PNNL

Abstract

The radiative effects of black carbon depend critically on its atmospheric lifetime, which is controlled by the rate at which freshly emitted combustion particles become internally mixed with other aerosol components. Global aerosol models strive to represent this process, but the timescale for aerosol mixing is not easily constrained using measurements. In this study, a parameterization derived from particle-resolved simulations is used to quantify, in a global aerosol model, the timescale for internal mixing. We show that, while highly variable, the average timescale for internal mixing is approximately three hours, which is much shorter than the 24-hour aging timescale commonly applied in bulk aerosol models. We then use the mixing timescale to constrain the aging criterion in the Modal Aerosol Module. Our analysis reveals that, to best reflect timescales for internal mixing, modal models should assume that particles transition from the hydrophobic (fresh) to the hydrophilic (aged) class once they accumulate a coating thickness equal to four monolayers of sulfuric acid, as opposed to the model's current aging criterion of eight monolayers. We show that, in remote regions like the Arctic and Antarctic, predictions of black carbon loading and its seasonal variation are particularly sensitive to the model representation of aging. By constraining aging in global models to reflect mixing timescales simulated by the particle-resolved model, we eliminate one of the free parameters governing black carbon's long-range transport and spatiotemporal distribution.