Quantum Spin Liquid State Research Articles

Thermally enhanced Majorana-mediated spin transport in the Kitaev model

We study how stable the Majorana-mediated spin transport in a quantum spin Kitaev model is against thermal fluctuations. Using the time-dependent thermal pure quantum state method, we examine finite-temperature spin dynamics in the Kitaev model. The model exhibits two characteristic temperatures $T_L$ and $T_H$, which correspond to energy scales of the local flux and the itinerant Majorana fermion, respectively. At low temperatures $(T\ll T_L)$, an almost flux-free state is realized and the spin excitation propagates in a similar way to that for the ground state. Namely, after the magnetic pulse is introduced at one of the edges, the itinerant Majorana fermions propagate the spin excitations even through the quantum spin liquid state region, and oscillations in the spin moment appear in the other edge with a tiny magnetic field. When $T\sim T_L$, larger oscillations in the spin moments are induced in the other edge, compared to the results at the ground state. At higher temperatures, excited $Z_2$ fluxes disturb the coherent motion of the itinerant Majorana fermions, which suppresses the spin propagation. Our results demonstrate a crucial role of thermal fluctuations in the Majorana-mediated spin transport.

Fermionic symmetry fractionalization in (2+1) dimensions

We develop a systematic theory of symmetry fractionalization for fermionic topological phases of matter in (2+1)D with a general fermionic symmetry group $G_f$. In general $G_f$ is a central extension of the bosonic symmetry group $G_b$ by fermion parity, $(-1)^F$, characterized by a non-trivial cohomology class $[\omega_2] \in \mathcal{H}^2(G_b, \mathbb{Z}_2)$. We show how the presence of local fermions places a number of constraints on the algebraic data that defines the action of the symmetry on the super-modular tensor category that characterizes the anyon content. We find two separate obstructions to defining symmetry fractionalization, which we refer to as the bosonic and fermionic symmetry localization obstructions. The former is valued in $\mathcal{H}^3(G_b, K(\mathcal{C}))$, while the latter is valued in either $\mathcal{H}^3(G_b,\mathcal{A}/\{1,\psi\})$ or $Z^2(G_b, \mathbb{Z}_2)$ depending on additional details of the theory. $K(\mathcal{C})$ is the Abelian group of functions from anyons to $\mathrm{U}(1)$ phases obeying the fusion rules, $\mathcal{A}$ is the Abelian group defined by fusion of Abelian anyons, and $\psi$ is the fermion. When these obstructions vanish, we show that distinct symmetry fractionalization patterns form a torsor over $\mathcal{H}^2(G_b, \mathcal{A}/\{1,\psi\})$. We study a number of examples in detail; in particular we provide a characterization of fermionic Kramers degeneracy arising in symmetry class DIII within this general framework, and we discuss fractional quantum Hall and $\mathbb{Z}_2$ quantum spin liquid states of electrons.

TMDs as a platform for spin liquid physics: A strong coupling study of twisted bilayer WSe2

The advent of twisted moiré heterostructures as a playground for strongly correlated electron physics has led to a plethora of experimental and theoretical efforts seeking to unravel the nature of the emergent superconducting and insulating states. Among these layered compositions of two-dimensional materials, transition metal dichalcogenides are now appreciated as highly tunable platforms to simulate reinforced electronic interactions in the presence of low-energy bands with almost negligible bandwidth. Here, we focus on the twisted homobilayer WSe2 and the insulating phase at half-filling of the flat bands reported therein. More specifically, we explore the possibility of realizing quantum spin liquid (QSL) physics on the basis of a strong coupling description, including up to second-nearest neighbor Heisenberg couplings J1 and J2 as well as Dzyaloshinskii–Moriya (DM) interactions. Mapping out the global phase diagram as a function of an out-of-plane displacement field, we indeed find evidence for putative QSL states, albeit only close to SU(2) symmetric points. In the presence of finite DM couplings and XXZ anisotropy, long-range order is predominantly present with a mix of both commensurate and incommensurate magnetic phases.

