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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. Tropospheric ozone is a major air pollutant and greenhouse gas. It is also the primary precursor of OH, the main tropospheric oxidant. Global atmospheric chemistry models show large differences in their simulations of tropospheric ozone budgets. Here we implement the widely used GEOS-Chem atmospheric chemistry module as an alternative to CAM-chem within the Community Earth System Model version 2 (CESM2). We compare the resulting GEOS-Chem and CAM-chem simulations of tropospheric ozone and related species within CESM2 to observations from ozonesondes, surface sites, the ATom-1 aircraft campaign over the Pacific and Atlantic, and the KORUS-AQ aircraft campaign over the Seoul Metropolitan Area. We find that GEOS-Chem and CAM-chem within CESM2 have similar tropospheric ozone budgets and concentrations usually within 5 ppb but important differences in the underlying processes including (1) photolysis scheme (no aerosol effects in CAM-chem), (2) aerosol nitrate photolysis, (3) N2O5 cloud uptake, (4) tropospheric halogen chemistry, and (5) ozone deposition to the oceans. Global tropospheric OH concentrations are the same in both models, but there are large regional differences reflecting the above processes. Carbon monoxide is lower in CAM-chem (and lower than observations), at least in part because of higher OH concentrations in the Northern Hemisphere and insufficient production from isoprene oxidation in the Southern Hemisphere. CESM2 does not scavenge water-soluble gases in convective updrafts, leading to some upper-tropospheric biases. Comparison to KORUS-AQ observations shows an overestimate of ozone above 4 km altitude in both models, which at least in GEOS-Chem is due to inadequate scavenging of particulate nitrate in convective updrafts in CESM2, leading to excessive NO production from nitrate photolysis. The KORUS-AQ comparison also suggests insufficient boundary layer mixing in CESM2. This implementation and evaluation of GEOS-Chem in CESM2 contribute to the MUSICA vision of modularizing tropospheric chemistry in Earth system models. 

Modern climate models were designed to simulate natural systems and changes mainly due to atmospheric carbon dioxide, rather than to predict effects of deliberate climate interventions. 

Abstract. We implement the GEOS-Chem chemistry module as a chemical mechanism in version 2 of the Community Earth System Model (CESM). Our implementation allowsthe state-of-the-science GEOS-Chem chemistry module to be used with identical emissions, meteorology, and climate feedbacks as the CAM-chemchemistry module within CESM. We use coupling interfaces to allow GEOS-Chem to operate almost unchanged within CESM. Aerosols are converted at eachtime step between the GEOS-Chem bulk representation and the size-resolved representation of CESM's Modal Aerosol Model (MAM4). Land-type informationneeded for dry-deposition calculations in GEOS-Chem is communicated through a coupler, allowing online land–atmosphere interactions. Wet scavengingin GEOS-Chem is replaced with the Neu and Prather scheme, and a common emissions approach is developed for both CAM-chem and GEOS-Chem in CESM. We compare how GEOS-Chem embedded in CESM (C-GC) compares to the existing CAM-chem chemistry option (C-CC) when used to simulate atmosphericchemistry in 2016, with identical meteorology and emissions. We compare the atmospheric composition and deposition tendencies between the twosimulations and evaluate the residual differences between C-GC and its use as a stand-alone chemistry transport model in the GEOS-Chem HighPerformance configuration (S-GC). We find that stratospheric ozone agrees well between the three models, with differences of less than 10 % inthe core of the ozone layer, but that ozone in the troposphere is generally lower in C-GC than in either C-CC or S-GC. This is likely due to greatertropospheric concentrations of bromine, although other factors such as water vapor may contribute to lesser or greater extents depending on theregion. This difference in tropospheric ozone is not uniform, with tropospheric ozone in C-GC being 30 % lower in the Southern Hemisphere whencompared with S-GC but within 10 % in the Northern Hemisphere. This suggests differences in the effects of anthropogenic emissions. Aerosolconcentrations in C-GC agree with those in S-GC at low altitudes in the tropics but are over 100 % greater in the upper troposphere due todifferences in the representation of convective scavenging. We also find that water vapor concentrations vary substantially between the stand-aloneand CESM-implemented version of GEOS-Chem, as the simulated hydrological cycle in CESM diverges from that represented in the source NASA Modern-Era Retrospective analysis for Research and Applications (Version 2; MERRA-2)reanalysis meteorology which is used directly in the GEOS-Chem chemistrytransport model (CTM). Our implementation of GEOS-Chem as a chemistry option in CESM (including full chemistry–climate feedback) is publicly available and is beingconsidered for inclusion in the CESM main code repository. This work is a significant step in the MUlti-Scale Infrastructure for Chemistry andAerosols (MUSICA) project, enabling two communities of atmospheric researchers (CESM and GEOS-Chem) to share expertise through a common modelingframework, thereby accelerating progress in atmospheric science. 

