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Neutron scattering signatures of a quantum spin ice

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 Added by Romain Sibille
 Publication date 2019
  fields Physics
and research's language is English




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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.



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Motivated by recent synthesis of the hyper-honeycomb material $beta$-$mathrm{Li_2 Ir O_3}$, we study the dynamical structure factor (DSF) of the corresponding 3D Kitaev quantum spin-liquid (QSL), whose fractionalised degrees of freedom are Majorana fermions and emergent flux-loops. Properties of this 3D model are known to differ in important ways from those of its 2D counterpart -- it has finite-temperature phase transition, as well as distinct features in Raman response. We show, however, that the qualitative behaviour of the DSF is broadly dimension-independent. Characteristics of the 3D DSF include a response gap even in the gapless QSL phase and an energy dependence deriving from the Majorana fermion density of states. Since the majority of the response is from states containing a single Majorana excitation, our results suggest inelastic neutron scattering as the spectroscopy of choice to illuminate the physics of Majorana fermions in Kitaev QSLs.
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.
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.
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.
We use numerical linked cluster (NLC) expansions to compute the specific heat, C(T), and entropy, S(T), of a quantum spin ice model of Yb2Ti2O7 using anisotropic exchange interactions recently determined from inelastic neutron scattering measurements and find good agreement with experimental calorimetric data. In the perturbative weak quantum regime, this model has a ferrimagnetic ordered ground state, with two peaks in C(T): a Schottky anomaly signalling the paramagnetic to spin ice crossover followed at lower temperature by a sharp peak accompanying a first order phase transition to the ferrimagnetic state. We suggest that the two C(T) features observed in Yb2Ti2O7 are associated with the same physics. Spin excitations in this regime consist of weakly confined spinon-antispinon pairs. We suggest that conventional ground state with exotic quantum dynamics will prove a prevalent characteristic of many real quantum spin ice materials.
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