Spin-orbital Liquid Research Articles

Wegner's Ising gauge spins versus Kitaev's Majorana partons: Mapping and application to anisotropic confinement in spin-orbital liquids

Emergent gauge theories take a prominent role in the description of quantum matter, supporting deconfined phases with topological order and fractionalized excitations. A common construction of \mathbb{Z}_2ℤ2 lattice gauge theories, first introduced by Wegner, involves Ising gauge spins placed on links and subject to a discrete \mathbb{Z}_2ℤ2 Gauss law constraint. As shown by Kitaev, \mathbb{Z}_2ℤ2 lattice gauge theories also emerge in the exact solution of certain spin systems with bond-dependent interactions. In this context, the \mathbb{Z}_2ℤ2 gauge field is constructed from Majorana fermions, with gauge constraints given by the parity of Majorana fermions on each site. In this work, we provide an explicit Jordan-Wigner transformation that maps between these two formulations on the square lattice, where the Kitaev-type gauge theory emerges as the exact solution of a spin-orbital (Kugel-Khomskii) Hamiltonian. We then apply our mapping to study local perturbations to the spin-orbital Hamiltonian, which correspond to anisotropic interactions between electric-field variables in the \mathbb{Z}_2ℤ2 gauge theory. These are shown to induce anisotropic confinement that is characterized by emergence of weakly-coupled one-dimensional spin chains. We study the nature of these phases and corresponding confinement transitions in both absence and presence of itinerant fermionic matter degrees of freedom. Finally, we discuss how our mapping can be applied to the Kitaev spin-1/2 model on the honeycomb lattice.

Long-range spin-orbital order in the spin-orbital SU(2)×SU(2)×U(1) model

By using the tensor-network state algorithm, we study a spin-orbital model with SU(2)$\times$SU(2)$\times$U(1) symmetry on the triangular lattice. This model was proposed to describe some triangular $d^1$ materials and was argued to host a spin-orbital liquid ground state. In our work the trial wavefunction of its ground state is approximated by an infinite projected entangled simplex state and optimized by the imaginary-time evolution. Contrary to the previous conjecture, we find that the two SU(2) symmetries are broken, resulting in a stripe spin-orbital order with the same magnitude $m=0.085(10)$. This value is about half of that in the spin-1/2 triangular Heisenberg antiferromagnet. Our result demonstrates that although the long-sought spin-orbital liquid is absent in this model the spin-orbital order is significantly reduced due to the enhanced quantum fluctuation. This suggests that high-symmetry spin-orbital models are promising in searching for exotic states of matter in condensed-matter physics.

Spin-orbital liquids and insulator-metal transitions on the pyrochlore lattice

The two orbital Hubbard model, with the electrons additionally coupled to a complex magnetic background, arises in the pyrochlore molybdates. The background involves local moments Hund's coupled to the electrons, driving double exchange ferromagnetism, and antiferromagnetic (AF) tendency arising from competing superexchange. The key scales include the Hubbard repulsion and the superexchange, both of which can be tuned in these materials. They control the phase transition from a ferromagnetic metal to a spin-glass metal and then to a spin-glass (Mott) insulator. We provide a comprehensive description of the ground state of this model using an unrestricted Hartree-Fock scheme implemented via a simulated annealing procedure and establish the metal-insulator transition line for varying Hubbard interaction and superexchange. The electrons see an effective disorder, due to orbital frustration, already in the ferromagnetic phase. The disorder is further enhanced by antiferromagnetic coupling and the resulting magnetic disorder. As a result, increasing AF coupling shifts the metal-insulator transition to lower Hubbard interaction and gives it an additional ``Anderson'' character. We provide detailed results on the magnetic and orbital correlations, the density of states, and the optical conductivity.

Thermodynamic signature of SU(4) spin-orbital liquid and symmetry fractionalization from Lieb-Schultz-Mattis theorem

The state-of-the-art numerical simulation of the SU(4) Heisenberg model on a honeycomb lattice reveals a characteristic peak-and-shoulder specific heat behavior. The low-temperature peak is associated with a color gap, which suggests the existence of a gapped symmetric ground state in this model.

