Abstract
Theoretical results on the rotational dependence of nonlinear parametric processes in diatomic molecules are generalized. Well-known results such as the parity of the nonvanishing nonlinear susceptibilities or the polarization effects are retrieved. Nonresonant susceptibility does not depend on the J rotational quantum number of the molecules involved in the process nor, consequently, on the temperature. It does depend on the J quantum numbers of both the ground and resonant state. The general rotational dependence of the resonant nth-order nonlinear susceptibility is derived in the general case of a single resonance. Three examples are given: /sup 1/ Sigma -/sup 1/ Pi three-photon resonant four-wave mixing, /sup 1/ Sigma -/sup 1/ Sigma two-photon resonant four-wave mixing, and /sup 2/ Pi -/sup 2/ Sigma two-photon resonant four-wave mixing. All the coefficients needed to compute the nonlinear susceptibility describing any four-wave mixing experiment are tabulated.< <ETX xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">></ETX>
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