Ising models on a pyrochlore oxide lattice are usually associated with spin ice materials and "magnetic monopoles". Ever more often effects connecting magnetic and elastic degrees of freedom are reported on these and other related frustrated materials. Here we extend a spin-ice Hamiltonian to include coupling between spins and the O$^{-2}$ ions mediating superexchange; we call it the Magnetoelastic Spin Ice model (MeSI). There has been a long search for a model in which monopoles would spontaneously become the building blocks of new ground-states: the MeSI Hamiltonian is such a model. In spite of its simplicity and classical approach, it describes (both spin and oxygen lattice) the double-layered monopole crystal observed in Tb$_2$Ti$_2$O$_7$. Remarkably, the dipolar electric moment of single monopoles emerges as a probe for magnetism. As an example we show that, in principle, pinch points related to Coulomb phases could be detected in association with the O$^{-2}$-ion displacements.
We propose the idea of a spin-lattice liquid, in which spin and lattice degrees of freedom are strongly coupled and remain disordered and fluctuating down to low temperatures. We show that such a state arises naturally from a microscopic analysis of a class of molybdate pyrochlore compounds, and is driven by a giant magnetoelastic effect. Finally, we argue that this could explain some of the experimental features of Y$_2$Mo$_2$O$_7$.
At low temperatures, Tb$_2$Ti$_2$O$_7$ enters a spin liquid state, despite expectations of magnetic order and/or a structural distortion. Using neutron scattering, we have discovered that in this spin liquid state an excited crystal field level is coupled to a transverse acoustic phonon, forming a hybrid excitation. Magnetic and phononlike branches with identical dispersion relations can be identified, and the hybridization vanishes in the paramagnetic state. We suggest that Tb$_2$Ti$_2$O$_7$ is aptly named a "magnetoelastic spin liquid" and that the hybridization of the excitations suppresses…
Motivated by puzzling aspects of spin-glass behavior reported in frustrated magnetic materials, we theoretically investigate effects of magnetoelastic coupling in geometrically frustrated classical spin models. In particular, we consider bond-disordered Heisenberg antiferromagnets on a pyrochlore lattice coupled to local lattice distortions. By integrating out the lattice degree of freedom, we derive an effective spin-only model, the bilinear-biquadratic model with bond disorder, which is analyzed by classical Monte Carlo simulations. First, we discuss the phase diagrams as well as thermodynam…
Recent experimental results have emphasized two aspects of Tb2Ti2O7 which have not been taken into account in previous attempts to construct theories of Tb2Ti2O7: the role of small levels of structural disorder, which appears to control the formation of a long-range ordered state of as yet unknown nature; and the importance of strong coupling between spin and lattice degrees of freedom, which results in the hybridization of crystal field excitons and transverse acoustic phonons. In this work we examine the juncture of these two phenomena and show that samples with strongly contrasting behavior…
We study Ising pyrochlores by means of Monte Carlo simulations. We cover a set of exchange constants ranging from the frustrated ferromagnetic case (spin-ice) to the fully-ordered "all-in--all-out" antiferromagnet in the dipolar model, reinterpreting the results --as in an ionic system-- in terms of a temperature vs. magnetic charge density phase diagram. In spite of its spin nature and the presence of both double and single non-conserved magnetic charges, the dipolar model gives place to a phase diagram which is quite comparable with those previously obtained for on-lattice systems of electri…
We report high resolution single crystal x-ray diffraction measurements of the frustrated pyrochlore magnet Tb2Ti2O7, collected using a novel low temperature pulsed magnet system. This instrument allows characterization of structural degrees of freedom to temperatures as low as 4.4 K, and in applied magnetic fields as large as 30 Tesla. We show that Tb2Ti2O7 manifests intriguing structural effects under the application of magnetic fields, including strongly anisotropic giant magnetostriction, a restoration of perfect pyrochlore symmetry in low magnetic fields, and ultimately a structural phase…