Metallic and Deconfined Quantum Criticality in Dirac Systems

Motivated by the physics of spin-orbital liquids, we study a model of interacting Dirac fermions on a bilayer honeycomb lattice at half filling, featuring an explicit global SO(3)×U(1) symmetry. Using large-scale auxiliary-field quantum MonteCarlo (QMC) simulations, we locate two zero-temperature phase transitions as function of increasing interaction strength. First, we observe a continuous transition from the weakly interacting semimetal to a different semimetallic phase in which the SO(3) symmetry is spontaneously broken and where two out of three Dirac cones acquire a mass gap. The associated quantum critical point can be understood in terms of a Gross-Neveu-SO(3) theory. Second, we subsequently observe a transition toward an insulating phase in which the SO(3) symmetry is restored and the U(1) symmetry is spontaneously broken. While strongly first order at the mean-field level, the QMC data are consistent with a direct and continuous transition. It is thus a candidate for a new type of deconfined quantum critical point that features gapless fermionic degrees of freedom.

Quantum phases of two-dimensional Z2 gauge theory coupled to single-component fermion matter

We investigate the rich quantum phase diagram of Wegner's theory of discrete Ising gauge fields interacting with $U(1)$ symmetric single-component fermion matter hopping on a two-dimensional square lattice. In particular limits the model reduces to (i) pure $\mathbb{Z}_2$ even and odd gauge theories, (ii) free fermions in a static background of deconfined $\mathbb{Z}_2$ gauge fields, (iii) the kinetic Rokhsar-Kivelson quantum dimer model at a generic dimer filling. We develop a local transformation that maps the lattice gauge theory onto a model of $\mathbb{Z}_2$ gauge-invariant spin $1/2$ degrees of freedom. Using the mapping, we perform numerical density matrix renormalization group calculations that corroborate our understanding of the limits identified above. Moreover, in the absence of the magnetic plaquette term, we reveal signatures of topologically ordered Dirac semimetal and staggered Mott insulator phases at half-filling. At strong coupling, the lattice gauge theory displays fracton phenomenology with isolated fermions being completely frozen and dimers exhibiting restricted mobility. In that limit, we predict that in the ground state dimers form compact clusters, whose hopping is suppressed exponentially in their size. We determine the band structure of the smallest clusters numerically using exact diagonalization. The rich phenomenology discussed in this paper can be probed in analog and digital quantum simulators of discrete gauge theories and in Kitaev spin-orbital liquids.

SU(4)-symmetric quantum spin-orbital liquids on various lattices

An emergent $\mathrm{SU}(4)$ symmetry discovered in the microscopic model for $d^1$ honeycomb materials [M.~G.~Yamada, M.~Oshikawa, and G.~Jackeli, Phys. Rev. Lett. \textbf{121}, 097201 (2018).] has enabled us to tailor exotic $\mathrm{SU}(4)$ models in real materials. In the honeycomb structure, the emergent $\mathrm{SU}(4)$ Heisenberg model would potentially have a quantum spin-orbital liquid ground state due to the \textit{multicomponent frustration}, and we can expect similar spin-orbital liquids also in three-dimensinal versions of the honeycomb lattice. In such quantum spin-orbital liquids, both the spin and orbital degrees of freedom become fractionalized and entangled together due to the strong frustrated interactions between them. Similarly to spinons in pure quantum spin liquids, quantum spin-orbital liquids can host not only spinon excitations, but also fermionic \textit{orbitalon} excitations at low temperature.

Spin transport in a quantum spin orbital liquid

Quantum spin-orbital liquids (QSOLs) are a novel phase of matter, similar to quantum spin liquids, with quantum fluctuations in both spin and orbital degrees of freedom. We use non-equilibrium Green's function theory to study out-of-equilibrium spin transport in an exactly solvable QSOL model put forward by Yao and Lee. We find that the spin transport problem can be mapped to that of a free fermion problem with effective fermionic baths that have rapidly varying density of states. In the gapless phase, the spin current $I_s-V_s$ relation is thus highly nonlinear, while in the chiral gapped phase, the spin current conductance is quantized to be $1/2\pi$ provided that the contacts are sufficiently wide. The quantized conductance is a signature of the topological nature of the chiral gapped QSOL.

Spin-orbital liquid in Ba3CuSb2O9 stabilized by oxygen holes

Both the Jahn-Teller distortion of Cu$^{2+}$O$_6$ octahedra and magnetic ordering are absent in hexagonal Ba$_3$CuSb$_2$O$_9$ suggesting a Cu 3$d$ spin-orbital liquid state. Here, by means of resonant x-ray scattering and absorption experiment, we show that oxygen 2$p$ holes play crucial role in stabilizing this spin-orbital liquid state. These oxygen holes appear due to the "reaction" Sb$^{5+}$$\rightarrow$Sb$^{3+}$ $+$ two oxygen holes, with these holes being able to attach to Cu ions. The hexagonal phase with oxygen 2$p$ holes exhibits also a novel charge-orbital dynamics which is absent in the orthorhombic phase of Ba$_3$CuSb$_2$O$_9$ with Jahn-Teller distortion and Cu 3$d$ orbital order. The present work opens up a new avenue towards spin-charge-orbital entangled liquid state in transition-metal oxides with small or negative charge transfer energy.

