Interference-free gas-phase thermometry at elevated pressure using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering

Rotational-level-dependent dephasing rates and nonresonant background can lead to significant uncertainties in coherent anti-Stokes Raman scattering (CARS) thermometry under high-pressure, low-temperature conditions if the gas composition is unknown. Hybrid femtosecond/picosecond rotational CARS is employed to minimize or eliminate the influence of collisions and nonresonant background for accurate, frequency-domain thermometry at elevated pressure. The ability to ignore these interferences and achieve thermometric errors of <5% is demonstrated for N-2 and O-2 at pressures up to 15 atm. Beyond 15 atm, the effects of collisions cannot be ignored but can be minimized using a short probe delay (similar to 6.5 ps) after Raman excitation, thereby improving thermometric accuracy with a time-and frequency-resolved theoretical model. (C) 2012 Optical Society of America