The paper presents results of time-resolved rotational temperature measurements, by pure rotational coherent anti-Stokes Raman spectroscopy and absolute O atom number density measurements, by two-photon absorption laser induced fluorescence. The experiments were conducted in nanosecond pulse discharges in H2–O2–Ar and C2H4–O2–Ar mixtures, initially at room temperature, operated at a high pulse repetition rate of 40 kHz, in a plane-to-plane double dielectric barrier geometry at a pressure of 40 Torr. Intensified charge-coupled device images show that O2–Ar and H2–O2–Ar plasmas remain diffuse and volume-filling during the entire burst. Images taken in C2H4–O2–Ar plasma demonstrate significant discharge filamentation and constriction along the center plane and in the corners of the test section. The experimental results demonstrate high accuracy of pure rotational psec CARS for thermometry measurements at low partial pressures of oxygen in nonequilibrium plasmas. The results are compared with kinetic modeling calculations, using two different H2–O2 chemistry and C2H4–O2 chemistry mechanisms. In H2–O2–Ar mixtures, the kinetic modeling predictions are in fairly good agreement with the data, predicting temperature rise and O atom accumulation in long discharge bursts, up to 450 pulses. The results show that adding hydrogen to the mixture results in an additional temperature rise, due to its partial oxidation by radicals generated in the plasma, essentially without chain branching. In C2H4–O2–Ar mixtures, the model consistently underpredicts both temperature and O atom number density. The most likely reason for the difference between the experimental data and model predictions is discharge filamentation developing when ethylene is added to the O2–Ar mixture, at fairly low temperatures.
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