skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Journal of Geophysical Research: Atmospheres
DOI:https://doi.org/10.1029/2018JD028271· OSTI ID:1493469
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
+ Show Author Affiliations

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.

Sponsoring Organization:
USDOE
OSTI ID:
1493469
Journal Information:
Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Vol. 123 Journal Issue: 14; ISSN 2169-897X
Publisher:
American Geophysical Union (AGU)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

References (73)

Scavenging of acidic gases (HCOOH, CH 3 COOH, HNO 3 , HCl, and SO 2 ) and ammonia in mixed liquid-solid water clouds at the Puy de Dôme mountain (France) journal March 2000
Combined Satellite- and Surface-Based Estimation of the Intracloud–Cloud-to-Ground Lightning Ratio over the Continental United States journal January 2001
Wind tunnel experiments on the retention of trace gases during riming: nitric acid, hydrochloric acid, and hydrogen peroxide journal January 2011
A New Vertical Diffusion Package with an Explicit Treatment of Entrainment Processes journal September 2006
Lightning-generated NO X and its impact on tropospheric ozone production: A three-dimensional modeling study of a Stratosphere-Troposphere Experiment: Radiation, Aerosols and Ozone (STERAO-A) thunderstorm : LIGHTNING NO journal July 2005
Effects of Horizontal and Vertical Grid Spacing on Mixing in Simulated Squall Lines and Implications for Convective Strength and Structure journal November 2015
A Diabatic Lagrangian Technique for the Analysis of Convective Storms. Part II: Application to a Radar-Observed Storm journal October 2013
The retention of ammonia and sulfur dioxide during riming of ice particles and dendritic snow flakes: laboratory experiments in the Mainz vertical wind tunnel journal June 2013
Kinetics of aqueous phase reactions of the SO 4 − radical with potential importance in cloud chemistry journal January 1989
Aqueous phase oxidation of sulfur(IV) by hydrogen peroxide, methylhydroperoxide, and peroxyacetic acid journal January 1987
A simple lightning parameterization for calculating global lightning distributions journal June 1992
A Diabatic Lagrangian Technique for the Analysis of Convective Storms. Part I: Description and Validation via an Observing System Simulation Experiment journal October 2013
Reactions of hydroxyl radicals with hydrogen peroxide at ambient and elevated temperatures journal April 1982
A cloud chemistry module for the 3-D cloud-resolving mesoscale model Meso-NH with application to idealized cases journal January 2013
Fully coupled “online” chemistry within the WRF model journal December 2005
Photodissociation in the atmosphere: 1. Actinic flux and the effects of ground reflections and clouds journal January 1987
A New Double-Moment Microphysics Parameterization for Application in Cloud and Climate Models. Part I: Description journal June 2005
Deep convective clouds with sustained supercooled liquid water down to -37.5 °C journal May 2000
The fate of volatile chemicals during wet growth of a hailstone journal January 2009
Numerical simulations of the July 10, 1996, Stratospheric-Tropospheric Experiment: Radiation, Aerosols, and Ozone (STERAO)-Deep Convection experiment storm: Redistribution of soluble tracers journal June 2001
Tropospheric Aerosol Optical Thickness from the GOCART Model and Comparisons with Satellite and Sun Photometer Measurements journal February 2002
The Shared Mobile Atmospheric Research and Teaching Radar: A Collaboration to Enhance Research and Teaching journal September 2005
Convective transport of formaldehyde to the upper troposphere and lower stratosphere and associated scavenging in thunderstorms over the central United States during the 2012 DC3 study: Formaldehyde Scavenging in Thunderstorms journal June 2016
Model sensitivity studies regarding the role of the retention coefficient for the scavenging and redistribution of highly soluble trace gases by deep convective cloud systems journal January 2007
Kinetics and mechanism of the formation of hydroxymethanesulfonic acid at low pH journal September 1984
Decomposition of ozone in water: rate of initiation by hydroxide ions and hydrogen peroxide journal October 1982
Laboratory and modelling studies of tropospheric multiphase conversions involving some C1 and C2 peroxyl radicals journal January 1999
Transport and scavenging of soluble gases in a deep convective cloud journal September 2000
‘Application of a New Spectral Theory of Stably Stratified Turbulence to the Atmospheric Boundary Layer over Sea Ice’ journal November 2005
Kinetics and mechanism of the oxidation of aquated sulfur dioxide by hydrogen peroxide at low pH journal December 1983
Sensitivity of simulated convection‐driven stratosphere‐troposphere exchange in WRF‐Chem to the choice of physical and chemical parameterization journal August 2017
Evaluating Mesoscale NWP Models Using Kinetic Energy Spectra journal December 2004
Rate Constants for Reactions of Inorganic Radicals in Aqueous Solution journal July 1988
An overview of the 29 May 2012 Kingfisher supercell during DC3: OBSERVATIONS OF THE 29 MAY 2012 DC3 CASE journal December 2016
The effect of freezing on the composition of supercooled droplets—I. Retention of HCl, HNO3, NH3 and H2O2 journal January 1990
Hydrogen peroxide, methyl hydroperoxide, and formaldehyde over North America and the North Atlantic journal January 2007
Wet scavenging of soluble gases in DC3 deep convective storms using WRF‐Chem simulations and aircraft observations journal April 2016
Aircraft Observations of Cumulus Microphysics Ranging from the Tropics to Midlatitudes: Implications for a “New” Secondary Ice Process journal September 2017
Chemistry of OH in remote clouds and its role in the production of formic acid and peroxymonosulfate journal January 1986
The Deep Convective Clouds and Chemistry (DC3) Field Campaign journal August 2015
Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone journal January 2012
Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3: Convective Transport of Peroxides journal April 2016
The Fire INventory from NCAR (FINN): a high resolution global model to estimate the emissions from open burning journal January 2011
Effect of clouds on photolysis and oxidants in the troposphere journal January 2003
Assessing Errors in Variational Dual-Doppler Wind Syntheses of Supercell Thunderstorms Observed by Storm-Scale Mobile Radars journal August 2012
Factors influencing the retention of hydrogen peroxide and molecular oxygen in rime ice journal January 1998
Radiative forcing by long-lived greenhouse gases: Calculations with the AER radiative transfer models journal January 2008
Transport of ozone to the surface by convective downdrafts at night journal January 2002
Simulations of the redistribution of formaldehyde, formic acid, and peroxides in the 10 July 1996 Stratospheric-Tropospheric Experiment: Radiation, Aerosols, and Ozone deep convection storm: SIMULATION OF MIDLATITUDE THUNDERSTORM AND CHEMISTRY journal July 2007
Radar and Lightning Observations of Deep Moist Convection across Northern Alabama during DC3: 21 May 2012 journal July 2015
Bulk Parameterization of the Snow Field in a Cloud Model journal June 1983
Aerosol transport and wet scavenging in deep convective clouds: A case study and model evaluation using a multiple passive tracer analysis approach journal August 2015
Sensitivity of a Simulated Squall Line to Horizontal Resolution and Parameterization of Microphysics journal January 2012
Evolution of ozone, particulates, and aerosol direct radiative forcing in the vicinity of Houston using a fully coupled meteorology-chemistry-aerosol model journal January 2006
Chemistry of riming: the retention of organic and inorganic atmospheric trace constituents journal January 2017
REEVALUATION OF THE SPECTRAL AND KINETIC PROPERTIES OF HO 2 AND O 2 - FREE RADICALS journal October 1978
Rate constants for some oxidations of S(IV) by radicals in aqueous solutions journal January 1987
Reaction of Dihydroxymethyl Radical with Molecular Oxygen in Aqueous Solution journal August 1980
Convective injection and photochemical decay of peroxides in the tropical upper troposphere: Methyl iodide as a tracer of marine convection journal March 1999
Resolution Requirements for the Simulation of Deep Moist Convection journal October 2003
The role of clouds in tropospheric photochemistry journal April 1991
Summary of the cloud chemistry modeling intercomparison: Photochemical box model simulation journal January 2003
Downward transport of ozone rich air and implications for atmospheric chemistry in the Amazon rainforest journal January 2016
A compilation of specific bimolecular rate constants for the reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals with inorganic and organic compounds in aqueous solution journal July 1967
Flash propagation and inferred charge structure relative to radar‐observed ice alignment signatures in a small Florida mesoscale convective system journal August 2017
Description and evaluation of the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) journal January 2010
Evaluation of deep convective transport in storms from different convective regimes during the DC3 field campaign using WRF-Chem with lightning data assimilation: Convective Transport in DC3 Storms journal July 2017
Hydrogen peroxide retention in rime ice journal January 1992
Impact of Cloud Microphysics on the Development of Trailing Stratiform Precipitation in a Simulated Squall Line: Comparison of One- and Two-Moment Schemes journal March 2009
Relationships between Lightning Location and Polarimetric Radar Signatures in a Small Mesoscale Convective System journal December 2009
TELEX The Thunderstorm Electrification and Lightning Experiment journal July 2008
The impact of North American anthropogenic emissions and lightning on long-range transport of trace gases and their export from the continent during summers 2002 and 2004 journal January 2011
Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature) journal January 2006

Similar Records

Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States
Journal Article · Fri Jul 27 00:00:00 EDT 2018 · Journal of Geophysical Research: Atmospheres · OSTI ID:1493469
+13 more
Wet scavenging of soluble gases in DC3 deep convective storms using WRF-Chem simulations and aircraft observations
Journal Article · Thu Apr 21 00:00:00 EDT 2016 · Journal of Geophysical Research: Atmospheres · OSTI ID:1493469
+23 more
Aerosol transport and wet scavenging in deep convective clouds: a case study and model evaluation using a multiple passive tracer analysis approach
Journal Article · Thu Aug 20 00:00:00 EDT 2015 · Journal of Geophysical Research. D. (Atmospheres), 120(16):8448-8468 · OSTI ID:1493469
+17 more

Related Subjects