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Mian Chin

Publications and source records attributed to Mian Chin.

At least 19 records

Where Dust Comes from: Global Assessment of Dust Source Attributions with AeroCom Models

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.

Dust source attribution, Aerosol, Model↗

Abrupt Reduction in Shipping Emission as an Inadvertent Geoengineering Termination Shock Produces Substantial Radiative Warming

Human activities affect the Earth’s climate through modifying the composition of the atmosphere, which then creates radiative forcing that drives climate change. The warming effect of anthropogenic greenhouse gases has been partially balanced by the cooling effect of anthropogenic aerosols. In 2020, fuel regulations abruptly reduced the emission of sulfur dioxide from international shipping by about 80% and created an inadvertent geoengineering termination shock with global impact. Here we estimate the regulation leads to a radiative forcing of +0.2±0.11Wm-2 averaged over the global ocean.The amount of radiative forcing could lead to a doubling (or more) of the warming rate in the 2020s compared with the rate since 1980 with strong spatiotemporal heterogeneity.The warming effect is consistent with the recent observed strong warming in 2023 and expected to make the 2020s anomalously warm. The forcing represents 80% to the measured increase in planetary heat uptake since 2020. The radiative forcing also has strong hemispheric contrast, which has important implications for precipitation pattern changes. Our result suggests marine cloud brightening may be a viable geoengineering method in temporarily cooling the climate that has its unique challenges due to inherent spatiotemporal heterogeneity.

Tianle Yuan↗

Benchmarking GOCART-2G in the Goddard Earth Observing System (GEOS)

The Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which controls the sources sinks and chemistry within the Goddard Earth Observing System, recently underwent a major refactoring and update to the representation of physical processes. This paper serves to document code changes that were included in GOCART 2nd Generation (GOCART-2G) and establishes a benchmark simulation that is to be used for future development of the system. The code refactoring increases flexibility such multiple instances of an aerosol species can be run and interact with radiation and cloud microphysics, in addition to the output of multiple wavelength aerosol optical properties in support of data assimilation. From a science perspective, a new radiatively active tracer, brown carbon, was added to distinguish smoke from other sources of organic aerosol thereby improving optical properties entering the radiative calculations. A four-year benchmark simulation was evaluated using in situ and space borne measurements to develop a baseline and prioritize future development. A comparison of simulated aerosol optical depth between GOCART-2G and MODIS retrievals indicates the model captures the overall spatial pattern and seasonal cycle of aerosol optical depth but overestimates aerosol extinction over dusty regions and underestimates aerosol extinction over northern hemisphere boreal forests, requiring further tuning of emissions. This MODIS-based analysis is corroborated by comparisons to MISR and selected AERONET stations. Despite the underestimate of aerosol optical depth in biomass burning regions in GEOS, there is an overestimate in the surface mass of organic carbon in the United States, especially during the summer months.

Allison B Collow↗

Mineral Dust Optical Properties for Remote Sensing and Global Modeling: A Review

Dust plays a key role in many Earth system processes and is ubiquitous in the Martian atmosphere. Various intensive field campaigns, laboratory analyses, space-based remote sensing missions, and global modeling efforts aim to characterize dust optical properties. This is a bountiful time for dust scientists, and yet the interpretation of retrievals and comparison to models remains complicated by various conflicting assumptions that are part of each algorithm. For example, the conversion of satellite radiance measurements into products like aerosol optical depth for model evaluation depends upon aerosol properties like particle size and shape that are often prescribed and not part of the retrieval. Conversely, the model calculation of aerosol optical depth often uses different assumptions. The goal of this review is to first document algorithmic assumptions by various satellite retrieval products and models, and identify where there is consistency and where there are differences. In general, the differences documented in this paper reflect uncertainties resulting from incomplete observational characterization of dust aerosols and limitations in our understanding. Second, we note what observations might reduce uncertainties in our knowledge and bring greater consistency to retrievals and models, allowing for a more rigorous and harmonious comparison. The lack of comprehensive and realistic shape models for dust is an outstanding issue, such that closure between forward modeling from particle refractive index, shape, and size and observed optical properties cannot be achieved. Limitations in the computational methods that must be applied to model scattering from complex shapes also makes accurate optical modeling for dust challenging. Field observations indicate the persistence of coarse and giant dust particles at higher altitudes and farther downwind from their source than previously expected. Remote sensing retrieval algorithms based on observations at visible wavelengths have limited sensitivity to these particles and generally do not consider them, although a recent product based on longwave radiances is encouraging. Current measurements of the refractive index of bulk dust and fundamental dust minerology components such as hematite vary widely, inhibiting attempts to represent the variability in dust optical properties and forcing, as expected from different major dust source regions on Earth that have varying mineralogical composition. Some remote sensing retrieval algorithms allow for limited refractive index variability in their inversion solutions through mixing with other fine mode aerosol models, or optimizing the single scattering albedo, but Earth system models surveyed for this paper assume a globally uniform, size-invariant refractive index. Although no Martian dust samples have yet been returned to Earth, remote sensing observations indicate that Martian dust is globally homogenous in composition, and a single spectral refractive index assumption has been widely adopted to represent Martian dust. The lack of comprehensive, statistically representative measurements of dust particle microphysical properties (size distribution, morphology, complex index of refraction spectra, internal structure heterogeneity), and the resulting optical properties, limits our ability to verify the fidelity of these assumptions. A chain of measurements is needed, ranging from characterizing individual dust mineralogy components (e.g., pure hematite and goethite) to in situ sampling of complex atmospheric aerosol mixtures. Such results could be applied to both remote sensing retrievals that characterize the optical properties of the total aerosol burden in the atmosphere from total radiance measurements, and to global models that represent the total aerosol burden in the atmosphere by building it up from the balance of individual aerosol sources and sinks.

