Condensed matter systems provide alternative `vacua' exhibiting emergent low-energy properties drastically different from those of the standard model. A case in point is the emergent quantum electrodynamics (QED) in the fractionalized topological magnet known as quantum spin ice, whose magnetic monopoles set it apart from the familiar QED of the world we live in. Here, we show that the two greatly differ in their fine-structure constant $α$, which parametrizes how strongly matter couples to light: $α_{\mathrm{QSI}}$ is more than an order of magnitude greater than $α_{\mathrm{QED}} \approx 1/137$. Furthermore, $α_{\mathrm{QSI}}$, the emergent speed of light, and all other parameters of the emergent QED, are tunable by engineering the microscopic Hamiltonian. We find that $α_{\mathrm{QSI}}$ can be tuned all the way from zero up to what is believed to be the \textit{strongest possible} coupling beyond which QED confines. In view of the small size of its constrained Hilbert space, this marks out quantum spin ice as an ideal platform for studying exotic quantum field theories and a target for quantum simulation. The large $α_{\mathrm{QSI}}$ implies that experiments probing candidate condensed-matter realizations of quantum spin ice should expect to observe phenomena arising due to strong interactions.
A quantum melting of the spin ice is proposed for pyrochlore-lattice magnets Pr$_2TM_2$O$_7$ ($TM=$Ir, Zr, and Sn). The quantum superexchange Hamiltonian having a nontrivial magnetic anisotropy is derived in the basis of atomic non-Kramers magnetic doublets. The ground states exhibit a cooperative ferroquadrupole and pseudospin chirality, forming a magnetic analog of smectic liquid crystals. Our theory accounts for dynamic spin-ice behaviors experimentally observed in Pr$_2TM_2$O$_7$.
Although initially introduced to mimic the spin-ice pyrochlores, no artificial spin ice has yet exhibited the expected degenerate ice-phase with critical correlations similar to the celebrated Coulomb phase in the pyrochlore lattice. Here we study a novel artificial spin ice based on a vertex-frustrated rather than pairwise frustrated geometry and show that it exhibits a quasicritical ice phase of extensive residual entropy and, significantly, algebraic correlations. Interesting in its own regard as a novel realization of frustration in a vertex system, our lattice opens new pathways to study …
We study the coupling between conventional (Maxwell) and emergent electrodynamics in quantum spin ice, a 3+1-dimensional $U(1)$ quantum spin liquid. We find that a uniform electric field can be used to tune the properties of both the ground state and excitations of the spin liquid. In particular, it induces emergent birefringence, rendering the speed of the emergent light anisotropic and polarization-dependent. A sufficiently strong electric field triggers a quantum phase transition into new $U(1)$ quantum spin liquid phases which trap emergent electric $π$-fluxes. The flux patterns of these n…
Experimental identification of quantum spin ice (QSI), a U(1) quantum spin liquid on the pyrochlore lattice hosting emergent photons, is a major challenge in frustrated magnets. In this work, we propose ultrasound measurements as a novel tool for probing the emergent photons of various QSI phases. Our analysis includes QSI phases in non-Kramers doublet compounds such as $\rm{Pr}_2 \rm{Zr}_2 \rm{O}_7$ as well as dipolar-octupolar Kramers doublet compounds such as $\rm{Ce}_2 \rm{Zr}_2 \rm{O}_7$. The latter may host emergent photons associated with an octupolar component which renders them diffic…
The "spin ice" state found in the rare earth pyrochlore magnets Ho2Ti2O7 and Dy2Ti2O7 offers a beautiful realisation of classical magnetostatics, complete with magnetic monopole excitations. It has been suggested that in "quantum spin ice" materials, quantum-mechanical tunnelling between different ice configurations could convert the magnetostatics of spin ice into a quantum spin liquid which realises a fully dynamical, lattice-analogue of quantum electromagnetism. Here we explore how such a state might manifest itself in experiment, within the minimal microscopic model of a such a quantum spi…
At low temperatures, spin dynamics in ideal spin ice is due mainly to dilute, thermally excited magnetic monopole excitations. I consider how these will affect the dynamics of a nuclear spin (the same theory applies to muon spin resonance if implanted muons do not diffuse). Up to the time scale for nearby monopoles to be rearranged, a stretched-exponential form of the relaxation functions is expected. I work out the expected exponent in that exponential and the formulas for the $T_1$ (longitudinal) and $T_2$ (dephasing) relaxations, as a function of the monopole density. Experimental NMR is in…
