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

Title: Representing effects of aqueous phase reactions in shallow cumuli in global models

Abstract

Aqueous phase reactions are important, sometimes dominant (e.g., for SO2), pathways for the oxidation of air pollutants at the local and/or global scale. In many current chemical transport models (CTMs), the transport and aqueous reactions of chemical species are treated as split processes, and the subgrid-scale heterogeneity between cloudy and environmental air is not considered. Here using large eddy simulation (LES) with idealized aqueous reactions mimicking the oxidation of surface-originated SO2 by H2O2 in shallow cumuli, we show that the eddy diffusivity mass flux (EDMF) approach with a bulk plume can represent those processes quite well when entrainment/detrainment rates and eddy diffusivity are diagnosed using a conservative thermodynamic variable such as total water content. The reason is that a typical aqueous reaction such as SO2 aqueous oxidation is relatively slow compared to the in-cloud residence time of air parcels in shallow cumuli. As a result, the surface-originated SO2 is well correlated with and behaves like conservative thermodynamic variables that also have sources at the surface. Experiments with various reaction rate constants and relative abundances of SO2 and H2O2 indicate that when the reaction timescale approaches the in-cloud residence time of air parcels, the errors of the bulk plume approach startmore » to increase. Finally, treating chemical tracer transport and aqueous reaction as split processes leads to significant errors, especially when the reaction is fast compared to the in-cloud residence time. Overall, the EDMF approach shows large improvement over the CTM-like treatments in matching the LES results.« less

Authors:
 [1];  [2];  [3];  [3]
  1. Columbia Univ., New York, NY (United States). Lamont-Doherty Earth Observatory
  2. Harvard Univ., Cambridge, MA (United States). Dept. of Earth and Planetary Sciences and John A. Paulson School of Engineering and Applied Sciences
  3. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
Publication Date:
Research Org.:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1469111
Grant/Contract Number:  
SC0008679
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Volume: 121; Journal Issue: 10; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Nie, Ji, Kuang, Zhiming, Jacob, Daniel J., and Guo, Jiahua. Representing effects of aqueous phase reactions in shallow cumuli in global models. United States: N. p., 2016. Web. doi:10.1002/2015JD024208.
Nie, Ji, Kuang, Zhiming, Jacob, Daniel J., & Guo, Jiahua. Representing effects of aqueous phase reactions in shallow cumuli in global models. United States. doi:10.1002/2015JD024208.
Nie, Ji, Kuang, Zhiming, Jacob, Daniel J., and Guo, Jiahua. Tue . "Representing effects of aqueous phase reactions in shallow cumuli in global models". United States. doi:10.1002/2015JD024208. https://www.osti.gov/servlets/purl/1469111.
@article{osti_1469111,
title = {Representing effects of aqueous phase reactions in shallow cumuli in global models},
author = {Nie, Ji and Kuang, Zhiming and Jacob, Daniel J. and Guo, Jiahua},
abstractNote = {Aqueous phase reactions are important, sometimes dominant (e.g., for SO2), pathways for the oxidation of air pollutants at the local and/or global scale. In many current chemical transport models (CTMs), the transport and aqueous reactions of chemical species are treated as split processes, and the subgrid-scale heterogeneity between cloudy and environmental air is not considered. Here using large eddy simulation (LES) with idealized aqueous reactions mimicking the oxidation of surface-originated SO2 by H2O2 in shallow cumuli, we show that the eddy diffusivity mass flux (EDMF) approach with a bulk plume can represent those processes quite well when entrainment/detrainment rates and eddy diffusivity are diagnosed using a conservative thermodynamic variable such as total water content. The reason is that a typical aqueous reaction such as SO2 aqueous oxidation is relatively slow compared to the in-cloud residence time of air parcels in shallow cumuli. As a result, the surface-originated SO2 is well correlated with and behaves like conservative thermodynamic variables that also have sources at the surface. Experiments with various reaction rate constants and relative abundances of SO2 and H2O2 indicate that when the reaction timescale approaches the in-cloud residence time of air parcels, the errors of the bulk plume approach start to increase. Finally, treating chemical tracer transport and aqueous reaction as split processes leads to significant errors, especially when the reaction is fast compared to the in-cloud residence time. Overall, the EDMF approach shows large improvement over the CTM-like treatments in matching the LES results.},
doi = {10.1002/2015JD024208},
journal = {Journal of Geophysical Research: Atmospheres},
number = 10,
volume = 121,
place = {United States},
year = {2016},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Cloud Resolving Modeling of the ARM Summer 1997 IOP: Model Formulation, Results, Uncertainties, and Sensitivities
journal, February 2003


