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Journal of Physics Condensed Matter

Response functions for electric field induced two-dimensional nonlinear spectroscopy in a Kitaev magnet

Wolfram Brenig, Olesia Krupnitska

Published Sep 13, 2024• 6 citations
Publisher

Abstract

We study the dynamical response functions relevant for electric field induced two-dimensional (2D) coherent nonlinear optical spectroscopy in a Kitaev magnet at finite temperature. We show that these response functions are 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 2D 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 a multi-particle continuum. While the 2D spectrum of the response is set by 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 2D nonlinear response as the temperature is increased beyond the flux proliferation crossover.

DOI
10.1088/1361-648x/ad7ac6

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We study the dynamical response functions relevant for electric field induced two-dimensional (2D) coherent nonlinear optical spectroscopy in a Kitaev magnet at finite temperature. We show that these response functions are 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 2D 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 a multi-particle continuum. While the 2D spectrum of the response is set by 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 2D nonlinear response as the temperature is increased beyond the flux proliferation crossover.
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.
We study electric-field-induced second harmonic generation (SHG) in the Kitaev model. This frustrated magnet hosts a quantum spin liquid, featuring fractionalization in terms of mobile Majorana fermion and static Z2{\mathbb{Z}}_{2}Z2​ flux-vison elementary excitations. We show that finite-temperature SHG allows to probe characteristic features of both fractional quasiparticle types. In the homogeneous flux state at low temperatures, the SHG susceptibility displays an oscillatory spectrum, which is set by only the fermionic excitations and is subject to temperature-induced Fermi blocking, generic to all higher harmonic generation (HHG). In the intermediate to high-temperature range, intrinsic randomness, which emerges from thermally excited visons leads to drastic changes of the SHG susceptibility, resulting from resonance decoupling over a wide range of energies. At the flux proliferation crossover, we suggest an interpolation between these two temperature regimes. Our results satisfy previously established symmetries for electric-field-induced SHG in Kitaev magnets.
Two-dimensional nonlinear dynamical response of the magnetoelectrically driven dimerized spin-1/21{/}21/2 chain
A study of the dynamical two-dimensional (2D) nonlinear response of the dimerized spin-1/21{/}21/2 chain to external electric fields is presented. The coupling of the spin system to those fields is set to arise from the inverse Dzyaloshinskii-Moriya interaction. In the XY-limit, we provide analytical expressions for the second-order nonlinear dynamical response function. Apart from multi spinon continua, this response displays a strong antidiagonal, i.e. galvanoelectric, feature in the 2D frequency plane. This allows to read off scattering rates of the fractional spinon excitations. For the XXZ-case, we focus on the interaction-driven renormalization of the light-matter coupling by considering vertex corrections which are induced by the zz-exchange. We show this renormalization to modify the spinon joint density of states significantly, potentially allowing for the formation of in-gap bound states. As a result, the vertex corrected light-matter coupling can induce a dramatic spectral weight transfer to lower energies for the dynamical response function within the 2D frequency plane.
A study of the dynamical two-dimensional (2D) nonlinear response of the dimerized spin-1/2 chain to external electric fields is presented. The coupling of the spin system to light is set to arise from the inverse Dzyaloshinskii-Moriya interaction. In the XY-limit, we provide analytical expressions for the second-order nonlinear dynamical response function. Apart from multi spinon continua, this response displays a strong antidiagonal, i.e. galvanoelectric, feature in the 2D frequency plane. This allows to read off scattering rates of the fractional spinon excitations. For the XXZ-case, we focus on the interaction-driven renormalization of the light-matter coupling by considering vertex corrections which are induced by the zz-exchange. We show this renormalization to modify the spinon joint density of states significantly, potentially allowing for the formation of in-gap bound states. As a result, the vertex corrected light-matter coupling can induce a dramatic spectral weight transfer to lower energies for the dynamical response function within the 2D frequency plane.
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.
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.