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Fig. 9.3 Scheme of pump-DFWM in the excited potential surface and the generation of CARS
(as well as CSRS) spectra during the relaxation. For each delay between the initial pump and the
DFWM sequence (delay T ), a DFWM transient is obtained by varying the delay τ 23 . After Fourier
transformation of each transient, snapshots of the vibrational spectra can be plotted during the
relaxation on the excited potential surface
to measure two complementary wavelengths. The main drawback of this setup is that
the signal amplitude at different detection wavelengths cannot be directly compared
due to different detection parameters in each detector (e.g. photomultiplier amplifi-
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