Global radiative forcing of coupled tropospheric ozone and aerosols in a unified general circulation model

Global simulations of sea salt and mineral dust aerosols are integrated into a previously developed unified general circulation model (GCM), the Goddard Institute for Space Studies (GISS) GCM II′, that simulates coupled tropospheric ozone-NO_x-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. The fully coupled gas-aerosol unified GCM allows one to evaluate the extent to which global burdens, radiative forcing, and eventually climate feedbacks of ozone and aerosols are influenced by gas-aerosol chemical interactions. Estimated present-day global burdens of sea salt and mineral dust are 6.93 and 18.1 Tg with lifetimes of 0.4 and 3.9 days, respectively. The GCM is applied to estimate current top of atmosphere (TOA) and surface radiative forcing by tropospheric ozone and all natural and anthropogenic aerosol components. The global annual mean value of the radiative forcing by tropospheric ozone is estimated to be +0.53 W m^(−2) at TOA and +0.07 W m^(−2) at the Earth's surface. Global, annual average TOA and surface radiative forcing by all aerosols are estimated as −0.72 and −4.04 W m^(−2), respectively. While the predicted highest aerosol cooling and heating at TOA are −10 and +12 W m^(−2), respectively, surface forcing can reach values as high as −30 W m^(−2), mainly caused by the absorption by black carbon, mineral dust, and OC. We also estimate the effects of chemistry-aerosol coupling on forcing estimates based on currently available understanding of heterogeneous reactions on aerosols. Through altering the burdens of sulfate, nitrate, and ozone, heterogeneous reactions are predicted to change the global mean TOA forcing of aerosols by 17% and influence global mean TOA forcing of tropospheric ozone by 15%

Projected effect of 2000-2050 changes in climate and emissions on aerosol levels in China and associated transboundary transport

We investigate projected 2000–2050 changes in concentrations of aerosols in China and the associated transboundary aerosol transport by using the chemical transport model GEOS-Chem driven by the Goddard Institute for Space Studies (GISS) general circulation model (GCM) 3 at 4° × 5° resolution. Future changes in climate and emissions projected by the IPCC A1B scenario are imposed separately and together through sensitivity simulations. Accounting for sulfate, nitrate, ammonium, black carbon (BC), and organic carbon (OC) aerosols, concentrations of individual aerosol species change by −1.5 to +0.8 μg m^(−3), and PM_(2.5) levels are projected to change by about 10–20% in eastern China as a result of 2000–2050 change in climate alone. With future changes in anthropogenic emissions alone, concentrations of sulfate, BC, and OC are simulated to decrease because of assumed reductions in emissions, and those of nitrate are predicted to increase because of higher NO_x emissions combined with decreases in sulfate. The net result is a predicted reduction of seasonal mean PM_(2.5) concentrations in eastern China by 1–8 μg m^(−3) (or 10–40%) over 2000–2050. It is noted that current emission inventories for BC and OC over China are judged to be inadequate at present. Transboundary fluxes of different aerosol species show different sensitivities to future changes in climate and emissions. The annual outflow of PM_(2.5) from eastern China to the western Pacific is estimated to change by −7.0%, −0.7%, and −9.0% over 2000–2050 owing to climate change alone, changes in emissions alone, and changes in both climate and emissions, respectively. The fluxes of nitrate and ammonium aerosols from Europe and Central Asia into western China increase over 2000–2050 in response to projected changes in emissions, leading to a 10.5% increase in annual inflow of PM_(2.5) to western China with future changes in both emissions and climate. Fluxes of BC and OC from South Asia to China in spring contribute a large fraction of the annual inflow of PM_(2.5). The annual inflow of PM_(2.5) from South Asia and Southeast Asia to China is estimated to change by −8%, +281%, and +227% over 2000–2050 owing to climate change alone, changes in emissions alone, and changes in both climate and emissions, respectively. While the 4° × 5° spatial resolution is a limitation of the present study, the direction of predicted changes in aerosol levels and transboundary fluxes still provides valuable insight into future air quality

Climatic effects of 1950-2050 changes in US anthropogenic aerosols - Part 2: Climate response

We investigate the climate response to changing US anthropogenic aerosol sources over the 1950–2050 period by using the NASA GISS general circulation model (GCM) and comparing to observed US temperature trends. Time-dependent aerosol distributions are generated from the GEOS-Chem chemical transport model applied to historical emission inventories and future projections. Radiative forcing from US anthropogenic aerosols peaked in 1970–1990 and has strongly declined since due to air quality regulations. We find that the regional radiative forcing from US anthropogenic aerosols elicits a strong regional climate response, cooling the central and eastern US by 0.5–1.0 °C on average during 1970–1990, with the strongest effects on maximum daytime temperatures in summer and autumn. Aerosol cooling reflects comparable contributions from direct and indirect (cloud-mediated) radiative effects. Absorbing aerosol (mainly black carbon) has negligible warming effect. Aerosol cooling reduces surface evaporation and thus decreases precipitation along the US east coast, but also increases the southerly flow of moisture from the Gulf of Mexico resulting in increased cloud cover and precipitation in the central US. Observations over the eastern US show a lack of warming in 1960–1980 followed by very rapid warming since, which we reproduce in the GCM and attribute to trends in US anthropogenic aerosol sources. Present US aerosol concentrations are sufficiently low that future air quality improvements are projected to cause little further warming in the US (0.1 °C over 2010–2050). We find that most of the warming from aerosol source controls in the US has already been realized over the 1980–2010 period

Effect of Changes in Climate and Emissions on Future Sulfate-Nitrate-Ammonium Aerosol Levels in the United States

Global simulations of sulfate, nitrate, and ammonium aerosols are performed for the present day and 2050 using the chemical transport model GEOS-Chem. Changes in climate and emissions projected by the IPCC A1B scenario are imposed separately and together, with the primary focus of the work on future inorganic aerosol levels over the United States. Climate change alone is predicted to lead to decreases in levels of sulfate and ammonium in the southeast U.S. but increases in the Midwest and northeast U.S. Nitrate concentrations are projected to decrease across the U.S. as a result of climate change alone. In the U.S., climate change alone can cause changes in annually averaged sulfate-nitrate-ammonium of up to 0.61 μg/m3, with seasonal changes often being much larger in magnitude. When changes in anthropogenic emissions are considered (with or without changes in climate), domestic sulfate concentrations are projected to decrease because of sulfur dioxide emission reductions, and nitrate concentrations are predicted to generally increase because of higher ammonia emissions combined with decreases in sulfate despite reductions in emissions of nitrogen oxides. The ammonium burden is projected to increase from 0.24 to 0.36 Tg, and the sulfate burden to increase from 0.28 to 0.40 Tg S as a result of globally higher ammonia and sulfate emissions in the future. The global nitrate burden is predicted to remain essentially constant at 0.35 Tg, with changes in both emissions and climate as a result of the competing effects of higher precursor emissions and increased temperature.Engineering and Applied Science

Quantifying the influence of agricultural fires in northwest India on urban air pollution in Delhi, India

Since at least the 1980s, many farmers in northwest India have switched to mechanized combine harvesting to boost efficiency. This harvesting technique leaves abundant crop residue on the fields, which farmers typically burn to prepare their fields for subsequent planting. A key question is to what extent the large quantity of smoke emitted by these fires contributes to the already severe pollution in Delhi and across other parts of the heavily populated Indo-Gangetic Plain located downwind of the fires. Using a combination of observed and modeled variables, including surface measurements of PM2.5, we quantify the magnitude of the influence of agricultural fire emissions on surface air pollution in Delhi. With surface measurements, we first derive the signal of regional PM2.5 enhancements (i.e. the pollution above an anthropogenic baseline) during each post-monsoon burning season for 2012–2016. We next use the Stochastic Time-Inverted Lagrangian Transport model (STILT) to simulate surface PM2.5 using five fire emission inventories. We reproduce up to 25% of the weekly variability in total observed PM2.5 using STILT. Depending on year and emission inventory, our method attributes 7.0%–78% of the maximum observed PM2.5 enhancements in Delhi to fires. The large range in these attribution estimates points to the uncertainties in fire emission parameterizations, especially in regions where thick smoke may interfere with hotspots of fire radiative power. Although our model can generally reproduce the largest PM2.5 enhancements in Delhi air quality for 1–3 consecutive days each fire season, it fails to capture many smaller daily enhancements, which we attribute to the challenge of detecting small fires in the satellite retrieval. By quantifying the influence of upwind agricultural fire emissions on Delhi air pollution, our work underscores the potential health benefits of changes in farming practices to reduce fires

Climatic effects of 1950–2050 changes in US anthropogenic aerosols – Part 1: Aerosol trends and radiative forcing

We use the GEOS-Chem chemical transport model combined with the GISS general circulation model to calculate the aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950–2050 period, based on historical emission inventories and future projections from the IPCC A1B scenario. The aerosol simulation is evaluated with observed spatial distributions and 1980–2010 trends of aerosol concentrations and wet deposition in the contiguous US. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that it peaked in 1970–1990, with values over the eastern US (east of 100° W) of −2.0 W m[superscript −2] for direct forcing including contributions from sulfate (−2.0 W m[superscript −2]), nitrate (−0.2 W m[superscript −2]), organic carbon (−0.2 W m[superscript −2]), and black carbon (+0.4 W m[superscript −2]). The aerosol indirect effect is of comparable magnitude to the direct forcing. We find that the forcing declined sharply from 1990 to 2010 (by 0.8 W m−2 direct and 1.0 W m[superscript −2] indirect), mainly reflecting decreases in SO[subscript 2] emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO[subscript 2] emissions have already declined by almost 60 % from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources may have already been realized by 2010, however some additional warming is expected through 2020. The small positive radiative forcing from US BC emissions (+0.3 W m[superscript −2] over the eastern US in 2010) suggests that an emission control strategy focused on BC would have only limited climate benefit

Radiative forcing in the 21st century due to ozone changes in the troposphere and the lower stratosphere

Radiative forcing due to changes in ozone is expected for the 21st century. An assessment on changes in the tropospheric oxidative state through a model intercomparison ("OxComp'') was conducted for the IPCC Third Assessment Report (IPCC-TAR). OxComp estimated tropospheric changes in ozone and other oxidants during the 21st century based on the "SRES'' A2p emission scenario. In this study we analyze the results of 11 chemical transport models (CTMs) that participated in OxComp and use them as input for detailed radiative forcing calculations. We also address future ozone recovery in the lower stratosphere and its impact on radiative forcing by applying two models that calculate both tropospheric and stratospheric changes. The results of OxComp suggest an increase in global-mean tropospheric ozone between 11.4 and 20.5 DU for the 21st century, representing the model uncertainty range for the A2p scenario. As the A2p scenario constitutes the worst case proposed in IPCC-TAR we consider these results as an upper estimate. The radiative transfer model yields a positive radiative forcing ranging from 0.40 to 0.78 W m(-2) on a global and annual average. The lower stratosphere contributes an additional 7.5-9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15-0.17 W m(-2). The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change