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来自太空的甲酸测量:TES反演算法及观测到的全球分布。

HCOOH measurements from space: TES retrieval algorithm and observed global distribution.

作者信息

Cady-Pereira K E, Chaliyakunnel S, Shephard M W, Millet D B, Luo M, Wells K C

机构信息

Atmospheric and Environmental Research, Inc., Lexington, Massachusetts, USA.

University of Minnesota, Minneapolis-St. Paul, Minnesota, USA.

出版信息

Atmos Meas Tech. 2014 Jul 1;7(7):2297-2311. doi: 10.5194/amt-7-2297-2014. Epub 2014 Jul 30.

Abstract

Presented is a detailed description of the TES (Tropospheric Emission Spectrometer)-Aura satellite formic acid (HCOOH) retrieval algorithm and initial results quantifying the global distribution of tropospheric HCOOH. The retrieval strategy, including the optimal estimation methodology, spectral microwindows, a priori constraints, and initial guess information, are provided. A comprehensive error and sensitivity analysis is performed in order to characterize the retrieval performance, degrees of freedom for signal, vertical resolution, and limits of detection. These results show that the TES HCOOH retrievals (i) typically provide at best 1.0 pieces of information; (ii) have the most vertical sensitivity in the range from 900 to 600 hPa with ~2 km vertical resolution; (iii) require at least 0.5 ppbv (parts per billion by volume) of HCOOH for detection if thermal contrast is greater than 5 K, and higher concentrations as thermal contrast decreases; and (iv) based on an ensemble of simulated retrievals, are unbiased with a standard deviation of ±0.4 ppbv. The relative spatial distribution of tropospheric HCOOH derived from TES and its associated seasonality are broadly correlated with predictions from a state-of-the-science chemical transport model (GEOS-Chem CTM). However, TES HCOOH is generally higher than is predicted by GEOS-Chem, and this is in agreement with recent work pointing to a large missing source of atmospheric HCOOH. The model bias is especially pronounced in summertime and over biomass burning regions, implicating biogenic emissions and fires as key sources of the missing atmospheric HCOOH in the model.

摘要

本文详细描述了对流层发射光谱仪(TES)-奥拉卫星的甲酸(HCOOH)反演算法以及量化对流层HCOOH全球分布的初步结果。文中提供了反演策略,包括最优估计方法、光谱微窗口、先验约束和初始猜测信息。为了表征反演性能、信号自由度、垂直分辨率和检测限,进行了全面的误差和灵敏度分析。这些结果表明,TES对HCOOH的反演结果:(i)通常最多提供1.0条信息;(ii)在900至600百帕范围内垂直灵敏度最高,垂直分辨率约为2千米;(iii)如果热对比度大于5K,检测所需的HCOOH浓度至少为0.5 ppbv(体积分数十亿分之一),且随着热对比度降低,所需浓度更高;(iv)基于一组模拟反演结果,无偏差,标准偏差为±0.4 ppbv。由TES得出的对流层HCOOH的相对空间分布及其相关的季节性与一个先进的化学传输模型(GEOS-Chem CTM)的预测大致相关。然而,TES测得的HCOOH含量通常高于GEOS-Chem的预测值,这与近期指出大气中HCOOH存在大量缺失源的研究结果一致。这种模型偏差在夏季和生物质燃烧区域尤为明显,这表明生物源排放和火灾是模型中大气HCOOH缺失的关键来源。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a6d9/7954082/0bfd93503cdb/nihms-1669543-f0001.jpg

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