Aeolian dust↗

The Emissions Model Intercomparison Project (Emissions-MIP): Quantifying Model Sensitivity to Emission Characteristics

Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO 2 injection, seasonality of SO 2 and black carbon (BC) particulate emissions, and the assumed fraction of SO 2 emissions that is injected into the atmosphere as particulate phase sulfate (SO 4 ) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO 2 , SO 4 , and BC, with a particularly large relative variation for SO 2 , which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO 2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m −2 ), SO 2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO 2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO 2 at height consistently increased SO 2 and SO 4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO 4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO 4 emission fraction are accurately and consistently represented in global models.

Emissions Model Intercomparison Project↗

Reducing Aerosol Forcing Uncertainty by Combining Models With Satellite and Within-The-Atmosphere Observations: A Three-Way Street

Aerosol forcing uncertainty represents the largest climate forcing uncertainty overall. Its magnitude has remained virtually undiminished over the past 20 years despite considerable advances in understanding most of the key contributing elements. Recent work has produced modest increases only in the confidence of the uncertainty estimate itself. This review summarizes the contributions toward reducing the uncertainty in the aerosol forcing of climate made by satellite observations, measurements taken within the atmosphere, as well as modeling and data assimilation. We adopt a more measurement-oriented perspective than most reviews of the subject in assessing the strengths and limitations of each; gaps and possible ways to fill them are considered. Currently planned programs supporting advanced, global-scale satellite and surface-based aerosol, cloud, and precursor gas observations, climate modeling, and intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved, are all essential. But in addition, new efforts are needed: (a) to obtain systematic aircraft in situ measurements capturing the multi-variate probability distribution functions of particle optical, microphysical, and chemical properties (and associated uncertainty estimates), as well as co-variability with meteorology, for the major aerosol airmass types; (b) to conceive, develop, and implement a suborbital (aircraft plus surface-based) program aimed at systematically quantifying the cloud-scale microphysics, cloud optical properties, and cloud-related vertical velocities associated with aerosol-cloud interactions; and (c) to focus much more research on integrating the unique contributions of satellite observations, suborbital measurements, and modeling, to reduce the persistent uncertainty in aerosol climate forcing.

aerosol climate forcing↗

A Multimodel Investigation of Asian Summer Monsoon UTLS Transport Over the Western Pacific

The Asian summer monsoon (ASM) as a chemical transport system is investigated using a suite of models in preparation for an airborne field campaign over the Western Pacific. Results show that the dynamical process of anticyclone eddy shedding in the upper troposphere rapidly transports convectively uplifted Asian boundary layer air masses to the upper troposphere and lower stratosphere over the Western Pacific. The models show that the transported air masses contain significantly enhanced aerosol loading and a complex chemical mixture of trace gases that are relevant to ozone chemistry. The chemical forecast models consistently predict the occurrence of the shedding events, but the predicted concentrations of transported trace gases and aerosols often differ between models. The airborne measurements to be obtained in the field campaign are expected to help reduce the model uncertainties. Furthermore, the large-scale seasonal chemical structure of the monsoon system is obtained from modeled carbon monoxide, a tracer of the convective transport of pollutants, which provides a new perspective of the ASM circulation, complementing the dynamical characterization of the monsoon.

