Interactions between tropospheric chemistry and aerosols in a unified general circulation model

[1] A unified tropospheric chemistry-aerosol model has been developed within the Goddard Institute for Space Studies general circulation model (GCM). The model includes a detailed simulation of tropospheric ozone-NOx-hydrocarbon chemistry as well as aerosols and aerosol precursors. Predicted aerosol species include sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon. The partitioning of ammonia and nitrate between gas and aerosol phases is determined by on-line thermodynamic equilibrium, and the formation of secondary organic aerosols is based on equilibrium partitioning and experimentally determined parameters. Two-way coupling between aerosols and chemistry provides consistent chemical fields for aerosol dynamics and aerosol mass for heterogeneous processes and calculations of gas-phase photolysis rates. Although the current version of the unified model does not include a prognostic treatment of mineral dust, we include its effects on photolysis and heterogeneous processes by using three-dimensional off-line fields. We also simulate sulfate and nitrate aerosols that are associated with mineral dust based on currently available chemical understanding. Considering both mineral dust uptake of HNO3 and wet scavenging of HNO3 on ice leads to closer agreement between predicted gas-phase HNO3 concentrations and measurements than in previous global chemical transport model simulations, especially in the middle to upper troposphere. As a result of the coupling between chemistry and aerosols, global burdens of both gas-phase and aerosol species are predicted to respond nonlinearly to changing emissions of NOx, NH3, and sulfur.

[1]  J. Seinfeld,et al.  Global distribution and climate forcing of carbonaceous aerosols , 2002 .

[2]  D. Jacob,et al.  Background ozone over the United States in summer: Origin, trend, and contribution to pollution episodes , 2002 .

[3]  D. Koch.  Transport and direct radiative forcing of carbonaceous and sulfate aerosols in the GISS GCM , 2001 .

[4]  G. Carmichael,et al.  A three‐dimensional modeling investigation of the evolution processes of dust and sea‐salt particles in east Asia , 2001 .

[5]  S. Woodward,et al.  Modeling the atmospheric life cycle and radiative impact of mineral dust in the Hadley Centre climate model , 2001 .

[6]  V. Grassian.  Heterogeneous uptake and reaction of nitrogen oxides and volatile organic compounds on the surface of atmospheric particles including oxides, carbonates, soot and mineral dust: Implications for the chemical balance of the troposphere , 2001 .

[7]  J. Lacaux,et al.  Heterogeneous processes involving nitrogenous compounds and saharan dust inferred from measurements and model calculations , 2001 .

[8]  V. Grassian,et al.  A Knudsen Cell Study of the Heterogeneous Reactivity of Nitric Acid on Oxide and Mineral Dust Particles , 2001 .

[9]  A. Goodman,et al.  Spectroscopic Study of Nitric Acid and Water Adsorption on Oxide Particles: Enhanced Nitric Acid Uptake Kinetics in the Presence of Adsorbed Water , 2001 .

[10]  D. Koch,et al.  Chemistry-climate interactions in the Goddard Institute for Space Studies general circulation model 2. New insights into modeling the preindustrial atmosphere , 2001 .

[11]  J. Crowley,et al.  Heterogeneous Reactivity of Gaseous Nitric Acid on Al2O3, CaCO3, and Atmospheric Dust Samples: A Knudsen Cell Study , 2001 .

[12]  J. Seinfeld,et al.  General circulation model assessment of direct radiative forcing by the sulfate-nitrate-ammonium-water inorganic aerosol system , 2001 .

[13]  A. Goodman,et al.  A laboratory study of the heterogeneous reaction of nitric acid on calcium carbonate particles , 2000 .

[14]  Jos Lelieveld,et al.  Tropospheric ozone simulation with a chemistry-general circulation model: Influence of higher hydrocarbon chemistry , 2000 .

[15]  A. Limbeck,et al.  Dependence of in-cloud scavenging of polar organic aerosol compounds on the water solubility , 2000 .

[16]  P. J. Rasch,et al.  Sulfur chemistry in the National Center for Atmospheric Research Community Climate Model: Description, evaluation, features, and sensitivity to aqueous chemistry , 2000 .

[17]  David Rind,et al.  Radiative forcing from tropospheric ozone calculated with a unified chemistry-climate model , 1999 .

[18]  U. Lohmann,et al.  Tropospheric sulfur cycle in the Canadian general circulation model , 1999 .

[19]  J. Seinfeld,et al.  Effects of aerosols on tropospheric photolysis rates in clear and cloudy atmospheres , 1999 .

[20]  M. Chin,et al.  Tropospheric sulfur simulation and sulfate direct radiative forcing in the Goddard Institute for Space Studies general circulation model , 1999 .