We report low-temperature thermal conductivity $κ$ of pyrochlore Yb$_2$Ti$_2$O$_7$, which contains frustrated spin-ice correlations with significant quantum fluctuations. In the disordered spin-liquid regime, $κ(H)$ exhibits a nonmonotonic magnetic field dependence, which is well explained by the strong spin-phonon scattering and quantum monopole excitations. We show that the excitation energy of quantum monopoles is strongly suppressed from that of dispersionless classical monopoles. Moreover, in stark contrast to the diffusive classical monopoles, the quantum monopoles have a very long mean …
While there is compelling evidence for the existence of magnetic monopoles in spin ice, the direct observation of a point-like source of magnetic field in these systems remains an open challenge. One promising approach is electron holography, which combines atomic-scale resolution with extreme sensitivity to magnetic vector potentials, through the Aharonov-Bohm effect. Here we explore what holography can teach us about magnetic monopoles in spin ice, through experiments on artificial spin ice, and numerical simulations of pyrochlore spin ice. In the case of artificial spin ice, we show that ho…
The ground state of a spin 1/2 nearest neighbor quantum Heisenberg antiferromagnet on the pyrochlore lattice is investigated using a large $N$ SU(N) fermionic mean field theory. We find several mean field states, of which the state of lowest energy upon Gutzwiller projection, is a parity and time reversal breaking chiral phase with a unit monopole flux exiting each tetrahedron. This "monopole flux" state has a Fermi surface consisting of 4 lines intersecting at a point. At mean field the low-energy excitations about the Fermi surface are gapless spinons. An analysis using the projective symmet…
"Magnetic monopole" is an exotic quantum excitation in pyrochlore U(1) spin liquid, and its emergence is purely of quantum origin and has no classical analogue. We predict topological thermal Hall effect (TTHE) of "magnetic monopoles" and present this prediction through non-Kramers doublets. We observe that, when the external magnetic field polarizes the Ising component of the local moment, internally this corresponds to the induction of emergent dual U(1) gauge flux for the "magnetic monopoles". The motion of "magnetic monopoles" is then twisted by the induced dual gauge flux. This emergent L…
Pyrochlore iridates and pyrochlore ices are two families of materials where novel quantum phenomena are intertwined with strong spin-orbit coupling, substantial electron correlation and geometrical frustration. Motivated by the puzzling experiments on two pyrochlore systems Pr2Ir2O7 and Yb2Ti2O7, we study the proximate Ising orders and the quantum phase transition out of quantum spin ice U(1) quantum spin liquid (QSL). We apply the electromagnetic duality of the compact quantum electrodynamics to analyze the "magnetic monopoles" condensation for U(1) QSL. The monopole condensation transition r…
Magnetic and magnetoelastic properties of terbium titanate pyrochlore in paramagnetic phase are simulated. The magnetic field and temperature dependences of magnetization and forced magnetostriction in Tb2Ti2O7 single crystals and polycrystalline samples are calculated in the framework of exchange charge model of crystal field theory and a mean field approximation. The set of electron-deformation coupling constants has been determined. Variations of elastic constants with temperature and applied magnetic field are discussed. Additional strong softening of the crystal lattice at liquid helium t…
At zero temperature, the classical antiferromagnetic Ising model on the pyrochlore lattice is a spin disorder phase of the critical spin correlation. It is a deconfined phase in that the binding energy of the monopole-anti-monopole pair is independent of their distance of separation. We show that turning on a transverse magnetic field turns it into the cooperative paramagnet, and the spin correlation becomes exponential decay. Furthermore, it introduces the quantum confinement (of magnetic monopoles), where the binding energy of the pair is proportional to their distance of separation. This di…
We study the U(1) quantum spin liquid on the pyrochlore spin ice systems. For the non-Kramers doublets such as Pr$^{3+}$ and Tb$^{3+}$, we point out that the inelastic neutron scattering not only detects the low-energy gauge photon, but also contains the continuum of the "magnetic monopole" excitations. Unlike the spinons, these "magnetic monopoles" are purely of quantum origin and have no classical analogue. We further point out that the "magnetic monopole" experiences a background dual "$π$" flux due to the spin-1/2 nature of the local moment when the "monopole" hops on the dual diamond latt…
