References

GMD

Geoscientific Model Development

GMD

Geosci. Model Dev.

1991-9603

Copernicus Publications

Göttingen, Germany

10.5194/gmd-6-1275-2013

A cloud chemistry module for the 3-D cloud-resolving mesoscale model Meso-NH with application to idealized cases

Leriche

¹ Pinty

J.-P.

¹ Mari

¹ Gazen

Laboratoire d'Aérologie, CNRS/INSU, UMR5560, Toulouse, France

22 08 2013

6 4 1275 1298

2013

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://gmd.copernicus.org/articles/6/1275/2013/gmd-6-1275-2013.html

The full text article is available as a PDF file from https://gmd.copernicus.org/articles/6/1275/2013/gmd-6-1275-2013.pdf

A complete chemical module has been developed for use in the Meso-NH three-dimensional cloud resolving mesoscale model. This module includes gaseous- and aqueous-phase chemical reactions that are analysed by a pre-processor generating the Fortran90 code automatically. The kinetic solver is based on a Rosenbrock algorithm, which is robust and accurate for integrating stiff systems and especially multiphase chemistry. The exchange of chemical species between the gas phase and cloud droplets and raindrops is computed kinetically by mass transfers considering non-equilibrium between the gas- and the condensed phases. Microphysical transfers of chemical species are considered for the various cloud microphysics schemes available, which are based on one-moment or two-moment schemes. The pH of the droplets and of the raindrops is diagnosed separately as the root of a high order polynomial equation. The chemical concentrations in the ice phase are modelled in a single phase encompassing the two categories of precipitating ice particles (snow and graupel) of the microphysical scheme. The only process transferring chemical species in ice is retention during freezing or riming of liquid hydrometeors. Three idealized simulations are reported, which highlight the sensitivity of scavenging efficiency to the choice of the microphysical scheme and the retention coefficient in the ice phase. A two-dimensional warm, shallow convection case is used to compare the impact of the microphysical schemes on the temporal evolution and rates of acid precipitation. Acid wet deposition rates are shown to be overestimated when a one-moment microphysics scheme is used compared to a two-moment scheme. The difference is induced by a better prediction of raindrop radius and raindrop number concentration in the latter scheme. A two-dimensional mixed-phase squall line and a three-dimensional mixed-phase supercell were simulated to test the sensitivity of cloud vertical transport to the retention efficiency of gases in the ice phase. The 2-D and 3-D simulations illustrate that the retention in ice of a moderately soluble gas such as formaldehyde substantially decreases its concentration in the upper troposphere. In these simulations, retention of highly soluble species in the ice phase significantly increased the wet deposition rates.

References 1

Adon, M., Galy-Lacaux, C., Yoboué, V., Delon, C., Lacaux, J. P., Castera, P., Gardrat, E., Pienaar, J., Al Ourabi, H., Laouali, D., Diop, B., Sigha-Nkamdjou, L., Akpo, A., Tathy, J. P., Lavenu, F., and Mougin, E.: Long term measurements of sulfur dioxide, nitrogen dioxide, ammonia, nitric acid and ozone in Africa using passive samplers, Atmos. Chem. Phys., 10, 7467–7487, <a href="http://dx.doi.org/10.5194/acp-10-7467-2010">https://doi.org/10.5194/acp-10-7467-2010</a>, 2010.

Amels, P., Elias, H., Götz, U., Steinges, U., and Wannowius, K. J.: Kinetic investigation of the stability of peroxonitric acid and of its reaction with sulfur(IV) in aqueous solution, in: Heterogeneous and Liquid Phase Processes, Transport and Chemical Transformation of Pollutants in the Troposphere, edited by: Warneck, P., Vol. 2, Springer, Berlin, 77–88, 1996.

Anastasio, C. and McGregor, K. G.: Chemistry of fog waters in California's Central Valley: 1. In situ photo-formation of hydroxyl radical and singlet molecular oxygen, Atmos. Environ., 35, 1079–1089, 2001.

Audiffren, N., Renard, M., Buisson, E., and Chaumerliac, N.: Deviations from the Henry's law equilibrium during cloud events: a numerical approach of the mass transfer between phases and specific numerical effects, Atmos. Res., 49, 139–161, 1998.

Barker, G. C., Fowles, P., and Stringer, B.: Pulse radiolytic induced transient electrical conductance in liquid solutions of NO3-, NO2-, and Fe(CN)63-, Trans. Faraday Soc., 66, 1509–1519, 1970.

Barth, M. C., Stuart, A. L., and Skamarock, W. C.: Numerical simulations of the July 10, 1996, Stratospheric-Tropospheric Experiment: Radiations, Aerosols, and Ozone (STERAO)-Deep Convection experiment storm: Redistribution of soluble tracers, J. Geophys. Res., 106, 12381–12400, 2001.

