Ozone air quality in 2030: a multi model assessment of risks for health and vegetation. K. Ellingsen1 , R. Van Dingenen2, F.J. Dentener2, L. Emberson22, A. Fiore14, M. Schultz4, D.S. Stevenson3, M. Gauss1, M. Amann7, C.S. Atherton8, N. Bell9, D.J. Bergmann8, I. Bey10, T. Butler11, J. Cofala7, W.J. Collins12, R.G. Derwent13, R.M. Doherty1, J. Drevet10, H. Eskes5, D. Hauglustaine15, I. Isaksen1, L. Horowitz14, M. Krol2, J.F. Lamarque16, M. Lawrence11, V. Montanaro17, J.F. Müller18, T. van Noije5, G. Pitari17, M.J. Prather19, J. Pyle6, S. Rast3, J. Rodriguez20, M. Sanderson12, N. Savage6, D. Shindell9, S. Strahan20, K. Sudo21, S. Szopa15, O. Wild21, G. Zeng6 NB Addresses currently don’t match up with numbers next to names. 1. University of Edinburgh, School of Geosciences, Edinburgh, United Kingdom. 2. Joint Research Centre, Institute for Environment and Sustainability, Ispra, Italy. 3. Max Planck Institute for Meteorology, Hamburg, Germany. 4. University of Oslo, Department of Geosciences, Oslo, Norway. 5. Royal Netherlands Meteorological Institute (KNMI), Atmospheric Composition Research, De Bilt, the Netherlands. 6. Frontier Research Center for Global Change, JAMSTEC, Yokohama, Japan. 7. University of Cambridge, Centre of Atmospheric Science, United Kingdom. 8. IIASA, International Institute for Applied Systems Analysis, Laxenburg, Austria. 9. Lawrence Livermore National Laboratory, Atmospheric Science Division, Livermore, USA. 10. NASA-Goddard Institute for Space Studies, New York, USA. 11. Ecole Polytechnique Fédéral de Lausanne (EPFL), Switzerland. 12. Max Planck Institute for Chemistry, Mainz, Germany. 13. Met Office, Exeter, United Kingdom. 14. rdscientific, Newbury, UK. 15. NOAA GFDL, Princeton, NJ, USA. 16. Laboratoire des Sciences du Climat et de l'Environnement, Gif-sur-Yvette, France. 1 17. National Center of Atmospheric Research, Atmospheric Chemistry Division, Boulder, CO, USA. 18. Università L'Aquila, Dipartimento dUniversity of Oslo, Department of Geosciences, Oslo, Norway. 19. Belgian Institute for Space Aeronomy, Brussels, Belgium. 20. Department of Earth System Science, University of California, Irvine, USA 21. Goddard Earth Science & Technology Center (GEST), Maryland, Washington, DC, USA. 22. Stockholm Environment Institute, University of York, Heslington, England. Abstract 1. Introduction High concentrations of the air pollutant ozone (O3) are toxic to many parts of the Earth’s biosphere, and can damage human health, crops and natural ecosystems. WHO [2003] reported that exposure to high ozone levels is linked to respiratory problems, such as asthma and inflammation of lung cells. Ozone may also aggravate chronic illnesses such as emphysema and bronchitis and weaken the immune system. Eventually, ozone may cause permanent lung damage. These effects can be aggravated in children and exercising adults [USEPA, 1999]. Elevated ground level ozone reduces agricultural and commercial forest yields, and increases plant vulnerability to disease, pests, insects, other pollutants and harsh weather [USEPA, 1999; Aunan et al., 2000; Mauzerall and Wang, 2001; Emberson et al., 2003; Wang and Mauzerall, 2004]. Model studies indicate that much of the world’s population and food production areas are currently exposed to dangerously high levels of ozone [West and Fiore, 2005], and that this situation is likely to significantly worsen over the coming century [e.g., Prather et al., 2003]. Despite these major concerns, there has been little research focused on quantifying the risks of future ozone exposure of the global biosphere. Ozone is formed when carbon monoxide (CO) and hydrocarbons are photo-oxidised in the presence of nitrogen oxides and sunlight. Elevated surface ozone levels are therefore 2 closely linked to emissions of CO, NOx, CH4 and other hydrocarbons from the industrial, power generation and transportation sectors. O3 has been considered to be an urban or regional problem connected to local pollution and short-term episodes of peak ozone concentrations. However, there are increasing concerns about transboundary and intercontinental transport of air pollution [e.g., Berntsen et al., 1999; Bey et al., 2001; Li et al., 2002]. The atmospheric lifetime of tropospheric O3 is long enough (1-2 weeks in summer to 1-2 months in winter) to be transported from a polluted region in one continent to another. Long-range transport can elevate the background level of ozone and add to locally or regionally produced ozone, sometimes leading to persistent exceedance of critical levels and air quality standards [e.g., Fiore et al., 2003]. Regional efforts to reduce emissions of ozone precursors could be counteracted by non-regulated processes on a global scale [e.g., Derwent et al., 2004]. Furthermore, recent epidemiological studies have revealed damage to human health not only during high-concentration ozone episodes, but also at much lower concentrations, even at typical present-day Northern Hemisphere background levels (i.e. 30-40 ppbv)[WHO, 2003]. The number of peak-level ozone episodes is currently stable or decreasing in Europe and the U.S. [USEPA, 2004, 2005; EMEP, 2004, 2005; Jonson et al., 2005]. However, in 2002 (or do you mean 2003, with the European heat-wave?) the EU threshold for informing the public (90 ppb) was exceeded in 17 of the 27 reporting countries [EMEP, 2004 (reports on 2002; or 2005 reports on 2003)]. France, Spain and Italy regularly reported hourly peak concentrations in excess of 120 ppb, levels which can cause serious health problems and damage to plants (EMEP). The critical level for agricultural crops (is this 40 ppbv? – based on AOT40 – or is it a flux (was exceeded in 2001) is regularly exceeded at most EMEP-stations in central Europe. The critical level for forest was exceeded in larger parts of central and Eastern Europe (EMEP). Simultaneously, there are strong indications that Northern Hemispheric background ozone levels are increasing [e.g., Staehelin et al., 1994; Simmonds et al., 2004], driven upwards by increases in global emissions of ozone precursors, mainly centered on rapid development in Asia (Martin: maybe a RETRO emissions reference?). 3 Future surface ozone levels will be mainly controlled by the development of emissions of ozone precursors. The implications of the IPCC SRES scenarios [Nakicenovic et al., 2000] on future surface ozone levels were discussed by Prather et al. [2003] indicating that surface ozone in the Northern Hemisphere was likely to increase by about 5 ppbv by 2030 (the range across all the SRES scenarios was 2-7 ppbv) and, under the most pessimistic scenarios, by over 20 ppbv in 2100. Climate change will also contribute to future surface ozone levels through chemistry-climate and emission-climate feedbacks [e.g., Murazaki and Hess, 2005; Sanderson et al., 2003]. Changes in temperature and water vapor will affect chemical conversion rates, and changes in global circulation dynamics may affect transport, mixing and deposition rates, altering important processes that govern the tropospheric distribution of ozone [e.g., Sudo et al., 2003; Zeng and Pyle, 2003; Stevenson et al., 2005]. This study is a part of a wider global model intercomparison ‘PHOTOCOMP-2030’ (Dentener et al, in preparation +submitted?, 2005; Stevenson et al accepted, van Nojie et al in preparation, Shindell D. et al in preparation) coordinated under Integrated Activity 3 of ACCENT (‘Atmospheric Composition Change: the European NeTwork of excellence’). ‘PHOTOCOMP-2030’ focuses on the global atmospheric environment between 2000 and 2030 using over 20 different state-of the-art global atmospheric chemistry models and three different emission scenarios. This paper presents surface ozone results and discusses the development of ozone air quality between 2000 and 2030 using a range of current air quality (AQ) standards with respect to vegetation and human health: AOT40 [Fuhrer et al., 1997], SUM06 [Mauzerall and Wang, 2001], W126 [Lefohn and Runeckles, 1987], the U.S. EPA [USEPA, 1997] and European [WHO, 2000] health standards as well as the recent WHO recommendation SOMO35 [UNECE, 2004]. This is the first study to comprehensively evaluate the possible development of global ozone AQ indices. In the following section, we describe the ozone air quality standards. In section 3, we describe the model simulations that were carried out, before briefly describing some of the participating models in section 4. In section 5 annual mean surface ozone levels are 4 discussed for all scenarios and surface ozone levels for 2000 are compared to observations. We then consider results for the calculated AQ indices for all scenarios, followed by a summary and conclusions in section 6. 