T. Butler

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.

Atmospheric oxidation capacity sustained by a tropical forest

Terrestrial vegetation, especially tropical rain forest, releases vast quantities of volatile organic compounds (VOCs) to the atmosphere, which are removed by oxidation reactions and deposition of reaction products. The oxidation is mainly initiated by hydroxyl radicals (OH), primarily formed through the photodissociation of ozone. Previously it was thought that, in unpolluted air, biogenic VOCs deplete OH and reduce the atmospheric oxidation capacity. Conversely, in polluted air VOC oxidation leads to noxious oxidant build-up by the catalytic action of nitrogen oxides (NOx = NO + NO2). Here we report aircraft measurements of atmospheric trace gases performed over the pristine Amazon forest. Our data reveal unexpectedly high OH concentrations. We propose that natural VOC oxidation, notably of isoprene, recycles OH efficiently in low-NOx air through reactions of organic peroxy radicals. Computations with an atmospheric chemistry model and the results of laboratory experiments suggest that an OH recycling efficiency of 40–80 per cent in isoprene oxidation may be able to explain the high OH levels we observed in the field. Although further laboratory studies are necessary to explore the chemical mechanism responsible for OH recycling in more detail, our results demonstrate that the biosphere maintains a remarkable balance with the atmospheric environment.

Assessing future nitrogen deposition and carbon cycle feedback using a multimodel approach: Analysis of nitrogen deposition

n this study, we present the results of nitrogen deposition on land from a set of 29 simulations from six different tropospheric chemistry models pertaining to present-day and 2100 conditions. Nitrogen deposition refers here to the deposition (wet and dry) of all nitrogen-containing gas phase chemical species resulting from NOx (NO + NO2) emissions. We show that under the assumed IPCC SRES A2 scenario the global annual average nitrogen deposition over land is expected to increase by a factor of ∼2.5, mostly because of the increase in nitrogen emissions. This will significantly expand the areas with annual average deposition exceeding 1 gN/m2/year. Using the results from all models, we have documented the strong linear relationship between models on the fraction of the nitrogen emissions that is deposited, regardless of the emissions (present day or 2100). On average, approximately 70% of the emitted nitrogen is deposited over the landmasses. For present-day conditions the results from this study suggest that the deposition over land ranges between 25 and 40 Tg(N)/year. By 2100, under the A2 scenario, the deposition over the continents is expected to range between 60 and 100 Tg(N)/year. Over forests the deposition is expected to increase from 10 Tg(N)/year to 20 Tg(N)/year. In 2100 the nitrogen deposition changes from changes in the climate account for much less than the changes from increased nitrogen emissions.

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.

The influence of megacities on global atmospheric chemistry: a modelling study

Environmental context. Over half of the population of the world now live in urban areas, and the number of so-called ‘megacities’, with populations of ~10 million or more, is growing at a tremendous rate. We show how these patterns of urbanisation have the potential to influence the atmospheric chemical environment on a global scale, particularly through the effects of emissions from megacities on the reactive nitrogen cycle. With the growing worldwide interest in the study of the effects of megacities at all spatial scales, such as current European Union projects MEGAPOLI and CityZen, our study represents the first of many future studies that examine the effects of megacities on atmospheric chemistry on the global scale. Abstract. We present the first study of the effects of megacities on global atmospheric chemistry using a global three-dimensional chemical transport model. The effects on air quality, radiative forcing and atmospheric oxidation capacity are disproportionately smaller than the proportion of anthropogenic emissions due to megacities. Disproportionately large effects of megacities are modelled for reactive nitrogen compounds, in particular PAN (peroxy acetyl nitrate), which has increased in abundance globally by 9% due to megacities under year 2000 conditions, with 23% of the Earth experiencing an increase of 10% or more. These influences decrease under two very different future emission scenarios. Under a low-emission future scenario, the influence of megacities is generally reduced, and under a high-emission future scenario, although the local influence of megacities is increased, the geographical extent of the influence becomes smaller. In our model, the individual grid cells that contain megacities respond to the megacity emissions differently depending on their latitude. Tropical megacity grid cells generally show increased ozone year-round, while northern extratropical megacities generally show reduced ozone year-round. Better parameterisation of the sub-grid effects of megacities is an important issue for future work.

