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一种基于观测的远程海洋对流层氧化简化模型。

An observation-based, reduced-form model for oxidation in the remote marine troposphere.

作者信息

Baublitz Colleen B, Fiore Arlene M, Ludwig Sarah M, Nicely Julie M, Wolfe Glenn M, Murray Lee T, Commane Róisín, Prather Michael J, Anderson Daniel C, Correa Gustavo, Duncan Bryan N, Follette-Cook Melanie, Westervelt Daniel M, Bourgeois Ilann, Brune William H, Bui T Paul, DiGangi Joshua P, Diskin Glenn S, Hall Samuel R, McKain Kathryn, Miller David O, Peischl Jeff, Thames Alexander B, Thompson Chelsea R, Ullmann Kirk, Wofsy Steven C

机构信息

Department of Earth and Environmental Sciences, Columbia University, New York, NY 10027.

Division of Ocean and Climate Physics, Lamont-Doherty Earth Observatory of Columbia University, Palisades, NY 10964.

出版信息

Proc Natl Acad Sci U S A. 2023 Aug 22;120(34):e2209735120. doi: 10.1073/pnas.2209735120. Epub 2023 Aug 14.

Abstract

The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short-term, spatial variations in OH (Proxy) in the remote marine troposphere using comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. Proxy is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. Proxy comprises only eight variables that are generally observed by routine ground- or satellite-based instruments. Proxy scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median = 0.90, interquartile range = 0.80 to 0.94 across 2-km altitude by 20° latitudinal regions). We deconstruct spatial variations in Proxy as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region Proxy variations-water vapor (HO) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer an avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both HO and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of Proxy as a process-based approach for evaluating intermodel differences in remote marine tropospheric OH.

摘要

羟基自由基(OH)作为甲烷的主要汇以及许多空气污染物形成和损耗的驱动因素,推动着大气化学循环,但对OH的直接观测较为稀少。我们利用美国国家航空航天局(NASA)大气层析成像(ATom)机载观测活动的综合测量数据,开发并评估了一种基于观测的代理指标(Proxy),用于反映偏远海洋对流层中OH的短期空间变化。根据用ATom观测数据约束的OH箱式模型模拟结果,Proxy是OH稳态方程的简化形式,代表了偏远海洋对流层中OH的主要产生和损耗途径。Proxy仅包含八个通常由常规地基或天基仪器观测的变量。Proxy与沿ATom飞行轨迹的原位[OH]空间变化呈线性比例关系(在2千米高度乘20°纬度区域内,中位数 = 0.90,四分位间距 = 0.80至0.94)。我们将Proxy中的空间变化解构为OH变化对各个项敏感度的一阶近似。有两个项调节区域内Proxy的变化——水汽(HO)以及在较小程度上的一氧化氮(NO)。这意味着一组有限的观测数据可以为绘制偏远海洋对流层大部分区域OH空间变化的基于观测的地图提供一条途径。预计HO和NO都会随气候而变化,而NO也会随人类活动发生强烈变化。我们还展示了Proxy作为一种基于过程的方法在评估偏远海洋对流层OH模型间差异方面的效用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccf6/10451388/30fdaa2e2060/pnas.2209735120fig01.jpg

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