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At least 19 records

Global Impacts of Gas-Phase Chemistry-Aerosol Interactions on Direct Radiative Forcing by Anthropogenic Aerosols and Ozone

We present here a first global modeling study on the influence of gas-phase chemistry/aerosol interactions on estimates of anthropogenic forcing by tropospheric O3 and aerosols. Concentrations of gas-phase species and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols in the preindustrial, present-day, and year 2100 (IPCC SRES A2) atmospheres are simulated online in the Goddard Institute for Space Studies general circulation model II' (GISS GCM II'). With fully coupled chemistry and aerosols, the preindustrial, presentday, and year 2100 global burdens of tropospheric ozone are predicted to be 190, 319, and 519 Tg, respectively. The burdens of sulfate, nitrate, black carbon, and organic carbon are predicted respectively to be 0.32. 0.18, 0.01, 0.33 Tg in preindustrial time, 1.40, 0.48, 0.23, 1.60 Tg in presentday, and 1.37, 1.97, 0.54, 3.31 Tg in year 2100. Anthropogenic O3 is predicted to have a globally and annually averaged present-day forcing of +0.22 W m(sup -2) and year 2100 forcing of +0.57 W m(sup -2) at the top of the atmosphere (TOA). Net anthropogenic TOA forcing by internally mixed sulfate, nitrate, organic carbon, and black carbon aerosols is estimated to be virtually zero in the present-day and +0.34 W m(sup -2) in year 2100, whereas it is predicted to be -0.39 W m(sup -2) in present-day and -0.61 W m(sup -2) in year 2100 if the aerosols are externally mixed. Heterogeneous reactions are shown to be important in affecting anthropogenic forcing. When reactions of N2O5, NO3, NO2, and HO2 on aerosols are accounted for, TOA anthropogenic O3 forcing is less by 20-45% in present-day and by 20-32% in year 2100 at mid to high latitudes in the Northern Hemisphere, as compared with values predicted in the absence of heterogeneous gas aerosol reactions. Mineral dust uptake of HNO3 and O3 is shown to have practically no influence on anthropogenic O3 forcing. Heterogeneous reactions of N2Os, NO3, NO2, and HO2 are predicted to have noticeable impacts on anthropogenic aerosol forcing over industrialized areas, leading to 0-2 W m(sup -2) more anthropogenic aerosol cooling in present-day and 2-8 W m(sup -2) more cooling in year 2100 in these areas as compared with forcings calculated in the absence of heterogeneous reactions. Sea salt uptake of SO2 reduces the magnitude of TOA aerosol cooling by 0.5-1 W m(sup -2) over the oceans around 60 N in the present-day and year 2100 scenarios. Near dust sources, mineral dust uptake of SO2 and HNO3 leads to less anthropogenic aerosol cooling by 0.5-1 W m(sup -2) in the present day and 1-2 W m(sup -2) in year 2100.

Liao, Hong↗

Estimation of the Relationship Between Remotely Sensed Anthropogenic Heat Discharge and Building Energy Use

This paper examined the relationship between remotely sensed anthropogenic heat discharge and energy use from residential and commercial buildings across multiple scales in the city of Indianapolis, Indiana, USA. The anthropogenic heat discharge was estimated with a remote sensing-based surface energy balance model, which was parameterized using land cover, land surface temperature, albedo, and meteorological data. The building energy use was estimated using a GIS-based building energy simulation model in conjunction with Department of Energy/Energy Information Administration survey data, the Assessor's parcel data, GIS floor areas data, and remote sensing-derived building height data. The spatial patterns of anthropogenic heat discharge and energy use from residential and commercial buildings were analyzed and compared. Quantitative relationships were evaluated across multiple scales from pixel aggregation to census block. The results indicate that anthropogenic heat discharge is consistent with building energy use in terms of the spatial pattern, and that building energy use accounts for a significant fraction of anthropogenic heat discharge. The research also implies that the relationship between anthropogenic heat discharge and building energy use is scale-dependent. The simultaneous estimation of anthropogenic heat discharge and building energy use via two independent methods improves the understanding of the surface energy balance in an urban landscape. The anthropogenic heat discharge derived from remote sensing and meteorological data may be able to serve as a spatial distribution proxy for spatially-resolved building energy use, and even for fossil-fuel CO2 emissions if additional factors are considered.

