Degenerate Four-Wave Mixing as a Nonlinear Optical Probe of the Fullerenes

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Abstract
Time-resolved degenerate four-wave mixing experiments were conducted on pure C60 and chemically modified C60 using a picosecond tunable dye laser. Photopolymerization, oxygen doping or formation of charge transfer complexes in the ground or excited states were used to alter the electronic and chemical structure of C60. The third-order optical response for C60 was largely unaffected by photopolymerization or oxygen-doping whereas significant enhancements were observed for a C60:phenylenediamine derivative charge transfer complex and for a C60/substituted-polyphenylenevinylene composite. The chemical modification of C60 has a strong influence on the dynamics of the third-order response and gives rise to differing mechanisms.