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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 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 basis, we find that the emission flux of dust with geometric diameter up to 20 μm (PM 20 ) is approximately 5,000 Tg/year, which is greater than most models account for. This larger PM 20 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 model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system., Competing Interests: Competing interests The authors declare that they have no conflict of interest.

Lockdown measures are essential to containing the spread of coronavirus disease 2019 (COVID-19), but they will slow down economic growth by reducing industrial and commercial activities. However, the benefits of activity control from containing the pandemic have not been examined and assessed. Here we use daily carbon dioxide (CO 2 ) emission reduction in China estimated from statistical data for energy consumption and satellite data for nitrogen dioxide (NO 2 ) measured by the Ozone Monitoring Instrument (OMI) as an indicator for reduced activities consecutive to a lockdown. We perform a correlation analysis to show that a 1% day -1 decrease in the rate of COVID-19 cases is associated with a reduction in daily CO 2 emissions of 0.22% ± 0.02% using statistical data for energy consumption relative to emissions without COVID-19, or 0.20% ± 0.02% using satellite data for atmospheric column NO 2 . We estimate that swift action in China is effective in limiting the number of COVID-19 cases <100,000 with a reduction in CO 2 emissions of up to 23% by the end of February 2020, whereas a 1-week delay would have required greater containment and a doubling of the emission reduction to meet the same goal. By analyzing the costs of health care and fatalities, we find that the benefits on public health due to reduced activities in China are 10-fold larger than the loss of gross domestic product. Our findings suggest an unprecedentedly high cost of maintaining activities and CO 2 emissions during the COVID-19 pandemic and stress substantial benefits of containment in public health by taking early actions to reduce activities during the outbreak of COVID-19., Competing Interests: The authors declare no competing interests., (© 2020 The Author(s).)

The emission and deposition of global atmospheric phosphorus (P) have long been considered unbalanced, and primary biogenic aerosol particles (PBAP) and phosphine (PH 3 ) are considered to be the only atmospheric P sources from the ecosystem. In this work, we found and quantified volatile organic phosphorus (VOP) emissions from plants unaccounted for in previous studies. In a greenhouse in which lemons were cultivated, the atmospheric total phosphorus (TP) concentration of particulate matter (PM) was 41.8% higher than that in a greenhouse containing only soil, and the proportion of organic phosphorus (OP) in TP was doubled. 31 P nuclear magnetic resonance tests ( 31 P-NMR) of PM showed that phosphate monoesters were the main components contributed by plants in both the greenhouse and at an outside observation site. Atmospheric gaseous P was directly measured to be 1-2 orders of magnitude lower than P in PM but appeared to double during plant growing seasons relative to other months. Bag-sampling and gas chromatography mass spectrometry (GCMS) tests showed that the gaseous P emitted by plants in the greenhouse was triethyl phosphate. VOP might be an important component of atmospheric P that has been underestimated in previous studies., Competing Interests: Declaration of competing interest There is no conflict of interest in this study., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

The 1783-1784 Laki eruption provides a natural experiment to evaluate the performance of chemistry-transport models in predicting the health impact of air particulate pollution. There are few existing daily meteorological observations during the second part of the 18 th century. Hence, creating reasonable climatological conditions for such events constitutes a major challenge. We reconstructed meteorological fields for the period 1783-1784 based on a technique of analogues described in the Methods. Using these fields and including detailed chemistry we describe the concentrations of sulphur (SO 2 /SO 4 ) that prevail over the North Atlantic, the adjoining seas and Western Europe during these 2 years. To evaluate the model, we analyse these results through the prism of two datasets contemporary to the Laki period: • The date of the first appearance of 'dry fogs' over Europe, • The excess mortality recorded in French parishes over the period June-September 1783. The sequence of appearances of the dry fogs is reproduced with a very-high degree of agreement to the first dataset. High concentrations of SO 2 /SO 4 are simulated in June 1783 that coincide with a rapid rise of the number of deceased in French parishes records. We show that only a small part of the deceased of the summer of 1783 can be explained by the present-day relationships between PM2.5 and relative risk. The implication of this result is that other external factors such as the particularly warm summer of 1783, and the lack of health care at the time, must have contributed to the sharp increase in mortality over France recorded from June to September 1783.

