Quantum spin liquids (QSLs) are strongly correlated systems displaying fascinating phenomena like long-range entanglement and fractionalized excitations. The research on these states has since its beginning followed trends generated by the synthesis of new compounds and the construction of new theoretical tools. In coherence with this history, a manifold of new results about QSLs were established during the past decade due to studies on the integrable Kitaev model on the honeycomb lattice. This j = 1/2 model displays bond-dependent and anisotropic exchanges that are essential to stabilize its QSL ground state with Majorana fermion excitations and emergent Z2 gauge field. Even more interestingly, this model is relevant to understand the magnetism of a certain class of 4/5d5 Mott insulators with specific lattice constraints, t2g orbital degeneracy and strong spin-orbit coupling (SOC). This mechanism defining these so-called Kitaev materials can be applied to similar compounds based on transition metal ions in different electronic configurations. In this thesis, I investigate minimal models for two types of 4/5d1 Mott insulators: the ones on the ordered double perovskite structure (ODP) and the ones isostructural to the Kitaev materials. Their effective models generically show bond-dependent and anisotropic interactions involving multipoles of an effective j = 3/2 angular momentum. Such degrees of freedom are conveniently written in terms of pseudospin s and pseudo-orbital τ operators resembling spin and orbital operators of Kugel-Khomskii models with twofold orbital degeneracy. Despite their anisotropy, the two realistic models display continuous global symmetries in the limit of vanishing Hund\'s coupling enhancing quantum fluctuations and possibly stabilizing a QSL phase. Parton mean-field theory was used to propose fermionic QSLs that will be called quantum spin-orbital liquids (QSOLs) due their dependence with s and τ. On ODPs, I studied a chiral QSOL with Majorana fermion excitations and a gapless spectrum characterized by nodal lines along the edges of the Brillouin zone. These nodal lines are topological defects of a non-Abelian Berry connection and the system exhibits dispersing surface states. Several experimental responses of the chiral QSOL within the mean-field approximation are compared with the experimental data available for the spin liquid candidate Ba2YMoO6. Moreover, based on a symmetry analysis, I discuss the operators involved in resonant inelastic X-ray scattering (RIXS) amplitudes for 4/5d1 Mott insulators and show that 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. The model for materials isostructural to the Kitaev materials has an emergent SU(4) symmetry that is made explicit by means of a Klein transformation on pseudospin degrees of freedom. The model is known to stabilize a QSOL on the honeycomb lattice and instigated the investigation of QSOLs on a generalization of this lattice to three dimensions. Parton mean-field theory was used once again to propose the liquid states, and a variational Monte Carlo (VMC) method was used to compute the energies of the projected wave functions. The numerical results show that the lowest-energy QSOL corresponds to a zero-flux state with a Fermi surface of four-color fermionic partons. Further VMC computations also revealed that this state is stable against formation of plaquette ordering (tetramerization). The energy of this QSOL is highly competitive even when Hund\'s coupling induced perturbations are included, as shown by comparison with simple ordered states. Extensions and perspectives for future work are discussed in the end of this thesis.
Quantum spin liquids (QSLs) are strongly correlated systems displaying fascinating phenomena like long-range entanglement and fractionalized excitations. The research on these states has since its beginning followed trends generated by the synthesis of new compounds and the construction of new theoretical tools. In coherence with this history, a manifold of new results about QSLs were established during the past decade due to studies on the integrable Kitaev model on the honeycomb lattice. This j = 1/2 model displays bond-dependent and anisotropic exchanges that are essential to stabilize its QSL ground state with Majorana fermion excitations and emergent Z2 gauge field. Even more interestingly, this model is relevant to understand the magnetism of a certain class of 4/5d5 Mott insulators with specific lattice constraints, t2g orbital degeneracy and strong spin-orbit coupling (SOC). This mechanism defining these so-called Kitaev materials can be applied to similar compounds based on transition metal ions in different electronic configurations. In this thesis, I investigate minimal models for two types of 4/5d1 Mott insulators: the ones on the ordered double perovskite structure (ODP) and the ones isostructural to the Kitaev materials. Their effective models generically show bond-dependent and anisotropic interactions involving multipoles of an effective j = 3/2 angular momentum. Such degrees of freedom are conveniently written in terms of pseudospin s and pseudo-orbital τ operators resembling spin and orbital operators of Kugel-Khomskii models with twofold orbital degeneracy. Despite their anisotropy, the two realistic models display continuous global symmetries in the limit of vanishing Hund's coupling enhancing quantum fluctuations and possibly stabilizing a QSL phase. Parton mean-field theory was used to propose fermionic QSLs that will be called quantum spin-orbital liquids (QSOLs) due their dependence with s and τ. On ODPs, I studied a chiral QSOL with Majorana fermion excitations and a gapless spectrum characterized by nodal lines along the edges of the Brillouin zone. These nodal lines are topological defects of a non-Abelian Berry connection and the system exhibits dispersing surface states. Several experimental responses of the chiral QSOL within the mean-field approximation are compared with the experimental data available for the spin liquid candidate Ba2YMoO6. Moreover, based on a symmetry analysis, I discuss the operators involved in resonant inelastic X-ray scattering (RIXS) amplitudes for 4/5d1 Mott insulators and show that 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. The model for materials isostructural to the Kitaev materials has an emergent SU(4) symmetry that is made explicit by means of a Klein transformation on pseudospin degrees of freedom. The model is known to stabilize a QSOL on the honeycomb lattice and instigated the investigation of QSOLs on a generalization of this lattice to three dimensions. Parton mean-field theory was used once again to propose the liquid states, and a variational Monte Carlo (VMC) method was used to compute the energies of the projected wave functions. The numerical results show that the lowest-energy QSOL corresponds to a zero-flux state with a Fermi surface of four-color fermionic partons. Further VMC computations also revealed that this state is stable against formation of plaquette ordering (tetramerization). The energy of this QSOL is highly competitive even when Hund's coupling induced perturbations are included, as shown by comparison with simple ordered states. Extensions and perspectives for future work are discussed in the end of this thesis.
