The effects of broadband excitation employing femtosecond laser pulses on the coherent anti-Stokes Raman scattering (CARS) spectroscopy of N2 are investigated. We have previously demonstrated that the dephasing rate of the coherence, established by the impulsive excitation of N2 using femtosecond pump and Stokes beams, can be used for measuring gas-phase temperature in chemically reacting flows. The objective of the current work is to investigate the effects of polarization beating ...
The feasibility is explored by single-beam coherent anti-Stokes Raman scattering CARS spectroscopy of gas-phase diatomic molecules related to combusting flows, with implications for gas-phase thermometry. We demonstrate CARS of gas-phase N2 using a shaped 7 fs laser pulse, investigate the dependence of the CARS signal on the total pressure of the probed environment, both in pure N2 and in mixtures with Ar, discuss the observed signal-to-noise ratio, and suggest improvements ...