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

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).

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

Aqueous-Phase Mechanism for Secondary Organic Aerosol Formation from Isoprene: Application to the Southeast United States and Co-Benefit of SO2 Emission Controls

NASA Technical Reports Server (NTRS)

Marais, E. A.; Jacob, D. J.; Jimenez, J. L.; Campuzano-Jost, P.; Day, D. A.; Hu, W.; Krechmer, J.; Zhu, L.; Kim, P. S.; Miller, C. C.;

Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

NASA Astrophysics Data System (ADS)

Liu, Tengyu; Li, Zijun; Chan, ManNin; Chan, Chak K.

2017-06-01

Cooking emissions can potentially contribute to secondary organic aerosol (SOA) but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils) was investigated in a potential aerosol mass (PAM) chamber. Experiments were conducted at 19-20 °C and 65-70 % relative humidity (RH). The characterization instruments included a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS). The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm-3 s, was 1. 35 ± 0. 30 µg min-1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5) from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol) in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc) of SOA was -1.51 to -0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA) and semi-volatile oxygenated organic aerosol (SV-OOA), indicating that SOA in these experiments was lightly oxidized.

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.

Complex Coupling of Air Quality and Climate-Relevant Aerosols in a Chemistry-Aerosol Microphysics Model

NASA Astrophysics Data System (ADS)

Yoshioka, M.; Carslaw, K. S.; Reddington, C.; Mann, G.

2013-12-01

Controlling emissions of aerosols and their precursors to improve air quality will impact the climate through direct and indirect radiative forcing. We have investigated the impacts of changes in a range of aerosol and gas-phase emission fluxes and changes in temperature on air quality and climate change metrics using a global aerosol microphysics and chemistry model, GLOMAP. We investigate how the responses of PM2.5 and cloud condensation nuclei (CCN) are coupled, and how attempts to improve air quality could have inadvertent effects on CCN, clouds and climate. The parameter perturbations considered are a 5°C increase in global temperature, increased or decreased precursor emissions of anthropogenic SO2, NH3, and NOx, and biogenic monoterpenes, and increased or decreased primary emissions of organic and black carbon aerosols from wildfire, fossil fuel, and biofuel. To quantify the interactions, we define a new sensitivity metric in terms of the response of CCN divided by the response of PM in different regions. .Our results show that the coupled chemistry and aerosol processes cause complex responses that will make any co-benefit policy decision problematic. In particular, we show that reducing SO2 emissions effectively reduces surface-level PM2.5 over continental regions in summer when background PM2.5 is high, with a relatively small reduction in marine CCN (and hence indirect radiative cooling over ocean), which is beneficial for near-term climate. Reducing NOx emissions does not improve summertime air quality very effectively but leads to a relatively high reduction of marine CCN. Reducing NH3 emissions has moderate effects on both PM2.5 and CCN. These three species are strongly coupled chemically and microphysically and the effects of changing emissions of one species on mass and size distributions of aerosols are very complex and spatially and temporally variable. For example, reducing SO2 emissions leads to reductions in sulphate and ammonium mass

Identifying robust regional precipitation responses to regional aerosol emissions perturbations in three coupled chemistry-climate models

NASA Astrophysics Data System (ADS)

Westervelt, D. M.; Fiore, A. M.; Lamarque, J. F.; Previdi, M. J.; Conley, A. J.; Shindell, D. T.; Mascioli, N. R.; Correa, G. J. P.; Faluvegi, G.; Horowitz, L. W.

2017-12-01

Regional emissions of anthropogenic aerosols and their precursors will likely decrease for the remainder of the 21st century, due to emission reduction policies enacted to protect human health. Although there is some evidence that regional climate effects of aerosols can be significant, we currently lack a robust understanding of the magnitude, spatio-temporal pattern, statistical significance, and physical processes responsible for these influences, especially for precipitation. Here, we aim to quantify systematically the precipitation response to regional changes in aerosols and investigate underlying mechanisms using three fully coupled chemistry-climate models: NOAA Geophysical Fluid Dynamics Laboratory Coupled Model 3 (GFDL-CM3), NCAR Community Earth System Model (CESM), and NASA Goddard Institute for Space Studies ModelE2 (GISS-E2). The central approach we use is to contrast a long control experiment (400 years, run with perpetual year 2000 emissions) with 14 individual aerosol emissions perturbation experiments ( 200 years each). We perturb emissions of sulfur dioxide (SO2) and carbonaceous aerosol (BC and OM) within several world regions and assess which responses are significant relative to internal variability determined by the control run and robust across the three models. Initial results show significant changes in precipitation in several vulnerable regions including the Western Sahel and the Indian subcontinent. SO2 emissions reductions from Europe and the United States have the largest impact on precipitation among most of the selected response regions. The precipitation response to emissions changes from these regions projects onto known modes of variability, such as the North Atlantic Oscillation (NAO) and the El Niño Southern Oscillation (ENSO). Across all perturbation experiments, we find a strong linear relationship between the responses of Sahel precipitation and the interhemispheric temperature difference, suggesting a common mechanism of an

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. H. J.; Denier van der Gon, H. A. C.; Kuenen, J. J. P.; van Meijgaard, E.; van Ulft, L. H.; Cofala, J.; Builtjes, P. J. H.

2014-07-01

In this study we present a dynamic model evaluation of the chemistry transport model LOTOS-EUROS 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 the regional climate model RACMO2. Observations at European rural background sites have been used as 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 day-to-day, 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 sulphur 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 1990's while smaller concentration changes and an increasing number of non-significant trends are observed and modelled between 2000-2009. Furthermore, the results confirm former studies showing that the observed trends in sulphate and total nitrate concentrations from 1990 to 2009 are significantly lower than the trends in precursor emissions and precursor concentrations. The model captured these non-linear responses to the emission changes well. Using the LOTOS-EUROS source apportionment module trends in formation efficiency of SIA have been quantified for four European regions. The exercise has revealed a 20-50% more efficient sulphate formation in 2009 compared to 1990 and an up to 20% more efficient nitrate formation per unit nitrogen oxide emission, which added to the

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

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

Climate Impacts From a Removal of Anthropogenic Aerosol Emissions

NASA Astrophysics Data System (ADS)

Samset, B. H.; Sand, M.; Smith, C. J.; Bauer, S. E.; Forster, P. M.; Fuglestvedt, J. S.; Osprey, S.; Schleussner, C.-F.

2018-01-01

Limiting global warming to 1.5 or 2.0°C requires strong mitigation of anthropogenic greenhouse gas (GHG) emissions. Concurrently, emissions of anthropogenic aerosols will decline, due to coemission with GHG, and measures to improve air quality. However, the combined climate effect of GHG and aerosol emissions over the industrial era is poorly constrained. Here we show the climate impacts from removing present-day anthropogenic aerosol emissions and compare them to the impacts from moderate GHG-dominated global warming. Removing aerosols induces a global mean surface heating of 0.5-1.1°C, and precipitation increase of 2.0-4.6%. Extreme weather indices also increase. We find a higher sensitivity of extreme events to aerosol reductions, per degree of surface warming, in particular over the major aerosol emission regions. Under near-term warming, we find that regional climate change will depend strongly on the balance between aerosol and GHG forcing.

Open burning of rice, corn and wheat straws: primary emissions, photochemical aging, and secondary organic aerosol formation

NASA Astrophysics Data System (ADS)

Fang, Zheng; Deng, Wei; Zhang, Yanli; Ding, Xiang; Tang, Mingjin; Liu, Tengyu; Hu, Qihou; Zhu, Ming; Wang, Zhaoyi; Yang, Weiqiang; Huang, Zhonghui; Song, Wei; Bi, Xinhui; Chen, Jianmin; Sun, Yele; George, Christian; Wang, Xinming

2017-12-01

Agricultural residues are among the most abundant biomass burned globally, especially in China. However, there is little information on primary emissions and photochemical evolution of agricultural residue burning. In this study, indoor chamber experiments were conducted to investigate primary emissions from open burning of rice, corn and wheat straws and their photochemical aging as well. Emission factors of NOx, NH3, SO2, 67 non-methane hydrocarbons (NMHCs), particulate matter (PM), organic aerosol (OA) and black carbon (BC) under ambient dilution conditions were determined. Olefins accounted for > 50 % of the total speciated NMHCs emission (2.47 to 5.04 g kg-1), indicating high ozone formation potential of straw burning emissions. Emission factors of PM (3.73 to 6.36 g kg-1) and primary organic carbon (POC, 2.05 to 4.11 gC kg-1), measured at dilution ratios of 1300 to 4000, were lower than those reported in previous studies at low dilution ratios, probably due to the evaporation of semi-volatile organic compounds under high dilution conditions. After photochemical aging with an OH exposure range of (1.97-4.97) × 1010 molecule cm-3 s in the chamber, large amounts of secondary organic aerosol (SOA) were produced with OA mass enhancement ratios (the mass ratio of total OA to primary OA) of 2.4-7.6. The 20 known precursors could only explain 5.0-27.3 % of the observed SOA mass, suggesting that the major precursors of SOA formed from open straw burning remain unidentified. Aerosol mass spectrometry (AMS) signaled that the aged OA contained less hydrocarbons but more oxygen- and nitrogen-containing compounds than primary OA, and carbon oxidation state (OSc) calculated with AMS resolved O / C and H / C ratios increased linearly (p < 0.001) with OH exposure with quite similar slopes.

Primary particulate emissions and secondary organic aerosol (SOA) formation from idling diesel vehicle exhaust in China.

PubMed

Deng, Wei; Hu, Qihou; Liu, Tengyu; Wang, Xinming; Zhang, Yanli; Song, Wei; Sun, Yele; Bi, Xinhui; Yu, Jianzhen; Yang, Weiqiang; Huang, Xinyu; Zhang, Zhou; Huang, Zhonghui; He, Quanfu; Mellouki, Abdelwahid; George, Christian

2017-09-01

In China diesel vehicles dominate the primary emission of particulate matters from on-road vehicles, and they might also contribute substantially to the formation of secondary organic aerosols (SOA). In this study tailpipe exhaust of three typical in-use diesel vehicles under warm idling conditions was introduced directly into an indoor smog chamber with a 30m 3 Teflon reactor to characterize primary emissions and SOA formation during photo-oxidation. The emission factors of primary organic aerosol (POA) and black carbon (BC) for the three types of Chinese diesel vehicles ranged 0.18-0.91 and 0.15-0.51gkg-fuel -1 , respectively; and the SOA production factors ranged 0.50-1.8gkg-fuel -1 and SOA/POA ratios ranged 0.7-3.7 with an average of 2.2. The fuel-based POA emission factors and SOA production factors from this study for idling diesel vehicle exhaust were 1-3 orders of magnitude higher than those reported in previous studies for idling gasoline vehicle exhaust. The emission factors for total particle numbers were 0.65-4.0×10 15 particleskg-fuel -1 , and particles with diameters less than 50nm dominated in total particle numbers. Traditional C 2 -C 12 precursor non-methane hydrocarbons (NMHCs) could only explain less than 3% of the SOA formed during aging and contribution from other precursors including intermediate volatile organic compounds (IVOC) needs further investigation. Copyright © 2017 Elsevier B.V. All rights reserved.

Primary Emission and the Potential of Secondary Aerosol Formation from Chinese Gasoline Engine Exhaust

NASA Astrophysics Data System (ADS)

Hu, Min; Peng, Jianfei; Qin, Yanhong; Du, Zhuofei; Li, Mengjin; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Lu, Sihua; Wu, Yusheng; Zeng, Limin; Guo, Song; Shao, Min; Wang, Yinhui; Shuai, Shijin

2017-04-01

Along with the urbanization and economic growth, vehicle population in China reached 269 million, ranked the second in the world in 2015. Gasoline vehicle is identified to be the main source for urban PM2.5 in China, accounting for 15%-31%. In this study the impact of fuel components on PM2.5 and volatile organic compounds (VOCs) emissions from a gasoline port fuel injection (PFI) engine and a gasoline direct injection (GDI) engine are discussed. Results show that, higher proportion of aromatics, alkenes or sulfur in gasoline fuel will lead to higher PM emissions. The PM from the PFI engine mainly consists of OC and a small amount of EC and inorganic ions, while the PM discharge from the GDI engine mainly consists of EC, OM and a small amount of inorganic ions. Since the GDI engines can reduce fuel consumption and CO2 emissions, and it would become more and more popular in the near future. The characteristics of POM component, emission factors and source profile were investigated from GDI engine, particularly focused on the effect of engine speed, load and the catalyst, which will be very much helpful for source identification as source indicators. Chamber experiments were conducted to quantify the potential of secondary aerosol formation from exhaust of a PFI gasoline engine and China V gasoline fuel. During 4-5 h simulation, equivalent to10 days of atmospheric photo-oxidation in Beijing, the extreme SOA production was 426 ± 85 mg/kg fuel, with high precursors and OH exposure. 14% of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatility organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reduction of emissions of aerosol precursor gases from vehicles is essential to mediate pollution in China.

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.

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

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

Dong, Xinyi; Li, Juan; Fu, Joshua S.

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 overmore » 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.« less

Secondary inorganic aerosols in Europe: sources and the significant influence of biogenic VOC emissions, especially on ammonium nitrate

NASA Astrophysics Data System (ADS)

Aksoyoglu, Sebnem; Ciarelli, Giancarlo; El-Haddad, Imad; Baltensperger, Urs; Prévôt, André S. H.

2017-06-01

Contributions of various anthropogenic sources to the secondary inorganic aerosol (SIA) in Europe as well as the role of biogenic emissions on SIA formation were investigated using the three-dimensional regional model CAMx (comprehensive air quality model with extensions). Simulations were carried out for two periods of EMEP field campaigns, February-March 2009 and June 2006, which are representative of cold and warm seasons, respectively. Biogenic volatile organic compounds (BVOCs) are known mainly as precursors of ozone and secondary organic aerosol (SOA), but their role on inorganic aerosol formation has not attracted much attention so far. In this study, we showed the importance of the chemical reactions of BVOCs and how they affect the oxidant concentrations, leading to significant changes, especially in the formation of ammonium nitrate. A sensitivity test with doubled BVOC emissions in Europe during the warm season showed a large increase in secondary organic aerosol (SOA) concentrations (by about a factor of two), while particulate inorganic nitrate concentrations decreased by up to 35 %, leading to a better agreement between the model results and measurements. Sulfate concentrations decreased as well; the change, however, was smaller. The changes in inorganic nitrate and sulfate concentrations occurred at different locations in Europe, indicating the importance of precursor gases and biogenic emission types for the negative correlation between BVOCs and SIA. Further analysis of the data suggested that reactions of the additional terpenes with nitrate radicals at night were responsible for the decline in inorganic nitrate formation, whereas oxidation of BVOCs with OH radicals led to a decrease in sulfate. Source apportionment results suggest that the main anthropogenic source of precursors leading to formation of particulate inorganic nitrate is road transport (SNAP7; see Table 1 for a description of the categories), whereas combustion in energy and

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.

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

Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

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

Mills, Michael J.; Schmidt, Anja; Easter, Richard

Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptionsmore » between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.« less

Climate and health implications of future aerosol emission scenarios

NASA Astrophysics Data System (ADS)

Partanen, Antti-Ilari; Landry, Jean-Sébastien; Damon Matthews, H.

2018-02-01

Anthropogenic aerosols have a net cooling effect on climate and also cause adverse health effects by degrading air quality. In this global-scale sensitivity study, we used a combination of the aerosol-climate model ECHAM-HAMMOZ and the University of Victoria Earth System Climate Model to assess the climate and health effects of aerosols emissions from three Representative Concentration Pathways (RCP2.6, RCP4.5, and RCP8.5) and two new (LOW and HIGH) aerosol emission scenarios derived from RCP4.5, but that span a wider spectrum of possible future aerosol emissions. All simulations had CO2 emissions and greenhouse gas forcings from RCP4.5. Aerosol forcing declined similarly in the standard RCP aerosol emission scenarios: the aerosol effective radiative forcing (ERF) decreased from -1.3 W m-2 in 2005 to between -0.1 W m-2 and -0.4 W m-2 in 2100. The differences in ERF were substantially larger between LOW (-0.02 W m-2 in 2100) and HIGH (-0.8 W m-2) scenarios. The global mean temperature difference between the simulations with standard RCP aerosol emissions was less than 0.18 °C, whereas the difference between LOW and HIGH reached 0.86 °C in 2061. In LOW, the rate of warming peaked at 0.48 °C per decade in the 2030s, whereas in HIGH it was the lowest of all simulations and never exceeded 0.23 °C per decade. Using present-day population density and baseline mortality rates for all scenarios, PM2.5-induced premature mortality was 2 371 800 deaths per year in 2010 and 525 700 in 2100 with RCP4.5 aerosol emissions; in HIGH, the premature mortality reached its maximum value of 2 780 800 deaths per year in 2030, whereas in LOW the premature mortality at 2030 was below 299 900 deaths per year. Our results show potential trade-offs in aerosol mitigation with respect to climate change and public health as ambitious reduction of aerosol emissions considerably increased warming while decreasing mortality.

Simplified aerosol modeling for variational data assimilation

NASA Astrophysics Data System (ADS)

Huneeus, N.; Boucher, O.; Chevallier, F.

2009-11-01

We have developed a simplified aerosol model together with its tangent linear and adjoint versions for the ultimate aim of optimizing global aerosol and aerosol precursor emission using variational data assimilation. The model was derived from the general circulation model LMDz; it groups together the 24 aerosol species simulated in LMDz into 4 species, namely gaseous precursors, fine mode aerosols, coarse mode desert dust and coarse mode sea salt. The emissions have been kept as in the original model. Modifications, however, were introduced in the computation of aerosol optical depth and in the processes of sedimentation, dry and wet deposition and sulphur chemistry to ensure consistency with the new set of species and their composition. The simplified model successfully manages to reproduce the main features of the aerosol distribution in LMDz. The largest differences in aerosol load are observed for fine mode aerosols and gaseous precursors. Differences between the original and simplified models are mainly associated to the new deposition and sedimentation velocities consistent with the definition of species in the simplified model and the simplification of the sulphur chemistry. Furthermore, simulated aerosol optical depth remains within the variability of monthly AERONET observations for all aerosol types and all sites throughout most of the year. Largest differences are observed over sites with strong desert dust influence. In terms of the daily aerosol variability, the model is less able to reproduce the observed variability from the AERONET data with larger discrepancies in stations affected by industrial aerosols. The simplified model however, closely follows the daily simulation from LMDz. Sensitivity analyses with the tangent linear version show that the simplified sulphur chemistry is the dominant process responsible for the strong non-linearity of the model.

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. Copyright © 2014 Elsevier B.V. All rights reserved.

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

Time-resolved analysis of primary volatile emissions and secondary aerosol formation potential from a small-scale pellet boiler

NASA Astrophysics Data System (ADS)

Czech, Hendryk; Pieber, Simone M.; Tiitta, Petri; Sippula, Olli; Kortelainen, Miika; Lamberg, Heikki; Grigonyte, Julija; Streibel, Thorsten; Prévôt, André S. H.; Jokiniemi, Jorma; Zimmermann, Ralf

2017-06-01

Small-scale pellet boilers and stoves became popular as a wood combustion appliance for domestic heating in Europe, North America and Asia due to economic and environmental aspects. Therefore, an increasing contribution of pellet boilers to air pollution is expected despite their general high combustion efficiency. As emissions of primary organic aerosol (POA) and permanent gases of pellet boilers are well investigated, the scope of this study was to investigate the volatile organic emissions and the formation potential of secondary aerosols for this type of appliance. Fresh and aged emissions were analysed by a soot-particle aerosol time-of-flight mass spectrometry (SP-AMS) and the molecular composition of the volatile precursors with single-photon ionisation time-of-flight mass spectrometry (SPI-TOFMS) at different pellet boiler operation conditions. Organic emissions in the gas phase were dominated by unsaturated hydrocarbons while wood-specific VOCs, e.g. phenolic species or substituted furans, were only detected during the starting phase. Furthermore, organic emissions in the gas phase were found to correlate with fuel grade and combustion technology in terms of secondary air supply. Secondary organic aerosols of optimised pellet boiler conditions (OPT, state-of-the-art combustion appliance) and reduced secondary air supply (RSA, used as a proxy for pellet boilers of older type) were studied by simulating atmospheric ageing in a Potential Aerosol Mass (PAM) flow reactor. Different increases in OA mass (55% for OPT, 102% for RSA), associated with higher average carbon oxidation state and O:C, could be observed in a PAM chamber experiment. Finally, it was found that derived SOA yields and emission factors were distinctly lower than reported for log wood stoves.

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.

2015-04-01

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 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 (internal, 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 +1.2 W m-2. The global-mean cloud-albedo aerosol indirect effect 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 effects is unclear due to uncertainties

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

Mechanism of organic aerosol formation and aging: Role of the precursor carbon skeleton

NASA Astrophysics Data System (ADS)

Hunter, J. F.; Carrasquillo, A. J.; Daumit, K. E.; Cross, E. S.; Worsnop, D. R.; Kroll, J. H.

2012-12-01

Oxidative aging of organic aerosol consists of a complex set of reactions coupled with gas-particle partitioning processes. Functionalization reactions involve adding oxygen containing functional groups onto a molecule, leading to reduced vapor pressures and promoting aerosol formation. In fragmentation reactions carbon-carbon bonds are broken as oxygen containing functional groups are added, which generally splits the parent molecule into two smaller and more volatile products. The initial structure of an aerosol-forming precursor molecule may influence what chemistry will occur both by changing the branching between fragmentation and functionalization processes as well as changing the effects of those processes. The fate of early generation oxidation products upon further aging is dependent on this initial chemistry, leading to a persistent effect of the precursor carbon skeleton. Aging experiments have been conducted using a high NOx smog chamber based aging technique. Long residence times and modestly elevated OH concentrations lead to typical maximum OH exposure of 3e11 molecule*seconds/cc, approaching several days equivalent exposure to ambient OH concentrations. A broad set of linear, branched and cyclic aliphatic hydrocarbons has been oxidized to determine the effects of carbon skeleton on the relative importance of fragmentation and functionalization and impacts on aerosol formation chemistry. Relative degree of fragmentation and functionalization is constrained by mass spectrometry of both the gas and particle phase. Measurements of the aerosol oxygen content and mass yield are reported, and structural effects on these properties are determined. Degree of unsaturation is hypothesized to have a significant impact on the effect of fragmentation reactions and to promote additional aerosol formation, extended aging and more oxygenated aerosol.

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...

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.

Aerosol reductions could dominate regional climate responses in low GHG emission scenarios

NASA Astrophysics Data System (ADS)

Samset, B. H.; Sand, M.; Smith, C. J.; Bauer, S.; Forster, P.; Fuglestvedt, J. S.; Osprey, S. M.; Schleussner, C. F.

2017-12-01

Limiting global warming to current political goals requires strong, rapid mitigation of anthropogenic greenhouse gas (GHG) emissions. Concurrently, emissions of anthropogenic aerosols will decline sharply, due to co-emission with greenhouse gases, and future measures to improve air quality. As the net climate effect of GHG and aerosol emissions over the industrial era is poorly constrained, predicting the impact of strong aerosol emission reductions remains challenging. Here we investigate the isolated and compound climate impacts from removing present day anthropogenic emissions of black carbon (BC), organic carbon (OC) and SO2, and moderate, near term GHG dominated global warming, using four coupled climate models. As the dominating effect of aerosol emission reduction is a removal of cooling from sulphur, the resulting climate impacts amplify those of GHG induced warming. BC emissions contribute little to reducing surface warming, but have stronger regional impacts. For the major aerosol emission regions, extreme weather indices are more sensitive to aerosol removal than to GHG increases, per degree of surface warming. East Asia in particular stands out, mainly due to the high present regional aerosol emissions. We show how present climate models indicate that future regional climate change will depend strongly on changes in loading and distribution of aerosols in the atmosphere, in addition to surface temperature change.

Identification of secondary aerosol precursors emitted by an aircraft turbofan

NASA Astrophysics Data System (ADS)

Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

2018-05-01

Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

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

NASA Astrophysics Data System (ADS)

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

2016-11-01

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

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

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

Potential of secondary aerosol formation from Chinese gasoline engine exhaust.

PubMed

Du, Zhuofei; Hu, Min; Peng, Jianfei; Guo, Song; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Qin, Yanhong; Niu, He; Li, Mengren; Yang, Yudong; Lu, Sihua; Wu, Yusheng; Shao, Min; Shuai, Shijin

2018-04-01

Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds (VOCs). However, little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4-5hr simulation, which was estimated to represent more than 10days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol (SOA) production was 426±85mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China. Copyright © 2017. Published by Elsevier B.V.

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

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

NASA Astrophysics Data System (ADS)

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

2014-11-01

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

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

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

2013-11-01

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

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

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

2013-07-01

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

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.

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.

Aerosol emission during human speech

NASA Astrophysics Data System (ADS)

Asadi, Sima; Wexler, Anthony S.; Cappa, Christopher D.; Bouvier, Nicole M.; Barreda-Castanon, Santiago; Ristenpart, William D.

2017-11-01

We show that the rate of aerosol particle emission during healthy human speech is strongly correlated with the loudness (amplitude) of vocalization. Emission rates range from approximately 1 to 50 particles per second for quiet to loud amplitudes, regardless of language spoken (English, Spanish, Mandarin, or Arabic). Intriguingly, a small fraction of individuals behave as ``super emitters,'' consistently emitting an order of magnitude more aerosol particles than their peers. We interpret the results in terms of the eggressive flowrate during vocalization, which is known to vary significantly for different types of vocalization and for different individuals. The results suggest that individual speech patterns could affect the probability of airborne disease transmission. The results also provide a possible explanation for the existence of ``super spreaders'' who transmit pathogens much more readily than average and who play a key role in the spread of epidemics.

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

Highly-controlled, reproducible measurements of aerosol emissions from African biomass combustion

NASA Astrophysics Data System (ADS)

Haslett, Sophie; Thomas, J. Chris; Morgan, William; Hadden, Rory; Liu, Dantong; Allan, James; Williams, Paul; Sekou, Keïta; Liousse, Catherine; Coe, Hugh

2017-04-01

Particulate emissions from biomass burning can alter the atmosphere's radiative balance and cause significant harm to human health. However, the relationship between these emissions and fundamental combustion processes is, to date, poorly characterised. In atmospheric models, aerosol emissions are represented by emission factors based on mass loss, which are averaged over an entire combustion event for each particulate species. This approach, however, masks huge variability in emissions during different phases of the combustion period. Laboratory tests have shown that even small changes to the burning environment can lead to huge variation in observed aerosol emission factors (Akagi et al., 2011). In order to address this gap in understanding, in this study, small wood samples sourced from Côte D'Ivoire were burned in a highly-controlled laboratory environment. The shape and mass of samples, available airflow and surrounding heat were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real-time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. Both of these instruments are used regularly to measure aerosol concentrations in the field. This methodology produced remarkably repeatable results, allowing three different phases of combustion to be identified by their emissions. Black carbon was emitted predominantly during flaming combustion; organic aerosols were emitted during pyrolysis before ignition and from smouldering-dominated behaviour near the end of combustion. During the flaming period, there was a strong correlation between the emission of black carbon and the rate of mass loss, which suggests there is value in employing a mass-based emission factor for this species. However, very little correlation was seen between organic aerosol and mass loss throughout the tests. As such, results here suggest that emission factors averaged over an entire combustion event are unlikely to be

Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols

NASA Technical Reports Server (NTRS)

Liao, Hong; Chen, Wei-Ting; Seinfeld, John H.

2006-01-01

A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2

Radiative effects of interannually varying vs. interannually invariant aerosol emissions from fires

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

Grandey, Benjamin S.; Lee, Hsiang-He; Wang, Chien

Open-burning fires play an important role in the earth's climate system. In addition to contributing a substantial fraction of global emissions of carbon dioxide, they are a major source of atmospheric aerosols containing organic carbon, black carbon, and sulfate. These “fire aerosols” can influence the climate via direct and indirect radiative effects. In this study, we investigate these radiative effects and the hydrological fast response using the Community Atmosphere Model version 5 (CAM5). Emissions of fire aerosols exert a global mean net radiative effect of −1.0 W m −2, dominated by the cloud shortwave response to organic carbon aerosol. The net radiative effectmore » is particularly strong over boreal regions. Conventionally, many climate modelling studies have used an interannually invariant monthly climatology of emissions of fire aerosols. However, by comparing simulations using interannually varying emissions vs. interannually invariant emissions, we find that ignoring the interannual variability of the emissions can lead to systematic overestimation of the strength of the net radiative effect of the fire aerosols. Globally, the overestimation is +23 % (−0.2 W m −2). Regionally, the overestimation can be substantially larger. For example, over Australia and New Zealand the overestimation is +58 % (−1.2 W m −2), while over Boreal Asia the overestimation is +43 % (−1.9 W m −2). The systematic overestimation of the net radiative effect of the fire aerosols is likely due to the non-linear influence of aerosols on clouds. However, ignoring interannual variability in the emissions does not appear to significantly impact the hydrological fast response. In order to improve understanding of the climate system, we need to take into account the interannual variability of aerosol emissions.« less

Radiative effects of interannually varying vs. interannually invariant aerosol emissions from fires

DOE PAGES

Grandey, Benjamin S.; Lee, Hsiang-He; Wang, Chien

2016-11-23

Open-burning fires play an important role in the earth's climate system. In addition to contributing a substantial fraction of global emissions of carbon dioxide, they are a major source of atmospheric aerosols containing organic carbon, black carbon, and sulfate. These “fire aerosols” can influence the climate via direct and indirect radiative effects. In this study, we investigate these radiative effects and the hydrological fast response using the Community Atmosphere Model version 5 (CAM5). Emissions of fire aerosols exert a global mean net radiative effect of −1.0 W m −2, dominated by the cloud shortwave response to organic carbon aerosol. The net radiative effectmore » is particularly strong over boreal regions. Conventionally, many climate modelling studies have used an interannually invariant monthly climatology of emissions of fire aerosols. However, by comparing simulations using interannually varying emissions vs. interannually invariant emissions, we find that ignoring the interannual variability of the emissions can lead to systematic overestimation of the strength of the net radiative effect of the fire aerosols. Globally, the overestimation is +23 % (−0.2 W m −2). Regionally, the overestimation can be substantially larger. For example, over Australia and New Zealand the overestimation is +58 % (−1.2 W m −2), while over Boreal Asia the overestimation is +43 % (−1.9 W m −2). The systematic overestimation of the net radiative effect of the fire aerosols is likely due to the non-linear influence of aerosols on clouds. However, ignoring interannual variability in the emissions does not appear to significantly impact the hydrological fast response. In order to improve understanding of the climate system, we need to take into account the interannual variability of aerosol emissions.« less

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

Source apportionments of aerosols and their direct radiative forcing and long-term trends over continental United States

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

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

Due to US air pollution regulations, aerosol and precursor emissions have decreased during recent decades, while changes in emissions in other regions of the world also influence US aerosol trends through long-range transport. We examine here the relative roles of these domestic and foreign emission changes on aerosol concentrations and direct radiative forcing (DRF) at the top of the atmosphere over the continental US. Long-term (1980-2014) trends and aerosol source apportionment are quantified in this study using a global aerosol-climate model equipped with an explicit aerosol source tagging technique. Due to US emission control policies, the annual mean near-surface concentrationmore » of particles, consisting of sulfate, black carbon, and primary organic aerosol, decreases by about –1.1 (±0.1) / –1.4 (±0.1) μg m -3 in western US and –3.3 (±0.2) / –2.9 (±0.2) μg m -3 in eastern US during 2010–2014, as compared to those in 1980–1984. Meanwhile, decreases in US emissions lead to a warming of +0.48 (±0.03) / –0.46 (±0.03) W m -2 in western US and +1.41 (±0.07) /+1.32 (±0.09) W m -2 in eastern US through changes in aerosol DRF. Increases in emissions from East Asia generally have a modest impact on US air quality, but mitigated the warming effect induced by reductions in US emissions by 25% in western US and 7% in eastern US. Thus, as US domestic aerosol and precursor emissions continue to decrease, foreign emissions may become increasingly important to radiative forcing over the US.« less

Source apportionments of aerosols and their direct radiative forcing and long-term trends over continental United States

DOE PAGES

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

2018-05-23

Due to US air pollution regulations, aerosol and precursor emissions have decreased during recent decades, while changes in emissions in other regions of the world also influence US aerosol trends through long-range transport. We examine here the relative roles of these domestic and foreign emission changes on aerosol concentrations and direct radiative forcing (DRF) at the top of the atmosphere over the continental US. Long-term (1980-2014) trends and aerosol source apportionment are quantified in this study using a global aerosol-climate model equipped with an explicit aerosol source tagging technique. Due to US emission control policies, the annual mean near-surface concentrationmore » of particles, consisting of sulfate, black carbon, and primary organic aerosol, decreases by about –1.1 (±0.1) / –1.4 (±0.1) μg m -3 in western US and –3.3 (±0.2) / –2.9 (±0.2) μg m -3 in eastern US during 2010–2014, as compared to those in 1980–1984. Meanwhile, decreases in US emissions lead to a warming of +0.48 (±0.03) / –0.46 (±0.03) W m -2 in western US and +1.41 (±0.07) /+1.32 (±0.09) W m -2 in eastern US through changes in aerosol DRF. Increases in emissions from East Asia generally have a modest impact on US air quality, but mitigated the warming effect induced by reductions in US emissions by 25% in western US and 7% in eastern US. Thus, as US domestic aerosol and precursor emissions continue to decrease, foreign emissions may become increasingly important to radiative forcing over the US.« less

Laboratory Measurements of Biomass Cook-stove Emissions Aged in an Oxidation Flow Reactor: Influence of Combustion and Aging Conditions on Aerosols

NASA Astrophysics Data System (ADS)

Grieshop, A. P.; Reece, S. M.; Sinha, A.; Wathore, R.

