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Abstract. Nitrate (NO3-) aerosol is projected to increase dramatically in the coming decades and may become the dominant inorganic particle species. This is due to the continued strong decrease in SO2 emissions, which is not accompanied by a corresponding decrease in NOx and especially NH3 emissions. Thus, the radiative effect (RE) of NO3- aerosol may become more important than that of SO42- aerosol in the future. The physicochemical interactions of mineral dust particles with gas and aerosol tracers play an important role in influencing the overall RE of dust and non-dust aerosols but can be a major source of uncertainty due to their lack of representation in many global climate models. Therefore, this study investigates how and to what extent dust affects the current global NO3- aerosol radiative effect through both radiation (REari) and cloud interactions (REaci) at the top of the atmosphere (TOA). For this purpose, multiyear simulations nudged towards the observed atmospheric circulation were performed with the global atmospheric chemistry and climate model EMAC, while the thermodynamics of the interactions between inorganic aerosols and mineral dust were simulated with the thermodynamic equilibrium model ISORROPIA-lite. The emission flux of the mineral cations Na+, Ca2+, K+, and Mg2+ is calculated as a fraction of the total aeolian dust emission based on the unique chemical composition of the major deserts worldwide. Our results reveal positive and negative shortwave and longwave radiative effects in different regions of the world via aerosol–radiation interactions and cloud adjustments. Overall, the NO3- aerosol direct effect contributes a global cooling of −0.11 W m−2, driven by fine-mode particle cooling at short wavelengths. Regarding the indirect effect, it is noteworthy that NO3- aerosol exerts a global mean warming of +0.17 W m−2. While the presence of NO3- aerosol enhances the ability of mineral dust particles to act as cloud condensation nuclei (CCN), it simultaneously inhibits the formation of cloud droplets from the smaller anthropogenic particles. This is due to the coagulation of fine anthropogenic CCN particles with the larger nitrate-coated mineral dust particles, which leads to a reduction in total aerosol number concentration. This mechanism results in an overall reduced cloud albedo effect and is thus attributed as warming. 

Abstract. Sedimentary records indicate that atmospheric dust has increased substantially since preindustrial times. However, state-of-the-art global Earth system models (ESMs) are unable to capture this historical increase, posing challenges in assessing the impacts of desert dust on Earth's climate. To address this issue, we construct a globally gridded dust emission dataset (DustCOMMv1) spanning 1841–2000. We do so by combining 19 sedimentary records of dust deposition with observational and modeling constraints on the modern-day dust cycle. The derived emission dataset contains interdecadal variability of dust emissions as forced by the deposition flux records, which increased by approximately 50 % from 1851–1870 to 1981–2000. We further provide future dust emission datasets for 2000–2100 by assuming three possible scenarios for how future dust emissions will evolve. We evaluate the historical dust emission dataset and illustrate its effectiveness in enforcing a historical dust increase in ESMs by conducting a long-term (1851–2000) dust cycle simulation with the Community Earth System Model (CESM2). The simulated dust depositions are in reasonable agreement with the long-term increase in most sedimentary dust deposition records and with measured long-term trends in dust concentration at sites in Miami and Barbados. This contrasts with the CESM2 simulations using a process-based dust emission scheme and with simulations from the Coupled Model Intercomparison Project (CMIP6), which show little to no secular trends in dust deposition, concentration, and optical depth. The DustCOMM emissions thus enable ESMs to account for the historical radiative forcings (RFs), including due to dust direct interactions with radiation (direct RF). Our CESM2 simulations estimate a 1981–2000 minus 1851–1870 direct RF of −0.10 W m−2 by dust aerosols up to 10 µm in diameter (PM10) at the top of atmosphere (TOA). This global dust emission dataset thus enables models to more accurately account for historical aerosol forcings, thereby improving climate change projections such as those in the Intergovernmental Panel on Climate Change (IPCC) assessment reports. 

