Anthropogenic Sulfate Aerosols Research Articles

Contribution of anthropogenic sulfate aerosols to the changing Euro‐Mediterranean climate since 1980

AbstractSince the 1980s anthropogenic aerosols have been considerably reduced in Europe and the Mediterranean area. This decrease is often considered as the likely cause of the brightening effect observed over the same period. This phenomenon is however hardly reproduced by global and regional climate models. Here we use an original approach based on reanalysis‐driven coupled regional climate system modeling to show that aerosol changes explain 81 ± 16% of the brightening and 23 ± 5% of the surface warming simulated for the period 1980–2012 over Europe. The direct aerosol effect is found to dominate in the magnitude of the simulated brightening. The comparison between regional simulations and homogenized ground‐based observations reveals that observed surface solar radiation and land and sea surface temperature spatiotemporal variations over the Euro‐Mediterranean region are only reproduced when simulations include the realistic aerosol variations.

Constraints on climate forcing by sulphate aerosols from seasonal changes in Earth's spin

AbstractAngular momentum exchanges between atmosphere and solid Earth are strongly modulated by variations in global atmospheric circulation. Geodetically determined length-of-day (LOD) fluctuations provide an independent resource to investigate climate changes. Here, I evaluate the effects of volcanic and anthropogenic sulphate aerosols on Earth's rotational energy variations. The period analysed, 1980–2002, shows that the strongest seasonal LOD variations are related to sulphate peak concentrations from the El-Chichón 1982, and Pinatubo and Cerro Hudson 1991 volcanic eruptions. The Earth's rotational energy budget implies that radiative forcing alone cannot produce the observed LOD anomalies. Rather, the required amount of atmospheric kinetic energy can be explained only by a strong influence of sulphate aerosols on energy partitioning into the atmosphere, for example, as sulphate aerosols affect latent heat release and transport during condensation–evaporation–freezing cycles. Overall, the effects of sulphate aerosols on Earth's spin changes are faster than those produced by greenhouse gases.

A numerical investigation of the impacts of anthropogenic sulfate aerosol on regional climate in East Asia

Aerosol and its effects, especially its indirect effects, on climate have drawn more and more attention in recent years. In this study, the first indirect radiative forcing (RF) of sulfate aerosol and its impacts on the regional climate in East Asia during the period from December 2008 to November 2009 were investigated. Affected by the general circulation and the conversion efficiency from SO2 to SO42− in aqueous phase, a remarkable seasonal variation of sulfate was found. The results show that the highest sulfate concentration as large as 24 g m−2 appears in the summer. The indirect RF due to sulfate aerosol at the top of atmosphere (TOA) and the surface is negative, which leads to a cooling effect on the surface by 0.12°C and a reduction of precipitation by 0.01 mm d−1. The tendencies of temperature and rainfall have significant diversity in space and time. The cloud feedback, associated with the hydrologic cycle and energy budget, is responsible for this discordant distribution. The variation of low cloud dominates the change of surface temperature. The subsidence due to the cooling effect in the mid atmosphere restrained and reduced the low clouds, leading to an apparent warm effect on the surface in Northeast Mongolia.

Anthropogenic and natural causes of climate change

We test for causality between radiative forcing and temperature using multivariate time series models and Granger causality tests that are robust to the non-stationary (trending) nature of global climate data. We find that both natural and anthropogenic forcings cause temperature change and also that temperature causes greenhouse gas concentration changes. Although the effects of greenhouse gases and volcanic forcing are robust across model specifications, we cannot detect any effect of black carbon on temperature, the effect of changes in solar irradiance is weak, and the effect of anthropogenic sulfate aerosols may be only around half that usually attributed to them.

Long-Term Behavior of the Atlantic Interhemispheric SST Gradient in the CMIP5 Historical Simulations

Abstract Multidecadal and longer changes to the Atlantic interhemispheric sea surface temperature gradient (AITG) in phase 5 of the Coupled Model Intercomparison Project (CMIP5) historical simulations are investigated. Observations show a secular trend to this gradient over most of the twentieth century, with the southern lobe warming faster relative to its northern counterpart. A previous study of phase 3 of the CMIP (CMIP3) suggests that this trend is partially forced by anthropogenic sulfate aerosols. This analysis collectively confirms the partially forced trend for the CMIP5 and by anthropogenic aerosols. Like the CMIP3, the CMIP5 also simulates a reversal in the AITG trend in the late 1970s, which was attributed to a leveling off of the anthropogenic aerosol influence and increased influence of greenhouse gases in the late twentieth century. Two (of 25) CMIP5 models, however, systematically simulate a twentieth-century trend opposite to observed, leading to some uncertainty regarding the forced nature of the AITG trend. The observed AITG also exhibits a pronounced multidecadal modulation on top of the trend, associated with the Atlantic multidecadal oscillation (AMO). Motivated by a recent suggestion that the AMO is a forced response to aerosols, the causes of this multidecadal behavior were also examined. A few of the CMIP5 models analyzed do produce multidecadal AITG variations that are correlated to the observed AMO-like variation, but only one, the Hadley Centre Global Environmental Model, version 2 (HadGEM2), systematically simulates AMO-like behavior with both the requisite amplitude and phase. The CMIP5 simulations thus point to a robust aerosol influence on the historical AITG trend but not to the AMO-like multidecadal behavior.

Anthropogenic sulfate aerosol and the southward shift of tropical precipitation in the late 20th century

In this paper, we demonstrate a global scale southward shift of the tropical rain belt during the latter half of the 20th century in observations and global climate models (GCMs). In rain gauge data, the southward shift maximizes in the 1980s and is associated with signals in Africa, Asia, and South America. A southward shift exists at a similar time in nearly all CMIP3 and CMIP5 historical simulations, and occurs on both land and ocean, although in most models the shifts are significantly less than in observations. Utilizing a theoretical framework based on atmospheric energetics, we perform an attribution of the zonal mean southward shift of precipitation across a large suite of CMIP3 and CMIP5 GCMs. Our results suggest that anthropogenic aerosol cooling of the Northern Hemisphere is the primary cause of the consistent southward shift across GCMs, although other processes affecting the atmospheric energy budget also contribute to the model‐to‐model spread.

Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations

Abstract. We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from −0.58 to −0.02 Wm−2, with a mean of −0.27 Wm−2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of −0.35 Wm−2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.

Changes in the variability of the North Pacific sea surface temperature caused by direct sulfate aerosol forcing in China in a coupled general circulation model

We examine the direct effect of anthropogenic sulfate aerosol from China on the sea surface temperature (SST) variability in the North Pacific, especially focusing on the Pacific Decadal Oscillation (PDO) using a coupled general circulation model (CGCM). We conduct two long‐term simulations, i.e., the Exp_Asia and the Exp_Asia_2x. Anthropogenic sulfate aerosols are prescribed in China only in the Exp_Asia. The conditions for the Exp_Asia_2x simulation are the same as in the Exp_Asia simulation, except the concentration of the anthropogenic sulfate aerosols in China is two times higher than that of the Exp_Asia simulation. It is found that the spatial structure of the PDO changes slightly despite an increase in the anthropogenic sulfate aerosol in China. In contrast, the temporal structure of the PDO is significantly altered between the two simulations. The variance in the PDO index in the boreal winter (December‐January‐February) and spring (March‐April‐May) is enhanced for the Exp_Asia_2x on low‐frequency timescales (>10 years) compared to that of the Exp_Asia simulation. Upon further analysis, the results of our study indicate that the change in the PDO index from the Exp_Asia to the Exp_Asia_2x is associated with the change in the mean SST in the Kuroshio‐Oyashio Extension (KOE) region through the modification of atmospheric circulation. The change in SST in the KOE region is primarily associated with a wave‐like temperature structure forced by the diabatic cooling in the low‐level atmosphere in China through the modification of atmospheric circulation, which is caused by an increase in the anthropogenic sulfate aerosols. Therefore, it is possible for the temporal structure of the North Pacific SST variability (i.e., PDO) to be altered through the mean SST change in the North Pacific Ocean caused by an increase in regional sulfate aerosols in China.

Numerical simulation study of temperature change over East China in the past millennium

Despite many studies on reconstructing the climate changes over the last millennium in China, the cause of the China’s climate change remains unclear. We used the UVic Earth System Climate Model (UVic Model), an Earth system model of intermediate complexity, to investigate the contributions of climate forcings (e.g. solar insolation variability, anomalous volcanic aerosols, greenhouse gas, solar orbital change, land cover changes, and anthropogenic sulfate aerosols) to surface air temperature over East China in the past millennium. The simulation of the UVic Model could reproduce the three main characteristic periods (e.g. the Medieval Warm Period (MWP), the Little Ice Age (LIA), and the 20th Century Warming Period (20CWP)) of the northern hemisphere and East China, which were consistent with the corresponding reconstructed air temperatures at century scales. The simulation result reflected that the air temperature anomalies of East China were larger than those of the global air temperature during the MWP and the first half of 20CWP and were lower than those during the LIA. The surface air temperature of East China over the past millennium has been divided into three periods in the MWP, four in the LIA, and one in the 20CWP. The MWP of East China was caused primarily by solar insolation and secondarily by volcanic aerosols. The variation of the LIA was dominated by the individual sizes of the contribution of solar insolation variability, greenhouse gas, and volcano aerosols. Greenhouse gas and volcano aerosols were the main forcings of the third and fourth periods of the LIA, respectively. We examined the nonlinear responses among the natural and anthropogenic forcings in terms of surface air temperature over East China. The nonlinear responses between the solar orbit change and anomalous volcano aerosols and those between the greenhouse gases and land cover change (or anthropogenic sulfate aerosols) all contributed approximately 0.2°C by the end of 20th century. However, the output of the energy-moisture balance atmospheric model from UVic showed no obvious nonlinear responses between anthropogenic and natural forcings. The nonlinear responses among all the climate forcings (both anthropogenic and natural forcings) contributed to a temperature increase of approximately 0.27°C at the end of the 20th century, accounting for approximately half of the warming during this period; the remainder was due to the climate forcings themselves.

Statistical technique seeks to reduce climate uncertainty

Three measures of the climate system—climate sensitivity, vertical ocean diffusivity, and sulfate aerosol forcing—underpin current understanding of the power of anthropogenic climate change. Climate sensitivity reflects the equilibrium temperature change that would occur given a doubling of atmospheric carbon dioxide, vertical ocean diffusivity affects the rate at which the ocean is able to redistribute heat, and sulfate aerosol forcing describes how anthropogenic sulfate aerosols affect the radiation budget. Other projections rest on these measures, such as changes in weather patterns or precipitation rates, with the derivative predictions sensitive to changes in the more fundamental properties. Given their importance, a key research effort revolves around minimizing the uncertainty in the portrayal of climate sensitivity, ocean diffusivity, and aerosol forcing in climate models. A conventional approach to doing so is to systematically vary climate model parameters in an attempt to minimize the discrepancy between model results and the observational record. The time and financial requirements of running large‐scale climate models, however, reduce this technique's viability. To overcome these barriers, Olson et al. refined an approach to statistically emulate a complex climate model, allowing them to simulate a massive number of model runs at a fraction of the cost.

A climate sensitivity estimate using Bayesian fusion of instrumental observations and an Earth System model

Current climate model projections are uncertain. This uncertainty is partly driven by the uncertainty in key model parameters such as climate sensitivity (CS), vertical ocean diffusivity (Kv), and strength of anthropogenic sulfate aerosol forcing. These parameters are commonly estimated using ensembles of model runs constrained by observations. Here we obtain a probability density function (pdf) of these parameters using the University of Victoria Earth System Climate Model (UVic ESCM) ‐ an intermediate complexity model with a dynamic three‐dimensional ocean. Specifically, we run an ensemble of UVic ESCM runs varying parameters that affectCS, ocean vertical diffusion, and the effects of anthropogenic sulfate aerosols. We use a statistical emulator that interpolates the UVic ESCM output to parameter settings where the model was not evaluated. We adopt a Bayesian approach to constrain the model output with instrumental surface temperature and ocean heat observations. Our approach accounts for the uncertainties in the properties of model‐data residuals. We use a Markov chain Monte Carlo method to obtain a posterior pdf of these parameters. The mode of the climate sensitivity estimate is 2.8°C, with the corresponding 95% credible interval ranging from 1.8 to 4.9°C. These results are generally consistent with previous studies. TheCS pdf is sensitive to the assumptions about the priors, to the effects of anthropogenic sulfate aerosols, and to the background vertical ocean diffusivity. Our method can be used with more complex climate models.

A study of uncertainties in the sulfate distribution and its radiative forcing associated with sulfur chemistry in a global aerosol model

Abstract. The direct radiative forcing by sulfate aerosols is still uncertain, mainly because the uncertainties are largely derived from differences in sulfate column burdens and its vertical distributions among global aerosol models. One possible reason for the large difference in the computed values is that the radiative forcing delicately depends on various simplifications of the sulfur processes made in the models. In this study, therefore, we investigated impacts of different parts of the sulfur chemistry module in a global aerosol model, SPRINTARS, on the sulfate distribution and its radiative forcing. Important studies were effects of simplified and more physical-based sulfur processes in terms of treatment of sulfur chemistry, oxidant chemistry, and dry deposition process of sulfur components. The results showed that the difference in the aqueous-phase sulfur chemistry among these treatments has the largest impact on the sulfate distribution. Introduction of all the improvements mentioned above brought the model values noticeably closer to in-situ measurements than those in the simplified methods used in the original SPRINTARS model. At the same time, these improvements also brought the computed sulfate column burdens and its vertical distributions into good agreement with other AEROCOM model values. The global annual mean radiative forcing due to the direct effect of anthropogenic sulfate aerosol was thus estimated to be −0.26 W m−2 (−0.30 W m−2 with a different SO2 inventory), whereas the original SPRINTARS model showed −0.18 W m−2 (−0.21 W m−2 with a different SO2 inventory). The magnitude of the difference between original and improved methods was approximately 50% of the uncertainty among estimates by the world's global aerosol models reported by the IPCC-AR4 assessment report. Findings in the present study, therefore, may suggest that the model differences in the simplifications of the sulfur processes are still a part of the large uncertainty in their simulated radiative forcings.

Reducing the Uncertainties in Direct Aerosol Radiative Forcing

Airborne particles, which include desert and soil dust, wildfire smoke, sea salt, volcanic ash, black carbon, natural and anthropogenic sulfate, nitrate, and organic aerosol, affect Earth's climate, in part by reflecting and absorbing sunlight. This paper reviews current status, and evaluates future prospects for reducing the uncertainty aerosols contribute to the energy budget of Earth, which at present represents a leading factor limiting the quality of climate predictions. Information from satellites is critical for this work, because they provide frequent, global coverage of the diverse and variable atmospheric aerosol load. Both aerosol amount and type must be determined. Satellites are very close to measuring aerosol amount at the level-of-accuracy needed, but aerosol type, especially how bright the airborne particles are, cannot be constrained adequately by current techniques. However, satellite instruments can map out aerosol air mass type, which is a qualitative classification rather than a quantitative measurement, and targeted suborbital measurements can provide the required particle property detail. So combining satellite and suborbital measurements, and then using this combination to constrain climate models, will produce a major advance in climate prediction.

Impacts of internally and externally mixed anthropogenic sulfate and carbonaceous aerosols on East Asian climate

A coupled regional climate and aerosol-chemistry model, RIEMS 2.0 (Regional Integrated Environmental Model System for Asia), in which anthropogenic sulfate, black carbon, and organic carbon were assumed to be externally mixed (EM), internally mixed (IM) or partially internally mixed (IEM), was used to simulate the impacts of these anthropogenic aerosols on East Asian climate for the entire year of 2006. The distributions of aerosol mass concentration, radiative forcing and hence the surface air temperature and precipitation variations under three mixing assumptions of aerosols were analyzed. The results indicated that the mass concentration of sulfate was sensitive to mixing assumptions, but carbonaceous aerosols were much less sensitive to the mixing types. Modeled results were compared with observations in a variety of sites in East Asia. It was found that the simulated concentrations of sulfate and carbonaceous aerosols were in accord with the observations in terms of magnitude. The simulated aerosol concentrations in IM case were closest to observation results. The regional average column burdens of sulfate, black carbon, and organic carbon, if internally mixed, were 11.49, 0.47, and 2.17 mg m−2, respectively. The radiative forcing of anthropogenic aerosols at the top of the atmosphere increased from −1.27 (EM) to −1.97 W m−2 (IM) while the normalized radiative forcing (NRF) decreased from −0.145 (EM) to −0.139 W mg−1 (IM). The radiative forcing and NRF were −1.82 W m−2 and −0.141 W mg−1 for IEM, respectively. The surface air temperature changes over the domain due to the anthropogenic sulfate and carbonaceous aerosols were −0.067, −0.078, and −0.072 K, with maxima of −0.47, −0.50, and −0.49 K, for EM, IM, and IEM, respectively. Meanwhile, the annual precipitation variations were −8.0 (EM), −20.6 (IM), and −21.9 mm (IEM), with maxima of 148, 122, and 102 mm, respectively, indicating that the climate effects were stronger if the sulfate and carbonaceous aerosols were internally mixed.

Seasonal variations in aerosol optical properties over China

[1] Seasonal variations in background aerosol optical depth (AOD) and aerosol type are investigated over various ecosystems in China based upon three years' worth of meteorological data and data collected by the Chinese Sun Hazemeter Network. In most parts of China, AODs are at a maximum in spring or summer and at a minimum in autumn or winter. Minimum values (0.10∼0.20) of annual mean AOD at 500 nm are found in the Qinghai-Tibetan Plateau, the remote northeast corner of China, the northern forest ecosystems and Hainan Island. Annual mean AOD ranges from 0.25 to 0.30 over desert and oasis areas, as well as the desertification grasslands in northern China; the annual mean AOD over the Loess Plateau is moderately high at 0.36. Regions where the highest density of agricultural and industrial activities are located and where anthropogenic sulphate aerosol and soil aerosol emissions are consistently high throughout the whole year (e.g., the central-eastern, southern and eastern coastal regions of China) experience annual mean AODs ranging from 0.50∼0.80. Remarkable seasonal changes in the main types of aerosol over northern China (characterized by the Angstrom exponent, α) are seen. Due to biomass and fossil fuel burning from extensive agricultural practices in northern rural areas, concentrations of smoke and soot aerosols rise dramatically during autumn and winter (high α), while the main types of aerosol during spring and summer are dust and soil aerosols (low α). Over southeastern Asia, biomass burning during the spring leads to increases in smoke and soot emissions. Over the Tibetan Plateau and Hainan Island where the atmosphere is pristine, the main types of aerosol are dust and sea salt, respectively.

CLARREO shortwave observing system simulation experiments of the twenty-first century: Simulator design and implementation

[1] Projected changes in the Earth system will likely be manifested in changes in reflected solar radiation. This paper introduces an operational Observational System Simulation Experiment (OSSE) to calculate the signals of future climate forcings and feedbacks in top-of-atmosphere reflectance spectra. The OSSE combines simulations from the Intergovernmental Panel on Climate Change (IPCC) Fourth Assessment Report for the NCAR Community Climate System Model (CCSM) with the MODTRAN radiative transfer code to calculate reflectance spectra for simulations of current and future climatic conditions over the 21st century. The OSSE produces narrowband reflectances and broadband fluxes, the latter of which have been extensively validated against archived CCSM results. The shortwave reflectance spectra contain atmospheric features including signals from water vapor, liquid and ice clouds, and aerosols. The spectra are also strongly influenced by the surface bidirectional reflectance properties of predicted snow and sea ice and the climatological seasonal cycles of vegetation. By comparing and contrasting simulated reflectance spectra based on emissions scenarios with increasing projected and fixed present-day greenhouse gas and aerosol concentrations, we find that prescribed forcings from increases in anthropogenic sulfate and carbonaceous aerosols are detectable and are spatially confined to lower latitudes. Also, changes in the intertropical convergence zone and poleward shifts in the subsidence zones and the storm tracks are all detectable along with large changes in snow cover and sea ice fraction. These findings suggest that the proposed NASA Climate Absolute Radiance and Refractivity Observatory (CLARREO) mission to measure shortwave reflectance spectra may help elucidate climate forcings, responses, and feedbacks.

Sulfate Aerosol Control of Tropical Atlantic Climate over the Twentieth Century

Abstract The tropical Atlantic interhemispheric gradient in sea surface temperature significantly influences the rainfall climate of the tropical Atlantic sector, including droughts over West Africa and Northeast Brazil. This gradient exhibits a secular trend from the beginning of the twentieth century until the 1980s, with stronger warming in the south relative to the north. This trend behavior is on top of a multidecadal variation associated with the Atlantic multidecadal oscillation. A similar long-term forced trend is found in a multimodel ensemble of forced twentieth-century climate simulations. Through examining the distribution of the trend slopes in the multimodel twentieth-century and preindustrial models, the authors conclude that the observed trend in the gradient is unlikely to arise purely from natural variations; this study suggests that at least half the observed trend is a forced response to twentieth-century climate forcings. Further analysis using twentieth-century single-forcing runs indicates that sulfate aerosol forcing is the predominant cause of the multimodel trend. The authors conclude that anthropogenic sulfate aerosol emissions, originating predominantly from the Northern Hemisphere, may have significantly altered the tropical Atlantic rainfall climate over the twentieth century.

Estimates of climate changes in the 20th-21st centuries based on the version of the IAP RAS climate model including the model of general ocean circulation

Numerical experiments are analyzed for 1860–2100 with the version of the climate model of intermediate complexity of the Obukhov Institute of Atmospheric Physics of the Russian Academy of Sciences (IAP RAS) including the model of general ocean circulation as the oceanic module (CM IAP RAS-GOC) taking account of concentration variations of anthropogenic greenhouse gases and tropospheric sulfate aerosols from the data of observations and reconstructions for the second half of the 19th and for the 20th century and, according to SRES scenarios, in the 21st century. In the 20th century, the model simulates realistically the variations of surface atmospheric temperature, characteristics of heat absorption by the ocean, and oceanic meridional heat transport. The linear trend of global surface atmospheric temperature in the 20th century (in its last 30 years) in this version of the model amounts to 0.5 ± 0.1 K/100 years (0.22 ± 0.05 K/10 years) that is agreed with the observational data. In the 21st century, the global increase in the surface temperature amounts to 2.5 K (3.5 and 4.1 K) for SRES B1 scenario (for SRES A1B and SRES A2 scenarios, respectively). The increase in the surface temperature is the most significant in high latitudes, especially in the Northern Hemisphere and it is higher, on the whole, over the land than over the ocean. The warming near the surface is larger in winter than in summer. The maximum warming is observed in the Arctic and over the land of subpolar latitudes of the Northern Hemisphere reaching 6–10 K by the end of the 21st century in these regions as compared with the end of the 20th century depending on the anthropogenic impact scenario. At the increase in surface temperature in the 20th–21st centuries, the increase in the heat flow to the ocean and the weakening of the heat transport by the ocean from the tropics to the polar area by 1.5–2 times are registered, on the whole. At the warming, the CM IAP RAS-GOC gives the general increase in the annual precipitation amount which is especially appreciable in the tropics and in the storm-track regions. At the global averaging, the precipitation in the 21st century increase by 20–25%.

Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean – potential impacts

Abstract. Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, indicating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols shows that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud, and by entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

Anthropogenic sulphate aerosols and large Cl-deficit in marine atmospheric boundary layer of tropical Bay of Bengal

Our long-term study provides an unequivocal evidence for near-quantitative (80–100%) depletion of chloride from sea-salts in the marine atmospheric boundary layer (MABL) of tropical Bay of Bengal. During the late NE-monsoon (Jan-Mar), continental outflow from south and south-east Asia dominate the wide-spread dispersal of pollutants over the Bay of Bengal. Among anthropogenic constituents, SO42− (range: 0.6–35 μg m−3) is the most dominant. The non-sea-salt SO42− (nss-SO42−) constitutes a major fraction (55–65%) of the aerosol water-soluble ionic composition (WSIC), whereas contribution of NO3− is relatively minor. The magnitude of Cl-deficit (with respect to its sea-salt proportion) exhibits linear increase with the excess-nss-SO42− (excess over NH4+). We propose that displacement of HCl from sea-salt aerosols by H2SO4 is a dominant reaction mechanism for the chloride-depletion. These results also suggest that sea-salts could serve as a potential sink for anthropogenic SO2 in the downwind polluted marine environment. Furthermore, loss of hydrogen chloride, representing a large source of reactive chlorine, has implications to the oxidant chemistry in the MABL (oxidation of hydrocarbons and dimethyl sulphide).