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Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by fourteen CMIP6 models, including organic carbon (OC, available in 14 models), black carbon (BC, 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (–1.5 %) and MPI-ESM-1-2-HAM (–1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available components output, underestimate the total PM2.5 concentrations, partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by –71.2 % to –37.8 % across the 14 models) and the smallest for BC (–47.9 % to –12.1 %). The multi-model mean (MMM) reproduces fairly well the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.75), yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a primary and inert pollutant often used as a traffic tracer. Even though its concentrations are generally low at regional scale, BC presents very high concentrations in streets (local scale), potentially causing important effects on human health and environment. modelling studies of BC concentrations usually underestimate BC concentrations, because of uncertainties in both emissions and modelling. Both exhaust and non-exhaust traffic emissions present uncertainties, but those on non-exhaust emissions, such as tyre, brake and road wear and particle resuspension, are particularly high. In terms of modelling, the street models do not always consider the two-way interactions between the local and regional scales, i.e. the influence of the high BC concentrations observed in streets on the urban background concentrations, which can enhance the BC concentrations in streets. This study uses the multi-scale Street-in-Grid model (SinG) to simulate BC concentrations in a Paris suburb street-network, taking into account the two-way coupling between local and regional scales. The BC concentrations in streets proved to have an important influence on urban background concentrations. The two-way dynamic coupling leads to an increase in BC concentrations in large streets with high traffic emissions (with a maximal increase of about 48 %), and a decrease in narrow streets with low traffic emissions and low BC concentrations (with a maximal decrease of about 50 %). A new approach to estimate particle resuspension in streets is implemented, strictly respecting the mass balance on the street surface. The resuspension rate is calculated from the available deposited mass on the street surface, which is estimated based on a particle deposition and wash-off parametrizations adapted to street-canyon geometries. The simulations show that particle resuspension presents a low contribution to black carbon concentrations, as the deposited mass is not significant enough to justify high resuspension rates. Non-exhaust emission, such as brake and tyre and road wear, largely contribute to BC emissions, with a contribution equivalent to exhaust emissions. Here, emission factors of tyre, brake and road wear are calculated based on the literature, and a sensitivity analysis of these emission factors on BC concentrations in streets is performed. The model to measurement comparison shows that tyre-emission factors usually used in Europe are probably under-estimated, and tyre-emission factors coherent with some studies of the literature and the comparison performed here are proposed. [ABSTRACT FROM AUTHOR]

In this work, we developed a numerical method to investigate the effects of black carbon morphology on the estimation of brown carbon (BrC) absorption using the Absorption Ã…ngström exponent (AAE) method. Pseudo measurements of the total absorption were generated based on several morphologically mixed black carbon (BC) models, then the BrC absorption was inferred based on different AAE methods. By comparing the estimated BrC absorption with "True" BrC absorption, we found that both AAE=1 and Mie AAE methods do not provide accurate estimation for the BrC absorption, and the estimated BrC absorption can deviate several times from "True" BrC absorption. The newly proposed Wavelength Dependent AAE (WDA) method does not necessarily improve the estimations, sometimes it may even provide worse estimations than the AAE=1 and Mie AAE methods. Fixing the fractal dimension to be 1.8, the deviation between the estimated BrC mass absorption cross-section (MAC) and "True" BrC MAC can reach approximately 9 m²/g, which is far more than brown carbon MAC itself. Therefore, the estimation of BrC absorption based on the AAE method should carefully consider the morphological effects of BC. Our findings highlight the BC morphological effects on the BrC absorption estimation. [ABSTRACT FROM AUTHOR]

In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol-climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the aerosol size and cloud droplet radii. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of small particles show a decrease, especially in the Arctic region. These results indicate that, compared to using fixed scavenging coefficients, nucleation scavenging is less efficient and impaction scavenging is increased in the scheme introduced here. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. The simulated vertical profiles of aerosol in these sensitivity studies were evaluated against aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with the new wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means. [ABSTRACT FROM AUTHOR]

Simple climate models (SCMs) are frequently used in research and decision-making communities because of their flexibility, tractability, and low computational cost. SCMs can be idealized, flexibly representing major climate dynamics as impulse response functions, or process-based, using explicit equations to model possibly nonlinear climate and earth system dynamics. Each of these approaches has strengths and limitations. Here we present and test a hybrid impulse response modeling framework (HIRM) that combines the strengths of process-based SCMs in an idealized impulse response model, with HIRM's input derived from the output of a process-based model. This structure allows it to capture the crucial nonlinear dynamics frequently encountered in going from greenhouse gas emissions to atmospheric concentration to radiative forcing to climate change. As a test, the HIRM framework was configured to emulate total temperature of the simple climate model Hector 2.0 under the four Representative Concentration Pathways and the temperature response of an abrupt four times CO2 concentration step. HIRM was able to reproduce near-term and long-term Hector global temperature with a high degree of fidelity. Additionally, we conducted two case studies to demonstrate potential applications for this hybrid model: examining the effect of aerosol forcing uncertainty on global temperature, and incorporating more process-based representations of black carbon into a SCM. The open-source HIRM framework has a range of applications including complex climate model emulation, uncertainty analyses of radiative forcing, attribution studies, and climate model development. [ABSTRACT FROM AUTHOR]

