Regulation of quantum spin conversions in a single molecular radical.

Autor: Yang C; Beijing National Laboratory for Molecular Sciences, National Biomedical Imaging Centre, College of Chemistry and Molecular Engineering, Peking University, Beijing, P. R. China.; School of Materials Science and Engineering, Peking University, Beijing, P. R. China., Chen Z; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China., Yu C; Department of Chemical Physics, University of Science and Technology of China, Hefei, P. R. China., Cao J; Beijing National Laboratory for Molecular Sciences, National Biomedical Imaging Centre, College of Chemistry and Molecular Engineering, Peking University, Beijing, P. R. China., Ke G; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China., Zhu W; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China., Liang W; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China., Huang J; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China., Cai W; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China., Saha C; Dave C. Swalm School of Chemical Engineering and Centre for Advanced Vehicular Systems, Mississippi State University, Mississippi State, MS, USA., Sabuj MA; Dave C. Swalm School of Chemical Engineering and Centre for Advanced Vehicular Systems, Mississippi State University, Mississippi State, MS, USA., Rai N; Dave C. Swalm School of Chemical Engineering and Centre for Advanced Vehicular Systems, Mississippi State University, Mississippi State, MS, USA., Li X; Department of Chemical Physics, University of Science and Technology of China, Hefei, P. R. China. lixx@ustc.edu.cn., Yang J; Department of Chemical Physics, University of Science and Technology of China, Hefei, P. R. China., Li Y; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China. celiy@scut.edu.cn., Huang F; Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, P. R. China. msfhuang@scut.edu.cn., Guo X; Beijing National Laboratory for Molecular Sciences, National Biomedical Imaging Centre, College of Chemistry and Molecular Engineering, Peking University, Beijing, P. R. China. guoxf@pku.edu.cn.; Centre of Single-Molecule Sciences, Institute of Modern Optics, Frontiers Science Centre for New Organic Matter, Tianjin Key Laboratory of Micro-scale Optical Information Science and Technology, College of Electronic Information and Optical Engineering, Nankai University, Tianjin, P. R. China. guoxf@pku.edu.cn.
Jazyk: angličtina
Zdroj: Nature nanotechnology [Nat Nanotechnol] 2024 Jul; Vol. 19 (7), pp. 978-985. Date of Electronic Publication: 2024 Mar 06.
DOI: 10.1038/s41565-024-01632-2
Abstrakt: Free radicals, generally formed through the cleavage of covalent electron-pair bonds, play an important role in diverse fields ranging from synthetic chemistry to spintronics and nonlinear optics. However, the characterization and regulation of the radical state at a single-molecule level face formidable challenges. Here we present the detection and sophisticated tuning of the open-shell character of individual diradicals with a donor-acceptor structure via a sensitive single-molecule electrical approach. The radical is sandwiched between nanogapped graphene electrodes via covalent amide bonds to construct stable graphene-molecule-graphene single-molecule junctions. We measure the electrical conductance as a function of temperature and track the evolution of the closed-shell and open-shell electronic structures in real time, the open-shell triplet state being stabilized with increasing temperature. Furthermore, we tune the spin states by external stimuli, such as electrical and magnetic fields, and extract thermodynamic and kinetic parameters of the transition between closed-shell and open-shell states. Our findings provide insights into the evolution of single-molecule radicals under external stimuli, which may proof instrumental for the development of functional quantum spin-based molecular devices.
(© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)
Databáze: MEDLINE
Externí odkaz: