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There is a large uncertainty in evaluating the radiative forcing from aerosol-radiation and aerosol-cloud interactions clue to the limited knowledge on aerosol properties. In-situ measurements of aerosol physical and chemical properties were carried out in 2012 at Mt. Huang (the Yellow Mountain), a continental background mountainous site in eastern China. An aerosol optical closure study was performed to verify the model outputs by using the measured aerosol optical properties, in which a spherical Mie model with assumptions of external and core shell mixtures on the basis of a two-component optical aerosol model and high size-segregated element carbon (EC) ratio was applied. Although the spherical Mie model would underestimate the real scattering with increasing particle diameters, excellent agreement between the calculated and measured values was achieved with correlation coefficients above 0.98. Sensitivity experiments showed that the EC ratio had a negligible effect on the calculated scattering coefficient, but largely influenced the calculated absorption coefficient. The high size segregated EC ratio averaged over the study period in the closure was enough to reconstruct the aerosol absorption coefficient in the Mie model, indicating EC size resolution was more important than time resolution in retrieving the absorption coefficient in the model. The uncertainties of calculated scattering and absorption coefficients due to the uncertainties of measurements and model assumptions yielded by a Monte Carlo simulation were +/- 6% and +/- 14% for external mixture and +/- 9% and +/- 31% for core-shell mixture, respectively. This study provided an insight into the inherent relationship between aerosol optical properties and physicochemical characteristics in eastern China, which could supplement the database of aerosol optical properties for background sites in eastern China and provide a method for regions with similar climate. (C) 2016 Elsevier B.v. All rights reserved.

期刊论文 2016-04-15 DOI: 10.1016/j.scitotenv.2016.01.205 ISSN: 0048-9697

Aerosols contribute the largest uncertainty to the total radiative forcing estimate, and black carbon (BC) that absorbs solar radiation plays an important role in the Earth's energy budget. This study analysed the aerosol optical properties from 22 February to 18 March 2014 at the China Meteorological Administration Atmospheric Watch Network (CAWNET) station in the Pearl River Delta (PRD), China. The representative values of dry-state particle scattering coefficient (sigma(sp)), hemispheric backscattering coefficient (sigma(hbsp)), absorption coefficient (sigma(absp)), extinction coefficient (sigma(ep)), hemispheric backscattering fraction (HBF), single scattering albedo (SSA), as well as scattering Angstrom exponent (alpha) were presented. A comparison between a polluted day and a clean day shows that the aerosol optical properties depend on particle number size distribution, weather conditions and evolution of the mixing layer. To investigate the mixing state of BC at the surface, an optical closure study of HBF between measurements and calculations based on a modified Mie model was employed for dry particles. The result shows that the mixing state of BC might be between the external mixture and the core-shell mixture. The average retrieved ratio of the externally mixed BC to the total BC mass concentration (r(ext-Bc)) was 0.58 +/- 0.12, and the diurnal pattern of r(ext-Bc) can be found. Furthermore, considering that non-light-absorbing particles measured by a Volatility-Tandem Differential Mobility Analyser (V-TDMA) exist independently with core-shell and homogenously internally mixed BC particles, the calculated optical properties were just slightly different from those based on the assumption that BC exist in each particle. This would help understand the influence of the BC mixing state on aerosol optical properties and radiation budget in the PRD. (C) 2016 Elsevier Ltd. All rights reserved.

期刊论文 2016-04-01 DOI: 10.1016/j.atmosenv.2016.02.003 ISSN: 1352-2310
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