Abstract. Carbonaceous aerosols affect the radiative balance of the Earth by absorbing and scattering light. While black carbon (BC) is highly absorbing, some organic carbon (OC) also has significant absorption, especially at near-ultraviolet and blue wavelengths. To the extent that OC absorbs visible light, it may be a non-negligible contributor to positive direct aerosol radiative forcing. Quantification of that absorption is necessary so that radiative-transfer models can evaluate the net radiative effect of OC. In this work, we examine absorption by primary OC emitted from solid fuel pyrolysis. We provide absorption spectra of this material, which can be related to the imaginary refractive index. This material has polar character but is not fully water-soluble: more than 92% was extractable by methanol or acetone, compared with 73% for water and 52% for hexane. Water-soluble OC contributes to light absorption at both ultraviolet and visible wavelengths. However, a larger portion of the absorption comes from OC that is extractable only by methanol. Absorption spectra of water-soluble OC are similar to literature reports. We compare spectra for material generated with different wood type, wood size and pyrolysis temperature. Higher wood temperature is the main factor creating OC with higher absorption; changing wood temperature from a devolatilizing state of 210 °C to a near-flaming state of 360 °C causes about a factor of four increase in mass-normalized absorption at visible wavelengths. A clear-sky radiative transfer model suggests that, despite the absorption, both high-temperature and low-temperature OC result in negative top-of-atmosphere radiative forcing over a surface with an albedo of 0.19 and positive radiative forcing over bright surfaces. Unless absorption by real ambient aerosol is higher than that measured here, it probably affects global average clear-sky forcing very little, but could be important in energy balances over bright surfaces.

Light Absorption by Organic Carbon From Wood Combustion

Abstract. A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.

Using the OMI Aerosol Index and Absorption Aerosol Optical Depth to Evaluate the NASA MERRA Aerosol Reanalysis.

. The light-absorbing organic aerosol (OA) commonly referred to as “brown carbon” (BrC) has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various volatile organic carbon (VOC) precursors, NOx concentrations, photolysis time, and relative humidity (RH) on the light absorption of selected secondary organic aerosols (SOA). Light absorption of chamber-generated SOA samples, especially aromatic SOA, was found to increase with NOx concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficient (MAC) value is observed from toluene SOA products formed under high-NOx conditions at moderate RH, in which nitro-aromatics were previously identified as the major light-absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organic nitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible (Vis) and ultraviolet (UV) light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.

Optical Properties and Aging of Light Absorbing Secondary Organic Aerosol

Abstract. Light absorbing organic carbon, often called brown carbon, has the potential to significantly contribute to the visible light-absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon, are poorly understood. With this in mind size-resolved direct measurements of brown carbon were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a representative urban site and a road-side site adjacent to a main highway. Fine particle absorption was measured with a multi-angle absorption photometer (MAAP) and seven-wavelength Aethalometer, and brown carbon absorption was estimated based on Mie calculations using direct size-resolved measurements of chromophores in solvents. Size-resolved samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light-absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with the highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The direct size-resolved measurement of brown carbon in solution definitively shows that it is present and optically important in the near-UV range in both a rural and urban environment during the summer when biomass burning emissions are low. These results allow estimates of brown carbon aerosol absorption from direct measurements of chromophores in aerosol extracts.

Size-Resolved Measurements of Brown Carbon in Water and Methanol Extracts and Estimates of Their Contribution to Ambient Fine Particle Light Absorption

Spatial distribution and sources of potentially toxic elements in road dust and its PM10 fraction of Moscow megacity.

Spatially resolved distribution, sources and health risks of heavy metals in size-fractionated road dust from 57 sites across megacity Kolkata, India.

Optical properties of aerosol brown carbon (BrC) in the eastern Indo-Gangetic Plain

Regional sulfate drives long-term rise in AOD over megacity Kolkata, India

This study was carried out to determine sources and health risks of fine particulate (PM2.5) bound polycyclic aromatic hydrocarbons (PAHs) and carbonaceous species in the ambient atmosphere of Delhi. Aerosol samples were collected from October 2017 to September 2018 in an institutional cum residential area of Delhi. Annual PM2.5 level was found to be 124.3 ± 107.6 µg/m3 which exceeded the Indian National Ambient Air Quality Standard (NAAQS) by over three times. Sixteen US EPA priority PAHs’ concentration exhibited a seasonal trend of winter > monsoon > summer with annual mean level of 83.6 ± 48.0 ng/m3. Winter and summer (p   summer ≈ monsoon. Molecular diagnostic ratios and principal component analysis identified vehicular emission as the leading source of these species followed by biomass and coal combustion, industrial emissions, and volatilization of petroleum and its products. Regional and trans-boundary incursion of pollutants was also identified with the help of back trajectories and concentration weighted trajectories. Carcinogenic PAHs contributed 41.4% to the aerosol PAHs load. Incremental cancer risk assessment estimated 25 additional cancer cases per million population due to lifetime inhalation exposure to PAHs at their observed concentration in Delhi.

Fine Particulate Matter Bound Polycyclic Aromatic Hydrocarbons and Carbonaceous Species in Delhi’s Atmosphere: Seasonal Variation, Sources, and Health Risk Assessment

Prashant Rawat

Papers

Spatially resolved distribution, sources and health risks of heavy metals in size-fractionated road dust from 57 sites across megacity Kolkata, India.

Optical properties of aerosol brown carbon (BrC) in the eastern Indo-Gangetic Plain

Regional sulfate drives long-term rise in AOD over megacity Kolkata, India

Fine Particulate Matter Bound Polycyclic Aromatic Hydrocarbons and Carbonaceous Species in Delhi’s Atmosphere: Seasonal Variation, Sources, and Health Risk Assessment