Chemical Insights into the Molecular Composition of Organic Aerosols in the Urban Region of Houston, Texas

Tania Gautam, Gregory W. Vandergrift, Nurun Nahar Lata, Zezhen Cheng, Ashfiqur Rahman, Annalisa Minke, Zhenli Lai, Darielle N. Dexheimer, Damao Zhang, Matthew A. Marcus, Maria A. Zawadowicz, Chongai Kuang, Ran Zhao, Allison L. Steiner and Swarup China*, 
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Abstract

Molecular functional groups, such as organosulfates (CHOS) and organonitrates (CHNO) are important tracers for field observations of secondary organic aerosols (SOA). While CHOS and CHNO are prevalent in the atmosphere, there is a lack of knowledge regarding daily and day- and night-time variations in these species in the urban atmosphere. Meteorological factors such as wind speed/direction, relative humidity (RH), and temperature can influence the formation of CHOS/CHNO. To investigate these trends, we utilized multimodal chemical imaging and advanced high resolution mass spectrometry techniques to acquire particle speciation and molecular formulas (MFs) associated with day and night sampling periods. Back trajectory analyses revealed the oceanic influence of southern wind airmasses in later June sampling periods with organic fractions <10%. Conversely, northern winds in early June sampling periods contributed to the episodic emergence of extremely low volatile organics (ELVOCs) and organic factions up to 41%. The observed unique MFs to June 3 (223 MFs) and to June 4 (144 MFs) were largely found to be of biogenic rather than anthropogenic origin. Our findings reveal episodic prevalence and temporal distribution of SOA constituents across the urban region of Houston, Texas.

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德克萨斯州休斯顿城市地区有机气溶胶分子组成的化学洞察力
有机硫酸盐(CHOS)和有机硝酸盐(CHNO)等分子官能团是实地观测二次有机气溶胶(SOA)的重要示踪剂。虽然 CHOS 和 CHNO 在大气中普遍存在,但人们对这些物种在城市大气中的日变化和昼夜变化缺乏了解。风速/风向、相对湿度(RH)和温度等气象因素会影响 CHOS/CHNO 的形成。为了研究这些趋势,我们利用多模态化学成像和先进的高分辨率质谱技术,获取了与白天和夜间采样时段相关的颗粒规格和分子式(MF)。回溯轨迹分析表明,在 6 月晚些时候的采样时段,南风气团受海洋影响,有机物含量为 10%。相反,6 月初采样时段的北风导致了极低挥发性有机物(ELVOCs)的偶发出现,有机物含量高达 41%。在 6 月 3 日(223 个 MFs)和 6 月 4 日(144 个 MFs)观测到的独特 MFs 大部分是生物源而非人为源。我们的研究结果揭示了得克萨斯州休斯顿城市地区 SOA 成分的偶发性流行和时间分布。
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