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Title: Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States

Abstract

Abstract Deep convective transport of gaseous precursors to ozone (O 3 ) and aerosols to the upper troposphere is affected by liquid phase and mixed‐phase scavenging, entrainment of free tropospheric air and aqueous chemistry. The contributions of these processes are examined using aircraft measurements obtained in storm inflow and outflow during the 2012 Deep Convective Clouds and Chemistry (DC3) experiment combined with high‐resolution (d x ≤3 km) WRF‐Chem simulations of a severe storm, an air mass storm, and a mesoscale convective system (MCS). The simulation results for the MCS suggest that formaldehyde (CH 2 O) is not retained in ice when cloud water freezes, in agreement with previous studies of the severe storm. By analyzing WRF‐Chem trajectories, the effects of scavenging, entrainment, and aqueous chemistry on outflow mixing ratios of CH 2 O, methyl hydroperoxide (CH 3 OOH), and hydrogen peroxide (H 2 O 2 ) are quantified. Liquid phase microphysical scavenging was the dominant process reducing CH 2 O and H 2 O 2 outflow mixing ratios in all three storms. Aqueous chemistry did not significantly affect outflow mixing ratios of all three species. In the severe storm and MCS, the higher than expected reductions in CH 3 OOH mixingmore » ratios in the storm cores were primarily due to entrainment of low‐background CH 3 OOH. In the air mass storm, lower CH 3 OOH and H 2 O 2 scavenging efficiencies (SEs) than in the MCS were partly due to entrainment of higher background CH 3 OOH and H 2 O 2 . Overestimated rain and hail production in WRF‐Chem reduces the confidence in ice retention fraction values determined for the peroxides and CH 2 O.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [9]; ORCiD logo [2]; ORCiD logo [10]; ORCiD logo [11]; ORCiD logo [11]; ORCiD logo [9]; ORCiD logo [9]; ORCiD logo [9]
  1. Department of Atmospheric and Oceanic Sciences University of Colorado Boulder Boulder CO USA, Laboratory for Atmospheric and Space Physics University of Colorado Boulder Boulder CO USA, Cooperative Institute for Research in the Environmental Sciences University of Colorado Boulder Boulder CO USA, Chemical Sciences Division, Earth System Research Laboratory National Oceanic and Atmospheric Administration Boulder CO USA
  2. National Center for Atmospheric Research Boulder CO USA
  3. Department of Atmospheric and Oceanic Sciences University of Colorado Boulder Boulder CO USA, Laboratory for Atmospheric and Space Physics University of Colorado Boulder Boulder CO USA
  4. Institute of Arctic and Alpine Research University of Colorado Boulder Boulder CO USA
  5. National Severe Storms Laboratory National Oceanic and Atmospheric Administration Norman OK USA
  6. Department of Atmospheric and Oceanic Science University of Maryland College Park MD USA, Kennedy Space Center National Aeronautics and Space Administration Merritt Island FL USA
  7. Department of Atmospheric and Oceanic Science University of Maryland College Park MD USA
  8. Department of Atmospheric and Oceanic Science University of Maryland College Park MD USA, Goddard Space Flight Center National Aeronautics and Space Administration Greenbelt MD USA
  9. School of Meteorology University of Oklahoma Norman OK USA
  10. Pacific Northwest National Laboratory Richland WA USA
  11. Department of Atmospheric Science University of Alabama Huntsville AL USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1493469
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Name: Journal of Geophysical Research: Atmospheres Journal Volume: 123 Journal Issue: 14; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union (AGU)
Country of Publication:
United States
Language:
English

Citation Formats

Bela, Megan M., Barth, Mary C., Toon, Owen Brian, Fried, Alan, Ziegler, Conrad, Cummings, Kristin A., Li, Yunyao, Pickering, Kenneth E., Homeyer, Cameron R., Morrison, Hugh, Yang, Qing, Mecikalski, Retha M., Carey, Larry, Biggerstaff, Michael I., Betten, Daniel P., and Alford, A. Addison. Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States. United States: N. p., 2018. Web. doi:10.1029/2018JD028271.
Bela, Megan M., Barth, Mary C., Toon, Owen Brian, Fried, Alan, Ziegler, Conrad, Cummings, Kristin A., Li, Yunyao, Pickering, Kenneth E., Homeyer, Cameron R., Morrison, Hugh, Yang, Qing, Mecikalski, Retha M., Carey, Larry, Biggerstaff, Michael I., Betten, Daniel P., & Alford, A. Addison. Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States. United States. https://doi.org/10.1029/2018JD028271
Bela, Megan M., Barth, Mary C., Toon, Owen Brian, Fried, Alan, Ziegler, Conrad, Cummings, Kristin A., Li, Yunyao, Pickering, Kenneth E., Homeyer, Cameron R., Morrison, Hugh, Yang, Qing, Mecikalski, Retha M., Carey, Larry, Biggerstaff, Michael I., Betten, Daniel P., and Alford, A. Addison. Thu . "Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States". United States. https://doi.org/10.1029/2018JD028271.
@article{osti_1493469,
title = {Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States},
author = {Bela, Megan M. and Barth, Mary C. and Toon, Owen Brian and Fried, Alan and Ziegler, Conrad and Cummings, Kristin A. and Li, Yunyao and Pickering, Kenneth E. and Homeyer, Cameron R. and Morrison, Hugh and Yang, Qing and Mecikalski, Retha M. and Carey, Larry and Biggerstaff, Michael I. and Betten, Daniel P. and Alford, A. Addison},
abstractNote = {Abstract Deep convective transport of gaseous precursors to ozone (O 3 ) and aerosols to the upper troposphere is affected by liquid phase and mixed‐phase scavenging, entrainment of free tropospheric air and aqueous chemistry. The contributions of these processes are examined using aircraft measurements obtained in storm inflow and outflow during the 2012 Deep Convective Clouds and Chemistry (DC3) experiment combined with high‐resolution (d x ≤3 km) WRF‐Chem simulations of a severe storm, an air mass storm, and a mesoscale convective system (MCS). The simulation results for the MCS suggest that formaldehyde (CH 2 O) is not retained in ice when cloud water freezes, in agreement with previous studies of the severe storm. By analyzing WRF‐Chem trajectories, the effects of scavenging, entrainment, and aqueous chemistry on outflow mixing ratios of CH 2 O, methyl hydroperoxide (CH 3 OOH), and hydrogen peroxide (H 2 O 2 ) are quantified. Liquid phase microphysical scavenging was the dominant process reducing CH 2 O and H 2 O 2 outflow mixing ratios in all three storms. Aqueous chemistry did not significantly affect outflow mixing ratios of all three species. In the severe storm and MCS, the higher than expected reductions in CH 3 OOH mixing ratios in the storm cores were primarily due to entrainment of low‐background CH 3 OOH. In the air mass storm, lower CH 3 OOH and H 2 O 2 scavenging efficiencies (SEs) than in the MCS were partly due to entrainment of higher background CH 3 OOH and H 2 O 2 . Overestimated rain and hail production in WRF‐Chem reduces the confidence in ice retention fraction values determined for the peroxides and CH 2 O.},
doi = {10.1029/2018JD028271},
journal = {Journal of Geophysical Research: Atmospheres},
number = 14,
volume = 123,
place = {United States},
year = {Thu Jul 19 00:00:00 EDT 2018},
month = {Thu Jul 19 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1029/2018JD028271

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Cited by: 14 works
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