Barth, M. C., Kim, S.-W., Wang, C., Pickering, K. E., Ott, L. E., Stenchikov, G., Leriche, M., Cautenet, S., Pinty, J.-P., Barthe, Ch., Mari, C., Helsdon, J. H., Farley, R. D., Fridlind, A. M., Ackerman, A. S., Spiridonov, V., and Telenta, B.: Cloud-scale model intercomparison of chemical constituent transport in deep convection, Atmos. Chem. Phys., 7, 4709–4731, <a href="http://dx.doi.org/10.5194/acp-7-4709-2007">https://doi.org/10.5194/acp-7-4709-2007</a>, 2007a.

Barth, M. C., Kim, S.-W., Skamarock, W. C., Stuart, A. L., Pickering, K. E., and Ott, L. E.: 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, J. Geophys. Res., 112, D13310, <a href="http://dx.doi.org/10.1029/2006JD008046">https://doi.org/10.1029/2006JD008046</a>, 2007b.

Barthe, C., Chong, M., Pinty, J.-P., Bovalo, C., and Escobar, J.: CELLS v1.0: updated and parallelized version of an electrical scheme to simulate multiple electrified clouds and flashes over large domains, Geosci. Model Dev., 5, 167–184, <a href="http://dx.doi.org/10.5194/gmd-5-167-2012">https://doi.org/10.5194/gmd-5-167-2012</a>, 2012.

Bechtold, P., Bazile, E., Guichard, F., Mascart, P., and Richard, E.: A mass-flux convection scheme for regional and global models, Q. J. Roy. Meteor. Soc., 127, 869–886, 2001.

Becker, K. H., Klemmann, R., Kurtenbach, R., and Wiesen, P.: Solubility of nitrous acid (HONO) in sulfuric acid solutions, J. Phys. Chem., 100, 14984–14990, 1996.

Bell, R. P.: The reversible hydration of carbonyl compounds, Advanc. Phys. Orga. Chem., 4, 1–29, 1966.

Berthet, S., Leriche, M., Pinty, J. -P., Cuesta, J., and Pigeon, G.: Scavenging of aerosol particles by rain in a cloud resolving model, Atmos. Res., 96, 325-336, 2010.

Bielski B. H. J., Cabelli, D. E., Arudi, R. L., and Ross, A. B.: Reactivity of HO2/O2- in aqueous solution, J. Phys. Chem. Ref. Data, 14, 1041–1100, 1985.

Bongartz, A., Kames, J., Schurath, U., George, C., Mirabel, P., and Ponche, J. L.: Experimental determination of HONO mass accommodation coefficients using two different techniques, J. Atmos. Chem., 18, 149–170, 1994.

Borbon, A., Ruiz, M., Bechara, J., Aumont, B., Chong, M., Huntrieser, H., Mari, C., Reeves, C. E., Scialom, G., Hamburger, T., Stark, H., Afif, C., Jambert, C., Mills, G., Schlager, H., and Perros, P. E.: Transport and chemistry of formaldehyde by mesoscale convective systems in West Africa during AMMA 2006, J. Geophys. Res., 117, D12301, <a href="http://dx.doi.org/10.1029/2011JD017121">https://doi.org/10.1029/2011JD017121</a>, 2012.

Bousserez, N., Attie, J.-L., Peuch, V.-H, Michou, M., Pfister, G., Edwards, D., Emmons, L., Mari, C., Barret, B., Arnold, S. R., Heckel, A., Richter, A., Schlager, H., Lewis, A., Avery, M., Sachse, G., Browell, E. V., and Hair, J. W.: Evaluation of the MOCAGE chemistry transport model during the ICARTT/ITOP experiment, J. Geophys. Res., 112, D10S42, <a href="http://dx.doi.org/10.1029/2006JD007595">https://doi.org/10.1029/2006JD007595</a>, 2007.

Buxton, G. V., McGowan, S., Salmon, G. A., Williams, J. E., and Wood, N. D.: A study of the spectra and reactivity of oxysulphur radical anions involved in the chain oxidation of S(IV): a pulse and γ-radiolysis study, Atmos. Environ., 30, 2483–2493, 1996.

Caniaux, G., Redelsperger, J.-L., and Lafore, J.-P.: A numerical study of the stratiform region of a fast-moving squall line, Part I: General description and water and heat budgets, J. Atmos. Sci., 51, 2046–2074, 1994.

Chang, J. S., Brost, R. A., Isaksen, I. S. A., Madronich, S., Middleton, P., Stockwell, W. R., and Walcek, C. J.: A three-dimensional Eulerian acid deposition model: Physical concepts and formulation, J. Geophys. Res., 92, 14681–14700, 1987.

Chen, J., Griffin, R. J., Grini, A., and Tulet, P.: Modeling secondary organic aerosol formation through cloud processing of organic compounds, Atmos. Chem. Phys., 7, 5343–5355, <a href="http://dx.doi.org/10.5194/acp-7-5343-2007">https://doi.org/10.5194/acp-7-5343-2007</a>, 2007.