Multi-scale↗

Global Scale Attribution of Anthropogenic and Natural Dust Sources and their Emission Rates Based on MODIS Deep Blue Aerosol Products

Our understanding of the global dust cycle is limited by a dearth of information about dust sources, especially small-scale features which could account for a large fraction of global emissions. Here we present a global-scale high-resolution (0.1 deg) mapping of sources based on Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue estimates of dust optical depth in conjunction with other data sets including land use. We ascribe dust sources to natural and anthropogenic (primarily agricultural) origins, calculate their respective contributions to emissions, and extensively compare these products against literature. Natural dust sources globally account for 75% of emissions; anthropogenic sources account for 25%. North Africa accounts for 55% of global dust emissions with only 8% being anthropogenic, mostly from the Sahel. Elsewhere, anthropogenic dust emissions can be much higher (75% in Australia). Hydrologic dust sources (e.g., ephemeral water bodies) account for 31% worldwide; 15% of them are natural while 85% are anthropogenic. Globally, 20% of emissions are from vegetated surfaces, primarily desert shrublands and agricultural lands. Since anthropogenic dust sources are associated with land use and ephemeral water bodies, both in turn linked to the hydrological cycle, their emissions are affected by climate variability. Such changes in dust emissions can impact climate, air quality, and human health. Improved dust emission estimates will require a better mapping of threshold wind velocities, vegetation dynamics, and surface conditions (soil moisture and land use) especially in the sensitive regions identified here, as well as improved ability to address small-scale convective processes producing dust via cold pool (haboob) events frequent in monsoon regimes.

aerosols↗

3-D Atmospheric Modeling of the Global Budget of N2O and its Isotopologues for 1980-2019: The Impact of Anthropogenic Emissions

Nitrous oxide (N2O) is the third most important anthropogenic greenhouse gas (GHG) and a major ozone-depleting substance (ODS). Its main sources include anthropogenic activities (mostly agriculture) and natural emissions from ocean and soils. However, emission estimates for individual sources are highly variable due to uncertainties in N2O lifetime estimates and partitioning among sources. We derive annual global N2O emissions for 1990-2019 using NOAA Global Monitoring Laboratory (GML) surface N2O observations and the N2O lifetime calculated in the NASA GEOS-5 chemistry climate model (CCM). The inferred global mean N2O emissions has gradually increased from ~15.8 TgN/yr in the early 1990s to ~17.8 TgN/yr in the 2010s. This implies that anthropogenic N2O emissions have grown rapidly from ~6.7 TgN/yr in the 1990s to about ~8.7 TgN/yr in the 2010s, a ~30% increase. With specially designed N2O isotopic tracers in 3-D GEOSCCM, we estimate that, on global average, stratospheric enrichment contributes about +7.7‰/yr, +7.6‰/yr, +8.0‰/yr to tropospheric N(sup α)-δ(sup 15), N(sup β)-δ(sup 15), and O-δ(sup 18) budget, respectively. To balance the global mean isotopic signature for pre-industrial terrestrial sources of N(sup α)-δ(sup 15) ~ 6.7‰, N(sup β)-δ(sup 15) ~ -12.6‰, O-δ(sup 18) ~ 35.4‰, our 3-D isotopic budget simulation using the GEOSCCM suggests global mean anthropogenic isotopic signatures in the recent decades are N(sup α)-δ(sup 15) ~ -18‰, N(sup β)-δ(sup 15) ~ -20‰, O-δ(sup 18) ~ 19‰. These anthropogenic isotopic estimates are significantly lighter than results from one-box atmospheric model-based estimates with the largest difference seen for N(sup β)-δ(sup 15). More surface isotopic measurements are needed to better quantify the N2O isotopic signatures.

