Anthropogenic Sulfur Dioxide Emissions Research Articles

Variability of sulfur and oxygen isotope values within wet precipitation and its correlation with diminished anthropogenic sulfur dioxide (SO2) emission

Atmospheric sulfate (SO42−) aerosols have the capacity to scatter solar radiation, thus exerting a cooling effect on the climate. It is widely acknowledged that SO42− deposition significantly contributes to ecosystem effect in aquatic and terrestrial environments worldwide. Over the course of several decades, considerable efforts have been undertaken to mitigate anthropogenic sulfur dioxide (SO2) emissions in China, leading to remarkably low SO2 concentrations. Nevertheless, the implications of reduced anthropogenic SO2 emission on atmospheric sulfate transformation and compositions of isotope values (δ34S-SO42–, δ18O-SO42–) remain inadequately understood. To address this knowledge gap, we conducted multiple rainfall sampling instances between 2010 and 2022 (n = 191), encompassing the period of transitioning anthropogenic SO2 emission from high to low levels. Remarkably, we observed a significant reduction in the volume-weighted mean value (VWMV) of SO42− concentrations, declining from 20.86 mg L−1 in 2010 to 2.41 mg L−1 in 2022, and the VWMV of SO42−/NO3− molar ratios also decreased from 12.90 in 2010 to 0.55 in 2022, reflecting the synchronously decreasing annual SO2 emissions and annual SO2 concentrations from 2010 to 2022. In contrast to the declining trends in VWMV of SO42− concentrations, the VWMV of δ34S-SO42– values exhibited a different pattern from 6.6‰ in 2010 to −0.1‰ in 2017 and slightly increased to 2.5‰ in 2022. Furthermore, the VWMV of δ18O-SO42– values demonstrated an increase from 8.8‰ in 2010 to 14.5‰ in 2018, but subsequently decreased to 5.4‰ in 2022. We attributed the sharply dropping VWMV of δ34S-SO42– values to the reduction in the input of primary sulfate with enriched δ34S-SO42– values. The strict desulfurization reduced SO2 emissions, leading to oxidation of these trace SO2 with negative δ34S values, resulting in low sulfate concentrations and negative δ34S-SO42– values. In addition, the monthly average δ18O-SO42– values exhibited a positive correlation with monthly mean δ18O-H2O values (p < 0.05), strongly indicating the water incorporation during SO2 heterogeneous oxidation. More importantly, during spring rainfall, positive δ18O-SO42– values but relatively negative δ34S-SO42– values were influenced by SO2 heterogeneous oxidation facilitated by air oxygen catalyzed under metal ions in dry weather condition, attributed to the low relative humidity (RH) coupled with high deuterium excess (dexcess) values. Conversely, in summer, negative δ18O-SO42– values but relatively positive δ34S-SO42– values resulted from the SO2 heterogeneous oxidation with H2O2 due to high RH and low dexcess values. Moreover, the VWMV of δ18O-H2O exhibited variations from −3.7‰ in 2019 to −9.7‰ in 2021, and displayed a positive correlation with annual temperature (p < 0.01) and a negative correlation with annual precipitation (p < 0.05), making it a valuable indicator of climate change alongside δ18O-SO42– values. Our findings underscore the importance of continued monitoring of atmospheric wet depositions in response to changes in anthropogenic SO2 emission activities. Furthermore, they highlight the substantial impact of variations in δ34S values of SO2 and primary sulfate on rainwater sulfate concentrations and isotope values.

