An airborne infrared laser spectrometer for in-situ trace gas measurements: application to tropical convection case studies

Abstract. A three-channel laser absorption spectrometer called SPIRIT (SPectromètre InfraRouge In situ Toute altitude) has been developed for airborne measurements of trace gases in the troposphere and lower stratosphere. More than three different species can be measured simultaneously with high time resolution (each 1.6 s) using three individual CW-DFB-QCLs (Continuous Wave Distributed FeedBack Quantum Cascade Lasers) coupled to a single Robert multipass optical cell. The lasers are operated in a time-multiplexed mode. Absorption of the mid-infrared radiations occur in the cell (2.8 L with effective path lengths of 134 to 151 m) at reduced pressure, with detection achieved using a HgCdTe detector cooled by Stirling cycle. The performances of the instrument are described, in particular precisions of 1, 1 and 3 %, and volume mixing ratio (vmr) sensitivities of 0.4, 6 and 2.4 ppbv are determined at 1.6 s for CO, CH₄ and N₂O, respectively (at 1σ confidence level). Estimated accuracies without calibration are about 6 %. Dynamic measuring ranges of about four decades are established. The first deployment of SPIRIT was realized aboard the Falcon-20 research aircraft operated by DLR (Deutsches Zentrum für Luft- und Raumfahrt) within the frame of the SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere) European project in November-December 2011 over Malaysia. The convective outflows from two large convective systems near Borneo Island (6.0° N–115.5° E and 5.5° N–118.5° E) were sampled above 11 km in altitude on 19 November and 9 December, respectively. Correlated enhancements in CO and CH₄ vmr were detected when the aircraft crossed the outflow anvil of both systems. These enhancements were interpreted as the fingerprint of transport from the boundary layer up through the convective system and then horizontal advection in the outflow. Using these observations, the fraction of boundary layer air contained in fresh convective outflow was calculated to range between 22 and 31 %, showing the variability of the mixing taking place during convective transport.