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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 × 105 model columns) versus the previous single‐node capability of GEOS‐Chem‐TOMAS (tens of cores, 200 km × 250 km, 1.3 × 104 model 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. Plain Language Summary: Small particles in the air have important effects on Earth's climate and air quality. Representing the number and size of these particles in global models is challenging because their processes are complex. This factor has often limited global‐model horizontal resolution because fine global resolution models (e.g., 25 km × 25 km or smaller) generally ran too slowly but would be useful for representing details missed at traditional coarse resolution (e.g., 200 km × 250 km). We start with a detailed particle scheme that previously only ran at coarse global resolution because fine resolution would take too long. We present the initial use of this scheme in an updated model version, with a structure allowing a fast‐running, high‐memory model with fine resolution, by using hundreds to thousands of computer cores. In the updated structure, model speed increases with the number of cores used. We find that the total number of particles in the model is more with fine compared to coarse model resolution. These increases are most in Earth's remote regions and for particles which come from gas. Using fine model resolution globally when representing particles could change our understanding of how they impact Earth's climate and air quality. Key Points: We couple aerosol microphysics with GEOS‐Chem's High‐Performance configuration for fine (25 km × 25 km) global‐resolution capabilityGlobal‐mean aerosol number increases with model resolution, dominated by particles smaller than 10 nm in the over‐ocean free troposphereToward finer horizontal resolution, enhanced particle precursor loading in the free troposphere promotes particle formation and growth [ABSTRACT FROM AUTHOR]

Many chemical transport models treat mineral dust as spherical. Solar backscatter retrievals of trace gases (e.g., OMI and TROPOMI) implicitly treat mineral dust as spherical. The impact of the morphology of mineral dust particles is studied to assess its implications for global chemical transport model (GEOS‐Chem) simulations and solar backscatter trace gas retrievals at ultraviolet and visible (UV‐Vis) wavelengths. We investigate how the morphology of mineral dust particles affects the simulated dust aerosol optical depth; surface area, reaction, and diffusion parameters for heterogeneous chemistry; phase function, and scattering weights for air mass factor (AMF) calculations used in solar backscatter retrievals. We use a mixture of various aspect ratios of spheroids to model the dust optical properties and a combination of shape and porosity to model the surface area, reaction, and diffusion parameters. We find that assuming spherical particles can introduce size‐dependent and wavelength‐dependent errors of up to 14% in simulated dust extinction efficiency with corresponding error in simulated dust optical depth typically within 5%. We find that use of spheroids rather than spheres increases forward scattered radiance and decreases backward scattering that in turn decrease the sensitivity of solar backscatter retrievals of NO2 to aerosols by factors of 2.0–2.5. We develop and apply a theoretical framework based on porosity and surface fractal dimension with corresponding increase in the reactive uptake coefficient driven by increased surface area and species reactivity. Differences are large enough to warrant consideration of dust non‐sphericity for chemical transport models and UV‐Vis trace gas retrievals. Plain Language Summary: Mineral dust is often treated as spherical in chemical transport and trace gas retrieval models. In this study, we investigate how dust shape affects gas‐particle and radiation‐particle interactions. We examine the impact of dust shape on optical properties and trace gas retrievals at ultraviolet and visible wavelengths. We find that treating dust as nonspherical in trace gas retrievals of nitrogen dioxide decreases the retrieval sensitivity to dust. We also examine the impact of dust shape on heterogeneous chemistry by developing and applying a theoretical model. We find that dust pores change particle surface area significantly and subsequently, reaction and diffusion parameters. Overall, this study signifies the importance of accounting for nonsphericity in chemical transport and trace gas retrieval models. Key Points: We implement a spheroidal model for dust shape along with the porosity to examine dust morphology effects in a chemical transport modelNonspherical dust particles with pores increase surface area available for reactive uptakeSpheroidal rather than spherical dust treatment reduces the effects of aerosols on UV‐Vis NO2 retrievals by factors of 2.0–2.5 [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for the modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, the use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate–nitrate–ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r=0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of the dry effective radius (Reff) for SNA and OM aerosol is designed to represent the airborne measurements (R2=0.74 ; slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2=0.72 ; slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73 and slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

