Temperature evolution in a pulsed CO2–N2 glow discharge measured using quantum cascade laser absorption spectroscopy

Abstract

This work uses in situ narrowband quantum cascade laser (QCL) absorption spectroscopy to study the effect of N2 on the time evolution of gas temperature, rotational temperature and the vibrational temperatures of CO2 and CO in a pulsed glow discharge. Three colinear QCLs are used to scan three regions of about 1 cm−1 between 2179.20 and 2253.51 cm−1, including transitions up to the asymmetric stretch level v3 = 6, as well as (vCO) → (vCO + 1) CO transitions up to vCO = 1. A fitting routine is used to extract temperatures from the measured absorption spectra. The time resolved measurements are performed in CO2, admixed with up to 90% N2, with the plasma operated with a 5–10 ms on-off cycle, a discharge current of 50 mA and a pressure of around 6.7 mbar. The time evolution of the gas temperature has been measured and agrees well with the time evolution of the rotational temperature. The asymmetric stretch vibrational temperature T3 of CO2 reaches a maximum of 1060 K at 0.7 ms for pure CO2, while T3 goes up to 2250 K for a N2 content of 90% and stays constant until the plasma is switched off. Both T3 and the vibrational temperature of CO TCO show a clear non-equilibrium with respect to the rotational temperature Trot. Both do not equilibrate with the rotational temperature Trot between consecutive plasma cycles for a N2 content above 70%, although T3 and TCO always equilibrate with each other in the afterglow. The symmetric stretch and bending mode temperature T12 is elevated more with respect to the rotational temperature for increasing N2 content, while the maximum of the rotational temperature decreases for increasing N2 admixtures, which might be attributed to the energy stored in the vibrational modes of N2, CO2 and CO. Additionally, an indication of an increase in the total pressure during the plasma on-time due to heating and a subsequent decrease in the afterglow due to cooling was found for a pure CO2 plasma.