2. O3 Air Quality indices 2.1. Vegetation Air Quality indices Ozone concentrations show characteristic diurnal variations (which may differ between e.g. urban, rural, coastal and mountainous locations) and variations over growing seasons, which are related to local and regional climatic conditions. Given these variations, there has been considerable discussion over the last two decades in North America and Europe as to how to summarize the effects on crop yield and forest growth of seasonal ozone exposure in a single index [e.g., Lefohn and Runeckles, 1987; Fuhrer et al., 1997; Mauzerall and Wang, 2001]. Initial analyses of the economic impacts of ozone in the US based on the NCLAN study in open-top chambers used 7h or 12h seasonal mean concentrations to derive exposure-yield relationships for a range of crops, using nonlinear Weibull (what are these?) weighting functions. There is a considerable body of evidence that ozone exposure indices should give greater weight to the higher ozone concentration, with the rationale that the plant’s natural detoxification capacity would negate the effect of lower concentrations. Within this study, three guidelines that account for this phenomenon have been applied at the global scale to provide an indication of risk resulting from ozone exposure to agriculture and forestry. They have been shown to perform well in terms of explaining variation in growth and yield (i.e. AOT40, SUM06 and W126). It is stressed that, since these indices have been developed under US and European conditions, for only a limited number of crop/forest species and crop cultivars they should not be considered to provide definitive risk assessments, neither in their region of origination nor in other regions of the world where different species and cultivars, climate and pollution patterns and management regimes occur. The three guideline indices used here are summarized in Table 1 and Figure 1 [Figure to be included] For all three indices, the hourly values are accumulated over a defined 5 growing season to obtain the exposure index. The AOT40 index (accumulated ozone concentration over a threshold of 40 ppb) is favored in Europe where analysis of experimental data for crops and young trees led to the adoption of this index by the UNECE (2004). A limit AOT40 value of 3 ppm.h (6000 µg/m3.h) for the protection of sensitive crops calculated from May to July during daylight hours is recommended. For forests the limit value is 5 ppm.h (10000 µg/m3.h) accumulated from April to September. In the US, the most widely used indices for risk assessment include SUM06 and W126. SUM06 only considers concentrations above 60ppb and then accumulates the total concentration. The W126 index uses a continuous rather than a step-weighting function, with a sigmoidal distribution, i.e. weights of 0.03, 0.11, 0.30, 0.61 and 0.84 at ozone volume mixing ratios of 40, 50, 60, 70, and 80 ppbv, respectively [cut this and show it in Figure 1?].. Hence, out of the indices discussed here, the AOT40 index implies the lowest threshold for significant effects (strictly speaking, W126 does register non-zero values below 40 ppbv) (Figure 1). For all indices there are some difficulties in applying these guidelines on a global scale. Perhaps the most problematic of these is the definition of the growing season over which the index should be applied. The AOT40 index should be applied over a three month period for agricultural crops and over a six month period for forest trees, respectively. This complicates the application of the index in multi-cropping areas where a number of different crops may be exposed sequentially to ozone episodes which could be causing damage throughout the year; or e.g. an evergreen tropical forest. In this work we assume a worst case scenario by estimating the maximum AOT40 over a consecutive three or six month period as appropriate for the receptor. However, it should be noted that this method will ignore risk to rotation crops grown outside this growth period that may still be subject to substantial ozone exposures. Only daytime ozone contributes to AOT. It should be noted that there is currently some debate both in the US and Europe as to whether elevated ozone levels during the night-time can damage plants both due to observed night-time stomatal opening (ref) in many species as well as to reduce detoxification levels (ref). Therefore, in this work we use the SUM06 index calculated in two ways: over 24 hours and over daylight-only hours (is that what you mean? Table 5 6 definition indicates 24 hours, should be clarified there are 2 ways to calculate); W126 is calculated over 24 hours. Finally, as discussed above, the ozone concentrations making up the indices should be at canopy height, whereas effectively models provided ozone concentrations at various heights. In this respect, the AQ indices resulting from this work may be somewhat overestimated since above-canopy ozone concentrations are probably higher than those at the canopy level. In addition to problems connected with the spatial scale, there are additional uncertainties related to the indices’ ability to represent actual risk for damage by ozone. They can largely be attributed to issues in extrapolation of chamber based experimentally derived dose-response relationships to field conditions. Key to these uncertainties are the modified environmental conditions experienced in chambers, resulting in i) environmental conditions that may enhance ozone uptake (e.g. via reduced atmospheric, boundary layer and stomatal resistance to pollutant transfer) and ii) enhanced ozone concentrations occurring under environmental conditions different to those that might be expected in the field. To address this problem a new “flux-based” approach has recently been adopted in Europe by the UNECE which characterizes ozone in terms of an absorbed dose rather than an ambient concentration, hence incorporating key factors (e.g. species, phenology and environmental conditions) that affect ozone uptake and subsequently modify plant sensitivity to ambient ozone concentrations. These new insights have not yet been adopted for this work. 2.2. Health Air Quality indices Currently, the European Ozone Directive 2002/3/EC EU requires Member States to inform the public when hourly average ozone mixing ratios (concentrations) (this is a bit pedantic, but I got asked to say mixing ratio rather than concentration when I used ppb in the JGR paper) exceed the ‘information’ threshold (i.e. the threshold when the public must be informed?) of 90 ppb (180 μg/m3), whereas an hourly average mixing ratio (concentration) in excess of 120 ppb (240 μg/m3), measured over three consecutive hours, is an ‘alert’ threshold. As a long term objective, the European Ozone Directive has introduced, next to information thresholds, a target value for the protection of human health, defined as a 7 maximum daily eight-hour mean value of 60 ppb (120 µg/m3) not to be exceeded on more than 25 days per year averaged over three years. In the following we will use the abbreviation EU60 as an AQ index indicating the number of days per year exceeding the eight-hour mean 60 ppb threshold. The European target is in line with WHO guidelines [WHO 2000]: “a guideline value for ambient air of 60 ppb (120 µg/m3) for a maximum period of 8 hours per day is established as a level at which acute effects on public health are likely to be small”. It was further considered that the 8-hour guideline would also protect against acute elevated 1-hour exposures. The WHO/CLRTAP Task Force on Health Aspects of Air Pollution has recently recommended a different metric for assessment of policy options [ESC-ECE, 2004], SOMO35 (annual Sum Of daily maximum 8-h Means Over 35 ppb; Table 5). This proposed exposure parameter is defined as the average excess of daily maximum eighthour means over a cut-off level of 35 ppb (70 μg/m3) calculated for all days in a year and is based on the newest insights of epidemiological studies on health effects. In the US, standards have been governed by the consecutive revisions of the Clean Air Act. In 1997, EPA revised and strengthened the ozone NAAQS to change from a standard measured over a 1-hour period (1-hour standard) to a standard measured over an 8-hour period (8-hour standard) [USEPA, 1997]. Previously, the 1-hour standard was 120 ppb. (see e.g. EPA, 2005) http://www.epa.gov/ttn/naaqs/ozone/o3imp8hr/documents/finalrule/NFR_NSR.pdf). If ozone levels from continuous monitoring averaged 120-125 ppb or more over one hour, the threshold is exceeded. A region earned non-attainment status if it exceeded the standard on three days over? three consecutive years. As a consequence, a county with generally good air quality could be labeled a non-attainment area because of one hot summer or some rare meteorological event that caused poor air quality for a brief time. The new U.S. standard lowers the acceptable ozone level to 80 ppb. To smooth out rapid variations, ozone concentrations are averaged over 8-hours. Whether or not the new standard is met is determined by taking the fourth highest 8-hour ozone levels of each 8 year for three consecutive years and averaging these three levels, equivalent to a maximum value of 3 exceedence days per year. A region is designated as a nonattainment area when this three years average exceeds 85 ppbv (80 ppb in Table 5?). In the following we will evaluate the latter US standard with index USEPA80, being the number of days per year the eight-hour-average limit value of 80 ppbv is exceeded. In our work, however, we generally only use one year to calculate the USEPA80 index. Although all based on 8 hourly averages (in contrast to the 1 hourly averages for vegetation) the three health indices focus on different aspects of trends and fluctuations in O3 concentrations: SOMO35 accumulates ozone levels exceeding a ‘background’ level of 35 ppbv. Consequently, this index will be sensitive to regional scale changes in background levels. On the other hand, EU60, and even more so USEPA80, are indicative of high peak levels during O3 episodes. 3. Participating models 20 different global atmospheric chemistry models have participated in the comparison. Four models were set up to run in different configurations giving a total of 25 model configurations described in detail in Table A.1. Thirteen of these models were chemistrytransport models (CTMs) driven by meteorological analyses. Most models used analyses from ECMWF (European Centre for Medium range Weather Forecasting). Twelve models had an underlying global circulation model (GCM) driving the CTMs (eleven different GCMs for twelve GCM-CTMs). The horizontal resolution ranged from 10°x22.5° to 1.8°x1.8°, with one model using a two-way nested grid of 1°x1° over Europe, North-America and Asia. The vertical resolution is highly variable among the models and by altitude. The thickness of the surface layer varies between 18 and 800 meters. The surface ozone levels produced by the models are compared to observations in section 5.a. Comparison of free tropospheric ozone to ozone soundings by Stevenson et al [2005], showed that the model ensemble mean agree well with the observations. A comparison of modeled NO2 columns with the results of three GOME retrieved NO2 9 columns will be given in van Noije et al, in preparation, 2005; nitrate deposition is evaluated by Dentener et al., manuscript in preparation 2005. 