[21]  C. Liousse,et al.  Construction of a 1° × 1° fossil fuel emission data set for carbonaceous aerosol and implementation and radiative impact in the ECHAM4 model , 1999 .

[22]  Donald Dabdub,et al.  Estimate of global atmospheric organic aerosol from oxidation of biogenic hydrocarbons , 1999 .

[23]  D. Stevenson,et al.  Relative roles of climate and emissions changes on future tropospheric oxidant concentrations , 1999 .

[24]  John H. Seinfeld,et al.  Global concentrations of tropospheric sulfate, nitrate, and ammonium aerosol simulated in a general circulation model , 1999 .

[25]  J. Lerner,et al.  Use of On-Line Tracers as a Diagnostic Tool in General Circulation Model Development , 1999 .

[26]  G. Carmichael,et al.  The Role of Mineral Aerosol in Tropospheric Chemistry in East Asia—A Model Study , 1999 .

[27]  John H. Seinfeld,et al.  Organic aerosol formation from the oxidation of biogenic hydrocarbons , 1999 .

[28]  Philip J. Rasch,et al.  MOZART, a global chemical transport model for ozone and related chemical tracers: 1. Model description , 1998 .

[29]  P. Rasch,et al.  MOZART, a global chemical transport model for ozone , 1998 .

[30]  M. Jacobson,et al.  Nitric acid scavenging by mineral and biomass burning aerosols , 1998 .

[31]  I. Tegen,et al.  A general circulation model study on the interannual variability of soil dust aerosol , 1998 .

[32]  C. Galy‐Lacaux,et al.  Precipitation Chemistry in the Sahelian Savanna of Niger, Africa , 1998 .

[33]  Mark Lawrence,et al.  The impact of cloud particle gravitational settling on soluble trace gas distributions , 1998 .

[34]  J. Lelieveld,et al.  Simulation of global sulfate distribution and the influence on effective cloud drop radii with a coupled photochemistry sulfur cycle model , 1998 .

[35]  M. Jacobson.  Studying the effects of aerosols on vertical photolysis rate coefficient and temperature profiles over an urban airshed , 1998 .

[36]  D. Jacob,et al.  Global simulation of tropospheric O3-NOx-hydrocarbon chemistry , 1998 .

[37]  V. Ramaswamy,et al.  Global sensitivity studies of the direct radiative forcing due to anthropogenic sulfate and black carbon aerosols , 1998 .

[38]  A. Nenes,et al.  ISORROPIA: A New Thermodynamic Equilibrium Model for Multiphase Multicomponent Inorganic Aerosols , 1998 .

[39]  Paul J. Crutzen,et al.  An efficient method for online calculations of photolysis and heating rates , 1998 .

[40]  A. Bouwman,et al.  A global high‐resolution emission inventory for ammonia , 1997 .

[41]  G. Stenchikov,et al.  The impact of aerosols on solar ultraviolet radiation and photochemical smog. , 1997, Science.

[42]  Jos Lelieveld,et al.  A three-dimensional chemistry/general circulation model simulation of anthropogenically derived ozone in the troposphere and its radiative climate forcing , 1997 .

[43]  E. Kjellström.  A Three-Dimensional Global Model Study of Carbonyl Sulfide in the Troposphere and the Lower Stratosphere , 1997 .

[44]  J. Abbatt.  Interaction of HNO3 with water‐ice surfaces at temperatures of the free troposphere , 1997 .

[45]  M. Zondlo,et al.  Uptake of HNO3 on ice under upper tropospheric conditions , 1997 .

[46]  A. Sinha,et al.  Tropospheric ozone, lightning, and climate change , 1997 .

[47]  P. Crutzen,et al.  Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry , 1997 .

[48]  J. Hansen,et al.  Radiative forcing and climate response , 1997 .

[49]  J. Lelieveld,et al.  Terrestrial sources and distribution of atmospheric sulphur , 1997 .

[50]  M. Molina,et al.  Sensitivity analysis of a UV radiation transfer model and experimental photolysis rates of NO2 in the atmosphere of Mexico City , 1997 .

[51]  Frank M. Bowman,et al.  Formation of Organic Aerosols from the Oxidation of Biogenic Hydrocarbons , 1997 .

[52]  I. Tang.  Thermodynamic and optical properties of mixed‐salt aerosols of atmospheric importance , 1997 .

[53]  Thomas E. Graedel,et al.  Global gridded inventories of anthropogenic emissions of sulfur and nitrogen , 1996 .

[54]  J. Lelieveld,et al.  Role of mineral aerosol as a reactive surface in the global troposphere , 1996 .