There is high uncertainty in the direct radiative forcing of black carbon (BC), an aerosol that strongly absorbs solar radiation. The observation-constrained estimate, which is several times larger than the bottom-up estimate, is influenced by the spatial representativeness error due to the mesoscale inhomogeneity of the aerosol fields and the relatively low resolution of global chemistry-transport models. Here we evaluated the spatial representativeness error for two widely used observational networks (AErosol RObotic NETwork and Global Atmosphere Watch) by downscaling the geospatial grid in a global model of BC aerosol absorption optical depth to 0.1° × 0.1°. Comparing the models at a spatial resolution of 2° × 2° with BC aerosol absorption at AErosol RObotic NETwork sites (which are commonly located near emission hot spots) tends to cause a global spatial representativeness error of 30%, as a positive bias for the current top-down estimate of global BC direct radiative forcing. By contrast, the global spatial representativeness error will be 7% for the Global Atmosphere Watch network, because the sites are located in such a way that there are almost an equal number of sites with positive or negative representativeness error.

Spatial patterns and temporal trends of nitrogen (N) and phosphorus (P) deposition are important for quantifying their impact on forest carbon (C) uptake. In a first step, we modeled historical and future change in the global distributions of the atmospheric deposition of N and P from the dry and wet deposition of aerosols and gases containing N and P. Future projections were compared between two scenarios with contrasting aerosol emissions. Modeled fields of N and P deposition and P concentration were evaluated using globally distributed in situ measurements. N deposition peaked around 1990 in European forests and around 2010 in East Asian forests, and both increased sevenfold relative to 1850. P deposition peaked around 2010 in South Asian forests and increased 3.5-fold relative to 1850. In a second step, we estimated the change in C storage in forests due to the fertilization by deposited N and P (∆C ν dep ), based on the retention of deposited nutrients, their allocation within plants, and C:N and C:P stoichiometry. ∆C ν dep for 1997-2013 was estimated to be 0.27 ± 0.13 Pg C year -1 from N and 0.054 ± 0.10 Pg C year -1 from P, contributing 9% and 2% of the terrestrial C sink, respectively. Sensitivity tests show that uncertainty of ∆C ν dep was larger from P than from N, mainly due to uncertainty in the fraction of deposited P that is fixed by soil. ∆C P dep was exceeded by ∆C N dep over 1960-2007 in a large area of East Asian and West European forests due to a faster growth in N deposition than P. Our results suggest a significant contribution of anthropogenic P deposition to C storage, and additional sources of N are needed to support C storage by P in some Asian tropical forests where the deposition rate increased even faster for P than for N., (© 2017 John Wiley & Sons Ltd.)

30 years after the Chernobyl Nuclear Power Plant (CNPP) accident, its radioactive releases still remain of great interest mainly due to the long half-lives of many radionuclides emitted. Observations from the terrestrial environment, which hosts radionuclides for many years after initial deposition, are important for health and environmental assessments. Furthermore, such measurements are the basis for validation of atmospheric transport models and can be used for constraining the still not accurately known source terms. However, although the "Atlas of cesium deposition on Europe after the Chernobyl accident" (hereafter referred to as "Atlas") has been published since 1998, less than 1% of the direct observations of (137)Cs deposition has been made publicly available. The remaining ones are neither accessible nor traceable to specific data providers and a large fraction of these data might have been lost entirely. The present paper is an effort to rescue some of the data collected over the years following the CNPP accident and make them publicly available. The database includes surface air activity concentrations and deposition observations for (131)I, (134)Cs and (137)Cs measured and provided by Former Soviet Union authorities the years that followed the accident. Using the same interpolation tool as the official authorities, we have reconstructed a deposition map of (137)Cs based on about 3% of the data used to create the Atlas map. The reconstructed deposition map is very similar to the official one, but it has the advantage that it is based exclusively on documented data sources, which are all made available within this publication. In contrast to the official map, our deposition map is therefore reproducible and all underlying data can be used also for other purposes. The efficacy of the database was proved using simulated activity concentrations and deposition of (137)Cs from a Langrangian and a Euleurian transport model., (Copyright © 2016. Published by Elsevier Ltd.)

The ability of 11 models in simulating the aerosol vertical distribution from regional to global scales, as part of the second phase of the AeroCom model intercomparison initiative (AeroCom II), is assessed and compared to results of the first phase. The evaluation is performed using a global monthly gridded data set of aerosol extinction profiles built for this purpose from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Layer Product 3.01. Results over 12 subcontinental regions show that five models improved, whereas three degraded in reproducing the interregional variability in Z α 0-6 km , the mean extinction height diagnostic, as computed from the CALIOP aerosol profiles over the 0-6 km altitude range for each studied region and season. While the models' performance remains highly variable, the simulation of the timing of the Z α 0-6 km peak season has also improved for all but two models from AeroCom Phase I to Phase II. The biases in Z α 0-6 km are smaller in all regions except Central Atlantic, East Asia, and North and South Africa. Most of the models now underestimate Z α 0-6 km over land, notably in the dust and biomass burning regions in Asia and Africa. At global scale, the AeroCom II models better reproduce the Z α 0-6 km latitudinal variability over ocean than over land. Hypotheses for the performance and evolution of the individual models and for the intermodel diversity are discussed. We also provide an analysis of the CALIOP limitations and uncertainties contributing to the differences between the simulations and observations.