Chin, M. and Wine, P. H.: A temperature-dependent competitive kinetics study of the aqueous-phase reactions of OH radicals with formate, formic acid, acetate, acetic acid, and hydrated formaldehyde, in: Aquatic and Surface Photochemistry, edited by: Helz, G. R., Zepp, R. G., and Crosby, D. G., CRC Press, Boca Raton, 85–98, 1994.

Christensen, H. and Sehested, K.: HO2 and O2- radicals at elevated temperatures, J. Phys. Chem., 92, 3007–3011, 1988.

Cohan, D. S., Schultz, M. G., Jacob, D. J., Heikes, B. G., and Blake, D. R.: Convective injection and photochemical decay of peroxides in the tropical upper troposphere: Methyl iodide as a tracer of marine convection, J. Geophys. Res., 104, 5717–5724, <a href="http://dx.doi.org/10.1029/98JD01963">https://doi.org/10.1029/98JD01963</a>, 1999.

Cohard, J.-M. and Pinty, J. -P.: A comprehensive two-moment warm microphysical bulk scheme. Part I: Description and selective tests, Q. J. R. Meteorol. Soc., 126, 1815–1842, 2000a.

Cohard, J.-M. and Pinty, J.-P.: A comprehensive two-moment warm microphysical bulk scheme, Part II: 2-D experiments with a non-hydrostatic model, Q. J. R. Meteorol. Soc., 126, 1843–1859, 2000b.

Cohard, J.-M., Pinty, J. -P., and Bedos, C.: Extending Twomey's analytical estimate of nucleated cloud droplet concentrations from CCN spectra, J. Atmos. Sci., 55, 3348–3357, 1998.

Crassier, V., Suhre, K., Tulet, P., and Rosset, R.: Development of a reduced chemical scheme for use in mesoscale meteorological models, Atmos. Environ., 34, 2633–2644, 2000.

Cuxart, J., Bougeault, P., and Redelsperger, J.-L.: A turbulence scheme allowing for mesoscale and large-eddy simulations, Q. J. Roy. Meteorol. Soc., 126, 1–30, 2000.

Damian, V., Sandu, A., Damian, M., Potra, F., and Carmichael, G. R.: The kinetic preprocessor KPP – a software environment for solving chemical kinetics, Comput. Chem. Eng., 26, 1567–1579, 2002.

Das, T. N.: Reactivity and role of SO5.- radical in aqueous medium chain oxidation of sulfite to sulfate and atmospheric sulfuric acid generation, J. Phys. Chem. A, 105, 9142–9155, 2001.

Davidovits, M., Hu, J. H., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Entry of gas molecules into liquids, Faraday Discus., 100, 65–82, 1995.

Dickerson, R. R., Huffman, G. J., Luke, W. T., Nunnermacker, L. J., Pickering, K. E., Leslie, A. C. D., Lindsey, C. G., Slinn, W. G. N., Kelly, T. J., Daum, P. H., Delany, A. C., Greenberg, J. P., Zimmerman, P. R., Boatman, J. F., Ray, J. D., and Stedman, D. H.: Thunderstorms: An important mechanism in the transport of pollutants, Science, 237, 460–465, 1987.

Dye, J. E., Ridley, B. A., Baumann, K., Skamarock, W. C., Barth, M. C., Venticinque, M., Defer, E., Blanchet, P., Thery, C., Laroche, P., Hubler, G., Parrish, D. D., Ryerson, T., Trainer, M., Frost, G., Holloway, J. S., Fehsenfeld, F. C., Tuck, A., Matejka, T., Bartels, D., Rutledge, S. A., Lang, T., Stith, J., and Zerr, R.: An Overview of the STERAO-Deep Convection Experiment with Results for the 10 July Storm, J. Geophys. Res., 105, 10023–10045, 2000.

Elliot, A. J.: A pulse radiolysis study of the temperature dependence of the reactions involving H, OH and e^-aq in aqueous solutions, Radiat. Phys. Chem., 34-5, 753–758, 1989.

Elliot, A. J. and Buxton, G.: Temperature dependence of the reactions OH+O2- and OH+HO2 in water up to 200°C, J. Chem. Soc. Faraday Transac., 88, 2465–2470, 1992.

Ervens, B., George, C., Williams, J. E., Buxton, G. V., Salmon, G. A., Bydder, M., Wilkinson, F., Dentener, F., Mirabel, P., and Herrmann, H.: CAPRAM 2.4 (MODAC mechanism): An extended and condensed tropospheric aqueous phase mechanism and its application, J. Geophys. Res., 108, 4426, <a href="http://dx.doi.org/10.1029/2002JD002202">https://doi.org/10.1029/2002JD002202</a>, 2003.

Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, <a href="http://dx.doi.org/10.5194/acp-11-11069-2011">https://doi.org/10.5194/acp-11-11069-2011</a>, 2011.

