Ultra-long-range spin coupling in graphene revealed by atomically resolved spin excitations

Abstract Magnetic interactions between localized spins-½ play a central role in quantum magnetism, spin-based quantum computing, and quantum simulation. The range and strength of these interactions are key figures of merit. Here, we probe exchange interactions in pairs of spins-½ introduced by chemisorption of individual hydrogen atoms on graphene. Using scanning tunneling microscopy and inelastic electron tunneling spectroscopy, supported by large-scale mean-field Hubbard calculations, we demonstrate 3 meV exchange couplings at separations beyond 10 nm, surpassing all prior systems. The couplings can be ferro- or antiferromagnetic depending on the relative sublattice arrangement. Real-space mapping of spin excitation amplitudes enables characterization with atomic-resolution. Through atomic manipulation we extend this control to spin trimers, revealing collective spin excitations when pairwise exchange couplings are comparable.