2016-12-01

Combustion in rudimentary and improved cook-stoves used by billions in developing countries can be a regionally dominant contributor to black carbon (BC), primary organic aerosols (POA) and precursors for secondary organic aerosol (SOA). Recent studies suggest that SOA formed during photo-oxidation of primary emissions from biomass burning may make important contribution to its atmospheric impacts. However, the extent to which stove type and operating conditions affect the amount, composition and characteristics of SOA formed from the aging of cookstoves emissions is still largely undetermined. Here we present results from experiments with a field portable oxidation flow reactor (F-OFR) designed to assess aging of cook-stove emissions in both laboratory and field settings. Laboratory tests results are used to compare the quantity and properties of fresh and aged emissions from a traditional open fire and twp alternative stove designs operated on the standard and alternate testing protocols. Diluted cookstove emissions were exposed to a range of oxidant concentrations in the F-OFR. Primary emissions were aged both on-line, to study the influence of combustion variability, and sampled from batched emissions in a smog chamber to examine different aging conditions. Data from real-time particle- and gas-phase instruments and integrated filter samples were collected up and down stream of the OFR. The properties of primary emissions vary strongly with stove type and combustion conditions (e.g. smoldering versus flaming). Experiments aging diluted biomass emissions from distinct phases of stove operation (smoldering and flaming) showed peak SOA production for both phases occurred between 3 and 6 equivalent days of aging with slightly greater production observed in flaming phase emissions. Changing combustion conditions had a stronger influence than aging on POA+SOA `emission factors'. Aerosol Chemical Speciation Monitor data show a substantial evolution of aerosol

Does Aerosol Geoengineering the Earth's Climate Pass a Cost-Benefit Test?

NASA Astrophysics Data System (ADS)

Keller, K.; Urban, N.; Tuana, N.

2007-12-01

Anthropogenic carbon dioxide (CO2) emissions are changing the Earth's climate with potentially dangerous consequences. Ratified international agreements call for a reduction of CO2 emissions to avoid dangerous anthropogenic interference with the climate system. Recent studies have, however, proposed an alternative strategy: to geoengineer Earth's climate by injecting aerosol precursors into the stratosphere. It is often claimed that aerosol geoengineering would provide net economic benefits because geoengineering requires far lower near-term investments compared to deep cuts in CO2 emissions. However, aerosol geoengineering projects can also cause nontrivial economic costs. This is because aerosol geoengineering hinges on successfully counterbalancing the forcing effects of CO2 emissions (which decay over centuries) with the forcing effects of aerosol emissions (which decay within years). A failure to maintain this delicate balance can lead to abrupt climatic changes, with potentially substantial economic damages. Deferring cuts in CO2 emissions in favor of aerosol geoengineering is hence a deeply uncertain gamble, as it requires so far unknown institutions to reliably control aerosol forcings over centuries. Here we use a simple economic model to evaluate potential costs and benefits of aerosol geoengineering for a wide range of the deeply uncertain parameters. We show that aerosol geoengineering projects may cause economic damages that can far exceed the benefits and may hence fail a cost-benefit test.

The impact of aerosol emissions on the 1.5 °C pathways

NASA Astrophysics Data System (ADS)

Hienola, Anca; Partanen, Antti-Ilari; Pietikäinen, Joni-Pekka; O’Donnell, Declan; Korhonen, Hannele; Damon Matthews, H.; Laaksonen, Ari

2018-04-01

To assess the impact of anthropogenic aerosol emission reduction on limiting global temperature increase to 1.5 °C or 2 °C above pre-industrial levels, two climate modeling approaches have been used (MAGICC6, and a combination of ECHAM-HAMMOZ and the UVic ESCM), with two aerosol control pathways under two greenhouse gas (GHG) reduction scenarios. We found that aerosol emission reductions associated with CO2 co-emissions had a significant warming effect during the first half of the century and that the near-term warming is dependent on the pace of aerosol emission reduction. The modeling results show that these aerosol emission reductions account for about 0.5 °C warming relative to 2015, on top of the 1 °C above pre-industrial levels that were already reached in 2015. We found also that the decreases in aerosol emissions lead to different decreases in the magnitude of the aerosol radiative forcing in the two models. By 2100, the aerosol forcing is projected by ECHAM–UVic to diminish in magnitude by 0.96 W m‑2 and by MAGICC6 by 0.76 W m‑2 relative to 2000. Despite this discrepancy, the climate responses in terms of temperature are similar. Aggressive aerosol control due to air quality legislation affects the peak temperature, which is 0.2 °C–0.3 °C above the 1.5 °C limit even within the most ambitious CO2/GHG reduction scenario. At the end of the century, the temperature differences between aerosol reduction scenarios in the context of ambitious CO2 mitigation are negligible.

Indirect effect of changing aerosol concentrations on methane and ozone radiative forcing

NASA Astrophysics Data System (ADS)

Rowlinson, Matthew; Rap, Alexandru; Arnold, Steve; Forster, Piers; Chipperfield, Martyn

2017-04-01

Atmospheric aerosols interact with climate in number of complex ways and quantifying the overall effect remains the dominant uncertainty in estimating anthropogenic climate forcing (IPCC, 2013). The radiative forcing (RF) caused by the direct effect of aerosol interacting with radiation is estimated at -0.35 (-0.85 to +0.15) Wm-2, while cloud-aerosol interactions are estimated at -0.45 (-1.2 to 0.0) Wm-2 (IPCC, 2013). The net impact is a cooling with an effective radiative forcing (ERF) of 0.9 (-1.9 to -0.1) Wm-2 (IPCC, 2013). One effect of aerosols which has not been well evaluated is their effect on atmospheric chemistry. Atmospheric aerosols provide a surface for homogeneous reactions to occur, altering reactions rates and the availability of oxidants, thereby influencing the removal/production of radiatively important species such as methane (CH4) and tropospheric ozone (O3). Oxidants such as the hydroxyl radical (OH) determine the atmospheric lifetime and hence burden of CH4, therefore changes to atmospheric aerosols which impact oxidation chemistry will also influence RF due to CH4. This effect could enhance or offset the negative RF of aerosols, depending on how the individual aerosol changes availability of oxidants. Quantifying the importance of this mechanism for RF is necessary to provide accurate estimates of the effect of aerosols, and assess relative effectiveness of measures to decrease aerosol emissions and precursors. Using a sophisticated aerosol micro-physics model (GLOMAP) coupled to the TOMCAT three-dimensional chemical transport model, we separately simulate changes in atmospheric composition resulting from a 50% decline in anthropogenic emissions of black carbon aerosol (BC), volatile organic compounds (VOCs) and anthropogenic precursors of sulphate and nitrate. The impact of changes to each aerosol on lifetime of CH4 is then calculated to establish the resulting impact on CH4 burden and RF. Cutting global anthropogenic SO2 emissions by 50

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.

The Influence of Emission Location on the Magnitude and Spatial Distribution of Aerosols' Climate Effects

NASA Astrophysics Data System (ADS)

Persad, G.; Caldeira, K.

2017-12-01

The global distribution of anthropogenic aerosol emissions has evolved continuously since the preindustrial era - from 20th century North American and Western European emissions hotspots to present-day South and East Asian ones. With this comes a relocation of the regional radiative, dynamical, and hydrological impacts of aerosol emissions, which may influence global climate differently depending on where they occur. A lack of understanding of this relationship between aerosol emissions' location and their global climate effects, however, obscures the potential influence that aerosols' evolving geographic distribution may have on global and regional climate change—a gap which we address in this work. Using a novel suite of experiments in the CESM CAM5 atmospheric general circulation model coupled to a slab ocean, we systematically test and analyze mechanisms behind the relative climate impact of identical black carbon and sulfate aerosol emissions located in each of 8 past, present, or projected future major emissions regions. Results indicate that historically high emissions regions, such as North America and Western Europe, produce a stronger cooling effect than current and projected future high emissions regions. Aerosol emissions located in Western Europe produce 3 times the global mean cooling (-0.34 °C) as those located in East Africa or India (-0.11 °C). The aerosols' in-situ radiative effects remain relatively confined near the emissions region, but large distal cooling results from remote feedback processes - such as ice albedo and cloud changes - that are excited more strongly by emissions from certain regions than others. Results suggest that aerosol emissions from different countries should not be considered equal in the context of climate mitigation accounting, and that the evolving geographic distribution of aerosol emissions may have a substantial impact on the magnitude and spatial distribution of global climate change.

Contributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiagvik, Alaska

DOE PAGES

Gunsch, Matthew J.; Kirpes, Rachel M.; Kolesar, Katheryn R.; ...

2017-09-14

Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiagvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13–4 µm projected area diameter) and real-time single-particle mass spectrometry (0.2–1.5 µm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 %more » of the study), our results show that fresh sea spray aerosol contributed ~20 %, by number, of particles between 0.13 and 0.4 µm, 40–70 % between 0.4 and 1 µm, and 80–100 % between 1 and 4 µm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13–1 µm) combustion-derived particles (20–50 % organic carbon, by number; 5–10% soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 µm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm -3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.« less

Contributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiagvik, Alaska

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

Gunsch, Matthew J.; Kirpes, Rachel M.; Kolesar, Katheryn R.

Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiagvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13–4 µm projected area diameter) and real-time single-particle mass spectrometry (0.2–1.5 µm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 %more » of the study), our results show that fresh sea spray aerosol contributed ~20 %, by number, of particles between 0.13 and 0.4 µm, 40–70 % between 0.4 and 1 µm, and 80–100 % between 1 and 4 µm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13–1 µm) combustion-derived particles (20–50 % organic carbon, by number; 5–10% soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 µm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm -3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.« less

Primary carbonaceous aerosols and climate modeling: Classifications, global emission inventories, and observations

NASA Astrophysics Data System (ADS)

Sun, H.; Bond, T.

2004-12-01

Carbonaceous aerosols, including black carbon (BC) and organic carbon (OC), make up a large fraction of the atmospheric aerosols and affect the radiative balance of the earth either by directly scattering and absorbing solar radiation or through indirect influence on cloud optical properties and cloud lifetimes. The major sources of BC and OC emissions are from combustion processes, mainly.fossil-fuel burning, biofuels burning, and open biomass burning. OC is nearly always emitted with BC. Because different combustion practices contribute to the emission of BC and OC to the atmosphere, the magnitude and characteristics of carbonaceous aerosols vary between regions. Since OC mainly scatters light and BC absorbs it, it is possible that OC can oppose the warming effect of BC, so that the net climatic effect of carbonaceous aerosols is not known. There is presently disagreement on whether carbonaceous aerosols produce a net warming or cooling effect on climate. Some differences in model prediction may result from model differences, such as dynamics and treatment of cloud feedbacks. However, large differences also result from initial assumptions about the properties of BC and OC: optical properties, size distribution, and interaction with water. Although there are hundreds of different organic species in atmospheric aerosols, with widely varying properties, global climate models to date have treated organics as one ¡°compound.¡± In addition, emissions of OC are often derived by multiplying BC emissions by a constant factor, so that the balance between these different compounds is assumed. Addressing these critical model assumptions is a necessary step toward estimating the net climatic impact of carbonaceous aerosols, and different human activities. We aim to contribute to this effort by tabulating important climate-relevant properties of both emissions and ambient measurements. Since one single organic ¡°compound¡± is not sufficient to represent all the

Smoke aerosol chemistry and aging of Siberian biomass burning emissions in a large aerosol chamber

NASA Astrophysics Data System (ADS)

Kalogridis, A.-C.; Popovicheva, O. B.; Engling, G.; Diapouli, E.; Kawamura, K.; Tachibana, E.; Ono, K.; Kozlov, V. S.; Eleftheriadis, K.

2018-07-01

Vegetation open fires constitute a significant source of particulate pollutants on a global scale and play an important role in both atmospheric chemistry and climate change. To better understand the emission and aging characteristics of smoke aerosols, we performed small-scale fire experiments using the Large Aerosol Chamber (LAC, 1800 m3) with a focus on biomass burning from Siberian boreal coniferous forests. A series of burn experiments were conducted with typical Siberian biomass (pine and debris), simulating separately different combustion conditions, namely, flaming, smoldering and mixed phase. Following smoke emission and dispersion in the combustion chamber, we investigated aging of aerosols under dark conditions. Here, we present experimental data on emission factors of total, elemental and organic carbon, as well as individual organic compounds, such as anhydrosugars, phenolic and dicarboxylic acids. We found that total carbon accounts for up to 80% of the fine mode (PM2.5) smoke aerosol. Higher PM2.5 emission factors were observed in the smoldering compared to flaming phase and in pine compared to debris smoldering phase. For low-temperature combustion, organic carbon (OC) contributed to more than 90% of total carbon, whereas elemental carbon (EC) dominated the aerosol composition in flaming burns with a 60-70% contribution to the total carbon mass. For all smoldering burns, levoglucosan (LG), a cellulose decomposition product, was the most abundant organic species (average LG/OC = 0.26 for pine smoldering), followed by its isomer mannosan or dehydroabietic acid (DA), an important constituent of conifer resin (DA/OC = 0.033). A levoglucosan-to-mannosan ratio of about 3 was observed, which is consistent with ratios reported for coniferous biomass and more generally softwood. The rates of aerosol removal for OC and individual organic compounds were investigated during aging in the chamber in terms of mass concentration loss rates over time under dark

Global mortality attributable to aircraft cruise emissions.

PubMed

Barrett, Steven R H; Britter, Rex E; Waitz, Ian A

2010-10-01

Aircraft emissions impact human health though degradation of air quality. The majority of previous analyses of air quality impacts from aviation have considered only landing and takeoff emissions. We show that aircraft cruise emissions impact human health over a hemispheric scale and provide the first estimate of premature mortalities attributable to aircraft emissions globally. We estimate ∼8000 premature mortalities per year are attributable to aircraft cruise emissions. This represents ∼80% of the total impact of aviation (where the total includes the effects of landing and takeoff emissions), and ∼1% of air quality-related premature mortalities from all sources. However, we note that the impact of landing and takeoff emissions is likely to be under-resolved. Secondary H(2)SO(4)-HNO(3)-NH(3) aerosols are found to dominate mortality impacts. Due to the altitude and region of the atmosphere at which aircraft emissions are deposited, the extent of transboundary air pollution is particularly strong. For example, we describe how strong zonal westerly winds aloft, the mean meridional circulation around 30-60°N, interaction of aircraft-attributable aerosol precursors with background ammonia, and high population densities in combination give rise to an estimated ∼3500 premature mortalities per year in China and India combined, despite their relatively small current share of aircraft emissions. Subsidence of aviation-attributable aerosol and aerosol precursors occurs predominantly around the dry subtropical ridge, which results in reduced wet removal of aviation-attributable aerosol. It is also found that aircraft NO(x) emissions serve to increase oxidation of nonaviation SO(2), thereby further increasing the air quality impacts of aviation. We recommend that cruise emissions be explicitly considered in the development of policies, technologies and operational procedures designed to mitigate the air quality impacts of air transportation.

Impacts of Future European Emission Reductions on Aerosol Particle Number Concentrations Accounting for Effects of Ammonia, Amines, and Organic Species.

PubMed

Julin, Jan; Murphy, Benjamin N; Patoulias, David; Fountoukis, Christos; Olenius, Tinja; Pandis, Spyros N; Riipinen, Ilona

2018-01-16

Although they are currently unregulated, atmospheric ultrafine particles (<100 nm) pose health risks because of, e.g., their capability to penetrate deep into the respiratory system. Ultrafine particles, often minor contributors to atmospheric particulate mass, typically dominate aerosol particle number concentrations. We simulated the response of particle number concentrations over Europe to recent estimates of future emission reductions of aerosol particles and their precursors. We used the chemical transport model PMCAMx-UF, with novel updates including state-of-the-art descriptions of ammonia and dimethylamine new particle formation (NPF) pathways and the condensation of organic compounds onto particles. These processes had notable impacts on atmospheric particle number concentrations. All three emission scenarios (current legislation, optimized emissions, and maximum technically feasible reductions) resulted in substantial (10-50%) decreases in median particle number concentrations over Europe. Consistent reductions were predicted in Central Europe, while Northern Europe exhibited smaller reductions or even increased concentrations. Motivated by the improved NPF descriptions for ammonia and methylamines, we placed special focus on the potential to improve air quality by reducing agricultural emissions, which are a major source of these species. Agricultural emission controls showed promise in reducing ultrafine particle number concentrations, although the change is nonlinear with particle size.

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

DOE PAGES

Wobus, Cameron; Flanner, Mark; Sarofim, Marcus C.; ...

2016-05-17

The Arctic temperature response to emissions of aerosols – specifically black carbon (BC), organic carbon (OC), and sulfate – depends on both the sector and the region where these emissions originate. Thus, the net Arctic temperature response to global aerosol emissions reductions will depend strongly on the blend of emissions sources being targeted. We use recently published equilibrium Arctic temperature response factors for BC, OC, and sulfate to estimate the range of present-day and future Arctic temperature changes from seven different aerosol emissions scenarios. Globally, Arctic temperature changes calculated from all of these emissions scenarios indicate that present-day emissions frommore » the domestic and transportation sectors generate the majority of present-day Arctic warming from BC. However, in all of these scenarios, this warming is more than offset by cooling resulting from SO 2 emissions from the energy sector. Thus, long-term climate mitigation strategies that are focused on reducing carbon dioxide (CO 2) emissions from the energy sector could generate short-term, aerosol-induced Arctic warming. As a result, a properly phased approach that targets BC-rich emissions from the transportation sector as well as the domestic sectors in key regions – while simultaneously working toward longer-term goals of CO 2 mitigation – could potentially avoid some amount of short-term Arctic warming.« less

The response of European and Asian climate to global and regional aerosol emissions

NASA Astrophysics Data System (ADS)

Wilcox, Laura; Dunstone, Nick; Highwood, Eleanor; Bollasina, Massimo; Dong, Buwen; Sutton, Rowan

2017-04-01

Asia has the world's highest anthropogenic aerosol loading and has experienced a dramatic increase in emissions since the 1950s, which has continued in the 21st century, in stark contrast with European (and North American) emissions which started to decrease in the 1970s. We use a set of transient coupled model experiments (HadGEM2-GC2) to explore the regional climate effects of anthropogenic aerosol changes since the 1980s, with a focus on the European and Asian responses. Comparing simulations with globally varying aerosol emissions to an equivalent set with Asian emissions fixed at their 1971-1980 mean over Asia, we identify the contribution of Asian emissions to the total impact. Identifying thermodynamic and dynamic responses to global and regional aerosol changes, we diagnose atmospheric teleconnections and their interactions with local processes, and the mechanisms by which aerosol affects both European and Asian climate. It is found that Asian aerosols led to substantial changes in Asian climate, weakening the summer monsoon, which is a key driver of the observed precipitation changes there in recent decades. Asian emissions are also able to induce planetary-scale teleconnection patterns in both winter and summer. The impact of the regional diabatic heating anomaly propagates remotely by exciting northern hemisphere wave-trains which, enhanced by regional feedbacks, cause changes in near-surface climate over Europe. To examine the robustness of the mechanisms we identify in HadGEM2, we analyse similar sets of experiments from NorESM1-M and GFDL-CM3: models with very different climatologies and representations of aerosol processes.

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.

Aqueous-phase mechanism for secondary organic aerosol ...

EPA Pesticide Factsheets

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 observati

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

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

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

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

Collier, Sonya; Zhou, Shan; Onasch, Timothy B.

Abstract Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, wildfire emissions in the Pacific Northwest region of the United States were characterized using real-time measurements near their sources using an aircraft, and farther downwind from a fixed ground site located at the Mt. Bachelor Observatory (~ 2700 m a.s.l.). The characteristics of aerosol emissions were found to depend strongly on the modified combustion efficiency (MCE), a qualitative index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereasmore » the carbon oxidation state of organic aerosol increased with MCE. The relationships between the aerosol properties and MCE were consistent between fresher emissions (~1 hour old) and emissions sampled after atmospheric transport (6 - 45 hours), suggesting that organic aerosol mass loading 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 regionally transported wildfire emissions and their impacts on regional air quality and global climate.« less

Characterization of fresh and aged organic aerosol emissions from meat charbroiling

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

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

DOE PAGES

Grandey, Benjamin S.; Cheng, Haiwen; Wang, Chien

2016-04-06

Fuel usage is an important driver of anthropogenic aerosol emissions. In Asia, it is possible that aerosol 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 as a result of the widespread adoption of cleaner technologies or a shift toward noncoal fuels, such as natural gas. In this study, the transient climate impacts of two aerosol emissions scenarios are investigated: a representative concentration pathway 4.5 (RCP4.5) control, which projects a decrease in anthropogenic aerosol emissions, and a scenario with enhanced anthropogenic aerosolmore » emissions from Asia. A coupled atmosphere–ocean configuration of the Community Earth System Model (CESM), including the Community Atmosphere Model, version 5 (CAM5), is used. Three sets of initial conditions are used to produce a three-member ensemble for each scenario. Enhanced Asian aerosol emissions are found to exert a large cooling effect across the Northern Hemisphere, partially offsetting greenhouse gas–induced warming. 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 Australia, austral summer monsoon precipitation is enhanced, an effect associated with a southward shift of the intertropical convergence zone, driven by the aerosol-induced cooling of the Northern Hemisphere. Over the Sahel, West African monsoon precipitation is suppressed, likely via a weakening of the West African westerly jet. These results indicate that fuel usage in Asia, through the consequent aerosol emissions and associated radiative effects, might significantly influence future climate both locally and globally.« less

Caribbean coral growth influenced by anthropogenic aerosol emissions

NASA Astrophysics Data System (ADS)

Kwiatkowski, Lester; Cox, Peter M.; Economou, Theo; Halloran, Paul R.; Mumby, Peter J.; Booth, Ben B. B.; Carilli, Jessica; Guzman, Hector M.

2013-05-01

Coral growth rates are highly dependent on environmental variables such as sea surface temperature and solar irradiance. Multi-decadal variability in coral growth rates has been documented throughout the Caribbean over the past 150-200 years, and linked to variations in Atlantic sea surface temperatures. Multi-decadal variability in sea surface temperatures in the North Atlantic, in turn, has been linked to volcanic and anthropogenic aerosol forcing. Here, we examine the drivers of changes in coral growth rates in the western Caribbean between 1880 and 2000, using previously published coral growth chronologies from two sites in the region, and a numerical model. Changes in coral growth rates over this period coincided with variations in sea surface temperature and incoming short-wave radiation. Our model simulations show that variations in the concentration of anthropogenic aerosols caused variations in sea surface temperature and incoming radiation in the second half of the twentieth century. Before this, variations in volcanic aerosols may have played a more important role. With the exception of extreme mass bleaching events, we suggest that neither climate change from greenhouse-gas emissions nor ocean acidification is necessarily the driver of multi-decadal variations in growth rates at some Caribbean locations. Rather, the cause may be regional climate change due to volcanic and anthropogenic aerosol emissions.

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.

Experimental Measurements of the Effects of Photo-chemical Oxidation on Aerosol Emissions in Aircraft Exhaust

NASA Astrophysics Data System (ADS)

Miracolo, M. A.; Presto, A. A.; Hennigan, C. J.; Nguyen, N.; Ranjan, M.; Reeder, A.; Lipsky, E.; Donahue, N. M.; Robinson, A. L.

2009-12-01

Many military and commercial airfields are located in non-attainment areas for particulate matter (PM2.5), but the contribution of emissions from in-use aircraft to local and regional PM2.5 concentrations is uncertain. In collaboration with the Pennsylvania Air National Guard 171st Air Refueling Wing, the Carnegie Mellon University (CMU) Mobile Laboratory was deployed to measure fresh and aged emissions from a CFM56-2B1 gas-turbine engine mounted on a KC-135 Stratotanker airframe. The CFM-56 family of engine powers many different types of military and civilian aircraft, including the Boeing 737 and several Airbus models. It is one of the most widely deployed models of engines in the world. The goal of this work was to measure the gas-particle partitioning of the fresh emissions at atmospherically relevant conditions and to investigate the effect of atmospheric oxidation on aerosol loadings as the emissions age. Emissions were sampled from an inlet installed one meter downstream of the engine exit plane and transferred into a portable smog chamber via a heated inlet line. Separate experiments were conducted at different engine loads ranging from ground idle to take-off rated thrust. During each experiment, some diluted exhaust was added to the chamber and the volatility of the fresh emissions was then characterized using a thermodenuder. After this characterization, the chamber was exposed to either ambient sunlight or UV lights to initiate photochemical oxidation, which produced secondary aerosol and ozone. A suite of gas and particle-phase instrumentation was used to characterize the evolution of the gas and particle-phase emissions, including an aerosol mass spectrometer (AMS) to measure particle size and composition distributions. Fresh emissions of fine particles varied with engine load with peak emission factors at low and high loads. At high engine loads, the fresh emissions were dominated by black carbon; at low loads volatile organic carbon emissions were

Highly controlled, reproducible measurements of aerosol emissions from combustion of a common African biofuel source

NASA Astrophysics Data System (ADS)

Haslett, Sophie L.; Thomas, J. Chris; Morgan, William T.; Hadden, Rory; Liu, Dantong; Allan, James D.; Williams, Paul I.; Keita, Sekou; Liousse, Cathy; Coe, Hugh

2018-01-01

Particulate emissions from biomass burning can both alter the atmosphere's radiative balance and cause significant harm to human health. However, due to the large effect on emissions caused by even small alterations to the way in which a fuel burns, it is difficult to study particulate production of biomass combustion mechanistically and in a repeatable manner. In order to address this gap, in this study, small wood samples sourced from Côte D'Ivoire in West Africa were burned in a highly controlled laboratory environment. The shape and mass of samples, available airflow and surrounding thermal environment were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. This methodology produced remarkably repeatable results, allowing aerosol emissions to be mapped directly onto different phases of combustion. Emissions from pyrolysis were visible as a distinct phase before flaming was established. After flaming combustion was initiated, a black-carbon-dominant flame was observed during which very little organic aerosol was produced, followed by a period that was dominated by organic-carbon-producing smouldering combustion, despite the presence of residual flaming. During pyrolysis and smouldering, the two phases producing organic aerosol, distinct mass spectral signatures that correspond to previously reported variations in biofuel emissions measured in the atmosphere are found. Organic aerosol emission factors averaged over an entire combustion event were found to be representative of the time spent in the pyrolysis and smouldering phases, rather than reflecting a coupling between emissions and the mass loss of the sample. Further exploration of aerosol yields from similarly carefully controlled fires and a careful comparison with data from macroscopic fires and real-world emissions will help to deliver greater constraints on the

Global radiative effects of solid fuel cookstove aerosol emissions

NASA Astrophysics Data System (ADS)

Huang, Yaoxian; Unger, Nadine; Storelvmo, Trude; Harper, Kandice; Zheng, Yiqi; Heyes, Chris

2018-04-01

We apply the NCAR CAM5-Chem global aerosol-climate model to quantify the net global radiative effects of black and organic carbon aerosols from global and Indian solid fuel cookstove emissions for the year 2010. Our assessment accounts for the direct radiative effects, changes to cloud albedo and lifetime (aerosol indirect effect, AIE), impacts on clouds via the vertical temperature profile (semi-direct effect, SDE) and changes in the surface albedo of snow and ice (surface albedo effect). In addition, we provide the first estimate of household solid fuel black carbon emission effects on ice clouds. Anthropogenic emissions are from the IIASA GAINS ECLIPSE V5a inventory. A global dataset of black carbon (BC) and organic aerosol (OA) measurements from surface sites and aerosol optical depth (AOD) from AERONET is used to evaluate the model skill. Compared with observations, the model successfully reproduces the spatial patterns of atmospheric BC and OA concentrations, and agrees with measurements to within a factor of 2. Globally, the simulated AOD agrees well with observations, with a normalized mean bias close to zero. However, the model tends to underestimate AOD over India and China by ˜ 19 ± 4 % but overestimate it over Africa by ˜ 25 ± 11 % (± represents modeled temporal standard deviations for n = 5 run years). Without BC serving as ice nuclei (IN), global and Indian solid fuel cookstove aerosol emissions have net global cooling radiative effects of -141 ± 4 mW m-2 and -12 ± 4 mW m-2, respectively (± represents modeled temporal standard deviations for n = 5 run years). The net radiative impacts are dominated by the AIE and SDE mechanisms, which originate from enhanced cloud condensation nuclei concentrations for the formation of liquid and mixed-phase clouds, and a suppression of convective transport of water vapor from the lower troposphere to the upper troposphere/lower stratosphere that in turn leads to reduced ice cloud formation. When BC is allowed

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

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

Collier, Sonya; Zhou, Shan; Onasch, Timothy B.

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. In addition, the regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), anmore » 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. In conclusion, 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.« less

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

DOE PAGES

Collier, Sonya; Zhou, Shan; Onasch, Timothy B.; ...

2016-07-11

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. In addition, the regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), anmore » 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. In conclusion, 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.« less

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.

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).

Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM)

NASA Astrophysics Data System (ADS)

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

2016-03-01

Accurate representation of global stratospheric aerosols from volcanic and nonvolcanic 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 2014 and developed a new prognostic capability for simulating stratospheric sulfate aerosols in the Community Earth System Model. We used these combined with other nonvolcanic emissions of sulfur sources to reconstruct global aerosol properties from 1990 to 2014. 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 middle 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.

Atmospheric Aerosol Emissions Related to the Mediterranean Seawater Biogeochemistry

NASA Astrophysics Data System (ADS)

Sellegri, K.; Schwier, A.; Rose, C.; Gazeau, F. P. H.; Guieu, C.; D'anna, B.; Ebling, A. M.; Pey, J.; Marchand, N.; Charriere, B.; Sempéré, R.; Mas, S.

2016-02-01

Marine aerosols contribute significantly to the global aerosol load and consequently has an important impact on the Earth's climate. Different factors influence the way they are produced at the air/seawater interface. The sea state (whitecap coverage, temperature, etc. ) influence the size and concentration of primarily produced particles but also biogeochemical characteristics of the seawater influence both the physical and chemical primary fluxes to the atmosphere. An additional aerosol source of marine aerosol to the atmosphere is the formation of new particles by gaz-to-particle conversion, i.e. nucleation. How the seawater and surface microlayer biogeochemical compositions influences the aerosol emissions is still a large debate. In order to study marine emissions, one approach is to use semi-controlled environments such as mesocosms. Within the MedSea and SAM projects, we characterize the primary Sea Spray Aerosol (SSA) during mesocosms experiments performed during different seasons in the Mediteranean Sea. Mesocosms were either left unchanged as control or enriched by addition of nutriments in order to create different levels of phytoplanctonic activities. The mesocosms waters were daily analyzed for their chemical and biological composition (DOC, CDOM, TEP, Chl-a, virus, bacteria, phytoplankton and zooplankton concentrations). SSA production by bubble bursting was daily simulated in a dedicated set-up. The size segregated SSA number fluxes, cloud condensation nuclei (CCN) properties, and chemical composition were determined as a function of the seawater characteristics. We show that the SSA organic content was clearly correlated to the seawater Chl-a level, provided that the mesocosm was not enriched to create an artificial phytoplanctonic bloom. In our experiments, the enrichment of the seawater with natural surface microlayer did not impact the SSA organic content nor its CCN properties. At last, nucleation of secondary particles were observed to occur in

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

On the future of carbonaceous aerosol emissions

NASA Astrophysics Data System (ADS)

Streets, D. G.; Bond, T. C.; Lee, T.; Jang, C.

2004-12-01

This paper presents the first model-based forecasts of future emissions of the primary carbonaceous aerosols, black carbon (BC) and organic carbon (OC). The forecasts build on a recent 1996 inventory of emissions that contains detailed fuel, technology, sector, and world-region specifications. The forecasts are driven by four IPCC scenarios, A1B, A2, B1, and B2, out to 2030 and 2050, incorporating not only changing patterns of fuel use but also technology development. Emissions from both energy generation and open biomass burning are included. We project that global BC emissions will decline from 8.0 Tg in 1996 to 5.3-7.3 Tg by 2030 and to 4.3-6.1 Tg by 2050, across the range of scenarios. We project that OC emissions will decline from 34 Tg in 1996 to 24-30 Tg by 2030 and to 21-28 Tg by 2050. The introduction of advanced technology with lower emission rates, as well as a shift away from the use of traditional solid fuels in the residential sector, more than offsets the increased combustion of fossil fuels worldwide. Environmental pressures and a diminishing demand for new agricultural land lead to a slow decline in the amount of open biomass burning. Although emissions of BC and OC are generally expected to decline around the world, some regions, particularly South America, northern Africa, the Middle East, South Asia, Southeast Asia, and Oceania, show increasing emissions in several scenarios. Particularly difficult to control are BC emissions from the transport sector, which increase under most scenarios. We expect that the BC/OC emission ratio for energy sources will rise from 0.5 to as much as 0.8, signifying a shift toward net warming of the climate system due to carbonaceous aerosols. When biomass burning is included, however, the BC/OC emission ratios are for the most part invariant across scenarios at about 0.2.

Characterising Brazilian biomass burning emissions using WRF-Chem with MOSAIC sectional aerosol

NASA Astrophysics Data System (ADS)

Archer-Nicholls, S.; Lowe, D.; Darbyshire, E.; Morgan, W. T.; Bela, M. M.; Pereira, G.; Trembath, J.; Kaiser, J. W.; Longo, K. M.; Freitas, S. R.; Coe, H.; McFiggans, G.

