Skip to main content
Log in

Reduction of Multiphase Atmospheric Chemistry

  • Published:
Journal of Atmospheric Chemistry Aims and scope Submit manuscript

Abstract

The aim of this article is to investigate the dynamical behaviour ofmultiphase atmospheric chemical mechanisms. Reducing procedures areapplied to a multiphase chemical box model including gas-phasereactions, aqueous-phase reactions and interfacial mass transfer. The lumping of species is computed in an automatic wayusing an efficient algorithm (apla). The computed lumped species arerelated to the fast behaviour of chemical and microphysical processessuch as Chapman cycle, ionic dissociations within the cloud drops andinterfacial Henry's equilibria. Depending on some parameters (liquidwater content, droplet radius) mixed lumped species (including both phases) may also becomputed. We show the existence of hierarchical reduced models due to the existence ofmultiple timescales. We use a special algorithm (dan2) in order tosolve the reduced models. Such models are accurate and the relative errorremains under the threshold of 1%. The speed-up is up to a factor 5comparedwith a fully implicit method (Gear) for the same accuracy. The key pointis that it provides a good qualitative understanding for the behaviourof the kinetic scheme.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Similar content being viewed by others

References

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

    Google Scholar 

  • Byrne, G. and Hindmarsh, A., 1987: Stiff ODE solvers: A review of current and coming attractions, J. Comp. Phys. 70, 1–62.

    Google Scholar 

  • Djouad, R. and Sportisse, B., 2002: Partitioning techniques for reduction in chemical kinetics. APLA: an Automatic Partitioning and Lumping Algorithm, Appl. Numeric. Math. 43(4), 383–398.

    Google Scholar 

  • Djouad, R. and Sportisse, B., 2003: Solving reduced models in Air Pollution Modelling, Appl. Numeric. Math. 44(1), 49–61.

    Google Scholar 

  • Djouad, R., Sportisse, B., and Audiffren, N., 2002a: Numerical simulation of aqueous-phase atmospheric models: Use of a non-autonomous Rosenbrock method, Atmos. Environ. 36, 873–879.

    Google Scholar 

  • Djouad, R., Sportisse, B., Audiffren, N., and Charpentier, I., 2002b: Modelling aqueous phase chemistry: Numerical integration and sensitivity analysis, in B. Sportisse (ed.), APMS 2001, pp. 444–457.

  • Fahey, K. and Pandis, S., 2001: The role of variable droplet size-resolution in aqueous phase atmospheric chemistry modeling, in B. Sportisse (ed.), Proceedings APMS 2001.

  • Gregoire, P. and Chaumerliac, N., 1994: Impact of cloud dynamics on tropospheric chemistry: Advances in modeling the interactions between microphysical and chemical processes, J. Atmos. Chem. 18, 247–266.

    Google Scholar 

  • Heard, A., Pilling, M., and Tomlin, A., 1998: Mechanism reduction techniques applied to tropospheric chemistry, Atmos. Environ. 32(6), 1059–1073.

    Google Scholar 

  • Herrmann, H., Ervens, B., Jacobi, H., Nowacki, P., Wolke, R., and Zellner, R., 2000: CAPRAM 2.3: A chemical aqueous phase radical mechanism for tropospheric chemistry, J. Atmos. Chem. 36, 231–284.

    Google Scholar 

  • Hindmarsh, A., 1983: Scientific Computing, Chapt. ODEPACK: A systematized collection of ODE solvers, New Holland, pp. 55–74.

  • Jacob, D., 1986: Chemistry of OH in remote clouds and its role in the production of formic acid and peroxymonosulfate, J. Geophys. Res. 91, 9807–9826.

    Google Scholar 

  • Jacobson, M. and Turco, R., 1994: SMVGEAR: A sparse-matrix, vectorized gear code for atmospheric models, Atmos. Environ. 28(2), 273–284.

    Google Scholar 

  • Kumar, S., 1989: The characteristic time to achieve interfacial phase equilibrium in cloud drops, Atmos. Environ. 23(10), 2299–2304.

    Google Scholar 

  • Lam, S. and Goussis, D., 1994: The CSP method for simplifying kinetics, Int. J. Chem. Kinet. 26, 462–484.

