Ionic Raman Effect. III. First- and Second-Order Ionic Raman Effects

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Abstract
The modulation of the ionic, rather than the electronic, contribution to the crystal polarizability by the atomic displacements is the dominant mechanism for scattering light when the incident light is in the infrared, and it is the ionic Raman effect that is studied in this paper. The problem considered is the effect of the second-order dipole moment on one- and two-phonon scattering spectra, in addition to the effect of the first-order dipole moment. An expression for the scattering efficiency is obtained and an order-of-magnitude estimate is included for the case of one-phonon scattering and for the case of two-phonon scattering in a crystal that passesses no first-order dipole moment. In the case of a crystal which also possesses a first-order dipole moment, there are additional contributions to the scattering efficiency, but these contributions are discussed qualitatively.

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