Determination of Vibrational Contributions to Linear and Nonlinear Optical Properties

Abstract

A review of methods for calculating vibrational contributions to linear and nonlinear optical properties is presented. Our aim is to provide an overview of the various approaches that have been developed using illustrative equations supplemented with references to the detailed formulations. The treatment of electrical and mechanical anharmonicity is considered in some detail for resonant as well as non-resonant processes. Issues such as the choice of basis set, the treatment of electron correlation, and the convergence of perturbation expansions are examined. Although much of the presentation is general, there is a special emphasis on organic pi-conjugated systems.