GENERALIZED THEORY OF INTRAMOLECULAR COORDINATE RELAXATION IN POLYATOMIC MOLECULES

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1979

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Ohio State University

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A classical generalized theory which describes the intramolecular relaxation to a minimum energy configuration after coordinate distortion is presented. The relaxation process is described, in internal coordinate space, in terms of a minimum energy direction (MED) which provides a quadratic approximation to the minimum energy path (MEP) for unimolecular dissociation or intramolecular rearrangement. The present treatment includes the general case of distortion of an arbitrary number of coordinates in both the constrained and the unconstrained cases. In addition, the intramolecular forces which bring about the relaxation are considered, and a new bonding parameter, the relaxed interaction force constant, is discussed. Application of this formalism to several polyatomic molecules resulted in excellent agreement with experimental investigations.

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