Abstract

This is the first reported observation of a second-order Raman spectrum by means of coherent Raman spectroscopy. Optically heterodyned Raman-induced Kerr-effect spectroscopy was used to study the two-phonon Raman peaks of a highly fluorescent sample of diamond with sensitivity exceeding that obtained in spontaneous scattering or other forms of coherent Raman techniques. The frequency of the one-phonon peak was measured to be 1333.1 ± 0.5 cm⁻¹. The frequency of the sharp two-phonon peak was measured to be 2668.6 ± 0.5 cm⁻¹, in agreement with lower-resolution spontaneous-scattering measurements.

© 1978 Optical Society of America

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