Abstract

The frequency-dependent susceptibilities describing the nonlinear-optical properties of individual molecules or of clusters of molecules outside resonances may be calculated either by using the well-known sum-over-states expressions or by solving consecutive systems of coupled inhomogeneous linear equations. The respective advantages and disadvantages of the two procedures are discussed. In the calculation of molecular aggregates the influence of intermolecular interactions is of central importance. An engineering model is proposed that invokes periodic boundary conditions and that considers the electrostatic interaction between neighboring molecules. The multipole expansion is broken off after the dipole–dipole terms.

© 1989 Optical Society of America

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