Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 3 3 2003 10.5194/acpd-3-2879-2003 http://www.atmos-chem-phys-discuss.net/3/2879/2003/ http://www.atmos-chem-phys-discuss.net/3/2879/2003/acpd-3-2879-2003.html http://www.atmos-chem-phys-discuss.net/3/2879/2003/acpd-3-2879-2003.pdf 2879 2929 2003-06-02 Global modelling of secondary organic aerosol in the troposphere: A sensitivity analysis K. Tsigaridis M. Kanakidou Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, P.O. Box 1470, 71409 Heraklion, Crete, Greece A global 3-dimensional chemistry/transport model able to describe O₃, NO_x, Volatile Organic Compounds (VOC), sulphur and NH₃ chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA) formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. Uncertainties in the model calculations related to the enthalpy of vaporization, the solubility and the activity coefficient of the condensable species, the chemical fate of the first generation low volatility oxidation products, the ageing of particles with regard to their hydrophilic properties, the partitioning of SOA on various aerosol surfaces and the evaporation of semi-volatiles from aerosol surfaces have been evaluated. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. The large uncertainties associated with the emissions of VOC have not been investigated in this study. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the lower ones.