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Interfullerene Electronic Interactions and Excited-State Dynamics in Fullerene Dumbbell Conjugates.

Yongqiang ChaiLiping LiuYanjun XuXiaolong LiuChong WangYifan BoYuhe ZhangZhuan WangYu-Xiang WengDirk Michael GuldiBo WuChun-Ru Wang
Published in: Journal of the American Chemical Society (2023)
Several dumbbell conjugates featuring M 3 N@ I h -C 80 (M = Sc, Y) and C 60 were prepared to systematically investigate interfullerene electronic interactions and excited state dynamics. From electrochemical investigations, we concluded that the redox potentials of our M 3 N@ I h -C 80 (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 Sc 3 N@C 80 -dumbbell to yield an unprecedented (Sc 3 N@C 80 ) •+ -(Sc 3 N@C 80 ) •- 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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