aimed at assessing the mutagenicity potential of the fraction of this polycyclic aromatic compound in particles (PM10) from domestic combustion by using the Ames assays with Salmonella typhimurium TA98 and TA100. Seven biofuels, including four types of pellets and three agro-fuels (olive pit, almond shell and shell of pine nuts), were tested in an automatic pellet stove, and two types of wood (Pinus pinaster, maritime pine, and Eucalyptus globulus, eucalypt) were burned in a traditional wood stove. For this latter appliance, two combustion phases-devolatilisation and flaming/smouldering-were characterised separately. A direct-acting mutagenic effect for the devolatilisation phase of pine combustion and for both phases of eucalypt combustion was found. Almond shell revealed a weak direct-acting mutagenic effect, while one type of pellets, made of recycled wastes, and pine (devolatilisation) presented a cytotoxic effect towards strain TA100. Compared to the manually fired appliance, the automatic pellet stove promoted lower polyaromatic mutagenic emissions. For this device, only two of the studied biofuels presented a weak mutagenic or cytotoxic potential.

  19. Arabian Sea tropical cyclones intensified by emissions of black carbon and other aerosols.

    PubMed

    Evan, Amato T; Kossin, James P; Chung, Chul Eddy; Ramanathan, V

    2011-11-02

    Throughout the year, average sea surface temperatures in the Arabian Sea are warm enough to support the development of tropical cyclones, but the atmospheric monsoon circulation and associated strong vertical wind shear limits cyclone development and intensification, only permitting a pre-monsoon and post-monsoon period for cyclogenesis. Thus a recent increase in the intensity of tropical cyclones over the northern Indian Ocean is thought to be related to the weakening of the climatological vertical wind shear. At the same time, anthropogenic emissions of aerosols have increased sixfold since the 1930s, leading to a weakening of the southwesterly lower-level and easterly upper-level winds that define the monsoonal circulation over the Arabian Sea. In principle, this aerosol-driven circulation modification could affect tropical cyclone intensity over the Arabian Sea, but so far no such linkage has been shown. Here we report an increase in the intensity of pre-monsoon Arabian Sea tropical cyclones during the period 1979-2010, and show that this change in storm strength is a consequence of a simultaneous upward trend in anthropogenic black carbon and sulphate emissions. We use a combination of observational, reanalysis and model data to demonstrate that the anomalous circulation, which is radiatively forced by these anthropogenic aerosols, reduces the basin-wide vertical wind shear, creating an environment more favourable for tropical cyclone intensification. Because most Arabian Sea tropical cyclones make landfall, our results suggest an additional impact on human health from regional air pollution.

  20. Radiative forcing and climate metrics for ozone precursor emissions: the impact of multi-model averaging

    NASA Astrophysics Data System (ADS)

    MacIntosh, C. R.; Shine, K. P.; Collins, W. J.

    2015-04-01

    Multi-model ensembles are frequently used to assess understanding of the response of ozone and methane lifetime to changes in emissions of ozone precursors such as NOx, VOCs (volatile organic compounds) and CO. When these ozone changes are used to calculate radiative forcing (RF) (and climate metrics such as the global warming potential (GWP) and global temperature-change potential (GTP)) there is a methodological choice, determined partly by the available computing resources, as to whether the mean ozone (and methane) concentration changes are input to the radiation code, or whether each model's ozone and methane changes are used as input, with the average RF computed from the individual model RFs. We use data from the Task Force on Hemispheric Transport of Air Pollution source-receptor global chemical transport model ensemble to assess the impact of this choice for emission changes in four regions (East Asia, Europe, North America and South Asia). We conclude that using the multi-model mean ozone and methane responses is accurate for calculating the mean RF, with differences up to 0.6% for CO, 0.7% for VOCs and 2% for NOx. Differences of up to 60% for NOx 7% for VOCs and 3% for CO are introduced into the 20 year GWP. The differences for the 20 year GTP are smaller than for the GWP for NOx, and similar for the other species. However, estimates of the standard deviation calculated from the ensemble-mean input fields (where the standard deviation at each point on the model grid is added to or subtracted from the mean field) are almost always substantially larger in RF, GWP and GTP metrics than the true standard deviation, and can be larger than the model range for short-lived ozone RF, and for the 20 and 100 year GWP and 100 year GTP. The order of averaging has most impact on the metrics for NOx, as the net values for these quantities is the residual of the sum of terms of opposing signs. For example, the standard deviation for the 20 year GWP is 2-3 times larger

  1. Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

    SciTech Connect

    Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.

    2013-05-10

    Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

  2. Combined trajectory clustering and aerosol fields analysis to evaluate the potential emission flux to aerosol pollutants in an urban and semi-urban atmospheres in eastern India

    NASA Astrophysics Data System (ADS)

    Kumar, B. D.; Verma, S.

    2015-12-01

    A hybrid source-receptor analysis was carried out to evaluate the potential emission flux to winter monsoon (WinMon) aerosols over eastern India urban (Kolkata, Kol) and semi-urban atmospheres (Kharagpur, Kgp). This was done through application of fuzzy c-mean clustering to back-trajectory data combined with emission flux and residence time weighted aerosols analysis. WinMon mean aerosol optical depth (AOD) and angstrom exponent (AE) at Kol were respectively slightly higher than and nearly equal to that at Kgp. Out of six source region clusters over Indian subcontinent and two over Indian oceanic region, the cluster mean AOD was the highest when associated with the mean path of air mass originating from the Bay of Bengal (BoB) and the Arabian sea (AS) clusters at Kol and that from the Indo-Gangetic plain (IGP)cluster at Kgp. Spatial distribution of weighted AOD fields showed the highest potential source of aerosols over the IGP, majorly over upper IGP (IGP-U), lower IGP (IGP-L) and eastern region (ER) clusters. The emission flux contribution potential (EFCP) of fossil fuel (FF) emissions at surface (SL) of Kol/Kgp , elevated layer (EL) of Kol, and of biomass burning (BB) emissions at SL of Kol were majorly from IGP-U, IGP-L and IGP-U/L clusters respectively. The EFCP of FF/BB emissions at Kgp-EL/SL, and that of BB at EL of Kol/Kgp were mainly from ER and Africa (AFR) clusters respectively. Though the AFR cluster was constituted of significantly high emission flux source potential of dust emissions, the EFCP of dust from NWI was comparable to that from AFR at Kol SL/EL.

  3. Time evolution and emission factors of aerosol particles from day and night time savannah fires

    NASA Astrophysics Data System (ADS)

    Vakkari, Ville; Beukes, Johan Paul; Tiitta, Petri; Venter, Andrew; Jaars, Kerneels; Josipovic, Miroslav; van Zyl, Pieter; Kulmala, Markku; Laakso, Lauri

    2013-04-01

    The largest uncertainties in the current global climate models originate from aerosol particle effects (IPCC, 2007) and at the same time aerosol particles also pose a threat to human health (Pope and Dockery, 2006). In southern Africa wild fires and prescribed burning are one of the most important sources of aerosol particles, especially during the dry season from June to September (e.g. Swap et al., 2003; Vakkari et al., 2012). The aerosol particle emissions from savannah fires in southern Africa have been studied in several intensive campaigns such as SAFARI 1992 and 2000 (Swap et al., 2003). However, all previous measurements have been carried out during the daytime, whereas most of the prescribed fires in southern Africa are lit up only after sunset. Furthermore, the previous campaigns followed the plume evolution for up to one hour after emission only. In this study, combining remote sensing fire observations to ground-based long-term measurements of aerosol particle and trace gas properties at the Welgegund measurement station (www.welgegund.org), we have been able to follow the time evolution of savannah fire plumes up to several hours in the atmosphere. For the first time the aerosol particle size distribution measurements in savannah fire plumes cover both day and night time plumes and also the ultrafine size range below 100 nm. During the period from May 20th 2010 to April 15th 2012 altogether 61 savannah fire plumes were observed at Welgegund. The evolution of the aerosol size distribution remained rapid for at least five hours after the fire: during this period the growth rate of the aerosol particle count mean diameter (size range 12 to 840 nm) was 24 nm h-1 for daytime plumes and 8 nm h-1 for night time plumes. The difference in the day and night time growth rate shows that photochemical reactions significantly increase the condensable vapour concentration in the plume. Furthermore, the condensable vapour concentration was found to affect both the

  4. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996-2010

    NASA Astrophysics Data System (ADS)

    Lu, Z.; Zhang, Q.; Streets, D. G.

    2011-09-01

    China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996-2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %-17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be -16 %-17 %, -43 %-93 %, and -43 %-80 % for China, and -15 %-16 %, -41 %-87 %, and -44 %-92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and

  5. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996-2010

    NASA Astrophysics Data System (ADS)

    Lu, Z.; Streets, D. G.

    2011-07-01

    China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996-2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly fractions for major sectors and gridded emissions at a resolution of 0.1° × 0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %-17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be -16 %-17 %, -43 %-93 %, and -43 %-80 % for China, and -15 %-16 %, -41 %-87 %, and -44 %-92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and the actual

  6. Model studies on the global impact of aviation emissions on aerosol and climate

    NASA Astrophysics Data System (ADS)

    Righi, M.; Hendricks, J.; Sausen, R.

    2015-12-01

    We use the EMAC global model with the aerosol module MADE to quantify the impact of aviation emissions on the global aerosol. We focus on the year 2000, prescribing the emissions according to the CMIP5 inventory, and on the year 2030, according to the four RCP scenarios. Various sensitivity experiments are performed to further quantify: (i) the uncertainty behind different assumptions on the size distribution of aviation-emitted particles; (ii) the effect of aviation fuel sulfur content on the simulated impacts; (iii) the linearity of the system's response to emission perturbation. The simulations show that the aviation impact on particle mass (black carbon and sulfate) is small, on the order of a few percent, whereas a large effect is found for particle number. In the northern mid-latitudes' upper troposphere (7-12 km), up to 30-40% of the modelled particle number concentration is attributable to aviation. Significant effects are also simulated at the ground, due to the emissions from landing and take-off cycles. The aviation induced perturbations to the particle number concentrations are very sensitive to the assumptions on the size distribution of emitted particles and on the fuel sulfur content. The simulated aviation-induced RF in the year 2000 is in the range of -69.5 to 2.4 mW/m2. The bulk of this RF is due to aerosol-cloud effects, in particular to the perturbation of low clouds. All RCP scenarios project an increase in the aviation impact in 2030, ranging between a factor of 2 to 4 with respect to 2000, albeit with large uncertainties.

  7. Monitoring of atmospheric aerosol emissions using a remotely piloted air vehicle (RPV)-Borne Sensor Suite

    SciTech Connect

    1996-05-01

    We have developed a small sensor system, the micro-atmospheric measurement system ({mu}-AMS), to monitor and track aerosol emissions. The system was developed to fly aboard a remotely piloted air vehicle, or other mobile platform, to provide real-time particle measurements in effluent plumes and to collect particles for chemical analysis. The {mu}-AMS instrument measures atmospheric parameters including particle mass concentration and size distribution, temperature, humidity, and airspeed, altitude and position (by GPS receiver) each second. The sensor data are stored onboard and are also down linked to a ground station in real time. The {mu}-AMS is battery powered, small (8 in. dia x 36 in.), and lightweight (15 pounds). Aerosol concentrations and size distributions from above ground explosive tests, airbone urban pollution, and traffic-produced particulates are presented.

  8. The Effect of Changes in Polar Sea Ice on Emissions of Marine Aerosols

    NASA Astrophysics Data System (ADS)

    Matrai, P.; Gabric, A. J.

    2015-12-01

    Cloud radiative effects remain a major weakness in our understanding of the climate system and consequently in developing accurate climate projections. This is mainly true for Arctic low-level clouds in their key role of regulating surface energy fluxes which affect the freezing and melting of sea ice. The radiative properties of clouds are strongly dependent on the number concentration of airborne water-soluble particles, known as cloud condensation nuclei (CCN). In the Arctic, the aerosol-cloud-radiation relationship is more complex than elsewhere and the clouds constitute a warming factor for climate, rather than cooling, most of the year. This is due to the semi-permanent ice cover, which raises the albedo of the surface, and the clean Arctic air, which decreases the albedo of the clouds. There has been much discussion on the relative magnitude of the biogenic source of polar CCN: Primary organic marine aerosols and/or sulfate-containing aerosols, derived from marine emissions. Regional field measurements and pan- (Ant)Arctic model simulations don't necessarily agree. Arctic CCN are formed primarily by aggregates of marine organic material and may grow in mass by condensation. Southern Ocean aerosols may be dominated by sulfate particles and organic particles at lower and higher Antarctic latitudes, respectively. The interaction of polar marine microorganisms, seasonality, sea ice cover, presence or absence of sea spray, and atmospheric heterogeneous processes combine to control natural aerosol concentrations and mass, thus modulating the sensitivity of cloud properties, including their reflectivity and the resulting regional radiation budget. We discuss Arctic and Antarctic field and satellite observations and establish a strong and fundamental link between the biology at the ocean/sea ice interface, clouds and climate over polar regions.

  9. Organic Aerosol Formation and Processing in the Los Angeles Basin: Role of Gasoline vs. Diesel Emissions

    NASA Astrophysics Data System (ADS)

    Bahreini, R.; Middlebrook, A. M.; De Gouw, J. A.; Warneke, C.; Trainer, M.; Brown, S. S.; Dube, B.; Holloway, J. S.; Perring, A. E.; Schwarz, J. P.; Spackman, J. R.; Stark, H.; Wagner, N.; Parrish, D. D.

    2011-12-01

    During the CalNex-2010 field project in May-June 2010, the NOAA WP-3D aircraft performed flights up- and down-wind of metropolitan, industrial, agricultural and animal feeding sites in central-southern California. Here airborne data on organic aerosol (OA) properties as measured by a compact time-of-flight aerosol mass spectrometer along with measurements of trace gases affecting secondary production of aerosols in the Los Angeles Basin are presented. The analysis presented indicates that the ratio of organic aerosol to carbon monoxide (OA/CO) is significantly higher than the previously observed ratios of primary OA/CO downwind of urban areas, indicating that even on short time scales of transport within the basin, there is significant production of secondary organic aerosol (SOA). The increase in the ratio of OA/CO is also accompanied by an increase in the fraction of oxygenated species of OA, providing evidence for production of more oxidized SOA as air masses are photochemically processed. Despite a smaller contribution from Diesel vehicles to traffic on weekends, analysis of the weekend vs. weekday data indicates that similar values of ΔOA/ΔCO are observed on the weekends compared to weekdays, for air masses with similar degrees of photochemical processing. This indicates that emissions of gas phase organic species from Diesel vehicles are not significant for OA production in the LA Basin. Our calculated steady-state concentrations of hydroxyl radical (OH) indicate that OH concentrations at mid-day are substantially higher on weekends compared to weekdays, indicating faster chemical processing of air masses during a fixed length of time on the weekends compared to weekdays.

  10. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States

    PubMed Central

    Xu, Lu; Guo, Hongyu; Boyd, Christopher M.; Klein, Mitchel; Bougiatioti, Aikaterini; Cerully, Kate M.; Hite, James R.; Kreisberg, Nathan M.; Knote, Christoph; Olson, Kevin; Koss, Abigail; Goldstein, Allen H.; Hering, Susanne V.; de Gouw, Joost; Baumann, Karsten; Lee, Shan-Hu; Nenes, Athanasios; Weber, Rodney J.; Ng, Nga Lee

    2015-01-01

    Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43–70% of total measured organic aerosol (29–49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic−biogenic interactions and consequently improve air quality and climate simulations. PMID:25535345

  11. Molecular characterization of urban organic aerosol in tropical India: contributions of primary emissions and secondary photooxidation

    NASA Astrophysics Data System (ADS)

    Fu, P. Q.; Kawamura, K.; Pavuluri, C. M.; Swaminathan, T.; Chen, J.

    2010-03-01

    Organic molecular composition of PM10 samples, collected at Chennai in tropical India, was studied using capillary gas chromatography/mass spectrometry. Fourteen organic compound classes were detected in the aerosols, including aliphatic lipids, sugar compounds, lignin products, terpenoid biomarkers, sterols, aromatic acids, hydroxy-/polyacids, phthalate esters, hopanes, Polycyclic Aromatic Hydrocarbons (PAHs), and photooxidation products from biogenic Volatile Organic Compounds (VOCs). At daytime, phthalate esters were found to be the most abundant compound class; however, at nighttime, fatty acids were the dominant one. Di-(2-ethylhexyl) phthalate, C16 fatty acid, and levoglucosan were identified as the most abundant single compounds. The nighttime maxima of most organics in the aerosols indicate a land/sea breeze effect in tropical India, although some other factors such as local emissions and long-range transport may also influence the composition of organic aerosols. However, biogenic VOC oxidation products (e.g., 2-methyltetrols, pinic acid, 3-hydroxyglutaric acid and β-caryophyllinic acid) showed diurnal patterns with daytime maxima. Interestingly, terephthalic acid was maximized at nighttime, which is different from those of phthalic and isophthalic acids. A positive relation was found between 1,3,5-triphenylbenzene (a tracer for plastic burning) and terephthalic acid, suggesting that the field burning of municipal solid wastes including plastics is a significant source of terephthalic acid. Organic compounds were further categorized into several groups to clarify their sources. Fossil fuel combustion (24-43%) was recognized as the most significant source for the total identified compounds, followed by plastic emission (16-33%), secondary oxidation (8.6-23%), and microbial/marine sources (7.2-17%). In contrast, the contributions of terrestrial plant waxes (5.9-11%) and biomass burning (4.2-6.4%) were relatively small. This study demonstrates that, in

  12. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States.

    PubMed

    Xu, Lu; Guo, Hongyu; Boyd, Christopher M; Klein, Mitchel; Bougiatioti, Aikaterini; Cerully, Kate M; Hite, James R; Isaacman-VanWertz, Gabriel; Kreisberg, Nathan M; Knote, Christoph; Olson, Kevin; Koss, Abigail; Goldstein, Allen H; Hering, Susanne V; de Gouw, Joost; Baumann, Karsten; Lee, Shan-Hu; Nenes, Athanasios; Weber, Rodney J; Ng, Nga Lee

    2015-01-01

    Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43-70% of total measured organic aerosol (29-49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic-biogenic interactions and consequently improve air quality and climate simulations. PMID:25535345

  13. Chamber bioaerosol study: human emissions of size-resolved fluorescent biological aerosol particles.

    PubMed

    Bhangar, S; Adams, R I; Pasut, W; Huffman, J A; Arens, E A; Taylor, J W; Bruns, T D; Nazaroff, W W

    2016-04-01

    Humans are a prominent source of airborne biological particles in occupied indoor spaces, but few studies have quantified human bioaerosol emissions. The chamber investigation reported here employs a fluorescence-based technique to evaluate bioaerosols with high temporal and particle size resolution. In a 75-m(3) chamber, occupant emission rates of coarse (2.5-10 μm) fluorescent biological aerosol particles (FBAPs) under seated, simulated office-work conditions averaged 0.9 ± 0.3 million particles per person-h. Walking was associated with a 5-6× increase in the emission rate. During both walking and sitting, 60-70% or more of emissions originated from the floor. The increase in emissions during walking (vs. while sitting) was mainly attributable to release of particles from the floor; the associated increased vigor of upper body movements also contributed. Clothing, or its frictional interaction with human skin, was demonstrated to be a source of coarse particles, and especially of the highly fluorescent fraction. Emission rates of FBAPs previously reported for lecture classes were well bounded by the experimental results obtained in this chamber study. In both settings, the size distribution of occupant FBAP emissions had a dominant mode in the 3-5 μm diameter range. PMID:25704637

  14. Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

    EPA Science Inventory

    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...

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

    NASA Astrophysics Data System (ADS)

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

    2015-11-01

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

  16. Epoxide as a Precursor to Secondary Organic Aerosol Formation from Isoprene Photooxidation in the Presence of Nitrogen Oxides

    EPA Science Inventory

    Isoprene is a substantial contributor to the global secondary organic aerosol (SOA) burden, with implications for public health and the climate system. The mechanism by which isoprene-derived SOA is formed and the influence of environmental conditions, however, remain unclear...

  17. Lagrangian Aerosol and Ozone Precursor Forecasts Utilizing NASA Aura OMI NO2 and NOAA GOES-GASP AOD Observations

    EPA Science Inventory

    Over the past decade, the remote sensing of trace gases and aerosols from space has dramatically improved. The emergence and application of these measurements adds a new dimension to air quality Management and forecasting by enabling consistent observations of pollutants over l...

  18. Light absorption properties and radiative effects of primary organic aerosol emissions.

    PubMed

    Lu, Zifeng; Streets, David G; Winijkul, Ekbordin; Yan, Fang; Chen, Yanju; Bond, Tami C; Feng, Yan; Dubey, Manvendra K; Liu, Shang; Pinto, Joseph P; Carmichael, Gregory R

    2015-04-21

    Organic aerosols (OAs) in the atmosphere affect Earth's energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called "brown carbon" (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (kOA, the fundamental optical parameter determining the particle's absorptivity) and their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the kOA of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based kOA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated kOA values of sectoral and total POA emissions are presented. Results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to ∼27% reduction in the amount of the net global average POA cooling compared to results from the nonabsorbing assumption. PMID:25811601

  19. Toxicological evaluation of realistic emission source aerosols (TERESA)--power plant studies: assessment of breathing pattern.

    PubMed

    Diaz, Edgar A; Lemos, Miriam; Coull, Brent; Long, Mark S; Rohr, Annette C; Ruiz, Pablo; Gupta, Tarun; Kang, Choong-Min; Godleski, John J

    2011-08-01

    Our approach to study multi-pollutant aerosols isolates a single emissions source, evaluates the toxicity of primary and secondary particles derived from this source, and simulates chemical reactions that occur in the atmosphere after emission. Three U.S. coal-fired power plants utilizing different coals and with different emission controls were evaluated. Secondary organic aerosol (SOA) derived from α-pinene and/or ammonia was added in some experiments. Male Sprague-Dawley rats were exposed for 6 h to filtered air or different atmospheric mixtures. Scenarios studied at each plant included the following: primary particles (P); secondary (oxidized) particles (PO); oxidized particles + SOA (POS); and oxidized and neutralized particles + SOA (PONS); additional control scenarios were also studied. Continuous respiratory data were obtained during exposures using whole body plethysmography chambers. Of the 12 respiratory outcomes assessed, each had statistically significant changes at some plant and with some of the 4 scenarios. The most robust outcomes were found with exposure to the PO scenario (increased respiratory frequency with decreases in inspiratory and expiratory time); and the PONS scenario (decreased peak expiratory flow and expiratory flow at 50%). PONS findings were most strongly associated with ammonium, neutralized sulfate, and elemental carbon (EC) in univariate analyses, but only with EC in multivariate analyses. Control scenario O (oxidized without primary particles) had similar changes to PO. Adjusted R(2) analyses showed that scenario was a better predictor of respiratory responses than individual components, suggesting that the complex atmospheric mixture was responsible for respiratory effects.

  20. Light absorption properties and radiative effects of primary organic aerosol emissions.

    PubMed

    Lu, Zifeng; Streets, David G; Winijkul, Ekbordin; Yan, Fang; Chen, Yanju; Bond, Tami C; Feng, Yan; Dubey, Manvendra K; Liu, Shang; Pinto, Joseph P; Carmichael, Gregory R

    2015-04-21

    Organic aerosols (OAs) in the atmosphere affect Earth's energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called "brown carbon" (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (kOA, the fundamental optical parameter determining the particle's absorptivity) and their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the kOA of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based kOA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated kOA values of sectoral and total POA emissions are presented. Results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to ∼27% reduction in the amount of the net global average POA cooling compared to results from the nonabsorbing assumption.

  1. Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols.

    PubMed

    Lee, Hyun Ji Julie; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A

    2013-06-01

    Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines, and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of water-soluble SOA generated from two monoterpenes, limonene and α-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ∼100 ppb ammonia in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (∼0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for λexcitation = 420 ± 50 nm and λemission = 475 ± 38 nm. The window of the strongest fluorescence shifted to λexcitation = 320 ± 25 nm and λemission = 425 ± 38 nm for the α-pinene-derived SOA. Both regions overlap with the EEM spectra of some of the fluorophores found in primary biological aerosols. Despite the low quantum yield, the aged SOA particles may have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

  2. The possible influence of volcanic emissions on atmospheric aerosols in the city of Colima, Mexico.

    PubMed

    Miranda, Javier; Zepeda, Francisco; Galindo, Ignacio

    2004-01-01

    An elemental composition study of atmospheric aerosols from the City of Colima, in the Western Coast of Mexico, is presented. Samples of PM(15)-PM(2.5) and PM(2.5) were collected with Stacked Filter Units (SFU) of the Davis design, in urban and rural sites, the latter located between the City of Colima and the Volcán de Colima, an active volcano. Elemental analyses were carried out using Particle Induced X-ray Emission (PIXE). The gravimetric mass concentrations for the fine fraction were slightly higher in the urban site, while the mean concentrations in the coarse fraction were equal within the uncertainties. High Cl contents were determined in the coarse fraction, a fact also observed in emissions from the Volcán de Colima by other authors. In addition to average elemental concentrations, cluster analysis based on elemental contents was performed, with wind speed and direction data, showing that there is an industrial contributor to aerosols North of the urban area. Moreover, a contribution from the volcanic emissions was identified from the grouping of S, Cl, Cu, and Zn, elements associated to particles emitted by the Volcán de Colima. PMID:14568726

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

    PubMed

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

    2009-04-01

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

  4. Quantification of free-base and protonated nicotine in electronic cigarette liquids and aerosol emissions

    PubMed Central

    El-Hellani, Ahmad; El-Hage, Rachel; Baalbaki, Rima; Talih, Soha; Shihadeh, Alan; Saliba, Najat

    2016-01-01

    Introduction Reliable characterization of the nicotine content and emissions from electronic cigarettes (ECIGs) is crucial for product regulation. Understanding nicotine delivery, and therefore efficacy and abuse potential, from ECIG products requires quantifying the total nicotine contained or emitted, as well as the partitioning between its free-base and protonated forms. To date, studies reporting nicotine content and emissions of ECIGs have not addressed whether the reported values correspond to the total nicotine or only one of its forms, making the reported results difficult to compare across studies, or to correlate against blood exposure measurements. In this study we investigate whether nicotine in ECIGs is indeed present in more than one form, whether measurements are affected by sampling media, and report a validated method for determining total, free-base (Nic) and protonated nicotine (NicH+) in ECIG liquids and aerosol emissions. Methods We developed an analytical method based on liquid-liquid extraction coupled with GC analysis to assess the respective amounts of Nic and NicH+. The method was first verified on pH-controlled solutions (5 < pH < 10) and then was applied to several ECIG liquids and aerosols generated using a smoking machine. Results The method showed high repeatability and efficiency, and the results were in agreement with theoretical predictions based on measured pH of the standard nicotine solutions. ECIG liquids and aerosols contained both Nic and NicH+, and their relative proportions varied widely. Free-base nicotine was found to account for 18-95% of the total nicotine depending on the product in question. Conclusions The wide variation in nicotine partitioning across products suggests that studies of nicotine delivery from ECIGs should account for this factor. A convenient method for analyzing nicotine fractions in electronic cigarettes has been demonstrated. PMID:26158618

  5. Monitoring and analysis of combustion aerosol emissions from fast moving diesel trains.

    PubMed

    Burchill, Michael J; Gramotnev, Dmitri K; Gramotnev, Galina; Davison, Brian M; Flegg, Mark B

    2011-02-01

    In this paper we report the results of the detailed monitoring and analysis of combustion emissions from fast moving diesel trains. A new highly efficient monitoring methodology is proposed based on the measurements of the total number concentration (TNC) of combustion aerosols at a fixed point (on a bridge overpassing the railway) inside the violently mixing zone created by a fast moving train. Applicability conditions for the proposed methodology are presented, discussed and linked to the formation of the stable and uniform mixing zone. In particular, it is demonstrated that if such a mixing zone is formed, the monitoring results are highly consistent, repeatable (with typically negligible statistical errors and dispersion), stable with respect to the external atmospheric turbulence and result in an unusual pattern of the aerosol evolution with two or three distinct TNC maximums. It is also shown that the stability and uniformity of the created mixing zone (as well as the repeatability of the monitoring results) increase with increasing length of the train (with an estimated critical train length of ~10 carriages, at the speed of ~150km/h). The analysis of the obtained evolutionary dependencies of aerosol TNC suggests that the major possible mechanisms responsible for the formation of the distinct concentration maximums are condensation (the second maximum) and thermal fragmentation of solid nanoparticle aggregates (third maximum). The obtained results and the new methodology will be important for monitoring and analysis of combustion emissions from fast moving trains, and for the determination of the impact of rail networks on the atmospheric environment and human exposure to combustion emissions.

  6. A new source of Southern Ocean and Antarctic aerosol from tropospheric polar cell chemistry of sea ice emissions

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Robinson, A. D.; Harris, N. R. P.; Keywood, M.; Ward, J.; Galbally, I.; Molloy, S.; Thomas, A.; Wilson, S. R.

    2014-12-01

    The Antarctic region is a pristine environment with minimal anthropogenic influence. Aerosol measurements in this environment allow the study of natural aerosols and polar atmospheric dynamics. Measurements in this region have been limited primarily to continental and coastal locations where permanent stations exist, with a handful of measurements in the sea ice region. The MAPS campaign (Measurements of Aerosols and Precursors during SIPEXII) occurred as part of SIPEX II (Sea Ice Physics and Ecosystems eXperiment II) voyage in Spring, 2012, and produced the first Antarctic pack-ice focused aerosol dataset aimed at characterizing new particle formation processes off the coast of East Antarctica (~65°S, 120°E). Numerous atmospheric parameters and species were measured, including the number of aerosol particles in the 3-10 nm size range, the range associated with nucleating particle formation. A latitudinal transect through the sea ice identified the Polar Front from sudden changes in nucleating particle concentrations, averaging 51cm-3 north of the front in the Ferrel cell, and 766 cm-3 south of the front, in the Polar cell region. The Polar Front location was also confirmed by meteorological and back-trajectory data. Background aerosol populations in the Polar cell fluctuated significantly but displayed no growth indicators, suggesting transport. Back-trajectories revealed that air parcels often descended from the free-troposphere within the previous 24-48 hrs. It is proposed that particle formation occurs in the free troposphere from precursors uplifted at the polar front region which, being a sea-ice/ocean region, is a significant precursor source. After tropospheric formation, populations descending at the poles are transported northward and reach the sea ice surface, missing continental stations. Current measurements of Antarctic aerosol suggest very low loading which may be explained by these circulation patterns and may underestimate total regional loading

  7. Regional-scale simulations of fungal spore aerosols using an emission parameterization adapted to local measurements of fluorescent biological aerosol particles

    NASA Astrophysics Data System (ADS)

    Hummel, M.; Hoose, C.; Gallagher, M.; Healy, D. A.; Huffman, J. A.; O'Connor, D.; Pöschl, U.; Pöhlker, C.; Robinson, N. H.; Schnaiter, M.; Sodeau, J. R.; Toprak, E.; Vogel, H.

    2014-04-01

    Fungal spores as a prominent type of primary biological aerosol particles (PBAP) have been incorporated into the COSMO-ART regional atmospheric model, using and comparing three different emission parameterizations. Two literature-based emission rates derived from fungal spore colony counts and chemical tracer measurements were used as a parameterization baseline for this study. A third, new emission parameterization was adapted to field measurements of fluorescent biological aerosol particles (FBAP) from four locations across Northern Europe. FBAP concentrations can be regarded as a lower estimate of total PBAP concentrations. Size distributions of FBAP often show a distinct mode at approx. 3 μm, corresponding to a diameter range characteristic for many fungal spores. Previous studies have suggested the majority of FBAP in several locations are dominated by fungal spores. Thus, we suggest that simulated fungal spore concentrations obtained from the emission parameterizations can be compared to the sum of total FBAP concentrations. A comparison reveals that parameterized estimates of fungal spore concentrations based on literature numbers underestimate measured FBAP concentrations. In agreement with measurement data, the model results show a diurnal cycle in simulated fungal spore concentrations, which may develop partially as a consequence of a varying boundary layer height between day and night. Measured FBAP and simulated fungal spore concentrations also correlate similarly with simulated temperature and humidity. These meteorological variables, together with leaf area index, were chosen to drive the new emission parameterization discussed here. Using the new emission parameterization on a model domain covering Western Europe, fungal spores in the lowest model layer comprise a fraction of 15% of the total aerosol mass over land and reach average number concentrations of 26 L-1. The results confirm that fungal spores and biological particles may account for a

  8. Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA): Introduction and overview

    PubMed Central

    Godleski, John J.; Rohr, Annette C.; Kang, Choong M.; Diaz, Edgar A.; Ruiz, Pablo A.; Koutrakis, Petros

    2013-01-01

    Determining the health impacts of sources and components of fine particulate matter (PM2.5) is an important scientific goal. PM2.5 is a complex mixture of inorganic and organic constituents that are likely to differ in their potential to cause adverse health outcomes. The Toxicological Evaluation of Realistic Emissions of Source Aerosols (TERESA) study focused on two PM sources—coal-fired power plants and mobile sources—and sought to investigate the toxicological effects of exposure to emissions from these sources. The set of papers published here document the power plant experiments. TERESA attempted to delineate health effects of primary particles, secondary (aged) particles, and mixtures of these with common atmospheric constituents. TERESA involved withdrawal of emissions from the stacks of three coal-fired power plants in the United States. The emissions were aged and atmospherically transformed in a mobile laboratory simulating downwind power plant plume processing. Toxicological evaluations were carried out in laboratory rats exposed to different emission scenarios with extensive exposure characterization. The approach employed in TERESA was ambitious and innovative. Technical challenges included the development of stack sampling technology that prevented condensation of water vapor from the power plant exhaust during sampling and transfer, while minimizing losses of primary particles; development and optimization of a photochemical chamber to provide an aged aerosol for animal exposures; development and evaluation of a denuder system to remove excess gaseous components; and development of a mobile toxicology laboratory. This paper provides an overview of the conceptual framework, design, and methods employed in the study. PMID:21639692

  9. Investigating the impacts of aviation NOX, SO2 and black carbon emissions on ozone, aerosol and climate.

    NASA Astrophysics Data System (ADS)

    Kapadia, Zarashpe; Borman, Duncan; Spracklen, Dominick; Arnold, Stephen; Mann, Graham; Williams, Paul

    2013-04-01

    Aviation is currently responsible for 3% of global anthropogenic CO2 emissions, but 2-14% of anthropogenic induced warming due to the co-emission of NOX, SO2 and black carbon and formation of contrails. The impact of aviation emissions on ozone and aerosol is uncertain with recent research demonstrating the need to include atmospheric nitrate chemistry. The inclusion of nitrate chemistry may lead to a 20% reduction in aviation induced ozone forcing estimates due to the competition for atmospheric oxidants such as OH . Compounding this, uncertainties relating to the effects of NOx on ozone and methane illustrate the need for refining the understanding of aviation induced impacts. Furthermore the role of aerosol microphysics in controlling the climate impacts of aviation has not yet been explored. Here we use the TOMCAT 3-D chemical transport model coupled to the GLOMAP-mode aerosol microphysics model to quantify the impacts of aviation NOX, SO2 and BC emissions on ozone, aerosol and climate. GLOMAP-mode treats size resolved aerosol using a two-moment modal approach. We evaluate the effects of nitrate processing on the diagnosed impacts of aviation emissions on atmospheric composition including the first assessment of the impact on the global concentrations of cloud condensation nuclei. We investigate interactions between gas-phase oxidant photochemistry and aerosol microphysics in regions influenced by aircraft emissions, using fully-coupled tropospheric chemistry and multi-component aerosol treatment (BC, sulphate, nitrate). Finally, we use a 3-D radiative transfer model to quantify the ozone and aerosol direct and indirect radiative effects of aviation emissions. The work presented here is part of a wider research project which will be the first study to combine aviation NOX, SO2 and black carbon emission in a global size-resolved model which considers atmospheric nitrate chemistry, which will aim to add to the science surrounding present day aviation impacts by

  10. Aerosol Radiative Forcing Estimates from South Asian Clay Brick Production Based on Direct Emission Measurements

    NASA Astrophysics Data System (ADS)

    Weyant, C.; Athalye, V.; Ragavan, S.; Rajarathnam, U.; Kr, B.; Lalchandani, D.; Maithel, S.; Malhotra, G.; Bhanware, P.; Thoa, V.; Phuong, N.; Baum, E.; Bond, T. C.

    2012-12-01

    About 150-200 billion clay bricks are produced in India every year. Most of these bricks are fired in small-scale traditional kilns that burn coal or biomass without pollution controls. Reddy and Venkataraman (2001) estimated that 8% of fossil fuel related PM2.5 emissions and 23% of black carbon emissions in India are released from brick production. Few direct emissions measurements have been done in this industry and black carbon emissions, in particular, have not been previously measured. In this study, 9 kilns representing five common brick kiln technologies were tested for aerosol properties and gaseous pollutant emissions, including optical scattering and absorption and thermal-optical OC/EC. Simple relationships are then used to estimate the radiative-forcing impact. Kiln design and fuel quality greatly affect the overall emission profiles and relative climate warming. Batch production kilns, such as the Downdraft kiln, produce the most PM2.5 (0.97 gPM2.5/fired brick) with an OC/EC fraction of 0.3. Vertical Shaft Brick kilns using internally mixed fuels produce the least PM (0.09 gPM2.5/kg fired brick) with the least EC (OC/EC = 16.5), but these kilns are expensive to implement and their use throughout Southern Asia is minimal. The most popular kiln in India, the Bull's Trench kiln, had fewer emissions per brick than the Downdraft kiln, but an even higher EC fraction (OC/EC = 0.05). The Zig-zag kiln is similar in structure to the Bull's Trench kiln, but the emission factors are significantly lower: 50% reduction for CO, 17% for PM2.5 and 60% for black carbon. This difference in emissions suggests that converting traditional Bull's Trench kilns into less polluting Zig-zag kilns would result in reduced atmospheric warming from brick production.

  11. Efficient formation of stratospheric aerosol for climate engineering by emission of condensible vapor from aircraft

    NASA Astrophysics Data System (ADS)

    Pierce, Jeffrey R.; Weisenstein, Debra K.; Heckendorn, Patricia; Peter, Thomas; Keith, David W.

    2010-09-01

    Recent analysis suggests that the effectiveness of stratospheric aerosol climate engineering through emission of non-condensable vapors such as SO2 is limited because the slow conversion to H2SO4 tends to produce aerosol particles that are too large; SO2 injection may be so inefficient that it is difficult to counteract the radiative forcing due to a CO2 doubling. Here we describe an alternate method in which aerosol is formed rapidly in the plume following injection of H2SO4, a condensable vapor, from an aircraft. This method gives better control of particle size and can produce larger radiative forcing with lower sulfur loadings than SO2 injection. Relative to SO2 injection, it may reduce some of the adverse effects of geoengineering such as radiative heating of the lower stratosphere. This method does not, however, alter the fact that such a geoengineered radiative forcing can, at best, only partially compensate for the climate changes produced by CO2.

  12. Efficient Formation of Stratospheric Aerosol for Climate Engineering by Emission of Condensible Vapor from Aircraft

    NASA Technical Reports Server (NTRS)

    Pierce, Jeffrey R.; Weisenstein, Debra K.; Heckendorn, Patricia; Peter. Thomas; Keith, David W.

    2010-01-01

    Recent analysis suggests that the effectiveness of stratospheric aerosol climate engineering through emission of non-condensable vapors such as SO2 is limited because the slow conversion to H2SO4 tends to produce aerosol particles that are too large; SO2 injection may be so inefficient that it is difficult to counteract the radiative forcing due to a CO2 doubling. Here we describe an alternate method in which aerosol is formed rapidly in the plume following injection of H2SO4, a condensable vapor, from an aircraft. This method gives better control of particle size and can produce larger radiative forcing with lower sulfur loadings than SO2 injection. Relative to SO2 injection, it may reduce some of the adverse effects of geoengineering such as radiative heating of the lower stratosphere. This method does not, however, alter the fact that such a geoengineered radiative forcing can, at best, only partially compensate for the climate changes produced by CO2.

  13. Carbonaceous aerosols over China--review of observations, emissions, and climate forcing.

    PubMed

    Wang, Linpeng; Zhou, Xuehua; Ma, Yujie; Cao, Zhaoyu; Wu, Ruidong; Wang, Wenxing

    2016-01-01

    Carbonaceous aerosols have been attracting attention due to the influence on visibility, air quality, and regional climate. Statistical analyses based on concentration levels, spatial-temporal variations, correlations, and organic carbon (OC) to element carbon (EC) ratios from published data of OC and EC in particulate matter (PM2.5 and PM10) were carried out in order to give a carbonaceous aerosol profile in China. The results showed maxima for OC of 29.5 ± 18.2 μg C m(-3) and for EC of 8.4 ± 6.3 μg C m(-3) in winter and minima for OC of 12.9 ± 7.7 μg C m(-3) in summer and for EC of 4.6 ± 2.8 μg C m(-3) in spring. In addition, OC and EC both had higher concentrations in urban than those in rural sites. Carbonaceous aerosol levels in China are about three to seven times higher compared to those in the USA and Europe. OC and EC occupied 20 ± 6 and 7 ± 3% of PM2.5 mass and 17 ± 7 and 5 ± 3% of PM10 mass, respectively, implying that carbonaceous aerosols are the main component of PM, especially OC. Secondary organic carbon (SOC) was a significant portion of PM and contributed 41 ± 26% to OC and 8 ± 6% to PM2.5 mass. The OC/EC ratio was 3.63 ± 1.73, which, along with the good correlation between OC and EC and the OC to EC slope of 2.29, signifies that coal combustion and/or vehicular exhaust is the dominated carbonaceous aerosol source in China. These provide a primary observation-based understanding of carbonaceous aerosol pollution in China and have a great significance in improving the emission inventory and climate forcing evaluation.

  14. Carbonaceous aerosols over China--review of observations, emissions, and climate forcing.

    PubMed

    Wang, Linpeng; Zhou, Xuehua; Ma, Yujie; Cao, Zhaoyu; Wu, Ruidong; Wang, Wenxing

    2016-01-01

    Carbonaceous aerosols have been attracting attention due to the influence on visibility, air quality, and regional climate. Statistical analyses based on concentration levels, spatial-temporal variations, correlations, and organic carbon (OC) to element carbon (EC) ratios from published data of OC and EC in particulate matter (PM2.5 and PM10) were carried out in order to give a carbonaceous aerosol profile in China. The results showed maxima for OC of 29.5 ± 18.2 μg C m(-3) and for EC of 8.4 ± 6.3 μg C m(-3) in winter and minima for OC of 12.9 ± 7.7 μg C m(-3) in summer and for EC of 4.6 ± 2.8 μg C m(-3) in spring. In addition, OC and EC both had higher concentrations in urban than those in rural sites. Carbonaceous aerosol levels in China are about three to seven times higher compared to those in the USA and Europe. OC and EC occupied 20 ± 6 and 7 ± 3% of PM2.5 mass and 17 ± 7 and 5 ± 3% of PM10 mass, respectively, implying that carbonaceous aerosols are the main component of PM, especially OC. Secondary organic carbon (SOC) was a significant portion of PM and contributed 41 ± 26% to OC and 8 ± 6% to PM2.5 mass. The OC/EC ratio was 3.63 ± 1.73, which, along with the good correlation between OC and EC and the OC to EC slope of 2.29, signifies that coal combustion and/or vehicular exhaust is the dominated carbonaceous aerosol source in China. These provide a primary observation-based understanding of carbonaceous aerosol pollution in China and have a great significance in improving the emission inventory and climate forcing evaluation. PMID:26385857

  15. Top-down constraints to aerosol emissions from open biomass burning: the role of gas-particle partitioning and secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Konovalov, Igor B.; Beekmann, Matthias; Berezin, Evgeny V.; Petetin, Hervé

    2014-05-01

    Open biomass burning (BB), including wildfires and controlled burns in agriculture and foresty, is known to provide an important contribution to organic aerosol (OA) and black carbon (BC) emissions on the global scale. However, quantitative estimates of BB aerosol emissions and their effects on climate and environment remain rather uncertain. A useful way to constrain the OA&BC emissions involves using atmospheric measurements in the framework of the inverse modeling approach. In such an approach, the relationship between the emissions and the measurements is simulated by a chemistry transport model; this means that top-down estimates may be sensitive to possible model uncertainties. As a result of assimilation of satellite measurements of aerosol optical depth, several recent studies (e.g. [1,2]) indicated that aerosol emissions provided by bottom-up emission inventories may be strongly underestimated relative to emissions of gaseous species (such as CO). Meanwhile, it was earlier shown (e.g. [3]) that the relationship between primary organic aerosol emissions and aerosol concentration in the atmosphere can be significantly affected by gas-particle partitioning and oxidation of lower-volatility organic emissions; these processes are usually not taken into account in typical chemistry transport models. The main goal of this study was to examine to what degree the discrepancy between the OA&BC/CO emission ratios predicted by the bottom-up inventories and derived from satellite observations can be associated with the mentioned processes and explained in the framework of the volatility basis set approach (VBS) [3] to OA modelling. To achieve this goal, a VBS scheme, which was recently implemented in the CHIMERE chemistry transport model (CTM), was first modified to account for OA emissions from biomass burning. An ensemble of simulations with the CHIMERE CTM was then performed for the case of the 2010 mega-fire event in European Russia [4]; each of the simulations

  16. Time-resolved inorganic chemical composition of fine aerosol and associated precursor gases over an urban environment in western India: Gas-aerosol equilibrium characteristics

    NASA Astrophysics Data System (ADS)

    Sudheer, A. K.; Rengarajan, R.

    2015-05-01

    Inorganic ionic constituents (Na+, NH4+, K+, Mg2+, Ca2+, Cl-, NO3- and SO42-) of PM2.5 and associated trace gases (NH3, HNO3 and HCl) were measured simultaneously by Ambient Ion Monitor - Ion Chromatograph (AIM-IC) system with a time resolution of one hour at an urban location in semi-arid region of western India during summer and winter. The average NH3, HNO3 and HCl concentrations were 11.6 ± 5.0, 2.9 ± 0.8 and 0.15 μg m-3, respectively, during winter. During summer, NH3 and HNO3 concentrations were of similar magnitude, whereas HCl concentration was less than ∼0.03 μg m-3. NH3 concentration exhibited a distinct diurnal variation during both seasons. However, HNO3 did not show a specific diurnal trend during the observation period in both seasons. The data obtained were used to study gas-aerosol equilibrium characteristics using a thermodynamic equilibrium model, ISORROPIA II. The results suggest that NH3 exists in equilibrium between measured fine-mode particle and gas phase with a systematic bias of ∼14%, whereas HCl and HNO3 deviate significantly from the modelled data. These observations have implications on thermodynamic equilibrium assumptions used for estimating various aerosol parameters such as liquid water content, pH, etc., thus causing significant bias in chemical transport model results over the study region.

  17. Quantitative evaluation of emission controls on primary and secondary organic aerosol sources during Beijing 2008 Olympics

    NASA Astrophysics Data System (ADS)

    Guo, S.; Hu, M.; Guo, Q.; Zhang, X.; Schauer, J. J.; Zhang, R.

    2013-08-01

    To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU) and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. The average PM2.5 concentrations were 72.5 ± 43.6 μg m-3 and 64.3 ± 36.2 μg m-3 (average ± standard deviation, below as the same) at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance) model and secondary organic aerosol (SOA) tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 ± 5.9% and 14.5 ± 4.1% and gasoline vehicles contributing 10.3 ± 8.7% and 7.9 ± 6.2% to organic carbon (OC) at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.

  18. Atmospheric emitted radiance interferometer (AERI): Status and the aerosol explanation for extra window region emissions

    SciTech Connect

    Revercomb, H.E.; Knuteson, R.O.; Best, F.A.; Dirkx, T.P.

    1996-04-01

    High spectral resolution observations of downwelling emission from 3 to 19 microns have been made by the Atmospheric Emitted Radiance Interferometer (AERI) Prototype at the Southern Great Plains (SGP) Cloud and Radiative Testbed (CART) site for over two years. The spectral data set from AERI provides a basis for improving clear sky radiative transfer; determining the radiative impact of clouds, including the derivation of cloud radiative properties; defining the influences of aerosols in the window regions; and retrieving boundary layer state properties, including temperature, water vapor, and other trace gases. The data stream of radiometrically and spectrally calibrated radiances is routinely provided by Pacific Northwest Laboratory (PNL) to those science teams requesting it, and further information on the instrument and data characteristics is available in the ARM Science Team proceedings for 1993 and 1994 and in several conference publications. This paper describes the AERI status, calibration, field experiment wit a new AERI-01 and schedule, window region emissions, and future AERI plans.

  19. Modelling African aerosol using updated fossil fuel and biofuel emission inventories for 2005 and 2030

    NASA Astrophysics Data System (ADS)

    Liousse, C.; Penner, J. E.; Assamoi, E.; Xu, L.; Criqui, P.; Mima, S.; Guillaume, B.; Rosset, R.

    2010-12-01

    A regional fossil fuel and biofuel emission inventory for particulates has been developed for Africa at a resolution of 0.25° x 0.25° for the year 2005. The original database of Junker and Liousse (2008) was used after modification for updated regional fuel consumption and emission factors. Consumption data were corrected after direct inquiries conducted in Africa, including a new emitter category (i.e. two-wheel vehicles including “zemidjans”) and a new activity sector (i.e. power plants) since both were not considered in the previous emission inventory. Emission factors were measured during the 2005 AMMA campaign (Assamoi and Liousse, 2010) and combustion chamber experiments. Two prospective inventories for 2030 are derived based on this new regional inventory and two energy consumption forecasts by the Prospective Outlook on Long-term Energy Systems (POLES) model (Criqui, 2001). The first is a reference scenario, where no emission controls beyond those achieved in 2003 are taken into account, and the second is for a "clean" scenario where possible and planned policies for emission control are assumed to be effective. BC and OCp emission budgets for these new inventories will be discussed and compared to the previous global dataset. These new inventories along with the most recent open biomass burning inventory (Liousse et al., 2010) have been tested in the ORISAM-TM5 global chemistry-climate model with a focus over Africa at a 1° x 1° resolution. Global simulations for BC and primary OC for the years 2005 and 2030 are carried out and the modelled particulate concentrations for 2005 are compared to available measurements in Africa. Finally, BC and OC radiative properties (aerosol optical depths and single scattering albedo) are calculated and the direct radiative forcing is estimated using an off line model (Wang and Penner, 2009). Results of sensitivity tests driven with different emission scenarios will be presented.

  20. Gas-particle partitioning of primary organic aerosol emissions: (1) Gasoline vehicle exhaust

    NASA Astrophysics Data System (ADS)

    May, Andrew A.; Presto, Albert A.; Hennigan, Christopher J.; Nguyen, Ngoc T.; Gordon, Timothy D.; Robinson, Allen L.

    2013-10-01

    The gas-particle partitioning of the primary organic aerosol (POA) emissions from fifty-one light-duty gasoline vehicles (model years 1987-2012) was investigated at the California Air Resources Board Haagen-Smit Laboratory. Each vehicle was operated over the cold-start unified cycle on a chassis dynamometer and its emissions were sampled using a constant volume sampler. Four independent yet complementary approaches were used to investigate POA gas-particle partitioning: sampling artifact correction of quartz filter data, dilution from the constant volume sampler into a portable environmental chamber, heating in a thermodenuder, and thermal desorption/gas chromatography/mass spectrometry analysis of quartz filter samples. This combination of techniques allowed gas-particle partitioning measurements to be made across a wide range of atmospherically relevant conditions - temperatures of 25-100 °C and organic aerosol concentrations of <1-600 μg m-3. The gas-particle partitioning of the POA emissions varied continuously over this entire range of conditions and essentially none of the POA should be considered non-volatile. Furthermore, for most vehicles, the low levels of dilution used in the constant volume sampler created particle mass concentrations that were greater than a factor of 10 or higher than typical ambient levels. This resulted in large and systematic partitioning biases in the POA emission factors compared to more dilute atmospheric conditions, as the POA emission rates may be over-estimated by nearly a factor of four due to gas-particle partitioning at higher particle mass concentrations. A volatility distribution was derived to quantitatively describe the measured gas-particle partitioning data using absorptive partitioning theory. Although the POA emission factors varied by more than two orders of magnitude across the test fleet, the vehicle-to-vehicle differences in gas-particle partitioning were modest. Therefore, a single volatility distribution

  1. Composition of Secondary Organic Aerosols Produced by Photo-Oxidation of Biomass Burning Emissions in a Smog Chamber

    NASA Astrophysics Data System (ADS)

    Desyaterik, Y.; Sullivan, A.; Hennigan, C. J.; Robinson, A. L.; Collett, J. L.

    2009-12-01

    Knowledge of the chemical composition of atmospheric organic aerosols (OA) is essential for accurate representation of OA in air quality and climate models. Both the sources of OA and their properties and effects remain poorly understood. In particular, we still know relatively little about the atmospheric formation of secondary organic aerosols (SOA). There is growing interest in the impact of biomass burning emissions on air quality, human health, and radiative forcing. Through a series of experiments, we are working to quantify changes in the chemical composition of wood smoke particles as a result of photochemical aging under well-controlled laboratory conditions. One specific objective of this study is to identify markers for biomass burning SOA and test whether these markers can be used in atmospheric samples to quantify SOA formation from aging of biomass burning emissions. We analyzed SOA generated in a smog chamber by photooxidation of smoke produced by burning oak wood. In order to initiate photochemistry, the chamber was irradiated with UV light. Aqueous extracts of collected aerosol samples were analyzed with Electrospray Ionization Time-of-Flight Mass Spectrometry. The high mass accuracy of these measurements reduces ambiguity in the assignment of elemental compositions for observed ions. Analysis has shown that primary oak smoke aerosol includes products of the thermal decomposition of cellulose (levoglucosan, cyclotene etc.) and lignin (guaiacol and syringol derivatives, mostly aldehydes and alcohols). After 2 hours of aging at typical summertime hydroxyl radical concentrations, the aerosol mass increased 2.5 fold due to the production of secondary organic aerosol. Mass spectra of the secondary organic aerosol formed are dominated by organic nitrates (nitrophenol, nitrocresol, nitrocatechol, and nitroguaiacol) and aromatic acids (benzoic acid, mono and di-hydroxybenzoic acid). Both nitrates and acids most likely are formed due to oxidation of the

  2. Properties of aerosols from sugar-cane burning emissions in Southeastern Brazil

    NASA Astrophysics Data System (ADS)

    Lara, L. L.; Artaxo, P.; Martinelli, L. A.; Camargo, P. B.; Victoria, R. L.; Ferraz, E. S. B.

    The influences of biomass burning emissions in the composition of aerosol have been studied during 1 year around the city of Piracicaba (Southeastern Brazil). Inhalable particles, separated in PM 2.5 and coarse particulate mode (CPM, with size in the range (2.5< dp<10 μm)), were sampled from April 1997 to March 1998 and analyzed for BC, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Se, Br, Rb, Sr, Zr, Pb. The average concentrations of PM 2.5, CPM, BC and chemical elements were statistically higher in the dry season than in the wet season. The results of absolute principal component analysis showed four and three different sources for PM 2.5 and CPM, respectively. Sugar-cane burning is the main source of PM 2.5 representing 60% of PM 2.5, soil dust accounted for 14%, and industries and oil combustion contributed with 12% each one. Resuspended soil is the main source of CPM followed by industrial emissions and sugar-cane burning. The sampling and analytical procedures applied in this study showed that sugar-cane burning and agricultural practices are the main sources of inhalable particles, possibly altering the aerosol composition around the city of Piracicaba.

  3. Analysis of particulate emissions from tropical biomass burning using a global aerosol model and long-term surface observations

    NASA Astrophysics Data System (ADS)

    Reddington, Carly L.; Spracklen, Dominick V.; Artaxo, Paulo; Ridley, David A.; Rizzo, Luciana V.; Arana, Andrea

    2016-09-01

    We use the GLOMAP global aerosol model evaluated against observations of surface particulate matter (PM2.5) and aerosol optical depth (AOD) to better understand the impacts of biomass burning on tropical aerosol over the period 2003 to 2011. Previous studies report a large underestimation of AOD over regions impacted by tropical biomass burning, scaling particulate emissions from fire by up to a factor of 6 to enable the models to simulate observed AOD. To explore the uncertainty in emissions we use three satellite-derived fire emission datasets (GFED3, GFAS1 and FINN1). In these datasets the tropics account for 66-84 % of global particulate emissions from fire. With all emission datasets GLOMAP underestimates dry season PM2.5 concentrations in regions of high fire activity in South America and underestimates AOD over South America, Africa and Southeast Asia. When we assume an upper estimate of aerosol hygroscopicity, underestimation of AOD over tropical regions impacted by biomass burning is reduced relative to previous studies. Where coincident observations of surface PM2.5 and AOD are available we find a greater model underestimation of AOD than PM2.5, even when we assume an upper estimate of aerosol hygroscopicity. Increasing particulate emissions to improve simulation of AOD can therefore lead to overestimation of surface PM2.5 concentrations. We find that scaling FINN1 emissions by a factor of 1.5 prevents underestimation of AOD and surface PM2.5 in most tropical locations except Africa. GFAS1 requires emission scaling factor of 3.4 in most locations with the exception of equatorial Asia where a scaling factor of 1.5 is adequate. Scaling GFED3 emissions by a factor of 1.5 is sufficient in active deforestation regions of South America and equatorial Asia, but a larger scaling factor is required elsewhere. The model with GFED3 emissions poorly simulates observed seasonal variability in surface PM2.5 and AOD in regions where small fires dominate, providing

  4. Heterocyclic dithiocarbamato-iron(III) complexes: single-source precursors for aerosol-assisted chemical vapour deposition (AACVD) of iron sulfide thin films.

    PubMed

    Mlowe, Sixberth; Lewis, David J; Malik, Mohammad Azad; Raftery, James; Mubofu, Egid B; O'Brien, Paul; Revaprasadu, Neerish

    2016-02-14

    Tris-(piperidinedithiocarbamato)iron(III) (1) and tris-(tetrahydroquinolinedithiocarbamato)iron(iii) (2) complexes have been synthesized and their single-crystal X-ray structures were determined. Thermogravimetric analysis (TGA) of the complexes showed decomposition to iron sulfide. Both complexes were then used as single-source precursors for the deposition of iron sulfide thin films by aerosol-assisted chemical vapour deposition (AACVD). Energy-dispersive X-ray (EDX) spectroscopy confirmed the formation of iron sulfide films. The addition of tert-butyl thiol almost doubled the sulfur content in the deposited films. Scanning electron microscopy (SEM) images of the iron sulfide films from both complexes showed flakes/leaves/sheets, spherical granules and nanofibres. The sizes and shapes of these crystallites depended on the nature of the precursor, temperature, solvent and the amount of tert-butyl thiol used. The observed optical properties are dependent upon the variation of reaction parameters such as temperature and solvent. Powder X-ray diffraction (p-XRD) studies revealed that pyrrhotite, hexagonal (Fe0.975S), marcasite and smythite (Fe3S4) phases were differently deposited. PMID:26732865

  5. Regional-scale simulations of fungal spore aerosols using an emission parameterization adapted to local measurements of fluorescent biological aerosol particles

    NASA Astrophysics Data System (ADS)

    Hummel, M.; Hoose, C.; Gallagher, M.; Healy, D. A.; Huffman, J. A.; O'Connor, D.; Pöschl, U.; Pöhlker, C.; Robinson, N. H.; Schnaiter, M.; Sodeau, J. R.; Stengel, M.; Toprak, E.; Vogel, H.

    2015-06-01

    Fungal spores as a prominent type of primary biological aerosol particles (PBAP) have been incorporated into the COSMO-ART (Consortium for Small-scale Modelling-Aerosols and Reactive Trace gases) regional atmospheric model. Two literature-based emission rates for fungal spores derived from fungal spore colony counts and chemical tracer measurements were used as a parameterization baseline for this study. A third, new emission parameterization for fluorescent biological aerosol particles (FBAP) was adapted to field measurements from four locations across Europe. FBAP concentrations can be regarded as a lower estimate of total PBAP concentrations. Size distributions of FBAP often show a distinct mode at approx. 3 μm, corresponding to a diameter range characteristic for many fungal spores. Previous studies for several locations have suggested that FBAP are in many cases dominated by fungal spores. Thus, we suggest that simulated FBAP and fungal spore concentrations obtained from the three different emission parameterizations can be compared to FBAP measurements. The comparison reveals that simulated fungal spore concentrations based on literature emission parameterizations are lower than measured FBAP concentrations. In agreement with the measurements, the model results show a diurnal cycle in simulated fungal spore concentrations, which may develop partially as a consequence of a varying boundary layer height between day and night. Temperature and specific humidity, together with leaf area index (LAI), were chosen to drive the new emission parameterization which is fitted to the FBAP observations. The new parameterization results in similar root mean square errors (RMSEs) and correlation coefficients compared to the FBAP observations as the previously existing fungal spore emission parameterizations, with some improvements in the bias. Using the new emission parameterization on a model domain covering western Europe, FBAP in the lowest model layer comprise a

  6. Stress-induced biogenic VOC emissions from typical European tree species, their impact on secondary organic aerosol formation and possible climate feedbacks

    NASA Astrophysics Data System (ADS)

    Kleist, E.; Mentel, T. F.; Andres, S.; Dal Maso, M.; Hohaus, T.; Kindler-Scharr, A.; Rudich, Y.; Springer, M.; Tillmann, R.; Uerlings, R.; Wahner, A.; Wildt, J.

    2011-12-01

    Biogenic volatile organic compounds (BVOC) are precursors of secondary organic aerosols (SOA), which can scatter and absorb radiation. BVOC therefore indirectly impact the Earth's climate. Earth's climate is projected to change, possibly putting and vegetation under stress due to intensive heat and drought periods. Such stress situations will alter BVOC emissions that may induce feedbacks between vegetation and climate change. The main aim of our study is to determine whether such effect exists. A first step was to determine the impacts of drought and heat on BVOC emissions and subsequent SOA formation. Experiments were performed in the Juelich plant atmosphere chamber. Pine and Spruce were taken as representatives for species exhibiting storage organs for monoterpenes (MT). Beech and Birch were used as species with MT emissions closely coupled to CO2 uptake. The plants were stored under well-defined conditions of temperature and light intensity. Heat stress was induced by increasing the chamber temperature; drought stress was induced by not irrigating the plants. A fraction of the air leaving the plant chamber was fed into a reaction chamber where SOA formation was induced by OH-initiated oxidation. During stress situations the plants' BVOC emissions changed significantly. As a general feature we found that combined heat and drought stress increased MT emissions from conifers but decreased MT emissions from the broadleaf species. The former was attributed to a heat-induced breakdown of storage organs. The latter was attributed to a general breakdown of biosynthetic activity. SOA formation potentials were changed together with the MT emissions. The decrease in SOA formation potential due to the decrease of MT emissions from broadleaf species was amplified by additional emissions of green leaf volatiles (GLV). Obviously, GLV can suppress SOA formation by suppressing OH concentrations. GLV were also emitted from the conifers under heat stress. However the

  7. An Overview of the DAURE Campaign: Aerosols Emissions and Evolution in the Western Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Pandolfi, Marco; Querol, Xavier; Alastuey, Andrés.; Jimenez, Jose L.

