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.

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.

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

conditions and compared to the loss rate of EC. The latter is used as an inert tracer for estimating aerosol mechanical deposition and wall losses of the otherwise chemically conserved aerosol species. The OC/EC ratio increased with smoke aging for the flaming phase, suggesting a production/partitioning of organic compounds after emission. On the other hand, for smoldering burns OC/EC ratios decreased further with aging due to additional sinks of OC, other than those related to deposition and wall losses alone, such as evaporation of semi-volatile compounds. The chemical fingerprints of the major PM components of fresh and aged smoke found in this study are proposed to be used for the assessment of contributions from Siberian biomass burning to atmospheric pollution in source apportionment studies like those using molecular marker approaches.

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

NASA Astrophysics Data System (ADS)

Sun, H.; Bond, T.

2004-12-01

organics in aerosols, we propose a Climate-Relevant Optical & Structural Subgroups of OC (CROSS-OC) which is a classification for organic aerosols based on structural and optical properties. We provide broad classes aiming at global models instead of very detailed classifications, which are not amenable for use in global-scale models due to the calculation cost. Organic matter (OM) which includes the hydrogen and oxygen bound to this carbon is divided into classes with varied absorption and scattering capabilities. Because our inventory tabulates emissions from specific sources, we make use of data available from source characterization. We present a global emission inventory of primary carbonaceous aerosols that has been designed for global climate modeling purpose. The inventory is based on our CROSS-OC classification and considers emissions from fossil fuels, biofuels, and open biomass burning. Fuel type, combustion type, and emission controls, and their prevalence on a regional basis are combined to determine emission factors for all types of carbonaceous aerosols. We also categorize surface concentration observations for BC and OC by region, size (super vs. sub micron), measurement type, time (including season) and date. We parallel the data format suggested by the Global Atmosphere Watch aerosol database. Work underway includes providing information on the CROSS-OC divisions in ambient aerosol when measurements contain sufficient detail.

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

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

Aerosol removal due to precipitation and wind forcings in Milan urban area

NASA Astrophysics Data System (ADS)

Cugerone, Katia; De Michele, Carlo; Ghezzi, Antonio; Gianelle, Vorne

2018-01-01

Air pollution represents a critical issue in Milan urban area (Northern Italy). Here, the levels of fine particles increase, overcoming the legal limits, mostly in wintertime, due to favourable calm weather conditions and large heating and vehicular traffic emissions. The main goal of this work is to quantify the aerosol removal effect due to precipitation at the ground. At first, the scavenging coefficients have been calculated for aerosol particles with diameter between 0.25 and 3 μm. The average values of this coefficient vary between 2 ×10-5 and 5 ×10-5 s-1. Then, the aerosol removal induced separately by precipitation and wind have been compared through the introduction of a removal index. As a matter of fact, while precipitation leads to a proper wet scavenging of the particles from the atmosphere, high wind speeds cause enhanced particle dispersion and dilution, that locally bring to a tangible decrease of aerosol particles' number. The removal triggered by these two forcings showed comparable average values, but different trends. The removal efficiency of precipitation lightly increases with the increase of particle diameters and vice versa happens with strong winds.

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.

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.

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

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

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

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

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.

Reductions in aircraft particulate emissions due to the use of Fischer-Tropsch fuels

NASA Astrophysics Data System (ADS)

Beyersdorf, A. J.; Timko, M. T.; Ziemba, L. D.; Bulzan, D.; Corporan, E.; Herndon, S. C.; Howard, R.; Miake-Lye, R.; Thornhill, K. L.; Winstead, E.; Wey, C.; Yu, Z.; Anderson, B. E.

2014-01-01

feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30-44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near zero for FT fuels) due to decreased fuel sulfur content. To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (-4 to 20 °C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to -8 × 1014 particles (kg fuel)-1 °C-1 for particle number emissions and -10 mm3 (kg fuel)-1 °C-1 for particle volume emissions. The temperature dependency of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft-produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols, with a smaller fraction as a soot coating. Conversion efficiencies of up to 2.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO2) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.

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.

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

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.

Reductions in aircraft particulate emissions due to the use of Fischer-Tropsch fuels

NASA Astrophysics Data System (ADS)

Beyersdorf, A. J.; Timko, M. T.; Ziemba, L. D.; Bulzan, D.; Corporan, E.; Herndon, S. C.; Howard, R.; Miake-Lye, R.; Thornhill, K. L.; Winstead, E.; Wey, C.; Yu, Z.; Anderson, B. E.

2013-06-01

The use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability and the sustainability of fuel sources. Concurrent reductions in particulate emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January-February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer-Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions of 84% averaged over all powers) and blended fuels (64%) relative to the JP-8 baseline with the largest reductions at idle conditions. The alternative fuels also produced smaller soot (e.g. at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84

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

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.

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

Impact of aerosol emission controls on future Arctic sea ice cover

NASA Astrophysics Data System (ADS)

Gagné, M.-Ã..; Gillett, N. P.; Fyfe, J. C.

2015-10-01

We examine the response of Arctic sea ice to projected aerosol and aerosol precursor emission changes under the Representative Concentration Pathway (RCP) scenarios in simulations of the Canadian Earth System Model. The overall decrease in aerosol loading causes a warming, largest over the Arctic, which leads to an annual mean reduction in sea ice extent of approximately 1 million km2 over the 21st century in all RCP scenarios. This accounts for approximately 25% of the simulated reduction in sea ice extent in RCP 4.5, and 40% of the reduction in RCP 2.5. In RCP 4.5, the Arctic ocean is projected to become ice-free during summertime in 2045, but it does not become ice-free until 2057 in simulations with aerosol precursor emissions held fixed at 2000 values. Thus, while reductions in aerosol emissions have significant health and environmental benefits, their substantial contribution to projected Arctic climate change should not be overlooked.

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.

Can scooter emissions dominate urban organic aerosol?

NASA Astrophysics Data System (ADS)

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

2014-05-01

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

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

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

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 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

-industrial temperature will be, making the 1.5◦C temperature goal impossible to reach. Although the global reduction of anthropogenic aerosols can greatly enforce the global warming effect due to GHGs, all our simulations resulted in temperature increase bellow (but not well bellow) 2◦C above preindustrial levels - a slightly more realistic target compared to 1.5◦C. The results of this study are based on simulations of only two climate models. As such, we do not regard these results as indisputable, but we consider that aerosols and their effect on climate deserve more attention when discussing future aerosol emission.

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.

Physico-Chemical Evolution of Organic Aerosol from Wildfire Emissions

NASA Astrophysics Data System (ADS)

Croteau, P.; Jathar, S.; Akherati, A.; Galang, A.; Tarun, S.; Onasch, T. B.; Lewane, L.; Herndon, S. C.; Roscioli, J. R.; Yacovitch, T. I.; Fortner, E.; Xu, W.; Daube, C.; Knighton, W. B.; Werden, B.; Wood, E.

2017-12-01

Wildfires are the largest combustion-related source of carbonaceous emissions to the atmosphere; these include direct emissions of black carbon (BC), primary organic aerosol (POA) and semi-volatile, intermediate-volatility, and volatile organic compounds (SVOCs, IVOCs, and VOCs). However, there are large uncertainties surrounding the evolution of these carbonaceous emissions as they are physically and chemically transformed in the atmosphere. To understand these transformations, we performed sixteen experiments using an environmental chamber to simulate day- and night-time chemistry of gas- and aerosol-phase emissions from 6 different fuels at the Fire Laboratory in Missoula, MT. Across the test matrix, the experiments simulated 2 to 8 hours of equivalent day-time aging (with the hydroxyl radical and ozone) or several hours of night-time aging (with the nitrate radical). Aging resulted in an average organic aerosol (OA) mass enhancement of 28% although the full range of OA mass enhancements varied between -10% and 254%. These enhancement findings were consistent with chamber and flow reactor experiments performed at the Fire Laboratory in 2010 and 2012 but, similar to previous studies, offered no evidence to link the OA mass enhancement to fuel type or oxidant exposure. Experiments simulating night-time aging resulted in an average OA mass enhancement of 10% and subsequent day-time aging resulted in a decrease in OA mass of 8%. While small, for the first time, these experiments highlighted the continuous nature of the OA evolution as the wildfire smoke cycled through night- and day-time processes. Ongoing work is focussed on (i) quantifying bulk compositional changes in OA, (ii) comparing the near-field aging simulated in this work with far-field aging simulated during the same campaign (via a mini chamber and flow tube) and (iii) integrating wildfire smoke aging datasets over the past decade to examine the relationship between OA mass enhancement ratios, modified

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.

The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

NASA Astrophysics Data System (ADS)

Sakamoto, Kimiko M.; Laing, James R.; Stevens, Robin G.; Jaffe, Daniel A.; Pierce, Jeffrey R.

2016-06-01

Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The

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

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

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

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.

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.

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

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

Future premature mortality due to O3, secondary inorganic aerosols and primary PM in Europe--sensitivity to changes in climate, anthropogenic emissions, population and building stock.

PubMed

Geels, Camilla; Andersson, Camilla; Hänninen, Otto; Lansø, Anne Sofie; Schwarze, Per E; Skjøth, Carsten Ambelas; Brandt, Jørgen

2015-03-04

Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000-2009, 2050-2059 and 2080-2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future.

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

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

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

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.

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.

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.

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.

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

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

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

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

Future Premature Mortality Due to O3, Secondary Inorganic Aerosols and Primary PM in Europe — Sensitivity to Changes in Climate, Anthropogenic Emissions, Population and Building Stock

PubMed Central

Geels, Camilla; Andersson, Camilla; Hänninen, Otto; Lansø, Anne Sofie; Schwarze, Per E.; Ambelas Skjøth, Carsten; Brandt, Jørgen

2015-01-01

Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000–2009, 2050–2059 and 2080–2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future. PMID:25749320

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

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.

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.

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

NASA Technical Reports Server (NTRS)

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

1999-01-01

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

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.

Sensitivity of inorganic aerosol radiative effects to U.S. emissions

NASA Astrophysics Data System (ADS)

Holt, J. I.; Solomon, S.; Selin, N. E.

2017-06-01

Between 2005 and 2012, U.S. emissions of nitrogen oxides (NOx) and sulfur dioxide (SO2) decreased by 42% and 62%, respectively. These species, as well as ammonia (NH3), are precursors of inorganic fine aerosols, which scatter incoming shortwave radiation and thus affect climate. Scaling aerosol concentrations to emissions, as might be done for near-term climate projections, neglects nonlinear chemical interactions. To estimate the magnitude of these nonlinearities, we conduct a suite of simulations with a chemical transport model and an off-line radiative transfer model. We find that the direct radiative effect (DRE) over the North American domain decreases by 59 and 160 mW m-2 in winter and summer, respectively, between 2005 and 2012. The sensitivities of DRE to NOx and SO2 emissions increase, by 11% and 21% in summer, while sensitivity to NH3 emissions decreases. The wintertime sensitivity of DRE to NOx emissions is small in 2005 but is 5 times as large in 2012. Scaling radiative effects from 2005 to 2012 based on 2005 sensitivities overestimates the magnitude of the DRE of 7% and 6% of the U.S. attributable DRE in January and July, respectively. The difference between the changes in DRE and the changes in sensitivity suggests that scaling to SO2 emissions alone has so far been an accurate approximation, but it may not be in the near future. These values represent the level of accuracy that can be expected in adjusting aerosol radiative effects in climate models without chemistry.

Investigation of air pollution and regional climate change due to anthropogenic aerosols

NASA Astrophysics Data System (ADS)

Nakata, Makiko; Sano, Itaru; Mukai, Sonoyo

2016-10-01

Increased emissions of anthropogenic aerosols associated with economic growth can lead to increased concentrations of hazardous air pollutants. In particular, large cities in East Asia have experienced numerous heavy haze episodes. Atmospheric aerosol distributions in East Asia are complex, being influenced by both natural phenomena and human activity, with urban areas in particular being dominated by fine anthropogenic aerosols released from diesel-powered vehicles and industrial activity. In Japan, air pollution levels have been reduced; nevertheless, in recent years, there is increasing concern regarding air pollution caused by fine particulate matter. The origins of air pollution were examined, focusing on the comparison between aerosol properties observed from satellites and that on the ground. Because of their short life spans, concentrations of anthropogenic aerosols are highest over the source regions, and as a result, the climatic impacts of anthropogenic aerosols are also found to be most pronounced in these regions. In this study, aerosol impacts on climate are assessed by numerical model simulations. The direct effects of aerosols include reduced solar radiation, and hence a decrease in surface temperatures. In addition to these changes in the radiation budget, aerosols have a significant potential to change cloud and precipitation fields. These climatic responses to aerosols can manifest far from their source regions with high industrial activities.

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

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.;

Review of Urban Secondary Organic Aerosol Formation from Gasoline and Diesel Motor Vehicle Emissions.

PubMed

Gentner, Drew R; Jathar, Shantanu H; Gordon, Timothy D; Bahreini, Roya; Day, Douglas A; El Haddad, Imad; Hayes, Patrick L; Pieber, Simone M; Platt, Stephen M; de Gouw, Joost; Goldstein, Allen H; Harley, Robert A; Jimenez, Jose L; Prévôt, André S H; Robinson, Allen L

2017-02-07

Secondary organic aerosol (SOA) is formed from the atmospheric oxidation of gas-phase organic compounds leading to the formation of particle mass. Gasoline- and diesel-powered motor vehicles, both on/off-road, are important sources of SOA precursors. They emit complex mixtures of gas-phase organic compounds that vary in volatility and molecular structure-factors that influence their contributions to urban SOA. However, the relative importance of each vehicle type with respect to SOA formation remains unclear due to conflicting evidence from recent laboratory, field, and modeling studies. Both are likely important, with evolving contributions that vary with location and over short time scales. This review summarizes evidence, research needs, and discrepancies between top-down and bottom-up approaches used to estimate SOA from motor vehicles, focusing on inconsistencies between molecular-level understanding and regional observations. The effect of emission controls (e.g., exhaust aftertreatment technologies, fuel formulation) on SOA precursor emissions needs comprehensive evaluation, especially with international perspective given heterogeneity in regulations and technology penetration. Novel studies are needed to identify and quantify "missing" emissions that appear to contribute substantially to SOA production, especially in gasoline vehicles with the most advanced aftertreatment. Initial evidence suggests catalyzed diesel particulate filters greatly reduce emissions of SOA precursors along with primary aerosol.

Impacts of controlling biomass burning emissions on wintertime carbonaceous aerosol in Europe

NASA Astrophysics Data System (ADS)

Fountoukis, C.; Butler, T.; Lawrence, M. G.; Denier van der Gon, H. A. C.; Visschedijk, A. J. H.; Charalampidis, P.; Pilinis, C.; Pandis, S. N.

2014-04-01

We use a 3-D regional chemical transport model, with the latest advancements in the organic aerosol (OA) treatment, and an updated emission inventory for wood combustion to study the organic aerosol change in response to the replacement of current residential wood combustion technologies with pellet stoves. Simulations show a large decrease of fine organic aerosol (more than 60%) in urban and suburban areas during winter and decreases of 30-50% in elemental carbon levels in large parts of Europe. There is also a considerable decrease (around 40%) of oxidized OA, mostly in rural and remote regions. Total PM2.5 mass is predicted to decrease by 15-40% on average during the winter in continental Europe. Accurate representation of the intermediate volatility precursors of organic aerosol in the emission inventory is crucial in assessing the efficiency of such abatement strategies.

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

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

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

concentrations and an increase in nitrate aerosol mass due to an increase in available NH3 for NOx to form aerosol. However, the rate of new particle formation increases due to a decrease in the condensation on pre-existing particles, so the effect of reduced SO2 on CCN is partly compensated. Controlling primary or precursor emissions of carbonaceous aerosols appears less effective in improving air quality, although it shows strong effects on marine CCN, which would constitute a detrimental effect on climate. Any policy decisions related to particulate matter, air quality and climate need to account for such couplings.

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.

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

Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

NASA Astrophysics Data System (ADS)

Jathar, Shantanu Hemant

Atmospheric aerosols exert a large influence on the Earth's climate and cause adverse public health effects, reduced visibility and material degradation. Secondary organic aerosol (SOA), defined as the aerosol mass arising from the oxidation products of gas-phase organic species, accounts for a significant fraction of the submicron atmospheric aerosol mass. Yet, there are large uncertainties surrounding the sources, atmospheric evolution and properties of SOA. This thesis combines laboratory experiments, extensive data analysis and global modeling to investigate the contribution of semi-volatile and intermediate volatility organic compounds (SVOC and IVOC) from combustion sources to SOA formation. The goals are to quantify the contribution of these emissions to ambient PM and to evaluate and improve models to simulate its formation. To create a database for model development and evaluation, a series of smog chamber experiments were conducted on evaporated fuel, which served as surrogates for real-world combustion emissions. Diesel formed the most SOA followed by conventional jet fuel / jet fuel derived from natural gas, gasoline and jet fuel derived from coal. The variability in SOA formation from actual combustion emissions can be partially explained by the composition of the fuel. Several models were developed and tested along with existing models using SOA data from smog chamber experiments conducted using evaporated fuel (this work, gasoline, fischertropschs, jet fuel, diesels) and published data on dilute combustion emissions (aircraft, on- and off-road gasoline, on- and off-road diesel, wood burning, biomass burning). For all of the SOA data, existing models under-predicted SOA formation if SVOC/IVOC were not included. For the evaporated fuel experiments, when SVOC/IVOC were included predictions using the existing SOA model were brought to within a factor of two of measurements with minor adjustments to model parameterizations. Further, a volatility

Roles of production, consumption and trade in global and regional aerosol radiative forcing

NASA Astrophysics Data System (ADS)

Lin, J.; Tong, D.; Davis, S. J.; Ni, R.; Tan, X.; Pan, D.; Zhao, H.; Lu, Z.; Streets, D. G.; Feng, T.; Zhang, Q.; Yan, Y.; Hu, Y.; Li, J.; Liu, Z.; Jiang, X.; Geng, G.; He, K.; Huang, Y.; Guan, D.

2016-12-01

Anthropogenic aerosols exert strong radiative forcing on the climate system. Prevailing view regards aerosol radiative forcing as a result of emissions from regions' economic production, with China and other developing regions having the largest contributions to radiative forcing at present. However, economic production is driven by global demand for computation, and international trade allows for separation of regions consuming goods and services from regions where goods and related aerosol pollution are produced. It has recently been recognized that regions' consumption and trade have profoundly altered the spatial distribution of aerosol emissions and pollution. Building upon our previous work, this study quantifies for the first time the roles of trade and consumption in aerosol climate forcing attributed to different regions. We contrast the direct radiative forcing of aerosols related to regions' consumption of goods and services against the forcing due to emissions produced in each region. Aerosols assessed include black carbon, primary organic aerosol, and secondary inorganic aerosols including sulfate, nitrate and ammonium. We find that global aerosol radiative forcing due to emissions produced in East Asia is much stronger than the forcing related to goods and services ultimately consumed in that region because of its large net export of emissions-intensive goods. The opposite is true for net importers like Western Europe and North America: global radiative forcing related to consumption is much greater than the forcing due to emissions produced in these regions. Overall, trade is associated with a shift of radiative forcing from net importing to net exporting regions. Compared to greenhouse gases such as carbon dioxide, the short atmospheric lifetimes of aerosols cause large localized differences in radiative forcing. International efforts to reduce emissions in the exporting countries will help alleviate trade-related climate and health impacts of

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.

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

coastal areas. The formation of 23, 27 and 27 %, respectively of, ammonium, nitrate and sulfate aerosols is due to the emissions within the marine and coastal area.

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.

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.

Relative Contributions of Regional and Sector Emissions to the Radiative Forcing of Aerosol-Radiation and Aerosol-Cloud Interactions Based on the AeroCOM Phase III/HTAP2 Experiment

NASA Astrophysics Data System (ADS)

Takemura, T.; Chin, M.

2014-12-01

It is important to understand relative contributions of each regional and sector emission of aerosols and their precursor gases to the regional and global mean radiative forcing of aerosol-radiation and aerosol-cloud interactions. This is because it is useful for international cooperation on controls of air pollution and anthropogenic climate change along most suitable reduction path of their emissions from each region and sector. The Task Force on Hemispheric Transport of Air Pollution (TF HTAP) under the United Nations researches the intercontinental transport of air pollutants including aerosols with strong support of the Aerosol Comparisons between Observations and Models (AeroCOM). The ongoing AeroCOM Phase III/HTAP2 experiment assesses relative contributions of regional and sector sources of aerosols and their precursor gases to the air quality using global aerosol transport models with latest emission inventories. In this study, the extended analyses on the relative contributions of each regional and sector emission to the radiative forcing of aerosol-radiation and aerosol-cloud interactions are done from the AeroCOM Phase III/HTAP2 experiment. Simulated results from MIROC-SPRINTARS and other some global aerosol models participating in the the AeroCOM Phase III/HTAP2 experiment are assessed. Acknowledgements: This study is based on the AeroCOM Phase III/HTAP2 experiment and partly supported by the Environment Research and Technology Development Fund (S-12-3) of the Ministry of the Environment, Japan.

