Nonlinear optical response in higher fullerenes

TL;DR

This paper theoretically investigates the nonlinear optical properties of higher fullerenes C70, C76, C78, and C84, revealing that their nonlinearities are significantly larger than C60 and increase as the optical gap decreases.

Contribution

It provides the first theoretical analysis of nonlinear optical responses in higher fullerenes using intermediate exciton theory.

Findings

Higher fullerenes exhibit 2-3 times larger nonlinearities than C60.

Nonlinearity magnitude increases as the optical gap decreases.

Off-resonant third-harmonic-generation is effectively calculated.

Abstract

Nonlinear optical properties of extracted higher fullerenes - C70, C76, C78, and C84 - are theoretically investigated. Magnitudes of off-resonant third-harmonic-generation are calculated by the intermediate exciton theory. We find that optical nonlinearities of higher fullerenes are a few times larger than those of C60. The magnitudes of nonlinearity tend to increase as the optical gap decreases in higher fullerenes.