    2010-05-01

    DAURE (Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean) is a multidisciplinary international measurement campaign mainly aimed at estimating the sources and origin of atmospheric fine aerosols in the Western Mediterranean Basin (WMB), with particular attention to the carbonaceous fraction. Main focuses of the campaign are the study of the origin of the intense pollution episodes frequently occurring at regional scale in summer and winter in the WMB (Perez et al., 2008) and the emission, formation, transport and transformation of aerosols during these polluted scenarios. The peculiar atmospheric dynamics in the WMB, regulated by complex climatic and orographic effects (Millán et al., 1997), together with the large pollutant emissions from densely populated areas, large industrial areas and ports located along the coastline, give rise to a complex phenomenology for aerosol formation and transformation. In this context, extremely high concentrations of fine particulate matter (mainly PM1, particulate matter with aerodynamic diameter < 1um) are usually registered at regional background stations, with levels even higher than those simultaneously registered at urban stations. DAURE brings together state-of-the-art measurements and modeling techniques from about 20 International and Spanish Institutions. The DAURE campaign took place during winter (February-March 2009) and summer (July 2009) at an urban site (Barcelona, 80 m a.s.l., NE Spain) and a regional background site (Montseny, 720 m a.s.l., NE Spain, a Supersite of the EUSAAR network). Widespread in situ aerosol sampling techniques (such as PM optical counters, PM samplers, MAAP, CPC, SMPS, Rotating Drum Impactor, among others) and remote sensing techniques (LIDAR, sunphotometer) have been applied together with state-of-the-art methods such as 14C (Szidat et al., 2006), Proton-Transfer Reaction Mass Spectrometry (PTRMS) for VOCs, and High

  8. Top-down constraints to aerosol emissions from open biomass burning: the role of gas-particle partitioning and secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Konovalov, Igor B.; Beekmann, Matthias; Berezin, Evgeny V.; Petetin, Hervé

    2014-05-01

    Open biomass burning (BB), including wildfires and controlled burns in agriculture and foresty, is known to provide an important contribution to organic aerosol (OA) and black carbon (BC) emissions on the global scale. However, quantitative estimates of BB aerosol emissions and their effects on climate and environment remain rather uncertain. A useful way to constrain the OA&BC emissions involves using atmospheric measurements in the framework of the inverse modeling approach. In such an approach, the relationship between the emissions and the measurements is simulated by a chemistry transport model; this means that top-down estimates may be sensitive to possible model uncertainties. As a result of assimilation of satellite measurements of aerosol optical depth, several recent studies (e.g. [1,2]) indicated that aerosol emissions provided by bottom-up emission inventories may be strongly underestimated relative to emissions of gaseous species (such as CO). Meanwhile, it was earlier shown (e.g. [3]) that the relationship between primary organic aerosol emissions and aerosol concentration in the atmosphere can be significantly affected by gas-particle partitioning and oxidation of lower-volatility organic emissions; these processes are usually not taken into account in typical chemistry transport models. The main goal of this study was to examine to what degree the discrepancy between the OA&BC/CO emission ratios predicted by the bottom-up inventories and derived from satellite observations can be associated with the mentioned processes and explained in the framework of the volatility basis set approach (VBS) [3] to OA modelling. To achieve this goal, a VBS scheme, which was recently implemented in the CHIMERE chemistry transport model (CTM), was first modified to account for OA emissions from biomass burning. An ensemble of simulations with the CHIMERE CTM was then performed for the case of the 2010 mega-fire event in European Russia [4]; each of the simulations

  9. Summer 2009 wildfires in Portugal: Emission of trace gases and aerosol composition

    NASA Astrophysics Data System (ADS)

    Alves, Célia; Vicente, Ana; Nunes, Teresa; Gonçalves, Cátia; Fernandes, Ana Patrícia; Mirante, Fátima; Tarelho, Luís; Sánchez de la Campa, Ana M.; Querol, Xavier; Caseiro, Alexandre; Monteiro, Cristina; Evtyugina, Margarita; Pio, Casimiro

    2011-01-01

    In summer 2009, emissions of trace gases and aerosols from several wildfires occurring in Portugal were sampled. A portable high-volume sampler was used to collect sequentially, on quartz fibre filters, coarse (PM 2.5-10) and fine (PM 2.5) smoke particles. Tedlar air sampling bags have been used for complementary chemical characterisation of the gaseous phase. The carbonaceous content (elemental and organic carbon, EC/OC) of particulate matter was analysed by a thermal-optical transmission technique. The levels of almost 50 elements were quantified by inductively coupled plasma-mass spectrometry. The water-soluble ions were obtained by ion chromatography. Emission factors of species that are favoured by the smouldering phase (e.g. CO) were above the values reported in the literature for biomass burning in other ecosystems. The CO emission factors were 231 ± 117 g kg -1 biomass (dry basis) burned. Emissions of compounds that are promoted in fresh plumes and during the flaming phase, such as CO 2, were generally lower than those proposed for savannah and tropical forest fires. The CO 2 emission factors ranged from about 1000 to 1700 g kg -1. Total hydrocarbons, PM 2.5, PM 10 and OC presented variable emissions, but in general substantially higher than values reported for wildfires in African and Amazonian biomes. The emission factors obtained in Portugal were as follows (in g kg -1 biomass, dry basis): 6-350 for total hydrocarbons, 0.5-42 for PM 2.5, 1-60 for PM 10, and 0.2-42 for OC (in PM 10). The organic carbon-to-elemental carbon ratios measured in the present study largely exceeded those obtained by other researchers. The aerosol mass was dominated by organic matter (OC/PM 2.5 = 50 ± 18%, OC/PM 2.5-10 = 36 ± 18%). The metal elements represented, on average, 1.23 and 0.91%, while the measured water-soluble ions accounted for 2.6 and 2.1% of the PM 2.5 and PM 2.5-10 mass, respectively. Carbonates accounted for 0.15-3.1% (average = 0.83%) of PM 2.5-10. The

  10. Agricultural ammonia emissions and ammonium concentrations associated with aerosols and precipitation in the southeast United States

    NASA Astrophysics Data System (ADS)

    Aneja, Viney P.; Nelson, Dena R.; Roelle, Paul A.; Walker, John T.; Battye, William

    2003-02-01

    Temporal and spatial variations in ammonia (NH3) emissions and ammonium (NH4+) concentrations associated with aerosols and volume-weighted NH4+ concentration in precipitation are investigated over the period 1990-1998 in the southeast United States (Alabama, Florida, Georgia, Kentucky, North Carolina, South Carolina, Mississippi, and Tennessee). These variations were analyzed using an NH3 emissions inventory developed for the southeast United States and ambient NH4+ data from the various Clean Air Status and Trends Network (CASTNet) and the National Atmospheric Deposition Program/National Trends Network (NADP/NTN). Results show that natural log-transformed annual NH4+ concentration associated with aerosols increases with natural log-transformed annual NH3 emission density within the same county (R2 = 0.86, p < 0.0001, N = 12). Natural log-transformed annual volume-weighted average NH4+ concentration in precipitation shows only a very weak positive correlation with natural log-transformed annual NH3 emission densities within the corresponding county (R2 = 0.12, p = 0.04, N = 29). Analysis of NH4+ concentration associated with aerosols at CASTNet sites revealed that temperature, precipitation amount, and relative humidity are the most statistically significant (p < 0.05) parameters in predicting the weekly concentrations of NH4+ during the period 1990-1998. Wind speed and wind direction were also statistically significant (p < 0.05) at several CASTNet sites, but the results were less consistent. Investigation into wet NH4+ concentration in precipitation consistently yielded temperature as a statistically significant (p < 0.05) parameter at individual sites. Trends over the period 1990-1998 revealed a slight decrease in NH4+ concentration at CASTNet site SPD, Claiborne County, Tennessee (2.14-1.88 μg m-3), while positive trends in NH4+ concentration in precipitation were evident at NADP sites NC35, Sampson County, North Carolina (0.2-0.48 mg L-1) and KY35, Rowan

  11. Chemical characterization of emissions from vegetable oil processing and their contribution to aerosol mass using the organic molecular markers approach.

    PubMed

    Kavouras, I G; Stratigakis, N; Stephanou, E G

    2001-04-01

    The organic fraction of aerosol emitted from a vegetable oil processing plant was studied to investigate the contribution of emissions to ambient particles in the surrounding area. Solvent-soluble particulate organic compounds emitted from the plant accounted for 10% of total suspended particles. This percentage was lower in the receptor sites (less than 6% of total aerosol mass). Nonpolar, moderate polar, polar, and acidic compounds were detected in both emitted and ambient aerosol samples. The processing and combustion of olive pits yielded a source with strong biogenic characteristics, such as the high values of the carbon preference index (CPI) for all compound classes. Polycyclic aromatic hydrocarbons (PAHs) detected in emissions were associated with both olive pits and diesel combustion. The chromatographic profile of dimethylphenanthrenes (DMPs) was characteristic of olive pit combustion. Organic aerosols collected in two receptor sites provided a different pattern. The significant contribution of vehicular emissions was identified by CPI values (approximately 1) of n-alkanes and the presence of the unresolved complex mixture (UCM). In addition, PAH concentration diagnostic ratios indicated that emissions from catalyst and noncatalyst automobiles and heavy trucks were significant. The strong even-to-odd predominance of n-alkanols, n-alkanoic acids, and their salts indicated the contribution of a source with biogenic characteristics. However, the profile of DMPs at receptor sites was similar to that observed for diesel particulates. These differences indicated that the contribution of vegetable oil processing emissions to the atmosphere was negligible.

  12. Influence of Jet Fuel Composition on Aircraft Engine Emissions: A Synthesis of Aerosol Emissions Data from the NASA APEX, AAFEX, and ACCESS Missions

    NASA Astrophysics Data System (ADS)

    Moore, R.; Shook, M.; Beyersdorf, A. J.; Corr, C.; Herndon, S. C.; Knighton, W. B.; Miake-Lye, R. C.; Thornhill, K. L., II; Winstead, E.; Yu, Z.; Ziemba, L. D.; Anderson, B. E.

    2015-12-01

    We statistically analyze the impact of jet fuel properties on aerosols emitted by the NASA McDonnell Douglas DC-8 CFM56-2-C1 engines burning fifteen different aviation fuels. Data were collected for this single engine type during four different, comprehensive ground tests conducted over the past decade, which allow us to clearly link changes in aerosol emissions to fuel compositional changes. It is found that the volatile aerosol fraction dominates the number and volume emissions indices (EIs) over all engine powers, which are driven by changes in fuel aromatic and sulfur content. Meanwhile, the naphthalenic content of the fuel determines the magnitude of the non-volatile number and volume EI as well as the black carbon mass EI. Linear regression coefficients are reported for each aerosol EI in terms of these properties, engine fuel flow rate, and ambient temperature, and show that reducing both fuel sulfur content and napththalenes to near-zero levels would result in roughly a ten-fold decrease in aerosol number emitted per kg of fuel burn. This work informs future efforts to model aircraft emissions changes as the aviation fleet gradually begins to transition toward low-aromatic, low-sulfur alternative jet fuels from bio-based or Fischer-Tropsch production pathways.

  13. Infrared spectroscopy of methoxyphenols involved as atmospheric secondary organic aerosol precursors: Gas-phase vibrational cross-sections

    NASA Astrophysics Data System (ADS)

    Cuisset, A.; Coeur, C.; Mouret, G.; Ahmad, W.; Tomas, A.; Pirali, O.

    2016-08-01

    Methoxyphenols are emitted in the atmosphere from biomass burning and recent works have shown the potential role of these oxygenated aromatic species in the formation of secondary organic aerosols. IR spectroscopic data that would enable their remote measurement in the atmosphere remain scarce in the literature. Room temperature Far-IR cross-sections of 4 methoxyphenols (2-methoxyphenol or guaiacol, 3-methoxyphenol, 4-methoxyphenol and 2,6-dimethoxyphenol or syringol) have been determined using the THz synchrotron radiation available at SOLEIL. Mid- and near-IR regions have also been investigated with a conventional Fourier transform IR setup and allowed to provide a set of vibrational cross-sections of the studied methoxyphenols. Finally, gas-phase cross sections of two nitroguaiacol isomers (4-nitroguaiacol and 5-nitroguaiacol), two intermediate products involved in the formation of secondary organic aerosols have been measured in the mid- and near-IR with a heated multi-pass cell. Harmonic and anharmonic density functional theory calculations were carried out for all the studied compounds and allowed a full assignment of the recorded rovibrational bands.

  14. A Global view on the Emission of Swift Gamma-Ray Bursts: From Precursors to Extended Emission Tails and Late X-ray Flares

    NASA Astrophysics Data System (ADS)

    Liang, En-Wei; Zhang, Bing; Hu, You-Dong

    We present a joint analysis of the GRB data observed with the BAT and XRT on board Swift mission. Our results show that a precursor is observed in about 10 percents of the BAT GRBs, and most of them are of long-type GRBs. About half of the precursors triggers BAT to alert the GRBs. The triggered precursors are usually composed of some sharp pulses and non-triggered precursors are preferred to be some continuous flickers with almost a constant amplitude. There is no statistical difference of the photon indices between the triggered and non-triggered precursors, and their photon indices are also roughly consistent with that of the main bursts. The extended emision tails in the BAT band are usually observed in those GRBs that their main bursts are shorter than 2 seconds. These GRBs may be classified into the short-type GRBs. The EE tails are statistically softer than the emission in the main bursts and the corresponding X-ray flares are shown up in the XRT band. Taking the EE tails and late flares as evidence for late GRB central engine activity, we find that the lifetime of the GRB central engines of about 2/3 GRBs are much longer than T90. Our results indicate that the prompt gamma-ray phase may be only a short episode of the life times of the GRB central engines and what we have seen in the gamma-ray band may be only the tip of an iceberg of the GRB phenomenon. Future GRB alert instruments in the soft X-ray band may imporve our understanding on the activity of the GRB central engine in the early stage and the jet shock break-out as well as photosphere radaition.

  15. Reduced-form modeling of public health impacts of inorganic PM2.5 and precursor emissions

    NASA Astrophysics Data System (ADS)

    Heo, Jinhyok; Adams, Peter J.; Gao, H. Oliver

    2016-07-01

    It is challenging to estimate the public health costs of fine particulate matter (PM2.5) and its precursor emissions accurately and quickly for policy research because of their complex physical and chemical processes occurring over a large downwind area. We developed a method for building statistical regressions that estimate public health cost of emissions accurately like a state-of-the-art chemical transport model (CTM) but without its high computational cost. This method achieves detailed spatial resolution according to the location of the emission source, accounting for differences in the exposed population downwind. Using tagged CTM simulations, our method builds a large dataset of air quality public health costs from marginal emissions throughout the United States. Two methods were developed to describe exposed population, one that assumes a generic downwind plume concentration profile derived from CTM outputs and a simpler method that uses the size of population within certain distances as variables. Using the former method, we parameterized marginal public health cost [/t] and intake fraction [ppm] as a function of exposed population and key atmospheric variables. We derived models for elemental carbon, sulfur dioxide, nitrogen oxides, and ammonia. Compared to estimates calculated directly using CTM outputs, our models generally show mean fractional errors of only 10%-30% and up to 50% for NOx in some seasons, which are generally similar to or less than CTM's performance. Our results show that the public health costs of emissions can be efficiently parameterized for policy analyses based on state-of-the-art CTMs.

  16. Organic aerosol emission ratios from the laboratory combustion of biomass fuels

    NASA Astrophysics Data System (ADS)

    Jolleys, Matthew D.; Coe, Hugh; McFiggans, Gordon; McMeeking, Gavin R.; Lee, Taehyoung; Kreidenweis, Sonia M.; Collett, Jeffrey L.; Sullivan, Amy P.

    2014-11-01

    Organic aerosol (OA) emission ratios (ER) have been characterized for 67 burns during the second Fire Laboratory at Missoula Experiment. These fires involved 19 different species representing 6 major fuels, each of which forms an important contribution to the U.S. biomass burning inventory. Average normalized ΔOA/ΔCO ratios show a high degree of variability, both between and within different fuel types and species, typically exceeding differen-ces between separate plumes in ambient measurements. This variability is strongly influenced by highly contrasting ΔOA levels between burns and the increased partitioning of semivolatile organic compounds to the particle phase at high ΔOA concentrations. No correlation across all fires was observed between ΔOA/ΔCO and modified combustion efficiency (MCE), which acts as an indicator of the proportional contributions of flaming and smoldering combustion phases throughout each burn. However, a negative correlation exists with MCE for some coniferous species, most notably Douglas fir, for which there is also an influence from fuel moisture content. Changes in fire efficiency were also shown to dramatically alter emissions for fires with very similar initial conditions. Although the relationship with MCE is variable between species, there is greater consistency with the level of oxygenation in OA. The ratio of the m/z 44 fragment to total OA mass concentration (f44) as measured by aerosol mass spectrometer provides an indication of oxygenation as influenced by combustion processes at source, with ΔOA/ΔCO decreasing with increasing f44 for all fuel types. Inconsistencies in the magnitude of the effects associated with each potential influence on ΔOA/ΔCO emphasize the lack of a single dominant control on fire emissions, and a dependency on both fuel properties and combustion conditions.

  17. Aerosol-CFD modelling of ultrafine and black carbon particle emission, dilution, and growth near roadways

    NASA Astrophysics Data System (ADS)

    Huang, L.; Gong, S. L.; Gordon, M.; Liggio, J.; Staebler, R. M.; Stroud, C. A.; Lu, G.; Mihele, C.; Brook, J. R.; Jia, C. Q.

    2014-05-01

    Many studies have shown that on-road vehicle emissions are the dominant source of ultrafine particles (UFP; diameter < 100 nm) in urban areas and near-roadway environments. In order to advance our knowledge on the complex interactions and competition among atmospheric dilution, dispersion and dynamics of UFPs, an aerosol dynamics-CFD coupled model is developed and validated against field measurements. A unique approach of applying periodic boundary conditions is proposed to model pollutant dispersion and dynamics in one unified domain from the tailpipe level to the ambient near-road environment. This approach significantly reduces the size of the computational domain, and therefore, allows fast simulation of multiple scenarios. The model is validated against measured turbulent kinetic energy (TKE) and pollution gradients near a major highway. Through a model sensitivity analysis, the relative importance of individual aerosol dynamical processes on the total particle number concentration (N) and particle number-size distribution (PSD) near a highway is investigated. The results demonstrate that (1) coagulation has a negligible effect on N and particle growth, (2) binary homogeneous nucleation (BHN) of H2SO4-H2O is likely responsible for elevated N closest to the road, (3) N and particle growth are very sensitive to the condensation of semi-volatile organics (SVOCs), particle dry deposition, and the interaction between these processes. The results also indicate that, without the proper treatment of atmospheric boundary layer (i.e. its wind profile and turbulence quantities), the nucleation rate would be underestimated by a factor of 5 in the vehicle wake region due to overestimated mixing. Therefore, introducing ABL conditions to activity-based emission models may potentially improve their performance in estimating UFP traffic emissions.

  18. Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory

    NASA Astrophysics Data System (ADS)

    McMeeking, Gavin R.; Kreidenweis, Sonia M.; Baker, Stephen; Carrico, Christian M.; Chow, Judith C.; Collett, Jeffrey L.; Hao, Wei Min; Holden, Amanda S.; Kirchstetter, Thomas W.; Malm, William C.; Moosmüller, Hans; Sullivan, Amy P.; Wold, Cyle E.

    2009-10-01

    We characterized the gas- and speciated aerosol-phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory-based emission factors have not previously been reported for many commonly burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern United States (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire-integrated emission factors for gas-phase CO2, CO, CH4, C2-4 hydrocarbons, NH3, SO2, NO, NO2, HNO3, and particle-phase organic carbon (OC), elemental carbon (EC), SO42-, NO3-, Cl-, Na+, K+, and NH4+ generally varied with both fuel type and with the fire-integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming- and smoldering-phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed emission factors for total fine particulate matter. Our measurements spanned a larger range of MCE than prior studies, and thus help to improve estimates of the variation of emissions with combustion conditions for individual fuels.

  19. Global top-down smoke-aerosol emissions estimation using satellite fire radiative power measurements

    NASA Astrophysics Data System (ADS)

    Ichoku, C.; Ellison, L.

    2014-07-01

    Fire emissions estimates have long been based on bottom-up approaches that are not only complex, but also fraught with compounding uncertainties. We present the development of a global gridded (1° × 1°) emission coefficients (Ce) product for smoke total particulate matter (TPM) based on a top-down approach using coincident measurements of fire radiative power (FRP) and aerosol optical thickness (AOT) from the Moderate-resolution Imaging Spectro-radiometer (MODIS) sensors aboard the Terra and Aqua satellites. This new Fire Energetics and Emissions Research version 1.0 (FEER.v1) Ce product has now been released to the community and can be obtained from http://feer.gsfc.nasa.gov/, along with the corresponding 1-to-1 mapping of their quality assurance (QA) flags that will enable the Ce values to be filtered by quality for use in various applications. The regional averages of Ce values for different ecosystem types were found to be in the ranges of 16-21 g MJ-1 for savanna and grasslands, 15-32 g MJ-1 for tropical forest, 9-12 g MJ-1 for North American boreal forest, and 18-26 g MJ-1 for Russian boreal forest, croplands and natural vegetation. The FEER.v1 Ce product was multiplied by time-integrated FRP data to calculate regional smoke TPM emissions, which were compared with equivalent emissions products from three existing inventories. FEER.v1 showed higher and more reasonable smoke TPM estimates than two other emissions inventories that are based on bottom-up approaches and already reported in the literature to be too low, but portrayed an overall reasonable agreement with another top-down approach. This suggests that top-down approaches may hold better promise and need to be further developed to accelerate the reduction of uncertainty associated with fire emissions estimation in air-quality and climate research and applications. Results of the analysis of FEER.v1 data for 2004-2011 show that 65-85 Tg yr-1 of

  20. Global Top-Down Smoke-Aerosol Emissions Estimation Using Satellite Fire Radiative Power Measurements

    NASA Technical Reports Server (NTRS)

    Ichoku, C.; Ellison, L.

    2014-01-01

    Fire emissions estimates have long been based on bottom-up approaches that are not only complex, but also fraught with compounding uncertainties. We present the development of a global gridded (1 deg ×1 deg) emission coefficients (Ce) product for smoke total particulate matter (TPM) based on a top-down approach using coincident measurements of fire radiative power (FRP) and aerosol optical thickness (AOT) from the Moderate-resolution Imaging Spectroradiometer (MODIS) sensors aboard the Terra and Aqua satellites. This new Fire Energetics and Emissions Research version 1.0 (FEER.v1) Ce product has now been released to the community and can be obtained from http://feer.gsfc. nasa.gov/, along with the corresponding 1-to-1 mapping of their quality assurance (QA) flags that will enable the Ce values to be filtered by quality for use in various applications. The regional averages of Ce values for different ecosystem types were found to be in the ranges of 16-21/gMJ-1 for savanna and grasslands, 15-32/gMJ-1 for tropical forest, 9-12/gMJ-1 for North American boreal forest, and 18- 26/MJ-1 for Russian boreal forest, croplands and natural vegetation. The FEER.v1 Ce product was multiplied by time-integrated FRP data to calculate regional smoke TPM emissions, which were compared with equivalent emissions products from three existing inventories. FEER.v1 showed higher and more reasonable smoke TPM estimates than two other emissions inventories that are based on bottom-up approaches and already reported in the literature to be too low, but portrayed an overall reasonable agreement with another top-down approach. This suggests that top-down approaches may hold better promise and need to be further developed to accelerate the reduction of uncertainty associated with fire emissions estimation in air-quality and climate research and applications. Results of the analysis of FEER.v1 data for 2004-2011 show that 65-85 Tg yr-1 of TPM is emitted globally from open biomass burning, with a

  1. Projections of mid-century summer air-quality for North America: effects of changes in climate and precursor emissions

    NASA Astrophysics Data System (ADS)

    Kelly, J.; Makar, P. A.; Plummer, D. A.

    2012-06-01

    Ten year simulations of North American current and future air-quality were carried out using a regional air-quality model driven by a regional climate model, in turn driven by a general circulation model. Three separate summer scenarios were performed: a scenario representing the years 1997 to 2006, and two SRES A2 climate scenarios for the years 2041 to 2050. The first future climate scenario makes use of 2002 anthropogenic precursor emissions, and the second applied emissions scaling factors derived from the IPCC Representative Concentration Pathway 6 (RCP 6) scenario to estimate emissions for 2050 from existing 2020 projections. Ten-year averages of ozone and PM2.5 at North American monitoring network stations were used to evaluate the model's current chemical climatology. The model was found to have a similar performance for ozone as when driven by an operational weather forecast model. The PM2.5 predictions had larger negative biases, likely resulting from the absence of rainwater evaporation, and from sub-regional negative biases in the surface temperature fields, in the version of the climate model used here. The differences between the two future climate simulations and the current climate simulation were used to predict the changes to air-quality that might be expected in a future warmer climate, if anthropogenic precursor emissions remain constant at their current levels, versus if the RCP 6 emissions controls were adopted. Metrics of concentration, human health, and ecosystem damage were compared for the simulations. The scenario with future climate and current anthropogenic emissions resulted in worse air-quality than for current conditions - that is, the effect of climate-change alone, all other factors being similar, would be a worsening of air-quality. These effects are spatially inhomogeneous, with the magnitude and sign of the changes varying with region. The scenario with future climate and RCP 6 emissions for 2050 resulted in an improved air

  2. Projections of mid-century summer air-quality for North America: effects of changes in climate and precursor emissions

    NASA Astrophysics Data System (ADS)

    Kelly, J.; Makar, P. A.; Plummer, D. A.

    2012-02-01

    Ten year simulations of North American current and future air-quality were carried out using a regional air-quality model driven by a regional climate model, in turn driven by a general circulation model. Three separate summer scenarios were performed: a scenario representing the years 1997 to 2006, and two SRES A2 climate scenarios for the years 2041 to 2050. The first future climate scenario makes use of 2002 anthropogenic precursor emissions, and the second applied emissions scaling factors derived from the IPCC Representative Concentration Pathway 6 (RCP 6) scenario to estimate emissions for 2050 from existing 2020 projections. Ten-year averages of ozone and PM2.5 at North American monitoring network stations were used to evaluate the model's current chemical climatology. The model was found to have a similar performance for ozone as when driven by an operational weather forecast model. The PM2.5 predictions had larger negative biases, likely resulting from the absence of rainwater evaporation, and from sub-regional negative biases in the surface temperature fields, in the version of the climate model used here. The differences between the two future climate simulations and the current climate simulation were used to predict the changes to air-quality that might be expected in a future warmer climate, if anthropogenic precursor emissions remain constant at their current levels, versus if the RCP 6 emissions controls were adopted. Metrics of concentration, human health, and ecosystem damage were compared for the simulations. The scenario with future climate and current anthropogenic emissions resulted in worse air-quality than for current conditions - that is, the effect of climate-change alone, all other factors being similar, would be a worsening of air-quality. These effects are spatially inhomogeneous, with the magnitude and sign of the changes varying with region. The scenario with future climate and RCP 6 emissions for 2050 resulted in an improved air

  3. Estimates of non-traditional secondary organic aerosols from aircraft SVOC and IVOC emissions using CMAQ

    NASA Astrophysics Data System (ADS)

    Woody, M. C.; West, J. J.; Jathar, S. H.; Robinson, A. L.; Arunachalam, S.

    2014-12-01

    Utilizing an aircraft-specific parameterization based on smog chamber data in the Community Multiscale Air Quality (CMAQ) model with the Volatility Basis Set (VBS), we estimated contributions of non-traditional secondary organic aerosols (NTSOA) for aircraft emissions during landing and takeoff (LTO) activities at the Hartsfield-Jackson Atlanta International Airport. NTSOA, formed from the oxidation of semi-volatile and intermediate volatility organic compounds (S/IVOCs), is a heretofore unaccounted component of fine particulate matter (PM2.5) in most air quality models. We expanded a prerelease version of CMAQ with VBS implemented for the Carbon Bond 2005 (CB05) chemical mechanism to use the Statewide Air Pollution Research Center 2007 (SAPRC-07) chemical mechanism, and added species representing aircraft S/IVOCs and corresponding NTSOA oxidation products. Results indicated the maximum monthly average NTSOA contributions occurred at the airport, and ranged from 2.4 ng m-3 (34% from idle and 66% from non-idle aircraft activities) in January to 9.1 ng m-3 (33 and 67%) in July. This represents 1.7% (of 140 ng m-3) in January and 7.4% in July (of 122 ng m-3) of aircraft-attributable PM2.5, compared to 41.0-42.0% from elemental carbon and 42.8-58.0% from inorganic aerosols. As a percentage of PM2.5, impacts were higher downwind of the airport, where NTSOA averaged 4.6-17.9% of aircraft-attributable PM2.5 and, considering alternative aging schemes, was high as 24.0% - thus indicating the increased contribution of aircraft-attributable SOA, as a component of PM2.5. However, NTSOA contributions were generally low compared to smog chamber results, particularly at idle, due to the considerably lower ambient organic aerosol concentrations in CMAQ, vs. those in the smog chamber experiments.

  4. Estimates of non-traditional secondary organic aerosols from aircraft SVOC and IVOC emissions using CMAQ

    NASA Astrophysics Data System (ADS)

    Woody, M. C.; West, J. J.; Jathar, S. H.; Robinson, A. L.; Arunachalam, S.

    2015-06-01

    Utilizing an aircraft-specific parameterization based on smog chamber data in the Community Multiscale Air Quality (CMAQ) model with the volatility basis set (VBS), we estimated contributions of non-traditional secondary organic aerosols (NTSOA) for aircraft emissions during landing and takeoff (LTO) activities at the Hartsfield-Jackson Atlanta International Airport. NTSOA, formed from the oxidation of semi-volatile and intermediate volatility organic compounds (S/IVOCs), is a heretofore unaccounted component of fine particulate matter (PM2.5) in most air quality models. We expanded a prerelease version of CMAQ with VBS implemented for the Carbon Bond 2005 (CB05) chemical mechanism to use the Statewide Air Pollution Research Center 2007 (SAPRC-07) chemical mechanism and added species representing aircraft S/IVOCs and corresponding NTSOA oxidation products. Results indicated that the maximum monthly average NTSOA contributions occurred at the airport and ranged from 2.4 ng m-3 (34 % from idle and 66 % from non-idle aircraft activities) in January to 9.1 ng m-3 (33 and 67 %) in July. This represents 1.7 % (of 140 ng m-3) in January and 7.4 % in July (of 122 ng m-3) of aircraft-attributable PM2.5 compared to 41.0-42.0 % from elemental carbon and 42.8-58.0 % from inorganic aerosols. As a percentage of PM2.5, impacts were higher downwind of the airport, where NTSOA averaged 4.6-17.9 % of aircraft-attributable PM2.5 and, considering alternative aging schemes, was as high as 24.0 % - thus indicating the increased contribution of aircraft-attributable SOA as a component of PM2.5. However, NTSOA contributions were generally low compared to smog chamber results, particularly at idle, due to the considerably lower ambient organic aerosol concentrations in CMAQ compared to those in the smog chamber experiments.

  5. Characterization of Primary Organic Aerosol Emissions from Meat Cooking, Trash Burning, and Combustion Engines with High-Resolution Aerosol Mass Spectrometry and Comparison with Ambient and Chamber Observations

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Huffman, J. A.; Cubison, M. J.; Aiken, A. C.; Docherty, K. S.; Kimmel, J. R.; Ulbrich, I. M.; Hannigan, M.; Garcia, J.; Jimenez, J. L.

    2009-04-01

    Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS) and supporting instrumentation. A semi-quantitative comparison of emission factors highlights the potential importance of meat cooking as an OA source. GC-MS and AMS mass spectra are compared for the first time and show high similarity, but with more fragmentation in the AMS due to higher vaporization temperatures. High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to mass spectral signatures from hydrocarbon-like OA or primary OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from any of these sources is very unlikely to be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/z's that may be useful for differentiating these sources from each other. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, while motor vehicle emissions have very low signal at this m/z.

  6. The FLAME Deluge: organic aerosol emission ratios from combustion chamber experiments

    NASA Astrophysics Data System (ADS)

    Jolleys, Matthew; Coe, Hugh; McFiggans, Gordon; McMeeking, Gavin; Lee, Taehyoung; Sullivan, Amy; Kreidenweis, Sonia; Collett, Jeff

    2014-05-01

    A high level of variability has been identified amongst organic aerosol (OA) emission ratios (ER) from biomass burning (BB) under ambient conditions. However, it is difficult to assess the influences of potential drivers for this variability, given the wide range of conditions associated with wildfire measurements. Chamber experiments performed under controlled conditions provide a means of examining the effects of different fuel types and combustion conditions on OA emissions from biomass fuels. ERs have been characterised for 67 burns during the second Fire Laboratory at Missoula Experiment (FLAME II), involving 19 different species from 6 fuel types widely consumed in BB events in the US each year. Average normalised dOA/dCO ratios show a high degree of variability, both between and within different fuel types and species, typically exceeding variability between separate plumes in ambient measurements. Relationships with source conditions were found to be complex, with little consistent influence from fuel properties and combustion conditions for the entire range of experiments. No strong correlation across all fires was observed between dOA/dCO and modified combustion efficiency (MCE), which is used as an indicator of the proportional contributions of flaming and smouldering combustion phases throughout each burn. However, a negative correlation exists between dOA/dCO and MCE for some coniferous species, most notably Douglas fir, for which there is also an apparent influence from fuel moisture content. Significant contrasts were also identified between combustion emissions from different fuel components of additional coniferous species. Changes in fire efficiency were also shown to dramatically alter emissions for fires with very similar initial conditions. Although the relationship with MCE is variable between species, there is greater consistency with the level of oxygenation in OA. The ratio of the m/z 44 fragment to total OA mass concentration (f44) as

  7. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

    EPA Science Inventory

    Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are...

  8. Thermal Emission Spectrometer Results: Mars Atmospheric Thermal Structure and Aerosol Distribution

    NASA Technical Reports Server (NTRS)

    Smith, Michael D.; Pearl, John C.; Conrath, Barney J.; Christensen, Philip R.; Vondrak, Richard R. (Technical Monitor)

    2001-01-01

    Infrared spectra returned by the Thermal Emission Spectrometer (TES) are well suited for retrieval of the thermal structure and the distribution of aerosols in the Martian atmosphere. Combined nadir- and limb-viewing spectra allow global monitoring of the atmosphere up to 0.01 mbar (65 km). We report here on the atmospheric thermal structure and the distribution of aerosols as observed thus far during the mapping phase of the Mars Global Surveyor mission. Zonal and temporal mean cross sections are used to examine the seasonal evolution of atmospheric temperatures and zonal winds during a period extending from northern hemisphere mid-summer through vernal equinox (L(sub s) = 104-360 deg). Temperature maps at selected pressure levels provide a characterization of planetary-scale waves. Retrieved atmospheric infrared dust opacity maps show the formation and evolution of regional dust storms during southern hemisphere summer. Response of the atmospheric thermal structure to the changing dust loading is observed. Maps of water-ice clouds as viewed in the thermal infrared are presented along with seasonal trends of infrared water-ice opacity. Uses of these observations for diagnostic studies of the dynamics of the atmosphere are discussed.

  9. Development of a United States - Mexico emissions inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study

    SciTech Connect

    Hampden Kuhns; Eladio M. Knipping; Jeffrey M. Vukovich,

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study investigated the sources of haze at Big Bend National Park in southwest Texas. The modeling domain includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) {lt}10 {mu}m in aerodynamic diameter, and PM {lt}2.5 {mu}m in aerodynamic diameter. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions inventory for Mexico with other emerging Mexican emission inventories illustrates their uncertainty. 65 refs., 4 figs., 9 tabs.

  10. The toxicological evaluation of realistic emissions of source aerosols study: statistical methods.

    PubMed

    Coull, Brent A; Wellenius, Gregory A; Gonzalez-Flecha, Beatriz; Diaz, Edgar; Koutrakis, Petros; Godleski, John J

    2011-08-01

    The Toxicological Evaluation of Realistic Emissions of Source Aerosols (TERESA) study involved withdrawal, aging, and atmospheric transformation of emissions of three coal-fired power plants. Toxicological evaluations were carried out in rats exposed to different emission scenarios with extensive exposure characterization. Data generated had multiple levels of resolution: exposure, scenario, and constituent chemical composition. Here, we outline a multilayered approach to analyze the associations between exposure and health effects beginning with standard ANOVA models that treat exposure as a categorical variable. The model assessed differences in exposure effects across scenarios (by plant). To assess unadjusted associations between pollutant concentrations and health, univariate analyses were conducted using the difference between the response means under exposed and control conditions and a single constituent concentration as the predictor. Then, a novel multivariate analysis of exposure composition and health was used based on Random Forests(™), a recent extension of classification and regression trees that were applied to the outcome differences. For each exposure constituent, this approach yielded a nonparametric measure of the importance of that constituent in predicting differences in response on a given day, controlling for the other measured constituent concentrations in the model. Finally, an R(2) analysis compared the relative importance of exposure scenario, plant, and constituent concentrations on each outcome. Peak expiratory flow (PEF) is used to demonstrate how the multiple levels of the analysis complement each other to assess constituents most strongly associated with health effects.

