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Abstract. We present the development and assessment of a new flight system that uses acommercially available continuous-wave, tunable infrared laser directabsorption spectrometer to measure N₂O, CO₂, CO, andH₂O. When the commercial system is operated in an off-the-shelfmanner, we find a clear cabin pressure–altitude dependency forN₂O, CO₂, and CO. The characteristics of this artifactmake it difficult to reconcile with conventional calibration methods. Wepresent a novel procedure that extends upon traditional calibrationapproaches in a high-flow system with high-frequency, short-duration samplingof a known calibration gas of near-ambient concentration. This approachcorrects for cabin pressure dependency as well as other sources of drift inthe analyzer while maintaining a ∼90% duty cycle for 1Hz sampling.Assessment and validation of the flight system with both extensive in-flightcalibrations and comparisons with other flight-proven sensors demonstrate thevalidity of this method. In-flight 1σ precision is estimated at0.05ppb, 0.10ppm, 1.00ppb, and 10ppm for N₂O,CO₂, CO, and H₂O respectively, and traceability to WorldMeteorological Organization (WMO) standards (1σ) is 0.28ppb,0.33ppm, and 1.92ppb for N₂O, CO₂, and CO. We showthe system is capable of precise, accurate 1Hz airborne observations ofN₂O, CO₂, CO, and H₂O and highlight flightdata, illustrating the value of this analyzer for studying N₂Oemissions on ∼100km spatial scales.

Carbon monoxide (CO) is an ozone precursor, oxidant sink, and widely used pollution tracer. The importance of anthropogenic versus other CO sources in the US is uncertain. Here, we interpret extensive airborne measurements with an atmospheric model to constrain US fossil and nonfossil CO sources. Measurements reveal a low bias in the simulated CO background and a 30% overestimate of US fossil CO emissions in the 2016 National Emissions Inventory. After optimization we apply the model for source partitioning. During summer, regional fossil sources account for just 9%–16% of the sampled boundary layer CO, and 32%–38% of the North American enhancement—complicating use of CO as a fossil fuel tracer. The remainder predominantly reflects biogenic hydrocarbon oxidation plus fires. Fossil sources account for less domain‐wide spatial variability at this time than nonfossil and background contributions. The regional fossil contribution rises in other seasons, and drives ambient variability downwind of urban areas.