Exner, M., Herrmann, H., and Zellner, R.: Laser-based studies of reactions of the nitrate radical in aqueous solution, Ber. Bunsenges. Phys. Chem., 96-3, 470–477, 1992.

Finlayson-Pitts, B. J. and Pitts, J. N.: Chemistry of the Upper and Lower Atmosphere: Theory, Experiments, and Applications, Academic Press, San Diego, USA, 969 pp., 2000.

Flossmann, A. I., and Wobrock, W.: Venting of gases by convective clouds, J. Geophys. Res., 101, 18639–18650, 1996.

Fried, A., Henry, B. E., Calvert, J. G., and Mozurkewich, M.: The reaction probability of N2O5 with sulfuric acid aerosols at stratospheric temperatures and composition, J. Geophys. Res., 99, 3517–3532, 1994.

Fried, A., Olson, J. R., Walega, J. G., Crawford, J. H., Chen, G., Weibring, P., Richter, D., Roller, C., Tittel, F., Porter, M., Fuelberg, H., Halland, J., Bertram, T. H., Cohen, R. C., Pickering, K., Heikes, B. G., Snow, J. A., Shen, H., O'Sullivan, D. W., Brune, W. H., Ren, X., Blake, D. R., Blake, N., Sachse, G., Diskin, G. S., Podolske, J., Vay, S. A., Shetter, R. E., Hall, S. R., Anderson, B. E., Thornhill, L., Clarke, A. D., McNaughton, C. S., Singh, H. B., Avery, M. A., Huey, G., Kim, S., and Millet, D. B.: Role of convection in redistributing formaldehyde to the upper troposphere over North America and the North Atlantic during the summer 2004 INTEX campaign, J. Geophys. Res., 113, D17306, <a href="http://dx.doi.org/10.1029/2007JD009760">https://doi.org/10.1029/2007JD009760</a>, 2008.

George, C., Ponche, J. L., Mirabel, P., Behnke, W., Scheer, V., and Zetzsch, C.: Study of uptake of N2O5 by water and NaCl solutions, J. Phys. Chem., 98, 8780–8784, 1994.

Goldstein, S. and Czapski, G.: Reactivity of peroxynitric acid (O2NOOH): A pulse radiolysis study, Inorg. Chem., 36, 4156–4162, 1997.

Goldstein, S., Czapski, G., Lind, J., and Merenyi, G.: Mechanism of decomposition of peroxynitric ion (O2NOO$^-)$: evidence for the formation of O2- and NO2 radicals, Inorg. Chem., 37, 3943–3947, 1998.

Graedel, T. E. and Weschler, C. J.: Chemistry within aqueous atmospheric aerosols and raindrops, Rev. Geophys. Space Phys., 19, 505–539, 1981.

Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, <a href="http://dx.doi.org/10.5194/acp-9-5155-2009">https://doi.org/10.5194/acp-9-5155-2009</a>, 2009.

Herrmann, H.: Kinetics of aqueous phase relevant for atmospheric chemistry, Chem. Rev., 103, 4691–4716, 2003.

Herrmann, H., Reese, A., Ervens, B., Wicktor, F., and Zellner, R.: Laboratory and modelling studies of tropospheric multiphase conversions involving some C1 and C2 peroxyl radicals, Phys. Chem. Earth, 24, 287–290, 1999.

Hindmarsh, A. C.: ODEPACK, a systematized collection of ODE solvers, in: Scientific Computing, edited by: Stepleman, R. S., North-Holland, Amsterdam, 55–64, 1983.

Iribarne, J. V. and Pyshnov, T.: The effect of freezing on the composition of the supercooled droplets, I: Retention of HCl, HNO3, NH3, and H2O2, Atmos. Environ., 24A, 383–387, 1990a.

Iribarne, J. V. and Pyshnov, T.: The effect of freezing on the composition of the supercooled droplets, II: Retention of S(IV), Atmos. Environ., 24A, 389–398, 1990b.

Jaeglé, L., Jacob, D. J., Wennberg, P. O., Spivakosky, C. M., Hanisco, T. F., Lanzendorf, E. J., Hintsa, E. J., Fahey, D. W., Keim, E. R., Proffitt, M. H., Atlas, E. L., Flocke, F. M., Schauffler, S. M., McElroy, C. T., Midwinter, C., Pfister, L., and Wilson, J. C.: Observed OH and HO2 in the upper troposphere suggest a major source from convective injection of peroxides, Geophys. Res. Lett., 24, 3181–3184, 1997.

Jaeglé, L., Jacob, D. J., Brune, W. H., Tan, D., Faloona, I. C., Weinheimer, A. J., and Sachse, G. W.: Sources of HOx and production of ozone in the upper troposphere over the United States, Geophys. Res. Lett., 25, 1709–1712, 1998.

Jaeglé, L., Jacob, D. J., Brune, W. H., and Wennberg, P. O.: Chemistry of HOx radicals in the upper troposphere, Atmos. Environ., 35, 469–489, 2001.

Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, <a href="http://dx.doi.org/10.5194/acp-5-1053-2005">https://doi.org/10.5194/acp-5-1053-2005</a>, 2005.

Kessler, E.: On the distribution and continuity of water substance in atmospheric circulations, Meteor. Monogr., No. 10, Amer. Meteor. Soc., Boston, 84 pp., 1969.

Khairoudinov, M. and Kogan, Y.: A new cloud physics parameterization in a large-eddy simulation model of marine stratocumulus, Mon. Weather Rev., 128, 229–243, 2000.

Lamb, D. and Blumenstein, R.: Measurements of the entrapment of sulphur dioxide by rime ice, Atmos. Environ., 21, 1765–1772, 1987.

Lafore, J. P., Stein, J., Asencio, N., Bougeault, P., Ducrocq, V., Duron, J., Fischer, C., Héreil, P., Mascart, P., Masson, V., Pinty, J. P., Redelsperger, J. L., Richard, E., and Vilà-Guerau de Arellano, J.: The Meso-NH Atmospheric Simulation System. Part I: adiabatic formulation and control simulations, Ann. Geophys., 16, 90–109, <a href="http://dx.doi.org/10.1007/s00585-997-0090-6">https://doi.org/10.1007/s00585-997-0090-6</a>, 1998.

Lawrence, M. G. and Crutzen, P. J.: The impact of cloud particle gravitational settling on soluble trace gas distributions, Tellus, 50B-3, 263–289, 1998.

Lelieveld, J. and Crutzen, P. J.: The role of clouds in tropospheric photochemistry, J. Atmos. Chem., 12, 229–267, 1991.

Leriche, M., Voisin, D., Chaumerliac, N., Monod, A., and Aumont, B.: A model for tropospheric multiphase chemistry: Application to one cloudy event during the CIME experiment, Atmos. Environ., 34, 5015–5036, 2000.

Leriche, M., Deguillaume, L., and Chaumerliac, N.: Modeling study of strong acids formation and partitioning in a polluted cloud during wintertime, J. Geophys. Res., 108, 4433, <a href="http://dx.doi.org/10.1029/2002JD002950">https://doi.org/10.1029/2002JD002950</a>, 2003.

Lim, Y. B., Tan, Y., Perri, M. J., Seitzinger, S. P., and Turpin, B. J.: Aqueous chemistry and its role in secondary organic aerosol (SOA) formation, Atmos. Chem. Phys., 10, 10521–10539, <a href="http://dx.doi.org/10.5194/acp-10-10521-2010">https://doi.org/10.5194/acp-10-10521-2010</a>, 2010.

Logager, T. and Sehested, K.: Formation and decay of peroxynitric acid: A pulse radiolysis study, J. Phys. Chem., 97, 10047–10052, 1993.

Logager, T., Sehested, K., and Holoman, J.: Rate constants of the equilibrium reactions SO4- + HNO3 $\leftrightarrow$ HSO4- + NO3 and SO4- + NO3- $\leftrightarrow$ SO42- + NO3, Radiat. Phys. Chem., 41, 539–543, 1993.

Long, Y., Chaumerliac, N., Deguillaume, L., Leriche, M., and Champeau, F.: Effect of mixed phase cloud on the chemical budget of trace gases: a modeling approach, Atmos. Res., 97, 540–554, 2010.

Maaß, F., Elias, H., and Wannowius, K. J.: Kinetics of oxidation of hydrogen sulfite by hydrogen peroxide in aqueous solution: ionic strength effects and temperature dependence, Atmos. Environ., 33, 4413–4419, 1999.

Madronich, S. and Flocke, S.: The role of solar radiation in atmospheric chemistry, in: Handbook of Environmental Chemistry, edited by: Boule, P., Springer-Verlag, Heidelberg, 1–26, 1999.

Mao, J., Fan, S., Jacob, D. J., and Travis, K. R.: Radical loss in the atmosphere from Cu-Fe redox coupling in aerosols, Atmos. Chem. Phys., 13, 509–519, <a href="http://dx.doi.org/10.5194/acp-13-509-2013">https://doi.org/10.5194/acp-13-509-2013</a>, 2013.

Marécal, V., Rivière, E. D., Held, G., Cautenet, S., and Freitas, S.: Modelling study of the impact of deep convection on the utls air composition – Part I: Analysis of ozone precursors, Atmos. Chem. Phys., 6, 1567–1584, <a href="http://dx.doi.org/10.5194/acp-6-1567-2006">https://doi.org/10.5194/acp-6-1567-2006</a>, 2006.

Mari, C., Suhre, K., Rosset, R., Bates, T. S., Huebert, B. J., Bandy, A. R., Thornton, D. C., and Businger, S.: One-dimensional modeling of sulfur species during the First Aerosol Characterization Experiment (ACE 1) Lagrangian B, J. Geophys. Res., 104, 21733–21749, 1999.