Laura L. Pan↗

Global Premature Mortality By Dust and Pollution PM 2.5 Estimated From Aerosol Reanalysis of the Modern-Era Retrospective Analysis for Research and Applications, Version 2

This study quantifies global premature deaths attributable to long-term exposure of ambient PM 2.5 , or PM 2.5 -attributable mortality, by dust and pollution sources. We used NASA’s Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) aerosol reanalysis product for PM 2.5 and the cause-specific relative risk (RR) from the integrated exposure-response (IER) model to estimate global PM2.5-attributable mortality for five causes of deaths, namely ischaemic heart disease (IHD), cerebrovascular disease (CEV) or stroke, lung cancer (LC), chronic obstructive pulmonary disease (COPD), and acute lower respiratory infection (ALRI). The estimated yearly global PM 2.5 -attributable mortality in 2019 amounts to 2.89 (1.38–4.48) millions, which is composed of 1.19 (0.73–1.84) million from IHD, 1.01 (0.35–1.55) million from CEV, 0.29 (0.11–0.48) million from COPD, 0.23 (0.14–0.33) million from ALRI, and 0.17 (0.04–0.28) million from LC (the numbers in parentheses represent the estimated mortality range due corresponding to RR spread at the 95% confidence interval). The mortality counts vary with geopolitical regions substantially, with the highest number of deaths occurring in Asia. China and India account for 40% and 23% of the global PM 2.5 -attributable deaths, respectively. In terms of sources of PM 2.5 , about 22% of the global all-cause PM 2.5 -attributable deaths are caused by desert dust. The largest dust attribution is 37% for ALRI. The relative contributions of dust and pollution sources vary with the causes of deaths and geographical regions. Enforcing air pollution regulations to transfer areas from PM 2.5 nonattainment to PM2.5 attainment can have great health benefits. Being attainable with the United States air quality standard (AQS) of 15 μg/m 3 globally would have avoided nearly 40% or 1.2 million premature deaths. The most recent update of PM 2.5 guideline from 10 to 5 μg/m 3 by the World Health Organization (WHO) would potentially save additional one million lives. Our study highlights the importance of distinguishing aerodynamic size from geometric size in accurately assessing the global health burden of PM 2.5 and particularly for dust. A use of geometric size in diagnosing dust PM 2.5 from the model simulation, a common approach in current health burden assessment, could overestimate the PM 2.5 level in the dust belt by 40–170%, leading to an overestimate of global all-cause mortality by 1 million or 32%.

PM2.5↗

Satellite-Based Evaluation of AeroCom Model Bias in Biomass Burning Regions

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

biomass burning aerosols↗

Inferring iron-oxide species content in atmospheric mineral dust from DSCOVR EPIC observations

The iron-oxide content of dust in the atmosphere and most notably its apportionment between hematite (α-Fe2O3) and goethite (α-FeOOH) are key determinants in quantifying dust’s light absorption, its top of atmosphere UV radiances used for dust monitoring, and ultimately shortwave dust direct radiative effects (DRE). Hematite and goethite column mass concentrations and iron-oxide mass fractions of total dust mass concentration were retrieved from the DeepSpace Climate Observatory (DSCOVR) Earth Polychromatic Imaging Camera (EPIC) measurements in the ultraviolet–visible (UV–Vis) channels. The retrievals were performed for dust-identified aerosol plumes over land using aerosol optical depth (AOD) and spectral imaginary refractive index provided by the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm over six continental regions (North America, North Africa, West Asia, Central Asia, EastAsia, and Australia). The dust particles are represented as an internal mixture of non-absorbing host and absorbing hematite and goethite. We use the Maxwell–Garnett effective medium approximation with carefully selected complex refractive indices of hematite and goethite that produce mass fractions of iron oxides species consistent with in situ values found in the literature to derive the hematite and goethite volumetric/mass concentrations from MAIAC EPIC products. We compared the retrieved hematite and goethite concentrations with in situ dust aerosol mineralogical content measurements, as well as with published data. Our data display variations within the published range of hematite, goethite, and iron-oxide mass fractions for pure mineral dust cases. A specific analysis is presented for 15 sites over the main dust source regions. Sites in the central Sahara, Sahel, and Middle East exhibit a greater temporal variability of iron oxides relative to other sites. Niger site(13.52°N, 2.63°E) is dominated by goethite over Harmattan season with median of ~2 weight percentage (wt.%) of iron-oxide. Saudi Arabia site (27.49°N, 41.98°E) over Middle East also exhibited surge of goethite content with the beginning of Shamal season. The Sahel dust is richer in iron-oxide than Saharan and northern China dust except in Summer. The Bodélé Depression area shows a distinctively lower iron-oxide concentration (~1 wt.%) throughout the year. Finally, we show that EPIC data allow to constrain the hematite refractive index. Specifically, we select 5 out of 13 different number of hematite refractive indices widely variable in published laboratory studies by constraining the iron-oxide mass ratio to the known measured values. Provided climatology of hematite and goethite mass fractions across main dust regions of the Earth will be useful for dust shortwave DRE studies and climate modeling.

