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Ultrafast dynamics and third-order nonlinearity of thin films of tert-butyl peripherally-substituted indium ph thalocyanine axially grafted polystyrene (tBu4PcIn-PS) are investigated by femtosecond optical-Kerr-effect (OKE) and z-scan experiments. The fastest component (＜ 200 fs) in the OKE traces of the film is related to the electron cloud distortion, where the phthalocyanine-polymer interaction may enhance this contribution.