The regulation of the emissions of 'traditional' primary air pollutants (fluorides, sulfur dioxide) has changed the pattern of exposure of ecological systems, with greatly reduced exposure close to sources, but with a smaller effect in some remote areas. Measurements show that recovery is occurring at some sites, in fresh water chemistry (reduced acidity) and in sensitive biota (sustainable fish populations). However, the pattern of change in exposure has not always been simply related to emission reductions. An understanding of responses to recent changes will improve our predictions of the response to future emission changes, both locally and globally. As exposure to 'traditional' pollutants is reduced, the potential for other pollutants to have effects becomes more evident. In the aqueous phase, we need to understand the role of soluble and suspended organics, but this also means explicit recognition of the possibility of phase exchange, and the role of photolytic reactions on plant, soil, and water surfaces. Do highly reactive free radicals in the atmosphere, formed by the action of sunlight on volatile organic compounds, have direct effects on plants? Organic compounds and heavy metals may be bioactive as gases and particles, but for many potentially toxic compounds, the experimental evidence for biotic response is very limited. To evaluate the potential effects of pollutants, we need to understand the pathways by which airborne pollutants enter and react within ecosystems. For vegetation, we have to consider bidirectional fluxes, and distinguish among uptake through stomata, through leaf surfaces, or through roots. There are several challenges for the future. (1) Can we devise experiments that permit exposure of vegetation to gases, particles, and/or aqueous pollutants at 'realistic' concentrations? (2) Can we include the potential interactions with photolytically derived free radicals, and the dynamics of exchange? (3) How do we allow for responses to pollutant mixtures, or the simultaneous exposure to pollutants in gas, particle, and aqueous phases? The recognition of the importance of the dynamic exchange of pollutants between phases will be the key to the development of effective experimental approaches to evaluating cause-effect relationships between pollutant mixtures and ecosystem responses.