Quantum paramagnetism in the hyperhoneycomb Kitaev magnet β−ZnIrO3

A polycrystalline sample of the hyperhoneycomb iridate $\beta$-ZnIrO$_3$ was synthesized via a topochemical reaction, and its structural, magnetic, and thermodynamic properties were investigated. The magnetization and heat capacity data show the absence of long-range magnetic order at least down to 2 K. A positive Curie-Weiss temperature $\theta_W \sim 45$ K probed by the temperature dependence of magnetic susceptibility indicates that a Kitaev interaction is dominant. These observations suggest that a quantum spin liquid may have been realized. Furthermore, the observation of linear temperature-dependent contribution to the heat capacity with no magnetic field effect evidences gapless excitation. These facts are surprisingly contrary to the chemical disorder evidenced by the crystallographic analysis. By discussing the differences in the size effect of Z$_2$-fluxes in 2D and 3D Kitaev magnets, we propose that there is a hidden mechanism to protect the quantum spin liquid state from chemical disorder.

Thermodynamic evidence for a field-angle-dependent Majorana gap in a Kitaev spin liquid

The exactly-solvable Kitaev model of two-dimensional honeycomb magnet leads to a quantum spin liquid (QSL) characterized by Majorana fermions, relevant for fault-tolerant topological quantum computations. In the high-field paramagnetic state of $\alpha$-RuCl3, half-integer quantization of thermal Hall conductivity has been reported as a signature of edge current, but the bulk nature of this state remains elusive. Here, from high-resolution heat capacity measurements under in-plane field rotation, we find strongly angle-dependent low-energy excitations in bulk $\alpha$-RuCl3. The excitation gap has a sextuple node structure, and the gap amplitude increases with field, exactly as expected for itinerant Majorana fermions in the Kitaev model. Our thermodynamic results are fully linked with the transport quantization properties, providing the first demonstration of the bulk-edge correspondence in a Kitaev QSL. Moreover, at higher fields where the quantum thermal Hall effect vanishes, we find the possible emergence of a novel nematic QSL state with two-fold rotational symmetry.

Spin and quadrupole correlations by three-spin interaction in the frustrated pyrochlore magnetTb2+xTi2−xO7+y

We have investigated the origin of the magnetic dipole correlations $\langle \sigma_{\boldsymbol{Q}}^z \sigma_{\boldsymbol{-Q}}^z \rangle$ characterized by the modulation wave vector $\boldsymbol{k} \sim (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$ observed in the frustrated pyrochlore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$. This magnetic short-range order cannot be accounted for by adding further-neighbor exchange interactions to the nearest-neighbor pseudospin-$\tfrac{1}{2}$ Hamiltonian for quantum pyrochlore magnets. Using classical Monte Carlo simulation and quantum simulation based on thermally pure quantum (TPQ) states we have shown that the spin correlations with $\boldsymbol{k} \sim (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$ are induced at low temperatures by a three-spin interaction of a form $\sigma_{\boldsymbol{r}}^{\pm} \sigma_{\boldsymbol{r}^{\prime}}^z \sigma_{\boldsymbol{r}^{\prime \prime}}^z $, which is a correction to the Hamiltonian due to the low crystal-field excitation. Simulations using TPQ states have shown that the spin correlations coexist with electric quadrupole correlations $\langle \sigma_{\boldsymbol{Q}}^{\alpha} \sigma_{\boldsymbol{-Q}}^{\beta} \rangle$ ($\alpha, \beta = x, y$) with $\boldsymbol{k} \sim \boldsymbol{0}$. These results suggest that the putative quantum spin liquid state of Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ is located close to phase boundaries of the spin-ice, quadrupole-ordered, and magnetic-ordered states in the classical approximation, and that the three-spin interaction brings about a quantum disordered ground state with both spin and quadrupole correlations.

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 ${\mathrm{Ce}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$.

Metastable Kitaev Magnets.