2015-03-01

The South American Biomass Burning Analysis (SAMBBA) field campaign took detailed in situ flight measurements of aerosol during the 2012 dry season to characterise biomass burning aerosol and improve understanding of its impacts on weather and climate. Developments have been made to the Weather Research and Forecast model with chemistry (WRF-Chem) model to improve the representation of biomass burning aerosol in the region, by coupling a sectional aerosol scheme to the plume-rise parameterisation. Brazilian Biomass Burning Emissions Model (3BEM) fire emissions are used, prepared using PREP-CHEM-SRC, and mapped to CBM-Z and MOSAIC species. Model results have been evaluated against remote sensing products, AERONET sites, and four case studies of flight measurements from the SAMBBA campaign. WRF-Chem predicted layers of elevated aerosol loadings (5-20 μg sm-3) of particulate organic matter at high altitude (6-8 km) over tropical forest regions, while flight measurements showed a sharp decrease above 2-4 km altitude. This difference was attributed to the plume-rise parameterisation overestimating injection height. The 3BEM emissions product was modified using estimates of active fire size and burned area for the 2012 fire season, which reduced the fire size. The enhancement factor for fire emissions was increased from 1.3 to 5 to retain reasonable aerosol optical depths (AODs). The smaller fire size lowered the injection height of the emissions, but WRF-Chem still showed elevated aerosol loadings between 4-5 km altitude. Over eastern cerrado (savannah-like) regions, both modelled and measured aerosol loadings decreased above approximately 4 km altitude. Compared with MODIS satellite data and AERONET sites, WRF-Chem represented AOD magnitude well (between 0.3-1.5) over western tropical forest fire regions in the first half of the campaign, but tended to over-predict them in the second half, when precipitation was more significant. Over eastern cerrado regions, WRF

Characterising Brazilian biomass burning emissions using WRF-Chem with MOSAIC sectional aerosol

NASA Astrophysics Data System (ADS)

Archer-Nicholls, S.; Lowe, D.; Darbyshire, E.; Morgan, W. T.; Bela, M. M.; Pereira, G.; Trembath, J.; Kaiser, J. W.; Longo, K. M.; Freitas, S. R.; Coe, H.; McFiggans, G.

2014-09-01

The South American Biomass Burning Analysis (SAMBBA) field campaign took detailed in-situ flight measurements of aerosol during the 2012 dry season to characterise biomass burning aerosol and improve understanding of its impacts on weather and climate. Developments have been made to the Weather research and Forecast model with chemistry (WRF-Chem) model to improve the representation of biomass burning aerosol in the region by coupling a sectional aerosol scheme to the plume rise parameterisation. Brazilian Biomass Burning Emissions Model (3BEM) fire emissions are used, prepared using PREP-CHEM-SRC, and mapped to CBM-Z and MOSAIC species. Model results have been evaluated against remote sensing products, AERONET sites, and four case studies of flight measurements from the SAMBBA campaign. WRF-Chem predicted layers of elevated aerosol loadings (5-20 μg sm-3) of particulate organic matter at high altitude (6-8 km) over tropical forest regions, while flight measurements showed a sharp decrease above 2-4 km altitude. This difference was attributed to the plume-rise parameterisation overestimating injection height. The 3BEM emissions product was modified using estimates of active fire size and burned area for the 2012 fire season, which reduced the fire size. The enhancement factor for fire emissions was increased from 1.3 to 5 to retain reasonable aerosol optical depths (AOD). The smaller fire size lowered the injection height of the emissions, but WRF-Chem still showed elevated aerosol loadings between 4-5 km altitude. Over eastern Cerrado (savannah-like) regions, both modelled and measured aerosol loadings decreased above approximately 4 km altitude. Compared with MODIS satellite data and AERONET sites, WRF-Chem represented AOD magnitude well (between 0.3-1.5) over western tropical forest fire regions in the first half of the campaign, but tended to over-predict them in the second half, when precipitation was more significant. Over eastern Cerrado regions, WRF

Traffic is a major source of atmospheric nanocluster aerosol

PubMed Central

Kuuluvainen, Heino; Karjalainen, Panu; Keskinen, Jorma; Hillamo, Risto; Niemi, Jarkko V.; Pirjola, Liisa; Timonen, Hilkka J.; Saarikoski, Sanna; Saukko, Erkka; Järvinen, Anssi; Silvennoinen, Henna; Rostedt, Antti; Olin, Miska; Yli-Ojanperä, Jaakko; Nousiainen, Pekka; Kousa, Anu; Dal Maso, Miikka

2017-01-01

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3–3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20–54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)−1 in a roadside environment, 2.6·1015 (kgfuel)−1 in a street canyon, and 2.9·1015 (kgfuel)−1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)−1 to a high value of 4.3·1015 (kgfuel)−1. These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds. PMID:28674021

Traffic is a major source of atmospheric nanocluster aerosol.

PubMed

Rönkkö, Topi; Kuuluvainen, Heino; Karjalainen, Panu; Keskinen, Jorma; Hillamo, Risto; Niemi, Jarkko V; Pirjola, Liisa; Timonen, Hilkka J; Saarikoski, Sanna; Saukko, Erkka; Järvinen, Anssi; Silvennoinen, Henna; Rostedt, Antti; Olin, Miska; Yli-Ojanperä, Jaakko; Nousiainen, Pekka; Kousa, Anu; Dal Maso, Miikka

2017-07-18

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·10 15 (kg fuel ) -1 in a roadside environment, 2.6·10 15 (kg fuel ) -1 in a street canyon, and 2.9·10 15 (kg fuel ) -1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·10 12 (kg fuel ) -1 to a high value of 4.3·10 15 (kg fuel ) -1 These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Transitions from functionalization to fragmentation reactions of laboratory secondary organic aerosol (SOA) generated from the OH oxidation of alkane precursors.

PubMed

Lambe, Andrew T; Onasch, Timothy B; Croasdale, David R; Wright, Justin P; Martin, Alexander T; Franklin, Jonathan P; Massoli, Paola; Kroll, Jesse H; Canagaratna, Manjula R; Brune, William H; Worsnop, Douglas R; Davidovits, Paul

2012-05-15

Functionalization (oxygen addition) and fragmentation (carbon loss) reactions governing secondary organic aerosol (SOA) formation from the OH oxidation of alkane precursors were studied in a flow reactor in the absence of NO(x). SOA precursors were n-decane (n-C10), n-pentadecane (n-C15), n-heptadecane (n-C17), tricyclo[5.2.1.0(2,6)]decane (JP-10), and vapors of diesel fuel and Southern Louisiana crude oil. Aerosol mass spectra were measured with a high-resolution time-of-flight aerosol mass spectrometer, from which normalized SOA yields, hydrogen-to-carbon (H/C) and oxygen-to-carbon (O/C) ratios, and C(x)H(y)+, C(x)H(y)O+, and C(x)H(y)O(2)+ ion abundances were extracted as a function of OH exposure. Normalized SOA yield curves exhibited an increase followed by a decrease as a function of OH exposure, with maximum yields at O/C ratios ranging from 0.29 to 0.74. The decrease in SOA yield correlates with an increase in oxygen content and decrease in carbon content, consistent with transitions from functionalization to fragmentation. For a subset of alkane precursors (n-C10, n-C15, and JP-10), maximum SOA yields were estimated to be 0.39, 0.69, and 1.1. In addition, maximum SOA yields correspond with a maximum in the C(x)H(y)O+ relative abundance. Measured correlations between OH exposure, O/C ratio, and H/C ratio may enable identification of alkane precursor contributions to ambient SOA.

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

Aerosol Emissions from Fuse-Deposition Modeling 3D Printers in a Chamber and in Real Indoor Environments.

PubMed

Vance, Marina E; Pegues, Valerie; Van Montfrans, Schuyler; Leng, Weinan; Marr, Linsey C

2017-09-05

Three-dimensional (3D) printers are known to emit aerosols, but questions remain about their composition and the fundamental processes driving emissions. The objective of this work was to characterize the aerosol emissions from the operation of a fuse-deposition modeling 3D printer. We modeled the time- and size-resolved emissions of submicrometer aerosols from the printer in a chamber study, gained insight into the chemical composition of emitted aerosols using Raman spectroscopy, and measured the potential for exposure to the aerosols generated by 3D printers under real-use conditions in a variety of indoor environments. The average aerosol emission rates ranged from ∼10 8 to ∼10 11 particles min -1 , and the rates varied over the course of a print job. Acrylonitrile butadiene styrene (ABS) filaments generated the largest number of aerosols, and wood-infused polylactic acid (PLA) filaments generated the smallest amount. The emission factors ranged from 6 × 10 8 to 6 × 10 11 per gram of printed part, depending on the type of filament used. For ABS, the Raman spectra of the filament and the printed part were indistinguishable, while the aerosol spectra lacked important peaks corresponding to styrene and acrylonitrile, which are both present in ABS. This observation suggests that aerosols are not a result of volatilization and subsequent nucleation of ABS or direct release of ABS aerosols.

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

SOURCES OF ORGANIC AEROSOL: SEMIVOLATILE EMISSIONS AND PHOTOCHEMICAL AGING

EPA Science Inventory

The proposed research integrates emissions testing, smog chamber experiments, and regional chemical transport models (CTMs) to investigate the sources of organic aerosol in urban and regional environments.

Limited Effect of Anthropogenic Nitrogen Oxides on Secondary Organic Aerosol Formation

NASA Astrophysics Data System (ADS)

Zheng, Y.; Unger, N.; Hodzic, A.; Knote, C. J.; Tilmes, S.; Emmons, L. K.; Lamarque, J. F.; Yu, P.

2014-12-01

Globally secondary organic aerosol (SOA) is mostly formed from biogenic vegetation emissions and as such is regarded as natural aerosol that cannot be reduced by emission control legislation. However, recent research implies that human activities facilitate SOA formation by affecting the amount of precursor emission, the chemical processing and the partitioning into the aerosol phase. Among the multiple human influences, nitrogen oxides (NO + NO2 = NOx) have been assumed to play a critical role in the chemical formation of low volatile compounds. The goal of this study is to improve the SOA scheme in the global NCAR Community Atmospheric Model version 4 with chemistry (CAM4-Chem) by implementing an updated 4-product Volatility Basis Set (VBS) scheme, and apply it to investigate the impact of anthropogenic NOx on SOA. We first compare three different SOA parameterizations: a 2-product model and the updated VBS model both with and without a SOA aging parameterization. Secondly we evaluate predicted organic aerosol amounts against surface measurement from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network and Aerosol Mass Spectrometer (AMS) measurements from 13 aircraft-based field campaigns. We then perform sensitivity experiments to examine how the SOA loading responds to a 50% reduction in anthropogenic NOx in different regions. We find limited SOA reductions of -2.3%, -5.6% and -4.0% for global, southeastern U.S. and Amazon NOx perturbations, respectively. To investigate the chemical processes in more detail, we also use a simplified box model with the same gas-phase chemistry and gas-aerosol partitioning mechanism as in CAM4-Chem to examine the SOA yields dependence on initial precursor emissions and background NOx level. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to buffering in chemical pathways (low- versus high-NOx pathways, OH versus NO3-initiated oxidation) and to offsetting

Decadal-scale trends in regional aerosol particle properties and their linkage to emission changes

NASA Astrophysics Data System (ADS)

Zhao, Bin; Jiang, Jonathan H.; Gu, Yu; Diner, David; Worden, John; Liou, Kuo-Nan; Su, Hui; Xing, Jia; Garay, Michael; Huang, Lei

2017-05-01

Understanding long-term trends in aerosol loading and properties is essential for evaluating the health and climatic effects of these airborne particulates as well as the effectiveness of pollution control policies. While many studies have used satellite data to examine the trends in aerosol optical depth (AOD), very few have investigated the trends in aerosol properties associated with particle size, morphology, and light absorption. In this study, we investigate decadal-scale (13-15 year) trends in aerosol loading and properties during 2001-2015 over three populous regions: the Eastern United States (EUS), Western Europe (WEU), and Eastern and Central China (ECC). We use observations from MISR (Multi-angle Imaging SpectroRadiometer) and MODIS (Moderate resolution Imaging Spectroradiometer). Relationships between aerosol property trends and air pollutant emission changes are examined. We find that annual mean AOD shows pronounced decreasing trends over EUS and WEU regions, as a result of considerable emission reductions in all major pollutants except for mineral dust and ammonia (NH3). Over the ECC region, AOD increases before 2006 due to emission increases induced by rapid economic development, fluctuates between 2006 and 2011, and subsequently decreases after 2011 in conjunction with effective emission reduction in anthropogenic primary aerosols, sulfur dioxide (SO2), and nitrogen oxides (NOx). The fraction of small-size AOD (<0.7 μm diameter), Ångstrom exponent and single-scattering albedo have generally decreased, while the fractions of large-size (>1.4 μm diameter), nonspherical and absorbing AOD have generally shown increasing trends over EUS and WEU regions, indicating that fine and light-scattering aerosol constituents have been more effectively reduced than coarse and light-absorbing constituents. These trends are consistent with the larger reduction ratios in SO2 and NOx emissions than in primary aerosols, including mineral dust and black carbon (BC

Precursor Wave Emission Enhanced by Weibel Instability in Relativistic Shocks

NASA Astrophysics Data System (ADS)

Iwamoto, Masanori; Amano, Takanobu; Hoshino, Masahiro; Matsumoto, Yosuke

2018-05-01

We investigated the precursor wave emission efficiency in magnetized purely perpendicular relativistic shocks in pair plasmas. We extended our previous study to include the dependence of upstream magnetic field orientations. We performed two-dimensional particle-in-cell simulations and focused on two magnetic field orientations: the magnetic field in the simulation plane (i.e., in-plane configuration) and that perpendicular to the simulation plane (i.e., out-of-plane configuration). Our simulations in the in-plane configuration demonstrated that not only extraordinary but also ordinary mode waves are excited. We quantified the emission efficiency as a function of the magnetization parameter σ e and found that the large-amplitude precursor waves are emitted for a wide range of σ e . We found that especially at low σ e , the magnetic field generated by Weibel instability amplifies the ordinary mode wave power. The amplitude is large enough to perturb the upstream plasma, and transverse density filaments are generated as in the case of the out-of-plane configuration investigated in the previous study. We confirmed that our previous conclusion holds regardless of upstream magnetic field orientations with respect to the two-dimensional simulation plane. We discuss the precursor wave emission in three dimensions and the feasibility of wakefield acceleration in relativistic shocks based on our results.

Aerosol impacts on regional trends in atmospheric stagnation

NASA Astrophysics Data System (ADS)

Mascioli, N. R.; Fiore, A. M.; Previdi, M. J.

2017-12-01

Extreme pollution events pose a significant threat to human health and are a leading cause of premature mortality worldwide. While emissions of atmospheric pollutants and their precursors are projected to decrease in the future due to air quality legislation, future climate change may affect the underlying meteorological conditions that contribute to extreme pollution events. Stagnation events, characterized by weak winds and an absence of precipitation, contribute to extreme pollution by halting the removal of pollutants via advection and wet deposition. Here, we use a global climate model (GFDL-CM3) to show that regional stagnation trends over the historical period (1860-2005) are driven by changes in anthropogenic aerosol emissions, rather than rising greenhouse gases. In the northeastern and central United States, aerosol-induced changes in surface and upper level winds have produced significant decreases in the number of stagnant summer days, while decreasing precipitation in the southeast US has increased the number of stagnant summer days. Significant drying over eastern China in response to aerosol forcing contributed to increased stagnation. Additionally, this region was found to be particularly sensitive to changes in local emissions, indicating that improving air quality will also lessen stagnation. In Europe, we find a dipole pattern wherein stagnation decreases over southern Europe and increases over northern Europe in response to global increases in aerosol emissions. We hypothesize that this is due to changes in the large-scale circulation patterns associated with a poleward shift of the North Atlantic storm track. We find that in the future, the combination of declining aerosol emissions and the continued rise of greenhouse gas emissions will lead to a reversal of the historical stagnation trends.

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

2002-06-06

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.

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

Developing and diagnosing climate change indictors of regional aerosol optical properties

NASA Astrophysics Data System (ADS)

Sullivan, Ryan C.; Levy, Robert C.; da Silva, Arlindo M.; Pryor, Sara C.

2017-04-01

The US Global Change Research Program has developed climate indicators (CIs) to track changes in the physical, chemical, biological, and societal components of the climate system. Given the importance of atmospheric aerosol particles to clouds and radiative forcing, human mortality and morbidity, and biogeochemical cycles, we propose new aerosol particle CIs applicable to the US National Climate Assessment (NCA). Here we define these aerosol CIs and use them to quantify temporal trends in each NCA region. Furthermore, we use a synoptic classification (e.g., meteorological variables), and gas and particle emissions inventories to diagnose and attribute causes of observed changes. Our CIs are derived using output from the satellite-constrained Modern-Era Retrospective Analysis for Research and Application, Version 2 (MERRA-2) reanalysis. MERRA-2 provides estimates of column-integrated aerosol optical properties at 0.625° by 0.5° resolution, including aerosol optical depth (AOD), Ångström exponent (AE), and single scattering albedo (SSA), which are related to aerosol loading, relative particle size, and chemical composition, respectively. For each NCA region, and for each aerosol variable, we derive statistics that describe mean and extreme values, as well as two metrics (spatial autocorrelation and coherence) that describe the spatial scales of aerosol variability. Consistent with previous analyses of aerosol precursor emissions and near-surface fine aerosol mass concentrations in the US, analyses of our aerosol CIs show that since 2000, both mean and extreme AOD have decreased over most NCA regions. There are significant (α = 0.05, using the non-parametric Kendall's tau) decreases in AOD for the Northeast (NE), Southeast (SE), Midwest (MW), and lower Great Plains (GPl) regions, and notable but not significant decreases in the Southwest (SW). AOD has increased for the Northwest (NW; significant) and upper Great Plains (GPu; not significant). Over all regions

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.

Impacts of Lowered Urban Air Temperatures on Precursor Emission and Ozone Air Quality.

PubMed

Taha, Haider; Konopacki, Steven; Akbari, Hashem

1998-09-01

Meteorological, photochemical, building-energy, and power plant simulations were performed to assess the possible precursor emission and ozone air quality impacts of decreased air temperatures that could result from implementing the "cool communities" concept in California's South Coast Air Basin (SoCAB). Two pathways are considered. In the direct pathway, a reduction in cooling energy use translates into reduced demand for generation capacity and, thus, reduced precursor emissions from electric utility power plants. In the indirect pathway, reduced air temperatures can slow the atmospheric production of ozone as well as precursor emission from anthropogenic and biogenic sources. The simulations suggest small impacts on emissions following implementation of cool communities in the SoCAB. In summer, for example, there can be reductions of up to 3% in NO x emissions from in-basin power plants. The photochemical simulations suggest that the air quality impacts of these direct emission reductions are small. However, the indirect atmospheric effects of cool communities can be significant. For example, ozone peak concentrations can decrease by up to 11% in summer and population-weighted exceedance exposure to ozone above the California and National Ambient Air Quality Standards can decrease by up to 11 and 17%, respectively. The modeling suggests that if these strategies are combined with others, such as mobile-source emission control, the improvements in ozone air quality can be substantial.

Chemical composition of ambient PM2. 5 over China and relationship to precursor emissions during 2005-2012

NASA Astrophysics Data System (ADS)

Geng, Guannan; Zhang, Qiang; Tong, Dan; Li, Meng; Zheng, Yixuan; Wang, Siwen; He, Kebin

2017-07-01

In this work, we presented the characteristics of PM2. 5 chemical composition over China for the period of 2005-2012 by synthesis of in situ measurement data collected from literatures and satellite-based estimates using aerosol optical depth (AOD) data and the GEOS-Chem chemical transport model. We revealed the spatiotemporal variations in PM2. 5 composition during 2005-2012 and investigated the driving forces behind the variations by examining the changes in precursor emissions using a bottom-up emission inventory. Both in situ observations and satellite-based estimates identified that secondary inorganic aerosols (i.e., sulfate, nitrate, and ammonium; SNA) ranked as the highest fraction of dust-free PM2. 5 concentrations, followed by organic matter (OM) and black carbon (BC). For instance, satellite-based estimates found that SNA, OM, and BC contributed to 59, 33, and 8 %, respectively, of national population-weighted mean dust-free PM2. 5 concentrations during 2005-2012. National population-weighted mean PM2. 5 concentration increased from 63.9 µg m-3 in 2005 to 75.2 µg m-3 in 2007 and subsequently decreased to 66.9 µg m-3 from 2007 to 2012. Variations in PM2. 5 concentrations are mainly driven by the decrease in sulfate and the increase in nitrate. Population-weighted mean sulfate concentration decreased by 2.4 % yr-1 during 2005-2012 (from 14.4 to 12.9 µg m-3), while population-weighted mean nitrate concentration increased by 3.4 % yr-1 during 2005-2012 (from 9.8 to 12.2 µg m-3), largely offsetting the decrease in sulfate concentrations. By examining the emission data from the Multi-resolution Emission Inventory for China (MEIC), we found that the changes in sulfate and nitrate concentrations were in line with the decrease in SO2 emissions and the increase in NOx emissions during the same period. The desulfurization regulation in power plants enforced around 2005 has been the primary contributor to the SO2 emission reduction since 2006. In contrast

Inverse modeling and mapping US air quality influences of inorganic PM2.5 precursor emissions using the adjoint of GEOS-Chem

NASA Astrophysics Data System (ADS)

Henze, D. K.; Seinfeld, J. H.; Shindell, D. T.

2009-08-01

Influences of specific sources of inorganic PM2.5 on peak and ambient aerosol concentrations in the US are evaluated using a combination of inverse modeling and sensitivity analysis. First, sulfate and nitrate aerosol measurements from the IMPROVE network are assimilated using the four-dimensional variational (4D-Var) method into the GEOS-Chem chemical transport model in order to constrain emissions estimates in four separate month-long inversions (one per season). Of the precursor emissions, these observations primarily constrain ammonia (NH3). While the net result is a decrease in estimated US~NH3 emissions relative to the original inventory, there is considerable variability in adjustments made to NH3 emissions in different locations, seasons and source sectors, such as focused decreases in the midwest during July, broad decreases throughout the US~in January, increases in eastern coastal areas in April, and an effective redistribution of emissions from natural to anthropogenic sources. Implementing these constrained emissions, the adjoint model is applied to quantify the influences of emissions on representative PM2.5 air quality metrics within the US. The resulting sensitivity maps display a wide range of spatial, sectoral and seasonal variability in the susceptibility of the air quality metrics to absolute emissions changes and the effectiveness of incremental emissions controls of specific source sectors. NH3 emissions near sources of sulfur oxides (SOx) are estimated to most influence peak inorganic PM2.5 levels in the East; thus, the most effective controls of NH3 emissions are often disjoint from locations of peak NH3 emissions. Controls of emissions from industrial sectors of SOx and NOx are estimated to be more effective than surface emissions, and changes to NH3 emissions in regions dominated by natural sources are disproportionately more effective than regions dominated by anthropogenic sources. NOx controls are most effective in northern states in

Inverse modeling and mapping US air quality influences of inorganic PM2.5 precursor emissions using the adjoint of GEOS-Chem

NASA Astrophysics Data System (ADS)

Henze, D. K.; Seinfeld, J. H.; Shindell, D. T.

2008-08-01

Influences of specific sources of inorganic PM2.5 on peak and ambient aerosol concentrations in the US are evaluated using a combination of inverse modeling and sensitivity analysis. First, sulfate and nitrate aerosol measurements from the IMPROVE network are assimilated using the four-dimensional variational (4D-Var) method into the GEOS-Chem chemical transport model in order to constrain emissions estimates in four separate month-long inversions (one per season). Of the precursor emissions, these observations primarily constrain ammonia (NH3). While the net result is a decrease in estimated US NH3 emissions relative to the original inventory, there is considerable variability in adjustments made to NH3 emissions in different locations, seasons and source sectors, such as focused decreases in the midwest during July, broad decreases throughout the US~in January, increases in eastern coastal areas in April, and an effective redistribution of emissions from natural to anthropogenic sources. Implementing these constrained emissions, the adjoint model is applied to quantify the influences of emissions on representative PM2.5 air quality metrics within the US. The resulting sensitivity maps display a wide range of spatial, sectoral and seasonal variability in the susceptibility of the air quality metrics to absolute emissions changes and the effectiveness of incremental emissions controls of specific source sectors. NH3 emissions near sources of sulfur oxides (SOx) are estimated to most influence peak inorganic PM2.5 levels in the East; thus, the most effective controls of NH3 emissions are often disjoint from locations of peak NH3 emissions. Controls of emissions from industrial sectors of SOx and NOx are estimated to be more effective than surface emissions, and changes to NH3 emissions in regions dominated by natural sources are disproportionately more effective than regions dominated by anthropogenic sources. NOx controls are most effective in northern states in

Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

NASA Astrophysics Data System (ADS)

Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

2014-12-01

Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

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.

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

The economics (or lack thereof) of aerosol geoengineering

NASA Astrophysics Data System (ADS)

Goes, M.; Keller, K.; Tuana, N.

2009-04-01

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 the deployment of a different approach: to geoengineer climate by injecting aerosol precursors into the stratosphere. Published economic studies typically suggest that substituting aerosol geoengineering for abatement of carbon dioxide emissions results in large net monetary benefits. However, these studies neglect the risks of aerosol geoengineering due to (i) the potential for future geoengineering failures and (ii) the negative impacts associated with the aerosol forcing. 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 forcing. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes severe caveats on the interpretation of the results. For example, the analysis is based on a globally aggregated model and is hence silent on the question of intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of endogenous learning about the climate system. We show that the risks associated with a future geoengineering failure and negative impacts of aerosol forcings can cause geoenginering strategies to fail an economic cost-benefit test. One key to this finding is that a geoengineering failure would lead to dramatic and abrupt climatic changes. The monetary damages due to this failure can

Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass

NASA Astrophysics Data System (ADS)

Bahreini, R.; Middlebrook, A. M.; de Gouw, J. A.; Warneke, C.; Trainer, M.; Brock, C. A.; Stark, H.; Brown, S. S.; Dube, W. P.; Gilman, J. B.; Hall, K.; Holloway, J. S.; Kuster, W. C.; Perring, A. E.; Prevot, A. S. H.; Schwarz, J. P.; Spackman, J. R.; Szidat, S.; Wagner, N. L.; Weber, R. J.; Zotter, P.; Parrish, D. D.

2012-03-01

Although laboratory experiments have shown that organic compounds in both gasoline fuel and diesel engine exhaust can form secondary organic aerosol (SOA), the fractional contribution from gasoline and diesel exhaust emissions to ambient SOA in urban environments is poorly known. Here we use airborne and ground-based measurements of organic aerosol (OA) in the Los Angeles (LA) Basin, California made during May and June 2010 to assess the amount of SOA formed from diesel emissions. Diesel emissions in the LA Basin vary between weekdays and weekends, with 54% lower diesel emissions on weekends. Despite this difference in source contributions, in air masses with similar degrees of photochemical processing, formation of OA is the same on weekends and weekdays, within the measurement uncertainties. This result indicates that the contribution from diesel emissions to SOA formation is zero within our uncertainties. Therefore, substantial reductions of SOA mass on local to global scales will be achieved by reducing gasoline vehicle emissions.

Modeling Trends in Aerosol Direct Radiative Effects over the Northern Hemisphere using a Coupled Meteorology-Chemistry Model

NASA Astrophysics Data System (ADS)

Mathur, R.; Pleim, J.; Wong, D.; Hogrefe, C.; Xing, J.; Wei, C.; Gan, M.

2013-12-01

While aerosol radiative effects have been recognized as some of the largest sources of uncertainty among the forcers of climate change, the verification of the spatial and temporal variability of the magnitude and directionality of aerosol radiative forcing has remained challenging. A detailed investigation of the processes regulating aerosol distributions, their optical properties, and their radiative effects and verification of their simulated effects for past conditions relative to measurements is needed in order to build confidence in the estimates of the projected impacts arising from changes in both anthropogenic forcing and climate change. Anthropogenic emissions of primary aerosol and gaseous precursors have witnessed dramatic changes over the past two decades across the northern hemisphere. During the period 1990-2010, SO2 and NOx emissions across the US have reduced by about 66% and 50%, respectively, mainly due to Title IV of the U.S. Clean Air Act Amendments (CAA). In contrast, anthropogenic emissions have increased dramatically in many developing regions during this period. We conduct a systematic investigation of changes in anthropogenic emissions of primary aerosols and gaseous precursors over the past two decades, their impacts on trends and spatial heterogeneity in anthropogenic aerosol loading across the northern hemisphere troposphere, and subsequent impacts on regional radiation budgets. The coupled WRF-CMAQ model is applied for selected time periods spanning the period 1990-2010 over a domain covering the northern hemisphere and a nested finer resolution continental U.S. domain. The model includes detailed treatment of direct effects of aerosols on photolysis rates as well as on shortwave radiation. Additionally, treatment of aerosol indirect effects on clouds has also recently been implemented. A methodology is developed to consistently estimate U.S. emission inventories for the 20-year period accounting for air quality regulations as well as

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.

Investigating the Climatic Impacts of Globally Shifted Anthropogenic Emissions

NASA Astrophysics Data System (ADS)

Wang, Y.; Jiang, J. H.; Su, H.

2014-12-01

With a quasi-exponential growth in industrialization since the mid-1990s, Asia has undergone a dramatic increase in anthropogenic emissions of aerosol and precursor gases to the atmosphere. Meanwhile, such emissions have been stabilized or reduced over North America and Europe. This geographical shift of global emission sources could potentially perturb the regional and global climate due to impact of aerosols on cloud properties, precipitation, and large-scale circulation. We use an atmospheric general circulation model (AGCM) with different aerosol scenarios to investigate the radiative and microphysical effects of anthropogenic aerosols on the large-scale circulation and regional climate over the globe. We conduct experiments to simulate the continental shift of aerosol distribution by contrasting two simulations using 1970 and 2010 anthropogenic emission sources. We found the elevation of aerosol concentrations in East and South Asia results in regional surface temperature cooling of -0.10° to -0.17°C, respectively, due to the enhanced solar extinction by aerosols and cloud reflectivity. The reduction of the local aerosol loadings in Europe causes a significant warming of +0.4°C. However, despite recent decreasing in aerosol emission, North America shows a cooling of -0.13°C, likely caused by increasing of cloudiness under the influence of modulated general circulation. These aerosol induced temperature changes are consistent with the observed temperature trends from 1980 to 2013 in the reanalysis data. Our study also predicts weaker East/South Asia summer monsoons due to strong regional aerosol forcing. Moreover, the ascending motion in the northern tropics is found to be weakened by asymmetrical aerosol forcing, resulting in the cross-equatorial shift of Hadley Circulation.

Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

NASA Astrophysics Data System (ADS)

Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

2014-06-01

Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photooxidation under a range of controlled conditions (RH ∼65-89%, VOC/NOx ∼3-9 and NOx ∼2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line, chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene, but low isoprene emitter, and its emissions were observed to produce measureable amounts of SOA via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e., in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photooxidation products of the minor VOCs co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally-isoprene emitting landscapes in Southeast Asia. Moreover, in general the amount of aerosol mass produced from the emissions of the principally

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

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

Gao, Yi; Liu, Xiaohong; Zhao, Chun

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 bymore » 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.« less

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...

