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Comprehensive characterization of atmospheric organic carbon at a forested site

机译:森林地区大气有机碳综合表征

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摘要

Atmospheric organic compounds are central to key chemical processes that influence air quality, ecological health, and climate. However, longstanding diffculties in predicting important quantities such as organic aerosol formation and oxidant lifetimes indicate that our understanding of atmospheric organic chemistry is fundamentally incomplete, probably due in part to the presence of organic species that are unmeasured using standard analytical techniques. Here we present measurements of a wide range of atmospheric organic compounds-including previously unmeasured species-taken concurrently at a single site (a ponderosa pine forest during summertime) by five state-of-the-art mass spectrometric instruments. The combined data set provides a comprehensive characterization of atmospheric organic carbon, covering a wide range in chemical properties (volatility, oxidation state, and molecular size), and exhibiting no obvious measurement gaps. This enables the first construction of a measurement-based local organic budget, highlighting the high emission, deposition, and oxidation fluxes in this environment. Moreover, previously unmeasured species, including semivolatile and intermediate-volatility organic species (S/IVOCs), account for one-third of the total organic carbon, and (within error) provide closure on both OH reactivity and potential secondary organic aerosol formation.
机译:大气有机化合物是关键化学过程的核心,影响空气质量,生态健康和气候。然而,长期的差异在预测有机气溶胶形成和氧化剂的寿命等重要量方面表明我们对大气有机化学的理解是根本不完整的,可能部分地归因于使用标准分析技术未测量的有机物种的存在。在这里,我们展示了各种大气有机化合物的测量 - 包括先前未测量的物种,在单个位点(夏季期间的丘疹松树林)上同时采用五种最先进的质谱仪器。组合数据集提供了大气有机碳的综合表征,覆盖了化学性质(挥发性,氧化状态和分子大小)的宽范围,并且没有明显的测量间隙。这使得能够首先构建基于测量的局部有机预算,突出显示该环境中的高发射,沉积和氧化通量。此外,先前未测量的物种,包括半萎缩和中间挥发性有机物质(S / IVOC),其占总有机碳的三分之一,并且(在误差内)提供闭合OH反应性和潜在的二次有机气溶胶形成。

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