  11. Gas-particle partitioning of primary organic aerosol emissions: (2) diesel vehicles.

    PubMed

    May, Andrew A; Presto, Albert A; Hennigan, Christopher J; Nguyen, Ngoc T; Gordon, Timothy D; Robinson, Allen L

    2013-08-01

    Experiments were performed to investigate the gas-particle partitioning of primary organic aerosol (POA) emissions from two medium-duty (MDDV) and three heavy-duty (HDDV) diesel vehicles. Each test was conducted on a chassis dynamometer with the entire exhaust sampled into a constant volume sampler (CVS). The vehicles were operated over a range of driving cycles (transient, high-speed, creep/idle) on different ultralow sulfur diesel fuels with varying aromatic content. Four independent yet complementary approaches were used to investigate POA gas-particle partitioning: artifact correction of quartz filter samples, dilution from the CVS into a portable environmental chamber, heating in a thermodenuder, and thermal desorption/gas chromatography/mass spectrometry (TD-GC-MS) analysis of quartz filter samples. During tests of vehicles not equipped with diesel particulate filters (DPF), POA concentrations inside the CVS were a factor of 10 greater than ambient levels, which created large and systematic partitioning biases in the emissions data. For low-emitting DPF-equipped vehicles, as much as 90% of the POA collected on a quartz filter from the CVS were adsorbed vapors. Although the POA emission factors varied by more than an order of magnitude across the set of test vehicles, the measured gas-particle partitioning of all emissions can be predicted using a single volatility distribution derived from TD-GC-MS analysis of quartz filters. This distribution is designed to be applied directly to quartz filter data that are the basis for existing emissions inventories and chemical transport models that have implemented the volatility basis set approach.

  12. Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory

    SciTech Connect

    McMeeking, Gavin R.; Kreidenweis, Sonia M.; Baker, Stephen; Carrico, Christian M.; Chow, Judith C.; Collett, Jr., Jeffrey L.; Hao, Wei Min; Holden, Amanda S.; Kirchstetter, Thomas W.; Malm, William C.; Moosmuller, Hans; Sullivan, Amy P.; Wold, Cyle E.

    2009-05-15

    We characterized the gas- and speciated aerosol-phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory-based emission factors have not previously been reported for many commonly-burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern US (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire-integrated emission factors for gas-phase CO{sub 2}, CO, CH{sub 4}, C{sub 2-4} hydrocarbons, NH{sub 3}, SO{sub 2}, NO, NO{sub 2}, HNO{sub 3} and particle-phase organic carbon (OC), elemental carbon (EC), SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, Cl{sup -}, Na{sup +}, K{sup +}, and NH{sub 4}{sup +} generally varied with both fuel type and with the fire-integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming- and smoldering-phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed EF for total fine particulate matter. Our measurements often spanned a larger range of MCE than prior studies, and thus help to improve estimates for individual fuels of the variation of emissions with combustion conditions.

  13. Examining the Effects of Anthropogenic Emissions on Isoprene-Derived Secondary Organic Aerosol Formation During the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee, Ground Site

    EPA Science Inventory

    A suite of offline and real-time gas- and particle-phase measurements was deployed atLook Rock, Tennessee (TN), during the 2013 Southern Oxidant and Aerosol Study (SOAS) to examine the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol (SOA) formatio...

  14. EVALUATION OF AEROSOL EMISSIONS DOWNSTREAM OF AN AMMONIA-BASED SO2 SCRUBBER

    SciTech Connect

    Dennis L. Laudal

    2002-04-01

    Depending on the size and type of boiler, the 1990 Clean Air Act Amendments required specific reductions in SO{sub 2} emissions from coal-fired electric utilities. To meet these requirements, SO{sub 2} reduction strategies have included installing scrubbing technology, switching to a more expensive low-sulfur coal, or purchasing SO{sub 2} allowances. It is expected that over the next 10 years there will be an increase in the price of low-sulfur coals, but that higher-sulfur coal costs will remain the same. Technologies must be strongly considered that allow the use of high-sulfur fuels while at the same time meeting current and future SO{sub 2} emission limits. One such technology is the ammonia based flue gas desulfurization (FGD) (NH{sub 3}-based FGD) system manufactured by Marsulex Environmental Technologies (MET). The MET scrubber is a patented NH{sub 3}-based FGD process that efficiently converts SO{sub 2} (>95%) into a fertilizer product, ammonium sulfate ([NH{sub 4}]{sub 2}SO{sub 4}). A point of concern for the MET technology, as well as other FGD systems, is the emission of sulfuric acid/SO{sub 3} aerosols that could result in increased opacity at the stack. This is a direct result of firing high-sulfur fuels that naturally generate more SO{sub 3} than do low-sulfur coals. SO{sub 3} is formed during the coal combustion process. SO{sub 3} is converted to gaseous H{sub 2}SO{sub 4} by homogeneous condensation, leading to a submicron acid fume that is very difficult to capture in a dry electrostatic precipitator (ESP). The condensed acid can also combine with the fly ash in the duct and scale the duct wall, potentially resulting in corrosion of both metallic and nonmetallic surfaces. Therefore, SO{sub 3} in flue gas can have a significant impact on the performance of coal-fired utility boilers, air heaters, and ESPs. In addition to corrosion problems, excess SO{sub 3} emissions can result in plume opacity problems. Thus the Energy & Environmental Research

  15. Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA)-power plant studies: assessment of cellular responses

    PubMed Central

    Godleski, John J.; Diaz, Edgar A.; Lemos, Miriam; Long, Mark; Ruiz, Pablo; Gupta, Tarun; Kang, Choong-Min; Coull, Brent

    2013-01-01

    The Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA) project assessed primary and secondary particulate by simulating the chemical reactions that a plume from a source might undergo during atmospheric transport and added other atmospheric constituents that might interact with it. Three coal-fired power plants with different coal and different emission controls were used. Male Sprague-Dawley rats were exposed for 6 h to either filtered air or aged aerosol from the power plant. Four exposure scenarios were studied: primary particles (P); primary + secondary (oxidized) particles (PO); primary + secondary (oxidized) particles + SOA (POS); and primary + secondary (oxidized) particles neutralized + SOA (PONS). Exposure concentrations varied by scenario to a maximum concentration of 257.1 ± 10.0 µg/m3. Twenty-four hours after exposure, pulmonary cellular responses were assessed by bronchoalveolar lavage (BAL), complete blood count (CBC), and histopathology. Exposure to the PONS and POS scenarios produced significant increases in BAL total cells and macrophage numbers at two plants. The PONS and P scenarios were associated with significant increases in BAL neutrophils and the presence of occasional neutrophils and increased macrophages in the airways and alveoli of exposed animals. Univariate analyses and random forest analyses showed that increases in total cell count and macrophage cell count were significantly associated with neutralized sulfate and several correlated measurements. Increases in neutrophils in BAL were associated with zinc. There were no significant differences in CBC parameters or blood vessel wall thickness by histopathology. The association between neutrophils increases and zinc raises the possibility that metals play a role in this response. PMID:21466245

  16. VLF/LF EM emissions as main precursor of earthquakes and their searching possibilities for Georgian s/a region

    NASA Astrophysics Data System (ADS)

    Kachakhidze, Manana; Kachakhidze, Nino

    2016-04-01

    Authors of abstract have created work which offers model of earth electromagnetic emissions generation detected in the process of earthquake preparation on the basis of electrodynamics. The model gives qualitative explanation of a mechanism of generation of electromagnetic waves emitted in the earthquake preparation period. Besides, scheme of the methodology of earthquake forecasting is created based on avalanche-like unstable model of fault formation and an analogous model of electromagnetic contour, synthesis of which, is rather harmonious. According to the authors of the work electromagnetic emissions in radiodiapason is more universal and reliable than other anomalous variations of various geophysical phenomena in earthquake preparation period; Besides, VLF/LF electromagnetic emissions might be declared as the main precursor of earthquake because it might turn out very useful with the view of prediction of large (M ≥5) inland earthquakes and to govern processes going on in lithosphere-atmosphere - ionosphere coupling (LAIC) system. Since the other geophysical phenomena, which may accompany earthquake preparation process and expose themselves several months, weeks or days prior to earthquakes are less informative with the view of earthquake forecasting, it is admissible to consider them as earthquake indicators. Physical mechanisms of mentioned phenomena are explained on the basis of the model of generation of electromagnetic emissions detected before earthquake, where a process of earthquake preparation and its realization are considered taking into account distributed and conservative systems properties. Up to these days electromagnetic emissions detection network did not exist in Georgia. European colleagues helped us (Prof. Dr. PF Biagi, Prof. Dr. Aydın BÜYÜKSARAÇ) and made possible the installation of a receiver. We are going to develop network and put our share in searching of earthquakes problem. Participation in conference is supported by financial

  17. Controlling pyridinic, pyrrolic, graphitic, and molecular nitrogen in multi-wall carbon nanotubes using precursors with different N/C ratios in aerosol assisted chemical vapor deposition.

    PubMed

    Bulusheva, L G; Okotrub, A V; Fedoseeva, Yu V; Kurenya, A G; Asanov, I P; Vilkov, O Y; Koós, A A; Grobert, N

    2015-10-01

    Nitrogen-containing multi-wall carbon nanotubes (N-MWCNTs) were synthesized using aerosol assisted chemical vapor deposition (CVD) techniques in conjunction with benzylamine:ferrocene or acetonitrile:ferrocene mixtures. Different amounts of toluene were added to these mixtures in order to change the N/C ratio of the feedstock. X-ray photoelectron and near-edge X-ray absorption fine structure spectroscopy detected pyridinic, pyrrolic, graphitic, and molecular nitrogen forms in the N-MWCNT samples. Analysis of the spectral data indicated that whilst the nature of the nitrogen-containing precursor has little effect on the concentrations of the different forms of nitrogen in N-MWCNTs, the N/C ratio in the feedstock appeared to be the determining factor. When the N/C ratio was lower than ca. 0.01, all four forms existed in equal concentrations, for N/C ratios above 0.01, graphitic and molecular nitrogen were dominant. Furthermore, higher concentrations of pyridinic nitrogen in the outer shells and N2 molecules in the core of the as-produced N-MWCNTs suggest that the precursors were decomposed into individual atoms, which interacted with the catalyst surface to form CN and NH species or in fact diffused through the bulk of the catalyst particles. These findings are important for a better understanding of possible growth mechanisms for heteroatom-containing carbon nanotubes (CNTs) and therefore paving the way for controlling the spatial distribution of foreign elements in the CNTs using CVD processes. PMID:26104737

  18. The Trimethylamine-Formic Acid Complex: Microwave Characterization of a Prototype for Potential Precursors to Atmospheric Aerosol.

    PubMed

    Mackenzie, Rebecca B; Dewberry, Christopher T; Leopold, Kenneth R

    2016-04-14

    The reactions of amines and carboxylic acids have recently received attention for their possible role in the formation of atmospheric aerosol. Here, we report a microwave study of the trimethylamine-formic acid hydrogen-bonded complex, a simple prototype in which to study amine-carboxylic acid interactions. Spectra of three isotopologues of the system have been observed using a tandem cavity and chirped-pulse Fourier transform microwave spectrometer. The complex has a plane of symmetry, with the acidic proton of the formic acid directed toward the lone pair of the nitrogen. The zero-point-averaged hydrogen bond length is 1.702 Å, and the O-H···N angle is 177°. (14)N nuclear quadrupole hyperfine structure has been used to assess the degree of proton transfer from the formic acid to the trimethylamine. Experimental results are supplemented with density functional theory calculations. M06-2X/6-311++G(3df,3pd) calculations indicate a binding energy of 16.8 kcal/mol with counterpoise correction (17.4 kcal/mol without counterpoise correction).

  19. Development of aroCACM/MPMPO 1.0: a model to simulate secondary organic aerosol from aromatic precursors in regional models

    NASA Astrophysics Data System (ADS)

    Dawson, Matthew L.; Xu, Jialu; Griffin, Robert J.; Dabdub, Donald

    2016-06-01

    The atmospheric oxidation of aromatic compounds is an important source of secondary organic aerosol (SOA) in urban areas. The oxidation of aromatics depends strongly on the levels of nitrogen oxides (NOx). However, details of the mechanisms by which oxidation occurs have only recently been elucidated. Xu et al. (2015) developed an updated version of the gas-phase Caltech Atmospheric Chemistry Mechanism (CACM) designed to simulate toluene and m-xylene oxidation in chamber experiments over a range of NOx conditions. The output from such a mechanism can be used in thermodynamic predictions of gas-particle partitioning leading to SOA. The current work reports the development of a model for SOA formation that combines the gas-phase mechanism of Xu et al. (2015) with an updated lumped SOA-partitioning scheme (Model to Predict the Multi-phase Partitioning of Organics, MPMPO) that allows partitioning to multiple aerosol phases and that is designed for use in larger-scale three-dimensional models. The resulting model is termed aroCACM/MPMPO 1.0. The model is integrated into the University of California, Irvine - California Institute of Technology (UCI-CIT) Airshed Model, which simulates the South Coast Air Basin (SoCAB) of California. Simulations using 2012 emissions indicate that "low-NOx" pathways to SOA formation from aromatic oxidation play an important role, even in regions that typically exhibit high-NOx concentrations.

  20. Effect of measurement protocol on organic aerosol measurements of exhaust emissions from gasoline and diesel vehicles

    NASA Astrophysics Data System (ADS)

    Kim, Youngseob; Sartelet, Karine; Seigneur, Christian; Charron, Aurélie; Besombes, Jean-Luc; Jaffrezo, Jean-Luc; Marchand, Nicolas; Polo, Lucie

    2016-09-01

    Exhaust emissions of semi-volatile organic compounds (SVOC) from passenger vehicles are usually estimated only for the particle phase via the total particulate matter measurements. However, they also need to be estimated for the gas phase, as they are semi-volatile. To better estimate SVOC emission factors of passenger vehicles, a measurement campaign using a chassis dynamometer was conducted with different instruments: (1) a constant volume sampling (CVS) system in which emissions were diluted with filtered air and sampling was performed on filters and polyurethane foams (PUF) and (2) a Dekati Fine Particle Sampler (FPS) in which emissions were diluted with purified air and sampled with on-line instruments (PTR-ToF-MS, HR-ToF-AMS, MAAP, CPC). Significant differences in the concentrations of organic carbon (OC) measured by the instruments are observed. The differences can be explained by sampling artefacts, differences between (1) the time elapsed during sampling (in the case of filter and PUF sampling) and (2) the time elapsed from emission to measurement (in the case of on-line instruments), which vary from a few seconds to 15 min, and by the different dilution factors. To relate elapsed times and measured concentrations of OC, the condensation of SVOC between the gas and particle phases is simulated with a dynamic aerosol model. The simulation results allow us to understand the relation between elapsed times and concentrations in the gas and particle phases. They indicate that the characteristic times to reach thermodynamic equilibrium between gas and particle phases may be as long as 8 min. Therefore, if the elapsed time is less than this characteristic time to reach equilibrium, gas-phase SVOC are not at equilibrium with the particle phase and a larger fraction of emitted SVOC will be in the gas phase than estimated by equilibrium theory, leading to an underestimation of emitted OC if only the particle phase is considered or if the gas-phase SVOC are estimated

  1. Highly efficient photocatalytic TiO2 coatings deposited by open air atmospheric pressure plasma jet with aerosolized TTIP precursor

    NASA Astrophysics Data System (ADS)

    Fakhouri, H.; Ben Salem, D.; Carton, O.; Pulpytel, J.; Arefi-Khonsari, F.

    2014-07-01

    A simple method to deposit photocatalytic TiO2 coatings, at a high rate (20-40 µm s-1), and with a high porosity, is reported in this paper. This method, which allows the treatment of membranes (with an 800 nm pore size), is based on the introduction of a liquid precursor sprayed into an open-air atmospheric pressure plasma jet (APPJ). The photocatalytic activity of the TiO2 thin films prepared by APPJ have been compared with our best N-doped TiO2 thin films, deposited by reactive radio frequency (RF) magnetron sputtering, previously reported in the literature. The morphology, chemical composition, photoelectrochemical, and photocatalytic properties of the coatings have been studied in this paper. Significant control of the porosity and crystallinity was achieved by varying the deposition parameters and the annealing temperature. Under optimized conditions, the TiO2 coatings deposited by APPJ are characterized by a higher photocatalytic activity as compared to the optimized thin films deposited by RF sputtering. This difference can be explained by the higher specific surface of the APPJ coatings. Finally, the most interesting characteristic of this APPJ-liquid spray process is its capacity to treat membranes without blocking the pores, and to produce photocatalytic membranes which can efficiently combine filtration and photocatalysis for water treatment.

  2. Characterizing particulate matter emissions from vehicles: chassis-dynamometer tests using a High-Resolution Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Collier, S.; Zhang, Q.; Forestieri, S.; Kleeman, M.; Cappa, C. D.; Kuwayama, T.

    2012-12-01

    During September of 2011 a suite of real-time instruments was used to sample vehicle emissions at the California Air Resources Board Haagen-Schmidt facility in El Monte, CA. A representative fleet of 8 spark ignition gasoline vehicles, a diesel passenger vehicle, a gasoline direct-injection vehicle and an ultra-low emissions vehicle were tested on a chassis dynamometer. The emissions were sampled into the facility's standard CVS tunnel and diluted to atmospherically relevant levels (5-30 μg/m3) while controlling other factors such as relative humidity or background black carbon particulate loading concentrations. An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-MS) was among the real-time instruments used and sampled vehicle emissions at 10 second time resolution in order to characterize the non-refractory organic and inorganic particulate matter (PM). PM composition and concentration were tracked throughout the cold start driving cycle which included periods of fast acceleration and high velocity cruise control, meant to recreate typical commuter driving behavior. Variations in inorganic and organic PM composition for a given vehicle throughout the driving cycle as well as for various vehicles with differing emissions loading were characterized. Differences in PM composition for a given vehicle whose emissions are being exposed to differing experimental conditions such as varying relative humidity will also be reported. In conjunction with measurements from a Multi Wavelength Photoacoustic Black Carbon Spectrometer (MWPA-BC) and real-time gas measurements from the CARB facility, we determine the real-time emission ratios of primary organic aerosols (POA) with respect to BC and common combustion gas phase pollutants and compared to different vehicle driving conditions. The results of these tests offer the vehicle emissions community a first time glimpse at the real-time behavior of vehicle PM emissions for a variety of conditions and

  3. UNITED STATES LAND USE INVENTORY FOR ESTIMATING BIOGENIC OZONE PRECURSOR EMISSIONS

    EPA Science Inventory

    The U.S. Geological Survey's (USGS) Earth Resources Observation System (EROS) Data Center's (EDC) 1-km classified land cover data are combined with other land use data using a Geographic Information System (GIS) to create the Biogenic Emissions Landcover Database (BELD). The land...

  4. Tracing impacts of local and regional emission sources on the aerosols over Central Himalayan region during GVAX

    NASA Astrophysics Data System (ADS)

    Sahai, Shivraj; Sagar, Ram; Pant, P.; Krishna Moorthy, K.; Venkata Phanikumar, Devulapalli; Dumka, Umesh Chandra; Pant, Vimlesh; Singh, Narendra; Kotamarthi, V. R.; Naja, Manish; Satheesh, S. K.

    2012-07-01

    -range transport impact, available satellite products over the Indo-Gangetic Plain (IGP) of relevance to biomass burning (Carbon monoxide, Aerosol Optical Depth, Fire products, etc) have been exploited to relate to the observed aerosol physical properties during GVAX. The findings are expected to reveal the linkages between local and regional emission sources (biomass burning in particular) and atmospheric perturbations.

  5. Seasonal differences in aerosol abundance and radiative forcing in months of contrasting emissions and rainfall over northern South Asia

    NASA Astrophysics Data System (ADS)

    Sadavarte, P.; Venkataraman, C.; Cherian, R.; Patil, N.; Madhavan, B. L.; Gupta, T.; Kulkarni, S.; Carmichael, G. R.; Adhikary, B.

    2016-01-01

    A modeling framework was used to examine gaps in understanding of seasonal and spatial heterogeneity in aerosol abundance and radiative forcing over northern South Asia, whose glimpses are revealed in observational studies. Regionally representative emissions were used in chemical transport model simulations at a spatial resolution of 60 × 60 km2, in April, July and September, chosen as months of contrasting emissions and rainfall. Modeled aerosol abundance in northern South Asia was predominantly found to be dust and carbonaceous in April, dust and sulfate in July and sulfate and carbonaceous in September. Anthropogenic aerosols arose from energy-use emissions (from industrial sources, residential biofuel cooking, brick kilns) in all months, additionally from field burning in April, and incursion from East Asia in September. In April, carbonaceous aerosols were abundant from open burning of agricultural fields even at high altitude locations (Godavari), and of forests in the eastern Gangetic Plain (Kolkata). Direct radiative forcing and heating rate, calculated from OPAC-SBDART, using modeled aerosol fields, and corrected by MODIS AOD observations, showed regionally uniform atmospheric forcing in April, compared to that in other months, influenced by both dust and black carbon abundance. A strong spatial heterogeneity of radiative forcing and heating rate was found, with factor of 2.5-3.5 lower atmospheric forcing over the Tibet plateau than that over the Ganga Plain and Northwest in July and September. However, even over the remote Tibet plateau, there was significant anthropogenic contribution to atmospheric forcing and heating rate (45% in Apr, 75% in Sep). Wind fields showed black carbon transport from south Asia in April and east Asia in September. Further evaluation of the transport of dust and anthropogenic emissions from various source regions and their deposition in the Himalaya and Tibet, is important in understanding regional air quality and climate

  6. Simultaneous reductions in emissions of black carbon and co-emitted species will weaken the aerosol net cooling effect

    NASA Astrophysics Data System (ADS)

    Wang, Z. L.; Zhang, H.; Zhang, X. Y.

    2015-04-01

    Black carbon (BC), a distinct type of carbonaceous material formed from the incomplete combustion of fossil and biomass based fuels under certain conditions, can interact with solar radiation and clouds through its strong light-absorption ability, thereby warming the Earth's climate system. Some studies have even suggested that global warming could be slowed down in the short term by eliminating BC emission due to its short lifetime. In this study, we estimate the influence of removing some sources of BC and other co-emitted species on the aerosol radiative effect by using an aerosol-climate atmosphere-only model BCC_AGCM2.0.1_CUACE/Aero with prescribed sea surface temperature and sea ice cover, in combination with the aerosol emissions from the Representative Concentration Pathways (RCPs) scenarios. We find that the global annual mean aerosol net cooling effect at the top of the atmosphere (TOA) will be enhanced by 0.12 W m-2 compared with recent past year 2000 levels if the emissions of only BC are reduced to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial~for the mitigation of global warming. However, both aerosol negative direct and indirect radiative effects are weakened when BC and its co-emitted species (sulfur dioxide and organic carbon) are simultaneously reduced. Relative to year 2000 levels, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 if the emissions of all these aerosols are decreased to the levels projected for 2100 in different ways based on the RCP2.6, RCP4.5, and RCP8.5 scenarios. Because there are no effective ways to remove the BC exclusively without influencing the other co-emitted components, our results therefore indicate that a reduction in BC emission can lead to an unexpected warming on the Earth's climate system in the future.

  7. Evidence for ships emissions in the Central Mediterranean Sea from aerosol chemical analyses at the island of Lampedusa

    NASA Astrophysics Data System (ADS)

    Becagli, S.; Sferlazzo, D. M.; Pace, G.; di Sarra, A.; Bommarito, C.; Calzolai, G.; Ghedini, C.; Lucarelli, F.; Meloni, D.; Monteleone, F.; Severi, M.; Traversi, R.; Udisti, R.

    2011-11-01

    Measurements of aerosol chemical composition made on the island of Lampedusa, south of the Sicily channel, during years 2004-2008, are used to identify the influence of ship emissions on aerosol particles in the Central Mediterranean. Evidence of ship emissions influence is found in 17% of the daily samples. Aerosol samples influenced by ships are characterized by elevated Ni and V soluble fraction (about 80% for aerosol from ships, versus about 40 % for crustal particles), high V and Ni to Si ratios, and values of Vsol>6 ng m-3. Back trajectories analysis on the selected events show that air masses prevalently come from the Sicily channel, where an intense ship traffic occurs. Vsol, Nisol, and non-sea salt SO42- (nssSO42-) show a marked seasonal behaviour, with an evident summer maximum. Such a pattern can be explained by several processes: (i) increased photochemical activity in summer, leading to a faster production of secondary aerosols, mainly nssSO42-, from the oxidation of SO2 in the ship plume; (ii) stronger marine boundary layer (MBL) stability in summer, leading to higher concentration of emitted compounds in the lowest atmospheric layers; (iii) more frequent meteorological conditions leading to consecutive days with trajectories from the Sicily channel in summer. A very intense event in spring 2008 was studied in detail, also using size segregated chemical measurements. These data show that elements arising from heavy oil combustion (V, Ni, Al, Fe) are distributed in the sub-micrometric fraction of the aerosol, and the metals are present as free metals, carbonates, oxides hydrates or labile complex with organic ligands, so that they are dissolved in mild condition (HNO3, pH1.5). Data suggest a characteristic nssSO42-/V ratio in the range 200-400 for ship emission aerosols in summer at Lampedusa. By using the value of 200 a lower limit for the ship contribution to total sulphates is estimated. Ship emissions account, as a summer average, at least for 1

  8. An experimental study quantifying pulmonary ventilation on inhalation of aerosol under steady and episodic emission.

    PubMed

    Poon, Carmen K M; Lai, Alvin C K

    2011-09-15

    Estimating inhalation dose accurately under realistic conditions can enhance the accuracy of risk assessment. Conventional methods to quantify aerosol concentration that susceptible victims in contaminated environments are exposed to use real time particle counters to measure concentrations in environments without occupancy. Breathing-induced airflow interacts and influences concentration around nostrils or mouth and alter the ultimate exposure. This subject has not yet been systematically studied, particularly under transient emission. In this work, an experimental facility comprising two manikins was designed and fabricated. One of them mimicked realistic breathing, acting as a susceptible victim. Both steady and episodic emissions were generated in an air-conditioned environmental chamber in which two different ventilation schemes were tested. The scaled-dose of the victim under different expiratory velocities and pulmonary ventilation was measured. Inferring from results obtained from comprehensive tests, it can be concluded that breathing has very significant influence on the ultimate dose compared with that without breathing. Majority of results show that breathing reduces inhalation quantity and the reduction magnitude increases with breathing rate. This is attributed to the fact that the exhalation process plays a more significant role in reducing the dose level than the enhanced effect during inhalation period. The higher the breathing rate, the sharper the decline of the resultant concentration would be leading to lower dose. Nevertheless, under low pulmonary ventilation, results show that breathing increases dose marginally. Results also reveals that ventilation scheme also affects the exposure.

  9. Detailed chemical characterization of unresolved complex mixtures in atmospheric organics: Insights into emission sources, atmospheric processing, and secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Chan, Arthur W. H.; Isaacman, Gabriel; Wilson, Kevin R.; Worton, David R.; Ruehl, Christopher R.; Nah, Theodora; Gentner, Drew R.; Dallmann, Timothy R.; Kirchstetter, Thomas W.; Harley, Robert A.; Gilman, Jessica B.; Kuster, William C.; Gouw, Joost A.; Offenberg, John H.; Kleindienst, Tadeusz E.; Lin, Ying H.; Rubitschun, Caitlin L.; Surratt, Jason D.; Hayes, Patrick L.; Jimenez, Jose L.; Goldstein, Allen H.

    2013-06-01

    Recent studies suggest that semivolatile organic compounds (SVOCs) are important precursors to secondary organic aerosol (SOA) in urban atmospheres. However, knowledge of the chemical composition of SVOCs is limited by current analytical techniques, which are typically unable to resolve a large number of constitutional isomers. Using a combination of gas chromatography and soft photoionization mass spectrometry, we characterize the unresolved complex mixture (UCM) of semivolatile aliphatic hydrocarbons observed in Pasadena, California (~16 km NE of downtown Los Angeles), and Bakersfield, California, during the California Research at the Nexus of Air Quality and Climate Change 2010. To the authors' knowledge, this work represents the most detailed characterization of the UCM in atmospheric samples to date. Knowledge of molecular structures, including carbon number, alkyl branching, and number of rings, provides important constraints on the rate of atmospheric processing, as the relative amounts of branched and linear alkanes are shown to be a function of integrated exposure to hydroxyl radicals. Emissions of semivolatile branched alkanes from fossil fuel-related sources are up to an order of magnitude higher than those of linear alkanes, and the gas-phase OH rate constants of branched alkanes are ~30% higher than their linear isomers. Based on a box model considering gas/particle partitioning, emissions, and reaction rates, semivolatile branched alkanes are expected to play a more important role than linear alkanes in the photooxidation of the UCM and subsequent transformations into SOA. Detailed speciation of semivolatile compounds therefore provides essential understanding of SOA sources and formation processes in urban areas.

  10. Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study.

    PubMed

    Kuhns, Hampden; Knipping, Eladio M; Vukovich, Jeffrey M

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions

  11. Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study.

    PubMed

    Kuhns, Hampden; Knipping, Eladio M; Vukovich, Jeffrey M

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions

  12. Characterization of vehicle emissions in São Paulo and the impacts on atmospheric chemistry and secondary aerosol formation

    NASA Astrophysics Data System (ADS)

    Ferreira De Brito, J.; Godoy, M.; Godoy, J.; Varanda Rizzo, L.; Artaxo, P.

    2012-12-01

    Megacities emissions are increasingly becoming a global issue, where emissions from the transportation sector play an important role. São Paulo, located in Southeast of Brazil, is a megacity with a population of 18 million people, 7 million cars and large-scale industrial emissions. As a result of the vehicular and industrial emissions, the air quality in São Paulo is considered one of the worst worldwide. Despite the large impact on human health and atmospheric chemistry/dynamics, 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 pattern, we are running a source apportionment study in São Paulo. 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) and diesel (heavy-duty vehicles). Whereas the latter shows usually much higher emission factors compared with ethanol or gasohol, heavy-duty vehicles have increasingly limited access within the São Paulo city limits, thus increasing the importance of light duty vehicles on air quality degradation. This study comprises four sampling sites, where trace elements and organic aerosol are being measured for PM2.5 and PM10 along with real-time NOx, ozone, 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 real-time VOC analysis and aerosol composition, respectively. Results show aerosol number concentrations ranging between 10^4 and 3.10^4 cm-3, mostly

  13. Positron emission tomography (PET) for assessing aerosol deposition of orally inhaled drug products.

    PubMed

    Dolovich, Myrna B; Bailey, Dale L

    2012-12-01

    The topical distribution of inhaled therapies in the lung can be viewed using radionuclides and imaging. Positron emission tomography (PET) is a three-dimensional functional imaging technique providing quantitatively accurate localization of the quantity and distribution of an inhaled or injected PET radiotracer in the lung. A series of transaxial slices through the lungs are obtained, comparable to an X-ray computed tomography (CT) scan. Subsequent reformatting allows coronal and sagittal images of the distribution of radioactivity to be viewed. This article describes procedures for administering [(18)F]-fluorodeoxyglucose aerosol to human subjects for the purpose of determining dose and distribution following inhalation from an aerosol drug delivery device (ADDD). The advantages of using direct-labeled PET drugs in the ADDD are discussed with reference to the literature. The methods for designing the inhalation system, determining proper radiation shielding, calibration, and validation of administered radioactivity, scanner setup, and data handling procedures are described. Obtaining an X-ray CT or radionuclide transmission scan to provide accurate geometry of the lung and also correct for tissue attenuation of the PET radiotracer is discussed. Protocols for producing accurate images, including factors that need to be incorporated into the data calibration, are described, as well as a proposed standard method for partitioning the lung into regions of interest. Alternate methods are described for more detailed assessments. Radiation dosimetry/risk calculations for the procedures are appended, as well as a sample data collection form and spreadsheet for calculations. This article should provide guidance for those interested in using PET to determine quantity and distribution of inhaled therapeutics. PMID:23215847

  14. Improved attribution of climate forcing to emissions.

    PubMed

    Shindell, Drew T; Faluvegi, Greg; Koch, Dorothy M; Schmidt, Gavin A; Unger, Nadine; Bauer, Susanne E

    2009-10-30

    Evaluating multicomponent climate change mitigation strategies requires knowledge of the diverse direct and indirect effects of emissions. Methane, ozone, and aerosols are linked through atmospheric chemistry so that emissions of a single pollutant can affect several species. We calculated atmospheric composition changes, historical radiative forcing, and forcing per unit of emission due to aerosol and tropospheric ozone precursor emissions in a coupled composition-climate model. We found that gas-aerosol interactions substantially alter the relative importance of the various emissions. In particular, methane emissions have a larger impact than that used in current carbon-trading schemes or in the Kyoto Protocol. Thus, assessments of multigas mitigation policies, as well as any separate efforts to mitigate warming from short-lived pollutants, should include gas-aerosol interactions.

  15. 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.

  16. 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.

  17. Observed Diel, Seasonal, and Long-Term Trends in O3, SO2, and Precursor Emissions over the Eastern US

    NASA Astrophysics Data System (ADS)

    Dickerson, R. R.; Vinnikov, K. Y.

    2009-12-01

    Ozone and particulate matter, pervasive pollution problems over the eastern US, have been the target of substantial controls on emissions. We apply a method of polynomial fit to long-term time series of hourly, surface O3 and SO2 concentrations as well as NOx and SO2 emissions to facilitate visualization of the annually and daily cycles, and to quantify the long-term (decadal) changes. These statistical methods show the influence of natural as well as anthropogenic ozone sources and allow us to address the question of efficacy of pollution control measures. Have ozone concentrations decreased when and where they matter most for human and ecosystem health? Have the concentrations of SO2 and sulfate fallen linearly with decreases in emissions? The analysis shows that controls of sulfur emissions have been more effective in some locations than others, and that ozone mixing ratios have improved despite increases in temperature. Figure Caption. Average diel (daily) and seasonal distribution of 1989-2007 ozone concentrations observed at five rural eastern US monitoring stations of the CASTNET network contour plotted across local standard time and month. The X-axis depicts season while the Y-axis shows the daily cycle. Ozone demonstrates a distinct maximum in the afternoon of summer days, with a secondary maximum in spring. Local photochemical smog production drives the summer maximum, but downward mixing from the stratosphere as well as free tropospheric production from long-lived precursors contribute to the spring maximum. The minima are seen at night in winter when photochemical production is slow and losses through dry deposition and titration with NO dominate.