Nearly two decades ago, Alexei Kitaev proposed a model for spin- particles with bond-directional interactions on a two-dimensional honeycomb lattice which had the potential to host a quantum spin-liquid ground state. This work initiated numerous investigations to design and synthesize materials that would physically realize the Kitaev Hamiltonian. The first generation of such materials, such as NaIrO, -LiIrO, and -RuCl, revealed the presence of non-Kitaev interactions such as the Heisenberg and off-diagonal exchange. Both physical pressure and chemical doping were used to tune the relative strength of the Kitaev and competing interactions; however, little progress was made towards achieving a purely Kitaev system. Here, we review the recent breakthrough in modifying Kitaev magnets via topochemical methods that has led to the second generation of Kitaev materials. We show how structural modifications due to the topotactic exchange reactions can alter the magnetic interactions in favor of a quantum spin-liquid phase.

Projected entangled pair states study of anisotropic-exchange magnets on the triangular lattice

The anisotropic-exchange spin-1/2 model on a triangular lattice has been used to describe the rare-earth chalcogenides, which may have exotic ground states. We investigate the quantum phase diagram of the model by using the projected entangled pair state (PEPS) method, and compare it to the classical phase diagram. Besides two stripe-ordered phase, and the 120$^\circ$ state, there is also a multi-\textbf{Q} phase. We identify the multi-\textbf{Q} phase as a $Z_{2}$ vortex state. No quantum spin liquid state is found in the phase diagram, contrary to the previous DMRG calculations.

Honeycomb-Structure RuI3 , A New Quantum Material Related to α-RuCl3.

The layered honeycomb lattice material α-RuCl3 has emerged as a prime candidate for displaying the Kitaev quantum spin liquid state, and as such has attracted much research interest. Here a new layered honeycomb lattice polymorph of RuI3 , a material that is strongly chemically and structurally related to α-RuCl3 is described. The material is synthesized at moderately elevated pressures and is stable under ambient conditions. Preliminary characterization reveals that it is a metallic conductor, with the absence of long-range magnetic order down to 0.35 K and an unusually large T-linear contribution to the heat capacity. It is proposed that this phase, with a layered honeycomb lattice and strong spin-orbit coupling, provides a new route for the characterization of quantum materials.

Proton-electron-coupled functionalities of conductivity, magnetism, and optical properties in molecular crystals.

Proton-electron-coupled reactions, specifically proton-coupled electron transfer (PCET), in biological and chemical processes have been extensively investigated for use in a wide variety of applications, including energy conversion and storage. However, the exploration of the functionalities of the conductivity, magnetism, and dielectrics by proton-electron coupling in molecular materials is challenging. Dynamic and static proton-electron-coupled functionalities are to be expected. This feature article highlights the recent progress in the development of functionalities of dynamic proton-electron coupling in molecular materials. Herein, single-unit conductivity by self-doping, quantum spin liquid state coupled with quantum fluctuation of protons, switching of conductivity and magnetism triggered by the disorder-order transition of deuterons, and their external responses under pressure and in the presence of an electric field are introduced. In addition, as for the functionalities of proton-d/π-electron coupling in metal dithiolene complexes, magnetic switching with multiple PCET and vapochromism induced by electron transfer through hydrogen-bond (H-bond) formation is introduced experimentally and theoretically. We also outlined the basic and applied issues and potential challenges for development of proton-electron-coupled molecular materials, functionalities, and devices.

Evidence for Magnetic Fractional Excitations in a Kitaev Quantum-Spin-Liquid Candidate α-RuCl3

It is known that α-RuCl3 has been studied extensively because of its proximity to the Kitaev quantum-spin-liquid (QSL) phase and the possibility of approaching it by tuning the competing interactions. Here we present the first polarized inelastic neutron scattering study on α-RuCl3 single crystals to explore the scattering continuum around the Γ point at the Brillouin zone center, which was hypothesized to be resulting from the Kitaev QSL state but without concrete evidence. With polarization analyses, we find that, while the spin-wave excitations around the M point vanish above the transition temperature T N, the pure magnetic continuous excitations around the Γ point are robust against temperature. Furthermore, by calculating the dynamical spin-spin correlation function using the cluster perturbation theory, we derive magnetic dispersion spectra based on the K–Γ model, which involves with a ferromagnetic Kitaev interaction of –7.2 meV and an off-diagonal interaction of 5.6 meV. We find this model can reproduce not only the spin-wave excitation spectra around the M point, but also the non-spin-wave continuous magnetic excitations around the Γ point. These results provide evidence for the existence of fractional excitations around the Γ point originating from the Kitaev QSL state, and further support the validity of the K–Γ model as the effective minimal spin model to describe α-RuCl3.

