title: Visible-Light Photoexcited Electron Dynamics of Scandium Endohedral Metallofullerenes: The Cage Symmetry and Substituent Effects.
abstract: Endohedral metallofullerenes (EMFs) have become an important class of molecular materials for optoelectronic applications. The performance of EMFs is known to be dependent on their symmetries and characters of the substituents, but the underlying electron dynamics remain unclear. Here we report a systematic study on several scandium EMFs and representative derivatives to examine the cage symmetry and substituent effects on their photoexcited electron dynamics using ultrafast transient absorption spectroscopy. Our attention is focused on the visible-light (530 nm as a demonstration) photoexcited electron dynamics, which is of broad interest to visible-light solar energy harvesting but is considered to be quite complicated as the visible-light photons would promote the system to a high-lying energy region where dense manifolds of electronic states locate. Our ultrafast spectroscopy study enables a full mapping of the photoinduced deactivation channels involved and reveals that the long-lived triplet exciton plays a decisive role in controlling the photoexcited electron dynamics under certain conditions. More importantly, it is found that the opening of the triplet channels is highly correlated to the fullerene cage symmetry as well as the electronic character of the substituents.
authors.affiliation: †Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Beijing National Laboratory for Molecular Sciences, Beijing 100190, China.
authors.forename: Bo
authors.initials: B
authors.lastname: Wu
authors.affiliation: §Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors.forename: Jiahua
authors.initials: J
authors.lastname: Hu
authors.affiliation: §Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors.forename: Peng
authors.initials: P
authors.lastname: Cui
authors.affiliation: †Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Beijing National Laboratory for Molecular Sciences, Beijing 100190, China.
authors.forename: Li
authors.initials: L
authors.lastname: Jiang
authors.affiliation: §Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors.forename: Zongwei
authors.initials: Z
authors.lastname: Chen
authors.affiliation: §Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors.forename: Qun
authors.initials: Q
authors.lastname: Zhang
authors.affiliation: †Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Beijing National Laboratory for Molecular Sciences, Beijing 100190, China.
authors.forename: Chunru
authors.initials: C
authors.lastname: Wang
authors.affiliation: §Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.|‡Department of Theoretical Chemistry, School of Biotechnology, Royal Institute of Technology, AlbaNova, S-106 91 Stockholm, Sweden.
authors.forename: Yi
authors.initials: Y
authors.lastname: Luo
mesh_terms: D004583:Electrons; D037741:Fullerenes / Q000737:chemistry*; D008027:Light; D008958:Models, Molecular; D017785:Photons; D012538:Scandium / Q000737:chemistry*; D012993:Solar Energy
chemical_list: D037741:Fullerenes; D012538:Scandium