Abstract The source of dust in the global atmosphere is an important factor to better understand the role of dust aerosols in the climate system. However, it is a difficult task to attribute the airborne dust over the remote land and ocean regions to their origins since dust from various sources are mixed during long‐range transport. Recently, a multi‐model experiment, namely the AeroCom‐III Dust Source Attribution (DUSA), has been conducted to estimate the relative contribution of dust in various locations from different sources with tagged simulations from seven participating global models. The BASE run and a series of runs with nine tagged regions were made to estimate the contribution of dust emitted in East‐ and West‐Africa, Middle East, Central‐ and East‐Asia, North America, the Southern Hemisphere, and the prominent dust hot spots of the Bodélé and Taklimakan Deserts. The models generally agree in large scale mean dust distributions, however models show large diversity in dust source attribution. The inter‐model differences are significant with the global model dust diversity in 30%–50%, but the differences in regional and seasonal scales are even larger. The multi‐model analysis estimates that North Africa contributes 60% of global atmospheric dust loading, followed by Middle East and Central Asia sources (24%). Southern hemispheric sources account for 10% of global dust loading, however it contributes more than 70% of dust over the Southern Hemisphere. The study provides quantitative estimates of the impact of dust emitted from different source regions on the globe and various receptor regions including remote land, ocean, and the polar regions synthesized from the seven models. 

Abstract. Estimating past aerosol radiative effects and their uncertainties is an important topic in climate science. Aerosol radiative effects propagate into large uncertainties in estimates of how present and future climate evolves with changing greenhouse gas emissions. A deeper understanding of how aerosols affected the atmospheric energy budget under past climates is hindered in part by a lack of relevant paleo-observations and in part because less attention has been paid to the problem. Because of the lack of information we do not seek here to determine the change in the radiative forcing due to aerosol changes but rather to estimate the uncertainties in those changes. Here we argue that current uncertainties from emission uncertainties (90 % confidence interval range spanning 2.8 W m−2) are just as large as model spread uncertainties (2.8 W m−2) in calculating preindustrial to present-day aerosol radiative effects. There are no estimates of radiative forcing for important aerosols such as wildfire and dust aerosols in most paleoclimate time periods. However, qualitative analysis of paleoclimate proxies suggests that changes in aerosols between different past climates are similar in magnitude to changes in aerosols between the preindustrial and present day; plus, there is the added uncertainty from the variability in aerosols and fires in the preindustrial. From the limited literature we crudely estimate a paleoclimate aerosol uncertainty for the Last Glacial Maximum relative to preindustrial of 4.8 W m−2, and we estimate the uncertainty in the aerosol feedback in the natural Earth system over the paleoclimate (Last Glacial Maximum to preindustrial) to be about 3.2 W m−2 K−1. In order to more accurately assess the uncertainty in historical aerosol radiative effects, we propose a new model intercomparison project, which would include multiple plausible emission scenarios tested across a range of state-of-the-art climate models over the historical period. These emission scenarios would then be compared to the available independent aerosol observations to constrain which are most probable. In addition, future efforts should work to characterize and constrain paleo-aerosol forcings and uncertainties. Careful propagation of aerosol uncertainties in the literature is required to ensure an accurate quantification of uncertainties in projections of future climate changes. 

Abstract Desert dust accounts for a large fraction of shortwave radiation absorbed by aerosols, which adds to the climate warming produced by greenhouse gases. However, it remains uncertain exactly how much shortwave radiation dust absorbs. Here, we leverage in-situ measurements of dust single-scattering albedo to constrain absorption at mid-visible wavelength by North African dust, which accounts for approximately half of the global dust. We find that climate and chemical transport models overestimate North African dust absorption aerosol optical depth (AAOD) by up to a factor of two. This occurs primarily because models overestimate the dust imaginary refractive index, the effect of which is partially masked by an underestimation of large dust particles. Similar factors might contribute to an overestimation of AAOD retrieved by the Aerosol Robotic Network, which is commonly used to evaluate climate and chemical transport models. The overestimation of dust absorption by models could lead to substantial biases in simulated dust impacts on the Earth system, including warm biases in dust radiative effects. 

Abstract. Desert dust is an important atmospheric aerosol that affects the Earth's climate, biogeochemistry, and air quality. However, current Earth system models (ESMs) struggle to accurately capture the impact of dust on the Earth's climate and ecosystems, in part because these models lack several essential aeolian processes that couple dust with climate and land surface processes. In this study, we address this issue by implementing several new parameterizations of aeolian processes detailed in our companion paper in the Community Earth System Model version 2 (CESM2). These processes include (1) incorporating a simplified soil particle size representation to calculate the dust emission threshold friction velocity, (2) accounting for the drag partition effect of rocks and vegetation in reducing wind stress on erodible soils, (3) accounting for the intermittency of dust emissions due to unresolved turbulent wind fluctuations, and (4) correcting the spatial variability of simulated dust emissions from native to higher spatial resolutions on spatiotemporal dust variability. Our results show that the modified dust emission scheme significantly reduces the model bias against observations compared with the default scheme and improves the correlation against observations of multiple key dust variables such as dust aerosol optical depth (DAOD), surface particulate matter (PM) concentration, and deposition flux. Our scheme's dust also correlates strongly with various meteorological and land surface variables, implying higher sensitivity of dust to future climate change than other schemes' dust. These findings highlight the importance of including additional aeolian processes for improving the performance of ESM aerosol simulations and potentially enhancing model assessments of how dust impacts climate and ecosystem changes. 

