Resonant optical nonlinearity of fullerenes in free-standing polymethyl methacrylate films

We have prepared films of polymethyl methacrylate in which fullerenes (a mixture of C60 and C70) are uniformly embedded. By performing both degenerate four‐wave mixing experiments and irradiance‐dependent transmission measurements with nanosecond laser pulses of 608‐nm wavelength, the third‐order nonlinear optical susceptibility of these films is determined to be of the order of 10−10 esu. This susceptibility is dominated by its imaginary part. Excited‐state absorption is the main mechanism responsible for the observed nonlinear susceptibility.

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