The idea of magnetic monopoles in spin ice has enjoyed much success at intermediate temperatures, but at low temperatures a description in terms of monopole dynamics alone is insufficient. Recently, numerical simulations were used to argue that magnetic impurities account for this discrepancy by introducing a magnetic equivalent of residual resistance in the system. Here we propose that oxygen deficiency is the leading cause of magnetic impurities in as-grown samples, and we determine the defect structure and magnetism in Y2Ti2O(7-δ) using diffuse neutron scattering and magnetization measureme…
We study the effects of magnetoelastic couplings on pyrochlore antiferromagnets. We employ Landau theory, extending an investigation begun by Yamashita and Ueda for the case of S=1, and semiclassical analyses to argue that such couplings generate bond order via a spin--Peierls transition. This is followed by, or concurrent with, a transition into one of several possible low-temperature Neel phases, with most simply collinear, but also coplanar or mixed spin patterns. In a collinear Neel phase, a dispersionless string-like magnon mode dominates the resulting excitation spectrum, providing a dis…
We study the ground state and thermodynamic properties of the spin-half XXZ model, with an Ising interaction $J_z$ and a transverse exchange interaction $J_{x}$, on a pyrochlore tube obtained by joining together elementary cubes in a one-dimensional array. Periodic boundary conditions in the transverse directions ensure that the bulk of the system consists of corner-sharing tetrahedra, with the same local geometry as the pyrochlore lattice. We use exact diagonalization, the density matrix renormalization group (DMRG), and minimally entangled typical thermal states (METTS) methods to study the …
Motivated by puzzling spin-glass behaviors observed in many pyrochlore-based magnets, effects of magnetoelastic coupling to local lattice distortions were recently studied by the authors for a bond-disordered antiferromagnet on a pyrochlore lattice [Phys. Rev. Lett. 107, 047204 (2011)]. Here, we extend the analyses with focusing on the critical property of the spin-glass transition which occurs concomitantly with a nematic transition. Finite-size scaling analyses are performed up to a larger system size with 8192 spins to estimate the transition temperature and critical exponents. The exponent…
Quantum spin ice, modeled for magnetic rare-earth pyrochlores, has attracted great interest for hosting a U(1) quantum spin liquid, which involves spin-ice monopoles as gapped deconfined spinons, as well as gapless excitations analogous to photons. However, the global phase diagram under a [111] magnetic field remains open. Here we uncover by means of unbiased quantum Monte-Carlo simulations that a supersolid of monopoles, showing both a superfluidity and a partial ionization, intervenes the kagomé spin ice and a fully ionized monopole insulator, in contrast to classical spin ice where a direc…
We theoretically investigate a $J_1$-$J_3$ classical Heisenberg model on the breathing pyrochlore lattice, where the nearest-neighbor (NN) exchange interactions for small and large tetrahedra, $J_1$ and $J_1'$, take different values due to the breathing bond-alternation and $J_3$ is the third NN antiferromagnetic interaction along the bond direction. It is found by means of Monte Carlo simulations that for large $J_3$, a hedgehog lattice, a three-dimensional periodic array of magnetic monopoles and antimonopoles, emerges in the form of a quadruple-${\bf Q}$ state characterized by the ordering …
The latest experimental advances have extended the scenario of coupling mechanical degrees of freedom in chiral magnets (MnSi/MnGe) to the topologically nontrivial skyrmion crystal and even monopole lattices. Equipped with a spin-wave theory highlighting the topological features, we devise an interacting model for acoustic phonons and magnons to explain the experimental findings in a monopole lattice with a topological phase transition, i.e., annihilation of monopole-antimonopole pairs. We reproduce the anisotropic magnetoelastic modulations of elastic moduli: drastic ultrasonic softening arou…
We investigate the transport properties of itinerant electrons interacting with a background of localized spins in a correlated paramagnetic phase of the pyrochlore lattice. We find a residual resistivity at zero temperature due to the scattering of electrons by the static dipolar spin-spin correlation that characterizes the metallic Coulomb phase. As temperature increases, thermally excited topological defects, also known as magnetic monopoles, reduce the spin correlation, hence suppressing electron scattering. Combined with the usual scattering processes in metals at higher temperatures, thi…
