Chemistry and the Environment, Contributed Talk (15min)
EV-014

Laboratory validation of a laser absorption spectrometer for balloon-borne measurements of upper air water vapor

S. Brunamonti1, M. Graf1, T. Bühlmann2, L. Emmenegger1, B. Tuzson1*
1Empa, Laboratory for Air Pollution/Environmental Technology, Dübendorf, Switzerland, 2METAS, Laboratory Gas Analysis, Bern, Switzerland

Water vapor (H2O) in the upper troposphere-lower stratosphere (UTLS) is of great importance to the Earth's radiative balance. However, accurate measurements of H2O in this region are notoriously difficult, and significant discrepancies were found in the past between different techniques. Currently, cryogenic frostpoint hygrometry is considered as the reference method for balloon-borne measurements of UTLS H2O [1]. However, these devices are currently undergoing a fundamental reconception due their use of fluoroform (HFC-23) as cooling agent, which must be phased out due of its high global warming potential. Here, we present a new mid-IR quantum-cascade laser absorption spectrometer for balloon-borne measurements of UTLS H2O (ALBATROSS). The spectrometer incorporates a specially designed segmented circular multipass cell that allows an optical path length of 6 m [3], while meeting stringent requirements in terms of mass (< 3.5 kg), size, and temperature resilience. Two successful test flights demonstrated the instrument's outstanding capabilities under real atmospheric conditions up to 28 km altitude [2].

The accuracy and precision of ALBATROSS at UTLS-relevant conditions were validated by a laboratory campaign at the Swiss Federal Institute of Metrology (METAS). Using a dynamic-gravimetric permeation method [4], we generated SI-traceable reference mixtures with H2O amount fractions as low as 2.5 ppmv in synthetic air. The results show that ALBATROSS achieves an accuracy better than ± 1.5 % at all investigated pressures (30-250 mbar) and H2O amount fractions (2.5-35 ppmv), and a precision of 0.3 % at 2.5 ppmv H2O and 1 s resolution. Precision can be further improved until 2 ppbv by integrating the measurements in time over approximately 100 s. ALBATROSS also achieves a linear response within ± 2 ppmv up to 180 ppmv H2O. Overall, this represents an unprecedented level of accuracy and precision for a balloon-borne hygrometer. ALBATROSS recently participated to the AquaVIT-4 international intercomparison of atmospheric hygrometers (Karlsruhe, Germany) [5], and further in-flight validation campaigns are planned in 2022.

[1] Brunamonti et al., J. Geophys. Res. Atmos., 2019, 124, 13, 7053-7068.
[2] Graf et al., Atmos. Meas. Tech., 2021, 14, 1365-1378.
[3] Graf, Emmenegger and Tuzson, Opt. Lett., 2018, 43, 2434-2437.
[4] Guillevic et al., Atmos. Meas. Tech., 2018, 11, 3351–3372.
[5] https://www.hemera-h2020.eu/aquavit-4/