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一次有机气溶胶排放物的光吸收特性和辐射效应。

Light absorption properties and radiative effects of primary organic aerosol emissions.

机构信息

†Energy Systems Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, United States.

‡Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, 205 North Mathews Avenue, Urbana, Illinois 61801, United States.

出版信息

Environ Sci Technol. 2015 Apr 21;49(8):4868-77. doi: 10.1021/acs.est.5b00211. Epub 2015 Apr 9.

Abstract

Organic aerosols (OAs) in the atmosphere affect Earth's energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called "brown carbon" (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (kOA, the fundamental optical parameter determining the particle's absorptivity) and their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the kOA of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based kOA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated kOA values of sectoral and total POA emissions are presented. Results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to ∼27% reduction in the amount of the net global average POA cooling compared to results from the nonabsorbing assumption.

摘要

大气中的有机气溶胶 (OAs) 通过存在所谓的“棕色碳” (BrC) 成分不仅散射而且吸收太阳辐射,从而影响地球的能量平衡。然而,目前的气候和化学输送模型并没有表示或不能很好地表示 OAs 的吸收率。在这项研究中,我们提供了一种方法,使用最近的实验室和现场观测来限制排放清单水平上的 BrC 吸收率。我们回顾了光吸收原始 OA (POA) 的可用测量值,并量化了从生物质/生物燃料、褐煤、丙烷和油燃烧源排放的整体 POA 的波长相关虚折射指数 (kOA,决定颗粒吸收率的基本光学参数) 及其不确定性。特别是,我们将生物质/生物燃料燃烧源的 kOA 参数化为 BC 与 OA 之比的函数,表明 POA 的吸收特性强烈依赖于燃烧条件。基于燃料类型的 kOA 分布被纳入全球含碳气溶胶排放清单,并提出了部门和总 POA 排放的综合 kOA 值。简单辐射传输模型的结果表明,POA 的吸收率显著使大气变暖,并导致与不吸收假设相比,全球平均净 POA 冷却量减少约 27%。

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