  18. Quantitative evaluation of emission control of primary and secondary organic aerosol sources during Beijing 2008 Olympics

    NASA Astrophysics Data System (ADS)

    Guo, S.; Hu, M.; Guo, Q.; Zhang, X.; Schauer, J. J.; Zhang, R.

    2012-12-01

    To explore the primary and secondary sources of fine organic particles after the aggressive implementation of air pollution controls during 2008 Beijing Olympic Games, 12-h PM2.5 concentrations were measured at one urban and one upwind rural site during the CAREBeijing-2008 (Campaigns of Air quality REsearch in Beijing and surrounding region) summer field campaign. The PM2.5 concentrations were 72.5±43.6μg m3 and 64.3±36.2μg m-3 at the urban site and rural site, respectively, which were the lowest in recent years due to the implementation of drastic control measures and favorable weather conditions. Five primary and four secondary fine organic particle sources were quantified using a CMB (chemical mass balance) model and tracer-yield method. Compared with previous studies in Beijing, the contribution of vehicle emission increased, with diesel engines contributing 16.2±5.9% and 14.5±4.1% to the total organic carbon (OC) concentrations and gasoline vehicles accounting for 10.3±8.7% and 7.9±6.2% of the OC concentrations at two sites. Due to the implementation of emission control measures, the OC concentrations from important primary sources have been reduced, and secondary formation has become an important contributor to fine organic aerosols. Compared with the non-controlled period, primary vehicle contributions were reduced by 30% and 24% in the urban and regional area, and reductions in the contribution from coal combustion were 57% and 7%, respectively. These results demonstrate the emission control measures significantly alleviated the primary organic particle pollution in and around Beijing. However, the control effectiveness of secondary organic particles was not significant.

  19. Chemical speciation of chlorine in atmospheric aerosol samples by high-resolution proton induced X-ray emission spectroscopy

    NASA Astrophysics Data System (ADS)

    Kertész, Zsófia; Furu, Enikő; Kavčič, Matjaž

    2013-01-01

    Chlorine is a main elemental component of atmospheric particulate matter (APM). The knowledge of the chemical form of chlorine is of primary importance for source apportionment and for estimation of health effects of APM. In this work the applicability of high-resolution wavelength dispersive proton induced X-ray emission (PIXE) spectroscopy for chemical speciation of chlorine in fine fraction atmospheric aerosols is studied. A Johansson-type crystal spectrometer with energy resolution below the natural linewidth of Cl K lines was used to record the high-resolution Kα and Kβ proton induced spectra of several reference Cl compounds and two atmospheric aerosol samples, which were collected for conventional PIXE analysis. The Kα spectra which refers to the oxidation state, showed very minor differences due to the high electronegativity of Cl. However, the Kβ spectra exhibited pronounced chemical effects which were significant enough to perform chemical speciation. The major chlorine component in two fine fraction aerosol samples collected during a 2010 winter campaign in Budapest was clearly identified as NaCl by comparing the high-resolution Cl Kβ spectra from the aerosol samples with the corresponding reference spectra. This work demonstrates the feasibility of high-resolution PIXE method for chemical speciation of Cl in aerosols.

  20. Sensitivity of nitrate aerosols to ammonia emissions and to nitrate chemistry: implications for present and future nitrate optical depth

    NASA Astrophysics Data System (ADS)

    Paulot, F.; Ginoux, P.; Cooke, W. F.; Donner, L. J.; Fan, S.; Lin, M.-Y.; Mao, J.; Naik, V.; Horowitz, L. W.

    2016-02-01

    We update and evaluate the treatment of nitrate aerosols in the Geophysical Fluid Dynamics Laboratory (GFDL) atmospheric model (AM3). Accounting for the radiative effects of nitrate aerosols generally improves the simulated aerosol optical depth, although nitrate concentrations at the surface are biased high. This bias can be reduced by increasing the deposition of nitrate to account for the near-surface volatilization of ammonium nitrate or by neglecting the heterogeneous production of nitric acid to account for the inhibition of N2O5 reactive uptake at high nitrate concentrations. Globally, uncertainties in these processes can impact the simulated nitrate optical depth by up to 25 %, much more than the impact of uncertainties in the seasonality of ammonia emissions (6 %) or in the uptake of nitric acid on dust (13 %). Our best estimate for fine nitrate optical depth at 550 nm in 2010 is 0.006 (0.005-0.008). In wintertime, nitrate aerosols are simulated to account for over 30 % of the aerosol optical depth over western Europe and North America. Simulated nitrate optical depth increases by less than 30 % (0.0061-0.010) in response to projected changes in anthropogenic emissions from 2010 to 2050 (e.g., -40 % for SO2 and +38 % for ammonia). This increase is primarily driven by greater concentrations of nitrate in the free troposphere, while surface nitrate concentrations decrease in the midlatitudes following lower concentrations of nitric acid. With the projected increase of ammonia emissions, we show that better constraints on the vertical distribution of ammonia (e.g., convective transport and biomass burning injection) and on the sources and sinks of nitric acid (e.g., heterogeneous reaction on dust) are needed to improve estimates of future nitrate optical depth.

  1. 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.

  2. 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.

  3. Comparative Analysis of Urban Atmospheric Aerosol by Particle-Induced X-ray Emission (PIXE), Proton Elastic Scattering Analysis (PESA), and Aerosol Mass Spectrometry (AMS)

    SciTech Connect

    Johnson, Kirsten S; Laskin, Alexander; Jimenez, Jose L; Shutthanandan, V; Molina, Luisa T; Salcedo, D; Dzepina, K; Molina, Mario J

    2008-09-01

    A multifaceted approach to atmospheric aerosol analysis is often desirable in field studies where an understanding of technical comparability among different measurement techniques is essential. Herein we report quantitative intercomparisons of Particle-Induced X-ray Emission (PIXE) and Proton Elastic Scattering Analysis (PESA), performed off-line under vacuum, with analysis by Aerosol Mass Spectrometry (AMS) carried out in real-time during the MCMA-2003 Field Campaign in the Mexico City Metropolitan Area. Good agreement was observed for mass concentrations of PIXE-measured sulfur (assuming it was dominated by SO42-) and AMS-measured sulfate during the most of the campaign. PESA-measured hydrogen mass was separated into sulfate H and organic H mass fractions assuming the only major contributions were (NH4)2SO4 and organic compounds. Comparison of the organic H mass with AMS organic aerosol measurements indicates that about 75% of the mass of these species evaporated under vacuum. However ~25% of the organics does remain under vacuum, which is only possible with low vapor pressure compounds, and which supports the presence of high molecular weight and/or highly oxidized organics consistent with atmospheric aging. Approximately 10% of the chloride detected by AMS was measured by PIXE, possibly in the form of metal-chloride complexes, while the majority of Cl was likely present as more volatile species including NH4Cl. This is the first comparison of PIXE/PESA and AMS, and to our knowledge also the first report of PESA hydrogen measurements for urban organic aerosols.

  4. Small global effect on terrestrial net primary production due to increased fossil fuel aerosol emissions from East Asia since the turn of the century

    PubMed Central

    Rap, A.; Reddington, C. L.; Spracklen, D. V.; Gloor, M.; Buermann, W.

    2016-01-01

    Abstract The global terrestrial carbon sink has increased since the start of this century at a time of growing carbon emissions from fossil fuel burning. Here we test the hypothesis that increases in atmospheric aerosols from fossil fuel burning enhanced the diffuse light fraction and the efficiency of plant carbon uptake. Using a combination of models, we estimate that at global scale changes in light regimes from fossil fuel aerosol emissions had only a small negative effect on the increase in terrestrial net primary production over the period 1998–2010. Hereby, the substantial increases in fossil fuel aerosol emissions and plant carbon uptake over East Asia were effectively canceled by opposing trends across Europe and North America. This suggests that if the recent increase in the land carbon sink would be causally linked to fossil fuel emissions, it is unlikely via the effect of aerosols but due to other factors such as nitrogen deposition or nitrogen‐carbon interactions. PMID:27773953

  5. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States.

    PubMed

    Jathar, Shantanu H; Gordon, Timothy D; Hennigan, Christopher J; Pye, Havala O T; Pouliot, George; Adams, Peter J; Donahue, Neil M; Robinson, Allen L

    2014-07-22

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10-20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y(-1) of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations.

  6. Impact of Emissions and Long-Range Transport on Multi-Decadal Aerosol Trends: Implications for Air Quality and Climate

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2012-01-01

    We present a global model analysis of the impact of long-range transport and anthropogenic emissions on the aerosol trends in the major pollution regions in the northern hemisphere and in the Arctic in the past three decades. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze the multi-spatial and temporal scale data, including observations from Terra, Aqua, and CALIPSO satellites and from the long-term surface monitoring stations. We will analyze the source attribution (SA) and source-receptor (SR) relationships in North America, Europe, East Asia, South Asia, and the Arctic at the surface and free troposphere and establish the quantitative linkages between emissions from different source regions. We will discuss the implications for regional air quality and climate change.

  7. Aerosol and trace gas vehicle emission factors measured in a tunnel using an Aerosol Mass Spectrometer and other on-line instrumentation

    NASA Astrophysics Data System (ADS)

    Chirico, Roberto; Prevot, Andre S. H.; DeCarlo, Peter F.; Heringa, Maarten F.; Richter, Rene; Weingartner, Ernest; Baltensperger, Urs

    2011-04-01

    In this study we present measurements of gas and aerosol phase composition for a mixed vehicle fleet in the Gubrist tunnel (Switzerland) in June 2008. PM 1 composition measurements were made with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (AMS) and a Multi Angle Absorption Photometer (MAAP). Gas-phase measurements of CO, CO 2, NO x and total hydrocarbons (THC) were performed with standard instrumentation. Weekdays had a characteristic diurnal pattern with 2 peaks in concentrations for all traffic related species corresponding to high vehicle density (˜300 ± 30 vehicles per 5 min) in the morning rush hour between 06:00 and 09:00 and in the afternoon rush hours from approximately 15:30 to 18:30. The emission factors (EF) of OA were heavily influenced by the OA mass loading. To exclude this partitioning effect, only organic aerosol mass concentrations from 60 μg m -3 to 90 μg m -3 were considered and for these conditions the EF(OA) value for HDV was 33.7 ± 2.3 mg km -1 for a temperature inside the tunnel of 20-25 °C. This value is not directly applicable to ambient conditions because it is derived from OA mass concentrations that are roughly a factor of 10 higher than typical ambient concentrations. An even higher EF(OA) HDV value of 47.4 ± 1.6 mg km -1 was obtained when the linear fit was applied to all data points including OA concentrations up to 120 μg m -3. Similar to the increasing EF, the OA/BC ratio in the tunnel was also affected by the organic loading and it increased by a factor of ˜3 over the OA range 10-120 μg m -3. This means that also the OA emission factors at ambient concentrations of around 5-10 μg m -3 would be 2-3 times lower than the emission factor given above. For OA concentrations lower than 40 μg m -3 the OA/BC mass ratio was below 1, while at an OA concentration of 100-120 μg m -3 the OA/BC ratio was ˜1.5. The AMS mass spectra (MS) acquired in the tunnel were highly correlated with the primary organic aerosol

  8. Atmospheric aerosol monitoring and characterization: An emission control strategy to protect tropical forests

    NASA Astrophysics Data System (ADS)

    Mateus, V. L.; do Valles, T. V.; de Oliveira, T. B.; de Almeida, A. C.; Maia, L. F. P. G.; Saint'Pierre, T. D.; Gioda, A.

    2013-12-01

    Human activity represents one of the most harmful activities for biodiversity. Population growth has caused increasing interferences in natural areas suffering agriculture or urbanization. As a consequence, tropical forests are at risk, since they shelter more than half of the global biodiversity. In this context, protected areas are indeed important to preserve natural populations as well as threatened habitats. Aerosol samples were collected in two protected areas in Rio de Janeiro, Brazil, in order to quantify water-soluble species and evaluate anthropogenic influences considering secondary aerosol formation and organic compounds. Samplings were conducted at the National Park of Serra dos Orgãos (Parnaso) and the National Forest Mario Xavier (Flonamax) during 24 h every six days using a high-volume sampler from July 2010 to June 2012 (PM10) and from July 2011 to August 2012 (TSP), respectively. The aerosol mass was determined by Gravimetry. The water-soluble ionic composition (WSIC) was obtained by Ion Chromatography in order to determine the major anions (Br-, Cl-, F-, NO2-, NO3-, PO43-, SO42-) and cations (Li+, Ca2+, K+, Mg2+, Na+, NH4+); total water-soluble carbon (TWSC), water-soluble organic carbon (WSOC) were determined by a TOC analyzer and the elements were determined by Inductively Coupled Plasma Optical Emission Spectrometry. PM10 average concentrations ranged from 11.1 to 67.6 μg m-3 and TSP from 5.7 to 242.6 μg m-3. Regarding the ions, the highest cation concentration was measured for Na+ at both Parnaso and Flonamax sites, respectively, 2.9 and 6.1 μg m-3. Both sites are near to the coast, justifying these results. On the other hand, SO42- was the predominant anion measured at both sites with average concentrations ranged from 2.3 to 2.7 μg m-3. Around 50% of sulphate had a non-marine origin in the former site, while in the latter the percentage was of circa 40%. The correlation between NO3- and nss-SO42- was much stronger at Parnaso (r = 0

  9. Historical (1850-2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols:methodology and application

    SciTech Connect

    Lamarque, J. F.; Bond, Tami C.; Eyring, Veronika; Granier, Claire; Heil, Angelika; Klimont, Z.; Lee, David S.; Liousse, Catherine; Mieville, Aude; Owen, Bethan; Schultz, Martin; Shindell, Drew; Smith, Steven J.; Stehfest, Eike; van Aardenne, John; Cooper, Owen; Kainuma, M.; Mahowald, Natalie; McConnell, J.R.; Naik, Vaishali; Riahi, Keywan; Van Vuuren, Detlef

    2010-08-11

    We present and discuss a new dataset of gridded emissions covering the historical period (1850-2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment report. Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available at this point; 40 regions and 12 sectors were used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, was then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Application of these emissions into two chemistry-climate models is used to test their ability to capture long-term changes in atmospheric ozone, carbon monoxide and aerosols distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations consistently underestimate the carbon monoxide trend, while capturing the long-term trend at the Mace Head station. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates.

  10. Brown carbon aerosols from burning of boreal peatlands: microphysical properties, emission factors, and implications for direct radiative forcing

    NASA Astrophysics Data System (ADS)

    Chakrabarty, Rajan K.; Gyawali, Madhu; Yatavelli, Reddy L. N.; Pandey, Apoorva; Watts, Adam C.; Knue, Joseph; Chen, Lung-Wen A.; Pattison, Robert R.; Tsibart, Anna; Samburova, Vera; Moosmüller, Hans

    2016-03-01

    The surface air warming over the Arctic has been almost twice as much as the global average in recent decades. In this region, unprecedented amounts of smoldering peat fires have been identified as a major emission source of climate-warming agents. While much is known about greenhouse gas emissions from these fires, there is a knowledge gap on the nature of particulate emissions and their potential role in atmospheric warming. Here, we show that aerosols emitted from burning of Alaskan and Siberian peatlands are predominantly brown carbon (BrC) - a class of visible light-absorbing organic carbon (OC) - with a negligible amount of black carbon content. The mean fuel-based emission factors for OC aerosols ranged from 3.8 to 16.6 g kg-1. Their mass absorption efficiencies were in the range of 0.2-0.8 m2 g-1 at 405 nm (violet) and dropped sharply to 0.03-0.07 m2 g-1 at 532 nm (green), characterized by a mean Ångström exponent of ≈ 9. Electron microscopy images of the particles revealed their morphologies to be either single sphere or agglomerated "tar balls". The shortwave top-of-atmosphere aerosol radiative forcing per unit optical depth under clear-sky conditions was estimated as a function of surface albedo. Only over bright surfaces with albedo greater than 0.6, such as snow cover and low-level clouds, the emitted aerosols could result in a net warming (positive forcing) of the atmosphere.

  11. Emissions of Black Carbon, Organic, and Inorganic Aerosols From Biomass Burning in North America and Asia in 2008

    NASA Technical Reports Server (NTRS)

    Kondo, Y.; Matsui, H.; Moteki, N.; Sahu, L.; Takegawa, N.; Kajino, M.; Zhao, Y.; Cubison, M. J.; Jimenez, J. L.; Vay, S.; Diskin, G. S.; Anderson, B.; Wisthaler, A.; Mikoviny, T.; Fuelberg, H. E.; Blake, D. R.; Huey, G.; Weinheimer, A. J.; Knapp, D. J.; Brune, W. H.

    2011-01-01

    Reliable assessment of the impact of aerosols emitted from boreal forest fires on the Arctic climate necessitates improved understanding of emissions and the microphysical properties of carbonaceous (black carbon (BC) and organic aerosols (OA)) and inorganic aerosols. The size distributions of BC were measured by an SP2 based on the laser-induced incandescence technique on board the DC-8 aircraft during the NASA ARCTAS campaign. Aircraft sampling was made in fresh plumes strongly impacted by wildfires in North America (Canada and California) in summer 2008 and in those transported from Asia (Siberia in Russia and Kazakhstan) in spring 2008. We extracted biomass burning plumes using particle and tracer (CO, CH3CN, and CH2Cl2) data. OA constituted the dominant fraction of aerosols mass in the submicron range. The large majority of the emitted particles did not contain BC. We related the combustion phase of the fire as represented by the modified combustion efficiency (MCE) to the emission ratios between BC and other species. In particular, we derived the average emission ratios of BC/CO = 2.3 +/- 2.2 and 8.5 +/- 5.4 ng/cu m/ppbv for BB in North America and Asia, respectively. The difference in the BC/CO emission ratios is likely due to the difference in MCE. The count median diameters and geometric standard deviations of the lognormal size distribution of BC in the BB plumes were 136-141 nm and 1.32-1.36, respectively, and depended little on MCE. These BC particles were thickly coated, with shell/core ratios of 1.3-1.6. These parameters can be used directly for improving model estimates of the impact of BB in the Arctic.

  12. The effect of large anthropogenic particulate emissions on atmospheric aerosols, deposition and bioindicators in the eastern Gulf of Finland region.

    PubMed

    Jalkanen, L; Mäkinen, A; Häsänen, E; Juhanoja, J

    2000-10-30

    The effect of the emissions from large oil shale fuelled power plants and a cement factory in Estonia on the elemental concentration of atmospheric aerosols, deposition, elemental composition of mosses and ecological effects on mosses, lichens and pine trees in the eastern Gulf of Finland region has been studied. In addition to chemical analysis, fly ash, moss and aerosol samples were analysed by a scanning electron microscope with an energy dispersive X-ray spectrometer (SEM/EDS). The massive particulate calcium emissions, approximately 60 kton/year (1992), is clearly observed in the aerosols, deposition and mosses. The calcium deposition is largest next to the Russian border downwind from the power plants and in south-eastern part of Finland. This deposition has decreased due to the application of dust removal systems at the particulate emission sources. At the Virolahti EMEP station approximately 140 km north from the emission sources, elevated elemental atmospheric aerosol concentrations are observed for Al, Ca, Fe, K and Si and during episodes many trace elements, such as As, Br, Mo, Ni, Pb and V. The acidification of the soil is negligible because of the high content of basic cations in the deposition. Visible symptoms on pine trees are negligible. However, in moss samples close to the power plants, up to 25% of the leaf surface was covered by particles. Many epiphytic lichen species do not tolerate basic stemflow and on the other hand most species are also very sensitive for the SO2 content in air. Consequently a large lichen desert is found in an area of 2500 km2 in the vicinity of the power plants with only one out of the investigated 12 species growing.

  13. Aerosol emissions from forest and grassland burnings in the southern amazon basin and central Brazil

    NASA Astrophysics Data System (ADS)

    Leslie, Alistair C. D.

    1981-03-01

    Forest and grassland clearing by means of prescribed fires in tropical areas of the world may be responsible for large inputs of fine particulates to the global atmosphere besides being a major source of trace gases. The major continents on which extensive biomass burning takes place are Africa and South America. Such agricultural practices of burning have been employed throughout man's existence, but the importance and significance of such burning relative to anthropogenic industrial emissions to the atmosphere has not until extremely recently been seriously studied. In August-September 1979 project "Brushfire 1979" took place based in Brasília, Brazil. The Air Quality Division of the National Center for Atmospheric Research made ground level and aircraft measurements of trace gases (e.g. CO 2, CO, CH 4, N 2O, H 2, CH 3Cl, COS, NO, NO 2, O 3) and Florida State University sampled ground level aerosol emissions from grass and forest burnings. Aerosols were sampled using plastic 7-stage single orifice cascade impactors and FSU type linear and circular "streakers". Long term sampling was made of regional background for total particulates (<15 μmad) with 2 h resolution using streakers and with impactors for 24 h resolution of 7 particle size fractions (<0.25 to >8 μmad). Short term sampling within grass or forest fires was made using impactors incorporated into portable kits containing 4 miniature 12-18 V dc Brailsford pumps and a disposable dry cell power pack. Sampling times of 5-15 min were found optimal under these conditions. Grass fires were sampled in the savannah area northeast of Brasília and forest fires in the state of Mato Grosso on the southern edge of the dryland forest of the Amazon basin. Residual ash samples were collected. All of the samples were analyzed at Florida State University using PIXE for 15-20 elements including Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Pb and Sr. Computer reduction of the X-ray spectra was made

  14. Application of mobile aerosol and trace gas measurements for the investigation of megacity air pollution emissions: the Paris metropolitan area

    NASA Astrophysics Data System (ADS)

    von der Weiden-Reinmüller, S.-L.; Drewnick, F.; Crippa, M.; Prévôt, A. S. H.; Meleux, F.; Baltensperger, U.; Beekmann, M.; Borrmann, S.

    2014-01-01

    For the investigation of megacity emission development and the impact outside the source region, mobile aerosol and trace gas measurements were carried out in the Paris metropolitan area between 1 July and 31 July 2009 (summer conditions) and 15 January and 15 February 2010 (winter conditions) in the framework of the European Union FP7 MEGAPOLI project. Two mobile laboratories, MoLa and MOSQUITA, were deployed, and here an overview of these measurements and an investigation of the applicability of such measurements for the analysis of megacity emissions are presented. Both laboratories measured physical and chemical properties of fine and ultrafine aerosol particles as well as gas phase constituents of relevance for urban pollution scenarios. The applied measurement strategies include cross-section measurements for the investigation of plume structure and quasi-Lagrangian measurements axially along the flow of the city's pollution plume to study plume aging processes. Results of intercomparison measurements between the two mobile laboratories represent the adopted data quality assurance procedures. Most of the compared measurement devices show sufficient agreement for combined data analysis. For the removal of data contaminated by local pollution emissions a video tape analysis method was applied. Analysis tools like positive matrix factorization and peak integration by key analysis applied to high-resolution time-of-flight aerosol mass spectrometer data are used for in-depth data analysis of the organic particulate matter. Several examples, including a combination of MoLa and MOSQUITA measurements on a cross section through the Paris emission plume, are provided to demonstrate how such mobile measurements can be used to investigate the emissions of a megacity. A critical discussion of advantages and limitations of mobile measurements for the investigation of megacity emissions completes this work.

  15. Application of mobile aerosol and trace gas measurements for the investigation of megacity air pollution emissions: the Paris metropolitan area

    NASA Astrophysics Data System (ADS)

    von der Weiden-Reinmüller, S.-L.; Drewnick, F.; Crippa, M.; Prévôt, A. S. H.; Meleux, F.; Baltensperger, U.; Beekmann, M.; Borrmann, S.

    2013-08-01

    For the investigation of megacity emission development and impact outside the source region mobile aerosol and trace gas measurements were carried out in the Paris metropolitan area between 1 July and 31 July 2009 (summer conditions) and 15 January and 15 February 2010 (winter conditions) in the framework of the European Union FP7 MEGAPOLI project. Two mobile laboratories, MoLa and MOSQUITA, were deployed, and here an overview of these measurements and an investigation of the applicability of such measurements for the analysis of megacity emissions are presented. Both laboratories measured physical and chemical properties of fine and ultrafine aerosol particles as well as gas phase constituents of relevance for urban pollution scenarios. The applied measurement strategies include cross section measurements for the investigation of plume structure and quasi-Lagrangian measurements radially away from the city center to study plume aging processes. Results of intercomparison measurements between the two mobile laboratories represent the adopted data quality assurance procedures. Most of the compared measurement devices show sufficient agreement for combined data analysis. For the removal of data contaminated by local pollution emissions a video tape analysis method was applied. Analysis tools like positive matrix factorization and peak integration by key analysis applied to high-resolution time-of-flight aerosol mass spectrometer data are used for in-depth data analysis of the organic particulate matter. Several examples, including a combination of MoLa and MOSQUITA measurements on a cross section through the Paris emission plume are provided to demonstrate how such mobile measurements can be used to investigate the emissions of a megacity. A critical discussion of advantages and limitations of mobile measurements for the investigation of megacity emissions completes this work.

  16. Temporal variability of primary and secondary aerosols over northern India: Impact of biomass burning emissions

    NASA Astrophysics Data System (ADS)

    Rastogi, N.; Singh, A.; Sarin, M. M.; Singh, D.

    2016-01-01

    The ambient particulate matter injected from biomass burning emissions (BBEs) over northern India has been a subject of major debate in the context of regional air quality and atmospheric chemistry of several organic and inorganic constituents. This necessitates an observational approach over a large spatial and temporal scale. We present an extensive data set on PM2.5 samples (n = 147) collected for one full year from a sampling site (Patiala: 30.2°N, 76.3°E) in the source region of BBEs in northern India. During the sampling period from October 2011 to September 2012, PM2.5 mass concentration varied from ˜20 to 400 μg m-3. Among the major constituents, contribution of total carbonaceous aerosols (OC + EC) ranged from 8 to 60%. The average OC/EC and K+/EC ratio, varying from 3.2 to 12 and 0.26 to 0.80, respectively, emphasizes the dominance of BBEs over the annual seasonal cycle. The average secondary organic matter (SOM) accounts for ˜10-40% of PM2.5 mass in different seasons; whereas contribution of secondary inorganics was maximum (˜40%) during the winter. The pronounced temporal variability in SOM suggests its contribution from varying sources, their emission strength and process of secondary organic formation. Diurnal differences in the chemical constituents are attributable to regional meteorological factors and boundary layer dynamics. The emerging data set from this study is important to understand feedback mechanism from anthropogenic activities to the regional climate change scenario.

  17. How Important Is Organic Aerosol Hygroscopicity to Aerosol Indirect Forcing?

    SciTech Connect

    Liu, Xiaohong; Wang, Jian

    2010-12-07

    Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation and yield of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR Community Atmospheric Model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (“κ” value) of POA and SOA. Our model simulation indicates that in the present-day condition changing “κ” value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S=0.1% by 40-60% over the POA source regions, while changing “κ” value of SOA by ±50% (from 0.14 to 0.07 and 0.21) changes the CCN within 30%. Changes in the in-cloud droplet number concentrations (CDNC) are within 20% in most locations on the globe with the above changes in “κ” value of POA and SOA. Global annual mean anthropogenic aerosol indirect forcing (AIF) between present-day (PD) and pre-industrial (PI) conditions change by 0.4 W m-2 with the control run of -1.3 W m-2. AIF reduces with the increase hygroscopicity of organic aerosol, indicating the important role of natural organic aerosol in buffering the relative change of CDNC from PI to PD.

  18. Functional group composition of organic aerosol from combustion emissions and secondary processes at two contrasted urban environments

    NASA Astrophysics Data System (ADS)

    El Haddad, Imad; Marchand, Nicolas; D'Anna, Barbara; Jaffrezo, Jean Luc; Wortham, Henri

    2013-08-01

    The quantification of major functional groups in atmospheric organic aerosol (OA) provides a constraint on the types of compounds emitted and formed in atmospheric conditions. This paper presents functional group composition of organic aerosol from two contrasted urban environments: Marseille during summer and Grenoble during winter. Functional groups were determined using a tandem mass spectrometry approach, enabling the quantification of carboxylic (RCOOH), carbonyl (RCOR‧), and nitro (RNO2) functional groups. Using a multiple regression analysis, absolute concentrations of functional groups were combined with those of organic carbon derived from different sources in order to infer the functional group contents of different organic aerosol fractions. These fractions include fossil fuel combustion emissions, biomass burning emissions and secondary organic aerosol (SOA). Results clearly highlight the differences between functional group fingerprints of primary and secondary OA fractions. OA emitted from primary sources is found to be moderately functionalized, as about 20 carbons per 1000 bear one of the functional groups determined here, whereas SOA is much more functionalized, as in average 94 carbons per 1000 bear a functional group under study. Aging processes appear to increase both RCOOH and RCOR‧ functional group contents by nearly one order of magnitude. Conversely, RNO2 content is found to decrease with photochemical processes. Finally, our results also suggest that other functional groups significantly contribute to biomass smoke and SOA. In particular, for SOA, the overall oxygen content, assessed using aerosol mass spectrometer measurements by an O:C ratio of 0.63, is significantly higher than the apparent O:C* ratio of 0.17 estimated based on functional groups measured here. A thorough examination of our data suggests that this remaining unexplained oxygen content can be most probably assigned to alcohol (ROH), organic peroxides (ROOH

  19. Overview of the impact of wood burning emissions on carbonaceous aerosols and PM in large parts of the Alpine region

    NASA Astrophysics Data System (ADS)

    Herich, H.; Gianini, M. F. D.; Piot, C.; Močnik, G.; Jaffrezo, J.-L.; Besombes, J.-L.; Prévôt, A. S. H.; Hueglin, C.

    2014-06-01

    During the past years, actions implemented for the reduction of particulate matter emissions have in many European countries focused on road traffic emissions. Much less attention was paid to emissions from domestic wood combustion though the importance of residential wood burning as a source of atmospheric particulate matter (PM) in the Alpine region has been shown in many studies. Here we review the current knowledge about the contribution of wood burning emissions to ambient concentrations of elemental carbon (EC), organic carbon (OC) and PM in the Alpine region. The published results obtained by different approaches (e.g. macro-tracer method, multivariate receptor modeling, chemical mass balance modelling, and so-called Aethalometer modeling) are used in an ambient mono-tracer approach to estimate representative relationships between wood burning tracers (levoglucosan and mannosan) and EC, OC and PM from wood burning. The relationships found are applied to available ambient measurements of levoglucosan and mannosan at Alpine sites for estimation of the contributions of wood burning emissions to average levels of carbonaceous aerosols and PM at these sites. Our results imply that PM from wood burning alone adds often up to 50% and more of the EU daily limit value for PM10 in several alpine valleys during days in winter. Concentrations of carbonaceous aerosols in these valleys are often up to six times higher than in urban or rural sites at the foothills of the Alps.

  20. Origin of surface and columnar Indian Ocean Experiment (INDOEX) aerosols using source- and region-tagged emissions transport in a general circulation model - article no. D24211

    SciTech Connect

    Verma, S.; Venkataraman, C.; Boucher, O.

    2008-12-15

    We study the relative influence of aerosols emitted from different sectors and geographical regions on aerosol loading in south Asia. Sectors contributing aerosol emissions include biofuel and fossil fuel combustion, open biomass burning, and natural sources. Geographical regions include India, southeast Asia, east Asia, Africa-west Asia, and the rest of the world. Simulations of the Indian Ocean Experiment (INDOEX), from January to March 1999, are made in the general circulation model of Laboratoire de Meteorologie Dynamique (LMD-ZT GCM) with emissions tagged by sector and geographical region. Anthropogenic emissions dominate (54-88%) the predicted aerosol optical depth (AOD) over all the receptor regions. Among the anthropogenic sectors, fossil fuel combustion has the largest overall influence on aerosol loading, primarily sulfate, with emissions from India (50-80%) and rest of the world significantly influencing surface concentrations and AOD. Biofuel combustion has a significant influence on both the surface and columnar black carbon (BC) in particular over the Indian subcontinent and Bay of Bengal with emissions largely from the Indian region (60-80%). Open biomass burning emissions influence organic matter (OM) significantly, and arise largely from Africa-west Asia. The emissions from Africa-west Asia affect the carbonaceous aerosols AOD in all receptor regions, with their largest influence (AOD-BC: 60%; and AOD-OM: 70%) over the Arabian Sea. Among Indian regions, the Indo-Gangetic Plain is the largest contributor to anthropogenic surface mass concentrations and AOD over the Bay of Bengal and India. Dust aerosols are contributed mainly through the long-range transport from Africa-west Asia over the receptor regions. Overall, the model estimates significant intercontinental incursion of aerosol, for example, BC, OM, and dust from Africa-west Asia and sulfate from distant regions (rest of the world) into the INDOEX domain.

  1. Historical emissions of black and organic carbon aerosol from energy-related combustion, 1850-2000 - article no. GB2018

    SciTech Connect

    Bond, T.C.; Bhardwaj, E.; Dong, R.; Jogani, R.; Jung, S.K.; Roden, C.; Streets, D.G.; Trautmann, N.M.

    2007-05-15

    We present an emission inventory of primary black carbon (BC) and primary organic carbon (OC) aerosols from fossil fuel and biofuel combustion between 1850 and 2000. We reconstruct fossil fuel consumption and represent changes in technology on a national and sectoral basis. Our estimates rely on new estimates of biofuel consumption, and updated emission factors for old technologies. Emissions of black carbon increase almost linearly, totaling about 1000 Gg in 1850, 2200 Gg in 1900, 3000 Gg in 1950, and 4400 Gg in 2000. Primary organic carbon shows a similar pattern, with emissions of 4100 Gg, 5800 Gg, 6700 Gg, and 8700 Gg in 1850, 1900, 1950, and 2000, respectively. Biofuel is responsible for over half of BC emission until about 1890, and dominates energy-related primary OC emission throughout the entire period. Coal contributes the greatest fraction of BC emission between 1880 and 1975, and is overtaken by emissions from biofuel around 1975, and by diesel engines around 1990. Previous work suggests a rapid rise in BC emissions between 1950 and 2000. This work supports a more gradual increase between 1950 and 2000, similar to the increase between 1850 and 1925; implementation of clean technology is a primary reason.

  2. Aerosol particle and trace gas emissions from earthworks, road construction, and asphalt paving in Germany: Emission factors and influence on local air quality

    NASA Astrophysics Data System (ADS)

    Faber, Peter; Drewnick, Frank; Borrmann, Stephan

    2015-12-01

    Aerosol emissions from construction sites have a strong impact on local air quality. The chemical and physical characteristics of particles and trace gases emitted by earthworks (excavation and loading of soil as well as traffic on unpaved roads) and road works (asphalt sawing, smashing, soil compacting, asphalt paving) have therefore been addressed in this study by using a mobile set-up of numerous modern online aerosol and trace gas instruments including a high-resolution aerosol mass spectrometer. Fuel-based emission factors for several variables have been determined, showing that earthwork activities and compacting by use of a plate compactor revealed the highest median emission factors for PM10 (up to 54 g l-1). Construction activities were assigned to contribute about 17% (36 000 t a-1) to total PM10 emissions and 3% (13 500 t a-1) to total traffic-related NOx emissions in Germany. In particular, calculated PM10 emissions by earthworks are about 15 800 t a-1 corresponding to 44% of total PM10 emissions by construction activities in Germany. Mechanical processes such as asphalt sawing (PM1/PM10 = 18 ± 31%), soil compacting by a plate compactor (PM1/PM10 = 5 ± 6%) and earthworks (PM1/PM10 = 2 ± 5%) emit predominantly coarse mineral dust particles. Contrary to that, particle emissions by thermal construction processes (asphalt paving: PM1/PM10 = 62 ± 14%) and by the internal combustion engines of heavy machinery (e.g. road roller PM1/PM10 = 94 ± 9%) are mostly in the submicron range. These particles were mainly composed of organics containing non-polar saturated and unsaturated hydrocarbons (e.g. asphalting: O:C < 0.01, H:C = 2.01). Besides construction activities, mineral dust is also emitted over cleared land by wind-driven resuspension depending on wind speed. PM10 emissions by construction activities often result in local concentrations > 100 μg m-3 and can easily breach the European limit level of PM10. This study also shows that particulate mineral

  3. Internal energy dissipation of gamma-ray bursts observed with Swift: Precursors, prompt gamma-rays, extended emission, and late X-ray flares

    SciTech Connect

    Hu, You-Dong; Liang, En-Wei; Xi, Shao-Qiang; Peng, Fang-Kun; Lu, Rui-Jing; Lü, Lian-Zhong; Zhang, Bing E-mail: Zhang@physics.unlv.edu

    2014-07-10

    We jointly analyze the gamma-ray burst (GRB) data observed with Burst Alert Telescope (BAT) and X-ray Telescope on board the Swift mission to present a global view on the internal energy dissipation processes in GRBs, including precursors, prompt gamma-ray emission, extended soft gamma-ray emission, and late X-ray flares. The Bayesian block method is utilized to analyze the BAT light curves to identify various emission episodes. Our results suggest that these emission components likely share the same physical origin, which is the repeated activation of the GRB central engine. What we observe in the gamma-ray band may be a small part of more extended underlying activities. The precursor emission, which is detected in about 10% of Swift GRBs, is preferably detected in those GRBs that have a massive star core-collapse origin. The soft extended emission tail, on the other hand, is preferably detected in those GRBs that have a compact star merger origin. Bright X-ray emission is detected during the BAT quiescent phases prior to subsequent gamma-ray peaks, implying that X-ray emission may be detectable prior the BAT trigger time. Future GRB alert instruments with soft X-ray capability are essential for revealing the early stages of GRB central engine activities, and shedding light on jet composition and the jet launching mechanism in GRBs.

  4. Intermediate Volatility Organic Compound Emissions from On-Road Diesel Vehicles: Chemical Composition, Emission Factors, and Estimated Secondary Organic Aerosol Production.

    PubMed

    Zhao, Yunliang; Nguyen, Ngoc T; Presto, Albert A; Hennigan, Christopher J; May, Andrew A; Robinson, Allen L

    2015-10-01

    Emissions of intermediate-volatility organic compounds (IVOCs) from five on-road diesel vehicles and one off-road diesel engine were characterized during dynamometer testing. The testing evaluated the effects of driving cycles, fuel composition and exhaust aftertreatment devices. On average, more than 90% of the IVOC emissions were not identified on a molecular basis, instead appearing as an unresolved complex mixture (UCM) during gas-chromatography mass-spectrometry analysis. Fuel-based emissions factors (EFs) of total IVOCs (speciated + unspeciated) depend strongly on aftertreatment technology and driving cycle. Total-IVOC emissions from vehicles equipped with catalyzed diesel particulate filters (DPF) are substantially lower (factor of 7 to 28, depending on driving cycle) than from vehicles without any exhaust aftertreatment. Total-IVOC emissions from creep and idle operations are substantially higher than emissions from high-speed operations. Although the magnitude of the total-IVOC emissions can vary widely, there is little variation in the IVOC composition across the set of tests. The new emissions data are combined with published yield data to investigate secondary organic aerosol (SOA) formation. SOA production from unspeciated IVOCs is estimated using surrogate compounds, which are assigned based on gas-chromatograph retention time and mass spectral signature of the IVOC UCM. IVOCs contribute the vast majority of the SOA formed from exhaust from on-road diesel vehicles. The estimated SOA production is greater than predictions by previous studies and substantially higher than primary organic aerosol. Catalyzed DPFs substantially reduce SOA formation potential of diesel exhaust, except at low speed operations.

  5. Intermediate Volatility Organic Compound Emissions from On-Road Diesel Vehicles: Chemical Composition, Emission Factors, and Estimated Secondary Organic Aerosol Production.

    PubMed

    Zhao, Yunliang; Nguyen, Ngoc T; Presto, Albert A; Hennigan, Christopher J; May, Andrew A; Robinson, Allen L

    2015-10-01

    Emissions of intermediate-volatility organic compounds (IVOCs) from five on-road diesel vehicles and one off-road diesel engine were characterized during dynamometer testing. The testing evaluated the effects of driving cycles, fuel composition and exhaust aftertreatment devices. On average, more than 90% of the IVOC emissions were not identified on a molecular basis, instead appearing as an unresolved complex mixture (UCM) during gas-chromatography mass-spectrometry analysis. Fuel-based emissions factors (EFs) of total IVOCs (speciated + unspeciated) depend strongly on aftertreatment technology and driving cycle. Total-IVOC emissions from vehicles equipped with catalyzed diesel particulate filters (DPF) are substantially lower (factor of 7 to 28, depending on driving cycle) than from vehicles without any exhaust aftertreatment. Total-IVOC emissions from creep and idle operations are substantially higher than emissions from high-speed operations. Although the magnitude of the total-IVOC emissions can vary widely, there is little variation in the IVOC composition across the set of tests. The new emissions data are combined with published yield data to investigate secondary organic aerosol (SOA) formation. SOA production from unspeciated IVOCs is estimated using surrogate compounds, which are assigned based on gas-chromatograph retention time and mass spectral signature of the IVOC UCM. IVOCs contribute the vast majority of the SOA formed from exhaust from on-road diesel vehicles. The estimated SOA production is greater than predictions by previous studies and substantially higher than primary organic aerosol. Catalyzed DPFs substantially reduce SOA formation potential of diesel exhaust, except at low speed operations. PMID:26322746

  6. Effects of emission reductions on organic aerosol in the southeastern United States

    NASA Astrophysics Data System (ADS)

    Blanchard, C. L.; Hidy, G. M.; Shaw, S.; Baumann, K.; Edgerton, E. S.

    2016-01-01

    Long-term (1999 to 2013) data from the Southeastern Aerosol Research and Characterization (SEARCH) network are used to show that anthropogenic emission reductions led to important decreases in fine-particle organic aerosol (OA) concentrations in the southeastern US On average, 45 % (range 25 to 63 %) of the 1999 to 2013 mean organic carbon (OC) concentrations are attributed to combustion processes, including fossil fuel use and biomass burning, through associations of measured OC with combustion products such as elemental carbon (EC), carbon monoxide (CO), and nitrogen oxides (NOx). The 2013 mean combustion-derived OC concentrations were 0.5 to 1.4 µg m-3 at the five sites operating in that year. Mean annual combustion-derived OC concentrations declined from 3.8 ± 0.2 µg m-3 (68 % of total OC) to 1.4 ± 0.1 µg m-3 (60 % of total OC) between 1999 and 2013 at the urban Atlanta, Georgia, site (JST) and from 2.9 ± 0.4 µg m-3 (39 % of total OC) to 0.7 ± 0.1 µg m-3 (30 % of total OC) between 2001 and 2013 at the urban Birmingham, Alabama (BHM), site. The urban OC declines coincide with reductions of motor vehicle emissions between 2006 and 2010, which may have decreased mean OC concentrations at the urban SEARCH sites by > 2 µg m-3. BHM additionally exhibits a decline in OC associated with SO2 from 0.4 ± 0.04 µg m-3 in 2001 to 0.2 ± 0.03 µg m-3 in 2013, interpreted as the result of reduced emissions from industrial sources within the city. Analyses using non-soil potassium as a biomass burning tracer indicate that biomass burning OC occurs throughout the year at all sites. All eight SEARCH sites show an association of OC with sulfate (SO4) ranging from 0.3 to 1.0 µg m-3 on average, representing ˜ 25 % of the 1999 to 2013 mean OC concentrations. Because the mass of OC identified with SO4 averages 20 to 30 % of the SO4 concentrations, the mean SO4-associated OC declined by ˜ 0.5 to 1 µg m-3 as SO4 concentrations decreased throughout the SEARCH region. The

  7. Effects of emission reductions on organic aerosol in the southeastern United States

    NASA Astrophysics Data System (ADS)

    Blanchard, C. L.; Hidy, G. M.; Shaw, S.; Baumann, K.; Edgerton, E. S.

    2015-06-01

    Long-term (1999 to 2013) data from the Southeastern Aerosol Research and Characterization (SEARCH) network are used to characterize the effects of anthropogenic emission reductions on fine particle organic aerosol (OA) concentrations in the southeastern US. On average, 45 % (range 25 to 63 %) of the 1999 to 2013 mean organic carbon (OC) concentrations are attributed to combustion processes, including fossil-fuel use and biomass burning, through associations of measured OC with combustion products such as elemental carbon (EC), carbon monoxide (CO), and nitrogen oxides (NOx). The 2013 mean combustion-derived OC concentrations were 0.5 to 1.4 μg m-3 at the five sites operating in that year. Mean annual combustion-derived OC concentrations declined from 3.8 ± 0.2 μg m-3 (68 % of total OC) to 1.4 ± 0.1 μg m-3 (60 % of total OC) between 1999 and 2013 at the urban Atlanta, Georgia, site (JST) and from 2.9 ± 0.4 μg m-3 (39 % of total OC) to 0.7 ± 0.1 μg m-3 (30 % of total OC) between 2001 and 2013 at the urban Birmingham, Alabama, site (BHM). The urban OC declines coincide with reductions of motor-vehicle emissions between 2006 and 2010, which may have decreased mean OC concentrations at the urban SEARCH sites by > 2 μg m-3. BHM additionally exhibits a decline in OC associated with SO2 from 0.4 ± 0.04 μg m-3 in 2001 to 0.2 ± 0.03 μg m-3 in 2013, interpreted as the result of reduced emissions from industrial sources within the city. Analyses using non-soil potassium as a biomass-burning tracer indicate that biomass-burning OC occurs throughout the year at all sites. All eight SEARCH sites show an association of OC with sulfate (SO4) ranging from 0.3 to 1.0 μg m-3 on average, representing ~ 25 % of the 1999 to 2013 mean OC concentrations. Because the mass of OC associated with SO4 averages 20 to 30 % of the SO4 concentrations, the mean SO4-associated OC declined by ~ 0.5 to 1 μg m-3 as SO4 decreased throughout the SEARCH region. The 2013 mean SO4

  8. The impact of biogenic carbon emissions on aerosol absorption inMexico City

    SciTech Connect

    Marley, N; Gaffney, J; Tackett, M J; Sturchio, N; Hearty, L; Martinez, N; Hardy, K D; Machany-Rivera, A; Guilderson, T P; MacMillan, A; Steelman, K

    2009-02-24

    In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbing secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.

  9. Effect of Hydrophobic Primary Organic Aerosols on Secondary Organic Aerosol Formation from Ozonolysis of α-Pinene

    SciTech Connect

    Song, Chen; Zaveri, Rahul A.; Alexander, M. Lizabeth; Thornton, Joel A.; Madronich, Sasha; Ortega, John V.; Zelenyuk, Alla; Yu, Xiao-Ying; Laskin, Alexander; Maughan, A. D.

    2007-10-16

    Semi-empirical secondary organic aerosol (SOA) models typically assume a well-mixed organic aerosol phase even in the presence of hydrophobic primary organic aerosols (POA). This assumption significantly enhances the modeled SOA yields as additional organic mass is made available to absorb greater amounts of oxidized secondary organic gases than otherwise. We investigate the applicability of this critical assumption by measuring SOA yields from ozonolysis of α-pinene (a major biogenic SOA precursor) in a smog chamber in the absence and in the presence of dioctyl phthalate (DOP) and lubricating oil seed aerosol. These particles serve as surrogates for urban hydrophobic POA. The results show that these POA did not enhance the SOA yields. If these results are found to apply to other biogenic SOA precursors, then the semi-empirical models used in many global models would predict significantly less biogenic SOA mass and display reduced sensitivity to anthropogenic POA emissions than previously thought.

  10. Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter.

    PubMed

    Sandradewi, Jisca; Prévôt, Andre S H; Szidat, Sönke; Perron, Nolwenn; Alfarra, M Rami; Lanz, Valentin A; Weingartner, Ernest; Baltensperger, Urs

    2008-05-01

    A source apportionment study was performed for particulate matter in the small village of Roveredo, Switzerland, where more than 70% of the households use wood burning for heating purposes. A two-lane trans-Alpine highway passes through the village and contributes to the total aerosol burden in the area. The village is located in a steep Alpine valley characterized by strong and persistent temperature inversions during winter, especially from December to February. During two winter and one early spring campaigns, a seven-wavelength aethalometer, high volume (HIVOL) samplers, an Aerodyne quadrupole aerosol mass spectrometer (AMS), an optical particle counter (OPC), and a Sunset Laboratory OCEC analyzer were deployed to study the contribution of wood burning and traffic aerosols to particulate matter. A linear regression model of the carbonaceous particulate mass in the submicrometer size range CM(PM1) as a function of aerosol light absorption properties measured by the aethalometer is introduced to estimate the particulate mass from wood burning and traffic (PM(wb), PM(traffic)). This model was calibrated with analyses from the 14C method using HIVOL filter measurements. These results indicate that light absorption exponents of 1.1 for traffic and 1.8-1.9 for wood burning calculated from the light absorption at 470 and 950 nanometers should be used to obtain agreement of the two methods regarding the relative wood burning and traffic emission contributions to CM(PM1) and also to black carbon. The resulting PM(wb) and PM(traffic) values explain 86% of the variance of the CM(PM1) and contribute, on average, 88 and 12% to CM(PM1), respectively. The black carbon is estimated to be 51% due to wood burning and 49% due to traffic emissions. The average organic carbon/total carbon (OC/TC) values were estimated to be 0.52 for traffic and 0.88 for wood burning particulate emissions.

  11. Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

    2014-02-01

    Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as directly in the exhaust plumes of individual heavy-duty (HD) diesel trucks. BC emission factor distributions for HD trucks were more skewed than OA distributions, with the highest 10% of trucks accounting for 56 and 42% of total measured BC and OA emissions, respectively. A comparison of measured OA and BC mass spectra across various sampling periods revealed a high degree of similarity in BC and OA emitted by gasoline and diesel engines. Cycloalkanes predominate in exhaust OA emissions relative to saturated alkanes (i.e., normal and iso-paraffins), suggesting that lubricating oil rather than fuel is the dominant source of primary organic aerosol (POA) emissions in diesel vehicle exhaust. This finding is supported by the detection of trace elements such as zinc and phosphorus in the exhaust plumes of individual trucks. Trace elements were emitted relative to total OA at levels that are consistent with typical weight fractions of commonly used additives present in lubricating oil. The presence of trace elements in vehicle exhaust raises the concern that ash deposits may accumulate over time in diesel particle filter systems, and may eventually lead to performance problems that require servicing.

  12. Spatial variations in immediate greenhouse gases and aerosol emissions and resulting radiative forcing from wildfires in interior Alaska

    NASA Astrophysics Data System (ADS)

    Huang, Shengli; Liu, Heping; Dahal, Devendra; Jin, Suming; Li, Shuang; Liu, Shuguang

    2016-02-01

    Boreal fires can cool the climate; however, this conclusion came from individual fires and may not represent the whole story. We hypothesize that the climatic impact of boreal fires depends on local landscape heterogeneity such as burn severity, prefire vegetation type, and soil properties. To test this hypothesis, spatially explicit emission of greenhouse gases (GHGs) and aerosols and their resulting radiative forcing are required as an important and necessary component towards a full assessment. In this study, we integrated remote sensing (Landsat and MODIS) and models (carbon consumption model, emission factors model, and radiative forcing model) to calculate the carbon consumption, GHGs and aerosol emissions, and their radiative forcing of 2001-2010 fires at 30 m resolution in the Yukon River Basin of Alaska. Total carbon consumption showed significant spatial variation, with a mean of 2,615 g C m-2 and a standard deviation of 2,589 g C m-2. The carbon consumption led to different amounts of GHGs and aerosol emissions, ranging from 593.26 Tg (CO2) to 0.16 Tg (N2O). When converted to equivalent CO2 based on global warming potential metric, the maximum 20 years equivalent CO2 was black carbon (713.77 Tg), and the lowest 20 years equivalent CO2 was organic carbon (-583.13 Tg). The resulting radiative forcing also showed significant spatial variation: CO2, CH4, and N2O can cause a 20-year mean radiative forcing of 7.41 W m-2 with a standard deviation of 2.87 W m-2. This emission forcing heterogeneity indicates that different boreal fires have different climatic impacts. When considering the spatial variation of other forcings, such as surface shortwave forcing, we may conclude that some boreal fires, especially boreal deciduous fires, can warm the climate.

  13. Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

    2014-07-01

    Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as directly in the exhaust plumes of individual heavy-duty (HD) diesel trucks. BC emission factor distributions for HD trucks were more skewed than OA distributions (N = 293), with the highest 10% of trucks accounting for 56 and 42% of total measured BC and OA emissions, respectively. OA mass spectra measured for HD truck exhaust plumes show cycloalkanes are predominate in exhaust OA emissions relative to saturated alkanes (i.e., normal and iso-paraffins), suggesting that lubricating oil rather than fuel is the dominant source of primary organic aerosol (POA) emissions in diesel vehicle exhaust. This finding is supported by the detection of trace elements such as zinc and phosphorus in the exhaust plumes of individual trucks. Trace elements were emitted relative to total OA at levels that are consistent with typical weight fractions of commonly used additives present in lubricating oil. A comparison of measured OA and BC mass spectra across various sampling periods revealed a high degree of similarity in OA and BC emitted by gasoline and diesel engines. This finding indicates a large fraction of OA in gasoline exhaust is lubricant-derived as well. The similarity in OA and BC mass spectra for gasoline and diesel engine exhaust is likely to confound ambient source apportionment efforts to determine contributions to air pollution from these two important sources.

  14. Plutonium-aerosol emission rates and human pulmonary deposition calculations for Nuclear Site 201, Nevada Test Site

    SciTech Connect

    Shinn, J.H.; Homan, D.N.

    1982-06-21

    This study determined the plutonium-aerosol fluxes from the soil to quantify (1) the extent of potential human exposure by deep-lung retention of alpha-emitting particles; (2) the source term should there be any significant, long-term, transport of plutonium aerosols; and (3) the resuspension factor and rate so that, for the first time at any nuclear site, one may calculate how long it will take for wind erosion to carry away a significant amount of the contaminated soil. High-volume air samplers and cascade impactors were used to characterize the plutonium aerosols. Meteorological flux-profile methods were used to calculate dust and plutonium aerosol emission rates. A floorless wind tunnel (10-m long) was used to examine resuspension under steady-state, high wind speed. The resuspension factor was two orders of magnitude lower than the other comparable sites at NTS and elsewhere, and the average resuspension rate of 5.3 x 10/sup -8//d was also very low, so that the half-time for resuspension by wind erosion was about 36,000 y.

  15. Estimating the influence of the secondary organic aerosols on present climate using ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    O'Donnell, D.; Tsigaridis, K.; Feichter, J.

    2011-01-01

    In recent years, several field measurement campaigns have highlighted the importance of the organic fraction of aerosol mass, and with such spatial diversity that one may assert that these aerosols are ubiquitous in the troposphere, with particular importance in continental areas. Investigation of the chemical composition of organic aerosol remains a work in progress, but it is now clear that a significant portion of the total organic mass is composed of secondary organic material, that is, aerosol chemically formed from gaseous volatile organic carbon (VOC) precursors. A number of such precursors, of both biogenic and anthropogenic origin, have been identified. Experimental, inventory building and modelling studies have followed. Laboratory studies have yielded information on the chemical pathways that lead to secondary organic aerosol (SOA) formation, and provided the means to estimate the aerosol yields from a given precursor-oxidant reaction. Global inventories of anthropogenic VOC emissions, and of biogenic VOC emitter species distribution and their emission potential have been constructed. Models have been developed that provide global estimates of precursor VOC emissions, SOA formation and atmospheric burdens of these species. This paper estimates the direct and indirect effects of these aerosols using the global climate-aerosol model ECHAM5-HAM. For year 2000 conditions, we estimate a global annual mean shortwave (SW) aerosol direct effect due to SOA of -0.3 W m-2. The model predicts a positive SW indirect effect due to SOA amounting to +0.23 W m-2, arising from enlargement of particles due to condensation of SOA, together with an enhanced coagulation sink for small particles. Longwave effects are small. Finally, we indicate of areas of research into SOA that are required in order to better constrain our estimates of the influence of aerosols on the climate system.

  16. A new description of Titan's aerosol optical properties from the analysis of VIMS Emission Phase Function observations

    NASA Astrophysics Data System (ADS)

    Rodriguez, Sebastien; Maltagliati, Luca; Sotin, Christophe; Rannou, Pascal; Bézard, Bruno; Cornet, Thomas

    2016-10-01

    The Huygens probe gave unprecedented information on the properties of Titan's aerosols (vertical distribution, opacity as a function of wavelength, phase function, single scattering albedo) by in-situ measurements (Tomasko et al. 2008). Being the only existing in-situ atmospheric probing for Titan, this aerosol model currently is the reference for many Titan studies (e.g. by being applied as physical input in radiative transfer models of the atmosphere). Recently a reanalysis of the DISR dataset, corroborated by data from the Downward-Looking Visible Spectrometer (DLVS), was carried out by the same group (Doose et al. 2016), leading to significant changes to the indications given by Tomasko et al. (2008).Here we present the analysis of the Emission Phase Function observation (EPF) performed by VIMS during the Cassini flyby T88 (November 2012). An EPF observes the same spot on the surface (and thus the same atmosphere) with the same emergence angle but with different incidence angles. In this way, our EPF allows, for the first time, to have direct information on the phase function of Titan's aerosols, as well as on other important physical parameters of the aerosols as the behavior of their extinction as a function of wavelength and the single scattering albedo (also as a function of wavelength) for the whole VIMS range (0.8-5.2 μm). The T88 EPF is composed of 25 VIMS datacubes spanning a scattering angle range approximately from 0°to 70°.We used the radiative transfer model described in Hirtzig et al. (2013) as baseline, updated with improved methane (+ related isotopes) spectroscopy. By changing the aerosol description in the model, we found the combination of aerosol optical parameters that fits best a constant aerosol column density over the whole set of the VIMS datacubes. We confirmed that the new results from Doose et al. (2016) do improve the fit for what concerns the vertical profile and the extinction as a function of wavelength. However, a different

  17. A new description of Titan's aerosol optical properties from the analysis of VIMS Emission Phase Function observations

    NASA Astrophysics Data System (ADS)

    Maltagliati, Luca; Rodriguez, Sebastien; Sotin, Christophe; Rannou, Pascal; Bezard, Bruno; Cornet, Thomas

    2016-06-01

    The Huygens probe gave unprecedented information on the properties of Titan's aerosols (vertical distribution, opacity as a function of wavelength, phase function, single scattering albedo) by in-situ measurements (Tomasko et al. 2008). Being the only existing in-situ atmospheric probing for Titan, this aerosol model currently is the reference for many Titan studies (e.g. by being applied as physical input in radiative transfer models of the atmosphere). Recently a reanalysis of the DISR dataset, corroborated by data from the Downward-Looking Visible Spectrometer (DLVS), was carried out by the same group (Doose et al. 2016), leading to significant changes to the indications given by Tomasko et al. (2008). Here we present the analysis of the Emission Phase Function observation (EPF) performed by VIMS during the Cassini flyby T88 (November 2012). An EPF observes the same spot on the surface (and thus the same atmosphere) with the same emergence angle but with different incidence angles. In this way, our EPF allows, for the first time, to have direct information on the phase function of Titan's aerosols, as well as on other important physical parameters of the aerosols as the behavior of their extinction as a function of wavelength and the single scattering albedo (also as a function of wavelength) for the whole VIMS range (0.8-5.2 µm). The T88 EPF is composed of 25 VIMS datacubes spanning a scattering angle range approximately from 0°to 70°. We used the radiative transfer model described in Hirtzig et al. (2013) as baseline, updated with improved methane (+ related isotopes) spectroscopy. By changing the aerosol description in the model, we found the combination of aerosol optical parameters that fits best a constant aerosol column density over the whole set of the VIMS datacubes. We confirmed that the new results from Doose et al. (2016) do improve the fit for what concerns the vertical profile and the extinction as a function of wavelength. However, a different

  18. Black carbon in aerosol during BIBLE B

    NASA Astrophysics Data System (ADS)

    Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

    2002-02-01

    The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

  19. Black carbon in aerosol during BIBLE B

    NASA Astrophysics Data System (ADS)

    Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

    2003-02-01

    The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

  20. Towards the regulation of aerosol emissions by their potential health impact: Assessing adverse effects of aerosols from wood combustion and ship diesel engine emissions by combining comprehensive data on the chemical composition and their toxicological effects on human lung cells

    NASA Astrophysics Data System (ADS)

    Zimmermann, R.; Streibel, T.; Dittmar, G.; Kanashova, T.; Buters, J.; Öder, S.; Paur, H. R.; Dilger, M.; Weiss, C.; Harndorf, H.; Stengel, B.; Hirvonen, M. R.; Jokiniemi, J.; Hiller, K.; Sapcariu, S.; Sippula, O.; Orasche, J.; Müller, L.; Rheda, A.; Passig, J.; Radischat, C.; Czech, H.; Tiita, P.; Jalava, P.; Kasurinen, S.; Schwemer, T.; Yli-Prilä, P.; Tissari, J.; Lamberg, H.; Schnelle-Kreis, J.

    2014-12-01

    Ship engine emissions are important regarding lung and cardiovascular diseases in coastal regions worldwide. Bio mass burning is made responsible for adverse health effects in many cities and rural regions. The Virtual Helmholtz Institute-HICE (www.hice-vi.eu) addresses chemical & physical properties and health effects of anthropogenic combustion emissions. Typical lung cell responses to combustion aerosols include inflammation and apoptosis, but a molecular link with the specific chemical composition in particular of ship emissions has not been established. Through an air-liquid interface exposure system (ALI), we exposed human lung cells at-site to exhaust fumes from a ship engine running on common heavy fuel oil (HFO) and cleaner-burning diesel fuel (DF) as well as to emissions of wood combustion compliances. A special field deployable ALI-exposition system and a mobile S2-biological laboratory were developed for this study. Human alveolar basal epithelial cells (A549 etc.) are ALI-exposed to fresh, diluted (1:40-1:100) combustion aerosols and subsequently were toxicologically and molecular-biologically characterized. Advanced chemical analyses of the exhaust aerosols were combined with transcriptional, proteomic and metabolomic profiling to characterise the cellular responses. The HFO ship emissions contained high concentrations of toxic compounds (transition metals, organic toxicants) and particle masses. The cellular responses included inflammation and oxidative stress. Surprisingly, the DF ship emissions, which predominantly contain rather "pure" carbonaceous soot and much less known toxicants, induced significantly broader biological effects, affecting essential cellular pathways (e.g., mitochondrial function and intracellular transport). Therefore the use of distillate fuels for shipping (this is the current emission reduction strategy of the IMO) appears insufficient for diminishing health effects. The study suggests rather reducing the particle emissions

  1. Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

    DOE PAGES

    Zhou, Shan; Collier, Sonya; Xu, Jianzhong; Mei, Fan; Wang, Jian; Lee, Yin -Nan; Sedlacek, III, Arthur J.; Springston, Stephen R.; Sun, Yele; Zhang, Qi

    2016-05-19

    Continuous real-time measurements of atmospheric aerosol with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the Department of Energy Aerosol Life Cycle Intensive Operational Period campaign. BNL was frequently downwind of emissions from the New York metropolitan area and was exposed to various combinations of anthropogenic, biogenic, and marine emissions based on air mass history. The average concentration of submicrometer aerosol (PM1) during this study was 12.6 µg m–3 with 64% of the mass being organic. Organic aerosol (OA) at BNLmore » was found to be overwhelmingly secondary, consisting of (1) a fresher, semivolatile oxygenated organic aerosol (SV-OOA; oxygen-to-carbon ratio (O/C) = 0.54; 63% of OA mass) that was strongly influenced by transported urban plumes; (2) a regional, more aged, low-volatility OOA (LV-OOA; O/C = 0.97; 29% of OA mass) influenced by aqueous-phase processing; and (3) a nitrogen-enriched OA (NOA; nitrogen-to-carbon ratio (N/C) = 0.185; 8% of OA mass) likely composed of amine salts formed from acid-base reactions in industrial emissions. Urban emissions from the New York metropolitan areas to the W and SW in particular led to elevated PM1 mass concentration and altered aerosol composition at BNL. Transported urban plumes and local biogenic emissions likely interacted to enhance secondary organic aerosol production, primarily represented by SV-OOA. Lastly, these results suggest an important role that urban anthropogenic emissions play in affecting ambient PM concentration, composition, and physical-chemical properties at rural areas in the Northeast U.S.« less

  2. Primary emissions and secondary organic aerosol formation from the exhaust of a flex-fuel (ethanol) vehicle

    NASA Astrophysics Data System (ADS)

    Suarez-Bertoa, R.; Zardini, A. A.; Platt, S. M.; Hellebust, S.; Pieber, S. M.; El Haddad, I.; Temime-Roussel, B.; Baltensperger, U.; Marchand, N.; Prévôt, A. S. H.; Astorga, C.

    2015-09-01

    Incentives to use biofuels may result in increasing vehicular emissions of compounds detrimental to air quality. Therefore, regulated and unregulated emissions from a Euro 5a flex-fuel vehicle, tested using E85 and E75 blends (gasoline containing 85% and 75% of ethanol (vol/vol), respectively), were investigated at 22 and -7 °C over the New European Driving Cycle, at the Vehicle Emission Laboratory at the European Commission Joint Research Centre Ispra, Italy. Vehicle exhaust was comprehensively analyzed at the tailpipe and in a dilution tunnel. A fraction of the exhaust was injected into a mobile smog chamber to study the photochemical aging of the mixture. We found that emissions from a flex-fuel vehicle, fueled by E85 and E75, led to secondary organic aerosol (SOA) formation, despite the low aromatic content of these fuel blends. Emissions of regulated and unregulated compounds, as well as emissions of black carbon (BC) and primary organic aerosol (POA) and SOA formation were higher at -7 °C. The flex-fuel unregulated emissions, mainly composed of ethanol and acetaldehyde, resulted in very high ozone formation potential and SOA, especially at low temperature (860 mg O3 km-1 and up to 38 mg C kg-1). After an OH exposure of 10 × 106 cm-3 h, SOA mass was, on average, 3 times larger than total primary particle mass emissions (BC + POA) with a high O:C ratio (up to 0.7 and 0.5 at 22 and -7 °C, respectively) typical of highly oxidized mixtures. Furthermore, high resolution organic mass spectra showed high 44/43 ratios (ratio of the ions m/z 44 and m/z 43) characteristic of low-volatility oxygenated organic aerosol. We also hypothesize that SOA formation from vehicular emissions could be due to oxidation products of ethanol and acetaldehyde, both short-chain oxygenated VOCs, e.g. methylglyoxal and acetic acid, and not only from aromatic compounds.