We study a spin-orbital model for 4d1 or 5d1 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=23 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 Ba2YMoO6. 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.
ABSTRACT Quantum spin liquids (QSLs) are magnetically frustrated phases characterized by spin fractionalization, emergent gauge fields, and long‐range entanglement. Quantum spin–orbital liquids (QSOLs) form a subset of QSLs with fluctuating orbital degrees of freedom, normally adding a layer of complexity to an already involved research field. This topical review provides guidelines for understanding a specific type of QSOL in which the orbital operators facilitate the analysis of quantum liquids, thereby providing adequate starting points for /exploring these phases. Such models are extensions of the spin‐1/2 Kitaev honeycomb model (KHM), in the sense that their exact solutions depend on an extensive number of conserved quantities, combined with a mapping to a problem of Majorana fermions hopping on a static gauge field. The starting points to understand such models are classical Hamiltonians characterized by bond‐dependent Ising interactions. Such classical models are exactly solvable in spin basis thanks to their extensive symmetries and can be directly connected to classical spin ice (CSI) systems that satisfy a Gauss law. QSOLs are easily stabilized in these models by applying a transverse field or introducing other exchange mechanisms that preserve the conserved local operators. The theory of such Ising QSOLs bridges the KHM to specific types of CSIs, thus providing further insight into paradigmatic forms of spin liquids. Furthermore, bond‐dependent Ising models are related to minimal Hamiltonians describing Rydberg‐atom simulations, which provide experimental grounds for investigating them.
Quantum spin liquids, systems in which quantum fluctuations prevent the magnetic ordering of the spin degrees of freedom down to zero temperature, have been the source of much recent theoretical and experimental interest. These systems are characterised by their long ranged entangled states, preserve symmetries down to zero Kelvin, and have been shown to exhibit fascinating properties such as a topological ground state degeneracy and fractionalised spin excitations. In this thesis, we study several of these phases. The first, Kitaev spin liquids, appear in strongly spin-orbit coupled systems, where the SU(2) spin symmetry is broken. Within our mean field approach, we study the quantum phase transition from the gapless Z 2 spin liquid to a magnetically ordered phase within the Heisenberg-Kitaev model. Beyond the mean field theory, we argue that the gauge structure of the spin liquid plays a crucial role in this transition, leading to a confinement of spinons and the generation of magnetic order. We also discuss the three-dimensional iridate compounds, where the Kitaev spin liquid phase has topologically protected bulk and surface excitations. We next discuss spin liquids appearing on the geometrically frustrated kagome lattice. First, we consider non-Kramers spin liquids, in which the spin structure of the theory is protected by lattice, rather than time-reversal, symmetry. As a result, more phases are allowed, which have different properties than those which transform as Kramers doublets. In addition, these may have positive experimental signatures in the Raman scattering intensity, offering a clear path to detect such a state. Finally, we examine possible spin liquid phases on a breathing kagome lattice, where we find a stable Z2 spin liquid to be the ground state. This may help to guide future numerical studies of the kagome lattice Heisenberg model, and may also be relevant to DQVOF, a recently discovered spin liquid candidate compound.