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

included. Shortwave heating rates increase in the aerosol layer by 18 % in the high emissions case. The mean surface temperature is reduced by 0.14 ± 0.24 °C and mean precipitation is reduced by 14.5 % in the peak biomass region due to both changes in cloud cover and cloud microphysical properties. If the increase in BBA occurs in a particularly dry year, the resulting reduction in precipitation may exacerbate the drought. The position of the South Atlantic high pressure is slightly altered by the presence of increased BBA, and the strength of the southward low-level jet to the east of the Andes is increased. There is some evidence that some impacts of increased BBA persist through the transition into the monsoon, particularly in precipitation, but the differences are only statistically significant in some small regions in November. This study therefore provides an insight into how variability in deforestation, realized through variability in biomass burning emissions, may contribute to the South American climate, and consequently on the possible impacts of future changes in BBA emissions.

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

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).

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.

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

NASA Technical Reports Server (NTRS)

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

2010-01-01

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

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

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

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.

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.

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.

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.

Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols.

PubMed

Jacobson, M Z

2001-02-08

Aerosols affect the Earth's temperature and climate by altering the radiative properties of the atmosphere. A large positive component of this radiative forcing from aerosols is due to black carbon--soot--that is released from the burning of fossil fuel and biomass, and, to a lesser extent, natural fires, but the exact forcing is affected by how black carbon is mixed with other aerosol constituents. From studies of aerosol radiative forcing, it is known that black carbon can exist in one of several possible mixing states; distinct from other aerosol particles (externally mixed) or incorporated within them (internally mixed), or a black-carbon core could be surrounded by a well mixed shell. But so far it has been assumed that aerosols exist predominantly as an external mixture. Here I simulate the evolution of the chemical composition of aerosols, finding that the mixing state and direct forcing of the black-carbon component approach those of an internal mixture, largely due to coagulation and growth of aerosol particles. This finding implies a higher positive forcing from black carbon than previously thought, suggesting that the warming effect from black carbon may nearly balance the net cooling effect of other anthropogenic aerosol constituents. The magnitude of the direct radiative forcing from black carbon itself exceeds that due to CH4, suggesting that black carbon may be the second most important component of global warming after CO2 in terms of direct forcing.

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

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

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.;

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

Evaluation of biogenic emission flux and its impact on oxidants and inorganic aerosols in East Asia

NASA Astrophysics Data System (ADS)

Han, K. M.; Song, C. H.; Park, R. S.; Woo, J.; Kim, H.

2010-12-01

As a major precursor during the summer season, biogenic species are of primary importance in the ozone and SOAs (secondary organic aerosols) formations. Isoprene and mono-terpene also influence the level of inorganic aerosols (i.e. sulfate and nitrate) by controlling OH radicals. However, biogenic emission fluxes are highly uncertain in East Asia. While isoprene emission fluxes from the GEIA (Global Emissions Inventory Activity) and POET (Precursors of Ozone and their Effects in the Troposphere) inventories estimate approximately 20 Tg yr-1 in East Asia, those from the MEGAN (Model of Emissions of Gases and Aerosols from Nature) and MOHYCAN (MOdel for Hydrocarbon emissions by the CANopy) estimate approximately 10 Tg yr-1 and 5 Tg yr-1, respectively. In order to evaluate and/or quantify the magnitude of biogenic emission fluxes over East Asia, the tropospheric HCHO columns obtained from the GOME (Global Ozone Monitoring Experiment) observations were compared with the HCHO columns from the CMAQ (Community Multi-scale Air Quality) simulations over East Asia. In this study, US EPA Models-3/CMAQ v4.5.1 model simulation using the ACE-ASIA (Asia Pacific Regional Aerosol Characterization Experiment) emission inventory for anthropogenic pollutants and GEIA, POET, MEGAN, and MOHYCAN emission inventories for biogenic species was carried out in conjunction with the Meteorological fields generated from the PSU/NCAR MM5 (Pennsylvania state University/National Center for Atmospheric Research Meso-scale Model 5) model for the summer episodes of the year 2002. In addition to an evaluation of the biogenic emission flux, we investigated the impact of the uncertainty in biogenic emission inventory on inorganic aerosol formations and variations of oxidants (OH, O3, and H2O2) in East Asia. In this study, when the GEIA and POET emission inventories are used, the CMAQ-derived HCHO columns are highly overestimated over East Asia, particularly South China compared with GOME-derived HCHO

Greenland records of aerosol source and atmospheric lifetime changes from the Eemian to the Holocene.

PubMed

Schüpbach, S; Fischer, H; Bigler, M; Erhardt, T; Gfeller, G; Leuenberger, D; Mini, O; Mulvaney, R; Abram, N J; Fleet, L; Frey, M M; Thomas, E; Svensson, A; Dahl-Jensen, D; Kettner, E; Kjaer, H; Seierstad, I; Steffensen, J P; Rasmussen, S O; Vallelonga, P; Winstrup, M; Wegner, A; Twarloh, B; Wolff, K; Schmidt, K; Goto-Azuma, K; Kuramoto, T; Hirabayashi, M; Uetake, J; Zheng, J; Bourgeois, J; Fisher, D; Zhiheng, D; Xiao, C; Legrand, M; Spolaor, A; Gabrieli, J; Barbante, C; Kang, J-H; Hur, S D; Hong, S B; Hwang, H J; Hong, S; Hansson, M; Iizuka, Y; Oyabu, I; Muscheler, R; Adolphi, F; Maselli, O; McConnell, J; Wolff, E W

2018-04-16

The Northern Hemisphere experienced dramatic changes during the last glacial, featuring vast ice sheets and abrupt climate events, while high northern latitudes during the last interglacial (Eemian) were warmer than today. Here we use high-resolution aerosol records from the Greenland NEEM ice core to reconstruct the environmental alterations in aerosol source regions accompanying these changes. Separating source and transport effects, we find strongly reduced terrestrial biogenic emissions during glacial times reflecting net loss of vegetated area in North America. Rapid climate changes during the glacial have little effect on terrestrial biogenic aerosol emissions. A strong increase in terrestrial dust emissions during the coldest intervals indicates higher aridity and dust storm activity in East Asian deserts. Glacial sea salt aerosol emissions in the North Atlantic region increase only moderately (50%), likely due to sea ice expansion. Lower aerosol concentrations in Eemian ice compared to the Holocene are mainly due to shortened atmospheric residence time, while emissions changed little.

Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models

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

Fan, Tianyi; Liu, Xiaohong; Ma, Po -Lun

Here, global climate models often underestimate aerosol loadings in China, and these biases can have significant implications for anthropogenic aerosol radiative forcing and climate effects. The biases may be caused by either the emission inventory or the treatment of aerosol processes in the models, or both, but so far no consensus has been reached. In this study, a relatively new emission inventory based on energy statistics and technology, Multi-resolution Emission Inventory for China (MEIC), is used to drive the Community Atmosphere Model version 5 (CAM5) to evaluate aerosol distribution and radiative effects against observations in China. The model results aremore » compared with the model simulations with the widely used Intergovernmental Panel on Climate Change Fifth Assessment Report (IPCC AR5) emission inventory. We find that the new MEIC emission improves the aerosol optical depth (AOD) simulations in eastern China and explains 22–28 % of the AOD low bias simulated with the AR5 emission. However, AOD is still biased low in eastern China. Seasonal variation of the MEIC emission leads to a better agreement with the observed seasonal variation of primary aerosols than the AR5 emission, but the concentrations are still underestimated. This implies that the atmospheric loadings of primary aerosols are closely related to the emission, which may still be underestimated over eastern China. In contrast, the seasonal variations of secondary aerosols depend more on aerosol processes (e.g., gas- and aqueous-phase production from precursor gases) that are associated with meteorological conditions and to a lesser extent on the emission. It indicates that the emissions of precursor gases for the secondary aerosols alone cannot explain the low bias in the model. Aerosol secondary production processes in CAM5 should also be revisited. The simulation using MEIC estimates the annual-average aerosol direct radiative effects (ADREs) at the top of the atmosphere (TOA), at

Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models

NASA Astrophysics Data System (ADS)

Fan, Tianyi; Liu, Xiaohong; Ma, Po-Lun; Zhang, Qiang; Li, Zhanqing; Jiang, Yiquan; Zhang, Fang; Zhao, Chuanfeng; Yang, Xin; Wu, Fang; Wang, Yuying

2018-02-01

Global climate models often underestimate aerosol loadings in China, and these biases can have significant implications for anthropogenic aerosol radiative forcing and climate effects. The biases may be caused by either the emission inventory or the treatment of aerosol processes in the models, or both, but so far no consensus has been reached. In this study, a relatively new emission inventory based on energy statistics and technology, Multi-resolution Emission Inventory for China (MEIC), is used to drive the Community Atmosphere Model version 5 (CAM5) to evaluate aerosol distribution and radiative effects against observations in China. The model results are compared with the model simulations with the widely used Intergovernmental Panel on Climate Change Fifth Assessment Report (IPCC AR5) emission inventory. We find that the new MEIC emission improves the aerosol optical depth (AOD) simulations in eastern China and explains 22-28 % of the AOD low bias simulated with the AR5 emission. However, AOD is still biased low in eastern China. Seasonal variation of the MEIC emission leads to a better agreement with the observed seasonal variation of primary aerosols than the AR5 emission, but the concentrations are still underestimated. This implies that the atmospheric loadings of primary aerosols are closely related to the emission, which may still be underestimated over eastern China. In contrast, the seasonal variations of secondary aerosols depend more on aerosol processes (e.g., gas- and aqueous-phase production from precursor gases) that are associated with meteorological conditions and to a lesser extent on the emission. It indicates that the emissions of precursor gases for the secondary aerosols alone cannot explain the low bias in the model. Aerosol secondary production processes in CAM5 should also be revisited. The simulation using MEIC estimates the annual-average aerosol direct radiative effects (ADREs) at the top of the atmosphere (TOA), at the surface, and

Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models

DOE PAGES

Fan, Tianyi; Liu, Xiaohong; Ma, Po -Lun; ...

2018-02-01

Here, global climate models often underestimate aerosol loadings in China, and these biases can have significant implications for anthropogenic aerosol radiative forcing and climate effects. The biases may be caused by either the emission inventory or the treatment of aerosol processes in the models, or both, but so far no consensus has been reached. In this study, a relatively new emission inventory based on energy statistics and technology, Multi-resolution Emission Inventory for China (MEIC), is used to drive the Community Atmosphere Model version 5 (CAM5) to evaluate aerosol distribution and radiative effects against observations in China. The model results aremore » compared with the model simulations with the widely used Intergovernmental Panel on Climate Change Fifth Assessment Report (IPCC AR5) emission inventory. We find that the new MEIC emission improves the aerosol optical depth (AOD) simulations in eastern China and explains 22–28 % of the AOD low bias simulated with the AR5 emission. However, AOD is still biased low in eastern China. Seasonal variation of the MEIC emission leads to a better agreement with the observed seasonal variation of primary aerosols than the AR5 emission, but the concentrations are still underestimated. This implies that the atmospheric loadings of primary aerosols are closely related to the emission, which may still be underestimated over eastern China. In contrast, the seasonal variations of secondary aerosols depend more on aerosol processes (e.g., gas- and aqueous-phase production from precursor gases) that are associated with meteorological conditions and to a lesser extent on the emission. It indicates that the emissions of precursor gases for the secondary aerosols alone cannot explain the low bias in the model. Aerosol secondary production processes in CAM5 should also be revisited. The simulation using MEIC estimates the annual-average aerosol direct radiative effects (ADREs) at the top of the atmosphere (TOA), at

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

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.

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

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.

Spectral solar attenuation due to aerosol loading over an urban area in India

NASA Astrophysics Data System (ADS)

Latha, K. Madhavi; Badarinath, K. V. S.

2005-06-01

Anthropogenic activities in urban areas are sources for atmospheric aerosols and are increasing due to population explosion and migration. Many large cities in the developing world are presently plagued by high levels of atmospheric pollution and long-term effect of urban aerosol on climate is an important topic. In the present study, ground-based measurements of solar irradiance, aerosol loading and black carbon (BC) aerosol concentration have been analyzed during different aerosol loading conditions during 2003 over an urban environment. BC aerosols concentration has been observed to be enhanced during high aerosol optical depth day suggesting influence of local anthropogenic activities. The analysis of wind fields over the study area during the measurement period is from north with continental air mass prevailing over the region. Spectral measurements of solar irradiance exhibited variations based on aerosol loading in urban atmosphere. Relative attenuations caused by aerosols have been found to be of the order of 21% and 17% on the irradiance on visible and near infrared respectively.

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.

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.

Fossil Fuel Combustion-Related Emissions Dominate Atmospheric Ammonia Sources during Severe Haze Episodes: Evidence from 15N-Stable Isotope in Size-Resolved Aerosol Ammonium

NASA Astrophysics Data System (ADS)

Pan, Y.; Tian, S.; Liu, D.; Fang, Y.; Zhu, X.; Zhang, Q.; Zheng, B.; Michalski, G. M.; Wang, Y.

2016-12-01

The reduction of ammonia (NH3) emissions is urgently needed due to its major contributions to nitrogen deposition and particle pollution. 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 15N (expressed using δ15N values) of ammonium (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 factoring the isotope exchange between NH3 gas and aerosol NH4+, the δ15N 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 δ15N 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. This work also shed lights on the sources of nitrogen deposition in downwind ecosystems.

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.

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.

Profile of heating rate due to aerosols using lidar and skyradiometer in SKYNET Hefei site

NASA Astrophysics Data System (ADS)

Wang, Z.; Liu, D.; Xie, C.

2015-12-01

Atmospheric aerosols have a significant impact on climate due to their important role in modifying atmosphere energy budget. On global scale, the direct radiative forcing is estimated to be in the range of -0.9 to -0.1 Wm-2 for aerosols [1]. Yet, these estimates are subject to very large uncertainties because of uncertainties in spatial and temporal variations of aerosols. At local scales, as aerosol properties can vary spatially and temporally, radiative forcing due to aerosols can be also very different and it can exceed the global value by an order of magnitude. Hence, it is very important to investigate aerosol loading, properties, and radiative forcing due to them in detail on local regions of climate significance. Haze and dust events in Hefei, China are explored by Lidar and Skyradiometer. Aerosol optical properties including the AOD, SSA, AAE and size distribution are analysed by using the SKYRAD.PACK [2] and presented in this paper. Furthermore, the radiative forcing due to aerosols and the heating rate in the ATM are also calculated using SBDART model [3]. The results are shown that the vertical heating rate is tightly related to aerosol profile. References: 1. IPCC. 2007. Climate Change 2007: The Physical Science Basic. Contribution of Working Group I Contribution to the Intergovernmental Panel on Climate Change Fourth Assessment Report. Solomon S, Qing D H, Manning M, et al. eds., Cambridge University Press, Cambridge, United Kingdom and New York, N Y, USA. 2. Nakajima, T., G. Tonna, R. Rao, Y. Kaufman, and B. Holben, 1996: Use of sky brightness measurements from ground for remote sensing of particulate poly dispersions, Appl. Opt., 35, 2672-2686. 3. Ricchiazzi et al 1998. SBDART: a research and teaching software tool for plane-parallel radiative transfer in the Earth's atmosphere,Bulletin of the American Meteorological Society,79,2101-2114.

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

NASA Astrophysics Data System (ADS)

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

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

Combining Multi-Sensor Measurements and Models to Constrain Time-Varying Aerosol Fire Emissions

NASA Astrophysics Data System (ADS)

Cohen, J. B.

2013-12-01

A significant portion of global Black Carbon (BC) and Organic Carbon (OC) aerosols are emitted into the atmosphere due to fires. However, due to their spatially and temporally heterogeneous nature, quantifying these emissions has proven to be difficult. Some of the problems stem from variability over multiple spatial and temporal scales: ranging from kilometers in size to thousands of kilometers in impact, and from month-to-month variations in the burning season to interannual variation in overall fire strength which follows such global phenomena as El-Nino. Yet, because of the unique absorbing properties that these aerosols have, they leave a distinct impact on the regional and global climate system, as well as the ability to intensely impact human health in downwind areas, proper quantification of the emissions is absolutely essential. To achieve such a critical understanding of their emissions in space and time, a start-of-the art modelling system of their chemical and physical processing, transport, and removal is implemented. This system is capable of effectively and uniquely simulating many impacts important in the atmosphere, including: enhanced absorption associated with internal mixing, mass and number conservation, the direct and semi-direct effects on atmospheric dynamics and circulation, and appropriate non-linear consideration of urban-scale chemical and physical processing. This modelling system has been used in connection with 3 separate sources of data, to achieve an end product that is heavily dependent on both. First of all, the model has been run in a data-assimilation mode to constrain the annual-average emissions of BC using the Kalman Filter technique. This global constraint, the first of its type, relies heavily on ground-based sensors from NASA as well as other organizations. Secondly, data of the decadal-scale variation in aerosol optical depth, surface reflectance, and radiative power have been obtained from the MODIS and MISR sensors

Seasonal dependence of aerosol processing in urban Philadelphia

NASA Astrophysics Data System (ADS)

Avery, A. M.; Waring, M. S.; DeCarlo, P. F.

2017-12-01

Urban aerosols pose an important threat to human health due to the conflation of emissions and concentrated population exposed. Winter and summer aerosol and trace gas measurements were taken in downtown Philadelphia in 2016. Measurements included aerosol composition and size with an Aerodyne Aerosol Mass Spectrometer (AMS), particle size distributions with an SMPS, and an aethalometer. Trace gas measurements of O3, NO, CH4, CO, and CO2 were taken concurrently. Sampling in seasonal extremes provided contrast in aerosol and trace gas composition, aerosol processing, and emission factors. Inorganic aerosol components contributed approximately 60% of the submicron aerosol mass, while summertime aerosol composition was roughly 70% organic matter. Positive Matrix Factorization (PMF) on the organic aerosol (OA) matrix revealed three factors in common in each season, including an oxygenated organic aerosol (OOA) factor with different temporal behavior in each season. In summertime, OOA varied diurnally with ozone and daytime temperature, but in the wintertime, it was anti-correlated with ozone and temperature, and instead trended with calculated liquid water, indicating a seasonally-dependent processing of organic aerosol in Philadelphia's urban environment. Due to the inorganic dominant winter aerosol, liquid water much higher (2.65 μg/m3) in winter than in summer (1.54 μg/m3). Diurnally varying concentrations of background gas phase species (CH4, CO2) were higher in winter and varied less as a result of boundary layer conditions; ozone was also higher in background in winter than summer. Winter stagnation events with low windspeed showed large buildup of trace gases CH4, CO, CO2, and NO. Traffic related aerosol was also elevated with black carbon and hydrocarbon-like OA (HOA) plumes of each at 3-5 times higher than the winter the average value for each. Winter ratios of HOA to black carbon were significantly higher in the winter than the summer due to lower

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

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

Climate Implications of the Heterogeneity of Anthropogenic Aerosol Forcing

NASA Astrophysics Data System (ADS)

Persad, Geeta Gayatri

Short-lived anthropogenic aerosols are concentrated in regions of high human activity, where they interact with radiation and clouds, causing horizontally heterogeneous radiative forcing between polluted and unpolluted regions. Aerosols can absorb shortwave energy in the atmosphere, but deplete it at the surface, producing opposite radiative perturbations between the surface and atmosphere. This thesis investigates climate and policy implications of this horizontal and vertical heterogeneity of anthropogenic aerosol forcing, employing the Geophysical Fluid Dynamics Laboratory's AM2.1 and AM3 models, both at a global scale and using East Asia as a regional case study. The degree of difference between spatial patterns of climate change due to heterogeneous aerosol forcing versus homogeneous greenhouse gas forcing deeply impacts the detection, attribution, and prediction of regional climate change. This dissertation addresses a gap in current understanding of these two forcings' response pattern development, using AM2.1 historical forcing simulations. The results indicate that fast atmospheric and land-surface processes alone substantially homogenize the global pattern of surface energy flux response to heterogeneous aerosol forcing. Aerosols' vertical redistribution of energy significantly impacts regional climate, but is incompletely understood. It is newly identified here, via observations and historical and idealized forcing simulations, that increased aerosol-driven atmospheric absorption may explain half of East Asia's recent surface insolation decline. Further, aerosols' surface and atmospheric effects counteract each other regionally---atmospheric heating enhances summer monsoon circulation, while surface dimming suppresses it---but absorbing aerosols' combined effects reduce summer monsoon rainfall. This thesis constitutes the first vertical decomposition of aerosols' impacts in this high-emissions region and elucidates the monsoonal response to aerosols

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

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.

Enhanced PM2.5 pollution in China due to aerosol-cloud interactions.

