Carbonaceous aerosols in the air masses transported from Indochina to Taiwan: Long-term observation at Mt. Lulin

NASA Astrophysics Data System (ADS)

Chuang, Ming-Tung; Lee, Chung-Te; Chou, Charles C.-K.; Lin, Neng-Huei; Sheu, Guey-Rong; Wang, Jia-Lin; Chang, Shuenn-Chin; Wang, Sheng-Hsiang; Chi, Kai Hsien; Young, Chea-Yuan; Huang, Hill; Chen, Horng-Wen; Weng, Guo-Hau; Lai, Sin-Yu; Hsu, Shao-Peng; Chang, Yu-Jia; Chang, Jia-Hon; Wu, Xyue-Chang

2014-06-01

Eight carbonaceous fractions from aerosols were resolved using the Interagency Monitoring of Protected Visual Environments (IMPROVE) protocol (Chow et al., 1993). The aerosols were collected at the Mountain Lulin Atmospheric Background Station (Mt. Lulin, 2862 m a.s.l.) in Central Taiwan from April 2003 to April 2012. The monthly and yearly levels of organic carbon (OC) and elemental carbon (EC) varied consistently with PM2.5 mass concentrations during biomass burning (BB) period. The highest monthly carbonaceous content was observed in March and the highest yearly carbonaceous concentration was observed in 2007. This finding is consistent with the BB activity in Indochina and indicates that carbonaceous content is a major component of BB aerosols. Lee et al. (2011) classified four trajectory groups from the air masses transported to Mt. Lulin during the aerosol collection period. For the air masses transported from the BB area (the BB group) in Indochina, the carbonaceous content was greater than the water-soluble ions in PM2.5, and the OC/EC ratio (4.8 ± 1.5) was high. With EC as the indicator of primary emission sources, the air masses of the BB group were found to contain more primary than secondary OC. The Anthropogenic group (from the local and free troposphere below the 700-hPa pressure level over the Asian continent) probably contained more secondary than primary OC or the sources of OC and EC could be quite diverse. The average char-EC/soot-EC (low-temperature EC/high-temperature EC) ratios were 3.9 ± 3.5, 0.4 ± 0.4, 0.9 ± 0.8, and 0.3 ± 0.4 for the trajectory groups BB, SNBB (from BB source areas during the non-BB period), Anthropogenic, and FT (from the oceanic area and the free troposphere above the 700-hPa pressure level over the Asian continent), respectively. The presence of a high char-EC/soot-EC ratio confirmed the correct classification of the BB group, whereas the low ratios from the other groups indicated the strong influence of vehicle

Assessment of the Aerosol Optics Component of the Coupled WRF-CMAQ Model usingCARES Field Campaign data and a Single Column Model

EPA Science Inventory

The Carbonaceous Aerosols and Radiative Effects Study (CARES), a field campaign held in central California in June 2010, provides a unique opportunity to assess the aerosol optics modeling component of the two-way coupled Weather Research and Forecasting (WRF) – Community Multisc...

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

Carbonaceous Aerosol Removal During Precipitation Events: Climate Implications

NASA Astrophysics Data System (ADS)

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

2009-12-01

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

[Study on pollution characteristics of carbonaceous aerosols in Xi'an City during the spring festival].

PubMed

Zhou, Bian-Hong; Zhang, Cheng-Zhong; Wang, Ge-Hui

2013-02-01

The samples of PM2.5 with 8 times periods were collected using Automated Cartridge Collection Unit (ACCU) of Rupprecht& Patashnick (R&P)Corporation, and monitored by R&P1400a instrument of TEOM series online during 2011 Spring Festival in Xi'an city. The organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and water-insoluble organic carbon (WIOC) contents of 3 h integrated PM2.5 were analyzed to evaluate the influence of firework display on the carbonaceous components in urban air. The mass concentration of PM2.5 was found increased significantly from 00:00 A. M. to 02:59 A. M. at the Chinese Lunar New Year's Eve than the non-firework periods, reaching 1514.8 microg.m-3 at 01:00 A. M. The mass concentrations of OC, EC, WSOC, and WIOC during the same time period were 123.3 microg.m-3, 18.6 microg.m-3, 66.7 microg.m-3, and 56.6 microg.m-3, about 1.7, 1.2, 1.4, and 2.2 times higher than the average in normal days, respectively. Correlation analysis among WSOC, OC, and EC contents in PM25 showed that firework emission was an obvious source of carbonaceous aerosol in the Spring Festival vacation. However, it only contributes to 9. 4% for aerosol in fireworks emission.

Sources of excess urban carbonaceous aerosol in the Pearl River delta region, China

EPA Science Inventory

Carbonaceous aerosol is one of the important constituents of fine particulate matter (PM2.5) in Southern China, including the Pearl River Delta (PRD) region and Hong Kong (HK). During the study period (October and December of 2002, and March and June of 2003), the monthly average...

Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

NASA Astrophysics Data System (ADS)

Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

2011-12-01

Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

Carbonaceous Aerosols Emitted from Light-Duty Vehicles Operating on Gasoline and Ethanol Fuel Blends

EPA Science Inventory

This study examines the chemical properties of carbonaceous aerosols emitted from three light-duty gasoline vehicles (LDVs) operating on gasoline (e0) and ethanol-gasoline fuel blends (e10 and e85). Vehicle road load simulations were performed on a chassis dynamometer using the t...

Characterization of carbonaceous aerosol by the stepwise-extraction thermal-optical-transmittance (SE-TOT) method

NASA Astrophysics Data System (ADS)

Cheng, Yuan; He, Ke-bin; Duan, Feng-kui; Du, Zhen-yu; Zheng, Mei; Ma, Yong-liang

2012-11-01

Carbonaceous aerosol collected in Beijing, China was characterized by a stepwise-extraction thermal-optical-transmittance (SE-TOT) method which allows for a quantitative separation of organic aerosol into distinct fractions. About 55% of the total organic carbon (OC) could be extracted by a mixture of hexane, methylene chloride and acetone. The extractable OC was further isolated into non-polar, low-polar and high-polar OC which constituted 10%, 23% and 22% of the total OC, respectively. The sum of low-polar and high-polar OC was found to coincide well with the secondary OC predicted by the elemental carbon tracer method, indicating that the low-polar and high-polar OC are strongly associated with secondary organic aerosol. Moreover, it was suggested that high relative humidity could enhance the production of high-polar OC through aqueous-phase reactions, because high-polar OC correlated strongly with oxalate and the ratio of high-polar OC to low-polar OC was significantly higher during the sampling events with high relative humidity (1.23 ± 0.35) comparing with results from the low relative humidity days (0.79 ± 0.23). In addition, the extractable OC was shown to be light-absorbing. The results of this study suggest that the SE-TOT method could provide new insights into the characterization of carbonaceous aerosol.

Quantifying the sources of atmospheric ice nuclei from carbonaceous combustion aerosol

NASA Astrophysics Data System (ADS)

Schill, G. P.; Jathar, S.; Galang, A.; Farmer, D.; Friedman, B.; Levin, E. J.; DeMott, P. J.; Kreidenweis, S. M.

2015-12-01

Ice nucleation on particles is a fundamental atmospheric process, which governs precipitation, cloud lifetimes, and climate. Despite being a basic atmospheric process, our current understanding of ice nucleation in the atmosphere is low. One reason for this low understanding is that ice nuclei concentrations are low (only ~1 in 105 particles in the free troposphere nucleate ice), making it challenging to identify both the composition and sources of ambient ice nuclei. Carbonaceous combustion aerosol produced from biomass and fossil fuel combustion are one potential source of these ice nuclei, as they contribute to over one-third of all aerosol in the North American free troposphere. Unfortunately, previous results from field measurements in-cloud, aircraft measurements, and laboratory studies are in conflict, with estimates of the impact of combustion aerosol ranging from no effect to rivaling the well-known atmospheric ice nuclei mineral dust. It is, however, becoming clear that aerosols from combustion processes are more complex than model particles, and their ice activity depends greatly on both fuel type and combustion conditions. Given these dependencies, we propose that sampling from real-world biomass burning and fossil fuel sources would provide the most useful new information on the contribution of carbonaceous combustion aerosols to atmospheric ice nuclei particles. To determine the specific contribution of refractory black carbon (rBC) to ice nuclei concentrations, we have coupled the Single Particle Soot Photometer (SP2) to the Colorado State University Continuous Flow Diffusion Chamber (CFDC). The SP2 utilizes laser-induced incandescence to quantify rBC mass on a particle-by-particle basis; in doing so, it also selectively destroys rBC particles by heating them to their vaporization temperature. Thus, the SP2 can be used as a selective pre-filter for rBC into the CFDC. In this work, we will present recent results looking at contribution of diesel

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.

Carbon isotope-constrained seasonality of carbonaceous aerosol sources from an urban location (Kanpur) in the Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Bikkina, Srinivas; Andersson, August; Ram, Kirpa; Sarin, M. M.; Sheesley, Rebecca J.; Kirillova, Elena N.; Rengarajan, R.; Sudheer, A. K.; Gustafsson, Örjan

2017-05-01

The Indo-Gangetic Plain (IGP) in northern India, Pakistan, and Bangladesh is a major source of carbonaceous aerosols in South Asia. However, poorly constrained seasonality of their sources over the IGP leads to large uncertainty in climate and health effects. Here we present a first data set for year-round radiocarbon (Δ14C) and stable carbon (δ13C)-based source apportionment of total carbon (TC) in ambient PM10 (n = 17) collected from an urban site (Kanpur: 26.5°N, 80.3°E) in the IGP during January 2007 to January 2008. The year-round 14C-based fraction biomass (fbio-TC) estimate at Kanpur averages 77 ± 7% and emphasizes an impact of biomass burning emissions (BBEs). The highest fbio-TC (%) is observed in fall season (October-November, 85 ± 6%) followed by winter (December-February, 80 ± 4%) and spring (March-May, 75 ± 8%), while lowest values are found in summer (June-September, 69 ± 2%). Since biomass/coal combustion and vehicular emissions mostly contribute to carbonaceous aerosols over the IGP, we predict δ13CTC (δ13Cpred) over Kanpur using known δ13C source signatures and the measured Δ14C value of each sample. The seasonal variability of δ13Cobs - δ13Cpred versus Δ14CTC together with air mass back trajectories and Moderate Resolution Imaging Spectroradiometer fire count data reveal that carbonaceous aerosols in winter/fall are significantly influenced by atmospheric aging (downwind transport of crop residue burning/wood combustion emissions in the northern IGP), while local sources (wheat residue combustion/vehicular emissions) dominate in spring/summer. Given the large temporal and seasonal variability in sources and emission strength of TC over the IGP, 14C-based constraints are, thus, crucial for reducing their uncertainties in carbonaceous aerosol budgets in climate models.

SOURCE APPORTIONMENT OF PRIMARY AND SECONDARY CARBONACEOUS AEROSOL IN THE UNITED STATES USING MODELS AND MEASUREMENTS

EPA Science Inventory

In this presentation, three diagnostic evaluation methods of model performance for carbonaceous aerosol are reviewed. The EC-tracer method is used to distinguish primary and secondary carbon, radiocarbon data are used to distinguish fossil-fuel and contemporary carbon, and organ...

The role of carbonaceous aerosols on short-term variations of precipitation over North Africa

DOE PAGES

Yoon, Jin -Ho; Rasch, Philip J.; Wang, Hailong; ...

2016-06-16

Northern Africa has been subject to extensive droughts in the late 20th century, which are frequently linked to changes in the Sea Surface Temperature (SST) in both the Atlantic and Indian Oceans. However, climate models forced by observed Sea Surface Temperatures have been unable to reproduce the magnitude of rainfall reduction over the last several decades. In this study, we propose that aerosol indirect effects (AIE) may be an important feedback mechanism to contribute this recent reduction. The climate model used here has a fully predictive aerosol life cycle. Results are presented for a set of sensitivity experiments designed tomore » distinguish the role of aerosol direct/semi-­direct and indirect effects on regional precipitation. Changes in cloud lifetime due to the presence of carbonaceous aerosols are proposed as a key mechanism to explain the reduced rainfall over the tropical and North Africa.« less

The role of carbonaceous aerosols on short-term variations of precipitation over North Africa

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

Yoon, Jin -Ho; Rasch, Philip J.; Wang, Hailong

Northern Africa has been subject to extensive droughts in the late 20th century, which are frequently linked to changes in the Sea Surface Temperature (SST) in both the Atlantic and Indian Oceans. However, climate models forced by observed Sea Surface Temperatures have been unable to reproduce the magnitude of rainfall reduction over the last several decades. In this study, we propose that aerosol indirect effects (AIE) may be an important feedback mechanism to contribute this recent reduction. The climate model used here has a fully predictive aerosol life cycle. Results are presented for a set of sensitivity experiments designed tomore » distinguish the role of aerosol direct/semi-­direct and indirect effects on regional precipitation. Changes in cloud lifetime due to the presence of carbonaceous aerosols are proposed as a key mechanism to explain the reduced rainfall over the tropical and North Africa.« less

Spatial variability of carbonaceous aerosol concentrations in East and West Jerusalem.

PubMed

von Schneidemesser, Erika; Zhou, Iiabin; Stone, Elizabeth A; Schauer, James I; Shpund, Jacob; Brenner, Shmuel; Qasrawi, Radwan; Abdeen, Ziad; Sarnat, Jeremy A

2010-03-15

Carbonaceous aerosol concentrations and sources were compared during a year long study at two sites in East and West Jerusalem that were separated by a distance of approximately 4 km. One in six day 24-h PM(2.5) elemental and organic carbon concentrations were measured, along with monthly average concentrations of particle-phase organic compound tracers for primary and secondary organic aerosol sources.Tracer compounds were used in a chemical mass balance ICMB) model to determine primary and secondary source contributions to organic carbon. The East Jerusalem sampling site at Al Quds University experienced higher concentrations of organic carbon (OC) and elemental carbon (EC) compared to the West Jerusalem site at Hebrew University. The annual average concentrations of OC and EC at the East Jerusalem site were 5.20 and 2.19 μg m(-3), respectively, and at the West Jerusalem site were 4.03 and 1.14 μg m(-3), respectively. Concentrations and trends of secondary organic aerosol and vegetative detritus were similar at both sites, but large differences were observed in the concentrations of organic aerosol from fossil fuel combustion and biomass burning, which was the cause of the large differences in OC and EC concentrations observed at the two sites.

Carbonaceous aerosol at two rural locations in New York State: Characterization and behavior

NASA Astrophysics Data System (ADS)

Sunder Raman, Ramya; Hopke, Philip K.; Holsen, Thomas M.

2008-06-01

Fine particle samples were collected to determine the chemical constituents in PM2.5 at two rural background sites (Potsdam and Stockton, N. Y.) in the northeastern United States from November 2002 to August 2005. Samples were collected every third day for 24 h with a speciation network sampler. The measured carbonaceous species included thermal-optical organic carbon (OC), elemental carbon (EC), pyrolytic carbon (OP), black carbon (BC), and water-soluble, short-chain (WSSC) organic acids. Concentration time series, autocorrelations, and seasonal variations of the carbonaceous species were examined. During this multiyear period, the contributions of the total carbon (OC + EC) to the measured fine particle mass were 31.2% and 31.1% at Potsdam and Stockton, respectively. The average sum of the WSSC acids carbon accounted for approximately 2.5% of the organic carbon at Potsdam and 3.0% at Stockton. At Potsdam, the seasonal differences in the autocorrelation function (ACF) and partial autocorrelation function (PACF) values for carbonaceous species suggest that secondary formation may be an important contributor to the observed concentrations of species likely to be secondary in origin, particularly during the photochemically active time of the year (May to October). This study also investigated the relationships between carbonaceous species to better understand the behavior of carbonaceous aerosol and to assess the contribution of secondary organic carbon (SOC) to the total organic carbon mass (the EC tracer method was used to estimate SOC). At Potsdam the average SOC contribution to total OC varied between 66% and 72%, while at Stockton it varied between 58% and 64%.

Temporal and diurnal variations of carbonaceous aerosols and major ions in biomass burning influenced aerosols over Mt. Tai in the North China Plain during MTX2006

NASA Astrophysics Data System (ADS)

Boreddy, Suresh K. R.; Kawamura, Kimitaka; Okuzawa, Kazuhiro; Kanaya, Yugo; Wang, Zifa

2017-04-01

To better understand the impact of agricultural waste burning on the air quality of free troposphere over the North China Plain (NCP), we collected total suspended particles (TSP) at the summit of Mt. Tai, located in the NCP using a high volume air sampler during 29 May to 28 June 2006, when the field burning of agricultural residue was intense. Temporal variations of all measured species showed that their concentration increases from late May to mid June (major BB period), peaking during 12-14 June, and then significantly decreased towards late June (minor BB period). We noticed that a significant reduction in the concentrations of carbonaceous aerosols during the period of 8-11 June, when the wind direction shifted from southerly to northerly. We found that concentrations of carbonaceous aerosols and some major ions showed several times higher during major BB period than those of minor BB period. We also found that nighttime concentrations are higher than daytime during major BB period, suggesting that a long-range atmospheric transport of biomass burning plumes in the free troposphere, which arrived at the summit of Mt. Tai. In contrast, daytime concentrations are higher than nighttime during minor BB period. We found higher concentrations of secondary organic carbon (SOC) during major BB period, suggesting that formation of secondary organic aerosols through aqueous phase chemistry under high NOx conditions during a long-range atmospheric transport. nss-K+ showed about four times higher concentrations during major BB than those of minor BB. Concentrations of nss-Ca2+ are higher in nighttime during major BB period, implying that a significant long-range atmospheric transport of mineral dust over the sampling site. These results are further supported by the positive matrix factorization (PMF) analysis, which showed that biomass burning was a major source for the carbonaceous aerosols followed by mineral dust sources over the summit of Mt. Tai.

Sources and characteristics of carbonaceous aerosols at Agra "World heritage site" and Delhi "capital city of India".

PubMed

Pipal, A S; Tiwari, S; Satsangi, P G; Taneja, Ajay; Bisht, D S; Srivastava, A K; Srivastava, M K

2014-01-01

Agra, one of the oldest cities "World Heritage site", and Delhi, the capital city of India are both located in the border of Indo-Gangetic Plains (IGP) and heavily loaded with atmospheric aerosols due to tourist place, anthropogenic activities, and its topography, respectively. Therefore, there is need for monitoring of atmospheric aerosols to perceive the scenario and effects of particles over northern part of India. The present study was carried out at Agra (AGR) as well as Delhi (DEL) during winter period from November 2011 to February 2012 of fine particulate (PM₂.₅: d < 2.5 μm) as well as associated carbonaceous aerosols. PM₂.₅ was collected at both places using medium volume air sampler (offline measurement) and analyzed for organic carbon (OC) and elemental carbon (EC). Also, simultaneously, black carbon (BC) was measured (online) at DEL. The average mass concentration of PM₂.₅ was 165.42 ± 119.46 μg m(-3) at AGR while at DEL it was 211.67 ± 41.94 μg m(-3) which is ~27% higher at DEL than AGR whereas the BC mass concentration was 10.60 μg m(-3). The PM₂.₅ was substantially higher than the annual standard stipulated by central pollution control board and United States Environmental Protection Agency standards. The average concentrations of OC and EC were 69.96 ± 34.42 and 9.53 ± 7.27 μm m(-3), respectively. Total carbon (TC) was 79.01 ± 38.98 μg m(-3) at AGR, while it was 50.11 ± 11.93 (OC), 10.67 ± 3.56 μg m(-3) (EC), and 60.78 ± 14.56 μg m(-3) (TC) at DEL. The OC/EC ratio was 13.75 at (AGR) and 5.45 at (DEL). The higher OC/EC ratio at Agra indicates that the formation of secondary organic aerosol which emitted from variable primary sources. Significant correlation between PM₂.₅ and its carbonaceous species were observed indicating similarity in sources at both sites. The average concentrations of secondary organic carbon (SOC) and primary organic carbon (POC) at AGR were 48.16 and 26

Satellite-Based Evidence of Wavelength-Dependent Aerosol Absorption in Biomass Burning Smoke Inferred from Ozone Monitoring Instrument

NASA Technical Reports Server (NTRS)

Jethva, H.; Torres, O.

2012-01-01

We provide satellite-based evidence of the spectral dependence of absorption in biomass burning aerosols over South America using near-UV measurements made by the Ozone Monitoring Instrument (OMI) during 2005-2007. In the current near-UV OMI aerosol algorithm (OMAERUV), it is implicitly assumed that the only absorbing component in carbonaceous aerosols is black carbon whose imaginary component of the refractive index is wavelength independent. With this assumption, OMI-derived aerosol optical depth (AOD) is found to be significantly over-estimated compared to that of AERONET at several sites during intense biomass burning events (August-September). Other well-known sources of error affecting the near-UV method of aerosol retrieval do not explain the large observed AOD discrepancies between the satellite and the ground-based observations. A number of studies have revealed strong spectral dependence in carbonaceous aerosol absorption in the near-UV region suggesting the presence of organic carbon in biomass burning generated aerosols. A sensitivity analysis examining the importance of accounting for the presence of wavelength-dependent aerosol absorption in carbonaceous particles in satellite-based remote sensing was carried out in this work. The results convincingly show that the inclusion of spectrally-dependent aerosol absorption in the radiative transfer calculations leads to a more accurate characterization of the atmospheric load of carbonaceous aerosols.

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Ferrare, R. A.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kassianov, E. I.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Kubátová, A.; Langford, A. O.; Laskin, A.; Laulainen, N.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Suski, K.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Worsnop, D. R.; Yu, X.-Y.; Zelenyuk, A.; Zhang, Q.

2012-08-01

Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Langford, A. O.; Laskin, A.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Yu, X.-Y.; Zelenyuk, A.; Zhang, Q.

2012-01-01

Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial results from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Technical Reports Server (NTRS)

Zaveri, R. A.; Shaw, W. J.; Cahill, J. F.; Cairns, Brian; Cappa, C. D.; Ottaviani, Matteo; Cziczo, D. J.; Ferrare, Richard A.; Alexander, M. L.; Alexandrov, Mikhail Dmitrievic;

Long-term (2001-2012) trends of carbonaceous aerosols from a remote island in the western North Pacific: an outflow region of Asian pollutants

NASA Astrophysics Data System (ADS)

Boreddy, Suresh K. R.; Mozammel Haque, M.; Kawamura, Kimitaka

2018-01-01

The present study reports on long-term trends of carbonaceous aerosols in total suspended particulate (TSP) samples collected at Chichijima in the western North Pacific during 2001-2012. Seasonal variations of elemental carbon (EC), organic carbon (OC), and water-soluble organic carbon (WSOC) concentrations showed maxima in winter to spring and minima in summer. These seasonal differences in the concentrations of carbonaceous aerosols were associated with the outflows of polluted air masses from East Asia, which are clearly distinguishable from pristine air masses from the central Pacific. The higher concentrations of carbonaceous aerosols during winter to spring are associated with long-range atmospheric transport of East Asian continental polluted air masses, whereas lower concentrations may be due to pristine air masses from the central Pacific in summer. The annual trends of OC / EC (+0.46 % yr-1), WSOC (+0.18 % yr-1) and WSOC / OC (+0.08 % yr-1) showed significant (p < 0.05) increases during the period of 2001-2012, suggesting that photochemical formation of WSOC and its contributions to secondary organic aerosols (SOAs) have increased over the western North Pacific via long-range atmospheric transport. We found a significant increase (+0.33 % yr-1) in nss-K+ / EC ratios, demonstrating that concentrations of biomass-burning-derived carbonaceous aerosols have increased, while those of primary fossil-fuel-derived aerosols have decreased over the western North Pacific. Further, secondary biogenic emissions are also important over the western North Pacific as inferred from a significant increase (+0.14 % yr-1) in the concentrations of methanesulfonate (MSA-, a tracer for biogenic sources). This point was further supported by a moderate correlation (r = 0.40) between WSOC and MSA-. We also found a significant increase in OC / TC (total carbon) and WSOC / TC ratios, further suggesting that photochemical formation of WSOC and its contributions to SOAs have increased

Comprehensive characterization of PM2.5 aerosols in Singapore

NASA Astrophysics Data System (ADS)

Balasubramanian, R.; Qian, W.-B.; Decesari, S.; Facchini, M. C.; Fuzzi, S.

2003-08-01

A comprehensive characterization of PM2.5 aerosols collected in Singapore from January through December 2000 is presented. The annual average mass concentration of PM2.5 was 27.2 μg/m3. The atmospheric loading of PM2.5 was elevated sporadically from March through May, mainly due to advection of biomass burning (deliberate fires to clear plantation areas) impacted air masses from Sumatra, Indonesia. Satellite images of the area, trajectory calculations, and surface wind direction data are in support of the transport of pyrogenic products from Sumatra toward Singapore. Aerosol samples collected during the dry season were analyzed for water-soluble ions, water-soluble organic compounds (WSOC), elemental carbon (EC), organic carbon, and trace elements using a number of analytical techniques. The major components were sulfate, EC, water-soluble carbonaceous materials, and water-insoluble carbonaceous materials. Aerosol WSOC were characterized based on a combination of chromatographic separations by ion exchange chromatography, functional group investigation by proton nuclear magnetic resonance, and total organic carbon determination. The comprehensive chemical characterization of PM2.5 particles revealed that both non-sea-salt sufate (nss-SO42-) and carbonaceous aerosols mainly contributed to the increase in the mass concentration of aerosols during the smoke haze period. Using a mass closure test (a mass balance), we determined whether the physical measurement of gravimetric fine PM concentration of a sample is equal to the summed concentrations of the individually identified chemical constituents (measured or inferred) in the sample. The sum of the determined groups of aerosol components and the gravimetrically determined mass agreed reasonably well. Principal component analysis was performed from the combined data set, and five factors were observed: a soil dust component, a metallurgical industry factor, a factor representing emissions from biomass burning and

Variability of carbonaceous aerosols in remote, rural, urban and industrial environments in Spain: implications for air quality policy

NASA Astrophysics Data System (ADS)

Querol, X.; Alastuey, A.; Viana, M.; Moreno, T.; Reche, C.; Minguillón, M. C.; Ripoll, A.; Pandolfi, M.; Amato, F.; Karanasiou, A.; Pérez, N.; Pey, J.; Cusack, M.; Vázquez, R.; Plana, F.; Dall'Osto, M.; de la Rosa, J.; Sánchez de la Campa, A.; Fernández-Camacho, R.; Rodríguez, S.; Pio, C.; Alados-Arboledas, L.; Titos, G.; Artíñano, B.; Salvador, P.; García Dos Santos, S.; Fernández Patier, R.

2013-07-01

We interpret here the variability of levels of carbonaceous aerosols based on a 12 yr database from 78 monitoring stations across Spain specially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m-3 of non-mineral carbon (nmC), mostly made of organic carbon (OC) with very little elemental carbon (EC), around 0.1 μg m-3; OC / EC = 12-15), to the highly polluted major cities (8-10 μg m-3 of nmC; 3-4 μg m-3 of EC; 4-5 μg m-3 of OC; OC / EC = 1-2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning and of biogenic emissions. Correlations between yearly averaged OC / EC and EC concentrations adjust very well to a potential equation (OC = 3.37 EC0.326, R2 = 0.8). A similar equation is obtained when including average concentrations obtained at other European sites (OC = 3.60EC0.491, R2 = 0.7). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance from road, traffic volume and density, mixing-layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend for

Variability of carbonaceous aerosols in remote, rural, urban and industrial environments in Spain: implications for air quality policy

NASA Astrophysics Data System (ADS)

Querol, X.; Alastuey, A.; Viana, M.; Moreno, T.; Reche, C.; Minguillón, M. C.; Ripoll, A.; Pandolfi, M.; Amato, F.; Karanasiou, A.; Pérez, N.; Pey, J.; Cusack, M.; Vázquez, R.; Plana, F.; Dall'Osto, M.; de la Rosa, J.; de la Campa Sánchez, A.; Fernández-Camacho, R.; Rodríguez, S.; Pío, C.; Alados-Arboledas, L.; Titos, G.; Artíñano, B.; Salvador, P.; Dos Santos García, S.; Patier Fernández, R.

2013-03-01

We interpret here the variability of levels of carbonaceous aerosols based on a 12-yr database from 78 monitoring stations across Spain especially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m-3 of non-mineral carbon (nmC), mostly made of organic carbon (OC), with very little elemental carbon (EC) 0.1 μg m-3; OC/EC = 12-15), to the highly polluted major cities (8-10 μg m-3 of nmC; 3-4 μg m-3 of EC; 4-5 μg m-3 of OC; OC/EC = 1-2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning. Correlations between yearly averaged OC/EC and EC concentrations adjust very well to a potential equation (OC/EC = 3.37 EC-0.67 R2 = 0.94). A similar equation is obtained when including average concentrations obtained at other European sites (y = 3.61x-0.5, R2 = 0.78). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance to road, traffic volume and density, mixing layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend of NO2/OC+EC ratios, because these

Radiative Effects of Carbonaceous and Inorganic Aerosols over California during CalNex and CARES: Observations versus Model Predictions

NASA Astrophysics Data System (ADS)

Vinoj, V.; Fast, J. D.; Liu, Y.

2012-12-01

Aerosols have been identified to be a major contributor to the uncertainty in understanding the present climate. Most of this uncertainty arises due to the lack of knowledge of their micro-physical and chemical properties as well as how to adequately represent their spatial and temporal distributions. Increased process level understanding can be achieved through carefully designed field campaigns and experiments. These measurements can be used to elucidate the aerosol properties, mixing, transport and transformation within the atmosphere and also to validate and improve models that include meteorology-aerosol-chemistry interactions. In the present study, the WRF-Chem model is used to simulate the evolution of carbonaceous and inorganic aerosols and their impact on radiation during May and June of 2010 over California when two field campaigns took place: the California Nexus Experiment (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES). We merged CalNex and CARES data along with data from operational networks such as, California Air Resources Board (CARB's) air quality monitoring network, the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, the AErosol RObotic NETwork (AERONET), and satellites into a common dataset for the Aerosol Modeling Test bed. The resulting combined dataset is used to rigorously evaluate the model simulation of aerosol mass, size distribution, composition, and optical properties needed to understand uncertainties that could affect regional variations in aerosol radiative forcing. The model reproduced many of the diurnal, multi-day, and spatial variations of aerosols as seen in the measurements. However, regionally the performance varied with reasonably good agreement with observations around Los Angeles and Sacramento and poor agreement with observations in the vicinity of Bakersfield (although predictions aloft were much better). Some aerosol species (sulfate and nitrate) were better represented

Feasibility study for GCOM-C/SGLI: Retrieval algorithms for carbonaceous aerosols

NASA Astrophysics Data System (ADS)

Mukai, Sonoyo; Sano, Itaru; Yasumoto, Masayoshi; Fujito, Toshiyuki; Nakata, Makiko; Kokhanovsky, Alexander

2016-04-01

The Japan Aerospace Exploration Agency (JAXA) has been developing the new Earth observing system, GCOM (Global Change Observation Mission) project, which consists of two satellite series of GCOM-W1 and GCOM-C1. The 1st GCOM-C satellite will board the SGLI (second generation global imager) which also includes polarimetric sensor and be planed to launch in early of 2017. The SGLI has multi (19)-channels including near UV channel (380 nm) and two polarization channels at red and near-infrared wavelengths of 670 and 870 nm. EUMETSAT plans to collect polarization measurements with a POLDER follow on 3MI / EPS-SG in 2021. Then the efficient retrieval algorithms for aerosol and/or cloud based on the combination use of radiance and polarization are strongly expected. This work focuses on serious biomass burning episodes in East Asia. It is noted that the near UV measurements are available for detection of the carbonaceous aerosols. The biomass burning aerosols (BBA) generated by forest fire and/or agriculture biomass burning have influenced on the severe air pollutions. It is known that the forest fire increases due to global warming and a climate change, and has influences on them vice versa. It is well known that this negative cycle decreases the quality of global environment and human health. We intend to consider not only retrieval algorithms of remote sensing for severe air pollutions but also detection and/or distinction of aerosols and clouds, because mixture of aerosols and clouds are often occurred in the severe air pollutions. Then precise distinction of aerosols and clouds, namely aerosols in cloudy scenes and/or clouds in heavy aerosol episode, is desired. Aerosol retrieval in the hazy atmosphere has been achieved based on radiation simulation method of successive order of scattering 1,2. In this work, we use both radiance and polarization measurements observed by GLI and POLDER-2 on Japanese ADEOS-2 satellite in 2003 as a simulated data. As a result the

Source apportionment of PM2.5 carbonaceous aerosol in Baghdad, Iraq

NASA Astrophysics Data System (ADS)

Hamad, Samera Hussein; Schauer, James Jay; Heo, Jongbae; Kadhim, Ahmed K. H.

2015-04-01

Baghdad is the second largest city in the Middle East and suffers from severe air quality degradation due to the high levels of the atmospheric particulate matter (PM). Limited information exists regarding the sources of PM in Baghdad, and the lack of information on sources inhibits the development of control strategies to reduce air pollution. To better understand the nature of fine particulate matter (PM2.5) in Baghdad and the Middle East, a one year sampling campaign to collect PM2.5 was conducted from September 2012 through September 2013, missing August 2013 samples due to the security situation. 24-hour integrated samples collected on a 1-in-6 day schedule were analyzed for the major components, and monthly average samples were analyzed by gas chromatography mass spectrometry (GCMS) methods to measure particle-phase organic molecular markers. The results of organic molecular markers were used in a chemical mass balance (CMB) model to quantify the sources of PM2.5 organic carbon (OC) and PM2.5 mass. Primary sources accounted for 44% of the measured PM2.5, and secondary sources were estimated to make up 28% of the measured PM2.5. Picene, a tracer of coal combustion detected in Baghdad where there is no evidence for coal combustion, can be attributed to burning crude oil and other low quality fuels in Baghdad. Source apportionment results showed that the dominant sources of the carbonaceous aerosols in Baghdad are gasoline (37 ± 6%) and diesel engines (17 ± 3%) which can be attributed to the extensive use of gasoline and diesel powered generators in Baghdad. Wood burning and residual oil combustion contributed to 5 ± 0.4 and 1 ± 0.2% respectively of OC. The unresolved sources contributed to 42 ± 19% of the OC which represented the secondary organic aerosol (SOA) and the unidentified sources.

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 variability of carbonaceous aerosols: Assessing the impact of biomass burning in the urban environment.

PubMed

Titos, G; Del Águila, A; Cazorla, A; Lyamani, H; Casquero-Vera, J A; Colombi, C; Cuccia, E; Gianelle, V; Močnik, G; Alastuey, A; Olmo, F J; Alados-Arboledas, L

2017-02-01

Biomass burning (BB) is a significant source of atmospheric particles in many parts of the world. Whereas many studies have demonstrated the importance of BB emissions in central and northern Europe, especially in rural areas, its impact in urban air quality of southern European countries has been sparsely investigated. In this study, highly time resolved multi-wavelength absorption coefficients together with levoglucosan (BB tracer) mass concentrations were combined to apportion carbonaceous aerosol sources. The Aethalometer model takes advantage of the different spectral behavior of BB and fossil fuel (FF) combustion aerosols. The model was found to be more sensitive to the assumed value of the aerosol Ångström exponent (AAE) for FF (AAE ff ) than to the AAE for BB (AAE bb ). As result of various sensitivity tests the model was optimized with AAE ff =1.1 and AAE bb =2. The Aethalometer model and levoglucosan tracer estimates were in good agreement. The Aethalometer model was further applied to data from three sites in Granada urban area to evaluate the spatial variation of CM ff and CM bb (carbonaceous matter from FF or BB origin, respectively) concentrations within the city. The results showed that CM bb was lower in the city centre while it has an unexpected profound impact on the CM levels measured in the suburbs (about 40%). Analysis of BB tracers with respect to wind speed suggested that BB was dominated by sources outside the city, to the west in a rural area. Distinguishing whether it corresponds to agricultural waste burning or with biomass burning for domestic heating was not possible. This study also shows that although traffic restrictions measures contribute to reduce carbonaceous concentrations, the extent of the reduction is very local. Other sources such as BB, which can contribute to CM as much as traffic emissions, should be targeted to reduce air pollution. Copyright © 2016 Elsevier B.V. All rights reserved.

Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

NASA Astrophysics Data System (ADS)

Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

2010-03-01

This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

NASA Astrophysics Data System (ADS)

Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

2016-04-01

The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle

Seasonal variation and light absorption property of carbonaceous aerosol in a typical glacier region of the southeastern Tibetan Plateau

NASA Astrophysics Data System (ADS)

Niu, Hewen; Kang, Shichang; Wang, Hailong; Zhang, Rudong; Lu, Xixi; Qian, Yun; Paudyal, Rukumesh; Wang, Shijin; Shi, Xiaofei; Yan, Xingguo

2018-05-01

Deposition and accumulation of light-absorbing carbonaceous aerosol on glacier surfaces can alter the energy balance of glaciers. In this study, 2 years (December 2014 to December 2016) of continuous observations of carbonaceous aerosols in the glacierized region of the Mt. Yulong and Ganhaizi (GHZ) basin are analyzed. The average elemental carbon (EC) and organic carbon (OC) concentrations were 1.51±0.93 and 2.57±1.32 µg m-3, respectively. Although the annual mean OC / EC ratio was 2.45±1.96, monthly mean EC concentrations during the post-monsoon season were even higher than OC in the high altitudes (approximately 5000 m a. s. l. ) of Mt. Yulong. Strong photochemical reactions and local tourism activities were likely the main factors inducing high OC / EC ratios in the Mt. Yulong region during the monsoon season. The mean mass absorption efficiency (MAE) of EC, measured for the first time in Mt. Yulong, at 632 nm with a thermal-optical carbon analyzer using the filter-based method, was 6.82±0.73 m2 g-1, comparable with the results from other studies. Strong seasonal and spatial variations of EC MAE were largely related to the OC abundance. Source attribution analysis using a global aerosol-climate model, equipped with a black carbon (BC) source tagging technique, suggests that East Asia emissions, including local sources, have the dominant contribution (over 50 %) to annual mean near-surface BC in the Mt. Yulong area. There is also a strong seasonal variation in the regional source apportionment. South Asia has the largest contribution to near-surface BC during the pre-monsoon season, while East Asia dominates the monsoon season and post-monsoon season. Results in this study have great implications for accurately evaluating the influences of carbonaceous matter on glacial melting and water resource supply in glacierization areas.

Assessment of carbonaceous aerosols in Shanghai, China - Part 1: long-term evolution, seasonal variations, and meteorological effects

NASA Astrophysics Data System (ADS)

Chang, Yunhua; Deng, Congrui; Cao, Fang; Cao, Chang; Zou, Zhong; Liu, Shoudong; Lee, Xuhui; Li, Jun; Zhang, Gan; Zhang, Yanlin

2017-08-01

Carbonaceous aerosols are major chemical components of fine particulate matter (PM2. 5) with major impacts on air quality, climate change, and human health. Gateway to fast-rising China and home of over twenty million people, Shanghai throbs as the nation's largest mega city and the biggest industrial hub. From July 2010 to December 2014, hourly mass concentrations of ambient organic carbon (OC) and elemental carbon (EC) in the PM2. 5 fraction were quasi-continuously measured in Shanghai's urban center. The annual OC and EC concentrations (mean ±1σ) in 2013 (8.9 ± 6.2 and 2.6 ± 2.1 µg m-3, n = 5547) and 2014 (7.8 ± 4.6 and 2.1 ± 1.6 µg m-3, n = 6914) were higher than those of 2011 (6.3 ± 4.2 and 2.4 ± 1.8 µg m-3, n = 8039) and 2012 (5.7 ± 3.8 and 2.0 ± 1.6 µg m-3, n = 4459). We integrated the results from historical field measurements (1999-2012) and satellite observations (2003-2013), concluding that carbonaceous aerosol pollution in Shanghai has gradually reduced since 2006. In terms of monthly variations, average OC and EC concentrations ranged from 4.0 to 15.5 and from 1.4 to 4.7 µg m-3, accounting for 13.2-24.6 and 3.9-6.6 % of the seasonal PM2. 5 mass (38.8-94.1 µg m-3), respectively. The concentrations of EC (2.4, 2.0, 2.2, and 3.0 µg m-3 in spring, summer, fall, and winter, respectively) showed little seasonal variation (except in winter) and weekend-weekday dependence, indicating EC is a relatively stable constituent of PM2. 5 in the Shanghai urban atmosphere. In contrast to OC (7.3, 6.8, 6.7, and 8.1 µg m-3 in spring, summer, fall, and winter, respectively), EC showed marked diurnal cycles and correlated strongly with CO across all seasons, confirming vehicular emissions as the dominant source of EC at the targeted site. Our data also reveal that both OC and EC showed concentration gradients as a function of wind direction (WD) and wind speed (WS), generally with higher values associated with winds from the southwest, west, and northwest

Sources and formation mechanisms of carbonaceous aerosol at a regional background site in the Netherlands: insights from a year-long radiocarbon study

NASA Astrophysics Data System (ADS)

Dusek, Ulrike; Hitzenberger, Regina; Kasper-Giebl, Anne; Kistler, Magdalena; Meijer, Harro A. J.; Szidat, Sönke; Wacker, Lukas; Holzinger, Rupert; Röckmann, Thomas

2017-03-01

We measured the radioactive carbon isotope 14C (radiocarbon) in various fractions of the carbonaceous aerosol sampled between February 2011 and March 2012 at the Cesar Observatory in the Netherlands. Based on the radiocarbon content in total carbon (TC), organic carbon (OC), water-insoluble organic carbon (WIOC), and elemental carbon (EC), we estimated the contribution of major sources to the carbonaceous aerosol. The main source categories were fossil fuel combustion, biomass burning, and other contemporary carbon, which is mainly biogenic secondary organic aerosol material (SOA). A clear seasonal variation is seen in EC from biomass burning (ECbb), with lowest values in summer and highest values in winter, but ECbb is a minor fraction of EC in all seasons. WIOC from contemporary sources is highly correlated with ECbb, indicating that biomass burning is a dominant source of contemporary WIOC. This suggests that most biogenic SOA is water soluble and that water-insoluble carbon stems mainly from primary sources. Seasonal variations in other carbon fractions are less clear and hardly distinguishable from variations related to air mass history. Air masses originating from the ocean sector presumably contain little carbonaceous aerosol from outside the Netherlands, and during these conditions measured carbon concentrations reflect regional sources. In these situations absolute TC concentrations are usually rather low, around 1.5 µg m-3, and ECbb is always very low ( ˜ 0.05 µg m-3), even in winter, indicating that biomass burning is not a strong source of carbonaceous aerosol in the Netherlands. In continental air masses, which usually arrive from the east or south and have spent several days over land, TC concentrations are on average by a factor of 3.5 higher. ECbb increases more strongly than TC to 0.2 µg m-3. Fossil EC and fossil WIOC, which are indicative of primary emissions, show a more moderate increase by a factor of 2.5 on average. An interesting case is

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

NASA Astrophysics Data System (ADS)

Fountoukis, Christos; Megaritis, Athanasios G.; Skyllakou, Ksakousti; Charalampidis, Panagiotis E.; Denier van der Gon, Hugo A. C.; Crippa, Monica; Prévôt, André S. H.; Fachinger, Friederike; Wiedensohler, Alfred; Pilinis, Christodoulos; Pandis, Spyros N.

2016-03-01

We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 µg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

NASA Astrophysics Data System (ADS)

Fountoukis, C.; Megaritis, A. G.; Skyllakou, K.; Charalampidis, P. E.; Denier van der Gon, H. A. C.; Crippa, M.; Prévôt, A. S. H.; Freutel, F.; Wiedensohler, A.; Pilinis, C.; Pandis, S. N.

2015-09-01

We use a three dimensional regional chemical transport model (PMCAMx) with high grid resolution and high resolution emissions (4 km × 4 km) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (Megacities: Emissions, urban, regional, and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 μg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 μg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 μg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

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

Davidovits, Paul

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign andmore » much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol

Sources of non-fossil-fuel emissions in carbonaceous aerosols during early winter in Chinese cities

NASA Astrophysics Data System (ADS)

Liu, Di; Li, Jun; Cheng, Zhineng; Zhong, Guangcai; Zhu, Sanyuan; Ding, Ping; Shen, Chengde; Tian, Chongguo; Chen, Yingjun; Zhi, Guorui; Zhang, Gan

2017-09-01

China experiences frequent and severe haze outbreaks from the beginning of winter. Carbonaceous aerosols are regarded as an essential factor in controlling the formation and evolution of haze episodes. To elucidate the carbon sources of air pollution, source apportionment was conducted using radiocarbon (14C) and unique molecular organic tracers. Daily 24 h PM2. 5 samples were collected continuously from October 2013 to November 2013 in 10 Chinese cities. The 14C results indicated that non-fossil-fuel (NF) emissions were predominant in total carbon (TC; average = 65 ± 7 %). Approximately half of the EC was derived primarily from biomass burning (BB) (average = 46 ± 11 %), while over half of the organic carbon (OC) fraction comprised NF (average = 68 ± 7 %). On average, the largest contributor to TC was NF-derived secondary OC (SOCnf), which accounted for 46 ± 7 % of TC, followed by SOC derived from fossil fuels (FF) (SOCf; 16 ± 3 %), BB-derived primary OC (POCbb; 13 ± 5 %), POC derived from FF (POCf; 12 ± 3 %), EC derived from FF (ECf; 7 ± 2 %) and EC derived from BB (ECbb; 6 ± 2 %). The regional background carbonaceous aerosol composition was characterized by NF sources; POCs played a major role in northern China, while SOCs contributed more in other regions. However, during haze episodes, there were no dramatic changes in the carbon source or composition in the cities under study, but the contribution of POC from both FF and NF increased significantly.

Direct radiative effect of carbonaceous aerosols from crop residue burning during the summer harvest season in East China

NASA Astrophysics Data System (ADS)

Yao, Huan; Song, Yu; Liu, Mingxu; Archer-Nicholls, Scott; Lowe, Douglas; McFiggans, Gordon; Xu, Tingting; Du, Pin; Li, Jianfeng; Wu, Yusheng; Hu, Min; Zhao, Chun; Zhu, Tong

2017-04-01

East China experiences extensive crop residue burnings in fields during harvest season. The direct radiative effect (DRE) of carbonaceous aerosols from crop residue burning in June 2013 in East China was investigated using the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem). Absorption of organic aerosol (OA) in the presence of brown carbon was considered using the parameterization of Saleh et al. (2014), in which the imaginary part of the OA refractive index is a function of wavelength and the ratio of black carbon (BC) and OA. The carbonaceous emissions from crop fires were estimated using the Moderate Resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) product with a localized crop-burning-sourced BC-to-organic carbon (OC) ratio emission ratio of 0.27. Evaluation of the model results with in situ measurements of particulate matter with aerodynamic diameter less than 2.5 µm (PM2. 5) chemical composition, MODIS aerosol optical depth (AOD) detections and meteorological observations showed that this model was able to reproduce the magnitude, spatial variation and optical characteristics of carbonaceous aerosol pollution. The observed BC and OC peak concentrations at the site in Suixi, Anhui province, during the 2013 wheat burning season reached 55.3 µg m-3 and 157.9 µg m-3. WRF-Chem simulations reproduced these trends with a correlation coefficient of 0.74, estimating that crop residue burning contributed 86 and 90 % of peak BC and OC, respectively. The simulated hourly DRE from crop residue burning at the top of atmosphere (TOA) reached a maximum of +22.66 W m-2 at the Suixi site. On average, the simulations showed that the crop residue burning introduced a net positive DRE of +0.14 W m-2 at TOA throughout East China, with BC from this source as the main heating contributor (+0.79 W m-2). The OA DRE from crop burning (-0.22 W m-2) was a combined effect of the positive DRE of absorption (+0.21 W m-2) and a stronger

Characteristics and sources of the fine carbonaceous aerosols in Haikou, China

NASA Astrophysics Data System (ADS)

Liu, Baoshuang; Zhang, Jiaying; Wang, Lu; Liang, Danni; Cheng, Yuan; Wu, Jianhui; Bi, Xiaohui; Feng, Yinchang; Zhang, Yufen; Yang, Haihang

2018-01-01

Ambient PM2.5 samples were collected from January to September 2015 in Haikou. The carbonaceous fractions included OC, EC, OC1, OC2, OC3, OC4, EC1, EC2, EC3, Char-EC (EC1 minus POC) and Soot-EC (EC2 plus EC3) were analysed in this study. The results indicate that the mean concentrations of OC and EC are 5.6 and 2.5 μg/m3 during the sampling period, respectively; and the concentrations of most of carbonaceous fractions are the highest in winter and the lowest in spring. The seasonal variations of Soot-EC and Char-EC concentrations show distinct differences. The concentrations of Char-EC are higher in winter and lower in spring; while those of Soot-EC are lower in winter and higher in summer. Compared to Char-EC, the concentrations of Soot-EC show smaller seasonal-variation in Haikou. The Char-EC has the higher correlations with OC and EC (r = 0.91 and 0.95, P < 0.01), while the correlation between the Soot-EC and either OC or EC is absent (r = 0.15 and 0.11, P > 0.05). The average ratios of Char-EC/Soot-EC are in the order of winter (15.9) > autumn (4.9) > summer (4.0) > spring (3.6), with an average value of 7.1. According to error estimation (EE) diagnostics analysis, four factors are revealed in Positive Matrix Factorization (PMF) analysis during each season. The combined gasoline/diesel vehicle exhaust, coal combustion, biomass burning and specific diesel vehicle exhaust are identified as the major sources of carbonaceous aerosols, and their contributions during the whole year are up to 29.3%, 27.4%, 17.9% and 15.9%, respectively. The transport trajectories of the air masses illustrate distinct differences during different seasons, and the transport trajectories are mainly derived from the mainland China (i.e. Jiangxi, Fujian and Guangdong provinces) in winter, likely caused by higher contribution of coal combustion.

Carbonaceous aerosols emitted from light-duty vehicles operating on gasoline and ethanol fuel blends.

PubMed

Hays, Michael D; Preston, William; George, Barbara J; Schmid, Judy; Baldauf, Richard; Snow, Richard; Robinson, James R; Long, Thomas; Faircloth, James

2013-12-17

This study examines the chemical properties of carbonaceous aerosols emitted from three light-duty gasoline vehicles (LDVs) operating on gasoline (e0) and ethanol-gasoline fuel blends (e10 and e85). Vehicle road load simulations were performed on a chassis dynamometer using the three-phase LA-92 unified driving cycle (UDC). Effects of LDV operating conditions and ambient temperature (-7 and 24 °C) on particle-phase semivolatile organic compounds (SVOCs) and organic and elemental carbon (OC and EC) emissions were investigated. SVOC concentrations and OC and EC fractions were determined with thermal extraction-gas chromatography-mass spectrometry (TE-GC-MS) and thermal-optical analysis (TOA), respectively. LDV aerosol emissions were predominantly carbonaceous, and EC/PM (w/w) decreased linearly with increasing fuel ethanol content. TE-GC-MS analysis accounted for up to 4% of the fine particle (PM2.5) mass, showing the UDC phase-integrated sum of identified SVOC emissions ranging from 0.703 μg km(-1) to 18.8 μg km(-1). Generally, higher SVOC emissions were associated with low temperature (-7 °C) and engine ignition; mixed regression models suggest these emissions rate differences are significant. Use of e85 significantly reduced the emissions of lower molecular weight PAH. However, a reduction in higher molecular weight PAH entities in PM was not observed. Individual SVOC emissions from the Tier 2 LDVs and fuel technologies tested are substantially lower and distributed differently than those values populating the United States emissions inventories currently. Hence, this study is likely to influence future apportionment, climate, and air quality model predictions that rely on source combustion measurements of SVOCs in PM.

Urban impacts on regional carbonaceous aerosols: case study in central Texas.

PubMed

Barrett, Tate E; Sheesley, Rebecca J

2014-08-01

Rural and background sites provide valuable information on the concentration and optical properties of organic, elemental, and water-soluble organic carbon (OC, EC, and WSOC), which are relevant for understanding the climate forcing potential of regional atmospheric aerosols. To quantify climate- and air quality-relevant characteristics of carbonaceous aerosol in the central United States, a regional background site in central Texas was chosen for long-term measurement. Back trajectory (BT) analysis, ambient OC, EC, and WSOC concentrations and absorption parameters are reported for the first 15 months of a long-term campaign (May 2011-August 2012). BT analysis indicates consistent north-south airflow connecting central Texas to the Central Plains. Central Texas aerosols exhibited seasonal trends with increased fine particulate matter (< 2.5 microm aerodynamic diameter, PM2.5) and OC during the summer (PM2.5 = 10.9 microg m(-3) and OC = 3.0 microg m(-3)) and elevated EC during the winter (0.22 microg m(-3)). When compared to measurements in Dallas and Houston, TX, central Texas OC appears to have mixed urban and rural sources. However central Texas EC appears to be dominated by transport of urban emissions. WSOC averaged 63% of the annual OC, with little seasonal variability in this ratio. To monitor brown carbon (BrC), absorption was measured for the aqueous WSOC extracts. Light absorption coefficients for EC and BrC were highest during summer (EC MAC = 11 m2 g(-1) and BRC MAE365 = 0.15 m2 g(-1)). Results from optical analysis indicate that regional aerosol absorption is mostly due to EC with summertime peaks in BrC attenuation. This study represents the first reported values of WSOC absorption, MAE365, for the central United States. Implications: Background concentration and absorption measurements are essential in determining regional potential radiative forcing due to atmospheric aerosols. Back trajectory, chemical, and optical analysis of PM2.5 was used to

Day-night differences in the composition and sources of carbonaceous aerosol at a polluted regional background site in the Netherlands

NASA Astrophysics Data System (ADS)

Dusek, Ulrike; Broekema, Elise; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro

2017-04-01

The origin of carbonaceous aerosol differs during day- and night-time, because emissions from major sources such as traffic, biomass combustion, and secondary organic aerosol formation show a distinct diurnal pattern. Moreover, photochemical processing and evaporation of semi-volatile organic compounds are enhanced during day-time, due to the availability of sunlight and higher temperatures. Assessing day-night differences in sources and chemical composition can give an indication of the importance of local/regional carbon sources and processing, since day-night differences should be averaged out during long-range transport. If local sources dominate, one could expect a strong diurnal variation in the source profile, but if long-range transport dominates the diurnal variation would be much weaker. In this study we measure the isotopic (14C and 13C) and detailed chemical composition of the organic fraction of the aerosol on high volume PM2.5 filter samples that were collected separately during day and night time. Radiocarbon (14C) measurements are used to estimate three main aerosol sources of organic and elemental carbon (OC and EC): Fossil fuel combustion (ff), biomass combustion (bb), and biogenic sources (bio). The detailed chemical and stable isotopic composition are measured at different desorption temperatures from the filter, which separates the more and less refractory organic compounds. The composition of the organic aerosol is measured using an thermal-desporption Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) method (Holzinger et al, 2010) and the stable isotopic composition is measured using a thermal desorption IRMS method (Dusek et al., 2013). Source apportionment results using 14C show that the contribution of fossil fuel combustion to EC and OC is higher during day-time than during night-time. This is valid for all seasons. During night-time biomass combustion plays a bigger role as a source of carbonaceous aerosol. Even in

Inorganic markers, carbonaceous components and stable carbon isotope from biomass burning aerosols in northeast China

NASA Astrophysics Data System (ADS)

Cao, F.; Zhang, Y.; Kawamura, K.

2015-12-01

To better characterize the sources of fine particulate matter (i.e. PM2.5) in Sanjiang Plain, Northeast China, aerosol chemical composition such total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied as well as stable carbon isotopic composition (δ13C) of TC. Intensively open biomass burning episodes were identified from late September to early October by satellite fire and aerosol optical depth maps. During the biomass burning episodes, concentrations of PM2.5, OC, EC, and WSOC increased by a factor of 4-12 compared to non-biomass-burning periods. Non-sea-salt potassium is strongly correlated with PM2.5, OC, EC and WSOC, suggesting an important contribution of biomass burning emission. The enrichment in both the non-sea-salt potassium and chlorine is significantly larger than other inorganic species, indicating that biomass burning aerosols in Sanjiang Plain is mostly fresh and less aged. In addition, WSOC to OC ratio is relatively lower compared to that reported in biomass burning aerosols in tropical regions, supporting that biomass burning aerosols in Sanjiang Plain is mostly primary and secondary organic aerosols is not significant. A lower average δ13C value (-26.2‰) is found for the biomass-burning aerosols, suggesting a dominant contribution from combustion of C3 plants in the studied region.

Source apportionment of carbonaceous aerosol in Sao Paulo using 13C and 14C measurements

NASA Astrophysics Data System (ADS)

Oyama, Beatriz; Andrade, Maria de Fatima; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro A. J.; Dusek, Ulrike

2016-04-01

The Metropolitan Area of Sao Paulo is affected by high aerosol concentrations, which contain a large fraction of organic material. Up to date, not much is known about the composition and origin of the organic aerosol in this city. We present the first source apportionment of the carbonaceous aerosol fraction in Sao Paulo, using stable (13C) and radioactive carbon isotopes (14C). 14C provides a clear-cut distinction between fossil sources, which contain no 14C, and contemporary sources such as biofuels, biomass burning, or biogenic sources, which contain a typical contemporary 14C/12C ratio. 13C can be used to distinguish C3 plants, such as maize and sugarcane, from C4 plants. This can help to identify a possible impact of sugarcane field burning in the rural areas of Sao Paulo State on the aerosol carbon in the city. In the first part of the study, we compare two tunnel studies: Tunnel 1 is frequented only by light duty vehicles, which run mainly on mixtures of gasoline with ethanol (gasohol, 25% ethanol and 85% gasoline) or hydrated ethanol (5% water and 95% ethanol). Tunnel 2 contains a significant fraction of heavy-duty diesel vehicles, and therefore the fraction of biofuels in the average fleet is lower. Comparison of 14C in organic and elemental carbon (OC and EC) shows that in both tunnels there is no significant contribution of biofuels to EC. Combusting ethanol-gasoline fuels in a vehicle engine does apparently not result in significant EC formation from ethanol. Biofuels contribute around 45% to OC in Tunnel 1 an only 20% in Tunnel 2, reflecting a strong impact of diesel vehicles in Tunnel 2. In the second part of the study we conduct a source apportionment of ambient aerosol carbon collected in a field study during winter (July-August) 2012. Ambient EC has two main sources, vehicular emissions and biomass burning. We estimate a contribution of vehicular sources to EC of roughly 90% during weekdays and 80% during weekends, using the 14C values measured in

Carbonaceous aerosols in the Western Mediterranean during summertime and their contribution to the aerosol optical properties at ground level: First results of the ChArMEx-ADRIMED 2013 intensive campaign in Corsica

NASA Astrophysics Data System (ADS)

Sciare, Jean; Dulac, Francois; Feron, Anais; Crenn, Vincent; Sarda Esteve, Roland; Baisnee, Dominique; Bonnaire, Nicolas; Hamonou, Eric; Mallet, Marc; Lambert, Dominique; Nicolas, Jose B.; Bourrianne, Thierry; Petit, Jean-Eudes; Favez, Olivier; Canonaco, Francesco; Prevot, Andre; Mocnik, Grisa; Drinovec, Luka; Marpillat, Alexandre; Serrie, Wilfrid

2014-05-01

As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx, http://charmex.lsce.ipsl.fr/), the CORSiCA (http://www.obs-mip.fr/corsica) and the ANR-ADRIMED programs, a large set of real-time measurements of carbonaceous aerosols was deployed in June 2013 at the Cape Corsica atmospheric supersite (http://gaw.empa.ch/gawsis/reports.asp?StationID=2076203042). Submicron organic aerosols (OA) were monitored every 30 min using an Aerosol Chemical Speciation Monitor (ACSM; Aerodyne Res. Inc. MA, USA); Fine (PM2.5) Organic Carbon (OC) and Elemental Carbon (EC) were measured every 2h using an OCEC Sunset Field Instrument (Sunset Lab, OR, USA) and every 12h using a low-vol (Leckel) filter sampler running at 2.3m3/h. Equivalent Black Carbon (BC) was monitored using two Aethalometers (models AE31 and AE33, Magee Scientific, US & Aerosol d.o.o., Slovenia) and a MAAP instrument (Thermo). Quality control of this large dataset was performed through chemical mass closure studies (using co-located SMPS and TEOM-FDMS) and direct comparisons with other real-time instruments running in parallel (Particle-Into-Liquid-Sampler-Ion-Chromatograph for ions, filter sampling, ...). Source apportionment of OA was then performed using the SourceFinder software (SoFi v4.5, http://www.psi.ch/acsm-stations/me-2) allowing the distinction between hydrogen- and oxygen-like organic aerosols (HOA and OOA, respectively) and highlighting the major contribution of secondary OA in the Western Mediterranean during summer. Using this time-resolved chemical information, reconstruction of the optical aerosol properties were performed and compared with integrating nephelometer (Model 3563, TSI, US) and photoacoustic extinctiometer (PAX, DMT, US) measurements performed in parallel. Results of these different closure studies (chemical/physical/optical) are presented and discussed here in details. They highlight the central role of carbonaceous aerosols on the optical properties of aerosols at ground level

Remote sensing of aerosols by synergy of caliop and modis

NASA Astrophysics Data System (ADS)

Kudo, Rei; Nishizawa, Tomoaki; Higurashi, Akiko; Oikawa, Eiji

2018-04-01

For the monitoring of the global 3-D distribution of aerosol components, we developed the method to retrieve the vertical profiles of water-soluble, light absorbing carbonaceous, dust, and sea salt particles by the synergy of CALIOP and MODIS data. The aerosol product from the synergistic method is expected to be better than the individual products of CALIOP and MODIS. We applied the method to the biomass-burning event in Africa and the dust event in West Asia. The reasonable results were obtained; the much amount of the water-soluble and light absorbing carbonaceous particles were estimated in the biomass-burning event, and the dust particles were estimated in the dust event.

Carbonaceous content of atmospheric aerosols in Lisbon urban atmosphere

NASA Astrophysics Data System (ADS)

Mirante, Fátima; Oliveira, C.; Martins, N.; Pio, C.; Caseiro, A.; Cerqueira, M.; Alves, C.; Oliveira, C.; Oliveira, J.; Camões, F.; Matos, M.; Silva, H.

2010-05-01

Lisbon is the capital city of Portugal with about 565,000 residents and a population density of 6,600 inhabitants per square kilometre. The town is surrounded by satellite cities, forming together a region known as "Lisbon Metropolitan Area" with about 3 million inhabitants. It is estimated that more than one million citizens come into the Lisbon area every day from the outskirts, leading to elevated traffic densities and intense traffic jams. Airborne particulate matter limit values are frequently exceeded, with important consequences on air pollution levels and obvious negative impacts on human health. Atmospheric aerosols are known to have in their structure significant amounts of carbonaceous material. The knowledge of the aerosols carbon content, particularly on their several carbon forms (as TC, EC and OC, meaning respectively Total, Elemental and Organic carbon) is often required to provide information for source attribution. In order to assess the vehicles PM input, two sampling campaigns (summer and winter periods) were carried out in 2008 in Lisbon in two contrasting sites, a roadside and an urban background site. Particulate matter was collected in two fractions on quartz fibre filters using Hi-Vol samplers (coarse fraction, 2.5µmaerosol sampling campaign was also performed inside an open and a closed tunnel on four size fractions (PM0.49, PM0.49-0.95, PM0.95-2.5 and PM2.5-10). Road dust was also collected in each sampling site. Samples were analysed for elemental carbon (EC) and organic carbon (OC) concentrations by a thermal-optical method. The urban site presented the highest aerosol PM concentrations for the two size ranges, with PM10 average values of about 48 µg.m-3 and 27 µg.m-3 respectively for the roadside and urban background sites in the summer period, and about 44 µg.m-3 and 27 µg.m-3 in the winter season. In general, the concentrations of TC were higher

Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode in 2013

NASA Astrophysics Data System (ADS)

Zhang, Y.-L.; Huang, R.-J.; El Haddad, I.; Ho, K.-F.; Cao, J.-J.; Han, Y.; Zotter, P.; Bozzetti, C.; Daellenbach, K. R.; Canonaco, F.; Slowik, J. G.; Salazar, G.; Schwikowski, M.; Schnelle-Kreis, J.; Abbaszade, G.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.; Szidat, S.

2014-10-01

During winter 2013, extremely high concentrations (i.e. 4-20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) were reported in several large cities in China. In this work, source apportionment of fine carbonaceous aerosols during this haze episode was conducted at four major cities in China including Xian, Beijing, Shanghai and Guangzhou. An effective statistical analysis of a combined dataset from elemental carbon (EC) and organic carbon (OC), radiocarbon (14C) and biomass-burning marker measurements using Latin-hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. We found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% at all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xian (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was rather from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10% and 48 ± 9% of OC and TC, respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8%, 48 ± 18%, 53 ± 4% and 65 ± 26% of non-fossil OC for Xian, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass-burning were mainly attributed to formation of secondary organic carbon

Estimation of the contributions of long range transported aerosol in East Asia to carbonaceous aerosol and PM concentrations in Seoul, Korea using highly time resolved measurements: a PSCF model approach.

PubMed

Jeong, Ukkyo; Kim, Jhoon; Lee, Hanlim; Jung, Jinsang; Kim, Young J; Song, Chul H; Koo, Ja-Ho

2011-07-01

The contributions of long range transported aerosol in East Asia to carbonaceous aerosol and particulate matter (PM) concentrations in Seoul, Korea were estimated with potential source contribution function (PSCF) calculations. Carbonaceous aerosol (organic carbon (OC) and elemental carbon (EC)), PM(2.5), and PM(10) concentrations were measured from April 2007 to March 2008 in Seoul, Korea. The PSCF and concentration weighted trajectory (CWT) receptor models were used to identify the spatial source distributions of OC, EC, PM(2.5), and coarse particles. Heavily industrialized areas in Northeast China such as Harbin and Changchun and East China including the Pearl River Delta region, the Yangtze River Delta region, and the Beijing-Tianjin region were identified as high OC, EC and PM(2.5) source areas. The conditional PSCF analysis was introduced so as to distinguish the influence of aerosol transported from heavily polluted source areas on a receptor site from that transported from relatively clean areas. The source contributions estimated using the conditional PSCF analysis account for not only the aerosol concentrations of long range transported aerosols but also the number of transport days effective on the measurement site. Based on the proposed algorithm, the condition of airmass pathways was classified into two types: one condition where airmass passed over the source region (PS) and another condition where airmass did not pass over the source region (NPS). For most of the seasons during the measurement period, 249.5-366.2% higher OC, EC, PM(2.5), and coarse particle concentrations were observed at the measurement site under PS conditions than under NPS conditions. Seasonal variations in the concentrations of OC, EC, PM(2.5), and coarse particles under PS, NPS, and background aerosol conditions were quantified. The contributions of long range transported aerosols on the OC, EC, PM(2.5), and coarse particle concentrations during several Asian dust events were

Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-04-01

Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and

Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-09-01

Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal

Classifying aerosol type using in situ surface spectral aerosol optical properties

NASA Astrophysics Data System (ADS)

Schmeisser, Lauren; Andrews, Elisabeth; Ogren, John A.; Sheridan, Patrick; Jefferson, Anne; Sharma, Sangeeta; Kim, Jeong Eun; Sherman, James P.; Sorribas, Mar; Kalapov, Ivo; Arsov, Todor; Angelov, Christo; Mayol-Bracero, Olga L.; Labuschagne, Casper; Kim, Sang-Woo; Hoffer, András; Lin, Neng-Huei; Chia, Hao-Ping; Bergin, Michael; Sun, Junying; Liu, Peng; Wu, Hao

2017-10-01

Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE), absorption Ångström exponent (AAE) and single scattering albedo (SSA) from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes.Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type) and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station.The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol), marine polluted (carbonaceous aerosol mixed with sea salt) and continental dust/biomass sites

Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July-August 2001: a multi-analytical approach

NASA Astrophysics Data System (ADS)

Sciare, J.; Cachier, H.; Oikonomou, K.; Ausset, P.; Sarda-Estève, R.; Mihalopoulos, N.

2003-07-01

During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T=550°C) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) concentrations were on average respectively 1.19±0.56 and 3.62±1.08 μgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 μgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope = 1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between

Carbonaceous and inorganic aerosols over a sub-urban site in peninsular India: Temporal variability and source characteristics

NASA Astrophysics Data System (ADS)

Aswini, A. R.; Hegde, Prashant; Nair, Prabha R.

2018-01-01

PM10 aerosol samples collected from a sub-urban site in Coimbatore during pre-monsoon, monsoon, post-monsoon and winter from 2014 to 2016 showed a large variability from 7.6 to 89 μg m- 3 with an annual average of 41 ± 21 μg m- 3 (N = 69). High abundance of PM10 and other components were recorded during winter and lowest during monsoon period. Total carbonaceous aerosols and water soluble ionic species contributed to 31% and 45% of PM10 mass respectively. SO42 - was the most abundant species (average 9.8 ± 4.8 μg m- 3) and constituted for 24% of total mass. Organic Carbon (OC) was the next most abundant species ranging from 1 to 16 μg m- 3 with an average of 7 ± 3.6 μg m- 3 accounting for 17% of PM10 mass concentration. POC (primary organic carbon) and SOC (secondary organic carbon) accounted for 56% and 44% of OC respectively. A major portion of OC ( 60%) was found to be water soluble. The correlation between OC and EC (elemental carbon) was found to be higher for night-time compared to daytime suggesting their origin from common sources during night-time. K+ was found to be strongly correlated with OC during night-time. WSOC showed good correlation with POC and K+ which was high especially during night-time. WSON (water soluble organic nitrogen) accounted for 34% of water soluble total nitrogen (WSTN). HCO3- exhibited significant positive correlation with Ca2 + during daytime indicating their crustal origin. The observations suggest that the region is influenced by biomass burning sources, however during day-time, secondary production and terrestrial sources (due to high temperature and wind) significantly influence the atmospheric aerosols over this region.

Nature and origin of the resistant carbonaceous polymorphs involved the fossilization of biogenic soil-aggregates

NASA Astrophysics Data System (ADS)

Courty, M.-A.

2012-04-01

which are all finely imbricated with phosphides, phosphates, sulphides, sulphates and native metals (Fe-Cr-Ni and Fe-Cr alloys, Ni, Al, Cu, Zn, Pb, As, Sn, Ag, Au, Bi). The 3D observations show that the carbonaceous filaments play a major role in the cohesion of the fine fraction. The carbonaceous components only start to decompose under HF attack and from 400°C heating. They do not display evidence of microbial degradation. The biogenic aggregates with high amount of carbonaceous polymorphs appear to have resisted to cryoturbation and to hard setting under water saturation. Biogenic micro-aggregates from present-day top soils only contain rare exotic components. In contrast to the ones of the soil archives, they display highly variable structural stability depending upon local edaphic conditions. The exotic assemblage of the stable biogenic micro-aggregates from the soil archives is shown to be similar to the range of terrestrial aerosols that are associated to meteor explosion (Courty et al., this volume). This suggests that the fossilized organic-rich surface horizons in soil archives would trace singular situations possibly marked by recurrent meteor explosion with high stratospheric aerosol production. Mechanisms explaining how the dual stratospheric/cosmic processes formed resistant carbon species from fossil combustible precursors yet remain to be investigated. Courty, Benoît and Vaillant (2012). Possible interaction of meteor explosion with stratospheric aerosols on cloud nucleation based on 2011 observations. Geophysical Research Abstracts Vol. 14, EGU2012.

Individual Aerosol Particles from Biomass Burning in Southern Africa. 1; Compositions and Size Distributions of Carbonaceous Particles

NASA Technical Reports Server (NTRS)

Posfai, Mihaly; Simonics, Renata; Li, Jia; Hobbs, Peter V.; Buseck, Peter R.

2003-01-01

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July August 2001: a multi-analytical approach

NASA Astrophysics Data System (ADS)

Sciare, J.; Cachier, H.; Oikonomou, K.; Ausset, P.; Sarda-Estève, R.; Mihalopoulos, N.

2003-10-01

During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T>550ºC) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) mass concentrations were on average respectively 1.19±0.56 and 3.62±1.08 mgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 mgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope=1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these

Inorganic markers, carbonaceous components and stable carbon isotope from biomass burning aerosols in Northeast China.

PubMed

Cao, Fang; Zhang, Shi-Chun; Kawamura, Kimitaka; Zhang, Yan-Lin

2016-12-01

To better characterize the chemical compositions and sources of fine particulate matter (i.e. PM 2.5 ) in Sanjiang Plain, Northeast China, total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions as well as stable carbon isotopic composition (δ 13 C) were measured in this study. Intensively open biomass burning episodes are identified from late September to early October by satellite fire and aerosol optical depth maps. During the biomass-burning episode, concentrations of PM 2.5 , OC, EC, and WSOC are increased by a factor of 4-12 compared to those during the non-biomass-burning period. Non-sea-salt potassium is strongly correlated with PM 2.5 , OC, EC and WSOC, demonstrating an important contribution from biomass-burning emissions. The enrichment in both the non-sea-salt potassium and chlorine is significantly larger than other inorganic species, suggesting that biomass-burning aerosols in Sanjiang Plain are mostly fresh and less aged. In addition, the WSOC-to-OC ratio is lower than that reported in biomass-burning aerosols in tropical regions, further supporting that biomass-burning aerosols in Sanjiang Plain are mostly primary and secondary organic aerosols may be not significant. A lower average δ 13 C value (-26.2‰) is observed during the biomass-burning period, indicating a dominant contribution from combustion of C3 plants in the studied region. Copyright © 2015. Published by Elsevier B.V.

Time-resolved measurements of PM2.5 carbonaceous aerosols at Gosan, Korea.

PubMed

Batmunkh, T; Kim, Y J; Lee, K Y; Cayetano, M G; Jung, J S; Kim, S Y; Kim, K C; Lee, S J; Kim, J S; Chang, L S; An, J Y

2011-11-01

In order to better understand the characteristics of atmospheric carbonaceous aerosol at a background site in Northeast Asia, semicontinuous organic carbon (OC) and elemental carbon (EC), and time-resolved water-soluble organic carbon (WSOC) were measured by a Sunset OC/ EC and a PILS-TOC (particle-into-liquid sampler coupled with an online total organic carbon) analyzer, respectively, at the Gosan supersite on Jeju Island, Korea, in the summer (May 28-June 17) and fall (August 24-September 30) of 2009. Hourly average OC concentration varied in the range of approximately 0.87-28.38 microgC m-3, with a mean of 4.07+/- 2.60 microgC m-3, while the hourly average EC concentration ranged approximately from 0.04 to 8.19 .microgC m-3, with a mean of 1.35 +/- 0.71 microgC m-3, from May 28 to June 17, 2009. During the fall season, OC varied in the approximate range 0.9-9.6 microgC m-3, with a mean of 2.30 +/-0.80 microgC m-3, whereas EC ranged approximately from 0.01 to 5.40 microgC m-3, with a mean of 0.66 +/- 0.38 microgC m-3. Average contributions of EC to TC and WSOC to OC were 26.0% +/- 9.7% and 20.6% +/-7.4%, and 37.6% +/- 23.5% and 57.2% +/- 22.2% during summer and fall seasons, respectively. As expected, clear diurnal variation of WSOC/OC was found in summer, varying from 0.22 during the nighttime up to 0.72 during the daytime, mainly due to the photo-oxidation process. In order to investigate the effect of air mass pathway on the characteristics of carbonaceous aerosol, 5-day back-trajectory analysis was conducted using the HYSPLIT model. The air mass pathways were classified into four types: Continental (CC), Marine (M), East Sea (ES) and Korean Peninsula (KP). The highest OC/EC ratio of 3.63 was observed when air mass originated from the Continental area (CC). The lowest OC/EC ratio of 0.79 was measured when air mass originated from the Marine area (M). A high OC concentration was occasionally observed at Gosan due to local biomass burning activities. The

Retrieving Smoke Aerosol Height from DSCOVR/EPIC

NASA Astrophysics Data System (ADS)

Xu, X.; Wang, J.; Wang, Y.

2017-12-01

Unlike industrial pollutant particles that are often confined within the planetary boundary layer, smoke from forest and agriculture fires can inject massive carbonaceous aerosols into the upper troposphere due to the intense pyro-convection. Sensitivity of weather and climate to absorbing carbonaceous aerosols is regulated by the altitude of those aerosol layers. However, aerosol height information remains limited from passive satellite sensors. Here we present an algorithm to estimate smoke aerosol height from radiances in the oxygen A and B bands measured by the Earth Polychromatic Imaging Camera (EPIC) from the Deep Space Climate Observatory (DSCOVR). With a suit of case studies and validation efforts, we demonstrate that smoke aerosol height can be well retrieved over both ocean and land surfaces multiple times daily.

Composition and sources of carbonaceous aerosols in Northern Europe during winter

NASA Astrophysics Data System (ADS)

Glasius, M.; Hansen, A. M. K.; Claeys, M.; Henzing, J. S.; Jedynska, A. D.; Kasper-Giebl, A.; Kistler, M.; Kristensen, K.; Martinsson, J.; Maenhaut, W.; Nøjgaard, J. K.; Spindler, G.; Stenström, K. E.; Swietlicki, E.; Szidat, S.; Simpson, D.; Yttri, K. E.

2018-01-01

Sources of elemental carbon (EC) and organic carbon (OC) in atmospheric aerosols (carbonaceous aerosols) were investigated by collection of weekly aerosol filter samples at six background sites in Northern Europe (Birkenes, Norway; Vavihill, Sweden; Risoe, Denmark; Cabauw and Rotterdam in The Netherlands; Melpitz, Germany) during winter 2013. Analysis of 14C and a set of molecular tracers were used to constrain the sources of EC and OC. During the four-week campaign, most sites (in particular those in Germany and The Netherlands) were affected by an episode during the first two weeks with high concentrations of aerosol, as continental air masses were transported westward. The analysis results showed a clear, increasing north to south gradient for most molecular tracers. Total carbon (TC = OC + EC) at Birkenes showed an average concentration of 0.5 ± 0.3 μg C m-3, whereas the average concentration at Melpitz was 6.0 ± 4.3 μg C m-3. One weekly mean TC concentration as high as 11 μg C m-3 was observed at Melpitz. Average levoglucosan concentrations varied by an order of magnitude from 25 ± 13 ng m-3 (Birkenes) to 249 ± 13 ng m-3 (Melpitz), while concentrations of tracers of fungal spores (arabitol and mannitol) and vegetative debris (cellulose) were very low, showing a minor influence of primary biological aerosol particles during the North European winter. The fraction of modern carbon generally varied from 0.57 (Melpitz) to 0.91 (Birkenes), showing an opposite trend compared to the molecular tracers and TC. Total concentrations of 10 biogenic and anthropogenic carboxylic acids, mainly of secondary origin, were 4-53 ng m-3, with the lowest concentrations observed at Birkenes and the highest at Melpitz. However, the highest relative concentrations of carboxylic acids (normalized to TC) were observed at the most northern sites. Levels of organosulphates and nitrooxy organosulphates varied more than two orders of magnitude, from 2 to 414 ng m-3, between

Seasonal variation and light absorption property of carbonaceous aerosol in a typical glacier region of the southeastern Tibetan Plateau

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

Niu, Hewen; Kang, Shichang; Wang, Hailong

Deposition and accumulation of light-absorbing carbonaceous aerosol on glacier surfaces can alter the energy balance of glaciers. In this study, 2 years (December 2014 to December 2016) of continuous observations of carbonaceous aerosols in the glacierized region of the Mt. Yulong and Ganhaizi (GHZ) basin are analyzed. The average elemental carbon (EC) and organic carbon (OC) concentrations were 1.51±0.93 and 2.57±1.32μg m -3, respectively. Although the annual mean OC/EC ratio was 2.45±1.96, monthly mean EC concentrations during the post-monsoon season were even higher than OC in the high altitudes (approximately 5000 m a.s.l.) of Mt. Yulong. Strong photochemical reactions and local tourism activitiesmore » were likely the main factors inducing high OC/EC ratios in the Mt. Yulong region during the monsoon season. The mean mass absorption efficiency (MAE) of EC, measured for the first time in Mt. Yulong, at 632 nm with a thermal-optical carbon analyzer using the filter-based method, was 6.82±0.73 m 2g -1, comparable with the results from other studies. Strong seasonal and spatial variations of EC MAE were largely related to the OC abundance. Source attribution analysis using a global aerosol–climate model, equipped with a black carbon (BC) source tagging technique, suggests that East Asia emissions, including local sources, have the dominant contribution (over 50%) to annual mean near-surface BC in the Mt. Yulong area. There is also a strong seasonal variation in the regional source apportionment. South Asia has the largest contribution to near-surface BC during the pre-monsoon season, while East Asia dominates the monsoon season and post-monsoon season. Results in this study have great implications for accurately evaluating the influences of carbonaceous matter on glacial melting and water resource supply in glacierization areas.« less

Seasonal variation and light absorption property of carbonaceous aerosol in a typical glacieri region of the southeastern Tibetan Plateau

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

Niu, Hewen; Kang, Shichang; Wang, Hailong

2018-05-07

Deposition and accumulation of light-absorbing carbonaceous aerosol on glacier surfaces can alter the energy balance of glaciers. In this study, 2 years (December 2014 to December 2016) of continuous observations of carbonaceous aerosols in the glacierized region of the Mt. Yulong and Ganhaizi (GHZ) basin are analyzed. The average elemental carbon (EC) and organic carbon (OC) concentrations were 1.51±0.93 and 2.57±1.32 µg m−3, respectively. Although the annual mean OC ∕ EC ratio was 2.45±1.96, monthly mean EC concentrations during the post-monsoon season were even higher than OC in the high altitudes (approximately 5000 m a. s. l. ) of Mt. Yulong. Strong photochemical reactions and local tourism activities weremore » likely the main factors inducing high OC ∕ EC ratios in the Mt. Yulong region during the monsoon season. The mean mass absorption efficiency (MAE) of EC, measured for the first time in Mt. Yulong, at 632 nm with a thermal-optical carbon analyzer using the filter-based method, was 6.82±0.73 m2 g−1, comparable with the results from other studies. Strong seasonal and spatial variations of EC MAE were largely related to the OC abundance. Source attribution analysis using a global aerosol–climate model, equipped with a black carbon (BC) source tagging technique, suggests that East Asia emissions, including local sources, have the dominant contribution (over 50 %) to annual mean near-surface BC in the Mt. Yulong area. There is also a strong seasonal variation in the regional source apportionment. South Asia has the largest contribution to near-surface BC during the pre-monsoon season, while East Asia dominates the monsoon season and post-monsoon season. Results in this study have great implications for accurately evaluating the influences of carbonaceous matter on glacial melting and water resource supply in glacierization areas.« less

Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors

NASA Astrophysics Data System (ADS)

Zhang, X. Y.; Wang, J. Z.; Wang, Y. Q.; Liu, H. L.; Sun, J. Y.; Zhang, Y. M.

2015-11-01

Since there have been individual reports of persistent haze-fog events in January 2013 in central-eastern China, questions on factors causing the drastic differences in changes in 2013 from changes in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributing to such changes is yet to be determined. The study intends to present the changes in daily based major water-soluble constituents, carbonaceous species, and mineral aerosol in PM10 at 13 stations within different haze regions in China from 2006 to 2013, which are associated with specific meteorological conditions that are highly related to aerosol pollution (parameterized as an index called Parameter Linking Aerosol Pollution and Meteorological Elements - PLAM). No obvious changes were found in annual mean concentrations of these various chemical components and PM10 in 2013, relative to 2012. By contrast, wintertime mass of these components was quite different. In Hua Bei Plain (HBP), sulfate, organic carbon (OC), nitrate, ammonium, element carbon (EC), and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21, and 130 μg m-3, respectively; these masses were approximately 2 to 4 times higher than those in background mass, which also exhibited a decline during 2006 to 2010 and then a rise till 2013. The mass of these concentrations and PM10, except minerals, respectively, increased by approximately 28 to 117 % and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze-fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In the Yangtze River Delta (YRD) area, winter masses of these components, unlike HBP, have not significantly increase since 2010; PLAM were also maintained at a similar level without

Carbonaceous particles and aerosol mass closure in PM2.5 collected in a port city

NASA Astrophysics Data System (ADS)

Genga, A.; Ielpo, P.; Siciliano, T.; Siciliano, M.

2017-01-01

Mass concentrations of PM2.5, mineral dust, organic carbon (OC) and elemental carbon (EC), water-soluble organic carbon (WSOC), sea salts and anthropogenic metals have been studied in a city-port of south Italy (Brindisi). This city is characterized by different emission sources (ship, vehicular traffic, biomass burning and industrial emissions) and it is an important port and industrial site of the Adriatic sea. Based on diagnostic ratios of carbonaceous species we assess the presence of biomass burning emissions (BBE), fossil fuel emissions (FFE) and ship emission (SE). Our proposed conversion factors from OC to OM are higher than those reported in the literature for urban site: the reason of this could be due to the existence of aged combustion aerosols during the sampling campaign (WSOC/OC = 0.6 ± 0.3).

Radiocarbon-based source apportionment of carbonaceous aerosols at a regional background site on Hainan Island, South China.

PubMed

Zhang, Yan-Lin; Li, Jun; Zhang, Gan; Zotter, Peter; Huang, Ru-Jin; Tang, Jian-Hui; Wacker, Lukas; Prévôt, André S H; Szidat, Sönke

2014-01-01

To assign fossil and nonfossil contributions to carbonaceous particles, radiocarbon ((14)C) measurements were performed on organic carbon (OC), elemental carbon (EC), and water-insoluble OC (WINSOC) of aerosol samples from a regional background site in South China under different seasonal conditions. The average contributions of fossil sources to EC, OC and WINSOC were 38 ± 11%, 19 ± 10%, and 17 ± 10%, respectively, indicating generally a dominance of nonfossil emissions. A higher contribution from fossil sources to EC (∼51%) and OC (∼30%) was observed for air-masses transported from Southeast China in fall, associated with large fossil-fuel combustion and vehicle emissions in highly urbanized regions of China. In contrast, an increase of the nonfossil contribution by 5-10% was observed during the periods with enhanced open biomass-burning activities in Southeast Asia or Southeast China. A modified EC tracer method was used to estimate the secondary organic carbon from fossil emissions by determining (14)C-derived fossil WINSOC and fossil EC. This approach indicates a dominating secondary component (70 ± 7%) of fossil OC. Furthermore, contributions of biogenic and biomass-burning emissions to contemporary OC were estimated to be 56 ± 16% and 44 ± 14%, respectively.

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

Using radiocarbon to constrain black and organic carbon aerosol sources in Salt Lake City

NASA Astrophysics Data System (ADS)

Mouteva, Gergana O.; Randerson, James T.; Fahrni, Simon M.; Bush, Susan E.; Ehleringer, James R.; Xu, Xiaomei; Santos, Guaciara M.; Kuprov, Roman; Schichtel, Bret A.; Czimczik, Claudia I.

2017-09-01

Black carbon (BC) and organic carbon (OC) aerosols are important components of fine particulate matter (PM2.5) in polluted urban environments. Quantifying the contribution of fossil fuel and biomass combustion to BC and OC concentrations is critical for developing and validating effective air quality control measures and climate change mitigation policy. We used radiocarbon (14C) to measure fossil and contemporary biomass contributions to BC and OC at three locations in Salt Lake City, Utah, USA, during 2012-2014, including during winter inversion events. Aerosol filters were analyzed with the Swiss_4S thermal-optical protocol to isolate BC. We measured fraction modern (fM) of BC and total carbon in PM2.5 with accelerator mass spectrometry and derived the fM of OC using isotope mass balance. Combined with 14C information of end-member composition, our data set of 31 14C aerosol measurements provided a baseline of the fossil and contemporary biomass components of carbonaceous aerosol. We show that fossil fuels were the dominant source of carbonaceous aerosol during winter, contributing 88% (80-98%) of BC and 58% (48-69%) of OC. While the concentration of both BC and OC increased during inversion events, the relative source contributions did not change. The sources of BC also did not vary throughout the year, while OC had a considerably higher contemporary biomass component in summer at 62% (49-76%) and was more variable. Our results suggest that in order to reduce PM2.5 levels in Salt Lake City to meet national standards, a more stringent policy targeting mobile fossil fuel sources may be necessary.

Increased absorption by coarse aerosol particles over the Gangetic–Himalayan region

DOE PAGES

Manoharan, Vani Starry; Kotamarthi, R.; Feng, Yan; ...

2014-02-03

Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be < 1 μm in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October–November), suggesting the presence of absorbing aerosols sized 1–10 μm. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by largermore » particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Furthermore, large absorbing particles could be an important component of the regional-scale atmospheric energy balance.« less

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

NASA Astrophysics Data System (ADS)

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

2011-10-01

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

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

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

A two-year study of carbonaceous aerosols in ambient PM2.5 at a regional background site for western Yangtze River Delta, China

NASA Astrophysics Data System (ADS)

Chen, Dong; Cui, Hongfei; Zhao, Yu; Yin, Lina; Lu, Yan; Wang, Qingeng

2017-01-01

To analyze the characteristics of regional background carbonaceous aerosols in western Yangtze River Delta (YRD), hourly organic carbon (OC) and elemental carbon (EC) in fine particular matter (PM2.5) were measured with a semi-continuous carbon analyzer at a suburban site in upwind Nanjing from June 2013 to May 2015. Relatively low OC, EC and OC/EC were observed compared to other studies conducted in Nanjing. The reasons include the limited primary emissions around the observation site, the improved emission controls in recent years, and the use of denuder to reduce positive artifact in OC measurement. Resulting from the stable atmosphere conditions and emission variations, the highest concentrations of carbonaceous aerosols were found in both winters, with average OC and EC observed at 11.8 ± 10.0 and 5.9 ± 3.4 μg/m3 for the first one, and 8.1 ± 5 and 4.5 ± 2.4 μg/m3 for the second one, respectively. Compared to 2013, reduced OC and EC were found in summer and autumn 2014, demonstrating the benefits of emission control polices implemented for the Nanjing Youth Olympic, while elevated OC observed in spring 2015 was attributed probably to the increased biomass burning. For the hazy event in winter 2013, the back trajectories of air masses suggested that heavy pollution were from eastern Jiangsu, northern Anhui and Jiangsu, downtown Nanjing, and Shanghai. Secondary aerosol formation played an important role indicated by the larger mass fraction of OC and increased OC/EC in PM2.5 during the heavy pollution period. In the harvest season, biomass burning was estimated to contribute 51% and 16% of OC and EC concentrations, respectively.

Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013

NASA Astrophysics Data System (ADS)

Zhang, Y.-L.; Huang, R.-J.; El Haddad, I.; Ho, K.-F.; Cao, J.-J.; Han, Y.; Zotter, P.; Bozzetti, C.; Daellenbach, K. R.; Canonaco, F.; Slowik, J. G.; Salazar, G.; Schwikowski, M.; Schnelle-Kreis, J.; Abbaszade, G.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.; Szidat, S.

2015-02-01

During winter 2013, extremely high concentrations (i.e., 4-20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), 14C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on 14C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass

Aerosol observation using multi-wavelength Mie-Raman lidars of the Ad-Net and aerosol component analysis

NASA Astrophysics Data System (ADS)

Nishizawa, Tomoaki; Sugimoto, Nobuo; Shimizu, Atsushi; Uno, Itsushi; Hara, Yukari; Kudo, Rei

2018-04-01

We deployed multi-wavelength Mie-Raman lidars (MMRL) at three sites of the AD-Net and have conducted continuous measurements using them since 2013. To analyze the MMRL data and better understand the externally mixing state of main aerosol components (e.g., dust, sea-salt, and black carbon) in the atmosphere, we developed an integrated package of aerosol component retrieval algorithms, which have already been developed or are being developed, to estimate vertical profiles of the aerosol components. This package applies to the other ground-based lidar network data (e.g., EARLINET) and satellite-borne lidar data (e.g., CALIOP/CALIPSO and ATLID/EarthCARE) as well as the other lidar data of the AD-Net.

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

EPA Science Inventory

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

The Magnetization of Carbonaceous Meteorites

NASA Technical Reports Server (NTRS)

Herndon, James Herndon

1974-01-01

Alternating field demagnetization experiments have been conducted on representative samples of the carbonaceous meteorites (carbonaceous chondrites and ureilites). The results indicate that many, if not all, of these meteorites possess an intense and stable magnetic moment of extraterrestrial origin. Thermomagnetic analyses have been conducted on samples of all known carbonaceous meteorites. In addition to yielding quantitative magnetite estimates, these studies indicate the presence of a thermally unstable component, troilite, which reacts with gaseous oxygen to form magnetite. It is proposed that the magnetite found in some carbonaceous chondrites resulted from the oxidation of troilite during the early history of the solar system. The formation of pyrrhotite is expected as a natural consequence of magnetite formation via this reaction. Consideration is given to the implications of magnetite formation on paleointensity studies.

Observation of carbonaceous aerosols and carbon monoxide in Mid-Atlantic region: Seasonal and inter-annual variations

NASA Astrophysics Data System (ADS)

Chen, L. A.; Doddridge, B. G.; Doddridge, B. G.; Dickerson, R. R.; Dickerson, R. R.

2001-05-01

As part of Maryland Aerosol Research and Characterization (MARCH-Atlantic) study, a long-term monitoring of ambient elemental and organic carbon (EC and OC) aerosols has been made at Fort Meade, MD (39.16° N 76.51° W; elevation 46 m MSL), a suburban site within the Baltimore-Washington (B-W) corridor, since July 1999. 24-hr average EC and OC are measured every day during the season-representative months (July 1999, October 1999, January 2000, April 2000 and July 2000). Carbon monoxide (CO) was also measured nearly continuously over the period. Strong correlation between EC and CO (r = 0.7 ~ 0.9) in every month suggests common or proximate sources, likely traffic emissions. The EC versus CO slope, however, varies in different seasons and is found to increase nonlinearly with the ambient temperature. EC source strength may peak in summer. OC shows strong correlation with EC (r ~ 0.95) only in winter, suggesting that OC is also of the same primary sources during wintertime. The Interagency Monitoring of Protected Visual Environments (IMPROVE) network has been measuring EC and OC around the United States since 1988. The FME data during July 1999 are also compared with simultaneous measurements at nearby IMPROVE sites, showing B-W corridor could be a major contributor to the carbonaceous aerosols in the Mid-Atlantic region. A decreasing trend of EC level is found in three IMPROVE sites in this region. This actually agrees with the decreasing trend of CO observed previously at Big Meadow, Shenandoah National Park if CO and EC are both influenced by traffic emissions.

Diamond, aromatic, aliphatic components of interstellar dust grains: Random covalent networks in carbonaceous grains

NASA Astrophysics Data System (ADS)

Duley, W. W.

1995-05-01

A formalism based on the theory of random covalent networks (RCNs) in amorphous solids is developed for carbonaceous dust grains. RCN solutions provide optimized structures and relative compositions for amorphous materials. By inclusion of aliphatic, aromatic, and diamond clusters, solutions specific to interstellar materials can be obtained and compared with infrared spectral data. It is found that distinct RCN solutions corresponding to diffuse cloud and molecular cloud materials are possible. Specific solutions are derived for three representative objects: VI Cyg No. 12, NGC 7538 (IRS 9), and GC IRS 7. While diffuse cloud conditions with a preponderance of sp2 and sp3 bonded aliphatic CH species can be reproduced under a variety of RCN conditions, the presence of an abundant tertiary CH or diamond component is highly constrained. These solutions are related quantitatively to carbon depletions and can be used to provide a quantitative estimate of carbon in these various dust components. Despite the abundance of C6 aromatic rings in many RCN solutions, the infrared absorption due to the aromatic stretch at approximately 3.3 micrometers is weak under all conditions. The RCN formalism is shown to provide a useful method for tracing the evolutionary properties of interstellar carbonaceous grains.

Revisiting AVHRR Tropospheric Aerosol Trends Using Principal Component Analysis

NASA Technical Reports Server (NTRS)

Li, Jing; Carlson, Barbara E.; Lacis, Andrew A.

2014-01-01

The advanced very high resolution radiometer (AVHRR) satellite instruments provide a nearly 25 year continuous record of global aerosol properties over the ocean. It offers valuable insights into the long-term change in global aerosol loading. However, the AVHRR data record is heavily influenced by two volcanic eruptions, El Chichon on March 1982 and Mount Pinatubo on June 1991. The gradual decay of volcanic aerosols may last years after the eruption, which potentially masks the estimation of aerosol trends in the lower troposphere, especially those of anthropogenic origin. In this study, we show that a principal component analysis approach effectively captures the bulk of the spatial and temporal variability of volcanic aerosols into a single mode. The spatial pattern and time series of this mode provide a good match to the global distribution and decay of volcanic aerosols. We further reconstruct the data set by removing the volcanic aerosol component and reestimate the global and regional aerosol trends. Globally, the reconstructed data set reveals an increase of aerosol optical depth from 1985 to 1990 and decreasing trend from 1994 to 2006. Regionally, in the 1980s, positive trends are observed over the North Atlantic and North Arabian Sea, while negative tendencies are present off the West African coast and North Pacific. During the 1994 to 2006 period, the Gulf of Mexico, North Atlantic close to Europe, and North Africa exhibit negative trends, while the coastal regions of East and South Asia, the Sahel region, and South America show positive trends.

Estimation of lifetime of carbonaceous aerosol from open crop residue burning during Mount Tai Experiment 2006 (MTX2006)

NASA Astrophysics Data System (ADS)

Pan, X. L.; Kanaya, Y.; Wang, Z. F.; Komazaki, Y.; Taketani, F.; Akimoto, H.; Pochanart, P.; Liu, Y.

2012-06-01

Studying the emission ratios of carbonaceous aerosols (element carbon, EC, and organic carbon, OC) from open biomass burning helps to reduce uncertainties in emission inventories and provides necessary constraints for model simulations. We measured apparent elemental carbon (ECa) and OC concentrations at the summit of Mount Tai (Mt. Tai) during intensive open crop residue burning (OCRB) episodes using a Sunset OCEC analyzer. Equivalent black carbon (BCe) concentrations were determined using a Multiple Angle Absorption Photometer (MAAP). In the fine particle mode, OC and EC showed strong correlations (r > 0.9) with carbon monoxide (CO). Footprint analysis using the FLEXPART_WRF model indicated that OCRB in central east China (CEC) had a significant influence on ambient carbonaceous aerosol loadings at the summit of Mt. Tai. ΔECa/ΔCO ratios resulting from OCRB plumes were 14.3 ± 1.0 ng m-3 ppbv-1 at Mt. Tai. This ratio was more than three times those resulting from urban pollution in CEC, demonstrating that significant concentrations of soot particles were released from OCRB. ΔOC/ΔCO ratio from fresh OCRB plumes was found to be 41.9 ± 2.6 ng m-3 ppbv-1 in PM1. The transport time of smoke particles was estimated using the FLEXPART_WRF tracer model by releasing inert particles from the ground layer inside geographical regions where large numbers of hotspots were detected by a MODIS satellite sensor. Fitting regressions using the e-folding exponential function indicated that the removal efficiency of OC (normalized to CO) was much larger than that of ECa mass, with mean lifetimes of 27 h (1.1 days) for OC and 105 h (4.3 days) for ECa, respectively. The lifetime of black carbon estimated for the OCRB events in east China was comparably lower than the values normally adopted in the transport models. Short lifetime of organic carbon highlighted the vulnerability of OC to cloud scavenging in the presence of water-soluble organic species from biomass combustion.

Characteristics of size-resolved atmospheric inorganic and carbonaceous aerosols in urban Shanghai

NASA Astrophysics Data System (ADS)

Ding, X. X.; Kong, L. D.; Du, C. T.; Zhanzakova, A.; Fu, H. B.; Tang, X. F.; Wang, L.; Yang, X.; Chen, J. M.; Cheng, T. T.

2017-10-01

Size-segregated aerosol particles were collected with a 10-stage Micro-Orifice Uniform Deposit Impactor (MOUDI) at an urban site in Shanghai, China for four non-consecutive months representing four seasons from 2015 to 2016. Chemical composition, including water-soluble ions as well as organic carbon (OC), elemental carbon (EC) and secondary organic carbon (SOC) of size-resolved (0.056-18 μm) atmospheric aerosols in four seasons and in different polluted cases were studied. The size distributions of sulfate, nitrate and ammonium (SNA) and carbonaceous aerosol (OC, EC and SOC) were discussed and the potential sources of PM1.8-associated secondary species (SO42-, NO3-, SNA and SOC) in different seasons were identified by potential source contribution function (PSCF) model. Results showed that atmospheric ultrafine and fine particle pollution in Shanghai were very serious during the study period. Most of the water-soluble ions tended to be enriched in fine particles, especially being abundant in the droplet mode in polluted cases. Compared with sulfate, size distributions of nitrate and ammonium presented more significant seasonal variations and showed distinctive characteristics in polluted days. Abundant nitrate was concentrated in fine particles in cold seasons (spring and winter), whereas it was enriched in coarse mode during summer and autumn. The droplet mode sulfate with high concentration did not result in the aggravation of air pollution, while the nucleation mode sulfate may have made a great contribution to the air pollution in urban Shanghai. It was also found that the formation of air pollution in urban Shanghai had a significant link with nitrate and ammonium, especially with nitrate and ammonium in condensation mode and droplet mode, and the contribution of sulfate to the pollution formation in Shanghai would somehow be surpassed by the increasing nitrate and ammonium. OC and EC concentrations from spring to winter were found to be 11.10, 7.10, 12

Remote sensing of soot carbon - Part 1: Distinguishing different absorbing aerosol species

NASA Astrophysics Data System (ADS)

Schuster, G. L.; Dubovik, O.; Arola, A.

2016-02-01

We describe a method of using the Aerosol Robotic Network (AERONET) size distributions and complex refractive indices to retrieve the relative proportion of carbonaceous aerosols and free iron minerals (hematite and goethite). We assume that soot carbon has a spectrally flat refractive index and enhanced imaginary indices at the 440 nm wavelength are caused by brown carbon or hematite. Carbonaceous aerosols can be separated from dust in imaginary refractive index space because 95 % of biomass burning aerosols have imaginary indices greater than 0.0042 at the 675-1020 nm wavelengths, and 95 % of dust has imaginary refractive indices of less than 0.0042 at those wavelengths. However, mixtures of these two types of particles can not be unambiguously partitioned on the basis of optical properties alone, so we also separate these particles by size. Regional and seasonal results are consistent with expectations. Monthly climatologies of fine mode soot carbon are less than 1.0 % by volume for West Africa and the Middle East, but the southern African and South American biomass burning sites have peak values of 3.0 and 1.7 %. Monthly averaged fine mode brown carbon volume fractions have a peak value of 5.8 % for West Africa, 2.1 % for the Middle East, 3.7 % for southern Africa, and 5.7 % for South America. Monthly climatologies of free iron volume fractions show little seasonal variability, and range from about 1.1 to 1.7 % for coarse mode aerosols in all four study regions. Finally, our sensitivity study indicates that the soot carbon retrieval is not sensitive to the component refractive indices or densities assumed for carbonaceous and free iron aerosols, and the retrieval differs by only 15.4 % when these parameters are altered from our chosen baseline values. The total uncertainty of retrieving soot carbon mass is ˜ 50 % (when uncertainty in the AERONET product and mixing state is included in the analysis).

Radiocarbon-based Source Apportionment of Organic, Elemental and Water-soluble Organic Carbon Aerosols and the Light Absorption of Water-soluble Organic Carbon Aerosols in the East Asia High-intensity Winter Campaigns in 2014

NASA Astrophysics Data System (ADS)

Fang, W.; Andersson, A.; Zheng, M.; Lee, M.; Kim, S. W.; Du, K.; Gustafsson, O.

