Abstract
Time resolved nonresonant CARS (Coherent Anti-Stokes Raman Spectroscopy) is applied to probe combustion relevant species with fs time resolution under extreme conditions. The experimental transients on the prototype molecule H2 show detailed beating structures, reflecting the rotational dynamics of all thermally populated ground state J-levels with high fidelity. Modelling of the experimental data yields temperatures and pressures with high accuracy and resolution. The good agreement with values determined by frequency-domain experiments demonstrates the suitability of this method for the determination of J-dependent line-shifting coefficients in gaseous mixtures at high pressures and temperatures, where frequency-domain CARS spectra are difficult to model.
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