  3. Effects of alkylate fuel on exhaust emissions and secondary aerosol formation of a 2-stroke and a 4-stroke scooter

    NASA Astrophysics Data System (ADS)

    Zardini, Alessandro A.; Platt, Stephen M.; Clairotte, Michael; El Haddad, Imad; Temime-Roussel, Brice; Marchand, Nicolas; Ježek, Irena; Drinovec, Luka; Močnik, Griša; Slowik, Jay G.; Manfredi, Urbano; Prévôt, André S. H.; Baltensperger, Urs; Astorga, Covadonga

    2014-09-01

    Regulated and unregulated emissions from a 2-stroke and a 4-stroke scooter were characterized during a legislative driving cycle in a certified laboratory. Scooter exhaust was analyzed at the tailpipe, in a dilution tunnel, and partly collected in a mobile smog chamber for photochemical ageing. We present evidence that the photochemically aged exhaust from a 2-stroke and a 4-stroke scooter produces considerable amounts of secondary organic aerosol: from 1.5 to 22.0 mg/km, and from 5.5 to 6.6 mg/km, respectively. Tests were repeated after replacing the standard petrol and synthetic lube oil with an alkylate fuel (with low content of aromatic compounds) and ultra-clean lube oil (low ash forming potential). We observed emission reduction (with some exceptions) for several gaseous and particulate phase species, in particular for carbon monoxide (from 8% up to 38% and from 31% to 50%, for the 2-stroke and the 4-stroke scooters, respectively), particulate mass (from 32% up to 75% for the 2-stroke scooter), aromatic compounds (89% and 97% for the 2-stroke and the 4-stroke scooter, respectively), and secondary organic aerosol (from 87% to 100% and 99% for the 2-stroke and the 4-stroke scooters, respectively). We attribute the organic aerosol reduction to the low content of aromatics in the alkylate fuel.

  4. Further evidence for charge transfer complexes in brown carbon aerosols from excitation-emission matrix fluorescence spectroscopy.

    PubMed

    Phillips, Sabrina M; Smith, Geoffrey D

    2015-05-14

    The light-absorbing fraction of organic molecules in ambient aerosols, known as "brown carbon," is an important yet poorly characterized component. Despite the fact that brown carbon could alter the radiative forcing of aerosols significantly, identification of specific chromophores has remained challenging. We recently demonstrated that charge transfer (CT) complexes formed in organic molecules could be responsible for a large fraction of absorption observed in water-extracted ambient particulate matter.1 In the present study, we use excitation-emission matrix fluorescence spectroscopy to further corroborate the importance of CT complexes in defining aerosol optical properties. Monotonically increasing and decreasing quantum yields, decreasing Stokes shifts, and red-shifting emission maxima are observed from ambient particulate matter collected in Athens, Georgia, strongly suggesting that a superposition of independent chromophores is not sufficient to explain brown carbon absorption and fluorescence. Instead, we show that a model in which such chromophores are energetically coupled to a dense manifold of CT complexes is consistent with all of the observations. Further, we suggest that a significant fraction of the observed fluorescence originates from CT complexes and that their contribution to brown carbon absorption is likely greater than we reported previously.

  5. A global emission inventory of carbonaceous aerosol from historic records of fossil fuel and biofuel consumption for the period 1860-1997

    NASA Astrophysics Data System (ADS)

    Junker, C.; Liousse, C.

    2006-06-01

    Country by country emission inventories for carbonaceous aerosol for the period 1860 to 1997 have been constructed on the basis of historic fuel production, use and trade data sets published by the United Nation's Statistical Division UNSTAT (1997), Etemad et al. (1991) and Mitchell (1992, 1993, 1995). The inventories use emission factors variable over time, which have been determined according to changes in technological development. The results indicate that the industrialisation period since 1860 was accompanied by a steady increase in black carbon (BC) and organic carbon (OC) emissions up to 1910. The calculations show a moderate decrease of carbonaceous aerosol emissions between 1920 and 1930, followed by an increase up to 1990, the year when emissions began to decrease again. Changes in BC and OC emissions prior to the year 1950 are essentially driven by the USA, Germany and the UK. The USSR, China and India become substantial contributors to carbonaceous aerosol emissions after 1950. Emission maps have been generated with a 1°×1° resolution based on the relative population density in each country. They will provide a helpful tool for assessing the effect of carbonaceous aerosol emissions on observed climate changes of the past.

  6. A global emission inventory of carbonaceous aerosol from historic records of fossil fuel and biofuel consumption for the period 1860-1997

    NASA Astrophysics Data System (ADS)

    Junker, C.; Liousse, C.

    2008-03-01

    Country by country emission inventories for carbonaceous aerosol for the period 1860 to 1997 have been constructed on the basis of historic fuel production, use and trade data sets published by the United Nation's Statistical Division UNSTAT (1997), Etemad et al. (1991) and Mitchell (1992, 1993, 1995). The inventories use emission factors variable over time, which have been determined according to changes in technological development. The results indicate that the industrialisation period since 1860 was accompanied by a steady increase in black carbon (BC) and primary organic carbon (POC) emissions up to 1910. The calculations show a moderate decrease of carbonaceous aerosol emissions between 1920 and 1930, followed by an increase up to 1990, the year when emissions began to decrease again. Changes in BC and POC emissions prior to the year 1950 are essentially driven by the USA, Germany and the UK. The USSR, China and India become substantial contributors to carbonaceous aerosol emissions after 1950. Emission maps have been generated with a 1°×1° resolution based on the relative population density in each country. They will provide a helpful tool for assessing the effect of carbonaceous aerosol emissions on observed climate changes of the past.

  7. Fast oxidation processes from emission to ambient air introduction of aerosol emitted by residential log wood stoves

    NASA Astrophysics Data System (ADS)

    Nalin, Federica; Golly, Benjamin; Besombes, Jean-Luc; Pelletier, Charles; Aujay-Plouzeau, Robin; Verlhac, Stéphane; Dermigny, Adrien; Fievet, Amandine; Karoski, Nicolas; Dubois, Pascal; Collet, Serge; Favez, Olivier; Albinet, Alexandre

    2016-10-01

    Little is known about the impact of post-combustion processes, condensation and dilution, on the aerosol concentration and chemical composition from residential wood combustion. The evolution of aerosol emitted by two different residential log wood stoves (old and modern technologies) from emission until it is introduced into ambient air was studied under controlled "real" conditions. The first objective of this research was to evaluate the emission factors (EF) of polycyclic aromatic hydrocarbons (PAH) and their nitrated and oxygenated derivatives from wood combustion. These toxic substances are poorly documented in the literature. A second objective was to evaluate the oxidation state of the wood combustion effluent by studying these primary/secondary compounds. EFs of Σ37PAHs and Σ27Oxy-PAHs were in the same range and similar to those reported in literature (4-240 mg kg-1). Σ31Nitro-PAH EFs were 2-4 orders of magnitude lower (3.10-2-8.10-2 mg kg-1) due to the low temperature and low emission of NO2 from wood combustion processes. An increase of equivalent EF of PAH derivatives was observed suggesting that the oxidation state of the wood combustion effluent from the emission point until its introduction in ambient air changed in a few seconds. These results were confirmed by the study of both, typical compounds of SOA formation from PAH oxidation and, PAH ratio-ratio plots commonly used for source evaluation.

  8. Megacity emission plume characteristics in summer and winter investigated by mobile aerosol and trace gas measurements: the Paris metropolitan area

    NASA Astrophysics Data System (ADS)

    von der Weiden-Reinmüller, S.-L.; Drewnick, F.; Zhang, Q. J.; Freutel, F.; Beekmann, M.; Borrmann, S.

    2014-12-01

    For the investigation of megacity emission plume characteristics mobile aerosol and trace gas measurements were carried out in the greater Paris region in July 2009 and January-February 2010 within the EU FP7 MEGAPOLI project (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation). The deployed instruments measured physical and chemical properties of sub-micron aerosol particles, gas phase constituents of relevance for urban air pollution studies and meteorological parameters. The emission plume was identified based on fresh pollutant (e.g., particle-bound polycyclic aromatic hydrocarbons, black carbon, CO2 and NOx) concentration changes in combination with wind direction data. The classification into megacity influenced and background air masses allowed a characterization of the emission plume during summer and winter environmental conditions. On average, a clear increase of fresh pollutant concentrations in plume compared to background air masses was found for both seasons. For example, an average increase of 190% (+ 8.8 ng m-3) in summer and of 130% (+ 18.1 ng m-3) in winter was found for particle-bound polycyclic aromatic hydrocarbons in plume air masses. The aerosol particle size distribution in plume air masses was influenced by nucleation and growth due to coagulation and condensation in summer, while in winter only the latter process (i.e., particle growth) seemed to be initiated by urban pollution. The observed distribution of fresh pollutants in the emission plume - its cross sectional Gaussian-like profile and the exponential decrease of pollutant concentrations with increasing distance to the megacity - are in agreement with model results. Differences between model and measurements were found for plume center location, plume width and axial plume extent. In general, dilution was identified as the dominant process determining the axial variations within the Paris

  9. Evolved gas analysis of secondary organic aerosols

    SciTech Connect

    Grosjean, D.; Williams, E.L. II; Grosjean, E. ); Novakov, T. )

    1994-11-01

    Secondary organic aerosols have been characterized by evolved gas analysis (EGA). Hydrocarbons selected as aerosol precursors were representative of anthropogenic emissions (cyclohexene, cyclopentene, 1-decene and 1-dodecene, n-dodecane, o-xylene, and 1,3,5-trimethylbenzene) and of biogenic emissions (the terpenes [alpha]-pinene, [beta]-pinene and d-limonene and the sesquiterpene trans-caryophyllene). Also analyzed by EGA were samples of secondary, primary (highway tunnel), and ambient (urban) aerosols before and after exposure to ozone and other photochemical oxidants. The major features of the EGA thermograms (amount of CO[sub 2] evolved as a function of temperature) are described. The usefulness and limitations of EGA data for source apportionment of atmospheric particulate carbon are briefly discussed. 28 refs., 7 figs., 4 tabs.

  10. Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

    SciTech Connect

    Setyan, Ari; Zhang, Qi; Merkel, M.; Knighton, Walter B.; Sun, Y.; Song, Chen; Shilling, John E.; Onasch, Timothy B.; Herndon, Scott C.; Worsnop, Douglas R.; Fast, Jerome D.; Zaveri, Rahul A.; Berg, Larry K.; Wiedensohler, A.; Flowers, B. A.; Dubey, Manvendra K.; Subramanian, R.

    2012-09-11

    The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project ({approx}40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 {micro}gm{sup -3} on average) and dominated by organics (80% of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at {approx}400nm in vacuum aerodynamic diameter (Dva), and a condensation mode at {approx}150 nm, while organics generally displayed a broad distribution in 60-600nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a nominal formula of C{sub 1}H{sub 1.38}N{sub 0.004}O{sub 0.44}, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90% of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly

  11. Assessing the nonlinear response of fine particles to precursor emissions: Development and application of an extended response surface modeling technique v1.0

    DOE PAGES

    Zhao, B.; Wang, S. X.; Xing, J.; Fu, K.; Fu, J. S.; Jang, C.; Zhu, Y.; Dong, X. Y.; Gao, Y.; Wu, W. J.; et al

    2015-01-30

    An innovative extended response surface modeling technique (ERSM v1.0) is developed to characterize the nonlinear response of fine particles (PM₂̣₅) to large and simultaneous changes of multiple precursor emissions from multiple regions and sectors. The ERSM technique is developed based on the conventional response surface modeling (RSM) technique; it first quantifies the relationship between PM₂̣₅ concentrations and the emissions of gaseous precursors from each single region using the conventional RSM technique, and then assesses the effects of inter-regional transport of PM₂̣₅ and its gaseous precursors on PM₂̣₅ concentrations in the target region. We apply this novel technique with a widelymore » used regional chemical transport model (CTM) over the Yangtze River delta (YRD) region of China, and evaluate the response of PM₂̣₅ and its inorganic components to the emissions of 36 pollutant–region–sector combinations. The predicted PM₂̣₅ concentrations agree well with independent CTM simulations; the correlation coefficients are larger than 0.98 and 0.99, and the mean normalized errors (MNEs) are less than 1 and 2% for January and August, respectively. It is also demonstrated that the ERSM technique could reproduce fairly well the response of PM₂̣₅ to continuous changes of precursor emission levels between zero and 150%. Employing this new technique, we identify the major sources contributing to PM₂̣₅ and its inorganic components in the YRD region. The nonlinearity in the response of PM₂̣₅ to emission changes is characterized and the underlying chemical processes are illustrated.« less

  12. Assessing the nonlinear response of fine particles to precursor emissions: Development and application of an extended response surface modeling technique v1.0

    SciTech Connect

    Zhao, B.; Wang, S. X.; Xing, J.; Fu, K.; Fu, J. S.; Jang, C.; Zhu, Y.; Dong, X. Y.; Gao, Y.; Wu, W. J.; Wang, J. D.; Hao, J. M.

    2015-01-30

    An innovative extended response surface modeling technique (ERSM v1.0) is developed to characterize the nonlinear response of fine particles (PM₂̣₅) to large and simultaneous changes of multiple precursor emissions from multiple regions and sectors. The ERSM technique is developed based on the conventional response surface modeling (RSM) technique; it first quantifies the relationship between PM₂̣₅ concentrations and the emissions of gaseous precursors from each single region using the conventional RSM technique, and then assesses the effects of inter-regional transport of PM₂̣₅ and its gaseous precursors on PM₂̣₅ concentrations in the target region. We apply this novel technique with a widely used regional chemical transport model (CTM) over the Yangtze River delta (YRD) region of China, and evaluate the response of PM₂̣₅ and its inorganic components to the emissions of 36 pollutant–region–sector combinations. The predicted PM₂̣₅ concentrations agree well with independent CTM simulations; the correlation coefficients are larger than 0.98 and 0.99, and the mean normalized errors (MNEs) are less than 1 and 2% for January and August, respectively. It is also demonstrated that the ERSM technique could reproduce fairly well the response of PM₂̣₅ to continuous changes of precursor emission levels between zero and 150%. Employing this new technique, we identify the major sources contributing to PM₂̣₅ and its inorganic components in the YRD region. The nonlinearity in the response of PM₂̣₅ to emission changes is characterized and the underlying chemical processes are illustrated.

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

    PubMed

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

    2015-04-21

    A fuel-based approach is used to assess long-term trends (1970-2010) in mobile source emissions of black carbon (BC) and organic aerosol (OA, including both primary emissions and secondary formation). The main focus of this analysis is the Los Angeles Basin, where a long record of measurements is available to infer trends in ambient concentrations of BC and organic carbon (OC), with OC used here as a proxy for OA. Mobile source emissions and ambient concentrations have decreased similarly, reflecting the importance of on- and off-road engines as sources of BC and OA in urban areas. In 1970, the on-road sector accounted for ∼90% of total mobile source emissions of BC and OA (primary + secondary). Over time, as on-road engine emissions have been controlled, the relative importance of off-road sources has grown. By 2010, off-road engines were estimated to account for 37 ± 20% and 45 ± 16% of total mobile source contributions to BC and OA, respectively, in the Los Angeles area. This study highlights both the success of efforts to control on-road emission sources, and the importance of considering off-road engine and other VOC source contributions when assessing long-term emission and ambient air quality trends. PMID:25793355

  14. Sesquiterpene emissions from loblolly pine and their potential contribution to biogenic aerosol formation in the Southeastern US

    NASA Astrophysics Data System (ADS)

    Helmig, Detlev; Ortega, John; Guenther, Alex; Herrick, Jeffrey D.; Geron, Chris

    Sesquiterpene (SQT) and montoterpene (MT) emissions from loblolly pine ( Pinus taeda L.) were studied by branch enclosure experiments at Duke Forest in Chapel Hill, NC. Four SQT ( β-caryophyllene, α-bergamotene, α-humulene, β-farnesene), five MT ( α-pinene, β-pinene, β-myrcene, β-phellandrene, limonene), and the oxygenated MT linalool were identified. Emission rates of both compound classes increased exponentially with temperature, albeit SQT temperature coefficients (0.12-0.18 K -1) were higher than for MT (0.068-0.15 K -1), resulting in an increased contribution of SQT to the overall biogenic volatile organic compound (BVOC) flux during warm temperature conditions. The highly correlated variables of light and temperature conditions preclude a rigorous characterization of their individual roles in driving these emissions. However, the observations indicate that there may be both temperature-only and temperature/light-dependent components contributing to SQT emission variations. When normalized to 30 °C using the best-fit temperature algorithm, total SQT basal emission rate was 450 ng g -1 h -1. The potential contribution of SQT from all pine trees (based on the loblolly pine emission factors) to secondary, biogenic organic aerosol in 12 southeastern US states was estimated to be 7×10 6 kg for the month of September which constitutes an appreciable portion of the overall PM 2.5 emission budget.

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

    PubMed

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

    2015-04-21

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

  16. Megacity emission plume characteristics in summer and winter investigated by mobile aerosol and trace gas measurements: the Paris metropolitan area

    NASA Astrophysics Data System (ADS)

    von der Weiden-Reinmüller, S.-L.; Drewnick, F.; Zhang, Q. J.; Freutel, F.; Beekmann, M.; Borrmann, S.

    2014-05-01

    For the investigation of megacity emission plume characteristics mobile aerosol and trace gas measurements were carried out in the greater Paris region in July 2009 and January/February 2010 within the EU FP7 MEGAPOLI project. The deployed instruments measured physical and chemical properties of sub-micron aerosol particles, gas phase constituents of relevance for urban air pollution studies and meteorological parameters. The emission plume was identified based on fresh pollutant (e.g. particle-bound polycyclic aromatic hydrocarbons, black carbon, CO2 and NOx) concentration changes in combination with wind direction data. The classification into megacity influenced and background air masses allowed a characterization of the emission plume during summer and winter environmental conditions. On average, a clear increase of fresh pollutant concentrations in plume compared to background air masses was found for both seasons. For example, an average increase of 190% (+8.8 ng m-3) in summer and of 130% (+18.1 ng m-3) in winter was found for particle-bound polycyclic aromatic hydrocarbons in plume air masses. The aerosol particle size distribution in plume air masses was influenced by nucleation and growth due to coagulation and condensation in summer, while in winter only the second process seemed to be initiated by urban pollution. The observed distribution of fresh pollutants in the emission plume - its cross sectional Gaussian-like profile and the exponential decrease of pollutant concentrations with increasing distance to the megacity - are in agreement with model results. Differences between model and measurements were found for plume center location, plume width and axial plume extent. In general, dilution was identified as the dominant process determining the axial variations within the Paris emission plume. For in-depth analysis of transformation processes occurring in the advected plume, simultaneous measurements at a suburban measurement site and a stationary

  17. Satellite perspective of aerosol intercontinental transport: From qualitative tracking to quantitative characterization

    NASA Astrophysics Data System (ADS)

    Yu, Hongbin; Remer, Lorraine A.; Kahn, Ralph A.; Chin, Mian; Zhang, Yan

    2013-04-01

    Evidence of aerosol intercontinental transport (ICT) is both widespread and compelling. Model simulations suggest that ICT could significantly affect regional air quality and climate, but the broad inter-model spread of results underscores a need of constraining model simulations with measurements. Satellites have inherent advantages over in situ measurements to characterize aerosol ICT, because of their spatial and temporal coverage. Significant progress in satellite remote sensing of aerosol properties during the Earth Observing System (EOS) era offers the opportunity to increase quantitative characterization and estimates of aerosol ICT beyond the capability of pre-EOS era satellites that could only qualitatively track aerosol plumes. EOS satellites also observe emission strengths and injection heights of some aerosols, aerosol precursors, and aerosol-related gases, which can help characterize aerosol ICT. We review how the current generation of satellite measurements have been used to (1) characterize the evolution of aerosol plumes (e.g., both horizontal and vertical transport, and properties) on an episodic basis, (2) understand the seasonal and inter-annual variations of aerosol ICT and their control factors, (3) estimate the export and import fluxes of aerosols, and (4) evaluate and constrain model simulations. Substantial effort is needed to further explore an integrated approach using measurements from on-orbit satellites (e.g., A-Train synergy) for observational characterization and model constraint of aerosol intercontinental transport and to develop advanced sensors for future missions.

  18. Satellite Perspective of Aerosol Intercontinental Transport: From Qualitative Tracking to Quantitative Characterization

    NASA Technical Reports Server (NTRS)

    Yu, Hongbin; Remer, Lorraine A.; Kahn, Ralph A.; Chin, Mian; Zhang, Yan

    2012-01-01

    Evidence of aerosol intercontinental transport (ICT) is both widespread and compelling. Model simulations suggest that ICT could significantly affect regional air quality and climate, but the broad inter-model spread of results underscores a need of constraining model simulations with measurements. Satellites have inherent advantages over in situ measurements to characterize aerosol ICT, because of their spatial and temporal coverage. Significant progress in satellite remote sensing of aerosol properties during the Earth Observing System (EOS) era offers opportunity to increase quantitative characterization and estimates of aerosol ICT, beyond the capability of pre-EOS era satellites that could only qualitatively track aerosol plumes. EOS satellites also observe emission strengths and injection heights of some aerosols, aerosol precursors, and aerosol-related gases, which can help characterize aerosol ICT. After an overview of these advances, we review how the current generation of satellite measurements have been used to (1) characterize the evolution of aerosol plumes (e.g., both horizontal and vertical transport, and properties) on an episodic basis, (2) understand the seasonal and inter-annual variations of aerosol ICT and their control factors, (3) estimate the export and import fluxes of aerosols, and (4) evaluate and constrain model simulations. Substantial effort is needed to further explore an integrated approach using measurements from on-orbit satellites (e.g., A-Train synergy) for observational characterization and model constraint of aerosol intercontinental transport and to develop advanced sensors for future missions.

  19. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

    DOE PAGES

    Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

    2016-05-02

    The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) andmore » an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m−3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C  =  0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C  =  0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C  =  0.33; BBOA2: 20 % of total OA, O / C  =  0.60) most likely

  20. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

    NASA Astrophysics Data System (ADS)

    Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

    2015-12-01

    The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. Aerosol Mass Spectrometer (HR-ToF-AMS) and an Ionicon Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 μg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi

  1. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

    NASA Astrophysics Data System (ADS)

    Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

    2016-05-01

    The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno-Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C = 0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C = 0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C = 0.33; BBOA2: 20 % of total OA, O / C = 0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV

  2. Toxicological Evaluation of Realistic Emission Source Aerosols (TERESA)—Power plant studies: assessment of breathing pattern

    PubMed Central

    Diaz, Edgar A.; Lemos, Miriam; Coull, Brent; Long, Mark S.; Rohr, Annette C.; Ruiz, Pablo; Gupta, Tarun; Kang, Choong-Min; Godleski, John J.

    2013-01-01

    Our approach to study multi-pollutant aerosols isolates a single emissions source, evaluates the toxicity of primary and secondary particles derived from this source, and simulates chemical reactions that occur in the atmosphere after emission. Three U.S. coal-fired power plants utilizing different coals and with different emission controls were evaluated. Secondary organic aerosol (SOA) derived from α-pinene and/or ammonia was added in some experiments. Male Sprague-Dawley rats were exposed for 6 h to filtered air or different atmospheric mixtures. Scenarios studied at each plant included the following: primary particles (P); secondary (oxidized) particles (PO); oxidized particles + SOA (POS); and oxidized and neutralized particles + SOA (PONS); additional control scenarios were also studied. Continuous respiratory data were obtained during exposures using whole body plethysmography chambers. Of the 12 respiratory outcomes assessed, each had statistically significant changes at some plant and with some of the 4 scenarios. The most robust outcomes were found with exposure to the PO scenario (increased respiratory frequency with decreases in inspiratory and expiratory time); and the PONS scenario (decreased peak expiratory flow and expiratory flow at 50%). PONS findings were most strongly associated with ammonium, neutralized sulfate, and elemental carbon (EC) in univariate analyses, but only with EC in multivariate analyses. Control scenario O (oxidized without primary particles) had similar changes to PO. Adjusted R2 analyses showed that scenario was a better predictor of respiratory responses than individual components, suggesting that the complex atmospheric mixture was responsible for respiratory effects. PMID:21639693

  3. The economics and ethics of aerosol geoengineering strategies

    NASA Astrophysics Data System (ADS)

    Goes, Marlos; Keller, Klaus; Tuana, Nancy

    2010-05-01

    Anthropogenic greenhouse gas emissions are changing the Earth's climate and impose substantial risks for current and future generations. What are scientifically sound, economically viable, and ethically defendable strategies to manage these climate risks? Ratified international agreements call for a reduction of greenhouse gas emissions to avoid dangerous anthropogenic interference with the climate system. Recent proposals, however, call for a different approach: geoengineering climate by injecting aerosol precursors into the stratosphere. Published economic studies typically neglect the risks of aerosol geoengineering due to (i) a potential failure to sustain the aerosol forcing and (ii) due to potential negative impacts associated with aerosol forcings. Here we use a simple integrated assessment model of climate change to analyze potential economic impacts of aerosol geoengineering strategies over a wide range of uncertain parameters such as climate sensitivity, the economic damages due to climate change, and the economic damages due to aerosol geoengineering forcings. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes considerable caveats. For example, the analysis is based on a globally aggregated model and is hence silent on intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of future learning and is based on a simple representation of climate change impacts. We use this integrated assessment model to show three main points. First, substituting aerosol geoengineering for the reduction of greenhouse gas emissions can fail the test of economic efficiency. One key to this finding is that a failure to sustain the aerosol forcing can lead to sizeable and abrupt climatic changes. The monetary damages due to such a discontinuous aerosol geoengineering can dominate the cost-benefit analysis because the monetary damages of climate change are expected to increase with

  4. Production-based emissions, consumption-based emissions and consumption-based health impacts of PM2.5 carbonaceous aerosols in Asia

    NASA Astrophysics Data System (ADS)

    Takahashi, Kei; Nansai, Keisuke; Tohno, Susumu; Nishizawa, Masato; Kurokawa, Jun-ichi; Ohara, Toshimasa

    2014-11-01

    This study determined the production-based emissions, the consumption-based emissions, and the consumption-based health impact of primary carbonaceous aerosols (black carbon: BC, organic carbon: OC) in nine countries and regions in Asia (Indonesia, Malaysia, the Philippines, Singapore, Thailand, China, Taiwan, South Korea, and Japan) in 2008. For the production-based emissions, sectoral emissions inventory of BC and OC for the year of 2008 based on the Asian international input-output tables (AIIOT) was compiled including direct emissions from households. Then, a multiregional environmental input-output analysis with the 2008 AIIOT which was originally developed by updating the table of 2000 was applied for calculating the consumption-based emissions for each country and region. For the production-based emissions, China had the highest BC and OC emissions of 4520 Gg-C in total, which accounted for 75% of the total emissions in the nine countries and regions. For consumption-based emissions, China was estimated to have had a total of 4849 Gg-C of BC and OC emissions, which accounted for 77% of the total emissions in the Asia studied. We also quantified how much countries and regions induced emissions in other countries and regions. Furthermore, taking account of the source-receptor relationships of BC and OC among the countries and regions, we converted their consumption-based emissions into the consumption-based health impact of each country and region. China showed the highest consumption-based health impact of BC and OC totaling 111 × 103 premature deaths, followed by Indonesia, Japan, Thailand and South Korea. China accounted for 87% of the sum total of the consumption-based health impacts of the countries/regions, indicating that China's contribution to consumption-based health impact in Asia was greater than its consumption-based emissions. By elucidating the health impacts that each country and region had on other countries and from which country the impacts

  5. Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

    NASA Technical Reports Server (NTRS)

    Diehl, Thomas L.; Chin, Mian; Bond, Tami C.; Carn, SImon A.; Duncan, Bryan N.; Krotkov, Nickolay A.; Streets, David G.

    2006-01-01

    The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthropogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ASTR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

  6. Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

    NASA Technical Reports Server (NTRS)

    Diehl, T. L.; Mian, Chin; Bond, T. C.; Carn, S. A.; Duncan, B. N.; Krotkov, N. A.; Streets, D. G.

    2007-01-01

    The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthopogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ATSR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

  7. Fossil Fuel Combustion-Related Emissions Dominate Atmospheric Ammonia Sources during Severe Haze Episodes: Evidence from (15)N-Stable Isotope in Size-Resolved Aerosol Ammonium.

    PubMed

    Pan, Yuepeng; Tian, Shili; Liu, Dongwei; Fang, Yunting; Zhu, Xiaying; Zhang, Qiang; Zheng, Bo; Michalski, Greg; Wang, Yuesi

    2016-08-01

    The reduction of ammonia (NH3) emissions is urgently needed due to its role in aerosol nucleation and growth causing haze formation during its conversion into ammonium (NH4(+)). However, the relative contributions of individual NH3 sources are unclear, and debate remains over whether agricultural emissions dominate atmospheric NH3 in urban areas. Based on the chemical and isotopic measurements of size-resolved aerosols in urban Beijing, China, we find that the natural abundance of (15)N (expressed using δ(15)N values) of NH4(+) in fine particles varies with the development of haze episodes, ranging from -37.1‰ to -21.7‰ during clean/dusty days (relative humidity: ∼ 40%), to -13.1‰ to +5.8‰ during hazy days (relative humidity: 70-90%). After accounting for the isotope exchange between NH3 gas and aerosol NH4(+), the δ(15)N value of the initial NH3 during hazy days is found to be -14.5‰ to -1.6‰, which indicates fossil fuel-based emissions. These emissions contribute 90% of the total NH3 during hazy days in urban Beijing. This work demonstrates the analysis of δ(15)N values of aerosol NH4(+) to be a promising new tool for partitioning atmospheric NH3 sources, providing policy makers with insights into NH3 emissions and secondary aerosols for regulation in urban environments. PMID:27359161

  8. Fossil Fuel Combustion-Related Emissions Dominate Atmospheric Ammonia Sources during Severe Haze Episodes: Evidence from (15)N-Stable Isotope in Size-Resolved Aerosol Ammonium.

    PubMed

    Pan, Yuepeng; Tian, Shili; Liu, Dongwei; Fang, Yunting; Zhu, Xiaying; Zhang, Qiang; Zheng, Bo; Michalski, Greg; Wang, Yuesi

    2016-08-01

    The reduction of ammonia (NH3) emissions is urgently needed due to its role in aerosol nucleation and growth causing haze formation during its conversion into ammonium (NH4(+)). However, the relative contributions of individual NH3 sources are unclear, and debate remains over whether agricultural emissions dominate atmospheric NH3 in urban areas. Based on the chemical and isotopic measurements of size-resolved aerosols in urban Beijing, China, we find that the natural abundance of (15)N (expressed using δ(15)N values) of NH4(+) in fine particles varies with the development of haze episodes, ranging from -37.1‰ to -21.7‰ during clean/dusty days (relative humidity: ∼ 40%), to -13.1‰ to +5.8‰ during hazy days (relative humidity: 70-90%). After accounting for the isotope exchange between NH3 gas and aerosol NH4(+), the δ(15)N value of the initial NH3 during hazy days is found to be -14.5‰ to -1.6‰, which indicates fossil fuel-based emissions. These emissions contribute 90% of the total NH3 during hazy days in urban Beijing. This work demonstrates the analysis of δ(15)N values of aerosol NH4(+) to be a promising new tool for partitioning atmospheric NH3 sources, providing policy makers with insights into NH3 emissions and secondary aerosols for regulation in urban environments.

  9. Simulation of Climate Forcing by Aerosols

    SciTech Connect

    Ghan, Steven J.; Bian, Xindi; Chapman, Elaine G.; Easter, Richard C.; Fann, George I.; Kothari, Suraj C.; Zaveri, Rahul A.; Zhang, Yang

    2004-05-03

    The largest source of uncertainty in estimates of the radiative forcing governing climate change is in the radiative forcing due to anthropogenic aerosols. Current estimates of the global mean of the aerosol radiative forcing range from –0.3 to –3.0 watts per square meter (Wm-2 ) which is opposite in sign and possibly comparable in magnitude to the +2 Wm-2 forcing due to increasing greenhouse gases. We have developed a global aerosol and climate modeling system that provides arguably the most detailed treatment of aerosols and their impact on the planetary radiation balance of any model, but our estimates of radiative forcing have been hindered by our lack of access to high performance computing resources. We propose to use the MSCF to conduct a series of simulations with and without emissions of a variety of aerosol particles and aerosol precursors. These extensive simulations will enable us to produce much more refined estimates of the impact of anthropogenic emissions on radiative forcing of climate change. To take full advantage of the parallelism available on the MSCF MPP1, we will apply the Global Array Toolkit to dynamically load balance the reactive chemistry component of our model. We will adapt our modifications of the serial NCAR Community Climate Model CCM2 to the parallel NCAR CCM3.10.

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

    NASA Astrophysics Data System (ADS)

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

    2013-09-01

    A series of smog chamber experiments were conducted to investigate the transformation of primary organic aerosol (POA) and formation of secondary organic aerosol (SOA) during the photo-oxidation of dilute gasoline and diesel motor vehicle exhaust. In half of the experiments POA was present in the chamber at the onset of photo-oxidation. In these experiments positive matrix factorization (PMF) was used to determine separate POA and SOA factors from aerosol mass spectrometer data. A two-factor solution, with one POA factor and one SOA factor, was sufficient to describe the organic aerosol in all but one experiment. In the other half of the experiments, POA was not present at the onset of photo-oxidation; these experiments are considered "pure SOA" experiments. The POA mass spectrum was similar to the mass spectra of the hydrocarbon-like organic aerosol factor determined from ambient datasets with one exception, a diesel vehicle equipped with a diesel oxidation catalyst. The SOA in all experiments had a constant composition over the course of photo-oxidation, and did not appear to age with continued oxidation. The SOA mass spectra for the various gasoline and diesel vehicles were similar to each other, but markedly different than ambient oxidized organic aerosol factors. Van Krevelen analysis of the POA and SOA factors for gasoline and diesel experiments reveal slopes of -0.68 and -0.43, respectively. This suggests that the oxidation chemistry in these experiments is a combination of carboxylic acid and alcohol/peroxide formation, consistent with ambient oxidation chemistry. These experiments also provide insight to the mixing behavior of the POA and SOA. Analysis of the time series of the POA factor concentration and a basis-set model both indicate that for all but one of the vehicles tested here, the POA and SOA seem to mix and form a single organic aerosol phase.