Magnetic skyrmions have been receiving growing attention as potential information storage and magnetic logic devices since an increasing number of materials have been identified that support skyrmion phases. Explorations of artificial frustrated systems have led to new insights into controlling and engineering new emergent frustration phenomena in frustrated and disordered systems. Here, we propose a skyrmion spin ice, giving a unifying framework for the study of geometric frustration of skyrmion crystals in a non-frustrated artificial geometrical lattice as a consequence of the structural con…
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…
We demonstrate the existence of orbital Coulomb phase as the exact ground state of p-orbital exchange Hamiltonian on the diamond lattice. The Coulomb phase is an emergent state characterized by algebraic dipolar correlations and a gauge structure resulting from local constraints (ice rules) of the underlying lattice models. For most ice models on the pyrochlore lattice, these local constraints are a direct consequence of minimizing the energy of each individual tetrahedron. On the contrary, the orbital ice rules are emergent phenomena resulting from the quantum orbital dynamics. We show that t…
Artificial spin ices are frustrated spin systems that can be engineered, wherein fine tuning of geometry and topology has allowed the design and characterization of exotic emergent phenomena at the constituent level. Here we report a realization of spin ice in a lattice of superconducting qubits. Unlike conventional artificial spin ice, our system is disordered by both quantum and thermal fluctuations. The ground state is classically described by the ice rule, and we achieve control over a fragile degeneracy point leading to a Coulomb phase. The ability to pin individual spins allows us to dem…
The low-temperature picture of dipolar spin ice in terms of the Coulomb fluid of its fractionalised magnetic monopole excitations has allowed analytic and conceptual progress far beyond its original microscopic spin description. Here we develop its thermodynamic treatment as a `magnetolyte', a fluid of singly and doubly charged monopoles, an analogue of the electrochemical system ${\rm 2 H_2O = H_3O^+ +OH^- = H_4O^{2+} + O^{2-}}$, but with perfect symmetry between oppositely charged ions. For this lattice magnetolyte, we present an analysis based on Debye-Hückel theory, which is accurate at al…
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…
We present a new mechanism for Raman scattering of phonons, which is based on the linear magnetoelastic coupling present in non-Kramers magnetic ions. This provides a direct coupling of Raman-active phonons to the magnet's quasiparticles. We propose to use this mechanism to probe the emergent magnetic monopoles, electric charges, and photons of the emergent quantum electrodynamics (eQED) of the U(1) quantum spin liquid known as quantum spin ice. Detecting this eQED in candidate rare-earth pyrochlore materials, or indeed signatures of topological magnetic phases more generally, is a challenging…
The spin ice compounds {\dys} and {\holm} are highly unusual magnets which epitomize a set of concepts of great interest in modern condensed matter physics: their low-energy physics exhibits an emergent gauge field and their excitations are magnetic monopoles which arise from the fractionalization of the microscopic magnetic spin degrees of freedom. In this review, we provide an elementary introduction to these concepts and we survey the thermodynamics, statics and dynamics---in and out of equilibrium---of spin ice from these vantage points. Along the way, we touch on topics such as emergent C…
Emergent quasiparticles that arise from the fractionalization of the microscopic degrees of freedom have been one of the central themes in modern condensed matter physics. The notion of magnetic monopoles, freely moving quasiparticles fragmented from local dipole excitations, has enjoyed much success in understanding the thermodynamic, static, and transport properties of the so-called spin-ice materials. The artificial version of spin ice, where a lattice of nanoscale magnetic dipoles is sculpted out of a ferromagnetic film, provides a unique opportunity to study these unusual quasiparticles i…
In a quantum spin liquid, 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 [1-2]. Such phases offer promising perspectives for device applications in quantum information technologies, and their study can reveal fundamentally novel physics in quantum matter. Quantum spin ice is an appealing proposal of one such state, in which the fundamental ground state properties and excitations are described by an emergent U(1) lattice gauge theory [3-7]. This quantum-coherent…
