Ferroelectricity from spin supercurrents in LiCuVO4

We have studied the magnetic structure of the ferroelectric frustrated spin-1/2 chain material LiCuVO4 in applied electric and magnetic fields using polarized neutrons. A symmetry and mean-field analysis of the data rules out the presence of static Dzyaloshinskii-Moriya interaction, while exchange striction is shown to be negligible by our specific-heat measurements. The experimentally observed magnetoelectric coupling is in excellent agreement with the predictions of a purely electronic mechanism based on spin supercurrents.Comment: 4 pages, 3 figures, final versio

Fractional spinon excitations in the quantum Heisenberg antiferromagnetic chain

Assemblies of interacting quantum particles often surprise us with properties that are difficult to predict. One of the simplest quantum many-body systems is the spin 1/2 Heisenberg antiferromagnetic chain, a linear array of interacting magnetic moments. Its exact ground state is a macroscopic singlet entangling all spins in the chain. Its elementary excitations, called spinons, are fractional spin 1/2 quasiparticles; they are created and detected in pairs by neutron scattering. Theoretical predictions show that two-spinon states exhaust only 71% of the spectral weight while higher-order spinon states, yet to be experimentally located, are predicted to participate in the remaining. Here, by accurate absolute normalization of our inelastic neutron scattering data on a compound realizing the model, we account for the full spectral weight to within 99(8)%. Our data thus establish and quantify the existence of higher-order spinon states. The observation that within error bars, the entire weight is confined within the boundaries of the two-spinon continuum, and that the lineshape resembles a rescaled two-spinon one, allow us to develop a simple physical picture for understanding multi-spinon excitations.Comment: 22 pages, 4 figures, Supplementary material

Field-induced decay dynamics in square-lattice antiferromagnet

Dynamical properties of the square-lattice Heisenberg antiferromagnet in applied magnetic field are studied for arbitrary value S of the spin. Above the threshold field for two-particle decays, the standard spin-wave theory yields singular corrections to the excitation spectrum with logarithmic divergences for certain momenta. We develop a self-consistent approximation applicable for S >= 1, which avoids such singularities and provides regularized magnon decay rates. Results for the dynamical structure factor obtained in this approach are presented for S = 1 and S = 5/2.Comment: 12 pages, 11 figures, final versio

Evidence of a bond-nematic phase in LiCuVO4

Polarized and unpolarized neutron scattering experiments on the frustrated ferromagnetic spin-1/2 chain LiCuVO4 show that the phase transition at HQ of 8 Tesla is driven by quadrupolar fluctuations and that dipolar correlations are short-range with moments parallel to the applied magnetic field in the high-field phase. Heat-capacity measurements evidence a phase transition into this high-field phase, with an anomaly clearly different from that at low magnetic fields. Our experimental data are consistent with a picture where the ground state above HQ has a next-nearest neighbour bond-nematic order along the chains with a fluid-like coherence between weakly coupled chains.Comment: 5 pages, 4 figures. To appear in Phys. Rev. Let

Hierarchy of exchange interactions in the triangular-lattice spin-liquid YbMgGaO4_{4}

The spin-1/2 triangular lattice antiferromagnet YbMgGaO$_{4}$ has attracted recent attention as a quantum spin-liquid candidate with the possible presence of off-diagonal anisotropic exchange interactions induced by spin-orbit coupling. Whether a quantum spin-liquid is stabilized or not depends on the interplay of various exchange interactions with chemical disorder that is inherent to the layered structure of the compound. We combine time-domain terahertz spectroscopy and inelastic neutron scattering measurements in the field polarized state of YbMgGaO$_{4}$ to obtain better microscopic insights on its exchange interactions. Terahertz spectroscopy in this fashion functions as high-field electron spin resonance and probes the spin-wave excitations at the Brillouin zone center, ideally complementing neutron scattering. A global spin-wave fit to all our spectroscopic data at fields over 4T, informed by the analysis of the terahertz spectroscopy linewidths, yields stringent constraints on $g$-factors and exchange interactions. Our results paint YbMgGaO$_{4}$ as an easy-plane XXZ antiferromagnet with the combined and necessary presence of sub-leading next-nearest neighbor and weak anisotropic off-diagonal nearest-neighbor interactions. Moreover, the obtained $g$-factors are substantially different from previous reports. This works establishes the hierarchy of exchange interactions in YbMgGaO$_{4}$ from high-field data alone and thus strongly constrains possible mechanisms responsible for the observed spin-liquid phenomenology