Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3

M. C. Barth, M. M. Bela, A. Fried, P. O. Wennberg, J. D. Crounse, J. M. St.Clair, N. J. Blake, D. R. Blake, C. R. Homeyer, William Henry Brune, L. Zhang, J. Mao, X. Ren, T. B. Ryerson, I. B. Pollack, J. Peischl, R. C. Cohen, B. A. Nault, L. G. Huey, X. LiuC. A. Cantrell

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Abstract

One of the objectives of the Deep Convective Clouds and Chemistry (DC3) field experiment was to determine the scavenging of soluble trace gases by thunderstorms. We present an analysis of scavenging of hydrogen peroxide (H2O2) and methyl hydrogen peroxide (CH3OOH) from six DC3 cases that occurred in Oklahoma and northeast Colorado. Estimates of H2O2 scavenging efficiencies are comparable to previous studies ranging from 79 to 97% with relative uncertainties of 5–25%. CH3OOH scavenging efficiencies ranged from 12 to 84% with relative uncertainties of 18–558%. The wide range of CH3OOH scavenging efficiencies is surprising, as previous studies suggested that CH3OOH scavenging efficiencies would be <10%. Cloud chemistry model simulations of one DC3 storm produced CH3OOH scavenging efficiencies of 26–61% depending on the ice retention factor of CH3OOH during cloud drop freezing, suggesting ice physics impacts CH3OOH scavenging. The highest CH3OOH scavenging efficiencies occurred in two severe thunderstorms, but there is no obvious correlation between the CH3OOH scavenging efficiency and the storm thermodynamic environment. We found a moderate correlation between the estimated entrainment rates and CH3OOH scavenging efficiencies. Changes in gas-phase chemistry due to lightning production of nitric oxide and aqueous-phase chemistry have little effect on CH3OOH scavenging efficiencies. To determine why CH3OOH can be substantially removed from storms, future studies should examine effects of entrainment rate, retention of CH3OOH in frozen cloud particles during drop freezing, and lightning-NOx production.

Original languageEnglish (US)
Pages (from-to)4272-4295
Number of pages24
JournalJournal of Geophysical Research
Volume121
Issue number8
DOIs
StatePublished - Jan 1 2016

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Thunderstorms
thunderstorms
Scavenging
scavenging
Peroxides
peroxides
thunderstorm
chemistry
lightning
entrainment
hydrogen peroxide
freezing
ice
uncertainty
gases
convective cloud
nitric oxide
physics
trace gas
thermodynamics

All Science Journal Classification (ASJC) codes

  • Geophysics
  • Forestry
  • Oceanography
  • Aquatic Science
  • Ecology
  • Water Science and Technology
  • Soil Science
  • Geochemistry and Petrology
  • Earth-Surface Processes
  • Atmospheric Science
  • Earth and Planetary Sciences (miscellaneous)
  • Space and Planetary Science
  • Palaeontology

Cite this

Barth, M. C., Bela, M. M., Fried, A., Wennberg, P. O., Crounse, J. D., St.Clair, J. M., ... Cantrell, C. A. (2016). Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3. Journal of Geophysical Research, 121(8), 4272-4295. https://doi.org/10.1002/2015JD024570
Barth, M. C. ; Bela, M. M. ; Fried, A. ; Wennberg, P. O. ; Crounse, J. D. ; St.Clair, J. M. ; Blake, N. J. ; Blake, D. R. ; Homeyer, C. R. ; Brune, William Henry ; Zhang, L. ; Mao, J. ; Ren, X. ; Ryerson, T. B. ; Pollack, I. B. ; Peischl, J. ; Cohen, R. C. ; Nault, B. A. ; Huey, L. G. ; Liu, X. ; Cantrell, C. A. / Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3. In: Journal of Geophysical Research. 2016 ; Vol. 121, No. 8. pp. 4272-4295.
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abstract = "One of the objectives of the Deep Convective Clouds and Chemistry (DC3) field experiment was to determine the scavenging of soluble trace gases by thunderstorms. We present an analysis of scavenging of hydrogen peroxide (H2O2) and methyl hydrogen peroxide (CH3OOH) from six DC3 cases that occurred in Oklahoma and northeast Colorado. Estimates of H2O2 scavenging efficiencies are comparable to previous studies ranging from 79 to 97{\%} with relative uncertainties of 5–25{\%}. CH3OOH scavenging efficiencies ranged from 12 to 84{\%} with relative uncertainties of 18–558{\%}. The wide range of CH3OOH scavenging efficiencies is surprising, as previous studies suggested that CH3OOH scavenging efficiencies would be <10{\%}. Cloud chemistry model simulations of one DC3 storm produced CH3OOH scavenging efficiencies of 26–61{\%} depending on the ice retention factor of CH3OOH during cloud drop freezing, suggesting ice physics impacts CH3OOH scavenging. The highest CH3OOH scavenging efficiencies occurred in two severe thunderstorms, but there is no obvious correlation between the CH3OOH scavenging efficiency and the storm thermodynamic environment. We found a moderate correlation between the estimated entrainment rates and CH3OOH scavenging efficiencies. Changes in gas-phase chemistry due to lightning production of nitric oxide and aqueous-phase chemistry have little effect on CH3OOH scavenging efficiencies. To determine why CH3OOH can be substantially removed from storms, future studies should examine effects of entrainment rate, retention of CH3OOH in frozen cloud particles during drop freezing, and lightning-NOx production.",
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Barth, MC, Bela, MM, Fried, A, Wennberg, PO, Crounse, JD, St.Clair, JM, Blake, NJ, Blake, DR, Homeyer, CR, Brune, WH, Zhang, L, Mao, J, Ren, X, Ryerson, TB, Pollack, IB, Peischl, J, Cohen, RC, Nault, BA, Huey, LG, Liu, X & Cantrell, CA 2016, 'Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3', Journal of Geophysical Research, vol. 121, no. 8, pp. 4272-4295. https://doi.org/10.1002/2015JD024570

Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3. / Barth, M. C.; Bela, M. M.; Fried, A.; Wennberg, P. O.; Crounse, J. D.; St.Clair, J. M.; Blake, N. J.; Blake, D. R.; Homeyer, C. R.; Brune, William Henry; Zhang, L.; Mao, J.; Ren, X.; Ryerson, T. B.; Pollack, I. B.; Peischl, J.; Cohen, R. C.; Nault, B. A.; Huey, L. G.; Liu, X.; Cantrell, C. A.

In: Journal of Geophysical Research, Vol. 121, No. 8, 01.01.2016, p. 4272-4295.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3

AU - Barth, M. C.

AU - Bela, M. M.

AU - Fried, A.

AU - Wennberg, P. O.

AU - Crounse, J. D.

AU - St.Clair, J. M.

AU - Blake, N. J.

AU - Blake, D. R.

AU - Homeyer, C. R.

AU - Brune, William Henry

AU - Zhang, L.

AU - Mao, J.

AU - Ren, X.

AU - Ryerson, T. B.

AU - Pollack, I. B.

AU - Peischl, J.

AU - Cohen, R. C.

AU - Nault, B. A.

AU - Huey, L. G.

AU - Liu, X.

AU - Cantrell, C. A.

PY - 2016/1/1

Y1 - 2016/1/1

N2 - One of the objectives of the Deep Convective Clouds and Chemistry (DC3) field experiment was to determine the scavenging of soluble trace gases by thunderstorms. We present an analysis of scavenging of hydrogen peroxide (H2O2) and methyl hydrogen peroxide (CH3OOH) from six DC3 cases that occurred in Oklahoma and northeast Colorado. Estimates of H2O2 scavenging efficiencies are comparable to previous studies ranging from 79 to 97% with relative uncertainties of 5–25%. CH3OOH scavenging efficiencies ranged from 12 to 84% with relative uncertainties of 18–558%. The wide range of CH3OOH scavenging efficiencies is surprising, as previous studies suggested that CH3OOH scavenging efficiencies would be <10%. Cloud chemistry model simulations of one DC3 storm produced CH3OOH scavenging efficiencies of 26–61% depending on the ice retention factor of CH3OOH during cloud drop freezing, suggesting ice physics impacts CH3OOH scavenging. The highest CH3OOH scavenging efficiencies occurred in two severe thunderstorms, but there is no obvious correlation between the CH3OOH scavenging efficiency and the storm thermodynamic environment. We found a moderate correlation between the estimated entrainment rates and CH3OOH scavenging efficiencies. Changes in gas-phase chemistry due to lightning production of nitric oxide and aqueous-phase chemistry have little effect on CH3OOH scavenging efficiencies. To determine why CH3OOH can be substantially removed from storms, future studies should examine effects of entrainment rate, retention of CH3OOH in frozen cloud particles during drop freezing, and lightning-NOx production.

AB - One of the objectives of the Deep Convective Clouds and Chemistry (DC3) field experiment was to determine the scavenging of soluble trace gases by thunderstorms. We present an analysis of scavenging of hydrogen peroxide (H2O2) and methyl hydrogen peroxide (CH3OOH) from six DC3 cases that occurred in Oklahoma and northeast Colorado. Estimates of H2O2 scavenging efficiencies are comparable to previous studies ranging from 79 to 97% with relative uncertainties of 5–25%. CH3OOH scavenging efficiencies ranged from 12 to 84% with relative uncertainties of 18–558%. The wide range of CH3OOH scavenging efficiencies is surprising, as previous studies suggested that CH3OOH scavenging efficiencies would be <10%. Cloud chemistry model simulations of one DC3 storm produced CH3OOH scavenging efficiencies of 26–61% depending on the ice retention factor of CH3OOH during cloud drop freezing, suggesting ice physics impacts CH3OOH scavenging. The highest CH3OOH scavenging efficiencies occurred in two severe thunderstorms, but there is no obvious correlation between the CH3OOH scavenging efficiency and the storm thermodynamic environment. We found a moderate correlation between the estimated entrainment rates and CH3OOH scavenging efficiencies. Changes in gas-phase chemistry due to lightning production of nitric oxide and aqueous-phase chemistry have little effect on CH3OOH scavenging efficiencies. To determine why CH3OOH can be substantially removed from storms, future studies should examine effects of entrainment rate, retention of CH3OOH in frozen cloud particles during drop freezing, and lightning-NOx production.

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