Bose-Einstein condensation of a two-magnon bound state in a spin-one triangular lattice

Abstract Interactions of collective excitations often lead to rich emergent phenomena in manyparticle quantum systems. In ordered magnets, the elementary excitations are spin waves (magnons), which obey Bose-Einstein statistics. Similar to the Cooper pairs in superconductors, magnons can be paired into bound states under attractive interactions. Even more interestingly, the Zeeman coupling to a magnetic field acts as a chemical potential that can tune the particle density through a quantum critical point (QCP), beyond which a “hidden order” is predicted to exist. However, experimental confirmation of this QCP and the associated new state of matter remain elusive. Here we report direct observation of the Bose-Einstein condensation (BEC) of the two-magnon bound state in Na2BaNi(PO4)2. Comprehensive thermodynamic measurements confirmed the existence of a two-dimensional BEC-QCP at the saturation field. Inelastic neutron scattering experiments were performed to accurately establish the magnetic exchange model. An exact solution of the model found stable 2-magnon bound states that were further confirmed by an electron spin resonance (ESR) experiment, demonstrating that the QCP is due to the pair condensation and the phase below saturation field is the long-sought-after spin nematic (SN) phase.