Abstract

Abstract. In the upper troposphere and lower stratosphere (UTLS), the accurate quantification of low water vapor concentrations has presented a significant measurement challenge. The instrumental uncertainties are passed on to estimates of H2O transport, cloud formation and the role of H2O in the UTLS energy budget and resulting effects on surface temperatures. To address the uncertainty in UTLS H2O determination, the airborne mass spectrometer AIMS-H2O, with in-flight calibration, has been developed for fast and accurate airborne water vapor measurements. We present a new setup to measure water vapor by direct ionization of ambient air. Air is sampled via a backward facing inlet that includes a bypass flow to assure short residence times (< 0.2 s) in the inlet line, which allows the instrument to achieve a time resolution of ∼ 4 Hz, limited by the sampling frequency of the mass spectrometer. From the main inlet flow, a smaller flow is extracted into the novel pressure-controlled gas discharge ion source of the mass spectrometer. The air is directed through the gas discharge region where ion–molecule reactions lead to the production of hydronium ion clusters, H3O+(H2O)n (n = 0, 1, 2), in a complex reaction scheme similar to the reactions in the D-region of the ionosphere. These ions are counted to quantify the ambient water vapor mixing ratio. The instrument is calibrated during flight using a new calibration source based on the catalytic reaction of H2 and O2 on a Pt surface to generate a calibration standard with well-defined and stable H2O mixing ratios. In order to increase data quality over a range of mixing ratios, two data evaluation methods are presented for lower and higher H2O mixing ratios respectively, using either only the H3O+(H2O) ions or the ratio of all water vapor dependent ions to the total ion current. Altogether, a range of water vapor mixing ratios from 1 to 500 parts per million by volume (ppmv) can be covered with an accuracy between 7 and 15 %. AIMS-H2O was deployed on two DLR research aircraft, the Falcon during CONCERT (CONtrail and Cirrus ExpeRimenT) in 2011, and HALO during ML-CIRRUS (Mid-Latitude CIRRUS) in 2014. The comparison of AIMS-H2O with the SHARC tunable diode laser hygrometer during ML-CIRRUS shows a correlation near to 1 in the range between 10 and 500 ppmv for the entire campaign.

Highlights

  • Airborne mass spectrometry is a powerful tool for the fast and accurate measurement of various trace gases relevant for atmospheric chemistry and climate

  • With the mass spectrometer Atmospheric Ionization Mass Spectrometer (AIMS)-H2O, which includes in-flight calibration, we have developed a significant contribution to the field of airborne water vapor measurements with a focus on the low H2O mixing ratios of the upper troposphere and lower stratosphere (UTLS)

  • In order to obtain a quantitative impression of the instrument performance over the entire campaign, Fig. 11 shows a scatter plot of H2O mixing ratios measured by AIMS-H2O and Sophisticated Hygrometer for Atmospheric ResearCh (SHARC) with an extensive set of 112 529 data points gathered in March/April 2014

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Summary

Introduction

Airborne mass spectrometry is a powerful tool for the fast and accurate measurement of various trace gases relevant for atmospheric chemistry and climate. The radiative impact of changes in water vapor concentrations is strong in the tropopause region and in the lower stratosphere (Solomon et al, 2010; Riese et al, 2012) where water vapor mixing ratios are in the range of only a few parts per million by volume (ppmv, 10−6 mol mol−1) Measurements in these regions, in situ as well as satellite-based instruments, showed significant discrepancies in the past with offsets of the order of several 10 % (e.g., Weinstock et al, 2009; Vömel et al, 2007). With the mass spectrometer AIMS-H2O, which includes in-flight calibration, we have developed a significant contribution to the field of airborne water vapor measurements with a focus on the low H2O mixing ratios of the UTLS. After a discussion of data reduction methods used to quantify ambient H2O mixing ratios, we derive the instrumental uncertainties and present the first airborne measurements on HALO during ML-CIRRUS including a comparison with the Sophisticated Hygrometer for Atmospheric ResearCh (SHARC) in situ tunable diode laser hygrometer

Setup of the mass spectrometer
Inlet line
Pressure regulation
Vacuum chamber
Custom gas-discharge ion source
Mechanical and electrical setup
Ion reaction scheme for AIMS-H2O
Mass spectrum for the detection of water vapor
Two data evaluation methods
Data quality and sources of uncertainty
Sensitivity and detection limits
Instrumental uncertainties
Cross-sensitivity
Flight performance of AIMS-H2O on HALO during ML-CIRRUS
A IM S SHARC
Findings
Summary and outlook
Full Text
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