Impact of present and future aircraft NOx and aerosol emissions on atmospheric composition and associated direct radiative forcing of climate

Aviation NOx emissions have not only an impact on global climate by changing ozone and methane levels but also contribute to deteriorate local air quality. In order to properly assess the co-benefit with air quality improvement and the trade-off with the climate change associated with CO2, it appears essential to better quantify the climate impact of aircraft NOx emissions. A new version of the LMDZ-INCA global model, including both tropospheric and stratospheric chemistry and the sulfate-nitrate-ammonium cycle, is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. The results confirm that the efficiency of NOx to produce ozone is very much dependent on the injection height. For the baseline simulation and reference scenario this efficiency is 6.6 TgO3/TgN. The efficiency increases with the background methane and NOx concentrations and with decreasing aircraft NOx emissions. The same findings translate to the associated ozone radiative forcing which exhibits a fairly constant value per ozone mass change of 3.4 mW/m2/TgO3. The methane lifetime variation is less sensitive to the aircraft NOx emission location than the ozone change. The change in CH4 mixing ratio itself represents 75 % of the total methane forcing. The indirect changes through long-term tropospheric ozone, stratospheric water vapour and methane oxidation to CO2 contribute for 19 %, 4 % and 1 %, respectively. The net NOx radiative forcing (O3 + CH4) is largely affected by the revised CH4 radiative forcing formula which increases the total CH4 negative forcing by 15 %. As a consequence, the ozone positive forcing and the methane negative forcing largely offset each other resulting in a slightly positive forcing for the present-day. However, in the future, the net forcing turns to negative due essentially to higher methane background concentrations. Additional radiative forcings involving particle formation arise from aircraft NOx emissions since the increased OH concentrations are responsible for an enhanced conversion of SO2 to sulfate particles. Aircraft NOx emissions also increase the formation of nitrate particles in the lower troposphere. However, in the upper-troposphere, increased sulfate concentrations favor the titration of ammonia leading to lower ammonium nitrate concentrations. The total forcing from sulfate and nitrate aerosols associated with NOx emissions is negative and is estimated to -3.0 mW/m2/TgN for the present-day. When these aerosol radiative forcings are considered, the total NOx forcing turns from a positive value to a negative value even for present-day conditions. Hence, total radiative forcing from aircraft emissions associated with changes in atmospheric chemistry and direct aerosols forcings is negative for both present-day and future (2050) conditions. NOx emissions only cause a negative forcing representing about 45 % of the total forcing. The negative forcing associated with sulfates largely dominates the effect of the other particles. The sulfate direct radiative forcing is estimated to be associated for about 50 % with the direct SO2 and SO4 aircraft emissions and for about 50 % with the increased conversion of SO2 to SO4 at higher OH concentrations, and hence related to the NOx emissions. The net effect of decreasing (resp. increasing) the flight altitude by 2000 ft (about 610 m) is to increase (resp. decrease) the total negative forcing by 57 % (resp. 65 %). The variation of the total forcing with flight altitude is dominated by the high sensitivity of the ozone positive forcing to the altitude of the perturbation. Several mitigation options involving flight aircraft operation and cruise altitude changes, traffic growth, engine technology, and fuel type, exist to reduce the climate impact of aircraft NOx emissions. However, the climate forcing of aircraft NOx emissions is likely to be small or even switch to negative (cooling) depending on atmospheric NOx or CH4 future background concentrations or when the NOx impact on sulfate and nitrate particles is considered. There remain large uncertainties on the NOx net impact on climate effect calculation. Nevertheless, the results suggest that reducing aircraft NOx emissions is primarily beneficial for improving air quality. For climate consideration, one option to reduce uncertainties in mitigation strategies might be to prioritize the reduction of CO2 aircraft emissions which have a well-established and long-term impact on climate, however this reduces the overall mitigation potential.