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模拟有机气溶胶光吸收的复杂性

Complexities in Modeling Organic Aerosol Light Absorption.

作者信息

Gorkowski Kyle, Benedict Katherine B, Carrico Christian M, Dubey Manvendra K

机构信息

Earth and Environmental Science, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.

New Mexico Institute of Mining and Technology, Socorro, New Mexico 87801, United States.

出版信息

J Phys Chem A. 2022 Jul 28;126(29):4827-4833. doi: 10.1021/acs.jpca.2c02236. Epub 2022 Jul 14.

Abstract

Aerosol particles dynamically evolve in the atmosphere by physicochemical interactions with sunlight, trace chemical species, and water. Current modeling approaches fix properties such as aerosol refractive index, introducing spatial and temporal errors in the radiative impacts. Further progress requires a process-level description of the refractive indices as the particles age and experience physicochemical transformations. We present two multivariate modeling approaches of light absorption by brown carbon (BrC). The initial approach was to extend the modeling framework of the refractive index at 589 nm (), but that result was insufficient. We developed a second multivariate model using aromatic rings and functional groups to predict the imaginary part of the complex refractive index. This second model agreed better with measured spectral absorption peaks, showing promise for a simplified treatment of BrC optics. In addition to absorption, organic functionalities also alter the water affinity of the molecules, leading to a hygroscopic uptake and increased light absorption, which we show through measurements and modeling.

摘要

气溶胶颗粒通过与阳光、痕量化学物质和水的物理化学相互作用在大气中动态演变。当前的建模方法固定了诸如气溶胶折射率等属性,从而在辐射影响方面引入了空间和时间误差。进一步的进展需要对颗粒老化和经历物理化学转变时的折射率进行过程级描述。我们提出了两种棕色碳(BrC)光吸收的多变量建模方法。最初的方法是扩展589纳米处折射率的建模框架(),但该结果并不充分。我们开发了第二个多变量模型,使用芳香环和官能团来预测复折射率的虚部。这第二个模型与测量的光谱吸收峰吻合得更好,显示出对BrC光学进行简化处理的前景。除了吸收外,有机官能团还会改变分子的亲水性,导致吸湿摄取并增加光吸收,我们通过测量和建模展示了这一点。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4a82/9340763/d638bfc6693d/jp2c02236_0001.jpg

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