Single-Beam Coherent Anti-Stokes Raman Scattering (CARS) Spectroscopy with Tailored Ultrashort Laser Pulses

The feasibility of single-beam coherent anti-Stokes Raman scattering (CARS) spectroscopy of gas-phase diatomic molecules related to combusting flows and the implications for gas-phase thermometry are explored. 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 to be considered for reliable single-shot measurements at flame temperatures.