Enhanced hydrophobicity and volatility of submicron aerosols under severe emission control conditions in Beijing

NASA Astrophysics Data System (ADS)

Wang, Yuying; Zhang, Fang; Li, Zhanqing; Tan, Haobo; Xu, Hanbing; Ren, Jingye; Zhao, Jian; Du, Wei; Sun, Yele

2017-04-01

A series of strict emission control measures was implemented in Beijing and the surrounding seven provinces to ensure good air quality during the 2015 China Victory Day parade, rendering a unique opportunity to investigate the anthropogenic impact of aerosol properties. Submicron aerosol hygroscopicity and volatility were measured during and after the control period using a hygroscopic and volatile tandem differential mobility analyzer (H/V-TDMA) system. Three periods, namely the control clean period (Clean1), the non-control clean period (Clean2), and the non-control pollution period (Pollution), were selected to study the effect of the emission control measures on aerosol hygroscopicity and volatility. Aerosol particles became more hydrophobic and volatile due to the emission control measures. The hygroscopicity parameter (κ) of 40-200 nm particles decreased by 32.0-8.5 % during the Clean1 period relative to the Clean2 period, while the volatile shrink factor (SF) of 40-300 nm particles decreased by 7.5-10.5 %. The emission controls also changed the diurnal variation patterns of both the probability density function of κ (κ-PDF) and the probability density function of SF (SF-PDF). During Clean1 the κ-PDF showed one nearly hydrophobic (NH) mode for particles in the nucleation mode, which was likely due to the dramatic reduction in industrial emissions of inorganic trace gases. Compared to the Pollution period, particles observed during the Clean1 and Clean2 periods exhibited a more significant nonvolatile (NV) mode throughout the day, suggesting a more externally mixed state particularly for the 150 nm particles. Aerosol hygroscopicities increased as particle sizes increased, with the greatest increases seen during the Pollution period. Accordingly, the aerosol volatility became weaker (i.e., SF increased) as particle sizes increased during the Clean1 and Clean2 periods, but no apparent trend was observed during the Pollution period. Based on a correlation

Enhanced hydrophobicity and volatility of submicron aerosols under severe emission control conditions in Beijing

NASA Astrophysics Data System (ADS)

Wang, Yuying; Zhang, Fang; Li, Zhanqing

2017-04-01

A series of strict emission control measures were implemented in Beijing and the surrounding seven provinces to ensure good air quality during the 2015 China Victory Day parade, rendering a unique opportunity to investigate anthropogenic impact of aerosol properties. Submicron aerosol hygroscopicity and volatility were measured during and after the control period using a hygroscopic and volatile tandem differential mobility analyzer (H/V-TDMA) system. Three periods, namely, the control clean period (Clean1), the non-control clean period (Clean2), and the non-control pollution period (Pollution), were selected to study the effect of the emission control measures on aerosol hygroscopicity and volatility. Aerosol particles became more hydrophobic and volatile due to the emission control measures. The hygroscopicity parameter (κ) of 40-200 nm particles decreased by 32.0%-8.5% during the Clean1 period relative to the Clean2 period, while the volatile shrink factor (SF) of 40-300 nm particles decreased by 7.5%-10.5%. The emission controls also changed the diurnal variation patterns of both the probability density function of κ (κ-PDF) and the probability density function of SF (SF-PDF). During Clean1 the κ-PDF showed one nearly-hydrophobic (NH) mode for particles in the nucleation mode, which was likely due to the dramatic reduction in industrial emissions of inorganic trace gases. Compared to the Pollution period, particles observed during the Clean1 and Clean2 periods exhibited a more significant non-volatile (NV) mode throughout the day, suggesting a more externally-mixed state particularly for the 150 nm particles. Aerosol hygroscopicities increased as particle sizes increased, with the greatest increases seen during the Pollution period. Accordingly, the aerosol volatility became weaker (i.e., SF increased) during the Clean1 and Clean2 periods, but no apparent trend was observed during the Pollution period. Based on a correlation analysis of the number fractions

Formation of halogen-induced secondary organic aerosol (XOA)

NASA Astrophysics Data System (ADS)

Kamilli, Katharina; Ofner, Johannes; Zetzsch, Cornelius; Held, Andreas

2013-04-01

Reactive halogen species (RHS) are very important due to their potential of stratospheric ozone depletion and surface ozone destruction. RHS seem to interact with precursors of secondary organic aerosol (SOA) similarly to common atmospheric oxidants like OH radicals and ozone. The potential interaction of RHS with preformed SOA has recently been studied (Ofner et al., 2012). Although aerosol formation from reaction of RHS with typical SOA precursors was previously studied (e.g. Cai et al., 2006), no data are available on bromine-induced aerosol formation from organic precursors yet. An aerosol smog-chamber was used to examine the halogen-induced secondary organic aerosol (XOA) formation under atmospheric conditions using simulated sunlight. With a concentration of 10 ppb for the organic precursor, 2 ppb for molecular chlorine, and 10 ppb for molecular bromine, the experimental setup is close to ambient conditions. By combined measurements of the aerosol size distribution, ozone and NOx mixing ratios, as well as the decay of the organic precursor, aerosol yields and aerosol growth rates were determined. The decay of the organic precursor was analyzed by capillary gas chromatography coupled with flame-ionization detection (GC-FID) and the aerosol size distribution was measured using a Scanning Mobility Particle Sizer (SMPS). Additionally, with the decay rate of the precursor and the calculated photolysis rates of molecular halogen species, based on the well-known spectrum of the solar simulator, mechanistic details on the XOA formation pathways can be determined. We observed XOA formation even at very low precursor and RHS concentrations with a diameter mode at 10-20 nm and a number concentration up to 1000000 particles cm-3. While the XOA formation from chlorine is very rapid, the interaction of bromine with the organic precursors is about five times slower. The aerosol yield reached maximum values of 0.01 for the reaction of chlorine with α-pinene and 0.0004 for

Estimating trace gas and aerosol emissions over South America: Relationship between fire radiative energy released and aerosol optical depth observations

NASA Astrophysics Data System (ADS)

Pereira, Gabriel; Freitas, Saulo R.; Moraes, Elisabete Caria; Ferreira, Nelson Jesus; Shimabukuro, Yosio Edemir; Rao, Vadlamudi Brahmananda; Longo, Karla M.

2009-12-01

Contemporary human activities such as tropical deforestation, land clearing for agriculture, pest control and grassland management lead to biomass burning, which in turn leads to land-cover changes. However, biomass burning emissions are not correctly measured and the methods to assess these emissions form a part of current research area. The traditional methods for estimating aerosols and trace gases released into the atmosphere generally use emission factors associated with fuel loading and moisture characteristics and other parameters that are hard to estimate in near real-time applications. In this paper, fire radiative power (FRP) products were extracted from Moderate Resolution Imaging Spectroradiometer (MODIS) and from the Geostationary Operational Environmental Satellites (GOES) fire products and new South America generic biomes FRE-based smoke aerosol emission coefficients were derived and applied in 2002 South America fire season. The inventory estimated by MODIS and GOES FRP measurements were included in Coupled Aerosol-Tracer Transport model coupled to the Brazilian developments on the Regional Atmospheric Modeling System (CATT-BRAMS) and evaluated with ground truth collected in Large Scale Biosphere-Atmosphere Smoke, Aerosols, Clouds, rainfall, and Climate (SMOCC) and Radiation, Cloud, and Climate Interactions (RaCCI). Although the linear regression showed that GOES FRP overestimates MODIS FRP observations, the use of a common external parameter such as MODIS aerosol optical depth product could minimize the difference between sensors. The relationship between the PM 2.5μm (Particulate Matter with diameter less than 2.5 μm) and CO (Carbon Monoxide) model shows a good agreement with SMOCC/RaCCI data in the general pattern of temporal evolution. The results showed high correlations, with values between 0.80 and 0.95 (significant at 0.5 level by student t test), for the CATT-BRAMS simulations with PM 2.5μm and CO.

Methods of analysis for complex organic aerosol mixtures from urban emission sources of particulate carbon

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

Mazurek, M.A.; Hildemann, L.M.; Cass, G.R.

1990-04-01

Extractable organic compounds having between 6 to 40 carbon atoms comprise an important mass fraction of the fine particulate matter samples from major urban emission sources. Depending on the emission source type, this solvent-soluble fraction accounts for <20% to 100% of the total organic aerosol mass, as measured by quantitative high-resolution has chromatography (HRGC) with flame ionization detection. In addition to total extract quantitation, HRGC can be applied to further analyses of the mass distributions of elutable organics present in the complex aerosol extract mixtures, thus generating profiles that serve as fingerprints'' for the sources of interest. This HRGC analyticalmore » method is applied to emission source samples that contain between 7 to 12,000 {mu}g/filter organic carbon. It is shown to be a sensitive technique for analysis of carbonaceous aerosol extract mixtures having diverse mass loadings and species distributions. This study describes the analytical chemical methods that have been applied to: the construction of chemical mass balances based on the mass of fine organic aerosol emitted for major urban sources of particulate carbon; and the generation of discrete emission source chemical profiles derived from chromatographic characteristics of the organic aerosol components. 21 refs., 1 fig., 2 tabs.« less

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

EPA Pesticide Factsheets

The uploaded data consists of the BRACE Na aerosol observations paired with CMAQ model output, the updated model's parameterization of sea salt aerosol emission size distribution, and the model's parameterization of the sea salt emission factor as a function of sea surface temperature. This dataset is associated with the following publication:Gantt , B., J. Kelly , and J. Bash. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2. Geoscientific Model Development. Copernicus Publications, Katlenburg-Lindau, GERMANY, 8: 3733-3746, (2015).

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.

Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony.

PubMed

Hinneburg, Detlef; Renner, Eberhard; Wolke, Ralf

2009-01-01

The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of 'free' sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium-sulfate-nitrate-water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10

Climate responses to anthropogenic emissions of short-lived climate pollutants

NASA Astrophysics Data System (ADS)

Baker, L. H.; Collins, W. J.; Olivié, D. J. L.; Cherian, R.; Hodnebrog, Ø.; Myhre, G.; Quaas, J.

2015-07-01

Policies to control air quality focus on mitigating emissions of aerosols and their precursors, and other short-lived climate pollutants (SLCPs). On a local scale, these policies will have beneficial impacts on health and crop yields, by reducing particulate matter (PM) and surface ozone concentrations; however, the climate impacts of reducing emissions of SLCPs are less straightforward to predict. In this paper we consider a set of idealized, extreme mitigation strategies, in which the total anthropogenic emissions of individual SLCP emissions species are removed. This provides an upper bound on the potential climate impacts of such air quality strategies. We focus on evaluating the climate responses to changes in anthropogenic emissions of aerosol precursor species: black carbon (BC), organic carbon (OC) and sulphur dioxide (SO2). We perform climate integrations with four fully coupled atmosphere-ocean global climate models (AOGCMs), and examine the effects on global and regional climate of removing the total land-based anthropogenic emissions of each of the three aerosol precursor species. We find that the SO2 emissions reductions lead to the strongest response, with all models showing an increase in surface temperature focussed in the Northern Hemisphere mid and (especially) high latitudes, and showing a corresponding increase in global mean precipitation. Changes in precipitation patterns are driven mostly by a northward shift in the ITCZ (Intertropical Convergence Zone), consistent with the hemispherically asymmetric warming pattern driven by the emissions changes. The BC and OC emissions reductions give a much weaker response, and there is some disagreement between models in the sign of the climate responses to these perturbations. These differences between models are due largely to natural variability in sea-ice extent, circulation patterns and cloud changes. This large natural variability component to the signal when the ocean circulation and sea-ice are

Climate responses to anthropogenic emissions of short-lived climate pollutants

NASA Astrophysics Data System (ADS)

Baker, L. H.; Collins, W. J.; Olivié, D. J. L.; Cherian, R.; Hodnebrog, Ø.; Myhre, G.; Quaas, J.; Samset, B. H.

2015-02-01

Policies to control air quality focus on mitigating emissions of aerosols and their precursors, and other short-lived climate pollutants (SLCPs). On a local scale, these policies will have beneficial impacts on health and crop yields, by reducing particulate matter (PM) and surface ozone concentrations; however, the climate impacts of reducing emissions of SLCPs are less straightforward to predict. In this paper we consider a set of idealised, extreme mitigation strategies, in which the total anthropogenic emissions of individual SLCP emissions species are removed. This provides an upper bound on the potential climate impacts of such air quality strategies. We focus on evaluating the climate responses to changes in anthropogenic emissions of aerosol precursor species: black carbon (BC), organic carbon (OC) and sulphur dioxide (SO2). We perform climate integrations with four fully coupled atmosphere-ocean global climate models (AOGCMs), and examine the effects on global and regional climate of removing the total land-based anthropogenic emissions of each of the three aerosol precursor species. We find that the SO2 emissions reductions lead to the strongest response, with all three models showing an increase in surface temperature focussed in the northern hemisphere high latitudes, and a corresponding increase in global mean precipitation and run-off. Changes in precipitation and run-off patterns are driven mostly by a northward shift in the ITCZ, consistent with the hemispherically asymmetric warming pattern driven by the emissions changes. The BC and OC emissions reductions give a much weaker forcing signal, and there is some disagreement between models in the sign of the climate responses to these perturbations. These differences between models are due largely to natural variability in sea-ice extent, circulation patterns and cloud changes. This large natural variability component to the signal when the ocean circulation and sea-ice are free-running means that the

Circulation responses to regional aerosol climate forcing in summer over East Asia

NASA Astrophysics Data System (ADS)

Chen, Guoxing; Wang, Wei-Chyung; Chen, Jen-Ping

2018-05-01

For East Asia, circulation responses to anthropogenic aerosol radiative forcing dominate aerosol-precipitation interactions. To gain insights, this study analyzed CESM simulated circulation changes related to the `north drought and south flood' pattern caused by aerosol increases between two cases. One case was driven by the year-1850 global emission inventory, whereas the other used identical emissions for all regions except East Asia where anthropogenic emissions of aerosols and precursors of the year-2000 were imposed. Results show that the cooling caused by increased aerosols, which peaks at the middle latitudes, induces two intervened anomalous circulations in the troposphere. Near the surface, the increased land pressure weakens the southerlies and reduces the moisture transport for the entire eastern China. Meanwhile, in the free troposphere, the anomalous circulation exhibits remarkable meridional variations. While convergence occurs over 25°-45°N which partially compensates the decrease of moisture transport from lower levels, divergence develops over regions to the north which enhances the moisture deficiency. In addition, the southward shift of the jet stream stimulates anomalous rising and sinking motions over the south and north of 32°N. The combination of these changes leads to precipitation increase in the Yangtze River Valley but decrease over North China.

Simulating Changes in Tropospheric Composition, Aerosol Radiative Effects, and Atmospheric Deposition across the Northern Hemisphere: Contrasting Multi-Decadal Trends between Asia and North America

EPA Science Inventory

Significant and contrasting changes in tropospheric composition across the Northern hemisphere have occurred over the past two decades as a result of changing patterns of emissions of primary aerosol and gaseous precursors. During this period, SO2 and NOx emissions across the US...

The role of anthropogenic aerosol emission reduction in achieving the Paris Agreement's objective

NASA Astrophysics Data System (ADS)

Hienola, Anca; Pietikäinen, Joni-Pekka; O'Donnell, Declan; Partanen, Antti-Ilari; Korhonen, Hannele; Laaksonen, Ari

2017-04-01

The Paris agreement reached in December 2015 under the auspices of the United Nation Framework Convention on Climate Change (UNFCCC) aims at holding the global temperature increase to well below 2◦C above preindustrial levels and "to pursue efforts to limit the temperature increase to 1.5◦C above preindustrial levels". Limiting warming to any level implies that the total amount of carbon dioxide (CO2) - the dominant driver of long-term temperatures - that can ever be emitted into the atmosphere is finite. Essentially, this means that global CO2 emissions need to become net zero. CO2 is not the only pollutant causing warming, although it is the most persistent. Short-lived, non-CO2 climate forcers also must also be considered. Whereas much effort has been put into defining a threshold for temperature increase and zero net carbon emissions, surprisingly little attention has been paid to the non-CO2 climate forcers, including not just the non-CO2 greenhouse gases (methane (CH4), nitrous oxide (N2O), halocarbons etc.) but also the anthropogenic aerosols like black carbon (BC), organic carbon (OC) and sulfate. This study investigates the possibility of limiting the temperature increase to 1.5◦C by the end of the century under different future scenarios of anthropogenic aerosol emissions simulated with the very simplistic MAGICC climate carbon cycle model as well as with ECHAM6.1-HAM2.2-SALSA + UVic ESCM. The simulations include two different CO2 scenarios- RCP3PD as control and a CO2 reduction leading to 1.5◦C (which translates into reaching the net zero CO2 emissions by mid 2040s followed by negative emissions by the end of the century); each CO2 scenario includes also two aerosol pollution control cases denoted with CLE (current legislation) and MFR (maximum feasible reduction). The main result of the above scenarios is that the stronger the anthropogenic aerosol emission reduction is, the more significant the temperature increase by 2100 relative to pre

Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

DOE PAGES

Parworth, Caroline; Tilp, Alison; Fast, Jerome; ...

2015-04-01

In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

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

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Stroud, C.; Bottenheim, J. W.; Brickell, P. C.; Chang, R. Y.-W.; Liggio, J.; Makar, P. A.; Martin, R. V.; Moran, M. D.; Shantz, N. C.; Sjostedt, S. J.; van Donkelaar, A.; Vlasenko, A.; Wiebe, H. A.; Xia, A. G.; Zhang, J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-03-01

Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.

Updating Sea Spray Aerosol Emissions in the Community Multiscale Air Quality Model

NASA Astrophysics Data System (ADS)

Gantt, B.; Bash, J. O.; Kelly, J.

2014-12-01

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, include sea surface temperature (SST) dependency, and revise surf zone emissions. Based on evaluation with several regional and national observational datasets in the continental U.S., the updated emissions generally improve surface concentrations predictions of primary aerosols composed of sea-salt and secondary aerosols affected by sea-salt chemistry in coastal and near-coastal sites. Specifically, the updated emissions lead to better predictions of the magnitude and coastal-to-inland gradient of sodium, chloride, and nitrate concentrations at Bay Regional Atmospheric Chemistry Experiment (BRACE) sites near Tampa, FL. Including SST-dependency to the SSA emission parameterization leads to increased sodium concentrations in the southeast U.S. and decreased concentrations along the Pacific coast and northeastern U.S., bringing predictions into closer agreement with observations at most Interagency Monitoring of Protected Visual Environments (IMPROVE) and Chemical Speciation Network (CSN) sites. Model comparison with California Research at the Nexus of Air Quality and Climate Change (CalNex) observations will also be discussed, with particular focus on the South Coast Air Basin where clean marine air mixes with anthropogenic pollution in a complex environment. These SSA emission updates enable more realistic simulation of chemical processes in coastal environments, both in clean marine air masses and mixtures of clean marine and polluted conditions.

The effect of future reduction in aerosol emissions on climate extremes in China

NASA Astrophysics Data System (ADS)

Wang, Zhili; Lin, Lei; Yang, Meilin; Xu, Yangyang

2016-11-01

This study investigates the effect of reduced aerosol emissions on projected temperature and precipitation extremes in China during 2031-2050 and 2081-2100 relative to present-day conditions using the daily data output from the Community Earth System Model ensemble simulations under the Representative Concentration Pathway (RCP) 8.5 with an applied aerosol reduction and RCP8.5 with fixed 2005 aerosol emissions (RCP8.5_FixA) scenarios. The reduced aerosol emissions of RCP8.5 magnify the warming effect due to greenhouse gases (GHG) and lead to significant increases in temperature extremes, such as the maximum of daily maximum temperature (TXx), minimum of daily minimum temperature (TNn), and tropical nights (TR), and precipitation extremes, such as the maximum 5-day precipitation amount, number of heavy precipitation days, and annual total precipitation from days ˃95th percentile, in China. The projected TXx, TNn, and TR averaged over China increase by 1.2 ± 0.2 °C (4.4 ± 0.2 °C), 1.3 ± 0.2 °C (4.8 ± 0.2 °C), and 8.2 ± 1.2 (30.9 ± 1.4) days, respectively, during 2031-2050 (2081-2100) under the RCP8.5_FixA scenario, whereas the corresponding values are 1.6 ± 0.1 °C (5.3 ± 0.2 °C), 1.8 ± 0.2 °C (5.6 ± 0.2 °C), and 11.9 ± 0.9 (38.4 ± 1.0) days under the RCP8.5 scenario. Nationally averaged increases in all of those extreme precipitation indices above due to the aerosol reduction account for more than 30 % of the extreme precipitation increases under the RCP8.5 scenario. Moreover, the aerosol reduction leads to decreases in frost days and consecutive dry days averaged over China. There are great regional differences in changes of climate extremes caused by the aerosol reduction. When normalized by global mean surface temperature changes, aerosols have larger effects on temperature and precipitation extremes over China than GHG.

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.

Characterization of Fine Particulate Matter (PM) and Secondary PM Precursor Gases in the Mexico City Metropolitan Area

DOE R&D Accomplishments Database

Molina, Luisa T.; Volkamer, Rainer; de Foy, Benjamin; Lei, Wenfang; Zavala, Miguel; Velasco, Erik; Molina; Mario J.

2008-10-31

This project was one of three collaborating grants funded by DOE/ASP to characterize the fine particulate matter (PM) and secondary PM precursors in the Mexico City Metropolitan Area (MCMA) during the MILAGRO Campaign. The overall effort of MCMA-2006, one of the four components, focused on i) examination of the primary emissions of fine particles and precursor gases leading to photochemical production of atmospheric oxidants and secondary aerosol particles; ii) measurement and analysis of secondary oxidants and secondary fine PM production, with particular emphasis on secondary organic aerosol (SOA), and iii) evaluation of the photochemical and meteorological processes characteristic of the Mexico City Basin. The collaborative teams pursued the goals through three main tasks: i) analyses of fine PM and secondary PM precursor gaseous species data taken during the MCMA-2002/2003 campaigns and preparation of publications; ii) planning of the MILAGRO Campaign and deployment of the instrument around the MCMA; and iii) analysis of MCMA-2006 data and publication preparation.

Cloud-Resolving Model Simulations of Aerosol-Cloud Interactions Triggered by Strong Aerosol Emissions in the Arctic

NASA Astrophysics Data System (ADS)

Wang, H.; Kravitz, B.; Rasch, P. J.; Morrison, H.; Solomon, A.

2014-12-01

Previous process-oriented modeling studies have highlighted the dependence of effectiveness of cloud brightening by aerosols on cloud regimes in warm marine boundary layer. Cloud microphysical processes in clouds that contain ice, and hence the mechanisms that drive aerosol-cloud interactions, are more complicated than in warm clouds. Interactions between ice particles and liquid drops add additional levels of complexity to aerosol effects. A cloud-resolving model is used to study aerosol-cloud interactions in the Arctic triggered by strong aerosol emissions, through either geoengineering injection or concentrated sources such as shipping and fires. An updated cloud microphysical scheme with prognostic aerosol and cloud particle numbers is employed. Model simulations are performed in pure super-cooled liquid and mixed-phase clouds, separately, with or without an injection of aerosols into either a clean or a more polluted Arctic boundary layer. Vertical mixing and cloud scavenging of particles injected from the surface is still quite efficient in the less turbulent cold environment. Overall, the injection of aerosols into the Arctic boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. The pure liquid clouds are more susceptible to the increase in aerosol number concentration than the mixed-phase clouds. Rain production processes are more effectively suppressed by aerosol injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. Aerosol injection into a clean boundary layer results in a greater cloud albedo increase than injection into a polluted one, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, the impact of dynamical feedback due to precipitation changes is small. According to these results, which are dependent upon the representation of ice nucleation

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.

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.

The Use of Satellite-Measured Aerosol Optical Depth to Constrain Biomass Burning Emissions Source Strength in a Global Model GOCART

NASA Technical Reports Server (NTRS)

Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Soja, Amber; Kuesera, Tom; harshvardhan, E. M.

2012-01-01

Small particles in the atmosphere, called "atmospheric aerosol" have a direct effect on Earth climate through scattering and absorbing sunlight, and also an indirect effect by changing the properties of clouds, as they interact with solar radiation as well. Aerosol typically stays in the atmosphere for several days, and can be transported long distances, affecting air quality, visibility, and human health not only near the source, but also far downwind. Smoke from vegetation fires is one of the main sources of atmospheric aerosol; other sources include anthropogenic pollution, dust, and sea salt. Chemistry transport models (CTMs) are among the major tools for studying the atmospheric and climate effects of aerosol. Due to the considerable variation of aerosol concentrations and properties on many temporal and spatial scales, and the complexity of the processes involved, the uncertainties in aerosol effects on climate are large, as is featured in the latest report of Intergovernmental Panel on Climate Change (IPCC) in 2007. Reducing this uncertainty in the models is very important both for predicting future climate scenarios and for regional air quality forecasting and mitigation. During vegetation fires, also called biomass burning (BB) events, complex mixture of gases and particles is emitted. The amount of BB emissions is usually estimated taking into account the intensity and size of the fire and the properties of burning vegetation. These estimates are input into CTMs to simulate BB aerosol. Unfortunately, due to large variability of fire and vegetation properties, the quantity of BB emissions is very difficult to estimate and BB emission inventories provide numbers that can differ by up to the order of magnitude in some regions. Larger uncertainties in data input make uncertainties in model output larger as well. A powerful way to narrow the range of possible model estimates is to compare model output to observations. We use satellite observations of aerosol

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

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

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

1990-06-01

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

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

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

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

1990-01-01

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

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

Inflammatory responses to secondary organic aerosols (SOA) generated from biogenic and anthropogenic precursors

NASA Astrophysics Data System (ADS)

Tuet, Wing Y.; Chen, Yunle; Fok, Shierly; Champion, Julie A.; Ng, Nga L.

2017-09-01

Cardiopulmonary health implications resulting from exposure to secondary organic aerosols (SOA), which comprise a significant fraction of ambient particulate matter (PM), have received increasing interest in recent years. In this study, alveolar macrophages were exposed to SOA generated from the photooxidation of biogenic and anthropogenic precursors (isoprene, α-pinene, β-caryophyllene, pentadecane, m-xylene, and naphthalene) under different formation conditions (RO2 + HO2 vs. RO2 + NO dominant, dry vs. humid). Various cellular responses were measured, including reactive oxygen and nitrogen species (ROS/RNS) production and secreted levels of cytokines, tumor necrosis factor-α (TNF-α) and interleukin-6 (IL-6). SOA precursor identity and formation condition affected all measured responses in a hydrocarbon-specific manner. With the exception of naphthalene SOA, cellular responses followed a trend where TNF-α levels reached a plateau with increasing IL-6 levels. ROS/RNS levels were consistent with relative levels of TNF-α and IL-6, due to their respective inflammatory and anti-inflammatory effects. Exposure to naphthalene SOA, whose aromatic-ring-containing products may trigger different cellular pathways, induced higher levels of TNF-α and ROS/RNS than suggested by the trend. Distinct cellular response patterns were identified for hydrocarbons whose photooxidation products shared similar chemical functionalities and structures, which suggests that the chemical structure (carbon chain length and functionalities) of photooxidation products may be important for determining cellular effects. A positive nonlinear correlation was also detected between ROS/RNS levels and previously measured DTT (dithiothreitol) activities for SOA samples. In the context of ambient samples collected during summer and winter in the greater Atlanta area, all laboratory-generated SOA produced similar or higher levels of ROS/RNS and DTT activities. These results suggest that the health

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

NASA Astrophysics Data System (ADS)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

NASA Astrophysics Data System (ADS)

Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

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.

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

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

Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen

Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the ‘climate sensitivity’). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through a combinationmore » of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic

How Will Aerosol-Cloud Interactions Change in an Ice-Free Arctic Summer?

NASA Astrophysics Data System (ADS)

Gilgen, Anina; Katty Huang, Wan Ting; Ickes, Luisa; Lohmann, Ulrike

2016-04-01

Future temperatures in the Arctic are expected to increase more than the global mean temperature, which will lead to a pronounced retreat in Arctic sea ice. Before mid-century, most sea ice will likely have vanished in late Arctic summers. This will allow ships to cruise in the Arctic Ocean, e.g. to shorten their transport passage or to extract oil. Since both ships and open water emit aerosol particles and precursors, Arctic clouds and radiation may be affected via aerosol-cloud and cloud-radiation interactions. The change in radiation feeds back on temperature and sea ice retreat. In addition to aerosol particles, also the temperature and the open ocean as a humidity source should have a strong effect on clouds. The main goal of this study is to assess the impact of sea ice retreat on the Arctic climate with focus on aerosol emissions and cloud properties. To this purpose, we conducted ensemble runs with the global climate model ECHAM6-HAM2 under present-day and future (2050) conditions. ECHAM6-HAM2 was coupled with a mixed layer ocean model, which includes a sea ice model. To estimate Arctic aerosol emissions from ships, we used an elaborated ship emission inventory (Peters et al. 2011); changes in aerosol emissions from the ocean are calculated online. Preliminary results show that the sea salt aerosol and the dimethyl sulfide burdens over the Arctic Ocean significantly increase. While the ice water path decreases, the total water path increases. Due to the decrease in surface albedo, the cooling effect of the Arctic clouds becomes more important in 2050. Enhanced Arctic shipping has only a very small impact. The increase in the aersol burden due to shipping is less pronounced than the increase due to natural emissions even if the ship emissions are increased by a factor of ten. Hence, there is hardly an effect on clouds and radiation caused by shipping. References Peters et al. (2011), Atmos. Chem. Phys., 11, 5305-5320

Aerosol-Assisted Chemical Vapor Deposited Thin Films for Space Photovoltaics

NASA Technical Reports Server (NTRS)

Hepp, Aloysius F.; McNatt, Jeremiah; Dickman, John E.; Jin, Michael H.-C.; Banger, Kulbinder K.; Kelly, Christopher V.; AquinoGonzalez, Angel R.; Rockett, Angus A.

2006-01-01

Copper indium disulfide thin films were deposited via aerosol-assisted chemical vapor deposition using single source precursors. Processing and post-processing parameters were varied in order to modify morphology, stoichiometry, crystallography, electrical properties, and optical properties in order to optimize device-quality material. Growth at atmospheric pressure in a horizontal hot-wall reactor at 395 C yielded best device films. Placing the susceptor closer to the evaporation zone and flowing a more precursor-rich carrier gas through the reactor yielded shinier, smoother, denser-looking films. Growth of (112)-oriented films yielded more Cu-rich films with fewer secondary phases than growth of (204)/(220)-oriented films. Post-deposition sulfur-vapor annealing enhanced stoichiometry and crystallinity of the films. Photoluminescence studies revealed four major emission bands (1.45, 1.43, 1.37, and 1.32 eV) and a broad band associated with deep defects. The highest device efficiency for an aerosol-assisted chemical vapor deposited cell was 1.03 percent.

The global impact of the transport sectors on atmospheric aerosol in 2030 - Part 2: Aviation

NASA Astrophysics Data System (ADS)

Righi, Mattia; Hendricks, Johannes; Sausen, Robert

2016-04-01

We use the EMAC (ECHAM/MESSy Atmospheric Chemistry) global climate-chemistry model coupled to the aerosol module MADE (Modal Aerosol Dynamics model for Europe, adapted for global applications) to simulate the impact of aviation emissions on global atmospheric aerosol and climate in 2030. Emissions of short-lived gas and aerosol species follow the four Representative Concentration Pathways (RCPs) designed in support of the Fifth Assessment Report of the Intergovernmental Panel on Climate Change. We compare our findings with the results of a previous study with the same model configuration focusing on year 2000 emissions. We also characterize the aviation results in the context of the other transport sectors presented in a companion paper. In spite of a relevant increase in aviation traffic volume and resulting emissions of aerosol (black carbon) and aerosol precursor species (nitrogen oxides and sulfur dioxide), the aviation effect on particle mass concentration in 2030 remains quite negligible (on the order of a few ng m-3), about 1 order of magnitude less than the increase in concentration due to other emission sources. Due to the relatively small size of the aviation-induced aerosol, however, the increase in particle number concentration is significant in all scenarios (about 1000 cm-3), mostly affecting the northern mid-latitudes at typical flight altitudes (7-12 km). This largely contributes to the overall change in particle number concentration between 2000 and 2030, which also results in significant climate effects due to aerosol-cloud interactions. Aviation is the only transport sector for which a larger impact on the Earth's radiation budget is simulated in the future: the aviation-induced radiative forcing in 2030 is more than doubled with respect to the year 2000 value of -15 mW m-2 in all scenarios, with a maximum value of -63 mW m-2 simulated for RCP2.6.

The Impact of US SO2 Emissions on Clouds and the Hydrological Cycle at Global and Regional Scales in Three Coupled Chemistry-Climate Models

NASA Astrophysics Data System (ADS)

Westervelt, D. M.

2016-12-01

It is widely expected that global and regional 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. Although there is some evidence that these aerosol reductions may lead to significant regional and global climate impacts, we currently lack a full understanding of the magnitude, spatial and temporal pattern, and statistical significance of these influences, especially for clouds and precipitation. Further, we often lack robust understanding of the processes by which regional aerosols influence local and remote climate. Here, we aim to quantify systematically the cloud and hydrological cycle response to regional changes in aerosols through model simulations using three fully coupled chemistry-climate models: NOAA Geophysical Fluid Dynamics Laboratory Coupled Model 3 (GFDL-CM3), NCAR Community Earth System Model (NCAR-CESM1), and NASA Goddard Institute for Space Studies ModelE2 (GISS-E2). The central approach we use is to contrast a long control experiment (400 years) with a collection of long individual perturbation experiments ( 200 years). We perturb emissions of sulfur dioxide (SO2; precursor to sulfate aerosol) in the United States and determine which responses are significant relative to internal variability and robust across the three models. Initial results show robust, statistically significant decreases in cloud droplet number and liquid water path in the source region across the three models due to decreases in sulfate aerosols. Setting SO2 emissions to zero over the U.S. causes both local and remote impacts in precipitation, with notable significant increases in Sahel and Arctic precipitation. In 13 of the 15 regions we analyze, the precipitation response to zero U.S. SO2 emissions agrees in sign, with agreement in magnitude to within one standard deviation in many of those regions. U.S. sulfate also impacts the timing

Multi-Model Simulations of Aerosol and Ozone Radiative Forcing Due to Anthropogenic Emission Changes During the Period 1990-2015

NASA Technical Reports Server (NTRS)

Myhre, Gunnar; Aas, Wenche; Ribu, Cherian; Collins, William; Faluvegi, Gregory S.; Flanner, Mark; Forster, Piers; Hodnebrog, Oivind; Klimont, Zbigniew; Lund, Marianne T.

2017-01-01

Over the past few decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and air pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990-2015, as simulated by seven global atmospheric composition models. The models broadly reproduce large-scale changes in surface aerosol and ozone based on observations (e.g. 1 to 3 percent per year in aerosols over the USA and Europe). The global mean radiative forcing due to ozone and aerosol changes over the 1990-2015 period increased by 0.17 plus or minus 0.08 watts per square meter, with approximately one-third due to ozone. This increase is more strongly positive than that reported in IPCC AR5 (Intergovernmental Panel on Climate Change Fifth Assessment Report). The main reasons for the increased positive radiative forcing of aerosols over this period are the substantial reduction of global mean SO2 emissions, which is stronger in the new emission inventory compared to that used in the IPCC analysis, and higher black carbon emissions.

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.