High-performance computing resources allow us to conduct numerical simulations with a horizontal grid spacing that is sufficiently high to resolve cloud systems on a global scale, and high-resolution models (HRMs) generally provide better simulation performances than low-resolution models (LRMs). In this study, we execute a next-generation model that is capable of simulating global aerosols on a nonhydrostatic icosahedral atmospheric model version 16 (NICAM.16). The simulated aerosol distributions are obtained for 3 years with a HRM in a global 14-km grid spacing, an unprecedentedly high horizontal resolution and long integration period. For comparison, a NICAM with a 56-km grid spacing is also run as an LRM, although this horizontal resolution is still high among current global climate models. The comparison elucidated that the differences in the various variables of meteorological fields, including the wind speed, precipitation, clouds, radiation fluxes and total aerosols, are generally within 10% of their annual averages, but most of the variables related to aerosols simulated by the HRM are slightly closer to the observations than are those simulated by the LRM. Upon investigating the aerosol components, the differences in the water-insoluble black carbon (WIBC) and sulfate concentrations between the HRM and LRM are large (up to 32%), even in the annual averages. This finding is attributed to the differences in the column burden of the aerosol wet deposition, which is determined by a conversion rate of precipitation to cloud and the difference between the HRM and LRM is approximately 20%. Additionally, the differences in the simulated aerosol concentrations at polluted sites during polluted months between the HRM and LRM are estimated with medians of -23% (-63% to -2.5%) for BC, -4% (-91% to +18%) for sulfate and -1% (-49% to +223%) for the aerosol optical thickness (AOT). These findings indicate that the differences in the secondary and tertiary products, such as the AOT, between the different horizontal grid spacings are not explained simply by the grid size. On a global scale, the subgrid variabilities in the simulated AOT and COT in the 1°×1° domain using 6-hourly data are estimated to be 28.5% and 80.0%, respectively, in the HRM, whereas the corresponding differences are 16.6% and 22.9% in the LRM. Over the Arctic, both the HRM and the LRM generally reproduce the observed aerosols, but the largest difference in the surface BC mass concentrations between the HRM and LRM reaches 30% in spring (the HRM-simulated results are closer to the observations). The vertical distributions of the HRM- and LRM-simulated aerosols are generally close to the measurements, but the differences between the HRM and LRM results are large above a height of approximately 3 km, mainly due to differences in the wet deposition of the aerosols. The global annual averages of the direct and indirect aerosol radiative forcings (ARFs) attributed to anthropogenic aerosols in the HRM are estimated to be -0.29Wm-2 and -0.93Wm-2, respectively, whereas those in the LRM are -0.24Wm-2 and -1.10Wm-2. The differences in the direct ARF between the HRM and LRM are primarily caused by those in the aerosol burden, whereas the differences in the indirect ARF are primarily caused by those in the cloud expression and performance, which are attributed to the grid spacing. Because one-tenth of the computer resources are required for the LRM (56-km grid) compared to the HRM (14-km grid), we recommend that the various tuning parameters associated with the aerosol distributions using the LRM can be applicable to those using the HRM under the limitation of the available computational resources or before the HRM integration. [ABSTRACT FROM AUTHOR]

Wet processes, including aqueous phase chemistry, wet scavenging, and wet surface uptakes during dry deposition, are important for global modeling of aerosol precursors and aerosols. In this study, we improved the treatments of these wet processes in the GEOS-Chem v12.6.0, including pH calculation for cloud, rain, and wet surface, fraction of cloud available for aqueous phase chemistry, rainout efficiencies for various types of cloud, empirical washout by rain and snow, and wet surface uptakes during dry deposition. We compared simulated surface mass concentrations of aerosol precursors and aerosols with surface monitoring networks over the United States, Europe, Asia, and Arctic regions, and showed that the model results with the updated wet processes agree better with measurements for most species. With the implementation of these updates, normalized mean biases (NMB) of surface nitric acid, nitrate, and ammonium are reduced from 78 %, 126 %, and 45 % to 13 %, 24 %, and 6.2 % over US sites, from 56 %, 105 %, and 91 % to -20 %, -5.1 %, and 22 % over Europe sites, and from 121 %, 269 %, and 167 % to -18 %, 40 %, and 86 % over Asia sites. Comparison with surface measured SO2, sulfate and black carbon at four Arctic sites indicated that these species simulated with the updated wet processes match well with observations except large underestimation of black carbon at one of the sites. Furthermore, we compared model simulation with aircraft measurement of nitric acid and aerosols during ATom-1 and ATom-2 periods and found seasonal variation and vertical profile of these species have been successfully improved by considering the updated wet processes. The investigation of impacts of updated wet process treatments on surface mass concentrations indicated that the updated wet processes have strong impacts on the global means of nitric acid, sulfate, nitrate, and ammonium and relative small impacts on the global means of sulfur dioxide, dust, sea salt, black carbon, and organic carbon. [ABSTRACT FROM AUTHOR]