Interfullerene Electronic Interactions and Excited-State Dynamics in Fullerene Dumbbell Conjugates
Yongqiang Chai1,2, Liping Liu1,3, Yanjun Xu4,5
1Beijing National Laboratory for Molecular Sciences, Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Abstract:
Several dumbbell conjugates featuring M3N@I-C80 (M = Sc, Y) and C60 were prepared to systematically investigate interfullerene electronic interactions and excited state dynamics. From electrochemical investigations, we concluded that the redox potentials of our M3N@I-C80 (M = Sc, Y) dumbbells depend largely on the interfullerene electronic interactions. Assisted by DFT calculation, the unique role of metal atoms was highlighted. Most importantly, ultrafast spectroscopy experiments revealed symmetry-breaking charge separation in Sc3N@C80-dumbbell to yield an unprecedented (Sc3N@C80)•+-(Sc3N@C80)•- charge separated state. This is, to the best of our knowledge, the first time that symmetry-breaking charge separation following photoexcitation is corroborated in a fullerene system. As such, our work shed light on the significance of interfullerene electronic interactions and their uniqueness for modulating excited state properties.
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