Fractionalized quantum criticality in spin-orbital liquids from field theory beyond the leading order

Two-dimensional spin-orbital magnets with strong exchange frustration have recently been predicted to facilitate the realization of a quantum critical point in the Gross-Neveu-SO(3) universality class. In contrast to previously known Gross-Neveu-type universality classes, this quantum critical point separates a Dirac semimetal and a long-range-ordered phase, in which the fermion spectrum is only partially gapped out. Here, we characterize the quantum critical behavior of the Gross-Neveu-SO(3) universality class by employing three complementary field-theoretical techniques beyond their leading orders. We compute the correlation-length exponent $\nu$, the order-parameter anomalous dimension $\eta_\phi$, and the fermion anomalous dimension $\eta_\psi$ using a three-loop $\epsilon$ expansion around the upper critical space-time dimension of four, a second-order large-$N$ expansion (with the fermion anomalous dimension obtained even at the third order), as well as a functional renormalization group approach in the improved local potential approximation. For the physically relevant case of $N=3$ flavors of two-component Dirac fermions in 2+1 space-time dimensions, we obtain the estimates $1/\nu = 1.03(15)$, $\eta_\phi = 0.42(7)$, and $\eta_\psi = 0.180(10)$ from averaging over the results of the different techniques, with the displayed uncertainty representing the degree of consistency among the three methods.

Flux crystals, Majorana metals, and flat bands in exactly solvable spin-orbital liquids

Spin-orbital liquids are quantum disordered states in systems with entangled spin and orbital degrees of freedom. We study exactly solvable spin-orbital models in two dimensions with selected Heisenberg-, Kitaev-, and $\mathrm{\ensuremath{\Gamma}}$-type interactions, as well as external magnetic fields. These models realize a variety of spin-orbital-liquid phases featuring dispersing Majorana fermions with Fermi surfaces, nodal Dirac or quadratic band touching points, or full gaps. In particular, we show that Zeeman magnetic fields can stabilize nontrivial flux patterns and induce metamagnetic transitions between states with different topological character. Solvable nearest-neighbor biquadratic spin-orbital perturbations can be tuned to stabilize zero-energy flat bands. We discuss in detail the examples of $\mathrm{SO}(2)$- and $\mathrm{SO}(3)$-symmetric spin-orbital models on the square and honeycomb lattices, and use group-theoretical arguments to generalize to $\mathrm{SO}(\ensuremath{\nu})$-symmetric models with arbitrary integer $\ensuremath{\nu}>1$. These results extend the list of exactly solvable models with spin-orbital-liquid ground states and highlight the intriguing general features of such exotic phases. Our models are thus excellent starting points for more realistic modelling of candidate materials.

Magnetic Raman continuum in single-crystalline H3LiIr2O6

Recently H$_3$LiIr$_2$O$_6$ has been reported as a spin-orbital entangled quantum spin liquid (QSL) [K. Kitagawa et al., Nature {\bf 554}, 341 (2018)], albeit its connection to Kitaev QSL has not been yet identified. To unveil the related Kitaev physics, we perform the first Raman spectroscopy studies on single crystalline H$_3$LiIr$_2$O$_6$ samples. We implement a soft chemical replacement of Li$^+$ with H$^+$ from $\alpha$-Li$_2$IrO$_3$ single crystals to synthesize the single crystal samples of the iridate second generation H$_3$LiIr$_2$O$_6$. The Raman spectroscopy can be used to diagnose the QSL state since the magnetic Raman continuum arises from a process involving pairs of fractionalized Majorana fermionic excitation in a pure Kitaev model. We observe a broad dome-shaped magnetic continuum in H$_3$LiIr$_2$O$_6$, in line with theoretical expectations for the two-spin process in the Kitaev QSL. Our results establish the close connection to the Kitaev QSL physics in H$_3$LiIr$_2$O$_6$.

SU(4) Heisenberg model on the honeycomb lattice with exchange-frustrated perturbations: Implications for twistronics and Mott insulators

The SU(4)-symmetric spin-orbital model on the honeycomb lattice was recently studied in connection to correlated insulators such as the $e_{g}$ Mott insulator Ba$_{3}$CuSb$_{2}$O$_{9}$ and the insulating phase of magic-angle twisted bilayer graphene at quarter filling. Here we provide a unified discussion of these systems by investigating an extended model that includes the effects of Hund's coupling and anisotropic, orbital-dependent exchange interactions. Using a combination of mean-field theory, linear flavor-wave theory, and variational Monte Carlo, we show that this model harbors a quantum spin-orbital liquid over a wide parameter regime around the SU(4)-symmetric point. For large Hund's coupling, a ferromagnetic antiferro-orbital ordered state appears, while a valence-bond crystal combined with a vortex orbital state is stabilized by dominant orbital-dependent exchange interactions.

