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A new mechanism for increasing the third-order nonlinear optical susceptibility, (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 III͒ relative to empty-cage fullerenes. A value of Ϫ8.7ϫ10 Ϫ32 esu is found for the molecular susceptibility, ␥ xyyx , of Er 2 @C 82 compared to previously reported values of ␥ xxxx ϭ3ϫ10 Ϫ34doi:10.1063/1.121456 fatcat:rsmftpeqzrepth5c3c22rxmzbe