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DOI | 10.5194/acp-22-14825-2022 |
Constraining the particle-scale diversity of black carbon light absorptionusing a unified framework | |
Beeler, Payton; Chakrabarty, Rajan K. | |
发表日期 | 2022 |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
起始页码 | 14825 |
结束页码 | 14836 |
卷号 | 22期号:22页码:12 |
英文摘要 | Atmospheric black carbon (BC), the strongest absorber of visible solar radiation in the atmosphere, manifests across a wide spectrum of morphologies and compositional heterogeneity. Phenomenologically, the distribution of BC among diverse particles of varied composition gives rise to enhancement of its light absorption capabilities by over twofold in comparison to that of nascent or unmixed homogeneous BC. This situation has challenged the modeling community to consider the full complexity and diversity of BC on a per-particle basis for accurate estimation of its light absorption. The conventionally adopted core-shell approximation, although computationally inexpensive, is inadequate not only in estimating but also capturing absorption trends for ambient BC. Here we develop a unified framework that encompasses the complex diversity in BC morphology and composition using a single metric, the phase shift parameter (rho BC), which quantifies how much phase shift the incoming light waves encounter across a particle compared to that in its absence. We systematically investigate variations in rho BC across the multi-space distribution of BC morphology, mixing state, mass, and composition as reported by field and laboratory observations. We find that rho BC > 1 leads to decreased absorption by BC, which explains the weaker absorption enhancements observed in certain regional BC compared to laboratory results of similar mixing state. We formulate universal scaling laws centered on rho BC and provide physics-based insights regarding core-shell approximation overestimating BC light absorption. We conclude by packaging our framework in an open-source Python application to facilitate community-level use in future BC-related research. The package has two main functionalities. The first functionality is for forward problems, wherein experimentally measured BC mixing state and assumed BC morphology are input, and the aerosol absorption properties are output. The second functionality is for inverse problems, wherein experimentally measured BC mixing state and absorption are input, and the morphology of BC is returned. Further, if absorption is measured at multiple wavelengths, the package facilitates the estimation of the imaginary refractive index of coating materials by combining the forward and inverse procedures. Our framework thus provides a computationally inexpensive source for calculation of absorption by BC and can be used to constrain light absorption throughout the atmospheric lifetime of BC. |
学科领域 | Environmental Sciences; Meteorology & Atmospheric Sciences |
语种 | 英语 |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
WOS记录号 | WOS:000890918300001 |
来源期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/273065 |
作者单位 | Washington University (WUSTL) |
推荐引用方式 GB/T 7714 | Beeler, Payton,Chakrabarty, Rajan K.. Constraining the particle-scale diversity of black carbon light absorptionusing a unified framework[J],2022,22(22):12. |
APA | Beeler, Payton,&Chakrabarty, Rajan K..(2022).Constraining the particle-scale diversity of black carbon light absorptionusing a unified framework.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(22),12. |
MLA | Beeler, Payton,et al."Constraining the particle-scale diversity of black carbon light absorptionusing a unified framework".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.22(2022):12. |
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