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Research Article

Stratospheric ozone over the United States in summer linked to observations of convection and temperature via chlorine and bromine catalysis

James G. Anderson, Debra K. Weisenstein, Kenneth P. Bowman, Cameron R. Homeyer, Jessica B. Smith, David M. Wilmouth, David S. Sayres, J. Eric Klobas, View ORCID ProfileStephen S. Leroy, John A. Dykema, and Steven C. Wofsy
  1. aDepartment of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138;
  2. bDepartment of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138;
  3. cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
  4. dDepartment of Atmospheric Sciences, Texas A&M University, College Station, TX 77843;
  5. eSchool of Meteorology, University of Oklahoma, Norman, OK 73019

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PNAS June 20, 2017 114 (25) E4905-E4913; first published June 5, 2017; https://doi.org/10.1073/pnas.1619318114
James G. Anderson
aDepartment of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138;
bDepartment of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138;
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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  • For correspondence: anderson@huarp.harvard.edu
Debra K. Weisenstein
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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Kenneth P. Bowman
dDepartment of Atmospheric Sciences, Texas A&M University, College Station, TX 77843;
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Cameron R. Homeyer
eSchool of Meteorology, University of Oklahoma, Norman, OK 73019
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Jessica B. Smith
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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David M. Wilmouth
aDepartment of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138;
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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David S. Sayres
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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J. Eric Klobas
aDepartment of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138;
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Stephen S. Leroy
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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  • ORCID record for Stephen S. Leroy
John A. Dykema
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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Steven C. Wofsy
bDepartment of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138;
cHarvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
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  1. Edited by John H. Seinfeld, California Institute of Technology, Pasadena, CA, and approved May 9, 2017 (received for review November 28, 2016)

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Significance

Stratospheric ozone is one of the most delicate aspects of habitability on the planet. Removal of stratospheric ozone over the polar regions in winter/spring has established the vulnerability of ozone to halogen catalytic cycles. Elevated ClO concentrations engendered, in part, by heterogeneous catalytic conversion of inorganic chlorine to free radical form on ubiquitous sulfate−water aerosols, govern the rate of ozone removal. We report here observations of the frequency and depth of penetration of convectively injected water vapor into the stratosphere, triggered by severe storms that are specific to the central United States in summer, and model their effect on lower stratospheric ozone. This effect implies, with observed temperatures, increased risk of ozone loss over the Great Plains in summer.

Abstract

We present observations defining (i) the frequency and depth of convective penetration of water into the stratosphere over the United States in summer using the Next-Generation Radar system; (ii) the altitude-dependent distribution of inorganic chlorine established in the same coordinate system as the radar observations; (iii) the high resolution temperature structure in the stratosphere over the United States in summer that resolves spatial and structural variability, including the impact of gravity waves; and (iv) the resulting amplification in the catalytic loss rates of ozone for the dominant halogen, hydrogen, and nitrogen catalytic cycles. The weather radar observations of ∼2,000 storms, on average, each summer that reach the altitude of rapidly increasing available inorganic chlorine, coupled with observed temperatures, portend a risk of initiating rapid heterogeneous catalytic conversion of inorganic chlorine to free radical form on ubiquitous sulfate−water aerosols; this, in turn, engages the element of risk associated with ozone loss in the stratosphere over the central United States in summer based upon the same reaction network that reduces stratospheric ozone over the Arctic. The summertime development of the upper-level anticyclonic flow over the United States, driven by the North American Monsoon, provides a means of retaining convectively injected water, thereby extending the time for catalytic ozone loss over the Great Plains. Trusted decadal forecasts of UV dosage over the United States in summer require understanding the response of this dynamical and photochemical system to increased forcing of the climate by increasing levels of CO2 and CH4.

  • stratospheric ozone
  • climate change
  • UV radiation human health effects
  • convection
  • water vapor

Footnotes

  • ↵1To whom correspondence should be addressed. Email: anderson{at}huarp.harvard.edu.
  • Author contributions: J.G.A. designed research; J.G.A. and D.K.W. performed research; D.K.W., K.P.B., C.R.H., J.B.S., D.M.W., D.S.S., J.E.K., S.S.L., J.A.D., and S.C.W. analyzed data; J.G.A. wrote the paper; K.P.B. and C.R.H. contributed NEXRAD data; and J.B.S., D.M.W., and D.S.S. contributed in situ data.

  • The authors declare no conflict of interest.

  • This article is a PNAS Direct Submission.

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Stratospheric ozone over United States in summer
James G. Anderson, Debra K. Weisenstein, Kenneth P. Bowman, Cameron R. Homeyer, Jessica B. Smith, David M. Wilmouth, David S. Sayres, J. Eric Klobas, Stephen S. Leroy, John A. Dykema, Steven C. Wofsy
Proceedings of the National Academy of Sciences Jun 2017, 114 (25) E4905-E4913; DOI: 10.1073/pnas.1619318114

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Stratospheric ozone over United States in summer
James G. Anderson, Debra K. Weisenstein, Kenneth P. Bowman, Cameron R. Homeyer, Jessica B. Smith, David M. Wilmouth, David S. Sayres, J. Eric Klobas, Stephen S. Leroy, John A. Dykema, Steven C. Wofsy
Proceedings of the National Academy of Sciences Jun 2017, 114 (25) E4905-E4913; DOI: 10.1073/pnas.1619318114
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Proceedings of the National Academy of Sciences: 114 (25)
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    • Advances in Stratospheric Observations
    • Two-Dimensional Model Calculations Exploring the Sensitivity of the Rate-Limiting Steps in the Dominant Ozone Loss Processes to Perturbations in Temperature and Water Vapor
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