Published online by Cambridge University Press: 25 February 2011
The low energy part of the linear optical response spectrum and lowest order hyperpolarizability γ(3) of C60 are calculated by a sum over state approach using single particle wavefunctions and. energy levels determined from local density calculations. Lorentz local field factors, as well as a RPA correction are introducedto facilitate comparison with the dielectric function ε(ω) determined fromfilms of C60. γ( 2 ) for a centrosymmetric molecule such asC60 is zero and the lowest non-zero contribution to the polarizability is γ( 3 ). Reasonable agreement is found with linear optical response experiments if a RPA screening is used. However, SHG and THG experiments on C60 in solid or solution form, yields values closer to the unscreened results.
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