[55]  J. Penner,et al.  A global three‐dimensional model study of carbonaceous aerosols , 1996 .

[56]  Mian Chin,et al.  A global three‐dimensional model of tropospheric sulfate , 1996 .

[57]  Andrew A. Lacis,et al.  Sensitivity of cirrus cloud albedo, bidirectional reflectance and optical thickness retrieval accuracy to ice particle shape , 1996 .

[58]  S. Madronich,et al.  Theoretical, actinometric, and radiometric determinations of the photolysis rate coefficient of NO2 during the Mauna Loa Observatory Photochemistry Experiment 2 , 1996 .

[59]  J. Lerner,et al.  Use of on-line tracers as a diagnostic tool in general circulation model development 1. Horizontal and vertical transport in the troposphere , 1996 .

[60]  J. Haigh,et al.  A tropospheric ozone‐lightning climate feedback , 1996 .

[61]  Johann Feichter,et al.  Simulation of the tropospheric sulfur cycle in a global climate model , 1996 .

[62]  Anthony D. Del Genio,et al.  A Prognostic Cloud Water Parameterization for Global Climate Models , 1996 .

[63]  M. Rossi,et al.  EXPERIMENTAL EVIDENCE FOR THE EFFICIENT "DRY DEPOSITION" OF NITRIC ACID ON CALCITE , 1995 .

[64]  Jos Lelieveld,et al.  Distribution and budget of O3 in the troposphere calculated with a chemistry general circulation model. , 1995 .

[65]  Inez Y. Fung,et al.  Contribution to the atmospheric mineral aerosol load from land surface modification , 1995 .

[66]  H. Levy,et al.  Empirical model of global soil‐biogenic NOχ emissions , 1995 .

[67]  C. N. Hewitt,et al.  A global model of natural volatile organic compound emissions , 1995 .

[68]  I. Fung,et al.  Modeling of mineral dust in the atmosphere: Sources, transport, and optical thickness , 1994 .

[69]  Teruyuki Nakajima,et al.  Modelling radiation quantities and photolysis frequencies in the troposphere , 1994 .

[70]  P. Crutzen,et al.  Acetone in the atmosphere: Distribution, sources, and sinks , 1994 .

[71]  Joyce E. Penner,et al.  Towards the development of a global inventory for black carbon emissions , 1993 .

[72]  Paul J. Crutzen,et al.  Reaction of N2O5 on tropospheric aerosols: Impact on the global distributions of NO x , O3, and OH , 1993 .

[73]  E. Robinson,et al.  The Mauna Loa Observatory photochemistry experiment , 1992 .

[74]  R. A. Cox,et al.  Evaluated kinetic and photochemical data for atmospheric chemistry: Supplement II , 1992 .

[75]  Roger Atkinson,et al.  Evaluated kinetic and photochemical data for atmospheric chemistry: Volume III - gas phase reactions of inorganic halogens , 2006 .

[76]  D. Jacob.  Chemistry of OH in remote clouds and its role in the production of formic acid and peroxymonosulfate , 1986 .

[77]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[78]  Peter H. Stone,et al.  Efficient Three-Dimensional Global Models for Climate Studies: Models I and II , 1983 .

[79]  J. Hansen,et al.  Light scattering in planetary atmospheres , 1974 .

[80]  S. Solberg,et al.  Atmospheric Chemistry and Physics , 2002 .

[81]  D. Jacob.  Heterogeneous chemistry and tropospheric ozone , 2000 .

[82]  Oliver Wild,et al.  Fast-J: Accurate Simulation of In- and Below-Cloud Photolysis in Tropospheric Chemical Models , 2000 .

[83]  J. Pankow.  An absorption model of GAS/Particle partitioning of organic compounds in the atmosphere , 1994 .

[84]  R. Turco,et al.  SMVGEAR: A sparse-matrix, vectorized gear code for atmospheric models , 1994 .

[85]  James F. Pankow,et al.  An absorption model of the gas/aerosol partitioning involved in the formation of secondary organic aerosol , 1994 .

[86]  M. Yao,et al.  Efficient Cumulus Parameterization for Long-Term Climate Studies: The GISS Scheme , 1993 .

[87]  Eric P. Shettle,et al.  Atmospheric Aerosols: Global Climatology and Radiative Characteristics , 1991 .

[88]  M. Wesely.  Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models , 1989 .

[89]  Stephen E. Schwartz,et al.  Mass-Transport Considerations Pertinent to Aqueous Phase Reactions of Gases in Liquid-Water Clouds , 1986 .

[90]  D D Wagman,et al.  Selected values of chemical thermodynamic properties , 1952 .