Department of Chemistry, University of Vermont , Burlington, Vermont 05405, United States.
School of Engineering and Applied Sciences, Harvard University , Cambridge, Massachusetts 02138, United States.
Environ Sci Technol. 2016 May 17;50(10):4997-5006. doi: 10.1021/acs.est.6b00625. Epub 2016 Apr 27.
Atmospheric aerosols play an important role in Earth's radiative balance directly, by scattering and absorbing radiation, and indirectly, by acting as cloud condensation nuclei (CCN). Atmospheric aerosol is dominated by secondary organic aerosol (SOA) formed by the oxidation of biogenic volatile organic compounds (BVOCs). Green leaf volatiles (GLVs) are a class of BVOCs that contribute to SOA, yet their role in the Earth's radiative budget is poorly understood. In this work we measured the scattering efficiency (at 450, 525, and 635 nm), absorption efficiency (between 190 and 900 nm), particle phase, bulk chemical properties (O:C, H:C), and molecular-level composition of SOA formed from the ozonolysis of two GLVs: cis-3-hexenol (HXL) and cis-3-hexenyl acetate (CHA). Both HXL and CHA produced SOA that was weakly absorbing, yet CHA-SOA was a more efficient absorber than HXL-SOA. The scatter efficiency of SOA from both systems was wavelength-dependent, with the stronger dependence exhibited by HXL-SOA, likely due to differences in particle size. HXL-SOA formed under both dry (10% RH) and wet (70% RH) conditions had the same bulk chemical properties (O:C), yet significantly different optical properties, which was attributed to differences in molecular-level composition. We have found that SOA derived from green leaf volatiles has the potential to affect the Earth's radiative budget, and also that bulk chemical properties can be insufficient to predict SOA optical properties.
大气气溶胶通过散射和吸收辐射直接在地球辐射平衡中发挥重要作用,通过作为云凝结核(CCN)间接发挥作用。大气气溶胶主要由生物源挥发性有机化合物(BVOCs)氧化形成的次生有机气溶胶(SOA)组成。绿叶挥发物(GLVs)是一类BVOCs,它们对 SOA 有贡献,但它们在地球辐射预算中的作用还不太清楚。在这项工作中,我们测量了由两种 GLVs 的臭氧氧化形成的 SOA 的散射效率(在 450、525 和 635nm 处)、吸收效率(在 190 和 900nm 之间)、颗粒相、体相化学性质(O:C、H:C)和分子水平组成。顺-3-己烯醇(HXL)和顺-3-己烯基乙酸酯(CHA)。HXL 和 CHA 都产生了 SOA,其吸收能力较弱,但 CHA-SOA 的吸收效率高于 HXL-SOA。两种体系形成的 SOA 的散射效率都随波长而变化,HXL-SOA 的依赖性更强,这可能是由于粒径的不同。在干燥(10%RH)和潮湿(70%RH)条件下形成的 HXL-SOA 具有相同的体相化学性质(O:C),但光学性质却有很大差异,这归因于分子水平组成的差异。我们已经发现,源自绿叶挥发物的 SOA 有可能影响地球的辐射预算,并且体相化学性质可能不足以预测 SOA 的光学性质。