Numerical study of pure rotational fs/ps CARS coherence beating at high pressure and for multi-species rotation-vibration non-equilibrium thermometry.

Coherent anti-Stokes Raman scattering (CARS) has long been the gold standard for non-intrusively measuring gas temperature in reacting flows such as flames and plasmas. Recently, the development of ultrafast hybrid fs/ps CARS has enabled the exploitation of coherence beating between neighboring spectral lines to simultaneously measure rotational and vibrational temperatures from a single pure rotational spectrum. However, the influence of non-Boltzmann vibrational state distributions and limitations due to collisional dephasing at pressures greater than 1 atm remains unclear. In this work, we use spectral simulations to investigate the effects of non-Boltzmann vibrational state distributions and the applicability of coherence beating at pressures up to 10 atm. We show that short probe pulses can be leveraged to quantify non-Boltzmann vibrational state distributions of N. Furthermore, we demonstrate that fs/ps CARS coherence beating can simultaneously provide sensitive measurements of rotational and vibrational temperatures of both O and N in air. A sensitivity analysis was conducted to qualitatively explain the accuracy and precision comparisons between probe delays.