Hidden SU(2) symmetries, the symmetry hierarchy, and the emergent eightfold way in spin-1 quantum magnets

The largest allowed symmetry in a spin-1 quantum system is an $SU(3)$ symmetry rather than the $SO(3)$ spin rotation. In this work, we reveal some $SU(2)$ symmetries as subgroups of $SU(3)$ that, to the best of our knowledge, have not previously been recognized. Then, we construct $SU(2)$ symmetric Hamiltonians and explore the ground-state phase diagram in accordance with the $SU(3)\supset SU(2)\times U(1)$ symmetry hierarchy. It is natural to treat the eight generators of the $SU(3)$ symmetry on an equal footing; this approach is called the eight-fold way. We find that the spin spectral functions and spin quadrupole spectral functions share the same structure, provided that the elementary excitations are flavor waves at low energies, which serves as a clue to the eight-fold way. An emergent $S=1/2$ quantum spin liquid is proposed to coexist with gapful spin nematic order in one of the ground states. In analogy to quantum chromodynamics, we find the gap relation for hydrodynamic modes in quantum spin-orbital liquid states, which is nothing but the Gell-Mann-Okubo formula.

Hopping-Induced Ground-State Magnetism in 6H Perovskite Iridates.

Investigation of elementary excitations has advanced our understanding of many-body physics governing most physical properties of matter. Recently spin-orbit excitons have drawn much attention, whose condensates near phase transitions exhibit Higgs mode oscillations, a long-sought-after physical phenomenon [A. Jain, etal., Nat. Phys. 13, 633 (2017)NPAHAX1745-247310.1038/nphys4077]. These critical transition points, resulting from competing spin-orbit coupling (SOC), local crystalline symmetry, and exchange interactions, are not obvious in iridium-based materials, where SOC prevails in general. Here, we present results of resonant inelastic x-ray scattering on a spin-orbital liquid Ba_{3}ZnIr_{2}O_{9} and three other 6H-hexagonal perovskite iridates that show magnetism, contrary to the nonmagnetic singlet ground state expected due to strong SOC. Our results show that substantial hopping between closely placed Ir^{5+} ions within Ir_{2}O_{9} dimers in these 6H iridates modifies spin-orbit coupled states and reduces spin-orbit excitation energies. Here, we are forced to use at least a two-site model to match the excitation spectrum going in-line with the strong intradimer hopping. Apart from SOC, low-energy physics of iridates is thus critically dependent on hopping and may not be ignored even for systems having moderate hopping, where the excitation spectra can be explained using an atomic model. SOC, which is generally found to be 0.4-0.5eV in iridates, is scaled in effect down to ∼0.26 eV for the 6H systems, sustaining the hope of achieving quantum criticality by tuning Ir-Ir separation.

SU(4)-symmetric spin-orbital liquids on the hyperhoneycomb lattice

We study the effective spin-orbital model that describes the magnetism of $4{d}^{1}$ or $5{d}^{1}$ Mott insulators in ideal tricoordinated lattices. In the limit of vanishing Hund's coupling, the model has an emergent SU(4) symmetry, which is made explicit by means of a Klein transformation on pseudospin degrees of freedom. Taking the hyperhoneycomb lattice as an example, we employ parton constructions with fermionic representations of the pseudospin operators to investigate possible quantum spin-orbital liquid states. We then use variational Monte Carlo (VMC) methods to compute the energies of the projected wave functions. Our numerical results show that the lowest-energy quantum liquid corresponds to a zero-flux state with a Fermi surface of four-color fermionic partons. In spite of the Fermi surface, we demonstrate that this state is stable against tetramerization. A combination of linear flavor wave theory and VMC applied to the complete microscopic model also shows that this liquid state is stable against the formation of collinear long-range order.