Heat Transport in Herbertsmithite: Can a Quantum Spin Liquid Survive Disorder?

One favorable situation for spins to enter the long-sought quantum spin liquid (QSL) state is when they sit on a kagome lattice. No consensus has been reached in theory regarding the true ground state of this promising platform. The experimental efforts, relying mostly on one archetypal material ZnCu_{3}(OH)_{6}Cl_{2}, have also led to diverse possibilities. Apart from subtle interactions in the Hamiltonian, there is the additional degree of complexity associated with disorder in the real material ZnCu_{3}(OH)_{6}Cl_{2} that haunts most experimental probes. Here we resort to heat transport measurement, a cleaner probe in which instead of contributing directly, the disorder only impacts the signal from the kagome spins. For ZnCu_{3}(OH)_{6}Cl_{2}, we observed no contribution by any spin excitation nor obvious field-induced change to the thermal conductivity. These results impose strong constraints on various scenarios about the ground state of this kagome compound: while certain quantum paramagnetic states other than a QSL may serve as natural candidates, a QSL state, gapless or gapped, must be dramatically modified by the disorder so that the kagome spin excitations are localized.

Strain-induced phase diagram of the S=32 Kitaev material CrSiTe3

The interplay among anisotropic magnetic terms, such as the bond-dependent Kitaev interactions and single-ion anisotropy, plays a key role in stabilizing the finite-temperature ferromagnetism in the two-dimensional compound $\rm{CrSiTe_3}$. While the Heisenberg interaction is predominant in this material, a recent work shows that it is rather sensitive to the compressive strain, leading to a variety of phases, possibly including a sought-after Kitaev quantum spin liquid [C. Xu, \textit{et. al.}, Phys. Rev. Lett. \textbf{124}, 087205 (2020)]. To further understand these states, we establish the quantum phase diagram of a related bond-directional spin-$3/2$ model by the density-matrix renormalization group method. As the Heisenberg coupling varies from ferromagnetic to antiferromagnetic, three magnetically ordered phases, i.e., a ferromagnetic phase, a $120^\circ$ phase and an antiferromagnetic phase, appear consecutively. All the phases are separated by first-order phase transitions, as revealed by the kinks in the ground-state energy and the jumps in the magnetic order parameters. However, no positive evidence of the quantum spin liquid state is found and possible reasons are discussed briefly.

Probing topological spin liquids on a programmable quantum simulator.

Quantum spin liquids, exotic phases of matter with topological order, have been a major focus in physics for the past several decades. Such phases feature long-range quantum entanglement that can potentially be exploited to realize robust quantum computation. We used a 219-atom programmable quantum simulator to probe quantum spin liquid states. In our approach, arrays of atoms were placed on the links of a kagome lattice, and evolution under Rydberg blockade created frustrated quantum states with no local order. The onset of a quantum spin liquid phase of the paradigmatic toric code type was detected by using topological string operators that provide direct signatures of topological order and quantum correlations. Our observations enable the controlled experimental exploration of topological matter and protected quantum information processing.

Spin liquid and ferroelectricity close to a quantum critical point in PbCuTe2O6

Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favor of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favorable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe2O6, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behavior is revealed for the single crystals. These crystals show ferroelectric order at TFE ≈ 1 K, accompanied by strong lattice distortions, and a modified magnetic response—still consistent with a quantum spin liquid—but with clear indications for quantum critical behavior.

Enhancement of Photoresponse on Narrow-Bandgap Mott Insulator α-RuCl3 via Intercalation.

