Abstract

Vibrational excitation of N2 beyond thermodynamic equilibrium enhances the reactivity of this molecule and the production of radicals. Experimentally measured temporal and spatial profiles of gas and vibrational temperature show that strong vibrational non-equilibrium is found in a pulsed microwave discharges at moderate pressure (25 mbar) in pure N2 outside the plasma core and as an effect of power pulsing. A one dimensional radial time-resolved self-consistent fluid model has been developed to study the mechanism of formation of vibrationally excited N2. In addition to the temperature maps, time-resolved measurements of spontaneous optical emission, electron density and electron temperature are used to validate the model and the choice of input power density. The model reveals two regions in the plasma: a core where chemistry is dominated by power deposition and where vibrational excitation starts within the first ∼10 µs and an outer region reliant on radial transport, where vibrational excitation is activated slowly during the whole length of the pulse (200 µs). The two regions are separated by a sharp gradient in the estimated deposited power density, which is revealed to be wider than the emission intensity profile used to estimate the plasma size. The low concentration of excited species outside the core prevents the gas from heating and the reduced quenching rates prevent the destruction of vibrationally excited N2, thereby maintaining the observed high non-equilibrium.

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