Idealized Particle-Resolved Large-Eddy Simulations to Evaluate the Impact of Emissions Spatial Heterogeneity on CCN Activity

Abstract. Aerosol-cloud interactions remain a large source of uncertainty in global climate models (GCMs) due to complex, nonlinear processes that alter aerosol properties and the inability to represent the full compositional complexity of aerosol populations within large-scale modeling frameworks. The spatial resolution of GCMs is often coarser than the scale of the spatially varying emissions in the modeled geographic region. This results in diffuse, uniform concentration fields of primary aerosol and gas-phase species instead of spatially heterogeneous concentrations. Aerosol processes such as gas-particle partitioning and coagulation are concentration-dependent in a non-linear manner, and thus the representation of spatially heterogeneous emissions impacts aerosol aging and properties. This includes climate-relevant quantities key to aerosol-cloud interactions including particle hygroscopicity and cloud condensation nuclei (CCN) activity. We investigate the impact of emissions spatial heterogeneity on aerosol properties including CCN activity via a series of first-of-a-kind particle-resolved large-eddy simulations with the modeling framework WRF-PartMC-MOSAIC-LES. CCN concentrations within the planetary boundary layer (PBL) are compared across numerous scenarios ranging in emissions spatial heterogeneity. CCN concentrations at low supersaturations (S_env = 0.1–0.3 %) increase in the upper PBL by up to 25 % for emissions scenarios with high spatial heterogeneity when compared to a uniform emissions base case. Process level analysis indicates that this increase is due to enhanced nitrate formation among scenarios with high emissions spatial heterogeneity.