2016-12-01

Improved understanding of anthropogenic aerosol effects on atmospheric chemistry and climate as well as efficient mitigation actions are hampered by the limited comprehension of the relative contributions of different sources of carbonaceous aerosols and of their subsequent atmospheric processing. Here, we present dual carbon isotope constrained source apportionment and optical properties of carbonaceous aerosols simultaneously both at urban and rural receptor sites, includes North China Plain (NCP, Beijing and Tianjin), Yangtze River Delta (YRD, Shanghai, Zhejiang), and Jeju Island (Korea Climate Observatory at Gosan) during January 2014 field campaigns. The radiocarbon (Δ14C) data show that fossil combustions contribute equally ˜80 ± 5% to elemental carbon (EC) aerosol in Beijing, Tianjin, and Shanghai, and 66 ± 9% to Gosan-EC aerosol, while the specific sources of the dominant fossil fuel component were dramatically different among these sites. The mean fraction coal combustion of Beijing-EC, Tianjin-EC, and Gosan-EC is double that of Shanghai-EC. The other large fraction (72―92%) of carbonaceous aerosol is organic carbon (OC) aerosol which contains water soluble and water insoluble organic carbon (WSOC and WISOC). OC, WISOC, and WSOC in Beijing and Gosan sites were still observed largely from fossil sources (53―75%). The more 13C-enriched signature of Gosan-WSOC (-22.8 ± 0.2‰) compared to Gosan-EC (-23.9 ± 0.4‰) and Beijing-WSOC (-23.5 ± 0.7‰) reflects that WSOC is likely more affected by atmospheric aging during long-rang transport than is EC. The high light absorption coefficients of PM2.5, PM1, and TSP were observed at Gosan during this study and was frequently reaching 20―60 Mm-1 by aethalometer and continuous light absorption photometer. The mass absorption cross section of WSOC (MAC365) for above sites is high (1.5 ± 0.8 m2/g), accounted for ˜14 ± 5% of the total direct absorbance relative to EC, which is significantly higher than

Estimate of the Aerosol Anthropogenic Component and Focusing from Satellite Data

NASA Technical Reports Server (NTRS)

Kaufman, Yoram; Remer, Lorraine A.; Chin, Mian

2004-01-01

Satellite measurements of aerosol do not contain information on the chemical composition needed to resolve anthropogenic vs. natural aerosol components. Besides, the same chemical species can have natural and anthropogenic origins. However the ability of the new satellite instruments (MODIS, MISR, POLDER) to distinguish fine from coarse aerosols over the oceans, can be used as a signature of the presence of anthropogenic component and used to measure the fraction of the aerosol originating from anthropogenic activity with an uncertainty of 10 percent for aerosol optical thickness larger than 0.1. We develop the methods and investigated it using model calculations (GOCART) and satellite data (MODIS). Preliminary application to 2 years of global MODIS data shows that 0.200.08 of the aerosol optical thickness and radiative effect has anthropogenic origin. The resultant aerosol forcing over cloud free oceans is 1.30.6 W/sq m, larger than model simulations. Further research until the presentation will probably modify these values.

Carbonaceous species in PM2.5 and PM10 in urban area of Zhengzhou in China: Seasonal variations and source apportionment

NASA Astrophysics Data System (ADS)

Wang, Qun; Jiang, Nan; Yin, Shasha; Li, Xiao; Yu, Fei; Guo, Yue; Zhang, Ruiqin

2017-07-01

PM2.5 and PM10 samples were simultaneously collected in an urban site in Zhengzhou, China from October 2014 to July 2015 representing the four seasons. Organic carbon (OC), elemental carbon (EC), and non-polar organic compounds including n-alkanes (C8-C40) and polycyclic aromatic hydrocarbons (PAHs) were quantified. The characteristics of their concentrations, seasonal variations, and sources of n-alkanes and PAHs were investigated. Diagnostic ratios and positive matrix factorization (PMF) were used to characterize carbonaceous species, identify their possible sources, and apportion the contributions from each possible source. The concentrations of the components exhibited distinct seasonal variation, that is, the concentrations are high in winter and low in summer. This finding could be associated with increase in air pollutant emissions during heating season and stable weather condition. The estimated total carbonaceous aerosol accounts for 32% of PM2.5 and 30% of PM10. Hence, carbonaceous compounds were the major components of particulate matter in the study area. Moreover, OC, EC, PAHs, and n-alkanes preferentially accumulated into fine particles. The carbonaceous components exhibited high correlation in PM2.5 and PM10, thereby indicating that their sources were similar. The PMF results revealed that the main sources of PAHs were coal combustion (40%) and motor vehicles (29%); n-alkanes were mainly from burning of fossil fuel (48%). These sources were consistent with the diagnostic ratios obtained. This study provides guidance for improving air quality and reducing human exposure to toxic air pollutants.

The OMI Aerosol Absorption Product: An A-train application

NASA Astrophysics Data System (ADS)

Torres, O.; Jethva, H. T.; Ahn, C.

2017-12-01

Because of the uniquely large sensitivity of satellite-measured near-UV radiances to absorption by desert dust, carbonaceous and volcanic ash aerosols, observations by a variety of UV-capable sensors have been routinely used over the last forty years in both qualitative and quantitative applications for estimating the absorption properties of these aerosol types. In this presentation we will discuss a multi-sensor application involving observations from A-train sensors OMI, AIRS and CALIOP for the creation of a 13-year record of aerosol optical depth (AOD) and single scattering albedo (SSA). Determination of aerosol type, in terms of particle size distribution and refractive index, is an important algorithmic step that requires using external information. AIRS CO measurements are used as carbonaceous aerosols tracer to differentiate this aerosol type from desert dust. On the other hand, the height of the absorbing aerosol layer, an important parameter in UV aerosol retrievals, is prescribed using a CALIOP-based climatology. The combined use of these observations in the developments of the OMI long-term AOD/SSA record will be discussed along with an evaluation of retrieval results using independent observations.

Characteristics of carbonaceous aerosols at a pair of suburban and downtown sites in Nanjing, China

NASA Astrophysics Data System (ADS)

Cui, H.; Zhang, J.; Zhao, Y.

2014-12-01

Carbonaceous species in PM2.5 were measured in three seasons (except winter) in downtown and around a year in suburban in Nanjing. In particular, the OC and EC concentrations were continuously measured with 1-h interval at both sites. The mean concentrations of PM2.5, OC, EC were 85.9 μg/m3, 10.4 μg/m3, 4.2 μg/m3 and 63.4 μg/m3, 8.1 μg/m3, 5.3μg/m3 for downtown and suburban respectively. At the suburban site, compared to the lowest average concentration in spring, the relatively higher concentration of carbonaceous aerosol in summer was caused by biomass-burning activities. Significant increasing peaks of OC (up to 122.9 ug/m3) and EC (up to 35.8 ug/m3) in suburban were recorded in the June 10th night, and it is indicated using back trajectory that the air mass came through nearby agriculture areas. On the other hand, the OC and EC concentrations during the 2nd AYG (Asian Youth Games, Aug 16th - 24th in 2013) compared to that in rest days in August reduced by 21% and 10%, respectively, attributing to the effective control measures on reduction of industrial point sources, temporary control of motor vehicle and fugitive dusts. Rations of OC/EC in suburban were much lower than that in downtown. This might be due to the fact that the sampling point in suburban is quite close (in 400 meters) to a main highway. Both OC and EC concentrations in suburban were higher in nighttime than daytime, except OC in summer, indicating the existence of strong SOC and supported by high OC/EC and O3 at noon. The annual average SOC estimated by EC-tracer methods occupied 34.5% and 36.7% of the total OC for the downtown and suburban areas, respectively. OC/EC correlations in suburban were much weaker than those from downtown areas, which shows suburban areas is much more affected by long-range transport of pollution and/or complex sources including domestic coal combustion, biomass burning, industrial and transportation, especially in three other seasons except winter, which is

Carbonaceous PM(2.5) and secondary organic aerosol across the Veneto region (NE Italy).

PubMed

Khan, Md Badiuzzaman; Masiol, Mauro; Formenton, Gianni; Di Gilio, Alessia; de Gennaro, Gianluigi; Agostinelli, Claudio; Pavoni, Bruno

2016-01-15

Organic and elemental carbon (OC-EC) were measured in 360 PM2.5 samples collected from April 2012 to February 2013 at six provinces in the Veneto region, to determine the factors affecting the carbonaceous aerosol variations. The 60 daily samples have been collected simultaneously in all sites during 10 consecutive days for 6 months (April, June, August, October, December and February). OC ranged from 0.98 to 22.34 μg/m(3), while the mean value was 5.5 μg/m(3), contributing 79% of total carbon. EC concentrations fluctuated from 0.19 to 11.90 μg/m(3) with an annual mean value of 1.31 μg/m(3) (19% of the total carbon). The monthly OC concentration gradually increased from April to December. The EC did not vary in accordance with OC. However the highest values for both parameters were recorded in the cold period. The mean OC/EC ratio is 4.54, which is higher than the values observed in most of the other European cities. The secondary organic carbon (SOC) contributed for 69% of the total OC and this was confirmed by both the approaches OC/EC minimum ratio and regression. The results show that OC, EC and SOC exhibited higher concentration during winter months in all measurement sites, suggesting that the stable atmosphere and lower mixing play important role for the accumulation of air pollutant and hasten the condensation or adsorption of volatile organic compounds over the Veneto region. Significant meteorological factors controlling OC and EC were investigated by fitting linear models and using a robust procedure based on weighted likelihood, suggesting that low wind speed and temperature favour accumulation of emissions from local sources. Conditional probability function and conditional bivariate probability function plots indicate that both biomass burning and vehicular traffic are probably the main local sources for carbonaceous particulate matter emissions in two selected cities. Copyright © 2015 Elsevier B.V. All rights reserved.

CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

EPA Science Inventory

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

Investigation of Carbonaceous Aerosol Optical Properties to Understand Impacts on Air Quality and Composition

NASA Astrophysics Data System (ADS)

Olson, Michael R.

The optical properties of carbonaceous aerosols were investigated to understand the impact source emissions and ambient particulate matter (PM) have on atmospheric radiative forcing. Black carbon (BC) is a strong absorber of visible light and contributes highly to atmospheric radiative forcing, therefore it is important to link BC properties to combustion emission sources. Brown carbon (BrC) is poorly understood and may be an important contributor to both positive and negative radiative forcing. The research investigates these primary knowledge gaps. The optical properties of carbonaceous aerosols were investigated to understand the impact source emissions and ambient particulate matter (PM) have on atmospheric radiative forcing. Black carbon (BC) is a strong absorber of visible light and contributes highly to atmospheric radiative forcing, therefore it is important to link BC properties to combustion emission sources. Brown carbon (BrC) is poorly understood and may be an important contributor to both positive and negative radiative forcing. The research investigates these primary knowledge gaps. Multiple methods were developed and applied to quantify the mass absorption cross-section (MAC) at multiple wavelengths of source and ambient samples. The MAC of BC was determined to be approximately 7.5 m2g-1 at 520nm. However, the MAC was highly variable with OC fraction and wavelength. The BrC MAC was similar for all sources, with the highest absorption in the UV at 370nm; the MAC quickly decreases at larger wavelengths. In the UV, the light absorption by BrC could exceed BC contribution by over 100 times, but only when the OC fraction is large (>90%) as compared to the total carbon. BrC was investigated by measuring the light absorption of solvent extracted fractions in water, dichloromethane, and methanol. Source emissions exhibited greater light absorption in methanol extractions as compared to water and DCM extracts. The BrC MAC was 2.4 to 3.7 m2g-1 at 370nm in

Origin of fine carbonaceous particulate matter in the Western Mediterranean Basin: fossil versus modern sources

NASA Astrophysics Data System (ADS)

Cruz Minguillón, María.; Perron, Nolwenn; Querol, Xavier; Szidat, Sönke; Fahrni, Simon; Wacker, Lukas; Reche, Cristina; Cusack, Michael; Baltensperger, Urs; Prévôt, André S. H.

2010-05-01

The present work was carried out in the frame of the international field campaign DAURE (Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). The objective of this campaign is to study the aerosol pollution episodes occurring at regional scale during winter and summer in the Western Mediterranean Basin. As part of this campaign, this work focuses on identifying the origin of fine carbonaceous aerosols. To this end, fine particulate matter (PM1) samples were collected during two different seasons (February-March and July 2009) at two sites: an urban site (Barcelona, NE Spain) and a rural European Supersite for Atmospheric Aerosol Research (Montseny, NE Spain). Subsequently, 14C analyses were carried out on these samples, both in the elemental carbon (EC) fraction and the organic carbon (OC) fraction, in order to distinguish between modern carbonaceous sources (biogenic emissions and biomass burning emissions) and fossil carbonaceous sources (mainly road traffic). Preliminary results from the winter period show that 40% of the OC at Barcelona has a fossil origin whereas at Montseny this percentage is 30%. These values can be considered as unexpected given the nature of the sites. Nevertheless, the absolute concentrations of fossil OC at Barcelona and Montseny differ by a factor of 2 (the first being higher), since the total OC at Montseny is lower than at Barcelona. Further evaluation of results and comparison with other measurements carried out during the campaign are required to better evaluate the origin of the fine carbonaceous matter in the Western Mediterranean Basin. Acknowledgements: Spanish Ministry of Education and Science, for a Postdoctoral Grant awarded to M.C. Minguillón in the frame of Programa Nacional de Movilidad de Recursos Humanos del Plan nacional de I-D+I 2008-2011. Spanish Ministry of Education and Science, for the Acción Complementaria DAURE CGL2007-30502-E/CLI.

Aerosol transport from Chiang Mai, Thailand to Mt. Lulin, Taiwan - Implication of aerosol aging during long-range transport

NASA Astrophysics Data System (ADS)

Chuang, Ming-Tung; Lee, Chung-Te; Chou, Charles C.-K.; Engling, Guenter; Chang, Shih-Yu; Chang, Shuenn-Chin; Sheu, Guey-Rong; Lin, Neng-Huei; Sopajaree, Khajornsak; Chang, You-Jia; Hong, Guo-Jun

2016-07-01

The transport of biomass burning (BB) aerosol from Indochina may cause a potential effect on climate change in Southeast Asia, East Asia, and the Western Pacific. Up to now, the understanding of BB aerosol composition modification during long-range transport (LRT) is still very limited due to the lack of observational data. In this study, atmospheric aerosols were collected at the Suthep/Doi Ang Khang (DAK) mountain sites in Chiang Mai, Thailand and the Lulin Atmospheric Background Station (Mt. Lulin) in central Taiwan from March to April 2010 and from February to April 2013, respectively. During the study period, an upwind and downwind relationship between the Suthep/DAK and Lulin sites (2400 km apart) was validated by backward trajectories. Comprehensive aerosol properties were resolved for PM2.5 water-soluble inorganic ions, carbonaceous content, water-soluble/insoluble organic carbon (WSOC/WIOC), dicarboxylic acids and their salts (DCAS), and anhydrosugars. A Modification Factor (MF) is proposed by employing non-sea-salt potassium ion (nss-K+) or fractionalized elemental carbon evolved at 580 °C after pyrolized OC correction (EC1-OP) as a BB aerosol tracer to evaluate the mass fraction changes of aerosol components from source to receptor regions during LRT. The MF values of nss-SO42-, NH4+, NO3-, OC1 (fractionalized organic carbon evolved from room temperature to 140 °C), OP (pyrolized OC fraction), DCAS, and WSOC were above unity, which indicated that these aerosol components were enhanced during LRT as compared with those in the near-source region. In contrast, the MF values of anhydrosugars ranged from 0.1 to 0.3, indicating anhydrosugars have degraded during LRT.

Aerosol Absorption Effects in the TOMS UV Algorithm

NASA Technical Reports Server (NTRS)

Torres, O.; Krotkov, N.; Bhartia, P. K.

2004-01-01

The availability of global long-term estimates of surface UV radiation is very important, not only for preventive medicine considerations, but also as an important tool to monitor the effects of the stratospheric ozone recovery expected to occur in the next few decades as a result of the decline of the stratospheric chlorine levels. In addition to the modulating effects of ozone and clouds, aerosols also affect the levels of UV-A and W-B radiation reaching the surface. Oscillations in surface W associated with the effects of aerosol absorption may be comparable in magnitude to variations associated with the stratospheric ozone recovery. Thus, the accurate calculation of surface W radiation requires that both the scattering and absorption effects of tropospheric aerosols be taken into account. Although absorption effects of dust and elevated carbonaceous aerosols are already accounted for using Aerosol Index technique, this approach does not work for urban/industrial aerosols in the planetary boundary layer. The use of the new TOMS long-term global data record on UV aerosol absorption optical depth, can improve the accuracy of TOMS spectral UV products, by properly including the spectral attenuation effects of carbonaceous, urban/industrial and mineral aerosols. The TOMS data set on aerosol properties will be discussed, and results of its use in the TOMS surface W algorithm will be presented.

Variations of carbonaceous aerosols from open crop residue burning with transport and its implication to estimate their lifetimes

NASA Astrophysics Data System (ADS)

Pan, X. L.; Kanaya, Y.; Wang, Z. F.; Komazaki, Y.; Taketani, F.; Akimoto, H.; Pochanart, P.

2013-08-01

Studying the correlations of carbonaceous aerosols (element carbon, EC, and organic carbon, OC) from open biomass burning helps to reduce uncertainties in emission inventories and provides necessary constraints for model simulations. In the present study, we measured apparent elemental carbon (ECa) and OC concentrations at the summit of Mount Tai (Mt. Tai) during intensive open crop residue burning (OCRB) episodes using a Sunset OCEC analyzer. In the fine particle mode, OC and ECa showed strong correlations (r > 0.9) with carbon monoxide (CO). Footprint analysis using the FLEXPART_WRF model indicated that OCRB in Central East China had a significant influence on ambient carbonaceous aerosol loadings at the summit of Mt. Tai. During campaign, ΔECa/ΔCO ratios of OCRB plumes were found to be 14.3 ± 1.0 ng m-3 ppbv at Mt. Tai. This ratio was twice larger than those for urban pollution in CEC, demonstrating that significant emissions of soot particles emitted from OCRB. ΔOC/ΔCO ratio of OCRB plumes was found to be 41.9 ± 2.6 ng m-3 ppbv averagely. The transport time of smoke particles was estimated using the FLEXPART_WRF tracer model by releasing particles from the ground layer inside geographical regions where large numbers of hotspots were detected by the MODIS sensor. The relationship between transport time and observed ΔECa/ΔCO and ΔOC/ΔCO ratios was fitted by an e-folding exponential function. Results showed that the loss rate of OC (normalized by CO) with transport was much quicker than that of ECa mass, and the corresponding lifetime of OC mass was estimated to be 28.0-44.2 h (1.2-1.8 days), much shorter than that 98.4-136.9 h (4.1-5.7 days) of ECa. Lifetime of ECa estimated for the OCRB events in CEC in the study was comparably lower than the values normally calculated by the transport models. Short lifetime of OC highlighted its vulnerability to cloud scavenging in the presence of water-soluble organic species from biomass combustion.

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

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

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

Cappa, Christopher D; Atkinson, Dean B

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

Aerosolization and Atmospheric Transformation of Engineered Nanoparticles

NASA Astrophysics Data System (ADS)

Tiwari, Andrea J.

While research on the environmental impacts of engineered nanoparticles (ENPs) is growing, the potential for them to be chemically transformed in the atmosphere has been largely ignored. The overall objective of this work was to assess the atmospheric transformation of carbonaceous nanoparticles (CNPs). The research focuses on C60 fullerene because it is an important member of the carbonaceous nanoparticle (CNP) family and is used in a wide variety of applications. The first specific objective was to review the potential of atmospheric transformations to alter the environmental impacts of CNPs. We described atmospheric processes that were likely to physically or chemically alter aerosolized CNPs and demonstrated their relevance to CNP behavior and toxicity in the aqueous and terrestrial environment. In order to investigate the transformations of CNP aerosols under controlled conditions, we developed an aerosolization technique that produces nano-scale aerosols without using solvents, which can alter the surface chemistry of the aerosols. We demonstrated the technique with carbonaceous (C60) and metal oxide (TiO2, CeO2) nanoparticle powders. All resulting aerosols exhibited unimodal size distributions and mode particle diameters below 100 nm. We used the new aerosolization technique to investigate the reaction between aerosolized C60 and atmospherically realistic levels of ozone (O3) in terms of reaction products, reaction rate, and oxidative stress potential. We identified C60O, C60O2, and C60O3 as products of the C60-O3 reaction. We demonstrated that the oxidative stress potential of C 60 may be enhanced by exposure to O3. We found the pseudo-first order reaction rate to be 9 x 10-6 to 2 x 10 -5 s-1, which is several orders of magnitude lower than the rate for several PAH species under comparable conditions. This research has demonstrated that a thorough understanding of atmospheric chemistry of ENPs is critical for accurate prediction of their environmental

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

NASA Astrophysics Data System (ADS)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

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

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

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

Xiaoyan Tang; Min Shao; Yuanhang Zhang

1996-12-31

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

Characterization of combustion-generated carbonaceous nanoparticles by size-dependent ultraviolet laser photoionization.

PubMed

Commodo, Mario; Sgro, Lee Anne; Minutolo, Patrizia; D'Anna, Andrea

2013-05-16

Photoelectric charging of particles is a powerful tool for online characterization of submicrometer aerosol particles. Indeed photoionization based techniques have high sensitivity and chemical selectivity. Moreover, they yield information on electronic properties of the material and are sensitive to the state of the surface. In the present study the photoionization charging efficiency, i.e., the ratio between the generated positive ions and the corresponding neutral ones, for different classes of flame-generated carbonaceous nanoparticles was measured. The fifth harmonics of a Nd:YAG laser, 213 nm (5.82 eV), was used as an ionization source for the combustion generated nanoparticles, whereas a differential mobility analyzer (DMA) coupled to a Faraday cup electrometer was used for particle classification and detection. Carbonaceous nanoparticles in the nucleation mode, i.e., sizes ranging from 1 to 10 nm, show a photoionization charging efficiency clearly dependent on the flame conditions. In particular, we observed that the richer the flame is, i.e., the higher the equivalent ratio is, the higher the photon charging efficiency is. We hypothesized that such an increase in the photoionization propensity of the carbonaceous nanoparticles from richer flame condition is associated to the presence within the particles of larger aromatic moieties. The results clearly show that photoionization is a powerful diagnostic tool for the physical-chemical characterization of combustion aerosol, and it may lead to further insights into the soot formation mechanism.

Enhanced UV Absorption in Carbonaceous Aerosols during MILAGRO and Identification of Potential Organic Contributors.

NASA Astrophysics Data System (ADS)

Mangu, A.; Kelley, K. L.; Marchany-Rivera, A.; Kilaparty, S.; Gunawan, G.; Gaffney, J. S.; Marley, N. A.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) during the month of March, 2006 by using a 7- channel aethalometer (Thermo-Anderson). These measurements, obtained at 370, 470, 520, 590, 660, 880, and 950 nm at a 5 minute time resolution, showed an enhanced absorption in the UV over that expected from carbon soot alone. Samples of fine atmospheric aerosols (less than 0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. The samples were collected on quartz fiber filters with high volume impactor samplers. The samples have been characterized for total carbon content (stable isotope ratio mass spectroscopy) and natural radionuclide tracers (210Pb, 210Po, 210Bi, 7Be, 13C, 14C, 40K, 15N). Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV-visible spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples (1). The continuous spectra also show an enhanced UV absorption over that expected from carbon soot and the general profiles are quite similar to those observed for humic and fulvic acids found as colloidal materials in surface and groundwaters (2), indicating the presence of humic-like substances (HULIS) in the fine aerosols. The spectra also show evidence of narrow band absorbers below 400 nm typical of polycyclic aromatics (PAH) and nitrated aromatic compounds. Spectra were also obtained on NIST standard diesel soot (SRM 2975), NIST standard air particulate matter (SRM 8785

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

NASA Technical Reports Server (NTRS)

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

1991-01-01

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

Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

NASA Astrophysics Data System (ADS)

Pfrang, C.; Shiraiwa, M.; Pöschl, U.

2011-04-01

Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles representative of atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant time scales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.

Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

NASA Astrophysics Data System (ADS)

Pfrang, C.; Shiraiwa, M.; Pöschl, U.

2011-07-01

Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.

Synergic use of TOMS and Aeronet Observations for Characterization of Aerosol Absorption

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.; Dubovik, O.; Holben, B.; Siniuk, A.

2003-01-01

The role of aerosol absorption on the radiative transfer balance of the earth-atmosphere system is one of the largest sources of uncertainty in the analysis of global climate change. Global measurements of aerosol single scattering albedo are, therefore, necessary to properly assess the radiative forcing effect of aerosols. Remote sensing of aerosol absorption is currently carried out using both ground (Aerosol Robotic Network) and space (Total Ozone Mapping Spectrometer) based observations. The satellite technique uses measurements of backscattered near ultraviolet radiation. Carbonaceous aerosols, resulting from the combustion of biomass, are one of the most predominant absorbing aerosol types in the atmosphere. In this presentation, TOMS and AERONET retrievals of single scattering albedo of carbonaceous aerosols, are compared for different environmental conditions: agriculture related biomass burning in South America and Africa and peat fires in Eastern Europe. The AERONET and TOMS derived aerosol absorption information are in good quantitative agreement. The most absorbing smoke is detected over the African Savanna. Aerosol absorption over the Brazilian rain forest is less absorbing. Absorption by aerosol particles resulting from peat fires in Eastern Europe is weaker than the absorption measured in Africa and South America. This analysis shows that the near UV satellite method of aerosol absorption characterization has the sensitivity to distinguish different levels of aerosol absorption. The analysis of the combined AERONET-TOMS observations shows a high degree of synergy between satellite and ground based observations.

Carbonaceous Components in the Comet Halley Dust

NASA Technical Reports Server (NTRS)

Fomenkova, M. N.; Chang, S.; Mukhin, L. M.

1994-01-01

Cometary grains containing large amounts of carbon and/or organic matter (CHON) were discovered by in situ measurements of comet Halley dust composition during VEGA and GIOTTO flyby missions. In this paper, we report the classification of these cometary, grains by means of cluster analysis, discuss the resulting compositional groups, and compare them with substances observed or hypothesized in meteorites, interplanetary dust particles, and the interstellar medium. Grains dominated by carbon and/or organic matter (CHON grains) represent approx. 22% of the total population of measured cometary dust particles. They, usually contain a minor abundance of rock-forming elements as well. Grains having organic material are relatively more abundant in the vicinity of the nucleus than in the outer regions of the coma, which suggests decomposition of the organics in the coma environment. The majority of comet Halley organic particles are multicomponent mixtures of carbon phases and organic compounds. Possibly, the cometary CHON grains may be related to kerogen material of an interstellar origin in carbonaceous meteorites. Pure carbon grains, hydrocarbons and polymers of cyanopolyynes, and multi-carbon monoxides are present in cometary dust as compositionally simple and distinctive components among a variety of others. There is no clear evidence of significant presence of pure formaldehyde or HCN polymers in Halley dust particles. The diversity of types of cometary organic compounds is consistent with the inter-stellar dust model of comets and probably reflects differences in composition of precursor dust. Preservation of this heterogeneity among submicron particles suggest the gentle formation of cometary, nucleus by aggregation of interstellar dust in the protosolar nebula without complete mixing or chemical homogenization at the submicron level.

Investigating the Use of a Diffusion Flame to Produce Black Carbon Standards for Thermal- Optical Analysis of Carbonaceous Aerosols

NASA Astrophysics Data System (ADS)

Ortiz Montalvo, D. L.; Kirchstetter, T. W.; Soto-García, L. L.; Mayol-Bracero, O. L.

2006-12-01

Combustion generated particles are a concern to both climate and public health due to their ability to scatter and absorb solar radiation and alter cloud properties, and because they are small enough to be inhaled and deposit in the lungs where they may cause respiratory and other health problems. Specific concern is focused on particles that originate from the combustion of diesel fuel. Diesels particles are composed mainly of carbonaceous material, especially in locations where diesel fuel sulfur is low. These particles are black due to the strongly light absorbing nature of the refractory carbon components, appropriately called black carbon (BC). This research project focuses on the uncertainty in the measurement of BC mass concentration, which is typically determined by analysis of particles collected on a filter using a thermal-optical analysis (TOA) method. Many studies have been conducted to examine the accuracy of the commonly used variations of the TOA method, which vary in their sample heating protocol, carrier gas, and optical measurement. These studies show that BC measurements are inaccurate due to the presence of organic carbon (OC) in the aerosols. OC may co-evolve with BC or char to form BC during analysis, both of which make it difficult to distinguish between the OC and BC in the sample. The goal of this study is to develop the capability of producing standard samples of known amounts of BC, either alone or mixed with other aerosol constituents, and then evaluate which TOA methods accurately determine the BC amount. An inverted diffusion flame of methane and air was used to produce particle samples containing only BC as well as samples of BC mixed with humic acid (HA). Our study found that HA is light absorbing and catalyzes the combustion of BC. It is expected that both of these attributes will challenge the ability of TOA methods in distinguishing between OC and BC, such as the simple two step TOA method which relies solely on temperature to

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

NASA Astrophysics Data System (ADS)

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

2012-06-01

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

MODELS-3 COMMUNITY MULTISCALE AIR QUALITY (CMAQ) MODEL AEROSOL COMPONENT 1: MODEL DESCRIPTION

EPA Science Inventory

The aerosol component of the Community Multiscale Air Quality (CMAQ) model is designed to be an efficient and economical depiction of aerosol dynamics in the atmosphere. The approach taken represents the particle size distribution as the superposition of three lognormal subdis...

Contribution of Biomass Burning to Carbonaceous Aerosols in Mexico City during may 2013

NASA Astrophysics Data System (ADS)

Tzompa Sosa, Z. A.; Sullivan, A.; Kreidenweis, S. M.

2014-12-01

The Mexico City Metropolitan Area (MCMA) is one of the largest megacities in the world with a population of 20 million people. Emissions transported from outside the basin, such as wildfires and agricultural burning, represent a potentially large contribution to air quality degradation. This study analyzed PM10 filter samples from six different stations located across the MCMA from May, 2013, which represented the month with the most reported fire counts in the region between 2002-2013. Two meteorological regimes were established considering the number of satellite derived fire counts, changes in predominant wind direction, ambient concentrations of CO, PM10 and PM2.5, and precipitation patterns inside MCMA. The filter samples were analyzed for biomass burning tracers including levoglucosan (LEV), water-soluble potassium (WSK+); and water-soluble organic carbon (WSOC). Results of these analyses show that LEV concentrations correlated positively with ambient concentrations of PM2.5 and PM10 (R2=0.61 and R2=0.46, respectively). Strong correlations were also found between WSOC and LEV (R2=0.94) and between WSK+ and LEV (R2=0.75). An average LEV/WSOC ratio of 0.0147 was estimated for Regime 1 and 0.0062 for Regime 2. Our LEV concentrations and LEV/WSOC ratios are consistent with results found during the MILAGRO campaign (March, 2006). To the best of our knowledge, only total potassium concentrations have been measured in aerosol samples from MCMA. Therefore, this is the first study in MCMA to measure ambient concentrations of WSK+. Analysis of gravimetric mass concentrations showed that PM2.5 accounted for 60% of the PM10 mass concentration with an estimated PM10/PM2.5 ratio of 1.68. Estimates from our laboratory filter sample characterization indicated that we measured 37% of the total PM10 mass concentration. The missing mass is most likely crustal material (soil or dust) and carbonaceous aerosols that were not segregated into WSOC fraction. Assuming that LEV is

Chapter 3: Evaluating the impacts of carbonaceous aerosols on clouds and climate

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

Menon, Surabi; Del Genio, Anthony D.

Any attempt to reconcile observed surface temperature changes within the last 150 years to changes simulated by climate models that include various atmospheric forcings is sensitive to the changes attributed to aerosols and aerosol-cloud-climate interactions, which are the main contributors that may well balance the positive forcings associated with greenhouse gases, absorbing aerosols, ozone related changes, etc. These aerosol effects on climate, from various modeling studies discussed in Menon (2004), range from +0.8 to -2.4 W m{sup -2}, with an implied value of -1.0 W m{sup -2} (range from -0.5 to -4.5 W m{sup -2}) for the aerosol indirect effects.more » Quantifying the contribution of aerosols and aerosol-cloud interactions remain complicated for several reasons some of which are related to aerosol distributions and some to the processes used to represent their effects on clouds. Aerosol effects on low lying marine stratocumulus clouds that cover much of the Earth's surface (about 70%) have been the focus of most of prior aerosol-cloud interaction effect simulations. Since cumulus clouds (shallow and deep convective) are short lived and cover about 15 to 20% of the Earth's surface, they are not usually considered as radiatively important. However, the large amount of latent heat released from convective towers, and corresponding changes in precipitation, especially in biomass regions due to convective heating effects (Graf et al. 2004), suggest that these cloud systems and aerosol effects on them, must be examined more closely. The radiative heating effects for mature deep convective systems can account for 10-30% of maximum latent heating effects and thus cannot be ignored (Jensen and Del Genio 2003). The first study that isolated the sensitivity of cumulus clouds to aerosols was from Nober et al. (2003) who found a reduction in precipitation in biomass burning regions and shifts in circulation patterns. Aerosol effects on convection have been included in

Aerosol Remote Sensing from AERONET, the Ground-Based Satellite

NASA Technical Reports Server (NTRS)

Holben, Brent N.

2012-01-01

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

Improvements to the OMI Near-uv Aerosol Algorithm Using A-train CALIOP and AIRS Observations

NASA Technical Reports Server (NTRS)

Torres, O.; Ahn, C.; Zhong, C.

2014-01-01

The height of desert dust and carbonaceous aerosols layers and, to a lesser extent, the difficulty in assessing the predominant size mode of these absorbing aerosol types, are sources of uncertainty in the retrieval of aerosol properties from near UV satellite observations. The availability of independent, near-simultaneous measurements of aerosol layer height, and aerosol-type related parameters derived from observations by other A-train sensors, makes possible the direct use of these parameters as input to the OMI (Ozone Monitoring Instrument) near UV retrieval algorithm. A monthly climatology of aerosol layer height derived from observations by the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) sensor, and real-time AIRS (Atmospheric Infrared Sounder) CO observations are used in an upgraded version of the OMI near UV aerosol algorithm. AIRS CO measurements are used as a reliable tracer of carbonaceous aerosols, which allows the identification of smoke layers in areas and times of the year where the dust-smoke differentiation is difficult in the near-UV. The use of CO measurements also enables the identification of elevated levels of boundary layer pollution undetectable by near UV observations alone. In this paper we discuss the combined use of OMI, CALIOP and AIRS observations for the characterization of aerosol properties, and show a significant improvement in OMI aerosol retrieval capabilities.

Anthropogenic iron oxide aerosols enhance atmospheric heating

NASA Astrophysics Data System (ADS)

Moteki, Nobuhiro; Adachi, Kouji; Ohata, Sho; Yoshida, Atsushi; Harigaya, Tomoo; Koike, Makoto; Kondo, Yutaka

2017-05-01

Combustion-induced carbonaceous aerosols, particularly black carbon (BC) and brown carbon (BrC), have been largely considered as the only significant anthropogenic contributors to shortwave atmospheric heating. Natural iron oxide (FeOx) has been recognized as an important contributor, but the potential contribution of anthropogenic FeOx is unknown. In this study, we quantify the abundance of FeOx over East Asia through aircraft measurements using a modified single-particle soot photometer. The majority of airborne FeOx particles in the continental outflows are of anthropogenic origin in the form of aggregated magnetite nanoparticles. The shortwave absorbing powers (Pabs) attributable to FeOx and to BC are calculated on the basis of their size-resolved mass concentrations and the mean Pabs(FeOx)/Pabs(BC) ratio in the continental outflows is estimated to be at least 4-7%. We demonstrate that in addition to carbonaceous aerosols the aggregate of magnetite nanoparticles is a significant anthropogenic contributor to shortwave atmospheric heating.

Anthropogenic iron oxide aerosols enhance atmospheric heating

PubMed Central

Moteki, Nobuhiro; Adachi, Kouji; Ohata, Sho; Yoshida, Atsushi; Harigaya, Tomoo; Koike, Makoto; Kondo, Yutaka

2017-01-01

Combustion-induced carbonaceous aerosols, particularly black carbon (BC) and brown carbon (BrC), have been largely considered as the only significant anthropogenic contributors to shortwave atmospheric heating. Natural iron oxide (FeOx) has been recognized as an important contributor, but the potential contribution of anthropogenic FeOx is unknown. In this study, we quantify the abundance of FeOx over East Asia through aircraft measurements using a modified single-particle soot photometer. The majority of airborne FeOx particles in the continental outflows are of anthropogenic origin in the form of aggregated magnetite nanoparticles. The shortwave absorbing powers (Pabs) attributable to FeOx and to BC are calculated on the basis of their size-resolved mass concentrations and the mean Pabs(FeOx)/Pabs(BC) ratio in the continental outflows is estimated to be at least 4–7%. We demonstrate that in addition to carbonaceous aerosols the aggregate of magnetite nanoparticles is a significant anthropogenic contributor to shortwave atmospheric heating. PMID:28508863

Carbonaceous Aerosol Characteristics over a Pinus taeda plantation: Results from the CELTIC experiment

EPA Science Inventory

Carbonaceous particles smaller than 2.5 um aerodynamic diameter (PM2.5) were collected in July, 2003 over a Loblolly Pine plantation at Duke Forest, NC during the Chemical Emission, Loss, Transformation and Interactions within Canopies (CELTIC) field study. Organic (OC) and eleme...

SOURCE APPORTIONMENT OF PRIMARY CARBONACEOUS AEROSOL USING THE COMMUNITY MULTISCALE AIR QUALITY MODEL

EPA Science Inventory

A substantial fraction of fine particulate matter (PM) across the United States is composed of carbon, which may be either emitted in particulate form (i.e., primary) or formed in the atmosphere through gas-to-particle conversion processes (i.e., secondary). Primary carbonaceous...

The impact of biogenic carbon emissions on aerosol absorption inMexico City

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

Marley, N; Gaffney, J; Tackett, M J

2009-02-24

In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbingmore » secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.« less

Improved measurement of carbonaceous aerosol in Beijing, China: intercomparison of sampling and thermal-optical analysis methods

NASA Astrophysics Data System (ADS)

Cheng, Y.; He, K. B.; Duan, F. K.; Zheng, M.; Ma, Y. L.; Tan, J. H.; Du, Z. Y.

2010-06-01

The sampling artifacts (both positive and negative) and the influence of thermal-optical methods (both charring correction method and the peak inert mode temperature) on the split of organic carbon (OC) and elemental carbon (EC) were evaluated in Beijing. The positive sampling artifact constituted 10% and 23% of OC concentration determined by the bare quartz filter during winter and summer, respectively. For summer samples, the adsorbed gaseous organics were found to continuously evolve off the filter during the whole inert mode when analyzed by the IMPROVE-A temperature protocol. This may be due to the oxidation of the adsorbed organics during sampling (reaction artifact) which would increase their thermal stability. The backup quartz approach was evaluated by a denuder-based method for assessing the positive artifact. The quartz-quartz (QBQ) in series method was demonstrated to be reliable, since all of the OC collected by QBQ was from originally gaseous organics. Negative artifact that could be adsorbed by quartz filter was negligible. When the activated carbon impregnated glass fiber (CIG) filter was used as the denuded backup filter, the denuder efficiency for removing gaseous organics that could be adsorbed by the CIG filter was only about 30%. EC values were found to differ by a factor of about two depending on the charring correction method. Influence of the peak inert mode temperature was evaluated based on the summer samples. The EC value was found to continuously decrease with the peak inert mode temperature. Premature evolution of light absorbing carbon began when the peak inert mode temperature was increased from 580 to 650 °C; when further increased to 800 °C, the OC and EC split frequently occurred in the He mode, and the last OC peak was characterized by the overlapping of two separate peaks. The discrepancy between EC values defined by different temperature protocols was larger for Beijing carbonaceous aerosol compared with North America and

Carbonaceous PM2.5 emitted from light-duty vehicles operating on low-level ethanol fuel blends.

EPA Science Inventory

This study aims to examine carbonaceous aerosol emissions from three Tier 2-certified 2008 model year LDVs burning e0, e10, and e85 fuel blends at -7°C and 24°C. The LDVs were tested on an electric chasis dynamometer using the LA-92 Urban Driving Cycle (UDC). Exhaust was ...

Assessing the impact of industrial source emissions on atmospheric carbonaceous aerosol concentrations using routine monitoring networks.

PubMed

Sheesley, Rebecca J; Schauer, James J; Orf, Marya L

2010-02-01

Industrial sources can have a significant but poorly defined impact on ambient particulate matter concentrations in select areas. Detailed emission profiles are often not available and are hard to develop because of the diversity of emissions across time and space at large industrial complexes. A yearlong study was conducted in an industrial area in Detroit, MI, which combined real-time particle mass (tapered element oscillating microbalance) and black carbon (aetholometer) measurements with molecular marker measurements of monthly average concentrations as well as daily concentrations of select high pollution days. The goal of the study was to use the real-time data to define days in which the particulate matter concentration in the atmosphere was largely impacted by local source emissions and to use daily speciation data to derive emission profiles for the industrial source. When combined with motor vehicle exhaust, wood smoke and road dust profiles, the industrial source profile was used to determine the contribution of the local industrial source to the total organic carbon (OC) concentrations using molecular marker-chemical mass balance modeling (MM-CMB). The MM-CMB analysis revealed that the industrial source had minimal impact on the monthly average carbonaceous aerosol concentration, but contributed approximately 2 microg m(-3), or a little over one-third of the total OC, on select high-impact days.

Simulation of Aerosol Transport and Radiative Effects In Lmd-gcm During Indoex-ifp 1999

NASA Astrophysics Data System (ADS)

Reddy, M. S.; Boucher, O.; Léon, J.-F.; Venkataraman, C.; Pham, M.

During the January-March 1999, an international collaborative field experiment, In- dian Ocean Experiment (INDOEX) was carried out to understand the anthropogenic aerosol effects on radiative forcing (Ramanathan, 2001). In the present work we sim- ulated the cycle of the multi-component aerosol (sulphate, black carbon, organic car- bon, dust, sea-salt and fly-ash) in the Laboratoire de Météorologie Dynamique General Circulation Model (LMD GCM) and estimated the consequent radiative forcing. Sim- ulations are carried out in the zoomed version of the model focusing on the Indian sub- continent and Indian Ocean regions, for January-April 1999. To account correctly for the aerosol emissions in the source regions (Indian subcontinent) we have integrated newly developed SO2 and aerosol emission inventory for India for 1999 (Reddy and Venkataraman, 2002a and b) into the global emission data set input to model. Model performance is evaluated by comparing the simulated aerosol concentration fields against measurements over continental and oceanic stations. Model predicted concentrations agree well in the oceanic stations but are in the lower end of mea- surements in the continental stations. A large plume of sulphate and other aerosols ex- tended from the Indian sub-continent into the Indian Ocean, from surface and elevated flows, extending down to 5S in the pristine southern Indian Ocean. Predicted spec- trally resolved aerosol optical depths (AOD) will be compared with sun-photometer measurements in the region. We also present a comparison of model predicted aerosol optical depths with satellite (Meteosat) derived AOD for the same period. An assess- ment of the multi-component aerosol radiative forcing will be made and results will be discussed in the context of the possible climate effects over the region. Finally, the regional source contributions to sulphate and carbonaceous aerosol loadings in the Indian Ocean will be presented.

Maritime Aerosol Network as a Component of AERONET - a Useful Tool for Evaluation of the Global Sea-Salt Aerosol Distribution

NASA Astrophysics Data System (ADS)

Smirnov, A.; Holben, B. N.; Kinne, S.; Nelson, N. B.; Stenchikov, G. L.; Broccardo, S. P.; Sowers, D.; Lobecker, E.; Ondrusek, M.; Zielinski, T. P.; Gray, L. M.; Frouin, R.; Radionov, V. F.; Smyth, T. J.; Zibordi, G.; Heller, M. I.; Slabakova, V.; Krüger, K.; Reid, E. A.; Istomina, L.; Vandermeulen, R. A.; O'Neill, N. T.; Levy, G.; Giles, D. M.; Slutsker, I.; Sorokin, M. G.; Eck, T. F.

2016-02-01

Sea-salt aerosol plays an important role in radiation balance and chemistry of marine atmosphere. Sea-salt production depends on various factors. There is a significant uncertainty in the parametrization of the sea-salt production and budget. Ship-based aerosol optical depth (AOD) measurements can be used as an important validation tool for various global models and in-situ measurements. The paper presents the current status of the Maritime Aerosol Network (MAN) which is a component of Aerosol Robotic Network. Since 2006 over 300 cruises were completed and data archive of more than 5500 measurement days is accessible at http://aeronet.gsfc.nasa.gov/new_web/maritime_aerosol_network.html . AOD measurements from ships of opportunity complemented island-based AERONET measurements and provided important reference points for satellite retrieved and modelled AOD climatology over the oceans. The program exemplifies mutually beneficial international, multi-agency effort in atmospheric aerosol optical studies over the oceans.

Aerosol carbon isotope composition over Baltic Sea

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

Beyond the Alphabet Soup: Molecular Properties of Aerosol Components Influence Optics. (Invited)

NASA Astrophysics Data System (ADS)

Thompson, J. E.

2013-12-01

Components within atmospheric aerosols exhibit almost every imaginable model of chemical bonding and physical diversity. The materials run the spectrum from crystalline to amorphous, covalent to ionic, and have varying viscosities, phase, and hygroscopicity. This seminar will focus on the molecular properties of materials that influence the optical behavior of aerosols. Special focus will be placed on the polarizability of materials, hygroscopic growth, and particle phase.

On the mixing and evaporation of secondary organic aerosol components.

PubMed

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

2013-06-18

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

Molybdenum isotopic evidence for the origin of chondrules and a distinct genetic heritage of carbonaceous and non-carbonaceous meteorites

NASA Astrophysics Data System (ADS)

Budde, Gerrit; Burkhardt, Christoph; Brennecka, Gregory A.; Fischer-Gödde, Mario; Kruijer, Thomas S.; Kleine, Thorsten

2016-11-01

Nucleosynthetic isotope anomalies are powerful tracers to determine the provenance of meteorites and their components, and to identify genetic links between these materials. Here we show that chondrules and matrix separated from the Allende CV3 chondrite have complementary nucleosynthetic Mo isotope anomalies. These anomalies result from the enrichment of a presolar carrier enriched in s-process Mo into the matrix, and the corresponding depletion of this carrier in the chondrules. This carrier most likely is a metal and so the uneven distribution of presolar material probably results from metal-silicate fractionation during chondrule formation. The Mo isotope anomalies correlate with those reported for W isotopes on the same samples in an earlier study, suggesting that the isotope variations for both Mo and W are caused by the heterogeneous distribution of the same carrier. The isotopic complementary of chondrules and matrix indicates that both components are genetically linked and formed together from one common reservoir of solar nebula dust. As such, the isotopic data require that most chondrules formed in the solar nebula and are not a product of protoplanetary impacts. Allende chondrules and matrix together with bulk carbonaceous chondrites and some iron meteorites (groups IID, IIIF, and IVB) show uniform excesses in 92Mo, 95Mo, and 97Mo that result from the addition of supernova material to the solar nebula region in which these carbonaceous meteorites formed. Non-carbonaceous meteorites (enstatite and ordinary chondrites as well as most iron meteorites) do not contain this material, demonstrating that two distinct Mo isotope reservoirs co-existed in the early solar nebula that remained spatially separated for several million years. This separation was most likely achieved through the formation of the gas giants, which cleared the disk between the inner and outer solar system regions parental to the non-carbonaceous and carbonaceous meteorites. The Mo isotope

Preliminary Results from an Assimilation of TOMS Aerosol Observations Into the GOCART Model

NASA Technical Reports Server (NTRS)

daSilva, Arlindo; Weaver, Clark J.; Ginoux, Paul; Torres, Omar; Einaudi, Franco (Technical Monitor)

2000-01-01

At NASA Goddard we are developing a global aerosol data assimilation system that combines advances in remote sensing and modeling of atmospheric aerosols. The goal is to provide high resolution, 3-D aerosol distributions to the research community. Our first step is to develop a simple assimilation system for Saharan mineral aerosol. The Goddard Chemistry and Aerosol Radiation model (GOCART) provides accurate 3-D mineral aerosol size distributions that compare well with TOMS satellite observations. Surface, mobilization, wet and dry deposition, convective and long-range transport are all driven by assimilated fields from the Goddard Earth Observing System Data Assimilation System, GEOS-DAS. Our version of GOCART transports sizes from.08-10 microns and only simulates Saharan dust. TOMS radiance observations in the ultra violet provide information on the mineral and carbonaceous aerosol fields. We use two main observables in this study: the TOMS aerosol index (AI) which is directly related to the ratio of the 340 and 380 radiances and the 380 radiance. These are sensitive to the aerosol optical thickness, the single scattering albedo and the height of the aerosol layer. The Goddard Aerosol Assimilation System (GAAS) uses the Data Assimilation Office's Physical-space Statistical Analysis System (PSAS) to combine TOMS observations and GOCART model first guess fields. At this initial phase we only assimilate observations into the the GOCART model over regions of Africa and the Atlantic where mineral aerosols dominant and carbonaceous aerosols are minimal, Our preliminary results during summer show that the assimilation with TOMS data modifies both the aerosol mass loading and the single scattering albedo. Assimilated aerosol fields will be compared with assimilated aerosol fields from GOCART and AERONET observations over Cape Verde.

Seasonal variability of carbonaceous aerosols in an urban background area in Southern Italy

NASA Astrophysics Data System (ADS)

Cesari, D.; Merico, E.; Dinoi, A.; Marinoni, A.; Bonasoni, P.; Contini, D.

2018-02-01

Organic (OC) and Elemental Carbon (EC) are important components of atmospheric aerosol particles, playing a key role in climate system and potentially affecting human health. There is a lack of data reported for Southern Italy and this work aims to fill this gap, focusing the attention on the long-term trends of OC and EC concentrations in PM2.5 and PM10, and on atmospheric processes and sources influencing seasonal variability. Measurements were taken at the Environmental-Climate Observatory of Lecce (SE Italy, 40°20‧8″N-18°07‧28″E, 37 m a.s.l.), regional station of the Global Atmosphere Watch program (GAW-WMO). Daily PM10 and PM2.5 samples were collected between July 2013 and July 2016. In addition, starting in December 2014, simultaneous equivalent Black Carbon (eBC) concentrations in PM10 were measured using a Multi Angle Absorption Photometer. A subset of 722 PM samples (361 for each size fraction) was analysed by using a thermo-optical method with a Sunset Laboratory OC/EC analyser, to determine elemental and organic carbon concentrations. The average PM10 and PM2.5 concentrations were 28.8 μg/m3 and 17.5 μg/m3. The average OC and EC concentrations in PM10 were 5.4 μg/m3 and 0.8 μg/m3, in PM2.5 these were 4.7 μg/m3 and 0.6 μg/m3. Carbonaceous content was larger during cold season with respect to warm season as well as secondary organic carbon (SOC) that was evaluated using the OC/EC minimum ratio method. SOC was mainly segregated in PM2.5 and represented 53% - 75% of the total OC. A subset of EC data was compared with eBC measurements, showing a good correlation (R2 = 0.80), however, eBC concentrations were higher than EC concentrations of an average factor of 1.95 (+/- 0.55 standard deviation). This could be explained by the presence of a contribution of Brown Carbon (BrC), for example from biomass burning, in eBC measurements. Weekly patterns showed a slight decrease of carbon content during weekends with respect to weekdays especially

Fine carbonaceous aerosol characteristics at a megacity during the Chinese Spring Festival as given by OC/EC online measurements

NASA Astrophysics Data System (ADS)

Liu, Baoshuang; Bi, Xiaohui; Feng, Yinchang; Dai, Qili; Xiao, Zhimei; Li, Liwei; Wu, Jianhui; Yuan, Jie; Zhang, YuFen

2016-11-01

The OC/EC online monitoring campaign was carried out in Tianjin of China from 8th February to 15th March 2015 during the Chinese Spring Festival period (CSFP). The concentrations of OC, EC, BC and other ambient pollutants (e.g. SO2, NO2 and PM2.5, etc.) in high time resolution were measured with related online-monitoring instruments. During the CSFP, according to the peaks of PM2.5 concentrations and number concentrations (NC) of aerosol particles with aerodynamic diameters between 0.3 and 2.5 μm, five pollution-events were generally identified and displayed. These pollution-events were closely associated with large-scale fireworks displaying, combustion activities such as heating for winter, and the stable meteorological conditions, etc. During the CSFP, EC and OC concentrations showed variations up to one order of magnitude. The uncertainty of instrument itself and the difference for measured methods, further caused the differences between thermal OC (measured OC by thermal method) and optical OC (measured OC by optical method) concentrations, as well as between thermal EC (measured EC by thermal method) and optical EC (measured EC by optical method) concentrations. The high-concentration carbonaceous aerosols could enlarge the uncertainty of measuring instrument, reducing the correlations between OC and EC, and enhance the differences among thermal EC, optical BC and optical EC. The OC/EC ratios and the percentages of SOC/OC would be declined, when the pollution-events formed during the CSFP. Due to the different sources for thermal POC and thermal SOC, the correlation of the two was relatively lower (R2 = 0.39). Thermal POC dominated over thermal OC during the CSFP.

