Evaluation of the airborne quantum cascade laser spectrometer (QCLS) measurements of the carbon and greenhouse gas suite – CO₂, CH₄, N₂O, and CO – during the CalNex and HIPPO campaigns

Abstract. We present an evaluation of aircraft observations of the carbon and greenhouse gases CO₂, CH₄, N₂O, and CO using a direct-absorption pulsed quantum cascade laser spectrometer (QCLS) operated during the HIPPO and CalNex airborne experiments. The QCLS made continuous 1 Hz measurements with 1σ Allan precisions of 20, 0.5, 0.09, and 0.15 ppb for CO₂, CH₄, N₂O, and CO, respectively, over > 500 flight hours on 79 research flights. The QCLS measurements are compared to two vacuum ultraviolet (VUV) CO instruments (CalNex and HIPPO), a cavity ring-down spectrometer (CRDS) measuring CO₂ and CH₄ (CalNex), two broadband non-dispersive infrared (NDIR) spectrometers measuring CO₂ (HIPPO), two onboard gas chromatographs measuring a variety of chemical species including CH₄, N₂O, and CO (HIPPO), and various flask-based measurements of all four species. QCLS measurements are tied to NOAA and WMO standards using an in-flight calibration system, and mean differences when compared to NOAA CCG flask data over the 59 HIPPO research flights were 100, 1, 1, and 2 ppb for CO₂, CH₄, N₂O, and CO, respectively. The details of the end-to-end calibration procedures and the data quality assurance and quality control (QA/QC) are presented. Specifically, we discuss our practices for the traceability of standards given uncertainties in calibration cylinders, isotopic and surface effects for the long-lived greenhouse gas tracers, interpolation techniques for in-flight calibrations, and the effects of instrument linearity on retrieved mole fractions.