Mari, C., Jacob, D. J., and Bechtold, P.: Transport and scavenging of soluble gases in a deep convective cloud, J. Geophys. Res., 105, 22255–22267, 2000.

Mari, C., Saüt, C., Jacob, D. J., Staudt, A., Avery, M. A., Brune, W. H., Faloona, I., Heikes, B. G., Sachse, G. W., Sandholm, S. T., Singh, H. B., and Tan, D.: On the relative role of convection, chemistry, and transport over the South Pacific Convergence Zone during PEM-Tropics B: A case study, J. Geophys. Res., 108, 8232, <a href="http://dx.doi.org/10.1029/2001JD001466">https://doi.org/10.1029/2001JD001466</a>, 2003.

Masson, V.: A physically-based scheme for the urban energy budget in atmospheric models, Bound. Lay. Meteorol., 1994, 357–397, 2000.

Monod, A. and Carlier, P.: Impact of clouds on the tropospheric ozone budget: Direct effect of multiphase photochemistry of soluble organic compounds, Atmos. Environ., 33, 4431–4446, 1999.

Noilhan, J. and Mahfouf, J.: The ISBA land surface parameterization scheme, Glob. Planet. Change, 13, 145–159, 1996.

Olson, T. M. and Hoffmann, M. R.: Hydroxyalkylsulfonate formation: its role as a S(IV) reservoir in atmospheric water droplets, Atmos. Environ., 23, 985–997, 1989.

Park, J. Y. and Lee, Y.-N.: Solubility and decomposition kinetics of nitrous acid in aqueous solution, J. Phys. Chem., 92, 6294–6302, 1988.

Paulot, F., Wunch, D., Crounse, J. D., Toon, G. C., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., González Abad, G., Notholt, J., Warneke, T., Hannigan, J. W., Warneke, C., de Gouw, J. A., Dunlea, E. J., De Mazière, M., Griffith, D. W. T., Bernath, P., Jimenez, J. L., and Wennberg, P. O.: Importance of secondary sources in the atmospheric budgets of formic and acetic acids, Atmos. Chem. Phys., 11, 1989–2013, <a href="http://dx.doi.org/10.5194/acp-11-1989-2011">https://doi.org/10.5194/acp-11-1989-2011</a>, 2011.

Pergaud, J., Masson, V. Malardel, S., and Couvreux, F.: A parameterization of dry thermals and shallow cumuli for mesoscale numerical weather prediction, Bound.-Lay. Meteorol., 132, 83–106, 2009.

Perrin, D. D.: Ionization constants of inorganic acids and bases in aqueous solution, Second Edition, Pergamon, Oxford, 1982.

Pickering, K. E., Wang, Y., Tao, W. K, Price, C., and Müller, J. F.: Vertical distributions of lightning NOx for use in regional and global chemical transport models, J. Geophys. Res., 103, 31203–31212, 1998.

Pinty, J.-P. and Jabouille, P.: A mixed-phase cloud parameterization for use in mesoscale non-hydrostatic model: simulations of a squall line and of orographic precipitations, Proc. Conf. of Cloud Physics, Everett, WA, USA, Amer. Meteor. Soc., Aug. 1999, 217–220, 1998.

Prather, M. J. and Jacob, D. J.: A persistent imbalance in HOx and NOx photochemistry of the upper troposphere driven by deep tropical convection, Geophys. Res. Lett., 24, 3189–3192, 1997.

Press, W. H., Teukolsky, S. A., Vetterling, W. T., and Flannery, B. P.: Numerical Recipes 3rd Edn, The Art of Scientific Computing, Cambridge University Press, New York, USA, 1256 pp., 2007.

Pruppacher, H. R. and Klett, J. D.: Microphysics of clouds and precipitation, 2nd Edn., Kluwer Academic Publishers, Dordrecht, The Netherlands, 954 pp., 1997.

Régimbal, J.-M. and Mozurkewich, M.: Peroxynitric acid decay mechanisms and kinetics at low pH, J. Phys. Chem. A, 101, 8822–8829, 1997.

Sander, S. P., Finlayson-Pitts, B. J., Friedl, R. R., Golden, D. M., Huie, R. E., Keller-Rudek, H., Kolb, C. E., Kurylo, M. J., Molina, M. J., Moortgat, G. K., Orkin, V. L., Ravishankara, A. R., and Wine, P. H.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation Number 15, JPL Publication 06-2, Jet Propulsion Laboratory, Pasadena, 2006.

Sandu, A. and Sander, R.: Technical note: Simulating chemical systems in Fortran90 and Matlab with the Kinetic PreProcessor KPP-2.1, Atmos. Chem. Phys., 6, 187–195, <a href="http://dx.doi.org/10.5194/acp-6-187-2006">https://doi.org/10.5194/acp-6-187-2006</a>, 2006.

Sandu, A., Verwer, J. G., Van Loon, M., Carmichael, G. R., Potra, F. A., Dabdub, D., and Seinfeld, J. H.: Benchmarking stiff ode solvers for atmospheric chemistry problems II: Rosenbrock solvers, Atmos. Environ., 31, 3459–3472, 1997b.

Schwartz, S. E.: Mass-transport considerations pertinent to aqueous phase reactions of gases in liquid water clouds, in: Chemistry of Multiphase Atmospheric Systems, NATO ASI Series, G6, edited by: Jaeschke, W., Spinger-Verlag, The Netherlands, 415–471, 1986.

Schwartz, S. E. and White, W. H.: Solubility equilibria of the nitrogen oxides and oxiacids in dilute aqueous solution, Adv. Environ. Sci. Engin., 4, 1–45, 1981.

Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics – from air pollution to climate change, Wiley-Interscience, New York, 1998.

Serjeant, E. P. and Dempsey, B.: Ionization constants of organic acids in aqueous solution, Pergamon, Oxford, 1979.

Skamarock,W. C., Powers, J., Barth, M. C., Dye, J. E., Matejka, T., Bartels, D., Baumann, K., Stith, J., Parrish, D. D., and Hubler, G.: Numerical simulations of the 10 July STERAO/Deep Convection Experiment convective system: Kinematics and transport, J. Geophys. Res., 105, 19973–19990, 2000.

Snider, J. R. and Huang, J.: Factors influencing the retention of hydrogen peroxide and molecular oxygen in rime ice, J. Geophys. Res., 103, 1405–1415, 1998.

100

Snider, J. R., Montague, D. C., and Vali, G.: Hydrogen peroxide retention in rime ice, J. Geophys. Res., 97, 7569–7578, 1992.

101

Stickler, A., Fischer, H., Williams, J., de Reus, M., Sander, R., Lawrence, M. G., Crowley, J. N., and Lelieveld, J.; Influence of summertime deep convection on formaldehyde in the middle and upper troposphere over Europe, J. Geophys. Res., 111, D14308, <a href="http://dx.doi.org/10.1029/2005JD007001">https://doi.org/10.1029/2005JD007001</a>, 2006.

102

Stone, D., Evans, M. J., Commane, R., Ingham, T., Floquet, C. F. A., McQuaid, J. B., Brookes, D. M., Monks, P. S., Purvis, R., Hamilton, J. F., Hopkins, J., Lee, J., Lewis, A. C., Stewart, D., Murphy, J. G., Mills, G., Oram, D., Reeves, C. E., and Heard, D. E.: HOx observations over West Africa during AMMA: impact of isoprene and NOx, Atmos. Chem. Phys., 10, 9415–9429, <a href="http://dx.doi.org/10.5194/acp-10-9415-2010">https://doi.org/10.5194/acp-10-9415-2010</a>, 2010.

103

Stuart, A. L. and Jacobson, M. Z.: Chemical retention during dry growth riming, J. Geophys. Res., 109, D07305, <a href="http://dx.doi.org/10.1029/2003JD004197">https://doi.org/10.1029/2003JD004197</a>, 2004.

104

Suhre, K., Crassier, V., Mari, C., Rosset, R., Johnson, D. W., Osborne, S., Wood, R., Andreae, M. O., Bandy, B., Bates, T. S. Businger, S., Gerbig, C., Raes, F., and Rudolph, J.: Chemistry and aerosols in the marine boundary layer: 1-D modelling of the three ACE-2 Lagrangian experiments, Atmos. Environ., 34, 5079–5094, 2000.

105

Szumowski, M., Grabowki, W. W., and Ochs, H. T.: A simple two–dimensional kinematic framework designed to test warm rain microphysical models, Atmos. Res., 45, 299–326, 1998.

106

Teyssèdre, H., Michou, M., Clark, H. L., Josse, B., Karcher, F., Olivié, D., Peuch, V.-H., Saint-Martin, D., Cariolle, D., Attié, J.-L., Nédélec, P., Ricaud, P., Thouret, V., van der A, R. J., Volz-Thomas, A., and Chéroux, F.: A new tropospheric and stratospheric Chemistry and Transport Model MOCAGE-Climat for multi-year studies: evaluation of the present-day climatology and sensitivity to surface processes, Atmos. Chem. Phys., 7, 5815–5860, <a href="http://dx.doi.org/10.5194/acp-7-5815-2007">https://doi.org/10.5194/acp-7-5815-2007</a>, 2007.

107

Tost, H., Jöckel, P., Kerkweg, A., Pozzer, A., Sander, R., and Lelieveld, J.: Global cloud and precipitation chemistry and wet deposition: tropospheric model simulations with ECHAM5/MESSy1, Atmos. Chem. Phys., 7, 2733–2757, <a href="http://dx.doi.org/10.5194/acp-7-2733-2007">https://doi.org/10.5194/acp-7-2733-2007</a>, 2007.