4. Experimental setup Five different simulations were performed (Table 1). S1 is the year 2000 reference simulation, whereas simulations S2-S4 use the same meteorological data as S1 and three different 2030 emission cases. The CTMs used meteorological data from year 2000, the GCMs performed 5-10 year simulations with meteorological data for the 1990s. Simulation S5 was performed by GCM-CTM models only, using the emission case of S2 and meteorology for the 2020s. All GCMs were configured as atmosphere-only models with prescribed sea-surface temperature (SSTs) and sea-ice distributions. Most GCMs used values from a simulation of HadCM3 (Hadley Centre Coupled Model, version 3 [Johns et al., 2003]) forced by the IS92a scenario [Leggett el al 1992; Cox et al 2000] for the 2030 climate. Some GCMs used their own climate simulations. Spin-ups of at least 3 months were used for all experiments. Table 2 gives a summary of the simulations performed by the individual models. Gridded anthropogenic emissions on 1˚x1˚ of NOx, CO, NMHC, SO2 and NH3 were specified. In order to reduce the spinning up time, global CH4 mixing ratios were prescribed across the model domain (Table 3). The choice of CH4 values were based on two earlier studies {Dentener, 2005 #1567; Stevenson, 2005 #1588}, together with IPCC recommendations for SRES-A2 [IPCC, 2001- Table II.2.2]. The emissions for the reference year 2000 were based on recent inventories developed by the International Institute for Applied System Analysis (IIASA). The global totals of the future scenarios ‘Current Legislation’ (CLE) and ‘Maximum Feasible Reduction’ (MFR) were developed by IIASA and distributed spatially according to EDGAR3.2 [Olivier et al 2001] as described in [Dentener et al 2005]. To evaluate a high emission case we also used the IPCC SRES A2 (A2) scenario [Nakicenovic et al, 2000]. EDGAR3.2 ship emissions for 1995 [Olivier et al 2001] were added to all scenarios, assuming a 1.5% growth from 1995 to 2030. Satellite-derived monthly-varying biomass-burning 1˚x1˚ 10 gridded distributions [van der Werf et al, 2004] were specified, scaling NOx emissions to those of CO. The values are averages for the period 1997-2002 and were used for all future scenarios as we felt that any other assumption would be highly speculative. The global totals for both the reference year and the future scenarios are reported in Table 3. In addition, aircraft emission totals of 0.8 Tg N/year for the year 2000 and 1.7 Tg N/year (all 2030 cases) and NASA {Isaksen, 1999 #1463} or ANCAT distributions [Henderson et al 1999] were recommended. Recommendations given on natural emissions are reported in Table 4. Lightning and soil NOx emissions were requested to be approximately 5 and 7 Tg (N)/year respectively. Modelers used values in the range of 3.7-7.0 Tg(N)/year for lightning and 5.5-8.0 Tg(N)/year for soil emissions. A total annual emission of 512 Tg/year isoprene [Guenther et al, 1999] were recommended, values in the range of 260-631 TgC/year were used. The NMHC totals were recommended distributed among individual species using the specification given by [Prather et al 2001, Table 4.7]. Species not included in the model were either ignored or lumped into higher species. Height distributions for biomass burning (boundaries at 0, 0.1, 0.5, 1.0, 2.0, 3.0 and 4.0 km) [van der Werf et al, 2004] and industrial emissions (height range 100-300 m) were recommended. However, some models added emissions to the lowest model layer only, whereas GMI, IASB, TM4, TM5 and OsloCTM2 used the recommendations for industrial emissions. These models as well as GFDL-MOZ2, LLNL-IMPACT and MOZECH also used the recommended height profile for biomass burning. The modelers provided hourly O3 surface concentrations. This allows, for the first time, a evaluation of the global distribution of various O3 air quality indices which are based on the accumulation of hourly (or 8-hourly) averaged concentrations above a given threshold (see section 5.3 below). 11 This work focuses on the use of the mean of the ensemble, however also individual model results were analysed. Individual model results were interpolated to 1°x1° and averaged to give the model ensemble mean values. Use of an ensemble should improve the robustness of model results, as individual model errors are likely to cancel, whereas the real signal should reinforce [e.g., Cubasch et al., 2001]. The standard deviation of the mean results gives an indication on the uncertainty. Stevenson et al (2005) tested the robustness of the computation of an ensemble mean by removing “outliers” from the model ensemble and found little influence on the mean. We assume the entire ensemble to represent the most robust method to assess future levels of ozone and to quantitatively assess uncertainties. 5. Model treatment of surface ozone All models reported surface ozone values from the mid-point of the first layer. In stable meteorological conditions the thickness of the model’s surface layer will strongly influence the vertical ozone gradient; especially when simultaneous NO emissions from surface sources are present. In this respect we note that probably the best reference level for comparing model results with ozone measurements and for calculating AQ indices would be around 5-10 m above the surface or at canopy level. Unfortunately, there is no straight-forward method to correct ozone computed at the model’s mid-level to this altitude. 6. Results 6.1. Annual mean surface ozone Figure 1a shows ensemble means and standard deviations of annually-averaged surface ozone. The model ensemble comprises all 25 models (Table 2). The calculated annual average surface O3 varies between 40 and 50 ppb over industrialized parts of NorthAmerica, Southern Europe, and Asia, south of 40°N. The Northern Hemisphere average 12 is found to be 33.7±3.8 ppb. The Southern Hemisphere average is calculated to be 23.7±3.8 ppb, with background values of 15-25 ppb and somewhat higher values (35-40 ppb) in biomass burning areas in Africa and Latin America. Figure 1b, 1c, 1d and 1e display the changes of annual-mean surface ozone for CLE (S2), MFR (S3), SRES A2 (S4) and CLE2030c (S5), respectively. The CLE scenario (Figure 1b) would stabilize O3 approximately at its 2000 levels by the year 2030 in large parts of North America, Europe and Asia. In areas where large increases in emissions from transport and power generation are expected, we see an increase in surface O3 levels, e.g. increases in the range of 5 ppb over South-East Asia and 10-15 ppb over the Indian subcontinent. Background O3 increases by 2-4 ppbv in the tropical and mid-latitude NH, related to the interaction of the increasing concentrations of CH4 and the worldwide increase of emissions of NOx, CO, and NMHCs. The MFR scenario (Figure 1c) demonstrates the effects of maximal implementation and use of currently available technologies to reduce emissions of ozone precursors. Ozone surface levels are reduced by 5-10 ppb in industrial areas, e.g. in large parts of North America, Southern Europe, the Middle East and Southern Asia. As in earlier studies [Prather et al. 2001] the SRES A2 scenario (Figure 1d) leads to worldwide increases in surface ozone levels with an average increase of 4.3 ppb. The largest increases (5-20 ppb) are seen in Southern parts of USA, Latin-America, Africa and South Asia. The change in tropospheric ozone abundancies due to climate change was discussed in Stevenson et al 2005. A slight decrease in tropospheric ozone was found in the lower troposphere, whereas increased stratospheric influx of ozone lead to an increase in the NH upper troposphere and reduced stratospheric influx lead to a decrease in SH the upper troposphere. For surface ozone, the effect of climate change (Figure 1e) is a reduction of 0.5-2 ppb over the ocean. Continental surface ozone levels are reduced by up to 1 ppb in remote regions. Increased temperature and water vapor leads to more OH and tend to 13 decrease ozone, especially over clean regions. Surface ozone levels over polluted areas in the ensemble mean model are increased by up to 0.7 ppb. 6.2. Comparison to observed surface ozone levels for year 2000 Figure 2 compares observed and model ensemble monthly mean surface ozone levels in selected regions [Figure xx] for year 2000. The model ensemble comprises all 25 models (Table 2). Modelled surface ozone levels were averaged over the land area of the respective regions (Table 7). The variation in the model ensemble mean is illustrated including the model maximum and minimum values as well as standard deviations. The observations are averages over data from several observational sites. The European data are from EMEP (Co-operative programme for monitoring and evaluation of the longrange transmissions of air pollutants in Europe (EMEP), http://www.nilu.no/projects/ccc/emepdata.html ) and Airbase (European Topic Centre on Air and Climate Change, Topic Centre of European Environment Agency, Airbase dataset through AirView, http://air- climate.eionet.eu.int/databases/airbase/airview/index.html ), including 100 observational sites for Central Europe and 22 stations for the Central Mediterranean. The US data (Clean Air Status and Trends Network (CASTNET), http://www.epa.gov/castnet/ozone.html) includes up to 13 different stations in each of the three regions (South East USA, South West USA and Great Lakes). The Central-West African data (Carmichael et al. 2003) includes 3 observational sites and the south-African data (Zunckel et al. 2004) covers 6 observational sites. The Indian data (Lal et al. 2000, Nair et al. 2002, Debaje et al. 2003, Naja and Lal 2002, Naja et al. 2003, Carmichael et al. 2003) represent 6 (North-India) and 4 (South India) stations. Central-East Asian data are taken from Carmichael et al., 2003 (3 sites). Northern China (http://gaw.kishou.go.jp/wdcgg.html, Akimoto and Pochanart (personal communication, 2004), Wang and Mauzerall 2004, Carmichael et al., 2003) is represented by 8 sites and the Middle East by a single station (Carmichael et al., 2003). 