Secondary organic aerosol production from diesel vehicle exhaust: impact of aftertreatment, fuel chemistry and driving cycle

NASA Astrophysics Data System (ADS)

Gordon, T. D.; Presto, A. A.; Nguyen, N. T.; Robertson, W. H.; Na, K.; Sahay, K. N.; Zhang, M.; Maddox, C.; Rieger, P.; Chattopadhyay, S.; Maldonado, H.; Maricq, M. M.; Robinson, A. L.

2014-05-01

Environmental chamber ("smog chamber") experiments were conducted to investigate secondary organic aerosol (SOA) production from dilute emissions from two medium-duty diesel vehicles (MDDVs) and three heavy-duty diesel vehicles (HDDVs) under urban-like conditions. Some of the vehicles were equipped with emission control aftertreatment devices, including diesel particulate filters (DPFs), selective catalytic reduction (SCR) and diesel oxidation catalysts (DOCs). Experiments were also performed with different fuels (100% biodiesel and low-, medium- or high-aromatic ultralow sulfur diesel) and driving cycles (Unified Cycle,~Urban Dynamometer Driving Schedule, and creep + idle). During normal operation, vehicles with a catalyzed DPF emitted very little primary particulate matter (PM). Furthermore, photooxidation of dilute emissions from these vehicles produced essentially no SOA (below detection limit). However, significant primary PM emissions and SOA production were measured during active DPF regeneration experiments. Nevertheless, under reasonable assumptions about DPF regeneration frequency, the contribution of regeneration emissions to the total vehicle emissions is negligible, reducing PM trapping efficiency by less than 2%. Therefore, catalyzed DPFs appear to be very effective in reducing both primary PM emissions and SOA production from diesel vehicles. For both MDDVs and HDDVs without aftertreatment substantial SOA formed in the smog chamber - with the emissions from some vehicles generating twice as much SOA as primary organic aerosol after 3 h of oxidation at typical urban VOC / NOx ratios (3 : 1). Comprehensive organic gas speciation was performed on these emissions, but less than half of the measured SOA could be explained by traditional (speciated) SOA precursors. The remainder presumably originates from the large fraction (~30%) of the nonmethane organic gas emissions that could not be speciated using traditional one-dimensional gas chromatography. The

Antarctic new particle formation from continental biogenic precursors

NASA Astrophysics Data System (ADS)

Kyrö, E.-M.; Kerminen, V.-M.; Virkkula, A.; Dal Maso, M.; Parshintsev, J.; Ruíz-Jimenez, J.; Forsström, L.; Manninen, H. E.; Riekkola, M.-L.; Heinonen, P.; Kulmala, M.

2012-12-01

Over Antarctica, aerosol particles originate almost entirely from marine areas, with minor contribution from long-range transported dust or anthropogenic material. The Antarctic continent itself, unlike all other continental areas, has been thought to be practically free of aerosol sources. Here we present evidence of local aerosol production associated with melt-water ponds in the continental Antarctica. We show that in air masses passing such ponds, new aerosol particles are efficiently formed and these particles grow up to sizes where they may act as cloud condensation nuclei (CCN). The precursor vapours responsible for aerosol formation and growth originate very likely from highly abundant cyanobacteria Nostoc commune (Vaucher) communities of local ponds. This is the first time when freshwater vegetation has been identified as an aerosol precursor source. The influence of the new source on clouds and climate may increase in future Antarctica, and possibly elsewhere undergoing accelerating summer melting of semi-permanent snow cover.

Antarctic new particle formation from continental biogenic precursors

NASA Astrophysics Data System (ADS)

Kyrö, E.-M.; Kerminen, V.-M.; Virkkula, A.; Dal Maso, M.; Parshintsev, J.; Ruíz-Jimenez, J.; Forsström, L.; Manninen, H. E.; Riekkola, M.-L.; Heinonen, P.; Kulmala, M.

2013-04-01

Over Antarctica, aerosol particles originate almost entirely from marine areas, with minor contribution from long-range transported dust or anthropogenic material. The Antarctic continent itself, unlike all other continental areas, has been thought to be practically free of aerosol sources. Here we present evidence of local aerosol production associated with melt-water ponds in continental Antarctica. We show that in air masses passing such ponds, new aerosol particles are efficiently formed and these particles grow up to sizes where they may act as cloud condensation nuclei (CCN). The precursor vapours responsible for aerosol formation and growth originate very likely from highly abundant cyanobacteria Nostoc commune (Vaucher) communities of local ponds. This is the first time freshwater vegetation has been identified as an aerosol precursor source. The influence of the new source on clouds and climate may increase in future Antarctica, and possibly elsewhere undergoing accelerating summer melting of semi-permanent snow cover.

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

NASA Astrophysics Data System (ADS)

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

2013-02-01

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

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

NASA Astrophysics Data System (ADS)

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

2012-08-01

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

Efficient transport of tropospheric aerosol into the stratosphere via the Asian summer monsoon anticyclone

NASA Astrophysics Data System (ADS)

Yu, Pengfei; Rosenlof, Karen H.; Liu, Shang; Telg, Hagen; Thornberry, Troy D.; Rollins, Andrew W.; Portmann, Robert W.; Bai, Zhixuan; Ray, Eric A.; Duan, Yunjun; Pan, Laura L.; Toon, Owen B.; Bian, Jianchun; Gao, Ru-Shan

2017-07-01

An enhanced aerosol layer near the tropopause over Asia during the June-September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (˜15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (˜35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.

Chemical transport model simulations of organic aerosol in ...

EPA Pesticide Factsheets

Gasoline- and diesel-fueled engines are ubiquitous sources of air pollution in urban environments. They emit both primary particulate matter and precursor gases that react to form secondary particulate matter in the atmosphere. In this work, we updated the organic aerosol module and organic emissions inventory of a three-dimensional chemical transport model, the Community Multiscale Air Quality Model (CMAQ), using recent, experimentally derived inputs and parameterizations for mobile sources. The updated model included a revised volatile organic compound (VOC) speciation for mobile sources and secondary organic aerosol (SOA) formation from unspeciated intermediate volatility organic compounds (IVOCs). The updated model was used to simulate air quality in southern California during May and June 2010, when the California Research at the Nexus of Air Quality and Climate Change (CalNex) study was conducted. Compared to the Traditional version of CMAQ, which is commonly used for regulatory applications, the updated model did not significantly alter the predicted organic aerosol (OA) mass concentrations but did substantially improve predictions of OA sources and composition (e.g., POA–SOA split), as well as ambient IVOC concentrations. The updated model, despite substantial differences in emissions and chemistry, performed similar to a recently released research version of CMAQ (Woody et al., 2016) that did not include the updated VOC and IVOC emissions and SOA data

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

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

Yan, Huiping; Qian, Yun; Zhao, Chun

2015-09-09

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

Bacterial aerosol emission rates from municipal wastewater aeration tanks.

PubMed Central

Sawyer, B; Elenbogen, G; Rao, K C; O'Brien, P; Zenz, D R; Lue-Hing, C

1993-01-01

In this report we describe the results of a study conducted to determine the rates of bacterial aerosol emission from the surfaces of the aeration tanks of the Metropolitan Water Reclamation District of Greater Chicago John E. Egan Water Reclamation Plant. This study was accomplished by conducting test runs in which Andersen six-stage viable samplers were used to collect bacterial aerosol samples inside a walled tower positioned above an aeration tank liquid surface at the John E. Egan Water Reclamation Plant. The samples were analyzed for standard plate counts (SPC), total coliforms (TC), fecal coliforms, and fecal streptococci. Two methods of calculation were used to estimate the bacterial emission rate. The first method was a conventional stack emission rate calculation method in which the measured air concentration of bacteria was multiplied by the air flow rate emanating from the aeration tanks. The second method was a more empirical method in which an attempt was made to measure all of the bacteria emanating from an isolated area (0.37 m2) of the aeration tank surface over time. The data from six test runs were used to determine bacterial emission rates by both calculation methods. As determined by the conventional calculation method, the average SPC emission rate was 1.61 SPC/m2/s (range, 0.66 to 2.65 SPC/m2/s). As determined by the empirical calculation method, the average SPC emission rate was 2.18 SPC/m2/s (range, 1.25 to 2.66 SPC/m2/s). For TC, the average emission rate was 0.20 TC/m2/s (range, 0.02 to 0.40 TC/m2/s) when the conventional calculation method was used and 0.27 TC/m2/s (range, 0.04 to 0.53 TC/m2/s) when the empirical calculation method was used.(ABSTRACT TRUNCATED AT 250 WORDS) PMID:8250547

Secondary organic aerosol production from diesel vehicle exhaust: impact of aftertreatment, fuel chemistry and driving cycle

NASA Astrophysics Data System (ADS)

Gordon, T. D.; Presto, A. A.; Nguyen, N. T.; Robertson, W. H.; Na, K.; Sahay, K. N.; Zhang, M.; Maddox, C.; Rieger, P.; Chattopadhyay, S.; Maldonado, H.; Maricq, M. M.; Robinson, A. L.

2013-09-01

Environmental chamber ("smog chamber") experiments were conducted to investigate secondary organic aerosol (SOA) production from dilute emissions from two medium-duty diesel vehicles (MDDVs) and three heavy-duty diesel vehicles (HDDVs) under urban-like conditions. Some of the vehicles were equipped with emission control aftertreatment devices including diesel particulate filters (DPF), selective catalytic reduction (SCR) and diesel oxidation catalysts (DOC). Experiments were also performed with different fuels (100% biodiesel and low-, medium- or high-aromatic ultralow sulfur diesel) and driving cycles (Unified Cycle, Urban Dynamometer Driving Schedule, and creep+idle). During normal operation, vehicles with a catalyzed DPF emitted very little primary particulate matter (PM). Furthermore, photo-oxidation of dilute emissions from these vehicles produced essentially no SOA (below detection limit). However, significant primary PM emissions and SOA production were measured during active DPF regeneration experiments. Nevertheless, under reasonable assumptions about DPF regeneration frequency, the contribution of regeneration emissions to the total vehicle emissions is negligible, reducing PM trapping efficiency by less than 2%. Therefore, catalyzed DPFs appear to be very effective in reducing both primary and secondary fine particulate matter from diesel vehicles. For both MDDVs and HDDVs without aftertreatment substantial SOA formed in the smog chamber - with the emissions from some vehicles generating twice as much SOA as primary organic aerosol after three hours of oxidation at typical urban VOC : NOx ratios (3:1). Comprehensive organic gas speciation was performed on these emissions, but less than half of the measured SOA could be explained by traditional (speciated) SOA precursors. The remainder presumably originates from the large fraction (~30%) of the non-methane organic gas emissions that could not be speciated using traditional one-dimensional gas

The Influence of Air-Sea Fluxes on Atmospheric Aerosols During the Summer Monsoon Over the Tropical Indian Ocean

NASA Astrophysics Data System (ADS)

Zavarsky, Alex; Booge, Dennis; Fiehn, Alina; Krüger, Kirstin; Atlas, Elliot; Marandino, Christa

2018-01-01

During the summer monsoon, the western tropical Indian Ocean is predicted to be a hot spot for dimethylsulfide emissions, the major marine sulfur source to the atmosphere, and an important aerosol precursor. Other aerosol relevant fluxes, such as isoprene and sea spray, should also be enhanced, due to the steady strong winds during the monsoon. Marine air masses dominate the area during the summer monsoon, excluding the influence of continentally derived pollutants. During the SO234-2/235 cruise in the western tropical Indian Ocean from July to August 2014, directly measured eddy covariance DMS fluxes confirm that the area is a large source of sulfur to the atmosphere (cruise average 9.1 μmol m-2 d-1). The directly measured fluxes, as well as computed isoprene and sea spray fluxes, were combined with FLEXPART backward and forward trajectories to track the emissions in space and time. The fluxes show a significant positive correlation with aerosol data from the Terra and Suomi-NPP satellites, indicating a local influence of marine emissions on atmospheric aerosol numbers.

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

NASA Technical Reports Server (NTRS)

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

2018-01-01

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

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

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

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

Donahue, Neil M.

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 ofmore » 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]« less

Stratospheric aerosols and precursor gases

NASA Technical Reports Server (NTRS)

1982-01-01

Measurements were made of the aerosol size, height and geographical distribution, their composition and optical properties, and their temporal variation with season and following large volcanic eruptions. Sulfur-bearing gases were measured in situ in the stratosphere, and studied of the chemical and physical processes which control gas-to-particle conversion were carried out in the laboratory.

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...

Chemical and Optical Properties of Water-Soluble Organic Aerosols from Biomass Burning Emissions

NASA Astrophysics Data System (ADS)

Yu, J. M.; Park, S.; Cho, S. Y.

2016-12-01

Light absorption property by organic aerosols is an important parameter to determine their radiative forcing on global and regional scales. However, the optical measurements by light absorbing aerosols from biomass burning emissions are rather lacking. This study explored the chemical and light-absorption properties of humic-like substances (HULIS) from biomass burning aerosols of three types; rice straw (RS), pine needles (PN), and sesame stem (SS). Water-soluble organic carbon (WSOC) contributed 42.5, 42.0, and 57.0% to the OC concentrations of the RS, PN, and SS emissions, respectively. Respective HULIS (=1.94´HULIS-C) concentrations accounted for 29.5±2.0, 15.3±3.1, and 25.8±4.0% of PM2.5, and contributed 63±5, 36±10, and 51±8% to WSOC concentration. Absorption Ångström exponents (AAEs) of the WSOC fitted between 300 and 400 nm wavelengths were 7.4-8.3, indicating no significant differences among the biomass types. These AAEs are similar to those reported for aqueous extracts of biomass burning HULIS and fresh secondary organic aerosols from ozonolysis of terpenes. HULIS, which is a hydrophobic part of WSOC and a significant fraction of brown carbon, showed absorption spectra similar to brown carbon. WSOC mass absorption efficiency (MAE365) at 365 nm were 1.37, 0.86, and 1.38 m2/g×C for RS, PN, and SS burning aerosols, respectively. The MAE values by WSOC were less than 10% of MAE caused by light-absorbing black carbon. The light absorption of the water extracts at 365 nm indicated that light absorption was more strongly associated with HULIS from biomass burning emissions than with the hydrophilic WSOC fraction.

Emission properties of Ce3+ centers in barium borate glasses prepared from different precursor materials

NASA Astrophysics Data System (ADS)

Torimoto, Aya; Masai, Hirokazu; Okada, Go; Kawaguchi, Noriaki; Yanagida, Takayuki; Ohkubo, Takahiro

2017-10-01

The photoluminescence (PL) and X-ray induced luminescence properties of Ce-doped barium borate glasses prepared from different precursor materials have been investigated. Oxidation of Ce3+ takes place during the melting process performed using a pre-vitrified non-doped glass. Residual groups originated from the precursor materials, such as fluorine atoms and OH groups, are found to affect the optical and emission properties of the glasses. Moreover, both the PL and the X-ray induced luminescence properties of the glasses depend on the precursor materials used for their synthesis. Based on a thorough analysis of the emission properties, we conclude that the best synthesis conditions involve melting a batch containing Ce(CH3COO)3·H2O, BaCO3, and B2O3 in Ar atmosphere.

High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

NASA Astrophysics Data System (ADS)

Satheesh, S. K.

2017-12-01

Synthesizing a series of ground-based and airborne measurements of aerosols over the Indian region during summer and pre-monsoon seasons have revealed the persistence of elevated absorbing aerosol layers over most of the Indian region; more than 50% of which located above clouds. Subsequent, in situ measurements of black carbon (BC) using high-altitude balloons, showed surprising layers with high concentrations in the middle and upper troposphere even at an altitude of 8 to 10 kms. Simultaneous measurements of the vertical thermal structure have shown localized warming due to BC absorption leading to large reduction in lapse rate and sharp temperature inversion, which in turn increases the atmospheric stability. This aerosol-induced stable layer is conducive for maintaining the black carbon layer longer at that level, leading thereby to further solar absorption and subsequently triggering dry convection. These observations support the `solar escalator' concept through which absorption-warming-convection cycles lead to self-lifting of BC to upper troposphere or even to lower stratosphere under favorable conditions in a matter of a few days. Employing an on-line regional chemistry transport model (WRF-Chem), incorporating aircraft emissions, it is shown that emissions from high-flying aircrafts as the most likely source of these elevated black carbon layers. These in-situ injected particles, produce significant warming of the thin air in those heights and lift these layers to even upper tropospheric/lower stratospheric heights, aided by the strong monsoonal convection occurring over the region, which are known to overshoot the tropical tropopause leading to injection of tropospheric air mass (along with its constituent aerosols) into the stratosphere, especially during monsoon season when the tropical tropopause layer is known to be thinnest. These simulations are further supported by the CALIPSO space-borne LIDAR derived extinction coefficient profiles. Based on

Primary and Photochemically Aged Aerosol Emissions from Biomass Cookstoves: Chemical and Physical Characterization.

PubMed

Reece, Stephen M; Sinha, Aditya; Grieshop, Andrew P

2017-08-15

Secondary organic aerosol (SOA) formation during photo-oxidation of primary emissions from cookstoves used in developing countries may make important contributions to their climate and air quality impacts. We present results from laboratory experiments with a field portable oxidation flow reactor (F-OFR) to study the evolution of emissions over hours to weeks of equivalent atmospheric aging. Lab tests, using dry red oak, measured fresh and aged emissions from a 3 stone fire (TSF), a "rocket" natural draft stove (NDS), and a forced draft gasifier stove (FDGS), in order of increasing modified combustion efficiency (MCE) and decreasing particulate matter emission factors (EF). SOA production was observed for all stoves/tests; organic aerosol (OA) enhancement factor ranged from 1.2 to 3.1, decreasing with increased MCE. In primary emissions, OA mass spectral fragments associated with oxygenated species (primary biomass burning markers) increased (decreased) with MCE; fresh OA from FDGS combustion was especially oxygenated. OA oxygenation increased with further oxidation for all stove emissions, even where minimal enhancement was observed. More efficient stoves emit particles with greater net direct specific warming than TSFs, with the difference increasing with aging. Our results show that the properties and evolution of cookstove emissions are a strong function of combustion efficiency and atmospheric aging.

Refined Use of Satellite Aerosol Optical Depth Snapshots to Constrain Biomass Burning Emissions in the GOCART Model

NASA Astrophysics Data System (ADS)

Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Limbacher, James

2017-10-01

Simulations of biomass burning (BB) emissions in global chemistry and aerosol transport models depend on external inventories, which provide location and strength for BB aerosol sources. Our previous work shows that to first order, satellite snapshots of aerosol optical depth (AOD) near the emitted smoke plume can be used to constrain model-simulated AOD, and effectively, the smoke source strength. We now refine the satellite-snapshot method and investigate where applying simple multiplicative emission adjustment factors alone to the widely used Global Fire Emission Database version 3 emission inventory can achieve regional-scale consistency between Moderate Resolution Imaging Spectroradiometer (MODIS) AOD snapshots and the Goddard Chemistry Aerosol Radiation and Transport model. The model and satellite AOD are compared globally, over a set of BB cases observed by the MODIS instrument during the 2004, and 2006-2008 biomass burning seasons. Regional discrepancies between the model and satellite are diverse around the globe yet quite consistent within most ecosystems. We refine our approach to address physically based limitations of our earlier work (1) by expanding the number of fire cases from 124 to almost 900, (2) by using scaled reanalysis-model simulations to fill missing AOD retrievals in the MODIS observations, (3) by distinguishing the BB components of the total aerosol load from background aerosol in the near-source regions, and (4) by including emissions from fires too small to be identified explicitly in the satellite observations. The small-fire emission adjustment shows the complimentary nature of correcting for source strength and adding geographically distinct missing sources. Our analysis indicates that the method works best for fire cases where the BB fraction of total AOD is high, primarily evergreen or deciduous forests. In heavily polluted or agricultural burning regions, where smoke and background AOD values tend to be comparable, this approach

Refined Use of Satellite Aerosol Optical Depth Snapshots to Constrain Biomass Burning Emissions in the GOCART Model

NASA Technical Reports Server (NTRS)

Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Limbacher, James

2017-01-01

Simulations of biomass burning (BB) emissions in global chemistry and aerosol transport models depend on external inventories, which provide location and strength of burning aerosol sources. Our previous work (Petrenko et al., 2012) shows that satellite snapshots of aerosol optical depth (AOD) near the emitted smoke plume can be used to constrain model-simulated AOD, and effectively, the assumed source strength. We now refine the satellite-snapshot method and investigate applying simple multiplicative emission correction factors for the widely used Global Fire Emission Database version 3 (GFEDv3) emission inventory can achieve regional-scale consistency between MODIS AOD snapshots and the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. The model and satellite AOD are compared over a set of more than 900 BB cases observed by the MODIS instrument during the 2004, and 2006-2008 biomass burning seasons. The AOD comparison presented here shows that regional discrepancies between the model and satellite are diverse around the globe yet quite consistent within most ecosystems. Additional analysis of including small fire emission correction shows the complimentary nature of correcting for source strength and adding missing sources, and also indicates that in some regions other factors may be significant in explaining model-satellite discrepancies. This work sets the stage for a larger intercomparison within the Aerosol Inter-comparisons between Observations and Models (AeroCom) multi-model biomass burning experiment. We discuss here some of the other possible factors affecting the remaining discrepancies between model simulations and observations, but await comparisons with other AeroCom models to draw further conclusions.

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

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

EPA Science Inventory

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

A Global Model Simulation of Aerosol Effects of Surface Radiation Budget- Toward Understanding of the "Dimming to Brightening" Transition

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Bian, Huisheng; Yu, Hongbin

2008-01-01

We present a global model study on the role aerosols play in the change of solar radiation at Earth's surface that transitioned from a decreasing (dimming) trend to an increasing (brightening) trend. Our primary objective is to understand the relationship between the long-term trends of aerosol emission, atmospheric burden, and surface solar radiation. More specifically, we use the recently compiled comprehensive global emission datasets of aerosols and precursors from fuel combustion, biomass burning, volcanic eruptions and other sources from 1980 to 2006 to simulate long-term variations of aerosol distributions and optical properties, and then calculate the multi-decadal changes of short-wave radiative fluxes at the surface and at the top of the atmosphere by coupling the GOCART model simulated aerosols with the Goddard radiative transfer model. The model results are compared with long-term observational records from ground-based networks and satellite data. We will address the following critical questions: To what extent can the observed surface solar radiation trends, known as the transition from dimming to brightening, be explained by the changes of anthropogenic and natural aerosol loading on global and regional scales? What are the relative contributions of local emission and long-range transport to the surface radiation budget and how do these contributions change with time?

Known and Newly Identified Semi-Volatile Organic Compounds from Biomass Burning in Amazonia: Variability and Relationship to Aerosol Physical Properties

NASA Astrophysics Data System (ADS)

Wernis, R. A.; Yee, L.; Isaacman-VanWertz, G. A.; Kreisberg, N. M.; de Sá, S. S.; Liu, Y.; Martin, S. T.; Alexander, M. L. L.; Palm, B. B.; Hu, W.; Campuzano-Jost, P.; Day, D. A.; Jimenez, J. L.; Artaxo, P.; Viegas, J.; Manzi, A. O.; Souza, R. A. F. D.; Hering, S. V.; Goldstein, A. H.

2016-12-01

Aerosols are a source of great uncertainty in radiative forcing predictions and have poorly understood impacts on human health. In many environments, biomass burning contributes a significant source of primary aerosol as well as reactive gas-phase precursors that can form secondary organic aerosol (SOA). One class of these precursors, semi-volatile organic compounds (SVOCs), has been shown to have a large contribution to the amount of SOA formed from fire emissions. At present, SVOC emissions from biomass burning are poorly constrained and understanding their contributions to SOA formation is an important research challenge. In the Amazonian dry season, biomass burning is a major source of gases and aerosols reducing regional air quality. As part of the GoAmazon 2014/5 field campaign, we deployed the Semi-Volatile Thermal desorption Aerosol Gas Chromatograph (SV-TAG) instrument at the rural T3 site, 60 km to the west of Manaus, Brazil to measure hourly concentrations of SVOCs in the gas and particle phases. This comprehensive technique detects thousands of compounds, enabling the discovery of previously unidentified compounds. In this work we explore compounds for which a correlation with well-known biomass burning tracers is observed to discover the identities of new markers. We discuss contributions to the total organic aerosol from over 30 well-known, rarely reported and newly identified biomass burning markers. We examine the relationship between biomass burning aerosol composition and aerosol physical properties as measured at the T3 site. Additionally, we report gas-particle partitioning of all identified compounds with comparison to theoretical predictions. We find that the commonly used biomass burning tracer levoglucosan existed entirely in the particle phase and contributed 0.6% and 0.3% of total organic aerosol mass in the dry and wet seasons, respectively.

Improved attribution of climate forcing to emissions by pollutant and sector

NASA Astrophysics Data System (ADS)

Shindell, D. T.

2009-12-01

Evaluating multi-component 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. I will show new calculations of atmospheric composition changes, radiative forcing, and the global warming potential (GWP) for increased emissions of tropospheric ozone and aerosol precursors in a coupled composition-climate model. The results demonstrate that gas-aerosol interactions substantially alter the relative importance of the various emissions, suggesting revisions to the GWPs used in international carbon trading. Additionally, I will present results showing how the net climate impact of particular activities depends strongly upon non-CO2 forcing agents for some sectors. These results will be highlighted by discussing the interplay between air quality emissions controls and climate for the case of emissions from coal-fired power plants. The changing balance between CO2 and air quality pollutants from coal plants may have contributed to the 20th century spatial and temporal patterns of climate change, and is likely to continue to do so as more and more plants are constructed in Asia.

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

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

Vibrational dynamic and spectroscopic molecular parameters of trans-Methylglyoxal, a gaseous precursor of secondary organic aerosols

NASA Astrophysics Data System (ADS)

Bteich, S.; Goubet, M.; Motiyenko, R. A.; Margulès, L.; Huet, T. R.

2018-06-01

Methylglyoxal is a secondary product of oxidation of isoprene and as such one of the most abundant α -dicarbonyls present in the atmosphere. Due to its low vapor pressure, it is highly suspected to be a secondary organic aerosols precursor. The rotational spectrum of Methylglyoxal in its vibrational ground state has been reinvestigated in the 4-500 GHz range and fitted to instrumental accuracies using a model taking into account the methyl group internal rotation motion and with the support of quantum chemistry calculations. Reliability of the line assignments and extracted molecular parameters is confirmed by the good agreement between experiments and calculations.

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;

Isoprene derived secondary organic aerosol in a global aerosol chemistry climate model

NASA Astrophysics Data System (ADS)

Stadtler, Scarlet; Kühn, Thomas; Taraborrelli, Domenico; Kokkola, Harri; Schultz, Martin

2017-04-01

Secondary organic aerosol (SOA) impacts earth's climate and human health. Since its precursor chemistry and its formation are not fully understood, climate models cannot catch its direct and indirect effects. Global isoprene emissions are higher than any other non-methane hydrocarbons. Therefore, SOA from isoprene-derived, low volatile species (iSOA) is simulated using a global aerosol chemistry climate model ECHAM6-HAM-SALSA-MOZ. Isoprene oxidation in the chemistry model MOZ is following a novel semi-explicit scheme, embedded in a detailed atmospheric chemical mechanism. For iSOA formation four low volatile isoprene oxidation products were identified. The group method by Nanoonlal et al. 2008 was used to estimate their evaporation enthalpies ΔHvap. To calculate the saturation concentration C∗(T) the sectional aerosol model SALSA uses the gas phase concentrations simulated by MOZ and their corresponding ΔHvap to obtain the saturation vapor pressure p∗(T) from the Clausius Clapeyron equation. Subsequently, the saturation concentration is used to calculate the explicit kinetic partitioning of these compounds forming iSOA. Furthermore, the irreversible heterogeneous reactions of IEPOX and glyoxal from isoprene were included. The possibility of reversible heterogeneous uptake was ignored at this stage, leading to an upper estimate of the contribution of glyoxal to iSOA mass.

AerChemMIP: Quantifying the effects of chemistry and aerosols in CMIP6

DOE PAGES

Collins, William J.; Lamarque, Jean -François; Schulz, Michael; ...

2017-02-09

The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) is endorsed by the Coupled-Model Intercomparison Project 6 (CMIP6) and is designed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. These are specifically near-term climate forcers (NTCFs: methane, tropospheric ozone and aerosols, and their precursors), nitrous oxide and ozone-depleting halocarbons. The aim of AerChemMIP is to answer four scientific questions. 1. How have anthropogenic emissions contributed to global radiative forcing and affected regional climate over the historical period? 2. How might future policies (on climate, air quality and land use) affect the abundances of NTCFs and theirmore » climate impacts? 3.How do uncertainties in historical NTCF emissions affect radiative forcing estimates? 4. How important are climate feedbacks to natural NTCF emissions, atmospheric composition, and radiative effects? These questions will be addressed through targeted simulations with CMIP6 climate models that include an interactive representation of tropospheric aerosols and atmospheric chemistry. These simulations build on the CMIP6 Diagnostic, Evaluation and Characterization of Klima (DECK) experiments, the CMIP6 historical simulations, and future projections performed elsewhere in CMIP6, allowing the contributions from aerosols and/or chemistry to be quantified. As a result, specific diagnostics are requested as part of the CMIP6 data request to highlight the chemical composition of the atmosphere, to evaluate the performance of the models, and to understand differences in behaviour between them.« less

AerChemMIP: Quantifying the effects of chemistry and aerosols in CMIP6

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

Collins, William J.; Lamarque, Jean -François; Schulz, Michael

The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) is endorsed by the Coupled-Model Intercomparison Project 6 (CMIP6) and is designed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. These are specifically near-term climate forcers (NTCFs: methane, tropospheric ozone and aerosols, and their precursors), nitrous oxide and ozone-depleting halocarbons. The aim of AerChemMIP is to answer four scientific questions. 1. How have anthropogenic emissions contributed to global radiative forcing and affected regional climate over the historical period? 2. How might future policies (on climate, air quality and land use) affect the abundances of NTCFs and theirmore » climate impacts? 3.How do uncertainties in historical NTCF emissions affect radiative forcing estimates? 4. How important are climate feedbacks to natural NTCF emissions, atmospheric composition, and radiative effects? These questions will be addressed through targeted simulations with CMIP6 climate models that include an interactive representation of tropospheric aerosols and atmospheric chemistry. These simulations build on the CMIP6 Diagnostic, Evaluation and Characterization of Klima (DECK) experiments, the CMIP6 historical simulations, and future projections performed elsewhere in CMIP6, allowing the contributions from aerosols and/or chemistry to be quantified. As a result, specific diagnostics are requested as part of the CMIP6 data request to highlight the chemical composition of the atmosphere, to evaluate the performance of the models, and to understand differences in behaviour between them.« less

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

PubMed Central

2009-01-01

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

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

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

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

PubMed

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

2014-06-12

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

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.

Primary emissions and secondary aerosol production potential from woodstoves for residential heating: Influence of the stove technology and combustion efficiency

NASA Astrophysics Data System (ADS)

Bertrand, Amelie; Stefenelli, Giulia; Bruns, Emily A.; Pieber, Simone M.; Temime-Roussel, Brice; Slowik, Jay G.; Prévôt, André S. H.; Wortham, Henri; El Haddad, Imad; Marchand, Nicolas

2017-11-01

To reduce the influence of biomass burning on air quality, consumers are encouraged to replace their old woodstove with new and cleaner appliances. While their primary emissions have been extensively investigated, the impact of atmospheric aging on these emissions, including secondary organic aerosol (SOA) formation, remains unknown. Here, using an atmospheric smog chamber, we aim at understanding the chemical nature and quantify the emission factors of the primary organic aerosols (POA) from three types of appliances for residential heating, and to assess the influence of aging thereon. Two, old and modern, logwood stoves and one pellet burner were operated under typical conditions. Emissions from an entire burning cycle (past the start-up operation) were injected, including the smoldering and flaming phases, resulting in highly variable emission factors. The stoves emitted a significant fraction of POA (up to 80%) and black carbon. After ageing, the total mass concentration of organic aerosol (OA) increased on average by a factor of 5. For the pellet stove, flaming conditions were maintained throughout the combustion. The aerosol was dominated by black carbon (over 90% of the primary emission) and amounted to the same quantity of primary aerosol emitted by the old logwood stove. However, after ageing, the OA mass was increased by a factor of 1.7 only, thus rendering OA emissions by the pellet stove almost negligible compared to the other two stoves tested. Therefore, the pellet stove was the most reliable and least polluting appliance out of the three stoves tested. The spectral signatures of the POA and aged emissions by a High Resolution - Time of Flight - Aerosol Mass Spectrometer (Electron Ionization (EI) at 70 eV) were also investigated. The m/z 44 (CO2+) and high molecular weight fragments (m/z 115 (C9H7+), 137 (C8H9O2+), 167 (C9H11O3+) and 181 (C9H9O4+, C14H13+)) correlate with the modified combustion efficiency (MCE) allowing us to discriminate further

Trends in multi-pollutant emissions from a technology-linked inventory for India: I. Industry and transport sectors

NASA Astrophysics Data System (ADS)

Sadavarte, Pankaj; Venkataraman, Chandra

2014-12-01

Emissions estimation, for research and regulatory applications including reporting to international conventions, needs treatment of detailed technology divisions and high-emitting technologies. Here we estimate Indian emissions, for 1996-2015, of aerosol constituents (PM2.5, BC and OC) and precursor gas SO2, ozone precursors (CO, NOx, NMVOC and CH4) and greenhouse gases (CO2 and N2O), using a common fuel consumption database and consistent assumptions. Six source categories and 45 technologies/activities in the industry and transport sectors were used for estimating emissions for 2010. Mean emission factors, developed at the source-category level, were used with corresponding fuel consumption data, available for 1996-2011, projected to 2015. New activities were included to account for fugitive emissions of NMVOC from chemical and petrochemical industries. Dynamic emission factors, reflecting changes in technology-mix and emission regulations, were developed for thermal power plants and on-road transport vehicles. Modeled emission factors were used for gaseous pollutants for on-road vehicles. Emissions of 2.4 (0.6-7.5) Tg y-1 PM2.5, 0.23 (0.1-0.7) Tg y-1 BC, 0.15 (0.04-0.5) Tg y-1 OC, 7.3 (6-10) Tg y-1 SO2, 19 (7.5-33) Tg y-1 CO, 1.5 (0.1-9) Tg y-1 CH4, 4.3 (2-9) Tg y-1 NMVOC, 5.6 (1.7-15.9) Tg y-1 NOx, 1750 (1397-2231) Tg y-1 CO2 and 0.13 (0.05-0.3) Tg y-1 N2O were estimated for 2015. Significant emissions of aerosols and their precursors were from coal use in thermal power and industry (PM2.5 and SO2), and on-road diesel vehicles (BC), especially superemitters. Emissions of ozone precursors were largely from thermal power plants (NOx), on-road gasoline vehicles (CO and NMVOC) and fugitive emissions from mining (CH4). Highly uncertain default emission factors were the principal contributors to uncertainties in emission estimates, indicating the need for region specific measurements.

