We demonstrate experimentally that coherent anti-Stokes Raman microspectroscopy with high spectral resolution is achieved using femtosecond laser pulses chirped up to a few picoseconds by glass elements of known group-velocity dispersion without significant intensity losses. By simply choosing the length of the glass, the chirp of Stokes and pump pulses is tailored to obtain a spectral resolution given by the Fourier limit of the chirped pulse duration. We show that for chirped pulse durations shorter than or comparable to the Raman coherence time, maximum signal occurs for a pump arriving after the Stokes pulse, a time-ordering effect confirmed by numerical simulations.
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Rocha‐Mendoza et al. (2008) studied this question.
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