14 The model ensemble is well representing the observed surface ozone levels in Northern Europe, and the United States. The discrepancy is larger in other regions such as the Middle East, Central West Africa and India. {I would propose to insert a figure with the regions indicated by rectangles, for the clarity.RVD} For South-West USA (30°N-40°N/125°W-110°W) the mean model closely resembles the observations within one standard deviation, whereas the model ensemble overestimates the observations by 5-15 ppb in South-East USA (25°N-35°N/90°W-80°W). The model ensemble represents the winter time and early spring values in the Great Lakes area (40°N-50°N/95°W-75°W) very well, but overestimates summertime ozone by about 10 ppbv. In the Central Mediterranean (35°N-45°N/5E-30E), the model ensemble mean is <10 ppbv higher than the observed average. The model ensemble mean is within one standard deviation of the observed monthly means, with except for the summertime maximum which is overestimated by 15 ppb. For Central Europe (48°N-54°N/7°E-17°E) the mean model closely resembles the winter and early spring observations, whereas the summer and autumn observations are overestimated by about 6-13 ppb. The model ensemble values for the African regions are generally too high. The Central West African (5°N-15°N/5°W-15°E) model ensemble is about 15 ppbv too high in the wet season and up to 20-30 ppb in the dry biomass burning season. The overestimation 15 of ozone in central Africa could be partly due to an overestimation of NOx biomass burning emissions. Indeed Andreae (personal communication, 2005) has revised the emission factor for NO emissions from savannah fires which was used in this study, with approximately -30 %. In southern Africa, the model overestimation is 10-20 ppb with the largest discrepancy around the SH spring ozone maximum; possibly the overestimation of ozone is related to an underestimation of the NO2 column by a factor of 2-3 in this region (Van Noije, in preparation, 2005); effectively leading to titration of ozone in high NOx conditions. The model ensemble fails to describe the observed seasonal cycle for the Middle East (30°N-40°N/30°E-55°E), and generally overestimates ozone by up to 25 ppb. It should be noted however that the Middle East is represented by a single observational site at high altitude (Camkoru, Turkey, 1350 m asl), whereas the model ensemble regional mean is dominated by high emissions related to oil-activity. For the Indian sub-continent (North India, 20N-30N/70E-90E, and South India, 10N-20N/75N-85N) the mean model ensemble are generally 15-20 ppb higher than the observational average. The discrepancy is highest (25 ppb) for the summer hemisphere in South-India. The observational average includes three coastal stations, which may have a higher content of clean air from the ocean compared to the regional average. The South-East Asian (20N-35N/110E-125E) model values are generally within one standard deviation of the observational average with exception for the monsoon season (June to August) where the model overestimates ozone by 20-25 ppb compared to the observations of one single station available for that period. The strong decrease in measured surface ozone levels during the monsoon transports ozone poor air into the region is a feature which is not resolved by the models. Finally, for Northern China and Japan (35N-45N/110E-145E), the model ensemble mean represents the observational average well being within one standard deviation. The model ensemble mean generally underestimates the observational average by 5-7 ppb, but overestimates ozone in July and August by 7 ppb. 16 We will further discuss possible reasons for the discrepancies and consequences for this work in section xx. 5.3. O3 Air Quality indices The 18 model configurations which provided hourly surface ozone values are shown in bold face in Table 2. AQ indices defined in Table 6 and 7 were calculated based on local time values. We focus on the analysis of the AQ indices for 14 selected regions given in Table 7 or Figure xx. These regions were chosen as a convolution of regions with high population density, expected high surface ozone and NO2 columns. The regional values are calculated as land-only averages. 5.3.1 Health Air Quality indices S1, Year 2000 Elevated values for SOMO35, EU60 and USEPA80 are found in industrialized areas, e.g. Southern USA, Southern Europe and South-East Asia due to emissions of ozone precursors from transport, industry and power generation exposing the population to health risk. Since the three indices are based on different thresholds, a somewhat different geographical pattern shows for the three indices. SOMO35 has high values in the southern parts of USA, Southern Europe, Central-West Africa and southern parts of the Asian continent. The EU and USEPA80 indices display high values in the same areas but with larger variations/gradients. The white line in Figure 3a and 3b shows the EU60 and USEPA80 thresholds for health risk, 25 days exceeding 60, and 3 days 80 ppb respectively. Figure 3b-c shows that the EU60 ozone standard is exceeded over larger areas than the USEPA80 standard, e.g. the EU60 threshold for health risk is exceeded in central Europe, whereas the USEPA80 index is within recommended thresholds. As illustrated in Figure 5a, the EU60 and USEPA80 limit values are surpassed in most of the 14 selected regions. According to our ensemble model calculations, the EU60 index is exceeded in South-Eastern USA during 105±58 days and 19±18 days for the USEPA80 17 limit. Other regions at risk are southern-India (89±58 days for EU60 and 9±22 for EPA80) and the Mediterranean (75±46 days for EU60 and 12±18 days for USEPA80). Of the 14 selected regions, only Australia has EU60 and USEPA80 indices below the recommended thresholds. The southern hemisphere average is 17±8 days (EU60) and 5±4 days (USEPA). The northern-hemisphere values are 32±16 days (EU60) and 4±3 days (USEPA). The higher SH USEPA80 index reflects that we find the highest most values in Africa and South-America due to biomass burning (Figure 3c). The highest SOMO35 index of 6822 ppb.days is found in south-eastern USA. The central Mediterranean, North-India, southern-India and the Middle-East all have values exceeding 5000 ppb.days. Relatively, high values are also found in S.W. USA, S.E. Asia and Northern China. The global average is 2619±910 ppb.days, the SH average is 1446±589 ppb.days and the NH average is 3172±1125 ppb.days. Australia and LatinAmerica are the only regions with SOMO35 values lower than 2500 ppb.days (Figure 5a). Australia and Latin-America are the only analysed regions with SOMO35 values lower than 2500 ppb.days (Figure 5a). Figure 6 shows the correlation of SOMO35 with EU60 and EPA80 based on the regionally averaged of air quality indices in Figure 5. SOMO35 and EU60 are well correlated for the regions considered (R² = 0.95). Although for SOMO35 no limit level is established, the good correlation leads to a correspondence of the EU60 threshold of 25 days with SOMO35 ~2500 ppb.days, whereas the number of days exceeding 60 ppb becomes zero at a SOMO35 value of 900 ppb.days. The correlation between SOMO35 and EPA80 is less strong (R² = 0.56); but we tentatively estimate that the 3 day threshold of EPA80 corresponds roughly with SOMO35~2000-2500 ppb.days. As most of the 14 regions are found not to be in compliance with the limit values of EU60 (25 days), EPA80 (3 days) or SOMO35 (≈2500 ppb days), we explored to which extent these regions would be compliant with somewhat less stringent regulations. Figure 5 indicates where limit values are exceeded by a factor of 3 (i.e. EU60>75 days, 18 EPA80>9 days, and SOMO35>5500 ppb.days, the latter value being consistent with the EU60 limit). Two regions would be exposed to ozone surpassing the 3xSOMO35 limit, whereas 5 and 7 regions would be non-conform with respect to 3xEU60 and 3xUSEPA80 limits respectively. The standard deviation for the computed EU60 and especially USEPA80 are much larger than for SOMO35 (Figure 5a). This reflects the higher consistency amongst the models in prediction of average ozone levels exceeding background values and the larger uncertainty connected with prediction of peak ozone levels. Therefore SOMO35 seems to be the most robust indictor for ozone air quality for our ensemble of global model calculations. Ozone health indices in 2030: scenario S2-S4 Figure 5b-d give the changes in the three air quality indices for cases S2 to S4 compared to S1 for the 14 selected regions. S2, Current Legislation (CLE) scenario CLE leads to a general increase in the computed health indices, with highest increases on the northern hemisphere and in particular over the Indian sub-continent. The SOMO35 index increases with 23% on the NH and with 15% on the SH. The increase over India is 60% or approximately 3400 additional ppb.days. The increase of background ozone (as indicated by SOMO35) is in general paired with increased peak ozone values (indicated by EU60 and USEPA80). Averaged over the continental northern hemisphere, the EU60 index augments with 47 % while the southern hemisphere is subject to a smaller change of 12%. The change is not uniformly distributed: we find the largest increase in 2030 over India with approximately 100 additional days of exceedence, a doubling compared to S1, which means that EU60 is exceeded during 215 and 180 days in North and South India, respectively. Opposed to the 19 general trend, there is a small decrease over the central Mediterranean (-3%) and central Europe (-15%) giving Central European values below the threshold for health risk. Considering the USEPA80 index, we find again dramatic increases over the Indian subcontinent, amounting to 320% and 400% over the northern- and southern India respectively giving a total of 34 and 27 days of excess. European values are decreased, giving 9 days of exceedence for the Central Mediterranean and central European values below the threshold for health risk. Europe is an interesting policy relevant case: according to the conventional EU60 and USEPA80 indices, air quality is improved in the CLE