Spatial sensitivities of human health risk to intercontinental and high-altitude pollution

We perform the first long-term (>1 year) continuous adjoint simulations with a global atmospheric chemistry transport model focusing on population exposure to fine particulate matter (PM2.5) and associated risk of early death. Sensitivities relevant to intercontinental and high-altitude PM pollution are calculated with particular application to aircraft emissions. Specifically, the sensitivities of premature mortality risk in different regions to NOx, SOx, CO, VOC and primary PM2.5 emissions as a function of location are computed. We apply the resultant sensitivity matrices to aircraft emissions, finding that NOx emissions are responsible for 93% of population exposure to aircraft-attributable PM2.5. Aircraft NOx accounts for all of aircraft-attributable nitrate exposure (as expected) and 53% of aircraft-attributable sulfate exposure due to the strong "oxidative coupling" between aircraft NOx emissions and non-aviation SO2 emissions in terms of sulfate formation. Of the health risk-weighted human PM2.5 exposure attributable to aviation, 73% occurs in Asia, followed by 18% in Europe. 95% of the air quality impacts of aircraft emissions in the US are incurred outside the US. We also assess the impact of uncertainty or changes in (non-aviation) ammonia emissions on aviation-attributable PM2.5 exposure by calculating second-order sensitivities. We note the potential application of the sensitivity matrices as a rapid policy analysis tool in aviation environmental policy contexts. (C) 2013 Elsevier Ltd. All rights reserved.