Abstract Sensitivity analysis with atmospheric chemical transport models may be used to quantify influences of specific emissions on pollutant concentrations. This information facilitates efficient environmental decision‐making regarding emissions control strategies for pollutants that affect human health and public welfare. The multicomplex step method (MCX) is a sensitivity analysis approach that enables calculation of first‐ and higher‐order sensitivities of a nonlinear algorithm with analytical accuracy. Compared to the well‐known finite difference method, the MCX method is also straight‐forward to compute yet does not suffer from precision errors due to subtracting numbers with common leading digits and eliminates the requirement of tuning the step size. The aerosol inorganic equilibrium thermodynamic model, ISORROPIA, which treats ammonium, chloride, nitrate, sodium, sulfate, calcium, potassium, and magnesium, was augmented to leverage the multicomplex step method (ISORROPIA‐MCX) to analyze the influence that the total amount of a pollutant has on concentrations partitioned into different phases. This enables simultaneous calculation of the first‐order, second‐order, and cross‐sensitivity terms in the Taylor Series expansion when evaluating the impact of changes in input parameters on an output variable, increasing the accuracy of the estimated effect when the functions are nonlinear. ISORROPIA encodes highly nonlinear processes which showcases the computational advantages of the multicomplex step method as well as the limitations of the approach for fractured solution surfaces. With ISORROPIA‐MCX, the influence of total concentrations of aerosol precursors on aerosol acidity are evaluated with cross‐sensitivity terms for the first time. 

Abstract. Emissions are a central component of atmosphericchemistry models. The Harmonized Emissions Component (HEMCO) is a softwarecomponent for computing emissions from a user-selected ensemble of emissioninventories and algorithms. It allows users to re-grid, combine, overwrite,subset, and scale emissions from different inventories through aconfiguration file and with no change to the model source code. Theconfiguration file also maps emissions to model species with appropriateunits. HEMCO can operate in offline stand-alone mode, but more importantlyit provides an online facility for models to compute emissions at runtime.HEMCO complies with the Earth System Modeling Framework (ESMF) forportability across models. We present a new version here, HEMCO 3.0, thatfeatures an improved three-layer architecture to facilitate implementationinto any atmospheric model and improved capability for calculatingemissions at any model resolution including multiscale and unstructuredgrids. The three-layer architecture of HEMCO 3.0 includes (1) the Data InputLayer that reads the configuration file and accesses the HEMCO library ofemission inventories and other environmental data, (2) the HEMCO Core thatcomputes emissions on the user-selected HEMCO grid, and (3) the ModelInterface Layer that re-grids (if needed) and serves the data to theatmospheric model and also serves model data to the HEMCO Core forcomputing emissions dependent on model state (such as from dust or vegetation). The HEMCO Core is common to the implementation in all models, whilethe Data Input Layer and the Model Interface Layer are adaptable to themodel environment. Default versions of the Data Input Layer and ModelInterface Layer enable straightforward implementation of HEMCO in any simplemodel architecture, and options are available to disable features such asre-gridding that may be done by independent couplers in more complexarchitectures. The HEMCO library of emission inventories and algorithms iscontinuously enriched through user contributions so that new inventoriescan be immediately shared across models. HEMCO can also serve as a generaldata broker for models to process input data not only for emissions but forany gridded environmental datasets. We describe existing implementations ofHEMCO 3.0 in (1) the GEOS-Chem “Classic” chemical transport model withshared-memory infrastructure, (2) the high-performance GEOS-Chem (GCHP)model with distributed-memory architecture, (3) the NASA GEOS Earth SystemModel (GEOS ESM), (4) the Weather Research and Forecasting model withGEOS-Chem (WRF-GC), (5) the Community Earth System Model Version 2 (CESM2),and (6) the NOAA Global Ensemble Forecast System – Aerosols(GEFS-Aerosols), as well as the planned implementation in the NOAA Unified ForecastSystem (UFS). Implementation of HEMCO in CESM2 contributes to theMulti-Scale Infrastructure for Chemistry and Aerosols (MUSICA) by providinga common emissions infrastructure to support different simulations ofatmospheric chemistry across scales. 

