Three-dimensional Quantum Spin Liquid Research Articles

Field-induced effects in the spin liquid candidate PbCuTe2O6

${\mathrm{PbCuTe}}_{2}{\mathrm{O}}_{6}$ is considered to be one of the rare candidate materials for a three-dimensional quantum spin liquid (QSL). This assessment was based on the results of various magnetic experiments, performed mainly on polycrystalline material. More recent measurements on single crystals revealed an even more exotic behavior, yielding ferroelectric order below ${T}_{\text{FE}}\ensuremath{\approx}1\phantom{\rule{0.28em}{0ex}}\text{K}$, accompanied by distinct lattice distortions, and a somewhat modified magnetic response which is still consistent with a QSL. Here we report on low-temperature measurements of various thermodynamic, magnetic, and dielectric properties of single-crystalline ${\mathrm{PbCuTe}}_{2}{\mathrm{O}}_{6}$ in magnetic fields $B\ensuremath{\le}14.5\phantom{\rule{0.28em}{0ex}}\text{T}$. The combination of these various probes allows us to construct a detailed $B\text{\ensuremath{-}}T$ phase diagram including a ferroelectric phase for $B\ensuremath{\le}8$ T and a $B$-induced magnetic phase at $B\ensuremath{\ge}11$ T. These phases are preceded by or coincide with a structural transition from a cubic high-temperature phase into a distorted noncubic low-temperature state. The phase diagram discloses a ferroelectric quantum critical point at ${B}_{c1}=7.9\phantom{\rule{0.28em}{0ex}}\text{T}$, where the second-order phase transition line associated with ferroelectric order is suppressed to zero. In addition, a magnetic quantum phase transition is revealed at ${B}_{c2}=11\phantom{\rule{0.28em}{0ex}}\text{T}$. The corresponding phase transition to a field-induced magnetic order at $B>{B}_{c2}$ is likely to be of first order. Field-induced lattice distortions, observed in the state at $T>1$ K and which are assigned to the effect of spin-orbit interaction of the ${\mathrm{Cu}}^{2+}$ ions, are considered as the key mechanism by which the magnetic field couples to the dielectric degrees of freedom in this material.

Possible realization of three-dimensional quantum spin liquid behavior in HoVO4

The study of geometrically frustrated magnetic systems with unusual crystal field ground states offers a possibility of realizing the new aspects of physics of disordered systems. In this study, we report our results of structural, magnetic susceptibility, heat capacity measurements, along with density functional theory (DFT) calculations on HoVO4; a compound in which the presence of a distorted kind of HoO8 polyhedral leads to multiple magnetic interaction paths. The observed broad maximum below 10 K in the temperature response of DC susceptibility curves implies the presence of short-range correlations. AC susceptibility rules out the possibility of any kind of spin freezing. Temperature dependent heat capacity measurement at zero field indicate towards the absence of long-range ordering, along with the presence of a broad maximum centered around 14 K. The residual heat capacity exhibits a characteristic power-law (Tα ) behavior with the exponent α nearly equal to 2, which is analogous to that observed for other three-dimensional (3D) quantum spin liquid (QSL) systems. The DFT calculations signify the presence of dominant second and third nearest neighbor interactions, which in turn lead to magnetic frustration in our system. Our investigations suggest that HoVO4 can be a candidate for realizing a 3D QSL state.

Uncovering Footprints of Dipolar-Octupolar Quantum Spin Ice from Neutron Scattering Signatures.

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 or octupolar channel, and two possible flux configurations of the emergent gauge field. In this Letter, using exact diagonalization and molecular dynamics, we investigate the equal-time and dynamical spin structure factors in all four quantum spin ice regimes using quantum and classical calculations. Contrasting the distinct signatures of quantum and classical results for the four possible quantum spin ice regimes and elucidating the role of quantum fluctuations, we show that the quantum structure factor computed for the π-flux octupolar quantum spin ice regime is most compatible with the neutron scattering results on Ce_{2}Zr_{2}O_{7}.

