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arXiv:2305.04920

Shedding Light on Microscopic Details: 2D Spectroscopy of 1D Quantum Ising Magnets

GiBaik Sim, Frank Pollmann, Johannes Knolle

Published May 8, 2023• 0 citations
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Abstract

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 CoNb$_2$O$_6$, 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.

DOI
10.48550/arxiv.2305.04920

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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.
This work explores the effectiveness of two-dimensional coherent spectroscopy for understanding the microscopic properties of quantum magnets. Motivated by experiments on the Ising chain magnet CoNb2{}_{2}2​O6{}_{6}6​, it is shown that the 2D spectra are markedly different for the two proposed microscopic Hamiltonians - the transverse field Ising model and the twisted Kitaev spin chain - even though the linear response is similar. The findings showcase the power of 2D spectroscopy for quantifying microscopic descriptions and understanding the dynamics of fractionalized excitations of quantum magnets.
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 .
Abstract With recent advances in terahertz (THz) sources and detection, two-dimensional coherent spectroscopy (2DCS), which allows one to probe nonlinear responses, now reaches the meV regime relevant for quasiparticle excitations in magnetic materials. This opens a promising route to reveal many-body phenomena that evade linear-response probes. To date, most experimental applications have focused on classical magnets, and a solid demonstration in a quantum magnet has yet to be established. Here we present a theoretical study of 2DCS in CoNb 2 O 6 , a quasi-one-dimensional Ising magnet that is believed to host fractionalized spinons which at low temperatures are confined by weak interchain coupling. Our analysis, which builds on an experimentally constrained effective S = 1/2 Hamiltonian, is found to reveal unambiguous 2DCS signatures of spinon deconfinement above the low-temperature ordered phase. Using a four-spinon approximation, we track these 2DCS signatures by sequentially building a faithful microscopic model for CoNb 2 O 6 , starting from the exactly solvable one-dimensional transverse-field Ising model (1 d TFIM) and successively adding additional interactions. In particular, adding a bond-dependent staggered YZ interaction to the 1 d -TFIM already reproduces many key spectral features of the full material Hamiltonian. Within this TFIM+YZ model, we find a series of bound states, including a four-spinon bound state that is distinct from the familiar two-spinon bound states. We further find that introducing a confinement potential suppresses sharp spinon-echo features, which are thought to reflect an underlying continuum of fractionalized excitations. Our results provide concrete predictions for future THz 2DCS experiments on CoNb 2 O 6 and related quasi-one-dimensional quantum magnets.
We show that the new technique of terahertz 2D coherent spectroscopy is capable of giving qualitatively new information about fractionalized spin systems. For the prototypical example of the transverse field Ising chain, we demonstrate theoretically that, despite the broad continuum of excitations in linear response, the 2D spectrum contains sharp features that are a coherent signature of a "spinon echo," which gives previously inaccessible information such as the lifetime of the two-spinon excited state. The effects of disorder and finite lifetime, which are practically indistinguishable in the linear optical or neutron response, manifest in dramatically different fashion in the 2D spectra. Our results may be directly applicable to model quasi-1D transverse field Ising chain systems such as CoNb_{2}O_{6}, but the concept can be applied to fractionalized spin systems in general.
We study the nonlinear response of nonintegrable one-dimensional (1D) spin models using infinite matrix-product state techniques. As a benchmark and demonstration of the method, we first calculate the two-dimensional (2D) coherent spectroscopy for the exactly soluble ferromagnetic transverse field Ising model where excitations are freely moving domain walls. We then investigate the distinct signatures of confined bound states by introducing a longitudinal field and observe the emergence of strong nonrephasinglike signals. To interpret the observed phenomena, we use a two-kink approximation to perturbatively compute the 2D spectra. We find good agreement in comparison with the exact results of the infinite matrix-product state method in the strongly confined regime. We discuss the relevance of our results for quasi-1D1\mathrm{D}1D Ising spin chain materials, such as CoNb2O6{\mathrm{CoNb}}_{2}{\mathrm{O}}_{6}CoNb2​O6​.
The dynamical structure factor of the transverse field Ising model (TFIM) shows universal power-law divergence at its quantum critical point, signatures of which have been arguably observed in inelastic neutron scattering studies of quantum spin chain materials, for example CoNb 2 O 6 . However, it has recently been suggested that its microscopic description is better captured in terms of a twisted Kitaev spin chain (TKSC) with bond-anisotropic couplings. Here, we present exact results for the dynamical structure factor of the TKSC across its quantum critical point, analyzing both the universal low-frequency response and the non-universal high-energy features. In addition, we explore extensions of the model including broken glide symmetry as well as the case of random, and incommensurate magnetic fields. Notably, in the latter case, the fermionic excitations exhibit a localization-delocalization transition, which is manifest in the dynamical response as a distinct signature at finite frequency. We discuss the relevance of these features for the observation of quantum critical response in experiments.