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arXiv:2404.16935

Disentangling spin excitation continua in classical and quantum magnets using 2D nonlinear spectroscopy

Emily Z. Zhang, Ciarán Hickey, Yong Baek Kim

Published Apr 25, 2024• 0 citations
arXivHTMLPDF

Abstract

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 $KΓΓ'$ 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.

DOI
10.48550/arxiv.2404.16935

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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.
Two-dimensional coherent spectroscopy ($2D\phantom{\rule{0}{0ex}}C\phantom{\rule{0}{0ex}}S$) has emerged as a powerful tool for probing nonlinear excitation dynamics in quantum magnets, overcoming the limitations of traditional inelastic neutron scattering as a linear probe. The authors use here classical molecular dynamics simulations to compare the $2D\phantom{\rule{0}{0ex}}C\phantom{\rule{0}{0ex}}S$ responses of various models with large Kitaev interactions, revealing distinct features between quantum spin liquids, classical spin liquids, and large unit cell magnetic orders. These findings underscore the potential for $2D\phantom{\rule{0}{0ex}}C\phantom{\rule{0}{0ex}}S$ in disentangling the complex dynamics of frustrated magnetic systems.
Identifying quantum spin liquids, magnon breakdown, or fractionalized excitations in quantum magnets is an ongoing challenge due to the ambiguity in interpreting excitation continua occurring in linear-response probes. Recently, it was proposed that techniques measuring higher-order response, such as two-dimensional coherent spectroscopy (2DCS), could resolve such ambiguities. Numerically simulating nonlinear response functions can, however, be computationally very demanding. We present an efficient Lanczos-based method to compute second-order susceptibilities χ 2 ( ω t , ω τ ) directly in the frequency domain. Applying this to extended Kitaev models describing α − RuCl 3 , we find qualitatively different nonlinear responses between intermediate magnetic field strengths and the high-field regime. To put these results into context, we derive the general 2DCS response of partially polarized magnets within the linear spin-wave approximation, establishing that χ 2 ( ω t , ω τ ) is restricted to a distinct universal form if the excitations are conventional magnons. Deviations from this form, as predicted in our Lanczos-based simulations for α − RuCl 3 , can hence serve in 2DCS experiments as direct criteria to determine whether an observed excitation continuum is of conventional two-magnon type or of different nature.
Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response χyzx(2)(ω1,ω2)χ^{(2)}_{yzx}(ω_1, ω_2)χyzx(2)​(ω1​,ω2​) when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by Z2\mathbb{Z}_2Z2​ flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.
Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response χ_{yzx}^{(2)}(ω_{1},ω_{2}) when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by Z_{2} flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wave functions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our Letter can guide future 2DCS experiments on Kitaev magnets.
We study electric field induced two-dimensional coherent nonlinear optical spectroscopy (2DCS) in a Kitaev magnet at finite temperature. We show that 2DCS is susceptible to both types of fractional quasiparticles of this quantum spin-liquid, i.e., fermions and flux visons. Focusing on the second order response, we find a strong antidiagonal feature in the two-dimensional frequency plane, related to the galvanoelectric effect of the fractional fermions. Perpendicular to the antidiagonal, the width of this feature is set by quasiparticle relaxation rates beyond the bare Kitaev magnet, thereby providing access to single-particle characteristics within the multi-particle 2DCS continuum. While the structure of the 2DCS susceptibility stems from the fermionic quasiparticles and displays Fermi blocking versus temperature, the emergent bond randomness which arises due to thermally populated visons strongly modifies the fermionic spectrum. Therefore also the presence of gauge excitations is manifest in the 2DCS susceptibility as the temperature is increased beyond the flux proliferation crossover. Our results are consistent with and extend previous findings on second harmonic generation in Kitaev magnets.
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.