Present-day and future lightning, and its impact on tropospheric chemistry

Lightning represents a key interaction with climate through its production of nitrogen oxides (NOx) which lead to ozone production. These NOx emissions are generally calculated interactively in chemistry-climate models but there has been little development of the representation of the lightning processes since the 1990s. In most models the parametrisation of lightning is based upon simulated cloud-top height. The aims of the thesis are: to explore existing schemes, and develop a new process-based scheme, to parametrise lightning; to use a new process-based lightning scheme to give insights regarding the role of lightning NOx in tropospheric chemistry; and to use alternative lightning schemes to improve the understanding of the response of lightning to climate change, and the consequent impacts on tropospheric chemistry. First, a new lightning parametrisation is developed using reanalysis data and satellite lightning observations which is based on upward cloud ice flux. This parametrisation is more closely linked to thunderstorm charging theory. It greatly improves the simulated zonal distribution of lightning compared to the cloud-top height approach, which overestimates lightning in the tropics. The new lightning scheme is then implemented in a chemistry-climate model, the UK Chemistry and Aerosol model (UKCA). It is evaluated against ozone sonde measurements with broad global coverage and improves the simulation of the annual cycle of upper tropospheric ozone concentration, compared to ozone simulated with the cloud-top height approach. This improvement in simulated ozone is attributed to the change in ozone production associated with the improved zonal distribution of simulated lightning. Subsequently, data from a chemistry-climate model intercomparison project (ACCMIP) are used to study the state-of-the-art in lightning NOx parametrisation along with its response to climate change. It is found that the models using the cloud-top height approach produce a very similar response of lightning NOx to changes in global mean surface temperature of +0.44± 0.05 TgNK-1, for a baseline emission of 5 TgN yr-1. However, two models using two alternative lightning schemes produce a weaker and a negative response of lightning to climate change. Finally, simulations in a future climate scenario for year 2100 in the UKCA model were performed with the cloud-top height and the ice flux parametrisations. The lightning response to climate change when using the cloud-top height scheme is in good agreement with the positive response found in the multi-model results of the cloud-top height approach. However, the new ice flux approach suggests that lightning will decrease in future. These opposing responses introduce large uncertainty into the projections of tropospheric ozone and methane lifetime in the future scenario. An analysis of the radiative forcing from these two species also shows the large uncertainty in the individual methane and ozone radiative forcings in the future. Due to the opposite effect that lightning NOx has on methane (loss) and ozone (production) the net radiative forcing effect of lightning in present-day and future is found to be close to zero. However, there is a small positive feedback suggested by the results of the cloud-top height approach, whereas no feedback is evident with the ice flux approach. These results show there are large and crucial uncertainties introduced by lightning parametrisation choice, not only in terms of the actual lightning distribution but also atmospheric composition and radiative forcing. The new ice-based parametrisation developed here offers a good alternative to the widely-used approach and can be used in future to model lightning and develop the understanding of associated uncertainties.