Continuum of quantum fluctuations in a three-dimensional $S=1$ Heisenberg magnet

Abstract

Conventional crystalline magnets are characterized by symmetry breaking and normal modes of excitation called magnons with quantized angular momentum $\hslash$. Neutron scattering correspondingly features extra magnetic Bragg diffraction at low temperatures and dispersive inelastic scattering associated with single magnon creation and annihilation. Exceptions are anticipated in so-called quantum spin liquids as exemplified by the one-dimensional spin-1/2 chain which has no magnetic order and where magnons accordingly fractionalize into spinons with angular momentum $\hslash /2$. This is spectacularly revealed by a continuum of inelastic neutron scattering associated with two-spinon processes and the absence of magnetic Bragg diffraction. Here, we report evidence for these same key features of a quantum spin liquid in the three-dimensional Heisenberg antiferromagnet NaCaNi${}_2$F${}_7$. Through specific heat and neutron scattering measurements, Monte Carlo simulations, and analytic approximations to the equal time correlations, we show that NaCaNi${}_2$F${}_7$ is an almost ideal realization of the spin-1 antiferromagnetic Heisenberg model on a pyrochlore lattice with weak connectivity and frustrated interactions. Magnetic Bragg diffraction is absent and 90\% of the spectral weight forms a continuum of magnetic scattering not dissimilar to that of the spin-1/2 chain but with low energy pinch points indicating NaCaNi${}_2$F${}_7$ is in a Coulomb phase. The residual entropy and diffuse elastic scattering points to an exotic state of matter driven by frustration, quantum fluctuations and weak exchange disorder.

arXiv comment21 pages, 4 figures

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