Updating and Evaluating Anthropogenic Emissions for NOAA’s Global Ensemble Forecast Systems for Aerosols (GEFS-Aerosols): Application of an SO2 Bias-Scaling Method

We updated the anthropogenic emissions inventory in NOAA’s operational Global Ensemble Forecast for Aerosols (GEFS-Aerosols) to improve the model’s prediction of aerosol optical depth (AOD). We used a methodology to quickly update the pivotal global anthropogenic sulfur dioxide (SO2) emissions using a speciated AOD bias-scaling method. The AOD bias-scaling method is based on the latest model predictions compared to NASA’s Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA2). The model bias was subsequently applied to the CEDS 2019 SO2 emissions for adjustment. The monthly mean GEFS-Aerosols AOD predictions were evaluated against a suite of satellite observations (e.g., MISR, VIIRS, and MODIS), ground-based AERONET observations, and the International Cooperative for Aerosol Prediction (ICAP) ensemble results. The results show that transitioning from CEDS 2014 to CEDS 2019 emissions data led to a significant improvement in the operational GEFS-Aerosols model performance, and applying the bias-scaled SO2 emissions could further improve global AOD distributions. The biases of the simulated AODs against the observed AODs varied with observation type and seasons by a factor of 3~13 and 2~10, respectively. The global AOD distributions showed that the differences in the simulations against ICAP, MISR, VIIRS, and MODIS were the largest in March–May (MAM) and the smallest in December–February (DJF). When evaluating against the ground-truth AERONET data, the bias-scaling methods improved the global seasonal correlation (r), Index of Agreement (IOA), and mean biases, except for the MAM season, when the negative regional biases were exacerbated compared to the positive regional biases. The effect of bias-scaling had the most beneficial impact on model performance in the regions dominated by anthropogenic emissions, such as East Asia. However, it showed less improvement in other areas impacted by the greater relative transport of natural emissions sources, such as India. The accuracies of the reference observation or assimilation data for the adjusted inputs and the model physics for outputs, and the selection of regions with less seasonal emissions of natural aerosols determine the success of the bias-scaling methods. A companion study on emission scaling of anthropogenic absorbing aerosols needs further improved aerosol prediction.

Modelling the influence of coral-reef-derived dimethylsulfide on the atmosphere of the Great Barrier Reef, Australia

Marine dimethylsulfide (DMS) is an important source of natural sulfur to the atmosphere, with potential implications for the Earth’s radiative balance. Coral reefs are important regional sources of DMS, yet their contribution is not accounted for in global DMS climatologies or in model simulations. This study accounts for coral-reef-derived DMS and investigates its influence on the atmosphere of the Great Barrier Reef (GBR), Australia, using the Australian Community Climate and Earth System Simulator Atmospheric Model version 2 (ACCESS-AM2). A climatology of seawater surface DMS (DMSw) concentration in the GBR and an estimate of direct coral-to-air DMS flux during coral exposure to air at low tide are incorporated into the model, increasing DMS emissions from the GBR region by 0.02 Tg yr-1. Inclusion of coral-reef-derived DMS increased annual mean atmospheric DMS concentration over north-eastern Australia by 29%, contributing to an increase in gas-phase sulfate aerosol precursors of up to 18% over the GBR. The findings suggest that the GBR is an important regional source of atmospheric sulfur, with the potential to influence local-scale aerosol-cloud processes. However, no influence on sulfate aerosol mass or number concentration was detected, even with a reduction in anthropogenic sulfur dioxide emissions, indicating that DMS may not significantly influence the regional atmosphere at monthly, annual or large spatial scales. Further research is needed to improve the representation of coral-reef-derived DMS in climate models and determine its influence on local, sub-daily aerosol-cloud processes, for which observational studies suggest that DMS may play a more important role.

The role of anthropogenic aerosols in the anomalous cooling from 1960 to 1990 in the CMIP6 Earth system models

Abstract. The Earth system models (ESMs) that participated in the sixth Coupled Model Intercomparison Project (CMIP6) tend to simulate excessive cooling in surface air temperature (TAS) between 1960 and 1990. The anomalous cooling is pronounced over the Northern Hemisphere (NH) midlatitudes, coinciding with the rapid growth of anthropogenic sulfur dioxide (SO2) emissions, the primary precursor of atmospheric sulfate aerosols. Structural uncertainties between ESMs have a larger impact on the anomalous cooling than internal variability. Historical simulations with and without anthropogenic aerosol emissions indicate that the anomalous cooling in the ESMs is attributed to the higher aerosol burden in these models. The aerosol forcing sensitivity, estimated as the outgoing shortwave radiation (OSR) response to aerosol concentration changes, cannot well explain the diversity of pothole cooling (PHC) biases in the ESMs. The relative contributions to aerosol forcing sensitivity from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs) can be estimated from CMIP6 simulations. We show that even when the aerosol forcing sensitivity is similar between ESMs, the relative contributions of ARI and ACI may be substantially different. The ACI accounts for between 64 % and 87 % of the aerosol forcing sensitivity in the models and is the main source of the aerosol forcing sensitivity differences between the ESMs. The ACI can be further decomposed into a cloud-amount term (which depends linearly on cloud fraction) and a cloud-albedo term (which is independent of cloud fraction, to the first order), with the cloud-amount term accounting for most of the inter-model differences.

ChAP 1.0: a stationary tropospheric sulfur cycle for Earth system models of intermediate complexity

Abstract. A stationary, computationally efficient scheme ChAP 1.0 (Chemical and Aerosol Processes, version 1.0) for the sulfur cycle in the troposphere is developed. This scheme is designed for Earth system models of intermediate complexity (EMICs). The scheme accounts for sulfur dioxide emissions into the atmosphere, its deposition to the surface, oxidation to sulfates, and dry and wet deposition of sulfates on the surface. The calculations with the scheme are forced by anthropogenic emissions of sulfur dioxide into the atmosphere for 1850–2000 adopted from the CMIP5 dataset and by the ERA-Interim meteorology assuming that natural sources of sulfur into the atmosphere remain unchanged during this period. The ChAP output is compared to changes of the tropospheric sulfur cycle simulations with the CMIP5 data, with the IPCC TAR ensemble, and with the ACCMIP phase II simulations. In addition, in regions of strong anthropogenic sulfur pollution, ChAP results are compared to other data, such as the CAMS reanalysis, EMEP MSC-W, and individual model simulations. Our model reasonably reproduces characteristics of the tropospheric sulfur cycle known from these information sources. In our scheme, about half of the emitted sulfur dioxide is deposited to the surface, and the rest is oxidised into sulfates. In turn, sulfates are mostly removed from the atmosphere by wet deposition. The lifetimes of the sulfur dioxide and sulfates in the atmosphere are close to 1 and 5 d, respectively. The limitations of the scheme are acknowledged, and the prospects for future development are figured out. Despite its simplicity, ChAP may be successfully used to simulate anthropogenic sulfur pollution in the atmosphere at coarse spatial scales and timescales.

Impact of regional Northern Hemisphere mid-latitude anthropogenic sulfur dioxide emissions on local and remote tropospheric oxidants

Abstract. The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.

Aerosol radiative forcings induced by substantial changes in anthropogenic emissions in China from 2008 to 2016

Abstract. Anthropogenic emissions in China play an important role in altering the global radiation budget. Over the past decade, the strong clean-air policies in China have resulted in substantial reductions of anthropogenic emissions of sulfur dioxide (SO2) and primary particulate matter, and air quality in China has consequently improved. However, the resultant aerosol radiative forcings have been poorly understood. In this study, we used an advanced global climate model integrated with the latest localized emission inventory to quantify the aerosol radiative forcings by the changes of anthropogenic emissions in China between 2008 and 2016. By comparing with multiple observation datasets, our simulations reproduced the considerable reductions of sulfate and black carbon (BC) mass loadings reasonably well over eastern China (the key region subject to stringent emission controls) during the period and accordingly showed a clear decline in both aerosol optical depth and absorption aerosol optical depth. The results revealed a regional annual mean positive direct radiative forcing (DRF) of +0.29 W m−2 at the top of the atmosphere (TOA) due to the reduction of SO2 emissions. This positive aerosol radiative forcing was comprised of diminished sulfate scattering (+0.58 W m−2), enhanced nitrate radiative effects (−0.29 W m−2), and could be completely offset by the concurrent reduction of BC emissions that induced a negative BC DRF of −0.33 W m−2. Despite the small net aerosol DRF (−0.05 W m−2) at the TOA, aerosol–radiation interactions could explain the surface brightening in China over the past decade. The overall reductions in aerosol burdens and associated optical effects mainly from BC and sulfate enhanced the regional annual mean downward solar radiation flux at the surface by +1.0 W m−2 between 2008 and 2016. The enhancement was in general agreement with a long-term observational record of surface energy fluxes in China. We also estimated that aerosol effects on cloud radiative forcings may have played a dominant role in the net aerosol radiative forcings at the TOA in China and over the northern Pacific Ocean during the study period. This study will facilitate more informed assessment of climate responses to projected emissions in the future as well as to sudden changes in human activities (e.g., the COVID-19 lockdown).

Increased new particle yields with largely decreased probability of survival to CCN size at the summit of Mt. Tai under reduced SO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; emissions

Abstract. Because anthropogenic sulfur dioxide (SO2) emissions have decreased considerably in the last decade, PM2.5 pollution in China has been alleviated to some extent. However, the effects of reduced SO2 on the particle number concentrations and subsequent contributions of grown new particles to cloud condensation nuclei (CCN) populations, particularly at high altitudes with low aerosol number loadings, are poorly understood. In contrast, the increase in provincial forest areas in China with rapid afforestation over the last few decades expectedly increases the biogenic emissions of volatile organic compounds and their oxidized products as nucleating precursors therein. In this study, we evaluated the campaign-based measurements made at the summit of Mt. Tai (1534 m a.s.l.) from 2007 to 2018. With the decrease in SO2 mixing ratios from 15 ± 13 ppb in 2007 to 1.6 ± 1.6 ppb in 2018, the apparent formation rate (FR) of new particles and the net maximum increase in the nucleation-mode particle number concentration (NMINP) in the spring campaign of 2018 was 2- to 3-fold higher than those in the spring campaign of 2007 with almost the same occurrence frequency of new particle formation (NPF) events. In contrast, the campaign-based comparison showed that the occurrence frequency, in which the maximum geometric median diameter of the grown new particles (Dpgmax) was &gt; 50 nm, decreased considerably from 43 %–78 % of the NPF events before 2015 to &lt; 12 % in 2017–2018. Assuming &gt; 50 nm as a CCN threshold size at high supersaturations, the observed net CCN production decreased from 3.7 × 103 cm−3 (on average) in the five campaigns before 2015 to 1.0 × 103 cm−3 (on average) in the two campaigns in 2017–2018. We argue that the increases in the apparent FR and NMINP are mainly determined by the availability of organic precursors that participate in nucleation and initial growth, whereas the decrease in the growth probability is caused by the reduced emissions of anthropogenic precursors. However, large uncertainties still exist because of a lack of data on the chemical composition of these smaller particles.

Thirty years of the Clean Air Act Amendments: Impacts on haze in remote regions of the United States (1990–2018)

The Clean Air Act Amendments of 1990 were aimed at reducing major environmental threats in the United States, such as acid rain, urban air pollution, toxic air emissions, and regional haze. To this end, there have been major reductions in anthropogenic gaseous emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx). SO2 and NOx are also major contributors to particulate haze, which affects visibility in both urban and rural environments. The Interagency Monitoring of Protected Visual Environments (IMPROVE) network has tracked trends in haze in remote regions of the United States since the late 1980s by reconstructing total light extinction (bext) from speciated particulate concentrations. Regional trends in bext were examined using aggregated data from individual sites. Regional, annual mean short-term trends analyses (2002–2018) indicated strong reductions in bext associated with reduced SO2 and NOx emissions, especially in the eastern United States (−4.3% yr−1, p < 0.001) where haze historically was dominated by sulfate particles. Less improvement occurred in the Intermountain West/Southwest (−0.9% yr−1, p = 0.03) and trends were negative but insignificant along the West Coast (−1.5% yr−1, p = 0.19). On average, across the continental remote United States, bext has decreased at a rate of −2.8% yr−1 (p < 0.001) from 2002 through 2018 and -1.8% yr−1 (p < 0.001) from 1992 through 2018. The composition of haze has shifted away from being sulfate-dominated to having higher contributions from carbonaceous and crustal aerosols. This shift points to the success of combined regulatory activities aimed at reducing anthropogenic emissions over the last three decades. As emissions from regulated sources of SO2 and NOx continue to decline, the contributions to haze from unregulated sources, both anthropogenic and natural, such as oil and gas extraction, international sources, biomass burning, and dust, have increased in importance. Reducing haze from these sources would require additional mitigation strategies and resource management plans.

Organosulfates in Ambient Aerosol: State of Knowledge and Future Research Directions on Formation, Abundance, Fate, and Importance.

Organosulfates (OSs), also referred to as organic sulfate esters, are well-known and ubiquitous constituents of atmospheric aerosol particles. Commonly, they are assumed to form upon mixing of air masses of biogenic and anthropogenic origin, that is, through multiphase reactions between organic compounds and acidic sulfate particles. However, in contrast to this simplified picture, recent studies suggest that OSs may also originate from purely anthropogenic precursors or even directly from biomass and fossil fuel burning. Moreover, besides classical OS formation pathways, several alternative routes have been discovered, suggesting that OS formation possibly occurs through a wider variety of formation mechanisms in the atmosphere than initially expected. During the past decade, OSs have reached a constantly growing attention within the atmospheric science community with evermore studies reporting on large numbers of OS species in ambient aerosol. Nonetheless, estimates on OS concentrations and implications on atmospheric physicochemical processes are still connected to large uncertainties, calling for combined field, laboratory, and modeling studies. In this Critical Review, we summarize the current state of knowledge in atmospheric OS research, discuss unresolved questions, and outline future research needs, also in view of reductions of anthropogenic sulfur dioxide (SO2) emissions. Particularly, we focus on (1) field measurements of OSs and measurement techniques, (2) formation pathways of OSs and their atmospheric relevance, (3) transformation, reactivity, and fate of OSs in atmospheric particles, and (4) modeling efforts of OS formation and their global abundance.

Emission influences on air pollutant concentrations in New York state: II. PM2.5 organic and elemental carbon constituents

Abstract Analyses of 20-year records of emissions and ambient air pollutant concentrations were combined with receptor modeling to enhance current understanding of the relative contributions of different emission source types to fine particle (PM2.5) elemental carbon (EC) and organic carbon (OC) fractions in New York State. Two receptor models, principal component analysis (PCA) and positive matrix factorization (PMF), were applied to determine trends in source contributions to OC and EC at the principal study site, Pinnacle State Park (PSP), between 2001 and 2015. The PSP results are interpreted in relation to state and regional emission and pollutant trends. Multi-site average SO4 concentrations showed a linear relationship to reductions in anthropogenic emissions of sulfur dioxide (SO2) in New York, surrounding states, and eastern Canada from 6.1 million metric tons in 1995 to 1.0 million metric tons in 2015. On average, 0.5 ± 0.1 μg m-3 sulfate (SO4) originated from natural SO2 emissions or from outside the region. Emission-reduction programs yielded measurable reductions of ambient OC, EC, and SO4 concentrations, but OC and EC improvements at PSP were partly offset by increasing concentrations of biomass-burning OC and EC. Between 2001 and 2015, biomass burning contributions increased the PSP 2001–2003 mean EC and OC concentrations by 13–18% and 23–30%, respectively. With decreases in other source contributions, net total reductions of PSP 2001–2003 mean EC and OC concentrations were 36–58% and 26–45%, respectively. Contributions to PSP EC and OC declined from four source types: (1) fossil-fuel combustion associated with SO2, (2) combustion not associated with SO2 (tentatively identified as mobile sources), (3) crustal OC and EC, and (4) sulfate-associated OC and EC. SO2-associated fossil-fuel and biomass-burning OC and EC concentrations were higher in winter, sulfate and non-SO2 combustion OC and EC concentrations were higher in summer, and crustal OC and EC were higher in spring. Spatial and temporal coherence of mean OC and EC concentrations, which was observed as a constant slope of annual-average OC-vs-EC across sites and years, indicates that multiple sites were influenced by similar emission source types and responded similarly to emission reductions during the study period. The lowest mean annual OC and EC concentrations were recorded at the most remote site, Whiteface Mountain Base (WMB), averaging 1.0 ± 0.05 μg m-3 and 0.2 ± 0.01 μg m-3, respectively; these values may represent regional background concentrations.

The Equilibrium Climate Response to Sulfur Dioxide and Carbonaceous Aerosol Emissions From East and Southeast Asia

AbstractWe investigate the equilibrium climate response to East and Southeast Asian emissions of carbonaceous aerosols and sulfur dioxide, a precursor of sulfate aerosol. Using the Community Earth System Model with the Community Atmosphere Model version 5.3, we find that anthropogenic aerosol emissions from East and Southeast Asia exert a global mean net radiative effect of −0.49 ± 0.04 W/m2. Approximately half of this cooling effect can be attributed to anthropogenic sulfur dioxide emissions. The aerosol emissions drive widespread cooling across the Northern Hemisphere. Strong suppression of precipitation occurs over East and Southeast Asia, indicating that anthropogenic aerosol emissions may impact water resources locally. However, in contrast to previous research, we find no clear evidence of remote effects on precipitation over Australia and West Africa. We recommend further investigation of possible remote effects.

Toward Synchronous Evaluation of Source Apportionments for Atmospheric Concentration and Deposition of Sulfate Aerosol Over East Asia

AbstractSource apportionments for atmospheric concentration, dry deposition, and wet deposition of sulfate aerosol (SO42−) were synchronously evaluated over East Asia, a main source of anthropogenic sulfur dioxide (SO2) emissions. Estimating dry deposition was difficult owing to the difficulty of measuring deposition velocity directly; therefore, sensitivity simulations using two dry deposition schemes were conducted. Moreover, sensitivity simulations for different emission inventories, the largest uncertainty source in the air quality model, were also conducted. In total, four experimental settings were used. Model performance was verified for atmospheric concentration and wet deposition using a ground‐based observation network in China, Korea, and Japan, and all four model settings captured the observations. The underestimation of wet deposition over China was improved by an adjusted approach that linearly scaled the modeled precipitation values to observations. The synchronous evaluation of source apportionments for atmospheric concentration and dry and wet deposition showed the dominant contribution of anthropogenic emissions from China to the atmospheric concentration and deposition in Japan. The contributions of emissions from volcanoes were more important for wet deposition than for atmospheric concentration. Differences in the dry deposition scheme and emission inventory did not substantially influence the relative ratio of source apportionments over Japan. Because the dry deposition was more attributed to local factors, the differences in dry deposition may be an important determinant of the source contributions from China to Japan. Verification of these findings, including the dry deposition velocity, is necessary for better understanding of the behavior of sulfur compound in East Asia.

Comment on “Rethinking the Lower Bound on Aerosol Radiative Forcing”

In an influential and interesting study, Stevens (2015) suggested that the global and also Northern Hemispheric warming during the early industrial period implies that the effective radiative forcing [Formula: see text] by anthropogenic aerosols in the year 2000 compared to 1850 cannot be more negative than −1.0 W m−2. Here results from phase 5 of the Coupled Model Intercomparison Project are analyzed and it is shown that there is little relationship between [Formula: see text] and the warming trend in the early industrial period in comprehensive climate models. In particular, some models simulate a warming in the early industrial period despite a strong (very negative) [Formula: see text]. The reason for this difference in results is that the global-mean log-linear scaling of [Formula: see text] with anthropogenic sulfur dioxide emissions introduced and used by Stevens tends to produce a substantially larger aerosol forcing compared to climate models in the first half of the twentieth century, when SO2emissions were concentrated over smaller regions. In turn, it shows smaller (less negative) [Formula: see text] in the recent period with comparatively more widespread SO2emissions.

Chinese province-scale source apportionments for sulfate aerosol in 2005 evaluated by the tagged tracer method

Appropriate policies to improve air quality by reducing anthropogenic emissions are urgently needed. This is typified by the particulate matter (PM) problem and it is well known that one type of PM, sulfate aerosol (SO42−), has a large-scale impact due to long range transport. In this study we evaluate the source–receptor relationships of SO42− over East Asia for 2005, when anthropogenic sulfur dioxide (SO2) emissions from China peaked. SO2 emissions from China have been declining since 2005–2006, so the possible maximum impact of Chinese contributions of SO42− is evaluated. This kind of information provides a foundation for policy making and the estimation of control effects. The tagged tracer method was applied to estimate the source apportionment of SO42− for 31 Chinese province-scale regions. In addition, overall one-year source apportionments were evaluated to clarify the seasonal dependency. Model performance was confirmed by comparing with ground-based observations over mainland China, Taiwan, Korea, and Japan, and the model results fully satisfied the performance goal for PM. We found the following results. Shandong and Hebei provinces, which were the largest and second largest SO2 sources in China, had the greatest impact over the whole of East Asia with apportionments of around 10–30% locally and around 5–15% in downwind receptor regions during the year. Despite large SO2 emissions, the impact of south China (e.g., Guizhou, Guangdong, and Sichuan provinces) was limited to local impact. These results suggest that the reduction policy in south China contributes to improving the local air quality, whereas policies in north and central China are beneficial for both the whole of China and downwind regions. Over Taiwan, Korea, and Japan, the impact of China was dominant; however, local contributions were important during summer.

A new approach for monthly updates of anthropogenic sulfur dioxide emissions from space: Application to China and implications for air quality forecasts

AbstractSO2 emissions, the largest source of anthropogenic aerosols, can respond rapidly to economic and policy driven changes. However, bottom‐up SO2 inventories have inherent limitations owing to 24–48 months latency and lack of month‐to‐month variation in emissions (especially in developing countries). This study develops a new approach that integrates Ozone Monitoring Instrument (OMI) SO2 satellite measurements and GEOS‐Chem adjoint model simulations to constrain monthly anthropogenic SO2 emissions. The approach's effectiveness is demonstrated for 14 months in East Asia; resultant posterior emissions not only capture a 20% SO2 emission reduction in Beijing during the 2008 Olympic Games but also improve agreement between modeled and in situ surface measurements. Further analysis reveals that posterior emissions estimates, compared to the prior, lead to significant improvements in forecasting monthly surface and columnar SO2. With the pending availability of geostationary measurements of tropospheric composition, we show that it may soon be possible to rapidly constrain SO2 emissions and associated air quality predictions at fine spatiotemporal scales.

Long-term temporal trends and spatial patterns in the acid-base chemistry of lakes in the Adirondack region of New York in response to decreases in acidic deposition

