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The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short term, spatial variations in OH (ProxyOH) in the remote marine troposphere using unprecedented and comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. ProxyOH is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. ProxyOH comprises only eight variables that are generally observed by routine ground- or satellite-based instruments. ProxyOH scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median r2 = 0.90, interquartile range = 0.80 – 0.94 across 2 km altitude by 20° latitudinal regions). We deconstruct spatial variations in ProxyOH as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region ProxyOH variations—water vapor (H2O) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer a novel avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both H2O and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of ProxyOH as a process-based approach for evaluating inter-model differences in remote marine tropospheric OH.

Accurate estimates of carbon–climate feedbacks require an independent means for evaluating surface flux models at regional scales. The altitude-integrated enhancement (AIE) derived from the Arctic Carbon Atmospheric Profiles (Arctic-CAP) project demonstrates the utility of this bulk quantity for surface flux model evaluation. This bulk quantity leverages background mole fraction values from the middle free troposphere, is agnostic to uncertainties in boundary layer height, and can be derived from model estimates of mole fractions and vertical gradients. To demonstrate the utility of the bulk quantity, six airborne profiling surveys of atmospheric carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) throughout Alaska and northwestern Canada between April and November 2017 were completed as part of NASA’s Arctic–Boreal Vulnerability Experiment (ABoVE). The Arctic-CAP sampling strategy involved acquiring vertical profiles of CO2, CH4, and CO from the surface to 5 km altitude at 25 sites around the ABoVE domain on a 4- to 6-week time interval. All Arctic-CAP measurements were compared to a global simulation using the Goddard Earth Observing System (GEOS) modeling system. Comparisons of the AIE bulk quantity from aircraft observations and GEOS simulations of atmospheric CO2, CH4, and CO highlight the fidelity of the modeled surface fluxes. The model–data comparison over the ABoVE domain reveals that while current state-of-the-art models and flux estimates are able to capture broad-scale spatial and temporal patterns in near-surface CO2 and CH4 concentrations, more work is needed to resolve fine-scale flux features that are captured in CO observations

This paper provides an overview of the validation of National Oceanic and Atmospheric Administration (NOAA) operational retrievals of atmospheric carbon trace gas profiles, specifically carbon monoxide (CO), methane (CH4) and carbon dioxide (CO2), from the NOAA-Unique Combined Atmospheric Processing System (NUCAPS), a NOAA enterprise algorithm that retrieves atmospheric profile environmental data records (EDRs) under global non-precipitating (clear to partly cloudy) conditions. Vertical information about atmospheric trace gases is obtained from the Cross-track Infrared Sounder (CrIS), an infrared Fourier transform spectrometer that measures high resolution Earth radiance spectra from NOAA operational low earth orbit (LEO) satellites, including the Suomi National Polar-orbiting Partnership (SNPP) and follow-on Joint Polar Satellite System (JPSS) series beginning with NOAA-20. The NUCAPS CO, CH4, and CO2 profile EDRs are rigorously validated in this paper using well-established independent truth datasets, namely total column data from ground-based Total Carbon Column Observing Network (TCCON) sites, and in situ vertical profile data obtained from aircraft and balloon platforms via the NASA Atmospheric Tomography (ATom) mission and NOAA AirCore sampler, respectively. Statistical analyses using these datasets demonstrate that the NUCAPS carbon gas profile EDRs generally meet JPSS Level 1 global performance requirements, with the absolute accuracy and precision of CO 5% and 15%, respectively, in layers where CrIS has vertical sensitivity; CH4 and CO2 product accuracies are both found to be within ±1%, with precisions of ≈1.5% and ⪅0.5%, respectively, throughout the tropospheric column.

Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime,influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although, throughout much of the free troposphere, the calculated OH reactivity was below the limit-of-detection for the ATom instrument used to measure OH reactivity, the instrument was able to measure the OH reactivity in and just above the marine boundary layer. The mean measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom deployments was 1.9 s-1, which is 0.5 s-1larger than the mean calculated OH reactivity. The missing OH reactivity, the difference between the measured and calculated OH reactivity, varied between 0 s-1to 3.5 s-1, with the highest values over the Northern Hemisphere Pacific Ocean. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.