Limitations of assuming internal mixing between different aerosol species: A case study with sulfate geoengineering simulations

Simulating the complex aerosol microphysical processes in a comprehensive Earth system model can be very computationally intensive; therefore many models utilize a modal approach, where aerosol size distributions are represented by observation-derived lognormal functions, and internal mixing between different aerosol species within an aerosol mode is often assumed. This approach has been shown to yield satisfactory results across a large array of applications, but there may be cases where the simplification in this approach may produce some shortcomings. In this work we show specific conditions under which the current approximations used in some modal approaches might yield incorrect answers. Using results from the Community Earth System Model v1 (CESM1) Geoengineering Large Ensemble (GLENS) project, we analyze the effects in the troposphere of a continuous increasing load of sulfate aerosols in the stratosphere, with the aim of counteracting the surface warming produced by non-mitigated increasing greenhouse gas (GHG) concentrations between 2020-2100. We show that the simulated results pertaining to the evolution of sea salt and dust aerosols in the upper troposphere are not realistic due to internal mixing assumptions in the modal aerosol treatment, which in this case reduces the size, and thus the settling velocities, of those particles and ultimately changes their mixing ratio below the tropopause. The unnatural increase of these aerosol species affects, in turn, the simulation of upper tropospheric ice formation, resulting in an increase in ice clouds that is not due to any meaningful physical mechanisms. While we show that this does not significantly affect the overall results of the simulations, we point to some areas where results should be interpreted with care in modeling simulations using similar approximations: in particular, in the evolution of upper tropospheric clouds when large amounts of sulfate are present in the stratosphere, as after a large explosive volcanic eruption or in similar stratospheric aerosol injection cases. Finally, we suggest that this can be avoided if sulfate aerosols in the coarse mode, the predominant species in these situations, are treated separately from other aerosol species in the model.