Density-functional-based linear and nonlinear polarizabilities of fullerene and benzene molecules.

Abstract

To address recent experiments showing a relatively large off-resonant nonlinear optical response of the fullerene molecule, we have calculated the static electronic response of fullerene molecules. While our linear polarizability is in good agreement with experimental measurements, we find that the third-order contribution is approximately one or two orders of magnitude lower than the experimental measurements. Using the same theoretical method, we have calculated the first- and third-order polarizabilities of benzene and find good agreement between our results and other experimental and theoretical results.