Abstract

Interference-free hybrid femtosecond/picosecond vibrational coherent anti-Stokes Raman scattering (CARS) of nitrogen is reported for temperature measurements of 1300–2300 K in high-pressure, laminar H2–air and CH4–air diffusion flames up to 10 bar. Following coherent Raman excitation by 100 fs duration pump and Stokes pulses, a time-asymmetric probe pulse is used for the detection of spectrally resolved N2 CARS signals at probe delays as early as 200300  fs. This allows for full rejection of nonresonant contributions while being independent of collisions for single-shot precision of ±2% at elevated pressures. The effects of collisions at longer probe-pulse delays are also investigated to determine the feasibility of varying the detection timing from 200 fs to 100 ps.

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