Knowledge of the contribution that individual countries have made to global radiative forcing is important to the implementation of the agreement on "common but differentiated responsibilities" reached by the United Nations Framework Convention on Climate Change. Over the past three decades, China has experienced rapid economic development, accompanied by increased emission of greenhouse gases, ozone precursors and aerosols, but the magnitude of the associated radiative forcing has remained unclear. Here we use a global coupled biogeochemistry-climate model and a chemistry and transport model to quantify China's present-day contribution to global radiative forcing due to well-mixed greenhouse gases, short-lived atmospheric climate forcers and land-use-induced regional surface albedo changes. We find that China contributes 10% ± 4% of the current global radiative forcing. China's relative contribution to the positive (warming) component of global radiative forcing, mainly induced by well-mixed greenhouse gases and black carbon aerosols, is 12% ± 2%. Its relative contribution to the negative (cooling) component is 15% ± 6%, dominated by the effect of sulfate and nitrate aerosols. China's strongest contributions are 0.16 ± 0.02 watts per square metre for CO2 from fossil fuel burning, 0.13 ± 0.05 watts per square metre for CH4, -0.11 ± 0.05 watts per square metre for sulfate aerosols, and 0.09 ± 0.06 watts per square metre for black carbon aerosols. China's eventual goal of improving air quality will result in changes in radiative forcing in the coming years: a reduction of sulfur dioxide emissions would drive a faster future warming, unless offset by larger reductions of radiative forcing from well-mixed greenhouse gases and black carbon.

Satellite data and models suggest that oceanic productivity is reduced in response to less nutrient supply under warming. In contrast, anthropogenic aerosols provide nutrients and exert a fertilizing effect, but its contribution to evolution of oceanic productivity is unknown. We simulate the response of oceanic biogeochemistry to anthropogenic aerosols deposition under varying climate from 1850 to 2010. We find a positive response of observed chlorophyll to deposition of anthropogenic aerosols. Our results suggest that anthropogenic aerosols reduce the sensitivity of oceanic productivity to warming from -15.2 ± 1.8 to -13.3 ± 1.6 Pg C yr -1  °C -1 in global stratified oceans during 1948-2007. The reducing percentage over the North Atlantic, North Pacific, and Indian Oceans reaches 40, 24, and 25%, respectively. We hypothesize that inevitable reduction of aerosol emissions in response to higher air quality standards in the future might accelerate the decline of oceanic productivity per unit warming.