Classical symmetry enriched topological orders and distinct monopole charges for dipole-octupole spin ices
International Center for Quantum Materials, Peking University（北京大学量子材料中心）；Tsung-Dao Lee Institute, Shanghai Jiao Tong University（上海交通大学李政道研究所）；Collaborative Innovation Center of Quantum Matter（量子物质协同创新中心）；The University of Hong Kong, Shenzhen Institute of Research and Innovation（香港大学深圳研究院）；Beijing Key Laboratory of Quantum Devices, Peking University（北京大学量子器件北京市重点实验室）
In this work we present a neutron Larmor diffraction study of the rare earth pyrochlores $R_2$Ti$_2$O$_7$, with $R$ = Tb, Dy, Ho. We measured the temperature dependence of the lattice parameter with precision $10^{-5}$, between 0.5 K and 300 K in each of the three compounds. The lattice parameter of the spin ices Dy$_2$Ti$_2$O$_7$ and Ho$_2$Ti$_2$O$_7$ enters into the derivation of the charge of the emergent magnetic monopole excitations suggested to exist in these materials. We found that throughout the range of applicability of the theory of emergent monopoles in the spin ices there will be …
The spin ice materials, including Ho2Ti2O7 and Dy2Ti2O7, are rare earth pyrochlore magnets which, at low temperatures, enter a constrained paramagnetic state with an emergent gauge freedom. Remarkably, the spin ices provide one of very few experimentally realised examples of fractionalization because their elementary excitations can be regarded as magnetic monopoles and, over some temperature range, the spin ice materials are best described as liquids of these emergent charges. In the presence of quantum fluctuations, one can obtain, in principle, a quantum spin liquid descended from the class…
A quantum spin liquid is a novel state of matter characterized by quantum entanglement and the absence of any broken symmetry. In condensed matter, the frustrated rare-earth pyrochlore magnets Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, so-called spin ices, exhibit a classical spin liquid state with fractionalized thermal excitations (magnetic monopoles). Evidence for a quantum spin ice, in which the magnetic monopoles become long range entangled and an emergent quantum electrodynamics arises, seems within reach. The magnetic properties of the quantum spin ice candidate Yb$_2$Ti$_2$O$_7$ have elu…
Unbiased quantum Monte-Carlo simulations are performed on the nearest-neighbor spin-$\frac{1}{2}$ pyrochlore XXZ model with an antiferromagnetic longitudinal and a weak ferromagnetic transverse exchange couplings, $J$ and $J_\perp$. The specific heat exhibits a broad peak at $T_{\mathrm{CSI}}\sim0.2J$ associated with a crossover to a classical Coulomb liquid regime showing a suppressed spin-ice monopole density, a broadened pinch-point singularity, and the Pauling entropy for $|J_\perp|\ll J$, as in classical spin ice. On further cooling, the entropy restarts decaying for $J_\perp>J_{\perp c}\…
The hedgehog lattice, a three-dimensional periodic array of magnetic monopoles and antimonopoles, is known to be realized in the presence of the Dzyaloshinskii-Moriya (DM) interaction. Here, we demonstrate by means of Monte Carlo simulations that the hedgehog lattice is induced by not the DM interaction but frustration in classical Heisenberg antiferromagnets on the breathing pyrochlore lattice. In the model, the breathing bond-alternation is characterized by the ratio of the nearest-neighbor (NN) antiferromagnetic exchange interaction for large tetrahedra to that for small ones, J1'/J1. A qua…
We study the two-dimensional kagome-ice model derived from a pyrochlore lattice with second- and third-neighbor interactions. The canted moments align along the local $\langle 111 \rangle$ axes of the pyrochlore and respond to both in-plane and out-of-plane external fields. We find that the combination of further-neighbor interactions together with the external fields introduces a rich phase diagram with different spin textures. Close to the phase boundaries, metastable $\textit{"snake"}$ domains emerge with extremely long relaxation time. Our kinetic Monte Carlo analysis of the magnetic-field…
An important and continuing theme of modern solid state physics is the realization of exotic excitations in materials (e.g. quasiparticles) that have no analogy (or have not yet been observed) in the actual physical vacuum of free space. Although they are not fundamental particles, such quasiparticles do constitute the most basic description of the excited states of the "vacuum" in which they reside. In this regard the magnetic textures of the excited states of spin ices, magnetic pyrochlore oxides with dominant Ising interactions, are proposed to be modeled as effective magnetic charge monopo…