Electrically charged particles, such as the electron, are ubiquitous. By contrast, no elementary particles with a net magnetic charge have ever been observed, despite intensive and prolonged searches. We pursue an alternative strategy, namely that of realising them not as elementary but rather as emergent particles, i.e., as manifestations of the correlations present in a strongly interacting many-body system. The most prominent examples of emergent quasiparticles are the ones with fractional electric charge e/3 in quantum Hall physics. Here we show that magnetic monopoles do emerge in a class…
We combine two aspects of magnetic frustration, multiferroicity and emergent quasi-particles in spin liquids, by studying magneto-electric monopoles. Spin ice offers to couple these emergent topological defects to external fields, and to each other, in unusual ways, making possible to lift the degeneracy underpinning the spin liquid and to potentially stabilize novel forms of charge crystals, opening the path to a "magnetic crystallography". In developing the general phase diagram including nearest-neighbour coupling, Zeeman energy, electric and magnetic dipolar interactions, we uncover the em…
Recent experiments on Ce$_2$Zr$_2$O$_7$ suggest that this material may host a novel form of quantum spin ice, a three-dimensional quantum spin liquid with an emergent photon. The Ce$^{3+}$ local moments on the pyrochlore lattice are described by pseudospin 1/2 degrees of freedom, whose components transform as dipolar and octupolar moments under symmetry operations. In principle, there exist four possible quantum spin ice regimes, depending on whether the Ising component is in the dipolar/octupolar channel, and two possible flux configurations of the emergent gauge field. In this work, using ex…
Magnetic monopoles are hypothetical particles that may exist as quantized sources and sinks of the magnetic field. In materials, they may appear in an emergent quantum electrodynamics described by a U(1) lattice gauge theory. Particularly, quantum spin ice hosts monopoles as bosonic spinons coupled to emergent gauge fields in a U(1) quantum spin liquid, namely, a deconfined Coulomb phase. When monopoles are condensed to form a long-range order, monopoles and gauge fields are screened and confined. Here we show, however, that monopole supercurrent flows across a junction of two ferromagnets tha…
The kagome lattice -- a two-dimensional (2D) arrangement of corner-sharing triangles -- is at the forefront of the search for exotic states generated by magnetic frustration. Such states have been observed experimentally for Heisenberg and planar spins. In contrast, frustration of Ising spins on the kagome lattice has previously been restricted to nano-fabricated systems and spin-ice materials under applied magnetic field. Here, we show that the layered Ising magnet Dy3Mg2Sb3O14 hosts an emergent order predicted theoretically for individual kagome layers of in-plane Ising spins. Neutron-scatte…
Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Rudolf Peierls Centre for Theoretical Physics（鲁道夫·派尔斯理论物理中心）；Hertford College（赫特福德学院）
Extensive work on single molecule magnets has identified a fundamental mode of relaxation arising from the nuclear-spin assisted quantum tunnelling of nearly independent and quasi-classical magnetic dipoles. Here we show that nuclear-spin assisted quantum tunnelling can also control the dynamics of purely emergent excitations: magnetic monopoles in spin ice. Our low temperature experiments were conducted on canonical spin ice materials with a broad range of nuclear spin values. By measuring the magnetic relaxation, or monopole current, we demonstrate strong evidence that dynamical coupling wit…
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…
Symmetry fractionalization is a ubiquitous feature of topologically ordered states that can be used to classify different symmetry-enriched topological phases and reveal some of their unique experimental signatures. Despite its vast popularity, there is currently no available framework to study symmetry fractionalization of quantum spin ice (QSI) -- a $U(1)$ quantum spin liquid (QSL) on the pyrochlore lattice supporting emergent photons -- within the most widely used theoretical framework to describe it, gauge mean-field theory (GMFT). In this work, we provide an extension of GMFT that allows …
Spin crossover materials contain metal ions that can access two spin-states: one low-spin (LS), the other high-spin (HS). We propose that frustrated elastic interactions can give rise to spin-state ices -- phases of matter without long-range order, characterized by a local constraint or `ice rule'. The low-energy physics of spin-state ices is described by an emergent divergence-less gauge field with a gap to topological excitations that are deconfined quasi-particles with spin fractionalized midway between the spins of the LS and HS states.