PubMed

Zhao, Bin; Liou, Kuo-Nan; Gu, Yu; Li, Qinbin; Jiang, Jonathan H; Su, Hui; He, Cenlin; Tseng, Hsien-Liang R; Wang, Shuxiao; Liu, Run; Qi, Ling; Lee, Wei-Liang; Hao, Jiming

2017-06-30

Aerosol-cloud interactions (aerosol indirect effects) play an important role in regional meteorological variations, which could further induce feedback on regional air quality. While the impact of aerosol-cloud interactions on meteorology and climate has been extensively studied, their feedback on air quality remains unclear. Using a fully coupled meteorology-chemistry model, we find that increased aerosol loading due to anthropogenic activities in China substantially increases column cloud droplet number concentration and liquid water path (LWP), which further leads to a reduction in the downward shortwave radiation at surface, surface air temperature and planetary boundary layer (PBL) height. The shallower PBL and accelerated cloud chemistry due to larger LWP in turn enhance the concentrations of particulate matter with diameter less than 2.5 μm (PM 2.5 ) by up to 33.2 μg m -3 (25.1%) and 11.0 μg m -3 (12.5%) in January and July, respectively. Such a positive feedback amplifies the changes in PM 2.5 concentrations, indicating an additional air quality benefit under effective pollution control policies but a penalty for a region with a deterioration in PM 2.5 pollution. Additionally, we show that the cloud processing of aerosols, including wet scavenging and cloud chemistry, could also have substantial effects on PM 2.5 concentrations.

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.

Elucidating secondary organic aerosol from diesel and gasoline vehicles through detailed characterization of organic carbon emissions

PubMed Central

Gentner, Drew R.; Isaacman, Gabriel; Worton, David R.; Chan, Arthur W. H.; Dallmann, Timothy R.; Davis, Laura; Liu, Shang; Day, Douglas A.; Russell, Lynn M.; Wilson, Kevin R.; Weber, Robin; Guha, Abhinav; Harley, Robert A.; Goldstein, Allen H.

2012-01-01

Emissions from gasoline and diesel vehicles are predominant anthropogenic sources of reactive gas-phase organic carbon and key precursors to secondary organic aerosol (SOA) in urban areas. Their relative importance for aerosol formation is a controversial issue with implications for air quality control policy and public health. We characterize the chemical composition, mass distribution, and organic aerosol formation potential of emissions from gasoline and diesel vehicles, and find diesel exhaust is seven times more efficient at forming aerosol than gasoline exhaust. However, both sources are important for air quality; depending on a region’s fuel use, diesel is responsible for 65% to 90% of vehicular-derived SOA, with substantial contributions from aromatic and aliphatic hydrocarbons. Including these insights on source characterization and SOA formation will improve regional pollution control policies, fuel regulations, and methodologies for future measurement, laboratory, and modeling studies. PMID:23091031

Elucidating secondary organic aerosol from diesel and gasoline vehicles through detailed characterization of organic carbon emissions.

PubMed

Gentner, Drew R; Isaacman, Gabriel; Worton, David R; Chan, Arthur W H; Dallmann, Timothy R; Davis, Laura; Liu, Shang; Day, Douglas A; Russell, Lynn M; Wilson, Kevin R; Weber, Robin; Guha, Abhinav; Harley, Robert A; Goldstein, Allen H

2012-11-06

Emissions from gasoline and diesel vehicles are predominant anthropogenic sources of reactive gas-phase organic carbon and key precursors to secondary organic aerosol (SOA) in urban areas. Their relative importance for aerosol formation is a controversial issue with implications for air quality control policy and public health. We characterize the chemical composition, mass distribution, and organic aerosol formation potential of emissions from gasoline and diesel vehicles, and find diesel exhaust is seven times more efficient at forming aerosol than gasoline exhaust. However, both sources are important for air quality; depending on a region's fuel use, diesel is responsible for 65% to 90% of vehicular-derived SOA, with substantial contributions from aromatic and aliphatic hydrocarbons. Including these insights on source characterization and SOA formation will improve regional pollution control policies, fuel regulations, and methodologies for future measurement, laboratory, and modeling studies.

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...

The Impact of Biogenic and Anthropogenic Atmospheric Aerosol on Climate in Egypt

NASA Astrophysics Data System (ADS)

Ibrahim, A. I.; Zakey, A.; Steiner, A. L.; Shokr, M. E.; El-Raey, M.; Ahmed, Y.; Al-Hadidi, A.; Zakey, A.

2014-12-01

Aerosols are indicators of air quality as they reduce visibility and adversely affect public health. Aerosol optical depth (AOD) is a measure of the radiation extinction due to interaction of radiation with aerosol particles in the atmosphere. Using this optical measure of atmospheric aerosols we explore the seasonal and annual patterns of aerosols from both anthropogenic and biogenic sources over Egypt. Here, we use an integrated environment-climate-aerosol model in conjunction with inversion technique to identify the aerosol particle size distribution over different locations in Egypt. The online-integrated Environment-Climate-Aerosol model (EnvClimA), which is based on the International Center for Theoretical Physics Regional Climate Model (ICTP-RegCM), is used to study the emission of different aerosols and their impact on climate parameters for a long-term base line simulation run over Egypt and North Africa. The global emission inventory is downscaled and remapping them over Egypt using local factors such as population, traffic and industrial activities to identify the sources of anthropogenic and biogenic emission from local emission over Egypt. The results indicated that the dominant natural aerosols over Egypt are dust emissions that frequently occur during the transitional seasons (Spring and Autumn). From the local observation we identify the number of dust and sand storm occurrences over Egypt. The Multiangle Imaging SpectroRadiometer (MISR) is used to identify the optical characterizations of different types of aerosols over Egypt. Modeled aerosol optical depth and MISR observed (at 555 nm) are compared from March 2000 through November 2013. The results identify that the MISR AOD captures the maximum peaks of AOD in March/April that coincide with the Khamasin dust storms. However, peaks in May are either due to photochemical reactions or anthropogenic activities. Note: This presentation is for a Partnerships for Enhanced Engagement in Research (PEER

Aerosol Properties and Radiative Forcing over Kanpur during Severe Aerosol Loading Conditions

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

Kaskaoutis, D. G.; Sinha, P. R.; Vinoj, V.

2013-11-01

Atmospheric aerosols over India exhibit large spatio-temporal fluctuation driven by the local monsoon system, emission rates and seasonally-changed air masses. The northern part of India is well-known for its high aerosol loading throughout the year due to anthropogenic emissions, dust influence and biomass burning. On certain circumstances and, under favorable weather conditions, the aerosol load can be severe, causing significant health concerns and climate implications. The present work analyzes the aerosol episode (AE) days and examines the modification in aerosol properties and radiative forcing during the period 2001-2010 based on Kanpur-AERONET sun photometer data. As AEs are considered the daysmore » having daily-mean aerosol optical depth (AOD) above the decadal mean + 1 STD (standard deviation); the threshold value is defined at 0.928. The results identify 277 out of 2095 days (13.2%) of AEs over Kanpur, which are most frequently observed during post-monsoon (78 cases, 18.6%) and monsoon (76, 14.7%) seasons due to biomass-burning episodes and dust influence, respectively. On the other hand, the AEs in winter and pre-monsoon are lower in both absolute and percentage values (65, 12.5% and 58, 9.1%, respectively). The modification in aerosol properties on the AE days is strongly related to season. Thus, in post-monsoon and winter the AEs are associated with enhanced presence of fine-mode aerosols and Black Carbon from anthropogenic pollution and any kind of burning, while in pre-monsoon and monsoon seasons they are mostly associated with transported dust. Aerosol radiative forcing (ARF) calculated using SBDART shows much more surface (~-69 to -97 Wm-2) and Top of Atmosphere cooling (-20 to -30 Wm-2) as well as atmospheric heating (~43 to 71 Wm-2) during the AE days compared to seasonal means. These forcing values are mainly controlled by the higher AODs and the modified aerosol characteristics (Angstrom α, SSA) during the AE days in each season and may

Production-based emissions, consumption-based emissions and consumption-based health impacts of PM2.5 carbonaceous aerosols in Asia

NASA Astrophysics Data System (ADS)

Takahashi, Kei; Nansai, Keisuke; Tohno, Susumu; Nishizawa, Masato; Kurokawa, Jun-ichi; Ohara, Toshimasa

2014-11-01

This study determined the production-based emissions, the consumption-based emissions, and the consumption-based health impact of primary carbonaceous aerosols (black carbon: BC, organic carbon: OC) in nine countries and regions in Asia (Indonesia, Malaysia, the Philippines, Singapore, Thailand, China, Taiwan, South Korea, and Japan) in 2008. For the production-based emissions, sectoral emissions inventory of BC and OC for the year of 2008 based on the Asian international input-output tables (AIIOT) was compiled including direct emissions from households. Then, a multiregional environmental input-output analysis with the 2008 AIIOT which was originally developed by updating the table of 2000 was applied for calculating the consumption-based emissions for each country and region. For the production-based emissions, China had the highest BC and OC emissions of 4520 Gg-C in total, which accounted for 75% of the total emissions in the nine countries and regions. For consumption-based emissions, China was estimated to have had a total of 4849 Gg-C of BC and OC emissions, which accounted for 77% of the total emissions in the Asia studied. We also quantified how much countries and regions induced emissions in other countries and regions. Furthermore, taking account of the source-receptor relationships of BC and OC among the countries and regions, we converted their consumption-based emissions into the consumption-based health impact of each country and region. China showed the highest consumption-based health impact of BC and OC totaling 111 × 103 premature deaths, followed by Indonesia, Japan, Thailand and South Korea. China accounted for 87% of the sum total of the consumption-based health impacts of the countries/regions, indicating that China's contribution to consumption-based health impact in Asia was greater than its consumption-based emissions. By elucidating the health impacts that each country and region had on other countries and from which country the impacts

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

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

Characterizing the Sources and Processing of Submicron Aerosols at a Coastal Site near Houston, TX, with a Specific Focus on the Impact of Regional Shipping Emissions

NASA Astrophysics Data System (ADS)

Schulze, B.; Wallace, H. W., IV; Bui, A.; Flynn, J. H., III; Erickson, M. H.; Griffin, R. J.

2017-12-01

The Texas Gulf Coast region historically has been influenced heavily by regional shipping emissions. However, the effects of the recent establishment of the North American Emissions Control Area (ECA) on aerosol properties in this region are presently unknown. In order to understand better the current sources and processing mechanisms influencing coastal aerosol near Houston, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed for three weeks at a coastal location during May-June 2016. Total mass loadings of organic and inorganic non-refractory aerosol components during onshore flow periods were similar to those published before establishment of the regulations. Using estimated methanesulfonic acid (MSA) mass loadings and published biogenic MSA:non-sea-salt-sulfate (nss-SO4) ratios, we determined that over 70% of nss-SO4 over the Gulf was from anthropogenic sources, predominantly shipping emissions. Mass spectral analysis indicated that for periods with similar backward-trajectory-averaged meteorological conditions, air masses influenced by shipping emissions have an increased mass fraction of ions related to carboxylic acids and a significantly larger oxygen-to-carbon (O:C) ratio than air masses that stay within the ECA boundary, suggesting that shipping emissions impact marine organic aerosol (OA) oxidation state. Amine fragment mass loadings were positively correlated with anthropogenic nss-SO4 during onshore flow, implying anthropogenic-biogenic interaction in marine OA production. Five OA factors were resolved by positive matrix factorization, corresponding to a hydrocarbon-like OA, a semi-volatile OA, and three different oxygenated organic aerosols ranked by their O:C ratio (OOA-1, OOA-2, and OOA-3). OOA-1 constituted the majority of OA mass during a period likely influenced by aqueous-phase processing and may be linked to local glyoxal/methylglyoxal-related sources. OOA-2 was produced within the Houston urban region and was

Dust-wind interactions can intensify aerosol pollution over eastern China.

PubMed

Yang, Yang; Russell, Lynn M; Lou, Sijia; Liao, Hong; Guo, Jianping; Liu, Ying; Singh, Balwinder; Ghan, Steven J

2017-05-11

Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with unusual meteorological conditions, including weaker wind speeds. Here we show, based on model simulations, that during years with decreased wind speed, large decreases in dust emissions (29%) moderate the wintertime land-sea surface air temperature difference and further decrease winds by -0.06 (±0.05) m s -1 averaged over eastern China. The dust-induced lower winds enhance stagnation of air and account for about 13% of increasing aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime aerosol concentrations, with important implications that need to be taken into account by air quality studies.

Dust-wind interactions can intensify aerosol pollution over eastern China

PubMed Central

Yang, Yang; Russell, Lynn M.; Lou, Sijia; Liao, Hong; Guo, Jianping; Liu, Ying; Singh, Balwinder; Ghan, Steven J.

2017-01-01

Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with unusual meteorological conditions, including weaker wind speeds. Here we show, based on model simulations, that during years with decreased wind speed, large decreases in dust emissions (29%) moderate the wintertime land–sea surface air temperature difference and further decrease winds by −0.06 (±0.05) m s−1 averaged over eastern China. The dust-induced lower winds enhance stagnation of air and account for about 13% of increasing aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime aerosol concentrations, with important implications that need to be taken into account by air quality studies. PMID:28492276

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

Influences of natural emission sources (wildfires and Saharan dust) on the urban organic aerosol in Barcelona (Western Mediterranean Basis) during a PM event.

PubMed

van Drooge, Barend L; Lopez, Jordi F; Grimalt, Joan O

2012-11-01

The urban air quality in Barcelona in the Western Mediterranean Basin is characterized by overall high particulate matter (PM) concentrations, due to intensive local anthropogenic emissions and specific meteorological conditions. Moreover, on several days, especially in summer, natural PM sources, such as long-range transported Saharan dust from Northern Africa or wildfires on the Iberian Peninsula and around the Mediterranean Basin, may influence the levels and composition of the organic aerosol. In the second half of July 2009, daily collected PM(10) filter samples in an urban background site in Barcelona were analyzed on organic tracer compounds representing several emission sources. During this period, an important PM peak event was observed. Individual organic compound concentrations increased two to five times during this event. Although highest increase was observed for the organic tracer of biomass burning, the contribution to the organic aerosol was estimated to be around 6 %. Organic tracers that could be related to Saharan dust showed no correlation with the PM and OC levels, while this was the case for those related to fossil fuel combustion from traffic emissions. Moreover, a change in the meteorological conditions gave way to an overall increase of the urban background contamination. Long-range atmospheric transport of organic compounds from primary emissions sources (i.e., wildfires and Saharan dust) has a relatively moderate impact on the organic aerosol in an urban area where the local emissions are dominating.

Delay in convection in nocturnal boundary layer due to aerosol-induced cooling

NASA Astrophysics Data System (ADS)

Singh, Dhiraj Kumar; Ponnulakshmi, V. K.; Subramanian, G.; Sreenivas, K. R.

2012-11-01

Heat transfer processes in the nocturnal boundary layer (NBL) influence the surface energy budget, and play an important role in many micro-meteorological processes including the formation of inversion layers, radiation fog, and in the control of air-quality near the ground. Under calm clear-sky conditions, radiation dominates over other transport processes, and as a result, the air layers just above ground cool the fastest after sunset. This leads to an anomalous post-sunset temperature profile characterized by a minimum a few decimeters above ground (Lifted temperature minimum). We have designed a laboratory experimental setup to simulate LTM, involving an enclosed layer of ambient air, and wherein the boundary condition for radiation is decoupled from those for conduction and convection. The results from experiments involving both ambient and filtered air indicate that the high cooling rates observed are due to the presence of aerosols. Calculated Rayleigh number of LTM-type profiles is of the order 105-107 in the field and of order 103-105 in the laboratory. In the LTM region, there is convective motion when the Rayleigh number is greater than 104 rather than the critical Rayleigh number (Rac = 1709). The diameter of convection rolls is a function of height of minimum of LTM-type profiles. The results obtained should help in the parameterization of transport process in the nocturnal boundary layer, and highlight the need to accounting the effects of aerosols and ground emissivity in climate models.

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.

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

An increase in aerosol burden due to the land-sea warming contrast

NASA Astrophysics Data System (ADS)

Hassan, T.; Allen, R.; Randles, C. A.

2017-12-01

Climate models simulate an increase in most aerosol species in response to warming, particularly over the tropics and Northern Hemisphere midlatitudes. This increase in aerosol burden is related to a decrease in wet removal, primarily due to reduced large-scale precipitation. Here, we show that the increase in aerosol burden, and the decrease in large-scale precipitation, is related to a robust climate change phenomenon—the land/sea warming contrast. Idealized simulations with two state of the art climate models, the National Center for Atmospheric Research Community Atmosphere Model version 5 (NCAR CAM5) and the Geophysical Fluid Dynamics Laboratory Atmospheric Model 3 (GFDL AM3), show that muting the land-sea warming contrast negates the increase in aerosol burden under warming. This is related to smaller decreases in near-surface relative humidity over land, and in turn, smaller decreases in large-scale precipitation over land—especially in the NH midlatitudes. Furthermore, additional idealized simulations with an enhanced land/sea warming contrast lead to the opposite result—larger decreases in relative humidity over land, larger decreases in large-scale precipitation, and larger increases in aerosol burden. Our results, which relate the increase in aerosol burden to the robust climate projection of enhanced land warming, adds confidence that a warmer world will be associated with a larger aerosol burden.

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.

Local and remote impacts of aerosol species on Indian summer monsoon rainfall in a GCM

NASA Astrophysics Data System (ADS)

Turner, A. G.; Guo, L.; Highwood, E.

2016-12-01

The HadGEM2 AGCM is used to determine the most important anthropogenic aerosols in the Indian monsoon using experiments in which observed trends in individual aerosol species are imposed. Sulphur dioxide (SD) emissions are shown to impact rainfall more strongly than black carbon (BC) aerosols, causing reduced rainfall especially over northern India. Significant perturbations due to BC are not noted until its emissions are scaled up in a sensitivity test, resulting in rainfall increases over northern India due to the Elevated Heat Pump mechanism, enhancing convection during the premonsoon and bringing forward the monsoon onset. Secondly, the impact of anthropogenic aerosols is compared to that of increasing greenhouse-gas concentrations and observed sea-surface temperature (SST) warming. The tropospheric temperature gradient driving the monsoon shows weakening when forced by either SD or imposed SST trends. However the observed SST trend is dominated by warming in the deep tropics; when the component of SST trend related to aerosol emissions is removed, further warming is found in the extratropical northern hemisphere that tends to offset monsoon weakening. This suggests caution is needed when using SST forcing as a proxy for greenhouse warming. Finally, aerosol emissions are decomposed into those from the Indian region and those elsewhere, in pairs of experiments with SD and BC. Both local and remote aerosol emissions are found to lead to rainfall changes over India; for SD, remote aerosols contribute around 75% of the rainfall decrease over India, while for BC the remote forcing is even more dominant.

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

Aerosol Optical Properties and Trace Gas Emissions From Laboratory-Simulated Western US Wildfires

NASA Astrophysics Data System (ADS)

Selimovic, V.; Yokelson, R. J.; Warneke, C.; Roberts, J. M.; De Gouw, J. A.; Reardon, J.; Griffith, D. W. T.

2017-12-01

Western wildfires have a major impact on air quality in the US. In the fall of 2016, 107 fires were burned in the large-scale combustion facility at the US Forest Service Missoula Fire Sciences Laboratory as part of the Fire Influence on Regional and Global Environments Experiment (FIREX). Canopy, litter, duff, dead wood, and other fuels from various widespread coniferous and chaparral ecosystems were burned in combinations to represent relevant configurations in the field and as pure components to investigate the effects of individual fuels. The smoke emissions were characterized by a large suite of state-of-the-art instruments. In this study we report emission factor (EF, g compound emitted per kg fuel burned) measurements in fresh smoke of a diverse suite of critically-important trace gases measured by open-path Fourier transform infrared spectroscopy (OP-FTIR). We also report aerosol optical properties (absorption EF, single scattering albedo (SSA) and Ångström absorption exponent (AAE)) as well as black carbon (BC) EF measured by photoacoustic extinctiometers (PAX) at 870 and 401 nm. A careful comparison with available field measurements of wildfires confirms that representative data can be extracted from the lab fire data. The OP-FTIR data show that ammonia (1.65 g kg-1), acetic acid (2.44 g kg-1), and other trace gases are significant emissions not previously measured for US wildfires. The PAX measurements show that brown carbon (BrC) absorption is most dominant for combustion of duff (AAE 7.13) and rotten wood (AAE 4.60): fuels that are consumed in greater amounts during wildfires than prescribed fires. We confirm that about 86% of the aerosol absorption at 401 nm in typical fresh wildfire smoke is due to BrC.

Aerosol contribution to the rapid warming of near-term climate under RCP 2.6

NASA Astrophysics Data System (ADS)

Chalmers, N.; Highwood, E. J.; Hawkins, E.; Sutton, R.; Wilcox, L. J.

2012-09-01

The importance of aerosol emissions for near term climate projections is investigated by analysing simulations with the HadGEM2-ES model under two different emissions scenarios: RCP2.6 and RCP4.5. It is shown that the near term warming projected under RCP2.6 is greater than under RCP4.5, even though the greenhouse gas forcing is lower. Rapid and substantial reductions in sulphate aerosol emissions due to a reduction of coal burning in RCP2.6 lead to a reduction in the negative shortwave forcing due to aerosol direct and indirect effects. Indirect effects play an important role over the northern hemisphere oceans, especially the subtropical northeastern Pacific where an anomaly of 5-10 Wm-2 develops. The pattern of surface temperature change is consistent with the expected response to this surface radiation anomaly, whilst also exhibiting features that reflect redistribution of energy, and feedbacks, within the climate system. These results demonstrate the importance of aerosol emissions as a key source of uncertainty in near term projections of global and regional climate.