Elementary excitations in the spin-ice compound Dy$_2$Ti$_2$O$_7$ can be described as magnetic monopoles propagating independently within the pyrochlore lattice formed by magnetic Dy ions. We studied the magnetic-field dependence of the thermal conductivity κ(B) for B || [001] and observe clear evidence for magnetic heat transport originating from the monopole excitations. The magnetic contribution κ_{mag} is strongly field-dependent and correlates with the magnetization M(B). The diffusion coefficient obtained from the ratio of κ_{mag} and the magnetic specific heat is strongly enhanced below…
We study geometrically frustrated antiferromagnets with magnetoelastic coupling. Frustration in these systems may be relieved by a structural transition to a low temperature phase with reduced lattice symmetry. We examine the statistical mechanics of this transition and the effects on it of quenched disorder, using Monte Carlo simulations of the classical Heisenberg model on the pyrochlore lattice with coupling to uniform lattice distortions. The model has a transition between a cubic, paramagnetic high-temperature phase and a tetragonal, Neel ordered low-temperature phase. It does not support…
We investigate the ground state properties of the spin-$1/2$ pyrochlore Heisenberg antiferromagnet using pseudofermion functional renormalization group techniques. The first part of our analysis is based on an enhanced parton mean-field approach which takes into account fluctuation effects from renormalized vertex functions. Our implementation of this technique extends earlier approaches and resolves technical difficulties associated with a diagrammatic overcounting. Using various parton ansätze for quantum spin liquids, dimerized and nematic states our results indicate a tendency for lattice …
The fundamental principles of electrodynamics allow an electron carrying both electric monopole (charge) and magnetic dipole (spin) but prohibit its magnetic counterpart. Recently it was predicted that the magnetic "monopoles" carrying emergent magnetic charges in spin ice systems can induce electric dipoles. The inspiring prediction offers a novel way to study magnetic monopole excitations and magnetoelectric coupling. However, no clear example has been identified up to now. Here, we report the experimental evidence for electric dipoles induced by magnetic monopoles in spin frustrated Tb2Ti2O…
While sources of magnetic fields - magnetic monopoles - have so far proven elusive as elementary particles, several scenarios have been proposed recently in condensed matter physics of emergent quasiparticles resembling monopoles. A particularly simple proposition pertains to spin ice on the highly frustrated pyrochlore lattice. The spin ice state is argued to be well-described by networks of aligned dipoles resembling solenoidal tubes - classical, and observable, versions of a Dirac string. Where these tubes end, the resulting defect looks like a magnetic monopole. We demonstrate, by diffuse …
Influence of controlled disorder on the dipolar spin ice state of Ho-based pyrochlores
Oak Ridge National Laboratory（橡树岭国家实验室）；University of California Santa Barbara（加州大学圣塔芭芭拉分校）；Perry College of Mathematics, Computing, and Sciences, University of West Georgia（佐治亚西部大学珀里数学、计算与科学学院）；Japan Atomic Energy Agency（日本原子能机构）；Brigham Young University（杨百翰大学）
We give a complete classification of fully symmetric as well as chiral $\mathbb{Z}_2$ quantum spin liquids on the pyrochlore lattice using a projective symmetry group analysis of Schwinger boson mean-field states. We find 50 independent ansätze, including the 12 fully symmetric nearest-neighbor $\mathbb{Z}_2$ spin liquids that have been classified by Liu et al. [https://journals.aps.org/prb/abstract/10.1103/PhysRevB.100.075125]. For each class we specify the most general symmetry-allowed mean-field Hamiltonian. Additionally, we test the properties of a subset of the spin liquid ansätze by solv…
Quantum spin liquid (QSL) is an exotic quantum phase of matter whose ground state is quantum-mechanically entangled without any magnetic ordering. A central issue concerns emergent excitations that characterize QSLs, which are hypothetically associated with quasiparticle fractionalization and topological order. Here we report highly unusual heat conduction generated by the spin degrees of freedom in a QSL state of the pyrochlore magnet Pr$_2$Zr$_2$O$_7$, which hosts spin-ice correlations with strong quantum fluctuations. The thermal conductivity in high temperature regime exhibits a two-gap be…