Competing U (1) and Z2 dipolar-octupolar quantum spin liquids on the pyrochlore lattice: Application to Ce2Zr2O7

Recent experiments on the dipolar-octupolar pyrochlore compound ${\mathrm{Ce}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$ indicate that it may realize a three-dimensional quantum spin liquid (QSL). In particular, the analyses of available data suggest that the system is in a region of parameter space, where the so-called $\ensuremath{\pi}$-flux $U(1)$ octupolar quantum spin ice (QSI) with an emergent photon could be realized. However, because the system is far from the perturbative classical spin ice regime, it is unclear whether the quantum ground state is primarily a coherent superposition of 2-in-2-out configurations as in the canonical QSI phases. In this work, we explore other possible competing quantum spin-liquid states beyond QSI using the Schwinger boson parton construction of the dipolar-octupolar pseudospin-1/2 model. After classifying all symmetric $U(1)$ and ${\mathbb{Z}}_{2}$ QSLs using the projective symmetry group (PSG), we construct a mean-field phase diagram that possesses a number of important features observed in an earlier exact diagonalization study. In the experimentally relevant frustrated region of the phase diagram, we find two closely competing gapped ${\mathbb{Z}}_{2}$ QSLs with a narrow spinon dispersion. The equal-time and dynamical spin structure factors of these states show key features similar to what was reported in neutron scattering experiments. Hence, these QSLs are closely competing ground states in addition to the $\ensuremath{\pi}$-flux $U(1)$ QSI, and they should be taken into account on equal footing for the interpretation of experiments on ${\mathrm{Ce}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$.

Ground-state phase diagram of dipolar-octupolar pyrochlores

The dipolar-octupolar pyrochlore oxides R$_2$M$_2$O$_7$ (R=Ce, Sm, Nd) represent an important opportunity in the search for three dimensional Quantum Spin Liquid (QSL) ground states. Their low energy physics is governed by an alluringly simple XYZ Hamiltonian, enabling theoretical description with only a small number of free parameters. Meanwhile, recent experiments on Ce pyrochlores strongly suggest QSL physics. Motivated by this, we present here a complete analysis of the ground state phase diagram of dipolar-octupolar pyrochlores. Combining cluster mean field theory, variational arguments and exact diagonalization we find multiple U(1) QSL phases which together occupy a large fraction of the parameter space. These results give a comprehensive picture of the ground state physics of an important class of QSL candidates and support the possibility of a $U(1)$ QSL ground state in Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$.

Distinguishing dipolar and octupolar quantum spin ices using contrasting magnetostriction signatures

Recently there have been a number of experiments on Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$, suggesting that these materials host a three-dimensional quantum spin liquid with emergent photons and fractionalized spinon excitations. However, the interpretation of the data to determine the precise nature of the quantum spin liquids is still under debate. The Kramers doublet in Ce$^{3+}$ local moment offers unusual pseudo-spin degrees of freedom as the $x$ and $z$ components transform as a dipole and $y$ component as an octupole. This leads to a variety of possible quantum spin liquid (or quantum spin ice) phases on the pyrochlore lattice of Ce$^{3+}$ moments. In this work, we theoretically propose that magnetostriction would be able to distinguish the dipolar (D-QSI) and octupolar (O-QSI) quantum spin ice, where the dipolar or octupolar components possess the respective spin ice correlations. We show that the magnetostriction in various configurations can be used as a selection rule to differentiate not only D-QSI and O-QSI, but also a number of competing broken symmetry states.

Evidence for a three-dimensional quantum spin liquid in PbCuTe2O6

The quantum spin liquid is a highly entangled magnetic state characterized by the absence of static magnetism in its ground state. Instead, the spins fluctuate in a highly correlated way down to the lowest temperatures. Quantum spin liquids are very rare and are confined to a few specific cases where the interactions between the magnetic ions cannot be simultaneously satisfied (known as frustration). Lattices with magnetic ions in triangular or tetrahedral arrangements, which interact via isotropic antiferromagnetic interactions, can generate such a frustration. Three-dimensional isotropic spin liquids have mostly been sought in materials where the magnetic ions form pyrochlore or hyperkagome lattices. Here we present a three-dimensional lattice called the hyper-hyperkagome that enables spin liquid behaviour and manifests in the compound PbCuTe2O6. Using a combination of experiment and theory, we show that this system exhibits signs of being a quantum spin liquid with no detectable static magnetism together with the presence of diffuse continua in the magnetic spectrum suggestive of fractional spinon excitations.

Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore

A quantum spin liquid is a state of matter where unpaired electrons’ spins, although entangled, do not show magnetic order even at the zero temperature. The realization of a quantum spin liquid is a long-sought goal in condensed-matter physics. Although neutron scattering experiments on the two-dimensional spin-1/2 kagome lattice ZnCu3(OD)6Cl2 and triangular lattice YbMgGaO4 have found evidence for the hallmark of a quantum spin liquid at very low temperature (a continuum of magnetic excitations), the presence of magnetic and non-magnetic site chemical disorder complicates the interpretation of the data. Recently, the three-dimensional Ce3+ pyrochlore lattice Ce2Sn2O7 has been suggested as a clean, effective spin-1/2 quantum spin liquid candidate, but evidence of a spin excitation continuum is still missing. Here, we use thermodynamic, muon spin relaxation and neutron scattering experiments on single crystals of Ce2Zr2O7, a compound isostructural to Ce2Sn2O7, to demonstrate the absence of magnetic ordering and the presence of a spin excitation continuum at 35 mK. With no evidence of oxygen deficiency and magnetic/non-magnetic ion disorder seen by neutron diffraction and diffuse scattering measurements, Ce2Zr2O7 may be a three-dimensional pyrochlore lattice quantum spin liquid material with minimum magnetic and non-magnetic chemical disorder. A detailed neutron scattering and muon spin relaxation study uncovers a continuum of magnetic excitations down to 35 mK in the pyrochlore lattice compound Ce2Zr2O7 with minimum chemical disorder, consistent with quantum spin liquid behaviour.

Simple anisotropic three-dimensional quantum spin liquid with fractonlike topological order

We present a three-dimensional cubic lattice spin model, anisotropic in the $\hat{z}$ direction, that exhibits fracton topological order. The latter is a novel type of topological order characterized by the presence of immobile pointlike excitations, named fractons, residing at the corners of an operator with two-dimensional support. As other recent fracton models, ours exhibits a subextensive ground state degeneracy: On an $L_x\times L_y\times L_z$ three-torus, it has a $2^{2L_z}$ topological degeneracy, and an additional non-topological degeneracy equal to $2^{L_xL_y-2}$. The fractons can be combined into composite excitations that move either in a straight line along the $\hat{z}$ direction, or freely in the $xy$ plane at a given height $z$. While our model draws inspiration from the toric code, we demonstrate that it cannot be adiabatically connected to a layered toric code construction. Additionally, we investigate the effects of imposing open boundary conditions on our system. We find zero energy modes on the surfaces perpendicular to either the $\hat{x}$ or $\hat{y}$ directions, and their absence on the surfaces normal to $\hat{z}$. This result can be explained using the properties of the two kinds of composite two-fracton mobile excitations.

Signatures of a gearwheel quantum spin liquid in a spin- 12 pyrochlore molybdate Heisenberg antiferromagnet

We theoretically investigate the low-temperature phase of the recently synthesized Lu$_2$Mo$_2$O$_5$N$_2$ material, an extraordinarily rare realization of a $S=1/2$ three-dimensional pyrochlore Heisenberg antiferromagnet in which Mo$^{5+}$ are the $S=1/2$ magnetic species. Despite a Curie-Weiss temperature ($\Theta_{\rm CW}$) of $-121(1)$ K, experiments have found no signature of magnetic ordering $or$ spin freezing down to $T^*\approx0.5$ K. Using density functional theory, we find that the compound is well described by a Heisenberg model with exchange parameters up to third nearest neighbors. The analysis of this model via the pseudofermion functional renormalization group method reveals paramagnetic behavior down to a temperature of at least $T=|\Theta_{\rm CW}|/100$, in agreement with the experimental findings hinting at a possible three-dimensional quantum spin liquid. The spin susceptibility profile in reciprocal space shows momentum-dependent features forming a "gearwheel" pattern, characterizing what may be viewed as a molten version of a chiral noncoplanar incommensurate spiral order under the action of quantum fluctuations. Our calculated reciprocal space susceptibility maps provide benchmarks for future neutron scattering experiments on single crystals of Lu$_2$Mo$_2$O$_5$N$_2$.

