Abstract This work studies the vibrational kinetics of CO2/N2 mixtures in a nanosecond pulsed near atmospheric pressure plasma jet. Quantum-cascade laser absorption spectroscopy is used to measure the populations of rovibrationally excited states of CO2 without any assumption on a particular vibrational distribution function and with a variable time resolution of as high as 8 ns. These studies are complemented by measurements using electric field induced second harmonic generation and electrical measurements to characterize the discharge. The nanosecond pulsing, combined with fast diagnostics, allows for a temporal separation of processes on different timescales, namely, electron impact excitation (e-V) during the discharge and vibrational-vibrational (V-V) and vibrational-translational (V-T) transfer in the afterglow. During the discharge, the Fermi resonant 10 0 01 state is excited at a higher rate than the energetically close 02 2 01 state of the bending mode, leading to different effective vibrational temperatures. In the afterglow, the two vibrational temperatures converge to a combined vibrational temperature T 12 within 200 ns . This equilibration process is observed here for the first time. In the afterglow, the populations of all vibrational states increase for several 10 μ s . This can be attributed to the V-V transfer from N2 to the asymmetric stretch mode of CO2 and from the latter to the other vibrational modes of CO2. An increase of the N2 admixture, which acts as an energy reservoir for the CO2, enhances the increase of the vibrational populations of CO2 in the afterglow and slows down the decay of the asymmetric mode in the late afterglow through continuous replenishment via V-V transfer. The combined data of all diagnostics allow for a detailed comparison with kinetic models.
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