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 provide an exact study of dynamical correlations for the quantum spin-orbital liquid phases of an SU(2)-symmetric Kitaev honeycomb lattice model. We show that the spin dynamics in this Kugel-Khomskii type model is exactly the density-density correlation function of S=1 fermionic magnons, which could be probed in resonant inelastic x-ray scattering experiments. We predict the characteristic signatures of spin-orbital fractionalization in inelastic scattering experiments and compare them to the ones of the spin-anisotropic Kitaev honeycomb spin liquid. In particular, the resonant inelastic x-ray scattering response shows a characteristic momentum dependence directly related to the dispersion of fermionic excitations. The neutron scattering cross section displays a mixed response of fermionic magnons as well as spin-orbital excitations. The latter has a bandwidth of broad excitations and a vison gap that is three times larger than that of the spin-1=2 Kitaev model.
Motivated by recent synthesis of the hyperhoneycomb material $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$, we study the dynamical structure factor (DSF) of the corresponding 3D Kitaev quantum spin-liquid (QSL), whose fractionalized degrees of freedom are Majorana fermions and emergent flux loops. The properties of this 3D model are known to differ in important ways from those of its 2D counterpart---it has a finite-temperature phase transition, as well as distinct features in the Raman response. We show, however, that the qualitative behavior of the DSF is broadly dimension-independent. Characteristics of the 3D DSF include a response gap even in the gapless QSL phase and an energy dependence deriving from the Majorana fermion density of states. Since the majority of the response is from states containing a single Majorana excitation, our results suggest inelastic neutron scattering as the spectroscopy of choice to illuminate the physics of Majorana fermions in Kitaev QSLs.
We calculate the resonant inelastic x-ray scattering (RIXS) response of the Kitaev honeycomb model, an exactly solvable quantum-spin-liquid model with fractionalized Majorana and flux excitations. We find that the fundamental RIXS channels, the spin-conserving (SC) and the non-spin-conserving (NSC) ones, do not interfere and give completely different responses. SC RIXS picks up exclusively the Majorana sector with a pronounced momentum dispersion, whereas NSC RIXS also creates immobile fluxes, thereby rendering the response only weakly momentum dependent, as in the spin structure factor measured by inelastic neutron scattering. RIXS can, therefore, pick up the fractionalized excitations of the Kitaev spin liquid separately, making it a sensitive probe to detect spin-liquid character in potential material incarnations of the Kitaev honeycomb model.
A prominent feature of quantum spin liquids is fractionalization of the spin degree of freedom. Fractionalized excitations have their own dynamics in different energy scales, and hence, affect finite-temperature (
T) properties in a peculiar manner even in the paramagnetic state harboring the quantum spin liquid state. We here present a comprehensive theoretical study of the spin dynamics in a wide
T range for the Kitaev model on a honeycomb lattice, whose ground state is a quantum spin liquid. In this model, the fractionalization occurs to break up quantum spins into itinerant matter fermions and localized
Z2 fluxes, which results in two crossovers at very different
T scales. Extending the previous study for the isotropic coupling case [J. Yoshitake, J. Nasu, and Y. Motome, Phys. Rev. Lett. 117, 157203 (2016)], we calculate the dynamical spin structure factor $S(\mathbf{q},\ensuremath{\omega})$, the NMR relaxation rate
1/T1, and the magnetic susceptibility $\ensuremath{\chi}$ while changing the anisotropy in the exchange coupling constants, by using the dynamical mean-field theory based on a Majorana fermion representation. We describe the details of the methodology including the continuous-time quantum Monte Carlo method for computing dynamical spin correlations and the maximum entropy method for analytic continuation. We confirm that the combined method provides accurate results in a wide
T range including the region where the spins are fractionalized. We find that also in the anisotropic cases the system exhibits peculiar behaviors below the high-
T crossover whose temperature is comparable to the average of the exchange constants: $S(\mathbf{q},\ensuremath{\omega})$ shows an inelastic response at the energy scale of the averaged exchange constant,
1/T1 continues to grow even though the equal-time spin correlations are saturated and almost
T independent, and $\ensuremath{\chi}$ deviates from the Curie-Weiss behavior. In particular, when the exchange interaction in one direction is stronger than the other two, the dynamical quantities exhibit qualitatively different
T dependences from the isotropic case at low
T, reflecting the opposite parity between the flux-free ground state and the flux-excited state, and a larger energy cost for flipping a spin in the strong interaction direction. On the other hand, when the exchange anisotropy is in the opposite way, the results are qualitatively similar to those in the isotropic case. All these behaviors manifest the spin fractionalization in the paramagnetic region. Among them, the dichotomy between the static and dynamical spin correlations is unusual behavior hardly seen in conventional magnets. We discuss the relation between the dichotomy and the spatial configuration of the
Z2 gauge fields. Our results could stimulate further experimental and theoretical analyses of candidate materials for the Kitaev quantum spin liquids.
We study the effective spin-orbital model that describes the magnetism of
4d1 or
5d1 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.