Kengo Sudo

Multimodel ensemble simulations of present-day and near-future tropospheric ozone

Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing optimistic, likely, and pessimistic options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of -50, 180, and 300 mW m-2, compared to a CO 2 forcing over the same time period of 800-1100 mW m-2. These values indicate the importance of air pollution emissions in short- to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%. The ensemble mean year 2000 tropospheric ozone budget indicates chemical production, chemical destruction, dry deposition and stratospheric input fluxes of 5100, 4650, 1000 and 550 Tg(O 3 ) yr-1, respectively. These values are significantly different to the mean budget documented by the Intergovernmental Panel on Climate Change (IPCC) Third Assessment Report (TAR). The mean ozone burden (340 Tg(O 3 )) is 10% larger than the IPCC TAR estimate, while the mean ozone lifetime (22 days) is 10% shorter. Results from individual models show a correlation between ozone burden and lifetime, and each models ozone burden and lifetime respond in similar ways across the emissions scenarios. The response to climate change is much less consistent. Models show more variability in the tropics compared to midlatitudes. Some of the most uncertain areas of the models include treatments of deep tropical convection, including lightning NO x production; isoprene emissions from vegetation and isoprenes degradation chemistry; stratosphere-troposphere exchange; biomass burning; and water vapor concentrations. Copyright 2006 by the American Geophysical Union.

Nitrogen and sulfur deposition on regional and global scales: A multimodel evaluation

We use 23 atmospheric chemistry transport models to calculate current and future (2030) deposition of reactive nitrogen (NOy, NHx) and sulfate (SOx) to land and ocean surfaces. The models are driven by three emission scenarios: (1) current air quality legislation (CLE); (2) an optimistic case of the maximum emissions reductions currently technologically feasible (MFR); and (3) the contrasting pessimistic IPCC SRES A2 scenario. An extensive evaluation of the present-day deposition using nearly all information on wet deposition available worldwide shows a good agreement with observations in Europe and North America, where 60–70% of the model-calculated wet deposition rates agree to within ±50% with quality-controlled measurements. Models systematically overestimate NHx deposition in South Asia, and underestimate NOy deposition in East Asia. We show that there are substantial differences among models for the removal mechanisms of NOy, NHx, and SOx, leading to ±1 σ variance in total deposition fluxes of about 30% in the anthropogenic emissions regions, and up to a factor of 2 outside. In all cases the mean model constructed from the ensemble calculations is among the best when comparing to measurements. Currently, 36–51% of all NOy, NHx, and SOx is deposited over the ocean, and 50–80% of the fraction of deposition on land falls on natural (nonagricultural) vegetation. Currently, 11% of the worlds natural vegetation receives nitrogen deposition in excess of the “critical load” threshold of 1000 mg(N) m−2 yr−1. The regions most affected are the United States (20% of vegetation), western Europe (30%), eastern Europe (80%), South Asia (60%), East Asia (40%), southeast Asia (30%), and Japan (50%). Future deposition fluxes are mainly driven by changes in emissions, and less importantly by changes in atmospheric chemistry and climate. The global fraction of vegetation exposed to nitrogen loads in excess of 1000 mg(N) m−2 yr−1 increases globally to 17% for CLE and 25% for A2. In MFR, the reductions in NOy are offset by further increases for NHx deposition. The regions most affected by exceedingly high nitrogen loads for CLE and A2 are Europe and Asia, but also parts of Africa.

Three decades of global methane sources and sinks

Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios-which differ in fossil fuel and microbial emissions-to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.

Multimodel simulations of carbon monoxide: Comparison with observations and projected near-future changes

We analyze present-day and future carbon monoxide (CO) simulations in 26 state-of-the-art atmospheric chemistry models run to study future air quality and climate change. In comparison with near-global satellite observations from the MOPITT instrument and local surface measurements, the models show large underestimates of Northern Hemisphere (NH) extratropical CO, while typically performing reasonably well elsewhere. The results suggest that year-round emissions, probably from fossil fuel burning in east Asia and seasonal biomass burning emissions in south-central Africa, are greatly underestimated in current inventories such as IIASA and EDGAR3.2. Variability among models is large, likely resulting primarily from intermodel differences in representations and emissions of nonmethane volatile organic compounds (NMVOCs) and in hydrologic cycles, which affect OH and soluble hydrocarbon intermediates. Global mean projections of the 2030 CO response to emissions changes are quite robust. Global mean midtropospheric (500 hPa) CO increases by 12.6 ± 3.5 ppbv (16%) for the high-emissions (A2) scenario, by 1.7 ± 1.8 ppbv (2%) for the midrange (CLE) scenario, and decreases by 8.1 ± 2.3 ppbv (11%) for the low-emissions (MFR) scenario. Projected 2030 climate changes decrease global 500 hPa CO by 1.4 ± 1.4 ppbv. Local changes can be much larger. In response to climate change, substantial effects are seen in the tropics, but intermodel variability is quite large. The regional CO responses to emissions changes are robust across models, however. These range from decreases of 10–20 ppbv over much of the industrialized NH for the CLE scenario to CO increases worldwide and year-round under A2, with the largest changes over central Africa (20–30 ppbv), southern Brazil (20–35 ppbv) and south and east Asia (30–70 ppbv). The trajectory of future emissions thus has the potential to profoundly affect air quality over most of the worlds populated areas.

Global premature mortality due to anthropogenic outdoor air pollution and the contribution of past climate change

Increased concentrations of ozone and fine particulate matter (PM2.5) since preindustrial times reflect increased emissions, but also contributions of past climate change. Here we use modeled concentrations from an ensemble of chemistry?climate models to estimate the global burden of anthropogenic outdoor air pollution on present-day premature human mortality, and the component of that burden attributable to past climate change. Using simulated concentrations for 2000 and 1850 and concentration?response functions (CRFs), we estimate that, at present, 470?000 (95% confidence interval, 140?000 to 900?000) premature respiratory deaths are associated globally and annually with anthropogenic ozone, and 2.1 (1.3 to 3.0) million deaths with anthropogenic PM2.5-related cardiopulmonary diseases (93%) and lung cancer (7%). These estimates are smaller than ones from previous studies because we use modeled 1850 air pollution rather than a counterfactual low concentration, and because of different emissions. Uncertainty in CRFs contributes more to overall uncertainty than the spread of model results. Mortality attributed to the effects of past climate change on air quality is considerably smaller than the global burden: 1500 (?20?000 to 27?000) deaths yr?1 due to ozone and 2200 (?350?000 to 140?000) due to PM2.5. The small multi-model means are coincidental, as there are larger ranges of results for individual models, reflected in the large uncertainties, with some models suggesting that past climate change has reduced air pollution mortality.

Simulation of tropospheric ozone changes during 1997–1998 El Niño: Meteorological impact on tropospheric photochemistry

The impact of the 1997–1998 El Nino event on the tropospheric ozone distribution and related processes is assessed by a simulation using a global chemical model. The changes in tropospheric ozone observed during the 1997–1998 El Nino are considered to have been caused by large-scale processes due to the shift in the tropical convection pattern associated with sea surface temperature (SST) changes and by large emissions of ozone precursors due to pronounced biomass burning in the Indonesian region (mainly in Sumatra and Borneo). This simulation study is focused on the effects of meteorological changes caused by the El Nino, aside from the effects of the Indonesian biomass burning. Our simulation results show that about half of the ozone increase observed over the equatorial western Pacific and Indonesia (6–12 Dobson units in tropospheric column ozone) can be explained by the meteorological effects of the El Nino with the remainder attributed to the Indonesian biomass burning, whereas the ozone decrease over the eastern Pacific (4–8 Dobson units) can be attributed to the meteorological effects alone. Moreover, our study suggests that a change in photochemical processes (e.g., water vapor concentration controlling the lifetimes of ozone and other related species, and wet scavenging associated with convective precipitation) also plays an important role in the tropical ozone distribution during the course of the 1997–1998 El Nino event.

Evaluation of long‐term tropospheric NO2 data obtained by GOME over East Asia in 1996–2002

Long-term tropospheric nitrogen dioxide (NO2) column data obtained by the Global Ozone Monitoring Experiment (GOME) (G-NO2) are evaluated to confirm the trends found in tropospheric NO2 abundances over East Asia between 1996 and 2002. For three locations in Central and East Asia, the G-NO2 values are compared with tropospheric columns estimated from coincident observations of total NO2 by ground-based UV/visible spectrometers and stratospheric NO2 by satellite solar occultation sensors (E-NO2). The comparisons show a slight linear drift in G-NO2 data from 1996 to 2002. However, it is much smaller than the standard deviation of the differences between G-NO2 and E-NO2 and much smaller than the increasing trends in NO2 seen by GOME over the industrial areas of China, demonstrating the validity of the trends estimated using the GOME data.

