The theory, practice and applications of Coherent Raman Spectroscopy are comprehensively reviewed. In addition to the now standard Coherent Anti-Stokes Raman Spectroscopy (CARS) technique, related methods such as Raman Induced Kerr Effect Spectroscopy (RIKES), Stimulated Raman Spectroscopy (SRS) and four-wave mixing are presented in detail. An extended two-level model is employed to calculate the nonlinear polarization and third-order nonlinear susceptibility in the cases where one-photon resonances are unimportant, and the results from a complete four-level density matrix treatment are quoted for the resonant case. Also included are discussions of symmetry and focusing geometries applicable to isotropic samples and to both centrosymmetric and accentric crystals. A general formulation of signal-to-noise considerations allows a comparison of the various techniques and configurations. Applications for which the coherent Raman techniques are superior to spontaneous scattering are emphasized with citations to the pre-1979 literature.
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