Spin-orbital Yu-Shiba-Rusinov states in single Kondo molecular magnet

Hui-Nan Xia, Emi Minamitani, Rok Žitko, Zhen-Yu Liu, Xin Liao, Min Cai, Zi-Heng Ling, Wen-Hao Zhang, Svetlana Klyatskaya, Mario Ruben and Ying-Shuang Fu ()
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Hui-Nan Xia: Huazhong University of Science and Technology
Emi Minamitani: Institute for Molecular Science
Rok Žitko: Jožef Stefan Institute
Zhen-Yu Liu: Huazhong University of Science and Technology
Xin Liao: Huazhong University of Science and Technology
Min Cai: Huazhong University of Science and Technology
Zi-Heng Ling: Huazhong University of Science and Technology
Wen-Hao Zhang: Huazhong University of Science and Technology
Svetlana Klyatskaya: Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT)
Mario Ruben: Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT)
Ying-Shuang Fu: Huazhong University of Science and Technology

Nature Communications, 2022, vol. 13, issue 1, 1-7

Abstract: Abstract Studies of single-spin objects are essential for designing emergent quantum states. We investigate a molecular magnet Tb2Pc3 interacting with a superconducting Pb(111) substrate, which hosts unprecedented Yu-Shiba-Rusinov (YSR) subgap states, dubbed spin-orbital YSR states. Upon adsorption of the molecule on Pb, the degeneracy of its lowest unoccupied molecular orbitals (LUMO) is lifted, and the lower LUMO forms a radical spin via charge transfer. This leads to Kondo screening and subgap states. Intriguingly, the YSR states display two pairs of resonances with clearly distinct behavior. The energy of the inner pair exhibits prominent inter and intra molecular variation, and it strongly depends on the tip height. The outer pair, however, shifts only slightly. As is unveiled through theoretical calculations, the two pairs of YSR states originate from the ligand spin and charge-fluctuating higher LUMO, coexisting in a single molecule, but only weakly coupled presumably due to different spatial distribution. Our work paves the way for understanding complex many-body excitations and constructing molecule-based topological superconductivity.

Date: 2022
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DOI: 10.1038/s41467-022-34187-8

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