Surface ferrimagnetic order in RuO2 film

Abstract

RuO2, widely proposed as a prototypical altermagnet, remains intensely debated with regard to its magnetic nature. Here, we demonstrate that RuO2 is non-magnetic in the bulk, but possesses a spontaneous surface ferrimagnetic order. Using spin- and angle-resolved photoemission spectroscopy, we directly detect a narrow surface state with identical spin polarizations at opposite momenta and at the Brillouin-zone center, incompatible with the spin texture of any altermagnetic order. First-principles calculations identify the non-magnetic bulk state and reveal that the detected magnetism is confined to the fully oxygen-terminated surface, where the charge transfer from Ru to O at surface triggers a ferrimagnetic alignment between adjacent Ru sublattices with antiparallel moments of +0.48 uB and -0.04 uB. Our findings provide a unified explanation reconciling debating reports on the magnetism of RuO2, establishing surface ferrimagnetism as the origin of the observed magnetic signals, and distinguishing it unambiguously from altermagnetism.