Emergence of Exotic Spin Texture in Supramolecular Metal Complexes on a 2D Superconductor

Designer heterostructures have offered a very powerful strategy to create exotic superconducting states by combining magnetism and superconductivity. In this Letter, we use a heterostructure platform combining supramolecular metal complexes (SMCs) with a quasi-2D van der Waals superconductor NbSe2. Our scanning tunneling microscopy measurements demonstrate the emergence of Yu-Shiba-Rusinov bands arising from the interaction between the SMC magnetism and the NbSe2 superconductivity. Using x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we show the presence of antiferromagnetic coupling between the SMC units. These result in the emergence of an unconventional 3×3 reconstruction in the magnetic ground state that is directly reflected in real space modulation of the Yu-Shiba-Rusinov bands. The combination of flexible molecular building blocks, frustrated magnetic textures, and superconductivity in heterostructures establishes a fertile starting point to fabricating tunable quantum materials, including unconventional superconductors and quantum spin liquids.