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Environmental policies in Europe have successfully eliminated the most visible and immediate harmful effects of air pollution in the last decades. However, there is ample and robust scientific evidence that even at present rates Europe's emissions to the atmosphere pose a significant threat to human health, ecosystems and the global climate, though in a less visible and immediate way. As many of the 'low hanging fruits' have been harvested by now, further action will place higher demands on economic resources, especially at a time when resources are strained by an economic crisis. In addition, interactions and interdependencies of the various measures could even lead to counter-productive outcomes of strategies if they are ignored. Integrated assessment models, such as the GAINS (Greenhouse gas - Air pollution Interactions and Synergies) model, have been developed to identify portfolios of measures that improve air quality and reduce greenhouse gas emissions at least cost. Such models bring together scientific knowledge and quality-controlled data on future socio-economic driving forces of emissions, on the technical and economic features of the available emission control options, on the chemical transformation and dispersion of pollutants in the atmosphere, and the resulting impacts on human health and the environment. The GAINS model and its predecessor have been used to inform the key negotiations on air pollution control agreements in Europe during the last two decades. This paper describes the methodological approach of the GAINS model and its components. It presents a recent policy analysis that explores the likely future development of emissions and air quality in Europe in the absence of further policy measures, and assesses the potential and costs for further environmental improvements. To inform the forthcoming negotiations on the revision of the Gothenburg Protocol of the Convention on Long-range Transboundary Air Pollution, the paper discusses the implications of alternative formulations of environmental policy targets on a cost-effective allocation of further mitigation measures.