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Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom

Gonzalez, Yenny and Commane, Róisín and Manninen, Ethan and Daube, Bruce C. and Schiferl, Luke D. and McManus, J. Barry and McKain, Kathryn and Hintsa, Eric J. and Elkins, James W. and Montzka, Stephen A. and Sweeney, Colm and Moore, Fred and Jimenez, Jose L. and Campuzano Jost, Pedro and Ryerson, Thomas B. and Bourgeois, Ilann and Peischl, Jeff and Thompson, Chelsea R. and Ray, Eric A. and Wennberg, Paul O. and Crounse, John and Kim, Michelle and Allen, Hannah M. and Newman, Paul A. and Stephens, Britton B. and Apel, Eric C. and Hornbrook, Rebecca S. and Nault, Benjamin A. and Morgan, Eric and Wofsy, Steven C. (2021) Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom. Atmospheric Chemistry and Physics, 21 (14). pp. 11113-11132. ISSN 1680-7324. doi:10.5194/acp-21-11113-2021.

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We measured the global distribution of tropospheric N₂O mixing ratios during the NASA airborne Atmospheric Tomography (ATom) mission. ATom measured concentrations of ∼ 300 gas species and aerosol properties in 647 vertical profiles spanning the Pacific, Atlantic, Arctic, and much of the Southern Ocean basins, nearly from pole to pole, over four seasons (2016–2018). We measured N₂O concentrations at 1 Hz using a quantum cascade laser spectrometer (QCLS). We introduced a new spectral retrieval method to account for the pressure and temperature sensitivity of the instrument when deployed on aircraft. This retrieval strategy improved the precision of our ATom QCLS N₂O measurements by a factor of three (based on the standard deviation of calibration measurements). Our measurements show that most of the variance of N₂O mixing ratios in the troposphere is driven by the influence of N₂O-depleted stratospheric air, especially at mid- and high latitudes. We observe the downward propagation of lower N₂O mixing ratios (compared to surface stations) that tracks the influence of stratosphere–troposphere exchange through the tropospheric column down to the surface. The highest N₂O mixing ratios occur close to the Equator, extending through the boundary layer and free troposphere. We observed influences from a complex and diverse mixture of N₂O sources, with emission source types identified using the rich suite of chemical species measured on ATom and the geographical origin calculated using an atmospheric transport model. Although ATom flights were mostly over the oceans, the most prominent N₂O enhancements were associated with anthropogenic emissions, including from industry (e.g., oil and gas), urban sources, and biomass burning, especially in the tropical Atlantic outflow from Africa. Enhanced N₂O mixing ratios are mostly associated with pollution-related tracers arriving from the coastal area of Nigeria. Peaks of N₂O are often associated with indicators of photochemical processing, suggesting possible unexpected source processes. In most cases, the results show how difficult it is to separate the mixture of different sources in the atmosphere, which may contribute to uncertainties in the N₂O global budget. The extensive data set from ATom will help improve the understanding of N₂O emission processes and their representation in global models.