Frustrated magnetism provides a rich platform for realizing exotic quantum phases in condensed matter systems. Among these, quantum spin liquids (QSLs) are a particularly intriguing class of states that exhibit no magnetic ordering and preserve all symmetries down to zero temperature. Just as conventional magnets can be thought of as spin crystals,QSLs represent their liquid analogs. This thesis explores two broad types of QSLs in two-dimensional magnets, with a focus on their dynamic properties and the nature of transitions from conventional magnetic states into QSL phases. QSLs are topological phases that host fractionalized excitations known as spinons. In these states, mobile spinons are coupled to an emergent gauge field, forming a highly entangled phase of matter. The first part of this thesis focuses on Dirac spin liquids (DSLs), a class of QSLs where spinons exhibit a gapless Dirac dispersion. To study the dynamicsof these spin liquids beyond leading-order mean-field theory, we develop a novel large-N fermionic limit of gapless spinons. In this limit, all gauge excitations are suppressed, and the leading-order corrections instead arise from order parameter fluctuations, which may condense and drive transitions into symmetry-broken phases from the parent DSL. Incorporating random phase approximation (RPA) corrections to the spin susceptibility, we find that sharp, spin-wave–like modes are recovered in the excitation spectrum. This methodology successfully captures characteristic features of the dynamics near phase transitions and in weakly symmetry-broken phases proximate to a DSL. We apply this approach to microscopic models, including the J1-J2 XXZ model on the triangular lattice and the J1-J3 XXZ model on the honeycomb lattice. These models closely represent a wide range of frustrated materials, such as triangular and honeycomb cobaltates and triangular ytterbium compounds. Our theoretical predictions show excellent agreement with experimentally measured inelastic neutron scattering spectra from these materials. Gapless spinons can also sometimes become gapped through chiral symmetry breaking, leading to the formation of a chiral spin liquid (CSL). The CSL is an archetypal bosonic realization of a fractional quantum Hall (FQH) state at half-filling, and has been proposed as a time-reversal–breaking ground state in a variety of frustrated spin models. The second part of this thesis addresses the intriguing possibility of realizing a CSL through the "melting" of a chiral spin crystal—a conventional magnet with non-coplanar ordering. Such a transition offers a physically appealing analogue to the melting of a Wigner crystal into a fermionic FQH liquid. Focusing on the kagome lattice, where chiral interactions are knownto stabilize a CSL ground state, we study the effects of additional long-range Heisenberg interactions and demonstrate a phase transition into a non-coplanar octahedral magnetic order. To describe the universal class of transition between a CSL and a non-coplanar anti-ferromagnetic order, we then develop a novel Chern-Simons–matter field theory framework, constrained by symmetry principles and symmetry fractionalization patterns. This thesis thus provides new insights into the dynamical signatures and phase transitions of quantum spin liquids, offering a bridge between theoretical models and experimental observations in frustrated magnetic systems.
Transition metal compounds have been central to the study of quantum magnetism in recent years. The multi-orbital nature of these compounds together with the interplay between electron-electron interactions, crystal field effects and spin-orbit coupling leads to spin-orbit entangled wave functions, known as pseudospins. Pseudospins depend highly on the electron filling of the transition metal, and are highly spatially anisotropic which leads to frustrated, bond-dependent exchange interactions. These interactions manifest themselves in a variety of non-trivial ways, depending on the structure and dimensionality of the underlying lattice, which we explore in this thesis. In one dimension we show that CoNb2O6, thought to be the best known candidate for the 1D transverse field Ising model, is an example of a rare 1D Kitaev chain where the bond-dependent pseudospin interactions are responsible for the transverse field Ising behaviour. On the two dimensional honeycomb lattice we propose a mechanism to generate the bond-dependent, exactly solvable, Yao-Lee interaction among others. We show at the exactly solveable point of our model, the ground state is a quantum spin-orbital liquid with emergent fermionic octupolar excitations. Finally, we study the three dimensional 5d double-perovskites (DPs), which have been proposed to be the first d-orbital candidates exhibiting hidden octupolar order. We develop a microscopic theory for these materials, and determine several microscopic mechanisms that may be responsible for stabilizing octupolar order.
Theory of Dirac Spin-Orbital Liquids: monopoles, anomalies, and applications to SU(4) honeycomb models
Dirac spin liquids represent a class of highly-entangled quantum phases in two dimensional Mott insulators, featuring exotic properties such as critical correlation functions and absence of well-defined low energy quasi-particles. Existing numerical works suggest that the spin-orbital SU(4) symmetric Kugel-Khomskii model of Mott insulators on the honeycomb lattice realizes a Dirac spin-orbital liquid, described at low energy by (2+1)d quantum electrodynamics (QED3) with Nf=8 Dirac fermions. We generalize methods previously developed for SU(2) spin systems to analyze the symmetry properties and stability of the Dirac spin-orbital liquid. We conclude that the standard Dirac state in the SU(4) honeycomb system, based on a simple parton mean-field ansatz, is intrinsically unstable at low energy due to the existence of a monopole perturbation that is allowed by physical symmetries and relevant under renormalization group flow. We propose two plausible alternative scenarios compatible with existing numerics. In the first scenario, we propose an alternative U(1) Dirac spin-orbital liquid, which is similar to the standard one except for its monopole symmetry quantum numbers. This alternative U(1) state represents a stable gapless phase. In the second scenario, we start from the standard U(1) Dirac liquid and Higgs the U(1) gauge symmetry down to Z4. The resulting Z4 Dirac spin-orbital liquid is stable. We also discuss the continuous quantum phase transitions from the Z4 Dirac liquids to conventional symmetry-breaking orders, described by the QED3 theory with Nf=8 supplemented with a critical charge-4 Higgs field. We discuss possible ways to distinguish these scenarios in numerics. We also extend previous calculations of the quantum anomalies of QED3 and match with generalized lattice Lieb-Schultz-Mattis constraints.