Chemistry-climate interactions of aerosol nitrate from lightning

Abstract

Lightning represents one of the dominant emission sources for NOx in the troposphere. The direct release of oxidised nitrogen in the upper troposphere does not only affect ozone formation, but also chemical and microphysical properties of aerosol particles in this region. This study investigates the direct impact of LNOx emissions on upper-tropospheric nitrate using a global chemistry climate model. The simulation results show a substantial influence of the lightning emissions on the mixing ratios of nitrate aerosol in the upper troposphere of more than 50 %. In addition to the impact on nitrate, lightning substantially affects the oxidising capacity of the atmosphere with substantial implications for gas-phase sulfate formation and new particle formation in the upper troposphere. In conjunction with the condensation of nitrates, substantial differences in the aerosol size distribution occur in the upper troposphere as a consequence of lightning. This has implications for the extinction properties of the aerosol particles and for the cloud optical properties. While the extinction is generally slightly enhanced due to the LNOx emissions, the response of the clouds is ambiguous due to compensating effects in both liquid and ice clouds. Resulting shortwave flux perturbations are of ∼ −100 mW m−2 as determined from several sensitivity scenarios, but an uncertainty range of almost 50 % has to be defined due to the large internal variability of the system and the uncertainties in the multitude of involved processes. Despite the clear statistical significance of the influence of lightning on the nitrate concentrations, the robustness of the findings gradually decreases towards the determination of the radiative flux perturbations.