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1 Supplementary Materials for From Acid Rain to Climate Change S. Reis,* P. Grennfelt, Z. Klimont, M. Amann, H. ApSimon, J.-P. Hettelingh, M. Holland, A.-C. LeGall, R. Maas, M. Posch, T. Spranger, M. A. Sutton, M. Williams This PDF file includes *To whom correspondence should be addressed. Figs. S1 and S2 Tables S1 and S2 Full References Published 30 November 2012, Science 338, 1153 (2012) DOI: /science Other Supplementary Material for this manuscript includes the following: (available at Eight data files used in constructing Figs. S1 and S2

2 mol c ha -1 a mol c ha -1 a mol c ha -1 a mol c ha -1 a Fig. S1. Exceedances of critical loads of acidity (moles of charge (H+) per hectare per year) for 1990, 2000, and 2010 and in 2020 under the revised Gothenburg Protocol. Grid colors reflect the level of exceedance. See Sources of Methods and Data below. 1

3 mol ha -1 a mol ha -1 a mol ha -1 a mol ha -1 a Fig. S2. Exceedances of critical loads of nutrient nitrogen (moles of N per hectare per year) for 1990, 2000, and 2010 and in 2020 under the revised Gothenburg Protocol. Grid colors reflect the level of exceedance. See Sources of Methods and Data below. 2

4 Table S1. Exceedance of critical loads of acidity and nutrient N in Europe [computed as average accumulated exceedance (AAE) (18)] and percent of ecosystem area exceeded (about 4 million km 2 ). Acidity reported in moles of charge (H + ) per hectare per year. Nutrient nitrogen reported in moles of N per hectare per year. See Sources of Methods and Data below. Acidity Nutrient N Year AAE Exceeded area AAE Exceeded area (mol c ha 1 yr 1 ) (%) (mol ha 1 yr 1 ) (%) * * According to the agreed revised commitments under the Gothenburg Protocol (1). Sources of Methods and Data: The European critical loads data base is held at the Coordination Centre for Effects (CCE; located at the Dutch National Institute for Public Health and the Environment (RIVM). Methods for calculating critical loads, levels and their exceedance have been reviewed and agreed by the Working Group on Effects (WGE) of the CLRTAP and are documented in the so-called Mapping Manual (18, 19). The critical loads data are provided to the CCE by the European parties to the CLRTAP upon request by the WGE (20). For countries that do not provide national data, critical loads are calculated with the same methods using open sources for the necessary input data [see, e.g., (21, 22)]. Depositions of sulfur and nitrogen compounds, used for calculating critical load exceedances, are provided by EMEP and are identical to those used in the integrated assessment modeling under the CLRTAP (2). For a popular summary of the (scientific) work under the LRTAP Convention see also the booklet Clearing the Air (23). Description of files holding the data for producing Figs. S1 & S2 and Table S1: The eight comma-separated ASCII files provided (4 AAEaci.yyyy and 4 AAEnut.yyyy with yyyy=1990,2000,2010,2020) in a zip-archive have identical structure. The first row is a header row, and subsequent rows hold the data (5 per row). The meaning of the data is the following: Column 1 ( I050 ) & Column 2 ( J050 ): Indices of the 50 km 50 km EMEP grid used in the maps [see (22] Column 3: The AAE for acidification ( AAEaci ) or nutrient N ( AAEnut ) of the respective grid cell (in mol c ha 1 yr 1 or mol ha 1 yr 1, respectively.) Column 4: ( Ex% ) Percent of ecosystem area in the grid cell that is exceeded Column 5: ( EcoArea ) Ecosystem area of that grid cell (km 2 ) The numbers in Table S1 can be obtained by applying the formula for calculating AAE [see (18) to all the grid cells. 3

5 Table S2. European emissions used in Fig. 1 in the main text in million tons (NO x as NO 2 ). Actual emissions 1990 and GP commitments 2010 originate from the GP text [see Tables 1 to 4 in Annex II of (24)] and for missing countries from (25); see Tables 3.1 to 3.4 of (25). Actual emissions 2010 are based on the emissions reported to EMEP under the obligations of the GP; data available from GP commitments 2020 lists emissions based on the emission reduction commitments provided in Table 1 of (6), and those for remaining countries originate from (26). Particulate matter emissions, including PM 2.5, have been recently reported to EMEP ( however, they remain incomplete for several countries, and a consistent time series cannot be retrieved from the official sources. Therefore, with exception of the 2020 commitments, we have used the results of the GAINS model following the methodology and scenarios discussed in (2). n.a., not applicable. Actual emissions Emissions relative to GP commitments Emission category SO NO X NMVOC NH PM n.a

