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arXiv:2206.10647 · Physical review. B./Physical review. B

Field-induced Kitaev multipolar liquid in spin-orbit coupled d2 honeycomb Mott insulators

Ahmed Rayyan, Derek Churchill, Hae‐Young Kee

Published Jan 23, 2023• 13 citations
arXivHTMLPDF

Abstract

The Kitaev model, characterized by bond-dependent Ising spin interactions among spin-orbit entangled dipole moments in Mott insulators, offered a new approach to quantum spin liquids. Motivated by another type of bond-dependent interaction among quadrupole moments in $5{d}^{2}$ Mott insulators, we provide a microscopic route to uncover the Kitaev multipolar liquid, featuring fractionalized excitations out of non-Kramers doublets carrying multipole moments. The key ingredient is the magnetic field that allows for bond-anisotropic quadrupole-octupole interactions via mixing with the excited triplet states. The conditions to realize signatures of this phase in real materials are also discussed.

DOI
10.1103/physrevb.107.l020408

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The Kitaev model, characterized by bond-dependent Ising spin interactions among spin-orbit entangled dipole moments in Mott insulators, offered a new approach to quantum spin liquids. Motivated by another type of bond-dependent interaction among quadrupole moments in 5d25{d}^{2}5d2 Mott insulators, we provide a microscopic route to uncover the Kitaev multipolar liquid, featuring fractionalized excitations out of non-Kramers doublets carrying multipole moments. The key ingredient is the magnetic field that allows for bond-anisotropic quadrupole-octupole interactions via mixing with the excited triplet states. The conditions to realize signatures of this phase in real materials are also discussed.
We study an exactly solvable model with bond-directional quadrupolar and octupolar interactions between spin-orbital entangled jeff=32{j}_{\mathrm{eff}}=\frac{3}{2}jeff​=23​ moments on the honeycomb lattice. We show that this model features a multipolar spin liquid phase with gapless fermionic excitations. In the presence of perturbations that break time-reversal and rotation symmetries, we find Abelian and non-Abelian topological phases in which the Chern number evaluates to 0, $\ifmmode\pm\else\textpm\fi{}1$, and $\ifmmode\pm\else\textpm\fi{}2$. We also investigate quantum phase transitions out of the multipolar spin liquid using a parton mean-field approach and orbital wave theory. In the regime of strong integrability-breaking interactions, the multipolar spin liquid gives way to ferroquadrupolar-vortex and antiferro-octupolar ordered phases that harbor a hidden spin-12\frac{1}{2}21​ Kitaev spin liquid. Our work unveils mechanisms for unusual multipolar orders and quantum spin liquids in Mott insulators with strong spin-orbit coupling.
In the field of quantum magnetism, the exactly solvable Kitaev honeycomb model serves as a paradigm for the fractionalization of spin degrees of freedom and the formation of [Formula: see text] quantum spin liquids. An intense experimental search has led to the discovery of a number of spin-orbit entangled Mott insulators that realize its characteristic bond-directional interactions and, in the presence of magnetic fields, exhibit no indications of long-range order. Here, we map out the complete phase diagram of the Kitaev model in tilted magnetic fields and report the emergence of a distinct gapless quantum spin liquid at intermediate field strengths. Analyzing a number of static, dynamical, and finite temperature quantities using numerical exact diagonalization techniques, we find strong evidence that this phase exhibits gapless fermions coupled to a massless U(1) gauge field. We discuss its stability in the presence of perturbations that naturally arise in spin-orbit entangled candidate materials.
In the search for quantum spin liquids, candidate materials for the Kitaev model and its extensions have been intensively explored during the past decade, as the models realize the exact quantum spin liquids in the ground state. Thus far, insulating magnets in the low-spin d5{d}^{5}d5 electron configuration under the strong spin-orbit coupling have been studied for realizing the Kitaev-type bond-dependent anisotropic interactions between the spin-orbital entangled Kramers doublets. To extend the candidates, here we investigate the systems in a high-spin d7{d}^{7}d7 electron configuration, whose ground state is described by the spin-orbital entangled Kramers doublet. By the second-order perturbation in terms of the ${t}_{2g}\ensuremath{-}{t}_{2g}$ and ${t}_{2g}\ensuremath{-}{e}_{g}$ hoppings, we show that the effective spin model possesses the