Source attribution of tropospheric ozone

Abstract:

Tropospheric ozone is a harmful pollutant with adverse effects on human health and ecosystems. As well as these effects, tropospheric ozone is also a powerful greenhouse gas, with an anthropogenic radiative forcing one quarter of that of CO2. Along with methane and atmospheric aerosol, tropospheric ozone belongs to the so-called Short Lived Climate forcing Pollutants, or SLCP. Recent work has shown that efforts to reduce concentrations of SLCP in the atmosphere have the potential to slow the rate of near-term climate change, while simultaneously improving public health and reducing crop losses. Unlike many other SLCP, tropospehric ozone is not directly emitted, but is instead influenced by two distinct sources: transport of air from the ozone-rich stratosphere; and photochemical production in the troposphere from the emitted precursors NOx (oxides of nitrogen), CO (Carbon Monoxide), and VOC (volatile organic compounds, including methane).

Better understanding of the relationship between ozone production and the emissions of its precursors is essential for the development of targeted emission reduction strategies. Several modeling methods have been employed to relate the production of tropospheric ozone to emissions of its precursors; emissions perturbation, tagging, and adjoint sensitivity methods all deliver complementary information about modelled ozone production. Most studies using tagging methods have focused on attribution of tropospheric ozone production to emissions of NOx, even though perturbation methods have suggested that tropospheric ozone is also sensitive to VOC, particularly methane.

In this study we describe the implementation into a global chemistry-climate model of a scheme for tagging emissions of NOx and VOC with an arbitrary number of labels, which are followed through the chemical reactions of tropospheric ozone production in order to perform attribution of tropospehric ozone to its emitted precursors. Attribution is performed to both geographical regions and to emission sectors. Source-receptor relationships are defined for intercontinental transport of ozone and its precursors, and the relative contributions of NOx, methane, CO, NMVOC, and stratosphere-troposphere exchange to tropospheric background ozone are determined.