Generic model for the hyperkagome iridateNa4Ir3O8in the local-moment regime

Hyperkagome iridate, Na$_4$Ir$_3$O$_8$, has been regarded as a promising candidate material for a three-dimensional quantum spin liquid. Here the three-dimensional network of corner-sharing triangles forms the hyperkagome lattice of Ir$^{4+}$ ions. Due to strong spin-orbit coupling, the local moments of Ir$^{4+}$ ions are described by the pseudospin $j_{\rm eff} = 1/2$ Kramers doublet. The Heisenberg model on this lattice is highly frustrated and quantum/classical versions have been studied in earlier literature. In this work, we derive a generic local-moment model beyond the Heisenberg limit for the hyperkagome iridate by considering multi-orbital interactions for all the $t_{2g}$ orbitals and spin-orbit coupling. The lifting of massive classical degeneracy in the Heisenberg model by various spin-anisotropy terms is investigated at the classical level and the resulting phase diagram is presented. We find that different anisotropy terms prefer distinct classes of magnetically ordered phases, often with various discrete degeneracy. The implications of our results for recent $\mu$SR and NMR experiments on this material and possible quantum spin liquid phases are discussed.

Thermal conductivity across the metal-insulator transition in the single-crystalline hyperkagome antiferromagnetNa3+xIr3O8

The hyperkagome antiferromagnet Na$_{4}$Ir$_3$O$_8$ represents the first genuine candidate for the realisation of a three-dimensional quantum spin-liquid. It can also be doped towards a metallic state, thus offering a rare opportunity to explore the nature of the metal-insulator transition in correlated, frustrated magnets. Here we report thermodynamic and transport measurements in both metallic and weakly insulating single crystals down to 150 mK. While in the metallic sample the phonon thermal conductivity ($\kappa^{ph}$) is almost in the boundary scattering regime, in the insulating sample we find a large reduction $\kappa^{ph}$ over a very wide temperature range. This result can be ascribed to the scattering of phonons off nanoscale disorder or off the gapless magnetic excitations that are seen in the low-temperature specific heat. This works highlights the peculiarity of the metal-insulator transition in Na$_{3+x}$Ir$_3$O$_8$ and demonstrates the importance of the coupling between lattice and spin degrees of freedom in the presence of strong spin-orbit coupling.

Spin liquid close to a quantum critical point in Na4Ir3O8

Na${}_{4}$Ir${}_{3}$O${}_{8}$ is a candidate material for a three-dimensional quantum spin liquid on the hyperkagome lattice. We present thermodynamic measurements of heat capacity $C$ and thermal conductivity $\ensuremath{\kappa}$ on high-quality polycrystalline samples of Na${}_{4}$Ir${}_{3}$O${}_{8}$ down to $T=500$ and 75 mK, respectively. Absence of long-range magnetic order down to $T=75$ mK strongly supports claims of a spin-liquid ground state. The constant magnetic susceptibility $\ensuremath{\chi}$ below $T\ensuremath{\approx}25$ K and the presence of a small but finite linear-$T$ term in $C(T)$ suggest the presence of gapless spin excitations. Additionally, the magnetic Gr$\stackrel{\ifmmode \ddot{}\else \"{}\fi{}}{\mathrm{u}}$neisen ratio shows a divergence as $T\ensuremath{\rightarrow}0$ K and a scaling behavior, which clearly demonstrates that Na${}_{4}$Ir${}_{3}$O${}_{8}$ is situated close to a zero-field QCP.

Frustrated three-dimensional quantum spin liquid in CuHpCl

Inelastic neutron scattering measurements are reported for the quantum antiferromagnetic material Cu_2(C_5H_12N_2)_2Cl_4 (CuHpCl). The magnetic excitation spectrum forms a band extending from 0.9 meV to 1.4 meV. The spectrum contains two modes that disperse throughout the a-c plane of the monoclinic unit cell with less dispersion along the unique b-axis. Simple arguments based on the measured dispersion relations and the crystal structure show that a spin ladder model is inappropriate for describing CuHpCl. Instead, it is proposed that hydrogen bond mediated exchange interactions between the bi-nuclear molecular units yield a three-dimensional interacting spin system with a recurrent triangular motif similar to the Shastry-Sutherland Model (SSM). Model independent analysis based on the first moment sum rule shows that at least four distinct spin pairs are strongly correlated and that two of these, including the dimer bond of the corresponding SSM, are magnetically frustrated. These results show that CuHpCl should be classified as a frustration induced three dimensional quantum spin liquid.