A numerical global meteorological sulfur transport model and its application to Arctic air pollution

Abstract The paper describes the construction of a dynamic atmospheric sulfur transport model and addresses the issue of long-range atmospheric sulfur transport to the Arctic as an application of the model. The global model includes the dynamics of meteorologial and tracer fields, thermodynamics, cloud processes, turbulent boundary layer mixing, multiple three-dimensional anthropogenic sulfur emission sources, dry and aqueous-phase chemical processes for sulfur, dry deposition and the precipitation scavenging of sulfur. So far, the incomplete description of clouds and precipitation has been a major limitation to the modeling of wet chemical processes on the global scale. One of the main features of our study is an attempt to a realistic representation of the interaction between clouds and chemical reactions. The model includes a detailed sub-grid scale convective and stratiform condensation scheme which includes cloud liquid water content as a predictive variable. It is shown that the model is able to reproduce important dynamic and physical structures in the atmospheric circulation leading to a realistic simulation of the important aspects of the long-range transport of sulfur to the Arctic. Realistic simulation of seasonal variations in atmospheric flow and cloud related processes provides reliable estimates of the sulfur deposition fluxes and reproduces the characteristic annual cycle of sulfur concentrations over the Arctic. Zonally averaged fields for the source and Arctic regions reveal important differences in the long-range transport mechanisms in different seasons. The model represents a powerful tool for further examining the mechanisms of sulfur transport and its impact on the atmosphere.

[1]  L. Barrie,et al.  Chemical components of lower tropospheric aerosols in the high arctic: Six years of observations , 1990 .

[2]  J. Dignon.  Trace gas emission data bases for atmospheric chemistry studies , 1991 .

[3]  J. V. Iribarne,et al.  Models of cloud chemistry , 1989 .

[4]  P. Fraser,et al.  Atmospheric Trends in Methylchloroform and the Global Average for the Hydroxyl Radical , 1987, Science.

[5]  Harold Ritchie.  Application of the semi-Lagrangian method to a multilevel spectral primitive-equations model , 1991 .

[6]  A. Dastoor,et al.  On numerical simulation of the global distribution of sulfate aerosol produced by a large volcanic eruption , 1995 .

[7]  A. Dastoor,et al.  Cloudiness parameterization and verification in a large‐scale atmospheric model , 1994 .

[8]  J. Kristjánsson,et al.  Condensation and Cloud Parameterization Studies with a Mesoscale Numerical Weather Prediction Model , 1989 .

[9]  L. Barrie,et al.  Arctic air pollution: An overview of current knowledge , 1986 .

[10]  Qing Liu,et al.  On the definition and persistence of blocking , 1994 .

[11]  E. Joranger,et al.  Air pollution studies in the Norwegian Arctic , 1984 .

[12]  N. Busch,et al.  A Multi-Level Model of the Planetary Boundary Layer Suitable for Use with Mesoscale Dynamic Models , 1976 .

[13]  Henning Rodhe,et al.  A global three-dimensional model of the tropospheric sulfur cycle , 1991 .

[14]  H. Kuo.  Further Studies of the Parameterization of the Influence of Cumulus Convection on Large-Scale Flow , 1974 .

[15]  T. Iversen,et al.  Arctic air pollution and large scale atmospheric flows , 1985 .

[16]  Christian Seigneur,et al.  A study of atmospheric acid formation in different environments , 1984 .

[17]  N. N. Yanenko,et al.  The Method of Fractional Steps , 1971 .

[18]  J. Galloway,et al.  The transatlantic transport of sulfur , 1988 .

[19]  The flux of anthropogenic sulphur into the arctic from mid-latitudes in 1979/80 , 1989 .

[20]  L. Martin,et al.  Aqueous oxidation of sulfur dioxide by hydrogen peroxide at low pH , 1981 .

[21]  Erik Berge,et al.  Coupling of wet scavenging of sulphur to clouds in a numerical weather prediction model , 1993 .

[22]  Jørgen Saltbones,et al.  Modelling of long-range transport of sulphur over Europe: A two-year model run and some model experiments , 1983 .

[23]  W. Raatz.  Tropospheric circulation patterns during the Arctic Gas and Aerosol Sampling Program (AGASP), March/April 1983 , 1984 .

[24]  Rodolfo Bermejo,et al.  The Conversion of Semi-Lagrangian Advection Schemes to Quasi-Monotone Schemes , 1992 .

[25]  Daniel F. Rex,et al.  Blocking Action in the Middle Troposphere and its Effect upon Regional Climate II. The Climatology of Blocking Action , 1950 .

[26]  P. Crutzen,et al.  The changing photochemistry of the troposphere , 1991 .

[27]  Janusz A. Pudykiewicz,et al.  Preliminary results From a partial LRTAP model based on an existing meteorological forecast model , 1985 .

[28]  Paulette Middleton,et al.  A three‐dimensional Eulerian acid deposition model: Physical concepts and formulation , 1987 .

[29]  P. Smolarkiewicz,et al.  A class of semi-Lagrangian approximations for fluids. , 1992 .

[30]  Jean Côté,et al.  Inclusion of a TKE Boundary Layer Parameterization in the Canadian Regional Finite-Element Model , 1989 .

[31]  Brian E. Eaton,et al.  Global biogeochemical cycling estimates with CZCS satellite data and general circulation models , 1993 .

[32]  P. Crutzen,et al.  Sulfur dioxide in remote oceanic air: Cloud transport of reactive precursors , 1984 .

[33]  D. Möller.  Kinetic model of atmospheric SO2 oxidation based on published data , 1980 .

[34]  Raymond M. Hoff,et al.  Five years of air chemistry observations in the Canadian Arctic , 1985 .

[35]  S. Ghan,et al.  A global-scale Lagrangian trace species model of transport, transformation, and removal processes , 1988 .

[36]  R. Charlson,et al.  On the efficiency of nucleation scavenging , 1984 .

[37]  R. Schnell,et al.  Vertical and horizontal characteristics of Arctic haze during AGASP: Alaskan Arctic , 1984 .

[38]  S. Oltmans,et al.  Observations of Arctic haze during polar flights from Alaska to Norway , 1985 .

[39]  E. F. Bradley,et al.  Flux-Profile Relationships in the Atmospheric Surface Layer , 1971 .

[40]  J. Austin.  The blocking of middle latitude westerly winds by planetary waves , 1980 .

[41]  T. Iversen.  Some statistical properties of ground level air pollution at norwegian arctic stations and their relation to large scale atmospheric flow systems , 1989 .

[42]  E. Berge.  A regional numerical sulfur dispersion model using a meteorological model with explicit treatment of clouds , 1990 .

[43]  G. R. Carmichael,et al.  An Eulerian transport/transformation/removal model for SO2 and sulfate—I. Model development , 1984 .

[44]  T. Iversen.  Numerical modelling of the long range atmospheric transport of sulphur dioxide and particulate sulphate to the arctic , 1989 .