Item Type:Article
Related URLs:
URLURL TypeDescription ItemData
Gonzalez, Yenny0000-0001-5153-3972
Commane, Róisín0000-0003-1373-1550
Schiferl, Luke D.0000-0002-5047-2490
McKain, Kathryn0000-0002-8323-5758
Hintsa, Eric J.0000-0002-5289-630X
Elkins, James W.0000-0003-4701-3100
Montzka, Stephen A.0000-0002-9396-0400
Sweeney, Colm0000-0002-4517-0797
Moore, Fred0000-0002-8461-2535
Jimenez, Jose L.0000-0001-6203-1847
Campuzano Jost, Pedro0000-0003-3930-010X
Ryerson, Thomas B.0000-0003-2800-7581
Bourgeois, Ilann0000-0002-2875-1258
Peischl, Jeff0000-0002-9320-7101
Thompson, Chelsea R.0000-0002-7332-9945
Ray, Eric A.0000-0001-8727-9849
Wennberg, Paul O.0000-0002-6126-3854
Crounse, John0000-0001-5443-729X
Kim, Michelle0000-0002-4922-4334
Allen, Hannah M.0000-0002-4218-5133
Newman, Paul A.0000-0003-1139-2508
Stephens, Britton B.0000-0002-1966-6182
Apel, Eric C.0000-0001-9421-818X
Hornbrook, Rebecca S.0000-0002-6304-6554
Nault, Benjamin A.0000-0001-9464-4787
Wofsy, Steven C.0000-0002-3990-6737
Additional Information:© Author(s) 2021. This work is distributed under the Creative Commons Attribution 4.0 License. Received: 25 February 2021 – Discussion started: 8 March 2021; Revised: 3 June 2021 – Accepted: 10 June 2021 – Published: 22 July 2021. We would like to thank the ATom leadership team, the science team, and the NASA DC-8 pilot, technicians, and mechanics for their contribution and support during the mission. We thank Karl Froyd for the aerosol products during ATom that support this study. We also thank the National Aeronautics and Space Administration and the National Science Foundation for providing the financial support that made possible this study. This research has been supported by the National Aeronautics and Space Administration (grant nos. NNX15AJ23G, NNX17AF54G, NNX15AG58A, NNX15AH33A, and 80NSSC19K0124) and the National Science Foundation (grant nos. 1852977, AGS-1547626, and AGS-1623745). Data availability: Data from the ATom mission can be found in the NASA ESPO archive (, last access: 10 February 2021), and in the ATom data repository at the NASA/ORNL DAAC (, Wofsy et al., 2018). The QCLS N2O data is available at (Commane et al., 2020). Supplement: The supplement related to this article is available online at: Author contributions: YG did the data analysis and wrote and revised the paper. SCW and RC actively contributed to the design of the study and data analysis. JBM designed the Neptune software for spectral re-analysis and contributed to the writing. RC and BCD performed and analyzed QCLS measurements of CH₄, N₂O, and CO and contributed to the discussions. EM and LDS contributed to the data analysis. KM performed and analyzed NOAA Picarro measurements of CH₄, CO, and CO₂. JWE, EJH, and FM performed and analyzed N₂O, SF₆, and CFC-12 measurements from PANTHER and UCATS instruments. FM, SM, and CS performed and analyzed N₂O measurements with the Programmable Flask Package Whole Air Sampler (PFP). POW, JC, MK, and HMA performed and analyzed the CIT-CIMS measurements of HCN and SO₂ shown here. KF performed and analyzed PALMS measurements. JLJ, PCJ, and BAN performed and analyzed HR-AMS measurements for a variety of aerosols. ER provided back trajectories for each minute during the flight tracks, and PN provided the GEOS5 FP meteorological products. TBR, IB, JP, and CRT performed and analyzed NO_yO₃ measurements of NO_y and O₃. BBS and EJM performed and analyzed AO2 and Medusa Whole Air Sampler measurements of O₂ / N₂ and CO₂ and assisted with the interpretation. ECA and RSH performed and analyzed TOGA measurements of volatile organic compounds. All coauthors provided comments on the paper. The authors declare that they have no conflict of interest. Review statement: This paper was edited by Andreas Engel and reviewed by three anonymous referees.
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Issue or Number:14
Record Number:CaltechAUTHORS:20210821-172128783
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Official Citation:Gonzalez, Y., Commane, R., Manninen, E., Daube, B. C., Schiferl, L. D., McManus, J. B., McKain, K., Hintsa, E. J., Elkins, J. W., Montzka, S. A., Sweeney, C., Moore, F., Jimenez, J. L., Campuzano Jost, P., Ryerson, T. B., Bourgeois, I., Peischl, J., Thompson, C. R., Ray, E., Wennberg, P. O., Crounse, J., Kim, M., Allen, H. M., Newman, P. A., Stephens, B. B., Apel, E. C., Hornbrook, R. S., Nault, B. A., Morgan, E., and Wofsy, S. C.: Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom, Atmos. Chem. Phys., 21, 11113–11132,, 2021.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:110374
Deposited By: Tony Diaz
Deposited On:21 Aug 2021 17:38
Last Modified:21 Aug 2021 17:38

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