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

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

Factors Affecting Aerosol Radiative Forcing from Both Production-based and Consumption-based View

NASA Astrophysics Data System (ADS)

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

2017-12-01

Aerosol radiative forcing (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. This problem becomes more complicated when taking into account the role of international trade, which means reallocated aerosol RF due to separation of regions producing goods and emissions and regions consuming those goods. Here we analyze major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA) and black carbon (BC), extending the work of Lin et al. (2016, Nature Geoscience). We contrast five factors determining production-based (RFp, due to a region's production of goods) and consumption-based (RFc, due to a region's consumption) forcing by 11 major regions, including population size, per capita output, emission intensity (emission per output), chemical efficiency (mass per unit emission) and radiative efficiency (RF per unit mass). Comparing across the 11 regions, East Asia produces the strongest RFp and RFc of SIOA and BC and the second largest RFp and RFc of POA primarily due to its high emission intensity. Although Middle East and North Africa has low emissions, its RFp is strengthened by its largest chemical efficiency for POA and BC and second largest chemical efficiency for SIOA. However, RFp of South-East Asia and Pacific is greatly weakened by its lowest chemical efficiency. Economic trade means that net importers (Western Europe, North America and Pacific OECD) have higher RFc than RFp by 50-100%. And such forcing difference is mainly due to the high emission intensity of the exporters supplying these regions. For North America, SIOA's RFc is 50% stronger than RFp, for that emission intensity of SIOA is 5.2 times in East Asia and 2.5 times in Latin America and Caribbean compared with that in North America, and the chemical efficiency in the top four exporters are

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.

A Study of Direct and Cloud-Mediated Radiative Forcing of Climate Due to Aerosols

NASA Technical Reports Server (NTRS)

Yu, Shao-Cai

1999-01-01

The Intergovernmental Panel on Climate Change (IPCC) has reported that in the southeastern US and eastern China, the general greenhouse warming due to anthropogenic gaseous emissions is dominated by the cooling effect of anthropogenic aerosols. To verify this model prediction in eastern China and southeastern US, we analyzed regional patterns of climate changes at 72 stations in eastern China during 1951- 94 (44 years), and at 52 stations in the southeastern US during 1949-94 (46 years) to detect the fingerprint of aerosol radiative forcing. It was found that the mean rates of change of annual mean daily, maximum, minimum temperatures and diurnal temperature range (DTR) in eastern China were 0.8, -0.2, 1.8, and -2.0 C/100 years respectively, while the mean rates of change of annual mean daily, maximum, minimum temperatures and DTR in the southeastern US were -0.2, -0.6, 0.2, and -0.8 C/100 years, respectively. This indicates that the high rate of increase in annual mean minimum temperature in eastern China results in a slightly warming trend of daily temperature, while the high rate of decrease in annual mean maximum temperature and low rate of increase in annual mean minimum temperature lead to the cooling trend of daily temperature in the southeastern US. We found that the warming from the longwave forcing due to both greenhouse gases and aerosols was completely counteracted by the shortwave aerosol forcing in the southeastern US in the past 46 years. A slightly overall warming trend in eastern China is evident; winters have become milder. This finding is explained by hypothesizing that increasing energy usage during the past 44 years has resulted in more coal and biomass burning, thus increasing the emission of absorbing soot and organic aerosols in eastern China. Such emissions, in addition to well-known Asia dust and greenhouse gases, may be responsible for the winter warming trend in eastern China that we have reported here. The sensitivity of aerosol

Estimation of global anthropogenic dust aerosol using CALIOP satellite

NASA Astrophysics Data System (ADS)

Chen, B.; Huang, J.; Liu, J.

2014-12-01

Anthropogenic dust aerosols are those produced by human activity, which mainly come from cropland, pasture, and urban in this paper. Because understanding of the emissions of anthropogenic dust is still very limited, a new technique for separating anthropogenic dust from natural dustusing CALIPSO dust and planetary boundary layer height retrievalsalong with a land use dataset is introduced. Using this technique, the global distribution of dust is analyzed and the relative contribution of anthropogenic and natural dust sources to regional and global emissions are estimated. Local anthropogenic dust aerosol due to human activity, such as agriculture, industrial activity, transportation, and overgrazing, accounts for about 22.3% of the global continentaldust load. Of these anthropogenic dust aerosols, more than 52.5% come from semi-arid and semi-wet regions. On the whole, anthropogenic dust emissions from East China and India are higher than other regions.

Climatological simulations of ozone and atmospheric aerosols in the Greater Cairo region

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

Steiner, A. L.; Tawfik, A. B.; Shalaby, A.

An integrated chemistry-climate model (RegCM4-CHEM) simulates present-day climate, ozone and tropospheric aerosols over Egypt with a focus on Greater Cairo (GC) region. The densley populated GC region is known for its severe air quality issues driven by high levels of anthropogenic pollution in conjuction with natural sources such as dust and agricultural burning events. We find that current global emission inventories underestimate key pollutants such as nitrogen oxides and anthropogenic aerosol species. In the GC region, average-ground-based NO2 observations of 40-60 ppb are substantially higher than modeled estimates (5-10 ppb), likely due to model grid resolution, improper boundary layer representation,more » and poor emissions inventories. Observed ozone concentrations range from 35 ppb (winter) to 80 ppb (summer). The model reproduces the seasonal cycle fairly well, but modeled summer ozone is understimated by approximately 15 ppb and exhibits little interannual variability. For aerosols, springtime dust events dominate the seasonal aerosol cycle. The chemistry-climate model captures the springtime peak aerosol optical depth (AOD) of 0.7-1 but is slightly greater than satellite-derived AOD. Observed AOD decreases in the summer and increases again in the fall due to agricultural burning events in the Nile Delta, yet the model underestimates this fall observed AOD peak, as standard emissions inventories underestimate this burning and the resulting aerosol emissions. Our comparison of modeled gas and particulate phase atmospheric chemistry in the GC region indicates that improved emissions inventories of mobile sources and other anthropogenic activities are needed to improve air quality simulations in this region.« less

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.

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.

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.

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...

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

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.

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...

Atmospheric heating due to black carbon aerosol during the summer monsoon period over Ballia: A rural environment over Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Tiwari, S.; Dumka, U. C.; Hopke, P. K.; Tunved, P.; Srivastava, A. K.; Bisht, D. S.; Chakrabarty, R. K.

2016-09-01

Black carbon (BC) aerosols are one of the most uncertain drivers of global climate change. The prevailing view is that BC mass concentrations are low in rural areas where industrialization and vehicular emissions are at a minimum. As part of a national research program called the "Ganga Basin Ground Based Experiment-2014 under the Cloud Aerosol Interaction and Precipitation Enhancement Experiment (CAIPEEX) Phase-III" of Ministry of Earth Sciences, Government of India, the continuous measurements of BC and particulate matter (PM) mass concentrations, were conducted in a rural environment in the highly-polluted Indo-Gangetic Plain region during 16th June to 15th August (monsoon period), 2014. The mean mass concentration of BC was 4.03 (± 0.85) μg m- 3 with a daily variability between 2.4 and 5.64 μg m- 3, however, the mean mass PM concentrations [near ultrafine (PM1.0), fine (PM2.5) and inhalable (PM10)] were 29.1(± 16.2), 34.7 (± 19.9) and 43.7 (± 28.3) μg m- 3, respectively. The contribution of BC in PM1.0 was approximately 13%, which is one of the highest being recorded. Diurnally, the BC mass concentrations were highest (mean: 5.89 μg m- 3) between 20:00 to 22:00 local time (LT) due to the burning of biofuels/biomass such as wood, dung, straw and crop residue mixed with dung by the local residents for cooking purposes. The atmospheric direct radiative forcing values due to the composite and BC aerosols were determined to be + 78.3, + 44.9, and + 45.0 W m- 2 and + 42.2, + 35.4 and + 34.3 W m- 2 during the months of June, July and August, respectively. The corresponding atmospheric heating rates (AHR) for composite and BC aerosols were 2.21, 1.26 and 1.26; and 1.19, 0.99 and 0.96 K day- 1 for the month of June, July and August, respectively, with a mean of 1.57 and 1.05 K day- 1 which was 33% lower AHR (BC) than for the composite particles during the study period. This high AHR underscores the importance of absorbing aerosols such as BC contributed by

Improving Aerosol Simulation over South Asia for Climate and Air Quality Studies

NASA Technical Reports Server (NTRS)

Pan, Xiaohua; Chin, Mian; Bian, Huisheng; Gautam, Ritesh

2014-01-01

Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, the water cycle, and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions found there. However, it has been proved quite challenging to adequately represent the aerosol spatial distribution and magnitude over this critical region in global models (Pan et al. 2014), with the surface concentrations, aerosol optical depth (AOD), and absorbing AOD (AAOD) significantly underestimated, especially in October-January when the agricultural waste burning and anthropogenic aerosol dominate over dust aerosol. In this study, we aim to investigate the causes for such discrepancy in winter by conducting sets of model experiments with NASA's GEOS-5 in terms of (1) spatial resolution, (2) emission amount, and (3) meteorological fields.

Climate and mortality changes due to reductions in household cooking emissions

NASA Astrophysics Data System (ADS)

Bergman, Tommi; Mielonen, Tero; Arola, Antti; Kokkola, Harri

2016-04-01

Household cooking is a significant cause for health and environmental problems in the developing countries. There are more than 3 billion people who use biomass for fuel in cooking stoves in their daily life. These cooking stoves use inadequate ventilation and expose especially women and children to indoor smoke. To reduce problems of the biomass burning, India launched an initiative to provide affordable and clean energy solutions for the poorest households by providing clean next-generation cooking stoves. The improved cooking stoves are expected to improve outdoor air quality and to reduce the climate-active pollutants, thus simultaneously slowing the climate change. Previous research has shown that the emissions of black carbon can be decreased substantially, as much as 90 % by applying better technology in cooking stoves. We have implemented reasonable (50% decrease) and best case (90% decrease) scenarios of the reductions in black and organic carbon due to improved cooking stoves in India into ECHAM-HAMMOZ aerosol-climate model. The global simulations of the scenarios will be used to study how the reductions of emissions in India affect the pollutant concentrations and radiation. The simulated reductions in particulate concentrations will also be used to estimate the decrease in mortality rates. Furthermore, we will study how the emission reductions would affect the global climate and mortality if a similar initiative would be applied in other developing countries.

Radiative Effects of Aerosol in the Marine Environment: Tales from the Two-Column Aerosol Project

NASA Astrophysics Data System (ADS)

Berg, L. K.; Fast, J. D.; Barnard, J.; Chand, D.; Chapman, E. G.; Comstock, J. M.; Ferrare, R. A.; Flynn, C. J.; Hair, J. W.; Hostetler, C. A.; Hubbe, J.; Johnson, R.; Kassianov, E.; Kluzek, C.; Laskin, A.; Lee, Y.; Mei, F.; Michalsky, J. J.; Redemann, J.; Rogers, R. R.; Russell, P. B.; Sedlacek, A. J.; Schmid, B.; Shilling, J. E.; Shinozuka, Y.; Springston, S. R.; Tomlinson, J. M.; Wilson, J. M.; Zelenyuk, A.; Berkowitz, C. M.

2013-12-01

There is still uncertainty associated with the direct radiative forcing by atmospheric aerosol and its representation in atmospheric models. This is particularly true in marine environments near the coast where the aerosol loading is a function of both naturally occurring and anthropogenic aerosol. These regions are also subject to variable synoptic and thermally driven flows (land-sea breezes) that transport aerosol between the continental and marine environments. The situation is made more complicated due to seasonal changes in aerosol emissions. Given these differences in emissions, we expect significant differences in the aerosol intensive and extensive properties between summer and winter and data is needed to evaluate models over the wide range of conditions. To address this issue, the recently completed Two Column Aerosol Project (TCAP) was designed to measure the key aerosol parameters in two atmospheric columns, one located over Cape Cod, Massachusetts and another approximately 200 km from the coast over the Atlantic Ocean. Measurements included aerosol size distribution, chemical composition, optical properties and vertical distribution. Several aspects make TCAP unique, including the year-long deployment of a suite of surface-based instruments by the US Department of Energy's Atmospheric Radiation Measurement (ARM) Climate Research Facility and two aircraft intensive operations periods supported by the ARM Airborne Facility, one conducted in July 2012 and a second in February 2013. The presentation will include a discussion of the impact of the aerosol optical properties and their uncertainty on simulations of the radiation budget within the TCAP domain in the context of both single column and regional scale models. Data from TCAP will be used to highlight a number of important factors, including diurnal variation in aerosol optical depth measured at the surface site, systematic changes in aerosol optical properties (including scattering, absorption, and

Comparison of two different dust emission mechanisms over the Horqin Sandy Land area: Aerosols contribution and size distributions

NASA Astrophysics Data System (ADS)

Ju, Tingting; Li, Xiaolan; Zhang, Hongsheng; Cai, Xuhui; Song, Yu

2018-03-01

Dust aerosols (PM10) emission fluxes due to convective turbulent dust emissions (CTDE) and saltation-bombardment and/or aggregation-disintegration dust emissions (SADE) events were comparatively studied using the data obtained from the Naiman station over the Horqin Sandy Land area in Inner Mongolia, China from 2011 to 2015. The annual cumulative dust fluxes released by CTDE events was about one third of that by SADE events, with the order of 103∼104 μg m-2 s-1. The particle size distributions (PSDs) with diameter between 0.1 and 20 μm during CTDE and SADE events over the Horqin Sandy Land area were simulated based on the fragmentation theory, respectively. The results indicated that an improved equation based on fragmentation theory could be applied to describe the PSDs over the Horqin site which may be because the scale-invariant fragmentation theory mainly explains the PSDs of free dust particles on the surface, which differ from the PSDs of suspend airborne dust and the improved equation was more applicable to the PSDs of SADE events because the dust emission mechanism of SADE are saltation bombardment and aggregation disintegration. The number-related mean aerosol diameters (DN) barely varied under different friction velocity (u*) for SADE events, while the volume-related mean aerosol diameters (DV) changed distinctly with the change of u*. For CTDE events, the DN and DV had no obvious relationship with the change of u* because the dominating influence factor during CTDE event was thermal convection rather than u*. The mass-related PSDs usually exhibited a peak between 0.45 and 0.70 μm during SADE events, while for CTDE events there was a wide peak in the range of 0.10 0.70 μm. The results suggest that DN should be not be recommended as an individual parameter to describe the PSDs. The mass-related PSDs can effectively distinguish the SADE and CTDE events.

Atmospheric Dispersion of Sodium Aerosol due to a Sodium Leak in a Fast Breeder Reactor Complex

NASA Astrophysics Data System (ADS)

Punitha, G.; Sudha, A. Jasmin; Kasinathan, N.; Rajan, M.

Liquid sodium at high temperatures (470 K to 825 K) is used as the primary and secondary coolant in Liquid Metal cooled Fast Breeder Reactors (LMFBR). In the event of a postulated sodium leak in the Steam Generator Building (SGB) of a LMFBR, sodium readily combusts in the ambient air, especially at temperatures above 523 K. Intense sodium fire results and sodium oxide fumes are released as sodium aerosols. Sodium oxides are readily converted to sodium hydroxide in air due to the presence of moisture in it. Hence, sodium aerosols are invariably in the form of particulate sodium hydroxide. These aerosols damage not only the equipment and instruments due to their corrosive nature but also pose health hazard to humans. Hence, it is essential to estimate the concentration of sodium aerosols within the plant boundary for a sodium leak event. The Gaussian Plume Dispersion Model can obtain the atmospheric dispersion of sodium aerosols in an open terrain. However, this model does not give accurate results for dispersion in spaces close to the point of release and with buildings in between. The velocity field due to the wind is altered to a large extent by the intervening buildings and structures. Therefore, a detailed 3-D estimation of the velocity field and concentration has to be obtained through rigorous computational fluid dynamics (CFD) approach. PHOENICS code has been employed to determine concentration of sodium aerosols at various distances from the point of release. The dispersion studies have been carried out for the release of sodium aerosols at different elevations from the ground and for different wind directions.

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

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,...

Proton-Induced X-Ray Emission Analysis of Crematorium Emissions

NASA Astrophysics Data System (ADS)

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

2014-09-01

There has been considerable debate in recent years about possible mercury emissions from crematoria due to amalgam tooth restorations. We have performed a proton-induced X-ray emission (PIXE) analysis of aerosol and soil samples taken near the Vale Cemetery Crematorium in Schenectady, NY, to address this concern. The aerosol samples were collected on the roof of the crematorium using a nine-stage, cascade impactor that separates the particulate matter by aerodynamic diameter and deposits it onto thin Kapton foils. The soil samples were collected at several different distances from the crematorium and compressed into pellets with a hydraulic press. The Kapton foils containing the aerosol samples and the soil pellets were bombarded with 2.2-MeV protons from the 1.1-MV tandem Pelletron accelerator in the Union College Ion-Beam Analysis Laboratory. We measured significant concentrations of sulfur, phosphorus, potassium, calcium, and iron, but essentially no mercury in the aerosol samples. The lower limit of detection for airborne mercury in this experiment was approximately 0.2 ng / m3. The PIXE analysis of the soil samples showed the presence of elements commonly found in soil (Si, K, Ca, Ti, Mn, Fe), but no trace of mercury. There has been considerable debate in recent years about possible mercury emissions from crematoria due to amalgam tooth restorations. We have performed a proton-induced X-ray emission (PIXE) analysis of aerosol and soil samples taken near the Vale Cemetery Crematorium in Schenectady, NY, to address this concern. The aerosol samples were collected on the roof of the crematorium using a nine-stage, cascade impactor that separates the particulate matter by aerodynamic diameter and deposits it onto thin Kapton foils. The soil samples were collected at several different distances from the crematorium and compressed into pellets with a hydraulic press. The Kapton foils containing the aerosol samples and the soil pellets were bombarded with 2.2-Me

Climatic effects of biogenic volatile organic compounds (BVOCs) emissions and associated feedbacks due to vegetation change in the boreal zone

NASA Astrophysics Data System (ADS)

Blichner, Sara Marie; Koren Berntsen, Terje; Stordal, Frode

2017-04-01

As our understanding of the earth system improves, it is becoming increasingly clear that vegetation and ecosystems are not only influenced by the atmosphere, but that changes in these also feed back to the atmosphere and induce changes here. One such feedback involves the emission of biogenic volatile organic compounds (BVOCs) emitted from vegetation. As BVOCs are oxidized, they become less volatile and contribute to aerosol growth and formation in the atmosphere, and can thus change the radiative balance of the atmosphere through both the direct and indirect aerosol effects. The amount and type of BVOCs emitted by vegetation depends on a myriad of variables; temperature, leaf area index (LAI), species, water availability and various types of stress (e.g. insects attacks). They generally increase with higher temperatures and under stress. These factors beg the question of how emissions will change in the future in response to both temperature increase and changes to vegetation patterns and densities. The boreal region is of particular interest because forest cover in general has been thought to have a warming effect due to trees reducing the albedo, especially when snow covers the ground. We investigate feedbacks through BVOC emissions related to the expected northward expansion of boreal forests in response to global warming with a development version of the Norwegian Earth System Model (NorESM). BVOC emissions are computed by the Model of Emissions of Gases and Aerosols from Nature 2.1 (MEGAN2.1) which is incorporated into the Community Land Model v4.5 (CLM4.5). The atmospheric component is CAM5.3-Oslo. We will present preliminary results of effects on clouds and aerosol concentrations resulting from a fixed poleward shift in boreal forests and compare the radiative effects of this to changes in surface energy fluxes. CO2-concentrations and sea surface temperatures are kept fixed in order to isolate the effects of the change in vegetation patterns. Finally

Causes and consequences of decreasing atmospheric organic aerosol in the United States.

PubMed

Ridley, D A; Heald, C L; Ridley, K J; Kroll, J H

2018-01-09

Exposure to atmospheric particulate matter (PM) exacerbates respiratory and cardiovascular conditions and is a leading source of premature mortality globally. Organic aerosol contributes a significant fraction of PM in the United States. Here, using surface observations between 1990 and 2012, we show that organic carbon has declined dramatically across the entire United States by 25-50%; accounting for more than 30% of the US-wide decline in PM. The decline is in contrast with the increasing organic aerosol due to wildfires and no clear trend in biogenic emissions. By developing a carbonaceous emissions database for the United States, we show that at least two-thirds of the decline in organic aerosol can be explained by changes in anthropogenic emissions, primarily from vehicle emissions and residential fuel burning. We estimate that the decrease in anthropogenic organic aerosol is responsible for averting 180,000 (117,000-389,000) premature deaths between 1990 and 2012. The unexpected decrease in organic aerosol, likely a consequence of the implementation of Clean Air Act Amendments, results in 84,000 (30,000-164,000) more lives saved than anticipated by the EPA between 2000 and 2010.

Causes and consequences of decreasing atmospheric organic aerosol in the United States

NASA Astrophysics Data System (ADS)

Ridley, D. A.; Heald, C. L.; Ridley, K. J.; Kroll, J. H.