Vertical separation of the atmospheric aerosol components by using poliphon retrieval in polarized micro pulse lidar (P-MPL) measurements: case studies of specific climate-relevant aerosol types

NASA Astrophysics Data System (ADS)

Córdoba-Jabonero, Carmen; Sicard, Michaël; Ansmann, Albert; Águila, Ana del; Baars, Holger

2018-04-01

POLIPHON (POlarization-LIdar PHOtometer Networking) retrieval consists in the vertical separation of two/three particle components in aerosol mixtures, highlighting their relative contributions in terms of the optical properties and mass concentrations. This method is based on the specific particle linear depolarization ratio given for different types of aerosols, and is applied to the new polarized Micro-Pulse Lidar (P-MPL). Case studies of specific climate-relevant aerosols (dust particles, fire smoke, and pollen aerosols, including a clean case as reference) observed over Barcelona (Spain) are presented in order to evaluate firstly the potential of P-MPLs measurements in combination with POLIPHON for retrieving the vertical separation of those particle components forming aerosol mixtures and their properties.

Radiocarbon-insights into temporal variations in the sources and concentrations of carbonaceous aerosols in the Los Angeles and Salt Lake City Metropolitan Areas

NASA Astrophysics Data System (ADS)

Czimczik, Claudia; Mouteva, Gergana; Simon, Fahrni; Guaciara, Santos; James, Randerson

2014-05-01

Increased fossil fuel consumption and biomass burning are contributing to significantly larger emissions of black carbon (BC) aerosols to the atmosphere. Together with organic carbon (OC), BC is a major constituent of fine particulate matter in urban air, contributes to haze and has been linked to a broad array of adverse health effects. Black carbon's high light absorption capacity and role in key (in-)direct climate feedbacks also lead to a range of impacts in the Earth system (e.g. warming, accelerated snow melt, changes in cloud formation). Recent work suggests that regulating BC emissions can play an important role in improving regional air quality and reducing future climate warming. However, BC's atmospheric transport pathways, lifetime and magnitudes of emissions by sector and region, particularly emissions from large urban centers, remain poorly constrained by measurements. Contributions of fossil and modern sources to the carbonaceous aerosol pool (corresponding mainly to traffic/industrial and biomass-burning/biogenic sources, respectively) can be quantified unambiguously by measuring the aerosol radiocarbon (14C) content. However, accurate 14C-based source apportionment requires the physical isolation of BC and OC, and minimal sample contamination with extraneous carbon or from OC charring. Compound class-specific 14C analysis of BC remains challenging due to very small sample sizes (5-15 ug C). Therefore, most studies to date have only analyzed the 14C content of the total organic carbonaceous aerosol fraction. Here, we present time-series 14C data of BC and OC from the Los Angeles (LA) metropolitan area in California - one of two megacities in the United States - and from Salt Lake City (SLC), UT. In the LA area, we analyzed 48h-PM10 samples near the LA port throughout 2007 and 2008 (with the exception of summer). We also collected monthly-PM2.5 samples at the University of California - Irvine, with shorter sampling periods during regional wildfire

Decadal trend of black carbon and refractory carbonaceous aerosol in the western rim of the North Pacific Ocean: atmospheric concentration and the retrieved record of deposition flux

NASA Astrophysics Data System (ADS)

Kaneyasu, Naoki; Yamaguchi, Takashi; Noguchi, Izumi; Akiyama, Masayuki; Matsumoto, Kiyoshi

2013-04-01

The long-term trend of light absorbing carbonaceous aerosols (or black carbon: BC) or refractory carbonaceous aerosol (or elemental carbon: EC) concentration is reported at European background sites such as Mace Head, and that of aerosol absorption coefficient are monitored in many GAW sites. On the contrary, such long-term data are relatively scarce at around the western part of the North Pacific Ocean. Thus, to understand the long-term variation of in the area, BC in fine aerosol fraction has been measured at Chichi-jima Islands, Japan. Chichi-jima Island is located 1000 km south of the Japanese mainland, and 1800 km west of the coast line of the Asian continent. BC has been measured with an Aethalometer (Magee, AE-16 and AE-30) since December, 1998 with 1 hr time resolution. Mass flowmeter embedded inside the Aethalometer is calibrated with a rotational dry gas-meter once a year. Monthly averaged BC concentration shows an obvious seasonal variation, i.e. high concentration during late autumn-winter-spring period resulting from the transport from East Asia, with maximum daily concentration above 500 ng m-3. In summer, daily concentration was usually less than 20 ng m-3, due to the clean background airmass originating from the North Pacific Anticyclone. Decadal trend of the annual averaged BC concentration showed a increasing trend from 2000 to 2007 and started to decrease after 2008, which roughly coincides with the reported emission trend of SO2 in China (Lu et al., 2010). In addition, total (i.e., wet + dry) deposition record of refractory carbon at two sites in the northern Japan (Rishiri Island: a remote island site, and Sapporo City: an urban site) are retrieved. At these sites, the local government have been measuring the chemical components in precipitation water collected by deposition gauges. In the deposition gauge, a membrane filter made of cellulose-acetate is fixed at the bottom of the funnel to remove water-insoluble particles from the precipitated

Time-resolved distributions of bulk parameters, diacids, ketoacids and α-dicarbonyls and stable carbon and nitrogen isotope ratios of TC and TN in tropical Indian aerosols: Influence of land/sea breeze and secondary processes

NASA Astrophysics Data System (ADS)

Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.

2015-02-01

To better understand the photochemical production and diurnal distributions of organic and inorganic aerosols in the tropical coastal Indian atmosphere, the aerosol (TSP) samples were collected every 3 h during 30-31 January, 14-15 February and 28-29 May 2007 from Chennai and studied for total carbon (TC) and nitrogen (TN) and their stable isotope ratios (δ13CTC and δ15NTN), carbonaceous components, inorganic ions, diacids, ketoacids and α-dicarbonyls. Time-resolved distributions of bulk parameters, inorganic ions, and diacids and related compounds, except for few species, did not show any clear diurnal trend but showed peaks at 6-9 h during all the study periods, except for the peak at 15-18 h on 28 May. SO42-, C2 - C6 diacids, ketoacids and α-dicarbonyls in February and on 29 May showed a diurnal trend. δ13CTC and δ15NTN stayed relatively constant during the study periods but showed 13C depletion (in January) and 15 N enrichment when TC and TN peaked. Based on these results together with air mass trajectories, we found that the diurnal distributions of Chennai aerosols are mainly influenced by land/sea breeze and the aged (photochemically processed) air masses, although in situ photochemical production and nighttime chemistry of secondary aerosol species, particularly C2-C4 diacids and SO42-, are significant. The characteristics of seasonal variations of carbonaceous components, and diacids and related compounds and comparisons of δ13CTC and δ15NTN of Chennai aerosols with the isotopic signatures of the point sources inferred that biofuel/biomass burning in South and Southeast Asia are the major sources of aerosols (TSP).

ANALYSIS OF CARBONACEOUS AEROSOLS USING THE THERMAL OPTICAL TRANSMITTANCE AND THERMAL OPTICAL REFLECTANCE METHODS

EPA Science Inventory

Carbonaceous particulate typically represents a large fraction of PM2.5 (20 - 40%). Two primary techniques presently used for the analysis of particulate carbon are Thermal Optical Transmission (TOT - NIOSH Method 5040) and Thermal Optical Reflectance (TOR). These two methods b...

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

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

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

2015-09-28

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

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

DOE PAGES

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

2015-08-26

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

Molecular marker characterization and source appointment of particulate matter and its organic aerosols.

PubMed

Choi, Jong-Kyu; Ban, Soo-Jin; Kim, Yong-Pyo; Kim, Yong-Hee; Yi, Seung-Muk; Zoh, Kyung-Duk

2015-09-01

This study was carried out to identify possible sources and to estimate their contribution to total suspended particle (TSP) organic aerosol (OA) contents. A total of 120 TSP and PM2.5 samples were collected simultaneously every third day over a one-year period in urban area of Incheon, Korea. High concentration in particulate matters (PM) and its components (NO3(-), water soluble organic compounds (WSOCs), and n-alkanoic acids) were observed during the winter season. Among the organics, n-alkanes, n-alkanoic acids, levoglucosan, and phthalates were major components. Positive matrix factorization (PMF) analysis identified seven sources of organic aerosols including combustion 1 (low molecular weight (LMW)-polycyclic aromatic hydrocarbons (PAHs)), combustion 2 (high molecular weight (HMW)-PAHs), biomass burning, vegetative detritus (n-alkane), secondary organic aerosol 1 (SOA1), secondary organic aerosol 2 (SOA2), and motor vehicles. Vegetative detritus increased during the summer season through an increase in biogenic/photochemical activity, while most of the organic sources were prominent in the winter season due to the increases in air pollutant emissions and atmospheric stability. The correlation factors were high among the main components of the organic carbon (OC) in the TSP and PM2.5. The results showed that TSP OAs had very similar characteristics to the PM2.5 OAs. SOA, combustion (PAHs), and motor vehicle were found to be important sources of carbonaceous PM in this region. Our results imply that molecular markers (MMs)-PMF model can provide useful information on the source and characteristics of PM. Copyright © 2015 Elsevier Ltd. All rights reserved.

Estimation of columnar concentrations of absorbing and scattering fine mode aerosol components using AERONET data

NASA Astrophysics Data System (ADS)

Choi, Yongjoo; Ghim, Young Sung

2016-11-01

Columnar concentrations of absorbing and scattering components of fine mode aerosols were estimated using Aerosol Robotic Network (AERONET) data for a site downwind of Seoul. The study period was between March 2012 and April 2013 including the period of the Distributed Regional Aerosol Gridded Observation Networks (DRAGON)-Asia campaign in March to May 2012. The Maxwell Garnett mixing rule was assumed for insoluble components embedded in a host solution, while the volume average mixing rule was assumed for the aqueous solution of soluble components. During the DRAGON-Asia campaign the surface concentrations of major components of fine particles were measured. The columnar mass fractions of black carbon (BC), organic carbon (OC), mineral dust (MD), and ammonium sulfate (AS) were 1.5, 5.9, 6.6, and 52%, respectively, which were comparable to the mass fractions measured at the surface for BC, OC, and secondary inorganic aerosols at 2.3, 18, and 55%. The vertical distributions of BC and AS were investigated by employing the concept of a column height. While the column height for BC was similar to the planetary boundary layer (PBL) height, that for AS was 4.4 times higher than the PBL height and increased with air temperature from March to May. The monthly variations of the columnar mass concentrations during the study period were generally well explained in term of meteorology and emission characteristics. However, certain variations of MD were different from those typically observed primarily because only fine mode aerosols were considered.

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.

Analysis of Individual Carbonaceous Particles Emitted from the Las Conchas Wildfire, Los Alamos, NM, in June-July 2011

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; China, S.; Gorkowski, K.; Flowers, B. A.; Aiken, A. C.; Dubey, M. K.

2012-12-01

Carbonaceous aerosol emitted from biomass burning contributes significantly to atmospheric aerosol loadings regionally and globally. The net direct radiative forcing of biomass burning aerosol can be positive and/or negative and this depends on its composition, morphology and mixing state. Biomass burning aerosols can also change the cloud properties as they can act as cloud condensation nuclei. In this study we investigated biomass burning particles emitted from the Las Conchas wildfire in northern New Mexico that started on June 26, 2011 and burned an area of 245 square miles. Aerosol samples were collected on nucleopore filters at the Los Alamos National Laboratory during the third week of the wildfire event. Individual particles (~4000) were investigated using field-emission scanning electron microscopy and energy dispersive X-ray spectroscopy (EDS) to distinguish different carbonaceous particles and their shape, size, elemental composition and mixing state. A thermo-denuder was used to remove compounds that are volatile at temperatures up to 200 C, leaving behind the black carbon and any compounds that did not volatize completely. Smoke particles consisted of a) tar balls, which are amorphous spherical carbonaceous organic aerosols; b) organic particles with inorganic inclusions, c) soot particles and (d) soot with various inclusions. Two distinct kinds of tar balls, "electronically" dark and bright, were found using the field-emission scanning electron microscopy and were characterized for ambient and denuded conditions to understand coating effects and aging. It was found that dark tar balls are generally larger in size than the bright ones. Additionally, the difference between the size of ambient-bright and the size of denuded-bright tar balls was larger than the difference between the size of ambient-dark and the size of denuded-dark tar balls. EDS analysis showed that 70% of the dark tar balls had higher (~60%) relative oxygen content than in the bright

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

PubMed

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

2002-11-15

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

What Controls the Vertical Distribution of Aerosol? Relationships Between Process Sensitivity in HadGEM3-UKCA and Inter-Model Variation from AeroCom Phase II

NASA Technical Reports Server (NTRS)

Kipling, Zak; Stier, Philip; Johnson, Colin E.; Mann, Graham W.; Bellouin, Nicolas; Bauer, Susanne E.; Bergman, Tommi; Chin, Mian; Diehl, Thomas; Ghan, Steven J.;

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

NASA Astrophysics Data System (ADS)

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

2012-12-01

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

Intra-urban spatial variability of PM2.5-bound carbonaceous components

NASA Astrophysics Data System (ADS)

Xie, Mingjie; Coons, Teresa L.; Dutton, Steven J.; Milford, Jana B.; Miller, Shelly L.; Peel, Jennifer L.; Vedal, Sverre; Hannigan, Michael P.

2012-12-01

The Denver Aerosol Sources and Health (DASH) study was designed to evaluate associations between PM2.5 species and sources and adverse human health effects. The DASH study generated a five-year (2003-2007) time series of daily speciated PM2.5 concentration measurements from a single, special-purpose monitoring site in Denver, CO. To evaluate the ability of this site to adequately represent the short term temporal variability of PM2.5 concentrations in the five county Denver metropolitan area, a one year supplemental set of PM2.5 samples was collected every sixth day at the original DASH monitoring site and concurrently at three additional sites. Two of the four sites, including the original DASH site, were located in residential areas at least 1.9 km from interstate highways. The other two sites were located within 0.3 km of interstate highways. Concentrations of elemental carbon (EC), organic carbon (OC), and 58 organic molecular markers were measured at each site. To assess spatial variability, site pairs were compared using the Pearson correlation coefficient (r) and coefficient of divergence (COD), a statistic that provides information on the degree of uniformity between monitoring sites. Bi-weekly co-located samples collected from July 2004 to September 2005 were also analyzed and used to estimate the uncertainty associated with sampling and analytical measurement for each species. In general, the two near-highway sites exhibited higher concentrations of EC, OC, polycyclic aromatic hydrocarbons (PAHs), and steranes than did the more residential sites. Lower spatial heterogeneity based on r and COD was inferred for all carbonaceous species after considering their divergence and lack of perfect correlations in co-located samples. Ratio-ratio plots combined with available gasoline- and diesel-powered motor vehicle emissions profiles for the region suggested a greater impact to high molecular weight (HMW) PAHs from diesel-powered vehicles at the near-highway sites

Special Issue for the 9th International Conference on Carbonaceous Particles in the Atmosphere

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

Strawa, A.W.; Kirchstetter, T.W.; Puxbaum, H.

2009-12-11

Carbonaceous particles are a minor constituent of the atmosphere but have a profound effect on air quality, human health, visibility and climate. The importance of carbonaceous particles has been increasingly recognized and become a mainstream topic at numerous conferences. Such was not the case in 1978, when the 1st International Conference on Carbonaceous Particles in the Atmosphere (ICCPA), or ''Carbon Conference'' as it is widely known, was introduced as a new forum to bring together scientists who were just beginning to reveal the importance and complexity of carbonaceous particles in the environment. Table 1 lists the conference dates, venues inmore » the series as well as the proceedings, and special issues resulting form the meetings. Penner and Novakov (Penner and Novakov, 1996) provide an excellent historical perspective to the early ICCPA Conferences. Thirty years later, the ninth in this conference series was held at its inception site, Berkeley, California, attended by 160 scientists from 31 countries, and featuring both new and old themes in 49 oral and 83 poster presentations. Topics covered such areas as historical trends in black carbon aerosol, ambient concentrations, analytic techniques, secondary aerosol formation, biogenic, biomass, and HULIS1 characterization, optical properties, and regional and global climate effects. The conference website, http://iccpa.lbl.gov/, holds the agenda, as well as many presentations, for the 9th ICCPA. The 10th ICCPA is tentatively scheduled for 2011 in Vienna, Austria. The papers in this issue are representative of several of the themes discussed in the conference. Ban-Weiss et al., (Ban-Weiss et al., accepted) measured the abundance of ultrafine particles in a traffic tunnel and found that heavy duty diesel trucks emit at least an order of magnitude more ultrafine particles than light duty gas-powered vehicles per unit of fuel burned. Understanding of this issue is important as ultrafine particles have been

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

Method for heating nongaseous carbonaceous material

DOEpatents

Lumpkin, Jr., Robert E.

1978-01-01

Nongaseous carbonaceous material is heated by a method comprising introducing tangentially a first stream containing a nongaseous carbonaceous material and carbon monoxide into a reaction zone; simultaneously and separately introducing a second stream containing oxygen into the reaction zone such that the oxygen enters the reaction zone away from the wall thereof and reacts with the first stream thereby producing a gaseous product and heating the nongaseous carbonaceous material; forming an outer spiralling vortex within the reaction zone to cause substantial separation of gases, including the gaseous product, from the nongaseous carbonaceous material; removing a third stream from the reaction zone containing the gaseous product which is substantially free of the nongaseous carbonaceous material before a major portion of the gaseous product can react with the nongaseous carbonaceous material; and removing a fourth stream containing the nongaseous carbonaceous material from the reaction zone.

A Global, Decadal, Quantitative Record of Absorbing Aerosols above Cloud Using OMI's Near-UV Observations

NASA Astrophysics Data System (ADS)

Torres, O.; Jethva, H. T.; Ahn, C.

2016-12-01

Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes of the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regions of the world. Contrary to the known cooling effects of these aerosols in cloud-free scenario over dark surface, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing (warming) at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud directly depends on the aerosol loading, microphysical and optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of above-cloud aerosol optical depth (ACAOD) of absorbing aerosols retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. Physically based on the strong `color ratio' effect in the near-UV caused by the spectral absorption of aerosols above cloud, the algorithm, formally named as OMACA, retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. Here, we present the algorithm architecture and results from an 11-year global record (2005-2015) including global climatology of frequency of occurrence and ACAOD. The theoretical uncertainty analysis and planned validation activities using measurements from upcoming field campaigns are also discussed.

Sensitivity of Multiangle Imaging to the Optical and Microphysical Properties of Biomass Burning Aerosols

NASA Technical Reports Server (NTRS)

Chen, Wei-Ting; Kahn, Ralph A.; Nelson, David; Yau, Kevin; Seinfeld, John H.

2008-01-01

The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

Visibility in the Netherlands during New Year's fireworks: The role of soot and salty aerosol products

NASA Astrophysics Data System (ADS)

ten Brink, Harry; Henzing, Bas; Otjes, René; Weijers, Ernie

2018-01-01

The visibility on New Year's nights in the Netherlands is low during stagnant weather. This is due to the scattering and absorption of light by the aerosol-smoke from the fireworks. We made an assessment of the responsible aerosol-species. The investigation took place during the New Year's night of 2009. Measurements were made at a regional site in the centre of the country away from specific local sources. An Integrating Nephelometer measured the light-scattering by the inherent compounds after removal of water from the aerosol by drying the air. The actual light-scattering was determined in an open-air scatterometer; it was a factor of five higher than the ;dry; value. The difference in actual and ;dry; light-scattering can only be explained by water-uptake of the salty hygroscopic components of the aerosol. This hypothesis is substantiated by measurements of the composition of the aerosol. The size-dependent concentrations of the salty ionic species were determined on-line with a MARGA-;sizer;. These components were for a large part in particles in the size range that most effectively scatter light. The ;dry; light-scattering was exerted by the inorganic salt components and the sooty carbonaceous material alike. However, the salty products from the fireworks are hygroscopic and take up water at the high relative humidities occurring that night. This explains the fivefold larger light-scattering by the wet ambient aerosol as compared to that by the dry aerosol in the integrating nephelometer. The visibility, which is the inverse of the open-air scattering, is thus indirectly governed by the salty products of the fireworks due to their uptake of water. Under stagnant weather conditions during New Year's nights in the Netherlands both the aerosol concentrations and the relative humidity are high; this implies that the ionic species govern the low visibilities in general, be it via their uptake of water.

Carbonaceous aerosols recorded in a southeastern Tibetan glacier: analysis of temporal variations and model estimates of sources and radiative forcing

DOE PAGES

Wang, Mo; Xu, B.; Cao, J.; ...

2015-02-02

High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956–2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of BC and OC with higher respective concentrations but a lower OC / BC ratio in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source–receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia hasmore » the largest contribution to the present-day (1996–2005) mean BC deposition at the ice-core drilling site during the non-monsoon season (October to May) (81%) and all year round (74%), followed by East Asia (14% to the non-monsoon mean and 21% to the annual mean). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from the late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia (as the primary contributor to annual mean BC deposition). Moreover, the increasing trend of the OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and/or biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing potential influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice-core record.« less

Carbonaceous material for production of hydrogen from low heating value fuel gases

DOEpatents

Koutsoukos, Elias P.

1989-01-01

A process for the catalytic production of hydrogen, from a wide variety of low heating value fuel gases containing carbon monoxide, comprises circulating a carbonaceous material between two reactors--a carbon deposition reactor and a steaming reactor. In the carbon deposition reactor, carbon monoxide is removed from a fuel gas and is deposited on the carbonaceous material as an active carbon. In the steaming reactor, the reactive carbon reacts with steam to give hydrogen and carbon dioxide. The carbonaceous material contains a metal component comprising from about 75% to about 95% cobalt, from about 5% to about 15% iron, and up to about 10% chromium, and is effective in suppressing the production of methane in the steaming reactor.

The Distinct Genetics of Carbonaceous and Non-Carbonaceous Meteorites Inferred from Molybdenum Isotopes

NASA Astrophysics Data System (ADS)

Budde, G.; Burkhardt, C.; Kleine, T.

2017-07-01

Mo isotope systematics manifest a fundamental dichotomy in the genetic heritage of carbonaceous and non-carbonaceous meteorites. We discuss its implications in light of the most recent literature data and new isotope data for primitive achondrites.

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

DOE PAGES

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

2018-01-31

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

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

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

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

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

“Assessment of the two-way Coupled WRF-CMAQ Model with Observations from the CARES”

EPA Science Inventory

The main goal of this assessment is to evaluate the improved aerosol component of two-way coupled WRF-CMAQ model particularly in representing aerosol physical and optical properties by utilizing observations from the Carbonaceous Aerosol and Radiative Effects Study (CARES) in May...

Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model

NASA Astrophysics Data System (ADS)

Liu, X.; Ma, P.-L.; Wang, H.; Tilmes, S.; Singh, B.; Easter, R. C.; Ghan, S. J.; Rasch, P. J.

2016-02-01

Atmospheric carbonaceous aerosols play an important role in the climate system by influencing the Earth's radiation budgets and modifying the cloud properties. Despite the importance, their representations in large-scale atmospheric models are still crude, which can influence model simulated burden, lifetime, physical, chemical and optical properties, and the climate forcing of carbonaceous aerosols. In this study, we improve the current three-mode version of the Modal Aerosol Module (MAM3) in the Community Atmosphere Model version 5 (CAM5) by introducing an additional primary carbon mode to explicitly account for the microphysical ageing of primary carbonaceous aerosols in the atmosphere. Compared to MAM3, the four-mode version of MAM (MAM4) significantly increases the column burdens of primary particulate organic matter (POM) and black carbon (BC) by up to 40 % in many remote regions, where in-cloud scavenging plays an important role in determining the aerosol concentrations. Differences in the column burdens for other types of aerosol (e.g., sulfate, secondary organic aerosols, mineral dust, sea salt) are less than 1 %. Evaluating the MAM4 simulation against in situ surface and aircraft observations, we find that MAM4 significantly improves the simulation of seasonal variation of near-surface BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons. However, it exacerbates the overestimation of modeled BC concentrations in the upper troposphere in the Pacific regions. The comparisons suggest that, to address the remaining model POM and BC biases, future improvements are required related to (1) in-cloud scavenging and vertical transport in convective clouds and (2) emissions of anthropogenic and biomass burning aerosols.

Impact of Tropospheric Aerosol Absorption on Ozone Retrieval from buv Measurements

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.

1998-01-01

The impact of tropospheric aerosols on the retrieval of column ozone amounts using spaceborne measurements of backscattered ultraviolet radiation is examined. Using radiative transfer calculations, we show that uv-absorbing desert dust may introduce errors as large as 10% in ozone column amount, depending on the aerosol layer height and optical depth. Smaller errors are produced by carbonaceous aerosols that result from biomass burning. Though the error is produced by complex interactions between ozone absorption (both stratospheric and tropospheric), aerosol scattering, and aerosol absorption, a surprisingly simple correction procedure reduces the error to about 1%, for a variety of aerosols and for a wide range of aerosol loading. Comparison of the corrected TOMS data with operational data indicates that though the zonal mean total ozone derived from TOMS are not significantly affected by these errors, localized affects in the tropics can be large enough to seriously affect the studies of tropospheric ozone that are currently undergoing using the TOMS data.

A Ten-Year Global Record of Absorbing Aerosols Above Clouds from OMI's Near-UV Observations

NASA Technical Reports Server (NTRS)

Jethva, Hiren; Torres, Omar; Ahn, Changwoo

2016-01-01

Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes associated with the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regional of the world. Contrary to the cloud-free scenario over dark surface, for which aerosols are known to produce a net cooling effect (negative radiative forcing) on climate, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud depends directly on the aerosol loading, microphysical-optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of optical depth of absorbing aerosols above clouds retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. The presence of absorbing aerosols above cloud reduces the upwelling radiation reflected by cloud and produces a strong 'color ratio' effect in the near-UV region, which can be unambiguously detected in the OMI measurements. Physically based on this effect, the OMACA algorithm retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. The algorithm architecture and results from a ten-year global record including global climatology of frequency of occurrence and above-cloud aerosol optical depth, and a discussion on related future field campaigns are presented.

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

NASA Astrophysics Data System (ADS)

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

2016-01-01

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

Aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing in Guangzhou during the 2006 Pearl River Delta campaign.

PubMed

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

2009-08-01

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

Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS

NASA Astrophysics Data System (ADS)

Hamilton, J. F.; Webb, P. J.; Lewis, A. C.; Hopkins, J. R.; Smith, S.; Davy, P.

2004-08-01

Partially oxidised organic compounds associated with PM2.5 aerosol collected in London, England, have been analysed using direct thermal desorption coupled to comprehensive gas chromatography-time of flight mass spectrometry (GCXGC-TOF/MS). Over 10000 individual organic components were isolated from around 10µg of aerosol material in a single procedure and with no sample pre-treatment. Chemical functionalities observed using this analytical technique ranged from alkanes to poly-oxygenated species. The chemical band structures commonly used in GCXGC for group type identifications overlap for this sample type, and have required mass spectrometry as an additional level of instrument dimensionality. An investigation of oxygenated volatile organic compounds (o-VOC) contained within urban aerosol has been performed and in a typical sample around 130 o-VOCs were identified based on retention behaviour and spectral match. In excess of 100 other oxygenated species were also observed but lack of mass spectral library or pure components prevents positive identification. Many of the carbonyl species observed could be mechanistically linked to gas phase aromatic hydrocarbon oxidation and there is good agreement in terms of speciation between the urban samples analysed here and those degradation products observed in smog chamber experiments of aromatic oxidation. The presence of partially oxidised species such as linear chain aldehydes and ketones and cyclic products such as furanones suggests that species generated early in the oxidative process may undergo gas to particle partitioning despite their relatively high volatility.

Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS

NASA Astrophysics Data System (ADS)

Hamilton, J.; Webb, P.; Lewis, A.; Hopkins, J.; Smith, S.; Davy, P.

2004-03-01

Partially oxidised organic compounds associated with PM2.5 aerosol collected in London, England, have been analysed using direct thermal desorption coupled to comprehensive gas chromatography-time of flight mass spectrometry (GCXGC-OF/MS). Over 10 000 individual organic components were isolated from around 10 μg of aerosol material in a single procedure and with no sample pre-treatment. Chemical functionalities observed using this analytical technique ranged from alkanes to poly-oxygenated species. The chemical band structures commonly used in GCXGC for group type identifications overlap for this sample type, and have required mass spectrometry as an additional level of instrument dimensionality. An investigation of oxygenated volatile organic compounds (o-VOC) contained within urban aerosol has been performed and in a typical sample around 130 o-VOCs were identified based on retention behaviour and spectral match. In excess of 100 other oxygenated species were also observed but lack of mass spectral library or pure components prevents positive identification. Many of the carbonyl species observed could be mechanistically linked to gas phase aromatic hydrocarbon oxidation and there is good agreement in terms of speciation between the urban samples analysed here and those degradation products observed in smog chamber experiments of aromatic oxidation. The presence of partially oxidised species such as linear chain aldehydes and ketones and cyclic products such as furanones suggests that species generated relatively early in the oxidative process may undergo gas to particle partitioning despite their relatively high volatility.

Characterizing the Asian Tropopause Aerosol Layer (ATAL) Using Satellite Observations, Balloon Measurements and a Chemical Transport Model

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.;

Characterization of biomass burning aerosols from forest fire in Indonesia

NASA Astrophysics Data System (ADS)

Fujii, Y.; Iriana, W.; Okumura, M.; Lestari, P.; Tohno, S.; Akira, M.; Okuda, T.

2012-12-01

Biomass burning (forest fire, wild fire) is a major source of pollutants, generating an estimate of 104 Tg per year of aerosol particles worldwide. These particles have adverse human health effects and can affect the radiation budget and climate directly and indirectly. Eighty percent of biomass burning aerosols are generated in the tropics and about thirty percent of them originate in the tropical regions of Asia (Andreae, 1991). Several recent studies have reported on the organic compositions of biomass burning aerosols in the tropical regions of South America and Africa, however, there is little data about forest fire aerosols in the tropical regions of Asia. It is important to characterize biomass burning aerosols in the tropical regions of Asia because the aerosol properties vary between fires depending on type and moisture of wood, combustion phase, wind conditions, and several other variables (Reid et al., 2005). We have characterized PM2.5 fractions of biomass burning aerosols emitted from forest fire in Indonesia. During the dry season in 2012, PM2.5 aerosols from several forest fires occurring in Riau, Sumatra, Indonesia were collected on quartz and teflon filters with two mini-volume samplers. Background aerosols in forest were sampled during transition period of rainy season to dry season (baseline period). Samples were analyzed with several analytical instruments. The carbonaceous content (organic and elemental carbon, OC and EC) of the aerosols was analyzed by a thermal optical reflectance technique using IMPROVE protocol. The metal, inorganic ion and organic components of the aerosols were analyzed by X-ray Fluorescence (XRF), ion chromatography and gas chromatography-mass spectrometry, respectively. There was a great difference of chemical composition between forest fire and non-forest fire samples. Smoke aerosols for forest fires events were composed of ~ 45 % OC and ~ 2.5 % EC. On the other hand, background aerosols for baseline periods were

Organic component vapor pressures and hygroscopicities of aqueous aerosol measured by optical tweezers.

PubMed

Cai, Chen; Stewart, David J; Reid, Jonathan P; Zhang, Yun-hong; Ohm, Peter; Dutcher, Cari S; Clegg, Simon L

2015-01-29

Measurements of the hygroscopic response of aerosol and the particle-to-gas partitioning of semivolatile organic compounds are crucial for providing more accurate descriptions of the compositional and size distributions of atmospheric aerosol. Concurrent measurements of particle size and composition (inferred from refractive index) are reported here using optical tweezers to isolate and probe individual aerosol droplets over extended timeframes. The measurements are shown to allow accurate retrievals of component vapor pressures and hygroscopic response through examining correlated variations in size and composition for binary droplets containing water and a single organic component. Measurements are reported for a homologous series of dicarboxylic acids, maleic acid, citric acid, glycerol, or 1,2,6-hexanetriol. An assessment of the inherent uncertainties in such measurements when measuring only particle size is provided to confirm the value of such a correlational approach. We also show that the method of molar refraction provides an accurate characterization of the compositional dependence of the refractive index of the solutions. In this method, the density of the pure liquid solute is the largest uncertainty and must be either known or inferred from subsaturated measurements with an error of <±2.5% to discriminate between different thermodynamic treatments.

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

NASA Technical Reports Server (NTRS)

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

2017-01-01

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

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

PubMed

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

2017-06-01

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

Chemical characteristics of PM2.5 aerosol in Incheon, Korea

NASA Astrophysics Data System (ADS)

Choi, Jong-Kyu; Heo, Jong-Bae; Ban, Soo-Jin; Yi, Seung-Muk; Zoh, Kyung-Duk

2012-12-01

We examined the characteristics, sources, and distribution of PM2.5 and carbonaceous species in particulate samples collected from June 2009 to May 2010 in Incheon, Korea. The average PM2.5 concentration (41.9 ± 9.0 μg m-3) exceeded the annual level set by the United States' National Ambient Air Quality Standards (15 μg m-3). The major fraction of PM2.5 consisted of ionic species (accounting for 38.9 ± 8.8%), such as NO3-, SO42-, and NH4+, as well as organic carbon (OC) (accounting for 18.9 ± 5.1%). We also analyzed the seasonal variation in PM2.5 and secondary aerosols such as NO3- and SO42- in PM2.5. While SO42- concentrations were higher in spring and summer, the concentration of PM2.5 and NO3- were the highest in winter. SO42- concentrations were higher during the spring and summer, but PM2.5 and NO3- were highest during the winter. As an important aerosol indicator, water-soluble organic carbon (WSOC) (mean 4.7 ± 0.8 μg m-3, 58.9 ± 10.7% of total OC) showed a strong relationship with NO3-, SO42-, and SOC (R2 = 0.56, 0.67, and 0.65, respectively), which was indicative of favorable conditions for SOC formation during the sampling period. Among the individual organic aerosols measured, n-alkanes, n-alkanoic acids, levoglucosan, and phthalates were major components, whereas PAHs (polycyclic aromatic hydrocarbons), oxy-PAHs, hopanes, and cholestanes were minor components. The concentration of organic compounds during smoggy periods was higher than during non-event periods. The n-alkane and n-alkanoic acid species during the smoggy periods were 10-14 times higher than during the normal period. Using principal component analysis coupled with multiple linear regression analysis, we identified the primary sources of PM2.5 to be motor vehicle/sea salt, secondary organic aerosols, combustion, biogenic/meat cooking, and soil sources.

Volatility of organic aerosol and its components in the Megacity of Paris

NASA Astrophysics Data System (ADS)

Paciga, A.; Karnezi, E.; Kostenidou, E.; Hildebrandt, L.; Psichoudaki, M.; Engelhart, G. J.; Lee, B.-H.; Crippa, M.; Prévôt, A. S. H.; Baltensperger, U.; Pandis, S. N.

2015-08-01

Using a mass transfer model and the volatility basis set, we estimate the volatility distribution for the organic aerosol (OA) components during summer and winter in Paris, France as part of the collaborative project MEGAPOLI. The concentrations of the OA components as a function of temperature were measured combining data from a thermodenuder and an aerosol mass spectrometer (AMS) with Positive Matrix Factorization (PMF) analysis. The hydrocarbon-like organic aerosol (HOA) had similar volatility distributions for the summer and winter campaigns with half of the material in the saturation concentration bin of 10 μg m-3 and another 35-40 % consisting of low and extremely low volatility organic compounds (LVOCs and ELVOCs, respectively). The winter cooking OA (COA) was more than an order of magnitude less volatile than the summer COA. The low volatility oxygenated OA (LV-OOA) factor detected in the summer had the lowest volatility of all the derived factors and consisted almost exclusively of ELVOCs. The volatility for the semi-volatile oxygenated OA (SV-OOA) was significantly higher than that of the LV-OOA, containing both semi-volatile organic components (SVOCs) and LVOCs. The oxygenated OA (OOA) factor in winter consisted of SVOCs (45 %), LVOCs (25 %) and ELVOCs (30 %). The volatility of marine OA (MOA) was higher than that of the other factors containing around 60 % SVOCs. The biomass burning OA (BBOA) factor contained components with a wide range of volatilities with significant contributions from both SVOCs (50 %) and LVOCs (30 %). Finally, combining the O : C ratio and volatility distributions of the various factors, we incorporated our results into the two-dimensional volatility basis set (2D-VBS). Our results show that the factors cover a broad spectrum of volatilities with no direct link between the average volatility and average O : C of the OA components. Agreement between our findings and previous publications is encouraging for our understanding of the

Volatility of organic aerosol and its components in the megacity of Paris

NASA Astrophysics Data System (ADS)

Paciga, Andrea; Karnezi, Eleni; Kostenidou, Evangelia; Hildebrandt, Lea; Psichoudaki, Magda; Engelhart, Gabriella J.; Lee, Byong-Hyoek; Crippa, Monica; Prévôt, André S. H.; Baltensperger, Urs; Pandis, Spyros N.

2016-02-01

Using a mass transfer model and the volatility basis set, we estimate the volatility distribution for the organic aerosol (OA) components during summer and winter in Paris, France as part of the collaborative project MEGAPOLI. The concentrations of the OA components as a function of temperature were measured combining data from a thermodenuder and an aerosol mass spectrometer (AMS) with Positive Matrix Factorization (PMF) analysis. The hydrocarbon-like organic aerosol (HOA) had similar volatility distributions for the summer and winter campaigns with half of the material in the saturation concentration bin of 10 µg m-3 and another 35-40 % consisting of low and extremely low volatility organic compounds (LVOCs with effective saturation concentrations C* of 10-3-0.1 µg m-3 and ELVOCs C* less or equal than 10-4 µg m-3, respectively). The winter cooking OA (COA) was more than an order of magnitude less volatile than the summer COA. The low-volatility oxygenated OA (LV-OOA) factor detected in the summer had the lowest volatility of all the derived factors and consisted almost exclusively of ELVOCs. The volatility for the semi-volatile oxygenated OA (SV-OOA) was significantly higher than that of the LV-OOA, containing both semi-volatile organic components (SVOCs with C* in the 1-100 µg m-3 range) and LVOCs. The oxygenated OA (OOA) factor in winter consisted of SVOCs (45 %), LVOCs (25 %) and ELVOCs (30 %). The volatility of marine OA (MOA) was higher than that of the other factors containing around 60 % SVOCs. The biomass burning OA (BBOA) factor contained components with a wide range of volatilities with significant contributions from both SVOCs (50 %) and LVOCs (30 %). Finally, combining the bulk average O : C ratios and volatility distributions of the various factors, our results are placed into the two-dimensional volatility basis set (2D-VBS) framework. The OA factors cover a broad spectrum of volatilities with no direct link between the average volatility and

Sources of PM2.5 carbonaceous aerosol in Riyadh, Saudi Arabia

NASA Astrophysics Data System (ADS)

Bian, Qijing; Alharbi, Badr; Shareef, Mohammed M.; Husain, Tahir; Pasha, Mohammad J.; Atwood, Samuel A.; Kreidenweis, Sonia M.

2018-03-01

Knowledge of the sources of carbonaceous aerosol affecting air quality in Riyadh, Saudi Arabia, is limited but needed for the development of pollution control strategies. We conducted sampling of PM2.5 from April to September 2012 at various sites in the city and used a thermo-optical semi-continuous method to quantify the organic carbon (OC) and elemental carbon (EC) concentrations. The average OC and EC concentrations were 4.7 ± 4.4 and 2.1 ± 2.5 µg m-3, respectively, during this period. Both OC and EC concentrations had strong diurnal variations, with peaks at 06:00-08:00 LT and 20:00-22:00 LT, attributed to the combined effect of increased vehicle emissions during rush hour and the shallow boundary layer in the early morning and at night. This finding suggested a significant influence of local vehicular emissions on OC and EC. The OC / EC ratio in primary emissions was estimated to be 1.01, close to documented values for diesel emissions. Estimated primary organic carbon (POC) and secondary organic carbon (SOC) concentrations were comparable, with average concentrations of 2.0 ± 2.4 and 2.8 ± 3.4 µg m-3, respectively.We also collected 24 h samples of PM10 onto quartz microfiber filters and analyzed these for an array of metals by inductively coupled plasma atomic emission spectroscopy (ICP-AES). Total OC was correlated with Ca (R2 of 0.63), suggesting that OC precursors and Ca may have similar sources, and the possibility that they underwent similar atmospheric processing. In addition to a ubiquitous dust source, Ca is emitted during desalting processes in the numerous refineries in the region and from cement kilns, suggesting these sources may also contribute to observed OC concentrations in Riyadh. Concentration weighted trajectory (CWT) analysis showed that high OC and EC concentrations were associated with air masses arriving from the Persian Gulf and the region around Baghdad, locations with high densities of oil fields and refineries as well as a

Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

NASA Astrophysics Data System (ADS)

Logan, Timothy S.

Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the

What controls the vertical distribution of aerosol? Relationships between process sensitivity in HadGEM3–UKCA and inter-model variation from AeroCom Phase II

DOE PAGES

Kipling, Zak; Stier, Philip; Johnson, Colin E.; ...

2016-02-26

The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3–UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficientlymore » coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3–UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN > 3 nm), while the profiles of larger particles (e.g. CN > 100 nm) are

Pulsed-Laser Irradiation Space Weathering Of A Carbonaceous Chondrite

NASA Technical Reports Server (NTRS)

Thompson, M. S.; Keller, L. P.; Christoffersen, R.; Loeffler, M. J.; Morris, R. V.; Graff, T. G.; Rahman, Z.

2017-01-01

Grains on the surfaces of airless bodies experience irradiation from solar energetic particles and melting, vaporization and recondensation processes associated with micrometeorite impacts. Collectively, these processes are known as space weathering and they affect the spectral properties, composition, and microstructure of material on the surfaces of airless bodies, e.g. Recent efforts have focused on space weathering of carbonaceous materials which will be critical for interpreting results from the OSIRIS-REx and Hayabusa2 missions targeting primitive, organic-rich asteroids. In addition to returned sample analyses, space weathering processes are quantified through laboratory experiments. For example, the short-duration thermal pulse from hypervelocity micrometeorite impacts have been simulated using pulsed-laser irradiation of target material e.g. Recent work however, has shown that pulsed-laser irradiation has variable effects on the spectral properties and microstructure of carbonaceous chondrite samples. Here we investigate the spectral characteristics of pulsed-laser irradiated CM2 carbonaceous chondrite, Murchison, including the vaporized component. We also report the chemical and structural characteristics of specific mineral phases within the meteorite as a result of pulsed-laser irradiation.

Nuclear magnetic biosignatures in the carbonaceous matter of ancient cherts: comparison with carbonaceous meteorites.

PubMed

Gourier, Didier; Delpoux, Olivier; Binet, Laurent; Vezin, Hervé

2013-10-01

The search for organic biosignatures is motivated by the hope of understanding the conditions of emergence of life on Earth and the perspective of finding traces of extinct life in martian sediments. Paramagnetic radicals, which exist naturally in amorphous carbonaceous matter fossilized in Precambrian cherts, were used as local structural probes and studied by electron paramagnetic resonance (EPR) spectroscopy. The nuclear magnetic resonance transitions of elements inside and around these radicals were detected by monitoring the nuclear modulations of electron spin echo in pulsed EPR. We found that the carbonaceous matter of fossilized microorganisms with age up to 3.5 billion years gives specific nuclear magnetic signatures of hydrogen (¹H), carbon (¹³C), and phosphorus (³¹P) nuclei. We observed that these potential biosignatures of extinct life are found neither in the carbonaceous matter of carbonaceous meteorites (4.56 billion years), the most ancient objects of the Solar System, nor in any carbonaceous matter resulting from carbonization of organic and bioorganic precursors. These results indicate that these nuclear signatures are sensitive to thermal episodes and can be used for Archean cherts with metamorphism not higher than the greenschist facies.

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

Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model

DOE PAGES

Liu, X.; Ma, P. -L.; Wang, H.; ...

2016-02-08

Atmospheric carbonaceous aerosols play an important role in the climate system by influencing the Earth's radiation budgets and modifying the cloud properties. Despite the importance, their representations in large-scale atmospheric models are still crude, which can influence model simulated burden, lifetime, physical, chemical and optical properties, and the climate forcing of carbonaceous aerosols. In this study, we improve the current three-mode version of the Modal Aerosol Module (MAM3) in the Community Atmosphere Model version 5 (CAM5) by introducing an additional primary carbon mode to explicitly account for the microphysical ageing of primary carbonaceous aerosols in the atmosphere. Compared to MAM3,more » the four-mode version of MAM (MAM4) significantly increases the column burdens of primary particulate organic matter (POM) and black carbon (BC) by up to 40 % in many remote regions, where in-cloud scavenging plays an important role in determining the aerosol concentrations. Differences in the column burdens for other types of aerosol (e.g., sulfate, secondary organic aerosols, mineral dust, sea salt) are less than 1 %. Evaluating the MAM4 simulation against in situ surface and aircraft observations, we find that MAM4 significantly improves the simulation of seasonal variation of near-surface BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons. However, it exacerbates the overestimation of modeled BC concentrations in the upper troposphere in the Pacific regions. As a result, the comparisons suggest that, to address the remaining model POM and BC biases, future improvements are required related to (1) in-cloud scavenging and vertical transport in convective clouds and (2) emissions of anthropogenic and biomass burning aerosols.« less

Impact of primary and secondary air supply intensity in stove on emissions of size-segregated particulate matter and carbonaceous aerosols from apple tree wood burning

NASA Astrophysics Data System (ADS)

Sun, Jian; Shen, Zhenxing; Zhang, Leiming; Zhang, Qian; Lei, Yali; Cao, Junji; Huang, Yu; Liu, Suixin; Zheng, Chunli; Xu, Hongmei; Liu, Hongxia; Pan, Hua; Liu, Pingping; Zhang, Renjian

2018-04-01

In order to assess emission factors (EF) more accurately from household biomass burning, a series of laboratory-controlled apple tree wood burning tests were conducted to measure the EFs of size-segregated particulate matter (PM) and carbonaceous aerosols. The controlled burning experiments were conducted with designed primary air (PA) and secondary air (SA) supply intensity. An optimum value of 7 m3·h- 1 was found for SA, resulting the highest modified combustion efficiency (92.4 ± 2.5%) as well as the lowest EFs of PM2.5 (0.13 ± 0.01 g·MJ- 1), OC (0.04 ± 0.03 g·MJ- 1) and EC (0.03 ± 0.01 g·MJ- 1). SA values of 7 and 10 m3·h- 1 resulted the lowest EFs for all the different PM sizes. In a test with PA of 6 m3·h- 1 and SA of 7 m3·h- 1, very low EFs were observed for OC1 (8.2%), OC2 (11.2%) and especially OP (Pyrolyzed OC) (0%, not detected), indicating nearly complete combustion under this air supply condition. Besides SA, higher PA was proved to have positive effects on PM and carbonaceous fraction emission reduction. For example, with a fixed SA of 1.5 m3·h- 1, EFs of PM2.5 decreased from 0.64 to 0.27 g·MJ- 1 when PA increased from 6 to 15 m3·h- 1 (P < 0.05). Similar reductions were also observed in EFs of OC, EC and size segregated PM.

The colors of biomass burning aerosols in the atmosphere.

PubMed

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

2016-06-16

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

Carbonaceous structures in the Tissint Martian Meteorite: evidence of a biogenetic origin

NASA Astrophysics Data System (ADS)

Wallis, Jamie; Wickramasinghe, N. C.; Wallis, Daryl H.; Miyake, Nori; Wallis, M. K.; Hoover, Richard B.

2015-09-01

We report for the first time in situ observations of 5-50μm spherical carbonaceous structures in the Tissint Martian meteorite comprising of pyrite (FeS2) cores and carbonaceous outer coatings. The structures are characterized as smooth immiscible spheres with curved boundaries occasionally following the contours of the pyrite inclusion. The structures bear striking resemblance to similar-sized immiscible carbonaceous spheres found in hydrothermal calcite vein deposits in the Mullaghwornia Quarry in central Ireland. Similar structures have been reported in Proterozoic and Ordovician sandstones from Canada as well as in a variety of astronomical sources including carbonaceous chondrites, chondritic IDPs and primitive chondritic meteorites. SEM and X-Ray elemental mapping confirmed the presence of organic carbon filling the crack and cleavage space in the pyroxene substrate, with further evidence of pyrite acting as an attractive substrate for the collection of organic matter. The detection of precipitated carbon collecting around pyrite grains is at variance with an igneous origin as proposed for the reduced organic component in Tissint, and is more consistent with a biogenetic origin.

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

PubMed Central

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

2018-01-01

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

Vertical Distribution of Black and Brown Carbon over Shanghai during Winter

NASA Astrophysics Data System (ADS)

Zheng, M.; Yan, C.; Wang, D.; Fu, Q.

2016-12-01

Carbonaceous aerosols (i.e., black carbon, BC, and organic aerosol, OA) have significant impact on Earth's energy budget by scattering and absorbing solar radiation. Extensive carbonaceous aerosols have been emitted in mainland China. It is essential to study the column burden of carbonaceous aerosol and associated light absorption to better understand its radiative forcing. In this study, a tethered balloon-based field campaign was conducted over a Chinese megacity, Shanghai, in December of 2015, with the primary goal to investigate the vertical profile of air pollutants within the lower troposphere, especially during the polluted days. A 7-wavelength Aethalometer (AE-31) were adopted in the observation to obtain vertical profiles of atmospheric carbonaceous aerosols within the lower troposphere. Light absorption by black and brown carbon, the light absorbing organic components, were distinguished and separated based on difference between light absorption at 450 nm versus 880 nm. Light absorption of brown carbon relative to black carbon were also estimated to pose the importance of brown carbon. Besides, diurnal variation of black and brown carbon vertical profiles would also be discussed, with consideration of variation of height of planetary boundary layer.

Carbonaceous species in PM2.5 at a pair of rural/urban sites in Beijing, 2005-2008

NASA Astrophysics Data System (ADS)

Yang, F.; Huang, L.; Duan, F.; Zhang, W.; He, K.; Ma, Y.; Brook, J. R.; Tan, J.; Zhao, Q.; Cheng, Y.

2011-08-01

One-week integrated PM2.5 samples were collected over four years (2005-2008) at a pair of sites, one rural and one urban site, in the area of Beijing, China. Weekly organic and elemental carbon (OC and EC) concentrations from these samples were measured to investigate their atmospheric concentrations, temporal variation patterns and the factors influencing these aspects. A slightly systematic decrease in annual mean concentration of OC and an opposite trend for EC at both sites was observed. Since OC accounted for about 70 % of total carbon (TC, i.e. OC + EC) the total carbonaceous mass experienced a slight decline on a yearly basis over the study period. Its fraction of PM2.5 mass at the urban site in 2008 was significantly lower than observed 10 years earlier (1999), indicating that the relative importance of carbonaceous species in PM2.5 has decreased. In urban Beijing clear seasonal variations (by factors of 1.35 ~ 3.0) were shown in both OC and EC with higher weekly concentrations and fluctuations in winter and much lower values in summer and spring. The minimum seasonal urban excesses of OC (3.0 μg m-3) and EC (1.3 μg m-3) occurred in the summer of 2008, which were only one-ninth and one-seventh of their corresponding maximum values, respectively. This reduction in the urban-difference, coupled with more positive stable carbon isotope values of EC at the urban site in that summer relative to the preceding summers, supports that the special clean air campaign for the 2008 Summer Olympic Games very likely had noticeable impact on the ambient concentrations of carbonaceous aerosols in the Beijing area, particularly on the local urban scale. Less consistent seasonal patterns in OC and EC, their scattered correlation, and higher mass ratios of OC to EC (OC/EC) at the rural site indicate more complex and variable major sources regarding aerosol formation in the rural area. These emission sources include biomass burning during the harvest seasons, widely used high

Simulation of Infrared Spectra of Carbonaceous Grains

NASA Astrophysics Data System (ADS)

Dadswell, G.; Duley, W. W.

1997-02-01

Random covalent network (RCN) theory is applied to describe the infrared spectroscopic properties of carbonaceous solids with compositions containing a mixture of aromatic, aliphatic, and diamond-like hydrocarbons. Application of this technique to carbonaceous dust is equivalent to the synthesis of solids whose structure and bonding satisfy stoicheometry while minimizing strain energy. The result involves a range of compositions compatible with carbon bonding and the hydrogen concentration incorporated in the network. In general, only a limited range of compositions is available rather than the infinite number of possible compositions expected without the inclusion of these constraints. When compositions have been defined in this way, infrared spectra may be synthesized for comparison with astronomical spectra of interstellar carbonaceous solids. Such spectra contain components corresponding to absorption by CHn groups in which n = 1-3. We find, however, that additional spectral features, not included in our simple chemical model, must be present also in dust. We give plots of such spectra in the 3100-2800 cm-1 (3.2-3.6 μm) region for comparison with infrared spectra of interstellar dust. We have also developed an RCN formalism that incorporates oxygen into the carbon network as OH groups, and we show that this inclusion introduces a strong additional absorption band in the 3300 cm-1 (3.0 μm) region.