Abstract. We present an updated mechanism for tropospheric halogen (Cl + Br + I) chemistry in the GEOS-Chem global atmospheric chemical transportmodel and apply it to investigate halogen radical cycling and implications for tropospheric oxidants. Improved representation of HOBr heterogeneouschemistry and its pH dependence in our simulation leads to less efficient recycling and mobilization of bromine radicals and enables the model toinclude mechanistic sea salt aerosol debromination without generating excessive BrO. The resulting global mean tropospheric BrO mixingratio is 0.19 ppt (parts per trillion), lower than previous versions of GEOS-Chem. Model BrO shows variable consistency and biases in comparison tosurface and aircraft observations in marine air, which are often near or below the detection limit. The model underestimates the daytimemeasurements of Cl2 and BrCl from the ATom aircraft campaign over the Pacific and Atlantic, which if correct would imply a very largemissing primary source of chlorine radicals. Model IO is highest in the marine boundary layer and uniform in the free troposphere, with a globalmean tropospheric mixing ratio of 0.08 ppt, and shows consistency with surface and aircraft observations. The modeled global meantropospheric concentration of Cl atoms is 630 cm−3, contributing 0.8 % of the global oxidation of methane, 14 % of ethane,8 % of propane, and 7 % of higher alkanes. Halogen chemistry decreases the global tropospheric burden of ozone by 11 %,NOx by 6 %, and OH by 4 %. Most of the ozone decrease is driven by iodine-catalyzed loss. The resulting GEOS-Chem ozonesimulation is unbiased in the Southern Hemisphere but too low in the Northern Hemisphere. 

Abstract. Bromine radicals influence global tropospheric chemistryby depleting ozone and by oxidizing elemental mercury and reduced sulfurspecies. Observations typically indicate a 50 % depletion of sea saltaerosol (SSA) bromide relative to seawater composition, implying that SSAdebromination could be the dominant global source of tropospheric bromine.However, it has been difficult to reconcile this large source with therelatively low bromine monoxide (BrO) mixing ratios observed in the marineboundary layer (MBL). Here we present a new mechanistic description of SSAdebromination in the GEOS-Chem global atmospheric chemistry model with adetailed representation of halogen (Cl, Br, and I) chemistry. We show thatobserved levels of SSA debromination can be reproduced in a mannerconsistent with observed BrO mixing ratios. Bromine radical sinks from theHOBr + S(IV) heterogeneous reactions and from ocean emission ofacetaldehyde are critical in moderating tropospheric BrO levels. Theresulting HBr is rapidly taken up by SSA and also deposited. Observations of SSA debromination at southern midlatitudes in summer suggest that modeluptake of HBr by SSA may be too fast. The model provides a successfulsimulation of free-tropospheric BrO in the tropics and midlatitudes in summer,where the bromine radical sink from the HOBr + S(IV) reactions iscompensated for by more efficient HOBr-driven recycling in clouds compared toprevious GEOS-Chem versions. Simulated BrO in the MBL is generally muchhigher in winter than in summer due to a combination of greater SSA emissionand slower conversion of bromine radicals to HBr. An outstanding issue inthe model is the overestimate of free-tropospheric BrO in extratropicalwinter–spring, possibly reflecting an overestimate of the HOBr∕HBr ratiounder these conditions where the dominant HOBr source is hydrolysis ofBrNO₃. 

Abstract. We present a comprehensive simulation of tropospheric chlorinewithin the GEOS-Chem global 3-D model of oxidant–aerosol–halogen atmosphericchemistry. The simulation includes explicit accounting of chloridemobilization from sea salt aerosol by acid displacement of HCl and by otherheterogeneous processes. Additional small sources of tropospheric chlorine(combustion, organochlorines, transport from stratosphere) are also included.Reactive gas-phase chlorine Cl*, including Cl, ClO, Cl2, BrCl, ICl,HOCl, ClNO3, ClNO2, and minor species, is produced by theHCl+OH reaction and by heterogeneous conversion of sea salt aerosolchloride to BrCl, ClNO2, Cl2, and ICl. The modelsuccessfully simulates the observed mixing ratios of HCl in marine air(highest at northern midlatitudes) and the associated HNO3decrease from acid displacement. It captures the high ClNO2 mixingratios observed in continental surface air at night and attributes thechlorine to HCl volatilized from sea salt aerosol and transported inlandfollowing uptake by fine aerosol. The model successfully simulates thevertical profiles of HCl measured from aircraft, where enhancements in thecontinental boundary layer can again be largely explained by transport inlandof the marine source. It does not reproduce the boundary layer Cl2mixing ratios measured in the WINTER aircraft campaign (1–5 ppt in thedaytime, low at night); the model is too high at night, which could be due touncertainty in the rate of the ClNO2+Cl- reaction, but we haveno explanation for the high observed Cl2 in daytime. The globalmean tropospheric concentration of Cl atoms in the model is 620 cm−3and contributes 1.0 % of the global oxidation of methane, 20 % ofethane, 14 % of propane, and 4 % of methanol. Chlorine chemistryincreases global mean tropospheric BrO by 85 %, mainly through theHOBr+Cl- reaction, and decreases global burdens of troposphericozone by 7 % and OH by 3 % through the associated bromine radicalchemistry. ClNO2 chemistry drives increases in ozone of up to8 ppb over polluted continents in winter.