Implementation and evaluation of updated photolysis rates in the EMEP MSC-W chemistry-transport model using Cloud-J v7.3e
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Published:2023-12-21
Issue:24
Volume:16
Page:7433-7459
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ISSN:1991-9603
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Container-title:Geoscientific Model Development
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language:en
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Short-container-title:Geosci. Model Dev.
Author:
van Caspel Willem E., Simpson DavidORCID, Jonson Jan Eiof, Benedictow Anna M. K., Ge Yao, di Sarra Alcide, Pace GiandomenicoORCID, Vieno Massimo, Walker Hannah L., Heal Mathew R.ORCID
Abstract
Abstract. The present work describes the implementation of the state of the art Cloud-J v7.3 photolysis rate calculation code in the EMEP MSC-W chemistry-transport model. Cloud-J calculates photolysis rates and accounts for cloud and aerosol optical properties at model run time, replacing the old system based on tabulated values. The performance of Cloud-J is evaluated against aerial photolysis rate observations made over the Pacific Ocean and against surface observations from three measurement sites in Europe. Numerical experiments are performed to investigate the sensitivity of the calculated photolysis rates to the spatial and temporal model resolution, input meteorology model, simulated ozone column, and cloud effect parameterization. These experiments indicate that the calculated photolysis rates are most sensitive to the choice of input meteorology model and cloud effect parameterization while also showing that surface ozone photolysis rates can vary by up to 20 % due to daily variations in total ozone column. Further analysis investigates the impact of Cloud-J on the oxidizing capacity of the troposphere, aerosol–photolysis interactions, and surface air quality predictions. Results find that the annual mean mass-weighted tropospheric hydroxyl concentration is increased by 26 %, while the photolytic impact of aerosols is mostly limited to large tropical biomass-burning regions. Overall, Cloud-J represents a major improvement over the tabulated system, leading to improved model performance for predicting carbon monoxide and daily maximum ozone surface concentrations.
Funder
Natural Environment Research Council
Publisher
Copernicus GmbH
Reference107 articles.
1. Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume IV – gas phase reactions of organic halogen species, Atmos. Chem. Phys., 8, 4141–4496, https://doi.org/10.5194/acp-8-4141-2008, 2008. a, b 2. Barnard, J. C., Chapman, E. G., Fast, J. D., Schmelzer, J. R., Slusser, J. R., and Shetter, R. E.: An evaluation of the FAST-J photolysis algorithm for predicting nitrogen dioxide photolysis rates under clear and cloudy sky conditions, Atmos. Environ., 38, 3393–3403, https://doi.org/10.1016/j.atmosenv.2004.03.034, 2004. a 3. Becagli, S., Anello, F., Bommarito, C., Cassola, F., Calzolai, G., Di Iorio, T., di Sarra, A., Gómez-Amo, J.-L., Lucarelli, F., Marconi, M., Meloni, D., Monteleone, F., Nava, S., Pace, G., Severi, M., Sferlazzo, D. M., Traversi, R., and Udisti, R.: Constraining the ship contribution to the aerosol of the central Mediterranean, Atmos. Chem. Phys., 17, 2067–2084, https://doi.org/10.5194/acp-17-2067-2017, 2017. a 4. Bergström, R., Hayman, G. D., Jenkin, M. E., and Simpson, D.: Update and comparison of atmospheric chemistry mechanisms for the EMEP MSC-W model system, The Norwegian Meteorological Institute, Oslo, Norway, http://emep.int/publ/reports/2022/MSCW_technical_1_2022.pdf (last access: 19 December 2023), 2022. a, b, c 5. Bian, H., Prather, M. J., and Takemura, T.: Tropospheric aerosol impacts on trace gas budgets through photolysis, J. Geophys. Res.-Atmos., 108, D8, https://doi.org/10.1029/2002JD002743, 2003. a, b, c, d, e
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