Global Burden of Tropospheric Ozone: Effects of Particulate Nitrate Photolysis and Assimilation of NO2 Measurements

Tropospheric ozone is a major pollutant, a greenhouse gas, and the primary source of the hydroxyl radical. It is largely produced in situ from the oxidation of CO and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2). Global atmospheric chemistry models generally underestimate NOx and CO concentrations in the northern hemisphere away from source regions, which would lead to an underestimate in the tropospheric ozone burden. Here we evaluate the tropospheric ozone simulation in the GEOS-Chem model (version 14) using observations from satellite, aircraft, and ozonesondes. We include GEOS-Chem simulations conducted in the standard offline mode, as well as in the online mode within the NASA GEOS earth system model which forms the basis for the GEOS Composition Forecasts (GEOS-CF). In both configurations, GEOS-Chem underestimates ozone concentrations in the northern midlatitude free troposphere in spring and summer. We find that we can improve the ozone simulation by including an additional NOx source over the oceans from particulate nitrate photolysis on sea salt aerosols at rates inferred from field studies over the Atlantic Ocean. We investigate whether further improvements in the ozone simulation can be achieved by assimilating satellite measurements of NO2 from the Ozone Monitoring Instrument (OMI) and CO from the Measurement of Pollution in the Troposphere (MOPITT) instruments.