We examined the response of lake water chemistry in the Adirondack Mountains of New York State, USA to decreases in acid deposition. Striking declines in the concentrations and fluxes of sulfate and hydrogen ion in wet deposition have been observed since the late 1970s, while significant decreases in nitrate have been evident since the early 2000s. Decreases in estimated dry sulfur and nitrate deposition have also occurred in the Adirondacks, but with no change in dry to wet deposition ratios. These patterns follow long-term decreases in anthropogenic emissions of sulfur dioxide and nitrogen oxides in the U.S. over the same interval. All of the 48 lakes monitored through the Adirondack Long-Term Monitoring program since 1992 have exhibited significant declines in sulfate concentrations, consistent with reductions in atmospheric deposition of sulfur. Nitrate concentrations have also significantly diminished at variable rates in many (33 of 48) lakes. Decreases in concentrations of sulfate plus nitrate (48 of 48) in lakes have driven widespread increases in acid neutralizing capacity (ANC; 42 of 48) and lab pH (33 of 48), and decreases in the toxic fraction, inorganic monomeric Al (45 of 48). Coincident with decreases in acid deposition, concentrations of dissolved organic carbon (DOC) have also increased in some (29 of 48) lakes. While recovery from elevated acid deposition is evident across Adirondack lakes, highly sensitive and impacted mounded seepages lakes and thin till drainage lakes are recovering most rapidly. Future research might focus on how much additional recovery could be achieved given the current deposition relative to future deposition anticipated under the Clean Power Plan, ecosystem effects of increased mobilization of dissolved organic matter, and the influence of changing climate on recovery from acidification.

Regional and global temperature response to anthropogenic SO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; emissions from China in three climate models

Abstract. We use the HadGEM3-GA4, CESM1, and GISS ModelE2 climate models to investigate the global and regional aerosol burden, radiative flux, and surface temperature responses to removing anthropogenic sulfur dioxide (SO2) emissions from China. We find that the models differ by up to a factor of 6 in the simulated change in aerosol optical depth (AOD) and shortwave radiative flux over China that results from reduced sulfate aerosol, leading to a large range of magnitudes in the regional and global temperature responses. Two of the three models simulate a near-ubiquitous hemispheric warming due to the regional SO2 removal, with similarities in the local and remote pattern of response, but overall with a substantially different magnitude. The third model simulates almost no significant temperature response. We attribute the discrepancies in the response to a combination of substantial differences in the chemical conversion of SO2 to sulfate, translation of sulfate mass into AOD, cloud radiative interactions, and differences in the radiative forcing efficiency of sulfate aerosol in the models. The model with the strongest response (HadGEM3-GA4) compares best with observations of AOD regionally, however the other two models compare similarly (albeit poorly) and still disagree substantially in their simulated climate response, indicating that total AOD observations are far from sufficient to determine which model response is more plausible. Our results highlight that there remains a large uncertainty in the representation of both aerosol chemistry as well as direct and indirect aerosol radiative effects in current climate models, and reinforces that caution must be applied when interpreting the results of modelling studies of aerosol influences on climate. Model studies that implicate aerosols in climate responses should ideally explore a range of radiative forcing strengths representative of this uncertainty, in addition to thoroughly evaluating the models used against observations.

Stratospheric aerosol-Observations, processes, and impact on climate

Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

An Anatomy of the Cooling of the North Atlantic Ocean in the 1960s and 1970s

Abstract In the 1960s and early 1970s, sea surface temperatures in the North Atlantic Ocean cooled rapidly. There is still considerable uncertainty about the causes of this event, although various mechanisms have been proposed. In this observational study, it is demonstrated that the cooling proceeded in several distinct stages. Cool anomalies initially appeared in the mid-1960s in the Nordic Seas and Gulf Stream extension, before spreading to cover most of the subpolar gyre. Subsequently, cool anomalies spread into the tropical North Atlantic before retreating, in the late 1970s, back to the subpolar gyre. There is strong evidence that changes in atmospheric circulation, linked to a southward shift of the Atlantic ITCZ, played an important role in the event, particularly in the period 1972–76. Theories for the cooling event must account for its distinctive space–time evolution. The authors’ analysis suggests that the most likely drivers were 1) the “Great Salinity Anomaly” of the late 1960s; 2) an earlier warming of the subpolar North Atlantic, which may have led to a slowdown in the Atlantic meridional overturning circulation; and 3) an increase in anthropogenic sulfur dioxide emissions. Determining the relative importance of these factors is a key area for future work.