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Abstract. We present a new 12 km nested resolution capability in the GEOS-Chem global model of atmospheric composition. This capability can be applied to simulations for any user-selected domain worldwide from March 2021 onward by accessing a new hourly cubed-sphere C720 (approximately 12 × 12 km2 resolution) global wind archive from the NASA GEOS-FP meteorological data assimilation system. We regridded the archive to support rectilinear GEOS-Chem Classic nested grid simulations worldwide at 0.125° × 0.15625° resolution and denote this as the 12 km GEOS-Chem capability. We evaluate this 12 km configuration of GEOS-Chem by comparison with the standard 25 km (0.25° × 0.3125° resolution) nested configuration in simulations of transport tracers, oxidant-aerosol chemistry, and inversions of satellite data using the Integrated Methane Inversion (IMI). The 12 km simulation features stronger vertical transport (up to 20 % lower surface 222Rn concentrations) because it better captures horizontal convergence both spatially and temporally. Aerosol lifetimes against deposition are shorter by a few percent. The 12 km oxidant-aerosol chemistry can better simulate urban observations of NO2, and shows stronger ozone urban titration together with slightly higher surface ozone background due to enhanced vertical transport. 12 km and 25 km inversions using the IMI show highly consistent results on the regional scale, but the 12 km inversion provides greater information and improved spatial detail to resolve emissions from different sectors. 

Abstract. Accurate representation of mineral dust remains a challenge for global air quality or climate models due to inadequate parametrization of the emission scheme, removal mechanisms, and size distribution. While various studies have constrained aspects of dust emission fluxes and/or dust optical depth, annual mean surface dust concentrations still vary by factors of 5–10 among models. In this study, we focus on improving the annual simulation of fine dust in the GEOS-Chem chemical transport model, leveraging recent mechanistic understanding of dust source and removal, and reconciling the size differences between models and ground-based measurements. Specifically, we conduct sensitivity simulations using GEOS-Chem in its high performance configuration (GCHP) version 14.4.1 to investigate the effects of mechanism or parameter updates on annual mean concentrations. The results are evaluated by comparisons versus Deep Blue satellite-based aerosol optical depth (AOD) and AErosol RObotic NETwork (AERONET) ground-based AOD for total column abundance, and versus the Surface Particulate Matter Network (SPARTAN) for novel measurements of surface PM2.5 dust concentrations. Reconciling modelled geometric diameter versus measured aerodynamic diameter is important for consistent comparison. The two-fold overestimation of surface fine dust in the standard model is alleviated by 39 % without degradation of total column abundance by implementing a new physics-based dust emission scheme with better spatial distribution. Further reduction by 20 % of the overestimation of surface PM2.5 dust is achieved through reducing the mass fraction of emitted fine dust based on the brittle fragmentation theory, and explicit tracking of three additional fine mineral dust size bins with updated parametrization for below-cloud scavenging. Overall, these developments reduce the normalized mean difference against surface fine dust measurements from SPARTAN from 94 % to 35 %, while retaining comparable skill of total column abundance against satellite and ground-based AOD. 

Abstract Global modeling of aerosol‐particle number and size is important for understanding aerosol effects on Earth's climate and air quality. Fine‐resolution global models are desirable for representing nonlinear aerosol‐microphysical processes, their nonlinear interactions with dynamics and chemistry, and spatial heterogeneity. However, aerosol‐microphysical simulations are computationally demanding, which can limit the achievable global horizontal resolution. Here, we present the first coupling of the TwO‐Moment Aerosol Sectional (TOMAS) microphysics scheme with the High‐Performance configuration of the GEOS‐Chem model of atmospheric composition (GCHP), a coupling termed GCHP‐TOMAS. GCHP's architecture allows massively parallel GCHP‐TOMAS simulations including on the cloud, using hundreds of computing cores, faster runtimes, more memory, and finer global horizontal resolution (e.g., 25 km × 25 km, 7.8 × 10⁵model columns) versus the previous single‐node capability of GEOS‐Chem‐TOMAS (tens of cores, 200 km × 250 km, 1.3 × 10⁴model columns). GCHP‐TOMAS runtimes have near‐ideal scalability with computing‐core number. Simulated global‐mean number concentrations increase (dominated by free‐tropospheric over‐ocean sub‐10‐nm‐diameter particles) toward finer GCHP‐TOMAS horizontal resolution. Increasing the horizontal resolution from 200 km × 200–50 km × 50 km increases the global monthly mean free‐tropospheric total particle number by 18.5%, and over‐ocean sub‐10‐nm‐diameter particles by 39.8% at 4‐km altitude. With a cascade of contributing factors, free‐tropospheric particle‐precursor concentrations increase (32.6% at 4‐km altitude) with resolution, promoting new‐particle formation and growth that outweigh coagulation changes. These nonlinear effects have the potential to revise current understanding of processes controlling global aerosol number and aerosol impacts on Earth's climate and air quality. 

Abstract. Accurate representation of the hourly variation in the NO2-column-to-surface relationship is essential for interpreting geostationary observations of NO2 columns. Previous research indicated inconsistencies in this hourly variation. This study employs the high-performance configuration of the GEOS-Chem model (GCHP) to analyze daytime hourly NO2 total columns and surface concentrations during summer. We use measurements from globally distributed Pandora sun photometers and aircraft observations over the United States. We correct Pandora total NO2 vertical columns for (1) hourly variations in effective temperature driven by vertically resolved contributions to the total column and (2) changes in local solar time along the Pandora line of sight. These corrections increase the total NO2 columns by 5–6 × 1014 molec. cm−2 at 09:00 and 18:00 across all sites. Fine-scale simulations from GHCP (∼12 km) reduce the normalized bias (NB) against Pandora total NO2 columns from 19 % to 10 % and against aircraft measurements from 25 % to 13 % in Maryland, Texas, and Colorado. Similar reductions are observed in NO2 columns over the eastern US (17 % to 9 %), the western US (22 % to 14 %), Europe (24 % to 15 %), and Asia (29 % to 21 %) when compared to 55 km simulations. Our analysis attributes the weaker hourly variability in the total NO2 column to (1) hourly variations in column effective temperature, (2) local solar time changes along the Pandora line of sight, and (3) differences in hourly NO2 variability from different atmospheric layers, with the lowest 500 m exhibiting greater variability, while the dominant residual column above 500 m exhibits weaker variability.