A framework for expanding aqueous chemistry in the Community Multiscale Air Quality (CMAQ) model version 5.1
-
Published:2017-04-13
Issue:4
Volume:10
Page:1587-1605
-
ISSN:1991-9603
-
Container-title:Geoscientific Model Development
-
language:en
-
Short-container-title:Geosci. Model Dev.
Author:
Fahey Kathleen M., Carlton Annmarie G.ORCID, Pye Havala O. T.ORCID, Baek Jaemeen, Hutzell William T., Stanier Charles O., Baker Kirk R., Appel K. Wyat, Jaoui Mohammed, Offenberg John H.ORCID
Abstract
Abstract. This paper describes the development and implementation of an extendable aqueous-phase chemistry option (AQCHEM − KMT(I)) for the Community Multiscale Air Quality (CMAQ) modeling system, version 5.1. Here, the Kinetic PreProcessor (KPP), version 2.2.3, is used to generate a Rosenbrock solver (Rodas3) to integrate the stiff system of ordinary differential equations (ODEs) that describe the mass transfer, chemical kinetics, and scavenging processes of CMAQ clouds. CMAQ's standard cloud chemistry module (AQCHEM) is structurally limited to the treatment of a simple chemical mechanism. This work advances our ability to test and implement more sophisticated aqueous chemical mechanisms in CMAQ and further investigate the impacts of microphysical parameters on cloud chemistry. Box model cloud chemistry simulations were performed to choose efficient solver and tolerance settings, evaluate the implementation of the KPP solver, and assess the direct impacts of alternative solver and kinetic mass transfer on predicted concentrations for a range of scenarios. Month-long CMAQ simulations for winter and summer periods over the US reveal the changes in model predictions due to these cloud module updates within the full chemical transport model. While monthly average CMAQ predictions are not drastically altered between AQCHEM and AQCHEM − KMT, hourly concentration differences can be significant. With added in-cloud secondary organic aerosol (SOA) formation from biogenic epoxides (AQCHEM − KMTI), normalized mean error and bias statistics are slightly improved for 2-methyltetrols and 2-methylglyceric acid at the Research Triangle Park measurement site in North Carolina during the Southern Oxidant and Aerosol Study (SOAS) period. The added in-cloud chemistry leads to a monthly average increase of 11–18 % in cloud SOA at the surface in the eastern United States for June 2013.
Publisher
Copernicus GmbH
Reference67 articles.
1. Appel, K. W., Napelenok, S. L., Foley, K. M., Pye, H. O. T., Hogrefe, C., Luecken, D. J., Bash, J. O., Roselle, S. J., Pleim, J. E., Foroutan, H., Hutzell, W. T., Pouliot, G. A., Sarwar, G., Fahey, K. M., Gantt, B., Gilliam, R. C., Kang, D., Mathur, R., Schwede, D. B., Spero, T. L., Wong, D. C., and Young, J. O.: Overview and evaluation of the Community Multiscale Air Quality (CMAQ) model version 5.1, Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2016-226, in review, 2016. 2. Audiffren, N., Chaumerliac, N., and Renard, M.: Effects of a polydisperse cloud on tropospheric chemistry, J. Geophys. Res., 101, 25949–25965, https://doi.org/10.1029/96JD01548, 1996. 3. Audiffren, N., Renard, M., Buisson, E., and Chaumerliac, N.: Deviations from the Henry's law equilibrium approach of the mass transfer between phases and its specific numerical effects, Atmos. Res., 49, 139–161, https://doi.org/10.1016/S0169-8095(98)00072-6, 1998. 4. Baek, J., Saide, P., Carmichael, G. R., Carlton, A. G., Carlson, J., and Stanier, C. O.: Developing Forward and Adjoint Aqueous Chemistry Module for CMAQ with Kinetic PreProcessor, 10th Annual CMAS Conference, Chapel Hill, NC, 24–26 October, 2011. 5. Barth, M. C., Stuart, A. L., and Skamarock, W. C.: Numerical simulations of the July 10, 1996, stratospheric-tropospheric experiment: radiation, aerosols, and ozone (STERAO)-deep convection experiment storm: redistribution of soluble tracers, J. Geophys. Res., 106, 12381–12400, https://doi.org/10.1029/2001JD900139, 2001.
Cited by
46 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|