OBSERVABLE INDICATORS OF THE SENSITIVITY OF PM 2.5 NITRATE TO EMISSION REDUCTIONS, PART II: SENSITIVITY TO ERRORS IN TOTAL AMMONIA AND TOTAL NITRATE OF THE CMAQ-PREDICTED NONLINEAR EFFECT OF SO 2 EMISSION REDUCTIONS

EPA Science Inventory

The inorganic aerosol system of sulfate, nitrate, and ammonium can respond nonlinearly to changes in precursor sulfur dioxide (SO₂) emissions. The potential increase in nitrate, when sulfate is reduced and the associated ammonia is released, can negate the sulfate mass...

Characterization of Wildfire-Induced Aerosol Emissions From the Maritime Continent Peatland and Central African Dry Savannah with MISR and CALIPSO Aerosol Products

NASA Astrophysics Data System (ADS)

Lee, Huikyo; Jeong, Su-Jong; Kalashnikova, Olga; Tosca, Mika; Kim, Sang-Woo; Kug, Jong-Seong

2018-03-01

Aerosol plumes from wildfires affect the Earth's climate system through regulation of the radiative budget and clouds. However, optical properties of aerosols from individual wildfire smoke plumes and their resultant impact on regional climate are highly variable. Therefore, there is a critical need for observations that can constrain the partitioning between different types of aerosols. Here we present the apparent influence of regional ecosystem types on optical properties of wildfire-induced aerosols based on remote sensing observations from two satellite instruments and three ground stations. The independent observations commonly show that the ratio of the absorbing aerosols is significantly lower in smoke plumes from the Maritime Continent than those from Central Africa, so that their impacts on regional climate are different. The observed light-absorbing properties of wildfire-induced aerosols are explained by dominant ecosystem types such as wet peatlands for the Maritime Continent and dry savannah for Central Africa, respectively. These results suggest that the wildfire-aerosol-climate feedback processes largely depend on the terrestrial environments from which the fires originate. These feedbacks also interact with climate under greenhouse warming. Our analysis shows that aerosol optical properties retrieved based on satellite observations are critical in assessing wildfire-induced aerosols forcing in climate models. The optical properties of carbonaceous aerosol mixtures used by state-of-the-art chemistry climate models may overestimate emissions for absorbing aerosols from wildfires over the Maritime Continent.

Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

NASA Astrophysics Data System (ADS)

Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

2017-12-01

Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

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

Assessing the effects of oil sands related ozone precursor emissions on ambient ozone levels in the Alberta oil sands region, Canada

NASA Astrophysics Data System (ADS)

Cho, Sunny; Vijayaraghavan, Krish; Spink, David; Cosic, Biljana; Davies, Mervyn; Jung, Jaegun

2017-11-01

A study was undertaken to determine whether, and the extent to which, increased ground-level ozone (O3) precursor emissions from oil sands development have impacted ambient air quality in the north-eastern Alberta, Canada, over the period 1998 to 2012. Temporal trends in emissions of O3 precursors (NOx and VOC) and ambient air concentrations of O3 precursors, and O3 were examined using the Theil-Sen statistical analysis method. Statistically significant correlations between NOx emissions and ambient NOx concentrations were found mainly near surface (open-pit) mining areas where mine fleets are a large source of NOx emissions. No statistically significant trends in the 4th highest daily maximum 8-hr average O3 at any of the continuous and passive ambient air monitoring stations were found. A significant long-term decrease in monthly averaged O3 is observed at some ambient monitoring sites in summer. A visual examination of long-term variations in annual NOx and VOC emissions and annual 4th highest daily maximum 8-hr O3 concentrations does not reveal any indication of a correlation between O3 concentrations and O3 precursor emissions or ambient levels in the study area. Despite a significant increase in oil sands NOx emissions (8%/yr), there is no statistically significant increase in long-term O3 concentrations at any of monitoring stations considered. This suggests that there is surplus NOx available in the environment which results in a titration of ambient O3 in the areas that have ambient monitoring. The limited ambient O3 monitoring data distant from NOx emission sources makes it impossible to assess the impact of these increased O3 precursor levels on O3 levels on a regional scale. As a precautionary measure, the increasing oil sands development O3 precursor emissions would require that priority be given to the management of these emissions to prevent possible future O3 ambient air quality issues.

Cross influences of ozone and sulfate precursor emissions changes on air quality and climate

PubMed Central

Unger, Nadine; Shindell, Drew T.; Koch, Dorothy M.; Streets, David G.

2006-01-01

Tropospheric O3 and sulfate both contribute to air pollution and climate forcing. There is a growing realization that air quality and climate change issues are strongly connected. To date, the importance of the coupling between O3 and sulfate has not been fully appreciated, and thus regulations treat each pollutant separately. We show that emissions of O3 precursors can dramatically affect regional sulfate air quality and climate forcing. At 2030 in an A1B future, increased O3 precursor emissions enhance surface sulfate over India and China by up to 20% because of increased levels of OH and gas-phase SO2 oxidation rates and add up to 20% to the direct sulfate forcing for that region relative to the present day. Hence, O3 precursors impose an indirect forcing via sulfate, which is more than twice the direct O3 forcing itself (compare −0.61 vs. +0.35 W/m2). Regulatory policy should consider both air quality and climate and should address O3 and sulfate simultaneously because of the strong interaction between these species. PMID:16537360

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; ...

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) atmore » BNL 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

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

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

Zhou, Shan; Collier, Sonya; Xu, Jianzhong

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) atmore » BNL 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

SOA formation potential of emissions from soil and leaf litter.

PubMed

Faiola, Celia L; Vanderschelden, Graham S; Wen, Miao; Elloy, Farah C; Cobos, Douglas R; Watts, Richard J; Jobson, B Thomas; Vanreken, Timothy M

2014-01-21

Soil and leaf litter are significant global sources of small oxidized volatile organic compounds, VOCs (e.g., methanol and acetaldehyde). They may also be significant sources of larger VOCs that could act as precursors to secondary organic aerosol (SOA) formation. To investigate this, soil and leaf litter samples were collected from the University of Idaho Experimental Forest and transported to the laboratory. There, the VOC emissions were characterized and used to drive SOA formation via dark, ozone-initiated reactions. Monoterpenes dominated the emission profile with emission rates as high as 228 μg-C m(-2) h(-1). The composition of the SOA produced was similar to biogenic SOA formed from oxidation of ponderosa pine emissions and α-pinene. Measured soil and litter monoterpene emission rates were compared with modeled canopy emissions. Results suggest surface soil and litter monoterpene emissions could range from 12 to 136% of canopy emissions in spring and fall. Thus, emissions from leaf litter may potentially extend the biogenic emissions season, contributing to significant organic aerosol formation in the spring and fall when reduced solar radiation and temperatures reduce emissions from living vegetation.

SOA formation potential of emissions from soil and leaf litter

DOE PAGES

Faiola, Celia L.; VanderSchelden, Graham S.; Wen, Miao; ...

2013-12-13

Soil and leaf litter are significant global sources of small oxidized volatile organic compounds, VOCs (e.g., methanol and acetaldehyde). They may also be significant sources of larger VOCs that could act as precursors to secondary organic aerosol (SOA) formation. To investigate this, soil and leaf litter samples were collected from the University of Idaho Experimental Forest and transported to the laboratory. There, the VOC emissions were characterized and used to drive SOA formation via dark, ozone-initiated reactions. Monoterpenes dominated the emission profile with emission rates as high as 228 μg-C m –2 h –1. The composition of the SOA producedmore » was similar to biogenic SOA formed from oxidation of ponderosa pine emissions and α-pinene. Measured soil and litter monoterpene emission rates were compared with modeled canopy emissions. Results suggest surface soil and litter monoterpene emissions could range from 12 to 136% of canopy emissions in spring and fall. Furthermore, emissions from leaf litter may potentially extend the biogenic emissions season, contributing to significant organic aerosol formation in the spring and fall when reduced solar radiation and temperatures reduce emissions from living vegetation.« less

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

NASA Astrophysics Data System (ADS)

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

2006-12-01

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

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

The effect of South American biomass burning aerosol emissions on the regional climate

NASA Astrophysics Data System (ADS)

Thornhill, Gillian D.; Ryder, Claire L.; Highwood, Eleanor J.; Shaffrey, Len C.; Johnson, Ben T.

2018-04-01

The impact of biomass burning aerosol (BBA) on the regional climate in South America is assessed using 30-year simulations with a global atmosphere-only configuration of the Met Office Unified Model. We compare two simulations of high and low emissions of biomass burning aerosol based on realistic interannual variability. The aerosol scheme in the model has hygroscopic growth and optical properties for BBA informed by recent observations, including those from the recent South American Biomass Burning Analysis (SAMBBA) intensive aircraft observations made during September 2012. We find that the difference in the September (peak biomass emissions month) BBA optical depth between a simulation with high emissions and a simulation with low emissions corresponds well to the difference in the BBA emissions between the two simulations, with a 71.6 % reduction from high to low emissions for both the BBA emissions and the BB AOD in the region with maximum emissions (defined by a box of extent 5-25° S, 40-70° W, used for calculating mean values given below). The cloud cover at all altitudes in the region of greatest BBA difference is reduced as a result of the semi-direct effect, by heating of the atmosphere by the BBA and changes in the atmospheric stability and surface fluxes. Within the BBA layer the cloud is reduced by burn-off, while the higher cloud changes appear to be responding to stability changes. The boundary layer is reduced in height and stabilized by increased BBA, resulting in reduced deep convection and reduced cloud cover at heights of 9-14 km, above the layer of BBA. Despite the decrease in cloud fraction, September downwelling clear-sky and all-sky shortwave radiation at the surface is reduced for higher emissions by 13.77 ± 0.39 W m-2 (clear-sky) and 7.37 ± 2.29 W m-2 (all-sky), whilst the upwelling shortwave radiation at the top of atmosphere is increased in clear sky by 3.32 ± 0.09 W m-2, but decreased by -1.36±1.67 W m-2 when cloud changes are

Distinguishing the roles of meteorology, emission control measures, regional transport, and co-benefits of reduced aerosol feedbacks in ;APEC Blue;

NASA Astrophysics Data System (ADS)

Gao, Meng; Liu, Zirui; Wang, Yuesi; Lu, Xiao; Ji, Dongsheng; Wang, Lili; Li, Meng; Wang, Zifa; Zhang, Qiang; Carmichael, Gregory R.

2017-10-01

Air quality are strongly influenced by both emissions and meteorological conditions. During the Asia Pacific Economic Cooperation (APEC) week (November 5-11, 2014), the Chinese government implemented unprecedented strict emission control measures in Beijing and surrounding provinces, and then a phenomenon referred to as ;APEC Blue; (rare blue sky) occurred. It is challenging to quantify the effectiveness of the implemented strict control measures solely based on observations. In this study, we use the WRF-Chem model to distinguish the roles of meteorology, emission control measures, regional transport, and co-benefits of reduced aerosol feedbacks during APEC week. In general, meteorological variables, PM2.5 concentrations and PM2.5 chemical compositions are well reproduced in Beijing. Positive weather conditions (lower temperature, lower relative humidity, higher wind speeds and enhanced boundary layer heights) play important roles in ;APEC Blue;. Applying strict emission control measures in Beijing and five surrounding provinces can only explain an average decrease of 17.7 μg/m3 (-21.8%) decreases in PM2.5 concentrations, roughly more than half of which is caused by emission controls that implemented in the five surrounding provinces (12.5 μg/m3). During the APEC week, non-local emissions contributed to 41.3% to PM2.5 concentrations in Beijing, and the effectiveness of implementing emission control measures hinges on dominant pathways and transport speeds. Besides, we also quantified the contribution of reduced aerosol feedbacks due to strict emission control measures in this study. During daytime, co-benefits of reduced aerosol feedbacks account for about 10.9% of the total decreases in PM2.5 concentrations in urban Beijing. The separation of contributions from aerosol absorption and scattering restates the importance of controlling BC to accelerate the effectiveness of aerosol pollution control.

Secondary Inorganic Aerosols over an Urban Location in North-Western Himalayan Region: Seasonal Variation in Composition and Formation Process(es)

NASA Astrophysics Data System (ADS)

Kaushal, D.; Tandon, A.

2017-12-01

Oxidative photo-chemical transformation of precursor gases, mainly of anthropogenic origin, produces secondary aerosols. Secondary inorganic aerosols constitute a significant fraction of total aerosol load over urban locations especially high altitude in wet-temperate climatic set-up. Towns situated in North-Western Himalayan region (NWHR) with sizable population and attractive tourist destinations have been facing ever increasing problem of gaseous and particulate air pollution from exponential increase in vehicular traffic and other anthropogenic emissions. The present study has been planned to investigate the seasonal variations in atmospheric processes responsible for the formation of Secondary Inorganic Aerosols (SIA) and to estimate contribution of SIA to PM­10 load over an Urban location, Dharamshala, in Dhauladhar region of NWHR. Twenty four hourly PM10 aerosol samples were collected, on quartz micro fibre filters in Dharamshala (1350 amsl) on weekly basis for complete one year time-period (February 2015 - January 2016). These samples were analyzed for Water Soluble Inorganic Ions (WSII) using Ion-Chromatographic System. On annual basis, SO42- ions contributed maximum (52%) followed by NO3- (13%) and NH4+ (12%) to WSII. Based upon Principal Component Analysis (PCA), dominant sources contributing to PM10 associated WSII were identified as: Fossil-Fuel and Bio-mass burning, Vehicular (mainly diesel) emissions and gaseous emissions from the microbial degradation of dead bio-mass. Throughout the year, significantly high proportion of SO42- and considerable thermodynamic stability of (NH4)2SO2 at ambient temperatures, made it the major contributor to SIA over NH4NO3 and NH4Cl. On seasonal basis, maximum contribution of SIA to PM10 was observed in monsoon followed by the winter season. Low ambient temperature in winter season favoured formation of NH4NO3 with significant contribution to SIA. It could be concluded that observed variability in the composition and

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.

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.

Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

NASA Astrophysics Data System (ADS)

Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Flynn, M. J.; Harrison, R. M.; Yin, J.; Gallagher, M. W.; Coe, H.

2014-07-01

For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±one standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52) and 0.15 (±0.24) μg m-3, contributing 43, 28, 14, 13 and 2% to the total submicron mass, respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF) where five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3, respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species, due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual pollution events influence London

Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

NASA Astrophysics Data System (ADS)

Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Flynn, M. J.; Harrison, R. M.; Yin, J.; Gallagher, M. W.; Coe, H.

2015-06-01

For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show that secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±1 standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52), and 0.15 (±0.24) μg m-3, contributing 44, 28, 14, 13, and 2 % to the total non-refractory submicron mass (NR-PM1) respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF), in which five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3 respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual

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.

Diurnal cycling of urban aerosols under different weather regimes

NASA Astrophysics Data System (ADS)

Gregorič, Asta; Drinovec, Luka; Močnik, Griša; Remškar, Maja; Vaupotič, Janja; Stanič, Samo

2016-04-01

A one month measurement campaign was performed in summer 2014 in Ljubljana, the capital of Slovenia (population 280,000), aiming to study temporal and spatial distribution of urban aerosols and the mixing state of primary and secondary aerosols. Two background locations were chosen for this purpose, the first one in the city center (urban background - KIS) and the second one in the suburban background (Brezovica). Simultaneous measurements of black carbon (BC) and particle number size distribution of submicron aerosols (PM1) were conducted at both locations. In the summer season emission from traffic related sources is expected to be the main local contribution to BC concentration. Concentrations of aerosol species and gaseous pollutants within the planetary boundary layer are controlled by the balance between emission sources of primary aerosols and gases, production of secondary aerosols, chemical reactions of precursor gases under solar radiation and the rate of dilution by mixing within the planetary boundary layer (PBL) as well as with tropospheric air. Only local emission sources contribute to BC concentration during the stable PBL with low mixing layer height, whereas during the time of fully mixed PBL, regionally transported BC and other aerosols can contribute to the surface measurements. The study describes the diurnal behaviour of the submicron aerosol at the urban and suburban background location under different weather regimes. Particles in three size modes - nucleation (< 25 nm, NUM), Aitken (25 - 90 nm, AIM) and accumulation mode (90 - 800 nm, ACM), as well as BC mass concentration were evaluated separately for sunny, cloudy and rainy days, taking into account modelled values of PBL height. Higher particle number and black carbon concentrations were observed at the urban background (KIS) than at the suburban background location (Brezovica). Significant diurnal pattern of total particle concentration and black carbon concentration was observed at both

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.

Indoor terpene emissions from cooking with herbs and pepper and their secondary organic aerosol production potential

PubMed Central

Klein, Felix; Farren, Naomi J.; Bozzetti, Carlo; Daellenbach, Kaspar R.; Kilic, Dogushan; Kumar, Nivedita K.; Pieber, Simone M.; Slowik, Jay G.; Tuthill, Rosemary N.; Hamilton, Jacqueline F.; Baltensperger, Urs; Prévôt, André S. H.; El Haddad, Imad

2016-01-01

Cooking is widely recognized as an important source of indoor and outdoor particle and volatile organic compound emissions with potential deleterious effects on human health. Nevertheless, cooking emissions remain poorly characterized. Here the effect of herbs and pepper on cooking emissions was investigated for the first time to the best of our knowledge using state of the art mass spectrometric analysis of particle and gas-phase composition. Further, the secondary organic aerosol production potential of the gas-phase emissions was determined by smog chamber aging experiments. The emissions of frying meat with herbs and pepper include large amounts of mono-, sesqui- and diterpenes as well as various terpenoids and p-cymene. The average total terpene emission rate from the use of herbs and pepper during cooking is estimated to be 46 ± 5 gg-1Herbs min-1. These compounds are highly reactive in the atmosphere and lead to significant amounts of secondary organic aerosol upon aging. In summary we demonstrate that cooking with condiments can constitute an important yet overlooked source of terpenes in indoor air. PMID:27830718

Indoor terpene emissions from cooking with herbs and pepper and their secondary organic aerosol production potential

NASA Astrophysics Data System (ADS)

Klein, Felix; Farren, Naomi J.; Bozzetti, Carlo; Daellenbach, Kaspar R.; Kilic, Dogushan; Kumar, Nivedita K.; Pieber, Simone M.; Slowik, Jay G.; Tuthill, Rosemary N.; Hamilton, Jacqueline F.; Baltensperger, Urs; Prévôt, André S. H.; El Haddad, Imad

2016-11-01

Cooking is widely recognized as an important source of indoor and outdoor particle and volatile organic compound emissions with potential deleterious effects on human health. Nevertheless, cooking emissions remain poorly characterized. Here the effect of herbs and pepper on cooking emissions was investigated for the first time to the best of our knowledge using state of the art mass spectrometric analysis of particle and gas-phase composition. Further, the secondary organic aerosol production potential of the gas-phase emissions was determined by smog chamber aging experiments. The emissions of frying meat with herbs and pepper include large amounts of mono-, sesqui- and diterpenes as well as various terpenoids and p-cymene. The average total terpene emission rate from the use of herbs and pepper during cooking is estimated to be 46 ± 5 gg-1Herbs min-1. These compounds are highly reactive in the atmosphere and lead to significant amounts of secondary organic aerosol upon aging. In summary we demonstrate that cooking with condiments can constitute an important yet overlooked source of terpenes in indoor air.

Indoor terpene emissions from cooking with herbs and pepper and their secondary organic aerosol production potential.

PubMed

Klein, Felix; Farren, Naomi J; Bozzetti, Carlo; Daellenbach, Kaspar R; Kilic, Dogushan; Kumar, Nivedita K; Pieber, Simone M; Slowik, Jay G; Tuthill, Rosemary N; Hamilton, Jacqueline F; Baltensperger, Urs; Prévôt, André S H; El Haddad, Imad

2016-11-10

Cooking is widely recognized as an important source of indoor and outdoor particle and volatile organic compound emissions with potential deleterious effects on human health. Nevertheless, cooking emissions remain poorly characterized. Here the effect of herbs and pepper on cooking emissions was investigated for the first time to the best of our knowledge using state of the art mass spectrometric analysis of particle and gas-phase composition. Further, the secondary organic aerosol production potential of the gas-phase emissions was determined by smog chamber aging experiments. The emissions of frying meat with herbs and pepper include large amounts of mono-, sesqui- and diterpenes as well as various terpenoids and p-cymene. The average total terpene emission rate from the use of herbs and pepper during cooking is estimated to be 46 ± 5 gg -1 Herbs min -1 . These compounds are highly reactive in the atmosphere and lead to significant amounts of secondary organic aerosol upon aging. In summary we demonstrate that cooking with condiments can constitute an important yet overlooked source of terpenes in indoor air.

The Impact of Pre-Industrial Land Use Change on Atmospheric Composition and Aerosol Radiative Forcing.

NASA Astrophysics Data System (ADS)

Hamilton, D. S.; Carslaw, K. S.; Spracklen, D. V.; Folberth, G.; Kaplan, J. O.; Pringle, K.; Scott, C.

2015-12-01

Anthropogenic land use change (LUC) has had a major impact on the climate by altering the amount of carbon stored in vegetation, changing surface albedo and modifying the levels of both biogenic and pyrogenic emissions. While previous studies of LUC have largely focused on the first two components, there has recently been a recognition that changes to aerosol and related pre-cursor gas emissions from LUC are equally important. Furthermore, it has also recently been recognised that the pre-industrial (PI) to present day (PD) radiative forcing (RF) of climate from aerosol cloud interactions (ACI) due to anthropogenic emissions is highly sensitive to the amount of natural aerosol that was present in the PI. This suggests that anthropogenic RF from ACI may be highly sensitive to land-use in the PI. There are currently two commonly used baseline reference years for the PI; 1750 and 1860. Rapid LUC occurred between 1750 and 1860, with large reductions in natural vegetation cover in Eastern Northern America, Europe, Central Russia, India and Eastern China as well as lower reductions in parts of Brazil and Africa. This LUC will have led to significant changes in biogenic and fire emissions with implications for natural aerosol concentrations and PI-to-PD RF. The focus of this study is therefore to quantify the impact of LUC between 1750 and 1860 on aerosol concentrations and PI-to-PD RF calculations from ACI. We use the UK Met Office HadGEM3-UKCA coupled-chemistry-climate model to calculate the impacts of anthropogenic emissions and anthropogenic LUC on aerosol size distributions in both 1750 and 1860. We prescribe LUC using the KK10 historical dataset of land cover change. Monoterpene emissions are coupled directly to the prescribed LUC through the JULES land surface scheme in HadGEM3. Fire emissions from LUC were calculated offline using the fire module LPJ-LMfire in the Lund-Potsdam-Jena dynamic global vegetation model. To separate out the impacts of LUC from

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

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

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 wasmore » 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.« less

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

2015-10-06

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.

Simulating and Analyzing Long-Term Changes in Emissions, Air Quality, Aerosol Feedback Effects and Human Health

EPA Science Inventory

This presentation covers work performed by the authors to characterize changes in emissions over the 1990 – 2010 time period, quantify the effects of these emission changes on air quality and aerosol/radiation feedbacks using both observations and model simulations, and fin...

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Multiday production of condensing organic aerosol mass in urban and forest outflow

DOE PAGES

Lee-Taylor, J.; Hodzic, A.; Madronich, S.; ...

2014-07-03

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1–2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products ofmore » both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

Ethylene glycol emissions from on-road vehicles: implications for aqueous phase secondary organic aerosol formation

NASA Astrophysics Data System (ADS)

Wood, E. C.; Knighton, W. B.; Fortner, E.; Herndon, S. C.; Onasch, T. B.; Franklin, J.; Harley, R. A.; Gentner, D. R.; Goldstein, A. H.

2012-12-01

Ethylene glycol (HOCH2CH2OH), used as an engine coolant for most on-road vehicles, is an intermediate volatility organic compound (IVOC) with a high Henry's Law Coefficient (kH > 10,000 M atm-1) . Oxidation of ethylene glycol, especially in the atmospheric aqueous phase (clouds, fog, wet aerosol), can lead to the formation of glycolaldehyde, oxalic acid, and ultimately secondary organic aerosol. We present measurements of unexpectedly high ethylene glycol emissions in the Caldecott Tunnel near San Francisco (Summer 2010) and the Washburn Tunnel near Houston (Spring 2009). Ethylene glycol was detected using a proton-transfer reaction mass spectrometer (PTR-MS) at m/z = 45, which is usually interpreted as acetaldehyde. Although not necessarily a tailpipe emission, effective fuel-based emission factors are calculated using the carbon balance method and range from 50 to 400 mg ethylene glycol per kg fuel. Total US and global emissions are estimated using these emission factors and fuel consumption rates and are compared to previous model estimates of ethylene glycol emissions (e.g., the Regional Atmospheric Chemistry Model). Compared to biogenically emitted isoprene, ethylene glycol is likely a minor source of glycolaldehyde globally, but may contribute significantly to glycolaldehyde, oxalate and SOA formation in areas dominated by urban emissions.

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,...

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. Copyright © 2010 Elsevier B.V. All rights reserved.

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...

Strong impacts on aerosol indirect effects from historical oxidant changes

NASA Astrophysics Data System (ADS)

Hafsahl Karset, Inger Helene; Koren Berntsen, Terje; Storelvmo, Trude; Alterskjær, Kari; Grini, Alf; Olivié, Dirk; Kirkevåg, Alf; Seland, Øyvind; Iversen, Trond; Schulz, Michael

2018-06-01

Uncertainties in effective radiative forcings through aerosol-cloud interactions (ERFaci, also called aerosol indirect effects) contribute strongly to the uncertainty in the total preindustrial-to-present-day anthropogenic forcing. Some forcing estimates of the total aerosol indirect effect are so negative that they even offset the greenhouse gas forcing. This study highlights the role of oxidants in modeling of preindustrial-to-present-day aerosol indirect effects. We argue that the aerosol precursor gases should be exposed to oxidants of its era to get a more correct representation of secondary aerosol formation. Our model simulations show that the total aerosol indirect effect changes from -1.32 to -1.07 W m-2 when the precursor gases in the preindustrial simulation are exposed to preindustrial instead of present-day oxidants. This happens because of a brightening of the clouds in the preindustrial simulation, mainly due to large changes in the nitrate radical (NO3). The weaker oxidative power of the preindustrial atmosphere extends the lifetime of the precursor gases, enabling them to be transported higher up in the atmosphere and towards more remote areas where the susceptibility of the cloud albedo to aerosol changes is high. The oxidation changes also shift the importance of different chemical reactions and produce more condensate, thus increasing the size of the aerosols and making it easier for them to activate as cloud condensation nuclei.

Multi-instrument comparison and compilation of non-methane organic gas emissions from biomass burning and implications for smoke-derived secondary organic aerosol precursors

NASA Astrophysics Data System (ADS)

Hatch, Lindsay E.; Yokelson, Robert J.; Stockwell, Chelsea E.; Veres, Patrick R.; Simpson, Isobel J.; Blake, Donald R.; Orlando, John J.; Barsanti, Kelley C.

2017-01-01

Multiple trace-gas instruments were deployed during the fourth Fire Lab at Missoula Experiment (FLAME-4), including the first application of proton-transfer-reaction time-of-flight mass spectrometry (PTR-TOFMS) and comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry (GC × GC-TOFMS) for laboratory biomass burning (BB) measurements. Open-path Fourier transform infrared spectroscopy (OP-FTIR) was also deployed, as well as whole-air sampling (WAS) with one-dimensional gas chromatography-mass spectrometry (GC-MS) analysis. This combination of instruments provided an unprecedented level of detection and chemical speciation. The chemical composition and emission factors (EFs) determined by these four analytical techniques were compared for four representative fuels. The results demonstrate that the instruments are highly complementary, with each covering some unique and important ranges of compositional space, thus demonstrating the need for multi-instrument approaches to adequately characterize BB smoke emissions. Emission factors for overlapping compounds generally compared within experimental uncertainty, despite some outliers, including monoterpenes. Data from all measurements were synthesized into a single EF database that includes over 500 non-methane organic gases (NMOGs) to provide a comprehensive picture of speciated, gaseous BB emissions. The identified compounds were assessed as a function of volatility; 6-11 % of the total NMOG EF was associated with intermediate-volatility organic compounds (IVOCs). These atmospherically relevant compounds historically have been unresolved in BB smoke measurements and thus are largely missing from emission inventories. Additionally, the identified compounds were screened for published secondary organic aerosol (SOA) yields. Of the total reactive carbon (defined as EF scaled by the OH rate constant and carbon number of each compound) in the BB emissions, 55-77 % was associated with compounds for

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

NASA Astrophysics Data System (ADS)

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

2015-08-01

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

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

Treesearch

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

2009-01-01

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...

Influence of fuel ethanol content on primary emissions and secondary aerosol formation potential for a modern flex-fuel gasoline vehicle

NASA Astrophysics Data System (ADS)

Timonen, Hilkka; Karjalainen, Panu; Saukko, Erkka; Saarikoski, Sanna; Aakko-Saksa, Päivi; Simonen, Pauli; Murtonen, Timo; Dal Maso, Miikka; Kuuluvainen, Heino; Bloss, Matthew; Ahlberg, Erik; Svenningsson, Birgitta; Pagels, Joakim; Brune, William H.; Keskinen, Jorma; Worsnop, Douglas R.; Hillamo, Risto; Rönkkö, Topi

2017-04-01

The effect of fuel ethanol content (10, 85 and 100 %) on primary emissions and on subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. Emissions were characterized during a New European Driving Cycle (NEDC) using a comprehensive set-up of high time-resolution instruments. A detailed chemical composition of the exhaust particulate matter (PM) was studied using a soot particle aerosol mass spectrometer (SP-AMS), and secondary aerosol formation was studied using a potential aerosol mass (PAM) chamber. For the primary gaseous compounds, an increase in total hydrocarbon emissions and a decrease in aromatic BTEX (benzene, toluene, ethylbenzene and xylenes) compounds was observed when the amount of ethanol in the fuel increased. In regard to particles, the largest primary particulate matter concentrations and potential for secondary particle formation was measured for the E10 fuel (10 % ethanol). As the ethanol content of the fuel increased, a significant decrease in the average primary particulate matter concentrations over the NEDC was found. The PM emissions were 0.45, 0.25 and 0.15 mg m-3 for E10, E85 and E100, respectively. Similarly, a clear decrease in secondary aerosol formation potential was observed with a larger contribution of ethanol in the fuel. The secondary-to-primary PM ratios were 13.4 and 1.5 for E10 and E85, respectively. For E100, a slight decrease in PM mass was observed after the PAM chamber, indicating that the PM produced by secondary aerosol formation was less than the PM lost through wall losses or the degradation of the primary organic aerosol (POA) in the chamber. For all fuel blends, the formed secondary aerosol consisted mostly of organic compounds. For E10, the contribution of organic compounds containing oxygen increased from 35 %, measured for primary organics, to 62 % after the PAM chamber. For E85, the contribution of organic compounds containing oxygen increased from 42 % (primary) to 57

Identifying organic aerosol sources by comparing functional group composition in chamber and atmospheric particles

PubMed Central

Russell, Lynn M.; Bahadur, Ranjit; Ziemann, Paul J.

2011-01-01

Measurements of submicron particles by Fourier transform infrared spectroscopy in 14 campaigns in North America, Asia, South America, and Europe were used to identify characteristic organic functional group compositions of fuel combustion, terrestrial vegetation, and ocean bubble bursting sources, each of which often accounts for more than a third of organic mass (OM), and some of which is secondary organic aerosol (SOA) from gas-phase precursors. The majority of the OM consists of alkane, carboxylic acid, hydroxyl, and carbonyl groups. The organic functional groups formed from combustion and vegetation emissions are similar to the secondary products identified in chamber studies. The near absence of carbonyl groups in the observed SOA associated with combustion is consistent with alkane rather than aromatic precursors, and the absence of organonitrate groups can be explained by their hydrolysis in humid ambient conditions. The remote forest observations have ratios of carboxylic acid, organic hydroxyl, and nonacid carbonyl groups similar to those observed for isoprene and monoterpene chamber studies, but in biogenic aerosols transported downwind of urban areas the formation of esters replaces the acid and hydroxyl groups and leaves only nonacid carbonyl groups. The carbonyl groups in SOA associated with vegetation emissions provides striking evidence for the mechanism of esterification as the pathway for possible oligomerization reactions in the atmosphere. Forest fires include biogenic emissions that produce SOA with organic components similar to isoprene and monoterpene chamber studies, also resulting in nonacid carbonyl groups in SOA. PMID:21317360

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,...