2018-01-01

Exposure to atmospheric particulate matter (PM) exacerbates respiratory and cardiovascular conditions and is a leading source of premature mortality globally. Organic aerosol contributes a significant fraction of PM in the United States. Here, using surface observations between 1990 and 2012, we show that organic carbon has declined dramatically across the entire United States by 25–50%; accounting for more than 30% of the US-wide decline in PM. The decline is in contrast with the increasing organic aerosol due to wildfires and no clear trend in biogenic emissions. By developing a carbonaceous emissions database for the United States, we show that at least two-thirds of the decline in organic aerosol can be explained by changes in anthropogenic emissions, primarily from vehicle emissions and residential fuel burning. We estimate that the decrease in anthropogenic organic aerosol is responsible for averting 180,000 (117,000–389,000) premature deaths between 1990 and 2012. The unexpected decrease in organic aerosol, likely a consequence of the implementation of Clean Air Act Amendments, results in 84,000 (30,000–164,000) more lives saved than anticipated by the EPA between 2000 and 2010.

Landscape fires dominate terrestrial natural aerosol - climate feedbacks

NASA Astrophysics Data System (ADS)

Scott, C.; Arnold, S.; Monks, S. A.; Asmi, A.; Paasonen, P.; Spracklen, D. V.

2017-12-01

The terrestrial biosphere is an important source of natural aerosol including landscape fire emissions and secondary organic aerosol (SOA) formed from biogenic volatile organic compounds (BVOCs). Atmospheric aerosol alters the Earth's climate by absorbing and scattering radiation (direct radiative effect; DRE) and by perturbing the properties of clouds (aerosol indirect effect; AIE). Natural aerosol sources are strongly controlled by, and can influence, climate; giving rise to potential natural aerosol-climate feedbacks. Earth System Models (ESMs) include a description of some of these natural aerosol-climate feedbacks, predicting substantial changes in natural aerosol over the coming century with associated radiative perturbations. Despite this, the sensitivity of natural aerosols simulated by ESMs to changes in climate or emissions has not been robustly tested against observations. Here we combine long-term observations of aerosol number and a global aerosol microphysics model to assess terrestrial natural aerosol-climate feedbacks. We find a strong positive relationship between the summertime anomaly in observed concentration of particles greater than 100 nm diameter and the anomaly in local air temperature. This relationship is reproduced by the model and driven by variability in dynamics and meteorology, as well as natural sources of aerosol. We use an offline radiative transfer model to determine radiative effects due to changes in two natural aerosol sources: landscape fire and biogenic SOA. We find that interannual variability in the simulated global natural aerosol radiative effect (RE) is negatively related to the global temperature anomaly. The magnitude of global aerosol-climate feedback (sum of DRE and AIE) is estimated to be -0.15 Wm-2 K-1 for landscape fire aerosol and -0.06 Wm-2 K-1 for biogenic SOA. These feedbacks are comparable in magnitude, but opposite in sign to the snow albedo feedback, highlighting the need for natural aerosol feedbacks to

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

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.

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.

Linkages Between Ozone-depleting Substances, Tropospheric Oxidation and Aerosols

NASA Technical Reports Server (NTRS)

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

2013-01-01

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

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.

Aerosol effect on climate extremes in Europe under different future scenarios

NASA Astrophysics Data System (ADS)

Sillmann, J.; Pozzoli, L.; Vignati, E.; Kloster, S.; Feichter, J.

2013-05-01

This study investigates changes in extreme temperature and precipitation events under different future scenarios of anthropogenic aerosol emissions (i.e., SO2 and black and organic carbon) simulated with an aerosol-climate model (ECHAM5-HAM) with focus on Europe. The simulations include a maximum feasible aerosol reduction (MFR) scenario and a current legislation emission (CLEmod) scenario where Europe implements the MFR scenario, but the rest of the world follows the current legislation scenario and a greenhouse gas scenario. The strongest changes relative to the year 2000 are projected for the MFR scenario, in which the global aerosol reduction greatly enforces the general warming effect due to greenhouse gases and results in significant increases of temperature and precipitation extremes in Europe. Regional warming effects can also be identified from aerosol reductions under the CLEmodscenario. This becomes most obvious in the increase of the hottest summer daytime temperatures in Northern Europe.

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

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

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

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

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...

Direct radiative effect due to brownness in organic carbon aerosols generated from biomass combustion

NASA Astrophysics Data System (ADS)

Rathod, T. D.; Sahu, S. K.; Tiwari, M.; Pandit, G. G.

2016-12-01

We report the enhancement in the direct radiative effect due the presence of Brown carbon (BrC) as a part of organic carbon aerosols. The optical properties of organic carbon aerosols generated from pyrolytic combustion of mango tree wood (Magnifera Indica) and dung cake at different temperatures were considered. Mie codes were used to calculate absorption and scattering coefficients coupled with experimentally derived imaginary complex refractive index. The direct radiative effect (DRE) for sampled organic carbon aerosols was estimated using a wavelength dependent radiative transfer equation. The BrC DRE was estimated taking virtually non absorbing organic aerosols as reference. The BrC DRE from wood and dung cake was compared at different combustion temperatures and conditions. The BrC contributed positively to the direct top of the atmosphere radiative effect. Dung cake generated BrC aerosols were found to be strongly light absorbing as compared to BrC from wood combustion. It was noted that radiative effects of BrC from wood depended on its generation temperature and conditions. For BrC aerosols from dung cake such strong dependence was not observed. The average BrC aerosol DRE values were 1.53±0.76 W g-1 and 17.84±6.45 W g-1 for wood and dung cake respectively. The DRE contribution of BrC aerosols came mainly (67-90%) from visible light absorption though they exhibited strong absorption in shorter wavelengths of the UV-visible spectrum.

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

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.

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.

Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign

NASA Technical Reports Server (NTRS)

DeCarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.;

Dust-wind interactions can intensify aerosol pollution over eastern China

DOE PAGES

Yang, Yang; Russell, Lynn M.; Lou, Sijia; ...

2017-05-11

Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution, which has adverse impacts on hundreds of millions of people across China1–4. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with abnormal meteorological conditions, including weaker wind speeds5–9. Using a global climate model and a chemical transport model, we show that variations in dust emissions decrease the wintertime land-sea surface air temperature difference between eastern China and the South China Sea and weaken winds below the lowest 10th percentile of wind speed by 0.06 mmore » s-1. Here, the weakened winds enhance stagnation and account for 13% of the increases in PM2.5 aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime PM2.5 concentrations, with important implications that should be considered in air quality studies.« less

Dust-wind interactions can intensify aerosol pollution over eastern China

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

Yang, Yang; Russell, Lynn M.; Lou, Sijia

Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution, which has adverse impacts on hundreds of millions of people across China1–4. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with abnormal meteorological conditions, including weaker wind speeds5–9. Using a global climate model and a chemical transport model, we show that variations in dust emissions decrease the wintertime land-sea surface air temperature difference between eastern China and the South China Sea and weaken winds below the lowest 10th percentile of wind speed by 0.06 mmore » s-1. Here, the weakened winds enhance stagnation and account for 13% of the increases in PM2.5 aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime PM2.5 concentrations, with important implications that should be considered in air quality studies.« less

Stratospheric aerosol modification by supersonic transport operations with climate implications

NASA Technical Reports Server (NTRS)

Toon, O. B.; Turco, R. P.; Pollack, J. B.; Whitten, R. C.; Poppoff, I. G.; Hamill, P.

1980-01-01

The potential effects on stratospheric aerosois of supersonic transport emissions of sulfur dioxide gas and submicron size soot granules are estimated. An interactive particle-gas model of the stratospheric aerosol is used to compute particle changes due to exhaust emissions, and an accurate radiation transport model is used to compute the attendant surface temperature changes. It is shown that a fleet of several hundred supersonic aircraft, operating daily at 20 km, could produce about a 20% increase in the concentration of large particles in the stratosphere. Aerosol increases of this magnitude would reduce the global surface temperature by less than 0.01 K.

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

Aerosol Emissions from Great Lakes Harmful Algal Blooms

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

May, Nathaniel W.; Olson, Nicole E.; Panas, Mark

In freshwater lakes, harmful algal blooms (HABs) of Cyanobacteria (blue-green algae) produce toxins that impact human health. However, little is known about the chemical species present in lake spray aerosol (LSA) produced from wave-breaking in freshwater HABs. In this study, a laboratory LSA generator produced aerosols from freshwater samples collected from Lake Michigan and Lake Erie during HAB and non-bloom conditions. Particles were analyzed for size and chemical composition by single particle mass spectrometry, electron microscopy, and fluorescence microscopy, with three distinct types of LSA identified with varying levels of organic carbon and biological material associated with calcium salts. LSAmore » autofluorescence increases with blue-green algae concentration, showing that organic molecules of biological origin are incorporated in LSA from HABs. The number fraction of LSA with biological mass spectral markers also increases with particle diameter (greater than 0.5 μm), showing that HABs have size-dependent impacts on aerosol composition. The highest number fraction of LSA enriched in organic carbon were observed in particles less than 0.5 μm in diameter. Understanding the transfer of organic and biogenic material from freshwater to the atmosphere via LSA particles is crucial for determining health and climate effects due to HABs.« 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

Climate forcing by anthropogenic aerosols

NASA Technical Reports Server (NTRS)

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

1992-01-01

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

Climate forcing by anthropogenic aerosols.

PubMed

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

1992-01-24

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

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.

Sugars in Antarctic aerosol

NASA Astrophysics Data System (ADS)

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

2015-10-01

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

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.

Increases in aerosol concentrations over eastern China due to the decadal-scale weakening of the East Asian summer monsoon

NASA Astrophysics Data System (ADS)

Zhu, Jianlei; Liao, Hong; Li, Jianping

2012-05-01

China has been experiencing increased concentrations of aerosols, commonly attributed to the large increases in emissions associated with the rapid economic development. We show by using a chemical transport model driven by the assimilated meteorological fields that the observed decadal-scale weakening of the East Asian summer monsoon also contributed to the increases in aerosols in China. We find that the simulated aerosol concentrations have strong negative correlations with the strength of the East Asian Summer monsoon. Accounting for sulfate, nitrate, ammonium, black carbon, and organic carbon aerosols, the summer surface-layer PM2.5 concentration averaged over eastern China (110°-125°E, 20°-45°N) can be 17.7% higher in the weakest monsoon years than in the strongest monsoon years. The weakening of the East Asian Summer monsoon increases aerosol concentrations mainly by the changes in atmospheric circulation (the convergence of air pollutants) in eastern China.

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

The impact of port emissions and marine biogenics on the single-particle chemistry of marine aerosol measured on board the R/V Atlantis during the CalNEX 2010 field campaign

NASA Astrophysics Data System (ADS)

Gaston, C. J.; Quinn, P.; Bates, T. S.; Prather, K. A.

2010-12-01

Marine environments are characterized by low particle concentrations and, as such, are sensitive to changes in particle number concentration and chemistry induced by biogenic and anthropogenic influences. Measurements of both gas phase and particle phase emissions on board the R/V Atlantis during the CalNEX 2010 field campaign provided an opportunity to examine the impact of anthropogenic and marine biogenic emissions on particle chemistry along the California coast. Real-time, single-particle measurements made using an aerosol time-of-flight mass spectrometer (ATOFMS) revealed the single-particle mixing state of the sampled marine aerosols. Submicron particles (0.2-1.0 um) containing organic carbon, elemental carbon mixed with organic carbon, and unique V-containing particles previously detected in port regions were prevalent throughout the Southern California coast; most of these particles were also associated with sulfate. Measurements made in the deep water channel near Sacramento, CA revealed dramatically different particle chemistry that was characterized by organic carbon and amines. Particles measured further away from the continent toward the open ocean were influenced by marine biological activity due to a phytoplankton bloom that was occurring off the California coast. During this sampling period, unique ocean-derived particles containing internal mixtures of Mg and organic carbon were detected in addition to unique particles containing elemental S ions, which were only detected at night. An aerosol generator used to bubble seawater in order to characterize primary emissions from the ocean confirmed that the Mg-organic carbon and S-containing particles were indeed emitted from the ocean. These measurements reveal the strong impact of both port emissions as well as marine biogenic emissions on aerosol chemistry along the California coast.

Local and remote impacts of aerosol species on Indian summer monsoon rainfall in a GCM

NASA Astrophysics Data System (ADS)

Guo, Liang; Turner, Andrew; Highwood, Eleanor

2016-04-01

The HadGEM2 AGCM is used to determine the most important anthropogenic aerosols in the Indian monsoon using experiments in which observed trends in individual aerosol species are imposed. Sulphur dioxide (SD) emissions are shown to impact rainfall more strongly than black carbon (BC) aerosols, causing reduced rainfall especially over northern India. Significant perturbations due to BC are not noted until its emissions are scaled up in a sensitivity test, in which rainfall increases over northern India as a result of the Elevated Heat Pump mechanism, enhancing convection during the pre-monsoon and bringing forward the monsoon onset. Secondly, the impact of anthropogenic aerosols is compared to that of increasing greenhouse-gas concentrations and observed sea-surface temperature (SST) warming. The tropospheric temperature gradient driving the monsoon shows weakening when forced by either SD or imposed SST trends. However the observed SST trend is dominated by warming in the deep tropics; when the component of SST trend related to aerosol emissions is removed, further warming is found in the extratropical northern hemisphere that tends to offset monsoon weakening. This suggests caution is needed when using SST forcing as a proxy for greenhouse warming. Finally, aerosol emissions are decomposed into those from the Indian region and those elsewhere, in pairs of experiments with SD and BC. Both local and remote aerosol emissions are found to lead to rainfall changes over India; for SD, remote aerosols contribute around 75% of the rainfall decrease over India, while for BC the remote forcing is even more dominant.

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.

Impacts of East Asian Sulfate Aerosols on Local and Remote Climate

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Impact of natural and anthropogenic aerosols on stratocumulus and precipitation in the Southeast Pacific: a regional modelling study using WRF-Chem

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

Yang, Q.; Gustafson, W. I.; Fast, J. D.

2012-09-28

Cloud-system resolving simulations with the chemistry version of the Weather Research and Forecasting (WRF-Chem) model are used to quantify the relative impacts of regional anthropogenic and oceanic emissions on changes in aerosol properties, cloud macro- and microphysics, and cloud radiative forcing over the Southeast Pacific (SEP) during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) (15 October–16 November 2008). Two distinct regions are identified. The near-coast polluted region is characterized by low surface precipitation rates, the strong suppression of non-sea-salt particle activation due to sea-salt particles, a predominant albedo effect in aerosol indirect effects, and limited impact of aerosols associated withmore » anthropogenic emissions on clouds. Opposite sensitivities to natural marine and anthropogenic aerosol perturbations are seen in cloud properties (e.g., cloud optical depth and cloud-top and cloud-base heights), precipitation, and the top-of-atmosphere and surface shortwave fluxes over this region. The relatively clean remote region is characterized by large contributions of aerosols from non-regional sources (lateral boundaries) and much stronger drizzle at the surface. Under a scenario of five-fold increase in regional anthropogenic emissions, this relatively clean region shows large cloud responses, for example, a 13% increase in cloud-top height and a 9% increase in albedo in response to a moderate increase (25% of the reference case) in cloud condensation nuclei (CCN) concentration. The reduction of precipitation due to this increase in anthropogenic aerosols more than doubles the aerosol lifetime in the clean marine boundary layer. Therefore, the aerosol impacts on precipitation are amplified by the positive feedback of precipitation on aerosol, which ultimately alters the cloud micro- and macro-physical properties, leading to strong aerosol-cloud-precipitation interactions. The high sensitivity is also

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.

A study of remotely sensed aerosol properties from ground-based sun and sky scanning radiometers

NASA Astrophysics Data System (ADS)

Giles, David M.

Aerosol particles impact human health by degrading air quality and affect climate by heating or cooling the atmosphere. The Indo-Gangetic Plain (IGP) of Northern India, one of the most populous regions in the world, produces and is impacted by a variety of aerosols including pollution, smoke, dust, and mixtures of them. The NASA Aerosol Robotic Network (AERONET) mesoscale distribution of Sun and sky-pointing instruments in India was established to measure aerosol characteristics at sites across the IGP and around Kanpur, India, a large urban and industrial center in the IGP, during the 2008 pre-monsoon (April-June). This study focused on detecting spatial and temporal variability of aerosols, validating satellite retrievals, and classifying the dominant aerosol mixing states and origins. The Kanpur region typically experiences high aerosol loading due to pollution and smoke during the winter and high aerosol loading due to the addition of dust to the pollution and smoke mixture during the pre-monsoon. Aerosol emissions in Kanpur likely contribute up to 20% of the aerosol loading during the pre-monsoon over the IGP. Aerosol absorption also increases significantly downwind of Kanpur indicating the possibility of the black carbon emissions from aerosol sources such as coal-fired power plants and brick kilns. Aerosol retrievals from satellite show a high bias when compared to the mesoscale distributed instruments around Kanpur during the pre-monsoon with few high quality retrievals due to imperfect aerosol type and land surface characteristic assumptions. Aerosol type classification using the aerosol absorption, size, and shape properties can identify dominant aerosol mixing states of absorbing dust and black carbon particles. Using 19 long-term AERONET sites near various aerosol source regions (Dust, Mixed, Urban/Industrial, and Biomass Burning), aerosol absorption property statistics are expanded upon and show significant differences when compared to previous work

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

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

NASA Astrophysics Data System (ADS)

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

2015-11-01

Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.

Black carbon aerosols and the third polar ice cap

NASA Astrophysics Data System (ADS)

Menon, S.; Koch, D.; Beig, G.; Sahu, S.; Fasullo, J.; Orlikowski, D.

2010-05-01

Recent thinning of glaciers over the Himalayas (sometimes referred to as the third polar region) have raised concern on future water supplies since these glaciers supply water to large river systems that support millions of people inhabiting the surrounding areas. Black carbon (BC) aerosols, released from incomplete combustion, have been increasingly implicated as causing large changes in the hydrology and radiative forcing over Asia and its deposition on snow is thought to increase snow melt. In India BC emissions from biofuel combustion is highly prevalent and compared to other regions, BC aerosol amounts are high. Here, we quantify the impact of BC aerosols on snow cover and precipitation from 1990 to 2010 over the Indian subcontinental region using two different BC emission inventories. New estimates indicate that Indian BC emissions from coal and biofuel are large and transport is expected to expand rapidly in coming years. We show that over the Himalayas, from 1990 to 2000, simulated snow/ice cover decreases by ~0.9% due to aerosols. The contribution of the enhanced Indian BC to this decline is ~36%, similar to that simulated for 2000 to 2010. Spatial patterns of modeled changes in snow cover and precipitation are similar to observations (from 1990 to 2000), and are mainly obtained with the newer BC estimates.

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

Toxicity of atmospheric aerosols on marine phytoplankton

USGS Publications Warehouse

Paytan, A.; Mackey, K.R.M.; Chen, Y.; Lima, I.D.; Doney, S.C.; Mahowald, N.; Labiosa, R.; Post, A.F.

2009-01-01

Atmospheric aerosol deposition is an important source of nutrients and trace metals to the open ocean that can enhance ocean productivity and carbon sequestration and thus influence atmospheric carbon dioxide concentrations and climate. Using aerosol samples from different back trajectories in incubation experiments with natural communities, we demonstrate that the response of phytoplankton growth to aerosol additions depends on specific components in aerosols and differs across phytoplankton species. Aerosol additions enhanced growth by releasing nitrogen and phosphorus, but not all aerosols stimulated growth. Toxic effects were observed with some aerosols, where the toxicity affected picoeukaryotes and Synechococcus but not Prochlorococcus.We suggest that the toxicity could be due to high copper concentrations in these aerosols and support this by laboratory copper toxicity tests preformed with Synechococcus cultures. However, it is possible that other elements present in the aerosols or unknown synergistic effects between these elements could have also contributed to the toxic effect. Anthropogenic emissions are increasing atmospheric copper deposition sharply, and based on coupled atmosphere-ocean calculations, we show that this deposition can potentially alter patterns of marine primary production and community structure in high aerosol, low chlorophyll areas, particularly in the Bay of Bengal and downwind of South and East Asia.

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: Results from DISCOVER-AQ California

DOE PAGES

Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; ...

2016-05-02

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) andmore » an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM 1) concentration was 31.0 µg m −3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C  =  0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C  =  0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C  =  0.33; BBOA2: 20 % of total OA, O / C  =  0.60) most likely

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

NASA Astrophysics Data System (ADS)

Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

2016-05-01

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno-Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C = 0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C = 0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C = 0.33; BBOA2: 20 % of total OA, O / C = 0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

NASA Astrophysics Data System (ADS)

Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

2015-12-01

The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. Aerosol Mass Spectrometer (HR-ToF-AMS) and an Ionicon Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 μg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi

"Investigation of Trends in Aerosol Direct Radiative Effects ...

