The airborne mass spectrometer AIMS – Part 2: Measurements of trace gases with stratospheric or tropospheric origin in the UTLS

摘要

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 SFsub5/subsup?/sup reagent ions for the simultaneous measurement of trace gas concentrations of HCl, HNOsub3/sub and SOsub2/sub in the ?pptv to ppmv (10sup?12/sup to 10sup?6/sup?mol?molsup?1/sup) 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, HNOsub3/sub, SOsub2/sub and HONO. HNOsub3/sub and HCl are routinely calibrated in-flight using permeation devices; SOsub2/sub is continuously calibrated during flight adding an isotopically labeled sup34/supSOsub2/sub standard. In addition, we report on trace gas measurements of HONO, which is sensitive to the reaction with SFsub5/subsup?/sup. 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.