6 References and Notes 1. UNECE, Clearing the Air (UNECE, Geneva, 2009); EB_30th_anniversary_brochure.pdf. 2. J.-P. Hettelingh et al., Critical loads and dynamic modelling to assess European areas at risk of acidification and eutrophication. Water Air Soil Pollut. Focus 7, 379 (2007). doi: /s A critical load is a quantitative estimate of an exposure to one or more pollutants below which significant harmful effects on specified elements of the environment do not occur. 4. P. Rafaj, M. Amann, J. Cofala, R. Sander, Factors determining recent changes of emissions of air pollutants in Europe: Service contract on monitoring and assessment of sectorial implementation actions (ENV.C.3/SER/2011/0009, International Institute for Applied Systems Analysis (IIASA), Laxenburg, Austria, 2012). 5. G. Sundqvist, in Governing the Air: The Dynamics of Science, Policy, and Citizen Interaction, R. Lidskog and G. Sundqvist, Eds. (MIT Press, Cambridge, MA, 2011), pp UNECE, Parties to UNECE Air Pollution Convention approve new emission reduction commitments for main air pollutants by 2020 (UNECE, Geneva, 2012); 7. United Nations Environment Programme, Near-Term Climate Protection and Clean Air Benefits: Actions for Controlling Short-Lived Climate Forcers (UNEP Synthesis Report, UNEP, Nairobi, 2011); 8. M. Amann et al., Cost-effective control of air quality and greenhouse gases in Europe: Modeling and policy applications. Environ. Model. Softw. 26, 1489 (2011). doi: /j.envsoft M. Posch, J. Aherne, J.-P. Hettelingh, Nitrogen critical loads using biodiversity-related critical limits. Environ. Pollut. 159, 2223 (2011). doi: /j.envpol Medline 10. G. Mills, H. Harmens, Ozone Pollution: A hidden threat to food security (ICP Vegetation, Bangor, Wales, 2011); Decision 2010/18, Long-term strategy for the Convention on Long-Range Transboundary Air Pollution and action plan for its implementation; M. Holland et al., Cost-Benefit Analysis for the Revision of the National Emission Ceilings Directive (AEA, Didcot, UK, 2011), l% pdf. 5

7 13. D. Shindell et al., Simultaneously mitigating near-term climate change and improving human health and food security. Science 335, 183 (2012). doi: /science Medline 14. A. R. Ravishankara, J. S. Daniel, R. W. Portmann, Nitrous oxide (N 2 O): the dominant ozone-depleting substance emitted in the 21st century. Science 326, 123 (2009). doi: /science Medline 15. F. Dentener, T. Keating, H. Akimoto, Eds., Hemispheric transport of air pollution 2010 (Air Pollution Studies no , ECE/EB.AIR/ , UN, New York, 2010); M. A. Sutton et al., Eds., The European Nitrogen Assessment (Cambridge Univ. Press, Cambridge, 2011). 17. F. Raes, R. Swart, Climate change. Climate assessment: what s next? Science 318, 1386 (2007). doi: /science Medline 18. M. Posch, J.-P. Hettelingh, P. A. M. de Smet, Characterization of critical load exceedances in Europe. Water Air Soil Pollut. 130, 1139 (2001). doi: /a: International Cooperative Programme on modelling and mapping of critical levels and loads and air pollution effects (2012); J.-P. Hettelingh, M. Posch, J. Slootweg, Eds., Critical Load, Dynamic Modelling and Impact Assessment in Europe: CCE Status Report 2008 (CCE, Bilthoven, Netherlands, 2008) (ISBN ); M. Posch, J. Slootweg, J.-P. Hettelingh, Eds., European Critical Load and Dynamic Modeling: CCE Status Report 2005 (CCE, Bilthoven, Netherlands, 2005) (ISBN ); G. J. Reinds, M. Posch, W. de Vries, J. Slootweg, J.-P. Hettelingh, Critical loads of sulphur and nitrogen for terrestrial ecosystems in Europe and Northern Asia using different soil chemical criteria. Water Air Soil Pollut. 193, 269 (2008). doi: /s x 23. J. Sliggers, W. Kakebeeke, Clearing the Air 25 years of the Convention on Longrange Transboundary Air Pollution (UN, Geneva, 2004). 24. UNECE, The 1999 Gothenburg Protocol to Abate Acidification, Eutrophication and Ground-level Ozone, (UNECE, Geneva, 1999); d.2005.pdf. 25. M. Amann et al., (1999). Integrated assessment modelling for the Protocol to Abate Acidification, Eutrophication and Ground-level Ozone in Europe [Lucht & Energie 132, Netherlands Ministry of Housing, Spatial Planning, and the Environment (VROM), The Hague, Netherlands]. 26. M. Amann et al., An updated set of scenarios of cost-effective emission reductions for the revision of the Gothenburg Protocol under the CLRATP (CIAM report 4/2011, Centre for Integrated Assessment Modelling, IIASA, Laxenburg, 6

8 Austria); CIAM4.pdf. 7