Organic Matrix Effect on the Molecular Light Absorption of Brown Carbon

Brown carbon (BrC) absorption impacts radiative forcing and climate change. Quantifying radiative forcing of BrC requires understanding its molecular composition and absorption characteristics. While organic molecules surrounding BrC may impact its absorption, their effects have not yet been investi...

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Veröffentlicht in:Geophysical research letters 2023-12, Vol.50 (24), p.n/a
Hauptverfasser: Zhang, Antai, Zeng, Yaling, Yang, Xin, Zhai, Jinghao, Wang, Yixiang, Xing, Chunbo, Cai, Baohua, Shi, Shao, Zhang, Yujie, Shen, Zhenxing, Fu, Tzung‐May, Zhu, Lei, Shen, Huizhong, Ye, Jianhuai, Wang, Chen
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Sprache:eng
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Zusammenfassung:Brown carbon (BrC) absorption impacts radiative forcing and climate change. Quantifying radiative forcing of BrC requires understanding its molecular composition and absorption characteristics. While organic molecules surrounding BrC may impact its absorption, their effects have not yet been investigated. This research determined matrix effect on BrC absorption by comparing individual BrC molecules and BrC within an organic matrix. Over 20,000 water‐soluble organic molecules constituted the water‐soluble BrC and associated organic matrix. The matrix enhanced aliphatic BrC absorption but suppressed aromatic BrC, especially with higher matrix O/C ratios indicating greater polarity and acidity. By directly measuring and modeling organic matrix effect on BrC, we can improve climate prediction precision and aerosol‐radiation interaction comprehension. Plain Language Summary In the atmosphere, organic carbon that absorb light are called brown carbon. Brown carbon can impact climate change. It is critical to understand potential factors affecting brown carbon's absorption of light. Our study proposed another potential influencing light absorbing of brown carbon, effect from organic matrix formed by co‐existing organic molecules. The matrix effect on brown carbon absorption was simulated by the absorption properties of individual molecules and the absorption contributions from the same molecules embedded within organic matrix. We found over 20,000 molecules in all samples, separating them into major contributing brown carbon molecules and co‐existing organic molecules. We found CHO and CHON formed the majority of these molecules. The organic matrix showed the different behavior to effect light absorption to different portion for organic molecules, namely aliphatic and aromatic brown carbon molecules. The brown carbon absorption was suppressed during the nighttime, with the high O/C ratio co‐existing organics. Through the direct measurement and modeling of organic matrix effect on brown carbon, the finding could improve the precision of climate predictions and enhance our comprehension of aerosol‐radiation interactions. Key Points Organic molecules co‐existing around brown carbon constituted the organic matrix The organic matrix enhanced aliphatic but suppressed aromatic brown carbon absorption Higher matrix O/C ratios indicating greater polarity and acidity especially suppressed aromatic brown carbon absorption
ISSN:0094-8276
1944-8007
DOI:10.1029/2023GL106541