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

TL;DR

This paper develops a self-consistent model for off-resonant nonlinear optical cascading in mesoscopic thin films and guest-host systems, revealing how geometry and boundary effects enhance higher-order susceptibilities.

Contribution

It introduces a new microscopic cascading model that accounts for geometrical and boundary effects in nonlinear optical responses of mesoscopic systems.

Findings

Higher-order susceptibilities are enhanced by geometrical and boundary orientation effects.

The model demonstrates dependence of nonlinear response on excitation beam structure.

Simplified derivation of cascading effects in guest-host systems is provided.

Abstract

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.