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

Abstract

A model for off-resonant microscopic cascading of (hyper)polarizabilities is developed using a selfconsistent 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.

Homotopy analysis method applied to second-order frequency mixing in nonlinear optical dielectric media

“….. Let us limit the study to three possible waves traveling at angular frequencies ω 1 , ω 2 , and ω 3 , where ω 1 + ω 2 − ω 3 = 0. For such cases, the only nonlinear scenario, ignoring higher-order nonlinearities from microscopic cascading effects, [31,32] occurs when two of the frequencies either add or subtract and results in the third possible frequency. Including all relevant frequency mixing terms in the nonlinear interaction summation, the three wave equations follow as…”