On the mixing and evaporation of secondary organic aerosol components.

PubMed

Loza, Christine L; Coggon, Matthew M; Nguyen, Tran B; Zuend, Andreas; Flagan, Richard C; Seinfeld, John H

2013-06-18

The physical state and chemical composition of an organic aerosol affect its degree of mixing and its interactions with condensing species. We present here a laboratory chamber procedure for studying the effect of the mixing of organic aerosol components on particle evaporation. The procedure is applied to the formation of secondary organic aerosol (SOA) from α-pinene and toluene photooxidation. SOA evaporation is induced by heating the chamber aerosol from room temperature (25 °C) to 42 °C over 7 h and detected by a shift in the peak diameter of the SOA size distribution. With this protocol, α-pinene SOA is found to be more volatile than toluene SOA. When SOA is formed from the two precursors sequentially, the evaporation behavior of the SOA most closely resembles that of SOA from the second parent hydrocarbon, suggesting that the structure of the mixed SOA resembles a core of SOA from the initial precursor coated by a layer of SOA from the second precursor. Such a core-and-shell configuration of the organic aerosol phases implies limited mixing of the SOA from the two precursors on the time scale of the experiments, consistent with a high viscosity of at least one of the phases.

Submicron particles influenced by mixed biogenic and anthropogenic emissions: high-resolution aerosol mass spectrometry results from the Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Setyan, A.; Zhang, Q.; Merkel, M.; Knighton, W. B.; Sun, Y.; Song, C.; Shilling, J. E.; Onasch, T. B.; Herndon, S. C.; Worsnop, D. R.; Fast, J. D.; Zaveri, R. A.; Berg, L. K.; Wiedensohler, A.; Flowers, B. A.; Dubey, M. K.; Subramanian, R.

2012-02-01

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 (~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 μg m-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 ˜400 nm in vacuum aerodynamic diameter (Dva), and a condensation mode at ~150 nm, while organics generally displayed a broad distribution in 60-600 nm (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 C1H1.38N0.004O0.44, 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 due to local traffic. Twenty three periods of

Influence of Aerosol Acidity on the Formation of Secondary Organic Aerosol from Biogenic Precursor Hydrocarbons

EPA Science Inventory

Secondary organic aerosol (SOA) formation and dynamics may be important factors for the role of aerosols in adverse health effects, visibility and climate change. Formation of SOA occurs when a parent volatile organic compound is oxidized to create products that form in a conden...

FDATMOS16 non-linear partitioning and organic volatility distributions in urban aerosols

DOE PAGES

Madronich, Sasha; Kleinman, Larry; Conley, Andrew; ...

2015-12-17

Gas-to-particle partitioning of organic aerosols (OA) is represented in most models by Raoult’s law, and depends on the existing mass of particles into which organic gases can dissolve. This raises the possibility of non-linear response of particle-phase OA to the emissions of precursor volatile organic compounds (VOCs) that contribute to this partitioning mass. Implications for air quality management are evident: A strong non-linear dependence would suggest that reductions in VOC emission would have a more-than-proportionate benefit in lowering ambient OA concentrations. Chamber measurements on simple VOC mixtures generally confirm the non-linear scaling between OA and VOCs, usually stated as amore » mass-dependence of the measured OA yields. However, for realistic ambient conditions including urban settings, no single component dominates the composition of the organic particles, and deviations from linearity are presumed to be small. Here we re-examine the linearity question using volatility spectra from several sources: (1) chamber studies of selected aerosols, (2) volatility inferred for aerosols sampled in two megacities, Mexico City and Paris, and (3) an explicit chemistry model (GECKO-A). These few available volatility distributions suggest that urban OA may be only slightly super-linear, with most values of the sensitivity exponent in the range 1.1-1.3, also substantially lower than seen in chambers for some specific aerosols. Furthermore, the rather low values suggest that OA concentrations in megacities are not an inevitable convergence of non-linear effects, but can be addressed (much like in smaller urban areas) by proportionate reductions in emissions.« less

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

Mitigating secondary aerosol generation potentials from biofuel use in the energy sector.

PubMed

Tiwary, Abhishek; Colls, Jeremy

2010-01-01

This paper demonstrates secondary aerosol generation potential of biofuel use in the energy sector from the photochemical interactions of precursor gases on a life cycle basis. The paper is divided into two parts-first, employing life cycle analysis (LCA) to evaluate the extent of the problem for a typical biofuel based electricity production system using five baseline scenarios; second, proposing adequate mitigation options to minimise the secondary aerosol generation potential on a life cycle basis. The baseline scenarios cover representative technologies for 2010 utilising energy crop (miscanthus), short rotation coppiced chips and residual/waste wood in different proportions. The proposed mitigation options include three approaches-biomass gasification prior to combustion, delaying the harvest of biomass, and increasing the geographical distance between the biomass plant and the harvest site (by importing the biofuels). Preliminary results indicate that the baseline scenarios (assuming all the biomass is sourced locally) bear significant secondary aerosol formation potential on a life cycle basis from photochemical neutralisation of acidic emissions (hydrogen chloride and sulphur dioxide) with ammonia. Our results suggest that gasification of miscanthus biomass would provide the best option by minimising the acidic emissions from the combustion plant whereas the other two options of delaying the harvest or importing biofuels from elsewhere would only lead to marginal reduction in the life cycle aerosol loadings of the systems.

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

Historical (1750-2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS)

NASA Astrophysics Data System (ADS)

Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang; Klimont, Zbigniew; Janssens-Maenhout, Greet; Pitkanen, Tyler; Seibert, Jonathan J.; Vu, Linh; Andres, Robert J.; Bolt, Ryan M.; Bond, Tami C.; Dawidowski, Laura; Kholod, Nazar; Kurokawa, June-ichi; Li, Meng; Liu, Liang; Lu, Zifeng; Moura, Maria Cecilia P.; O'Rourke, Patrick R.; Zhang, Qiang

2018-01-01

We present a new data set of annual historical (1750-2014) anthropogenic chemically reactive gases (CO, CH4, NH3, NOx, SO2, NMVOCs), carbonaceous aerosols (black carbon - BC, and organic carbon - OC), and CO2 developed with the Community Emissions Data System (CEDS). We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the same activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.

Recent changes in particulate air pollution over China observed from space and the ground: effectiveness of emission control.

PubMed

Lin, Jintai; Nielsen, Chris P; Zhao, Yu; Lei, Yu; Liu, Yang; McElroy, Michael B

2010-10-15

The Chinese government has moved aggressively since 2005 to reduce emissions of a number of pollutants including primary particulate matter (PM) and sulfur dioxide (SO(2)), efforts inadvertently aided since late 2008 by economic recession. Satellite observations of aerosol optical depth (AOD) and column nitrogen dioxide (NO(2)) provide independent indicators of emission trends, clearly reflecting the sharp onset of the recession in the fall of 2008 and rebound of the economy in the latter half of 2009. Comparison of AOD with ground-based observations of PM over a longer period indicate that emission-control policies have not been successful in reducing concentrations of aerosol pollutants at smaller size range over industrialized regions of China. The lack of success is attributed to the increasing importance of anthropogenic secondary aerosols formed from precursor species including nitrogen oxides (NO(x)), non-methane volatile organic compounds (NMVOC), and ammonia (NH(3)).

Webinar Presentation: Linking Regional Aerosol Emission Changes with Multiple Impact Measures through Direct and Cloud-Related Forcing Estimates

EPA Pesticide Factsheets

This presentation, Linking Regional Aerosol Emission Changes with Multiple Impact Measures through Direct and Cloud-Related Forcing Estimates, was given at the STAR Black Carbon 2016 Webinar Series: Accounting for Impact, Emissions, and Uncertainty.

Emission of intermediate, semi and low volatile organic compounds from traffic and their impact on secondary organic aerosol concentrations over Greater Paris

NASA Astrophysics Data System (ADS)

Sartelet, K.; Zhu, S.; Moukhtar, S.; André, M.; André, J. M.; Gros, V.; Favez, O.; Brasseur, A.; Redaelli, M.

2018-05-01

Exhaust particle emissions are mostly made of black carbon and/or organic compounds, with some of these organic compounds existing in both the gas and particle phases. Although emissions of volatile organic compounds (VOC) are usually measured at the exhaust, emissions in the gas phase of lower volatility compounds (POAvapor) are not. However, these gas-phase emissions may be oxidised after emission and enhance the formation of secondary organic aerosols (SOA). They are shown here to contribute to most of the SOA formation in Central Paris. POAvapor emissions are usually estimated from primary organic aerosol emissions in the particle phase (POA). However, they could also be estimated from VOC emissions for both gasoline and diesel vehicles using previously published measurements from chamber measurements. Estimating POAvapor from VOC emissions and ageing exhaust emissions with a simple model included in the Polyphemus air-quality platform compare well to measurements of SOA formation performed in chamber experiments. Over Greater Paris, POAvapor emissions estimated using POA and VOC emissions are compared using the HEAVEN bottom-up traffic emissions model. The impact on the simulated atmospheric concentrations is then assessed using the Polyphemus/Polair3D chemistry-transport model. Estimating POAvapor emissions from VOC emissions rather than POA emissions lead to lower emissions along motorway axes (between -50% and -70%) and larger emissions in urban areas (up to between +120% and +140% in Central Paris). The impact on total organic aerosol concentrations (gas plus particle) is lower than the impact on emissions: between -8% and 25% along motorway axes and in urban areas respectively. Particle-phase organic concentrations are lower when POAvapor emissions are estimated from VOC than POA emissions, even in Central Paris where the total organic aerosol concentration is higher, because of different assumptions on the emission volatility distribution, stressing the

Factors Affecting Aerosol Radiative Forcing

NASA Astrophysics Data System (ADS)

Wang, Jingxu; Lin, Jintai; Ni, Ruijing

2016-04-01

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

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

Impact of pollutant emission reductions on summertime aerosol feedbacks: A case study over the PO valley

NASA Astrophysics Data System (ADS)

Carnevale, C.; Finzi, G.; Pederzoli, A.; Turrini, E.; Volta, M.; Ferrari, F.; Gianfreda, R.; Maffeis, G.

2015-12-01

This study presents an evaluation of the impact by future pollutant anthropogenic emission reductions on summertime aerosol feedbacks over the Po valley. The fully coupled on line model Wrf/Chem has been used to examine the air quality and meteorology response over the region to 2020 emission reductions with respect to a simulation base case (2013). Future changes in net short wave radiation flux (SW) are also analyzed. The model domain is a 6 × 6 km2 resolution grid over Northern Italy; the simulation period covers two summer months (July-August). The work is divided into two parts. In the first, model results for the Base Case simulation (BC) are evaluated by comparing Wrf/Chem output to surface observations provided by two monitoring networks. Approximately 25 sites belonging to the regional ARPA Lombardia Network are used for both chemistry (NO2, O3 and PM10 concentrations) and meteorology (wind speed and 2-meters temperature) evaluation; 4 stations part of the global AEROsol Robotic Network (AERONET) are used for the evaluation of Aerosol Optical Depth (AOD). In the second part, a Maximum Feasible Reduction (MFR) scenario at 2020 have been simulated for the same months; monthly direct, indirect and overall aerosols feedbacks for both BC and MFR have been computed and analyzed. The emission reductions in the MFR 2020 lead to a sensible change in the aerosol overall feedbacks for all variables; a drop of SW over the valley (cooling effect) is visible in both BC and MFR, but it is less significant in the MFR (-5 W m-2) compared to the BC (-45 W m-2). This difference is mainly due to the abatement of SO2 primary emissions, which leads to lower sulfates concentrations scattering radiation, thus mitigates the cooling effect and favors the warming. As SW is higher in the MFR, T2 also increases over land with respect to the BC (the cooling of -0.5 °C estimated in the Base Case almost disappears). The overall effects lead to an enhancement of PM10 concentration in

Simulating ozone concentrations using precursor emission inventories in Delhi - National Capital Region of India

NASA Astrophysics Data System (ADS)

Sharma, Sumit; Khare, Mukesh

2017-02-01

This study simulates ground level ozone concentrations in a heavily populated and polluted National Capital Region (NCR- Delhi) in India. Multi-sectoral emission inventories of ozone precursors are prepared at a high resolution of 4 × 4 km2 for the whole region covering the capital city of Delhi along with other surrounding towns and rural regions in NCR. Emission inventories show that transport sector accounts for 55% of the total NOx emissions, followed by power plants (23%) and diesel generator sets (7%). In NMVOC inventories, transport sector again accounts for 33%, followed by evaporative emissions released from solvent use and fuel handling activities (30%), and agricultural residue burning (28%). Refuse burning contributes to 73% of CO emissions mainly due to incomplete combustion, followed by agricultural residue burning (14%). These emissions are spatially and temporally distributed across the study domain and are fed into the WRF-CMAQ models to predict ozone concentrations for the year 2012. Model validations are carried out with the observed values at different monitoring stations in Delhi. The performance of the models over various metrics used for evaluation was found to be satisfactory. Summers and post-monsoon seasons were better simulated than monsoon and winter seasons. Simulations have shown higher concentrations of ozone formation during summers and lesser during winters and monsoon seasons, mainly due to varying solar radiation affecting photo-chemical activities. Ozone concentrations are observed lower at those locations where NOx emissions are higher, and concentrations increase close to the boundary of study domain when compared to the center of Delhi city. Downwind regions to Delhi are influenced by the ozone formed due to plume of precursor emissions released from Delhi. Considering significant background contributions, regional scale controls are required for reducing ozone in NCR.

Aerosol chemical vapor deposition of metal oxide films

DOEpatents

Ott, Kevin C.; Kodas, Toivo T.

1994-01-01

A process of preparing a film of a multicomponent metal oxide including: forming an aerosol from a solution comprised of a suitable solvent and at least two precursor compounds capable of volatilizing at temperatures lower than the decomposition temperature of said precursor compounds; passing said aerosol in combination with a suitable oxygen-containing carrier gas into a heated zone, said heated zone having a temperature sufficient to evaporate the solvent and volatilize said precursor compounds; and passing said volatilized precursor compounds against the surface of a substrate, said substrate having a sufficient temperature to decompose said volatilized precursor compounds whereby metal atoms contained within said volatilized precursor compounds are deposited as a metal oxide film upon the substrate is disclosed. In addition, a coated article comprising a multicomponent metal oxide film conforming to the surface of a substrate selected from the group consisting of silicon, magnesium oxide, yttrium-stabilized zirconium oxide, sapphire, or lanthanum gallate, said multicomponent metal oxide film characterized as having a substantially uniform thickness upon said FIELD OF THE INVENTION The present invention relates to the field of film coating deposition techniques, and more particularly to the deposition of multicomponent metal oxide films by aerosol chemical vapor deposition. This invention is the result of a contract with the Department of Energy (Contract No. W-7405-ENG-36).

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.

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

Light absorption properties and radiative effects of primary organic aerosol emissions

DOE PAGES

Lu, Zifeng; Streets, David G.; Winijkul, Ekbordin; ...

2015-03-26

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 (k OA, the fundamental optical parameter determining the particle’s absorptivity) andmore » their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the k OA 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 k OA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated k OA values of sectoral and total POA emissions are presented. The 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.« less

Geochemistry of regional background aerosols in the Western Mediterranean

NASA Astrophysics Data System (ADS)

Pey, J.; Pérez, N.; Castillo, S.; Viana, M.; Moreno, T.; Pandolfi, M.; López-Sebastián, J. M.; Alastuey, A.; Querol, X.

2009-11-01

The chemical composition of regional background aerosols, and the time variability and sources in the Western Mediterranean are interpreted in this study. To this end 2002-2007 PM speciation data from an European Supersite for Atmospheric Aerosol Research (Montseny, MSY, located 40 km NNE of Barcelona in NE Spain) were evaluated, with these data being considered representative of regional background aerosols in the Western Mediterranean Basin. The mean PM 10, PM 2.5 and PM 1 levels at MSY during 2002-2007 were 16, 14 and 11 µg/m 3, respectively. After compiling data on regional background PM speciation from Europe to compare our data, it is evidenced that the Western Mediterranean aerosol is characterised by higher concentrations of crustal material but lower levels of OM + EC and ammonium nitrate than at central European sites. Relatively high PM 2.5 concentrations due to the transport of anthropogenic aerosols (mostly carbonaceous and sulphate) from populated coastal areas were recorded, especially during winter anticyclonic episodes and summer midday PM highs (the latter associated with the transport of the breeze and the expansion of the mixing layer). Source apportionment analyses indicated that the major contributors to PM 2.5 and PM 10 were secondary sulphate, secondary nitrate and crustal material, whereas the higher load of the anthropogenic component in PM 2.5 reflects the influence of regional (traffic and industrial) emissions. Levels of mineral, sulphate, sea spray and carbonaceous aerosols were higher in summer, whereas nitrate levels and Cl/Na were higher in winter. A considerably high OC/EC ratio (14 in summer, 10 in winter) was detected, which could be due to a combination of high biogenic emissions of secondary organic aerosol, SOA precursors, ozone levels and insolation, and intensive recirculation of aged air masses. Compared with more locally derived crustal geological dusts, African dust intrusions introduce relatively quartz-poor but clay

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;

Origin of particulate matter and gaseous precursors in the Paris Megacity: Results from intensive campaigns, long term measurements and modelling

NASA Astrophysics Data System (ADS)

Beekmann, Matthias; Petetin, Hervé; Zhang, Qijie; Prevot, André S. H.; Sciare, Jean; Gros, Valérie; Ghersi, Véronique; Rosso, Amandine; Crippa, Monica; Zotter, Peter; Freutel, Fredericke; Poulain, Laurent; Freney, Evelyne; Sellegri, Karine; Drewnick, Frank; Borbon, Agnès; Wiedensohler, Aflred; Pandis, Spyros N.; Baltensperger, Urs

2016-04-01

Uncertainties on the origin of primary and secondary particulate matter and its gaseous precursors in megacities is still large and needs to be reduced. A detailed characterization of air quality in Paris (France), a megacity of more than 10 million inhabitants, during two one month intensive campaigns (MEGAPOLI) and from additional one year observations (PARTICULATE and FRANCIPOL), revealed that about 70% of the fine particulate matter (PM) at urban background is transported on average into the megacity from upwind regions. While advection of sulfate is well documented for other megacities, there was a surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The data set of urban local and advected PM concentrations in the Paris area were used for a thorough evaluation of the CHIMERE model and revealed error compensation for the local and advected components of organic matter and nitrate. During spring time, CHIMERE simulations overestimate the sensitivity of ammonium nitrate peaks to NH3, because (i) they underestimate the urban background NH3 levels, probably due to neglecting enhanced NH3 emissions for larger temperatures, and because they overestimate HNO3. However, from an ensemble of mobile Max-DOAS NO2 column and airborne NOy measurements around Paris, no clear sign on a NOx emission bias in the TNO-Airparif data set was made evident. The origin of organic PM was investigated by a comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions contributed less than 20% in winter and 40% in summer to carbonaceous fine PM, unexpectedly little for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e. from biogenic precursors and from wood burning. Implementation

Assessment of biomass burning smoke influence on environmental conditions for multiyear tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints

NASA Astrophysics Data System (ADS)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-09-01

We use the Weather Research and Forecasting (WRF) system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the U.S. during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included, and smoke emissions are constrained using an inverse modeling technique and satellite-based aerosol optical depth observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low-level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics, and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations.

Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

NASA Astrophysics Data System (ADS)

Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

2015-12-01

Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi

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

Treesearch

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

2014-01-01

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

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...

Traffic congestion and ozone precursor emissions in Bilbao, Spain.

PubMed

Ibarra-Berastegi, Gabriel; Madariaga, Imanol

2003-01-01

In urban environments, the measured levels of ozone are the result of the interaction between emissions of precursors (mainly VOCs and NOx) and meteorological effects. In this work, time series of daily values of ozone, measured at three locations in Bilbao (Spain), have been built. Then, after removing meteorological effects from them, ozone and traffic data have been analyzed jointly. The goal was to identify traffic situations and link them to ozone levels in the area of Bilbao. To remove meteorological effects from the selected ozone time series, the technique developed by Rao and Zurbenko was used. This is a widely used technique and, after its application, the fraction obtained from a given ozone time series represents an ozone forming capability attributable to emissions of precursors. This fraction is devoid of any meteorological influence and includes only the apportion of periodicities above 1.7 years. In the case of Bilbao, the ozone fractions obtained at three locations have been compared on that time scale with traffic data from the area. For the 1993-1996 period, a regression analysis of the ozone and traffic fractions due to periodicities above 1.7 years (long-term fractions), shows that traffic is the main explanatory factor for ozone with R2 ranging from 0.916 to 0.996 at the three locations studied. Analysis of these longterm fractions has made it possible to identify two traffic regimes for the whole area, associated to different profiles of ozone forming capability. The first one favors low ozone forming capability, and is associated with a situation of fluent traffic. The second one shows high ozone forming capability and represents congestion. Joint analysis of raw data of ozone and traffic do not show any clear pattern due to the strong masking effects that seasonal-meteorological effects (mainly radiation) have on the measured ozone signal. If only immission data of ozone are available, as in this case, a comparison between ozone and traffic

Factors Affecting Aerosol Radiative Forcing

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Evaluation of Organic Aerosol Formation and Apportionment in a polluted Megacity

NASA Astrophysics Data System (ADS)

Tsimpidi, A. P.; Karydis, V. A.; Zavala, M.; Lei, W.; Decarlo, P. F.; Ulbrich, I.; Jimenez, J. L.; Molina, L. T.; Pandis, S. N.

2009-04-01

Pollution from megacities and large urban areas is important not only for local effects on health, visibility, and ecosystems but also because of their collective influence on atmospheric chemistry and radiative forcing in regional and global scale. Organic species account for a large fraction of the submicron aerosol mass at most megacities. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) have been difficult to quantify. In this study, new primary and secondary organic aerosol modules were added to PMCAMx, a three dimensional chemical transport model (Gaydos et al., 2007). The new modeling framework is based on the volatility basis-set approach (Lane et al., 2007): both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments (Robinson et al., 2007). PMCAMx is applied in the Mexico City Metropolitan Area during April 2003 and March 2006. The model predictions are compared with Aerodyne's Aerosol Mass Spectrometer (AMS) observations from the MCMA and MILAGRO campaigns respectively. Furthermore, the predicted concentrations over Mexico City are compared against measurements from a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) which was onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign (DeCarlo et al., 2008). The organic aerosol (OA) to CO ratio is used as an indicator in order to evaluate the photo-oxidation of the predicted OA after its horizontal and vertical advection. References Gaydos, T.M.; Pinder, R.W.; Koo, B.; Fahey, K.M.; Pandis, S.N., 2007. Development and application of a three-dimensional aerosol chemical transport model, PMCAMx. Atmospheric Environment 41, 2594-2611. Lane, T

Multiday production of condensing organic aerosol mass in urban and forest outflow

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

Lee-Taylor, J.; Hodzic, A.; Madronich, S.

2015-01-16

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

Multiday production of condensing organic aerosol mass in urban and forest outflow

DOE PAGES

Lee-Taylor, J.; Hodzic, A.; Madronich, S.; ...

2015-01-16

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. Here, the results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

Quantifying Wildfire Emissions and associated Aerosol Species using Assimilation of Satellite Carbon Monoxide Retrievals

NASA Astrophysics Data System (ADS)

Edwards, David; Barre, Jerome; Worden, Helen; Gaubert, Benjamin

2017-04-01

Intense and costly wildfires tend are predicted to increase in frequency under a warming climate. For example, the recent August 2015 Washington State fires were the largest in the state's history. Also in September and October 2015 very intense fires over Indonesia produced some of the highest concentrations of carbon monoxide (CO) ever seen from satellite. Such larges fires impact not only the local environment but also affect air quality far downwind through the long-range transport of pollutants. Global to continental scale coverage showing the evolution of CO resulting from fire emission is available from satellite observations. Carbon monoxide is the only atmospheric trace gas for which satellite multispectral retrievals have demonstrated reliable independent profile information close to the surface and also higher in the free troposphere. The unique CO profile product from Terra/MOPITT clearly distinguishes near-surface CO from the free troposphere CO. Also previous studies have suggested strong correlations between primary emissions of fire organic and black carbon aerosols and CO. We will present results from the Ensemble Adjustement Kalman Filter (DART) system that has been developed to assimilate MOPITT CO in the global-scale chemistry-climate model CAM-Chem. The ensemble technique allows inference on various fire model state variables such as CO emissions, and also aerosol species resulting from fires such as organic and black carbon. The benefit of MOPITT CO profile assimilation for estimating the CO emissions from the Washington and Indonesian fire cases will be discussed, along with the ability of the ensemble approach to infer information on the black and organic carbon aerosol distribution. This study builds on capability to quantitatively integrate satellite observations and models developed in recent years through projects funded by the NASA ACMAP Program.

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

PubMed Central

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.

2013-01-01

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 (NOx = 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 NOx. PMID:23553832

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).

Small global effect on terrestrial net primary production due to increased fossil fuel aerosol emissions from East Asia since the turn of the century

DOE PAGES

O'Sullivan, M.; Rap, A.; Reddington, C. L.; ...

2016-07-29

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 carbonmore » 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.« less

Small global effect on terrestrial net primary production due to increased fossil fuel aerosol emissions from East Asia since the turn of the century

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

O'Sullivan, M.; Rap, A.; Reddington, C. L.

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 carbonmore » 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.« less

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

O'Sullivan, M; Rap, A; Reddington, C L; Spracklen, D V; Gloor, M; Buermann, W

2016-08-16

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.

Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS)

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

Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang

Here, we present a new data set of annual historical (1750–2014) anthropogenic chemically reactive gases (CO, CH 4, NH 3, NO x, SO 2, NMVOCs), carbonaceous aerosols (black carbon – BC, and organic carbon – OC), and CO 2 developed with the Community Emissions Data System (CEDS). We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the samemore » activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.« less

Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS)

DOE PAGES

Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang; ...

2018-01-29

Here, we present a new data set of annual historical (1750–2014) anthropogenic chemically reactive gases (CO, CH 4, NH 3, NO x, SO 2, NMVOCs), carbonaceous aerosols (black carbon – BC, and organic carbon – OC), and CO 2 developed with the Community Emissions Data System (CEDS). We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the samemore » activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.« less

Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

DOE PAGES

Quan, Jiannong; Liu, Yangang; Liu, Quan; ...

2015-09-30

In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM 2.5), nitrate (NO 3), sulfate (SO 4), ammonium (NH 4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO 2), and ozone (O 3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (N ratio) andmore » S from SO 2 to sulfate (S ratio) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO 2 to their corresponding particle phases in the late haze period. Further analysis shows that N ratio and S ratio increased with increasing RH, with N ratio and S ratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of N ratio and S ratio to O 3: the conversion ratios increase with decreasing O 3 concentration when O 3 concentration is lower than <15 ppb but increased with increasing O 3 when O 3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO 2 and

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

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

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

2009-02-02

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

Urban emission, Santa Ana wind, and fire sources of aerosol nitrogen in Southern California

NASA Astrophysics Data System (ADS)

Mackey, K. R.; Stragier, S.; Robledo, L.; Cat, L. A.; Czimczik, C. I.

2017-12-01

Southern California is a highly urbanized region surrounded by extensive areas of agriculture and wilderness. While emissions from fossil fuel combustion are a large source of aerosol NOx in urban areas, fires contribute considerable aerosol NOx and ammonium in undeveloped regions. Southern California also has frequent wildfires, particularly during dry Santa Ana wind events that occur periodically throughout the winter. To explore the relative contributions of these sources to aerosol nitrogen content, we collected aerosol samples over two years in Irvine, a city in Southern California approximately 6 km from the Pacific coast. Samples were analyzed for total nitrogen and carbon content and isotopic composition (δ15N and δ13C), and nitrate and ammonium content. Carbon content was higher and δ13C values were lower in the winter than the summer. The C/N ratios of two samples collected during a Santa Ana wind event in January of 2012 were particularly elevated (C/N of 22 and 30) relative to other samples (C/N 3-6). We found that ammonium comprised 35% of total aerosol N across samples (R2=0.65), and that the δ15N of aerosol nitrogen decreased logarithmically as the proportion of nitrate in the sample increased (R2=0.60). Aerosol deposition of bioavailable nitrate and ammonium from these sources may support primary productivity in Southern California's coastal waters, particularly during the winter months and El Nino periods when upwelled nutrient sources are limited.

Aerosol chemical vapor deposition of metal oxide films

DOEpatents

Ott, K.C.; Kodas, T.T.

1994-01-11

A process of preparing a film of a multicomponent metal oxide including: forming an aerosol from a solution comprised of a suitable solvent and at least two precursor compounds capable of volatilizing at temperatures lower than the decomposition temperature of said precursor compounds; passing said aerosol in combination with a suitable oxygen-containing carrier gas into a heated zone, said heated zone having a temperature sufficient to evaporate the solvent and volatilize said precursor compounds; and passing said volatilized precursor compounds against the surface of a substrate, said substrate having a sufficient temperature to decompose said volatilized precursor compounds whereby metal atoms contained within said volatilized precursor compounds are deposited as a metal oxide film upon the substrate is disclosed. In addition, a coated article comprising a multicomponent metal oxide film conforming to the surface of a substrate selected from the group consisting of silicon, magnesium oxide, yttrium-stabilized zirconium oxide, sapphire, or lanthanum gallate, said multicomponent metal oxide film characterized as having a substantially uniform thickness upon said substrate.

Will Aerosol Hygroscopicity Change with Biodiesel, Renewable Diesel Fuels and Emission Control Technologies?

PubMed

Vu, Diep; Short, Daniel; Karavalakis, Georgios; Durbin, Thomas D; Asa-Awuku, Akua

2017-02-07

The use of biodiesel and renewable diesel fuels in compression ignition engines and aftertreatment technologies may affect vehicle exhaust emissions. In this study two 2012 light-duty vehicles equipped with direct injection diesel engines, diesel oxidation catalyst (DOC), diesel particulate filter (DPF), and selective catalytic reduction (SCR) were tested on a chassis dynamometer. One vehicle was tested over the Federal Test Procedure (FTP) cycle on seven biodiesel and renewable diesel fuel blends. Both vehicles were exercised over double Environmental Protection Agency (EPA) Highway fuel economy test (HWFET) cycles on ultralow sulfur diesel (ULSD) and a soy-based biodiesel blend to investigate the aerosol hygroscopicity during the regeneration of the DPF. Overall, the apparent hygroscopicity of emissions during nonregeneration events is consistently low (κ < 0.1) for all fuels over the FTP cycle. Aerosol emitted during filter regeneration is significantly more CCN active and hygroscopic; average κ values range from 0.242 to 0.439 and are as high as 0.843. Regardless of fuel, the current classification of "fresh" tailpipe emissions as nonhygroscopic remains true during nonregeneration operation. However, aftertreatment technologies such as DPF, will produce significantly more hygroscopic particles during regeneration. To our knowledge, this is the first study to show a significant enhancement of hygroscopic materials emitted during DPF regeneration of on-road diesel vehicles. As such, the contribution of regeneration emissions from a growing fleet of diesel vehicles will be important.

Influence of local production and vertical transport on the organic aerosol budget over Paris

NASA Astrophysics Data System (ADS)

Janssen, R. H. H.; Tsimpidi, A. P.; Karydis, V. A.; Pozzer, A.; Lelieveld, J.; Crippa, M.; Prévôt, A. S. H.; Ait-Helal, W.; Borbon, A.; Sauvage, S.; Locoge, N.

2017-08-01

We performed a case study of the organic aerosol (OA) budget during the MEGAPOLI campaign during summer 2009 in Paris. We combined aerosol mass spectrometer, gas phase chemistry, and atmospheric boundary layer (ABL) data and applied the MXL/MESSy column model. We find that during daytime, vertical mixing due to ABL growth has opposing effects on secondary organic aerosol (SOA) and primary organic aerosol (POA) concentrations. POA concentrations are mainly governed by dilution due to boundary layer expansion and transport of POA-depleted air from aloft, while SOA concentrations are enhanced by entrainment of SOA-rich air from the residual layer (RL). Further, local emissions and photochemical production control the diurnal cycle of SOA. SOA from intermediate volatility organic compounds constitutes about half of the locally formed SOA mass. Other processes that previously have been shown to influence the urban OA budget, such as aging of semivolatile and intermediate volatility organic compounds (S/IVOC), dry deposition of S/IVOCs, and IVOC emissions, are found to have minor influences on OA. Our model results show that the modern carbon content of the OA is driven by vertical and long-range transport, with a minor contribution from local cooking emissions. SOA from regional sources and resulting from aging and long-lived precursors can lead to high SOA concentrations above the ABL, which can strongly influence ground-based observations through downward transport. Sensitivity analysis shows that modeled SOA concentrations in the ABL are equally sensitive to ABL dynamics as to SOA concentrations transported from the RL.

Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China during 2014 APEC summit

NASA Astrophysics Data System (ADS)

Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

2015-08-01

The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the 325 m Beijing Meteorological Tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition at near ground level using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3-/SO42- mass ratios illustrate an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed by secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors such as SO2, NOx, and volatile organic compounds (VOCs). In addition to emission controls, the routine

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.