In this study we conduct a detailed comparison of the modelling response of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident with global and local observations. We use five different model versions characterized by different horizontal and vertical resolutions of the same General Circulation Model (GCM). Transport efficiencies of (137)Cs across the world are presented as an indication of the expected radioactive impact. Activity concentrations were well represented showing lower Normalized Mean Biases (NMBs) when the better resolved versions of the GCM were used. About 95% of the results using the zoom configuration over Europe (zEur) remained within a factor of 10 from the observations. Close to Japan, the model reproduced well (137)Cs concentrations using the zoom version over Asia (zAsia) showing high correlations, while more than 64% of the modelling results were found within a factor of two from the observations and more than 92% within a factor of 10. Labile and refractory rare radionuclides calculated indirectly showed larger deviations, with about 60% of the simulated concentrations within a factor of 10 from the observations. We estimate that around 23% of the released (137)Cs remained into Japan, while 76% deposited in the oceans. Around 163 TBq deposited over North America, among which 95 TBq over USA, 40 TBq over Canada and 5 TBq over Greenland). About 14 TBq deposited over Europe (mostly in the European part of Russia, Sweden and Norway) and 47 TBq over Asia (mostly in the Asian part of Russia, Philippines and South Korea), while traces were observed over Africa, Oceania and Antarctica. Since the radioactive plume followed a northward direction before its arrival to USA and then to Europe, a significant amount of about 69 TBq deposited in the Arctic, as well. These patterns of deposition are fully consistent with the most recent reports for the accident., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Radioactive contamination in Ukraine, Belarus and Russia after the Chernobyl accident left large rural and forest areas to their own fate. Forest succession in conjunction with lack of forest management started gradually transforming the landscape. During the last 28 years dead wood and litter have dramatically accumulated in these areas, whereas climate change has increased temperature and favored drought. The present situation in these forests suggests an increased risk of wildfires, especially after the pronounced forest fires of 2010, which remobilized Chernobyl-deposited radioactive materials transporting them thousand kilometers far. For the aforementioned reasons, we study the consequences of different forest fires on the redistribution of (137)Cs. Using the time frequency of the fires that occurred in the area during 2010, we study three scenarios assuming that 10%, 50% and 100% of the area are burnt. We aim to sensitize the scientific community and the European authorities for the foreseen risks from radioactivity redistribution over Europe. The global model LMDZORINCA that reads deposition density of radionuclides and burnt area from satellites was used, whereas risks for the human and animal population were calculated using the Linear No-Threshold (LNT) model and the computerized software ERICA Tool, respectively. Depending on the scenario, whereas between 20 and 240 humans may suffer from solid cancers, of which 10-170 may be fatal. ERICA predicts insignificant changes in animal populations from the fires, whereas the already extreme radioactivity background plays a major role in their living quality. The resulting releases of (137)Cs after hypothetical wildfires in Chernobyl's forests are classified as high in the International Nuclear Events Scale (INES). The estimated cancer incidents and fatalities are expected to be comparable to those predicted for Fukushima. This is attributed to the fact that the distribution of radioactive fallout after the wildfires occurred to the intensely populated Western Europe, whereas after Fukushima it occurred towards the Pacific Ocean. The situation will be exacerbated near the forests not only due to the expected redistribution of refractory radionuclides (also trapped there), but also due to the nutritional habits of the local human and animal population., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

The present paper studies how a random event (earthquake) and the subsequent disaster in Japan affect transport and deposition of fallout and the resulting health consequences. Therefore, except for the original accident in March 2011, three additional scenarios are assessed assuming that the same releases took place in winter 2010, summer 2011 and autumn 2011 in order to cover a full range of annual seasonality. This is also the first study where a large number of fission products released from the accident are used to assess health risks with the maximum possible efficiency. Xenon-133 and (137)Cs are directly estimated within the model, whereas 15 other radionuclides are calculated indirectly using reported isotopic ratios. As much as 85% of the released (137)Cs would be deposited in continental regions worldwide if the accident occurred in winter 2010, 22% in spring 2011 (when it actually happened), 55% in summer 2011 and 48% if it occurred during autumn 2011. Solid cancer incidents and mortalities from Fukushima are estimated to be between 160 and 880 and from 110 to 640 close to previous estimations. By adding thyroid cancers, the total number rises from 230 to 850 for incidents and from 120 to 650 for mortalities. Fatalities due to worker exposure and mandatory evacuation have been reported to be around 610 increasing total estimated mortalities to 730-1260. These estimates are 2.8 times higher than previously reported ones for radiocaesium and (131)I and 16% higher than those reported based on radiocaesium only. Total expected fatalities from Fukushima are 32% lower than in the winter scenario, 5% that in the summer scenario and 30% lower than in the autumn scenario. Nevertheless, cancer fatalities are expected to be less than 5% of those from the tsunami (~20,000)., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Black carbon (BC) plays an important role in both climate change and health impact. Still, BC emissions as well as the historical trends are associated with high uncertainties in existing inventories. In the present study, global BC emissions from 1960 to 2007 were estimated for 64 sources, by using recompiled fuel consumption and emission factor data sets. Annual BC emissions had increased from 5.3 (3.4-8.5 as an interquartile range) to 9.1 (5.6-14.4) teragrams during this period. Our estimations are 11-16% higher than those in previous inventories. Over the period, we found that the BC emission intensity, defined as the amount of BC emitted per unit of energy production, had decreased for all the regions, especially China and India. Improvements in combustion technology and changes in fuel composition had led to an increase in energy use efficiency, and subsequently a decline of BC emission intensities in power plants, the residential sector, and transportation. On the other hand, the BC emission intensities had increased in the industrial and agricultural sectors, mainly due to an expansion of low-efficiency industry (coke and brick production) in developing countries and to an increasing usage of diesel in agriculture in developed countries.