  11. Lead isotopes in trade wind aerosols at Barbados: the influence of European emissions over the North Atlantic

    SciTech Connect

    Hamelin, B.; Grousset, F.E.; Biscaye, P.E.; Zindler, A. ); Prospero, J.M. )

    1989-11-15

    Previous studies have shown that Pb can be used as a transient tracer in the atmosphere and the ocean because of strong time-variability of industrial inputs and because Pb isotopic composition can be used to identify contribution from different sources. We present Pb isotopic measurements on aerosols collected from the North Atlantic Ocean in the trade wind belt. Aerosols sampled at Barbados during the 1969--1985 period have a Pb isotopic compositions different from that observed by previous investigators in Bermuda corals and Sargasso Sea waters. Barbados aerosols appear to contain significant amounts of relatively unradiogenic industrial and automotive Pb that is derived from Europe and carried to Barbados by the trade winds. In contrast, Bermuda corals and Sargasso sea waters are influenced mainly by U.S.-derived emissions, which contain more radiogenic Pb originating from Missouri-type ores. This difference generates a strong latitudinal Europe-U.S.A. isotopic gradient, thus allowing study of trans-Atlantic atmospheric transport and ocean mixing processes. {copyright} American Geophysical Union 1989

  12. Lead isotopes in trade wind aerosols at Barbados - The influence of European emissions over the North Atlantic

    NASA Technical Reports Server (NTRS)

    Hamelin, B.; Grousset, F. E.; Biscaye, P. E.; Zindler, A.; Prospero, J. M.

    1989-01-01

    Previous studies have shown that Pb can be used as a transient tracer in the atmosphere and the ocean because of strong time-variability of industrial inputs and because Pb isotopic composition can be used to identify contributions from different sources. Pb isotopic measurements on aerosols collected from the North Atlantic Ocean in the trade wind belt are presented. Aerosols sampled at Barbados during the 1969-1985 period have a Pb isotopic composition different from that observed by previous investigators in Bermuda corals and Sargasso Sea waters. Barbados aerosols appear to contain significant amounts of relatively unradiogenic industrial and automotive Pb that is derived from Europe and carried to Barbados by the trade winds. In contrast, Bermuda corals and Sargasso sea waters are influenced mainly by U.S.-derived emissions, which contain more radiogenic Pb originating from Missouri-type ores. This difference generates a strong latitudinal Europe-U.S.A. isotopic gradient, thus allowing study of trans-Atlantic atmospheric transport and ocean mixing processes.

  13. TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

    SciTech Connect

    Annette Rohr

    2006-03-01

    TERESA (Toxicological Evaluation of Realistic Emissions of Source Aerosols) involves exposing laboratory rats to realistic coal-fired power plant and mobile source emissions to help determine the relative toxicity of these PM sources. There are three coal-fired power plants in the TERESA program; this report describes the results of fieldwork conducted at the first plant, located in the Upper Midwest. The project was technically challenging by virtue of its novel design and requirement for the development of new techniques. By examining aged, atmospherically transformed aerosol derived from power plant stack emissions, we were able to evaluate the toxicity of PM derived from coal combustion in a manner that more accurately reflects the exposure of concern than existing methodologies. TERESA also involves assessment of actual plant emissions in a field setting--an important strength since it reduces the question of representativeness of emissions. A sampling system was developed and assembled to draw emissions from the stack; stack sampling conducted according to standard EPA protocol suggested that the sampled emissions are representative of those exiting the stack into the atmosphere. Two mobile laboratories were then outfitted for the study: (1) a chemical laboratory in which the atmospheric aging was conducted and which housed the bulk of the analytical equipment; and (2) a toxicological laboratory, which contained animal caging and the exposure apparatus. Animal exposures were carried out from May-November 2004 to a number of simulated atmospheric scenarios. Toxicological endpoints included (1) pulmonary function and breathing pattern; (2) bronchoalveolar lavage fluid cytological and biochemical analyses; (3) blood cytological analyses; (4) in vivo oxidative stress in heart and lung tissue; and (5) heart and lung histopathology. Results indicated no differences between exposed and control animals in any of the endpoints examined. Exposure concentrations for the

  14. The use of satellite-measured aerosol optical depth to constrain biomass burning emissions source strength in a global model GOCART

    NASA Astrophysics Data System (ADS)

    Petrenko, Mariya

    Biomass burning (BB) is one of the major contributors to emissions of carbonaceous atmospheric aerosol. Optically and chemically potent BB particles play important roles in atmospheric processes through their impact on air quality, visibility, human health, and as one of the factors affecting global climate through direct and indirect radiative effects. As chemistry transport models are among the major tools for studying earth and atmospheric processes, it is important to represent BB processes as accurately as possible. Simulations of BB emissions in aerosol models strongly depend on the inventories that define emission source locations and strength. In this work, we use 13 global biomass burning emission estimates, including widely used Global Fire Emission Database (GFED) monthly and daily versions, Fire Radiative Power (FRP)-based Quick Fire Emission Dataset QFED, and several combinations of fuel consumption estimates, aerosol emission factors and Moderate Resolution Imaging Spectroradiometer (MODIS)-based burned area products as alternative inputs to the global Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. The resultant simulated aerosol optical depth (AOD) and its spatial distributions are compared to AOD snapshots measured by the MODIS instrument for 124 fire events occurring between 2006 and 2007. BB aerosol emission estimates by all 13 emission options are compared on a global scale and implications of regional differences are discussed. Performance of all emission options, with the exception of FRP-based QFED, when used as a source of BB emissions in the GOCART model, were assessed on a regional basis, showing where and to what degree the different options overestimate, underestimate and provide good agreement with the observation. QFED developers use MODIS AOD as one of the parameters to calibrate their product during its production, so comparison of QFED-based GOCART-simulated AOD with MODIS measurements was not performed. It is also

  15. Optical Properties and Mixing State of Aerosols from Residential Wood Burning and Vehicle Emissions in Central and Southern California

    NASA Astrophysics Data System (ADS)

    Zhang, X.; Cappa, C. D.; Collier, S.; Zhang, Q.; Williams, L. R.; Lee, A.; Abbatt, J.; Russell, L. M.; Liu, J.; Chen, C. L.; Betha, R.

    2015-12-01

    Light-absorbing materials such as black carbon (BC) and brown carbon (BrC) in atmospheric aerosols play important roles in regulating the earth's radiative budget and climate. However, the representations of BC and BrC in state-of-the-art climate models remain highly uncertain, in part due to the poor understanding of their microphysical and optical properties. Direct observations and characterizations of the mixing state and absorption enhancement of ambient aerosols could provide invaluable constraints for current model representations of aerosol radiative effects. Here, we will discuss results from measurements of aerosol light absorption and absorption enhancement (Eabs), using a thermodenuder-absorption method, made during two recent field studies in central and southern California. The winter study took place in Dec/Jan of 2014/2015 in Fresno, CA. This region is severely impacted by particulate matter from local and regional residential biomass burning. The summer study took place in July 2015 in Fontana, CA, a region ~80 km downwind of Los Angeles and strongly impacted by vehicular emissions, and thus provides a sharp contrast to the Fresno study. Eabs of BC particles due to the "lensing" effect from coatings to BC core and/or the presence of BrC will be quantified and compared between the two studies. Additionally, the chemical composition of bulk and the BC-containing particles are determined via a HR-ToF-AMS and a SP-AMS, respectively. Variations in the composition and mixing state of the ambient particles and how these affect the observed Eabs will be examined. The overall measurements suggest a relatively small role for lensing-induced absorption enhancements for ambient particles in these regions.

  16. The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions

    NASA Astrophysics Data System (ADS)

    Guenther, A. B.; Jiang, X.; Heald, C. L.; Sakulyanontvittaya, T.; Duhl, T.; Emmons, L. K.; Wang, X.

    2012-11-01

    The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1) is a modeling framework for estimating fluxes of biogenic compounds between terrestrial ecosystems and the atmosphere using simple mechanistic algorithms to account for the major known processes controlling biogenic emissions. It is available as an offline code and has also been coupled into land surface and atmospheric chemistry models. MEGAN2.1 is an update from the previous versions including MEGAN2.0, which was described for isoprene emissions by Guenther et al. (2006) and MEGAN2.02, which was described for monoterpene and sesquiterpene emissions by Sakulyanontvittaya et al. (2008). Isoprene comprises about half of the total global biogenic volatile organic compound (BVOC) emission of 1 Pg (1000 Tg or 1015 g) estimated using MEGAN2.1. Methanol, ethanol, acetaldehyde, acetone, α-pinene, β-pinene, t-β-ocimene, limonene, ethene, and propene together contribute another 30% of the MEGAN2.1 estimated emission. An additional 20 compounds (mostly terpenoids) are associated with the MEGAN2.1 estimates of another 17% of the total emission with the remaining 3% distributed among >100 compounds. Emissions of 41 monoterpenes and 32 sesquiterpenes together comprise about 15% and 3%, respectively, of the estimated total global BVOC emission. Tropical trees cover about 18% of the global land surface and are estimated to be responsible for ~80% of terpenoid emissions and ~50% of other VOC emissions. Other trees cover about the same area but are estimated to contribute only about 10% of total emissions. The magnitude of the emissions estimated with MEGAN2.1 are within the range of estimates reported using other approaches and much of the differences between reported values can be attributed to land cover and meteorological driving variables. The offline version of MEGAN2.1 source code and driving variables is available from

  17. The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions

    NASA Astrophysics Data System (ADS)

    Guenther, A. B.; Jiang, X.; Heald, C. L.; Sakulyanontvittaya, T.; Duhl, T.; Emmons, L. K.; Wang, X.

    2012-06-01

    The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1) is a modeling framework for estimating fluxes of 147 biogenic compounds between terrestrial ecosystems and the atmosphere using simple mechanistic algorithms to account for the major known processes controlling biogenic emissions. It is available as an offline code and has also been coupled into land surface models and atmospheric chemistry models. MEGAN2.1 is an update from the previous versions including MEGAN2.0 for isoprene emissions and MEGAN2.04, which estimates emissions of 138 compounds. Isoprene comprises about half of the estimated total global biogenic volatile organic compound (BVOC) emission of 1 Pg (1000 Tg or 1015 g). Another 10 compounds including methanol, ethanol, acetaldehyde, acetone, α-pinene, β-pinene, t-β-ocimene, limonene, ethene, and propene together contribute another 30% of the estimated emission. An additional 20 compounds (mostly terpenoids) are associated with another 17% of the total emission with the remaining 3% distributed among 125 compounds. Emissions of 41 monoterpenes and 32 sesquiterpenes together comprise about 15% and 3%, respectively, of the total global BVOC emission. Tropical trees cover about 18% of the global land surface and are estimated to be responsible for 60% of terpenoid emissions and 48% of other VOC emissions. Other trees cover about the same area but are estimated to contribute only about 10% of total emissions. The magnitude of the emissions estimated with MEGAN2.1 are within the range of estimates reported using other approaches and much of the differences between reported values can be attributed to landcover and meteorological driving variables. The offline version of MEGAN2.1 source code and driving variables is available from http://acd.ucar.edu/~guenther/MEGAN/MEGAN.htm and the version integrated into the Community Land Model version 4 (CLM4) can

  18. Spatial variations in immediate greenhouse gases and aerosol emissions and resulting radiative forcing from wildfires in interior Alaska

    USGS Publications Warehouse

    Huang, Shengli; Liu, Heping; Dahal, Devendra; Jin, Suming; Li, Shuang; Liu, Shu-Guang

    2016-01-01

    Boreal fires can cool the climate; however, this conclusion came from individual fires and may not represent the whole story. We hypothesize that the climatic impact of boreal fires depends on local landscape heterogeneity such as burn severity, prefire vegetation type, and soil properties. To test this hypothesis, spatially explicit emission of greenhouse gases (GHGs) and aerosols and their resulting radiative forcing are required as an important and necessary component towards a full assessment. In this study, we integrated remote sensing (Landsat and MODIS) and models (carbon consumption model, emission factors model, and radiative forcing model) to calculate the carbon consumption, GHGs and aerosol emissions, and their radiative forcing of 2001–2010 fires at 30 m resolution in the Yukon River Basin of Alaska. Total carbon consumption showed significant spatial variation, with a mean of 2,615 g C m−2 and a standard deviation of 2,589 g C m−2. The carbon consumption led to different amounts of GHGs and aerosol emissions, ranging from 593.26 Tg (CO2) to 0.16 Tg (N2O). When converted to equivalent CO2 based on global warming potential metric, the maximum 20 years equivalent CO2 was black carbon (713.77 Tg), and the lowest 20 years equivalent CO2 was organic carbon (−583.13 Tg). The resulting radiative forcing also showed significant spatial variation: CO2, CH4, and N2O can cause a 20-year mean radiative forcing of 7.41 W m−2 with a standard deviation of 2.87 W m−2. This emission forcing heterogeneity indicates that different boreal fires have different climatic impacts. When considering the spatial variation of other forcings, such as surface shortwave forcing, we may conclude that some boreal fires, especially boreal deciduous fires, can warm the climate.

  19. Impact of the March 2009 dust event in Saudi Arabia on aerosol optical properties, meteorological parameters, sky temperature and emissivity

    NASA Astrophysics Data System (ADS)

    Maghrabi, A.; Alharbi, B.; Tapper, N.

    2011-04-01

    On 10th March 2009 a widespread and severe dust storm event that lasted several hours struck Riyadh, and represented one of the most intense dust storms experienced in Saudi Arabia in the last two decades. This short-lived storm caused widespread and heavy dust deposition, zero visibility and total airport shutdown, as well as extensive damage to buildings, vehicles, power poles and trees across the city of Riyadh. Changes in Meteorological parameters, aerosol optical depth (AOD), Angstrom exponent α, infrared (IR) sky temperature and atmospheric emissivity were investigated before, during, and after the storm. The analysis showed significant changes in all of the above parameters due to this event. Shortly after the storm arrived, air pressure rapidly increased by 4 hPa, temperature decreased by 6 °C, relative humidly increased from 10% to 30%, the wind direction became northerly and the wind speed increased to a maximum of 30 m s -1. AOD at 550 nm increased from 0.396 to 1.71. The Angstrom exponent α rapidly decreased from 0.192 to -0.078. The mean AOD at 550 nm on the day of the storm was 0.953 higher than during the previous clear day, while α was -0.049 in comparison with 0.323 during the previous day. Theoretical simulations using SMART software showed remarkable changes in both spectral and broadband solar radiation components. The global and direct radiation components decreased by 42% and 68%, respectively, and the diffuse components increased by 44% in comparison with the previous clear day. IR sky temperatures and sky emissivity increased by 24 °C and 0.3, respectively, 2 h after the arrival of the storm. The effect of aerosol loading by the storm on IR atmospheric emission was investigated using MODTRAN software. It was found that the effect of aerosols caused an increase of the atmospheric emission in the atmospheric window (8-14 μm) such that the window emissions resembled those of a blackbody and the atmospheric window was almost closed.

  20. TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

    SciTech Connect

    Annette Rohr

    2005-03-31

    This report documents progress made on the subject project during the period of September 1, 2004 through February 28, 2005. The TERESA Study is designed to investigate the role played by specific emissions sources and components in the induction of adverse health effects by examining the relative toxicity of coal combustion and mobile source (gasoline and/or diesel engine) emissions and their oxidative products. The study involves on-site sampling, dilution, and aging of coal combustion emissions at three coal-fired power plants, as well as mobile source emissions, followed by animal exposures incorporating a number of toxicological endpoints. The DOE-EPRI Cooperative Agreement (henceforth referred to as ''the Agreement'') for which this technical progress report has been prepared covers the performance and analysis of field experiments at the first TERESA plant, located in the Upper Midwest and henceforth referred to as Plant 0, and at two additional coal-fired power plants (Plants 1 and 2) utilizing different coal types and with different plant configurations. During this reporting period, all fieldwork at Plant 0 was completed. Stack sampling was conducted in October to determine if there were significant differences between the in-stack PM concentrations and the diluted concentrations used for the animal exposures. Results indicated no significant differences and therefore confidence that the revised stack sampling methodology described in the previous semiannual report is appropriate for use in the Project. Animal exposures to three atmospheric scenarios were carried out. From October 4-7, we conducted exposures to oxidized emissions with the addition of secondary organic aerosol (SOA). Later in October, exposures to the most complex scenario (oxidized, neutralized emissions plus SOA) were repeated to ensure comparability with the results of the June/July exposures where a different stack sampling setup was employed. In November, exposures to oxidized

  1. Multi-Decadal Variation of Aerosols: Sources, Transport, and Climate Effects

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Diehl, Thomas; Bian, Huisheng; Streets, David

    2008-01-01

    We present a global model study of multi-decadal changes of atmospheric aerosols and their climate effects using a global chemistry transport model along with the near-term to longterm data records. We focus on a 27-year time period of satellite era from 1980 to 2006, during which a suite of aerosol data from satellite observations, ground-based measurements, and intensive field experiments have become available. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which involves a time-varying, comprehensive global emission dataset that we put together in our previous investigations and will be improved/extended in this project. This global emission dataset includes emissions of aerosols and their precursors from fuel combustion, biomass burning, volcanic eruptions, and other sources from 1980 to the present. Using the model and satellite data, we will analyze (1) the long-term global and regional aerosol trends and their relationship to the changes of aerosol and precursor emissions from anthropogenic and natural sources, (2) the intercontinental source-receptor relationships controlled by emission, transport pathway, and climate variability.

  2. A New Approach to Modeling Aerosol Effects on East Asian Climate: Parametric Uncertainties Associated with Emissions, Cloud Microphysics and their Interactions

    SciTech Connect

    Yan, Huiping; Qian, Yun; Zhao, Chun; Wang, Hailong; Wang, Minghuai; Yang, Ben; Liu, Xiaohong; Fu, Qiang

    2015-09-16

    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. The 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.

  3. Dimethyl Sulfide Emissions from Dairies and Agriculture as a Potential Contributor to Sulfate Aerosols in the California Central Valley

    NASA Astrophysics Data System (ADS)

    Lebel, E.; Marrero, J. E.; Bertram, T. H.; Blake, D. R.

    2014-12-01

    Whole air samples have been collected throughout Southern California during the previous five years of the NASA Student Airborne Research Program (SARP). During a flight over the Salton Sea in 2014, higher concentrations of dimethyl sulfide (DMS), a known marine emitted gas, were observed over neighboring agricultural land than over the sea itself. A comparison of DMS to methyl iodide, another known marine emitted gas, showed minimal correlation, revealing that DMS was being emitted from local sources. Ground samples at the Salton Sea verified that the DMS was not transported from the Pacific Ocean. Previous SARP studies have shown that DMS is emitted from dairies. The enhancements in ethanol (another dairy tracer) and DMS in several airborne samples collected south of the Salton Sea suggest dairy emissions of the observed DMS. DMS is a compound of interest because its oxidation can form cloud condensation nuclei. Based on data from all six SARP flights between 2009-2014, we propose that dairy and farming emissions of DMS in the San Joaquin Valley may be impacting aerosol loading in this region. A simple model that takes into account the particulate matter mass loadings was used to calculate the percent contribution of DMS to aerosol formation for the San Joaquin Valley.

  4. Radiative forcing and climate response to projected 21st century aerosol decreases

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Horowitz, L. W.; Naik, V.; Golaz, J.-C.; Mauzerall, D. L.

    2015-11-01

    It is widely expected that global emissions of atmospheric aerosols and their precursors will decrease strongly throughout the remainder of the 21st century, due to emission reduction policies enacted to protect human health. For instance, global emissions of aerosols and their precursors are projected to decrease by as much as 80 % by the year 2100, according to the four Representative Concentration Pathway (RCP) scenarios. The removal of aerosols will cause unintended climate consequences, including an unmasking of global warming from long-lived greenhouse gases. We use the Geophysical Fluid Dynamics Laboratory Coupled Climate Model version 3 (GFDL CM3) to simulate future climate over the 21st century with and without the aerosol emission changes projected by each of the RCPs in order to isolate the radiative forcing and climate response resulting from the aerosol reductions. We find that the projected global radiative forcing and climate response due to aerosol decreases do not vary significantly across the four RCPs by 2100, although there is some mid-century variation, especially in cloud droplet effective radius, that closely follows the RCP emissions and energy consumption projections. Up to 1 W m-2 of radiative forcing may be unmasked globally from 2005 to 2100 due to reductions in aerosol and precursor emissions, leading to average global temperature increases up to 1 K and global precipitation rate increases up to 0.09 mm day-1. However, when using a version of CM3 with reduced present-day aerosol radiative forcing (-1.0 W m-2), the global temperature increase for RCP8.5 is about 0.5 K, with similar magnitude decreases in other climate response parameters as well. Regionally and locally, climate impacts can be much larger than the global mean, with a 2.1 K warming projected over China, Japan, and Korea due to the reduced aerosol emissions in RCP8.5, as well as nearly a 0.2 mm day-1 precipitation increase, a 7 g m-2 LWP decrease, and a 2 μm increase in

  5. Light Absorption Properties and Radiative Effects of Primary Organic Aerosol Emissions

    EPA Science Inventory

    Organic aerosols (OA) in the atmosphere affect Earth’s energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called “brown carbon” (BrC) component. However, the absorptivities of OA are not or poorly represented in current climate m...

  6. Development of a speciated, hourly, and gridded air pollutants emission modeling system--a case study on the precursors of photochemical smog in the Seoul metropolitan area, Korea.

    PubMed

    Kim, D Y; Kim, J W

    2000-03-01

    A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO2) and ozone (O3) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas. The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO2, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO2 and O3 concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.

  7. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

    NASA Astrophysics Data System (ADS)

    Gantt, B.; Kelly, J. T.; Bash, J. O.

    2015-11-01

    Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.

  8. MODELING PHOTOCHEMISTRY AND AEROSOL FORMATION IN POINT SOURCE PLUMES WITH THE CMAQ PLUME-IN-GRID

    EPA Science Inventory

    Emissions of nitrogen oxides and sulfur oxides from the tall stacks of major point sources are important precursors of a variety of photochemical oxidants and secondary aerosol species. Plumes released from point sources exhibit rather limited dimensions and their growth is gradu...

  9. Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

    NASA Astrophysics Data System (ADS)

    Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

    2010-03-01

    This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

  10. Air pollution from gas flaring: new emission factor estimates and detection in a West African aerosol remote-sensing climatology

    NASA Astrophysics Data System (ADS)

    MacKenzie, Rob; Fawole, Olusegun Gabriel; Levine, James; Cai, Xiaoming

    2016-04-01

    Gas flaring, the disposal of gas through stacks in an open-air flame, is a common feature in the processing of crude oil, especially in oil-rich regions of the world. Gas flaring is a prominent source of volatile organic compounds (VOCs), polycyclic aromatic hydrocarbons (PAH), CO, CO2, nitrogen oxides (NOx), SO2 (in "sour" gas only), and soot (black carbon), as well as the release of locally significant amounts of heat. The rates of emission of these pollutants from gas flaring depend on a number of factors including, but not limited to, fuel composition and quantity, stack geometry, flame/combustion characteristics, and prevailing meteorological conditions. Here, we derive new estimated emission factors (EFs) for carbon-containing pollutants (excluding PAH). The air pollution dispersion model, ADMS5, is used to simulate the dispersion of the pollutants from flaring stacks in the Niger delta. A seasonal variation of the dispersion pattern of the pollutant within a year is studied in relation to the movements of the West Africa Monsoon (WAM) and other prevailing meteorological factors. Further, we have clustered AERONET aerosol signals using trajectory analysis to identify dominant aerosol sources at the Ilorin site in West Africa (4.34 oE, 8.32 oN). A 10-year trajectory-based analysis was undertaken (2005-2015, excluding 2010). Of particular interest are air masses that have passed through the gas flaring region in the Niger Delta area en-route the AERONET site. 7-day back trajectories were calculated using the UK Universities Global Atmospheric Modelling Programme (UGAMP) trajectory model which is driven by analyses from the European Centre for Medium-Range Weather Forecasts (ECMWF). From the back-trajectory calculations, dominant sources are identified, using literature classifications: desert dust (DD); Biomass burning (BB); and Urban-Industrial (UI). We use a combination of synoptic trajectories and aerosol optical properties to distinguish a fourth source

  11. Changes in inorganic fine particulate matter sensitivities to precursors due to large-scale US emissions reductions.

    PubMed

    Holt, Jareth; Selin, Noelle E; Solomon, Susan

    2015-04-21

    We examined the impact of large US emissions changes, similar to those estimated to have occurred between 2005 and 2012 (high and low emissions cases, respectively), on inorganic PM2.5 sensitivities to further NOx, SO2, and NH3 emissions reductions using the chemical transport model GEOS-Chem. Sensitivities to SO2 emissions are larger year-round and across the US in the low emissions case than the high emissions case due to more aqueous-phase SO2 oxidation. Sensitivities to winter NOx emissions are larger in the low emissions case, more than 2× those of the high emissions case in parts of the northern Midwest. Sensitivities to NH3 emissions are smaller (∼40%) in the low emissions case, year-round, and across the US. Differences in NOx and NH3 sensitivities indicate an altered atmospheric acidity. Larger sensitivities to SO2 and NOx in the low emissions case imply that reducing these emissions may improve air quality more now than they would have in 2005; conversely, NH3 reductions may not improve air quality as much as previously assumed.

  12. Aerosol-computational fluid dynamics modeling of ultrafine and black carbon particle emission, dilution, and growth near roadways

    NASA Astrophysics Data System (ADS)

    Huang, L.; Gong, S. L.; Gordon, M.; Liggio, J.; Staebler, R.; Stroud, C. A.; Lu, G.; Mihele, C.; Brook, J. R.; Jia, C. Q.

    2014-12-01

    Many studies have shown that on-road vehicle emissions are the dominant source of ultrafine particles (UFPs; diameter < 100 nm) in urban areas and near-roadway environments. In order to advance our knowledge on the complex interactions and competition among atmospheric dilution, dispersion, and dynamics of UFPs, an aerosol dynamics-computational fluid dynamics (CFD) coupled model is developed and validated against field measurements. A unique approach of applying periodic boundary conditions is proposed to model pollutant dispersion and dynamics in one unified domain from the tailpipe level to the ambient near-road environment. This approach significantly reduces the size of the computational domain, and therefore allows fast simulation of multiple scenarios. The model is validated against measured turbulent kinetic energy (TKE) and horizontal gradient of pollution concentrations perpendicular to a major highway. Through a model sensitivity analysis, the relative importance of individual aerosol dynamical processes on the total particle number concentration (N) and particle number-size distribution (PSD) near a highway is investigated. The results demonstrate that (1) coagulation has a negligible effect on N and particle growth, (2) binary homogeneous nucleation (BHN) of H2SO4-H2O is likely responsible for elevated N closest to the road, and (3) N and particle growth are very sensitive to the condensation of semi-volatile organics (SVOCs), particle dry deposition, and the interaction between these processes. The results also indicate that, without the proper treatment of the atmospheric boundary layer (i.e., its wind profile and turbulence quantities), the nucleation rate would be underestimated by a factor of 5 in the vehicle wake region due to overestimated dilution. Therefore, introducing atmospheric boundary layer (ABL) conditions to activity-based emission models may potentially improve their performance in estimating UFP traffic emissions.

  13. Stratospheric aerosol, climatology derived from satellite solar occultation and infrared emission measurements

    NASA Astrophysics Data System (ADS)

    Bauman, Jill J.

    A global climatology has been produced on the stratospheric aerosol that spans nearly 15 years, from December 1984 to August 1999. The climatology includes values and uncertainties of measured extinction and optical depth from 0.385 μm to 12.82 μm, as well as retrieved particle effective radius Reff, distribution width σg, surface area S and volume V. As a basis for aerosol retrievals, a multi-wavelength Look-Up- Table (LUT) algorithm has been developed that uses a combination of 4wavelength Stratospheric Aerosol and Gas Experiment (SAGE) II extinction spectra (0.385-1.02 gym) and the Cryogenic Limb Array Etalon Spectrometer (CLASS) 7.96 and 12.82 gm extinction measurements. The LUT matches SAGE II/CLASS extinction ratios to pre- computed ratios that are based on a range of unimodal lognormal size distributions. By varying the distribution width, the uncertainties in measured extinction are propagated to corresponding uncertainties in Reff, S and V. The LUT includes an altitude- and time-dependent procedure to estimate and remove bias introduced by assuming a unimodal functional form. Bias correction reduces uncertainty in Reff, S and V by approximately 7%, 5% and 1%, respectively. This suggests that aerosol volume, and to a lesser extent surface area, are not as sensitive to a priori assumptions about distribution shape as retrievals of Reff. Aerosol retrievals show notable increases after most major volcanic eruptions, with increases in Reff lagging increases in other parameters. Post-volcanic increases in σg, indicative of broader size distributions, are consistent with sudden increases in both small and large particle sizes. After Pinatubo, retrieved Reff and σg took nearly 5 years to return to pre-eruption values, while slightly shorter recovery times are obtained for S and V. Seasonal variations in S and V are observed at high latitudes (with high values occurring in winter), but are less obvious in Reff. Latitudinal banding is often noted in retrievals

  14. Evidence of aqueous secondary organic aerosol formation from biogenic emissions in the North American Sonoran Desert

    PubMed Central

    Youn, Jong-Sang; Wang, Zhen; Wonaschütz, Anna; Arellano, Avelino; Betterton, Eric A.; Sorooshian, Armin

    2013-01-01

    This study examines the role of aqueous secondary organic aerosol formation in the North American Sonoran Desert as a result of intense solar radiation, enhanced moisture, and biogenic volatile organic compounds (BVOCs). The ratio of water-soluble organic carbon (WSOC) to organic carbon (OC) nearly doubles during the monsoon season relative to other seasons of the year. When normalized by mixing height, the WSOC enhancement during monsoon months relative to preceding dry months (May–June) exceeds that of sulfate by nearly a factor of 10. WSOC:OC and WSOC are most strongly correlated with moisture parameters, temperature, and concentrations of O3 and BVOCs. No positive relationship was identified between WSOC or WSOC:OC and anthropogenic tracers such as CO over a full year. This study points at the need for further work to understand the effect of BVOCs and moisture in altering aerosol properties in understudied desert regions. PMID:24115805

  15. Aerosol-fluorescence spectrum analyzer: real-time measurement of emission spectra of airborne biological particles

    NASA Astrophysics Data System (ADS)

    Hill, Steven C.; Pinnick, Ronald G.; Nachman, Paul; Chen, Gang; Chang, Richard K.; Mayo, Michael W.; Fernandez, Gilbert L.

    1995-10-01

    We have assembled an aerosol-fluorescence spectrum analyzer (AFS), which can measure the fluorescence spectra and elastic scattering of airborne particles as they flow through a laser beam. The aerosols traverse a scattering cell where they are illuminated with intense (50 kW/cm 2) light inside the cavity of an argon-ion laser operating at 488 nm. This AFS can obtain fluorescence spectra of individual dye-doped polystyrene microspheres as small as 0.5 mu m in diameter. The spectra obtained from microspheres doped with pink and green-yellow dyes are clearly different. We have also detected the fluorescence spectra of airborne particles (although not single particles) made from various

  16. Aerosol Direct, Indirect, Semidirect, and Surface Albedo Effects from Sector Contributions Based on the IPCC AR5 Emissions for Preindustrial and Present-day Conditions

    NASA Technical Reports Server (NTRS)

    Bauer, Susanne E.; Menon, Surabi

    2012-01-01

    The anthropogenic increase in aerosol concentrations since preindustrial times and its net cooling effect on the atmosphere is thought to mask some of the greenhouse gas-induced warming. Although the overall effect of aerosols on solar radiation and clouds is most certainly negative, some individual forcing agents and feedbacks have positive forcing effects. Recent studies have tried to identify some of those positive forcing agents and their individual emission sectors, with the hope that mitigation policies could be developed to target those emitters. Understanding the net effect of multisource emitting sectors and the involved cloud feedbacks is very challenging, and this paper will clarify forcing and feedback effects by separating direct, indirect, semidirect and surface albedo effects due to aerosols. To this end, we apply the Goddard Institute for Space Studies climate model including detailed aerosol microphysics to examine aerosol impacts on climate by isolating single emission sector contributions as given by the Coupled Model Intercomparison Project Phase 5 (CMIP5) emission data sets developed for Intergovernmental Panel on Climate Change (IPCC) AR5. For the modeled past 150 years, using the climate model and emissions from preindustrial times to present-day, the total global annual mean aerosol radiative forcing is -0.6 W/m(exp 2), with the largest contribution from the direct effect (-0.5 W/m(exp 2)). Aerosol-induced changes on cloud cover often depends on cloud type and geographical region. The indirect (includes only the cloud albedo effect with -0.17 W/m(exp 2)) and semidirect effects (-0.10 W/m(exp 2)) can be isolated on a regional scale, and they often have opposing forcing effects, leading to overall small forcing effects on a global scale. Although the surface albedo effects from aerosols are small (0.016 W/m(exp 2)), triggered feedbacks on top of the atmosphere (TOA) radiative forcing can be 10 times larger. Our results point out that each

  17. Effects of anthropogenic emissions on the molecular composition of urban organic aerosols: An ultrahigh resolution mass spectrometry study

    NASA Astrophysics Data System (ADS)

    Kourtchev, I.; O'Connor, I. P.; Giorio, C.; Fuller, S. J.; Kristensen, K.; Maenhaut, W.; Wenger, J. C.; Sodeau, J. R.; Glasius, M.; Kalberer, M.

    2014-06-01

    Identification of the organic composition of atmospheric aerosols is necessary to develop effective air pollution mitigation strategies. However, the majority of the organic aerosol mass is