scenario, explained by imposed reductions in anthropogenic emissions. However, the European SOMO35 index is found to increase, caused by a continued increase in European background ozone values due to the increased global emissions of ozone precursors and intercontinental transport. This is contradictory to the general SOMO35 – EU60 correlation established before, showing that the change of indices is not necessarily coupled in all cases. Following our previous analysis, in 2030 CLE the “3x threshold” limits are exceeded in 7; 6 and 9 regions, for SOMO35, EU60 and EPA80, respectively (Figure 5). The relatively “clean” regions are mostly limited to the extra-tropics, where photochemistry is less intense. In the analysis above we have to consider the potentially large discrepancy with measurements which will be further discussed in section ?? S3, maximum feasible reduction (MFR) scenario The MFR scenario leads to a worldwide improvement of ozone air pollution. The global distribution for SOMO35 and EU60 are shown in Figure 4. Regional averages are represented in Figure 5c. The largest reductions appear in polluted areas, i.e. southern parts of USA, southern Europe, the Middle East, India and South-east Asia in response to the reduced anthropogenic emissions of ozone precursors. Reductions in SOMO35 are more than 40% over S.W. and S.E. USA, Central Mediterranean, the Middle East and S.E. Asia. SOMO35 in the most polluted regions is generally not exceeding 4000 20 ppb.days. The highest values are found over Northern-India (4541 ppb.days) and S.E. USA (3639 ppb.days). Also for the EU60 and USEPA80 indices (not shown), there is a clear reduction in the area surpassing the recommended threshold of health risk. Figure 5 shows a reduction in all of the 14 averaged regions. The reduction in the USEPA80 index is largest for the North-American continent, S.E. Asia and North-China. These regions also display the largest reductions in EU60, along with the European regions and the Middle East. Figure 5 also shows that ozone in most regions is now below the respective limit levels. Exceptions are the South-Eastern USA where the EU60 and USEPA80 are exceeded by 25 and 0 days respectively, and Central Europe where we find 3 (EU60) and 0 (EPA80) days of exceedance. Also over the Indian subcontinent the EU60 and EPA80 health risk thresholds remain exceeded by 31 (EU60) and 5 (USEPA) days for South-India and 48 (EU60) and 7 (USEPA) for Northern-India. In Central-West Africa during 41 (EU60) and 12 (USEPA) days the thresholds are exceeded. We note however, that in our study we did not assume that biomass burning emissions would decrease. Thus in general, a reduction of emissions as indicated by the MFR scenario has a positive effect on future surface ozone levels; the general compliance to all three health indices clearly demonstrates the scope of this emission reduction scenario to reduce undesirable health effects. S4, IPCC SRES A2 scenario The SRES A2 scenario health indices increase the health indices worldwide and especially over industrialized regions (Figure 4 and 5). The area with elevated values is extending into larger parts of northern Europe, northern Asia and Africa. Both background ozone and peak ozone episodes increase, but with a relatively stronger increase in peak ozone episodes, giving NH values of 5548 ppb.days for SOMO35 (75 % increase), 81 days for EU60 (153% increase) and 16 days for USEPA (300% increase). In the Indian subcontinent we find air quality indices higher than anywhere else in the world: 12797 ppb.days (SOMO35), 177 days (EU60) and 103 days of exceedance (USEPA80) for Northern India. Very high values are also found over North America, e.g. 9434 ppb.days (SOMO35), 164 days of exc. (EU60) and 48 days of exc. (USEPA) over S.E. USA. Also in the Central Mediterranean, the Middle East and S.E. Asia we find 21 high values, i.e. SOMO35 values of approximately 8000 ppb.days, EU60 values around 100 days of exc. and USEPA values surpassing 30 days of exc. Figure 5 demonstrates the large increase in peak ozone episodes (EU60 and USEPA80 indices) compared to the increase in background ozone (SOMO35), due to the impact of large increases in regional emission? In particular, the increase in number of days exceeding 80 ppb (USEPA index) over the Indian sub-continent and the Middle East is prominent. The large increase in the number of days exceeding 60 ppbv over Australia is probably due to transport of pollution from the southern part of Asia. The increase in SOMO35 is largest over Latin-America, the African regions and India. The EU60 and USEPA thresholds for health risk are largely surpassed in all regions and on a global average, demonstrating an alarming development if emissions are augmented as anticipated in the A2 scenario. Vegetation indices S1, Year 2000 Figure 6 shows the model ensemble mean AOT40 considering a 3 months (AOT403m) and a 6 months (AOT406m) growing season for crops and forests respectively), SUM06 accumulated both over 24 hours (SUM0624h) and daylight hours only (SUM06day), and W126 indices for the baseline scenario (S1). Figure 8 gives the ensemble mean weighted averages and standard deviations of these indices for the 14 selected regions. As for the health indices, ‘hot spots’ with elevated values in the vegetation indices are found in industrialized areas of Europe, the US and Asia as well as in biomass burning areas in Latin-America and Africa. Note, that the Latin-American and African regions in Figure 7, do not include these biomass burning areas. The 5 vegetation indices in the 14 selected regions show high mutual correlation coefficients, between R2 = 0.85 (AOT406m vs. SUMO624h) and R2 = 0.99 (SUM0624h vs. W126). The AOT40 ensemble means show lower standard deviations than SUM06 and W126, confirming the higher consistency amongst the models when predicting exceedance of background ozone levels compared to exceedance of high ozone levels. 22 AOT403m indices larger than 20000 ppb.h are found over the Central Mediterranean, South-East USA, the Middle East and North-India. The lowest values are found over Australia and Latin-America. Only in Australia AOT403m is below the threshold for yield reduction (3000 ppb.h) of agricultural crops. When we calculate the same AOT403m solely based on the set of observations given in section xxx, we calculate for Central Europe and the Central Mediterranean AOT40 of 9350±2830 ppb.h and 12970±6530 ppb.h, respectively (ref EMEP). The corresponding model ensemble values of 10285±5893 ppb.h are consistent for Central Europe .However, the computed 23230±10680 ppb.h for the Central Mediterranean is a factor of two higher. The larger model ensemble values for the Central Mediterranean can partially be explained by the fact that the growing season is defined as the 3 consecutive months with highest AOT40 index. Using this definition of growing season produces ‘worst case scenario’ values, however for the European data the difference between the two approaches is never larger than 15%. (Don’t understand fd) Furthermore, the surface ozone summer maximum is overestimated by the model ensemble mean (Figure 2). For AOT406m (6 months) values are exceeding 30000 ppb.h in the US regions, the Central Mediterranean and the Middle East. Of the 14 regions, only Australia does not exceed the threshold for reduction of forest growth (5000 ppb.h.). The SUM06 indices exceed 50000 ppb.h over South-Eastern USA, the Central Mediterranean, North-India and the Middle East and have the lowest value over Australia. Night time ozone levels have only a minor contribution to SUM0624h. SUM06day values increase with less than 3%, except in Latin America (13%), CentralWest (9%) and Southern (8%) Africa, North (4.6%) and Southern (7.2%) India and a remarkable 75% increase in Australia, the latter on top of a very low SUM06day value. As opposed to AOT40 and SUM06, the W126 index uses a continuous rather than a discontinuous weighting function (Figure 1). However, W126 correlates very well with AOT403m and SUM06day. The highest W126 values are found in the Central Mediterranean, South-East US, India and the Middle East (exceeding 40000 ppb.h) 23 whereas the lowest-most values are found over Australia, Latin-America and Central Europe. Limit levels have not been established for the SUM06 and W126 indices, but empirical (non-linear) exposure-yield response equations are available for SUM06day and W126 (Wang and Mauzerall, 2004). From these relations, we obtain a 5% yield loss ‘limit values’ of 13000 ppb.hr and 9000 ppb.hr for SUM06day and W126 respectively. In the S1 case, in all regions except Australia these limit levels are exceeded. KE: SJEKK W&M SUM06day ??????? KE: How do we treat the model overestimation ? Do we consider 3xthreshold as for health? This would be based on 5 % damage of wheat; 3x13000 and 3x9000???? [I’m not sure if it makes sense to apply a 3x less stringent level analogous to the health indices as the dose-response curves are not linear for W126 and SUM06, but linear for AOT40; it would make more sense to look at levels corresponding to yield reduction of 10% or 15%] KE: What would the corresponding 15 % levels be? It is probably defendable that at 15 % levels- there is at least some damage due to ozone. RITA for you to answer! Vegetation indices in 2030: scenario S2-S4 Figure 7 illustrates the changes in the vegetation AQ indices over the relevant areas (shown are AOT403m and SUM06day for crops, AOT406m for forests). Figure 8b-d give the changes of all vegetation air quality indices for CLE, MFR and A2 compared to S1 for 14 selected regions. General trends and geographical distributions are similar to the health AQ indices; hence we limit the discussion to some salient features. S2, current legislation (CLE) scenario 24 As expected, CLE leads to a general increase in the vegetation indices in the year 2030. The increase over the northern hemisphere for the vegetation indices ranges between 21 – 38%. On the Indian subcontinent, where no restrictive measures on emissions of O3 precursors are implemented, the