    Google Scholar 

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

    Google Scholar 

  • Lowe, R. and Tomlin, A., 2000: Low-dimensional manifolds and reduced chemical models for tropospheric chemistry simulations, Atmos. Environ. 34, 2425–2436.

    Google Scholar 

  • Maas, U. and Pope, S., 1992: Simplifying chemical kinetics: Intrinsic low-dimensional manifolds in composition space, Combustion Flame 88, 239–264.

    Google Scholar 

  • Madronich, S., 1987: Photodissocation in the atmosphere. 1. Actinic flux and the effects of ground reflections and clouds, J. Geophys. Res. 92, 9740–9752.

    Google Scholar 

  • McRae, G., Goodin, W., and Seinfeld, J., 1982: Numerical solution of the atmospheric diffusion equation for chemically reacting flows, J. Comp. Phys. 45, 1–42.

    Google Scholar 

  • PAM, 2003: PAM Project (Multiphase Air Pollution) supported by the French Research Program devoted to Air Quality (Primequal).

  • Poppe, D. et al., 2000: Scenarios for modelling of multi-phase tropospheric chemistry VERSION: 2, Technical report, The Multi-Phase Modelling (MPM) Group of the EUROTRAC2 subproject Chemical Mechanism Development (CMD).

  • Sartelet, K., Boutahar, J., Qulo, D., Coll, I., Plion, P., and Sportisse, B., 2002: Development and validation of a 3D chemistry-transport model, POLAIR3D, by comparison with data from ESQUIF campaign, in Proceedings of the 6th Gloream Workshop: Global and Regional Atmospheric Modelling, pp. 140–146.

  • Schwartz, S., 1986: Mass-transport considerations pertinent to aqueous phase reactions of gases in liquid-water clouds, NATO ASI Series, Vol. G6, Springer Verlag, Chemistry of multiphase atmospheric systems.

  • Seinfeld, J., 1985: Atmospheric Physics and Chemistry of Air Pollution, Wiley.

  • Shi, B. and Seinfeld, J., 1991: On mass transport limitation to the rate of reaction of gases in liquid droplets, Atmos. Environ. 25A(10), 2371–2383.

    Google Scholar 

  • Sportisse, B., 2000: An analysis of operator splitting techniques in the stiff case, J. Comp. Phys. 161, 140–168.

    Google Scholar 

  • Sportisse, B. and Djouad, R., 2000: Reduction of chemical kinetics in air pollution modelling, J. Comp. Phys. 164, 354–376.

    Google Scholar 

  • Sportisse, B. and Djouad, R., 2002: Mathematical investigation of mass transfer for atmospheric pollutants into a fixed droplet with aqueous chemistry, J. Geophys. Res., accepted for publication.

  • Stockwell, W., Middleton, P., Chang, J., and Tang, X., 1990: The second regional acid deposition model chemical mechanism for regional air quality modeling, J. Geophys. Res. 95(D10), 16343-16367.

    Google Scholar 

  • Verwer, J., Spee, E., Blom, J., and Hundsdorfer, W., 1999: A second order Rosenbrock method applied to photochemical dispersion problem, SIAM J. Sci. Comput. 20(4), 1456–1480.

    Google Scholar 

  • Wild, O., Zhu, X., and Prather, M., 2000: Fast-J: Accurate simulation of in and below cloud photolysis in tropospheric chemical models, J. Atmos. Chem. 37, 245–282.

    Google Scholar 

  • Wolke, R., Knoth, O., Ervens, B., and Herrmann, H., 2001: Numerical treatment of size resolved multiphase chemistry in atmospheric modeling, in B. Sportisse (ed.), Proceedings APMS 2001.

  • Wolke, R., Knoth, O., and H. H., 2000: Numerical treatment of aqueous phase chemistry in atmospheric chemistry-transport modeling, in Proceedings of EUROTRAC Conference.

Download references

Author information

Authors and Affiliations

Authors

Rights and permissions

Reprints and permissions

About this article

Cite this article

Djouad, R., Sportisse, B. & Audiffren, N. Reduction of Multiphase Atmospheric Chemistry. Journal of Atmospheric Chemistry 46, 131–157 (2003). https://doi.org/10.1023/A:1026067610565

Download citation

  • Issue Date:

  • DOI: https://doi.org/10.1023/A:1026067610565

Navigation