Investigation of splitting gas and aqueous operators in atmospheric multiphase box models

Operator splitting techniques are widely used in atmospheric modeling in order to reduce the cost of time integration and allow more flexibility by treating each operator separately. However, this is not error free and the magnitude of the error depends on whether the splitted operators commute or not and the magnitude of the splitting time step. In multiphase models, the gas and the aqueous phase chemistries are related through the gas-droplet mass transfer processes. In the present paper, we show that splitting the gas chemistry operator from the aqueous chemistry and mass transfer operator is not appropriate and leads to errors beyond the tolerated thresholds. Analytical expressions for the splitting errors are derived and numerical experiments are conducted. The lamp chemical mechanism is employed. Time integration is performed with lsode.