Atmospheric Condensational Properties of Ultrafine Chain and Fractal Aerosol Particles

NASA Technical Reports Server (NTRS)

Marlow, William H.

1997-01-01

The purpose for the research sponsored by this grant was to lay the foundations for qualitative understanding and quantitative description of the equilibrium vapor pressure of water vapor over the irregularly shaped, carbonaceous particles that are present in the atmosphere. This work apparently was the first systematic treatment of the subject. Research was conducted in two complementary components: 1. Calculations were performed of the equilibrium vapor pressure of water over particles comprised of aggregates of spheres in the 50-200 nm radius range. The purposes of this work were two-fold. First, since no systematic treatment of this subject had previously been conducted, its availability would be directly useful for quantitative treatment for a limited range of atmospheric aerosols. Second, it would provide qualitative indications of the effects of highly irregular particle shape on equilibrium vapor pressure of aggregates comprised of smaller spheres.

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.

Light Absorption and Excitation-Emission Fluorescence of Urban Organic Aerosol Components and Their Relationship to Chemical Structure.

PubMed

Chen, Qingcai; Ikemori, Fumikazu; Mochida, Michihiro

2016-10-18

The present study used a combination of solvent and solid-phase extractions to fractionate organic compounds with different polarities from total suspended particulates in Nagoya, Japan, and their optical characteristics were obtained on the basis of their UV-visible absorption spectra and excitation-emission matrices (EEMs). The relationship between their optical characteristics and chemical structures was investigated based on high-resolution aerosol mass spectra (HR-AMS spectra), soft ionization mass spectra and Fourier transform infrared (FT-IR) spectra. The major light-absorption organics were less polar organic fractions, which tended to have higher mass absorption efficiencies (MAEs) and lower wavelength dependent Ångström exponents (Å) than the more polar organic fractions. Correlation analyses indicate that organic compounds with O and N atoms may contribute largely to the total light absorption and fluorescence of the organic aerosol components. The extracts from the aerosol samples were further characterized by a classification of the EEM profiles using a PARAFAC model. Different fluorescence components in the aerosol organic EEMs were associated with specific AMS ions and with different functional groups from the FT-IR analysis. These results may be useful to determine and further classify the chromophores in atmospheric organic aerosols using EEM spectroscopy.

NOAA's National Air Quality Prediction and Development of Aerosol and Atmospheric Composition Prediction Components for NGGPS

NASA Astrophysics Data System (ADS)

Stajner, I.; McQueen, J.; Lee, P.; Stein, A. F.; Wilczak, J. M.; Upadhayay, S.; daSilva, A.; Lu, C. H.; Grell, G. A.; Pierce, R. B.

2017-12-01

NOAA's operational air quality predictions of ozone, fine particulate matter (PM2.5) and wildfire smoke over the United States and airborne dust over the contiguous 48 states are distributed at http://airquality.weather.gov. The National Air Quality Forecast Capability (NAQFC) providing these predictions was updated in June 2017. Ozone and PM2.5 predictions are now produced using the system linking the Community Multiscale Air Quality model (CMAQ) version 5.0.2 with meteorological inputs from the North American Mesoscale Forecast System (NAM) version 4. Predictions of PM2.5 include intermittent dust emissions and wildfire emissions from an updated version of BlueSky system. For the latter, the CMAQ system is initialized by rerunning it over the previous 24 hours to include wildfire emissions at the time when they were observed from the satellites. Post processing to reduce the bias in PM2.5 prediction was updated using the Kalman filter analog (KFAN) technique. Dust related aerosol species at the CMAQ domain lateral boundaries now come from the NEMS Global Aerosol Component (NGAC) v2 predictions. Further development of NAQFC includes testing of CMAQ predictions to 72 hours, Canadian fire emissions data from Environment and Climate Change Canada (ECCC) and the KFAN technique to reduce bias in ozone predictions. NOAA is developing the Next Generation Global Predictions System (NGGPS) with an aerosol and gaseous atmospheric composition component to improve and integrate aerosol and ozone predictions and evaluate their impacts on physics, data assimilation and weather prediction. Efforts are underway to improve cloud microphysics, investigate aerosol effects and include representations of atmospheric composition of varying complexity into NGGPS: from the operational ozone parameterization, GOCART aerosols, with simplified ozone chemistry, to CMAQ chemistry with aerosol modules. We will present progress on community building, planning and development of NGGPS.

A 3-D Model Study of Aerosol Composition and Radiative Forcing in the Asian-Pacific Region

NASA Technical Reports Server (NTRS)

Chin, Mian; Ginoux, Paul; Torres, Omar; Zhao, Xuepeng; Einaudi, Franco (Technical Monitor)

2000-01-01

The Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model will be used in analyzing the aerosol data in the ACE-Asia program. Our objectives are (1) to understand the physical, chemical, and optical properties of aerosol and the processes that control these properties over the Asian-Pacific region, (2) to determine the aerosol radiative forcing over the Asian-Pacific region, and (3) to investigate the interaction between aerosol and tropospheric chemistry. We will present the GOCART aerosol simulations of sulfate, dust, carbonaceous, and sea salt concentrations, their optical thicknesses, and their radiative effects. We will also show the comparisons of model results with data taken from previous field campaigns, ground-based sun photometer measurements, and satellite observations. Finally, we will present our plan for the ACE-Asia study.

Testing of an automated online EA-IRMS method for fast and simultaneous carbon content and stable isotope measurement of aerosol samples

NASA Astrophysics Data System (ADS)

Major, István; Gyökös, Brigitta; Túri, Marianna; Futó, István; Filep, Ágnes; Hoffer, András; Molnár, Mihály

2016-04-01

Comprehensive atmospheric studies have demonstrated that carbonaceous aerosol is one of the main components of atmospheric particulate matter over Europe. Various methods, considering optical or thermal properties, have been developed for quantification of the accurate amount of both organic and elemental carbon constituents of atmospheric aerosol. The aim of our work was to develop an alternative fast and easy method for determination of the total carbon content of individual aerosol samples collected on prebaked quartz filters whereby the mass and surface concentration becomes simply computable. We applied the conventional "elemental analyzer (EA) coupled online with an isotope ratio mass spectrometer (IRMS)" technique which is ubiquitously used in mass spectrometry. Using this technique we are able to measure simultaneously the carbon stable isotope ratio of the samples, as well. During the developing process, we compared the EA-IRMS technique with an off-line catalytic combustion method worked out previously at Hertelendi Laboratory of Environmental Studies (HEKAL). We tested the combined online total carbon content and stable isotope ratio measurement both on standard materials and real aerosol samples. Regarding the test results the novel method assures, on the one hand, at least 95% of carbon recovery yield in a broad total carbon mass range (between 100 and 3000 ug) and, on the other hand, a good reproducibility of stable isotope measurements with an uncertainty of ± 0.2 per mill. Comparing the total carbon results obtained by the EA-IRMS and the off-line catalytic combustion method we found a very good correlation (R2=0.94) that proves the applicability of both preparation method. Advantages of the novel method are the fast and simplified sample preparation steps and the fully automated, simultaneous carbon stable isotope ratio measurement processes. Furthermore stable isotope ratio results can effectively be applied in the source apportionment

CARBON CONTAINING COMPONENT OF THE LOS ANGELES AEROSOL: SOURCE APPORTIONMENT AND CONTRIBUTIONS TO THE VISIBILITY BUDGET

EPA Science Inventory

Source resolution of the organic component of the fine fraction of the ambient aerosol (d(sub p) < 3.5 micrometers) has been carried out by combining source information from the organic component with thermal analysis and local emission inventories. The primary and secondary carb...

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.

Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution

NASA Technical Reports Server (NTRS)

Gao, Song; Hegg, Dean A.; Hobbs, Peter V.; Kirchstetter, Thomas W.; Magi, Brian I.; Sadilek, Martin

2003-01-01

During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.

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

Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

EPA Science Inventory

ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

Temporal variability in aerosol composition at an urban site, Varanasi in the eastern Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Ram, Kirpa; Norra, Stefan; Yuan, Chen; Venkata Satish, Rangu; Rastogi, Neeraj

2017-04-01

PM2.5 aerosol samples (n=31) were collected from an urban site, Varanasi (25° 28'N, 83°0' E) in the eastern Indo-Gangetic Plain during May 2015 to March 2016 using a mini-volume sampler (Leckel GmbH, Germany) at a flow rate of 200 l/hr. The PM2.5 samples were integrated for 7 days and were analyzed for organic and elemental carbon (OC & EC), water-soluble OC (WSOC), organic and inorganic nitrogen (ON & IN) and water-soluble inorganic species (WSIS) to study the geochemical behavior of aerosols. The mass concentration of OC and EC varies from 4.2 to 105.2 (average: 32.8) μg m-3 and 1.2 to 7.0 (average: 4.6) μg m-3 during the study period with total carbonaceous aerosols (TCA=1.6*OC+EC), on an average, accounting for ˜59% of PM2.5 mass. Relatively high WSOC/OC ratio (average: 0.55±0.18; range 0.18-0.86) indicate a significant contribution from the secondary organic aerosols at Varanasi. The concentration of ON varies from less than detection limit to 5.3 (average: 2.4) μg m-3 which contribute to ˜12% of WSOC highlighting the presence of nitro-organic compounds in aerosols at Varanasi. The average WSIS contribution to PM2.5 is only 17% with a strong seasonal variability (range: 4-36%). Generally, carbonaceous and inorganic aerosol concentration is higher during winter, fall and post-monsoon that those in the summer when dust aerosol contribution is significant (as high as 75% of PM2.5 mass). This study highlights the role of nitro-organic compounds in secondary organic aerosols which is lacking in Indian aerosols. Furthermore, these aerosol samples could be very important for the study of particle morphology and composition using scanning-electron Microscope-Energy Dispersive X-ray due to lower impaction in the mini-volume sampler.

Atmospheric pressure MALDI for the noninvasive characterization of carbonaceous ink from Renaissance documents.

PubMed

Grasso, Giuseppe; Calcagno, Marzia; Rapisarda, Alessandro; D'Agata, Roberta; Spoto, Giuseppe

2017-06-01

The analytical methods that are usually applied to determine the compositions of inks from ancient manuscripts usually focus on inorganic components, as in the case of iron gall ink. In this work, we describe the use of atmospheric pressure/matrix-assisted laser desorption ionization-mass spectrometry (AP/MALDI-MS) as a spatially resolved analytical technique for the study of the organic carbonaceous components of inks used in handwritten parts of ancient books for the first time. Large polycyclic aromatic hydrocarbons (L-PAH) were identified in situ in the ink of XVII century handwritten documents. We prove that it is possible to apply MALDI-MS as a suitable microdestructive diagnostic tool for analyzing samples in air at atmospheric pressure, thus simplifying investigations of the organic components of artistic and archaeological objects. The interpretation of the experimental MS results was supported by independent Raman spectroscopic investigations. Graphical abstract Atmospheric pressure/MALDI mass spectrometry detects in situ polycyclic aromatic hydrocarbons in the carbonaceous ink of XVII century manuscripts.

Physicochemical characterization of smoke aerosol during large-scale wildfires: Extreme event of August 2010 in Moscow

NASA Astrophysics Data System (ADS)

Popovicheva, O.; Kistler, M.; Kireeva, E.; Persiantseva, N.; Timofeev, M.; Kopeikin, V.; Kasper-Giebl, A.

2014-10-01

Enhancement of biomass burning-related research is essential for the assessment of large-scale wildfires impact on pollution at regional and global scale. Starting since 6 August 2010 Moscow was covered with thick smoke of unusually high PM10 and BC concentrations, considerably affected by huge forest and peat fires around megacity. This work presents the first comprehensive physico-chemical characterization of aerosols during extreme smoke event in Moscow in August 2010. Sampling was performed in the Moscow center and suburb as well as one year later, in August 2011 during a period when no biomass burning was observed. Small-scale experimental fires of regional biomass were conducted in the Moscow region. Carbon content, functionalities of organic/inorganic compounds, tracers of biomass burning (anhydrosaccharides), ionic composition, and structure of smoke were analyzed by thermal-optical analysis, FTIR spectroscopy, liquid and ion chromatography, and electron microscopy. Carbonaceous aerosol in August 2010 was dominated by organic species with elemental carbon (EC) as minor component. High average OC/EC near 27.4 is found, comparable to smoke of regional biomass smoldering fire, and exceeded 3 times the value observed in August 2011. Organic functionalities of Moscow smoke aerosols were hydroxyl, aliphatic, aromatic, acid and non-acid carbonyl, and nitro compound groups, almost all of them indicate wildfires around city as the source of smoke. The ratio of levoglucosan (LG) to mannosan near 5 confirms the origin of smoke from coniferous forest fires around megacity. Low ratio of LG/OC near 0.8% indicates the degradation of major molecular tracer of biomass burning in urban environment. Total concentration of inorganic ions dominated by sulfates SO4 2 - and ammonium NH4+ was found about 5 times higher during large-scale wildfires than in August 2011. Together with strong sulfate and ammonium absorbance in smoke aerosols, these observations prove the formation of

Characterization of aerosol particles at the forested site in Lithuania

NASA Astrophysics Data System (ADS)

Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

2009-04-01

Atmospheric particulate matter (PM), especially fine particles (particles with aerodynamic diameter less than 1 m, PM1), has been found to play an important role in global climate change, air quality, and human health. The continuous study of aerosol parameters is therefore imperative for better understanding the environmental effects of the atmospheric particles, as well as their sources, formation and transformation processes. The particle size distribution is particularly important, since this physical parameter determines the mass and number density, lifetime and atmospheric transport, or optical scattering behavior of the particles in the atmosphere (Jaenicke, 1998). Over the years several efforts have been made to improve the knowledge about the chemical composition of atmospheric particles as a function of size (Samara and Voutsa, 2005) and to characterize the relative contribution of different components to the fine particulate matter. It is well established that organic materials constitute a highly variable fraction of the atmospheric aerosol. This fraction is predominantly found in the fine size mode in concentrations ranging from 10 to 70% of the total dry fine particle mass (Middlebrook et al., 1998). Although organic compounds are major components of the fine particles, the composition, formation mechanism of organic aerosols are not well understood. This is because particulate organic matter is part of a complex atmospheric system with hundreds of different compounds, both natural and anthropogenic, covering a wide range of chemical properties. The aim of this study was to characterize the forest PM1, and investigate effects of air mass transport on the aerosol size distribution and chemical composition, estimate and provide insights into the sources and characteristics of carbonaceous aerosols through analysis ^13C/12C isotopic ratio as a function of the aerosol particles size. The measurements were performed at the Rugšteliškis integrated

Variability of Marine Aerosol Fine-Mode Fraction and Estimates of Anthropogenic Aerosol Component Over Cloud-Free Oceans from the Moderate Resolution Imaging Spectroradiometer (MODIS)

NASA Technical Reports Server (NTRS)

Yu, Hongbin; Chin, Mian; Remer, Lorraine A.; Kleidman, Richard G.; Bellouin, Nicolas; Bian, Huisheng; Diehl, Thomas

2009-01-01

In this study, we examine seasonal and geographical variability of marine aerosol fine-mode fraction (f(sub m)) and its impacts on deriving the anthropogenic component of aerosol optical depth (tau(sub a)) and direct radiative forcing from multispectral satellite measurements. A proxy of f(sub m), empirically derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 5 data, shows large seasonal and geographical variations that are consistent with the Goddard Chemistry Aerosol Radiation Transport (GOCART) and Global Modeling Initiative (GMI) model simulations. The so-derived seasonally and spatially varying f(sub m) is then implemented into a method of estimating tau(sub a) and direct radiative forcing from the MODIS measurements. It is found that the use of a constant value for fm as in previous studies would have overestimated Ta by about 20% over global ocean, with the overestimation up to 45% in some regions and seasons. The 7-year (2001-2007) global ocean average tau(sub a) is 0.035, with yearly average ranging from 0.031 to 0.039. Future improvement in measurements is needed to better separate anthropogenic aerosol from natural ones and to narrow down the wide range of aerosol direct radiative forcing.

Electron microscopy of carbonaceous matter in Allende acid residues

NASA Technical Reports Server (NTRS)

Lumpkin, G. R.

1982-01-01

On the basis of characteristic diffuse ring diffraction patterns, much of the carbonaceous matter in a large suite of Allende acid residues has been identified as a variety of turbostratic carbon. Crystallites of this phase contain randomly stacked sp(2) hybridized carbon layers and diffraction patterns resemble those from carbon black and glassy carbon. Carbynes are probably absent, and are certainly restricted to less than 0.5% of these acid residues. The work of Ott et al. (1981) provides a basis for the possibility that turbostratic carbon is a carrier of noble gases, but an additional component - amorphous carbon - may be necessary to explain the high release temperatures of noble gases as well as the glassy character of many of the carbonaceous particles. Carbynes are considered to be questionable as important carriers of noble gases in the Allende acid residues.

Microbial structure and chemical components of aerosols caused by rotating brushes in a wastewater treatment plant.

PubMed

Han, Yunping; Li, Lin; Liu, Junxin; Zhang, Mengzhu

2012-11-01

Bacterial community structure and the chemical components in aerosols caused by rotating brushes in an Orbal oxidation ditch were assessed in a Beijing municipal wastewater treatment plant. Air samples were collected at different distances from the aerosol-generating rotating brushes. Molecular culture-independent methods were used to characterize the community structure of the airborne bacteria in each sample regardless of cell culturability. A clone library of 16S rDNA directly amplified from air DNA of each sample was constructed and sequenced to analyze the community composition and diversity. Insoluble particles and water-soluble ions emitted with microorganisms in aerosols were analysis by a scanning electron microscope together with energy dispersive X-ray spectroscopy and ion chromatogram analyzer. In total, most of the identified bacteria were Proteobacteria. The majority of sequences near the rotating brushes (the main source of the bioaerosols) were Proteobacteria (62.97 %) with β-(18.52 %) and γ-(44.45 %) subgroups and Bacteroidetes (29.63 %). Complex patterns were observed for each sampling location, suggesting a highly diverse community structure, comparable to that found in water in the Orbal oxidation ditch. Accompany with microorganisms, 46.36 μg/m(3) of SO (4) (2-) , 29.35 μg/m(3) of Cl(-), 21.51 μg/m(3) of NO (3) (-) , 19.76 μg/m(3) of NH (4) (+) , 11.42 μg/m(3) of PO (4) (3-) , 6.18 μg/m(3) of NO (2) (-) , and elements of Mg, Cl, K, Na, Fe, S, and P were detected from the air near the aerosols source. Differences in the structure of the bacterial communities and chemical components in the aerosols observed between sampling sites indicated important site-related variability. The composition of microorganisms in water was one of the most important sources of bacterial communities in bioaerosols. Chemical components in bioaerosols may provide a media for airborne microorganism attachment, as well as a suitable microenvironment for

Formation of high-molecular-weight compounds via the heterogeneous reactions of gaseous C8-C10 n-aldehydes in the presence of atmospheric aerosol components

NASA Astrophysics Data System (ADS)

Han, Yuemei; Kawamura, Kimitaka; Chen, Qingcai; Mochida, Michihiro

2016-02-01

A laboratory study on the heterogeneous reactions of straight-chain aldehydes was performed by exposing n-octanal, nonanal, and decanal vapors to ambient aerosol particles. The aerosol and blank filters were extracted using methanol. The extracts were nebulized and the resulting compositions were examined using a high-resolution time-of-flight aerosol mass spectrometer. The mass spectral analysis showed that the exposures of the aldehydes to aerosol samples increased the peak intensities in the high mass range. The peaks in the mass spectra of the aerosol samples after exposure to different aldehydes were characterized by a homologous series of peak shifts due to the addition of multiple CH2 units. This result is explained by the formation of high-molecular-weight (HMW) compounds that contain single or multiple aldehyde moieties. The HMW fragment peaks for the blank filters exposed to n-aldehydes were relatively weak, indicating an important contribution from the ambient aerosol components to the formation of the HMW compounds. Among the factors affecting the overall interaction of aldehydes with atmospheric aerosol components, gas phase diffusion possibly limited the reactions under the studied conditions; therefore, their occurrence to a similar degree in the atmosphere is not ruled out, at least for the reactions involving n-nonanal and decanal. The major formation pathways for the observed HMW products may be the self-reactions of n-aldehydes mediated by atmospheric aerosol components and the reactions of n-aldehydes with organic aerosol components. The observed formation of HMW compounds encourages further investigations into their effects on the aerosol properties as well as the organic aerosol mass in the atmosphere.

Evaluation of traffic exhaust contributions to ambient carbonaceous submicron particulate matter in an urban roadside environment in Hong Kong

NASA Astrophysics Data System (ADS)

Lee, Berto Paul; Kwok Keung Louie, Peter; Luk, Connie; Keung Chan, Chak

2017-12-01

Road traffic has significant impacts on air quality particularly in densely urbanized and populated areas where vehicle emissions are a major local source of ambient particulate matter. Engine type (i.e., fuel use) significantly impacts the chemical characteristics of tailpipe emission, and thus the distribution of engine types in traffic impacts measured ambient concentrations. This study provides an estimation of the contribution of vehicles powered by different fuels (gasoline, diesel, LPG) to carbonaceous submicron aerosol mass (PM1) based on ambient aerosol mass spectrometer (AMS) and elemental carbon (EC) measurements and vehicle count data in an urban inner city environment in Hong Kong with the aim to gauge the importance of different engine types to particulate matter burdens in a typical urban street canyon. On an average per-vehicle basis, gasoline vehicles emitted 75 and 93 % more organics than diesel and LPG vehicles, respectively, while EC emissions from diesel vehicles were 45 % higher than those from gasoline vehicles. LPG vehicles showed no appreciable contributions to EC and thus overall represented a small contributor to traffic-related primary ambient PM1 despite their high abundance (˜ 30 %) in the traffic mix. Total carbonaceous particle mass contributions to ambient PM1 from diesel engines were only marginally higher (˜ 4 %) than those from gasoline engines, which is likely an effect of recently introduced control strategies targeted at commercial vehicles and buses. Overall, gasoline vehicles contributed 1.2 µg m-3 of EC and 1.1 µ m-3 of organics, LPG vehicles 0.6 µg m-3 of organics and diesel vehicles 2.0 µg m-3 of EC and 0.7 µg m-3 of organics to ambient carbonaceous PM1.

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.

Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

DOE PAGES

Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

2017-02-04

Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

Seasonal variations of stable carbon isotopic composition of bulk aerosol carbon from Gosan site, Jeju Island in the East China Sea

NASA Astrophysics Data System (ADS)

Kundu, Shuvashish; Kawamura, Kimitaka

2014-09-01

This study explores the usefulness of stable isotopic composition (δ13C) along with other chemical tracers and air mass trajectory to identify the primary and secondary sources of carbonaceous aerosols. Aerosol samples (n = 84) were collected continuously from April 2003 to April 2004 at Gosan site in Jeju Island, South Korea. The concentrations of total carbon (TC), HCl fumed carbonate-free total carbon (fumed-TC) and their δ13C were measured online using elemental analyzer interfaced to isotope ratio mass spectrometer (EA-IRMS). Similar concentrations of TC and fumed-TC and their similar δ13C values suggest the insignificant contribution of inorganic carbon to Gosan aerosols. The monthly averaged δ13CTC showed the lowest in April/May (-24.2 to -24.4‰), which is related with the highest concentrations of oxalic acid (a secondary tracer). The result indicates an enhanced contribution of TC from secondary sources. The monthly averaged δ13CTC in July/August (-23.0 to -22.5‰) were similar to those in January/February (-23.1‰ to -22.7‰). However, chemical tracers and air mass transport pattern suggest that the pollution source regions in January/February are completely different from those in July/August. Higher δ13C values in July/August are aligned with higher concentration ratios of marine tracers (azelaic acid/TC and methanesulfonate/TC), suggesting an enhanced contribution of marine organic matter to the aerosol loading. Higher δ13C values in January/February are associated with higher concentrations of phthalic acid and K+/TC, indicating more contributions of carbonaceous aerosols from fossil fuel and C4-plant biomass combustion. This study demonstrates that δ13CTC, along with other chemical tracers and air mass trajectory, can be used as a tracer to understand the importance of primary versus secondary pollution sources of carbonaceous aerosols in the atmosphere.

Raman Spectrum of Quenched Carbonaceous Composites

NASA Technical Reports Server (NTRS)

Wada, S.; Hayashi, S.; Miyaoka, H.; Tokunaga, A. T.

1996-01-01

Quenched Carbonaceous Composites (QCC's) are products from the ejecta of a hydrocarbon plasma. Two types of QCC, dark QCC and thermally-altered (heated) filmy QCC, have been shown to have a 220 nm absorption feature similar to that seen in the interstellar extinction curve. We present here Raman spectra of the QCCs and compare them with various carbonaceous materials to better understand the structure QCC. We find that structure of QCC is different from that of graphite and more similar to carbonaceous material found in some interplanetary dust particles and chondritic meteorites.

The Oxygen Isotope Composition of Dark Inclusions in HEDs, Ordinary and Carbonaceous Chondrites

NASA Technical Reports Server (NTRS)

Greenwood, R. C.; Zolensky, M. E.; Buchanan, P. C.; Franchi, I. A.

2015-01-01

Dark inclusions (DIs) are lithic fragments that form a volumetrically small, but important, component in carbonaceous chondrites. Carbonaceous clasts similar to DIs are also found in some ordinary chondrites and HEDs. DIs are of particular interest because they provide a record of nebular and planetary processes distinct from that of their host meteorite. DIs may be representative of the material that delivered water and other volatiles to early Earth as a late veneer. Here we focus on the oxygen isotopic composition of DIs in a variety of settings with the aim of understanding their formational history and relationship to the enclosing host meteorite.

Indian aerosols: present status.

PubMed

Mitra, A P; Sharma, C

2002-12-01

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

Engineering Bacteria to Catabolize the Carbonaceous Component of Sarin: Teaching E. coli to Eat Isopropanol

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

Brown, Margaret E.; Mukhopadhyay, Aindrila; Keasling, Jay D.

In this paper, we report an engineered strain of Escherichia coli that catabolizes the carbonaceous component of the extremely toxic chemical warfare agent sarin. Enzymatic decomposition of sarin generates isopropanol waste that, with this engineered strain, is then transformed into acetyl-CoA by enzymatic conversion with a key reaction performed by the acetone carboxylase complex (ACX). We engineered the heterologous expression of the ACX complex from Xanthobacter autotrophicus PY2 to match the naturally occurring subunit stoichiometry and purified the recombinant complex from E. coli for biochemical analysis. Incorporating this ACX complex and enzymes from diverse organisms, we introduced an isopropanol degradationmore » pathway in E. coli, optimized induction conditions, and decoupled enzyme expression to probe pathway bottlenecks. Our engineered E. coli consumed 65% of isopropanol compared to no-cell controls and was able to grow on isopropanol as a sole carbon source. Finally, in the process, reconstitution of this large ACX complex (370 kDa) in a system naïve to its structural and mechanistic requirements allowed us to study this otherwise cryptic enzyme in more detail than would have been possible in the less genetically tractable native Xanthobacter system.« less

Dependence of columnar aerosol size distribution, optical properties, and chemical components on regional transport in Beijing

NASA Astrophysics Data System (ADS)

Wang, Shuo; Zhao, Weixiong; Xu, Xuezhe; Fang, Bo; Zhang, Qilei; Qian, Xiaodong; Zhang, Weijun; Chen, Weidong; Pu, Wei; Wang, Xin

2017-11-01

Seasonal dependence of the columnar aerosol optical and chemical properties on regional transport in Beijing over 10 years (from January 2005 to December 2014) were analyzed by using the ground-based remote sensing combined with backward trajectory analysis. Daily air mass backward trajectories terminated in Beijing were computed with HYSPLIT-4 model and were categorized into five clusters. The columnar mass concentrations of black carbon (BC), brown carbon (BrC), dust (DU), aerosol water content (AW), and ammonium sulfate like aerosol (AS) of each cluster were retrieved from the optical data obtained from the Aerosol Robotic NETwork (AERONET) with five-component model. It was found that the columnar aerosol properties in different seasons were changed, and they were related to the air mass origins. In spring, aerosol was dominated by coarse particles. Summer was characterized by higher single scattering albedo (SSA), lower real part of complex refractive index (n), and obvious hygroscopic growth due to humid air from the south. During autumn and winter, there was an observable increase in absorption aerosol optical thickness (AAOT) and the imaginary part of complex refraction (k), with high levels of retrieved BC and BrC. However, concentrations of BC showed less dependence on the clusters during the two seasons owing to the widely spread coal heating in north China.

Chiral Biomarkers and Microfossils in Carbonaceous Meteorites

NASA Technical Reports Server (NTRS)

Hoover, Richard B.

2010-01-01

Homochirality of the biomolecules (D-sugars of DNA and RNA and L-amino acids of proteins) is a fundamental property of all life on Earth. Abiotic mechanisms yield racemic mixtures (D/L=1) of chiral molecules and after the death of an organism, the enantiopure chiral biomolecules slowly racemize. Several independent investigators have now established that the amino acids present in CI1 and CM2 carbonaceous meteorites have a moderate to strong excess of the L-enantiomer. Stable isotope data have established that these amino acids are both indigenous and extraterrestrial. Carbonaceous meteorites also contain many other strong chemical biomarkers including purines and pyrimidines (nitrogen heterocycles of nucleic acids); pristine and phytane (components of the chlorophyll pigment) and morphological biomarkers (microfossils of filamentous cyanobacteria). Energy dispersive X-ray Spectroscopy (EDS) analysis reveals that nitrogen is below the detectability level in most of the meteorite filaments as well as in Cambrian Trilobites and filaments of 2.7 Gya Archaean cyanobacteria from Karelia. The deficiency of nitrogen in the filaments and the total absence of sugars, of twelve of the life-critical protein amino acids, and two of the nucleobases of DNA and RNA provide clear and convincing evidence that these filaments are not modern biological contaminants. This paper reviews the chiral, chemical biomarkers morphological biomarkers and microfossils in carbonaceous meteorites. This paper reviews chiral and morphological biomarkers and discusses the missing nitrogen, sugars, protein amino acids, and nucleobases as ?bio-discriminators? that exclude modern biological contaminants as a possible explanation for the permineralized cyanobacterial filaments found in the meteorites.

Maritime Aerosol Network (MAN) as a Component of AERONET

NASA Technical Reports Server (NTRS)

Smirnov, A.; Holben, B. N.; Slutsker, I.; Giles, D. M.; McClain, C. R.; Eck, T. F.; Sakerin, S. M.; Macke, A.; Croot, P.; Zibordi, G.;

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

NASA Astrophysics Data System (ADS)

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

2012-02-01

The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project (~40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 μg m-3 on average) and dominated by organics (80 % of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at ˜400 nm in vacuum aerodynamic diameter (Dva), and a condensation mode at ~150 nm, while organics generally displayed a broad distribution in 60-600 nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a~nominal formula of C1H1.38N0.004O0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90 % of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high-resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly due to local traffic. Twenty three periods of

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

NASA Astrophysics Data System (ADS)

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

2010-05-01

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

Aerosol in the Pacific troposphere

NASA Technical Reports Server (NTRS)

Clarke, Antony D.

1989-01-01

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

Secondary organic aerosol: a comparison between foggy and nonfoggy days.

PubMed

Kaul, D S; Gupta, Tarun; Tripathi, S N; Tare, V; Collett, J L

2011-09-01

Carbonaceous species, meteorological parameters, trace gases, and fogwater chemistry were measured during winter in the Indian city of Kanpur to study secondary organic aerosol (SOA) during foggy and clear (nonfoggy) days. Enhanced SOA production was observed during fog episodes. It is hypothesized that aqueous phase chemistry in fog drops is responsible for increasing SOA production. SOA concentrations on foggy days exceeded those on clear days at all times of day; peak foggy day SOA concentrations were observed in the evening vs peak clear day SOA concentrations which occurred in the afternoon. Changes in biomass burning emissions on foggy days were examined because of their potential to confound estimates of SOA production based on analysis of organic to elemental carbon (OC/EC) ratios. No evidence of biomass burning influence on SOA during foggy days was found. Enhanced oxidation of SO(2) to sulfate during foggy days was observed, possibly causing the regional aerosol to become more acidic. No evidence was found in this study, either, for effects of temperature or relative humidity on SOA production. In addition to SOA production, fogs can also play an important role in cleaning the atmosphere of carbonaceous aerosols. Preferential scavenging of water-soluble organic carbon (WSOC) by fog droplets was observed. OC was found to be enriched in smaller droplets, limiting the rate of OC deposition by droplet sedimentation. Lower EC concentrations were observed on foggy days, despite greater stagnation and lower mixing heights, suggesting fog scavenging and removal of EC was active as well.

Carbonaceous fuel combustion with improved desulfurization

DOEpatents

Yang, Ralph T.; Shen, Ming-shing

1980-01-01

Lime utilization for sulfurous oxides adsorption in fluidized combustion of carbonaceous fuels is improved by impregnation of porous lime particulates with iron oxide. The impregnation is achieved by spraying an aqueous solution of mixed iron sulfate and sulfite on the limestone before transfer to the fluidized bed combustor, whereby the iron compounds react with the limestone substrate to form iron oxide at the limestone surface. The iron oxide present in the spent limestone is found to catalyze the regeneration rate of the spent limestone in a reducing environment. Thus both the calcium and iron components may be recycled.

Environmental Health Hazards of e-Cigarettes and their Components: Oxidants and Copper in e-cigarette aerosols

PubMed Central

Lerner, Chad A.; Sundar, Isaac K.; Watson, Richard M.; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J.; Robinson, Risa; McIntosh, Scott; Rahman, Irfan

2014-01-01

To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. PMID:25577651

A review of current knowledge concerning PM2. 5 chemical composition, aerosol optical properties and their relationships across China

NASA Astrophysics Data System (ADS)

Tao, Jun; Zhang, Leiming; Cao, Junji; Zhang, Renjian

2017-08-01

To obtain a thorough knowledge of PM2. 5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2. 5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2. 5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2. 5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2. 5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2. 5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2. 5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2. 5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM2. 5 mass in applicable cities. The geographical pattern of scattering coefficient (bsp) was similar to that of PM2. 5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions

Spatial and Temporal Variations of EC and OC Aerosol Combustion Sources in a Polluted Metropolitan Area

NASA Astrophysics Data System (ADS)

Mouteva, G.; Randerson, J. T.; Fahrni, S.; Santos, G.; Bush, S. E.; Ehleringer, J. R.; Czimczik, C. I.

2015-12-01

Anthropogenic emissions of carbonaceous aerosols are a major component of fine air particulate matter (PM2.5) in polluted metropolitan areas and in the global atmosphere. Elemental (EC) and organic carbon (OC) aerosols influence Earth's energy balance by means of direct and indirect pathways and EC has been suggested as a better indicator of public health impacts from combustion-related sources than PM mass. Quantifying the contribution of fossil fuel and biomass combustion to the EC and OC emissions and their temporal and spatial variations is critical for developing efficient legislative air pollution control measures and successful climate mitigation strategies. In this study, we used radiocarbon (14C) to separate and quantify fossil and biomass contributions to a time series of EC and OC collected at 3 locations in Salt Lake City (SLC). Aerosol samples were collected on quartz fiber filters and a modified OC/EC analyzer was used with the Swiss_4S protocol to isolate and trap the EC fraction. Together with the total carbon (TC) content of the samples, the EC was analyzed for its 14C content with accelerator mass spectrometry. The 14C of OC was derived as a mass balance difference between TC and EC. EC had an annual average fraction modern of 0.13±0.06 and did not vary significantly across seasons. OC had an annual average FM of 0.49±0.13, with the winter mean (0.43±0.11) lower than the summer mean (0.64±0.13) at the 5% significance level. While the 3 stations were chosen to represent a variety of environmental conditions within SLC, no major differences in this source partitioning were observed between stations. During winter, the major sources of air pollutants in SLC are motor vehicles and wood stove combustion and determining their relative contributions has been the subject of debate. Our results indicated that fossil fuels were the dominant source of carbonaceous aerosols during winter, contributing 87% or more of the total EC mass and 40-75% of the OC

Raman Spectroscopy of Single Light-Absorbing Carbonaceous Particles Levitated in Air Using an Annular Laser Beam.

PubMed

Uraoka, Masaru; Maegawa, Keisuke; Ishizaka, Shoji

2017-12-05

A laser trapping technique is a powerful means to investigate the physical and chemical properties of single aerosol particles in a noncontact manner. However, optical trapping of strongly light-absorbing particles such as black carbon or soot is quite difficult because the repulsive force caused by heat is orders of magnitude larger than the attractive force of radiation pressure. In this study, a laser trapping and Raman microspectroscopy system using an annular laser beam was constructed to achieve noncontact levitation of single light-absorbing particles in air. Single acetylene carbon black or candle soot particles were arbitrarily selected with a glass capillary connected to a three-axis oil hydraulic micromanipulator and introduced into a minute space surrounded by a repulsive force at the focal point of an objective lens. Using the developed system, we achieved optical levitation of micrometer-sized carbonaceous particles and observation of their Raman spectra in air. Furthermore, we demonstrated in situ observations of changes in the morphology and chemical composition of optically trapped carbonaceous particles in air, which were induced by heterogeneous oxidation reactions with ozone and hydroxyl radicals.

Biochemical transformation of solid carbonaceous material

DOEpatents

Lin, Mow S.; Premuzic, Eugene T.

2001-09-25

A method of biochemically transforming macromolecular compounds found in solid carbonaceous materials, such as coal is provided. The preparation of new microorganisms, metabolically weaned through challenge growth processes to biochemically transform solid carbonaceous materials at extreme temperatures, pressures, pH, salt and toxic metal concentrations is also disclosed.

Carbonaceous aerosol characterization in the Amazon basin, Brazil: novel dicarboxylic acids and related compounds

NASA Astrophysics Data System (ADS)

Kubátová, Alena; Vermeylen, Reinhilde; Claeys, Magda; Cafmeyer, Jan; Maenhaut, Willy; Roberts, Greg; Artaxo, Paulo

High-resolution capillary gas chromatography (GC) and GC/mass spectrometry (MS) were employed for the quantitative determination of dichloromethane-extractable organic compounds in total and size-fractionated aerosol samples which were collected in the Amazon basin, Brazil, during the wet season, as part of the LBA-CLAIRE-98 experiment. Special emphasis was placed on the characterization and identification of several novel unknown dicarboxylic acids and related oxidative degradation products. This class of acidic products was enriched in the fine size fraction, suggesting that they were secondary organic aerosol products formed by gas-to-particle conversion. Some of the unknowns contributed more to the class of dicarboxylic acids than the major known compound, nonadioic acid (azelaic acid). The same unknowns were also observed in urban aerosol samples collected on hot summer days in Gent, Belgium. For the characterization and structure elucidation of the unknowns, various types of derivatizations and fractionation by solid-phase extraction were employed in combination with GC/MS. Four unknowns were identified. The most abundant were two derivatives of glutaric acid, 3-isopropyl pentanedioic acid and 3-acetyl pentanedioic acid. The other two identified unknowns were another oxo homologue, 3-acetyl hexanedioic acid, and, interestingly, 3-carboxy heptanedioic acid. To our knowledge, the occurrence of these four compounds in atmospheric aerosols has not yet been reported. The biogenic precursors of the novel identified compounds could not be pinpointed, but most likely include monoterpenes and fatty acids.

Carbonaceous electrode materials for supercapacitors.

PubMed

Hao, Long; Li, Xianglong; Zhi, Linjie

2013-07-26

Supercapacitors have been widely studied around the world in recent years, due to their excellent power density and long cycle life. As the most frequently used electrode materials for supercapacitors, carbonaceous materials attract more and more attention. However, their relatively low energy density still holds back the widespread application. Up to now, various strategies have been developed to figure out this problem. This research news summarizes the recent advances in improving the supercapacitor performance of carbonaceous materials, including the incorporation of heteroatoms and the pore size effect (subnanopores' contribution). In addition, a new class of carbonaceous materials, porous organic networks (PONs) has been managed into the supercapacitor field, which promises great potential in not only improving the supercapacitor performances, but also unraveling the related mechanisms. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The implementation of NEMS GFS Aerosol Component (NGAC) Version 1.0 for global dust forecasting at NOAA/NCEP

PubMed Central

Lu, Cheng-Hsuan; da Silva, Arlindo; Wang, Jun; Moorthi, Shrinivas; Chin, Mian; Colarco, Peter; Tang, Youhua; Bhattacharjee, Partha S.; Chen, Shen-Po; Chuang, Hui-Ya; Juang, Hann-Ming Henry; McQueen, Jeffery; Iredell, Mark

2018-01-01

The NOAA National Centers for Environmental Prediction (NCEP) implemented NEMS GFS Aerosol Component (NGAC) for global dust forecasting in collaboration with NASA Goddard Space Flight Center (GSFC). NGAC Version 1.0 has been providing 5 day dust forecasts at 1°×1° resolution on a global scale, once per day at 00:00 Coordinated Universal Time (UTC), since September 2012. This is the first global system capable of interactive atmosphere aerosol forecasting at NCEP. The implementation of NGAC V1.0 reflects an effective and efficient transitioning of NASA research advances to NCEP operations, paving the way for NCEP to provide global aerosol products serving a wide range of stakeholders as well as to allow the effects of aerosols on weather forecasts and climate prediction to be considered. PMID:29652411

The implementation of NEMS GFS Aerosol Component (NGAC) Version 1.0 for global dust forecasting at NOAA/NCEP.

PubMed

Lu, Cheng-Hsuan; da Silva, Arlindo; Wang, Jun; Moorthi, Shrinivas; Chin, Mian; Colarco, Peter; Tang, Youhua; Bhattacharjee, Partha S; Chen, Shen-Po; Chuang, Hui-Ya; Juang, Hann-Ming Henry; McQueen, Jeffery; Iredell, Mark

2016-01-01

The NOAA National Centers for Environmental Prediction (NCEP) implemented NEMS GFS Aerosol Component (NGAC) for global dust forecasting in collaboration with NASA Goddard Space Flight Center (GSFC). NGAC Version 1.0 has been providing 5 day dust forecasts at 1°×1° resolution on a global scale, once per day at 00:00 Coordinated Universal Time (UTC), since September 2012. This is the first global system capable of interactive atmosphere aerosol forecasting at NCEP. The implementation of NGAC V1.0 reflects an effective and efficient transitioning of NASA research advances to NCEP operations, paving the way for NCEP to provide global aerosol products serving a wide range of stakeholders as well as to allow the effects of aerosols on weather forecasts and climate prediction to be considered.

Trans-Pacific transport and evolution of aerosols: Evaluation of quasi-global WRF-Chem simulation with multiple observations

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

Hu, Zhiyuan; Zhao, Chun; Huang, Jianping

A fully coupled meteorology-chemistry model (WRF-Chem, the Weather Research and Forecasting model coupled with chemistry) has been configured to conduct quasi-global simulation for 5 years (2010–2014) and evaluated with multiple observation data sets for the first time. The evaluation focuses on the simulation over the trans-Pacific transport region using various reanalysis and observational data sets for meteorological fields and aerosol properties. The simulation generally captures the overall spatial and seasonal variability of satellite retrieved aerosol optical depth (AOD) and absorbing AOD (AAOD) over the Pacific that is determined by the outflow of pollutants and dust and the emissions of marine aerosols.more » The assessment of simulated extinction Ångström exponent (EAE) indicates that the model generally reproduces the variability of aerosol size distributions as seen by satellites. In addition, the vertical profile of aerosol extinction and its seasonality over the Pacific are also well simulated. The difference between the simulation and satellite retrievals can be mainly attributed to model biases in estimating marine aerosol emissions as well as the satellite sampling and retrieval uncertainties. Compared with the surface measurements over the western USA, the model reasonably simulates the observed magnitude and seasonality of dust, sulfate, and nitrate surface concentrations, but significantly underestimates the peak surface concentrations of carbonaceous aerosol likely due to model biases in the spatial and temporal variability of biomass burning emissions and secondary organic aerosol (SOA) production. A sensitivity simulation shows that the trans-Pacific transported dust, sulfate, and nitrate can make significant contribution to surface concentrations over the rural areas of the western USA, while the peaks of carbonaceous aerosol surface concentrations are dominated by the North American emissions. Both the retrievals and simulation show

Trans-Pacific transport and evolution of aerosols: Evaluation of quasi-global WRF-Chem simulation with multiple observations

DOE PAGES

Hu, Zhiyuan; Zhao, Chun; Huang, Jianping; ...

2016-05-10

A fully coupled meteorology-chemistry model (WRF-Chem, the Weather Research and Forecasting model coupled with chemistry) has been configured to conduct quasi-global simulation for 5 years (2010–2014) and evaluated with multiple observation data sets for the first time. The evaluation focuses on the simulation over the trans-Pacific transport region using various reanalysis and observational data sets for meteorological fields and aerosol properties. The simulation generally captures the overall spatial and seasonal variability of satellite retrieved aerosol optical depth (AOD) and absorbing AOD (AAOD) over the Pacific that is determined by the outflow of pollutants and dust and the emissions of marine aerosols.more » The assessment of simulated extinction Ångström exponent (EAE) indicates that the model generally reproduces the variability of aerosol size distributions as seen by satellites. In addition, the vertical profile of aerosol extinction and its seasonality over the Pacific are also well simulated. The difference between the simulation and satellite retrievals can be mainly attributed to model biases in estimating marine aerosol emissions as well as the satellite sampling and retrieval uncertainties. Compared with the surface measurements over the western USA, the model reasonably simulates the observed magnitude and seasonality of dust, sulfate, and nitrate surface concentrations, but significantly underestimates the peak surface concentrations of carbonaceous aerosol likely due to model biases in the spatial and temporal variability of biomass burning emissions and secondary organic aerosol (SOA) production. A sensitivity simulation shows that the trans-Pacific transported dust, sulfate, and nitrate can make significant contribution to surface concentrations over the rural areas of the western USA, while the peaks of carbonaceous aerosol surface concentrations are dominated by the North American emissions. Both the retrievals and simulation show

Trans-Pacific transport and evolution of aerosols: evaluation of quasi-global WRF-Chem simulation with multiple observations

NASA Astrophysics Data System (ADS)

Hu, Zhiyuan; Zhao, Chun; Huang, Jianping; Leung, L. Ruby; Qian, Yun; Yu, Hongbin; Huang, Lei; Kalashnikova, Olga V.

2016-05-01

A fully coupled meteorology-chemistry model (WRF-Chem, the Weather Research and Forecasting model coupled with chemistry) has been configured to conduct quasi-global simulation for 5 years (2010-2014) and evaluated with multiple observation data sets for the first time. The evaluation focuses on the simulation over the trans-Pacific transport region using various reanalysis and observational data sets for meteorological fields and aerosol properties. The simulation generally captures the overall spatial and seasonal variability of satellite retrieved aerosol optical depth (AOD) and absorbing AOD (AAOD) over the Pacific that is determined by the outflow of pollutants and dust and the emissions of marine aerosols. The assessment of simulated extinction Ångström exponent (EAE) indicates that the model generally reproduces the variability of aerosol size distributions as seen by satellites. In addition, the vertical profile of aerosol extinction and its seasonality over the Pacific are also well simulated. The difference between the simulation and satellite retrievals can be mainly attributed to model biases in estimating marine aerosol emissions as well as the satellite sampling and retrieval uncertainties. Compared with the surface measurements over the western USA, the model reasonably simulates the observed magnitude and seasonality of dust, sulfate, and nitrate surface concentrations, but significantly underestimates the peak surface concentrations of carbonaceous aerosol likely due to model biases in the spatial and temporal variability of biomass burning emissions and secondary organic aerosol (SOA) production. A sensitivity simulation shows that the trans-Pacific transported dust, sulfate, and nitrate can make significant contribution to surface concentrations over the rural areas of the western USA, while the peaks of carbonaceous aerosol surface concentrations are dominated by the North American emissions. Both the retrievals and simulation show small

Exposure ages of carbonaceous chondrites, 1

NASA Technical Reports Server (NTRS)

Nishiizumi, K.; Arnold, J. R.; Caffee, M. W.; Finkel, R. C.; Southon, J. R.; Nagai, H.; Honda, M.; Sharma, P.; Imamura, M.; Kobayashi, K.

1993-01-01

The recent exposure histories of carbonaceous chondrites have been investigated using cosmogenic radionuclides. Our results may indicate a clustering of exposure ages of C1 and C2 chondrites into two peaks, 0.2 My and 0.6 My, perhaps implying two collisional events of Earth-crossing parent bodies. Among carbonaceous chondrites are some having short exposure ages which Mazor et al. hypothesized cluster into a small number of families. This hypothesis is based on spallogenic Ne-21 exposure ages, which in some instances are difficult to determine owing to the large amounts of trapped noble gases in carbonaceous chondrites. Also, since Ne-21 is stable, it integrates a sample's entire exposure history, so meteorites with complex exposure histories are difficult to understand using exclusively Ne-21. Cosmogenic radionuclides provide an alternative means of determining the recent cosmic ray exposure duration. To test the hypothesis of Mazor et al. we have begun a systematic investigation of exposure histories of Antarctic and non-Antarctic carbonaceous chondrites especially C2s.

Mixed Calcium Dust and Carbonaceous Particles from Asia Contributing to Precipitation Changes in California

NASA Astrophysics Data System (ADS)

Kristensen, L.; Cornwell, G.; Sedlacek, A. J., III; Prather, K. A.

2016-12-01

Mineral dust particles can serve as cloud condensation nuclei (CCN), with enhanced CCN activity observed when the dust is mixed with additional soluble species. Long range atmospheric transport can change the composition of dust particles through aging, cloud processing and mixing with other particles. The CalWater2 campaign measured single particles and cloud dynamics to investigate the influence aerosols have on the hydrological cycle in California. An Aircraft Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) was used to characterize and identify single particles within clouds potentially acting as ice and cloud nuclei. Two matching flights over California's mountains in March 2015 detected significantly different particle types that resulted in different precipitation totals. Calcium dust dominated the particle composition during the first flight which had an observed decrease in orographic precipitation. Particle composition and air mass back trajectories indicate an Asian desert origin. The calcium dust particles contained secondary acids, in particular oxalic acid, acquired during transport from Asia to California. This chemical processing likely increased the solubility of the dust, enabling the particles to act as more effective CCN. The chemical composition also showed oligomeric carbonaceous species were mixed with the calcium dust particles, potentially further increasing the solubility the particles. A single particle soot photometer (SP2) measured black carbon concurrently and returned intense incandescence when calcium dust was present, confirming the calcium dust particles were internally mixed with a carbonaceous species. Dust particles were greatly reduced during the second flight with local biomass burning particles the dominant type. Observed precipitation in California were within forecast levels during the second flight. These single particle measurements from CalWater2 show that dust particles from Asia can affect cloud process and thus

Highly Siderophile Elements and Osmium Isotope Systematics in Ureilites: Are the Carbonaceous Veins Primary Components?

NASA Technical Reports Server (NTRS)

Rankenburg, K.; Brandon, A. D.; Humayun, M.

2005-01-01

Ureilites are an enigmatic group of primitive carbon-bearing achondrites of ultramafic composition. The majority of the 143 ureilite meteorites consist primarily of olivine and pyroxene (and occasionally chromite) [1]. They are coarse-grained, slowly cooled, and depleted in incompatible lithophile elements. Minor amounts of dark interstitial material consisting of carbon, metal, sulfides, and fine-grained silicates occur primarily along silicate grain boundaries, but also intrude the silicates along fractures and cleavage planes. Variable degrees of impact shock features have also been imparted on ureilites. The prevailing two origins proposed for these rocks are either as melting residues of carbonaceous chondritic material [2], [3], or alternatively, derivation as mineral cumulates from such melts [4], [5], [6]. It has recently been proposed that ureilites are the residues of a smelting event, i.e. residues of a partial melting event under highly reducing conditions, where a solid Fe-bearing phase reacts with a melt and carbon to form Fe metal and carbon monoxide [7]. Rapid, localized extraction and loss of the basaltic component into space resulting from high eruption velocities could preserve unequilibrated oxygen isotopes and produce the observed olivine-pyroxene residues via 25-30% partial melting of chondritic-like precursor material.

Environmental health hazards of e-cigarettes and their components: Oxidants and copper in e-cigarette aerosols.

PubMed

Lerner, Chad A; Sundar, Isaac K; Watson, Richard M; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J; Robinson, Risa; McIntosh, Scott; Rahman, Irfan

2015-03-01

To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery Systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. Copyright © 2014 Elsevier Ltd. All rights reserved.