Sujung Go↗

Spring Dust in Western North America and its Interannual Variability – Understanding the Role of Local and Transported Dust

Mineral dust over western North America is an important aerosol type contributing up to one half of surface aerosol concentrations in spring. In the present study, we use data from in-situ and remote-sensing observations and the NASA Unified WRF (NU-WRF) model to investigate the sources and interannual variations of the springtime fine-mode dust over western North America. The horizontal distribution, seasonality, and interannual variability of the springtime dust over the region are characterized with observations of fine dust concentrations at the Interagency Monitoring of Protected Visual Environments (IMPROVE) sites and dust optical depth (DOD) from the Aerosol Robotic Network (AERONET) measurements. We have conducted detailed modeling and analysis for April in selected years of 2005, 2008, and 2009, to understand the causes of interannual variabilities of the springtime dust with model experiments that separate the dust generated from local deserts with that transported across the Pacific Ocean. The results suggest that although several permanent deserts and semi-arid regions in the western North America are the major source of surface fine dust concentrations in the immediate vicinity, long-range transpacific transported dust is a dominant dust source in springtime, especially over the coastal regions and areas remote from the local deserts. Interannual variability of fine dust over western North America is explained with both local dust emission and long-range transported dust.

North America spring dust↗

Aerosol Absorption in Global Models From AeroCom Phase III

Aerosol-induced absorption of shortwave radiation can modify the climate through local atmospheric heating, which affects lapse rates, precipitation, and cloud formation. Presently, the total amount of aerosol absorption is poorly constrained, and the main absorbing aerosol species (black carbon (BC), organic aerosols (OA), and mineral dust) are diversely quantified in global climate models. As part of the third phase of the Aerosol Comparisons between Observations and Models (AeroCom) intercomparison initiative (AeroCom phase III), we here document the distribution and magnitude of aerosol absorption in current global aerosol models and quantify the sources of intermodel spread, highlighting the difficulties of attributing absorption to different species. In total, 15 models have provided total present-day absorption at 550 nm (using year 2010 emissions), 11 of which have provided absorption per absorbing species. The multi-model global annual mean total absorption aerosol optical depth (AAOD) is 0.0054 (0.0020 to 0.0098; 550 nm), with the range given as the minimum and maximum model values. This is 28 % higher compared to the 0.0042 (0.0021 to 0.0076) multi-model mean in AeroCom phase II (using year 2000 emissions), but the difference is within 1 standard deviation, which, in this study, is 0.0023 (0.0019 in Phase II). Of the summed component AAOD, 60 % (range 36 %–84 %) is estimated to be due to BC, 31 % (12 %–49 %) is due to dust, and 11 % (0 %–24 %) is due to OA; however, the components are not independent in terms of their absorbing efficiency. In models with internal mixtures of absorbing aerosols, a major challenge is the lack of a common and simple method to attribute absorption to the different absorbing species. Therefore, when possible, the models with internally mixed aerosols in the present study have performed simulations using the same method for estimating absorption due to BC, OA, and dust, namely by removing it and comparing runs with and without the absorbing species. We discuss the challenges of attributing absorption to different species; we compare burden, refractive indices, and density; and we contrast models with internal mixing to models with external mixing. The model mean BC mass absorption coefficient (MAC) value is 10.1 (3.1 to 17.7) m 2 g −1 (550 nm), and the model mean BC AAOD is 0.0030 (0.0007 to 0.0077). The difference in lifetime (and burden) in the models explains as much of the BC AAOD spread as the difference in BC MAC values. The difference in the spectral dependency between the models is striking. Several models have an absorption Ångstrøm exponent (AAE) close to 1, which likely is too low given current knowledge of spectral aerosol optical properties. Most models do not account for brown carbon and underestimate the spectral dependency for OA.