Evaluating ethane and methane emissions associated with the development of oil and natural gas extraction in North America

Sharp rises in the atmospheric abundance of ethane (C2H6)have been detected from2009 onwards in theNorthernHemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight oil reservoirs inNorthAmerica. Using time series of C2H6 total columns derived from groundbased Fourier transform infrared (FTIR) observationsmade atfive selectedNetwork for theDetection of Atmospheric CompositionChange sites, we characterize the recent C2H6 evolution and determine growth rates of∼5% yr atmid-latitudes and of∼3% yr at remote sites. Results fromCAM-chem simulations with theHemispheric Transport of Air Pollutants, Phase II bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C2H6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009.We further estimate thatNorthAmerican anthropogenic C2H6 emissions have increased from1.6 Tg yr −1 in 2008 to 2.8 Tg yr in 2014, i.e. by 75%over these six years.We also completed a second simulation with new top-down emissions of C2H6 fromNorthAmerican oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations ofmethane (CH4) from GreenhouseGasesObserving SATellite. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at themid-latitudinal sites, underscoring the impact of theNorthAmerican oil and gas development on the current C2H6 abundance. Finally we estimate that theNorthAmerican oil and gas emissions of CH4, amajor greenhouse gas, grew from20 to 35 Tg yr −1 over the period 2008–2014, in associationwith the recent C2H6 rise.

Evaluation of methane emissions from West Siberian wetlands based on inverse modeling

West Siberia contains the largest extent of wetlands in the world, including large peat deposits; the wetland area is equivalent to 27% of the total area of West Siberia. This study used inverse modeling to refine emissions estimates for West Siberia using atmospheric CH4 observations and two wetland CH4 emissions inventories: (1) the global wetland emissions dataset of the NASA Goddard Institute for Space Studies (the GISS inventory), which includes emission seasons and emission rates based on climatology of monthly surface air temperature and precipitation, and (2) the West Siberian wetland emissions data (the Bc7 inventory), based on in situ flux measurements and a detailed wetland classification. The two inversions using the GISS and Bc7 inventories estimated annual mean flux from West Siberian wetlands to be 2.9 ± 1. 7a nd 3.0 ± 1. 4T g yr −1 , respectively, which are lower than the 6.3 Tg yr −1 predicted in the GISS inventory, but similar to those of the Bc7 inventory (3.2 Tg yr −1 ). The well-constrained monthly fluxes and a comparison between the predicted CH4 concentrations in the two inversions suggest that the Bc7 inventory predicts the seasonal cycle of West Siberian wetland CH4 emissions more reasonably, indicating that the GISS inventory predicts more emissions from wetlands in northern and middle taiga.

The effect of future ambient air pollution on human premature mortality to 2100 using output from the ACCMIP model ensemble

Ambient air pollution from ground-level ozone and fine particulate matter (PM2.5) is associated with premature mortality. Future concentrations of these air pollutants will be driven by natural and anthropogenic emissions and by climate change. Using anthropogenic and biomass burning emissions projected in the four Representative Concentration Pathway scenarios (RCPs), the ACCMIP ensemble of chemistry-climate models simulated future concentrations of ozone and PM2.5 at selected decades between 2000 and 2100. We use output from the ACCMIP ensemble, together with projections of future population and baseline mortality rates, to quantify the human premature mortality impacts of future ambient air pollution. Future air pollution-related premature mortality in 2030, 2050 and 2100 is estimated for each scenario and for each model using a health impact function based on changes in concentrations of ozone and PM2.5 relative to 2000 and projected future population and baseline mortality rates. Additionally, the global mortality burden of ozone and PM2.5 in 2000 and each future period is estimated relative to 1850 concentrations, using present-day and future population and baseline mortality rates. The change in future ozone concentrations relative to 2000 is associated with excess global premature mortality in some scenarios/periods, particularly in RCP8.5 in 2100 (316 thousand deaths/year), likely driven by the large increase in methane emissions and by the net effect of climate change projected in this scenario, but it leads to considerable avoided premature mortality for the three other RCPs. However, the global mortality burden of ozone markedly increases from 382,000 (121,000 to 728,000) deaths/year in 2000 to between 1.09 and 2.36 million deaths/year in 2100, across RCPs, mostly due to the effect of increases in population and baseline mortality rates. PM2.5 concentrations decrease relative to 2000 in all scenarios, due to projected reductions in emissions, and are associated with avoided premature mortality, particularly in 2100: between -2.39 and -1.31 million deaths/year for the four RCPs. The global mortality burden of PM2.5 is estimated to decrease from 1.70 (1.30 to 2.10) million deaths/year in 2000 to between 0.95 and 1.55 million deaths/year in 2100 for the four RCPs, due to the combined effect of decreases in PM2.5 concentrations and changes in population and baseline mortality rates. Trends in future air pollution-related mortality vary regionally across scenarios, reflecting assumptions for economic growth and air pollution control specific to each RCP and region. Mortality estimates differ among chemistry-climate models due to differences in simulated pollutant concentrations, which is the greatest contributor to overall mortality uncertainty for most cases assessed here, supporting the use of model ensembles to characterize uncertainty. Increases in exposed population and baseline mortality rates of respiratory diseases magnify the impact on premature mortality of changes in future air pollutant concentrations and explain why the future global mortality burden of air pollution can exceed the current burden, even where air pollutant concentrations decrease.