Carbonaceous aerosols cause strong atmospheric heating and large surface cooling that is as important to South Asian climate forcing as greenhouse gases, yet the aerosol sources are poorly understood. Emission inventory models suggest that biofuel burning accounts for 50 to 90% of emissions, whereas the elemental composition of ambient aerosols points to fossil fuel combustion. We used radiocarbon measurements of winter monsoon aerosols from western India and the Indian Ocean to determine that biomass combustion produced two-thirds of the bulk carbonaceous aerosols, as well as one-half and two-thirds of two black carbon subfractions, respectively. These constraints show that both biomass combustion (such as residential cooking and agricultural burning) and fossil fuel combustion should be targeted to mitigate climate effects and improve air quality.

[1] Throughout South Asia biomass is commonly used as a fuel source for cooking and heating homes. The smoke from domestic use of these fuels is expected to be a major source of atmospheric particulate matter in the region and needs to be characterized for input in regional source apportionment models and global climate models. Biomass fuel samples including coconut leaves, rice straw, jackfruit branches, dried cowdung patties, and biomass briquettes manufactured from compressed biomass material were obtained from Bangladesh. The fuel samples were burned in a wood stove to collect and characterize the particulate matter emissions. The bulk chemical composition including total organic and elemental carbon, sulfate, nitrate, ammonium and chloride ions, and bulk elements such as potassium and sodium did not show conclusive differences among the biomass samples tested. Unique features, however, exist in the detailed organic characterization of the combustion smoke from the different sources. The organic compound fingerprints of the particulate matter are shown to be distinct from one another and distinct from North American wood fuels. Fecal stanols including 5b-stigmastanol, coprostanol, and cholestanol are found to be good molecular markers for the combustion of cowdung. Additionally, the patterns of methoxyphenols and plant sterols provide a unique signature for each biomass sample and are conducive as source apportionment tracers.

[1] Water-soluble organic carbon (WSOC) is typically a large component of carbonaceous aerosols with a high propensity for inducing cloud formation. The sources of WSOC, which may be both of primary and secondary origins, are in general poorly constrained. This study assesses the concentrations and dual-carbon isotope ( 14 C and 13 C) signatures of South Asian WSOC during a 15-month continuous campaign in [2008][2009]. Total suspended particulate matter samples were collected at Sinhagad (SINH) India and at the Maldives Climate Observatory at Hanimaadhoo (MCOH). Monsoon-driven meteorology yields significant WSOC concentration differences between the dry winter season (0.94 AE 0.43 mg m À3 MCOH and 3.6 AE 2.3 mg m À3 SINH) and the summer monsoon season (0.10 AE 0.04 mg m À3 MCOH and 0.35 AE 0.21 mg m À3 SINH). Radiocarbon-based source apportionment of WSOC not only shows the dominance of biogenic/biomass combustion sources but also a substantial anthropogenic fossil-fuel contribution (17 AE 4% MCOH and 23 AE 4% SINH). Aerosols reaching MCOH after long-range over-ocean transport were enriched by 3-4% in d 13 C-WSOC relative to SINH. This is consistent with particle-phase aging processes influencing the d 13 C-WSOC signal in the South Asian regional receptor atmosphere.Citation: Kirillova, E. N., A. Andersson, R. J. Sheesley, M. Krusa˚, P. S. Praveen, K. Budhavant, P. D. Safai, P. S. P. Rao, and Ö . Gustafsson (2013), 13 C-and 14 C-based study of sources and atmospheric processing of water-soluble organic carbon

Prescribed burning is a significant source of fine particulate matter (PM2.5) in the southeastern United States. However, limited data exist on the emission characteristics from this source. Various organic and inorganic compounds both in the gas and particle phase were measured in the emissions of prescribed burnings conducted at two pine-dominated forest areas in Georgia. The measurements of volatile organic compounds (VOCs) and PM2.5 allowed the determination of emission factors for the flaming and smoldering stages of prescribed burnings. The VOC emission factors from smoldering were distinctly higher than those from flaming except for ethene, ethyne, and organic nitrate compounds. VOC emission factors show that emissions of certain aromatic compounds and terpenes such as alpha and beta-pinenes, which are important precursors for secondary organic aerosol (SOA), are much higher from active prescribed burnings than from fireplace wood and laboratory open burning studies. Levoglucosan is the major particulate organic compound (POC) emitted for all these studies, though its emission relative to total organic carbon (mg/g OC) differs significantly. Furthermore, cholesterol, an important fingerprint for meat cooking, was observed only in our in situ study indicating a significant release from the soil and soil organisms during open burning. Source apportionment of ambient primary fine particulate OC measured at two urban receptor locations 20-25 km downwind yields 74 +/- 11% during and immediately after the burns using our new in situ profile. In comparison with the previous source profile from laboratory simulations, however, this OC contribution is on average 27 +/- 5% lower.

Abstract. Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiaġvik, formerly known as Barrow (Alaska), Ny-Ålesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Ålesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to −5 ∘C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.

Ambient PM2.5 samples were collected in five midwestern United States cities throughout 2004: East St. Louis, Illinois; Detroit Michigan; Cincinnati, Ohio; Bondville, Illinois; and Northbrook, Illinois. Monthly composites were analyzed using chemical derivatization coupled with GC-MS analysis to estimate the contributions of several sources to the total ambient organic carbon. A chemical mass balance (CMB) approach was used to estimate contributions from several primary sources. An additional, organic tracer-based technique was employed to estimate secondary contributions, including secondary organic carbon derived from isoprene, alpha-pinene, beta-caryophyllene, and toluene. The sum of these contributions was compared with the total organic carbon measured at each sampling site, and reasonable carbon mass balances were observed for four of the five sites. In Bondville, Northbrook, Cincinnati, and Detroit a strong correlation was observed between the sum of the estimated primary and secondary contributions and the measured organic carbon (R2 = 0.73). The estimated secondary organic carbon concentrations were observed to vary considerably with season, with the strongest contributions coming from isoprene and alpha-pinene during the summer. While further research is required, there is some evidence that the contribution estimates for alpha-pinene, beta-caryophyllene, and toluene SOC may to some degree represent the contributions from the broader classes of monoterpenes, sesquiterpenes, and aromatics.

Abstract. Organic carbon (OC) comprises a large fraction of fine particulate matter (PM 2.5 ) in Mexico City. Daily and select 12-h PM 2.5 samples were collected in urban and peripheral sites in Mexico City from 17-30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time watersoluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 49% of OC in the urban area and 32% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5-26% at the urban site and 7-39% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MI-LAGRO 2006 field campaign.

Abstract. Organic carbon (OC) comprises a large fraction of fine particulate matter (PM2.5) in Mexico City. Daily and select 12-h PM2.5 samples were collected in urban and peripheral sites in Mexico City from 17–30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time water-soluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 47% of OC in the urban area and 31% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5–30% at the urban site and 11–50% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MILAGRO 2006 field campaign.