A fully integrated isoprenoid emissions model coupling emissions to photosynthetic characteristics

The lack of a mechanistic basis has hampered modelling isoprene emission responses to environmental drivers, in particular the simulation of isoprene emissions under different CO₂ concentrations. Here, we advance previous semi-mechanistic model formulations by introducing a model that explicitly links electron availability for other purpose than carbon assimilation (or available energy for secondary metabolism processes; supply-constraint) and enzyme activity (capacity-constraint) to emissions. We furthermore investigate the sensitivity of the model to variations in photosynthetic and emission-specific parameters. By comparing species-specific simulations with experimental data, we demonstrate that differences in photosynthetic characteristics can explain inter-species differences in emissions. Interestingly, the seasonal development of emissions could also be explained to some degree by the change in energy supply from photosynthesis throughout the season. In addition, we show that the principal responses are not limited to isoprene but can be formulated to describe the emission of other light-dependent volatile species. The proposed model is suitable for implementation into regional and global models, particularly those that already provide species-specific photosynthesis estimates.

Exploring CO pollution episodes observed at Rishiri Island by chemical weather simulations and AIRS satellite measurements: long-range transport of burning plumes and implications for emissions inventories.

The summer of 2003 was an active forest fire season in Siberia. Several events of elevated carbon monoxide (CO) were observed at Rishiri Island in northern Japan during an intensive field campaign in September 2003. A simulation with a global chemistry-transport model is able to reproduce the general features of the baseline levels and variability in the observed CO, and a source attribution for CO in the model suggests that the contribution from North Asia dominated, accounting for approximately 50% on average, with contributions of 7% from North America and 8% from Europe and 30% from oxidation of hydrocarbons. With consideration of recent emission estimates for East Asian fossil fuel and Siberian biomass burning sources, the model captures the timing and magnitude of the CO enhancements in two pollution episodes well (17 and 24 September). However, it significantly underestimates the amplitude during another episode (11–13 September), requiring additional CO emissions for this event. Daily satellite images from AIRS reveal CO plumes transported from western Siberia toward northern Japan. These results suggest that CO emissions from biomass burning in western Siberia in 2003 are likely underestimated in the inventory and further highlight large uncertainties in estimating trace gas emissions from boreal fires.

Effect of VOC Emissions from Vegetation on Air Quality in Berlin during a Heatwave

The potential of emissions from urban vegetation combined with anthropogenic emissions to produce ozone and particulate matter has long been recognized. This potential increases with rising temperatures and may lead to severe problems with air quality in densely populated areas during heat waves. Here, we investigate how heat waves affect emissions of volatile organic compounds from urban/suburban vegetation and corresponding ground-level ozone and particulate matter. We use the Weather Research and Forecasting Model with atmospheric chemistry (WRF-Chem) with emissions of volatile organic compounds (VOCs) from vegetation simulated with MEGAN to quantify some of these feedbacks in Berlin, Germany, during the heat wave in 2006. The highest ozone concentration observed during that period was ∼200 μg/m3 (∼101 ppbV). The model simulations indicate that the contribution of biogenic VOC emissions to ozone formation is lower in June (9-11%) and August (6-9%) than in July (17-20%). On particular days within the analyzed heat wave period, this contribution increases up to 60%. The actual contribution is expected to be even higher as the model underestimates isoprene concentrations over urban forests and parks by 0.6-1.4 ppbv. Our study demonstrates that biogenic VOCs can considerably enhance air pollution during heat waves. We emphasize the dual role of vegetation for air quality and human health in cities during warm seasons, which is removal and lessening versus enhancement of air pollution. The results of our study suggest that reduction of anthropogenic sources of NOx, VOCs, and PM, for example, reduction of the motorized vehicle fleet, would have to accompany urban tree planting campaigns to make them really beneficial for urban dwellers.

Global reactive nitrogen deposition from lightning NOx

We present results of the deposition of nitrogen compounds formed from lightning (LNO x ) using the global chemical transport Model of Atmospheric Transport and Chemistry?Max Planck Institute for Chemistry version. The model indicates an approximately equal deposition of LNO x in both terrestrial and oceanic ecosystems, primarily in the tropics and midlatitudes open ocean, despite much higher intensities of lightning flashes above landmasses. The highest values of deposition are due to wet convective deposition, with highest values concentrated in the tropical continents. Nonconvective wet deposition, associated with large-scale weather patterns, occurs over large areas of the ocean amid lower values per square meter, manifesting the long-range transport of NO y , including long-lived species such as HNO3 at high altitudes and PAN. Dry deposition is concentrated primarily above landmasses, yet oceanic deposition over wide areas is still observed. Combined together, the total LNO x deposition exhibits maximal influx values over land, whereas oceanic deposition over wider areas renders the integrated deposition over both ecosystems almost identical. Peaks of terrestrial deposition values (located in Africa, South America, and Asia) show seasonal variability by meridionally penetrating the northern or southern midlatitude following the corresponding summer hemisphere, in accordance with the migration of LNO x production sites. On land, wet and dry deposition rates are more or less equal with a small bias toward wet deposition, whereas above the ocean, wet deposition is markedly higher because of a small water uptake efficiency and relatively small surface roughness. Further work of modeling additional species and obtaining more information on different compounds is required