Spin ice magnetic monopoles are fractionalized emergent excitations in a class of frustrated magnets called spin ices. The classical spin ice model has an extensive number of ground state spin configurations, whereas magnetic monopoles can be thought of as the endpoints of string operators applied to these ground states. Introducing quantum fluctuations into the model induces monopoles with dynamics, which would normally lift the degeneracy of the two-monopole energy level at the linear order of the perturbation. Contrary to this expectation, we find that quantum fluctuations in the form of a …
Competing interactions in the so-called spin-ice compounds stabilize a frustrated ground-state with finite zero-point entropy and, interestingly, emergent magnetic monopole excitations. The properties of these monopoles are at the focus of recent research with particular emphasis on their quantum dynamics. It is predicted that each monopole also possesses an electric dipole moment, which allows to investigate their dynamics via the dielectric function ε(ν). Here, we report on broadband spectroscopic measurements of ε(ν) in Dy2Ti2O7 down to temperatures of 200mK with a specific focus on the cri…
A non-Ohmic current that grows exponentially with the square root of applied electric field is well known from thermionic field emission (the Schottky effect), electrolytes (the second Wien effect) and semiconductors (the Poole-Frenkel effect). It is a universal signature of the attractive Coulomb force between positive and negative electrical charges, which is revealed as the charges are driven in opposite directions by the force of an applied electric field. Here we apply thermal quenches to spin ice to prepare metastable populations of bound pairs of positive and negative emergent magnetic …
Quantum spin liquids are highly entangled ground states of quantum systems with emergent gauge structure, fractionalized spinon excitations, and other unusual properties. While these features clearly distinguish quantum spin liquids from conventional, mean-field-like states at zero temperature (T), their status at T>0 is less clear. Strictly speaking, it is known that most quantum spin liquids lose their identity at non-zero temperature, being in that case adiabatically transformable into a trivial paramagnet. This is the case for the U(1) quantum spin liquid states recently proposed to occur …
We propose that in a certain class of magnetic materials, known as non-Kramers 'spin ice,' disorder induces quantum entanglement. Instead of driving glassy behavior, disorder provokes quantum superpositions of spins throughout the system, and engenders an associated emergent gauge structure and set of fractional excitations. More precisely, disorder transforms a classical phase governed by a large entropy, classical spin ice, into a quantum spin liquid governed by entanglement. As the degree of disorder is increased, the system transitions between (i) a "regular" Coulombic spin liquid, (ii) a …
We calculate the effect of the emergent photon on threshold production of spinons in $U(1)$ Coulomb spin liquids such as quantum spin ice. The emergent Coulomb interaction modifies the threshold production cross-section dramatically, changing the weak turn-on expected from the density of states to an abrupt onset reflecting the basic coupling parameters. The slow photon typical in existing lattice models and materials suppresses the intensity at finite momentum and allows profuse Cerenkov radiation beyond a critical momentum. These features are broadly consistent with recent numerical and expe…
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…
Insulating magnetic rare-earth pyrochlores related to spin ice host emergent bosonic monopolar spinons, which obey a magnetic analogue of quantum electrodynamics and may open a route to a magnetic analogue of electronics. However, the energy scales of the interactions among rare-earth moments are so low as 1 K that the possible quantum coherence can only be achieved at a sub-Kelvin. Here, we desgin high-temperature quantum spin ice materials from first principles. It is shown that the A-site deintercalated spinel iridate Ir2O4, which has been experimentally grown as epitaxial thin films, is a …