Attribution of modeled atmospheric sulfate and SO<sub>2</sub> in the Northern Hemisphere for June–July 1997
journal, January 2006

  • Benkovitz, C. M.; Schwartz, S. E.; Jensen, M. P.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 12
  • DOI: 10.5194/acp-6-4723-2006

The multi-scale aerosol-climate model PNNL-MMF: model description and evaluation
journal, January 2011


Sulfate formation in sea-salt aerosols: Constraints from oxygen isotopes
journal, January 2005


Atmospheric hydrogen peroxide
journal, October 1990

  • Sakugawa, Hiroshi; Kaplan, Isaac R.; Tsai, Wangteng
  • Environmental Science & Technology, Vol. 24, Issue 10
  • DOI: 10.1021/es00080a002

A Multiparcel Model for Shallow Cumulus Convection
journal, May 2002


Tracer Transport in Deep Convective Updrafts: Plume Ensemble versus Bulk Formulations
journal, August 2005

  • Lawrence, Mark G.; Rasch, Philip J.
  • Journal of the Atmospheric Sciences, Vol. 62, Issue 8
  • DOI: 10.1175/JAS3505.1

Influence of fair-weather cumulus clouds on isoprene chemistry: IMPACT OF SHALLOW CONVECTION ON ISOPRENE
journal, May 2012

  • Kim, S. -W.; Barth, M. C.; Trainer, M.
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D10
  • DOI: 10.1029/2011JD017099

Evaluation of Parametric Assumptions for Shallow Cumulus Convection
journal, March 1995


Eddy Diffusivity/Mass Flux and Shallow Cumulus Boundary Layer: An Updraft PDF Multiple Mass Flux Scheme
journal, May 2012

  • Sušelj, Kay; Teixeira, João; Matheou, Georgios
  • Journal of the Atmospheric Sciences, Vol. 69, Issue 5
  • DOI: 10.1175/JAS-D-11-090.1

Global modeling of aerosol dynamics: Model description, evaluation, and interactions between sulfate and nonsulfate aerosols
journal, January 2005


Transport and chemical transformations influenced by shallow cumulus over land
journal, January 2005

  • Vilà-Guerau de Arellano, J.; Kim, S. -W.; Barth, M. C.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 12
  • DOI: 10.5194/acp-5-3219-2005

Observations of the first aerosol indirect effect in shallow cumuli: FIRST AEROSOL INDIRECT EFFECT IN CUMULI
journal, February 2011

  • Berg, Larry K.; Berkowitz, Carl M.; Barnard, James C.
  • Geophysical Research Letters, Vol. 38, Issue 3
  • DOI: 10.1029/2010GL046047

Measurements of the Atmospheric Mass, Energy, and Momentum Budgets Over a 500-Kilometer Square of Tropical Ocean
journal, January 1973


Large-eddy simulation of turbulent diffusion with chemical reactions in the convective boundary layer
journal, January 1989


Sulfur chemistry in the National Center for Atmospheric Research Community Climate Model: Description, evaluation, features, and sensitivity to aqueous chemistry
journal, January 2000

  • Barth, M. C.; Rasch, P. J.; Kiehl, J. T.
  • Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D1
  • DOI: 10.1029/1999JD900773

The atmospheric chemistry general circulation model ECHAM5/MESSy1: consistent simulation of ozone from the surface to the mesosphere
journal, January 2006

  • Jöckel, P.; Tost, H.; Pozzer, A.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 12
  • DOI: 10.5194/acp-6-5067-2006

A Large Eddy Simulation Intercomparison Study of Shallow Cumulus Convection
journal, May 2003


Modeling chemical and aerosol processes in the transition from closed to open cells during VOCALS-REx
journal, January 2011


A description of the global sulfur cycle and its controlling processes in the National Center for Atmospheric Research Community Climate Model, Version 3
journal, January 2000

  • Rasch, Philip J.; Barth, Mary C.; Kiehl, Jeffrey T.
  • Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D1
  • DOI: 10.1029/1999JD900777

Effects of entrainment and mixing on droplet size distributions in warm cumulus clouds
journal, April 2014

  • Tölle, Merja H.; Krueger, Steven K.
  • Journal of Advances in Modeling Earth Systems, Vol. 6, Issue 2
  • DOI: 10.1002/2012MS000209

MIRAGE: Model description and evaluation of aerosols and trace gases
journal, January 2004


A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli
journal, January 2015

  • Berg, L. K.; Shrivastava, M.; Easter, R. C.
  • Geoscientific Model Development, Vol. 8, Issue 2
  • DOI: 10.5194/gmd-8-409-2015

