Kinetics of metastable N2(A3Σu + , v) molecules in high-pressure nonequilibrium plasmas

Abstract

Absolute, time-resolved populations of N2(A3Σu +, v = 0–5) vibrational levels in high-pressure ns pulse discharge plasmas are measured by Tunable Diode Laser Absorption Spectroscopy (TDLAS). The diffuse plasma is generated by a repetitively pulsed, double dielectric barrier, ns discharge across a 10 mm gap in a plane-to-plane geometry, at pressures of up to 400 Torr. The results of TDLAS measurements in nitrogen and in H2–N2, O2–N2, and NO–N2 plasmas are compared with kinetic modeling predictions, identifying the mechanisms of N2(A3Σu +) generation and decay during the discharge pulses and in the afterglow. Comparison with the modeling predictions indicates that electron impact dissociation of N2 from the ground electronic state significantly underpredicts the yield of N atoms. The present data suggest that N2 dissociation in the plasma also occurs during the energy pooling process in collisions of two N2(A3Σu +) molecules. The results also show that high-pressure, high repetition rate, volume-scalable ns pulse discharges can be used for efficient generation of atomic species for plasma chemical and plasma catalysis syntheses. In an NO–N2 mixture, it is shown that the N2(A3Σu +) decay is controlled by the rapid energy transfer to NO, resulting in its electronic excitation and UV emission (NO γ bands). The diagnostics used in the present work can be used for the accurate characterization of both high-pressure, low-temperature gas discharge plasmas and high-temperature nonequilibrium flows generated in pulsed facilities such as shock tubes and expansion tunnels.