EPA Pesticide Factsheets

While aerosol radiative effects have been recognized as some of the largest sources of uncertainty among the forcers of climate change, there has been little effort devoted to verification of the spatial and temporal variability of the magnitude and directionality of aerosol radiative forcing. A comprehensive 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. This study aims at addressing this issue through a systematic investigation of changes in anthropogenic emissions of SO2 and NOx over the past two decades in the United States, their impacts on anthropogenic aerosol loading in the North American troposphere, and subsequent impacts on regional radiation budgets. 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). A methodology is developed to consistently estimate emission inventories for the 20-year period accounting for air quality regulations as well as population trends, economic conditions, and technology changes in motor vehicles and electric power generation. The coupled WRF-CMAQ model is applied for time periods pre a

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

Biomass Burning Emissions of Black Carbon from African Sources

NASA Astrophysics Data System (ADS)

Aiken, A. C.; Leone, O.; Nitschke, K. L.; Dubey, M. K.; Carrico, C.; Springston, S. R.; Sedlacek, A. J., III; Watson, T. B.; Kuang, C.; Uin, J.; McMeeking, G. R.; DeMott, P. J.; Kreidenweis, S. M.; Robinson, A. L.; Yokelson, R. J.; Zuidema, P.

2016-12-01

Biomass burning (BB) emissions are a large source of carbon to the atmosphere via particles and gas phase species. Carbonaceous aerosols are emitted along with gas-phase carbon monoxide (CO) and carbon dioxide (CO2) that can be used to determine particulate emission ratios and modified combustion efficiencies. Black carbon (BC) aerosols are potentially underestimated in global models and are considered to be one of the most important global warming factors behind CO2. Half or more BC in the atmosphere is from BB, estimated at 6-9 Tg/yr (IPCC, 5AR) and contributing up to 0.6 W/m2 atmospheric warming (Bond et al., 2013). With a potential rise in drought and extreme events in the future due to climate change, these numbers are expected to increase. For this reason, we focus on BC and organic carbon aerosol species that are emitted from forest fires and compare their emission ratios, physical and optical properties to those from controlled laboratory studies of single-source BB fuels to understand BB carbonaceous aerosols in the atmosphere. We investigate BC in concentrated BB plumes as sampled from the new U.S. DOE ARM Program campaign, Layered Atlantic Smoke Interactions with Clouds (LASIC). The ARM Aerosol Mobile Facility 1 (AMF1) and Mobile Aerosol Observing System (MAOS) are currently located on Ascension Island in the South Atlantic Ocean, located midway between Angola and Brazil. The location was chosen for sampling maximum aerosol outflow from Africa. The far-field aged BC from LASIC is compared to BC from indoor generation from single-source fuels, e.g. African grass, sampled during Fire Lab At Missoula Experiments IV (FLAME-IV). BC is measured with a single-particle soot photometer (SP2) alongside numerous supporting instrumentation, e.g. particle counters, CO and CO2 detectors, aerosol scattering and absorption measurements, etc. FLAME-IV includes both direct emissions and well-mixed aerosol samples that have undergone dilution, cooling, and condensation. BC

Aerosol Indirect Effects on Cirrus Clouds in Global Aerosol-Climate Models

NASA Astrophysics Data System (ADS)

Liu, X.; Zhang, K.; Wang, Y.; Neubauer, D.; Lohmann, U.; Ferrachat, S.; Zhou, C.; Penner, J.; Barahona, D.; Shi, X.

2015-12-01

Cirrus clouds play an important role in regulating the Earth's radiative budget and water vapor distribution in the upper troposphere. Aerosols can act as solution droplets or ice nuclei that promote ice nucleation in cirrus clouds. Anthropogenic emissions from fossil fuel and biomass burning activities have substantially perturbed and enhanced concentrations of aerosol particles in the atmosphere. Global aerosol-climate models (GCMs) have now been used to quantify the radiative forcing and effects of aerosols on cirrus clouds (IPCC AR5). However, the estimate uncertainty is very large due to the different representation of ice cloud formation and evolution processes in GCMs. In addition, large discrepancies have been found between model simulations in terms of the spatial distribution of ice-nucleating aerosols, relative humidity, and temperature fluctuations, which contribute to different estimates of the aerosol indirect effect through cirrus clouds. In this presentation, four GCMs with the start-of-the art representations of cloud microphysics and aerosol-cloud interactions are used to estimate the aerosol indirect effects on cirrus clouds and to identify the causes of the discrepancies. The estimated global and annual mean anthropogenic aerosol indirect effect through cirrus clouds ranges from 0.1 W m-2 to 0.3 W m-2 in terms of the top-of-the-atmosphere (TOA) net radiation flux, and 0.5-0.6 W m-2 for the TOA longwave flux. Despite the good agreement on global mean, large discrepancies are found at the regional scale. The physics behind the aerosol indirect effect is dramatically different. Our analysis suggests that burden of ice-nucleating aerosols in the upper troposphere, ice nucleation frequency, and relative role of ice formation processes (i.e., homogeneous versus heterogeneous nucleation) play key roles in determining the characteristics of the simulated aerosol indirect effects. In addition to the indirect effect estimate, we also use field campaign

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.

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.

an aerosol climatology optical properties and its associated direct radiative forcing

NASA Astrophysics Data System (ADS)

Kinne, Stefan

2010-05-01

Aerosol particles are quite complex in nature. Aerosol impacts on the distribution of radiative energy and on cloud microphysics have been debated climate impact issues. Here, a new aerosol-climatology is presented, combining the consistency and completeness of global modelling with quality data by ground-monitoring. It provides global monthly maps for spectral aerosol optical properties and for concentrations of CCN and IN. Based on the optical properties the aerosol direct forcing is determined. And with environmental data for clouds and estimates on the anthropogenic fraction from emission experiments with global modelling even the climate relevant aerosol direct forcing at the top of the atmosphere (ToA) is determined. This value is rather small near -0.2W/m2 with limited uncertainty estimated at (+/-0.3) due to uncertainties in aerosol absorption and underlying surface conditions or clouds.

Three Dimensional Modeling Analysis of the Transpacific Transport of Aerosols During PACDEX

NASA Astrophysics Data System (ADS)

Carmichael, G. R.; Adhikary, B.; Hatch, C.; Kulkarni, S.; Moen, J.; Mena, M.

2007-12-01

Mineral dust and aerosols emitted from Asia are known to traverse long distances across the Pacific Ocean and can reach North America within a few days. A pilot field study, the PACific Dust Experiment (PACDEX), was carried out in April and May of 2007, during the peak East Asian dust emission season. The NSF/NCAR-HIAPER (High Performance Instrumented Airborne Platform for Environmental Research) platform allowed for sampling the evolution of mineral aerosol/pollution plumes and their physical and chemical characteristics as they traverse the Pacific Ocean and interact with the Pacific cloud systems en route to North America in both the upper and lower troposphere. A comprehensive 3-dimensional regional-scale model developed at The University of Iowa (Sulfur Transport dEposition Model, STEM) has been used for the analysis of aerosol interactions to help define key measurement strategies during the mission and to help interpret observations from the HIAPER platform. In this study we will present model aerosol distribution inter-comparison with cloud fields and aircraft observations. Model analysis provides further insight into cloud/pollution/dust interactions as East Asian emissions transit the Pacific Ocean en route to North America. Trajectory analysis and emission markers are used to help understand the air mass history and aerosol aging processes of the aerosols sampled by the HIAPER platform. Estimates of the fluxes of aerosol dust, BC and sulfate due to transpacific transport will also be presented.

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

Air pollution from gas flaring: new emission factor estimates and detection in a West African aerosol remote-sensing climatology

NASA Astrophysics Data System (ADS)

MacKenzie, Rob; Fawole, Olusegun Gabriel; Levine, James; Cai, Xiaoming

2016-04-01

Gas flaring, the disposal of gas through stacks in an open-air flame, is a common feature in the processing of crude oil, especially in oil-rich regions of the world. Gas flaring is a prominent source of volatile organic compounds (VOCs), polycyclic aromatic hydrocarbons (PAH), CO, CO2, nitrogen oxides (NOx), SO2 (in "sour" gas only), and soot (black carbon), as well as the release of locally significant amounts of heat. The rates of emission of these pollutants from gas flaring depend on a number of factors including, but not limited to, fuel composition and quantity, stack geometry, flame/combustion characteristics, and prevailing meteorological conditions. Here, we derive new estimated emission factors (EFs) for carbon-containing pollutants (excluding PAH). The air pollution dispersion model, ADMS5, is used to simulate the dispersion of the pollutants from flaring stacks in the Niger delta. A seasonal variation of the dispersion pattern of the pollutant within a year is studied in relation to the movements of the West Africa Monsoon (WAM) and other prevailing meteorological factors. Further, we have clustered AERONET aerosol signals using trajectory analysis to identify dominant aerosol sources at the Ilorin site in West Africa (4.34 oE, 8.32 oN). A 10-year trajectory-based analysis was undertaken (2005-2015, excluding 2010). Of particular interest are air masses that have passed through the gas flaring region in the Niger Delta area en-route the AERONET site. 7-day back trajectories were calculated using the UK Universities Global Atmospheric Modelling Programme (UGAMP) trajectory model which is driven by analyses from the European Centre for Medium-Range Weather Forecasts (ECMWF). From the back-trajectory calculations, dominant sources are identified, using literature classifications: desert dust (DD); Biomass burning (BB); and Urban-Industrial (UI). We use a combination of synoptic trajectories and aerosol optical properties to distinguish a fourth source

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.

Impacts of Different Anthropogenic Aerosol Emission Scenarios on Hydrology in the Mekong Basins and their Effects on Irrigation and Hydropower

NASA Astrophysics Data System (ADS)

Yeo, L. K.; Wang, C.

2016-12-01

Water distribution is closely linked to food and energy security. Aerosol emissions affect cloud properties, as well as atmospheric stability, changing the distribution of precipitation. These changes in precipitation causes changes in water availability, affecting food production and energy generation. These impacts are especially important in Southeast Asia, which uses up to 90% of their water supply for irrigation. In addition, the Mekong river, the largest inland fishery in the world, has 30,000MW of hydropower potential in its lower reaches alone. Modelling the impacts of these anthropogenic emission scenarios will allow us to better understand their downstream effects on hydrology, and any potential feedbacks it may have on future aerosol emissions. In the first step, we run the WRF model using FNL reanlaysis data from 2014 and 2015 to generate the WRF-hydro model forcing inputs. We then run the WRF-hydro model and compare the output with current measurements of soil moisture, river flow, and precipitation. Secondly, we run the WRF-Chem model with various anthropogenic emission scenarios and put the results through the WRF-hydro model to determine the impact of these emission scenarios on soil moisture and river flow. The scenarios include enhanced anthropogenic emissions in Asia, anologous to widespread adoption of coal burning as an energy source in Asia. Anthropogenic emissions have the potential to affect energy policy in countries affected by these emissions. When hydropower generation is affected by changes in precipitation, the affected countries will have to switch to alternative sources of fuel to meet their energy needs. These sources typically result in changes in anthropogenic aerosol emisssions, especially if coal is used as an alternative source of energy.

Temperature and burning history affect emissions of greenhouse gases and aerosol particles from tropical peatland fire

NASA Astrophysics Data System (ADS)

Kuwata, Mikinori; Kai, Fuu Ming; Yang, Liudongqing; Itoh, Masayuki; Gunawan, Haris; Harvey, Charles F.

2017-01-01

Tropical peatland burning in Asia has been intensifying over the last decades, emitting huge amounts of gas species and aerosol particles. Both laboratory and field studies have been conducted to investigate emission from peat burning, yet a significant variability in data still exists. We conducted a series of experiments to characterize the gas and particulate matter emitted during burning of a peat sample from Sumatra in Indonesia. Heating temperature of peat was found to regulate the ratio of CH4 to CO2 in emissions (ΔCH4/ΔCO2) as well as the chemical composition of particulate matter. The ΔCH4/ΔCO2 ratio was larger for higher temperatures, meaning that CH4 emission is more pronounced at these conditions. Mass spectrometric analysis of organic components indicated that aerosol particles emitted at higher temperatures had more unsaturated bonds and ring structures than that emitted from cooler fires. The result was consistently confirmed by nuclear magnetic resonance analysis. In addition, CH4 emitted by burning charcoal, which is derived from previously burned peat, was lower by at least an order of magnitude than that from fresh peat. These results highlight the importance of both fire history and heating temperature for the composition of tropical peat-fire emissions. They suggest that remote sensing technologies that map fire histories and temperatures could provide improved estimates of emissions.

Biomass burning aerosol transport and vertical distribution over the South African-Atlantic region: Aerosol Transport Over SE Atlantic

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

Das, Sampa; Harshvardhan, H.; Bian, Huisheng

Aerosols from wild-land fires could significantly perturb the global radiation balance and induce the climate change. In this study, the Community Atmospheric Model version 5 (CAM5) with prescribed daily fire aerosol emissions is used to investigate the spatial and seasonal characteristics of radiative forcings of wildfire aerosols including black carbon (BC) and particulate organic matter (POM). The global annual mean direct radiative forcing (DRF) of all fire aerosols is 0.15 W m-2, mainly due to the absorption of fire BC (0.25 W m-2), while fire POM induces a weak negative forcing (-0.05 W m-2). Strong positive DRF is found inmore » the Arctic and in the oceanic regions west of South Africa and South America as a result of amplified absorption of fire BC above low-level clouds, in general agreement with satellite observations. The global annual mean cloud radiative forcing due to all fire aerosols is -0.70 W m-2, resulting mainly from the fire POM indirect forcing (-0.59 W m-2). The large cloud liquid water path over land areas of the Arctic favors the strong fire aerosol indirect forcing (up to -15 W m-2) during the Arctic summer. Significant surface cooling, precipitation reduction and low-level cloud amount increase are also found in the Arctic summer as a result of the fire aerosol indirect effect. The global annual mean surface albedo forcing over land areas (0.03 W m-2) is mainly due to the fire BC-on-snow forcing (0.02 W m-2) with the maximum albedo forcing occurring in spring (0.12 W m-2) when snow starts to melt.« less

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

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

Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia

2013-05-10

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

A multi-model evaluation of aerosols over South Asia: common problems and possible causes

NASA Astrophysics Data System (ADS)

Pan, X.; Chin, M.; Gautam, R.; Bian, H.; Kim, D.; Colarco, P. R.; Diehl, T. L.; Takemura, T.; Pozzoli, L.; Tsigaridis, K.; Bauer, S.; Bellouin, N.

2015-05-01

Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, water cycle and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions. In this study, the spatio-temporal aerosol distributions over South Asia from seven global aerosol models are evaluated against aerosol retrievals from NASA satellite sensors and ground-based measurements for the period of 2000-2007. Overall, substantial underestimations of aerosol loading over South Asia are found systematically in most model simulations. Averaged over the entire South Asia, the annual mean aerosol optical depth (AOD) is underestimated by a range 15 to 44% across models compared to MISR (Multi-angle Imaging SpectroRadiometer), which is the lowest bound among various satellite AOD retrievals (from MISR, SeaWiFS (Sea-Viewing Wide Field-of-View Sensor), MODIS (Moderate Resolution Imaging Spectroradiometer) Aqua and Terra). In particular during the post-monsoon and wintertime periods (i.e., October-January), when agricultural waste burning and anthropogenic emissions dominate, models fail to capture AOD and aerosol absorption optical depth (AAOD) over the Indo-Gangetic Plain (IGP) compared to ground-based Aerosol Robotic Network (AERONET) sunphotometer measurements. The underestimations of aerosol loading in models generally occur in the lower troposphere (below 2 km) based on the comparisons of aerosol extinction profiles calculated by the models with those from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data. Furthermore, surface concentrations of all aerosol components (sulfate, nitrate, organic aerosol (OA) and black carbon (BC)) from the models are found much lower than in situ measurements in winter. Several possible causes for these common problems of underestimating aerosols in models during the post-monsoon and wintertime periods are identified: the aerosol hygroscopic growth and formation of

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

EPA Science Inventory

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

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

NASA Astrophysics Data System (ADS)

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

2013-04-01

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

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

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

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.

Black carbon reduction will weaken the aerosol net cooling effect

NASA Astrophysics Data System (ADS)

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

2014-12-01

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 a 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 coupled model BCC_AGCM2.0.1_CUACE/Aero, 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 present-day conditions if the BC emission is reduced exclusively to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial for the mitigation of global warming. However, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 relative to present-day conditions if emissions of BC and co-emitted sulfur dioxide and organic carbon are simultaneously reduced as the most close conditions to the actual situation to the level 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.

Secondary Organic Aerosol Production from Gasoline Vehicle Exhaust: Effects of Engine Technology, Cold Start, and Emission Certification Standard.

PubMed

Zhao, Yunliang; Lambe, Andrew T; Saleh, Rawad; Saliba, Georges; Robinson, Allen L

2018-02-06

Secondary organic aerosol (SOA) formation from dilute exhaust from 16 gasoline vehicles was investigated using a potential aerosol mass (PAM) oxidation flow reactor during chassis dynamometer testing using the cold-start unified cycle (UC). Ten vehicles were equipped with gasoline direct injection engines (GDI vehicles) and six with port fuel injection engines (PFI vehicles) certified to a wide range of emissions standards. We measured similar SOA production from GDI and PFI vehicles certified to the same emissions standard; less SOA production from vehicles certified to stricter emissions standards; and, after accounting for differences in gas-particle partitioning, similar effective SOA yields across different engine technologies and certification standards. Therefore the ongoing, dramatic shift from PFI to GDI vehicles in the United States should not alter the contribution of gasoline vehicles to ambient SOA and the natural replacement of older vehicles with newer ones certified to stricter emissions standards should reduce atmospheric SOA levels. Compared to hot operations, cold-start exhaust had lower effective SOA yields, but still contributed more SOA overall because of substantially higher organic gas emissions. We demonstrate that the PAM reactor can be used as a screening tool for vehicle SOA production by carefully accounting for the effects of the large variations in emission rates.

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

PubMed Central

Jathar, Shantanu H.; Gordon, Timothy D.; Hennigan, Christopher J.; Pye, Havala O. T.; Pouliot, George; Adams, Peter J.; Donahue, Neil M.; Robinson, Allen L.

2014-01-01

Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10–20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y−1 of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations. PMID:25002466

Long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Xu, J.; Zhang, X.; Liu, Y.; Shichang, K.; Ma, Y.

2017-12-01

An intensive measurement was conducted at a remote, background, and high-altitude site (Qomolangma station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from April 12 to May 12, 2016 to chemically characterize high time-resolved submicron particulate matter (PM1) and obtain the influence of biomass burning emissions to the Himalayas, frequently transported from south Asia during pre-monsoon season. Two high aerosol loading periods were observed during the study. Overall, the average (± 1σ) PM1 mass concentration was 4.44 (± 4.54) µg m-3 for the entire study, comparable with those observed at other remote sites worldwide. Organic aerosols (OA) was the dominant PM1 species (accounting for 54.3% of total PM1 mass on average) and its contribution increased with the increase of total PM1 mass loading. The average size distributions of PM1 species all peaked at an overlapping accumulation mode ( 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transportations. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a biomass burning related OA (BBOA, 43.7%) and two oxygenated OA (Local-OOA and LRT-OOA; 13.9% and 42.4%) represented sources from local emissions and long-range transportations, respectively. Two polluted air mass origins (generally from the west and southwest of QOMS) and two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions were observed, respectively, suggesting the important sources of wildfires from south Asia. One of polluted aerosol plumes was investigated in detail to illustrate the evolution of aerosol characteristics at QOMS driving by different impacts of wildfires, air mass origins, meteorological conditions and

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 impacts on climate and environment over East Asia

NASA Astrophysics Data System (ADS)

Nakata, M.; Sano, I.; Mukai, S.

2014-12-01

It is well known that the aerosol distribution in East Asia is complex due to both the increasing emissions of the anthropogenic aerosols associated with economic growth and the behavior of natural dusts. Therefore, detailed observations of atmospheric particles in East Asian are important. It is concerned about the change of concentration of aerosols causes various effects on the climate by directly and indirectly modifying the optical properties and lifetimes of cloud. In addition to radiation budget change, aerosol has a significant potential to change cloud and precipitation. These circulation fields change influence on emission of natural aerosols such as dust aerosols and sea salt aerosols. Also, air pollution in megacities in East Asia has become a serious problem. Especially problematic are fine particles called PM2.5, whose diameter is 2.5 mm or less. Particulate matter (PM) pollution as indicated by high PM2.5 readings will cause a spike in the mortality rate of patients suffering from heart and lung diseases. Because fine particles are much smaller than inhalable coarse particles, the can penetrate deeper into the lungs and cause more severe effects on human health. Anthropogenic sources of PM2.5 include automobiles, factories, coal-burning power plants, and heaters in homes. It is well known that the size of dust particles decreases during long-range transport via westerly winds, and the resulting dust storms can contain high concentrations of fine particles. Accordingly, PM2.5 concentrations correspond well to both anthropogenic and dust aerosols. This work intends to investigate impacts of aerosol on regional climate change and environment over East Asia using observations and model simulations.

Temporal variability in aerosol characteristics and its radiative properties over Patiala, northwestern part of India: Impact of agricultural biomass burning emissions.

