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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.