The Local Field Factor and Microscopic Cascading: A Self-Consistent Method Applied to Confined Systems of Molecules

TL;DR

This paper presents a self-consistent method to analyze microscopic cascading effects in nonlinear optics, emphasizing geometric constraints and applying it to thin films of C60 molecules to estimate their fifth-order susceptibility.

Contribution

It introduces a simplified self-consistent approach that captures microscopic cascading contributions in high-order nonlinear susceptibilities, considering geometric effects.

Findings

Microscopic cascading significantly influences fifth-order susceptibilities.

Geometric constraints alter cascading contributions and enable new material design options.

The method effectively estimates susceptibilities in C60 thin films.

Abstract

We use a simplified self-consistent method to address nonlinear-optical cascading phenomena, which shows added microscopic cascading contributions in high-ordered nonlinear susceptibilities through fifth order. These cascading terms in the microscopic regime encompass all possible scalar cascading configurations. The imposition of geometric constraints further influences the predicted cascading contributions and opens up additional design parameters for nonlinear-optical materials. These results are used in approximating the effective fifth-order susceptibility in thin films of C60 monomers of varying thickness and concentration. This paper contains the corrections to the original paper that appeared in the Journal of Physics B as reflected in the content of the corrigendum that followed.