Charge doping to Mott insulators is critical to realize high-temperature superconductivity, quantum spin liquid state, and Majorana fermion, which would contribute to quantum computation. Mott insulators also have a great potential for optoelectronic applications; however, they showed insufficient photoresponse in previous reports. To enhance the photoresponse of Mott insulators, charge doping is a promising strategy since it leads to effective modification of electronic structure near the Fermi level. Intercalation, which is the ion insertion into the van der Waals gap of layered materials, is an effective charge-doping method without defect generation. Herein, we showed significant enhancement of optoelectronic properties of a layered Mott insulator, α-RuCl3, through electron doping by organic cation intercalation. The electron-doping results in substantial electronic structure change, leading to the bandgap shrinkage from 1.2 eV to 0.7 eV. Due to localized excessive electrons in RuCl3, distinct density of states is generated in the valence band, leading to the optical absorption change rather than metallic transition even in substantial doping concentration. The stable near-infrared photodetector using electronic modulated RuCl3 showed 50 times higher photoresponsivity and 3 times faster response time compared to those of pristine RuCl3, which contributes to overcoming the disadvantage of a Mott insulator as a promising optoelectronic device and expanding the material libraries.

Synthesis and anisotropic magnetism in quantum spin liquid candidates AYbSe2 (A = K and Rb)

The quantum spin liquid (QSL) state in rare-earth triangular lattices has attracted much attention recently due to its potential application in quantum computing and communication. Here, we report the single-crystal growth synthesis, crystal structure characterizations, and magnetic properties of AYbSe2 (A = K and Rb) compounds. The x-ray diffraction analysis shows that AYbSe2 (A = K and Rb) crystallizes in a trigonal space group, R-3m (No. 166) with Z = 3. AYbSe2 possesses a two-dimensional (2D) Yb–Se–Yb layered structure formed by edged-shared YbSe6 octahedra. The magnetic properties are highly anisotropic for both title compounds, and no long-range order is found down to 0.4 K, revealing the possible QSL ground state in these compounds. The isothermal magnetization exhibits a one-third magnetization plateau when the magnetic fields are applied in the ab-plane. Heat capacity is performed along both ab-plane and c axis and features the characteristic dome for triangular magnetic lattice compounds as a function of magnetic fields. Due to the change in the interlayer and intralayer distance of Yb3+, the dome shifts to low fields from KYbSe2 to RbYbSe2. All these results indicate that the AYbSe2 family presents unique frustrated magnetism close to the possible QSL and noncollinear spin states.

Magnetic Field Induced Quantum Spin Liquid in the Two Coupled Trillium Lattices of K_{2}Ni_{2}(SO_{4})_{3}.

Quantum spin liquids are exotic states of matter that form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K_{2}Ni_{2}(SO_{4})_{3} forming a three-dimensional network of Ni^{2+} spins. Using density functional theory calculations, we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering, and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field B≳4 T diminishes the ordered component and drives the system into a pure quantum spin liquid state. This shows that a system of interconnected S=1 trillium lattices exhibits a significantly elevated level of geometrical frustration.

Fractional spin fluctuations and quantum liquid signature in Gd2ZnIrO6

Hitherto, the discrete identification of quantum spin liquid phase, holy grail of condensed matter physics, remains a challenging task experimentally. However, the precursor of quantum spin liquid state may reflect in the spin dynamics even in the paramagnetic phase over a wide temperature range as conjectured theoretically. Here we report comprehensive inelastic light (Raman) scattering measurements on the Ir based double perovskite, Gd2ZnIrO6, as a function of different incident photon energies and polarization in a broad temperature range. Our results evidenced the spin fractionalization within the paramagnetic phase reflected in the emergence of a polarization independent quasi-elastic peak at low energies with lowering temperature. Also, the fluctuating scattering amplitude measured via dynamic Raman susceptibility increases with lowering temperature and decreases mildly upon entering into long-range magnetic ordering phase, below 23 K, suggesting the magnetic origin of these fluctuations. This anomalous scattering response is thus indicative of fluctuating fractional spin evincing the quantum spin liquid phase in a three-dimensional double perovskite system.