Aerosol absorption↗

The Response of the Amazon Ecosystem to the Photosynthetically Active Radiation Fields: Integrating Impacts of Biomass Burning Aerosol and Clouds in the NASA GEOS Earth System Model

The Amazon experiences fires every year, and the resulting biomass burning aerosols, together with cloud particles, influence the penetration of sunlight through the atmosphere, increasing the ratio of diffuse to direct photosynthetically active radiation (PAR) reaching the vegetation canopy and thereby potentially increasing ecosystem productivity. In this study, we use the NASA Goddard Earth Observing System (GEOS) model with coupled aerosol, cloud, radiation, and ecosystem modules to investigate the impact of Amazon biomass burning aerosols on ecosystem productivity, as well as the role of the Amazon’s clouds in tempering this impact. The study focuses on a seven-year period (2010-2016) during which the Amazon experienced a variety of dynamic environments (e.g., La Niña, normal years, and El Niño). The direct radiative impact of biomass burning aerosols on ecosystem productivity—called here the aerosol diffuse radiation fertilization effect —is found to increase Amazonian Gross Primary Production (GPP) by 2.6% via a 3.8% increase in diffuse PAR (DFPAR) despite a 5.4% decrease in direct PAR (DRPAR) on multiyear average during burning seasons. On a monthly basis, this increase in GPP can be as large as 9.9% (occurring in August 2010). Consequently, the net primary production (NPP) in Amazon is increased by 1.5%, or ~92 Tg C a-1– equivalent to ~37% of the average carbon lost due to Amazon fires over the seven years considered. Clouds, however, strongly regulate the effectiveness of the aerosol diffuse radiation fertilization effect. The efficiency of this fertilization effect is the highest in cloud-free conditions and linearly decreases with increasing cloud amount until the cloud fraction reaches ~0.8, at which point the aerosol-influenced light changes from being a stimulator to an inhibitor of plant growth. Nevertheless, interannual changes in the overall strength of the aerosol diffuse radiation fertilization effect are primarily controlled by the large interannual changes in biomass burning aerosols rather than by changes in cloudiness during the studied period.

biomass burning aerosols on ecosystem productivity↗

Improved Representation of the Global Dust Cycle Using Observational Constraints on Dust Properties and Abundance

Even though desert dust is the most abundant aerosol by mass in Earth’s atmosphere, atmospheric models 25 struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused byfundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, 30 extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of two relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global 35 basis, we find that the emission flux of dust with geometric diameter up to 20 μm (PM20) is approximately 5,000 Tg/year, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded data sets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this data set is more accurate than current 40 model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.

aerosols, dust↗

Contribution of the World's Main Dust Source Regions to the Global Cycle of Desert Dust

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, the relative contributions of the world's major source regions to the global dust cycle remain poorly constrained. This problem hinders accounting for the potentially large impact of regional differences in dust properties on clouds, the Earth's energy balance, and terrestrial and marine biogeochemical cycles. Here, we constrain the contribution of each of the world's main dust source regions to the global dust cycle. We use an analytical framework that integrates an ensemble of global aerosol model simulations with observationally informed constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth (DAOD). We obtain a dataset that constrains the relative contribution of nine major source regions to size-resolved dust emission, atmospheric loading, DAOD, concentration, and deposition flux. We find that the 22–29 Tg (1 standard error range) global loading of dust with a geometric diameter up to 20 µm is partitioned as follows: North African source regions contribute ∼ 50 % (11–15 Tg), Asian source regions contribute ∼ 40 % (8–13 Tg), and North American and Southern Hemisphere regions contribute ∼ 10 % (1.8–3.2 Tg). These results suggest that current models on average overestimate the contribution of North African sources to atmospheric dust loading at ∼ 65 %, while underestimating the contribution of Asian dust at ∼ 30 %. Our results further show that each source region's dust loading peaks in local spring and summer, which is partially driven by increased dust lifetime in those seasons. We also quantify the dust deposition flux to the Amazon rainforest to be ∼ 10 Tg yr−1, which is a factor of 2–3 less than inferred from satellite data by previous work that likely overestimated dust deposition by underestimating the dust mass extinction efficiency. The data obtained in this paper can be used to obtain improved constraints on dust impacts on clouds, climate, biogeochemical cycles, and other parts of the Earth system.

Dust↗

Improved representation of the global dust cycle using observational constraints on dust properties and abundance

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, atmospheric models struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused by fundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of 2 relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global basis, we find that the emission flux of dust with a geometric diameter up to 20 µm (PM20) is approximately 5000 Tg yr−1, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded datasets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this dataset is more accurate than current model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.

Dust cycle↗

Chemical Transport Models Often Underestimate Inorganic Atmospheric Aerosol Acidity in Remote Regions of the Atmosphere

The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about -1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R(exp 2) < 0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15-39%.

Chemical transport model↗