The past several years have seen a considerable interest in the development of photochemical molecular devices based on the combination of C₆₀ with π-conjugated oligomers. In particular, such hybrid systems have shown interesting excited state properties and have found applications in the field of solar energy conversion. Whereas the photophysical properties of a wide range of fullerene-(π-conjugated oligomer) dyads have been reported so far, research focused on related assemblies combining C₆₀ and conjugated oligomers with strong multi-photon absorption (MPA) cross sections has been probed to a lesser degree. Such hybrid systems are however potentially interesting since they should be capable of generating singlet oxygen upon multi-photon absorption followed by energy transfer to the fullerene sensitizing unit. This could broaden the applicability of C₆₀ derivatives in photodynamic therapy which is currently highly limited by both the weak linear and the low induced absorptions of fullerene-based sensitizers in the 650-750 nm region. As part of our research on compounds combining C₆₀ with π-conjugated oligomers, we now report the synthesis and the excited state properties of compound 1 assembling C₆₀ with a new MPA chromophore. In the design of the MPA dye, we have selected a star-shaped system. Actually, whereas the optimization of MPA like TPA compounds has largely focused on one-dimensional structures, it has been recently shown that increased dimensionality and branched structures lead to highly effective multiphoton absorption.

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