Abstract
The first Raman spectrograms are reported for fifth order coherent anti-Stokes Raman scattering. The 992 cm −1 `ring breathing' mode of liquid benzene is examined using broadband, nontransform-limited, quasi-cw noisy laser light. The fifth order signal is entirely dominated by a sequential CARS process called I (3)SCARS. The vibrational Raman frequency and the dephasing rate constant for this mode is extracted from combined I (3)SCARS and I (2)CARS spectrograms with high precision and potentially high accuracy.
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