Aerosols in the CALIOPE air quality modelling system: evaluation and analysis of PM levels, optical depths and chemical composition over Europe

NASA Astrophysics Data System (ADS)

Basart, S.; Pay, M. T.; Jorba, O.; Pérez, C.; Jiménez-Guerrero, P.; Schulz, M.; Baldasano, J. M.

2012-04-01

The CALIOPE air quality modelling system is developed and applied to Europe with high spatial resolution (12 km × 12 km). The modelled daily-to-seasonal aerosol variability over Europe in 2004 is evaluated and analysed. Aerosols are estimated from two models, CMAQv4.5 (AERO4) and BSC-DREAM8b. CMAQv4.5 calculates biogenic, anthropogenic and sea salt aerosol and BSC-DREAM8b provides the natural mineral dust contribution from North African deserts. For the evaluation, we use daily PM10, PM2.5 and aerosol components data from 55 stations of the EMEP/CREATE network and total, coarse and fine aerosol optical depth (AOD) data from 35 stations of the AERONET sun photometer network. Annual correlations between modelled and observed values for PM10 and PM2.5 are 0.55 and 0.47, respectively. Correlations for total, coarse and fine AOD are 0.51, 0.63, and 0.53, respectively. The higher correlations of the PM10 and the coarse mode AOD are largely due to the accurate representation of the African dust influence in the forecasting system. Overall PM and AOD levels are underestimated. The evaluation of the aerosol components highlights underestimations in the fine fraction of carbonaceous matter (EC and OC) and secondary inorganic aerosols (SIA; i.e. nitrate, sulphate and ammonium). The scores of the bulk parameters are significantly improved after applying a simple model bias correction based on the observed aerosol composition. The simulated PM10 and AOD present maximum values over the industrialized and populated Po Valley and Benelux regions. SIA are dominant in the fine fraction representing up to 80% of the aerosol budget in latitudes north of 40° N. In southern Europe, high PM10 and AOD are linked to the desert dust transport from the Sahara which contributes up to 40% of the aerosol budget. Maximum seasonal ground-level concentrations (PM10 > 30 μg m-3) are found between spring and early autumn. We estimate that desert dust causes daily exceedances of the PM10 European

FORMATION OF POLYCYCLIC AROMATIC HYDROCARBONS AND CARBONACEOUS SOLIDS IN GAS-PHASE CONDENSATION EXPERIMENTS

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

Jaeger, C.; Huisken, F.; Henning, Th.

2009-05-01

Carbonaceous grains represent a major component of cosmic dust. In order to understand their formation pathways, they have been prepared in the laboratory by gas-phase condensation reactions such as laser pyrolysis and laser ablation. Our studies demonstrate that the temperature in the condensation zone determines the formation pathway of carbonaceous particles. At temperatures lower than 1700 K, the condensation by-products are mainly polycyclic aromatic hydrocarbons (PAHs) that are also the precursors or building blocks for the condensing soot grains. The low-temperature condensates contain PAH mixtures that are mainly composed of volatile three to five ring systems. At condensation temperatures highermore » than 3500 K, fullerene-like carbon grains and fullerene compounds are formed. Fullerene fragments or complete fullerenes equip the nucleating particles. Fullerenes can be identified as soluble components. Consequently, condensation products in cool and hot astrophysical environments such as cool and hot asymptotic giant branch stars or Wolf-Rayet stars should be different and should have distinct spectral properties.« less

Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

NASA Technical Reports Server (NTRS)

da Silva, Arlindo

2010-01-01

A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

The Implementation of NEMS GFS Aerosol Component (NGAC) Version 1.0 for Global Dust Forecasting at NOAA NCEP

NASA Technical Reports Server (NTRS)

Lu, Cheng-Hsuan; Da Silva, Arlindo M.; Wang, Jun; Moorthi, Shrinivas; Chin, Mian; Colarco, Peter; Tang, Youhua; Bhattacharjee, Partha S.; Chen, Shen-Po; Chuang, Hui-Ya;

The GRAPE aerosol retrieval algorithm

NASA Astrophysics Data System (ADS)

Thomas, G. E.; Poulsen, C. A.; Sayer, A. M.; Marsh, S. H.; Dean, S. M.; Carboni, E.; Siddans, R.; Grainger, R. G.; Lawrence, B. N.

2009-11-01

The aerosol component of the Oxford-Rutherford Aerosol and Cloud (ORAC) combined cloud and aerosol retrieval scheme is described and the theoretical performance of the algorithm is analysed. ORAC is an optimal estimation retrieval scheme for deriving cloud and aerosol properties from measurements made by imaging satellite radiometers and, when applied to cloud free radiances, provides estimates of aerosol optical depth at a wavelength of 550 nm, aerosol effective radius and surface reflectance at 550 nm. The aerosol retrieval component of ORAC has several incarnations - this paper addresses the version which operates in conjunction with the cloud retrieval component of ORAC (described by Watts et al., 1998), as applied in producing the Global Retrieval of ATSR Cloud Parameters and Evaluation (GRAPE) data-set. The algorithm is described in detail and its performance examined. This includes a discussion of errors resulting from the formulation of the forward model, sensitivity of the retrieval to the measurements and a priori constraints, and errors resulting from assumptions made about the atmospheric/surface state.

The GRAPE aerosol retrieval algorithm

NASA Astrophysics Data System (ADS)

Thomas, G. E.; Poulsen, C. A.; Sayer, A. M.; Marsh, S. H.; Dean, S. M.; Carboni, E.; Siddans, R.; Grainger, R. G.; Lawrence, B. N.

2009-04-01

The aerosol component of the Oxford-Rutherford Aerosol and Cloud (ORAC) combined cloud and aerosol retrieval scheme is described and the theoretical performance of the algorithm is analysed. ORAC is an optimal estimation retrieval scheme for deriving cloud and aerosol properties from measurements made by imaging satellite radiometers and, when applied to cloud free radiances, provides estimates of aerosol optical depth at a wavelength of 550 nm, aerosol effective radius and surface reflectance at 550 nm. The aerosol retrieval component of ORAC has several incarnations - this paper addresses the version which operates in conjunction with the cloud retrieval component of ORAC (described by Watts et al., 1998), as applied in producing the Global Retrieval of ATSR Cloud Parameters and Evaluation (GRAPE) data-set. The algorithm is described in detail and its performance examined. This includes a discussion of errors resulting from the formulation of the forward model, sensitivity of the retrieval to the measurements and a priori constraints, and errors resulting from assumptions made about the atmospheric/surface state.

Variability in aerosol optical properties over an urban site, Kanpur, in the Indo-Gangetic Plain: A case study of haze and dust events

NASA Astrophysics Data System (ADS)

Ram, Kirpa; Singh, Sunita; Sarin, M. M.; Srivastava, A. K.; Tripathi, S. N.

2016-06-01

In this study, we report on three important optical parameters, viz. absorption and scattering coefficients (babs, bscat) and single scattering abledo (SSA) based on one-year chemical-composition data collected from an urban site (Kanpur) in the Indo-Gangetic-Plain (IGP) of northern India. In addition, absorption Ängstrom exponent (AAE) was also estimated in order to understand the wavelength dependence of absorption and to decipher emission sources of carbonaceous aerosols, in particular of black carbon. The absorption and scattering coefficients ranged between 8.3 to 95.2 Mm- 1 (1 Mm- 1 = 10- 6 m- 1) and 58 to 564 Mm- 1, respectively during the study period (for n = 66; from January 2007 to March 2008) and exhibit large seasonal variability with higher values occurring in winter and lower in the summer. Single scattering albedo varied from 0.65 to 0.92 whereas AAE ranged from 0.79 to 1.40 during pre-monsoon and winter seasons, respectively. The strong seasonal variability in aerosol optical properties is attributed to varying contribution from different emission sources of carbonaceous aerosols in the IGP. A case study of haze and dust events further provide information on extreme variability in aerosol optical parameters, particularly SSA, a crucial parameter in atmospheric radiative forcing estimates.

Climatology of the Aerosol Optical Depth by Components from the Multi-Angle Imaging Spectroradiometer (MISR) and Chemistry Transport Models

NASA Technical Reports Server (NTRS)

Lee, Huikyo; Kalashnikova, Olga V.; Suzuki, Kentaroh; Braverman, Amy; Garay, Michael J.; Kahn, Ralph A.

2016-01-01

The Multi-angle Imaging Spectroradiometer (MISR) Joint Aerosol (JOINT_AS) Level 3 product has provided a global, descriptive summary of MISR Level 2 aerosol optical depth (AOD) and aerosol type information for each month over 16+ years since March 2000. Using Version 1 of JOINT_AS, which is based on the operational (Version 22) MISR Level 2 aerosol product, this study analyzes, for the first time, characteristics of observed and simulated distributions of AOD for three broad classes of aerosols: spherical nonabsorbing, spherical absorbing, and nonspherical - near or downwind of their major source regions. The statistical moments (means, standard deviations, and skew-nesses) and distributions of AOD by components derived from the JOINT_AS are compared with results from two chemistry transport models (CTMs), the Goddard Chemistry Aerosol Radiation and Transport (GOCART) and SPectral RadIatioN-TrAnSport (SPRINTARS). Overall, the AOD distributions retrieved from MISR and modeled by GOCART and SPRINTARS agree with each other in a qualitative sense. Marginal distributions of AOD for each aerosol type in both MISR and models show considerable high positive skewness, which indicates the importance of including extreme AOD events when comparing satellite retrievals with models. The MISR JOINT_AS product will greatly facilitate comparisons between satellite observations and model simulations of aerosols by type.

Sugar-Related Organic Compounds in Carbonaceous Meteorites

NASA Technical Reports Server (NTRS)

Cooper, G.; Kimmich, N.; Belisle, W.; Sarinana, J.; Brabham, K.; Garrel, L.; DeVincenzi, Donald L. (Technical Monitor)

2001-01-01

Sugars and related polyols are critical components of all organisms and may have been necessary for the origin of life. To date, this class of organic compounds had not been definitively identified in meteorites. This study was undertaken to determine if polyols were present in the early Solar System as constituents of carbonaceous meteorites. Results of analyses of the Murchison and Murray meteorites indicate that formaldehyde and sugar chemistry may be responsible for the presence of a variety of polyols. We conclude that polyols were present on the early Earth through delivery by asteroids and possibly comets.

CCN activity of thermodenuded aerosol particles downwind of the Sacramento area urban plume

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Cziczo, D. J.; Nelson, D.; Zhang, Q.; Setyan, A.; Song, C.; Shrivastava, M.; Shilling, J. E.

2010-12-01

This study focuses on the characterization of cloud condensation nuclei (CCN) properties of aerosol particles measured during the Carbonaceous Aerosols and Radiative Effects Study (CARES) near Sacramento, CA in June 2010. Supersaturation-dependant CCN activity (0.07 - 0.5% supersaturation) was measured with DMT CCN counters at two locations; one near the city center (T0) and the other in Cool, CA, a small town located ~40 kilometers downwind of the urban plume in the Sierra Nevada foothills (T1). The T1 CCN counter was operated behind a thermodenuder to study volatility-dependant CCN activity of the urban aerosol plume as it was transported into the biogenically influenced foothills. Preliminary analysis indicated that activated fraction was inversely proportional to the thermodenuder temperature, suggesting that the more-volatile fraction of the aerosol might have played an important role in the CCN activity of the aerosol. The relationship between the chemical composition and CCN activity of the aerosol will be discussed. The physical and chemical transformations of particles aged in the foothills as well as the diurnal profiles of CCN both at T0 and T1 will also be discussed for the transport event of 15 June 2010.

Comets: Cosmic connections with carbonaceous meteorites, interstellar molecules and the origin of life

NASA Technical Reports Server (NTRS)

Chang, S.

1979-01-01

The ions, radicals, and molecules observed in comets may be derived intact or by partial decomposition from parent compounds of the sort found either in the interstellar medium or in carbonaceous meteorites. The early loss of highly reducing primitive atmosphere and its replacement by a secondary atmosphere dominated by H2O, CO2, and N2, as depicted in current models of the earth's evolution, pose a dilemma for the origin of life: the synthesis of organic compounds necessary for life from components of the secondary atmosphere appears to be difficult, and plausible mechanisms have not been evaluated. Both comets and carbonaceous meteorites are implicated as sources for the earth's atmophilic and organogenic elements. A mass balance argument involving the estimated ratios of hydrogen to carbon in carbonaceous meteorites, comets, and the crust and upper mantle suggests that comets supplied the earth with a large fraction of its volatiles. The probability that comets contributed significantly to the earth's volatile inventory suggests a chemical evolutionary link between comets, prebiotic organic synthesis, and the origin of life.

Opaque Assemblages in CK and CV Carbonaceous Chondrites

NASA Technical Reports Server (NTRS)

Neff, K. E.; Righter, K.

2006-01-01

CK carbonaceous chondrites are the only group of carbonaceous chondrites that exhibit thermal metamorphism. As a result, CKs display features of metamorphism such as silicate darkening, recrystallization and shock veins. Calcium Aluminum Inclusions and Fe-Ni metal are rare. CV carbonaceous chondrites are unequilibrated and have two subgroups; oxidized and reduced. The CV and CK carbonaceous chondrite groups have been compared to each other often because of petrographic similarities, such as overlapping oxygen isotopic ratios. Scientists have suggested the two groups of carbonaceous chondrites formed from the same parent body and CKs are equilibrated CV chondrites [1, 2]. The oxidized CV group has been most closely related to CKs. This study examines the petrology and mineralogy of CKs and CVs focusing on opaque minerals found in the meteorites. Using the oxide, metal and sulfide assemblages, constraints can be placed on the temperature and oxygen fugacity at which the meteorites equilibrated. The temperature and oxygen fugacity of the CK and CV chondrites can be compared in order to help define their formation history.

Absorbing Aerosols Above Cloud: Detection, Quantitative Retrieval, and Radiative Forcing from Satellite-based Passive Sensors

NASA Astrophysics Data System (ADS)

Jethva, H.; Torres, O.; Remer, L. A.; Bhartia, P. K.

2012-12-01

Light absorbing particles such as carbonaceous aerosols generated from biomass burning activities and windblown dust particles can exert a net warming effect on climate; the strength of which depends on the absorption capacity of the particles and brightness of the underlying reflecting background. When advected over low-level bright clouds, these aerosols absorb the cloud reflected radiation from ultra-violet (UV) to shortwave-IR (SWIR) and makes cloud scene darker-a phenomenon commonly known as "cloud darkening". The apparent "darkening" effect can be seen by eyes in satellite images as well as quantitatively in the spectral reflectance measurements made by space borne sensors over regions where light absorbing carbonaceous and dust aerosols overlay low-level cloud decks. Theoretical radiative transfer simulations support the observational evidence, and further reveal that the strength of the cloud darkening and its spectral signature (or color ratio) between measurements at two wavelengths are a bi-function of aerosol and cloud optical thickness (AOT and COT); both are measures of the total amount of light extinction caused by aerosols and cloud, respectively. Here, we developed a retrieval technique, named as the "color ratio method" that uses the satellite measurements at two channels, one at shorter wavelength in the visible and one at longer wavelength in the shortwave-IR for the simultaneous retrieval of AOT and COT. The present technique requires assumptions on the aerosol single-scattering albedo and aerosol-cloud separation which are supplemented by the Aerosol Robotic Network (AERONET) and space borne CALIOP lidar measurements. The retrieval technique has been tested making use of the near-UV and visible reflectance observations made by the Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) for distinct above-cloud smoke and dust aerosol events observed seasonally over the southeast and tropical Atlantic Ocean

Aerosols in Northern Morocco: Input pathways and their chemical fingerprint

NASA Astrophysics Data System (ADS)

Benchrif, A.; Guinot, B.; Bounakhla, M.; Cachier, H.; Damnati, B.; Baghdad, B.

2018-02-01

The Mediterranean basin is one of the most sensitive regions in the world regarding climate change and air quality. Deserts and marine aerosols combine with combustion aerosols from maritime traffic, large urban centers, and at a larger scale from populated industrialized regions in Europe. From Tetouan city located in the North of Morocco, we attempted to better figure out the main aerosol transport pathways and their respective aerosol load and chemical profile by examining air mass back trajectory patterns and aerosol chemical compositions from May 2011 to April 2012. The back trajectory analysis throughout the sampling period led to four clusters, for which meteorological conditions and aerosol chemical characteristics have been investigated. The most frequent cluster (CL3: 39%) corresponds to polluted air masses coming from the Mediterranean Basin, characterized by urban and marine vessels emissions out of Spain and of Northern Africa. Two other polluted clusters were characterized. One is of local origin (CL1: 22%), with a marked contribution from urban aerosols (Rabat, Casablanca) and from biomass burning aerosols. The second (CL2: 32%) defines air masses from the near Atlantic Ocean, affected by pollutants emitted from the Iberian coast. A fourth cluster (CL4: 7%) is characterized by rather clean, fast and rainy oceanic air masses, influenced during their last 24 h before reaching Tetouan by similar sources with those affecting CL2, but to a lesser extent. The chemical data show that carbonaceous species are found in the fine aerosols fraction and are generally from local primary sources (low OC/EC) rather than long-range transported. In addition to fresh traffic and maritime vessel aerosols, our results suggest the contribution of local biomass burning.

Impact of anomalous forest fire on aerosol radiative forcing and snow cover over Himalayan region

NASA Astrophysics Data System (ADS)

Bali, Kunal; Mishra, Amit Kumar; Singh, Sachchidanand

2017-02-01

Forest fires are very common in tropical region during February-May months and are known to have significant impact on ecosystem dynamics. Moreover, aerosols emitted from these burning activities significantly modulate the Earth's radiation budget. In present study, we investigated the anomalous forest fire events and their impact on atmospheric radiation budget and glaciated snow cover over the Himalayan region. We used multiple dataset derived from satellites [Moderate Resolution Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO)] and reanalysis models [Global Fire Assimilation System (GFAS), Second Modern-Era Retrospective analysis for Research and Application (MERRA-2) and ERA-interim] to evaluate the effect of biomass burning aerosols on radiation budget. April 2016 is associated with anomalous fire activities over lower Himalayan region in the last fourteen years (2003-2016). The model estimated organic carbon (OC) and black carbon (BC) emission reaches up to ∼3 × 104 and ∼2 × 103 μg/m2/day, respectively during the biomass burning period of April 2016. The meteorological data analysis accompanied with CALIOP aerosol vertical profile shows that these carbonaceous aerosols could reach up to ∼5-7 km altitude and could be transported towards glaciated region of upper Himalayas. The large amount of BC/OC from biomass burning significantly modulates the atmospheric radiation budget. The estimated columnar heating rate shows that these carbonaceous aerosols could heat up the atmosphere by ∼0.04-0.06 K/day in April-2016 with respect to non-burning period (2015). The glaciated snow cover fractions are found to be decreasing by ∼5-20% in 2016 as compared to long term mean (2003-2016). The combined analyses of various climatic factors, fires and associated BC emissions show that the observed snow cover decrease could be results of increased surface/atmospheric temperature due to combined effect of

Aerosol retrieval experiments in the ESA Aerosol_cci project

NASA Astrophysics Data System (ADS)

Holzer-Popp, T.; de Leeuw, G.; Griesfeller, J.; Martynenko, D.; Klüser, L.; Bevan, S.; Davies, W.; Ducos, F.; Deuzé, J. L.; Graigner, R. G.; Heckel, A.; von Hoyningen-Hüne, W.; Kolmonen, P.; Litvinov, P.; North, P.; Poulsen, C. A.; Ramon, D.; Siddans, R.; Sogacheva, L.; Tanre, D.; Thomas, G. E.; Vountas, M.; Descloitres, J.; Griesfeller, J.; Kinne, S.; Schulz, M.; Pinnock, S.

2013-08-01

Within the ESA Climate Change Initiative (CCI) project Aerosol_cci (2010-2013), algorithms for the production of long-term total column aerosol optical depth (AOD) datasets from European Earth Observation sensors are developed. Starting with eight existing pre-cursor algorithms three analysis steps are conducted to improve and qualify the algorithms: (1) a series of experiments applied to one month of global data to understand several major sensitivities to assumptions needed due to the ill-posed nature of the underlying inversion problem, (2) a round robin exercise of "best" versions of each of these algorithms (defined using the step 1 outcome) applied to four months of global data to identify mature algorithms, and (3) a comprehensive validation exercise applied to one complete year of global data produced by the algorithms selected as mature based on the round robin exercise. The algorithms tested included four using AATSR, three using MERIS and one using PARASOL. This paper summarizes the first step. Three experiments were conducted to assess the potential impact of major assumptions in the various aerosol retrieval algorithms. In the first experiment a common set of four aerosol components was used to provide all algorithms with the same assumptions. The second experiment introduced an aerosol property climatology, derived from a combination of model and sun photometer observations, as a priori information in the retrievals on the occurrence of the common aerosol components. The third experiment assessed the impact of using a common nadir cloud mask for AATSR and MERIS algorithms in order to characterize the sensitivity to remaining cloud contamination in the retrievals against the baseline dataset versions. The impact of the algorithm changes was assessed for one month (September 2008) of data: qualitatively by inspection of monthly mean AOD maps and quantitatively by comparing daily gridded satellite data against daily averaged AERONET sun photometer

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.

Carbonaceous cathode with enhanced wettability for aluminum production

DOEpatents

Keller, Rudolf; Gatty, David G.; Barca, Brian J.

2003-09-09

A method of preparing carbonaceous blocks or bodies for use in a cathode in an electrolytic cell for producing aluminum wherein the cell contains an electrolyte and has molten aluminum contacting the cathode, the cathode having improved wettability with molten aluminum. The method comprises the steps of providing a carbonaceous block and a boron oxide containing melt. The carbonaceous block is immersed in the melt and pressure is applied to the melt to impregnate the melt into pores in the block. Thereafter, the carbonaceous block is withdrawn from the melt, the block having boron oxide containing melt intruded into pores therein, the boron oxide capable of reacting with a source of titanium or zirconium or like metal to form titanium or zirconium diboride during heatup or operation of said cell.

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

PubMed

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

2011-02-01

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

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

NASA Astrophysics Data System (ADS)

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

2011-07-01

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

Photoacoustic and filter measurements related to aerosol light absorption during the Northern Front Range Air Quality Study (Colorado 1996/1997)

NASA Astrophysics Data System (ADS)

Moosmüller, H.; Arnott, W. P.; Rogers, C. F.; Chow, J. C.; Frazier, C. A.; Sherman, L. E.; Dietrich, D. L.

1998-11-01

A new photoacoustic instrument for the measurement of aerosol light absorption was collocated with conventional aerosol instrumentation during the 1996-1997 winter intensive monitoring period of the Northern Front Range Air Quality Study. Measurements of the light absorption efficiency for black carbon were 5 m2/g at 685 nm and 10 m2/g at 532 nm, and for elemental carbon, they were 3.6 m2/g at 685 nm. We show that these values together with previous photoacoustic measurements of aerosol light absorption shed some light on the wavelength dependence of absorption efficiency for carbonaceous aerosol in the visible and near-visible region. Integrating plate type filter measurements of aerosol light absorption result in far larger values than those measured with the photoacoustic instrument. We demonstrate that a recently published correction technique [Horvath, 1997] can yield improved agreement.

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

NASA Astrophysics Data System (ADS)

Vlachou, Athanasia; Daellenbach, Kaspar R.; Bozzetti, Carlo; Chazeau, Benjamin; Salazar, Gary A.; Szidat, Soenke; Jaffrezo, Jean-Luc; Hueglin, Christoph; Baltensperger, Urs; El Haddad, Imad; Prévôt, André S. H.

2018-05-01

Carbonaceous aerosols are related to adverse human health effects. Therefore, identification of their sources and analysis of their chemical composition is important. The offline AMS (aerosol mass spectrometer) technique offers quantitative separation of organic aerosol (OA) factors which can be related to major OA sources, either primary or secondary. While primary OA can be more clearly separated into sources, secondary (SOA) source apportionment is more challenging because different sources - anthropogenic or natural, fossil or non-fossil - can yield similar highly oxygenated mass spectra. Radiocarbon measurements provide unequivocal separation between fossil and non-fossil sources of carbon. Here we coupled these two offline methods and analysed the OA and organic carbon (OC) of different size fractions (particulate matter below 10 and 2.5 µm - PM10 and PM2.5, respectively) from the Alpine valley of Magadino (Switzerland) during the years 2013 and 2014 (219 samples). The combination of the techniques gave further insight into the characteristics of secondary OC (SOC) which was rather based on the type of SOC precursor and not on the volatility or the oxidation state of OC, as typically considered. Out of the primary sources separated in this study, biomass burning OC was the dominant one in winter, with average concentrations of 5.36 ± 2.64 µg m-3 for PM10 and 3.83 ± 1.81 µg m-3 for PM2.5, indicating that wood combustion particles were predominantly generated in the fine mode. The additional information from the size-segregated measurements revealed a primary sulfur-containing factor, mainly fossil, detected in the coarse size fraction and related to non-exhaust traffic emissions with a yearly average PM10 (PM2.5) concentration of 0.20 ± 0.24 µg m-3 (0.05 ± 0.04 µg m-3). A primary biological OC (PBOC) was also detected in the coarse mode peaking in spring and summer with a yearly average PM10 (PM2.5) concentration of 0.79 ± 0.31 µg m-3 (0.24 ± 0

Hygroscopicity and volatility of semi-volatile organic components in optical levitated single organic/inorganic aqueous aerosol droplet

NASA Astrophysics Data System (ADS)

Cai, C.; Zhao, C.

2017-12-01

Quantifying the gas/particle partitioning of organic compounds is of great significance to the understanding of atmospheric aerosol indirect effect. Accurate determination of the hygroscopicities and vapor pressures of semi-volatile organic compounds (SVOC) is of crucial importance in studying their partitioning behavior into atmospheric aerosol, as current published vapor pressures results of compounds of interest (usually with vapor pressures smaller than 0.01 Pa) vary by several orders of magnitude. On the other hand, influences on SVOCs evaporation from participation of inorganic species remains ambiguous. In this study we present quantitative investigation of hygroscopicities and volatilities of single aerosol droplets in an aerosol optical tweezers. The trapped droplet (3-7 µm radii) in the aerosol optical tweezers acts as a micro cavity, which stimulates the cavity enhanced Raman spectroscopy (CERS) signal. Size and composition of the particle are calculated from Mie fit to the positions of the "whispering gallery modes" in the CERS fingerprint. Hygroscopic behaviors and SVOC pure component vapor pressure can then be extracted from the correlation between the changing droplet radius and solute concentration (derived from experimentally determined RI real part). We will further present the influences between mass transfer on the gas-particle interface and within the droplet.

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

NASA Astrophysics Data System (ADS)

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

2007-12-01

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

Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles.

PubMed

China, Swarup; Mazzoleni, Claudio; Gorkowski, Kyle; Aiken, Allison C; Dubey, Manvendra K

2013-01-01

Biomass burning is one of the largest sources of carbonaceous aerosols in the atmosphere, significantly affecting earth's radiation budget and climate. Tar balls, abundant in biomass burning smoke, absorb sunlight and have highly variable optical properties, typically not accounted for in climate models. Here we analyse single biomass burning particles from the Las Conchas fire (New Mexico, 2011) using electron microscopy. We show that the relative abundance of tar balls (80%) is 10 times greater than soot particles (8%). We also report two distinct types of tar balls; one less oxidized than the other. Furthermore, the mixing of soot particles with other material affects their optical, chemical and physical properties. We quantify the morphology of soot particles and classify them into four categories: ~50% are embedded (heavily coated), ~34% are partly coated, ~12% have inclusions and~4% are bare. Inclusion of these observations should improve climate model performances.

Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements

NASA Technical Reports Server (NTRS)

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

2011-01-01

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

CARES Helps Explain Secondary Organic Aerosols

ScienceCinema

Zaveri, Rahul

2018-01-16

What happens when urban man-made pollution mixes with what we think of as pristine forest air? To know more about what this interaction means for the climate, the Carbonaceous Aerosol and Radiative Effects Study, or CARES, field campaign was designed in 2010. The sampling strategy during CARES was coordinated with CalNex 2010, another major field campaign that was planned in California in 2010 by the California Air Resources Board (CARB), the National Oceanic and Atmospheric Administration (NOAA), and the California Energy Commission (CEC). "We found two things. When urban pollution mixes with forest pollutions we get more secondary organic aerosols," said Rahul Zaveri, FCSD scientist and project lead on CARES. "SOAs are thought to be formed primarily from forest emissions but only when they interact with urban emissions. The data is saying that there will be climate cooling over the central California valley because of these interactions." Knowledge gained from detailed analyses of data gathered during the CARES campaign, together with laboratory experiments, is being used to improve existing climate models.

CARES Helps Explain Secondary Organic Aerosols

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

Zaveri, Rahul

2014-03-28

What happens when urban man-made pollution mixes with what we think of as pristine forest air? To know more about what this interaction means for the climate, the Carbonaceous Aerosol and Radiative Effects Study, or CARES, field campaign was designed in 2010. The sampling strategy during CARES was coordinated with CalNex 2010, another major field campaign that was planned in California in 2010 by the California Air Resources Board (CARB), the National Oceanic and Atmospheric Administration (NOAA), and the California Energy Commission (CEC). "We found two things. When urban pollution mixes with forest pollutions we get more secondary organic aerosols,"more » said Rahul Zaveri, FCSD scientist and project lead on CARES. "SOAs are thought to be formed primarily from forest emissions but only when they interact with urban emissions. The data is saying that there will be climate cooling over the central California valley because of these interactions." Knowledge gained from detailed analyses of data gathered during the CARES campaign, together with laboratory experiments, is being used to improve existing climate models.« less

Organic aerosol components derived from 25 AMS datasets across Europe using a newly developed ME-2 based source apportionment strategy

NASA Astrophysics Data System (ADS)

Crippa, M.; Canonaco, F.; Lanz, V. A.; Äijälä, M.; Allan, J. D.; Carbone, S.; Capes, G.; Dall'Osto, M.; Day, D. A.; DeCarlo, P. F.; Di Marco, C. F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J.-L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Mensah, A. A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S. N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

2013-09-01

Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of EUCAARI and the intensive campaigns of EMEP during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we propose a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 datasets accounting for urban, rural, remote and high altitude sites and therefore it is likely suitable for the treatment of AMS-related ambient datasets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling evaluation purposes.

Radiative Forcing Due to Major Aerosol Emitting Sectors in China and India

NASA Technical Reports Server (NTRS)

Streets, David G.; Shindell, Drew Todd; Lu, Zifeng; Faluvegi, Greg

2013-01-01

Understanding the radiative forcing caused by anthropogenic aerosol sources is essential for making effective emission control decisions to mitigate climate change. We examined the net direct plus indirect radiative forcing caused by carbonaceous aerosol and sulfur emissions in key sectors of China and India using the GISS-E2 chemistry-climate model. Diesel trucks and buses (67 mW/ sq. m) and residential biofuel combustion (52 mW/ sq. m) in India have the largest global mean, annual average forcings due mainly to the direct and indirect effects of BC. Emissions from these two sectors in China have near-zero net global forcings. Coal-fired power plants in both countries exert a negative forcing of about -30 mW/ sq. m from production of sulfate. Aerosol forcings are largest locally, with direct forcings due to residential biofuel combustion of 580 mW/ sq. m over India and 416 mW/ sq. m over China, but they extend as far as North America, Europe, and the Arctic

Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach

NASA Astrophysics Data System (ADS)

Crippa, M.; Canonaco, F.; Lanz, V. A.; Äijälä, M.; Allan, J. D.; Carbone, S.; Capes, G.; Ceburnis, D.; Dall'Osto, M.; Day, D. A.; DeCarlo, P. F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J. L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Laaksonen, A.; Mensah, A. A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S. N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

2014-06-01

Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.

Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

NASA Astrophysics Data System (ADS)

Xu, Lingling; Chen, Jinsheng

2016-04-01

Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

A dual origin for water in carbonaceous asteroids revealed by CM chondrites

NASA Astrophysics Data System (ADS)

Piani, Laurette; Yurimoto, Hisayoshi; Remusat, Laurent

2018-04-01

Carbonaceous asteroids represent the principal source of water in the inner Solar System and might correspond to the main contributors for the delivery of water to Earth. Hydrogen isotopes in water-bearing primitive meteorites, for example carbonaceous chondrites, constitute a unique tool for deciphering the sources of water reservoirs at the time of asteroid formation. However, fine-scale isotopic measurements are required to unravel the effects of parent-body processes on the pre-accretion isotopic distributions. Here, we report in situ micrometre-scale analyses of hydrogen isotopes in six CM-type carbonaceous chondrites, revealing a dominant deuterium-poor water component (δD = -350 ± 40‰) mixed with deuterium-rich organic matter. We suggest that this deuterium-poor water corresponds to a ubiquitous water reservoir in the inner protoplanetary disk. A deuterium-rich water signature has been preserved in the least altered part of the Paris chondrite (δDParis ≥ -69 ± 163‰) in hydrated phases possibly present in the CM rock before alteration. The presence of the deuterium-enriched water signature in Paris might indicate that transfers of ice from the outer to the inner Solar System were significant within the first million years of the history of the Solar System.

Bacterial Paleontology and Studies of Carbonaceous Chondrites

NASA Technical Reports Server (NTRS)

Gerasimenko, L. M.; Hoover, Richard B.; Rozanov, Alexei Y.; Zhegallo, E. A.; Zhmur, S. I.

1999-01-01

The study of the fossilization processes of modern cyanobacteria provides insights needed to recognize bacterial microfossils. The fossilization of cyanobacteria is discussed and images of recent and fossil bacteria and cyanobacteria from the Early Proterozoic to Neogene carbonaceous rocks (kerites, shungites, and black shales) and phosphorites are provided. These are compared with biomorphic microstructures and possible microfossils encountered in-situ in carbonaceous meteorites.

Method for co-processing waste rubber and carbonaceous material

DOEpatents

Farcasiu, Malvina; Smith, Charlene M.

1991-01-01

In a process for the co-processing of waste rubber and carbonaceous material to form a useful liquid product, the rubber and the carbonaceous material are combined and heated to the depolymerization temperature of the rubber in the presence of a source of hydrogen. The depolymerized rubber acts as a liquefying solvent for the carbonaceous material while a beneficial catalytic effect is obtained from the carbon black released on depolymerization the reinforced rubber. The reaction is carried out at liquefaction conditions of 380.degree.-600.degree. C. and 70-280 atmospheres hydrogen pressure. The resulting liquid is separated from residual solids and further processed such as by distillation or solvent extraction to provide a carbonaceous liquid useful for fuels and other purposes.

Method for generating methane from a carbonaceous feedstock

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

Snyder, Seth W.; Urgun-Demirtas, Meltem; Shen, Yanwen

The present invention provides a method for generating methane from a carbonaceous feedstock with simultaneous in situ sequestration of carbon dioxide to afford a biogas comprising at least 85 percent by volume methane, the method comprising anaerobically incubating a particulate additive in contact with a carbonaceous feedstock in a neutral or alkaline aqueous culture medium containing a culture of methanogenic consortia and collecting methane generated therefrom. The additive comprises at least one material selected from a biochar, an ash produced by gasification or combustion of a carbonaceous material, a black carbon soil, and a Terra Preta soil.

Progress and Understanding Spatial and Temporal Variability of PM2.5 and its Components in the Detroit Exposure and Aerosol Research Study (DEARS)

EPA Science Inventory

The Detroit Exposure and Aerosol Research Study (DEARS) measured personal exposures, ambient, residential indoor and residential outdoor concentrations of select PM_2.5 aerosol components (SO₄, NO₃, Fe, Si, Ca, K, Mn, Pb, Zn, EC and OC) over a thr...

Chemical Properties of Brown Carbon Aerosol Generated at the Missoula Fire Sciences Laboratory

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Womack, C.; Franchin, A.; Middlebrook, A. M.; Wagner, N.; Manfred, K.

2017-12-01

Aerosol scattering and absorption are still among the largest uncertainties in quantifying radiative forcing. Biomass burning is a major source of light-absorbing carbonaceous aerosol in the United States. These aerosol are generally classified into two categories: black carbon (graphitic-like aerosol that absorbs broadly across the ultraviolet and visible spectral regions) and brown carbon (organic aerosol that absorbs strongly in the ultraviolet and near-visible spectral regions). The composition, volatility, and chemical aging of brown carbon are poorly known, but are important to understanding its radiative effects. We deployed three novel instruments to the Missoula Fire Sciences Laboratory in 2016 to measure brown carbon absorption: a photoacoustic spectrometer, broadband cavity enhanced spectrometer, and particle-into-liquid sampler coupled to a liquid waveguide capillary cell. The instruments sampled from a shared inlet with well-characterized dilution and thermal denuding. We sampled smoke from 32 controlled burns of fuels relevant to western U.S. wildfires. We use these measurements to determine the volatility of water-soluble brown carbon, and compare this to the volatility of water-soluble organic aerosol and total organic aerosol. We further examine the wavelength-dependence of the water-soluble brown carbon absorption as a function of denuder temperature. Together this gives new information about the solubility, volatility, and chemical composition of brown carbon.

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

NASA Astrophysics Data System (ADS)

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

2008-12-01

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

The Carbonaceous - Non-Carbonaceous Chondrite Reservoir Dichotomy and the Challenge of Ureilites

NASA Astrophysics Data System (ADS)

Goodrich, C. A.

2017-08-01

Solar system materials are strongly divided into CC (carbonaceous chondrite) and NCC (non-CC) groups in terms of nucleosynthetic isotope anomalies. Ureilites are in the NCC group but seem to have had volatile-rich precursors. How could this be?

Carbonaceous Material in Extraterrestrial Matter

NASA Astrophysics Data System (ADS)

Martins, Zita

2015-08-01

Comets, asteroids and their fragments (i.e. meteorite, micrometeorites and interplanetary dust particles (IDPs)) are known to contain carbonaceous material. IDPs have ~10% of carbon by mass [1-3], while both micrometeorites and IDPs contain organic molecules. However, it is not certain whether these molecules are indigenous or terrestrial contamination [4-7]. On the other hand, ultra-carbonaceous Antarctic micrometeorites (UCAMMs) contain 50-80% of carbonaceous material, which is one of the highest organic matter contents detected in an extraterrestrial body [8]. Comets also have several extraterrestrial organic molecules [9, 10], including the simplest amino acid glycine [11]. In addition, the impact-shock of a typical comet ice mixture produces several amino acids from simple precursors [12]. Carbonaceous meteorites contain up to 5wt% of organic carbon [13], which is either locked in an insoluble kerogen-like polymer, or in a rich organic inventory of soluble organic compounds [14-16]. Bulk analysis of the meteoritic soluble organic fraction has revealed a high molecular diversity of tens of thousands of different molecular compositions [17]. The analysis of the carbonaceous content of comets, asteroids and their fragments provides a window into the resources delivered to the early Earth.[1] Brownlee (1985) Ann. Rev. Earth and Plan. Sci. 13, 147. [2] Schramm et al. (1989) Meteoritics 24, 99. [3] Messenger (2002) MAPS 37, 1491. [4] Clemett et al. (1993) Science 262, 721. [5] Brinton et al. (1998) OLEB 28, 413. [6] Flynn (2003) GCA 67, 4791. [7] Matrajt et al. (2004) MAPS 39, 1849. [8] Duprat et al. (2010) Science 328, 742-745. [9] Bockelée-Morvan et al. (2004) in: Comets II. pp. 391-423. [10] Mumma and Charnley (2011) ARAA 49, 471. [11] Elsila et al. (2009) MAPS 44, 1323. [12] Martins et al. (2013) Nature Geoscience 6, 1045. [13] Alexander et al. (2013) GCA 123, 244. [14] Cronin and Chang (1993) in: The Chemistry of Life’s Origin. pp. 209-258. [15] Cody and

The Biological Potency Of Carbonaceous Nanoparticles Is Associated With The State Of Oxidation Of Surface Carbon Atoms

EPA Science Inventory

Epidemiological studies have shown that exposure to ambient particulate matter (PM) is associated with excess morbidity and mortality. An important component of PM consists of inorganic and organic compounds adsorbed onto a carbonaceous particle core. Toxicological studies indica...

Nature, Origin, Potential Composition, and Climate Impact of the Asian Tropopause Aerosol Layer (ATAL)

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Thomason, L. W.; Natarajan, M.; Bedka, K.; Wienhold, F.; Bian J.; Martinsson, B.

2015-01-01

Satellite observations from SAGE II and CALIPSO indicate that summertime aerosol extinction has more than doubled in the Asian Tropopause Aerosol Layer (ATAL) since the late 1990s. Here we show remote and in-situ observations, together with results from a chemical transport model (CTM), to explore the likely composition, origin, and radiative forcing of the ATAL. We show in-situ balloon measurements of aerosol backscatter, which support the high levels observed by CALIPSO since 2006. We also show in situ measurements from aircraft, which indicate a predominant carbonaceous contribution to the ATAL (Carbon/Sulfur ratios of 2- 10), which is supported by the CTM results. We show that the peak in ATAL aerosol lags by 1 month the peak in CO from MLS, associated with deep convection over Asia during the summer monsoon. This suggests that secondary formation and growth of aerosols in the upper troposphere on monthly timescales make a significant contribution to ATAL. Back trajectory calculations initialized from CALIPSO observations provide evidence that deep convection over India is a significant source for ATAL through the vertical transport of pollution to the upper troposphere.

Size distributions of secondary and primary aerosols in Asia: A 3-D modeling

NASA Astrophysics Data System (ADS)

Yu, F.; Luo, G.; Wang, Z.

2009-12-01

Asian aerosols have received increasing attention because of their potential health and climate effects and the rapid increasing of Asian emissions associated with accelerating economic expansion. Aerosol particles appear in the atmosphere due to either in-situ nucleation (i.e, secondary particles) or direct emissions (i.e., primary particles), and their environmental impacts depend strongly on their concentrations, sizes, compositions, and mixing states. A size-resolved (sectional) particle microphysics model with a number of computationally efficient schemes has been incorporated into a global chemistry transport model (GEOS-Chem) to simulate the number size distributions of secondary and primary particles in the troposphere (Yu and Luo, Atmos. Chem. Phys. Discuss., 9, 10597-10645, 2009). The growth of nucleated particles through the condensation of sulfuric acid vapor and equilibrium uptake of nitrate, ammonium, and secondary organic aerosol is explicitly simulated, along with the coating of primary particles (dust, black carbon, organic carbon, and sea salt) by volatile components via condensation and coagulation with secondary particles. Here we look into the spatiotemporal variations of the size distributions of secondary and primary aerosols in Asia. The annual mean number concentration of the accumulation mode particles (dry diameter > ~ 100 nm) in the lower troposphere over Asia (especially China) is very high and is dominated (~70-90%) by carbonaceous primary particles (with coated condensable species). Coagulation and condensation turn the primary particles into mixed particles and on average increase the dry sizes of primary particles by a factor of ~ 2-2.5. Despite of high condensation sink, sulfuric acid vapor concentration in many parts of Asian low troposphere is very high (annual mean values above 1E7/cm3) and significant new particle formation still occurs. Secondary particles generally dominate the particles small than 100 nm and the equilibrium

Abodes for life in carbonaceous asteroids?

NASA Astrophysics Data System (ADS)

Abramov, Oleg; Mojzsis, Stephen J.

2011-05-01

Thermal evolution models for carbonaceous asteroids that use new data for permeability, pore volume, and water circulation as input parameters provide a window into what are arguably the earliest habitable environments in the Solar System. Plausible models of the Murchison meteorite (CM) parent body show that to first-order, conditions suitable for the stability of liquid water, and thus pre- or post-biotic chemistry, could have persisted within these asteroids for tens of Myr. In particular, our modeling results indicate that a 200-km carbonaceous asteroid with a 40% initial ice content takes almost 60 Myr to cool completely, with habitable temperatures being maintained for ˜24 Myr in the center. Yet, there are a number of indications that even with the requisite liquid water, thermal energy sources to drive chemical gradients, and abundant organic "building blocks" deemed necessary criteria for life, carbonaceous asteroids were intrinsically unfavorable sites for biopoesis. These controls include different degrees of exothermal mineral hydration reactions that boost internal warming but effectively remove liquid water from the system, rapid (1-10 mm yr -1) inward migration of internal habitable volumes in most models, and limitations imposed by low permeabilities and small pore sizes in primitive undifferentiated carbonaceous asteroids. Our results do not preclude the existence of habitable conditions on larger, possibly differentiated objects such as Ceres and the Themis family asteroids due to presumed longer, more intense heating and possible long-lived water reservoirs.

Staged heating by oxidation of carbonaceous material

DOEpatents

Knell, Everett W.; Green, Norman W.

1978-01-31

A carbonaceous material is pyrolyzed in the presence of a particulate source of heat obtained by the partial oxidation of a carbon containing solid residue of the carbonaceous material. The heat obtained from the oxidation of the carbon containing solid residue is maximized by preheating the carbon containing solid residue with a hot gas stream obtained by oxidizing the gaseous combustion products of the carbon containing solid residue.

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

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

Tar balls are processed, weakly absorbing, primary aerosol particles formed downwind of boreal forest fires

NASA Astrophysics Data System (ADS)

Sedlacek, A. J., III; Buseck, P. R.; Adachi, K.; Kleinman, L. I.; Onasch, T. B.; Springston, S. R.

2017-12-01

Biomass burning is a major source of light-absorbing black and brown carbonaceous aerosols Brown carbon is a poorly characterized mixture that includes tar balls (TBs), a type of carbonaceous particle unique to biomass burning. Here we describe the first atmospheric observations of the formation and evolution of TBs Aerosol particles were collected on TEM grids during individual aircraft transects at varying downwind distances from the Colockum Tarp wildland fire. The TEM images show primary particles transforming from viscous, impact-deformed particles to spherical TBs. The number fraction of TBs in the wildfire smoke plume increased from less than 5% in samples collected close to the emission source to greater than 40% after 3 hours of aging, with little change in downwind TB diameters. The TB mass fraction increased from 2% near the fire to 23±9% downwind. Single-scatter albedo determined from scattering and absorption measurements increased slightly with downwind distance. Mie calculations show this observation is consistent with weak light absorbance by TBs (m=1.56 - 0.02i) but not consistent with order-of-magnitude stronger absorption observed in different settings. The field-derived TB mass fractions reported here indicate that this particle type should be accounted for in biomass-burn emission inventories.

Constraining Carbonaceous Aerosol Sources in a Receptor Model Using Combined 14C, Redox Species, Organic Tracers, and Elementary/Organic Carbon Measurements

EPA Science Inventory

Sources of carbonaceous PM_2.5 were quantified in downtown Cleveland, OH and Chippewa Lake, OH located ~40 miles southwest of Cleveland during the Cleveland Multiple Air Pollutant Study (CMAPS). PM_2.5 filter samples were collected daily during July-August 200...

The aerosol optical properties and PM2.5 components over the world's largest industrial zone in Tangshan, North China

NASA Astrophysics Data System (ADS)

Zhang, Kequan; Ma, Yongjing; Xin, Jinyuan; Liu, Zirui; Ma, Yining; Gao, Dongdong; Wu, Junsong; Zhang, Wenyu; Wang, Yuesi; Shen, Pengke

2018-03-01

To achieve an in-depth understanding of the aerosol optical properties in the highly-industrial region of Tangshan, we provided systematic aerosol optical properties analysis in this largest industrial zone for the first time. The aerosol optical datasets (2013.05-2015.04) and chemical component data of PM2.5 (2014-2015) obtained from the Tangshan site of the campaign on atmospheric aerosol research (CARE-China) network were analyzed. The results showed that the Tangshan region was seriously affected by fine-mode industrial aerosols all year, which would promote the accumulation of pollutants and influence the atmospheric circulation through changing the vertical temperature gradient. The annual average aerosol optical depth (AOD) and Ångstrӧm exponent (α) were 0.80 ± 0.26 and 1.05 ± 0.10, respectively. The aerosol optical properties revealed significant seasonal characteristics. The maximum seasonal average AOD (1.03 ± 0.62) and α (1.12 ± 0.19) accompanied the highest seasonal secondary inorganic aerosol concentrations (SIA: SO42 -, NO3-, NH4+), 53.33 μg/m3, occurred in summer, and this phenomenon was attributed to the photochemical reactions favored by the high temperature and humidity. During the spring, frequent dust events led to the maximum Ca2 + concentration of 6.57 μg/m3 and the lowest seasonal α of 0.98 ± 0.31. Coal was used for generating heat in winter, resulting in the highest levels of pollutant emissions (Cl-, Elemental carbon (EC) and organic carbon (OC)). The aerosol type classifications showed that the industrial aerosols were the main controls in the summer and fall, representing 56%-58% of the total aerosols. While for spring and winter, mixed aerosols represented 53%-54% of the total aerosols. Hygroscopic growth effect of aerosols existed all year, which could enhance the negative radiative forcing and eventually cool the earth-atmosphere system. The classification Wing for Tangshan data showed high AOD values (> 0.70) were mainly

Process for hydrocracking carbonaceous material in liquid carrier

DOEpatents

Duncan, Dennis A.

1980-01-01

Solid carbonaceous material is hydrocracked to provide aliphatic and aromatic hydrocarbons for use as gaseous and liquid fuels or chemical feed stock. Particulate carbonaceous material such as coal in slurry with recycled product oil is preheated in liquid state to a temperature of 600.degree.-1200.degree. F. in the presence of hydrogen gas. The product oil acts as a sorbing agent for the agglomerating bitumins to minimize caking within the process. In the hydrocracking reactor, the slurry of oil and carbonaceous particles is heated within a tubular passageway to vaporize the oil and form a gas-solid mixture which is further heated to a hydropyrolysis temperature in excess of 1200.degree. F. The gas-solid mixture is quenched by contact with additional oil to condense normally liquid hydrocarbons for separation from the gases. A fraction of the hydrocarbon liquid product is recycled for quenching and slurrying with the carbonaceous feed. Hydrogen is recovered from the gas for recycle and additional hydrogen is produced by gasification of residual char.

simplified aerosol representations in global modeling

NASA Astrophysics Data System (ADS)

Kinne, Stefan; Peters, Karsten; Stevens, Bjorn; Rast, Sebastian; Schutgens, Nick; Stier, Philip

2015-04-01

The detailed treatment of aerosol in global modeling is complex and time-consuming. Thus simplified approaches are investigated, which prescribe 4D (space and time) distributions of aerosol optical properties and of aerosol microphysical properties. Aerosol optical properties are required to assess aerosol direct radiative effects and aerosol microphysical properties (in terms of their ability as aerosol nuclei to modify cloud droplet concentrations) are needed to address the indirect aerosol impact on cloud properties. Following the simplifying concept of the monthly gridded (1x1 lat/lon) aerosol climatology (MAC), new approaches are presented and evaluated against more detailed methods, including comparisons to detailed simulations with complex aerosol component modules.

Effect of Dust and Anthropogenic Aerosols on Columnar Aerosol Optical Properties over Darjeeling (2200 m asl), Eastern Himalayas, India

PubMed Central

Chatterjee, Abhijit; Ghosh, Sanjay K.; Adak, Anandamay; Singh, Ajay K.; Devara, Panuganti C. S.; Raha, Sibaji

2012-01-01

Background The loading of atmospheric particulate matter (aerosol) in the eastern Himalaya is mainly regulated by the locally generated anthropogenic aerosols from the biomass burning and by the aerosols transported from the distance sources. These different types of aerosol loading not only affect the aerosol chemistry but also produce consequent signature on the radiative properties of aerosol. Methodology/Principal Findings An extensive study has been made to study the seasonal variations in aerosol components of fine and coarse mode aerosols and black carbon along with the simultaneous measurements of aerosol optical depth on clear sky days over Darjeeling, a high altitude station (2200 masl) at eastern Himalayas during the year 2008. We observed a heavy loading of fine mode dust component (Ca2+) during pre-monsoon (Apr – May) which was higher by 162% than its annual mean whereas during winter (Dec – Feb), the loading of anthropogenic aerosol components mainly from biomass burning (fine mode SO4 2− and black carbon) were higher (76% for black carbon and 96% for fine mode SO4 2−) from their annual means. These high increases in dust aerosols during pre-monsoon and anthropogenic aerosols during winter enhanced the aerosol optical depth by 25 and 40%, respectively. We observed that for every 1% increase in anthropogenic aerosols, AOD increased by 0.55% during winter whereas for every 1% increase in dust aerosols, AOD increased by 0.46% during pre-monsoon. Conclusion/Significance The natural dust transport process (during pre-monsoon) plays as important a role in the radiation effects as the anthropogenic biomass burning (during winter) and their differential effects (rate of increase of the AOD with that of the aerosol concentration) are also very similar. This should be taken into account in proper modeling of the atmospheric environment over eastern Himalayas. PMID:22792264

Effect of dust and anthropogenic aerosols on columnar aerosol optical properties over Darjeeling (2200 m asl), eastern Himalayas, India.

