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

Yu-Shiba-Rusinov (YSR) states result from the exchange coupling between a localized magnetic moment and a superconductor. Traditionally, the YSR states have been studied for magnetic atoms. For molecular magnets with extended ligand spin, the entanglement of spin and ligand orbital gives rise to new forms of YSR excitations. Here, Xia et al uncovered spin-orbital YSR states in an unpaired ligand spin in the molecular magnet Tb2Pc3 on Pb. 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.