AOT40 indices increase 50-63%, whereas the SUM06 and W126 indices increase with 75-97%. This indicates a larger increase in episodic peak levels compared to the increase in O3 background levels in this region. Large increases are found also in South-East Asia where increases in emissions from transport and power generation are anticipated, i.e. 20-30 % for AOT40 and 30-40 % for SUM06 and W126. Increases of the same order are also found over the African regions due to increased biomass burning. Despite the implementation of policies for air quality improvement, the selected US regions show an increase between 20 and 30% for SUM06 and W126 (i.e. the US favoured indices) and between 12 and 16% for AOT40. In contrast, currently implemented European legislation stabilize or slightly decrease the vegetation indices over Europe by 2030. In particular the Mediterranean area is the only region out of the 14 selected ones where all indices show a decreasing trend. In agreement with the findings for the health AQ indices, we find larger reductions over Europe for indices based on higher threshold values (SUM06 and W126) than for the lower threshold AOT40 indices. S3, maximum feasible reduction (MFR) scenario The MFR scenario leads to a worldwide decrease or stabilization of the vegetation indices. The reductions appear in polluted areas with the largest reductions in southern parts of USA, Europe, the Middle East, N. China and S.E. Asia, i.e. AOT40 decrease by 50-70 %, SUM06 and W126 by 70 -200 % in these regions The Indian sub-continent shows the largest reductions, however, the highest absolute values are still found over India (e.g. in North-India AOT403m is 12757 ppb.h, W126 is 23784 ppb.h and SUM06day is 22642 ppb.h.) The analysis of health indices demonstrated how the MFR scenario reduced the health indices below critical levels in polluted regions. Although strongly reduced, the MFR emission reductions do not bring AOT40 values below the threshold for yield reduction of agricultural crops (3000 ppb.h) or forest growth (5000 ppb.h). In the US regions and C. Mediterranean, W126 and SUM06 values are in the range 10000-15000 ppb.h close to the 5% reduction limit (9000 and 13000 25 ppb.h). In Central Europe and South-East Asia the values are well below the 5% reduction limit, i.e. SUM06 in the range of 3500-4000 ppb.h and W126 in the range of 6000-7000 ppb.h. The differences between Northern and Southern Hemisphere averages are strongly reduced, caused by large reductions on the Northern Hemisphere and a stabilization on the Southern Hemisphere. e.g. SUM06day is 5980 ppb.h on the Northern Hemisphere and 5652 on the Southern Hemisphere S4, IPCC SRES A2 scenario As for the health indices the SRES A2 scenario leads to large worldwide increases in the vegetation indices and in particular over industrialized regions (Figure 6 and 7). The largest increases are found in South-East Asia and India. where AOT40 increases by 80100 %, SUM06 and W126 by 90-160 %. Very high levels are found over India, the Middle East, S.E. Asia, USA, C. Med. and N. China/Japan, e.g AOT40 values in USA and the Central Mediterranean exceed 40000 ppb.h, SUM06 and W126 are in the range 60-95000 ppb.h. 5. Discussion 5.1 Can we understand the discrepancy of models and measurements? The description of emissions, chemical and meteorological processes (e.g. deposition and mixing in the boundary layer) will affect the model ensemble results. We showed in section 5.2 that in North America, Europe and Northern China computed monthly average surface ozone concentrations are relatively well in agreement by measurements. However, in other regions such as Central West Africa, Southern Africa, the Middle East, North and South India all models systematically showed overestimates of the limited amount of measurements to our disposal. Several possible reasons may explain these discrepancies. 1. Incorrect emissions of NOx, and/or NMVOC 2. Incorrect description of meteorological processes in the models 3. Incorrect description of chemical processes in the models 26 4. Inaccuracies of measurements and non-representativity of these measurements for the large scale model calculations. In our study we used estimates by IIASA for the year 2000 for anthropogenic NOx, NMVOC and CO emissions [Cofala et al., 2005]. Whereas relatively much knowledge on emissions and technology levels is available in Europe and North America, the uncertainties are much larger in other continents. Especially the emissions from biofuels, which are important fuel types in Asia and Africa, are poorly quantified. Nevertheless, analysis of GOME satellite data [van Noije et al., in preparation, 2005] indicates a too low NOx column (by a factor of two) over Southern Africa, and relatively good agreement over India [TWAN VAN NOIJE CHECK]. Also the analysis of nitrate wet deposition reveals no systematic deviations over Africa and India [Dentener et al., in preparation, 2005]. The open-fire NOx emissions were calculated from the GFED [Van der Werf et al., 2003] database using the emission factors of [Andreae and Merlot, 2001]. A recent revision of these emission factors revealed an approximately 30 % lower emission factor for NO emissions from grass-land (savannah) fires. Sensitivity calculations with the TM4 model [Van Noije et al.., in preparation, 2005] show that the use of these lower emission factors would lead to lower mixing ratios by 10-15 % and 610% in Central West Africa and Southern African dry-season, respectively, explaining a small part of the discrepancy. An incorrect description of meteorological processes in the models could also explain some discrepancies. Most models are driven by meteorological parent models that are better tested and constrained in middle latitudes than in tropical regions. For instance in South East Asia it important to have a correct description of the monsoon circulation, which can not done in the coarse resolution models. It is notoriously difficult to give a correct description of mixing by turbulent and convective mixing [Dentener et al., 1999; Jacob et al., 1997]; the effect of different mixing parameterizations on surface ozone is not easy to predict. The variation in horizontal resolution and the thickness of the surface layers from model to model will also lead to variations in the model ensemble. Higher resolution models 27 tend to produce less ozone from the same levels of precursor emissions, due to less forced ‘mixing’ when emissions are added to large grid boxes [e.g., Esler, 2003]. Dry deposition schemes in models are generally based the well-known [Wesely, 1989] scheme; however the over-all effect on e.g. ozone removal and vertical ozone profiles in the model surface layer is strongly dependent on the assumptions on surface properties, boundary layer turbulence and surface layer thickness [Ganzeveld and Lelieveld, 1995]. Indeed our preliminary analysis of ozone deposition distributions from the models suggest that the schemes generate quite variable deposition velocities over different terrains [Stevenson et al., 2005]. All models included NMVOC degradation chemistry schemes in various degrees of detail; Stevenson et al.. [Stevenson et al., 2005] show that the gross tropospheric ozone production terms is rather similar between models. However, the description of heterogeneous chemistry is in most models relatively simplified. Earlier studies [Dentener et al., 1996.; Grassian, 2001; Jacob, 2000] suggested an important role for ozone destruction on mineral aerosol; however there is no consensus on the overall impact. The atmosphere in e.g. Southern Africa, India and China in the dry season can be loaded with dust and pollution aerosol- and if heterogeneous chemistry is important these are place were the impact is likely to be largest. Finally, inaccuracies of measurements and non-representativity of these measurements for large scale model calculations may also contribute to discrepancies of models and measurements. Whereas there are a substantial amount of measurements used for North America and Europe; the number of measurements in other regions is rather small; and they are not necessarily representative for the whole region. E.g. for the Middle East we used only one measurement taken in Turkey. This can however not explain the systematic overestimate of the models in other regions. A significant fraction of the measurements in Africa and Asia was taken from the passive sampler network of [Carmichael et al., 2003]. There have been discussions in the past about the accuracy of passive samplers to measure O3 at high concentration levels, and possible interference with humidity. 28 Comparison with in-situ analyzers on a limited amount of locations did however not reveal systematic differences. Another important issue is the fact that we compare the ozone concentrations of models averaged for their lowest gridbox; which may be not representative for the O3 concentrations at measurement height (often at 10 m). Especially at polluted places relatively much O3 is titrated by fresh NO emissions in first 10-20 meters above the ground. An indication for the importance of this effect is the much better agreement of ‘well mixed’ afternoon ozone concentrations on sites in China and India (e.g. analysis with the TM5 and FRSG model). Since the air quality indices assess elevated concentrations we expect that these can be better represented by models than 24 hours averaged concentrations. For future model studies, as well as for measurement, we strongly recommend to also evaluate Ox=NO2+O3; which parameter should be less dependent on local conditions. RITA can we give one or two examples; e.g. based on Chinese measurements? Therefore we think that even in regions with apparent discrepancies of models and measurements we are able to do a meaningful analysis for exceedances of air quality and vegetation indices. To give further credibility to our analysis of regions at risk for health and vegetation damage by ozone, we have further analyzed our results in terms regions where the thresholds are exceeded by a factor of 3. The results were relatively consistent for the three different AQ indices. 