Spatially dependent f-π exchange interaction within a single-molecule magnet TbPc2

Xin Liao, Yun Chen, Tao Xie, Rui-Jing Sun, Lian-Zhi Yang, Chao-Fei Liu, Rui Wang, Svetlana Klyatskaya, Mario Ruben, Wenhao Zhang () and Ying-Shuang Fu ()
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Xin Liao: Huazhong University of Science and Technology
Yun Chen: Nanjing University
Tao Xie: Huazhong University of Science and Technology
Rui-Jing Sun: Huazhong University of Science and Technology
Lian-Zhi Yang: Huazhong University of Science and Technology
Chao-Fei Liu: Huazhong University of Science and Technology
Rui Wang: Nanjing University
Svetlana Klyatskaya: Karlsruhe Institute of Technology
Mario Ruben: Karlsruhe Institute of Technology
Wenhao Zhang: Huazhong University of Science and Technology
Ying-Shuang Fu: Huazhong University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract Electrically probing the spin state of localized f electrons in a rare-earth-based single-molecule magnet, along with understanding its intramolecular magnetic coupling, is of crucial importance for applications in quantum information and advanced spintronics, yet it remains experimentally challenging. Herein, within a single-molecule magnet terbium(III) bis(phthalocyaninato) (TbPc2) double-decker molecule adsorbed on a bilayer graphene epitaxially grown on a SiC(0001) substrate, we experimentally demonstrate a spatially dependent exchange interaction between the magnetic moment of the localized Tb 4f electron and the unpaired spin of the Pc π-radical. The magnetic state of TbPc2, associated with the f-π interaction, is evidently detected through the spectroscopic Kondo resonance and a zero-field Kondo splitting, which can be reversibly switched in a charge/discharge process triggered by the tip-molecule distance. Furthermore, we theoretically describe how the Kondo resonance evolves at the molecular scale, which is mediated by the f-π exchange interaction with its strength varying spatially in a radial decay fashion. Our spatially resolved Kondo characteristics offer a quantitative understanding of the many-body spin correlation, which is coupled with the charge states in a nonuniform and spatially extended system.

Date: 2025
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DOI: 10.1038/s41467-025-61594-4

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