Nitrous oxide↗

Estimate of the Aerosol Anthropogenic Component and Focusing from Satellite Data

Satellite measurements of aerosol do not contain information on the chemical composition needed to resolve anthropogenic vs. natural aerosol components. Besides, the same chemical species can have natural and anthropogenic origins. However the ability of the new satellite instruments (MODIS, MISR, POLDER) to distinguish fine from coarse aerosols over the oceans, can be used as a signature of the presence of anthropogenic component and used to measure the fraction of the aerosol originating from anthropogenic activity with an uncertainty of 10 percent for aerosol optical thickness larger than 0.1. We develop the methods and investigated it using model calculations (GOCART) and satellite data (MODIS). Preliminary application to 2 years of global MODIS data shows that 0.200.08 of the aerosol optical thickness and radiative effect has anthropogenic origin. The resultant aerosol forcing over cloud free oceans is 1.30.6 W/sq m, larger than model simulations. Further research until the presentation will probably modify these values.

Kaufman, Yoram↗

Monitoring Anthropogenic Disturbance Trends in an Industrialized Boreal Forest with Landsat Time Series

Human transformation of the terrestrial biosphere via resource utilization is a critical impetus for monitoring and characterizing anthropogenic change to vegetation condition. The primary objective of this research was to detect anthropogenic forest disturbance for a recent Landsat time series. A novel combination of an autonomous change detection procedure and spectral classification scheme was applied and tested in a landscape that has undergone significant resource development over the last 30 years. Anthropogenic disturbance was detected with greater than 93% accuracy. Most disturbances were correctly classified as within +/-1 year. The signal of anthropogenic disturbance was significant in the landscape, accounting for more than 91% of all disturbances and 86% of total disturbed area during the 23-year study period. The study demonstrated a robust approach for examining historical disturbance trends related to human-modification of the environment

industrialized↗

Exacerbation of the 2013-2016 Pan-Caribbean Drought by Anthropogenic Warming

The Caribbean islands are expected to see more frequent and severe droughts from reduced precipitation and increased evaporative demand due to anthropogenic climate change. Between 2013 and 2016 the region experienced a "Pan-Caribbean" drought that was the most widespread event since 1950, due in part to El Niño in 2015/2016, but it is unknown whether its severity was exacerbated by anthropogenic climate change. We examine the role of recent warming on this drought, using new high-resolution self-calibrating Palmer Drought Severity Index datasets. Our findings suggest that anthropogenic warming has accounted for ~15-17% of drought severity, and ~7% of the Pan-Caribbean drought's spatial extent. These findings strongly suggest that climate model projected anthropogenic drying in the Caribbean is already underway, with major implications for more than 43 million people living in this region.

Anthropogenic warming↗

Influence of regional anthropogenic changes over Nile region on the climate system during the late Holocene (~2500 years before present)

The societal impacts of climate change during the late Holocene leads to regional anthropogenic changes over the Nile region floodplain and could have acted in tandem with natural factors like major volcanic eruptions on the regional climate system to magnify the local climatic impacts. This study aims to explore and investigate the sensitivity of climatic changes to the regional anthropogenic changes due to various factors over the Nile river floodplains during the late-Holocene (2.5K years before present). The GISS ModelE Earth system model will be used to simulate the various scenarios of regional increasing/decreasing river fraction, changes in vegetation type and cover, along with changes in land surface type against the no-changes scenario in absence of volcanic eruptions. The spatial coverage of the Nile river basin is estimated using the GIS shapefile based on elevation data from Shuttle Radar Topography Mission (SRTM) at 3 Arc-seconds (approx. 90-meter) horizontal resolution. The extent of flooding in the model grid (2.0°x2.5° in latitude and longitude) is estimated using the existing high-resolution (0.125°x0.125°) gridded topographic elevation information and mapped over the Nile river floodplains. This study also focuses on evaluating the NASA GISS ModelE for resolving the climate feedbacks and response on climate system due to anthropogenic changes and volcanic eruptions. It is also aimed to analyze and quantify the impact of various anthropogenic factors over the African monsoon system and rainfall over the region, which feeds the Nile River.

Anthropogenic changes↗

Responses of Compound Daytime and Nighttime Warm-Dry and Warm-H Events to Individual Anthropogenic Forcings

Daytime heat is often associated with reduced soil moisture and cloud cover, while nighttime heat is connected to high humidity and increased cloud cover. Due to these differing mechanisms, compound daytime and nighttime heat events may respond differently to major anthropogenic forcings (greenhouse gases, anthropogenic aerosols, land-use and land-cover change). Here, we use GISS ModelE2.1-G historical single-forcing runs from 1955 to 2014 to examine how individual anthropogenic forcings affect compound heat events—specifically warm daytime and nighttime temperatures compounded with dry precipitation or high humidity conditions. We show that greenhouse gases alone amplify the natural frequency of warm-dry events by 1.5–5 times and warm-humid events by 2–9 times in tropical and extratropical latitudes. Conversely, aerosols and land-use/land-cover change reduce the frequency of these events, resulting in more modest increases and in some regions, declines, in the historical 'all-forcings' scenario. Individually, aerosol effects are stronger and more widespread compared to land-use, oftentimes reducing the natural frequency of these events by 60%–100%. The responses of these compound events are primarily driven by changes in daytime and nighttime temperatures through large-scale warming via greenhouse gases and cooling from aerosols and land-use/land-cover change. However, changes in warm-dry events are amplified in regions with concurrent precipitation declines (e.g. Central America, Mediterranean regions) and warm-humid events are amplified by global concurrent humidity increases. Additionally, we find differences between daytime and nighttime compound responses in the historical experiment that can be traced back to the individual forcings. In particular, aerosols produce a greater cooling effect on daytime relative to nighttime temperatures, which notably results in a historical reduction of Northern Hemisphere daytime warm-dry events relative to natural conditions. Our analysis provides a more comprehensive understanding of the significant impacts of different anthropogenic climate forcings on daytime and nighttime warm-dry and warm-humid events, informing future risk and impact assessments.

Anthropogenic forcings↗

General Circulation Models Simulate Negative Liquid Water Path­–Droplet Number Correlations, but Anthropogenic Aerosols Still Increase Simulated Liquid Water Path

General circulation models' (GCMs) estimates of the liquid water path adjustment to anthropogenic aerosol emissions differ in sign from other lines of evidence. This reduces confidence in estimates of the effective radiative forcing of the climate by aerosol–cloud interactions (ERFaci). The discrepancy is thought to stem in part from GCMs' inability to represent the turbulence–microphysics interactions in cloud-top entrainment, a mechanism that leads to a reduction in liquid water in response to an anthropogenic increase in aerosols. In the real atmosphere, enhanced cloud-top entrainment is thought to be the dominant adjustment mechanism for liquid water path, weakening the overall ERFaci. We show that the latest generation of GCMs includes models that produce a negative correlation between the present-day cloud droplet number and liquid water path, a key piece of observational evidence supporting liquid water path reduction by anthropogenic aerosols and one that earlier-generation GCMs could not reproduce. However, even in GCMs with this negative correlation, the increase in anthropogenic aerosols from preindustrial to present-day values still leads to an increase in the simulated liquid water path due to the parameterized precipitation suppression mechanism. This adds to the evidence that correlations in the present-day climate are not necessarily causal. We investigate sources of confounding to explain the noncausal correlation between liquid water path and droplet number. These results are a reminder that assessments of climate parameters based on multiple lines of evidence must carefully consider the complementary strengths of different lines when the lines disagree.

General circulation models↗

Climate forcing by anthropogenic aerosols

Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol, in particular, has imposed a major perturbation to this forcing. Both the direct scattering of short-wavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

Charlson, R. J.↗

Anthropogenic Sulfate, Clouds, and Climate Forcing

This research work is a joint effort between research groups at the Battelle Pacific Northwest Laboratory, Virginia Tech University, Georgia Institute of Technology, Brookhaven National Laboratory, and Texas A&M University. It has been jointly sponsored by the National Aeronautics and Space Administration, the U.S. Department of Energy, and the U.S. Environmental Protection Agency. In this research, a detailed tropospheric aerosol-chemistry model that predicts oxidant concentrations as well as concentrations of sulfur dioxide and sulfate aerosols has been coupled to a general circulation model that distinguishes between cloud water mass and cloud droplet number. The coupled model system has been first validated and then used to estimate the radiative impact of anthropogenic sulfur emissions. Both the direct radiative impact of the aerosols and their indirect impact through their influence on cloud droplet number are represented by distinguishing between sulfuric acid vapor and fresh and aged sulfate aerosols, and by parameterizing cloud droplet nucleation in terms of vertical velocity and the number concentration of aged sulfur aerosols. Natural sulfate aerosols, dust, and carbonaceous and nitrate aerosols and their influence on the radiative impact of anthropogenic sulfate aerosols, through competition as cloud condensation nuclei, will also be simulated. Parallel simulations with and without anthropogenic sulfur emissions are performed for a global domain. The objectives of the research are: To couple a state-of-the-art tropospheric aerosol-chemistry model with a global climate model. To use field and satellite measurements to evaluate the treatment of tropospheric chemistry and aerosol physics in the coupled model. To use the coupled model to simulate the radiative (and ultimately climatic) impacts of anthropogenic sulfur emissions.

Ghan, Steven J.↗

A Study of the Relationship Between Anthropogenic Sulfate and Cloud Drop Nucleation

The characteristics of the cloud drop size distribution near cloud base are initially determined by the aerosol particles that serve as CCN and by the local updraft velocity. Chemical reactions of the emitted gaseous sulfur compounds due to human activities will alter, through gas-to-particle conversion, the aerosol size distribution, total number, and its chemical composition. Recently, Boucher and Rodhe and Jones et.al have each developed parameterizations relating cloud drop concentration to sulfate mass or aerosol number concentration, respectively, and used them to develop estimates of the indirect forcing by anthropogenic sulfate aerosols. THese parameterizations made use of measure relationships in continental and maritime clouds. However, these relationships are inherently noisy, yielding more than a factor of 2 variation in cloud drop concentration for a given aerosol number (or for a given sulfate mass) concentration. The large spatial and temporal variabilities in the concentration, chemical characteristics, and size distribution of aerosols have made it difficult to develop such a parameterization from data. In this paper, our focus is to develop a means for relating the predicted anthropogenic sulfate mass to cloud drop number concentration over the range of expected conditions associated with continental and marine aerosol. We start with an assumed pre-existing particle size distribution and develop an approximation of the altered distribution after addition of anthropogenic sulfate. We thereby develop a conservative estimate of the possible change in cloud drop number concentration due to anthropogenic sulfate.

Chuang, Catherine C.↗

Future Climate Impacts of Direct Radiative Forcing Anthropogenic Aerosols, Tropospheric Ozone, and Long-lived Greenhouse Gases

