Advances in OH reactivity instruments for airborne field measurements

IF 3.2 3区 地球科学 Q2 METEOROLOGY & ATMOSPHERIC SCIENCES
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, Anna Novelli
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Abstract

Abstract. Hydroxyl radical OH reactivity, which is the inverse lifetime of the OH radical, provides information on the burden of air pollutants, since almost all air pollutants react with OH. OH reactivity measurements from field experiments can help to identify gaps in the measurement of individual reactants and serve as a proxy for the potential formation of secondary pollutants, including ozone and particles. However, OH reactivity is not regularly measured specifically on airborne platforms due to the technical complexity of the instruments and/or the need for careful instrumental characterisation to apply accurate correction factors to account for secondary chemistry in the instruments. The method used in this work, based on the time-resolved measurement of OH radicals produced by laser flash photolysis in a flow tube, does not require corrections as secondary chemistry in the instrument is negligible for typical atmospheric conditions. However, the detection of OH radicals by laser-induced fluorescence is challenging. In this work, an OH reactivity instrument has been further developed specifically for airborne measurements. The laser system used to detect the OH radicals has been simplified compared to previous setups, thereby significantly reducing the need for user interaction. The improved sensitivity allows measurements to be made with high time resolution on the order of seconds with a measurements precision of 0.3 s−1. The OH reactivity measurements were validated by using a propane gas standard, which allowed the determination of the reaction rate constant of the OH reaction with propane. The values are in excellent agreement with literature recommendations within a range of 4 to 8 %. Deviations are well within the combined uncertainties. The accuracy of the OH reactivity measurements is mainly limited by the determination of the instrumental zero, which has a typical maximum uncertainty of 0.5 s−1. The high sensitivity of the improved instrument facilitates the data acquisition on board an aircraft as demonstrated by its deployment during the AEROMMA campaign in 2023.
用于机载实地测量的 OH 反应性仪器的进步
摘要羟基自由基的羟基反应性是羟基自由基寿命的倒数,它提供了有关空气污染物负荷的信息,因为几乎所有空气污染物都会与羟基自由基发生反应。通过现场实验测量羟基自由基反应性,有助于找出个别反应物测量的不足之处,并可作为臭氧和颗粒物等二次污染物潜在形成的替代物。然而,由于仪器的技术复杂性和/或需要仔细的仪器特性分析,以应用准确的校正因子来考虑仪器中的二次化学反应,因此没有定期对机载平台上的羟基反应性进行专门测量。这项工作中使用的方法是通过激光闪光灯光解在流动管中产生的 OH 自由基进行时间分辨测量,不需要校正,因为在典型大气条件下,仪器中的二次化学反应可以忽略不计。然而,利用激光诱导荧光检测 OH 自由基是一项挑战。在这项工作中,进一步开发了一种专门用于机载测量的 OH 反应性仪器。与以前的装置相比,用于检测 OH 自由基的激光系统得到了简化,从而大大减少了用户交互的需要。灵敏度提高后,测量时间分辨率可达到秒级,测量精度为 0.3 s-1。通过使用丙烷气体标准,对羟基反应性测量进行了验证,从而确定了羟基与丙烷反应的反应速率常数。测量值与文献推荐值非常吻合,范围在 4% 到 8%。偏差在综合不确定度范围内。OH 反应性测量的准确性主要受限于仪器零点的确定,其典型的最大不确定性为 0.5 s-1。改进后的仪器灵敏度高,便于在飞机上获取数据,2023 年 AEROMMA 行动期间的部署就证明了这一点。
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来源期刊
Atmospheric Measurement Techniques
Atmospheric Measurement Techniques METEOROLOGY & ATMOSPHERIC SCIENCES-
CiteScore
7.10
自引率
18.40%
发文量
331
审稿时长
3 months
期刊介绍: Atmospheric Measurement Techniques (AMT) is an international scientific journal dedicated to the publication and discussion of advances in remote sensing, in-situ and laboratory measurement techniques for the constituents and properties of the Earth’s atmosphere. The main subject areas comprise the development, intercomparison and validation of measurement instruments and techniques of data processing and information retrieval for gases, aerosols, and clouds. The manuscript types considered for peer-reviewed publication are research articles, review articles, and commentaries.
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