<title>Structure property relationships for the nonlinear optical response of fullerenes</title>

Abstract

We present a phenomenological theory of nonlinear optical response of fullerenes. An empirical tight-binding model is used in conjunction with a classical electromagnetic picture for the screening. Since in bulk media such a picture of screening corresponds to the self-consistent field approach, the only additional approximation involved in our approach is the neglect of nonlocality. We obtain reliable estimates for the linear and nonlinear susceptibilities of C60, C70, C76 and other pure carbon fullerenes and also substituted fullerenes. The relatively large values of /3 that we obtain for C76 and substituted fullerenes appear promising for the development of fullerene-based nonlinear optical materials.Our phenomenological picture of screening provides a good understanding of the linear absorption spectra of higher fullerenes and predicts that a comparison of the one-photon and multi-photon spectra will provide an insight into screening effects in these systems.