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

Y. Gonzalez; Y. Gonzalez; Y. Gonzalez; R. Commane; R. Commane; R. Commane; E. Manninen; B. C. Daube; L. D. Schiferl; J. B. McManus; K. McKain; K. McKain; E. J. Hintsa; E. J. Hintsa; J. W. Elkins; S. A. Montzka; C. Sweeney; F. Moore; F. Moore; J. L. Jimenez; P. Campuzano Jost; T. B. Ryerson; I. Bourgeois; I. Bourgeois; J. Peischl; J. Peischl; C. R. Thompson; E. Ray; E. Ray; P. O. Wennberg; P. O. Wennberg; J. Crounse; M. Kim; H. M. Allen; P. A. Newman; B. B. Stephens; E. C. Apel; R. S. Hornbrook; B. A. Nault; E. Morgan; S. C. Wofsy

doi:10.5194/acp-21-11113-2021

Atmospheric Chemistry and Physics (Jul 2021)

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

Y. Gonzalez,
Y. Gonzalez,
Y. Gonzalez,
R. Commane,
R. Commane,
R. Commane,
E. Manninen,
B. C. Daube,
L. D. Schiferl,
J. B. McManus,
K. McKain,
K. McKain,
E. J. Hintsa,
E. J. Hintsa,
J. W. Elkins,
S. A. Montzka,
C. Sweeney,
F. Moore,
F. Moore,
J. L. Jimenez,
P. Campuzano Jost,
T. B. Ryerson,
I. Bourgeois,
I. Bourgeois,
J. Peischl,
J. Peischl,
C. R. Thompson,
E. Ray,
E. Ray,
P. O. Wennberg,
P. O. Wennberg,
J. Crounse,
M. Kim,
H. M. Allen,
P. A. Newman,
B. B. Stephens,
E. C. Apel,
R. S. Hornbrook,
B. A. Nault,
E. Morgan,
S. C. Wofsy

Affiliations

Y. Gonzalez: John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Y. Gonzalez: CIMEL Electronique, Paris, 75011, France
Y. Gonzalez: Izaña Atmospheric Research Centre, Santa Cruz de Tenerife, 38001, Spain
R. Commane: John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
R. Commane: Dept. of Earth and Environmental Science, Columbia University, New York, NY 10027, USA
R. Commane: Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, USA
E. Manninen: John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
B. C. Daube: John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
L. D. Schiferl: Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, USA
J. B. McManus: Center for Atmospheric and Environmental Chemistry, Aerodyne Research Inc., Billerica, MA 01821, USA
K. McKain: NOAA Global Monitoring Laboratory, Boulder, CO 80305, USA
K. McKain: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
E. J. Hintsa: NOAA Global Monitoring Laboratory, Boulder, CO 80305, USA
E. J. Hintsa: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
J. W. Elkins: NOAA Global Monitoring Laboratory, Boulder, CO 80305, USA
S. A. Montzka: NOAA Global Monitoring Laboratory, Boulder, CO 80305, USA
C. Sweeney: NOAA Global Monitoring Laboratory, Boulder, CO 80305, USA
F. Moore: NOAA Global Monitoring Laboratory, Boulder, CO 80305, USA
F. Moore: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
J. L. Jimenez: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
P. Campuzano Jost: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
T. B. Ryerson: NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
I. Bourgeois: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
I. Bourgeois: NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
J. Peischl: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
J. Peischl: NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
C. R. Thompson: NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
E. Ray: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USA
E. Ray: NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
P. O. Wennberg: Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, USA
P. O. Wennberg: Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125, USA
J. Crounse: Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, USA
M. Kim: Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, USA
H. M. Allen: Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
P. A. Newman: NASA Goddard Space Flight Center, Greenbelt, MD 20771, USA
B. B. Stephens: Earth Observing Laboratory, National Center for Atmospheric Research (NCAR), Boulder, CO 80301, USA
E. C. Apel: Atmospheric Chemistry Observations and Modeling Lab, NCAR, Boulder, CO 80301, USA
R. S. Hornbrook: Atmospheric Chemistry Observations and Modeling Lab, NCAR, Boulder, CO 80301, USA
B. A. Nault: Center for Aerosol and Cloud Chemistry, Aerodyne Research, Inc., Billerica, MA 01821, USA
E. Morgan: Scripps Institution of Oceanography, University of California San Diego, CA 92037, USA
S. C. Wofsy: John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA

DOI: https://doi.org/10.5194/acp-21-11113-2021
Journal volume & issue: Vol. 21
pp. 11113 – 11132

Abstract

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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.

Published in Atmospheric Chemistry and Physics

ISSN: 1680-7316 (Print); 1680-7324 (Online)
Publisher: Copernicus Publications
Country of publisher: Germany
LCC subjects: Science: Physics; Science: Chemistry
Website: http://www.atmospheric-chemistry-and-physics.net/

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