anisotropic Kitaev interactions as well as the isotropic Heisenberg ones. While the Kitaev interaction is always ferromagnetic, the Heisenberg interaction can become either ferromagnetic or antiferromagnetic depending on the Coulomb interactions and the crystalline electric fields. We also derive the effective model for the low-spin d5{d}^{5}d5 electron configuration within the same perturbation scheme, in which the Kitaev interaction becomes both ferromagnetic and antiferromagnetic, while the Heisenberg one is always ferromagnetic. Referring to the previous study for the Kitaev-Heisenberg model, we find that the quantum spin liquid phase exists in the reasonable parameter region in both d7{d}^{7}d7 and d5{d}^{5}d5 cases, while the former has a richer structure of the phase diagram. We discuss the advantages of the d7{d}^{7}d7 case in comparison with the d5{d}^{5}d5 case. Our results indicate that the high-spin d7{d}^{7}d7 state provides another platform for the Kitaev-type quantum spin liquid.
Abstract The Kitaev spin liquid, a ground state of the bond-dependent Kitaev model in a honeycomb lattice has been a center of attraction, since a microscopic theory to realize such an interaction in solid-state materials was discovered. A challenge in real materials though is the presence of the Heisenberg and another bond-dependent Gamma interactions detrimental to the Kitaev spin liquid, and there have been many debates on their relative strengths. Here we offer a strategy to extract the Kitaev interaction out of a full microscopic model by utilizing the symmetries of the Hamiltonian. Two tilted magnetic field directions related by a two-fold rotational symmetry generate distinct spin excitations originated from a specific combination of the Kitaev and Gamma interactions. Together with the in- and out-of-plane magnetic anisotropy, one can determine the Kitaev and Gamma interactions separately. Dynamic spin structure factors are presented to motivate future experiments. The proposed setups will advance the search for Kitaev materials.
Quantum spin liquids, a highly topologically entangled, dynamically correlated state where quantum fluctuations preclude any long-range ordering down to absolute zero. In the search for a topologically robust qubit, the scientific community has been in continuous hunt for real quantum spin liquid systems. Alexei Kitaev in his exactly solvable model for a spin-1/2 two-dimensional honeycomb lattice, presented a system that hosts a topologically protected state (Majorana zero-modes). Under an applied external field, the Kitaev spin liquids turn into a topologically non-trivial chiral spin-liquid state with non-abelian anionic excitations, which is crucial for quantum computing. Earlier theoretical predictions advocated that Kitaev physics can be realized in spin-orbit-coupled Mott insulators such as honeycomb irradiates and ruthenates. However, the experimental findings continuously challenge the theoretical aspects, indicating the presence of non-Kitaev interactions in real materials, where the dimensionality, disorder (vacancy), chemical composition, generalized spin-S, and external perturbations (pressure, magnetic field, temperature) can actively tune the Kitaev interactions and the ground state excitations. In this review article, a comprehensive discussion is included with an updated literature survey in the context of the potential of Raman spectroscopy as a probe for Kitaev quantum spin liquids.
The exact solution of Kitaev's spin-1/21/21/2 honeycomb spin-liquid model has sparked an intense search for Mott insulators hosting bond-dependent Kitaev interactions, of which Na2IrO3{\mathrm{Na}}_{2}{\mathrm{IrO}}_{3}Na2​IrO3​ and $\ensuremath{\alpha}\text{\ensuremath{-}}\mathrm{Ru}{\mathrm{Cl}}_{3}$ are prime examples. Subsequently, it has been proposed that also spin-1 and spin-3/23/23/2 analogs of Kitaev interactions may occur in materials with strong spin-orbit coupling. As a minimal model to describe these Kitaev materials, we study the Heisenberg-Kitaev Hamiltonian in a consistent 1/S1/S1/S expansion, with SSS being the spin size. We present a comprehensive study of this model in the presence of an external magnetic field applied along two different directions, [001] and [111], for which an intricate classical phase diagram has been reported. In both settings, we employ spin-wave theory in a number of ordered phases to compute phase boundaries at the next-to-leading order in 1/S1/S1/S and show that quantum corrections substantially modify the classical phase diagram. More broadly, our work presents a consistent route to investigate the leading quantum corrections in spin models that break spin-rotational symmetry.