The lifetime and concentration of nitrogen oxides (NO x) are susceptible to nonlinear production and loss and to the resolution of a chemical transport model (CTM). This is due to the strong spatial gradients of NO x and the dependence of its own chemical loss on such gradients. In this study, we use the GEOS-Chem CTM in its high-performance implementation (GCHP) to investigate NO x simulations over the eastern United States across a wide range of spatial model resolutions (six different horizontal grids from 13 to 181 km). Following increasing grid size, afternoon surface NO x mixing ratios over July 2015 generally decrease over the Great Lakes region (GL) and increase over the southern states of the US region (SS), yielding regional differences (181 km vs. 13 km) of -16 % (in the GL) to 7 % (in the SS); meanwhile, hydrogen oxide radicals (HO x) increase over both regions, consistent with their different chemical regimes (i.e., NO x -saturated in the GL and NO x -limited in the SS). Nighttime titration of ozone by surface nitric oxide (NO) was found to be more efficient at coarser resolutions, leading to longer NO x lifetimes and higher surface mixing ratios of nitrogen dioxide (NO 2) over the GL in January 2015. The tropospheric NO 2 column density at typical afternoon satellite overpass time has spatially more coherent negative biases (e.g., -8 % over the GL) at coarser resolutions in July, which reversed the positive biases of surface NO x over the SS. The reduced NO x aloft (>1 km altitude) at coarser resolutions was attributable to the enhanced HO x that intrudes into the upper troposphere. Application of coarse-resolution simulations for interpreting satellite NO 2 columns will generally underestimate surface NO 2 over the GL and overestimate surface NO 2 over the SS in summer, but it will uniformly overestimate NO x emissions over both regions. This study significantly broadens understanding of factors contributing to NO x resolution effects and the role of fine-resolution data in accurately simulating and interpreting NO x and its relevance to air quality. [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate-nitrate-ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r = 0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM, and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of dry effective radius (Reff) for SNA and OM aerosol is proposed, which well represents the airborne measurements (R² = 0.74, slope = 1.00) and the GEOS-Chem-TOMAS simulation (R² = 0.72, slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R² from 0.68 to 0.73, slope from 0.75 to 34 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate-nitrate-ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r = 0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM, and the ratio between the two components are the major indicators for SNA and OM dry aerosol size. A parameterization of dry effective radius (Reff) for SNA and OM aerosol is proposed, which well represents the airborne measurements (R2 = 0.74, slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2 = 0.72, slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73, slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

The lifetime and concentration of nitrogen oxides (NOx) are susceptible to non-linear production and loss, and con- sequently to the resolution of a chemical transport model (CTM). Here we use the GEOS-Chem CTM in its high performance implementation (GCHP) to investigate NOx simulations over the eastern United States across a wide range of resolutions (13–181 km). Following increasing grid size, daytime surface NOx concentrations over July 2015 generally decrease over the Great Lakes (GL) region and increase over the Southern States (SS), yielding regional biases (181 km vs. 13 km) of −18 % to 9 %; meanwhile hydrogen oxide radicals (HOx) increase over both regions, consistent with their different chemical regimes. Night- time titration of ozone by surface nitric oxide (NO) was found to be more efficient at coarser resolutions, leading to longer NOx lifetimes and higher surface concentrations of nitrogen dioxide (NO2) over the GL in January 2015. The tropospheric NO2 column density at typical afternoon satellite overpass time has spatially more coherent negative biases (e.g., −10 % over the GL) at coarser resolutions in July, which reversed the positive biases of surface NOx over the SS. The reduced NO2 aloft (> 1 km altitude) at coarser resolutions was attributable to the enhanced HOx that intrudes into the upper troposphere. Application of coarse resolution simulations for interpreting satellite NO2 columns will generally underestimate surface NO2 over the GL and overestimate surface NO2 over the SS in summer, while uniformly overestimating NOx emissions over both regions. This study significantly broadens understanding of factors contributing to NOx resolution effects, and the role of fine resolution to accurately simulate and interpret NOx and its relevance to air quality. [ABSTRACT FROM AUTHOR]

Modeling atmospheric chemistry at fine resolution globally is computationally expensive; the capability to focus on specific geographic regions using a multiscale grid is desirable. Here, we develop, validate, and demonstrate stretched-grids in the GEOS-Chem atmospheric chemistry model in its high performance implementation (GCHP). These multiscale grids are specified at runtime by four parameters that offer users nimble control of the region that is refined and the resolution of the refinement. We validate the stretched-grid simulation versus global cubed-sphere simulations. We demonstrate the operation and flexibility of stretched-grid simulations with two case studies that compare simulated tropospheric NO2 column densities from stretched-grid and cubed-sphere simulations to retrieved column densities from the TROPOspheric Monitoring Instrument (TROPOMI). The first case study uses a stretched-grid with a broad refinement covering the contiguous US to produce simulated columns that perform similarly to a C180 (~50 km) cubed-sphere simulation at less than one-ninth the computational expense. The second case study experiments with a large stretch-factor for a global stretched-grid simulation with a highly localized refinement with ~10 km resolution for California. We find that the refinement improves spatial agreement with TROPOMI columns compared to a C90 cubed-sphere simulation of comparable computational demands, despite conducting the simulation at a finer resolution than parent meteorological fields. Overall we find that stretched-grids in GEOS-Chem are a practical tool for fine resolution regional- or continental-scale simulations of atmospheric chemistry. Stretched-grids are available in GEOS-Chem version 13.0.0. [ABSTRACT FROM AUTHOR]