In this computational study, we explore a viable route to access the Kitaev-quantum spin liquid (QSL) state in a recently synthesized monolayer of a so-called spin-orbit assisted Mott insulator OsCl 3 . In addition to other magnetic ground states in different regions, a substantial region of small J H / U in our Hubbard U –Hund's J H quantum phase diagram, obtained by combining second-order perturbation and pseudo-fermion functional renormalization group calculations, hosts Kitaev-QSL phase. Only the first neighbor Kitaev interaction of a smaller magnitude, nearly independent of the choice of U , is obtained in this region. Experimental tuning of the single parameter J H to access the QSL state can purportedly be achieved with epitaxial strain in advanced crystal growth techniques. Furthermore, negligibly small farther neighbor interactions appear as a distinct feature of monolayer OsCl 3 , suggesting this material to be a better candidate for the exploration of the possible Kitaev-QSL state than previously proposed materials. Published by the American Physical Society 2024
The Kitaev model, whose ground state is a quantum spin liquid (QSL), was originally conceived for spin
S=1/2 moments on a honeycomb lattice. In recent years, the model has been extended to higher
S from both theoretical and experimental interests, but the stability of the QSL ground state has not been systematically clarified for general
S, especially in the presence of other additional interactions, which inevitably exist in candidate materials. Here we study the spin-
S Kitaev-Heisenberg models by using an extension of the pseudofermion functional renormalization group method to general
S. We show that, similar to the
S=1/2 case, the phase diagram for higher
S contains the QSL phases in the vicinities of the pristine ferromagnetic and antiferromagnetic Kitaev models, in addition to four magnetically ordered phases. We find, however, that the QSL phases shrink rapidly with increasing
S, becoming vanishingly narrow for $S\ensuremath{\ge}2$, whereas the phase boundaries between the ordered phases remain almost intact. Our results provide a reference for the search for higher-
S Kitaev materials.
The quantum spin liquid (QSL) state of Kitaev-like materials, such as iridium oxides A 2IrO3 and α-RuCl3, has been explored in depth. The half-filled Kitaev–Hubbard model with bond-dependent hopping terms is used to describe the Kitaev-like materials, which is calculated using the state-of-the-art fermionic projected entangled pair states method. We find a QSL phase near the Mott insulator transition, which has a strong first-order transition to the semi-metal phase with the decrease of Hubbard U. We suggest that a promising approach to finding QSL states is by finding iridium oxides that are near the Mott insulator transition.
The quantum spin liquid (QSL) state has been searched intensively in Kitaev-like materials, such as the Iridium oxides
A2IrO
3 and
α-RuCl
3. The half-filled Kitaev-Hubbard model with bond dependent hopping terms is used to describe the Kitaev-like materials, which is calculated using the state-of-the-art fermionic projected entangled pair states (fPEPS) method. We find a QSL phase near the Mott insulator transition, which has a strong first-order transition to the semi-metal phase with the decrease of Hubbard
U. We suggest that a promising routine to find the QSL is to find the Iridium oxides that are near the Mott insulator transitions.
In the quest for materials hosting Kitaev spin liquids, much of the efforts have been focused on the fourth- and fifth-row transition metal compounds, which are spin-orbit coupling--assisted Mott insulators. Here we study the structural and magnetic properties of
3d transition metal oxides,
Na2Co2TeO6 and
Na3Co2SbO6. The partial occupancy of sodium in former compound is addressed using a cluster expansion, and a honeycomb lattice of sodiums is found to be energetically favored. Starting from the ab initio band structures, a many-body second-order perturbation theory leads to a pseudospin-
21 Hamiltonian with estimated magnetic interactions. We show that the experimentally observed zigzag magnetic state is stabilized only when the first-neighbor Kitaev coupling dominates over the Heisenberg term, both of which are highly suppressed due to presence of
eg orbitals. A third-neighbor Heisenberg interaction is found dominant in both these compounds. We also present a phase diagram for
Na2Co2TeO6 by varying the electron-electron and spin-orbit interactions. The computed spin excitation spectra are found to capture essential features of recent experimental magnon spectrum, lending support to our results.
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.
Unambiguous identification of the Kitaev quantum spin liquid (QSL) in materials remains a huge challenge despite many encouraging signs from various measurements. To facilitate the experimental detection of the Kiteav QSL, here we propose to use remnant charge response in Mott insulators hosting QSL to identify the key signatures of QSL. We predict an emergent orbital magnetization in a Kitaev system in an external magnetic field. The direction of the orbital magnetization can be flipped by rotating the external magnetic field in the honeycomb plane. The orbital magnetization is demonstrated explicitly through a detailed microscopic analysis of the multiorbital Hubbard-Kanamori Hamiltonian and also supported by a phenomenological picture. We first derive the localized electrical loop current operator in terms of the spin degrees of freedom. Thereafter, utilizing the Majorana representation, we estimate the loop currents in the ground state of the chiral Kitaev QSL state, and obtain the consequent current textures, which are responsible for the emergent orbital magnetization. Finally, we discuss the possible experimental techniques to visualize the orbital magnetization which can be considered as the signatures of the underlying excitations.