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Enhanced Quantum-Confined Stark Effect in Sc3N@Ih-C80 Fullerene Dimers Via Intermolecular Coupling
Shaohua Wei1, Xiaowei Yang2, Yang Zhao3
1Key Laboratory of Materials Modification by Laser, Ion and Electron Beams (Dalian University of Technology), Ministry of Education, Dalian116024, China.
None:
The modulation of molecular excited states and luminescence properties by external electric fields provides a fundamental physical basis for developing tunable optical and quantum functional devices at the molecular scale. In this work, density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations were employed to investigate the electric-field response of the quantum-confined Stark effect (QCSE) in a covalently [2 + 2] cycloaddition-bridged Sc3N@Ih-C80 endohedral metallofullerene dimer. The results showed that, compared with the monomer, covalent bridging significantly enhances the electric-field tunability of energy levels. In the low-to-moderate field regime, the response is mainly governed by the polarizability term, whereas stronger fields promote electron-hole separation and exciton evolution from a Frenkel to a charge-transfer type. These findings elucidate the underlying physical mechanism of electric-field regulated excited states in assembled endohedral metallofullerene dimers and provide theoretical guidance for the design of molecular-scale optoelectronic and quantum devices.
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