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arXiv:2512.20209

Unveiling the Phase Diagram and Nonlinear Optical Responses of a Twisted Kitaev Chain

Ya‐Min Quan, Shi-Qing Jia, Xiang‐Long Yu, Hai-Qing Lin, Liang-Jian Zou

Published Dec 23, 2025• 0 citations
arXivHTMLPDF

Abstract

Detecting Kitaev interactions in real materials remains challenge, as conventional experimental techniques often have difficulty distinguishing fractionalized excitations from other normal contributions. Terahertz two-dimensional coherent spectroscopy (2DCS) offers a novel approach for probing many-body phenomena, such as exotic excitations in quantum magnets. Motivated by recent experiments on CoNb$_2$O$_6$ and the development of the terahertz spectroscopy in Kitaev quantum spin liquid, we proposed a twisted Kitaev model for CoNb$_2$O$_6$ and determined the precise twist angle according to experimental specific-heat phase diagram. With this calibrated model, we found that non-rephasing diagonal and rephasing anti-diagonal signals appear in the 2DCS nonlinear response. The $x$ and $y$ components of the spin superexchange interactions split the rephasing signals into a grid of discrete peaks. We further demonstrate that the diagonal and the discrete rephasing signals primarily originate from two-spinon and four-spinon excitation processes based on numerical projection method. These findings indicate that even weak Kitaev interactions in quantum materials can be effectively detected via two-dimensional coherent spectroscopy .

DOI
10.48550/arxiv.2512.20209

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Detecting Kitaev interactions in real materials remains challenge, as conventional experimental techniques often have difficulty distinguishing fractionalized excitations from other normal contributions. Terahertz two-dimensional coherent spectroscopy (2DCS) offers a novel approach for probing many-body phenomena, such as exotic excitations in quantum magnets. Motivated by recent experiments on CoNb2_22​O6_66​ and the development of the terahertz spectroscopy in Kitaev quantum spin liquid, we proposed a twisted Kitaev model for CoNb2_22​O6_66​ and determined the precise twist angle according to experimental specific-heat phase diagram. With this calibrated model, we found that non-rephasing diagonal and rephasing anti-diagonal signals appear in the 2DCS nonlinear response. The xxx and yyy components of the spin superexchange interactions split the rephasing signals into a grid of discrete peaks. We further demonstrate that the diagonal and the discrete rephasing signals primarily originate from two-spinon and four-spinon excitation processes based on numerical projection method. These findings indicate that even weak Kitaev interactions in quantum materials can be effectively detected via two-dimensional coherent spectroscopy .
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The identification of microscopic models describing the low-energy properties of correlated materials has been a central goal of spectroscopic measurements. We demonstrate how 2D non-linear spectroscopy can be used to distinguish effective spin models whose linear responses show similar behavior. Motivated by recent experiments on the quasi-1D Ising magnet CoNb2_22​O6_66​, we focus on two proposed models, the ferromagnetic twisted Kitaev chain with bond dependent interactions and the transverse field Ising model. The dynamical spin structure factor probed in linear response displays similar broad spectra for both models from their fermionic domain wall excitations. In sharp contrast, the 2D non-linear spectra of the two models show clear qualitative differences: those of the twisted Kitaev model contain off-diagonal peaks originating from the bond dependent interactions and transitions between different fermion bands absent in the transverse field Ising model. We discuss the different signatures of spin fractionalization in integrable and non-integrable regimes of the models and their connection to experiments.
Inelastic neutron scattering (INS) has traditionally been one of the primary methods for investigating quantum magnets, particularly in identifying a continuum of excitations as a hallmark of spin fractionalization in quantum spin liquids (QSLs). However, INS faces severe limitations due to its inability to distinguish between such QSL signatures and similar excitation continua arising from highly frustrated magnetic orders with large unit cells or classical spin liquids. In contrast, two-dimensional coherent spectroscopy (2DCS) has emerged as a powerful tool to probe nonlinear excitation dynamics, offering insights into the underlying mechanisms behind these broad spectral features. In this paper, we utilize classical molecular dynamics (MD) techniques to explore the 2DCS responses of frustrated magnets with dominant Kitaev interactions. Comparing the classical and quantum versions of the pure Kitaev model our results indicate both clear similarities, in the form of sharp line features, and clear distinctions, in the locations of these features and in selection rules. Moreover, in the extended KΓΓ′KΓΓ'KΓΓ′ model, we show that the 2DCS response of the Kitaev spin liquid is completely distinct from that of large unit cell magnetic orders, despite both generating a broad continuum in INS. Additionally, we demonstrate the extreme sensitivity of classical 2DCS to thermal fluctuations and discuss the potential significance of quantum coherence in experimental settings. Overall, our work illustrates the potential of 2DCS in resolving the complex physics underlying ambiguous spin excitation continua, thereby enhancing our understanding of the dynamics in these frustrated systems.