Abstract

We designed and synthesized amphiphilic oligo(ethylene glycolated) C60-(light-harvesting fluorene antenna) nanostructures C60(>DPAF-EG12C1) by incorporating a donor–acceptor antenna component of C60–DPAF with highly hydrophilic oligo(ethylene glycol) (EGn) side-chains to increase the amphiphilicity of the molecule. The chain length of EGn arms was selected to match with the overall molecular radius and to achieve a balance between the hydrophobicity and hydrophilicity of resulting molecules Molecular self-assembly of C60(>DPAF-EG12C1) forming bilayered fullerosome nanovesicles led to the observation of ultrafast femtosecond nonlinear optical (NLO) absorption characteristics. Two-photon absorption phenomena were found to be the dominating photophysical events showing a large molar concentration-insensitive 2PA cross-section value equivalent to 8500 GM in a form of vesicles, on average, at the estimated effective nanovesicle concentration as low as 5.5 × 10−8 MV (molecular molar concentration of 5.0 × 10−4 M) in H2O.

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