PubMed

Sharma, D; Srivastava, A K; Ram, K; Singh, A; Singh, D

2017-12-01

A comprehensive measurements of aerosol optical depth (AOD), particulate matter (PM) and black carbon (BC) mass concentrations have been carried out over Patiala, a semi-urban site in northwest India during October 2008 to September 2010. The measured aerosol data was incorporated in an aerosol optical model to estimate various aerosol optical parameters, which were subsequently used for radiative forcing estimation. The measured AOD at 500 nm (AOD 500 ) shows a significant seasonal variability, with maximum value of 0.81 during post-monsoon (PoM) and minimum of 0.56 during winter season. The Ångström exponent (α) has higher values (i.e. more fine-mode fraction) during the PoM/winter periods, and lower (i.e. more coarse-mode fraction) during pre-monsoon (PrM). In contrast, turbidity coefficient (β) exhibits an opposite trend to α during the study period. BC mass concentration varies from 2.8 to 13.9 μg m -3 (mean: 6.5 ± 3.2 μg m -3 ) during the entire study period, with higher concentrations during PoM/winter and lower during PrM/monsoon seasons. The average single scattering albedo (SSA at 500 nm) values are 0.70, 0.72, 0.82 and 0.75 during PoM, winter, PrM and monsoon seasons, respectively. However, inter-seasonal and inter-annual variability in measured aerosol parameters are statistically insignificant at Patiala. These results suggest strong changes in emission sources, aerosol composition, meteorological parameters as well as transport of aerosols over the station. Higher values of AOD, α and BC, along with lower SSA during PoM season are attributed to agriculture biomass burning emissions over and around the station. The estimated aerosol radiative forcing within the atmosphere is positive (i.e. warming) during all the seasons with higher values (∼60 Wm -2 ) during PoM-08/PoM-09 and lower (∼40 Wm -2 ) during winter-09/PrM-10. The present study highlights the role of BC aerosols from agricultural biomass burning emissions during post

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

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Li, X.; Bairai, S. T.; Renfro, J.; Liu, Y.; Liu, Y. J.; McKinney, K. A.; Martin, S. T.; McNeill, V. F.; Pye, H. O. T.; Nenes, A.; Neff, M. E.; Stone, E. A.; Mueller, S.; Knote, C.; Shaw, S. L.; Zhang, Z.; Gold, A.; Surratt, J. D.

2015-08-01

A suite of offline and real-time gas- and particle-phase measurements was deployed at Look 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) formation. High- and low-time-resolution PM2.5 samples were collected for analysis of known tracer compounds in isoprene-derived SOA by gas chromatography/electron ionization-mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography/diode array detection-electrospray ionization-high-resolution quadrupole time-of-flight mass spectrometry (UPLC/DAD-ESI-HR-QTOFMS). Source apportionment of the organic aerosol (OA) was determined by positive matrix factorization (PMF) analysis of mass spectrometric data acquired on an Aerodyne Aerosol Chemical Speciation Monitor (ACSM). Campaign average mass concentrations of the sum of quantified isoprene-derived SOA tracers contributed to ~ 9 % (up to 28 %) of the total OA mass, with isoprene-epoxydiol (IEPOX) chemistry accounting for ~ 97 % of the quantified tracers. PMF analysis resolved a factor with a profile similar to the IEPOX-OA factor resolved in an Atlanta study and was therefore designated IEPOX-OA. This factor was strongly correlated (r2 > 0.7) with 2-methyltetrols, C5-alkene triols, IEPOX-derived organosulfates, and dimers of organosulfates, confirming the role of IEPOX chemistry as the source. On average, IEPOX-derived SOA tracer mass was ~ 26 % (up to 49 %) of the IEPOX-OA factor mass, which accounted for 32 % of the total OA. A low-volatility oxygenated organic aerosol (LV-OOA) and an oxidized factor with a profile similar to 91Fac observed in areas where emissions are biogenic-dominated were also resolved by PMF analysis, whereas no primary organic aerosol (POA) sources could be resolved. These findings were consistent with low levels of primary pollutants, such as nitric oxide (NO ~ 0.03 ppb), carbon monoxide (CO ~ 116 ppb), and black

Changes in the physico-chemical properties of Amazonian aerosols from background conditions due to urban impacts in Central Amazonia.

NASA Astrophysics Data System (ADS)

Artaxo, P.; Barbosa, H. M.; Brito, J.; Carbone, S.; Fiorese, C.; Andre, B.; Rizzo, L. V.; Ditas, F.; Pöhlker, C.; Pöhlker, M. L.; Saturno, J.; Holanda, B. A.; Wang, J.; Souza, R. A. F. D.; Machado, L.; Andreae, M. O.; Martin, S. T.

2016-12-01

The GoAmazon 2014/15 experiment (Observations and Modeling of the Green Ocean Amazon) was a great opportunity to study how urbanization can change aerosol properties under pristine conditions in a tropical rain forest. The experiment took place from January 2014 to December 2015 in the vicinity of Manaus, Brazil, where several sampling stations were operated. Natural biogenic aerosol properties were studied in 3 sampling stations upwind of Manaus (ATTO (T0a), ZF2 (T0z) and EMBRAPA (T0e)). Urban impacted aerosols were analysed in two downwind sampling stations at Tiwa (T2) and Manacapuru (T3). Properties analysed were size distribution, scattering and absorption, composition, vertical profiles and others. Remote sensing measurements were done using AERONET and MODIS, while extensive ground based measurements were done in all sampling stations. Remote sensing measurements shows important changes in aerosol optical depth (AOD), especially in the aerosol absorption component. It was also observed a reduction in cloud droplet size downwind of Manaus for liquid phase clouds. Changes in particle number and size were also very significant, that reflected in changes in the aerosol radiative forcing (RF) before and after Manaus plume. In the dry season, an average RF of -24 w/m² was observed upwind, while -17 w/m² was observed downwind, due to large scale biomass burning aerosols. Single scattering albedo (SSA) at 550 nm changed from a high value of 0.96 upwind to 0.84 downwind due to the increase in absorbing aerosols in the wet season. In the dry season, SSA at 550nm changed from 0.95 to 0.87. Aerosol composition showed a large dominance of organic aerosols for all sites, accounting for 65-75% of PM1 non refractory aerosol. Most of these were secondary organic aerosol (SOA), with very low sulfate and nitrate concentrations. The influence of the Manaus plume on aerosol properties was more intense during the wet season, because in the dry season a significant amount of

Impact of Emissions and Long-Range Transport on Multi-Decadal Aerosol Trends: Implications for Air Quality and Climate

NASA Technical Reports Server (NTRS)

Chin, Mian

2012-01-01

We present a global model analysis of the impact of long-range transport and anthropogenic emissions on the aerosol trends in the major pollution regions in the northern hemisphere and in the Arctic in the past three decades. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze the multi-spatial and temporal scale data, including observations from Terra, Aqua, and CALIPSO satellites and from the long-term surface monitoring stations. We will analyze the source attribution (SA) and source-receptor (SR) relationships in North America, Europe, East Asia, South Asia, and the Arctic at the surface and free troposphere and establish the quantitative linkages between emissions from different source regions. We will discuss the implications for regional air quality and climate change.

OH-initiated Aging of Biomass Burning Aerosol during FIREX

NASA Astrophysics Data System (ADS)

Lim, C. Y.; Hagan, D. H.; Cappa, C. D.; Kroll, J. H.; Coggon, M.; Koss, A.; Sekimoto, K.; De Gouw, J. A.; Warneke, C.

2017-12-01

Biomass burning emissions represent a major source of fine particulate matter to the atmosphere, and this source will likely become increasingly important in the future due to changes in the Earth's climate. Understanding the effects that increased fire emissions have on both air quality and climate requires understanding the composition of the particles emitted, since chemical and physical composition directly impact important particle properties such as absorptivity, toxicity, and cloud condensation nuclei activity. However, the composition of biomass burning particles in the atmosphere is dynamic, as the particles are subject to the condensation of low-volatility vapors and reaction with oxidants such as the hydroxyl radical (OH) during transport. Here we present a series of laboratory chamber experiments on the OH-initiated aging of biomass burning aerosol performed at the Fire Sciences Laboratory in Missoula, MT as part of the Fire Influences on Regional and Global Environments Experiment (FIREX) campaign. We describe the evolution of biomass burning aerosol produced from a variety of fuels operating the chamber in both particle-only and gas + particle mode, focusing on changes to the organic composition. In particle-only mode, gas-phase biomass burning emissions are removed before oxidation to focus on heterogeneous oxidation, while gas + particle mode includes both heterogeneous oxidation and condensation of oxidized volatile organic compounds onto the particles (secondary organic aerosol formation). Variability in fuels and burning conditions lead to differences in aerosol loading and secondary aerosol production, but in all cases aging results in a significant and rapid increases in the carbon oxidation state of the particles.

CARBON MONOXIDE EMISSIONS FROM ROAD DRIVING: EVIDENCE OF EMISSIONS DUE TO POWER ENRICHMENT

EPA Science Inventory

The paper examines one aspect of motor vehicle emissions behavior; i.e. emissions due to engine power enrichment, a factor not well represented in existing models. Database reflecting 46 instrumented vehicles was used to analyze the importance of enrichment emissions to overall v...

Quantifying fire emissions and associated aerosols species using assimilation of satellite carbon monoxide retrievals.

NASA Astrophysics Data System (ADS)

Barre, J.; Edwards, D. P.; Worden, H. M.

2016-12-01

Wildfires tend to be more intense and hence costly and 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 concentration of carbon monoxide (CO) ever seen from space. Such larges fires impact not only the local environment but also affects 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 assimilation on the Washington and Indonesian fire cases studies will be diagnosed regarding the CO fire emissions, black and organic carbon inference using the ensemble information.

Transient climate and ambient health impacts due to national solid fuel cookstove emissions

PubMed Central

Lacey, Forrest G.; Henze, Daven K.; Lee, Colin J.; van Donkelaar, Aaron; Martin, Randall V.

2017-01-01

Residential solid fuel use contributes to degraded indoor and ambient air quality and may affect global surface temperature. However, the potential for national-scale cookstove intervention programs to mitigate the latter issues is not yet well known, owing to the spatial heterogeneity of aerosol emissions and impacts, along with coemitted species. Here we use a combination of atmospheric modeling, remote sensing, and adjoint sensitivity analysis to individually evaluate consequences of a 20-y linear phase-out of cookstove emissions in each country with greater than 5% of the population using solid fuel for cooking. Emissions reductions in China, India, and Ethiopia contribute to the largest global surface temperature change in 2050 [combined impact of −37 mK (11 mK to −85 mK)], whereas interventions in countries less commonly targeted for cookstove mitigation such as Azerbaijan, Ukraine, and Kazakhstan have the largest per cookstove climate benefits. Abatement in China, India, and Bangladesh contributes to the largest reduction of premature deaths from ambient air pollution, preventing 198,000 (102,000–204,000) of the 260,000 (137,000–268,000) global annual avoided deaths in 2050, whereas again emissions in Ukraine and Azerbaijan have the largest per cookstove impacts, along with Romania. Global cookstove emissions abatement results in an average surface temperature cooling of −77 mK (20 mK to −278 mK) in 2050, which increases to −118 mK (−11 mK to −335 mK) by 2100 due to delayed CO2 response. Health impacts owing to changes in ambient particulate matter with an aerodynamic diameter of 2.5 μm or less (PM2.5) amount to ∼22.5 million premature deaths prevented between 2000 and 2100. PMID:28115698

Light Absorption Properties and Radiative Effects of Primary Organic Aerosol Emissions

EPA Science Inventory

Organic aerosols (OA) in the atmosphere affect Earth’s energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called “brown carbon” (BrC) component. However, the absorptivities of OA are not or poorly represented in current climate m...

A HTAP Multi-Model 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, J. Jason; Atherton, Cynthia S.; Bellouin, Nicolas; Bergmann, Dan; Bey, Isabelle; Bian, Huisheng; Diehl, Thomas; Forberth, Gerd;

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.

Emissions of NO , TVOC, CO 2, and aerosols from a pilot-scale wastewater treatment plant with intermittent aeration

NASA Astrophysics Data System (ADS)

Schmid, Heidrun; Bauer, Heidi; Ellinger, Reinhard; Fuerhacker, Maria; Sree, Usha; Puxbaum, Hans

Atmospheric emissions from a pilot wastewater treatment plant performing aerobic and anoxic processes were investigated. The experiment was performed by sealing the whole aeration tank with an airtight cover of polyethylene in order to obtain a defined flow rate of the off-gas. By measuring concentrations in the known flux of the off-gas emission rates were determined. Due to the dimensions of the pilot plant and the air and water flows these emission rates represent upper limits. The emission rates were put into relation to CO 2 to obtain normalized data that can be used for emission inventories. Normalized emission rates (g component×g -1 CO 2) were 8.9×10 -3 for TVOC, 6.6×10 -6 for non-methane hydrocarbons C 2-C 7 (NMHC), 2.1×10 -5 for NO and 3.0×10 -6 for particulate organic carbon (POC). Emission rates per capita equivalent per year accounted at the most for 244 g C TVOC, 0.18 g C NMHC, 0.58 g NO and 0.08 g C POC on a basis of 27,400 g CO 2 per capita. The non-aeration periods also contributed to the production of NO and TVOC emissions of approximately one-third of the total emissions. From this, we conclude that the implementation of denitrification stages in European wastewater treatment plants according to the EU-directive 91/271/EEC will increase trace gas emissions in Europe. However, according to our estimates, emissions of trace gases and aerosols from wastewater treatment compared to anthropogenic sources will still remain very low.

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.

Aerosol composition and source apportionment in Santiago de Chile

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

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

Environment, Health and Climate: Impact of African aerosols

NASA Astrophysics Data System (ADS)

Liousse, C.; Doumbia, T.; Assamoi, E.; Galy-Lacaux, C.; Baeza, A.; Penner, J. E.; Val, S.; Cachier, H.; Xu, L.; Criqui, P.

2012-12-01

Fossil fuel and biofuel emissions of particles in Africa are expected to significantly increase in the near future, particularly due to rapid growth of African cities. In addition to biomass burning emissions prevailing in these areas, air quality degradation is then expected with important consequences on population health and climatic/radiative impact. In our group, we are constructing a new integrated methodology to study the relations between emissions, air quality and their impacts. This approach includes: (1) African combustion emission characterizations; (2) joint experimental determination of aerosol chemistry from ultrafine to coarse fractions and health issues (toxicology and epidemiology). (3) integrated environmental, health and radiative modeling. In this work, we show some results illustrating our first estimates of African anthropogenic emission impacts: - a new African anthropogenic emission inventory adapted to regional specificities on traffic, biofuel and industrial emissions has been constructed for the years 2005 and 2030. Biomass burning inventories were also improved in the frame of AMMA (African Monsoon) program. - carbonaceous aerosol radiative impact in Africa has been modeled with TM5 model and Penner et al. (2011) radiative code for these inventories for 2005 and 2030 and for two scenarios of emissions : a reference scenario, with no further emission controls beyond those achieved in 2003 and a ccc* scenario including planned policies in Kyoto protocol and regulations as applied to African emission specificities. In this study we will show that enhanced heating is expected with the ccc* scenarios emissions in which the OC fraction is relatively lower than in the reference scenario. - results of short term POLCA intensive campaigns in Bamako and Dakar in terms of aerosol chemical characterization linked to specific emissions sources and their inflammatory impacts on the respiratory tract through in vitro studies. In this study, organic

Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

NASA Technical Reports Server (NTRS)

Diehl, T. L.; Mian, Chin; Bond, T. C.; Carn, S. A.; Duncan, B. N.; Krotkov, N. A.; Streets, D. G.

2007-01-01

The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthopogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ATSR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

NASA Technical Reports Server (NTRS)

Diehl, Thomas L.; Chin, Mian; Bond, Tami C.; Carn, SImon A.; Duncan, Bryan N.; Krotkov, Nickolay A.; Streets, David G.

2006-01-01

The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthropogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ASTR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

The primary volcanic aerosol emission from Mt Etna: Size-resolved particles with SO2 and role in plume reactive halogen chemistry

NASA Astrophysics Data System (ADS)

Roberts, T. J.; Vignelles, D.; Liuzzo, M.; Giudice, G.; Aiuppa, A.; Coltelli, M.; Salerno, G.; Chartier, M.; Couté, B.; Berthet, G.; Lurton, T.; Dulac, F.; Renard, J.-B.

2018-02-01

Volcanoes are an important source of aerosols to the troposphere. Within minutes after emission, volcanic plume aerosol catalyses conversion of co-emitted HBr, HCl into highly reactive halogens (e.g. BrO, OClO) through chemical cycles that cause substantial ozone depletion in the dispersing downwind plume. This study quantifies the sub-to-supramicron primary volcanic aerosol emission (0.2-5 μm diameter) and its role in this process. An in-situ ground-based study at Mt Etna (Italy) during passive degassing co-deployed an optical particle counter and Multi-Gas SO2 sensors at high time resolution (0.1 Hz) enabling to characterise the aerosol number, size-distribution and emission flux. A tri-modal volcanic aerosol size distribution was found, to which lognormal distributions are fitted. Total particle volume correlates to SO2 (as a plume tracer). The measured particle volume:SO2 ratio equates to a sulfate:SO2 ratio of 1-2% at the observed meteorological conditions (40% Relative Humidity). A particle mass flux of 0.7 kg s-1 is calculated for the measured Mt Etna SO2 flux of 1950 tonnes/day. A numerical plume atmospheric chemistry model is used to simulate the role of the hygroscopic primary aerosol surface area and its humidity dependence on volcanic plume BrO and OClO chemistry. As well as predicting volcanic BrO formation and O3 depletion, the model achieves OClO/SO2 in broad quantitative agreement with recently reported Mt Etna observations, with a predicted maximum a few minutes downwind. In addition to humidity - that enhances aerosols surface area for halogen cycling - background ozone is predicted to be an important control on OClO/SO2. Dependence of BrO/SO2 on ambient humidity is rather low near-to-source but increases further downwind. The model plume chemistry also exhibits strong across-plume spatial variations between plume edge and centre.

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

PubMed

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

2005-05-01

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

Source apportionment of secondary organic aerosol in China using a regional source-oriented chemical transport model and two emission inventories.

PubMed

Wang, Peng; Ying, Qi; Zhang, Hongliang; Hu, Jianlin; Lin, Yingchao; Mao, Hongjun

2018-06-01

A Community Multiscale Air Quality (CMAQ) model with source-oriented lumped SAPRC-11 (S11L) photochemical mechanism and secondary organic aerosol (SOA) module was applied to determine the contributions of anthropogenic and biogenic sources to SOA concentrations in China. A one-year simulation of 2013 using the Multi-resolution Emission Inventory for China (MEIC) shows that summer SOA are generally higher (10-15 μg m -3 ) due to large contributions of biogenic (country average 60%) and industrial sources (17%). In winter, SOA formation was mostly due to anthropogenic emissions from industries (40%) and residential sources (38%). Emissions from other countries in southeast China account for approximately 14% of the SOA in both summer and winter, and 46% in spring due to elevated open biomass burning in southeast Asia. The Regional Emission inventory in ASia v2.1 (REAS2) was applied in this study for January and August 2013. Two sets of simulations with the REAS2 inventory were conducted using two different methods to speciate total non-methane carbon into model species. One approach uses total non-methane hydrocarbon (NMHC) emissions and representative speciation profiles from the SPECIATE database. The other approach retains the REAS2 speciated species that can be directly mapped to S11L model species and uses source specific splitting factors to map other REAS2 lumped NMHC species. Biogenic emissions are still the most significant contributor in summer based on these two sets of simulations. However, contributions from the transportation sector to SOA in January are predicted to be much more important based on the two REAS2 emission inventories (∼30-40% vs. ∼5% by MEIC), and contributions from residential sources according to REAS2 was much lower (∼21-24% vs. ∼42%). These discrepancies in source contributions to SOA need to be further investigated as the country seeks for optimal emission control strategies to fight severe air pollution. Copyright �

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

EPA Science Inventory

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

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

NASA Astrophysics Data System (ADS)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

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

Response of northern hemisphere environmental and atmospheric conditions to climate changes using Greenland aerosol records from the Eemian to the Holocene

NASA Astrophysics Data System (ADS)

Fischer, H.

