Enhanced nonlinear optical response of an endohedral metallofullerene through metal-to-cage charge transfer

A new mechanism for increasing the third-order nonlinear optical susceptibility, X-(3), is described for endohedral metallofullerenes. A two to three orders of magnitude increase in the nonlinear response is reported for degenerate four-wave mixing experiments conducted with solutions of Er-2@C-82 (isomer III) relative to empty-cage fullerenes. A value of - 8.7x 10(-32) esu is found for the molecular susceptibility, gamma(xyyx), of Er-2@C-82 compared to previously reported values of gamma(xxxx) = 3 x 10(-34) esu and gamma(xyyx) = 4 x 10(-35) esu for C-60. The results confirm the importance of the metal-to-cage charge-transfer mechanism for enhancing the nonlinear optical response in endohedral metallofullerenes. (C) 1998 American Institute of Physics.