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We develop a theory of the dynamical response of a minimal model of quantum spin ice (QSI) by means of inelastic light scattering. In particular, we are interested in the Raman response of the fractionalized U(1) spin liquid realized in the XXZ QSI. We show that the low-energy Raman intensity is dominated by spinon and gauge fluctuations. We find that the Raman response in the QSI state of that model appears only in the $T_{2g}$ polarization channel. We show that the Raman intensity profile displays a broad continuum from the spinons and coupled spinon and gauge fluctuations, and a low-energy peak arising entirely from gauge fluctuations. Both features originate from the exotic interaction between photon and the fractionalized excitations of QSI. Our theoretical results suggest that inelastic Raman scattering can in principle serve as a promising experimental probe of the nature of a U(1) spin liquid in QSI.
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Quantum spin ice is an appealing proposal of a quantum spin liquid - systems where the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales. Such phases are at the edge of our current knowledge in condensed matter as they go beyond the established paradigm of symmetry-breaking order and associated excitations. Neutron scattering experiments on the pyrochlore material Pr$_2$Hf$_2$O$_7$ reveal signatures of a quantum spin ice state that were predicted by theory.
Recent work has highlighted remarkable effects of classical thermal fluctuations in the dipolar spin ice compounds, such as artificial magnetostatics, manifesting as Coulombic power-law spin correlations and particles behaving as diffusive magnetic monopoles. In this paper, we address quantum spin ice, giving a unifying framework for the study of magnetism of a large class of magnetic compounds with the pyrochlore structure, and in particular discuss Yb2Ti2O7 and extract its full set of Hamiltonian parameters from high field inelastic neutron scattering experiments. We show that fluctuations in Yb2Ti2O7 are strong, and that the Hamiltonian may support a Coulombic Quantum Spin Liquid ground state in low field and host an unusual quantum critical point at larger fields. This appears consistent with puzzling features in prior experiments on Yb2Ti2O7. Thus Yb2Ti2O7 is the first quantum spin liquid candidate in which the Hamiltonian is quantitatively known.
Long-range entanglement in quantum spin liquids (QSLs) lead to novel low energy excitations with fractionalised quantum numbers and (in 2D) statistics. Experimental detection and manipulation of these excitations present a challenge particularly in view of diverse candidate magnets. A promising probe of fractionalisation is their coupling to phonons. Here we present Raman scattering results for the S = 1/2 honeycomb iridate Cu2IrO3, a candidate Kitaev QSL with fractionalised Majorana fermions and Ising flux excitations. We observe anomalous low temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum both of which, we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at ~120 K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide for evidence of spin fractionalisation in Cu2IrO3.
We report on diffuse neutron scattering experiments providing evidence for the presence of random strains in the quantum spin ice candidate Pr2Zr2O7. Since Pr is a non-Kramers ion, the strain deeply modifies the picture of Ising magnetic moments governing the low temperature properties of this material. It is shown that the derived strain distribution accounts for the temperature dependence of the specific heat and of the spin excitation spectra. Taking advantage of mean field and spin dynamics simulations, we argue that the randomness in Pr2Zr2O7, promotes a new state of matter, which is disordered, yet characterized by short range antiferroquadrupolar correlations, and from which emerge spin-ice like excitations. This study thus opens an original research route in the field of quantum spin ice.
A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-body model of quantum tunneling. Here, we show that the tripod kagome lattice material Ho3Mg2Sb3O14 unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho3+ ground-state doublet, realizing a frustrated transverse Ising model. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at T*~0.32 K to a remarkable quantum state with three peculiarities: a continuous magnetic excitation spectrum down to T~0.12K; a macroscopic degeneracy of ice-like states; and a fragmentation of the spin into periodic and aperiodic components strongly affected by quantum fluctuations. Our results establish that Ho3Mg2Sb3O14 realizes a spin-fragmented state on the kagome lattice, with intrinsic quantum dynamics generated by a homogeneous transverse field.
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