Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom
<p>We measured the global distribution of tropospheric N<span class="inline-formula"><sub>2</sub></span>O mixing ratios during the NASA airborne Atmospheric Tomography (ATom) mission. ATom measured concentrations of <span class="inline-formula">...
Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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Format: | Article |
Language: | English |
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Copernicus Publications
2021-07-01
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Series: | Atmospheric Chemistry and Physics |
Online Access: | https://acp.copernicus.org/articles/21/11113/2021/acp-21-11113-2021.pdf |
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record_format |
Article |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
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 |
spellingShingle |
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 Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom Atmospheric Chemistry and Physics |
author_facet |
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 |
author_sort |
Y. Gonzalez |
title |
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom |
title_short |
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom |
title_full |
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom |
title_fullStr |
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom |
title_full_unstemmed |
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom |
title_sort |
impact of stratospheric air and surface emissions on tropospheric nitrous oxide during atom |
publisher |
Copernicus Publications |
series |
Atmospheric Chemistry and Physics |
issn |
1680-7316 1680-7324 |
publishDate |
2021-07-01 |
description |
<p>We measured the global distribution of tropospheric N<span class="inline-formula"><sub>2</sub></span>O
mixing ratios during the NASA airborne Atmospheric Tomography (ATom)
mission. ATom measured concentrations of <span class="inline-formula">∼</span> 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 N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O measurements by a factor of three (based
on the standard deviation of calibration measurements). Our measurements show that most
of the variance of N<span class="inline-formula"><sub>2</sub></span>O mixing ratios in the troposphere is driven by
the influence of N<span class="inline-formula"><sub>2</sub></span>O-depleted stratospheric air, especially at mid- and
high latitudes. We observe the downward propagation of lower N<span class="inline-formula"><sub>2</sub></span>O mixing
ratios (compared to surface stations) that tracks the influence of
stratosphere–troposphere exchange through the tropospheric column down to
the surface. The highest N<span class="inline-formula"><sub>2</sub></span>O mixing ratios occur close to the Equator,
extending through the boundary layer and<span id="page11114"/> free troposphere. We observed
influences from a complex and diverse mixture of N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O 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
N<span class="inline-formula"><sub>2</sub></span>O mixing ratios are mostly associated with pollution-related tracers
arriving from the coastal area of Nigeria. Peaks of N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O global budget. The
extensive data set from ATom will help improve the understanding of N<span class="inline-formula"><sub>2</sub></span>O
emission processes and their representation in global models.</p> |
url |
https://acp.copernicus.org/articles/21/11113/2021/acp-21-11113-2021.pdf |
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doaj-31481aace19749b9945229df648b2b2a2021-07-22T12:57:12ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242021-07-0121111131113210.5194/acp-21-11113-2021Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATomY. Gonzalez0Y. Gonzalez1Y. Gonzalez2R. Commane3R. Commane4R. Commane5E. Manninen6B. C. Daube7L. D. Schiferl8J. B. McManus9K. McKain10K. McKain11E. J. Hintsa12E. J. Hintsa13J. W. Elkins14S. A. Montzka15C. Sweeney16F. Moore17F. Moore18J. L. Jimenez19P. Campuzano Jost20T. B. Ryerson21I. Bourgeois22I. Bourgeois23J. Peischl24J. Peischl25C. R. Thompson26E. Ray27E. Ray28P. O. Wennberg29P. O. Wennberg30J. Crounse31M. Kim32H. M. Allen33P. A. Newman34B. B. Stephens35E. C. Apel36R. S. Hornbrook37B. A. Nault38E. Morgan39S. C. Wofsy40John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USACIMEL Electronique, Paris, 75011, FranceIzaña Atmospheric Research Centre, Santa Cruz de Tenerife, 38001, SpainJohn A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USADept. of Earth and Environmental Science, Columbia University, New York, NY 10027, USALamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, USAJohn A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USAJohn A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USALamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, USACenter for Atmospheric and Environmental Chemistry, Aerodyne Research Inc., Billerica, MA 01821, USANOAA Global Monitoring Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USANOAA Global Monitoring Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USANOAA Global Monitoring Laboratory, Boulder, CO 80305, USANOAA Global Monitoring Laboratory, Boulder, CO 80305, USANOAA Global Monitoring Laboratory, Boulder, CO 80305, USANOAA Global Monitoring Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USANOAA Chemical Sciences Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USANOAA Chemical Sciences Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USANOAA Chemical Sciences Laboratory, Boulder, CO 80305, USANOAA Chemical Sciences Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, USANOAA Chemical Sciences Laboratory, Boulder, CO 80305, USADivision of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, USADivision of Engineering and Applied Science, California Institute of Technology, Pasadena, CA 91125, USADivision of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, USADivision of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, USADivision of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USANASA Goddard Space Flight Center, Greenbelt, MD 20771, USAEarth Observing Laboratory, National Center for Atmospheric Research (NCAR), Boulder, CO 80301, USAAtmospheric Chemistry Observations and Modeling Lab, NCAR, Boulder, CO 80301, USAAtmospheric Chemistry Observations and Modeling Lab, NCAR, Boulder, CO 80301, USACenter for Aerosol and Cloud Chemistry, Aerodyne Research, Inc., Billerica, MA 01821, USAScripps Institution of Oceanography, University of California San Diego, CA 92037, USAJohn A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA<p>We measured the global distribution of tropospheric N<span class="inline-formula"><sub>2</sub></span>O mixing ratios during the NASA airborne Atmospheric Tomography (ATom) mission. ATom measured concentrations of <span class="inline-formula">∼</span> 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 N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O measurements by a factor of three (based on the standard deviation of calibration measurements). Our measurements show that most of the variance of N<span class="inline-formula"><sub>2</sub></span>O mixing ratios in the troposphere is driven by the influence of N<span class="inline-formula"><sub>2</sub></span>O-depleted stratospheric air, especially at mid- and high latitudes. We observe the downward propagation of lower N<span class="inline-formula"><sub>2</sub></span>O mixing ratios (compared to surface stations) that tracks the influence of stratosphere–troposphere exchange through the tropospheric column down to the surface. The highest N<span class="inline-formula"><sub>2</sub></span>O mixing ratios occur close to the Equator, extending through the boundary layer and<span id="page11114"/> free troposphere. We observed influences from a complex and diverse mixture of N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O mixing ratios are mostly associated with pollution-related tracers arriving from the coastal area of Nigeria. Peaks of N<span class="inline-formula"><sub>2</sub></span>O 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 N<span class="inline-formula"><sub>2</sub></span>O global budget. The extensive data set from ATom will help improve the understanding of N<span class="inline-formula"><sub>2</sub></span>O emission processes and their representation in global models.</p>https://acp.copernicus.org/articles/21/11113/2021/acp-21-11113-2021.pdf |