PubMed

Chatterjee, Abhijit; Ghosh, Sanjay K; Adak, Anandamay; Singh, Ajay K; Devara, Panuganti C S; Raha, Sibaji

2012-01-01

The loading of atmospheric particulate matter (aerosol) in the eastern Himalaya is mainly regulated by the locally generated anthropogenic aerosols from the biomass burning and by the aerosols transported from the distance sources. These different types of aerosol loading not only affect the aerosol chemistry but also produce consequent signature on the radiative properties of aerosol. An extensive study has been made to study the seasonal variations in aerosol components of fine and coarse mode aerosols and black carbon along with the simultaneous measurements of aerosol optical depth on clear sky days over Darjeeling, a high altitude station (2200 masl) at eastern Himalayas during the year 2008. We observed a heavy loading of fine mode dust component (Ca(2+)) during pre-monsoon (Apr-May) which was higher by 162% than its annual mean whereas during winter (Dec-Feb), the loading of anthropogenic aerosol components mainly from biomass burning (fine mode SO(4)(2-) and black carbon) were higher (76% for black carbon and 96% for fine mode SO(4)(2-)) from their annual means. These high increases in dust aerosols during pre-monsoon and anthropogenic aerosols during winter enhanced the aerosol optical depth by 25 and 40%, respectively. We observed that for every 1% increase in anthropogenic aerosols, AOD increased by 0.55% during winter whereas for every 1% increase in dust aerosols, AOD increased by 0.46% during pre-monsoon. The natural dust transport process (during pre-monsoon) plays as important a role in the radiation effects as the anthropogenic biomass burning (during winter) and their differential effects (rate of increase of the AOD with that of the aerosol concentration) are also very similar. This should be taken into account in proper modeling of the atmospheric environment over eastern Himalayas.

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

Retrieval of Aerosol Optical Depth Above Clouds from OMI Observations: Sensitivity Analysis, Case Studies

NASA Technical Reports Server (NTRS)

Torres, O.; Jethva, H.; Bhartia, P. K.

2012-01-01

A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originated in arid and semi-arid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth atmosphere system is especially important. The generally negative (cooling) top of the atmosphere direct effect of absorbing aerosols, may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. In this paper we discuss the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol-cloud separation. The technique was applied to above-cloud aerosol events over the Southern Atlantic Ocean yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.

Petrology of Amoeboid Olivine Aggregates in Antarctic CR Chondrites: Comparison With Other Carbonaceous Chondrites

NASA Technical Reports Server (NTRS)

Komatsu, M.; Fagan, T. J.; Yamaguchi, A.; Mikouchi, T.; Zolensky, M. E.; Yasutake, M.

2016-01-01

Amoeboid olivine aggregates (AOAs) are important refractory components of carbonaceous chondrites and have been interpreted to represent solar nebular condensates that experienced high-temperature annealing, but largely escaped melting. In addition, because AOAs in primitive chondrites are composed of fine-grained minerals (forsterite, anorthite, spinel) that are easily modified during post crystallization alteration, the mineralogy of AOAs can be used as a sensitive indicator of metamorphic or alteration processes. AOAs in CR chondrites are particularly important because they show little evidence for secondary alteration. In addition, some CR AOAs contain Mn-enriched forsterite (aka low-iron, Mn-enriched or LIME olivine), which is an indicator of nebular formation conditions. Here we report preliminary results of the mineralogy and petrology of AOAs in Antarctic CR chondrites, and compare them to those in other carbonaceous chondrites.

Occurrence and possible significance of rare Ti oxides (Magneli phases) in carbonaceous chondrite matrices

NASA Technical Reports Server (NTRS)

Brearley, Adrian J.

1993-01-01

Rare, ultrafine-grained Ti oxides (Ti3O5 and the Magneli phases, Ti5O9 and Ti8O15) have been identified by TEM in the CM2 carbonaceous chondrite, Bells, and a carbonaceous chondrite matrix clast from the Nilpena polymict ureilite. In both meteorites the Ti oxides occur in the matrix as isolated grains and clusters of two or more grains. They are euhedral in shape and have grain sizes of 0.05-0.3 micron. Magneli phases have been recently shown to be a common component in some interplanetary dust particles, but this is the first reported occurrence in a meteorite. The morphological properties and grain size of the Ti oxides are consistent with formation by vapor phase condensation either within the solar nebula or possibly in a presolar environment.

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.

Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers

NASA Astrophysics Data System (ADS)

Liu, Junwen; Li, Jun; Liu, Di; Ding, Ping; Shen, Chengde; Mo, Yangzhi; Wang, Xinming; Luo, Chunling; Cheng, Zhineng; Szidat, Sönke; Zhang, Yanlin; Chen, Yingjun; Zhang, Gan

2016-03-01

Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities in China, yet few studies simultaneously focus on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers

NASA Astrophysics Data System (ADS)

Liu, J.; Li, J.; Liu, D.; Ding, P.; Shen, C.; Mo, Y.; Wang, X.; Luo, C.; Cheng, Z.; Szidat, S.; Zhang, Y.; Chen, Y.; Zhang, G.

2015-12-01

Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities of China, yet seldom study simultaneously focuses on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), respectively, using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 % in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 % in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

Sources of primary and secondary organic aerosol and their diurnal variations.

PubMed

Zheng, Mei; Zhao, Xiuying; Cheng, Yuan; Yan, Caiqing; Shi, Wenyan; Zhang, Xiaolu; Weber, Rodney J; Schauer, James J; Wang, Xinming; Edgerton, Eric S

2014-01-15

PM(2.5), as one of the criteria pollutants regulated in the U.S. and other countries due to its adverse health impacts, contains more than hundreds of organic pollutants with different sources and formation mechanisms. Daytime and nighttime PM2.5 samples from the August Mini-Intensive Gas and Aerosol Campaign (AMIGAS) in the southeastern U.S. were collected during summer 2008 at one urban site and one rural site, and were analyzed for organic carbon (OC), elemental carbon (EC), water soluble organic carbon (WSOC), and various individual organic compounds including some important tracers for carbonaceous aerosol sources by gas chromatography-mass spectrometry. Most samples exhibited higher daytime OC concentration, while higher nighttime OC was found in a few events at the urban site. Sources, formation mechanisms and composition of organic aerosol are complicated and results of this study showed that it exhibited distinct diurnal variations. With detailed organic tracer information, sources contributing to particulate OC were identified: higher nighttime OC concentration occurring in several occasions was mainly contributed by the increasing primary emissions at night, especially diesel exhaust and biomass burning; whereas sources responsible for higher daytime OC concentration included secondary organic aerosol (SOA) formation (e.g., cis-pinonic acid and non-biomass burning WSOC) together with traffic emissions especially gasoline engine exhaust. Primary tracers from combustion related sources such as EC, polycyclic aromatic hydrocarbons, and hopanes and steranes were significantly higher at the urban site with an urban to rural ratio between 5 and 8. However, this urban-rural difference for secondary components was less significant, indicating a relatively homogeneous distribution of SOA spatially. We found cholesterol concentrations, a typical tracer for meat cooking, were consistently higher at the rural site especially during the daytime, suggesting the likely

Steady increase of secondary organic aerosol mass concentration and light extinction during the CARES 2010 Field Campaign

NASA Astrophysics Data System (ADS)

Gyawali, M. S.; Arnott, W. P.; Flowers, B. A.; Dubey, M. K.; Atkinson, D. B.; Song, C.; Zaveri, R. A.; Setyan, A.; Zhang, Q.; Mazzoleni, C.; Gorkowski, K.

2011-12-01

We present multispectral (355, 375, 405, 532, 870, 781, and 1047 nm) aerosol light absorption and scattering measurements for the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) campaign in Sacramento, CA and the Sierra Nevada foothills. The short wavelength scattering at both sites gradually increased during the last 10 days of the campaign as diagnosed by a systematic increase in the Ångström exponent of scattering. The UV and near UV enhanced scattering was likely a consequence of the ultra and sub-micron aerosol which began to grow vigorously in the size range where scattering at shorter wavelengths begins to increase. Multispectral aerosol light absorption coefficients suggest the absence of short wavelength light absorption by brown carbon. Aerosol mass spectrometer data also shows the steady increase of secondary organic aerosol during the last 10 days of CARES. The time series of the measurements made between the two sites (T0 and T1) separated by the slope of the foothills are strikingly similar, except for isolated night time episodes of enhanced absorption at T0. This is possibly due to paving events or other nocturnal emissions markers

Aerosol retrieval experiments in the ESA Aerosol_cci project

NASA Astrophysics Data System (ADS)

Holzer-Popp, T.; de Leeuw, G.; Martynenko, D.; Klüser, L.; Bevan, S.; Davies, W.; Ducos, F.; Deuzé, J. L.; Graigner, R. G.; Heckel, A.; von Hoyningen-Hüne, W.; Kolmonen, P.; Litvinov, P.; North, P.; Poulsen, C. A.; Ramon, D.; Siddans, R.; Sogacheva, L.; Tanre, D.; Thomas, G. E.; Vountas, M.; Descloitres, J.; Griesfeller, J.; Kinne, S.; Schulz, M.; Pinnock, S.

2013-03-01

Within the ESA Climate Change Initiative (CCI) project Aerosol_cci (2010-2013) algorithms for the production of long-term total column aerosol optical depth (AOD) datasets from European Earth Observation sensors are developed. Starting with eight existing pre-cursor algorithms three analysis steps are conducted to improve and qualify the algorithms: (1) a series of experiments applied to one month of global data to understand several major sensitivities to assumptions needed due to the ill-posed nature of the underlying inversion problem, (2) a round robin exercise of "best" versions of each of these algorithms (defined using the step 1 outcome) applied to four months of global data to identify mature algorithms, and (3) a comprehensive validation exercise applied to one complete year of global data produced by the algorithms selected as mature based on the round robin exercise. The algorithms tested included four using AATSR, three using MERIS and one using PARASOL. This paper summarizes the first step. Three experiments were conducted to assess the potential impact of major assumptions in the various aerosol retrieval algorithms. In the first experiment a common set of four aerosol components was used to provide all algorithms with the same assumptions. The second experiment introduced an aerosol property climatology, derived from a combination of model and sun photometer observations, as a priori information in the retrievals on the occurrence of the common aerosol components and their mixing ratios. The third experiment assessed the impact of using a common nadir cloud mask for AATSR and MERIS algorithms in order to characterize the sensitivity to remaining cloud contamination in the retrievals against the baseline dataset versions. The impact of the algorithm changes was assessed for one month (September 2008) of data qualitatively by visible analysis of monthly mean AOD maps and quantitatively by comparing global daily gridded satellite data against daily

New Evidence for the Presence of Indigenous Microfossils in Carbonaceous Chondrites

NASA Technical Reports Server (NTRS)

Hoover, Richard B.; Rozanov, Alexei Yu.

2004-01-01

We present additional evidence for the presence of indigenous microfossils in carbonaceous meteorites scanning electron micrograph studies of freshly fractured interior surfaces of pristine samples of the Murchison CM2 carbonaceous meteorite have revealed forms in-situ that are recognizable as biofilms as well as complex and highly structured forms similar to calcareous and siliceous microfossils. Some of the forms encountered are very well-preserved and exhibit complex associated microstructures similar to bacterial flagella. New images will be presented of forms recently encountered in carbonaceous meteorites and they will be compared with those of known microbial extremophiles. KEYWORDS: carbonaceous chondrites, Murchison, microfossils, extremophiles

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

NASA Astrophysics Data System (ADS)

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

2014-05-01

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

Optical Properties of Black and Brown Carbon Aerosols from Laboratory Combustion of Wildland Fuels

NASA Astrophysics Data System (ADS)

Beres, N. D.; Molzan, J.

2015-12-01

Aerosol light absorption in the solar spectral region (300 nm - 2300 nm) of the atmosphere is key for the direct aerosol radiative forcing, which is determined by aerosol single scattering albedo (SSA), asymmetry parameter, and by the albedo of the underlying surface. SSA is of key importance for the sign and quantity of aerosol direct radiative forcing; that is, does the aerosol make the earth look darker (heating) or whiter (cooling)? In addition, these optical properties are needed for satellite retrievals of aerosol optical depth and properties. During wildland fires, aerosol optical absorption is largely determined by black carbon (BC) and brown carbon (BrC) emissions. BC is strongly absorbing throughout the solar spectrum, while BrC absorption strongly increases toward shorter wavelength and can be neglected in the red and infrared. Optical properties of BrC emitted from wildland fires are poorly understood and need to be studied as function of fuel type and moisture content and combustion conditions. While much more is known about BC optical properties, knowledge for the ultraviolet (UV) spectral region is still lacking and critically needed for satellite remote sensing (e.g., TOMS, OMI) and for modeling of tropospheric photochemistry. Here, a project to better characterize biomass burning aerosol optical properties is described. It utilizes a laboratory biomass combustion chamber to generate aerosols through combustion of different wildland fuels of global and regional importance. Combustion aerosol optics is characterized with an integrating nephelometer to measure aerosol light scattering and a photoacoustic instrument to measure aerosol light absorption. These measurements will yield optical properties that are needed to improve qualitative and quantitative understanding of aerosol radiative forcing and satellite retrievals for absorbing carbonaceous aerosols from combustion of wildland fuels.

Seasonality of major aerosol species and their transformations in Cairo megacity

NASA Astrophysics Data System (ADS)

Favez, Olivier; Cachier, Hélène; Sciare, Jean; Alfaro, Stéphane C.; El-Araby, Tarek M.; Harhash, Maha A.; Abdelwahab, Magdy M.

Bulk aerosols sampled on a weekly basis at two Cairo (Egypt) urban sites from January 2003 to May 2006 were analysed for their chemical composition of major aerosol species (elemental carbon, water soluble/insoluble organic carbon, nitrate, sulphate, ammonium, chloride, sodium and calcium). Data subsequently obtained constitute one of the longest and more detailed dataset related to Cairo aerosols, and offer the opportunity to investigate seasonal trends. Dust aerosols (derived from calcium measurements) displayed maximum concentrations in spring and winter, due to frequent dust storms, but also high background concentration levels (˜50 μg m -3) all year long. Within these particles, about 40% on average of Ca 2+ was found to be associated with SO 42-, NO 3- and/or Cl -, pointing out "dust anthropization" processes and their subsequent climatic impact on a regional scale. Seasonal variations of non-dust aerosols, equally distributed between carbonaceous aerosols and ions, were also observed, with concentrations of the order of 100 μg m -3 in autumn and winter, and of 60 μg m -3 in spring and summer. High concentration levels of non-sea-salt chloride (up to 15 μg m -3 on a monthly basis), likely of industrial origin, were observed in autumn and winter. During the autumn "Black Cloud" event, biomass burning aerosols originating from rice straw burning in the Nile Delta have shown to account for 12%, 35% and 50% of Cairo EC, WIOC and WSOC mass concentrations, respectively. Finally, relatively low WSOC/OC ratios (˜1/3) were obtained all the year long, calling for more investigation on the water-solubility of organic aerosols originating from the burning of agricultural waste, and on that of secondary organic aerosols formed in dry urban atmospheres.

Extraterrestrial Nucleobases in Carbonaceous Chondrites

NASA Astrophysics Data System (ADS)

Martins, Z.; Botta, O.; Fogel, M.; Sephton, M.; Glavin, D.; Watson, J.; Dworkin, J.; Schwartz, A.; Ehrenfreund, P.

Nucleobases in Carbonaceous Chondrites Z. Martins (1), O. Botta (2), M. L. Fogel (3), M. A. Sephton (4), D. P. Glavin (2), J. S. Watson (5), J. P. Dworkin (2), A. W. Schwartz (6) and P. Ehrenfreund (1,6). (1) Astrobiology Laboratory, Leiden Institute of Chemistry, Leiden, The Netherlands, (2) NASA Goddard Space Flight Center, Goddard Center for Astrobiology, Greenbelt, MD, USA, (3) GL, Carnegie Institution of Washington, Washington DC, USA, (4) Impacts and Astromaterials Research Centre, Department of Earth Science and Engineering, South Kensington Campus, Imperial College, London, UK, (5) Planetary and Space Sciences Research Institute, The Open University, Walton Hall, Milton Keynes, UK, (6) Radboud University Nijmegen, Nijmegen, The Netherlands. E-mail: z.martins@chem.leidenuniv.nl/Phone:+31715274440 Nucleobases are crucial compounds in terrestrial biochemistry, because they are key components of DNA and RNA. Carbonaceous meteorites have been analyzed for nucleobases by different research groups [1-5]. However, significant quantitative and qualitative differences were observed, leading to the controversial about the origin of these nucleobases. In order to establish the origin of these compounds in carbonaceous chondrites and to assess the plausibility of their exogenous delivery to the early Earth, we have performed formic acid extraction of samples of the Murchison meteorite [6], followed by an extensive purification procedure, analysis and quantification by high-performance liquid chromatography with UV absorption detection and gas chromatography-mass spectrometry. Our results were qualitatively consistent with previous results [3, 4], but showed significant quantitative differences. Compound specific carbon isotope values were obtained, using gas chromatography-combustion- isotope ratio mass spectrometry. A soil sample collected in the proximity of the Murchison meteorite fall site was subjected to the same extraction, purification and analysis procedure

Process for gasifying carbonaceous material from a recycled condensate slurry

DOEpatents

Forney, Albert J.; Haynes, William P.

1981-01-01

Coal or other carbonaceous material is gasified by reaction with steam and oxygen in a manner to minimize the problems of effluent water stream disposal. The condensate water from the product gas is recycled to slurry the coal feed and the amount of additional water or steam added for cooling or heating is minimized and preferably kept to a level of about that required to react with the carbonaceous material in the gasification reaction. The gasification is performed in a pressurized fluidized bed with the coal fed in a water slurry and preheated or vaporized by indirect heat exchange contact with product gas and recycled steam. The carbonaceous material is conveyed in a gas-solid mixture from bottom to top of the pressurized fluidized bed gasifier with the solids removed from the product gas and recycled steam in a supported moving bed filter of the resulting carbonaceous char. Steam is condensed from the product gas and the condensate recycled to form a slurry with the feed coal carbonaceous particles.

Evaluation of applicability of high-resolution multiangle imaging photo-polarimetric observations for aerosol atmospheric correction

NASA Astrophysics Data System (ADS)

Kalashnikova, Olga; Garay, Michael; Xu, Feng; Diner, David; Seidel, Felix

2016-07-01

Multiangle spectro-polarimetric measurements have been advocated as an additional tool for better understanding and quantifying the aerosol properties needed for atmospheric correction for ocean color retrievals. The central concern of this work is the assessment of the effects of absorbing aerosol properties on remote sensing reflectance measurement uncertainty caused by neglecting UV-enhanced absorption of carbonaceous particles and by not accounting for dust nonsphericity. In addition, we evaluate the polarimetric sensitivity of absorbing aerosol properties in light of measurement uncertainties achievable for the next generation of multi-angle polarimetric imaging instruments, and demonstrate advantages and disadvantages of wavelength selection in the UV/VNIR range. In this work a vector Markov Chain radiative transfer code including bio-optical models was used to quantitatively evaluate in water leaving radiances between atmospheres containing realistic UV-enhanced and non-spherical aerosols and the SEADAS carbonaceous and dust-like aerosol models. The phase matrices for the spherical smoke particles were calculated using a standard Mie code, while those for non-spherical dust particles were calculated using the numerical approach developed for modeling dust for the AERONET network of ground-based sunphotometers. As a next step, we have developed a retrieval code that employs a coupled Markov Chain (MC) and adding/doubling radiative transfer method for joint retrieval of aerosol properties and water leaving radiance from Airborne Multiangle SpectroPolarimetric Imager-1 (AirMSPI-1) polarimetric observations. The AirMSPI-1 instrument has been flying aboard the NASA ER-2 high altitude aircraft since October 2010. AirMSPI typically acquires observations of a target area at 9 view angles between ±67° at 10 m resolution. AirMSPI spectral channels are centered at 355, 380, 445, 470, 555, 660, and 865 nm, with 470, 660, and 865 reporting linear polarization. We

High Contributions of Secondary Inorganic Aerosols to PM2.5 under Polluted Levels at a Regional Station in Northern China.

PubMed

Li, Yang; Tao, Jun; Zhang, Leiming; Jia, Xiaofang; Wu, Yunfei

2016-12-15

Daily PM 2.5 samples were collected at Shangdianzi (SDZ) regional site in Beijing-Tianjin-Hebei (BTH) region in 2015. Samples were subject to chemical analysis for organic carbon (OC), elemental carbon (EC), and major water-soluble inorganic ions. The annual average PM 2.5 mass concentration was 53 ± 36 μg·m -3 with the highest seasonal average concentration in spring and the lowest in summer. Water-soluble inorganic ions and carbonaceous aerosols accounted for 34% ± 15% and 33% ± 9%, respectively, of PM 2.5 mass on annual average. The excellent, good, lightly polluted, moderately polluted, and heavily polluted days based on the Air Quality Index (AQI) of PM 2.5 accounted for 40%, 42%, 11%, 4%, and 3%, respectively, of the year. The sum of the average concentration of sulfate, nitrate, and ammonium (SNA) increased from 4.2 ± 2.9 μg·m -3 during excellent days to 85.9 ± 22.4 μg·m -3 during heavily polluted days, and their contributions to PM 2.5 increased from 15% ± 8% to 49% ± 10% accordingly. In contrast, the average concentration of carbonaceous aerosols increased from 9.2 ± 2.8 μg·m -3 to 51.2 ± 14.1 μg·m -3 , and their contributions to PM 2.5 decreased from 34% ± 6% to 29% ± 7%. Potential source contribution function (PSCF) analysis revealed that the major sources for high PM 2.5 and its dominant chemical components were within the area mainly covering Shandong, Henan, and Hebei provinces. Regional pollutant transport from Shanxi province and Inner Mongolia autonomous region located in the west direction of SDZ was also important during the heating season.

High Contributions of Secondary Inorganic Aerosols to PM2.5 under Polluted Levels at a Regional Station in Northern China

PubMed Central

Li, Yang; Tao, Jun; Zhang, Leiming; Jia, Xiaofang; Wu, Yunfei

2016-01-01

Daily PM2.5 samples were collected at Shangdianzi (SDZ) regional site in Beijing–Tianjin–Hebei (BTH) region in 2015. Samples were subject to chemical analysis for organic carbon (OC), elemental carbon (EC), and major water-soluble inorganic ions. The annual average PM2.5 mass concentration was 53 ± 36 μg·m−3 with the highest seasonal average concentration in spring and the lowest in summer. Water-soluble inorganic ions and carbonaceous aerosols accounted for 34% ± 15% and 33% ± 9%, respectively, of PM2.5 mass on annual average. The excellent, good, lightly polluted, moderately polluted, and heavily polluted days based on the Air Quality Index (AQI) of PM2.5 accounted for 40%, 42%, 11%, 4%, and 3%, respectively, of the year. The sum of the average concentration of sulfate, nitrate, and ammonium (SNA) increased from 4.2 ± 2.9 μg·m−3 during excellent days to 85.9 ± 22.4 μg·m−3 during heavily polluted days, and their contributions to PM2.5 increased from 15% ± 8% to 49% ± 10% accordingly. In contrast, the average concentration of carbonaceous aerosols increased from 9.2 ± 2.8 μg·m−3 to 51.2 ± 14.1 μg·m−3, and their contributions to PM2.5 decreased from 34% ± 6% to 29% ± 7%. Potential source contribution function (PSCF) analysis revealed that the major sources for high PM2.5 and its dominant chemical components were within the area mainly covering Shandong, Henan, and Hebei provinces. Regional pollutant transport from Shanxi province and Inner Mongolia autonomous region located in the west direction of SDZ was also important during the heating season. PMID:27983711

What is the "Clim-Likely" aerosol product?

Atmospheric Science Data Center

2014-12-08

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

Catalyst for hydrotreating carbonaceous liquids

DOEpatents

Berg, Lloyd; McCandless, Frank P.; Ramer, Ronald J.

1982-01-01

A catalyst for denitrogenating and desulfurating carbonaceous liquid such as solvent refined coal includes catalytic metal oxides impregnated within a porous base of mostly alumina with relatively large pore diameters, surface area and pore volume. The base material includes pore volumes of 0.7-0.85 ml/g, surface areas of 200-350 m.sup.2 /g and pore diameters of 85-200 Angstroms. The catalytic metals impregnated into these base materials include the oxides of Group VI metals, molybdenum and tungsten, and the oxides of Group VIII metals, nickel and cobalt, in various combinations. These catalysts and bases in combination have effectively promoted the removal of chemically combined sulfur and nitrogen within a continuous flowing mixture of carbonaceous liquid and hydrogen gas.

Spectral parameters for Dawn FC color data: Carbonaceous chondrites and aqueous alteration products as potential cerean analog materials

NASA Astrophysics Data System (ADS)

Schäfer, Tanja; Nathues, Andreas; Mengel, Kurt; Izawa, Matthew R. M.; Cloutis, Edward A.; Schäfer, Michael; Hoffmann, Martin

2016-02-01

We identified a set of spectral parameters based on Dawn Framing Camera (FC) bandpasses, covering the wavelength range 0.4-1.0 μm, for mineralogical mapping of potential chondritic material and aqueous alteration products on dwarf planet Ceres. Our parameters are inferred from laboratory spectra of well-described and clearly classified carbonaceous chondrites representative for a dark component. We additionally investigated the FC signatures of candidate bright materials including carbonates, sulfates and hydroxide (brucite), which can possibly be exposed on the cerean surface by impact craters or plume activity. Several materials mineralogically related to carbonaceous chondrites, including pure ferromagnesian phyllosilicates, and serpentinites were also investigated. We tested the potential of the derived FC parameters for distinguishing between different carbonaceous chondritic materials, and between other plausible cerean surface materials. We found that the major carbonaceous chondrite groups (CM, CO, CV, CK, and CR) are distinguishable using the FC filter ratios 0.56/0.44 μm and 0.83/0.97 μm. The absorption bands of Fe-bearing phyllosilicates at 0.7 and 0.9 μm in terrestrial samples and CM carbonaceous chondrites can be detected by a combination of FC band parameters using the filters at 0.65, 0.75, 0.83, 0.92 and 0.97 μm. This set of parameters serves as a basis to identify and distinguish different lithologies on the cerean surface by FC multispectral data.

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.

Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility

NASA Astrophysics Data System (ADS)

Zappoli, S.; Andracchio, A.; Fuzzi, S.; Facchini, M. C.; Gelencsér, A.; Kiss, G.; Krivácsy, Z.; Molnár, Á.; Mészáros, E.; Hansson, H.-C.; Rosman, K.; Zebühr, Y.

A chemical mass balance of fine aerosol (<1.5 μm AED) collected at three European sites was performed with reference to the water solubility of the different aerosol classes of components. The sampling sites are characterised by different pollution conditions and aerosol loading in the air. Aspvreten is a background site in central Sweden, K-puszta is a rural site in the Great Hungarian Plain and San Pietro Capofiume is located in the polluted Po Valley, northern Italy. The average fine aerosol mass concentration was 5.9 μg m -3 at the background site Aspvreten, 24 μg m -3 at the rural K-puszta and 38 μg m -3 at the polluted site San Pietro Capofiume. However, a similarly high soluble fraction of the aerosol (65-75%) was measured at the three sites, while the percentage of water soluble organic species with respect to the total soluble mass was much higher at the background site (ca. 50%) than at the other two sites (ca. 25%). A very high fraction (over 70%) of organic compounds in the aerosol consisted of polar species. The presence of water soluble macromolecular compounds was revealed in the samples from K-puszta and San Pietro Capofiume. At both sites these species accounted for between ca. 20-50% of the water soluble organic fraction. The origin of the compounds was tentatively attributed to biomass combustion.

Aerosol typing - key information from aerosol studies

NASA Astrophysics Data System (ADS)

Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

2016-04-01

Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

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

NASA Astrophysics Data System (ADS)

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

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

CONTINUOUS BLACK CARBON MEASUREMENTS INDOORS AND OUTDOORS AT AN OCCUPIED HOUSE FOR ONE YEAR

EPA Science Inventory

Black carbon is one of the components of particulate matter, and is of importance because the only known source of aerosol black carbon in the atmosphere is the combustion of carbonaceous fuels (Hansen, 1997). Polyaromatic hydrocarbons (PAH) formed in the combustion process ar...

Reactor and method for hydrocracking carbonaceous material

DOEpatents

Duncan, Dennis A.; Beeson, Justin L.; Oberle, R. Donald; Dirksen, Henry A.

1980-01-01

Solid, carbonaceous material is cracked in the presence of hydrogen or other reducing gas to provide aliphatic and aromatic hydrocarbons of lower molecular weight for gaseous and liquid fuels. The carbonaceous material, such as coal, is entrained as finely divided particles in a flow of reducing gas and preheated to near the decomposition temperature of the high molecular weight polymers. Within the reactor, small quantities of oxygen containing gas are injected at a plurality of discrete points to burn corresponding amounts of the hydrogen or other fuel and elevate the mixture to high temperatures sufficient to decompose the high molecular weight, carbonaceous solids. Turbulent mixing at each injection point rapidly quenches the material to a more moderate bulk temperature. Additional quenching after the final injection point can be performed by direct contact with quench gas or oil. The reactions are carried out in the presence of a hydrogen-containing reducing gas at moderate to high pressure which stabilizes the products.

Origin and abundance of water in carbonaceous asteroids

NASA Astrophysics Data System (ADS)

Marrocchi, Yves; Bekaert, David V.; Piani, Laurette

2018-01-01

The origin and abundance of water accreted by carbonaceous asteroids remains underconstrained, but would provide important information on the dynamic of the protoplanetary disk. Here we report the in situ oxygen isotopic compositions of aqueously formed fayalite grains in the Kaba and Mokoia CV chondrites. CV chondrite bulk, matrix and fayalite O-isotopic compositions define the mass-independent continuous trend (δ17O = 0.84 ± 0.03 × δ18O - 4.25 ± 0.1), which shows that the main process controlling the O-isotopic composition of the CV chondrite parent body is related to isotopic exchange between 16O-rich anhydrous silicates and 17O- and 18O-rich fluid. Similar isotopic behaviors observed in CM, CR and CO chondrites demonstrate the ubiquitous nature of O-isotopic exchange as the main physical process in establishing the O-isotopic features of carbonaceous chondrites, regardless of their alteration degree. Based on these results, we developed a new approach to estimate the abundance of water accreted by carbonaceous chondrites (quantified by the water/rock ratio) with CM (0.3-0.4) ≥ CR (0.1-0.4) ≥ CV (0.1-0.2) > CO (0.01-0.10). The low water/rock ratios and the O-isotopic characteristics of secondary minerals in carbonaceous chondrites indicate they (i) formed in the main asteroid belt and (ii) accreted a locally derived (inner Solar System) water formed near the snowline by condensation from the gas phase. Such results imply low influx of D- and 17O- and 18O-rich water ice grains from the outer part of the Solar System. The latter is likely due to the presence of a Jupiter-induced gap in the protoplanetary disk that limited the inward drift of outer Solar System material at the exception of particles with size lower than 150 μm such as presolar grains. Among carbonaceous chondrites, CV chondrites show O-isotopic features suggesting potential contribution of 17-18O-rich water that may be related to their older accretion relative to other hydrated

Wet, Carbonaceous Asteroids: Altering Minerals, Changing Amino Acids

NASA Astrophysics Data System (ADS)

Taylor, G. J.

2011-04-01

Many carbonaceous chondrites contain alteration products from water-rock interactions at low temperature and organic compounds. A fascinating fact known for decades is the presence in some of them of an assortment of organic compounds, including amino acids, sometimes called the building blocks of life. Murchison and other CM carbonaceous chondrites contain hundreds of amino acids. Early measurements indicated that the amino acids in carbonaceous chondrites had equal proportions of L- and D-structures, a situation called racemic. This was in sharp contrast to life on Earth, which heavily favors L- forms. However, beginning in 1997, John Cronin and Sandra Pizzarello (Arizona State University) found L- excesses in isovaline and several other amino acids in the Murchison carbonaceous chondrite. In 2009, Daniel Glavin and Jason Dworkin (Astrobiology Analytical Lab, Goddard Space Flight Center) reported the first independent confirmation of L-isovaline excesses in Murchison using a different analytical technique than employed by Cronin and Pizzarello. Inspired by this work, Daniel Glavin, Michael Callahan, Jason Dworkin, and Jamie Elsila (Astrobiology Analytical Lab, Goddard Space Flight Center), have done an extensive study of the abundance and symmetry of amino acids in carbonaceous chondrites that experienced a range of alteration by water in their parent asteroids. The results show that amino acids are more abundant in the less altered meteorites, implying that aqueous processing changes the mix of amino acids. They also confirmed the enrichment in L-structures of some amino acids, especially isovaline, confirming earlier work. The authors suggest that aqueously-altered planetesimals might have seeded the early Earth with nonracemic amino acids, perhaps explaining why life from microorganisms to people use only L- forms to make proteins. The initial imbalance caused by non-biologic processes in wet asteroids might have been amplified by life on Earth. Alternatively

Carbonaceous adsorbent regeneration and halocarbon displacement by hydrocarbon gases

DOEpatents

Senum, G.I.; Dietz, R.N.

1994-04-05

This invention describes a process for regeneration of halocarbon bearing carbonaceous adsorbents through which a carbonaceous adsorbent is contacted with hydrocarbon gases, preferably propane, butane and pentane at near room temperatures and at atmospheric pressure. As the hydrocarbon gases come in contact with the adsorbent, the hydrocarbons displace the halocarbons by physical adsorption. As a result of using this process, the halocarbon concentration and the hydrocarbon eluant is increased thereby allowing for an easier recovery of pure halocarbons. By using the process of this invention, carbonaceous adsorbents can be regenerated by an inexpensive process which also allows for subsequent re-use of the recovered halocarbons. 8 figures.

Carbonaceous adsorbent regeneration and halocarbon displacement by hydrocarbon gases

DOEpatents

Senum, Gunnar I.; Dietz, Russell N.

1994-01-01

This invention describes a process for regeneration of halocarbon bearing carbonaceous adsorbents through which a carbonaceous adsorbent is contacted with hydrocarbon gases, preferably propane, butane and pentane at near room temperatures and at atmospheric pressure. As the hydrocarbon gases come in contact with the adsorbent, the hydrocarbons displace the halocarbons by physical adsorption. As a result of using this process, the halocarbon concentration and the hydrocarbon eluant is increased thereby allowing for an easier recovery of pure halocarbons. By using the process of this invention, carbonaceous adsorbents can be regenerated by an inexpensive process which also allows for subsequent re-use of the recovered halocarbons.

Coupling a versatile aerosol apparatus to a synchrotron: Vacuum ultraviolet light scattering, photoelectron imaging, and fragment free mass spectrometry

NASA Astrophysics Data System (ADS)

Shu, Jinian; Wilson, Kevin R.; Ahmed, Musahid; Leone, Stephen R.

2006-04-01

An aerosol apparatus has been coupled to the Chemical Dynamics Beamline of the Advanced Light Source at Lawrence Berkeley National Laboratory. This apparatus has multiple capabilities for aerosol studies, including vacuum ultraviolet (VUV) light scattering, photoelectron imaging, and mass spectroscopy of aerosols. By utilizing an inlet system consisting of a 200μm orifice nozzle and aerodynamic lenses, aerosol particles of ˜50nm-˜1μm in diameter can be sampled directly from atmospheric pressure. The machine is versatile and can probe carbonaceous aerosols generated by a laboratory flame, nebulized solutions of biological molecules, hydrocarbon aerosol reaction products, and synthesized inorganic nanoparticles. The sensitivity of this apparatus is demonstrated by the detection of nanoparticles with VUV light scattering, photoelectron imaging, and charged particle detection. In addition to the detection of nanoparticles, the thermal vaporization of aerosols on a heater tip leads to the generation of intact gas phase molecules. This phenomenon coupled to threshold single photon ionization, accessible with tunable VUV light, allows for fragment-free mass spectrometry of complex molecules. The initial experiments with light scattering, photoelectron imaging, and aerosol mass spectrometry reported here serve as a demonstration of the design philosophy and multiple capabilities of the apparatus.

Adsorption of dyes onto carbonaceous materials produced from coffee grounds by microwave treatment.

PubMed

Hirata, Mizuho; Kawasaki, Naohito; Nakamura, Takeo; Matsumoto, Kazuoki; Kabayama, Mineaki; Tamura, Takamichi; Tanada, Seiki

2002-10-01

Organic wastes have been burned for reclamation. However, they have to be recycled and reused for industrial sustainable development. Carbonaceous materials were produced from coffee grounds by microwave treatment. There are many phenolic hydroxyl and carboxyl groups on the surface of carbonaceous materials. The base consumption of the carbonaceous materials was larger than that of the commercially activated carbon. The carbonaceous materials produced from coffee grounds were applied to the adsorbates for the removal of basic dyes (methylene blue and gentian violet) in wastewater. This result indicated that the adsorption of dyes depended upon the surface polar groups on the carbonaceous materials. Moreover, the Freundlich constants of isotherms for the adsorption of methylene blue and gentian violet onto the carbonaceous materials produced from coffee grounds were greater than those for adsorption onto activated carbon or ceramic activated carbon. The interaction was greatest between the surface or porosity of the carbonaceous materials and methylene blue and gentian violet. The microwave treatment would be useful for the carbonization of organic wastes to save energy.

Biomass-derived sponge-like carbonaceous hydrogels and aerogels for supercapacitors.

PubMed

Wu, Xi-Lin; Wen, Tao; Guo, Hong-Li; Yang, Shubin; Wang, Xiangke; Xu, An-Wu

2013-04-23

As a newly developed material, carbon gels have been receiving considerable attention due to their multifunctional properties. Herein, we present a facile, green, and template-free route toward sponge-like carbonaceous hydrogels and aerogels by using crude biomass, watermelon as the carbon source. The obtained three-dimensional (3D) flexible carbonaceous gels are made of both carbonaceous nanofibers and nanospheres. The porous carbonaceous gels (CGs) are highly chemically active and show excellent mechanical flexibility which enable them to be a good scaffold for the synthesis of 3D composite materials. We synthesized the carbonaceous gel-based composite materials by incorporating Fe3O4 nanoparticles into the networks of the carbonaceous gels. The Fe3O4/CGs composites further transform into magnetite carbon aerogels (MCAs) by calcination. The MCAs keep the porous structure of the original CGs, which allows the sustained and stable transport of both electrolyte ions and electrons to the electrode surface, leading to excellent electrochemical performance. The MCAs exhibit an excellent capacitance of 333.1 F·g(-1) at a current density of 1 A·g(-1) within a potential window of -1.0 to 0 V in 6 M KOH solution. Meanwhile, the MCAs also show outstanding cycling stability with 96% of the capacitance retention after 1000 cycles of charge/discharge. These findings open up the use of low-cost elastic carbon gels for the synthesis of other 3D composite materials and show the possibility for the application in energy storage.

Importance of the mixing state for ice nucleating capabilities of individual aerosol particles

NASA Astrophysics Data System (ADS)

Ebert, Martin; Worringen, Annette; Benker, Nathalie; Weinbruch, Stephan

2010-05-01

The effects of aerosol particles on heterogeneous ice formation are currently insufficiently understood. Modelling studies have shown that the type and quantity of atmospheric aerosol particles acting as ice nuclei (IN) can influence ice cloud microphysical and radiative properties as well as their precipitation efficiency. Therefore, the physicochemical identification of IN and a quantitative description of the ice nucleation processes are crucial for a better understanding of formation, life cycles, and the optical properties of clouds as well as for numerical precipitation forecast. During the CLACE 5 campaign in 2006 at the high alpine research station Jungfraujoch (3580 m asl), Switzerland, the physicochemical parameters of IN within mixed-phase clouds were studied. By the use of special Ice-Counterflow Virtual Impactor, residual particles of small ice nuclei (IN) and the interstitial aerosol fraction were sampled seperately within mixed-phase clouds. The size, morphology, elemental composition and mixing state of more than 7000 particles of selected IN- and interstitial-samples were analyzed by scanning electron microscopy (SEM) combined with energy-dispersive X-ray analysis (EDX). For selected particles, the mineralogical phase composition was determined by transmission electron microscopy. In order to receive detailed information about the mixing state (coatings, agglomerates, heterogeneous inclusions) of the IN- and interstitial-samples, the complete individual particle analysis was performed operator controlled. Four different particle types were identified to act as IN. 1) Carbonaceous particles, which were identified to be a complex mixture of soot (main component), sulfate and nitrate. 2) Complex mixtures of two or more diverse particle groups. In almost 75% of these particles silicates or metal oxides are the main-component. 3) Aluminium oxide particles, which were internally mixed with calcium and sulphate rich material and 4) Pb bearing particles

Monthly and diurnal variations in aerosol size distributions, downwind of the Seoul metropolitan area

NASA Astrophysics Data System (ADS)

Kim, B. S.; Choi, Y.; Ghim, Y. S.

2014-12-01

The size distribution of aerosols is a physical property. However, since major aerosol types such as mineral dust, secondary inorganic ions, and carbonaceous aerosols are typically in specific size ranges, we can estimate the chemical composition of aerosols from the size distribution. We measured the mass size distribution of aerosols using an optical particle counter (Grimm Model 1.109) for a year from February 2013 to February 2014 at intervals of 10 minutes. The optical particle counter measures number concentrations between 0.25 and 32 μm in 31 bins and converts them into mass concentrations assuming a sphere and densities of aerosols in urban environment which originate from traffic and other combustion sources and are secondarily formed from photochemical reactions. The measurement site is at the rooftop of the five-story building on the hill (37.34 °N, 127.27 °E, 167 m above sea level), about 35 km southeast of downtown Seoul, the downwind area of which is affected by prevailing northwesterlies. There are no major emission sources nearby except a 4-lane road running about 1.4 km to the west. We tried to characterize the bimodal property of the mass size distribution, consisting of fine and coarse modes, in terms of mass concentration and mean diameter. Monthly and diurnal variations in mass concentration and mean diameter of each mode were investigated to estimate major aerosol types as well as major factors causing those variations.

Hydrothermal pretreatment to prevent scale during liquefaction of certain solid carbonaceous materials

DOEpatents

Stone, John B.; Floyd, Frank M.

1984-01-01

Scale formation during the liquefaction of lower ranking coals and similar carbonaceous materials is significantly reduced and/or prevented by hydrothermal pretreatment. The said pretreatment is believed to convert the scale-forming components to the corresponding carbonate prior to liquefaction. The said pretreatment is accomplished at a total pressure within the range from about 1000 to about 4400 psia. Temperature during said pretreatment will generally be within the range from about 500.degree. to about 700.degree. F.

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

Comparison of methods for the quantification of the different carbon fractions in atmospheric aerosol samples

NASA Astrophysics Data System (ADS)

Nunes, Teresa; Mirante, Fátima; Almeida, Elza; Pio, Casimiro

2010-05-01

to evaluate the possibility of continue using, for trend analysis, the historical data set, we performed an inter-comparison between our method and an adaptation of EUSAAR-2 protocol, taking into account that this last protocol will possibly be recommended for analysing carbonaceous aerosols at European sites. In this inter-comparison we tested different types of samples (PM2,5, PM2,5-10, PM10) with large spectra of carbon loadings, with and without pre-treatment acidification. For a reduced number of samples, five replicates of each one were analysed by each method for statistical purposes. The inter-comparison study revealed that when the sample analysis were performed in similar room conditions, the two thermo-optic methods give similar results for TC, OC and EC, without significant differences at a 95% confidence level. The correlation between the methods, DAO and EUSAAR-2 for EC is smaller than for TC and OC, although showing a coefficient correlation over 0,95, with a slope close to one. For samples performed in different periods, room temperatures seem to have a significant effect over OC quantification. The sample pre-treatment with HCl fumigation tends to decrease TC quantification, mainly due to the more volatile organic fraction release during the first heating step. For a set of 20 domestic biomass burning samples analyzed by the DAO method we observed an average decrease in TC quantification of 3,7 % in relation to non-acidified samples, even though this decrease is accompanied by an average increase in the less volatile organic fraction. The indirect measurement of carbon carbonate, usually a minor carbon component in the carbonaceous aerosol, based on the difference between TC measured by TOM of acidified and non-acidified samples is not a robust measurement, considering the biases affecting his quantification. The present study show that the two thermo-optic temperature program used for OC and EC quantification give similar results, and if in the

Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Despiau, S.; Dubovik, O.; Putaud, J. P.

2003-10-01

Microphysical and optical properties of the main aerosol species on a peri-urban site have been investigated during the ESCOMPTE experiment. Ammonium sulfate (AS), nitrate (N), black carbon (BC), particulate organic matter (POM), sea salt (SS) and mineral aerosol (D) size distributions have been used, associated with their refractive index, to compute, from the Mie theory, the key radiative aerosol properties as the extinction coefficient Kext, the mass extinction efficiencies σext, the single scattering albedo ω0 and the asymmetry parameter g at the wavelength of 550 nm. Optical computations show that 90% of the light extinction is due to anthropogenic aerosol and only 10% is due to natural aerosol (SS and D). 44±6% of the extinction is due to (AS) and 40±6% to carbonaceous particles (20±4% to BC and 21±4% to POM). Nitrate aerosol has a weak contribution of 5±2%. Computations of the mass extinction efficiencies σext, single scattering albedo ω0 and asymmetry parameter g indicate that the optical properties of the anthropogenic aerosol are often quite different from those yet published and generally used in global models. For example, the (AS) mean specific mass extinction presents a large difference with the value classically adopted at low relative humidity ( h<60%) (2.6±0.5 instead of 6 m 2 g -1 at 550 nm). The optical properties of the total aerosol layer, including all the aerosol species, indicate a mean observed single-scattering albedo ω0=0.85±0.05, leading to an important absorption of the solar radiation and an asymmetry parameter g=0.59±0.05 which are in a reasonably good agreements with the AERONET retrieval of ω0 (=0.86±0.05) and g (=0.64±0.05) at this wavelength.

Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide

NASA Astrophysics Data System (ADS)

Konovalov, Igor B.; Beekmann, Matthias; Berezin, Evgeny V.; Formenti, Paola; Andreae, Meinrat O.

2017-04-01

Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there is substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes under different environmental conditions and at various temporal scales hinders development of their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol photochemical age (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but that is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from MODIS and IASI measurements, respectively, are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with spatial average PM2. 5 concentration exceeding 100 µg m-3). For such plumes, the ER is found to increase almost 2-fold on the scale of ˜ 10 h of daytime aerosol

Quantification of Optical and Physical Properties of Combustion-Generated Carbonaceous Aerosols (

PubMed Central

Perera, Inoka Eranda; Litton, Charles D.

2016-01-01

A series of experiments were conducted to quantify and characterize the optical and physical properties of combustion-generated aerosols during both flaming and smoldering combustion of three materials common to underground mines—Pittsburgh Seam coal, Styrene Butadiene Rubber (a common mine conveyor belt material), and Douglas-fir wood—using a combination of analytical and gravimetric measurements. Laser photometers were utilized in the experiments for continuous measurement of aerosol mass concentrations and for comparison to measurements made using gravimetric filter samples. The aerosols of interest lie in the size range of tens to a few hundred nanometers, out of range of the standard photometer calibration. To correct for these uncertainties, the photometer mass concentrations were compared to gravimetric samples to determine if consistent correlations existed. The response of a calibrated and modified combination ionization/photoelectric smoke detector was also used. In addition, the responses of this sensor and a similar, prototype ionization/photoelectric sensor, along with discrete angular scattering, total scattering, and total extinction measurements, were used to define in real time the size, morphology, and radiative transfer properties of these differing aerosols that are generally in the form of fractal aggregates. SEM/TEM images were also obtained in order to compare qualitatively the real-time, continuous experimental measurements with the visual microscopic measurements. These data clearly show that significant differences exist between aerosols from flaming and from smoldering combustion and that these differences produce very different scattering and absorption signatures. The data also indicate that ionization/photoelectric sensors can be utilized to measure continuously and in real time aerosol properties over a broad spectrum of applications related to adverse environmental and health effects. PMID:27546898

Quantification of Optical and Physical Properties of Combustion-Generated Carbonaceous Aerosols (

PubMed

Perera, Inoka Eranda; Litton, Charles D

2015-03-01

A series of experiments were conducted to quantify and characterize the optical and physical properties of combustion-generated aerosols during both flaming and smoldering combustion of three materials common to underground mines-Pittsburgh Seam coal, Styrene Butadiene Rubber (a common mine conveyor belt material), and Douglas-fir wood-using a combination of analytical and gravimetric measurements. Laser photometers were utilized in the experiments for continuous measurement of aerosol mass concentrations and for comparison to measurements made using gravimetric filter samples. The aerosols of interest lie in the size range of tens to a few hundred nanometers, out of range of the standard photometer calibration. To correct for these uncertainties, the photometer mass concentrations were compared to gravimetric samples to determine if consistent correlations existed. The response of a calibrated and modified combination ionization/photoelectric smoke detector was also used. In addition, the responses of this sensor and a similar, prototype ionization/photoelectric sensor, along with discrete angular scattering, total scattering, and total extinction measurements, were used to define in real time the size, morphology, and radiative transfer properties of these differing aerosols that are generally in the form of fractal aggregates. SEM/TEM images were also obtained in order to compare qualitatively the real-time, continuous experimental measurements with the visual microscopic measurements. These data clearly show that significant differences exist between aerosols from flaming and from smoldering combustion and that these differences produce very different scattering and absorption signatures. The data also indicate that ionization/photoelectric sensors can be utilized to measure continuously and in real time aerosol properties over a broad spectrum of applications related to adverse environmental and health effects.

Thermo-optical properties of residential coals and combustion aerosols

NASA Astrophysics Data System (ADS)

Pintér, Máté; Ajtai, Tibor; Kiss-Albert, Gergely; Kiss, Diána; Utry, Noémi; Janovszky, Patrik; Palásti, Dávid; Smausz, Tomi; Kohut, Attila; Hopp, Béla; Galbács, Gábor; Kukovecz, Ákos; Kónya, Zoltán; Szabó, Gábor; Bozóki, Zoltán

2018-04-01

In this study, we present the inherent optical properties of carbonaceous aerosols generated from various coals (hard through bituminous to lignite) and their correlation with the thermochemical and energetic properties of the bulk coal samples. The nanoablation method provided a unique opportunity for the comprehensive investigation of the generated particles under well controlled laboratory circumstances. First, the wavelength dependent radiative features (optical absorption and scattering) and the size distribution (SD) of the generated particulate matter were measured in-situ in aerosol phase using in-house developed and customised state-of-the-art instrumentation. We also investigated the morphology and microstructure of the generated particles using Transmission Electron Microscopy (TEM) and Electron Diffraction (ED). The absorption spectra of the measured samples (quantified by Absorption Angström Exponent (AAE)) were observed to be distinctive. The correlation between the thermochemical features of bulk coal samples (fixed carbon (FC) to volatile matter (VM) ratio and calorific value (CV)) and the AAE of aerosol assembly were found to be (r2 = 0.97 and r2 = 0.97) respectively. Lignite was off the fitted curves in both cases most probably due to its high optically inactive volatile material content. Although more samples are necessary to be investigated to draw statistically relevant conclusion, the revealed correlation between CV and Single Scattering Albedo (SSA) implies that climatic impact of coal combusted aerosol could depend on the thermal and energetic properties of the bulk material.