Frustration in magnetic systems is fertile ground for complex behaviour, including unconventional ground states with emergent symmetries, topological properties, and exotic excitations. A canonical example is the emergence of magnetic-charge-carrying quasiparticles in spin-ice compounds. Despite extensive work, a reliable experimental indicator of the density of these magnetic monopoles in spin-ice systems is yet to be found. Here, using measurements on single crystals of Ho$_{2}$Ir$_{2}$O$_{7}$ in combination with dipolar Monte Carlo simulations, we show that the magnetoresistance is highly s…
The pyrochlore oxides Dy$_{2}$Ti$_{2}$O$_{7}$ and Ho$_{2}$Ti$_{2}$O$_{7}$ are well studied spin ice systems and have shown the evidences of magnetic monopole excitations. Unlike these, Dy$_{2}$Zr$_{2}$O$_{7}$ is reported to crystallize in a distorted fluorite structure. We present here the magnetic and heat capacity studies of La substituted Dy$_{2}$Zr$_{2}$O$_{7}$. Our findings suggest the absence of spin ice state in Dy$_{2}$Zr$_{2}$O$_{7}$ but the emergence of the magnetic field induced spin freezing near T $\approx$ 10 K in ac susceptibility measurements which is similar to Dy$_{2}$Ti$_{2}…
Frustration in magnetic interactions can give rise to disordered ground states with subtle and beautiful properties. The spin ices Ho2Ti2O7 and Dy2Ti2O7 exemplify this phenomenon, displaying a classical spin liquid state, with fractionalized magnetic--monopole excitations. Recently there has been great interest in closely-related "quantum spin ice" materials, following the realization that anisotropic exchange interactions could convert spin ice into a massively-entangled, quantum, spin liquid, where magnetic monopoles become the charges of an emergent quantum electrodynamics. Here we show tha…
Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr$_2$Se$_4$ is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three-orders of magnitude faster than the canonical spin ice Dy$_2$Ti$_2$O$_7$. In this letter we use diffuse neutron scattering to show that both CdEr$_2$Se$_4$ and CdEr$_2$S$_4$ support a dipolar spin ice state -- the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to that in Dy$_2$Ti$_2$O…
We study the S=1/2 Heisenberg antiferromagnet on the pyrochlore lattice in the limit of strong easy-axis exchange anisotropy. We find, using only standard techniques of degenerate perturbation theory, that the model has a U(1) gauge symmetry generated by certain local rotations about the z-axis in spin space. Upon addition of an extra local interaction in this and a related model with spins on a three-dimensional network of corner-sharing octahedra, we can write down the exact ground state wavefunction with no further approximations. Using the properties of the soluble point we show that these…
The complexity embedded in condensed matter fertilizes the discovery of new states of matter, enriched by ingredients like frustration. Illustrating examples in magnetic systems are Kitaev spin liquids, skyrmions phases, or spin ices. These unconventional ground states support exotic excitations, for example the magnetic charges in spin ices, also called monopoles. Beyond their discovery, an important challenge is to be able to control and manipulate them. Here, we propose a new mechanism to inject monopoles in a spin ice through a staggered magnetic field. We show theoretically, and demonstra…
The pyrochlore compounds Ho2Ti2O7 and Dy2Ti2O7 show an exotic form of magnetism called the spin ice state, resulting from the interplay between geometrical frustration and ferromagnetic coupling. A fascinating feature of this state is the appearance of magnetic monopoles as emergent excitations above the degenerate ground state. Over the past years, strong effort has been devoted to the investigation of these monopoles and other properties of the spin ice state in bulk crystals. A tantalising prospect is to incorporate spin ice materials into devices for spintronics and devices that can manipu…
Magnetic monopoles are hypothetical elementary particles exhibiting quantized magnetic charge $m_0=\pm(h/μ_0e)$ and quantized magnetic flux $Φ_0=\pm h/e$. A classic proposal for detecting such magnetic charges is to measure the quantized jump in magnetic flux $Φ$ threading the loop of a superconducting quantum interference device (SQUID) when a monopole passes through it. Naturally, with the theoretical discovery that a plasma of emergent magnetic charges should exist in several lanthanide-pyrochlore magnetic insulators, including Dy$_2$Ti$_2$O$_7$, this SQUID technique was proposed for their …
