Quasiparticle breakdown in a quantum spin liquid

Much of modern condensed matter physics is understood in terms of elementary excitations, or quasiparticles-fundamental quanta of energy and momentum(1,2). Various strongly interacting atomic systems are successfully treated as a collection of quasiparticles with weak or no interactions. However, there are interesting limitations to this description: in some systems the very existence of quasiparticles cannot be taken for granted. Like unstable elementary particles, quasiparticles cannot survive beyond a threshold where certain decay channels become allowed by conservation laws; their spectrum terminates at this threshold. Such quasiparticle breakdown was first predicted for an exotic state of matter-super-fluid He-4 at temperatures close to absolute zero, a quantum Bose liquid where zero-point atomic motion precludes crystallization(1-4). Here we show, using neutron scattering, that quasiparticle breakdown can also occur in a quantum magnet and, by implication, in other systems with Bose quasiparticles. We have measured spin excitations in a two-dimensional quantum magnet, piperazinium hexachlorodicuprate (PHCC)(5), in which spin-1/2 copper ions form a non-magnetic quantum spin liquid, and find remarkable similarities with excitations in superfluid He-4. We observe a threshold momentum beyond which the quasiparticle peak merges with the two-quasiparticle continuum. It then acquires a finite energy width and becomes indistinguishable from a leading-edge singularity, so that excited states are no longer quasiparticles but occupy a wide band of energy. Our findings have important ramifications for understanding excitations with gapped spectra in many condensed matter systems, ranging from band insulators to high-transition-temperature superconductors(6).