Computation of nonlinear optical properties of molecules with large amplitude anharmonic motions. III. Arbitrary double-well potentials

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Previously, a treatment of the vibrational contribution to nonlinear optical properties for molecules with large amplitude modes in a symmetric double-minimum potential well was devised. The vibronic energies were written as a power series in the field for two limiting cases of the ratio between the field-induced energy and the zero-field splitting energy of the two lowest vibronic states. This treatment is extended here to include all values of the ratio and also an asymmetric double-well potential. It is shown that a consistent treatment of NLO effects in the general case leads to new field expansion coefficients, which are formulated in terms of the usual dipole moment and (hyper)polarizabilities. As an example, the new treatment is applied to the inversion motion of CH3- ​
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