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Estimation of aerosol radiative forcing continues to suffer from large uncertainties, partially from a lack of observations of aerosol optical properties. Limited measurements of the atmospheric aerosol imaginary refractive index (iRI) have been made, especially in some of the world's most polluted regions. In this study, we measured aerosol optical and micro-physical properties at a regional site, Rohtak, India, representative of polluted cities in the Indo-Gangetic plains in northern India. The average PM2.5 measured during the campaign was 163 mu g/m(3) with a single-scatter albedo of 0.7, indicating the presence of strongly absorbing aerosol components. Measurements of aerosol absorption, scattering, and particle number size distributions were used to estimate the effective refractive index using an established Mie inversion technique. The calculated iRI was spectrally invariant in the visible region with values ranging between 0.076 and 0.145. Brown carbon absorption, estimated using an existing Mie optimization method, ranged 34-88 Mm(-1), with strongly absorbing mass absorption cross-sections (similar to 1.9 m(2)/g). Higher iRI were observed during periods with higher brown carbon absorption, which are likely directly emitted from combustion sources. Low volatility organic carbon fractions dominated during these periods, with likely persistence of atmospheric absorption. The iRI values are at the upper end of previously reported ranges of urban aerosol iRI. In a sensitivity analysis to measured parameters, the absorption had the dominant effect on estimated iRI. Measured single scatter albedos, were lower than those from climate model simulations over the region, demonstrating the need for intrinsic property measurements to evaluate and constrain climate models.

期刊论文 2023-07-27 DOI: 10.1029/2022JD038272 ISSN: 2169-897X

Effective density (peff) is an important property describing particle transportation in the atmosphere and in the human respiratory tract. In this study, the particle size dependency of peff was determined for fresh and photochemically aged particles from residential combustion of wood logs and brown coal, as well as from an aerosol standard (CAST) burner. peff increased considerably due to photochemical aging, especially for soot agglomerates larger than 100 nm in mobility diameter. The increase depends on the presence of condensable vapors and agglomerate size and can be explained by collapsing of chain-like agglomerates and filling of their voids and formation of secondary coating. The measured and modeled particle optical properties suggest that while light absorption, scattering, and the single-scattering albedo of soot particle increase during photochemical processing, their radiative forcing remains positive until the amount of nonabsorbing coating exceeds approximately 90% of the particle mass.

期刊论文 2023-04-04 DOI: 10.1021/acs.est.2c04151 ISSN: 0013-936X
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