Michael G. Sanderson

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.

When could global warming reach 4°C?

The Intergovernmental Panel on Climate Change (IPCC) Fourth Assessment Report (AR4) assessed a range of scenarios of future greenhouse-gas emissions without policies to specifically reduce emissions, and concluded that these would lead to an increase in global mean temperatures of between 1.6°C and 6.9°C by the end of the twenty-first century, relative to pre-industrial. While much political attention is focused on the potential for global warming of 2°C relative to pre-industrial, the AR4 projections clearly suggest that much greater levels of warming are possible by the end of the twenty-first century in the absence of mitigation. The centre of the range of AR4-projected global warming was approximately 4°C. The higher end of the projected warming was associated with the higher emissions scenarios and models, which included stronger carbon-cycle feedbacks. The highest emissions scenario considered in the AR4 (scenario A1FI) was not examined with complex general circulation models (GCMs) in the AR4, and similarly the uncertainties in climate–carbon-cycle feedbacks were not included in the main set of GCMs. Consequently, the projections of warming for A1FI and/or with different strengths of carbon-cycle feedbacks are often not included in a wider discussion of the AR4 conclusions. While it is still too early to say whether any particular scenario is being tracked by current emissions, A1FI is considered to be as plausible as other non-mitigation scenarios and cannot be ruled out. (A1FI is a part of the A1 family of scenarios, with ‘FI’ standing for ‘fossil intensive’. This is sometimes erroneously written as A1F1, with number 1 instead of letter I.) This paper presents simulations of climate change with an ensemble of GCMs driven by the A1FI scenario, and also assesses the implications of carbon-cycle feedbacks for the climate-change projections. Using these GCM projections along with simple climate-model projections, including uncertainties in carbon-cycle feedbacks, and also comparing against other model projections from the IPCC, our best estimate is that the A1FI emissions scenario would lead to a warming of 4°C relative to pre-industrial during the 2070s. If carbon-cycle feedbacks are stronger, which appears less likely but still credible, then 4°C warming could be reached by the early 2060s in projections that are consistent with the IPCC’s ‘likely range’.

Simulation of Global Hydrogen Levels Using a Lagrangian Three-Dimensional Model

Many previous assessments of the global hydrogen budget have used assumed global averages of temperatures and levels of key reactants to calculate the magnitudes of the various sinks. Dry deposition is by far the largest hydrogen sink but has not been considered in detail in previous estimates of the hydrogen budget. Simulations of hydrogen using a global three-dimensional Lagrangian chemistry-transport model and two different dry deposition schemes were compared with surface measurements. An improved dry deposition scheme which included the effects of soil moisture gave better agreement between the modelled hydrogen levels and surface measurements. The seasonal variation in the hydrogen levels was also simulated much more accurately with the new dry deposition scheme. The model results at high southern latitudes were insensitive to the relative partitioning of the sources between fossil fuel combustion and biomass burning. The results indicate a global mean hydrogen dry deposition velocity of 5.3×10−4 m s−1 which is lower than the previously used 7×10−4 m s−1.

Impacts of climate change and variability on tropospheric ozone and its precursors

Two coupled climate-chemistry model experiments for the period 1990-2030 were conducted: one with a fixed climate and the other with a varying climate forced by the is92a scenario. By comparing results from these experiments we have attempted to identify changes and variations in physical climate that may have important influences upon tropospheric chemical composition. Climate variables considered include: temperature, humidity, convective mass fluxes, precipitation, and the large-scale circulation. Increases in humidity, directly related to increases in temperature, exert a major influence on the budgets of ozone and the hydroxyl radical: decreasing 03 and increasing OH. Warming enhances decomposition of PAN, releasing NOx, and increases the rate of methane oxidation. Surface warming enhances vegetation emissions of isoprene, an important ozone precursor. In the changed climate, tropical convection generally reduces, but penetrates to higher levels. Over northern continents, convection tends to increase. These changes in convection affect both vertical mixing and lightning NOx emissions. We find no global trend in lightning emissions, but significant changes in its distribution. Changes in precipitation and the large-scale circulation are less important for composition, at least in these experiments. Higher levels of the oxidants OH and H202 lead to increases in aerosol formation and concentrations. These results indicate that climate-chemistry feedbacks are dominantly negative (less 03, a shorter CH4 lifetime, and more aerosol). The major mode of inter-annual variability in the is92a climate experiment is ENSO. This strongly modulates isoprene emissions from vegetation via tropical land surface temperatures. ENSO is also clearly the dominant source of variability in tropical column ozone, mainly through changes in the distribution of convection. The magnitude of inter-annual variability in ozone is comparable to the changes brought about by emissions and climate changes between the 1990s and 2020s, suggesting that it will be difficult to disentangle the different components of near-future changes.