2017-12-01

The Northern Hemisphere experienced dramatic climate changes over the last glacial cycle, including vast ice sheet expansion and frequent abrupt climate events. Moreover, high northern latitudes during the last interglacial (Eemian) were warmer than today and may provide guidance for future climate change scenarios. However, little evidence exists regarding the environmental alterations connected to these climate changes. Using aerosol concentration records in decadal resolution from the North Greenland Eemian Ice Drilling (NEEM) over the last 128,000 years we extract quantitative information on environmental changes, including the first comparison of northern hemisphere environmental conditions between the warmer than present Eemian and the early Holocene. Separating source changes from transport effects, we find that changes in the ice concentration greatly overestimate the changes in atmospheric concentrations in the aerosol source region, the latter mirroring changes in aerosol emissions. Glacial times were characterized by a strong reduction in terrestrial biogenic emissions (only 10-20% of the early Holocene value) reflecting the net loss of vegetated area in mid to high latitudes, while rapid climate changes during the glacial had essentially no effect on terrestrial biogenic aerosol emissions. An increase in terrestrial dust emissions of approximately a factor of eight during peak glacial and cold stadial intervals indicates higher aridity and dust storm activity in Asian deserts. Glacial sea salt aerosol emissions increased only moderately (by approximately 50%), likely due to sea ice expansion, while marked stadial/interstadial variations in sea salt concentrations in the ice reflect mainly changes in wet deposition en route. Eemian ice contains lower aerosol concentrations than ice from the early Holocene, due to shortened atmospheric residence time during the warmer Eemian, suggesting that generally 2°C warmer climate in high northern latitudes did not

Recent intensification of winter haze in China linked to foreign emissions and meteorology

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

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

Wintertime aerosol pollution in Northern China has increased over the past several decades as anthropogenic emissions in China have increased, and has increased dramatically since the beginning of the 21st century, but the causes and their quantitative contributions remain uncertain. Here we use an aerosol source tagging capability implemented in a global aerosol-climate model to assess long-term trends of PM2.5 (particulate matter less than 2.5 μm in diameter) in Northern China. Our analysis suggests that increasing PM2.5 concentrations due to local emission increases within China were obscured (~13%) by foreign emission reductions between 1980–2000. As foreign emissions stabilized during 2000-2014,more » their counteracting effect almost disappeared, uncovering China’s pollution potential from domestic emission increases. The meteorology dominated PM2.5 trend during 1990–1996 and also uncovered the pollution potential due to decadal variations in winds. The stabilized foreign emissions together with changing meteorology explain a quarter of the larger increasing trend of PM2.5 since the beginning of the 21st century. Future foreign emissions are not expected to help hiding China’s pollution, reductions in local emissions are the efficient way to improve future air quality in Northern China.« less

Recent intensification of winter haze in China linked to foreign emissions and meteorology

DOE PAGES

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

2018-02-01

Wintertime aerosol pollution in Northern China has increased over the past several decades as anthropogenic emissions in China have increased, and has increased dramatically since the beginning of the 21st century, but the causes and their quantitative contributions remain uncertain. Here we use an aerosol source tagging capability implemented in a global aerosol-climate model to assess long-term trends of PM2.5 (particulate matter less than 2.5 μm in diameter) in Northern China. Our analysis suggests that increasing PM2.5 concentrations due to local emission increases within China were obscured (~13%) by foreign emission reductions between 1980–2000. As foreign emissions stabilized during 2000-2014,more » their counteracting effect almost disappeared, uncovering China’s pollution potential from domestic emission increases. The meteorology dominated PM2.5 trend during 1990–1996 and also uncovered the pollution potential due to decadal variations in winds. The stabilized foreign emissions together with changing meteorology explain a quarter of the larger increasing trend of PM2.5 since the beginning of the 21st century. Future foreign emissions are not expected to help hiding China’s pollution, reductions in local emissions are the efficient way to improve future air quality in Northern China.« less

Polar and non-polar organic aerosols from large-scale agricultural-waste burning emissions in Northern India: Implications to organic mass-to-organic carbon ratio.

PubMed

Rajput, Prashant; Sarin, M M

2014-05-01

This study focuses on characteristics of organic aerosols (polar and non-polar) and total organic mass-to-organic carbon ratio (OM/OC) from post-harvest agricultural-waste (paddy- and wheat-residue) burning emissions in Northern India. Aerosol samples from an upwind location (Patiala: 30.2°N, 76.3°E) in the Indo-Gangetic Plain were analyzed for non-polar and polar fractions of organic carbon (OC1 and OC2) and their respective mass (OM1 and OM2). On average, polar organic aerosols (OM2) contribute nearly 85% of the total organic mass (OM) from the paddy- and wheat-residue burning emissions. The water-soluble-OC (WSOC) to OC2 ratio, within the analytical uncertainty, is close to 1 from both paddy- and wheat-residue burning emissions. However, temporal variability and relatively low WSOC/OC2 ratio (Av: 0.67±0.06) is attributed to high moisture content and poor combustion efficiency during paddy-residue burning, indicating significant contribution (∼30%) of aromatic carbon to OC2. The OM/OC ratio for non-polar (OM1/OC1∼1.2) and polar organic aerosols (OM2/OC2∼2.2), hitherto unknown for open agricultural-waste burning emissions, is documented in this study. The total OM/OC ratio is nearly identical, 1.9±0.2 and 1.8±0.2, from paddy- and wheat-residue burning emissions. Copyright © 2013 Elsevier Ltd. All rights reserved.

Linking Load, Fuel, and Emission Controls to Photochemical Production of Secondary Organic Aerosol from a Diesel Engine.

PubMed

Jathar, Shantanu H; Friedman, Beth; Galang, Abril A; Link, Michael F; Brophy, Patrick; Volckens, John; Eluri, Sailaja; Farmer, Delphine K

2017-02-07

Diesel engines are important sources of fine particle pollution in urban environments, but their contribution to the atmospheric formation of secondary organic aerosol (SOA) is not well constrained. We investigated direct emissions of primary organic aerosol (POA) and photochemical production of SOA from a diesel engine using an oxidation flow reactor (OFR). In less than a day of simulated atmospheric aging, SOA production exceeded POA emissions by an order of magnitude or more. Efficient combustion at higher engine loads coupled to the removal of SOA precursors and particle emissions by aftertreatment systems reduced POA emission factors by an order of magnitude and SOA production factors by factors of 2-10. The only exception was that the retrofitted aftertreatment did not reduce SOA production at idle loads where exhaust temperatures were low enough to limit removal of SOA precursors in the oxidation catalyst. Use of biodiesel resulted in nearly identical POA and SOA compared to diesel. The effective SOA yield of diesel exhaust was similar to that of unburned diesel fuel. While OFRs can help study the multiday evolution, at low particle concentrations OFRs may not allow for complete gas/particle partitioning and bias the potential of precursors to form SOA.

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

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Li, X.; Bairai, S. T.; Renfro, J.; Liu, Y.; Liu, Y. J.; McKinney, K. A.; Martin, S. T.; McNeill, V. F.; Pye, H. O. T.; Nenes, A.; Neff, M. E.; Stone, E. A.; Mueller, S.; Knote, C.; Shaw, S. L.; Zhang, Z.; Gold, A.; Surratt, J. D.

2015-03-01

A suite of offline and real-time gas- and particle-phase measurements was deployed at Look 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) formation. High- and low-time resolution PM2.5 samples were collected for analysis of known tracer compounds in isoprene-derived SOA by gas chromatography/electron ionization-mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography/diode array detection-electrospray ionization-high-resolution quadrupole time-of-flight mass spectrometry (UPLC/DAD-ESI-HR-QTOFMS). Source apportionment of the organic aerosol (OA) was determined by positive matrix factorization (PMF) analysis of mass spectrometric data acquired on an Aerodyne Aerosol Chemical Speciation Monitor (ACSM). Campaign average mass concentrations of the sum of quantified isoprene-derived SOA tracers contributed to ~9% (up to 26%) of the total OA mass, with isoprene-epoxydiol (IEPOX) chemistry accounting for ~97% of the quantified tracers. PMF analysis resolved a factor with a profile similar to the IEPOX-OA factor resolved in an Atlanta study and was therefore designated IEPOX-OA. This factor was strongly correlated (r2>0.7) with 2-methyltetrols, C5-alkene triols, IEPOX-derived organosulfates, and dimers of organosulfates, confirming the role of IEPOX chemistry as the source. On average, IEPOX-derived SOA tracer mass was ~25% (up to 47%) of the IEPOX-OA factor mass, which accounted for 32% of the total OA. A low-volatility oxygenated organic aerosol (LV-OOA) and an oxidized factor with a profile similar to 91Fac observed in areas where emissions are biogenic-dominated were also resolved by PMF analysis, whereas no primary organic aerosol (POA) sources could be resolved. These findings were consistent with low levels of primary pollutants, such as nitric oxide (NO~0.03ppb), carbon monoxide (CO~116 ppb), and black carbon (BC~0

Aerosol climate change effects on land ecosystem services.

PubMed

Unger, N; Yue, X; Harper, K L

2017-08-24

A coupled global aerosol-carbon-climate model is applied to assess the impacts of aerosol physical climate change on the land ecosystem services gross primary productivity (GPP) and net primary productivity (NPP) in the 1996-2005 period. Aerosol impacts are quantified on an annual mean basis relative to the hypothetical aerosol-free world in 1996-2005, the global climate state in the absence of the historical rise in aerosol pollution. We examine the separate and combined roles of fast feedbacks associated with the land and slow feedbacks associated with the ocean. We consider all fossil fuel, biofuel and biomass burning aerosol emission sources as anthropogenic. The effective radiative forcing for aerosol-radiation interactions is -0.44 W m -2 and aerosol-cloud interactions is -1.64 W m -2 . Aerosols cool and dry the global climate system by -0.8 °C and -0.08 mm per day relative to the aerosol-free world. Without aerosol pollution, human-induced global warming since the preindustrial would have already exceeded the 1.5 °C aspirational limit set in the Paris Agreement by the 1996-2005 decade. Aerosol climate impacts on the global average land ecosystem services are small due to large opposite sign effects in the tropical and boreal biomes. Aerosol slow feedbacks associated with the ocean strongly dominate impacts in the Amazon and North American Boreal. Aerosol cooling of the Amazon by -1.2 °C drives NPP increases of 8% or +0.76 ± 0.61 PgC per year, a 5-10 times larger impact than estimates of diffuse radiation fertilization by biomass burning aerosol in this region. The North American Boreal suffers GPP and NPP decreases of 35% due to aerosol-induced cooling and drying (-1.6 °C, -0.14 mm per day). Aerosol-land feedbacks play a larger role in the eastern US and Central Africa. Our study identifies an eco-climate teleconnection in the polluted earth system: the rise of the northern hemisphere mid-latitude reflective aerosol pollution layer causes long range

Aerosol beam-focus laser-induced plasma spectrometer device

DOEpatents

Cheng, Meng-Dawn

2002-01-01

An apparatus for detecting elements in an aerosol includes an aerosol beam focuser for concentrating aerosol into an aerosol beam; a laser for directing a laser beam into the aerosol beam to form a plasma; a detection device that detects a wavelength of a light emission caused by the formation of the plasma. The detection device can be a spectrometer having at least one grating and a gated intensified charge-coupled device. The apparatus may also include a processor that correlates the wavelength of the light emission caused by the formation of the plasma with an identity of an element that corresponds to the wavelength. Furthermore, the apparatus can also include an aerosol generator for forming an aerosol beam from bulk materials. A method for detecting elements in an aerosol is also disclosed.

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.

A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

NASA Technical Reports Server (NTRS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-01-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

A global modeling study on carbonaceous aerosol microphysical characteristics and radiative effects

NASA Astrophysics Data System (ADS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-08-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

Functional group composition of organic aerosol from combustion emissions and secondary processes at two contrasted urban environments

NASA Astrophysics Data System (ADS)

El Haddad, Imad; Marchand, Nicolas; D'Anna, Barbara; Jaffrezo, Jean Luc; Wortham, Henri

2013-08-01

The quantification of major functional groups in atmospheric organic aerosol (OA) provides a constraint on the types of compounds emitted and formed in atmospheric conditions. This paper presents functional group composition of organic aerosol from two contrasted urban environments: Marseille during summer and Grenoble during winter. Functional groups were determined using a tandem mass spectrometry approach, enabling the quantification of carboxylic (RCOOH), carbonyl (RCOR‧), and nitro (RNO2) functional groups. Using a multiple regression analysis, absolute concentrations of functional groups were combined with those of organic carbon derived from different sources in order to infer the functional group contents of different organic aerosol fractions. These fractions include fossil fuel combustion emissions, biomass burning emissions and secondary organic aerosol (SOA). Results clearly highlight the differences between functional group fingerprints of primary and secondary OA fractions. OA emitted from primary sources is found to be moderately functionalized, as about 20 carbons per 1000 bear one of the functional groups determined here, whereas SOA is much more functionalized, as in average 94 carbons per 1000 bear a functional group under study. Aging processes appear to increase both RCOOH and RCOR‧ functional group contents by nearly one order of magnitude. Conversely, RNO2 content is found to decrease with photochemical processes. Finally, our results also suggest that other functional groups significantly contribute to biomass smoke and SOA. In particular, for SOA, the overall oxygen content, assessed using aerosol mass spectrometer measurements by an O:C ratio of 0.63, is significantly higher than the apparent O:C* ratio of 0.17 estimated based on functional groups measured here. A thorough examination of our data suggests that this remaining unexplained oxygen content can be most probably assigned to alcohol (ROH), organic peroxides (ROOH

Impacts of Future Climate, Emission, and Land Use Changes on Aerosols and Air Quality over the Continental

EPA Science Inventory

Changes in climate, emission, and land use in the U.S. over the next century are imminent. The response of geologic, biogenic, and anthropogenic aerosol to interactions between these changes, however, are more uncertain and difficult to quantify. To explore these interactions, ...

Radiative Forcing Due to Enhancements in Tropospheric Ozone and Carbonaceous Aerosols Caused by Asian Fires During Spring 2008

NASA Technical Reports Server (NTRS)

Natarajan, Murali; Pierce, R. Bradley; Lenzen, Allen J.; Al-Saadi, Jassim A.; Soja, Amber J.; Charlock, Thomas P.; Rose, Fred G.; Winker, David M.; Worden, John R.

2012-01-01

Simulations of tropospheric ozone and carbonaceous aerosol distributions, conducted with the Real-time Air Quality Modeling System (RAQMS), are used to study the effects of major outbreaks of fires that occurred in three regions of Asia, namely Thailand, Kazakhstan, and Siberia, during spring 2008. RAQMS is a global scale meteorological and chemical modeling system. Results from these simulations, averaged over April 2008, indicate that tropospheric ozone column increases by more than 10 Dobson units (DU) near the Thailand region, and by lesser amounts in the other regions due to the fires. Widespread increases in the optical depths of organic and black carbon aerosols are also noted. We have used an off-line radiative transfer model to evaluate the direct radiative forcing due to the fire-induced changes in atmospheric composition. For clear sky, the monthly averaged radiative forcing at the top of the atmosphere (TOA) is mostly negative with peak values less than -12 W/sq m occurring near the fire regions. The negative forcing represents the increased outgoing shortwave radiation caused by scattering due to carbonaceous aerosols. At high latitudes, the radiative forcing is positive due to the presence of absorbing aerosols over regions of high surface albedo. Regions of positive forcing at TOA are more pronounced under total sky conditions. The monthly averaged radiative forcing at the surface is mostly negative, and peak values of less than -30 W/sq m occur near the fire regions. Persistently large negative forcing at the surface could alter the surface energy budget and potentially weaken the hydrological cycle.

Spatial and temporal variations of aerosols around Beijing in summer 2006: 2. Local and column aerosol optical properties

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Fast, J. D.; PöSchl, U.; Garland, R. M.; Andreae, M. O.; Wiedensohler, A.; Sugimoto, N.; Zhu, T.

2010-11-01

Model calculations were conducted using the Weather Research and Forecasting model coupled with chemistry (WRF-chem) for the region around Beijing, China, in the summer of 2006, when the CAREBeijing-2006 intensive campaign was conducted. In this paper, we interpret aerosol optical properties in terms of aerosol mass concentrations and their chemical compositions by linking model calculations with measurements. The model calculations generally captured the observed variability of various surface and column aerosol optical parameters in and around Beijing. At the surface, the spatial and temporal variations of aerosol absorption and scattering coefficients corresponded well to those of elemental carbon and sulfate mass concentrations, respectively, and were controlled by local-scale (<100 km and <24 hours) and regional-scale (<500 km and <3 days) emissions, respectively. The contribution of secondary aerosols and their water uptake increased with altitude within the planetary boundary layer. This variation led to a considerable increase in column aerosol optical depth and was responsible for the differences in regional and temporal variations between surface and column aerosol optical properties around Beijing. These processes are expected to be common in other megacity regions as well. Model calculations, however, underestimated or overestimated the absolute levels of aerosol optical properties in and around Beijing by up to 60%. Sensitivity studies showed that these discrepancies were mostly due to the uncertainties in aerosol mixing state and aerosol density (affecting mass extinction efficiency) in the model calculations. Good agreement with measurements is achieved when these aerosol properties are accurately predicted or assumed; however, significant bias can result when these properties are inadequately treated, even if total aerosol mass concentrations are reproduced well in the model calculations.

Evaluation of the health impact of aerosols emitted from different combustion sources: Comprehensive characterization of the aerosol physicochemical properties as well as the molecular biological and toxicological effects of the aerosols on human lung cells and macrophages.

NASA Astrophysics Data System (ADS)

Zimmermann, R.; Dittmar, G.; Kanashova, T.; Buters, J.; Öder, S.; Paur, H. R.; Mülhopt, S.; Dilger, M.; Weiss, C.; Harndorf, H.; Stengel, B.; Hirvonen, M. R.; Jokiniemi, J.; Hiller, K.; Sapcariu, S.; Sippula, O.; Streibel, T.; Karg, E.; Weggler, B.; Schnelle-Kreis, J.; Lintelmann, J.; Sklorz, M.; Orasche, J.; Müller, L.; Passig, J.; Gröger, T.; Jalava, P. I.; Happo, M.; Uski, O.

2016-12-01

A novel approach to evaluate the health effects of anthropogenic combustion emissions is the detailed comparison of comprehensive physicochemical data on the combustion aerosol properties with the biological response of aerosol-exposed lung cells. In this context the "HICE-Aerosol and Health" project consortium studies the properties as well as the biological and toxicological effects on lung cells induced by different combustion aerosol emissions (e.g. ship diesel exhaust, wood combustion effluents or automobile aerosol). Human alveolar epithelial cells (e.g. A549 cells) as well as murine macrophages were exposed to diluted emissions, using field deployable ALI-exposition systems in a mobile S2-biological laboratory. This allows a realistic lung-cell exposure by simulation of the lung situation. The cellular effects were then comprehensively characterized (cytotoxicology, transcriptomics, proteomics etc.) effects monitoring and put in context with the chemical and physical aerosol data. Emissions of wood combustion, a ship engine as well as diesel and gasoline engines were investigated. Furthermore for some experiments the atmospheric aging of the emission was simulated in a flow tube reactor using UV-light and ozone. Briefly the following order of cellular response-strength was observed: A relatively mild cellular effect is observed for the diluted wood combustion emissions, regardless if log-wood and pellet burner emissions are investigated. Similarly mild biological effects are observed for gasoline car emissions. The ship diesel engine emissions and construction machine diesel engine induced much more intense biological responses. A surprising result in this context is, that heavy fuel oil (HFO)-emissions show lower biological effect strengths than the supposedly cleaner diesel fuel emissions (DF). The HFO-emissions contain high concentrations of known toxicants (metals, polycyclic aromatics). This result was confirmed by experiments with murine macrophages

Evaluation of the health impact of aerosols emitted from different combustion sources: Comprehensive characterization of the aerosol physicochemical properties as well as the molecular biological and toxicological effects of the aerosols on human lung cells and macrophages.

NASA Astrophysics Data System (ADS)

Zimmermann, R.; Dittmar, G.; Kanashova, T.; Buters, J.; Öder, S.; Paur, H. R.; Mülhopt, S.; Dilger, M.; Weiss, C.; Harndorf, H.; Stengel, B.; Hirvonen, M. R.; Jokiniemi, J.; Hiller, K.; Sapcariu, S.; Sippula, O.; Streibel, T.; Karg, E.; Weggler, B.; Schnelle-Kreis, J.; Lintelmann, J.; Sklorz, M.; Orasche, J.; Müller, L.; Passig, J.; Gröger, T.; Jalava, P. I.; Happo, M.; Uski, O.

2017-12-01

A novel approach to evaluate the health effects of anthropogenic combustion emissions is the detailed comparison of comprehensive physicochemical data on the combustion aerosol properties with the biological response of aerosol-exposed lung cells. In this context the "HICE-Aerosol and Health" project consortium studies the properties as well as the biological and toxicological effects on lung cells induced by different combustion aerosol emissions (e.g. ship diesel exhaust, wood combustion effluents or automobile aerosol). Human alveolar epithelial cells (e.g. A549 cells) as well as murine macrophages were exposed to diluted emissions, using field deployable ALI-exposition systems in a mobile S2-biological laboratory. This allows a realistic lung-cell exposure by simulation of the lung situation. The cellular effects were then comprehensively characterized (cytotoxicology, transcriptomics, proteomics etc.) effects monitoring and put in context with the chemical and physical aerosol data. Emissions of wood combustion, a ship engine as well as diesel and gasoline engines were investigated. Furthermore for some experiments the atmospheric aging of the emission was simulated in a flow tube reactor using UV-light and ozone. Briefly the following order of cellular response-strength was observed: A relatively mild cellular effect is observed for the diluted wood combustion emissions, regardless if log-wood and pellet burner emissions are investigated. Similarly mild biological effects are observed for gasoline car emissions. The ship diesel engine emissions and construction machine diesel engine induced much more intense biological responses. A surprising result in this context is, that heavy fuel oil (HFO)-emissions show lower biological effect strengths than the supposedly cleaner diesel fuel emissions (DF). The HFO-emissions contain high concentrations of known toxicants (metals, polycyclic aromatics). This result was confirmed by experiments with murine macrophages

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.

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