Nonequilibrium processes are probed by ultrasound waves in the spin-ice material Dy2Ti2O7 at low temperatures. The sound velocity and the sound attenuation exhibit a number of anomalies versus applied magnetic field for temperatures below the "freezing" temperature of ~500 mK. These robust anomalies can be seen for longitudinal and transverse acoustic modes for different field directions. The anomalies show a broad hysteresis. Most notable are peaks in the sound velocity, which exhibit two distinct regimes: an intrinsic (extrinsic) one in which the data collapse for different sweep rates when …
Here we calculate the dynamic susceptibility and dynamic correlation function in spin ice using the model of emergent magnetic monopoles. Calculations are based on a method originally suggested for the description of dynamic processes in water ice (non-equilibrium thermodynamics approach). We show that for zero temperature the dynamic correlation function reproduces the transverse dipole correlations (static correlation function) characteristic of spin ice in its ground state. At non-zero temperatures the dynamic correlation function includes an additional longitudinal component which decrease…
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…
We investigate thermal transport in square ice, a two-dimensional analogue of spin ice, exploring the role played by emergent magnetic monopoles in transporting energy. Using kinetic Monte Carlo simulations based on energy preserving extensions of single-spin-flip dynamics, we explicitly compute the (longitudinal) thermal conductivity, $κ$, over a broad range of temperatures. We use two methods to determine $κ$: a measurement of the energy current between thermal baths at the boundaries, and the Green-Kubo formula, yielding quantitatively consistent values for the thermal conductivity. We inte…
Spin-ices are frustrated magnets that support a particularly rich variety of emergent physics. Typically, it is the interplay of magnetic dipole interactions, spin anisotropy, and geometric frustration on the pyrochlore lattice that drives spin-ice formation. The relevant physics occurs at temperatures commensurate with the magnetic interaction strength, which for most systems is 1--5\,K. This low energy scale poses severe challenges for experimental studies of spin-ices and the practical exploitation of their unusual properties. Here, we show that non-magnetic cadmium cyanide (Cd(CN)$_2$) exh…
The original proposal to achieve superconductivity by starting from a quantum spin-liquid (QSL) and doping it with charge carriers, as proposed by Anderson in 1987, has yet to be realized. Here we propose an alternative strategy: use a QSL as a substrate for heterostructure growth of metallic films to design exotic superconductors. By spatially separating the two key ingredients of superconductivity, i.e., charge carriers (metal) and pairing interaction (QSL), the proposed setup naturally lands on the parameter regime conducive to a controlled theoretical prediction. Moreover, the proposed set…
Although most quantum systems thermalize locally on short time scales independent of initial conditions, recent developments have shown this is not always the case. Lattice geometry and quantum mechanics can conspire to produce constrained quantum dynamics and associated glassy behavior, a phenomenon that falls outside the rubric of the eigenstate thermalization hypothesis. Constraints "fragment" the many-body Hilbert space due to which some states remain insulated from others and the system fails to attain thermal equilibrium. Such fragmentation is a hallmark of geometrically frustrated magne…
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 …
We present an experimental determination of the isothermal magnetic susceptibility of the spin ice materials Dy2Ti2O7 and Ho2Ti2O7 in the temperature range 1.8-300 K. The use of spherical crystals has allowed the accurate correction for demagnetizing fields and allowed the true bulk isothermal susceptibility X_T(T) to be estimated. This has been compared to a theoretical expression based on a Husimi tree approximation to the spin ice model. Agreement between experiment and theory is excellent at T > 10 K, but systematic deviations occur below that temperature. Our results largely resolve an ap…