108

Tost, H., Lawrence, M. G., Br\"ihl, C., Jöckel, P., The GABRIEL Team, and The SCOUT-O3-DARWIN/ACTIVE Team: Uncertainties in atmospheric chemistry modelling due to convection parameterisations and subsequent scavenging, Atmos. Chem. Phys., 10, 1931–1951, <a href="http://dx.doi.org/10.5194/acp-10-1931-2010">https://doi.org/10.5194/acp-10-1931-2010</a>, 2010.

109

Tulet, P., Crassier, V., Solmon, F., Guedalia, D., and Rosset, R.: Description of the mesoscale nonhydrostatic chemistry model and application to a transboundary pollution episode between northern France and southern England, J. Geophys. Res., 108, 4021, <a href="http://dx.doi.org/10.1029/2000JD000301">https://doi.org/10.1029/2000JD000301</a>, 2003.

110

Tulet, P., Crassier, V., Cousin, F., Shure, K., and Rosset, R.: ORILAM, a three moment lognormal aerosol scheme for mesoscale atmospheric model. On-line coupling into the MesoNH-C model and validation on the Escompte campaign, J. Geophys. Res., 110, D18201, <a href="http://dx.doi.org/10.1029/2004JD005716">https://doi.org/10.1029/2004JD005716</a>, 2005.

111

Tulet, P., Grini, A., Griffin, R., and Petitcol, S.: ORILAM-SOA: a computationally efficient model for predicting secondary organic aerosols in 3-D atmospheric models, J. Geophys. Res., 111, D23208, <a href="http://dx.doi.org/10.1029/2006JD007152">https://doi.org/10.1029/2006JD007152</a>, 2006.

112

Twomey, S.: The nuclei of natural cloud formation. Part II: The supersaturation in natural clouds and the variation of cloud droplet concentration, Geophys. Pure Appl., 43, 243–249, 1959.

113

Voisin, D., Legrand, M., and Chaumerliac, N.: Scavenging of acidic gases (HCOOH, CH3COOH, HNO3, HCl, and SO2) and ammonia in mixed liquid-solid water clouds at the Puy de Dôme mountain (France), J. Geophys. Res., 105, 6817–6835, 2000.

114

von Blohn, N., Diehl, K., Mitra, S. K., and Borrmann, S.: Wind tunnel experiments on the retention of trace gases during riming: nitric acid, hydrochloric acid, and hydrogen peroxide, Atmos. Chem. Phys., 11, 11569–11579, <a href="http://dx.doi.org/10.5194/acp-11-11569-2011">https://doi.org/10.5194/acp-11-11569-2011</a>, 2011.

115

Waddicor, D. A., Vaughan, G., Choularton, T. W., Bower, K. N., Coe, H., Gallagher, M., Williams, P. I., Flynn, M., Volz-Thomas, A., Pätz, H. -W., Isaac, P., Hacker, J., Arnold, F., Schlager, H., and Whiteway, J. A.: Aerosol observations and growth rates downwind of the anvil of a deep tropical thunderstorm, Atmos. Chem. Phys., 12, 6157–6172, <a href="http://dx.doi.org/10.5194/acp-12-6157-2012">https://doi.org/10.5194/acp-12-6157-2012</a>, 2012.

116

Wennberg, P. O., Hanisco, T. F., Jaeglé, L., Jacob, D. J., Hintsa, E. J., Lanzendorf, E. J., Anderson, J. G., Gao, R., Keim, E. R., Donnelly, S. G., Negro, L. A. D., Fahey, D. W., McKeen, S. A., Salawitch, R. J., Webster, C. R., May, R. D., Herman, R. L., Proffitt, M. H., Margitan, J. J., Atlas, E. L., Schauffler, S. M., Flocke, F., McElroy, C. T., and Bui, T. P.: Hydrogen radicals, nitrogen radicals, and the production of O3 in the upper troposphere, Science, 279, 49–53, 1998.

117

Yin, Y., Carslaw, K. S., and Parker, D. J.: Redistribution of trace gases by convective clouds – mixed-phase processes, Atmos. Chem. Phys., 2, 293–306, <a href="http://dx.doi.org/10.5194/acp-2-293-2002">https://doi.org/10.5194/acp-2-293-2002</a>, 2002.

118

Yu, X.-Y. and Barker, J. R.: Hydrogen peroxide photolysis in acidic solutions containing chloride ions, I. Chemical mechanism, J. Phys. Chem. A, 107, 1313–1324, 2003.

119

Yu, X.-Y., Bao, Z.-C., and Barker, J. R.: Free radical reactions involving Cl, Cl2-, and SO4- in the 248 nm photolysis of aqueous solutions containing S2O$_8^2-$ and Cl-, J. Phys. Chem. A, 108-2, 295–308, 2004.

120

Zellner, R., Exner, M., and Herrmann, H.: Absolute OH quantum yields in the laser photolysis of nitrate, nitrite and dissolved H2O2 at 308 and 351 nm in the temperature range 278–353K, J. Atmos. Chem., 10, 411–425, 1990.