Abstract
Expressions for the hyperpolarizabilities for second- and third-harmonic generations and for the induced Kerr effect are derived using a variation-perturbation method. This method requires only the wave function Ψ of the ground state of the unperturbed molecule and yields the hyperpolarizability tensors, the components of which are determined by a variational calculus. By using a decomposition of the molecule into loges, we show that this method allows one to make calculations on complex molecules perturbed by static and dynamic electric fields.
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