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Abstract: 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 NO x , SO x , 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 NO x emissions are responsible for 93% of population exposure to aircraft-attributable PM2.5. Aircraft NO x 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 NO x 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. [Copyright &y& Elsevier]