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arXiv:2503.10226 · npj Quantum Materials

Quantum spin liquid phases in Kitaev materials

Po-Hao Chou, Chung‐Yu Mou, Chung‐Hou Chung, Sungkit Yip

Published Aug 16, 2025• 4 citations
arXivHTMLPDF

Abstract

We develop a gauge-invariant renormalized mean-field theory (RMFT) to reliably find the quantum spin liquid (QSL) states and their field response for realistic Kitaev materials under strong magnetic fields and described by the generalized Kitaev J-K-Γ- $${\Gamma }^{{\prime} }$$ model. Remarkably, while our RMFT reproduces previous results based on using more complicated numerical methods, it also predicts several new stable QSL states. In particular, since Kitaev spin liquid (KSL) is no longer a saddle point solution, a new exotic 2-cone state distinct from the KSL is found to describe experimental observations well, and hence should be the candidate state realized in the Kitaev material, α-RuCl3. We further explore the mechanism for the suppression of the observed thermal Hall conductivity at low temperatures within the fermionic framework, and show that the polar-angle dependence of the fermionic gap can distinguish the found 2-cone state from the KSL state in further experiments.

DOI
10.1038/s41535-025-00811-1

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We develop a gauge-invariant renormalized mean-field theory (RMFT) to reliably find the quantum spin liquid (QSL) states and their field response for realistic Kitaev materials under strong magnetic fields and described by the generalized Kitaev J-K-Γ- Γ′{\Gamma }^{{\prime} }Γ′ model. Remarkably, while our RMFT reproduces previous results based on using more complicated numerical methods, it also predicts several new stable QSL states. In particular, since Kitaev spin liquid (KSL) is no longer a saddle point solution, a new exotic 2-cone state distinct from the KSL is found to describe experimental observations well, and hence should be the candidate state realized in the Kitaev material, α-RuCl3. We further explore the mechanism for the suppression of the observed thermal Hall conductivity at low temperatures within the fermionic framework, and show that the polar-angle dependence of the fermionic gap can distinguish the found 2-cone state from the KSL state in further experiments.
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Abstract Elementary excitations in entangled states such as quantum spin liquids may exhibit exotic statistics different from those obeyed by fundamental bosons and fermions. Non-Abelian anyons exist in a Kitaev spin liquid—the ground state of an exactly solvable model. A smoking-gun signature of these excitations, namely a half-integer quantized thermal Hall conductivity, was recently reported in α-RuCl3. While fascinating, a microscopic theory for this phenomenon remains elusive because the pure Kitaev model cannot display this effect in an intermediate magnetic field. Here we present a microscopic theory of the Kitaev spin liquid emerging between the low- and high-field states. Essential to this result is an antiferromagnetic off-diagonal symmetric interaction which allows the Kitaev spin liquid to protrude from the ferromagnetic Kitaev limit under a magnetic field. This generic model displays a strong field anisotropy, and we predict a wide spin liquid regime when the field is perpendicular to the honeycomb plane.
Abstract Elementary excitations in entangled states such as quantum spin liquids may exhibit exotic statistics different from those obeyed by fundamental bosons and fermions. Non-Abelian anyons exist in a Kitaev spin liquid—the ground state of an exactly solvable model. A smoking-gun signature of these excitations, namely a half-integer quantized thermal Hall conductivity, was recently reported in α-RuCl3. While fascinating, a microscopic theory for this phenomenon remains elusive because the pure Kitaev model cannot display this effect in an intermediate magnetic field. Here we present a microscopic theory of the Kitaev spin liquid emerging between the low- and high-field states. Essential to this result is an antiferromagnetic off-diagonal symmetric interaction which allows the Kitaev spin liquid to protrude from the ferromagnetic Kitaev limit under a magnetic field. This generic model displays a strong field anisotropy, and we predict a wide spin liquid regime when the field is perpendicular to the honeycomb plane.
Abstract Pursuing the exotic quantum spin liquid (QSL) state in the Kitaev material α-RuCl3 has intrigued great research interest recently. A fascinating question is on the possible existence of a field-induced QSL phase in this compound. Here we perform high-field magnetization measurements of α-RuCl3 up to 102 T employing the non-destructive and destructive pulsed magnets. Under the out-of-plane field along the c* axis (i.e., perpendicular to the honeycomb plane), two quantum phase transitions are uncovered at respectively 35 T and about 83 T, between which lies an intermediate phase as the predicted QSL. This is in sharp contrast to the case with in-plane fields, where a single transition is found at around 7 T and the intermediate QSL phase is absent instead. By measuring the magnetization data with fields tilted from the c* axis up to 90° (i.e., in-plane direction), we obtain the field-angle phase diagram that contains the zigzag, paramagnetic, and QSL phases. Based on the K-J-Γ- Γ′{{{\Gamma }}}^{{\prime} }Γ′ Γ ′ model for α-RuCl3 with a large Kitaev term we perform density matrix renormalization group simulations and reproduce the quantum phase diagram in excellent agreement with experiments.
The Kitaev model is an exactly solvable quantum spin model within the language of constrained real fermions. In spite of numerous studies for magnetic fields along special orientations, there is a limited amount of knowledge on the complete field-angle characterization, which can provide valuable information on the existence of fractionalized excitations. For this purpose, we first study the pure ferromagnetic and antiferromagnetic Kitaev models for arbitrary external magnetic field directions via a mean-field theory, showing that there are many topological phases with different (or zero) Chern numbers, depending on the magnetic field strength and orientations. However, a realistic description of the candidate Kitaev materials, within the edge-sharing octahedra paradigm, requires additional coupling terms, including a large off-diagonal term $\mathrm{\ensuremath{\Gamma}}$ along with possible anisotropic corrections ${\mathrm{\ensuremath{\Gamma}}}_{p}$. It is therefore not sufficient to rely on the topological properties of the bare Kitaev model as the basis for the observed thermal Hall-conductivity signals, and an understanding of these extended Kitaev models with a complete field response is demanded. Starting from the zero-field phase diagram of $\mathrm{K}\text{\ensuremath{-}}\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}{\mathrm{\ensuremath{\Gamma}}}_{p}$ models, we identify, besides the Kitaev spin liquid phase, antiferromagnetic zigzag, ferromagnetic phases, as well as an unusual Kitaev(-$\mathrm{\ensuremath{\Gamma}}$) spin liquid phase. The magnetic field response of these phases for arbitrary field orientations provides a remarkably rich phase diagram. For an extended parameter range and just above the critical field where the zigzag phase is suppressed, there is an intermediate phase region with suppressed energy gaps and substantial spin fractionalization. To comply our findings with experiments, we also reproduce a large asymmetry in the extent of this intermediate phases specifically for the two different field directions $\ensuremath{\theta}=\ifmmode\pm\else\textpm\fi{}{60}^{o}$ with respect to the normal to the plane of the honeycomb lattice.