The accident at the Fukushima Daiichi Nuclear Power Plant (NPP) in Japan resulted in the release of a large number of fission products that were transported worldwide. We study the effects of two of the most dangerous radionuclides emitted, (137)Cs (half-life: 30.2years) and (134)Cs (half-life: 2.06years), which were transported across the world constituting the global fallout (together with iodine isotopes and noble gasses) after nuclear releases. The main purpose is to provide preliminary cancer risk estimates after the Fukushima NPP accident, in terms of excess lifetime incident and death risks, prior to epidemiology, and compare them with those occurred after the Chernobyl accident. Moreover, cancer risks are presented for the local population in the form of high-resolution risk maps for 3 population classes and for both sexes. The atmospheric transport model LMDZORINCA was used to simulate the global dispersion of radiocaesium after the accident. Air and ground activity concentrations have been incorporated with monitoring data as input to the LNT-model (Linear Non-Threshold) frequently used in risk assessments of all solid cancers. Cancer risks were estimated to be small for the global population in regions outside Japan. Women are more sensitive to radiation than men, although the largest risks were recorded for infants; the risk is not depended on the sex at the age-at-exposure. Radiation risks from Fukushima were more enhanced near the plant, while the evacuation measures were crucial for its reduction. According to our estimations, 730-1700 excess cancer incidents are expected of which around 65% may be fatal, which are very close to what has been already published (see references therein). Finally, we applied the same calculations using the DDREF (Dose and Dose Rate Effectiveness Factor), which is recommended by the ICRP, UNSCEAR and EPA as an alternative reduction factor instead of using a threshold value (which is still unknown). Excess lifetime cancer incidents were estimated to be between 360 and 850, whereas 220-520 of them will be fatal. Nevertheless, these numbers are expected to be even smaller, as the response of the Japanese official authorities to the accident was rapid. The projected cancer incidents are much lower than the casualties occurred from the earthquake itself (>20,000) and also smaller than the accident of Chernobyl., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Black carbon (BC) is increasingly recognized as a significant air pollutant with harmful effects on human health, either in its own right or as a carrier of other chemicals. The adverse impact is of particular concern in those developing regions with high emissions and a growing population density. The results of recent studies indicate that BC emissions could be underestimated by a factor of 2-3 and this is particularly true for the hot-spot Asian region. Here we present a unique inventory at 10-km resolution based on a recently published global fuel consumption data product and updated emission factor measurements. The unique inventory is coupled to an Asia-nested (∼50 km) atmospheric model and used to calculate the global population exposure to BC with fully quantified uncertainty. Evaluating the modeled surface BC concentrations against observations reveals great improvement. The bias is reduced from -88% to -35% in Asia when the unique inventory and higher-resolution model replace a previous inventory combined with a coarse-resolution model. The bias can be further reduced to -12% by downscaling to 10 km using emission as a proxy. Our estimated global population-weighted BC exposure concentration constrained by observations is 2.14 μg⋅m(-3); 130% higher than that obtained using less detailed inventories and low-resolution models.

The earthquake and the subsequent tsunami that occurred offshore of Japan resulted in an important loss of life and a serious accident at the nuclear facility of Fukushima. The "hot spots" of the release are evaluated here applying the model LMDZORINCA for (137)Cs. Moreover, an assessment is attempted for the population and the environment using the dosimetric scheme of the WHO and the interactive tool ERICA, respectively. Cesium-137 was deposited mostly in Pacific and Atlantic Oceans and North Pole (80%), whereas the rest in the continental areas of North America and Eurasia contributed slightly to the natural background (0.5-5.0 kBq m(-2)). The effective dose from (137)Cs and (134)Cs (radiocesium) irradiation during the first 3 months was estimated between 1-5 mSv in Fukushima and the neighboring prefectures. In the rest of Japan, the respective doses were found to be less than 0.5 mSv, whereas in the rest of the world it was less than 0.1 mSv. Such doses are equivalent with the obtained dose from a simple X-ray; for the highly contaminated regions, they are close to the dose limit for exposure due to radon inhalation (10 mSv). The calculated dose rates from radiocesium exposure on reference organisms ranged from 0.03 to 0.18 μGy h(-1), which are 2 orders of magnitude below the screening dose limit (10 μGy h(-1)) that could result in obvious effects on the population. However, these results may underestimate the real situation, since stable soil density was used in the calculations, a zero radiocesium background was assumed, and dose only from two radionuclides was estimated, while more that 40 radionuclides have been deposited in the vicinity of the facility. When monitoring data applied, much higher dose rates were estimated certifying ecological risk for small mammals and reptiles in terms of cytogenetic damage and reproduction.