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

JD Miller, CE Dedic, S Roy, JR Gord, TR Meyer - Optics express, 2012 - opg.optica.org
Optics express, 2012opg.optica.org
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 …
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 (~6.5 ps) after Raman excitation, thereby improving thermometric accuracy with a time- and frequency-resolved theoretical model.
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