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arXiv:2602.09709

Raman Spectroscopic Investigation of Kitaev Quantum Spin Liquids

Vivek Kumar, Pradeep Kumar

Published Feb 10, 2026• 0 citations
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2602.09709

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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.
Quantum spin liquids have fascinated condensed matter physicists for decades because of their unusual properties such as spin fractionalization and long-range entanglement. Unlike conventional symmetry breaking, the topological order underlying quantum spin liquids is hard to detect experimentally. Even theoretical models are scarce for which the ground state is established to be a quantum spin liquid. The Kitaev honeycomb model and its generalizations to other tricoordinated lattices are chief counterexamples—they are exactly solvable, harbor a variety of quantum spin liquid phases, and are also relevant for certain transition metal compounds including the polymorphs of (Na,Li) 2 IrO 3 iridates and RuCl 3 . In this review, we give an overview of the rich physics of the Kitaev model, including two-dimensional and three-dimensional fractionalization as well as dynamic correlations and behavior at finite temperatures. We discuss the different materials and argue how the Kitaev model physics can be relevant even though most materials show magnetic ordering at low temperatures.
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.
A Majorana fermion is a fermionic particle that is its own antiparticle. Since the theoretical discovery in 1937, the exotic particle has long been searched in particle physics. In the last few decades, however, it has attracted renewed interest in condensed matter physics, where it can be realized as an elementary excitation (quasiparticle) in quantum states of matter. In this review, we discuss another platform for Majorana fermions, the quantum spin liquid, in which interacting magnetic moments remain disordered down to the lowest temperature under strong quantum fluctuations. They are characterized by topological entanglement and fractional excitations, whose possible application to topological quantum computation is recently discussed intensively. As a prime candidate for such exotic states, we here focus on the Kitaev magnets, a subgroup of the spin-orbit Mott insulators. After a brief overview of the Kitaev model and the fractionalization of spins in the exact ground state, we review recent explosive development in this rapidly growing field, with a focus on numerical solutions of the Kitaev model at finite temperatures and the comparison with experiments. The key concept is thermal fractionalization --- two types of fractional excitations manifest themselves at largely different temperatures. This leads to distinct thermodynamics and spin dynamics in a variety of experimentally measurable quantities. We discuss such peculiar behaviors as the signatures of fractional quasiparticles, in careful comparison with the available experimental data for the candidate materials of the Kitaev magnets. Our review gives an overview of the current status of the identification of Majorana fermions in the Kitaev magnets, which would serve as a basis for further experimental and theoretical studies toward the manipulation of the exotic particles for topological quantum computation.
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.
The formation of quantum spin liquids in frustrated magnets represents an exciting possibility due to the rather exotic features they harbor, including fractionalized excitations and emergent gauge fields. \nUnfortunately, they are notoriously difficult to study as there are often no good analytical methods available and quantum Monte Carlo simulations are hindered by the negative sign problem. \nThe Kitaev honeycomb model is a notable exception of a frustrated quantum model which is exactly solvable and which hosts a number of distinct quantum spin liquid ground states. \nAs such, it allows for a rare opportunity to study the physics of spin liquids with full analytical control. \n \nIn this thesis, we study the fractionalization of spin-1/2 moments into Majorana fermions and an emergent Z2 gauge field in a generalization of the Kitaev honeycomb model to a number of three-dimensional lattices. \nWhile the excitations of the gauge field are always gapped, the fermionic quasiparticles may exhibit a gapless dispersion, forming fully two-dimensional Fermi surfaces, symmetry protected nodal lines, or topological Weyl nodes. \nWe show that one can deduce rather general constraints on the possible gapless excitations by making use of an object called the projective symmetry group. \nIn doing so we provide a scheme for classifying the various gapless Kitaev spin liquids. \nA thorough analysis is carried out for a number of these spin liquids, primarily investigating the stability of the gapless modes and the novel features resulting from their sometimes non-trivial topology, as well as their effects on certain equal-time correlation functions.
Three-dimensional Kitaev models -- generalizations of the well known exactly solvable Kitaev honeycomb model -- exhibit a rich variety of quantum spin liquid phases. Their fractionalized excitations are Majorana fermions that may form topological band structures. These can be enriched by lattice symmetries, as shown in the present work. In particular, the authors propose two new instances of Kitaev spin liquids that exhibit nodal chains and 3D Dirac nodes in the bulk. Such crystalline Kitaev spin liquids are direct generalizations of crystalline topological insulators, albeit in an interacting spin system. A potential material realization in metal-organic frameworks is also discussed.