Abstract. Most global aerosol models approximate dust as sphericalparticles, whereas most remote sensing retrieval algorithms approximate dust as spheroidal particles with a shape distribution that conflicts withmeasurements. These inconsistent and inaccurate shape assumptions generatebiases in dust single-scattering properties. Here, we obtain dustsingle-scattering properties by approximating dust as triaxial ellipsoidalparticles with observationally constrained shape distributions. We findthat, relative to the ellipsoidal dust optics obtained here, the sphericaldust optics used in most aerosol models underestimate dust single-scattering albedo, mass extinction efficiency, and asymmetry parameter for almost all dust sizes in both the shortwave and longwave spectra. We further find that the ellipsoidal dust optics are in substantially better agreement with observations of the scattering matrix and linear depolarization ratio than the spheroidal dust optics used in most retrieval algorithms. However, relative to observations, the ellipsoidal dust optics overestimate the lidar ratio by underestimating the backscattering intensity by a factor of ∼2. This occurs largely because the computational method used to simulate ellipsoidal dust optics (i.e., the improved geometric optics method) underestimates the backscattering intensity by a factor of ∼2 relative to other computational methods (e.g., the physical geometric optics method). We conclude that the ellipsoidal dust optics with observationally constrained shape distributions can help improve global aerosol models and possibly remote sensing retrieval algorithms that do not use the backscattering signal. 

Abstract. In this study, we developed a novel algorithm based on the collocatedModerate Resolution Imaging Spectroradiometer (MODIS) thermal infrared (TIR)observations and dust vertical profiles from the Cloud–Aerosol Lidar withOrthogonal Polarization (CALIOP) to simultaneously retrieve dust aerosoloptical depth at 10 µm (DAOD10 µm) and the coarse-mode dusteffective diameter (Deff) over global oceans. The accuracy of theDeff retrieval is assessed by comparing the dust lognormal volumeparticle size distribution (PSD) corresponding to retrieved Deff withthe in situ-measured dust PSDs from the AERosol Properties – Dust(AER-D), Saharan Mineral Dust Experiment (SAMUM-2), and Saharan Aerosol Long-Range Transport and Aerosol–Cloud-InteractionExperiment (SALTRACE) fieldcampaigns through case studies. The new DAOD10 µm retrievals wereevaluated first through comparisons with the collocated DAOD10.6 µmretrieved from the combined Imaging Infrared Radiometer (IIR) and CALIOPobservations from our previous study (Zheng et al., 2022). The pixel-to-pixelcomparison of the two DAOD retrievals indicates a good agreement(R∼0.7) and a significant reduction in (∼50 %) retrieval uncertainties largely thanks to the better constraint ondust size. In a climatological comparison, the seasonal and regional(2∘×5∘) mean DAOD10 µm retrievals basedon our combined MODIS and CALIOP method are in good agreement with the twoindependent Infrared Atmospheric Sounding Interferometer (IASI) productsover three dust transport regions (i.e., North Atlantic (NA; R=0.9),Indian Ocean (IO; R=0.8) and North Pacific (NP; R=0.7)). Using the new retrievals from 2013 to 2017, we performed a climatologicalanalysis of coarse-mode dust Deff over global oceans. We found thatdust Deff over IO and NP is up to 20 % smaller than that over NA.Over NA in summer, we found a ∼50 % reduction in the numberof retrievals with Deff>5 µm from 15 to35∘ W and a stable trend of Deff average at 4.4 µm from35∘ W throughout the Caribbean Sea (90∘ W). Over NP inspring, only ∼5 % of retrieved pixels with Deff>5 µm are found from 150 to 180∘ E, whilethe mean Deff remains stable at 4.0 µm throughout eastern NP. To the best of our knowledge, this study is the first to retrieve both DAOD andcoarse-mode dust particle size over global oceans for multiple years. Thisretrieval dataset provides insightful information for evaluating dustlongwave radiative effects and coarse-mode dust particle size in models.