Single-shot fs/ns rotational CARS for temporally and spectrally resolved gas-phase diagnostics

We report thermometry and new Raman linewidth data using a novel method for time-domain rotational coherent anti-Stokes Raman spectroscopy (RCARS) on single-shot basis. The coherences are generated by two fs pulses and probed by a ns pulse. The resulting signal is detected using a combined spectrograph/streak camera setup with high spectral and temporal resolution. Rotational CARS spectrograms of nitrogen (N2), ethylene (C2H4), ethane (C2H6), and argon (Ar) are demonstrated at ambient condition. Self-broadened N2–N2 S-branch Raman linewidths were measured on single-shot basis and show excellent agreement with literature values. Furthermore, Raman linewidths of N2 S-branch perturbed by C2H4 and C2H6 were measured for the first time. The time-resolved approach was also utilized to separate complex spectra from a mixture of species through their difference in coherence lifetimes. Since the Raman coherences decay much faster for both ethane and ethylene than for nitrogen, pure nitrogen spectra could be obtained by analyzing only the temporal tail of the signal. Moreover, a model for time-resolved RCARS of N2 was developed, which employs the single-shot measured Raman linewidths to calculate the corresponding spectro-temporally resolved spectrograms at different temperatures. The model was used to evaluate the temperature from single-shot data of an N2/C2H6 mixture, showing very high accuracy. The demonstrated method constitutes an essential improvement for single-shot thermometry as it does not require pre-knowledge about collider species concentrations and their impact on linewidths