5.2 Robustness of AQ indices We showed before the interesting correspondence of the health related AQ indices SOMO35; EU60 and EPA80. Then discuss the correlation between AOT40; SUM06; W126. KE: Is discussed in the Veg. indices part as for health. How is SOMO35 correlated with the vegetation indices? It is worth noting that the vegetation indices show a good correlation with the health indices SOMO35 and EU60 (R2 > 0.80 for all mutual correlations between the latter two health indices and all vegetation indices, except for AOT406m vs. EU60 where R2 = 0.69), 29 whereas the USEPA80 index has an R2 < 0.6 with any of the vegetation indices. More in particular, the European indices AOT403m and EU60 have a R2 = 0.84 and are related through AOT403m = 1300xEU600.62. This implies that the limit levels of these indices are in fact not consistent with each other: 25 allowed exceedence days under EU60 corresponds with AOT403m near 10000 ppb.hr, more than 3 times the limit level for the latter index. KE: It is not very clear to me what we try to say here. Is it a big point that the limit levels are not consistent between health and veg. indices ? As the receptors are so different (humans and plants) the limits are expected to be different. The limit values are worked out using completely different considerations (exposure-effect relations). What we see is that vegetation is damaged at lower ozone levels that human health. Is the point to see if there is an index appropriate to human health and veg ? 6. Summary and conclusions We compute current and future ozone air quality indices for health and vegetation using a xx member ensemble of models. The models are driven by 3 different emission scenarios for the year 2030. The first (CLE) reflects worldwide currently decided air quality legislation, whilst the second (MFR) represents an optimistic case assuming that that all technology currently available would be used to achieve all possible emissions reductions. It however does not consider progressive energy use scenarios, or for instance a substantial fuel-shift towards hydrogen, which would have similar effects on emissions as MFR. We contrast these scenarios with the pessimistic IPCC SRES A2 scenario. The three scenarios reflect current insight regarding the possible range of future air pollution and emission developments. This study represents, to our knowledge, the most extensive evaluation of surface ozone calculated by global chemistry transport models. Comparison with a host of measurements in North America, Europe, and a limited amount of measurements in Northern China are in relatively good agreement. However, large 30 overestimates of computed ozone are found for almost all models in Africa, the Middle East and India. Problems with emissions, chemical and meteorological descriptions of the coarse resolution global models may contribute to the discrepancy, but we can not exclude that the few measurements available in these regions were not representative for the larger model scales. Until these measurements become available model improvement and testing of reasons for discrepancies is precluded. To evaluate current and future ozone air quality xx models generated hourly surface ozone fields; since typically ozone AQ indices are derived from the correlation of results of epidemiological studies with measured hourly surface ozone concentrations [WHO, 2003]. We evaluated three health related AQ indices, the recently recommended SOMO35, evaluating ozone concentrations above a threshold of 35 ppbv; EU60 using a threshold of 60 ppbv; and the USEPA80 evaluating the exceedance of 80 ppbv. Correlation EU60 and EPA80 with SOMO35 shows that a SOMO35 threshold of ca. 2000-2500 ppb days is consistent with 25 days of exceedance of EU60 and 3 days of exceedance of EPA80. The variation of SOMO35 calculated by the individual model ensemble members is substantial less than for EU60 and EPA80. Thus SOMO35 is probably the most robust AQ index when evaluating results from individual models. This result is probably independent from the models’ ability to accurately calculate worldwide surface ozone. In which regions is the population currently and in future at risk to ozone related health problems? Air quality standards in the European Union and in the United States state that the EU60 and EPA80 should not be exceeded by 25 and 3 days, respectively. According to our calculations presently in 10/12 out 14 selected regions the standards are exceeded for SOMO35, EU60 and EPA80. Even if we choose less stringent criteria of 6000 ppb days, 75 and 9 days for SOMO35, EU60 and EPA80, respectively, 5 to 6 out of 12 world regions are above the limits. The currently decided legislation is not enough change this situation; only in Europe the ozone air quality somewhat improves; but regional emission reductions measures are counteracted by an increase in global background O3. Large increase of ozone and in 31 exceedance of air quality standards are predicted for India and too a lesser extent for all world regions, 6-7 world regions will not conform to any O3 AQ standard. In contrast, we show that implementation of all currently possible technical measures can dramatically improve O3 AQ; using the MFR scenario almost all regions comply with currently regulations on Air quality. We show that considering the pessimistic SRES A2 scenario leads to a dramatic detoriation of global airquality in almost all polluted regions of the world. 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Zunckel M., Venjonoka K., Pienaar J.J., Brunke E.G., Pretorius O., Koosialee A., Raghunandan A., van Tienhoven A.M., 2004, Surface ozone over Southern Africa: synthesis of monitoring results during the Cross Border Air pollution Impact Assessment Project, Atmospheric Environment, 38, 6139-6147 37 Tables Code Scenario Meteorology Emissions S1 Y2000 2000 (CTMs) 2000 1995-2004 (GCMs) (EDGAR3.2) Olivier et al. 2001 S2 CLE 2000 (CTMs) 2030 IIASA CLE 1995-2004 (GCMs) Dentener et al. 2004 S3 MFR 2000 (CTMs) 2030 IIASA MFR 1995-2004 (GCMs) Dentener et al. 2004 S4 A2 2000 (CTMs) 2030 SRES A2 1995-2004 (GCMs) Nakicenovic et al. 2000 S5 CLE-2030c 2025-2034 (GCMs) 2030 IIASA CLE Table 1 Reference Stevenson et al. 2005 Specifications of the simulations. 38 CHASER_CTM CHASER_GCM FRSGC_UCI GEOS-CHEM GISS GMI/CCM GMI/DAO GMI/GIS IASB LLNL-IMPACT LMDz/INCA (CTM) LMDz/INCAc (GCM) MATCH-MPIC-ECMWF MATCH-MPIC-NCEP MOZ2-GFDL MOZART4 (NCAR) MOZECH p-TOMCAT STOCHEM-HadAM3 STOCHEM-HadGEM TM4 TM5 OsloCTM2 ULAQ UM_CAM S1 S2 S3 S4 S5c 1 9 1 1 5 1 1 1 1 1 1 5 1 1 2 2 5 1 1(10) 5 1 1 1 10 1(10) 1 9 1 1 5 1 1 1 1 1 1 5 1 1 2 2 5 1 1(6) 5 1 1 1 10 1 1 -1 1 5 1 1 1 1 1 1 -1 1 2 2 -1 1 5 1 -1 10 1 1 -1 1 5 1 1 1 1 1 1 -1 1 2 2 -1 1 5 1 -1 10 1 -9 --5 ------5 ---2 5 -10 5 ---10 10 Table 2 Number of simulated years (excluding spin-up) performed by individual models. Two models (STOCHEM_HadAM3 and UM_CAM) performed multi-annual simulations to compare with S5c, as well as single year simulations to compare with S3 and S4. Models shown in bold face provided hourly surface ozone concentrations for calculation of ozone indices. 39 NOx (Tg N) CO (Tg) NMVOC (Tg) SO2 (Tg S) NH3 (Tg N) CH4 (ppbv) Table 3 S1 S2 S3 S4 S5c 124.8 977 147.1 111.1 64.8 1760 141.1 904.1 145.5 117.6 84.8 2088 76.0 728.7 104.4 35.8 84.8 1760 206.7 1268.2 206.7 202.3 89.2 2163 141.1 904.1 145.5 117.6 84.8 2012 Specified global annual anthropogenic emission totals for each scenario. 40 NOx (Tg N) CO (Tg) NMHC (Tg) SO2 (Tg S) DMS (Tg S) NH3 (Tg N) Soils Lightning Oceans/vegetation Vegetation isoprene Vegetation terpenes Volcanos Oceans/terrestrial biosphere Oceans Soils 7 5 100 512 260 14.6 20 8.3 2.4 Table 4 Recommended natural emissions sources. 41 Vegetation index AOT40 Units ppb.h Definition Receptor Sum of hourly daylight (> 50 W/m2 PAR) O3 Agricultural crops volume mixing ratio (vmr) above 40 ppb. Accumulated over 3 consecutive n months of the growing season. [CO3 40]i for CO3 > 40 ppb Threshold: 3, 000 ppb.h i 1 Effect: Yield reduction where CO3 is the hourly O3 vmr in ppb, i is the index, and n is the number of hours with CO3 Forest trees > 40 ppb. Accumulated over 6 consecutive months of the growing season. Threshold: 5, 000 ppb.h Effect: Growth reduction SUM06 Units ppb.h Sum of 24-hourly O3 vmr at or above 60 ppb. W126 Units ppb.h Weighted sum of 24-hourly O3 vmr. Vegetation Accumulated over 3 consecutive [CO3]i for CO3 60 ppb months of the growing season. i 1 Threshold: No threshold defined where CO3 is the hourly O3 vmr in ppb, i is the Effect: Yield reduction index, and n is the number of hours with CO3 ≥ 60 ppb. n n C * w i i i 1 where wi = 1/(1+4403 * exp(-0.126*Ci)) and Ci is the hourly O3 vmr in ppb. Use CO3 here, or use C above, for consistency. Vegetation Accumulated over 3 consecutive months of the growing season. Threshold: No threshold defined Effect: Yield reduction Table 5 Definition of vegetation indices used in the risk assessment. 42 Index SOMO35 Units ppb.days. Definition n [max_ 8h _ mean 35] i 1 i Threshold: No threshold defined Effect: Health risk. for max_8h_mean > 35 ppb. Max_8h_mean is the daily maximum 8 hour average O3 vmr in ppb, n is the number of days in a year. EU60 Number of days with maximum 8-h Threshold: 25 days per year (during a Units days of average ozone vmr exceeding 60 ppb three years period) exccedence Effect: Health risk. USEPA80 Number of days with maximum 8-h Threshold: the 3-year average of the Units days of average ozone vmr exceeding 80 ppb. 4-th highest daily maximum at each exceedence location must not exceed 80 ppb (equivalent to a maximum value of 3 days exceedance per year) Effect: Health risk Table 6 Definition of health indices used in the risk assessment. 