A Unified Model for Moist Convective Boundary Layers Based on a Stochastic Eddy-Diffusivity/Mass-Flux Parameterization
journal, July 2013

  • Sušelj, Kay; Teixeira, João; Chung, Daniel
  • Journal of the Atmospheric Sciences, Vol. 70, Issue 7
  • DOI: 10.1175/JAS-D-12-0106.1

Measurements of the chemical composition of stratiform clouds
journal, January 1984


A cloud resolving model as a cloud parameterization in the NCAR Community Climate System Model: Preliminary results
journal, September 2001

  • Khairoutdinov, Marat F.; Randall, David A.
  • Geophysical Research Letters, Vol. 28, Issue 18
  • DOI: 10.1029/2001GL013552

A Combined Eddy-Diffusivity Mass-Flux Approach for the Convective Boundary Layer
journal, April 2007

  • Siebesma, A. Pier; Soares, Pedro M. M.; Teixeira, João
  • Journal of the Atmospheric Sciences, Vol. 64, Issue 4
  • DOI: 10.1175/JAS3888.1

The Influence of the Cloud Shell on Tracer Budget Measurements of LES Cloud Entrainment
journal, December 2011

  • Dawe, Jordan T.; Austin, Philip H.
  • Journal of the Atmospheric Sciences, Vol. 68, Issue 12
  • DOI: 10.1175/2011JAS3658.1

Subsiding Shells around Shallow Cumulus Clouds
journal, March 2008

  • Heus, Thijs; Jonker, Harm J. J.
  • Journal of the Atmospheric Sciences, Vol. 65, Issue 3
  • DOI: 10.1175/2007JAS2322.1

Evaluation and intercomparison of global atmospheric transport models using 222 Rn and other short-lived tracers
journal, March 1997

  • Jacob, Daniel J.; Prather, Michael J.; Rasch, Philip J.
  • Journal of Geophysical Research: Atmospheres, Vol. 102, Issue D5
  • DOI: 10.1029/96JD02955

Control of Chemical Reactions by Convective Turbulence in the Boundary Layer
journal, February 1998


A Direct Measure of Entrainment
journal, June 2010


Marine boundary layer cloud regimes and POC formation in a CRM coupled to a bulk aerosol scheme
journal, January 2013

  • Berner, A. H.; Bretherton, C. S.; Wood, R.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 24
  • DOI: 10.5194/acp-13-12549-2013

A Simple Parameterization Coupling the Convective Daytime Boundary Layer and Fair-Weather Cumuli
journal, June 2005

  • Berg, Larry K.; Stull, Roland B.
  • Journal of the Atmospheric Sciences, Vol. 62, Issue 6
  • DOI: 10.1175/JAS3437.1

Modeling and analysis of aerosol processes in an interactive chemistry general circulation model
journal, January 2007

  • Verma, Sunita; Boucher, O.; Reddy, M. S.
  • Journal of Geophysical Research, Vol. 112, Issue D3
  • DOI: 10.1029/2005JD006077

Global and regional modeling of clouds and aerosols in the marine boundary layer during VOCALS: the VOCA intercomparison
journal, January 2015

  • Wyant, M. C.; Bretherton, C. S.; Wood, R.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 1
  • DOI: 10.5194/acp-15-153-2015

Effects of turbulence and heterogeneous emissions on photochemically active species in the convective boundary layer
journal, March 2000

  • Krol, Maarten C.; Molemaker, M. Jeroen; de Arellano, Jordi Vilà Guerau
  • Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D5
  • DOI: 10.1029/1999JD900958

Modeling Entrainment and Finescale Mixing in Cumulus Clouds
journal, December 1997


Atmospheric H2O2 field measurements in a tropical environment: Bahia, Brazil
journal, January 1990

  • Jacob, P.; Tavares, T. M.; Rocha, V. C.
  • Atmospheric Environment. Part A. General Topics, Vol. 24, Issue 2
  • DOI: 10.1016/0960-1686(90)90117-6

The Explicit-Cloud Parameterized-Pollutant hybrid approach for aerosol–cloud interactions in multiscale modeling framework models: tracer transport results
journal, April 2008

  • Gustafson Jr, William I.; Berg, Larry K.; Easter, Richard C.
  • Environmental Research Letters, Vol. 3, Issue 2
  • DOI: 10.1088/1748-9326/3/2/025005

Why are there large differences between models in global budgets of tropospheric ozone?
journal, January 2007

  • Wu, Shiliang; Mickley, Loretta J.; Jacob, Daniel J.
  • Journal of Geophysical Research, Vol. 112, Issue D5
  • DOI: 10.1029/2006JD007801