Modeling off-resonant nonlinear-optical cascading in mesoscopic thin films and guest-host molecular systems

A model for off-resonant microscopic cascading of (hyper)polarizabilities is developed using a self-consistent field approach to study mesoscopic systems of nonlinear polarizable atoms and molecules. We find enhancements in the higher-order susceptibilities resulting from geometrical and boundary orientation effects. We include an example of the dependence on excitation beam cross sectional structure and a simplified derivation of the microscopic cascading of the nonlinear optical response in guest-host systems.