43 region Lat Lon # of stations References 1. S.W. USA LA regions 30N-40N 125W-110W 11 A. Fiore, CASTNET 2. S.E. USA 25N-35N 90W-80W 12 A. Fiore, CASTNET 3.Great Lakes 40N-50N 95W-75W 13 A. Fiore, CASTNET 4. Latin America/Brazil 25S-15S 50W-30W N.a. 5. Central-West Africa 5N-15N 5W-15E 3 Carmichael et al., 2003 6.Southern Africa/High Field 30S-20S 20E-35E 6 Zunckel et al., 2004 7. Central Mediterranean 35N-45N 5E-30E 21 EMEP, Airbase 8. Central Europe 48N-54N 7E-17E 101 EMEP, Airbase 9. Middle East 30N-40N 30E-55E 1 Carmichael et al., 2003 10. North India + Nepal 20N-30N 70E-90E 6 Naja et al., 2003 Lal et al., 2000 Carmichael et al., 2003 11. Southern India 10N-20N 75E-85E 4 Naja and Lal, 2002 Debaje et al., 2003 Nair et al., 2002 Carmichael et al., 2003 12. S.E. Asia 20N-35N 110E-125E 3 Carmichael et al., 2003 35N-45N 110E-145E 8 WMO-WDC-GG Akimoto and Pochanart Wang and Mauzerall, 2004 Carmichael et al., 2004 25S-40S 145E-155E N.a. (Guangzhou Hongkong) 13. Northern China (Beijing)-Japan 14. Australia Table 7: Fourteen regions selected in this study 44 Figures a) b) 45 c) d) e) 46 Figure 1: Yearly mean surface ozone for model ensemble mean. Figure a displays year 2000 (S1) mean and standard deviation. Figure b, c, and d displays differences between scenario CLE (S2), MFR (S3) and SRES A4. Figure e) shows the change in yearly mean surface ozone due to climate change. Ensemble differences are calculated taking the average of the individual model simulation differences. Units are ppb. 47 3 4 5 6 7 month 8 9 10 11 12 1 2 3 4 5 6 7 month 8 9 4 5 6 7 month 8 9 SRFC O3 (ppb) 8 9 2 3 4 5 6 7 month 8 9 1 1 2 3 4 5 6 7 month 8 9 10 11 12 3 4 5 6 7 month 8 9 10 11 12 2 3 4 5 6 7 month 8 9 10 11 12 2 3 4 5 6 7 month 8 9 10 11 12 S. Africa - High Field 2 3 4 5 6 7 month 8 9 90 80 70 60 50 40 30 20 10 0 10 11 12 1 2 N. India + Nepal 2 3 4 5 6 7 month 8 9 90 80 70 60 50 40 30 20 10 0 10 11 12 1 SE Asia 90 80 70 60 50 40 30 20 10 0 10 11 12 90 80 70 60 50 40 30 20 10 0 10 11 12 SRFC O3 (ppb) 1 SRFC O3 (ppb) SRFC O3 (ppb) 6 7 month S. India 90 80 70 60 50 40 30 20 10 0 2 3 4 5 6 7 month 8 9 10 11 12 2 3 4 5 6 7 month 8 9 10 11 12 90 80 70 60 50 40 30 20 10 0 1 Australia SRFC O3 (ppb) 90 80 70 60 50 40 30 20 10 0 1 5 90 80 70 60 50 40 30 20 10 0 10 11 12 N. China SRFC O3 (ppb) 1 SRFC O3 (ppb) 3 Middle East 1 4 C. Europe 90 80 70 60 50 40 30 20 10 0 2 3 90 80 70 60 50 40 30 20 10 0 10 11 12 C. Mediterranean 1 2 CE Africa 90 80 70 60 50 40 30 20 10 0 SRFC O3 (ppb) SRFC O3 (ppb) Latin A./Brazil 1 SRFC O3 (ppb) 2 SRFC O3 (ppb) 1 US Great Lakes SRFC O3 (ppb) 90 80 70 60 50 40 30 20 10 0 SRFC O3 (ppb) SE US 90 80 70 60 50 40 30 20 10 0 SRFC O3 (ppb) SW US 2 3 4 5 6 7 month 8 9 10 11 12 90 80 70 60 50 40 30 20 10 0 1 48 Figure 2 Comparison of observed surface ozone levels (black squares) and model ensemble mean (blue line). The observations are averages over several sites, and the black line represents the standard deviation. The blue shaded area gives the standard deviations of the model ensemble. The green area indicates the variation among the models, the upper line of the green shaded region gives the maxima of the model ensemble, the lower line gives the model ensemble minima. a) b) 49 c) Figure 3 Model ensemble mean health indices for year 2000 (S1). A) SOMO35 (ppb.days) B) EU60 (days of exceedence). The white line indicates the recommended threshold not to be exceeded (25 days pr year). C) USEPA60 (days of exceedence). The white line indicates the recommended threshold not to be exceeded (3 days pr year). a) 50 b) Figure 4 Differences of ensemble mean health indices. Ensemble differences are calculated taking the average of the individual model simulation differences. a) SOMO35 (ppb.days), difference between CLE (S2) and year 2000 (S1). b) EU60 (days of exceedence), difference between MFR (S3) and year 2000 (S1). 51 7000 6000 5000 4000 3000 2000 1000 0 S.W. USA S.E. USA Great Lakes Latin CentralCentral Southern America/ East Mediterr Africa Brazil Africa anean 350 300 250 200 150 100 50 0 Central Europe North India Middle East Southern Northern S.E. Asia Australia India China 5654 6822 3412 1869 3733 2895 5559 2795 6780 5874 5656 4564 4559 540 EEA 67 105 44 20 47 29 75 26 109 83 89 55 58 0.6 USEPA *10 84 188 88 29 139 26 121 4 128 51 93 60 93 0 SOMO35 days of exceedence ppb.days S1 7000 6000 5000 4000 3000 2000 1000 0 -1000 Latin CentralCentral Southern America/ East Mediterr Africa Brazil Africa anean S.W. USA S.E. USA Great Lakes SOMO35 756 896 372 169 823 1018 EEA 28 27 6 2 12 15 USEPA *5 19 36 12 1 14 7 350 300 250 200 150 100 50 0 -50 Central Europe North India 234 341 3726 463 3453 743 479 50 -2 -4 106 12 89 20 11 0 -13 -1 208 2 179 18 20 0 days of exceedence ppb.days S2 - S1 Middle Southern Northern S.E. Asia Australia East India China 0 -1000 -2000 -3000 -4000 -5000 -6000 -7000 S.W. USA S.E. USA Great Lakes Latin CentralCentral Southern America/ East Mediterr Africa Brazil Africa anean 0 -50 -100 -150 -200 -250 -300 -350 Central Europe North India Middle East Southern Northern S.E. Asia Australia India China -2394 -3183 -1464 -530 -542 -668 -2318 -935 -2239 -2549 -2214 -2612 -1854 -217 EEA -49 -80 -31 -5 -6 -7 -55 -23 -61 -65 -58 -49 -44 0 USEPA *5 -30 -99 -45 -4 -9 -3 -35 -2 -31 -10 -19 -28 -38 0 SOMO35 days of exceedence ppb.days S3 - S1 52 7000 6000 5000 4000 3000 2000 1000 0 S.W. USA S.E. USA Great Lakes Latin CentralCentral Southern America/ East Mediterr Africa Brazil Africa anean 350 300 250 200 150 100 50 0 Central Europe North India Middle East Southern Northern S.E. Asia Australia India China 2480 2612 1403 2371 3130 2596 2136 1133 6017 3103 4737 3126 2048 410 EEA 60 59 58 60 63 62 64 64 68 57 51 40 32 27 USEPA *5 99 144 53 23 53 26 57 21 452 133 304 194 99 0 SOMO35 days of exceedence ppb.days S4 - S1 Figure5 Model ensemble mean regional averages of health indices. Averages for S1 have been normalized to the respective values for S.E. US. The scenario differences are expressed in relative changes compared to S1 absolute values. Standard deviations are given by black lines. Regions with values exceeding 3x threshold for health risk are marked in red, and regions with values below recommended thresholds in green. 53 a) b) c) 54 d) e) 55 Figure 6 Model ensemble mean, vegetation indices for agricultural areas in ppb.h. The growing season is in each gridbox defined as the three or six consecutive months with the highest index. a) AOT40 (3 months, daylight hours) b) AOT40 (6 months, daylight hours) c) SUM06 (3 months growing season, 24 hours) d) SUM06 (3 months growing season, daylight hours) e) W126 (3 months growing season, 24 hours) a) 56 b) c) 57 Figure 7 Differences of ensemble mean vegetation indices (ppb.h) Ensemble differences are calculated taking the average of the individual model simulation differences. a) AOT40 (3 months, daylight hours) b) AOT40 (6 months, daylight hours) c) SUM06 (3 months growing season, daylight hours) S1, vegetation 100000 ppb.hr 80000 60000 40000 20000 0 S.W. USA S.E. USA LA regions Great Lakes Latin America/B razil CentralEast Africa Southern Central Africa/Hig Mediterran h Field ean Central Europe North India Middle East Southern India S.E. Asia (Guangzh ou Northern China (Beijing)- Australia AOT40 (3m) 19000 22508 13132 8491 13125 11249 23285 10310 20103 21690 18419 13760 17590 920 AOT40 (6m) 30877 36825 19165 10048 14087 15085 35966 16326 25541 34541 21424 22211 26143 1802 SUM06 (d) 46179 55997 29383 15312 28879 24048 60007 16695 55917 57470 43513 27573 40384 247 SUM06 (24) 47305 56551 29925 17362 31449 26109 60858 16786 58383 58044 46493 28231 40581 433 W126 36705 44865 25024 15810 27370 22073 47105 15208 42903 41471 35146 23903 32997 1744 58 (S2-S1) vegetation ppb.hr 70000 50000 30000 10000 -10000 S.W. USA S.E. USA LA regions Great Lakes Latin America/B razil CentralEast Africa Southern Central Africa/Hig Mediterran h Field ean Central Europe North India Middle East Southern India S.E. Asia Northern China (Beijing)- Australia AOT40 (3m) 2476 3343 1535 618 2330 2008 -1202 117 9920 786 10252 3037 1957 92 AOT40 (6m) 4485 5993 2195 828 3073 4171 -991 508 16235 1826 13536 5304 2985 117 SUM06 (d) 10867 13078 5235 1403 6288 7539 -4813 -2477 40492 5327 41947 10462 7796 19 SUM06 (24) 13922 10869 6561 830 6647 10608 -5149 -1769 43717 5368 43652 11518 7455 -146 W126 7651 9419 3916 1292 5319 5834 -3488 -604 33761 3331 33720 7306 5442 126 Central Europe North India Middle East Northern China (Beijing)- Australia (S3-S1) vegetation 0 ppb.hr -20000 -40000 -60000 -80000 -100000 S.W. USA S.E. USA LA regions Great Lakes Latin America/B razil CentralEast Africa Southern Central Africa/Hig Mediterran h Field ean S.E. Asia Southern (Guangzh India ou AOT40 (3m) -9265 -11932 -6662 -1560 -1795 -1449 -11032 -4488 -6330 -10298 -6985 -8893 -8299 -353 AOT40 (6m) -17142 -21629 -10791 -2352 -2026 -2662 -19460 -8122 -9043 -18951 -8372 -15310 -13652 -711 SUM06 (d) -31246 -31311 -14937 -357 -2081 -7117 -31248 -9148 -24451 -39321 -26220 -18069 -22974 -66 SUM06 (24) -35066 -41775 -21462 -4024 -4206 -4770 -42218 -13513 -26910 -45396 -28325 -25020 -29137 -286 W126 -42194 -14630 -14979 4875 -7384 -14751 -18597 -5455 -84635 -42513 -73385 -14880 -30712 -3003 Central Europe North India Middle East Southern India S.E. Asia Northern China (Beijing)- Australia (S4-S1) vegetation 100000 ppb.hr 80000 60000 40000 20000 0 S.W. USA S.E. USA LA regions Great Lakes Latin America/B razil CentralEast Africa Southern Central Africa/Hig Mediterran h Field ean AOT40 (3m) 8891 10259 5776 4939 8652 4687 7828 4733 15816 11353 14182 14061 9584 741 AOT40 (6m) 16205 17769 8963 9095 12302 11027 14401 8087 27323 20884 17859 24042 15725 1307 SUM06 (d) 37198 41010 17726 16618 31761 22432 36240 16665 65093 53993 61456 45887 35590 202 SUM06 (24) 37917 40313 17359 16474 32718 20554 35475 16766 60723 51014 61587 46204 35212 38 W126 29058 32364 14774 12540 22035 13804 26485 12049 53422 39054 50326 38530 28239 799 Figure 8 Model ensemble mean regional averages of vegetation indices. Averages for S1 have been normalized to the respective values for S.E. US. The scenario differences are 59 expressed in relative changes compared to S1 absolute values. Standard deviations are given by the black lines. 60 Andreae, M.O., and P. Merlot, Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cycles, 15, 955-966, 2001. 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