Long-lived greenhouse gases (GHGs) are the most important driver of climate change over the next century. Aerosols and tropospheric ozone (O3) are expected to induce significant perturbations to the GHG-forced climate. To distinguish the equilibrium climate responses to changes in direct radiative forcing of anthropogenic aerosols, tropospheric ozone, and GHG between present day and year 2100, four 80-year equilibrium climates are simulated using a unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies (GISS) general circulation model (GCM) 110. Concentrations of sulfate, nitrate, primary organic (POA) carbon, secondary organic (SOA) carbon, black carbon (BC) aerosols, and tropospheric ozone for present day and year 2100 are obtained a priori by coupled chemistry-aerosol GCM simulations, with emissions of aerosols, ozone, and precursors based on the Intergovernmental Panel on Climate Change (IPCC) Special Report on Emissions Scenario (SRES) A2. Changing anthropogenic aerosols, tropospheric ozone, and GHG from present day to year 2100 is predicted to perturb the global annual mean radiative forcing by +0.18 (considering aerosol direct effects only), +0.65, and +6.54 W m(sup -2) at the tropopause, and to induce an equilibrium global annual mean surface temperature change of +0.14, +0.32, and +5.31 K, respectively, with the largest temperature response occurring at northern high latitudes. Anthropogenic aerosols, through their direct effect, are predicted to alter the Hadley circulation owing to an increasing interhemispheric temperature gradient, leading to changes in tropical precipitation. When changes in both aerosols and tropospheric ozone are considered, the predicted patterns of change in global circulation and the hydrological cycle are similar to those induced by aerosols alone. GHG-induced climate changes, such as amplified warming over high latitudes, weakened Hadley circulation, and increasing precipitation over the Tropics and high latitudes, are consistent with predictions of a number of previous GCM studies. Finally, direct radiative forcing of anthropogenic aerosols is predicted to induce strong regional cooling over East and South Asia. Wintertime rainfall over southeastern China and the Indian subcontinent is predicted to decrease because of the increased atmospheric stability and decreased surface evaporation, while the geographic distribution of precipitation is also predicted to be altered as a result of aerosol-induced changes in wind flow.

Chen, Wei-Ting↗

Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols: Aerosol Trends and Radiative Forcing - Part 1

We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of −2.0Wm(exp−2 for direct forcing including contributions from sulfate (−2.0Wm−2), nitrate (−0.2Wm(exp−2), organic carbon (−0.2Wm(exp−2), and black carbon (+0.4Wm(exp−2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp−2) direct and 1.0Wm(exp−2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

climate change↗

Large Contribution from Anthropogenic Warming to an Emerging North American Megadrought

Severe and persistent 21st-century drought in southwestern North America (SWNA) motivates comparisons to medieval megadroughts and questions about the role of anthropogenic climate change. We use hydrological modeling and new 1200-year tree-ring reconstructions of summer soil moisture to demonstrate that the 2000–2018 SWNA drought was the second driest 19-year period since 800 CE, exceeded only by a late-1500s megadrought. The megadrought-like trajectory of 2000–2018 soil moisture was driven by natural variability superimposed on drying due to anthropogenic warming. Anthropogenic trends in temperature, relative humidity, and precipitation estimated from 31 climate models account for 47% (model interquartiles of 35 to 105%) of the 2000–2018 drought severity, pushing an otherwise moderate drought onto a trajectory comparable to the worst SWNA megadroughts since 800 CE.

Anthropogenic warming↗

Impact of Regional Northern Hemisphere Mid-latitude Anthropogenic Sulfur Dioxide Emissions on Local and Remote Tropospheric Oxidants

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.

anthropogenic sulfur dioxide emissions↗

Effect of anthropogenic sulfate aerosols on low-level cloud albedo over oceans

By reducing cloud droplet size, anthropogenic sulfate aerosols are capable of increasing cloud albedo and thus possibly changing the climate. To test the detectability of this effect, we examined satellite-measured low-level cloud albedo off the east coasts of North America and Asia at midlatitudes where anthropogenic sulfate sources are large and aerosols are transported eastward over the oceans by prevailing westerlies. The satellite data demonstrate enhanced cloud albedo near the coastal boundaries where sulfate concentrations are large. Similar trends are absent over ocean regions of the Southern Hemisphere that are removed from anthropogenic sulfate sources.

Kim, Youngseung↗