Regional temperature and precipitation changes under high-end (≥4°C) global warming

Climate models vary widely in their projections of both global mean temperature rise and regional climate changes, but are there any systematic differences in regional changes associated with different levels of global climate sensitivity? This paper examines model projections of climate change over the twenty-first century from the Intergovernmental Panel on Climate Change Fourth Assessment Report which used the A2 scenario from the IPCC Special Report on Emissions Scenarios, assessing whether different regional responses can be seen in models categorized as ‘high-end’ (those projecting 4°C or more by the end of the twenty-first century relative to the preindustrial). It also identifies regions where the largest climate changes are projected under high-end warming. The mean spatial patterns of change, normalized against the global rate of warming, are generally similar in high-end and ‘non-high-end’ simulations. The exception is the higher latitudes, where land areas warm relatively faster in boreal summer in high-end models, but sea ice areas show varying differences in boreal winter. Many continental interiors warm approximately twice as fast as the global average, with this being particularly accentuated in boreal summer, and the winter-time Arctic Ocean temperatures rise more than three times faster than the global average. Large temperature increases and precipitation decreases are projected in some of the regions that currently experience water resource pressures, including Mediterranean fringe regions, indicating enhanced pressure on water resources in these areas.

A multi‐model study of the hemispheric transport and deposition of oxidised nitrogen

Fifteen chemistry-transport models are used to quantify, for the first time, the export of oxidised nitrogen (NOy) to and from four regions (Europe, North America, South Asia, and East Asia), and to estimate the uncertainty in the results. Between 12 and 24% of the NOx emitted is exported from each region annually. The strongest impact of each source region on a foreign region is: Europe on East Asia, North America on Europe, South Asia on East Asia, and East Asia on North America. Europe exports the most NOy, and East Asia the least. East Asia receives the most NOy from the other regions. Between 8 and 15% of NOx emitted in each region is transported over distances larger than 1000 km, with 3–10% ultimately deposited over the foreign regions.

The contribution from shipping emissions to air quality and acid deposition in Europe

Abstract A global three-dimensional Lagrangian chemistry-transport model STOCHEM is used to describe the European regional acid deposition and ozone air quality impacts along the Atlantic Ocean seaboard of Europe, from the SO2, NOx, VOCs and CO emissions from international shipping under conditions appropriate to the year 2000. Model-derived total sulfur deposition from international shipping reaches over 200 mg S m−2 yr−1 over the southwestern approaches to the British Isles and Brittany. The contribution from international shipping to surface ozone concentrations during the summertime, peaks at about 6 ppb over Ireland, Brittany and Portugal. Shipping emissions act as an external influence on acid deposition and ozone air quality within Europe and may require control actions in the future if strict deposition and air quality targets are to be met.

Stomatal conductance changes due to increasing carbon dioxide levels: Projected impact on surface ozone levels

The impact of increasing levels of carbon dioxide on stomatal conductance and surface ozone levels was investigated using a global three-dimensional general circulation model (GCM) coupled to an interactive land surface scheme and a chemistry model. Pre-industrial, present day and doubled present day levels of carbon dioxide were used. This approach was used to examine the sensitivity of modelled surface ozone levels to changes in stomatal conductance via dry deposition. A doubled level of carbon dioxide was found to increase surface ozone levels by between 2 and 8 ppb in all four seasons owing to reduced dry deposition fluxes, although the location and extent of the changes were very different between each season. No change in levels of nitrogen oxides (NO and NO2) was modelled. A similar experiment to examine the same effect on modelled pre-industrial ozone levels showed that the ozone levels over Europe were only slightly smaller (by 1–1.5 ppb) when the CO2 level was decreased from 369 ppm to 280 ppm.

Impact of increasing ship emissions on air quality and deposition over Europe by 2030

A global chemistry-transport model has been used to study the effect of shipping emissions on air quality and ecosystems over Europe, through changes in surface ozone and surface sulphate aerosols, and changes in the deposition of sulphur and oxidised nitrogen. Scenarios are chosen to determine the impact of current (2000) shipping emissions, and the combined impact of changes in land-based and shipping emissions by 2030. The effects of shipping on ozone are small, compared to land-based emissions changes, and can be both positive and negative. Due to the non-linear nature of ozone chemistry, the effects of shipping depend on the magnitude of the emission change, and on the choice of scenario for the land-based emissions. The effects on sulphate aerosol levels and deposition fluxes of sulphate aerosols and oxidised nitrogen species are larger, and are comparable to expected changes in land-based emissions. This is particularly true for SO 2 emissions from shipping. SO 2 has a sufficiently short lifetime that most of the impacts are felt within the European region, although much of that is over the sea. The increase in sulphate aerosols and sulphur deposition due to the SO 2 from shipping will offset 75 % of the benefits in air quality that would be expect from land-based emission controls under the SRES A2 scenario.