The airborne mass spectrometer AIMS – Part 2: Measurements of trace gases with stratospheric or tropospheric origin in the UTLS
The airborne mass spectrometer AIMS – Part 2: Measurements of trace gases with stratospheric or tropospheric origin in the UTLS
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DOI：
10.5194/amt-9-1907-2016
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发表时间：
2015-12
影响因子：
3.8
通讯作者：
T. Jurkat;S. Kaufmann;C. Voigt;D. Schäuble;P. Jeßberger;H. Ziereis
中科院分区：
文献类型：
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作者：
T. Jurkat;S. Kaufmann;C. Voigt;D. Schäuble;P. Jeßberger;H. Ziereis
抽象的。要了解对流层上层和平流层下层对气候敏感的微量气体变化的作用及其对辐射收支的影响，需要进行准确的测量。UTLS的组成取决于平流层和对流层成分的输送和化学，如氯、氮氧化物和硫化合物。大气化学电离质谱仪旨在通过化学电离的方法精确地测量飞机上的一组这些成分。本文介绍了一种使用SF5−试剂离子同时测量PPTV至ppmv(10−12~10−6−1)范围内微量气体浓度的装置，称为AIMS-TG(大气化学电离质谱仪，用于痕量气体测量)。这篇论文的第一部分(Kaufmann等人，2016)报告了利用AIMS-H2O配置进行的UTLS水汽测量。该仪器可以根据任务的科学目标在两种配置之间灵活切换。对于AIMS-TG，已经开发了一种定制的气体放电离子源，用于产生与HCl、HNO3、SO2和HONO选择性反应的试剂离子。HNO3和HCl通常在飞行中使用渗透设备进行校准；SO2在飞行过程中不断进行校准，并添加同位素标记的34SO2标准。此外，我们还报道了对与SF_5−反应敏感的HONO的痕量气体测量。在S 1的时间分辨率下，各种痕量气体的检测下限在10pptv的低范围内，测量的总不确定度在20%量级。AIMS已在德国航天中心的猎鹰和HALO(高空远程研究飞机)研究飞机上集成并成功运行。作为一个例子，介绍了2012年与HALO进行的TACTS/ESMVal(LMS/UT和地球系统模型验证的传输和组成)飞行任务期间进行的测量，重点是对UTLS区域对流层和平流层的影响进行分类。将AIMS测量与其他测量技术相结合，可以全面了解UTLS中的硫、氯和活性氮氧化物的收支情况。用AIMS测量的不同微量气体有可能更好地了解对流层顶及其附近的微量气体的来源和变化。
Abstract. Understanding the role of climate-sensitive trace gas variabilities in the upper troposphere and lower stratosphere region (UTLS) and their impact on its radiative budget requires accurate measurements. The composition of the UTLS is governed by transport and chemistry of stratospheric and tropospheric constituents, such as chlorine, nitrogen oxide and sulfur compounds. The Atmospheric chemical Ionization Mass Spectrometer AIMS has been developed to accurately measure a set of these constituents on aircraft by means of chemical ionization. Here we present a setup using SF5− reagent ions for the simultaneous measurement of trace gas concentrations of HCl, HNO3 and SO2 in the pptv to ppmv (10−12 to 10−6 mol mol−1) range with in-flight and online calibration called AIMS-TG (Atmospheric chemical Ionization Mass Spectrometer for measurements of trace gases). Part 1 of this paper (Kaufmann et al., 2016) reports on the UTLS water vapor measurements with the AIMS-H2O configuration. The instrument can be flexibly switched between two configurations depending on the scientific objective of the mission. For AIMS-TG, a custom-made gas discharge ion source has been developed for generation of reagent ions that selectively react with HCl, HNO3, SO2 and HONO. HNO3 and HCl are routinely calibrated in-flight using permeation devices; SO2 is continuously calibrated during flight adding an isotopically labeled 34SO2 standard. In addition, we report on trace gas measurements of HONO, which is sensitive to the reaction with SF5−. The detection limit for the various trace gases is in the low 10 pptv range at a 1 s time resolution with an overall uncertainty of the measurement of the order of 20 %. AIMS has been integrated and successfully operated on the DLR research aircraft Falcon and HALO (High Altitude LOng range research aircraft). As an example, measurements conducted during the TACTS/ESMVal (Transport and Composition of the LMS/UT and Earth System Model Validation) mission with HALO in 2012 are presented, focusing on a classification of tropospheric and stratospheric influences in the UTLS region. The combination of AIMS measurements with other measurement techniques yields a comprehensive picture of the sulfur, chlorine and reactive nitrogen oxide budget in the UTLS. The different trace gases measured with AIMS exhibit the potential to gain a better understanding of the trace gas origin and variability at and near the tropopause.