Two-dimensional triangular-lattice Cu(OH)Cl, belloite, as a magnetodielectric system

Quantum spins on a triangular lattice may bring out intriguing and exotic quantum ground states. Here we report a magnetodielectric system of CuOHCl wherein $S=1/2\mathrm{C}{\mathrm{u}}^{2+}$ spins constitute a two-dimensional triangular lattice with the layers weakly coupled via Cl-H-O bonding. Despite strong magnetic interactions, as expected from the relatively high value of ${\ensuremath{\theta}}_{\mathrm{CW}}=\ensuremath{-}100\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, antiferromagnetic transition occurred at ${T}_{N}=11\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, followed by an uprising turn of the magnetic susceptibility below \ensuremath{\sim}7 K. Neutron-diffraction experiment revealed a coplanar spin structure on the triangular lattice below the ${T}_{N}$, with each spin pointing toward the center of a triangle. Of the three spins on a triangle, two are antiparallel and the third one is angled ${120}^{\ensuremath{\circ}}$ to the antiparallel spins. A concerted effect of geometric frustration in the triangular lattice and superexchange interactions through a zig-zag path via double Cu-O-Cu and double Cu-Cl-Cu bridges counted for this spin arrangement. Further investigation using dielectric constant and heat capacity measurements, as well as a microscopic probe of muon spin rotation, revealed a magnetodielectric effect and the possibility of multiferroic transition at ${T}^{*}\ensuremath{\sim}5\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, which is suspected to be in close relation to geometric frustration in this triangular lattice. The present paper presents a magnetodielectric system on a two-dimensional triangular lattice with chemical stoichiometry. It can also serve as a rare reference to the hotly debated quantum spin-orbital liquid compound $\mathrm{LiNi}{\mathrm{O}}_{2}$.

Emergent SU(4) Symmetry in α-ZrCl_{3} and Crystalline Spin-Orbital Liquids.

While the enhancement of spin-space symmetry from the usual SU(2) to SU(N) is promising for finding nontrivial quantum spin liquids, its realization in magnetic materials remains challenging. Here, we propose a new mechanism by which SU(4) symmetry emerges in the strong spin-orbit coupling limit. In d^{1} transition metal compounds with edge-sharing anion octahedra, the spin-orbit coupling gives rise to strongly bond-dependent and apparently SU(4)-breaking hopping between the J_{eff}=3/2 quartets. However, in the honeycomb structure, a gauge transformation maps the system to an SU(4)-symmetric Hubbard model. In the strong repulsion limit at quarter filling, as realized in α-ZrCl_{3}, the low-energy effective model is the SU(4) Heisenberg model on the honeycomb lattice, which cannot have a trivial gapped ground state and is expected to host a gapless spin-orbital liquid. By generalizing this model to other three-dimensional lattices, we also propose crystalline spin-orbital liquids protected by this emergent SU(4) symmetry and space group symmetries.

Cu-Sb dumbbell arrangement in the spin-orbital liquid candidate Ba3CuSb2O9

The absence of both spin freezing and of a static Jahn-Teller effect have lead to the proposition that Ba$_3$CuSb$_2$O$_9$ is a quantum spin-orbital liquid. However, theoretical understanding of the microscopic origin of this behavior has been hampered by a lack of consensus on the lattice structure. Cu ions have been proposed to realize either a triangular lattice, a short-range ordered honeycomb lattice or a disordered lattice with stripelike correlations. Here we analyze the stability of idealized versions of these arrangements using density functional theory. We find stripe order of Cu ions to be energetically favored, hinting towards stripelike local Cu-Cu arrangements, while long-range order is presumably hindered due to disorder effects. Furthermore, we find evidence of significant interlayer interactions between Cu-Sb dumbbells, which affects the out-of-plane arrangement. Analysis of the relaxed crystal structures, electronic properties and tight-binding parameters provides clues as to the nature of the Jahn-Teller distortions.

Dynamics of a j=32 quantum spin liquid

We study a spin-orbital model for $4{d}^{1}$ or $5{d}^{1}$ Mott insulators in ordered double perovskites with strong spin-orbit coupling. This model is conveniently written in terms of pseudospin and pseudo-orbital operators representing multipoles of the effective $j=\frac{3}{2}$ angular momentum. Similarities between this model and the effective theories of Kitaev materials motivate the proposal of a chiral spin-orbital liquid with Majorana fermion excitations. The thermodynamic and spectroscopic properties of this quantum spin liquid are characterized using parton mean-field theory. The heat capacity, spin-lattice relaxation rate, and dynamic structure factor for inelastic neutron scattering are calculated and compared with the experimental data for the spin liquid candidate ${\mathrm{Ba}}_{2}{\mathrm{YMoO}}_{6}$. Moreover, based on a symmetry analysis, we discuss the operators involved in resonant inelastic x-ray scattering (RIXS) amplitudes for double-perovskite compounds. In general, the RIXS cross sections allow one to selectively probe pseudospin and pseudo-orbital degrees of freedom. For the chiral spin-orbital liquid in particular, these cross sections provide information about the spectrum for different flavors of Majorana fermions.