Sobhan Kumar Kompalli
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Surendran Nair Suresh Babu
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Krishnaswamy Krishnamoorthy
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Sreedharan Krishnakumari Satheesh
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Mukunda M. Gogoi
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Abstract. Regional climatic implications of aerosol black carbon (BC) are well recognized over South Asia, which has a wide variety of anthropogenic sources in a large abundance. Significant uncertainties remain in its quantification due to lack of sufficient information on the microphysical properties (its concentration, size, and mixing state with other aerosol components), which determine the absorption potential of BC. Especially the information on mixing state of BC is extremely sparse over this region. In this study, first-ever observations of the size distribution and mixing state of individual refractory black carbon (rBC) particles in the south Asian outflow to Southeastern Arabian Sea, northern and equatorial Indian Ocean regions are presented based on measurements using a single particle soot photometer (SP2) aboard the ship cruise of the Integrated Campaign for Aerosols, gases, and Radiation Budget (ICARB-2018) during winter-2018 (16 January to 13 February). The results revealed significant spatial heterogeneity of BC characteristics. Highest rBC mass concentrations (~ 938 ± 293 ng m−3) with the highest relative coating thickness (RCT; the ratio of BC core to its coating diameters) of ~ 2.16 ± 0.19 are found over the Southeast Arabian Sea (SEAS) region, which is in the proximity of the continental outflow. As we move to farther oceanic regions, though the mass concentrations decreased by nearly half (~ 546 ± 80 ng m−3), BC still remained thickly coated (RCT ~ 2.05 ± 0.07). The air over the remote equatorial Indian Ocean, which received considerable marine air masses compared to the other regions, showed the lowest rBC mass concentrations (~ 206 ± 114 ng m−3), with a moderately thick coating (RCT ~ 1.73 ± 0.16). Even over oceanic regions far from the landmass, regions which received the outflow from more industrialized east coast/the Bay of Bengal had thicker coating (~ 104 nm) compared to regions that received outflow from the west coast/peninsular India (~ 86 nm). Although different regions of the ocean depicted contrasting concentrations and mixing state parameters due to varying extent and nature of the continental outflow as well as the atmospheric lifetime of air masses, the modal parameters of rBC mass-size distributions were similar over all the regions. The observed mono-modal distribution with mean mass median diameters (MMD) in the range of 0.19–0.20 μm suggested mixed sources of BC. The mean fraction of BC containing particles (FBC) varied in the range 0.20–0.28 (suggesting significant amounts of non-BC particles), whereas the bulk mixing ratio of coating mass to rBC mass was highest (8.77 ± 2.77) over the outflow regions compared to the remote ocean (4.29 ± 1.54) highlighting the role of outflow in providing condensable material for coating on rBC. These parameters, along with the information on size-resolved mixing state of BC cores, throw light on the role of sources and secondary processing of their complex mixtures for coating on BC under highly polluted conditions. Examination of the non-refractory sub-micrometre aerosol chemical composition obtained using the aerosol chemical speciation monitor (ACSM) suggested that the overall aerosol system was sulfate dominated over the far-oceanic regions. In contrast, organics were equally prominent adjacent to the coastal landmass. Association between the BC mixing state and aerosol chemical composition suggested that sulfate was the probable dominant coating material on rBC cores.
Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization
