Nonlinear optical properties of extracted higher fullerenes – C 70 , C 76 , C 78 , and C 84 – are theoretically investigated. Magnitudes of off-resonant third-harmonic generation are calculated using the intermediate exciton theory. We find that optical nonlinearities of higher fullerenes are a few times larger than those of C 60 . The magnitudes of nonlinearity tend to increase as the optical gap decreases in higher fullerenes.
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