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  1. Abstract

    We use TROPOMI (TROPOspheric Monitoring Instrument) tropospheric nitrogen dioxide (NO2) measurements to identify cropland soil nitrogen oxide (NOx = NO + NO2) emissions at daily to seasonal scales in the U.S. Southern Mississippi River Valley. Evaluating 1.5 years of TROPOMI observations with a box model, we observe seasonality in local NOxenhancements and estimate maximum cropland soil NOxemissions (15–34 ng N m−2 s−1) early in growing season (May–June). We observe soil NOxpulsing in response to daily decreases in volumetric soil moisture (VSM) as measured by the Soil Moisture Active Passive (SMAP) satellite. Daily NO2enhancements reach up to 0.8 × 1015 molecules cm−24–8 days after precipitation when VSM decreases to ~30%, reflecting emissions behavior distinct from previously defined soil NOxpulse events. This demonstrates that TROPOMI NO2observations, combined with observations of underlying process controls (e.g., soil moisture), can constrain soil NOxprocesses from space.

     
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  2. Abstract

    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.

     
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  3. Abstract

    Agricultural activity is a significant source of greenhouse gas emissions. The fertilizer production process emits N2O, CO2, and CH4, and fertilized croplands emit N2O. We present continuous airborne observations of these trace gases in the Lower Mississippi River Basin to quantify emissions from both fertilizer plants and croplands during the early growing season. Observed hourly emission rates from two fertilizer plants are compared with reported inventory values, showing agreement for N2O and CO2emissions but large underestimation in reported CH4emissions by up to a factor of 100. These CH4emissions are consistent with loss rates of 0.6–1.2%. We quantify regional emission fluxes (100 km) of N2O using the airborne mass balance technique, a first application for N2O, and explore linkages to controlling processes. Finally, we demonstrate the ability to use airborne measurements to distinguish N2O emission differences between neighboring fields, determining we can distinguish different emission behaviors of regions on the order of 2.5 km2with emissions differences of approximately 0.026μmol m−2s−1. This suggests airborne approaches such as outlined here could be used to evaluate the impact of different agricultural practices at critical field‐size spatial scales.

     
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  4. null (Ed.)
    Abstract. We apply airborne measurements across three seasons(summer, winter and spring 2017–2018) in a multi-inversion framework toquantify methane emissions from the US Corn Belt and Upper Midwest, a keyagricultural and wetland source region. Combing our seasonal results withprior fall values we find that wetlands are the largest regional methanesource (32 %, 20 [16–23] Gg/d), while livestock (enteric/manure; 25 %,15 [14–17] Gg/d) are the largest anthropogenic source. Naturalgas/petroleum, waste/landfills, and coal mines collectively make up theremainder. Optimized fluxes improve model agreement with independentdatasets within and beyond the study timeframe. Inversions reveal coherentand seasonally dependent spatial errors in the WetCHARTs ensemble meanwetland emissions, with an underestimate for the Prairie Pothole region butan overestimate for Great Lakes coastal wetlands. Wetland extent andemission temperature dependence have the largest influence on predictionaccuracy; better representation of coupled soil temperature–hydrologyeffects is therefore needed. Our optimized regional livestock emissionsagree well with the Gridded EPA estimates during spring (to within 7 %) butare ∼ 25 % higher during summer and winter. Spatial analysisfurther shows good top-down and bottom-up agreement for beef facilities (withmainly enteric emissions) but larger (∼ 30 %) seasonaldiscrepancies for dairies and hog farms (with > 40 % manureemissions). Findings thus support bottom-up enteric emission estimates butsuggest errors for manure; we propose that the latter reflects inadequatetreatment of management factors including field application. Overall, ourresults confirm the importance of intensive animal agriculture for regionalmethane emissions, implying substantial mitigation opportunities throughimproved management. 
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  5. 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.

     
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