Excitations in the ordered and paramagnetic states of honeycomb magnet Na2Co2TeO6

Abstract: Na2Co2TeO6 is a proposed approximate Kitaev magnet, yet its actual magnetic interactions are elusive due to a lack of knowledge on the full excitation spectrum. Here, using inelastic neutron scattering and single crystals, we determine the system's temperature-dependent magnetic excitations over the entire Brillouin zone. Without committing to specific models, we unveil a distinct signature of the third-nearest-neighbor coupling in the spin waves, which signifies the associated distance as an emerging "soft link" in the ordered state. The presence of at least six non-overlapping spin-wave branches is at odds with all models proposed to date. Above the ordering temperature, persisting dynamic correlations can be described by equal-time magnetic structure factors of a hexagonal cluster, which reveal the leading instabilities. Our result sets definitive constraint on theoretical models for Na2Co2TeO6 and provides new insight for the materialization of the Kitaev model.