NOx Production by Ionisation Processes in Air

Abstract: The study presented in this thesis was motivated by the large uncertainty on the concentration of atmospheric electrical discharges to the global nitrogen budget. This uncertainty is partly due to the fact that information concerning the NOx production efficiency of electrical discharges having current signatures similar to those of lightning flashes is not available in the literature. Another reason for this uncertainty is the fact that energy is used as a figure of merit in evaluating NOx production from lightning flashes even though insufficient knowledge is available concerning the energy dissipation in lightning flashes. The third reason for this uncertainty is the lack of knowledge concerning the contribution of discharge processes other than return strokes to the NOx production in the atmosphere. Lightning is not the only process in the atmosphere that causes ionisation and dissociation of atmospheric air. Cosmic rays continuously bombard the Earth with high energetic particles and radiation causing ionization and dissociation of air leading to the production of NOx in the atmosphere. The work carried out in this thesis is an attempt to improve the current knowledge on the way in which these processes contribute to the global NOx production. Experiments have been conducted in this thesis to estimate the NOx production efficiency of streamer discharges, laser-induced plasma, laboratory sparks having current signatures similar to those of lightning flashes, alpha particle impact in air and finally with the lightning flash itself. The results obtained from laboratory electrical discharges show the following: (a) The NOx production efficiency, in terms of energy, of positive streamer discharges is more or less similar to those of hot discharges. (b) The NOx production efficiency of an electrical discharge depends not only on the energy but also on the peak and the shape of the current waveform. (c) The current signature is a better figure of merit in evaluating the NOx yield of electrical discharges. As a part of this thesis work a direct measurement of NOx generated by lightning flashes was conducted and the results show that slow discharge processes such as continuing currents could be the main source of NOx in lightning flashes. Concerning NOx production by other ionisation processes such as alpha particle impacts in the atmosphere, the data gathered in this thesis show that each ionising event in air leads to the creation of one NOx molecule. In terms of energy the NOx production efficiency of alpha particles is similar to that of electrical discharges. The theoretical studies conducted within this thesis indicate that M-components contribute more than the return strokes to the NOx production. The calculations also show that the contribution to the global NOx budget by return stroke is not as high as that assumed in the current literature.