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

NASA Technical Reports Server (NTRS)

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

2001-01-01

A primary, ACE-Asia objective was to quantify the interactions between aerosols and radiation in the Asia-Pacific region. Toward this end, radiometric and related aerosol measurements were made from ocean, land, air and space platforms. Models that predict aerosol fields guided the measurements and are helping integrate and interpret results. Companion overview's survey these measurement and modeling components. Here we illustrate how these components were combined to determine aerosol radiative. impacts and their relation to aerosol properties. Because clouds can obscure or change aerosol direct radiative effects, aircraft and ship sorties to measure these effects depended on predicting and finding cloud-free areas and times with interesting aerosols present. Pre-experiment satellite cloud climatologies, pre-flight aerosol and cloud forecasts, and in-flight guidance from satellite imagery all helped achieve this. Assessments of aerosol regional radiative impacts benefit from the spatiotemporal coverage of satellites, provided satellite-retrieved aerosol properties are accurate. Therefore, ACE-Asia included satellite retrieval tests, as part of many comparisons to judge the consistency (closure) among, diverse measurements. Early results include: (1) Solar spectrally resolved and broadband irradiances and optical depth measurements from the C-130 aircraft and at Kosan, Korea yielded aerosol radiative forcing efficiencies, permitting comparisons between efficiencies of ACE-Asia and INDOEX aerosols, and between dust and "pollution" aerosols. Detailed results will be presented in separate papers. (2) Based on measurements of wavelength dependent aerosol optical depth (AOD) and single scattering albedo the estimated 24-h a average aerosol radiative forcing efficiency at the surface for photosynthetically active radiation (400 - 700 nm) in Yulin, China is approx. 30 W sq m per AOD(500 nm). (3) The R/V Brown cruise from Honolulu to Sea of Japan sampled an aerosol optical

ORGANIC AEROSOL SAMPLING AND ANALYSIS METHODS RESEARCH

EPA Science Inventory

Carbonaceous material is a major component of ambient PM at all locations in the U.S. and it is composed of two major classes: organic carbon (OC, composed of hundreds of individual compounds) and elemental carbon (EC, also referred to as soot, black carbon, or light adsorbing ca...

The Asian Tropopause Aerosol Layer: Balloon-Borne Measurements, Satellite Observations and Modeling Approaches

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Natarajan, M.; Deshler, Terry; Liu, H.; Wegner, T.; Baker, N.; Gadhavi, H.; Jayaraman, A.; Pandit, A.;

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

NASA Technical Reports Server (NTRS)

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

2004-01-01

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

Increase in upper tropospheric and lower stratospheric aerosol levels and its potential connection with Asian pollution.

PubMed

Vernier, J-P; Fairlie, T D; Natarajan, M; Wienhold, F G; Bian, J; Martinsson, B G; Crumeyrolle, S; Thomason, L W; Bedka, K M

2015-02-27

Satellite observations have shown that the Asian Summer Monsoon strongly influences the upper troposphere and lower stratosphere (UTLS) aerosol morphology through its role in the formation of the Asian Tropopause Aerosol Layer (ATAL). Stratospheric Aerosol and Gas Experiment II solar occultation and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations show that summertime UTLS Aerosol Optical Depth (AOD) between 13 and 18 km over Asia has increased by three times since the late 1990s. Here we present the first in situ balloon measurements of aerosol backscatter in the UTLS from Western China, which confirm high aerosol levels observed by CALIPSO since 2006. Aircraft in situ measurements suggest that aerosols at lower altitudes of the ATAL are largely composed of carbonaceous and sulfate materials (carbon/sulfur elemental ratio ranging from 2 to 10). Back trajectory analysis from Cloud-Aerosol Lidar with Orthogonal Polarization observations indicates that deep convection over the Indian subcontinent supplies the ATAL through the transport of pollution into the UTLS. Time series of deep convection occurrence, carbon monoxide, aerosol, temperature, and relative humidity suggest that secondary aerosol formation and growth in a cold, moist convective environment could play an important role in the formation of ATAL. Finally, radiative calculations show that the ATAL layer has exerted a short-term regional forcing at the top of the atmosphere of -0.1 W/m 2 in the past 18 years. Increase of summertime upper tropospheric aerosol levels over Asia since the 1990s Upper tropospheric enhancement also observed by in situ backscatter measurements Significant regional radiative forcing of -0.1 W/m 2 .

Characterizing and sourcing ambient PM2.5 over key emission regions in China I: Water-soluble ions and carbonaceous fractions

NASA Astrophysics Data System (ADS)

Zhou, Jiabin; Xing, Zhenyu; Deng, Junjun; Du, Ke

2016-06-01

During the past decade, huge research resources have been devoted into studies of air pollution in China, which generated abundant datasets on emissions and pollution characterization. Due to the complex nature of air pollution as well as the limitations of each individual investigating approach, the published results were sometimes perplexing and even contradicting. This research adopted a multi-method approach to investigate region-specific air pollution characteristics and sources in China, results obtained using different analytical and receptor modeling methods were inter-compared for validation and interpretation. A year-round campaign was completed for comprehensive characterization of PM2.5 over four key emission regions: Beijing-Tianjin-Hebei (BTH), Yangzi River Delta (YRD), Pearl River Delta (PRD), and Sichuan Basin (SB). Atmospheric PM2.5 samples were collected from 10/2012 to 08/2013 at four regional sites, located on the diffusion paths of air masses from their corresponding megacities (i.e., Beijing, Shanghai, Guangzhou, and Chengdu). The annual average PM2.5 mass concentrations showed distinct regional difference, with the highest observed at BTH and lowest at PRD site. Nine water-soluble ions together contributed 33-41% of PM2.5 mass, with three dominant ionic species being SO42-, NO3-, NH4+, and carbonaceous particulate matter contributed 16-23% of PM2.5 mass. This implied that combustion and secondary formation were the main sources for PM2.5 in China. In addition, SO42-, NO3-, NH4+, and carbonaceous components (OC, EC) showed clear seasonal patterns with the highest concentration occurring in winter while the lowest in summer. Principal component analysis performed on aerosol data revealed that vehicular emissions, coal/biomass combustion, industry source, soil dust as well as secondary formation were the main potential sources for the ionic components of PM2.5. The characteristic chemical species combined with back trajectory analysis indicated

Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur.

PubMed

Shamjad, P M; Tripathi, S N; Thamban, Navaneeth M; Vreeland, Heidi

2016-11-24

Atmospheric aerosols influence Earth's radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species.

Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur

PubMed Central

Shamjad, P. M.; Tripathi, S. N.; Thamban, Navaneeth M.; Vreeland, Heidi

2016-01-01

Atmospheric aerosols influence Earth’s radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species. PMID:27883083

Mineralogical, Spectral, and Compositional Changes During Heating of Hydrous Carbonaceous Chondrites

NASA Technical Reports Server (NTRS)

Nakamura, T.; Matsuoka, M.; Yamashita, S.; Sato, Y.; Mogi, K.; Enokido, Y.; Nakata, A.; Okumura, S.; Furukawa, Y.; Zolensky, M.

2017-01-01

Hydrous carbonaceous chondrites experienced hydration and subsequent dehydration by heating, which resulted in a variety of mineralogical and spectral features [e. g., 1-6]. The degree of heating is classified according to heating stage (HS) II to IV based on mineralogy of phyllosilicates [2], because they change, with elevating temperature, to poorly crystal-line phases and subsequently to aggregates of small secondary anhydrous silicates of mainly olivine. Heating of hydrous carbonaceous chondrites also causes spectral changes and volatile loss [3-6]. Experimental heating of Murchison CM chondrite showed flattening of whole visible-near infrared spectra, especially weakening of the 3µm band strength [1, 4, 7]. In order to understand mineralogical, spectral, and compositional changes during heating of hydrous carbonaceous chondrites, we have carried out systematic investigation of mineralogy, reflectance spectra, and volatile composition of hydrated and dehydrated carbonaceous chondrites as well as experimentally-heated hydrous carbonaceous chondrites. In addition, we investigated reflectance spectra of tochilinite that is a major phase of CM chondrites and has a low dehydration temperature (250degC).

Remote sensing of soot carbon - Part 2: Understanding the absorption Ångström exponent

NASA Astrophysics Data System (ADS)

Schuster, G. L.; Dubovik, O.; Arola, A.; Eck, T. F.; Holben, B. N.

2016-02-01

Recently, some authors have suggested that the absorption Ångström exponent (AAE) can be used to deduce the component aerosol absorption optical depths (AAODs) of carbonaceous aerosols in the AERONET database. This AAE approach presumes that AAE ≪ 1 for soot carbon, which contrasts the traditional small particle limit of AAE = 1 for soot carbon. Thus, we provide an overview of the AERONET retrieval, and we investigate how the microphysics of carbonaceous aerosols can be interpreted in the AERONET AAE product. We find that AAE ≪ 1 in the AERONET database requires large coarse mode fractions and/or imaginary refractive indices that increase with wavelength. Neither of these characteristics are consistent with the current definition of soot carbon, so we explore other possibilities for the cause of AAE ≪ 1. AAE is related to particle size, and coarse mode particles have a smaller AAE than fine mode particles for a given aerosol mixture of species. We also note that the mineral goethite has an imaginary refractive index that increases with wavelength, is very common in dust regions, and can easily contribute to AAE ≪ 1. We find that AAE ≪ 1 can not be caused by soot carbon, unless soot carbon has an imaginary refractive index that increases with wavelength throughout the visible and near-infrared spectrums. Finally, AAE is not a robust parameter for separating carbonaceous absorption from dust aerosol absorption in the AERONET database.

A Decade of Field Changing Atmospheric Aerosol Research ...

EPA Pesticide Factsheets

Conference: Gordon Research Conference in Atmospheric Chemistry, July 28 – August 2, 2013, VermontPresentation Type: PosterTitle: An Analysis of EPA’s STAR Program and a Decade of Field Changing Research in Atmospheric AerosolsAuthors: Kristina M. Wagstrom1,2, Sherri W. Hunt31Chemical and Biomolecular Engineering, University of Connecticut, Storrs, CT2AAAS Science and Technology Policy Fellow hosted by U.S. Environmental Protection Agency, National Center for Environmental Research3U.S. Environmental Protection Agency, National Center for Environmental ResearchA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isoprene oxidation, and understanding the role of aqueous oxidation of organics on SOA formation. A series of grants funded by EPA just under ten years ago supported many of these advances. These projects make up the body of work awarded under two solicitations released by the EPA’s Science to Achieve Results (STAR) program: “Measurement, Modeling, and Analysis Methods for Airborne Carbonaceous Fine Particulate Matter” (2003) and “Source Apportionment of Particulate Matter” (2004). Our goal is to present the impact of the STAR solicitations and to show how they have pushed the field forward and led to new questions.In particular

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

NASA Astrophysics Data System (ADS)

Tian, Mi; Wang, Huanbo; Chen, Yang; Yang, Fumo; Zhang, Xiaohua; Zou, Qiang; Zhang, Renquan; Ma, Yongliang; He, Kebin

2016-06-01

Extremely severe haze weather events occurred in many cities in China, especially in the east part of the country, in January 2013. Comprehensive measurements including hourly concentrations of PM2.5 and its major chemical components (water-soluble inorganic ions, organic carbon (OC), and elemental carbon (EC)) and related gas-phase precursors were conducted via an online monitoring system in Suzhou, a medium-sized city in Jiangsu province, just east of Shanghai. PM2.5 (particulate matter with an aerodynamic diameter of 2.5 µm or less) frequently exceeded 150 µg m-3 on hazy days, with the maximum reaching 324 µg m-3 on 14 January 2013. Unfavorable weather conditions (high relative humidity (RH), and low rainfall, wind speed, and atmospheric pressure) were conducive to haze formation. High concentrations of secondary aerosol species (including SO42-, NO3-, NH4+, and SOC) and gaseous precursors were observed during the first two haze events, while elevated primary carbonaceous species emissions were found during the third haze period, pointing to different haze formation mechanisms. Organic matter (OM), (NH4)2SO4, and NH4NO3 were found to be the major contributors to visibility impairment. High concentrations of sulfate and nitrate might be explained by homogeneous gas-phase reactions under low RH conditions and by heterogeneous processes under relatively high RH conditions. Analysis of air mass trajectory clustering and potential source contribution function showed that aerosol pollution in the studied areas was mainly caused by local activities and surrounding sources transported from nearby cities.

Influence of Bulk Carbonaceous Matter on Pluto's Structure and Evolution

NASA Astrophysics Data System (ADS)

McKinnon, W. B.; Stern, S. A.; Weaver, H. A., Jr.; Spencer, J. R.; Moore, J. M.; Young, L. A.; Olkin, C.

2017-12-01

The rock/ice mass ratio of the Pluto system is about 2/1 (McKinnon et al., Icarus 287, 2017) [1], though this neglects the potential role of bulk carbonaceous matter ("CHON"), an important cometary component and one likely important in the ancestral Kuiper belt. The wealth of measurements at comet 67P/Churyumov-Gerasimenko (a Jupiter-family comet and thus one formed in the same region of the outer Solar System as Pluto) by Rosetta are particularly instructive. E.g., Davidsson et al. (A&A 592, 2016) [2] propose in their "composition A" that 67P/Ch-G is 25% metal/sulfides, 42% rock/organics, and 32% ice by mass. For their assumed component densities, the overall grain density is 1820 kg/m3. Fulle et al. (MNRAS 462, 2016) [3] posit 5 ± 2 volume % Fe-sulfides of density 4600 kg/m3, 28 ± 5% Mg,Fe-olivines and -pyroxenes of density 3200 kg/m3, 52 ± 12% hydrocarbons of density 1200 kg/m3, and 15 ± 6% ices of 917 kg/m3. This composition yields a primordial grain density (dust + ice) of 1885 ± 240 kg/m3. Both of these cometary density estimates [2,3] are consistent with Pluto-Charon, especially as Pluto's uncompressed (STP) density is close to 1820 kg/m3 and that of the system as a whole is close to 1800 kg/m3 [1]. We consider the potential compositional and structural implications of these proposed 67P/Ch-G compositions when applied to Pluto and Charon. The amount of ice in model A of [2] is a good match to Pluto structural models. Their rock/organics component, however, is taken to be half graphite (2000 kg/m3) by volume. The composition in [3] is more divergent: very ice poor, and on the order of 50% light hydrocarbons by volume. Regardless of the differences between [2] and [3], the possibility of massive internal graphite or carbonaceous layers within Pluto is real. We discuss the possible consequences for Pluto's structure, rock/ice ratio, thermal and chemical evolution, and even interpretation of its gravity field from tectonics. For example, radiogenic heat

The role of semi-volatile organic compounds in the mesoscale evolution of biomass burning aerosol: a modelling case study of the 2010 mega-fire event in Russia

NASA Astrophysics Data System (ADS)

Konovalov, I. B.; Beekmann, M.; Berezin, E. V.; Petetin, H.; Mielonen, T.; Kuznetsova, I. N.; Andreae, M. O.

2015-03-01

Chemistry transport models (CTMs) are an indispensable tool for studying and predicting atmospheric and climate effects associated with carbonaceous aerosol from open biomass burning (BB); this type of aerosol is known to contribute significantly to both global radiative forcing and to episodes of air pollution in regions affected by wildfires. Improving model performance requires systematic comparison of simulation results with measurements of BB aerosol and elucidating possible reasons for discrepancies between them, which, "by default", are frequently attributed in the literature to uncertainties in emission data. Based on published laboratory data regarding atmospheric evolution of BB aerosol and by using the volatility basis set (VBS) approach to organic aerosol modeling along with a "conventional" approach, we examined the importance of taking gas-particle partitioning and oxidation of semi-volatile organic compounds (SVOCs) into account in simulations of the mesoscale evolution of smoke plumes from intense wildfires that occurred in western Russia in 2010. BB emissions of primary aerosol components were constrained with the PM10 and CO data from the air pollution monitoring network in the Moscow region. The results of the simulations performed with the CHIMERE CTM were evaluated by considering, in particular, the ratio of smoke-related enhancements in PM10 and CO concentrations (ΔPM10 and ΔCO) measured in Finland (in the city of Kuopio), nearly 1000 km downstream of the fire emission sources. It is found that while the conventional approach (disregarding oxidation of SVOCs and assuming organic aerosol material to be non-volatile) strongly underestimates values of ΔPM10/ΔCO observed in Kuopio (by almost a factor of two), the VBS approach is capable to bring the simulations to a reasonable agreement with the ground measurements both in Moscow and in Kuopio. Using the VBS instead of the conventional approach is also found to result in a major improvement of

Matrices of carbonaceous chondrite meteorites

NASA Technical Reports Server (NTRS)

Buseck, Peter R.; Hua, Xin

1993-01-01

The morphology, classification, and chemistry of the matrices of carbonaceous chondrite (CC) meteorites is reviewed based on recent research results. The various kinds of CCs are examined in terms of their matrix mineralogy. Alteration processes in CCs are discussed.

A contribution of black and brown carbon to the aerosol light absorption

NASA Astrophysics Data System (ADS)

Kim, Sang-Woo; Cho, Chaeyoon; Jo, Duseong; Park, Rokjin

2017-04-01

Black carbon (BC) is functionally defined as the absorbing component of atmospheric total carbonaceous aerosols and is typically dominated by soot-like elemental carbon (EC). Organic carbon (OC) has also been shown to absorb strongly at visible to UV wavelengths and the absorbing organics are referred to as brown carbon (BrC; Alexander et al., 2008). These two aerosols contribute to solar radiative forcing through absorption of solar radiation and heating of the absorbing aerosol layer, but most optical instruments that quantify light absorption are unable to distinguish one type of absorbing aerosol from another (Moosmüller et al. 2009). In this study, we separate total aerosol absorption from these two different light absorbers from co-located simultaneous in-situ measurements, such as Continuous Soot Monitoring System (COSMOS), Continuous Light Absorption Photometer (CLAP) and Sunset EC/OC analyzer, at Gosan climate observatory, Korea. We determine the mass absorption cross-section (MAC) of BC, and then estimate the contribution of BC and BrC on aerosol light absorption, together with a global 3-D chemical transport model (GEOS-Chem) simulation. At 565 nm wavelength, BC MAC is found to be about 5.4±2.8 m2 g-1 from COSMOS and Sunset EC/OC analyzer measurements during January-May 2012. This value is similar to those from Alexander et al. (2008; 4.3 ˜ 4.8 m2 g-1 at 550 nm) and Chung et al. (2012; 5.1 m2 g-1 at 520 nm), but slightly lower than Bond and Bergstrom (2006; 7.5±1.2 m2 g-1 at 550 nm). The COMOS BC mass concentration calculated with 5.4 m2 g-1 of BC MAC shows a good agreement with thermal EC concentration, with a good slope (1.1). Aerosol absorption coefficient and BC mass concentration from COSMOS, meanwhile, are approximately 25 ˜ 30 % lower than those of CLAP. This difference can be attributable to the contribution of volatile light-absorbing aerosols (i.e., BrC). The absorption coefficient of BrC, which is determined by the difference of

Seasonal variation of organic aerosol in PM2.5 at Anmyeondo, a background site in Korea

NASA Astrophysics Data System (ADS)

Lee, J.; Kim, E. S.; Kim, Y. P.; Jung, C. H.; Lee, J.

2016-12-01

Routine measurements of PM2.5 and chemical speciation for 100 individual organic compounds were carried out to understand seasonal variation of organic compounds at a background area in Korea between 2015 and 2016. Organic compounds analyzed in this study were classified into five groups, n-alkanes, polycyclic aromatic hydrocarbons (PAHs), fatty acids (FA), dicarboxylic acids (DCAs), and sugar. Further, organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and Humic Like Substance-Carbon (HULIS-C) in PM2.5 were simultaneously analyzed to make mass balance of carbonaceous aerosol in PM2.5 at a background site in Korea. PAHs concentrations at this site was lower than that at Seoul, a representative urban site in Korea. PAHs and n-Alkanes concentrations showed clear seasonal variation with summer minimum and winter maximum, while, seasonal variation of DCAs and Sugars were different with PAHs and n-Alkanes.WSOC concentrations were highly correlated with SOC (Secondary Organic Carbon) concentrations which were estimated by the EC tracer method. The results indicate the formation of secondary organic aerosol (SOA) is major factor for the determination of WSOC concentrations in this region. HULIS-C as known one of brown carbon was major component of WSOC which accounts for 39 to 99% in WSOC. The average concentrations of HULIS-C was 2.02±1.42 and the highest concentration was observed in fall.

Feasibility study of aerosol retrieval for GCOM-C/SGLI with simulated data

NASA Astrophysics Data System (ADS)

Mukai, S.; Sano, I.; Yasumoto, M.; Nakata, M.; Nishi, N.

2016-12-01

The Japan Aerospace Exploration Agency (JAXA) has been developing the new Earth observing system, GCOM (Global Change Observation Mission) project, which consists of two satellite series of GCOM-W1 and GCOM-C1. The 1st GCOM-C satellite will board the SGLI (second generation global imager) to be launched in early of 2017. The SGLI has multi (19)-channels including near ultra violet (NUV) channels (380, 412 nm) and two polarization channels at red and near-infrared wavelengths of 670 and 870 nm. Global aerosol retrieval is achieved with both polarization and total radiance. It is noted that NUV measurements are available for detection of the carbonaceous aerosols. The biomass burning aerosols (BBA) generated by forest fire and/or burn agriculture have influenced on the severe air pollutions. It is known that the forest fire increases due to global warming and a climate change, and has influences on them vice versa. It is well known that this negative cycle decreases the quality of global environment and human health. In this work, we use both radiance and polarization measurements observed by GLI and POLDER-2 on Japanese ADEOS-2 satellite in 2003 as a simulated data set for coming GCOM-C/SGLI sensor. As a result the possibility of GCOM-C1/SGLI related to remote sensing for aerosols, especially in the hazardous aerosol episodes including biomass burning case, can be examined.

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

Contrasting diurnal variations in fossil and nonfossil secondary organic aerosol in urban outflow, Japan.

PubMed

Morino, Yu; Takahashi, Katsuyuki; Fushimi, Akihiro; Tanabe, Kiyoshi; Ohara, Toshimasa; Hasegawa, Shuichi; Uchida, Masao; Takami, Akinori; Yokouchi, Yoko; Kobayashi, Shinji

2010-11-15

Diurnal variations of fossil secondary organic carbon (SOC) and nonfossil SOC were determined for the first time using a combination of several carbonaceous aerosol measurement techniques, including radiocarbon (¹⁴C) determinations by accelerator mass spectrometry, and a receptor model (chemical mass balance, CMB) at a site downwind of Tokyo during the summer of 2007. Fossil SOC showed distinct diurnal variation with a maximum during daytime, whereas diurnal variation of nonfossil SOC was relatively small. This behavior was reproduced by a chemical transport model (CTM). However, the CTM underestimated the concentration of anthropogenic secondary organic aerosol (ASOA) by a factor of 4-7, suggesting that ASOA enhancement during daytime is not explained by production from volatile organic compounds that are traditionally considered major ASOA precursors. This result suggests that unidentified semivolatile organic compounds or multiphase chemistry may contribute largely to ASOA production. As our knowledge of production pathways of secondary organic aerosol (SOA) is still limited, diurnal variations of fossil and nonfossil SOC in our estimate give an important experimental constraint for future development of SOA models.

Direct radiative effect by multicomponent aerosol over China

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

Huang, Xin; Song, Yu; Zhao, Chun

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

Slurry burner for mixture of carbonaceous material and water

DOEpatents

Nodd, Dennis G.; Walker, Richard J.

1987-01-01

A carbonaceous material-water slurry burner includes a high pressure tip-emulsion atomizer for directing a carbonaceous material-water slurry into a combustion chamber for burning therein without requiring a support fuel or oxygen enrichment of the combustion air. Introduction of the carbonaceous material-water slurry under pressure forces it through a fixed atomizer wherein the slurry is reduced to small droplets by mixing with an atomizing air flow and directed into the combustion chamber. The atomizer includes a swirler located immediately adjacent to where the fuel slurry is introduced into the combustion chamber and which has a single center channel through which the carbonaceous material-water slurry flows into a plurality of diverging channels continuous with the center channel from which the slurry exits the swirler immediately adjacent to an aperture in the combustion chamber. The swirler includes a plurality of slots around its periphery extending the length thereof through which the atomizing air flows and by means of which the atomizing air is deflected so as to exert a maximum shear force upon the carbonaceous material-water slurry as it exits the swirler and enters the combustion chamber. A circulating coolant system or boiler feed water is provided around the periphery of the burner along the length thereof to regulate burner operating temperature, eliminate atomizer plugging, and inhibit the generation of sparklers, thus increasing combustion efficiency. A secondary air source directs heated air into the combustion chamber to promote recirculation of the hot combustion gases within the combustion chamber.

A carbon and nitrogen isotope study of carbonaceous vein material in ureilite meteorites

NASA Technical Reports Server (NTRS)

Russell, S. S.; Arden, J. W.; Franchi, I. A.; Pillinger, C. T.

1993-01-01

The ureilite meteorite group is known to be rich in carbon in the form of graphite/diamond veins that are associated with planetary type noble gases. This paper reports preliminary data from a systematic study of the carbon and nitrogen isotopic composition of this carbonaceous vein material. A previous study focused on the whole rock signatures and reported that the carbon inventory appeared to be dominated by the graphitic/diamond intergrowths, whereas the nitrogen was clearly composed of several distinct components including one that was isotopically light, possibly associated with the carbonaceous material. Recent studies have demonstrated that diamonds in the solar system formed in many different environments. C and N measurements from ureilitic diamond made in a similar way would be a useful addition to this overall study. The methods used for isolating diamonds of possible presolar origin from primitive meteorites are equally applicable to the processing of carbon bearing components in the ureilite group so that their stable isotopic composition can be determined. Herein we discuss conjoint C and N stepped combustion measurements made on crushed whole rock ureilite samples that have been treated with 1M HCl/9M HF to dissolve silicate and free metal. In addition, two samples have been further treated with oxidizing acids to leave a diamond rich residue.

Estimation of gas-particle partitioning coefficients (Kp) of carcinogenic polycyclic aromatic hydrocarbons in carbonaceous aerosols collected at Chiang-Mai, Bangkok and Hat-Yai, Thailand.

PubMed

Pongpiachan, Siwatt; Ho, Kin Fai; Cao, Junji

2013-01-01

To assess environmental contamination with carcinogens, carbonaceous compounds, water-soluble ionic species and trace gaseous species were identified and quantified every three hours for three days at three different atmospheric layers at the heart of Chiang-Mai, Bangkok and Hat-Yai from December 2006 to February 2007. A DRI Model 2001 Thermal/Optical Carbon Analyzer with the IMPROVE thermal/optical reflectance (TOR) protocol was used to quantify the organic carbon (OC) and elemental carbon (EC) contents in PM10. Diurnal and vertical variability was also carefully investigated. In general, OC and EC mass concentration showed the highest values at the monitoring period of 21.00-00.00 as consequences of human activities at night bazaar coupled with reduction of mixing layer, decreased wind speed and termination of photolysis at nighttime. Morning peaks of carbonaceous compounds were observed during the sampling period of 06:00-09:00, emphasizing the main contribution of traffic emission in the three cities. The estimation of incremental lifetime particulate matter exposure (ILPE) raises concern of high risk of carbonaceous accumulation over workers and residents living close to the observatory sites. The average values of incremental lifetime particulate matter exposure (ILPE) of total carbon at Baiyoke Suit Hotel and Baiyoke Sky Hotel are approximately ten times higher than those air samples collected at Prince of Songkla University Hat-Yai campus corpse incinerator and fish-can manufacturing factory but only slightly higher than those of rice straw burning in Songkla province. This indicates a high risk of developing lung cancer and other respiratory diseases across workers and residents living in high buildings located in Pratunam area. Using knowledge of carbonaceous fractions in PM10, one can estimate the gas-particle partitioning of polycyclic aromatic hydrocarbons (PAHs). Dachs-Eisenreich model highlights the crucial role of adsorption in gas

Aerosol studies during the ESCOMPTE experiment: an overview

NASA Astrophysics Data System (ADS)

Cachier, Hélène; Aulagnier, Fabien; Sarda, Roland; Gautier, François; Masclet, Pierre; Besombes, Jean-Luc; Marchand, Nicolas; Despiau, Serge; Croci, Delphine; Mallet, Marc; Laj, Paolo; Marinoni, Angela; Deveau, Pierre-Alexandre; Roger, Jean-Claude; Putaud, Jean-Philippe; Van Dingenen, Rita; Dell'Acqua, Alessandro; Viidanoja, Jyrkki; Martins-Dos Santos, Sebastiao; Liousse, Cathy; Cousin, Frédéric; Rosset, Robert; Gardrat, Eric; Galy-Lacaux, Corinne

2005-03-01

The "Expérience sur Site pour COntraindre les Modèles de Pollution atmosphérique et de Transport d'Emissions" (ESCOMPTE) experiment took place in the Southern part of France in the Marseilles/Fos-Berre region during 6 weeks in June and July 2001. One task was to document the regional sources of atmospheric particles and to gain some insight into the aerosol transformations in the atmosphere. For this purpose, seven sites were chosen and equipped with the same basic instrumentation to obtain the chemical closure of the bulk aerosol phase and size-segregated samples. Some specific additional experiments were conducted for the speciation of the organic matter and the aerosol size distribution in number. Finally, four multiwavelength sun-photometers were also deployed during the experiment. Interestingly, in this region, three intense aerosol sources (urban, industrial and biogenic) are very active, and data show consistent results, enlightening an important background of particles over the whole ESCOMPTE domain. Notable is the overwhelming importance of the carbonaceous fraction (comprising primary and secondary particles), which is always more abundant than sulphates. Particle size studies show that, on average, more than 90% of the mean regional aerosol number is found on a size range smaller than 300 nm in diameter. The most original result is the evidence of the rapid formation of secondary aerosols occurring in the whole ESCOMPTE domain. This formation is much more important than that usually observed at these latitudes since two thirds of the particulate mass collected off source zones is estimated to be generated during atmospheric transport. On the other hand, the marine source has poor influence in the region, especially during the overlapping pollution events of Intensive Observation Periods (IOP). Preliminary results from the 0D and 3D versions of the MesoNH-aerosol model show that, with optimised gas and particle sources, the model accounts

The role of semi-volatile organic compounds in the mesoscale evolution of biomass burning aerosol: a modeling case study of the 2010 mega-fire event in Russia

NASA Astrophysics Data System (ADS)

Konovalov, I. B.; Beekmann, M.; Berezin, E. V.; Petetin, H.; Mielonen, T.; Kuznetsova, I. N.; Andreae, M. O.

2015-12-01

Chemistry transport models (CTMs) are an indispensable tool for studying and predicting atmospheric and climate effects associated with carbonaceous aerosol from open biomass burning (BB); this type of aerosol is known to contribute significantly to both global radiative forcing and to episodes of air pollution in regions affected by wildfires. Improving model performance requires systematic comparison of simulation results with measurements of BB aerosol and elucidation of possible reasons for discrepancies between them, which, by default, are frequently attributed in the literature to uncertainties in emission data. Based on published laboratory data on the atmospheric evolution of BB aerosol and using the volatility basis set (VBS) framework for organic aerosol modeling, we examined the importance of taking gas-particle partitioning and oxidation of semi-volatile organic compounds (SVOCs) into account in simulations of the mesoscale evolution of smoke plumes from intense wildfires that occurred in western Russia in 2010. Biomass burning emissions of primary aerosol components were constrained with PM10 and CO data from the air pollution monitoring network in the Moscow region. The results of the simulations performed with the CHIMERE CTM were evaluated by considering, in particular, the ratio of smoke-related enhancements in PM10 and CO concentrations (ΔPM10 and ΔCO) measured in Finland (in the city of Kuopio), nearly 1000 km downstream of the fire emission sources. It is found that while the simulations based on a "conventional" approach to BB aerosol modeling (disregarding oxidation of SVOCs and assuming organic aerosol material to be non-volatile) strongly underestimated values of ΔPM10/ΔCO observed in Kuopio (by a factor of 2), employing the "advanced" representation of atmospheric processing of organic aerosol material resulted in bringing the simulations to a much closer agreement with the ground measurements. Furthermore, taking gas

Charactering biomass burning aerosol in the Weather Research and Forecasting model with Chemistry (WRF-Chem), with evaluation against SAMBBA flight data.

NASA Astrophysics Data System (ADS)

Archer-Nicholls, S.; Lowe, D.; Darbyshire, E.; Morgan, W.; Freitas, S. R.; Longo, K.; Coe, H.; McFiggans, G.

2014-12-01

The burning of forests in the Amazonia region is a globally significant source of carbonaceous aerosol, containing both absorbing and scattering components. Biomass burning aerosol (BBA) are efficient CCN, modifying cloud properties and influencing atmospheric circulation and precipitation tendencies. The impacts of BBA are highly dependent on their size distribution and composition. Studies in this region can therefore benefit greatly from the use of state-of-the-art sectional aerosol representations. A bottom-up fire emissions inventory, 3BEM, has been developed by Longo et al.1. It uses satellite products to identify fire locations, applying the emissions factors of Andrei and Merlot3 to generate daily emission maps. Flaming emissions are very buoyant, and a method for injecting emissions at altitude is needed to accurately describe the vertical profile of BBA. A parameterisation has been developed to simulate this sub-grid process4, and previously implemented in WRF-Chem using a modal aerosol scheme5. For this work we have modified the WRF-Chem model to simulate 3BEM emissions using the MOSAIC sectional aerosol scheme6. This modified version of WRF-Chem v3.4.1 has been run for September 2012 over South America (25km grid-spacing). We will present model results evaluating the modelled aerosol vertical distribution, size distribution, composition and optical properties against measurements taken by the FAAM BAe-146 research aircraft during the SAMBBA field campaign. The plume-rise parameterisation was found to inject flaming emissions too high over most fires, resulting in high modelled aerosol loadings at high altitude. We probed the behaviour of the parameterisation by developing a new SAMBBA-tuned 3BEM emissions scenario, which uses more realistic estimates of fire size. Results from high-resolution (5 and 1km) nested simulations will also be presented, in order to evaluate the impacts of explicit aerosol-cloud interactions in non-parameterised clouds. 1. K

Liquefaction process for solid carbonaceous materials containing alkaline earth metal humates

DOEpatents

Epperly, William R.; Deane, Barry C.; Brunson, Roy J.

1982-01-01

An improved liquefaction process wherein wall scale and particulate agglomeration during the liquefaction of solid carbonaceous materials containing alkaline earth metal humates is reduced and/or eliminated by subjecting the solid carbonaceous materials to controlled cyclic cavitation during liquefaction. It is important that the solid carbonaceous material be slurried in a suitable solvent or diluent during liquefaction. The cyclic cavitation may be imparted via pressure cycling, cyclic agitation and the like. When pressure cycling or the like is employed an amplitude equivalent to at least 25 psia is required to effectively remove scale from the liquefaction vessel walls.

AERONET derived (BC) aerosol absorption

NASA Astrophysics Data System (ADS)

Kinne, S.

2015-12-01

AERONET is a ground-based sun-/sky-photometer network with good annual statistics at more than 400 sites worldwide. Inversion methods applied to these data define all relevant column aerosol optical properties and reveal even microphysical detail. The extracted data include estimates for aerosol size-distributions and for aerosol refractive indices at four different solar wavelengths. Hereby, the imaginary parts of the refractive indices define the aerosol column absorption. For regional and global averages and radiative impact assessment with off-line radiative transfer, these local data have been extended with distribution patterns offered by AeroCom modeling experiments. Annual and seasonal absorption distributions for total aerosol and estimates for component contributions (such as BC) are presented and associated direct forcing impacts are quantified.

Pyrolysis of carbonaceous materials with solvent quench recovery

DOEpatents

Green, Norman W.; Duraiswamy, Kandaswamy; Lumpkin, Robert E.; Knell, Everett W.; Mirza, Zia I.; Winter, Bruce L.

1978-04-18

In a continuous process for recovery of values contained in a solid carbonaceous material, the carbonaceous material is comminuted and then subjected to flash pyrolysis in the presence of a particulate heat source to form a pyrolysis product stream containing a carbon containing solid residue and volatilized hydrocarbons. After the carbon containing solid residue is separated from the pyrolysis product stream, values are obtained by condensing volatilized hydrocarbons. The particulate source of heat is formed by oxidizing carbon in the solid residue. Apparatus useful for practicing this process are disclosed.

Absorption Properties of Mediterranean Aerosols Obtained from Multi-year Ground-based and Satellite Remote Sensing Observations

NASA Technical Reports Server (NTRS)

Mallet, M.; Dubovik, O.; Nabat, P.; Dulac, F.; Kahn, R.; Sciare, J.; Paronis, D.; Leon, J. F.

2013-01-01

Aerosol absorption properties are of high importance to assess aerosol impact on regional climate. This study presents an analysis of aerosol absorption products obtained over the Mediterranean Basin or land stations in the region from multi-year ground-based AERONET and satellite observations with a focus on the Absorbing Aerosol Optical Depth (AAOD), Single Scattering Albedo (SSA) and their spectral dependence. The AAOD and Absorption Angstrom Exponent (AAE) data set is composed of daily averaged AERONET level 2 data from a total of 22 Mediterranean stations having long time series, mainly under the influence of urban-industrial aerosols and/or soil dust. This data set covers the 17 yr period 1996-2012 with most data being from 2003-2011 (approximately 89 percent of level-2 AAOD data). Since AERONET level-2 absorption products require a high aerosol load (AOD at 440 nm greater than 0.4), which is most often related to the presence of desert dust, we also consider level-1.5 SSA data, despite their higher uncertainty, and filter out data with an Angstrom exponent less than 1.0 in order to study absorption by carbonaceous aerosols. The SSA data set includes both AERONET level-2 and satellite level-3 products. Satellite-derived SSA data considered are monthly level 3 products mapped at the regional scale for the spring and summer seasons that exhibit the largest aerosol loads. The satellite SSA dataset includes the following products: (i) Multi-angle Imaging SpectroRadiometer (MISR) over 2000-2011, (ii) Ozone Monitoring Instrument (OMI) near-UV algorithm over 2004-2010, and (iii) MODerate resolution Imaging Spectroradiometer (MODIS) Deep-Blue algorithm over 2005-2011, derived only over land in dusty conditions. Sun-photometer observations show that values of AAOD at 440 nm vary between 0.024 +/- 0.01 (resp. 0.040 +/- 0.01) and 0.050 +/- 0.01 (0.055 +/- 0.01) for urban (dusty) sites. Analysis shows that the Mediterranean urban-industrial aerosols appear "moderately

Characterization of Florida red tide aerosol and the temporal profile of aerosol concentration.

PubMed

Cheng, Yung Sung; Zhou, Yue; Pierce, Richard H; Henry, Mike; Baden, Daniel G

2010-05-01

Red tide aerosols containing aerosolized brevetoxins are produced during the red tide bloom and transported by wind to coastal areas of Florida. This study reports the characterization of Florida red tide aerosols in human volunteer studies, in which an asthma cohort spent 1h on Siesta Beach (Sarasota, Florida) during aerosolized red tide events and non-exposure periods. Aerosol concentrations, brevetoxin levels, and particle size distribution were measured. Hourly filter samples were taken and analyzed for brevetoxin and NaCl concentrations. In addition, the aerosol mass concentration was monitored in real time. The results indicated that during a non-exposure period in October 2004, no brevetoxin was detected in the water, resulting in non-detectable levels of brevetoxin in the aerosol. In March 2005, the time-averaged concentrations of brevetoxins in water samples were moderate, in the range of 5-10 microg/L, and the corresponding brevetoxin level of Florida red tide aerosol ranged between 21 and 39 ng/m(3). The temporal profiles of red tide aerosol concentration in terms of mass, NaCl, and brevetoxin were in good agreement, indicating that NaCl and brevetoxins are components of the red tide aerosol. By continuously monitoring the marine aerosol and wind direction at Siesta Beach, we observed that the marine aerosol concentration varied as the wind direction changed. The temporal profile of the Florida red tide aerosol during a sampling period could be explained generally with the variation of wind direction. Copyright 2009 Elsevier Ltd. All rights reserved.

Type-segregated aerosol effects on regional monsoon activity: A study using ground-based experiments and model simulations

NASA Astrophysics Data System (ADS)

Vijayakumar, K.; Devara, P. C. S.; Sonbawne, S. M.

2014-12-01

Classification of observed aerosols into key types [e.g., clean-maritime (CM), desert-dust (DD), urban-industrial/biomass-burning (UI/BB), black carbon (BC), organic carbon (OC) and mixed-type aerosols (MA)] would facilitate to infer aerosol sources, effects, and feedback mechanisms, not only to improve the accuracy of satellite retrievals but also to quantify the assessment of aerosol radiative impacts on climate. In this paper, we report the results of a study conducted in this direction, employing a Cimel Sun-sky radiometer at the Indian Institute of Tropical Meteorology (IITM), Pune, India during 2008 and 2009, which represent two successive contrasting monsoon years. The study provided an observational evidence to show that the local sources are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle over Pune, a tropical urban station in India. The results revealed the absence of CM aerosols in the pre-monsoon as well as in the monsoon seasons of 2009 as opposed to 2008. Higher loading of dust aerosols is observed in the pre-monsoon and monsoon seasons of 2009; majority may be coated with fine BC aerosols from local emissions, leading to reduction in regional rainfall. Further, significant decrease in coarse-mode AOD and presence of carbonaceous aerosols, affecting the aerosol-cloud interaction and monsoon-rain processes via microphysics and dynamics, is considered responsible for the reduction in rainfall during 2009. Additionally, we discuss how optical depth, contributed by different types of aerosols, influences the distribution of monsoon rainfall over an urban region using the Monitoring Atmospheric Composition and Climate (MACC) aerosol reanalysis. Furthermore, predictions of the Dust REgional Atmospheric Model (DREAM) simulations combined with HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) cluster model are also discussed in support of the

Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

NASA Astrophysics Data System (ADS)

Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

2008-12-01

The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

Detecting Thin Cirrus in Multiangle Imaging Spectroradiometer Aerosol Retrievals

NASA Technical Reports Server (NTRS)

Pierce, Jeffrey R.; Kahn, Ralph A.; Davis, Matt R.; Comstock, Jennifer M.

2010-01-01

Thin cirrus clouds (optical depth (OD) < 03) are often undetected by standard cloud masking in satellite aerosol retrieval algorithms. However, the Mu]tiangle Imaging Spectroradiometer (MISR) aerosol retrieval has the potential to discriminate between the scattering phase functions of cirrus and aerosols, thus separating these components. Theoretical tests show that MISR is sensitive to cirrus OD within Max{0.05 1 20%l, similar to MISR's sensitivity to aerosol OD, and MISR can distinguish between small and large crystals, even at low latitudes, where the range of scattering angles observed by MISR is smallest. Including just two cirrus components in the aerosol retrieval algorithm would capture typical MISR sensitivity to the natural range of cinus properties; in situations where cirrus is present but the retrieval comparison space lacks these components, the retrieval tends to underestimate OD. Generally, MISR can also distinguish between cirrus and common aerosol types when the proper cirrus and aerosol optical models are included in the retrieval comparison space and total column OD is >-0.2. However, in some cases, especially at low latitudes, cirrus can be mistaken for some combinations of dust and large nonabsorbing spherical aerosols, raising a caution about retrievals in dusty marine regions when cirrus is present. Comparisons of MISR with lidar and Aerosol Robotic Network show good agreement in a majority of the cases, but situations where cirrus clouds have optical depths >0.15 and are horizontally inhomogeneous on spatial scales shorter than 50 km pose difficulties for cirrus retrieval using the MISR standard aerosol algorithm..

Characteristics and composition of atmospheric aerosols in Phimai, central Thailand during BASE-ASIA

NASA Astrophysics Data System (ADS)

Li, Can; Tsay, Si-Chee; Hsu, N. Christina; Kim, Jin Young; Howell, Steven G.; Huebert, Barry J.; Ji, Qiang; Jeong, Myeong-Jae; Wang, Sheng-Hsiang; Hansell, Richard A.; Bell, Shaun W.

2013-10-01

Comprehensive measurements of atmospheric aerosols were made in Phimai, central Thailand (15.183°N, 102.565°E, elevation: 206 m) during the BASE-ASIA field experiment from late February to early May in 2006. The observed aerosol loading was sizable for this rural site (mean aerosol scattering: 108 ± 64 Mm-1; absorption: 15 ± 8 Mm-1; PM10 concentration: 33 ± 17 μg m-3), and dominated by submicron particles. Major aerosol compounds included carbonaceous (OC: 9.5 ± 3.6 μg m-3; EC: 2.0 ± 2.3 μg m-3) and secondary species (SO42-: 6.4 ± 3.7 μg m-3, NH4+: 2.2 ± 1.3 μg m-3). While the site was seldom under the direct influence of large forest fires to its north, agricultural fires were ubiquitous during the experiment, as suggested by the substantial concentration of K+ (0.56 ± 0.33 μg m-3). Besides biomass burning, aerosols in Phimai during the experiment were also strongly influenced by industrial and vehicular emissions from the Bangkok metropolitan region and long-range transport from southern China. High humidity played an important role in determining the aerosol composition and properties in the region. Sulfate was primarily formed via aqueous phase reactions, and hygroscopic growth could enhance the aerosol light scattering by up to 60%, at the typical morning RH level of 85%. The aerosol single scattering albedo demonstrated distinct diurnal variation, ranging from 0.86 ± 0.04 in the evening to 0.92 ± 0.02 in the morning. This experiment marks the first time such comprehensive characterization of aerosols was made for rural central Thailand. Our results indicate that aerosol pollution has developed into a regional problem for northern Indochina, and may become more severe as the region's population and economy continue to grow.

Development of the GC-MS organic aerosol monitor (GC-MS OAM) for in-field detection of particulate organic compounds

NASA Astrophysics Data System (ADS)

Cropper, Paul M.; Overson, Devon K.; Cary, Robert A.; Eatough, Delbert J.; Chow, Judith C.; Hansen, Jaron C.

2017-11-01

Particulate matter (PM) is among the most harmful air pollutants to human health, but due to its complex chemical composition is poorly characterized. A large fraction of PM is composed of organic compounds, but these compounds are not regularly monitored due to limitations in current sampling and analysis techniques. The Organic Aerosol Monitor (GC-MS OAM) combines a collection device with thermal desorption, gas chromatography and mass spectrometry to quantitatively measure the carbonaceous components of PM on an hourly averaged basis. The GC-MS OAM is fully automated and has been successfully deployed in the field. It uses a chemically deactivated filter for collection followed by thermal desorption and GC-MS analysis. Laboratory tests show that detection limits range from 0.2 to 3 ng for 16 atmospherically relevant compounds, with the possibility for hundreds more. The GC-MS OAM was deployed in the field for semi-continuous measurement of the organic markers, levoglucosan, dehydroabietic acid, and polycyclic aromatic hydrocarbons (PAHs) from January to March 2015. Results illustrate the significance of this monitoring technique to characterize the organic components of PM and identify sources of pollution.

Characterization of carbonaceous materials in PM2.5 and PM10 size fractions in Morogoro, Tanzania, during 2006 wet season campaign

NASA Astrophysics Data System (ADS)

Mkoma, Stelyus L.; Chi, Xuguang; Maenhaut, Willy

2010-05-01

Atmospheric aerosol samples in PM10 and PM2.5 size fractions were collected in parallel at a rural site in Morogoro during wet season in March and April 2006. All samples were analysed for the particulate matter mass, for organic, elemental, and total carbon (OC, EC, and TC), and for water-soluble OC (WSOC). The average PM10 and PM2.5 mass concentrations and associated standard deviations were 14 ± 13 μg/m 3 and 7.3 ± 4 μg/m 3 respectively. On average, TC accounted for 33% of the PM10 mass and 44% of the PM2.5 mass for the campaign. The average OC/PM percentage ratios were 27% and 33% in PM10 and PM2.5 size fractions respectively and a larger fraction of the OC was water-soluble. The observed low EC/TC mean percentage ratios of 10-14% respectively for PM10 and PM2.5 fractions indicate that the carbonaceous aerosol originates mainly from biogenic aerosols and/or biomass burning. A simple source apportionment approach was used to apportion the OC to biofuel and charcoal burning. On average, 93% of the PM10 OC was attributed to biofuel and 7% to charcoal burning in the 2006 wet season campaign. However, it is suggested that a contribution to the OC at Morogoro could also come from other natural biogenic matter, and/or biomass burning aerosols. The results for the sources of OC at Morogoro should therefore be considered with great caution.

Carbonaceous film coating

DOEpatents

Maya, Leon

1989-01-01

A method of making a carbonaceous film comprising heating tris(1,3,2-benzodiazaborolo)borazine or dodecahydro tris[1,3,2]diazaborine[1,2-a:1'2'-c:1"2"-e]borazine in an inert atmosphere in the presence of a substrate to a temperature at which the borazine compound decomposes, and the decomposition products deposit onto the substrate to form a thin, tenacious, highly reflective conductive coating having a narrow band gap which is susceptible of modification and a relatively low coefficient of friction.

Carbonaceous film coating

DOEpatents

Maya, L.

1988-04-27

A method of making a carbonaceous film comprising heating tris(1,3,2-benzodiazaborolo)borazine or dodecahydro tris(1,3,2)diazaborine(1,2-a:1'2'-c:1''2''-e)borazine in an inert atmosphere in the presence of a substrate to a temperature at which the borazine compound decomposes, and the decomposition products deposit onto the substrate to form a thin, tenacious, highly reflective conductive coating having a narrow band gap which is susceptible of modification and a relatively low coefficient of friction.

In Situ Aerosol Profile Measurements and Comparisons with SAGE 3 Aerosol Extinction and Surface Area Profiles at 68 deg North

NASA Technical Reports Server (NTRS)

2005-01-01

Under funding from this proposal three in situ profile measurements of stratospheric sulfate aerosol and ozone were completed from balloon-borne platforms. The measured quantities are aerosol size resolved number concentration and ozone. The one derived product is aerosol size distribution, from which aerosol moments, such as surface area, volume, and extinction can be calculated for comparison with SAGE III measurements and SAGE III derived products, such as surface area. The analysis of these profiles and comparison with SAGE III extinction measurements and SAGE III derived surface areas are provided in Yongxiao (2005), which comprised the research thesis component of Mr. Jian Yongxiao's M.S. degree in Atmospheric Science at the University of Wyoming. In addition analysis continues on using principal component analysis (PCA) to derive aerosol surface area from the 9 wavelength extinction measurements available from SAGE III. Ths paper will present PCA components to calculate surface area from SAGE III measurements and compare these derived surface areas with those available directly from in situ size distribution measurements, as well as surface areas which would be derived from PCA and Thomason's algorithm applied to the four wavelength SAGE II extinction measurements.

Distribution and radiative forcing of Asian dust and anthropogenic aerosols from East Asia simulated by SPRINTARS

NASA Astrophysics Data System (ADS)

Takemura, T.; Nakajima, T.; Uno, I.

2002-12-01

A three-dimensional aerosol transport-radiation model, SPRINTARS (Spectral Radiation-Transport Model for Aerosol Species), has been developed based on an atmospheric general circulation model of the Center for Climate System Research, University of Tokyo/National Institute for Environmental Studies, Japan to research the effects of aerosols on the climate system and atmospheric environment. SPRINTARS successfully simulates the long-range transport of the large-scale Asian dust storms from East Asia to North America by crossing the North Pacific Ocean in springtime 2001 and 2002. It is found from the calculated dust optical thickness that 10 to 20% of Asian dust around Japan reached North America. The simulation also reveals the importance of anthropogenic aerosols, which are carbonaceous and sulfate aerosols emitted from the industrialized areas in the East Asian continent, to air turbidity during the large-scale Asian dust storms. The simulated results are compared with a volume of observation data regarding the aerosol characteristics over East Asia in the spring of 2001 acquired by the intensive observation campaigns of ACE-Asia (Asian Pacific Regional Aerosol Characterization Experiment) and APEX (Asian Atmospheric Particulate Environmental Change Studies). The comparisons are carried out not only for aerosol concentrations but also for aerosol optical properties, such as optical thickness, Angstrom exponent which is a size index calculated by the log-slope exponent of the optical thickness between two wavelengths, and single scattering albedo. The consistence of Angstrom exponent between the simulation and observations means the reasonable simulation of the ratio of anthropogenic aerosols to Asian dust, which supports the suggestion by the simulation on the importance of anthropogenic aerosols to air turbidity during the large-scale Asian dust storms. SPRINTARS simultaneously calculates the aerosol direct and indirect radiative forcings. The direct radiative

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

NASA Astrophysics Data System (ADS)

Ulevicius, V.; Byčenkienė, S.; Bozzetti, C.; Vlachou, A.; Plauškaitė, K.; Mordas, G.; Dudoitis, V.; Abbaszade, G.; Remeikis, V.; Garbaras, A.; Masalaite, A.; Blees, J.; Fröhlich, R.; Dällenbach, K. R.; Canonaco, F.; Slowik, J. G.; Dommen, J.; Zimmermann, R.; Schnelle-Kreis, J.; Salazar, G. A.; Agrios, K.; Szidat, S.; El Haddad, I.; Prévôt, A. S. H.

2015-09-01

In early spring the Baltic region is frequently affected by high pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m-3 and black carbon (BC) up to 17 μg m-3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26-44 % and 13-23 % to the TC, respectively. 5-8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4-13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13-24 % and 7-12 %, respectively. Isotope ratio of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe