Anthropogenic Sulfur Emissions Research Articles

Chemical composition of cloud and rainwater at a high-altitude mountain site in western India: source apportionment and potential factors.

This study focuses on the chemical composition of cloud water (CW) and rainwater (RW) collected at Sinhagad, a high-altitude station (1450m AMSL) located in the western region of India. The samples were collected during the monsoon over two years (2016-2017). The chemical analysis suggests that the concentration of total ionic constituents was three times higher in CW than in RW, except for NH4+ (1.0) and HCO3- (0.6). Compared to RW, high concentrations of SO42- and NO3- were observed in CW. The weighted average RW pH (6.5 ± 0.3) was slightly more alkaline than CW pH (6.1 ± 0.5). This can be attributed to the high concentrations of neutralizing ions such as nss-Ca2+, nss-Mg2+, K+, and NH4+, indicating the greater extent of wet scavenging during rainfall. These ions counteract the acidity generated by SO42- and NO3-. A high correlation between Ca2+, Na+, K+, NO3-, and SO42- makes it difficult to estimate the contribution of SO42- from different sources. Anthropogenic sulfur emissions and soil dust significantly influence the ionic composition of clouds and rain. Positive matrix factorization (PMF) was used to identify the contribution of different sources to the samples. In the CW, the extracted factors were cooking and vehicles, aging sea salt, agriculture, and dust. In RW, the factors were industries, cooking and vehicles, agriculture and dust, and aging sea salt. The findings of this study have significant implications for the monsoon build-up, ecosystems, agriculture, and climate change.

Neutralization of Anthropogenic Acidic Particles by NH3 From Wildfire Over Tropical Peatland

AbstractAcidity is an essential characteristic of aerosol particles that influences chemical and physical properties. Aerosol particles in tropical Asia, such as Singapore, have been reported as highly acidic due to intense anthropogenic sulfur emissions. At the same time, the region has also been experiencing wildfire over tropical peatlands, which is recognized as an intense source of NH3. Here, we investigated the role of NH3 from wildfire on aerosol particles in Singapore by employing the aerosol mass spectrometric technique. The observation was conducted both during wildfire haze (2015 October and 2019 September–October) and non‐haze (2018 October and 2019 April) periods. The observation result demonstrated that inorganic ionic species in Singapore were neutralized by NH4+ during the haze periods. Namely, the degree of neutralization of aerosol particles (i.e., measured NH4+ concentration/predicted NH4+ concentration by assuming that NH4+ fully neutralized SO42−, NO3−, and Cl−) was lower than 0.77during the non‐haze periods. On the other hand, the corresponding values were higher than 0.93 during the haze periods. In addition, NO3− concentration during the daytime of the haze period in 2015 was higher than that in other observation periods. A thermodynamic model calculation suggested that the regime shifts from the “NH3 sensitive region” to the “NH3 and HNO3 sensitive region” or “HNO3 sensitive region” might have occurred during the haze period. In the future, continuous monitoring of both gas‐ and particle‐phase inorganic chemical species will need to be conducted to investigate the impact of wildfire haze on atmospheric chemical processes in more detail.

Sulfur isotopes quantify the impact of anthropogenic activities on industrial-era Arctic sulfate in a Greenland ice core

Anthropogenic sulfate aerosols are estimated to have offset 60% of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling plot to determine the anthropogenic sulfur isotopic signature (δ34Santhro = +2.9 ± 0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ34Santhro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 67 ± 7% of non-sea-salt sulfate (65.1 ± 20.2 µg kg−1) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8 µg kg−1) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g. volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era.

Revealing the chemical characteristics of Arctic low-level cloud residuals – in situ observations from a mountain site

Abstract. The role aerosol chemical composition plays in Arctic low-level cloud formation is still poorly understood. In this study we address this issue by combining in situ observations of the chemical characteristics of cloud residuals (dried liquid cloud droplets or ice crystals) and aerosol particles from the Zeppelin Observatory in Ny-Ålesund, Svalbard (approx. 480 m a.s.l.). These measurements were part of the 1-year-long Ny-Ålesund Aerosol and Cloud Experiment 2019–2020 (NASCENT). To obtain the chemical composition of cloud residuals at molecular level, we deployed a Filter Inlet for Gases and AEROsols coupled to a Chemical Ionization Mass Spectrometer (FIGAERO-CIMS) with iodide as the reagent ion behind a ground-based counterflow virtual impactor (GCVI). The station was enshrouded in clouds roughly 15 % of the time during NASCENT, out of which we analyzed 14 cloud events between December 2019 and December 2020. During the entire year, the composition of the cloud residuals shows contributions from oxygenated organic compounds, including organonitrates, and traces of the biomass burning tracer levoglucosan. In summer, methanesulfonic acid (MSA), an oxidation product of dimethyl sulfide (DMS), shows large contributions to the sampled mass, indicating marine natural sources of cloud condensation nuclei (CCN) and ice nucleating particle (INP) mass during the sunlit part of the year. In addition, we also find contributions of the inorganic acids nitric acid and sulfuric acid, with outstanding high absolute signals of sulfuric acid in one cloud residual sample in spring and one in late summer (21 May and 12 September 2020), probably caused by high anthropogenic sulfur emissions near the Barents Sea and Kara Sea. During one particular cloud event, on 18 May 2020, the air mass origin did not change before, during, or after the cloud. We therefore chose it as a case study to investigate cloud impact on aerosol physicochemical properties. We show that the overall chemical composition of the organic aerosol particles was similar before, during, and after the cloud, indicating that the particles had already undergone one or several cycles of cloud processing before being measured as residuals at the Zeppelin Observatory and/or that, on the timescales of the observed cloud event, cloud processing of the organic fraction can be neglected. Meanwhile, there were on average fewer particles but relatively more in the accumulation mode after the cloud. Comparing the signals of sulfur-containing compounds of cloud residuals with aerosols during cloud-free conditions, we find that sulfuric acid had a higher relative contribution to the cloud residuals than to aerosols during cloud-free conditions, but we did not observe an increase in particulate MSA due to the cloud. Overall, the chemical composition, especially of the organic fraction of the Arctic cloud residuals, reflected the overall composition of the general aerosol population well. Our results thus suggest that most aerosols can serve as seeds for low-level clouds in the Arctic.

Uncovering the chemistry of color change in rock art in Leang Tedongnge (Pangkep Regency, South Sulawesi, Indonesia)

The color change process is among the various threats endangering the preservation of the Maros-Pangkep rock art. It is necessary to be concerned about this issue because it can cause rock art to lose its original hue, fade, obscure, or darken. Among the rock art sites in the Maros-Pangkep Region experiencing the color change of rock art pigments is Leang Tedongnge. The color change process is indicated by several hand stencils with bright red and yellow colors, while others show a dark, dull red hue or a greyish tone. In this work, we aim to assess the mechanism of the color change process by studying the physicochemical properties of the pigment. Here, we employed a combined multi-analytical characterization, including optical microscopy observation, elemental analyzes of X-ray fluorescence (XRF), scanning electron microscopy coupled with energy dispersive electron spectroscopy (SEM-EDS), and Raman spectroscopy. The result indicates that the color-change process of the rock art of Leang Tedongnge was due to the formation of a greyish crust layer made up predominantly of gypsum minerals. The layer caused the pigment to become dull, fade or darken and obscured the original color of the rock art. The layer is formed by the reaction between calcium ion dissolved in the seeping of karst water with sulphate ions from the minerals deposited at the rock's surface. Moreover, the reaction might also involve the sulfate ions derived from anthropogenic sulfur emissions produced by post-harvesting straw burning near the rock art site. To the best of our knowledge, this work is the first report to present a detailed-physicochemical assessment of pigment material regarding the color change for Indonesian rock art.

The historical impact of anthropogenic air-borne sulphur on the Pleistocene rock art of Sulawesi

The Maros-Pangkep karst in southwest Sulawesi, Indonesia, contains some of the world’s oldest rock art. However, the Pleistocene images survive only as weathered patches of pigment on exfoliated limestone surfaces. Salt efflorescence underneath the case-hardened limestone substrate causes spall-flaking, and it has been proposed that the loss of artwork has accelerated over recent decades. Here, we utilise historical photographs and superposition constraints to show that the bulk of the damage was present before 1950 CE, and describe the role of anthropogenic sulphur emissions in promoting gypsum-salt efflorescence and rock art decay. The rock art shelters have been exposed to domestic fire-use and intensive rice cultivation with post-harvest burning of straw for hundreds (if not thousands) of years, both of which release chemically reactive sulphur oxides for gypsum formation, with cumulative effects. Analysis of time-lapse photography indicates that the rate of rock art loss may be on the decline, consistent with the history of fire-use in southwest Sulawesi. At present, vandalism and sulphur emissions from diesel-powered traffic and cement-based infrastructure development constitute localised threats. Our findings indicate that there are grounds for being cautiously optimistic that targeted conservation measures will ensure the longevity of some of our oldest artistic treasures.

Simulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimates

Abstract. Dimethylsulfide (DMS) emitted from seawater is a key precursor to new particle formation and acts as a regulator in Earth's warming climate system. However, DMS's effects are not well understood in various ocean regions. In this study, we estimated DMS emissions based on a machine learning method and used the GEOS-Chem global 3D chemical transport model coupled with the TwO Moment Aerosol Sectional (TOMAS) microphysics scheme to simulate the atmospheric chemistry and radiative effects of DMS. The contributions of DMS to atmospheric SO42- aerosol and cloud condensation nuclei (CCN) concentrations along with the radiative effects over the Asian region were evaluated for the first time. First, we constructed novel monthly resolved DMS emissions (0.5∘×0.5∘) for the year 2017 using a machine learning model; 4351 seawater DMS measurements (including the recent measurements made over the Chinese seas) and 12 relevant environment parameters were selected for model training. We found that the model could predict the observed DMS concentrations with a correlation coefficient of 0.75 and fill the values in regions lacking observations. Across the Asian seas, the highest seasonal mean DMS concentration occurred in March–April–May (MAM), and we estimate the annual DMS emission flux of 1.25 Tg (S), which is equivalent to 15.4 % of anthropogenic sulfur emissions over the entire simulation domain (which covered most of Asia) in 2017. The model estimates of DMS and methane sulfonic acid (MSA), using updated DMS emissions, were evaluated by comparing them with cruise survey experiments and long-term online measurement site data. The improvement in model performance can be observed compared with simulation results derived from the global-database DMS emissions. The relative contributions of DMS to SO42- and CCN were higher in remote oceanic areas, contributing 88 % and 42 % of all sources, respectively. Correspondingly, the sulfate direct radiative forcing (DRF) and indirect radiative forcing (IRF) contributed by DMS ranged from −200 to −20 mW m−2 and from −900 to −100 mW m−2, respectively, with levels varying by season. The strong negative IRF is mainly over remote ocean regions (−900 to −600 mW m−2). Generally, the magnitude of IRF derived by DMS was twice as large as its DRF. This work provides insights into the source strength of DMS and the impact of DMS on climate and addresses knowledge gaps related to factors controlling aerosols in the marine boundary layer and their climate impacts.

Reductions in the deposition of sulfur and selenium to agricultural soils pose risk of future nutrient deficiencies

Atmospheric deposition is a major source of the nutrients sulfur and selenium to agricultural soils. Air pollution control and cleaner energy production have reduced anthropogenic emissions of sulfur and selenium, which has led to lower atmospheric deposition fluxes of these elements. Here, we use a global aerosol-chemistry-climate model to map recent (2005–2009) sulfur and selenium deposition, and project future (2095–2099) changes under two socioeconomic scenarios. Across the Northern Hemisphere, we find substantially decreased deposition to agricultural soils, by 70 to 90% for sulfur and by 55 to 80% for selenium. Recent trends in sulfur and selenium concentrations in USA streams suggest that catchment mass balances of these elements are already changing due to the declining atmospheric supply. Sustainable fertilizer management strategies will need to be developed to offset the decrease in atmospheric nutrient supply and ensure future food security and nutrition, while avoiding consequences for downstream aquatic ecosystems.

The Elbrus (Caucasus, Russia) ice core record – Part 1: reconstruction of past anthropogenic sulfur emissions in south-eastern Europe

Abstract. This study reports on the glaciochemistry of a deep ice core (182 m long) drilled in 2009 at Mount Elbrus in the Caucasus, Russia. Radiocarbon dating of the particulate organic carbon fraction in the ice suggests that the basal ice dates to 280±400 CE (Common Era). Based on chemical stratigraphy, the upper 168.6 m of the core was dated by counting annual layers. The seasonally resolved chemical records cover the years 1774–2009 CE, thus being useful to reconstruct many aspects of atmospheric pollution in south-eastern Europe from pre-industrial times to the present day. After having examined the extent to which the arrival of large dust plumes originating from the Sahara and Middle East modifies the chemical composition of the Elbrus (ELB) snow and ice layers, we focus on the dust-free sulfur pollution. The ELB dust-free sulfate levels indicate a 6- and 7-fold increase from 1774–1900 to 1980–1995 in winter and summer, respectively. Remaining close to 55±10 ppb during the 19th century, the annual dust-free sulfate levels started to rise at a mean rate of ∼3 ppb per year from 1920 to 1950. The annual increase accelerated between 1950 and 1975 (8 ppb per year), with levels reaching a maximum between 1980 and 1990 (376±10 ppb) and subsequently decreasing to 270±18 ppb at the beginning of the 21st century. Long-term dust-free sulfate trends observed in the ELB ice cores are compared with those previously obtained in Alpine and Altai (Siberia) ice, with the most important differences consisting in a much earlier onset and a more pronounced decrease in the sulfur pollution over the last 3 decades in western Europe than south-eastern Europe and Siberia.

The Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP): motivation and experimental design

Abstract. The Stratospheric Sulfur and its Role in Climate (SSiRC) Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP) explores uncertainties in the processes that connect volcanic emission of sulfur gas species and the radiative forcing associated with the resulting enhancement of the stratospheric aerosol layer. The central aim of ISA-MIP is to constrain and improve interactive stratospheric aerosol models and reduce uncertainties in the stratospheric aerosol forcing by comparing results of standardized model experiments with a range of observations. In this paper we present four co-ordinated inter-model experiments designed to investigate key processes which influence the formation and temporal development of stratospheric aerosol in different time periods of the observational record. The Background (BG) experiment will focus on microphysics and transport processes under volcanically quiescent conditions, when the stratospheric aerosol is controlled by the transport of aerosols and their precursors from the troposphere to the stratosphere. The Transient Aerosol Record (TAR) experiment will explore the role of small- to moderate-magnitude volcanic eruptions, anthropogenic sulfur emissions, and transport processes over the period 1998–2012 and their role in the warming hiatus. Two further experiments will investigate the stratospheric sulfate aerosol evolution after major volcanic eruptions. The Historical Eruptions SO2 Emission Assessment (HErSEA) experiment will focus on the uncertainty in the initial emission of recent large-magnitude volcanic eruptions, while the Pinatubo Emulation in Multiple models (PoEMS) experiment will provide a comprehensive uncertainty analysis of the radiative forcing from the 1991 Mt Pinatubo eruption.

Emission control in the combustion of coal–water and organic coal–water fuels

Promising methods for decreasing anthropogenic emissions due to the combustion of coals of different ranks and coal–water fuel (CWF) and organic coal–water fuel (OCWF) slurries on their basis are considered. The maximum concentrations of the main anthropogenic emissions of sulfur, nitrogen, and carbon oxides (SO x , NO x , and CO x ) formed upon the combustion of solid fuels in a powdered state and as the components of CWF and OCWF slurries were determined. The concentrations of the most hazardous oxides formed upon the combustion of coals of different ranks (brown and black coals) and CWF and OCWF slurries were compared. The experimental results substantiated the use of CWF and OCWF slurries for emission control in coal-burning power engineering. The addition of a combustible liquid component to a CWF slurry (the production of an OCWF slurry) makes it possible to ensure acceptable environmental and energy characteristics.

Impacts to ecosystem services from aquatic acidification: using FEGS‐CS to understand the impacts of air pollution

AbstractIncreases in anthropogenic emissions of sulfur (S) and nitrogen (N) have resulted in increases in the associated atmospheric deposition of acidic compounds. In sensitive watersheds, this deposition has initiated a cascade of negative environmental effects on aquatic ecosystems, resulting in a degradation or loss of valuable ecosystem goods and services. Here, we report the activities of an expert workgroup to synthesize information on acidic deposition‐induced aquatic acidification from the published literature and to link critical load exceedances with ecosystem services and beneficiaries, using the Stressor–Ecological Production function–Final Ecosystem Services (STEPS) Framework and the Final Ecosystem Goods and Services Classification System (FEGS‐CS). Experts identified and documented the sensitive aquatic ecosystem ecological endpoints valued by humans, and the environmental pathways through which these endpoints may experience degradation in response to acidification. Beneficiary groups were then identified for each sensitive ecological endpoint to clarify relationships between humans and the effects of aquatic acidification, and to lay the foundation for future research and analysis to value these FEGS.

Environmentally and economically efficient utilization of coal processing waste

High concentrations of hazardous anthropogenic emissions (sulfur, nitrogen and carbon oxides) from solid fuel combustion in coal burning plants cause environmental problems that have been especially pressing over the last 20–30 years. A promising solution to these problems is a switch from conventional pulverized coal combustion to coal-water slurry fuel. In this paper, we pay special attention to the environmental indicators characterizing the combustion of different coal ranks (gas, flame, coking, low-caking, and nonbaking coals) and coal-water slurry fuels based on the coal processing waste – filter cakes. There have been no consistent data so far on the acceptable intervals for the anthropogenic emissions of sulfur (SOx), nitrogen (NOx) and carbon (CO, CO2) oxides. Using a specialized combustion chamber and gas analyzing system, we have measured the concentrations of typical coal and filter-cake-based CWS combustion products. We have also calculated the typical combustion heat of the fuels under study and measured the ratio between environmental and energy attributes. The research findings show that the use of filter cakes in the form of CWS is even better than coals in terms of environment and economy. Wide utilization of filter cakes solves many environmental problems: the areas of contaminated sites shrink, anthropogenic emissions decrease, and there is no need to develop new coal mines anymore.

Radiative forcing from anthropogenic sulfur and organic emissions reaching the stratosphere

AbstractStratospheric aerosols cool the Earth by scattering sunlight. Although sulfuric acid dominates the stratospheric aerosol, this study finds that organic material in the lowermost stratosphere contributes 30–40% of the nonvolcanic stratospheric aerosol optical depth (sAOD). Simulations indicate that nonvolcanic sAOD has increased 77% since 1850. Stratospheric aerosol accounts for 21% of the total direct aerosol radiative forcing (which is negative) and 12% of the total aerosol optical depth (AOD) increase from organics and sulfate. There is a larger stratospheric influence on radiative forcing (i.e., 21%) relative to AOD (i.e., 12%) because an increase of tropospheric black carbon warms the planet while stratospheric aerosols (including black carbon) cool the planet. Radiative forcing from nonvolcanic stratospheric aerosol mass of anthropogenic origin, including organics, has not been widely considered as a significant influence on the climate system.

Optimized approach to retrieve information on atmospheric carbonyl sulfide (OCS) above the Jungfraujoch station and change in its abundance since 1995

In this paper, we present an optimized retrieval strategy for carbonyl sulfide (OCS), using Fourier transform infrared (FTIR) solar observations made at the high-altitude Jungfraujoch station in the Swiss Alps. More than 200 lines of the ν3 fundamental band of OCS have been systematically evaluated and we selected 4 microwindows on the basis of objective criteria minimizing the effect of interferences, mainly by solar features, carbon dioxide and water vapor absorption lines, while maximizing the information content. Implementation of this new retrieval strategy provided an extended time series of the OCS abundance spanning the 1995–2015 time period, for the study of the long-term trend and seasonal variation of OCS in the free troposphere and stratosphere.Three distinct periods characterize the evolution of the tropospheric partial columns: a first decreasing period (1995–2002), an intermediate increasing period (2002–2008), and the more recent period (2008–2015) which shows no significant trend. Our FTIR tropospheric and stratospheric time series are compared with new in situ gas chromatography mass spectrometry (GCMS) measurements performed by Empa (Laboratory for Air Pollution/Environmental Technology) at the Jungfraujoch since 2008, and with space-borne solar occultation observations by the ACE-FTS instrument on-board the SCISAT satellite, respectively, and they show good agreement. The OCS signal recorded above Jungfraujoch appears to be closely related to anthropogenic sulfur emissions.

Characterization of sulfur deposition over the period of industrialization in Japan using sulfur isotope ratio in Japanese cedar tree rings taken from stumps.

We characterized the sulfur deposition history over the period of industrialization in Japan based on the sulfur isotope ratio (δ(34)S) in tree rings of Japanese cedar (Cryptomeria japonica D. Don) stumps. We analyzed and compared δ(34)S values in the rings from two types of disk samples from 170-year-old stumps that had been cut 5years earlier (older forest stand) and from 40-year-old living trees (younger forest stand) in order to confirm the validity of using stump disks for δ(34)S analysis. No differences in δ(34)S values by age were found between the sample types, indicating that stump disks can be used for δ(34)S analysis. The δ(34)S profile in tree rings was significantly correlated with anthropogenic SO2 emissions in Japan (r=-0.76, p<0.05) and, thus, tree rings serve as a record of anthropogenic sulfur emissions. In addition, the values did not change largely from pre-industrialization to the 1940s (+4.2 to +6.1‰). The values before the 1940s are expected to reflect the background sulfur conditions in Japan and, thus, disks containing rings formed before the 1940s contain information about the natural environmental sulfur, which is useful for biogeochemical studies.

Natural or anthropogenic? On the origin of atmospheric sulfate deposition in the Andes of southeastern Ecuador

Abstract. Atmospheric sulfur deposition above certain limits can represent a threat to tropical forests, causing nutrient imbalances and mobilizing toxic elements that impact biodiversity and forest productivity. Atmospheric sources of sulfur deposited by precipitation have been roughly identified in only a few lowland tropical forests. Even scarcer are studies of this type in tropical mountain forests, many of them mega-diversity hotspots and especially vulnerable to acidic deposition. In these places, the topographic complexity and related streamflow conditions affect the origin, type, and intensity of deposition. Furthermore, in regions with a variety of natural and anthropogenic sulfur sources, like active volcanoes and biomass burning, no source emission data has been used for determining the contribution of each source to the deposition. The main goal of the current study is to evaluate sulfate (SO4- deposition by rain and occult precipitation at two topographic locations in a tropical mountain forest of southern Ecuador, and to trace back the deposition to possible emission sources applying back-trajectory modeling. To link upwind natural (volcanic) and anthropogenic (urban/industrial and biomass-burning) sulfur emissions and observed sulfate deposition, we employed state-of-the-art inventory and satellite data, including volcanic passive degassing as well. We conclude that biomass-burning sources generally dominate sulfate deposition at the evaluated sites. Minor sulfate transport occurs during the shifting of the predominant winds to the north and west. Occult precipitation sulfate deposition and likely rain sulfate deposition are mainly linked to biomass-burning emissions from the Amazon lowlands. Volcanic and anthropogenic emissions from the north and west contribute to occult precipitation sulfate deposition at the mountain crest Cerro del Consuelo meteorological station and to rain-deposited sulfate at the upriver mountain pass El Tiro meteorological station.

Regional climate feedbacks in Central Chile and their effect on air quality episodes and meteorology

Santiago, an emerging megacity of 7 million plus inhabitants has shown great improvement in its air quality reducing PM2.5 concentrations from 69μg/m3 in 1989 to 24μg/m3 in 2013 with a comprehensive air quality management strategy. An operational air quality forecasting model that has shown great potential in predicting air quality episodes is used to establish how the climate A1B scenario can impact the frequency of bad air days. In comparison to 2011, in 2050 extreme air quality episodes will be reduced in 20%. WRF-Chem is used to evaluate the effect of anthropogenic emissions on the regional climate including aerosol radiative feedbacks for October–November 2008. Anthropogenic emissions of sulfur and black carbon show different geographical patterns which result in local cooling (0.2–1°C) in coastal Chile, due to large sources of SO2. Central Chile, where most of the population of the country lives, shows transportation of black carbon emissions into the Andes mountain range, resulting in local warming of 0.4°C. While global forcings may cause regional heating for 2050, reducing current black carbon emissions in Central Chile can reduce anthropogenic warming with immediate benefits to the regional climate, and simultaneously reducing local air pollution.

Boundary layer nucleation as a source of new CCN in savannah environment

Abstract. The South African savannah region is a complex environment of air pollution and natural emissions influenced by a strong seasonal cycle in biomass burning and strong precipitation. However, the scarcity of long-term observations means that the knowledge of controlling aerosol processes in this environment is limited. Here we use a recent dataset of 18 months of aerosol size distribution observations trying to understand the annual cycle of cloud condensation nuclei (CCN). Our observations show that the concentration of CCN-sized particles remains, in line with previous studies, high throughout the year with the highest concentrations during the dry winter and the lowest during the wet summer. During the wet season with reduced anthropogenic and biomass burning primary emissions, this pool of CCN is partly filled by boundary layer nucleation with subsequent growth. The enhanced importance of formation and growth during the wet season is addressed to increased biogenic activity together with enhanced free tropospheric removal decreasing the concentration of pre-existing CCN. During the dry season, while frequent new particle formation takes place, particle growth is reduced due to reduced condensing vapour concentrations. Thus in the dry season particles are not able to grow to sizes where they may act as CCN nearly as efficiently as during the wet season. The observations are compared to simulations by a global aerosol model GLOMAP. To our surprise, the global aerosol model utilized to explain the observations was not capable of re-producing the characteristics of particle formation and the annual CCN cycle, despite earlier good performance in predicting the particle concentrations in a number of diverse environments, including the South African savannah region. While the average yearly CCN concentrations of modelled CCN is close to observed concentrations, the characteristics of nucleation bursts and subsequent growth are not captured satisfactory by the model. Our sensitivity tests using different nucleation parameterizations and condensing organic vapour production rates show that neither of these is likely to explain the differences between observed and modelled nucleation and growth rates. A sensitivity study varying 28 modelling parameters indicates that the main uncertainties in the result are due to uncertainties in biomass burning emissions during the dry season, and anthropogenic sulphur emissions during the wet season, both in terms or emitted mass and particle sizes. The uncertainties appear to be mostly related to uncertainties in primary particle emissions, including the emissions variability not captured by monthly emission inventories. The results of this paper also highlights the fact that deficiencies in emissions estimates may result in deficiencies in particle production fluxes, while the end product such as modelled CCN concentration may be in line with observations.

Climate impacts of ice nucleation

Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present‐day ice crystal number concentrations than in‐situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (−0.06 Wm−2) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm−2. Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 ± 0.10 Wm−2 (1σ uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of −1.6 Wm−2.