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