Micrometeorological flux measurements of aerosol and gases above Beijing

NASA Astrophysics Data System (ADS)

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

2017-04-01

less sensitive to transport effects. However, not only fluxes, but also these CO2-ratioed fluxes are highly variable in both space and time, indicating a complex mix of sources, which will be further investigated. The organic aerosol fluxes were the largest we have recorded to date at any urban measurement site. Nitrate, sulphate, chloride and ammonium all showed emissions that followed a similar diurnal cycle as the organic aerosol. Much of this aerosol is likely to have been formed by chemistry below the measurement height, but it nevertheless indicates significant sources of the precursor gases within the footprint. Comparing the measured fluxes of gas-phase NH3 and aerosol NH4+, at 102 m the aerosol phase makes a significant contribution to the reduced nitrogen emission.

Historical (1850-2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols:methodology and application

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

Lamarque, J. F.; Bond, Tami C.; Eyring, Veronika

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 atmore » 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.« less

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

2016-08-02

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.

Aerosol composition and the contribution of SOA formation over Mediterranean forests

NASA Astrophysics Data System (ADS)

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

2018-05-01

, ISOPOOH). Despite a significantly high mixing ratio of isoprene (0.4 to 1.2 ppbV) and its oxidation products (0.2 and 0.8 ppbV), the contribution of specific signatures for isoprene epoxydiols SOA (IEPOX-SOA) within the aerosol organic mass spectrum (m/z 53 and m/z 82) were very weak, suggesting that the presence of isoprene-derived SOA was either too low to be detected by the cToF-AMS, or that SOA was not formed through IEPOX. This was corroborated through simulations performed with the Polyphemus model showing that although 60 to 80 % of SOA originated from biogenic precursors, only about 15 to 32 % was related to isoprene (non-IEPOX) SOA; the remainder was 10 % sesquiterpene SOA and 35 to 40 % monoterpene SOA. The model results show that despite the zone of sampling being far from industrial or urban sources, a total contribution of 20 to 34 % of the SOA was attributed to purely anthropogenic precursors (aromatics and intermediate or semi-volatile compounds). The measurements obtained during this study allow us to evaluate how biogenic emissions contribute to increasing SOA concentrations over Mediterranean forested areas. Directly comparing these measurements with the Polyphemus model provides insight into the SOA formation pathways that are prevailing in these forested areas as well as processes that need to be implemented in future simulations.

Transformation of logwood combustion emissions in a smog chamber: formation of secondary organic aerosol and changes in the primary organic aerosol upon daytime and nighttime aging

NASA Astrophysics Data System (ADS)

Tiitta, Petri; Leskinen, Ari; Hao, Liqing; Yli-Pirilä, Pasi; Kortelainen, Miika; Grigonyte, Julija; Tissari, Jarkko; Lamberg, Heikki; Hartikainen, Anni; Kuuspalo, Kari; Kortelainen, Aki-Matti; Virtanen, Annele; Lehtinen, Kari E. J.; Komppula, Mika; Pieber, Simone; Prévôt, André S. H.; Onasch, Timothy B.; Worsnop, Douglas R.; Czech, Hendryk; Zimmermann, Ralf; Jokiniemi, Jorma; Sippula, Olli

2016-10-01

Organic aerosols (OA) derived from small-scale wood combustion emissions are not well represented by current emissions inventories and models, although they contribute substantially to the atmospheric particulate matter (PM) levels. In this work, a 29 m3 smog chamber in the ILMARI facility of the University of Eastern Finland was utilized to investigate the formation of secondary organic aerosol (SOA) from a small-scale modern masonry heater commonly used in northern Europe. Emissions were oxidatively aged in the smog chamber for a variety of dark (i.e., O3 and NO3) and UV (i.e., OH) conditions, with OH concentration levels of (0.5-5) × 106 molecules cm-3, achieving equivalent atmospheric aging of up to 18 h. An aerosol mass spectrometer characterized the direct OA emissions and the SOA formed from the combustion of three wood species (birch, beech and spruce) using two ignition processes (fast ignition with a VOC-to-NOx ratio of 3 and slow ignition with a ratio of 5).Dark and UV aging increased the SOA mass fraction with average SOA productions 2.0 times the initial OA mass loadings. SOA enhancement was found to be higher for the slow ignition compared with fast ignition conditions. Positive matrix factorization (PMF) was used to separate SOA, primary organic aerosol (POA) and their subgroups from the total OA mass spectra. PMF analysis identified two POA and three SOA factors that correlated with the three major oxidizers: ozone, the nitrate radical and the OH radical. Organonitrates (ONs) were observed to be emitted directly from the wood combustion and additionally formed during oxidation via NO3 radicals (dark aging), suggesting small-scale wood combustion may be a significant ON source. POA was oxidized after the ozone addition, forming aged POA, and after 7 h of aging more than 75 % of the original POA was transformed. This process may involve evaporation and homogeneous gas-phase oxidation as well as heterogeneous oxidation of particulate organic matter

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.

Marine Aerosols and Clouds.

PubMed

Brooks, Sarah D; Thornton, Daniel C O

2018-01-03

The role of marine bioaerosols in cloud formation and climate is currently so uncertain that even the sign of the climate forcing is unclear. Marine aerosols form through direct emissions and through the conversion of gas-phase emissions to aerosols in the atmosphere. The composition and size of aerosols determine how effective they are in catalyzing the formation of water droplets and ice crystals in clouds by acting as cloud condensation nuclei and ice nucleating particles, respectively. Marine organic aerosols may be sourced both from recent regional phytoplankton blooms that add labile organic matter to the surface ocean and from long-term global processes, such as the upwelling of old refractory dissolved organic matter from the deep ocean. Understanding the formation of marine aerosols and their propensity to catalyze cloud formation processes are challenges that must be addressed given the major uncertainties associated with aerosols in climate models.

Historical emissions of carbonaceous aerosols from biomass and fossil fuel burning for the period 1870-2000

NASA Astrophysics Data System (ADS)

Ito, Akinori; Penner, Joyce E.

2005-06-01

Historical changes of black carbon (BC) and particulate organic matter (POM) emissions from biomass burning (BB) and fossil fuel (FF) burning are estimated from 1870 to 2000. A bottom-up inventory for open vegetation (OV) burning is scaled by a top-down estimate for the year 2000. Monthly and interannual variations are derived over the time period from 1979 to 2000 based on the TOMS satellite aerosol index (AI) and this global map. Prior to 1979, emissions are scaled to a CH4 emissions inventory based on land-use change. Biofuel (BF) emissions from a recent inventory for developing countries are scaled forward and backward in time using population statistics and crop production statistics. In developed countries, wood consumption data together with emission factors for cooking and heating practices are used for biofuel estimates. For fossil fuel use, we use fuel consumption data and specific emission factors for different fuel use categories to develop an inventory over 1950-2000, and emissions are scaled to a CO2 inventory prior to that time. Technology changes for emissions from the diesel transport sector are included. During the last decade of this time period, the BC and POM emissions from biomass burning (i.e., OV + BF) contribute a significant amount to the primary sources of BC and POM and are larger than those from FF. Thus 59% of the NH BC emissions and 90% of the NH POM emissions are from BB in 2000. Fossil fuel consumption technologies are needed prior to 1990 in order to improve estimates of fossil fuel emissions during the twentieth century. These results suggest that the aerosol emissions from biomass burning need to be represented realistically in climate change assessments. The estimated emissions are available on a 1° × 1° grid for global climate modeling studies of climate changes.

Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China, during the 2014 APEC summit

NASA Astrophysics Data System (ADS)

Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

2015-11-01

The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3- / SO42- mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play

Infrared Emission from Gas-Aerosol Reactions

DTIC Science & Technology

1982-09-01

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

Modelling carbonaceous aerosol from residential solid fuel burning with different assumptions for emissions

NASA Astrophysics Data System (ADS)

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

2018-04-01

Evidence is accumulating that emissions of primary particulate matter (PM) from residential wood and coal combustion in the UK may be underestimated and/or spatially misclassified. In this study, different assumptions for the spatial distribution and total emission of PM from solid fuel (wood and coal) burning in the UK were tested using an atmospheric chemical transport model. Modelled concentrations of the PM components were compared with measurements from aerosol mass spectrometers at four sites in central and Greater London (ClearfLo campaign, 2012), as well as with measurements from the UK black carbon network.The two main alternative emission scenarios modelled were Base4x and combRedist. For Base4x, officially reported PM2.5 from the residential and other non-industrial combustion source sector were increased by a factor of four. For the combRedist experiment, half of the baseline emissions from this same source were redistributed by residential population density to simulate the effect of allocating some emissions to the smoke control areas (that are assumed in the national inventory to have no emissions from this source). The Base4x scenario yielded better daily and hourly correlations with measurements than the combRedist scenario for year-long comparisons of the solid fuel organic aerosol (SFOA) component at the two London sites. However, the latter scenario better captured mean measured concentrations across all four sites. A third experiment, Redist - all emissions redistributed linearly to population density, is also presented as an indicator of the maximum concentrations an assumption like this could yield.The modelled elemental carbon (EC) concentrations derived from the combRedist experiments also compared well with seasonal average concentrations of black carbon observed across the network of UK sites. Together, the two model scenario simulations of SFOA and EC suggest both that residential solid fuel emissions may be higher than inventory

Impact of future climate policy scenarios on air quality and aerosol-cloud interactions using an advanced version of CESM/CAM5: Part II. Future trend analysis and impacts of projected anthropogenic emissions

NASA Astrophysics Data System (ADS)

Glotfelty, Timothy; Zhang, Yang

2017-03-01

Following a comprehensive evaluation of the Community Earth System Model modified at the North Carolina State University (CESM-NCSU), Part II describes the projected changes in the future state of the atmosphere under the representative concentration partway scenarios (RCP4.5 and 8.5) by 2100 for the 2050 time frame and examine the impact of climate change on future air quality under both scenarios, and the impact of projected emission changes under the RCP4.5 scenario on future climate through aerosol direct and indirect effects. Both the RCP4.5 and RCP8.5 simulations predict similar changes in air quality by the 2050 period due to declining emissions under both scenarios. The largest differences occur in O3, which decreases by global mean of 1.4 ppb under RCP4.5 but increases by global mean of 2.3 ppb under RCP8.5 due to differences in methane levels, and PM10, which decreases by global mean of 1.2 μg m-3 under RCP4.5 and increases by global mean of 0.2 μg m-3 under RCP8.5 due to differences in dust and sea-salt emissions under both scenarios. Enhancements in cloud formation in the Arctic and Southern Ocean and increases of aerosol optical depth (AOD) in central Africa and South Asia dominate the change in surface radiation in both scenarios, leading to global average dimming of 1.1 W m-2 and 2.0 W m-2 in the RCP4.5 and RCP8.5 scenarios, respectively. Declines in AOD, cloud formation, and cloud optical thickness from reductions of emissions of primary aerosols and aerosol precursors under RCP4.5 result in near surface warming of 0.2 °C from a global average increase of 0.7 W m-2 in surface downwelling solar radiation. This warming leads to a weakening of the Walker Circulation in the tropics, leading to significant changes in cloud and precipitation that mirror a shift in climate towards the negative phase of the El Nino Southern Oscillation.

Aerosol direct, indirect, semidirect, and surface albedo effects from sector contributions based on the IPCC AR5 emissions for preindustrial and present-day conditions

NASA Astrophysics Data System (ADS)

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/m2, with the largest contribution from the direct effect (-0.5 W/m2). 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/m2) and semidirect effects (-0.10 W/m2) 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/m2), triggered feedbacks on top of the atmosphere (TOA) radiative forcing can be 10 times larger. Our results point out that each emission sector has varying

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

Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability.

PubMed

Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

2016-05-24

A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.

Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability

PubMed Central

Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G.; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

2016-01-01

A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing. PMID:26921324

Assessment of biomass burning smoke influence on environmental conditions for multi-year tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints.

PubMed

Saide, Pablo E; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M; Pierce, R Bradley; Carmichael, Gregory R

2016-09-16

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations.

Assessment of Biomass Burning Smoke Influence on Environmental Conditions for Multi-Year Tornado Outbreaks by Combining Aerosol-Aware Microphysics and Fire Emission Constraints

NASA Technical Reports Server (NTRS)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; Da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRFChem for its use in applications such as NWP and cloud-resolving simulations.

Assessment of biomass burning smoke influence on environmental conditions for multi-year tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints

PubMed Central

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2018-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations. PMID:29619287

Contributions to Pliocene Arctic warmth from removal of anthropogenic aerosol and enhanced forest fire emissions

NASA Astrophysics Data System (ADS)

Feng, R.; Otto-Bliesner, B. L.; Fletcher, T.; Ballantyne, A.; Brady, E. C.

2016-12-01

Changing atmosphere chemistry in the past has been hypothesized to have altered the earth's radiation budget, and hence the climate. Here, we use an advanced climate model to test whether this hypothesis can help explain the amplified warming in the northern high latitudes during the mid-Pliocene warm period (mPWP, 3.0 - 3.3 Ma). The amplified warming, suggested by terrestrial proxy records of northern high latitudes, is underestimated in previous climate simulations. This mismatch between observations and models may be partially due to proxy uncertainties, but also to insufficient model sensitivity, or incomplete knowledge of mPWP climate forcings. To explore the latter aspect, we conducted three coupled simulations using the same mPWP geography and topography, vegetation and CO2 level according to the PRISM3 reconstructions, but alternating emission scenarios among clean, polluted, and clean plus forest fire case. In the clean and polluted case, year-1850 emission and year-1850 natural plus year-2000 industrial emission are prescribed respectively. For the clean-plus-forest fire simulation, emissions from mPWP forest fire are constrained with a process-based prognostic fire model using fixed proxy SSTs. Preliminary results suggest that mPWP Arctic warmth is largely attributable to the removal of anthropogenic aerosols and enhanced deposition of the black carbon on snow and ice emitted from northern high latitude forest fires. Cloud radiative responses are shown to accelerate the summer sea ice melting from the continental margins, triggering the positive surface albedo and water vapor feedback that maintain a low perennial sea ice state in the Arctic Ocean. These results identify the important role that changes in aerosol chemistry may play in amplifying arctic surface temperatures of mPWP and insights on the role that aerosols may play in amplifying future Arctic temperatures.

Aerosol reduction/expansion synthesis (A-RES) for zero valent metal particles

DOEpatents

Leseman, Zayd; Luhrs, Claudia; Phillips, Jonathan; Soliman, Haytham

2016-04-12

Various embodiments provide methods of forming zero valent metal particles using an aerosol-reductive/expansion synthesis (A-RES) process. In one embodiment, an aerosol stream including metal precursor compound(s) and chemical agent(s) that produces reducing gases upon thermal decomposition can be introduced into a heated inert atmosphere of a RES reactor to form zero valent metal particles corresponding to metals used for the metal precursor compound(s).

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

NASA Technical Reports Server (NTRS)

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

2012-01-01

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

Inter-comparison of Speciated Aerosol Loading over India for Global and Regional Emission Inventory using a Chemical Transport Model

NASA Astrophysics Data System (ADS)

Upadhyay, Abhishek; Dey, Sagnik; Goyal, Pramila

2017-04-01

Air quality of a region directly affects health of entire biotic and abiotic components of ecosystem. Exposure to particulate matter smaller than 2.5 µm (PM2.5) in atmosphere has been directly related to mortality and mobility in various studies. India is one of the aerosol hotspots globally with 0.8 million premature death attributed to exposure to ambient PM2.5. Robust long-term in-situ data of speciated PM2.5 is lacking in India. The problem cannot be resolved by utilizing satellite data as inferring composition is difficult. Therefore a modelling approach is required. We examine spatial and temporal distribution of PM2.5 and its constituent species with a regional and global inventory through chemical transport model (WRF-Chem) over India. The simulation is conducted with RADM2 chemistry and GOCART aerosol module for 8 years (2007-2014). Emissions are interpolated for domain from global anthropogenic emission inventory RETRO and EDGAR for species other than BC, OC and Sulfate. Results from GOCART global inventory are compared with results from a regional inventory for species OC, BC and Sulfate. Validation of CTM simulations against observations (ground based monitoring stations and satellite observations) demonstrates the capability of the CTM to represent space-time variation of aerosols in this region. For example, the build-up of aerosols over the eastern part of the Indo-Gangetic Basin (IGB) during winter (as observed by space-borne sensors) due to the meteorological influence is well captured by the CTM. A correlation of 0.51 and 0.52 has been observed between monitored and model simulated PM2.5 at the two big cities of India, New Delhi and Mumbai respectively. Distribution of PM2.5 is high in the Indo-Gangetic Basin (IGB) and distribution of OC and BC is also more in IGB region with both emission inventories. In the IGB region OC and BC contribute 8 - 20 % and 2.5 - 5 % to total PM2.5. Global and regional emission inventories are showing similar

Modeling and Evaluation of the Global Sea-Salt Aerosol Distribution: Sensitivity to Emission Schemes and Resolution Effects at Coastal/Orographic Sites

NASA Technical Reports Server (NTRS)

Spada, M.; Jorba, O.; Perez Garcia-Pando, C.; Janjic, Z.; Baldasano, J. M.

2013-01-01

One of the major sources of uncertainty in model estimates of the global sea-salt aerosol distribution is the emission parameterization. We evaluate a new sea-salt aerosol life cycle module coupled to the online multi-scale chemical transport model NMMB/BSC-CTM. We compare 5 year global simulations using five state-of-the-art sea-salt open-ocean emission schemes with monthly averaged coarse aerosol optical depth (AOD) from selected AERONET sun photometers, surface concentration measurements from the University of Miami's Ocean Aerosol Network, and measurements from two NOAA/PMEL cruises (AEROINDOEX and ACE1). Model results are highly sensitive to the introduction of sea-surface-temperature (SST)-dependent emissions and to the accounting of spume particles production. Emission ranges from 3888 teragrams per year to 8114 teragrams per year, lifetime varies between 7.3 hours and 11.3 hours, and the average column mass load is between 5.0 teragrams and 7.2 teragrams. Coarse AOD is reproduced with an overall correlation of around 0.5 and with normalized biases ranging from +8.8 percent to +38.8 percent. Surface concentration is simulated with normalized biases ranging from minus 9.5 percent to plus 28 percent and the overall correlation is around 0.5. Our results indicate that SST-dependent emission schemes improve the overall model performance in reproducing surface concentrations. On the other hand, they lead to an overestimation of the coarse AOD at tropical latitudes, although it may be affected by uncertainties in the comparison due to the use of all-sky model AOD, the treatment of water uptake, deposition and optical properties in the model and/or an inaccurate size distribution at emission.

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.

Monitoring biological aerosols using UV fluorescence

NASA Astrophysics Data System (ADS)

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

1999-01-01

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

Carbonaceous Aerosol Removal During Precipitation Events: Climate Implications

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Bridges, G. L.; Marchany-Rivera, A.; Begum, M.

2009-12-01

Atmospheric aerosols and their links to clouds are one of the main focus areas of the Department of Energy’s Atmospheric Systems Research, due to the fact that aerosols and clouds constitute the major uncertainties in radiative forcing that need to be reduced for more accurate modeling of climate, particularly regional climate. The impact of absorbing aerosols on radiative balance of the atmosphere will depend on their atmospheric lifetimes as well as their UV-visible absorption profiles. Aerosol lifetimes depend on the aerosols ability to take up water and grow to sufficient size to be either removed by gravitational settling or to act as cloud condensation nuclei and be removed by precipitation scavenging. The investigation of uv-visible absorbing aerosols is underway using a seven-channel aethalometer to evaluate the change in aerosol optical absorption during precipitation events. Angstrom absorption exponents (AAEs) are determined before, during, and after rain events to examine the impact on the aerosol absorption profiles anticipated by removal of the water soluble short-wave absorbing species (i.e. HULIS) that can be produced by photochemical oxidation of biogenic emissions (isoprene, monoterpenes, sesquiterpenes). Aerosol absorption data are presented from observations made at the University of Arkansas at Little Rock and other sites, which clearly show that a significant amount of absorbing carbon is not removed during rain events, and that the organic matter removed is likely secondary organics produced from biogenic precursors. The dissolved organic carbon measured in precipitation samples along with determinations of natural radionuclide tracers are also used to help examine the extent of carbonaceous aerosol removal by precipitation. The data are discussed in terms of the potential impacts of anthropogenic enhancement of aerosol absorption by secondary organic aerosols adding to atmospheric heating and changes in atmospheric dynamics. The potential

Aromatic Structure in Simulates Titan Aerosol

NASA Technical Reports Server (NTRS)

Trainer, Melissa G.; Loeffler, M. J.; Anderson, C. M.; Hudson, R. L.; Samuelson, R. E.; Moore, M. A.

2011-01-01

Observations of Titan by the Cassini Composite Infrared Spectrometer (CIRS) between 560 and 20 per centimeter (approximately 18 to 500 micrometers) have been used to infer the vertical variations of Titan's ice abundances, as well as those of the aerosol from the surface to an altitude of 300 km [1]. The aerosol has a broad emission feature centered approximately at 140 per centimeter (71 micrometers). As seen in Figure 1, this feature cannot be reproduced using currently available optical constants from laboratory-generated Titan aerosol analogs [2]. The far-IR is uniquely qualified for investigating low-energy vibrational motions within the lattice structures of COITIDlex aerosol. The feature observed by CIRS is broad, and does not likely arise from individual molecules, but rather is representative of the skeletal movements of macromolecules. Since Cassini's arrival at Titan, benzene (C6H6) has been detected in the atmosphere at ppm levels as well as ions that may be polycyclic aromatic hydrocarbons (PAHs) [3]. We speculate that the feature may be a blended composite that can be identified with low-energy vibrations of two-dimensional lattice structures of large molecules, such as PAHs or nitrogenated aromatics. Such structures do not dominate the composition of analog materials generated from CH4 and N2 irradiation. We are performing studies forming aerosol analog via UV irradiation of aromatic precursors - specifically C6H6 - to understand how the unique chemical architecture of the products will influence the observable aerosol characteristics. The optical and chemical properties of the aromatic analog will be compared to those formed from CH4/N2 mixtures, with a focus on the as-yet unidentified far-IR absorbance feature. Preliminary results indicate that the photochemically-formed aromatic aerosol has distinct chemical composition, and may incorporate nitrogen either into the ring structure or adjoined chemical groups. These compositional differences are

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.;

Seasonality of Forcing by Carbonaceous Aerosols

NASA Astrophysics Data System (ADS)

Habib, G.; Bond, T.; Rasch, P. J.; Coleman, D.

2006-12-01

Aerosols can influence the energy balance of Earth-Atmosphere system with profound effect on regional climate. Atmospheric processes, such as convection, scavenging, wet and dry deposition, govern the lifetime and location of aerosol; emissions affect its quantity and location. Both affect climate forcing. Here we investigate the effect of seasonality in emissions and atmospheric processes on radiative forcing by carbonaceous aerosols, focusing on aerosol from fossil fuel and biofuel. Because aerosol lifetime is seasonal, ignoring the seasonality of sources such as residential biofuel may introduce a bias in aerosol burden and therefore in predicted climate forcing. We present a global emission inventory of carbonaceous aerosols with seasonality, and simulate atmospheric concentrations using the Community Atmosphere Model (CAM). We discuss where and when the seasonality of emissions and atmospheric processes has strong effects on atmospheric burden, lifetime, climate forcing and aerosol optical depth (AOD). Previous work has shown that aerosol forcing is higher in summer than in winter, and has identified the importance of aerosol above cloud in determining black carbon forcing. We show that predicted cloud height is a very important factor in determining normalized radiative forcing (forcing per mass), especially in summer. This can affect the average summer radiative forcing by nearly 50%. Removal by cloud droplets is the dominant atmospheric cleansing mechanism for carbonaceous aerosols. We demonstrate the modeled seasonality of removal processes and compare the importance of scavenging by warm and cold clouds. Both types of clouds contribute significantly to aerosol removal. We estimate uncertainty in direct radiative forcing due to scavenging by tagging the aerosol which has experienced cloud interactions. Finally, seasonal variations offer an opportunity to assess modeled processes when a single process dominates variability. We identify regions where aerosol

Long term atmospheric aerosol characterization in the Amazon Basin

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Gerab, Fábio; Yamasoe, Marcia A.

This chapter presents a characterization of atmospheric aerosols collected in different places in the Amazon Basin. Both the biogenic aerosol emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burns during the dry season were studied. The samples were collected during a three year period at three different locations in the Amazon (Cuiabá, Alta Floresta and Serra do Navio), using stacked filter units. Aerosol samples were also collected directly over fires of cerrado vegetation and tropical primary forest burns The samples were analyzed using several techniques for a number of elements. Gravimetric analyses were used to determine the total atmospheric aerosol concentration. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. Cerrado burning emissions were enriched compared to forest ones, specially for Cl, K and Zn. High atmospheric aerosol concentrations were observed in large amazonian areas due to emissions from man-made burns in the period from June to September. The emissions from burns dominate the fine fraction of the atmospheric aerosol with characteristic high contents of black carbon, S and K. Aerosols emitted in biomass burning process are correlated to the increase in the aerosol optical thickness of the atmosphere during the Amazonian dry season. The Serra do Navio aerosol is characterized by biogenic emissions with strong marine influence. The presence of trace elements characteristic of soil particulate associated with this marine contribution indicates the existence of aerosol transport from Africa to South America. Similar composition characteristics were observed in the biogenic emission aerosols from Serra do Navio and Alta Floresta.

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

New aerosol particles formation in the Sao Paulo Metropolitan Area

NASA Astrophysics Data System (ADS)

Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

2016-04-01

The Sao Paulo Metropolitan Area (SPMA), in the southeast region of Brazil, is considered a megalopolis comprised of Sao Paulo city and more 38 municipalities. The air pollutant emissions in the SPMA are related to the burning of the fuels: etanol, gasohol (gasoline with 25% ethanol) and diesel. According to CETESB (2013), the road vehicles contributed up to about 97, 87, and 80% of CO, VOCs and NOx emissions in 2012, respectively, being most of NOx associated to diesel combustion and most of CO and VOCs from gasohol and ethanol combustion. Studies conducted on ambient air pollution in the SPMA have shown that black carbon (BC) explains 21% of mass concentration of PM2.5 compared with 40% of organic carbon (OC), 20% of sulfates, and 12% of soil dust (Andrade et al., 2012). Most of the observed ambient PM2.5 mass concentration usually originates from precursors gases such as sulphur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOx) and VOCs as well as through the physico-chemical processes such as the oxidation of low volatile hydrocarbons transferring to the condensed phase (McMurry et al., 2004). The Weather Research and Forecasting with Chemistry model (WRF-Chem; Grell et al. 2005), configured with three nested grid cells: 75, 15, and 3 km, is used as photochemical modeling to describe the physico-chemical processes leading to evolution of particles number and mass size distribution from a vehicular emission model developed by the IAG-USP laboratory of Atmospheric Processes and based on statistical information of vehicular activity. The spatial and temporal distributions of emissions in the finest grid cell are based on road density products compiled by the OpenStreetMap project and measurements performed inside tunnels in the SPMA, respectively. WRF-Chem simulation with coupled primary aerosol (dust and sea-salt) and biogenic emission modules and aerosol radiative effects turned on is conducted as the baseline simulation (Case_0) to evaluate the model

Physico-chemical properties of aerosols in Sao Paulo, Brazil and mechanisms of secondary organic aerosol formation.

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Ferreira de Brito, Joel; Varanda Rizzo, Luciana; Luiza Godoy, Maria; Godoy, Jose Marcus

2013-04-01

Megacities emissions are increasingly becoming a global issue, where emissions from the transportation sector play an increasingly important role. Sao Paulo is a megacity with a population of about 18 million people, 7 million cars and large-scale industrial emissions. As a result of the vehicular and industrial emissions, the air quality in Sao Paulo is bellow WMO standards for aerosol particles and ozone. Many uncertainties are found on gas- and particulate matter vehicular emission factors and their following atmospheric processes, e.g. secondary organic aerosol formation. Due to the uniqueness of the vehicular fuel in Brazil, largely based on ethanol use, such characterization currently holds further uncertainties. To improve the understanding of the role of this unique emission characteristics, we are running a source apportionment study in Sao Paulo focused on the mechanisms of organic aerosol formation. One of the goals of this study is a quantitative aerosol source apportionment focused on vehicular emissions, including ethanol and gasohol (both fuels used by light-duty vehicles). This study comprises four sampling sites with continuous measurements for one year, where trace elements and organic aerosol are being measured for PM2.5 and PM10 along with real-time NOx, O3, PM10 and CO measurements. Aerosol optical properties and size distribution are being measured on a rotation basis between sampling stations. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to measure in real time VOCs and aerosol composition, respectively. Trace elements were measured using XRF and OC/EC analysis was determined with a Sunset OC/EC instrument. A TSI Nephelometer with 3 wavelengths measure light scattering and a MAAP measure black carbon. Results show aerosol number concentrations ranging between 10,000 and 35,000 cm-3, mostly concentrated in the nucleation and Aitken modes, with a peak in size at 80

Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols. Part 1; Aerosol Trends and Radiative Forcing

NASA Technical Reports Server (NTRS)

Leibensperger, E. M.; Mickley, L. J.; Jacob, D. J.; Chen, W.-T.; Seinfeld, J. H.; Nenes, A.; Adams, P. J.; Streets, D. G.; Kumar, N.; Rind, D.

2012-01-01

We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of -2.0Wm(exp-2 for direct forcing including contributions from sulfate (-2.0Wm-2), nitrate (-0.2Wm(exp-2), organic carbon (-0.2Wm(exp-2), and black carbon (+0.4Wm(exp-2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp-2) direct and 1.0Wm(exp-2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp-2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

The impact of anthropogenic emissions on the otherwise pristine Amazonian rainforest: Insights on aerosol dynamics as observed during GoAmazon2014/5

NASA Astrophysics Data System (ADS)

Carbone, S.; Ferreira De Brito, J.; Cirino, G. G.; Rizzo, L. V.; Holanda, B. A.; Barbosa, H. M.; Ditas, F.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Moran, D.; Saturno, J.; Andreae, M. O.; de Sá, S. S.; Liu, Y.; Martin, S. T.; Souza, R. A. F. D.; Wang, J.; Palm, B. B.; Jimenez, J. L.; Artaxo, P.

2015-12-01

The Amazon Basin during the wet season has one of the lowest aerosol concentrations worldwide, with air masses with negligible human impact covering thousands of kilometers of pristine forest. The natural environment is strongly modified near urbanized areas, in particular Manaus, a city of nearly two million people. This unique location provides the ideal laboratory to study isolated urban emissions as well the pristine environment by perturbing it in a relatively known fashion. The GoAmazon2014/5 experiment was designed with these questions in mind, combining remote sensing, in situ, and airborne measurements. This manuscript describes the measurements taken at the T0 site, upwind of Manaus, (the Amazonian Tall Tower Observatory, ATTO site), at the T2 site, near Manaus, frequently impacted by relatively fresh emissions from the city and at T3, 60 km downwind of Manaus. This work relates the aerosol dynamics of the mixture of anthropogenic emissions from Manaus and the biogenic air masses, and how it evolves from T2 to T3 under different atmospheric conditions. Focus is on the aerosol size distribution, supported by aerosol mass spectrometry and gas-phase composition, in particular at the T2 site. At T0, the aerosol number concentration has been observed to increase from an average of 380 cm-3 to 1750 cm-3 from the wet to the dry season. The mean geometric diameter increased as well, from 95 nm to 145 nm. Interestingly, at the T2 site no significant difference was observed in number concentration between wet and dry seasons (approximately 4300 cm-3) with an average diameter of 60 nm during the former and 97 nm in the latter. Such measurements provide a unique dataset to understand the aerosol life cycle and the impact of urban emissions in the heart of the Amazon Forest.

SOA precursors at the T0 site during the 2010 CARES campaign

NASA Astrophysics Data System (ADS)

Wallace, H. W.; Jobson, B. T.; Erickson, M. H.

2010-12-01

Continuous measurements of C5 to C12 Volatile Organic Compounds (VOC) have been made using the Washington State University Mobile Atmospheric Chemistry Laboratory (MACL), at the T0 site during the month of June 2010 Carbonaceous Aerosol Carbonaceous Aerosols and Radiative Effects Study (CARES). These measurements were made to better understand aerosol formation and growth in Sacramento, CA and the surrounding areas. Using a sorbent based preconcentration sampling technique for our quadrupole ion trap gas chromatography mass spectrometer (GCMS), we have measured anthropogenic and biogenic secondary organic aerosol (SOA) precursors. Major biogenic VOCs identified include: α-pinene, limonene, isoprene, phellanderene and β-pinene. Diurnal profiles of the concentrations will be presented. Monoterpenes were highest in the mornings while isoprene was highest in the afternoon. In addition to understanding the diurnal profiles the SOA precursors at the T0 site, the relative contributions of biogenic and anthropogenic compounds to SOA formation will be presented.

Aerosol fabrication methods for monodisperse nanoparticles

DOEpatents

Jiang, Xingmao; Brinker, C Jeffrey

2014-10-21

Exemplary embodiments provide materials and methods for forming monodisperse particles. In one embodiment, the monodisperse particles can be formed by first spraying a nanoparticle-containing dispersion into aerosol droplets and then heating the aerosol droplets in the presence of a shell precursor to form core-shell particles. By removing either the shell layer or the nanoparticle core of the core-shell particles, monodisperse nanoparticles can be formed.

Characterization of Fine Particulate Matter (PM) and Secondary PM Precursor Gases in the Mexico City Metropolitan Area

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