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Theory of Nonlinear Spectroscopy of Quantum Magnets

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arxiv 2502.17554 v1 pith:YKX7A24Z submitted 2025-02-24 cond-mat.str-el

Anubhav Srivastava , Stefan Birnkammer , GiBaik Sim , Michael Knap , Johannes Knolle This is my paper · ORCID
classification cond-mat.str-el
keywords quantummagnetsspincontributionscouplingsexcitationsexoticfield
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abstract

Two-dimensional coherent spectroscopy (2DCS) is an established method for characterizing molecules and has been proposed in the THz regime as a new tool for probing exotic excitations of quantum magnets; however, the precise nature of the coupling between pump field and spin degrees of freedom has remained unclear. Here, we develop a general response theory of 2DCS and show how magneto-electric as well as polarization couplings contribute to 2DCS in addition to the typically assumed magnetization. We propose experimental protocols to distill individual contributions, for instance from exchange-striction or spin current mechanism, when the electric field couples to terms quadratic in spin operators. We provide example calculations for the paradigmatic twisted Kitaev chain material $\mathrm{CoNb}_{2}\mathrm{O}_{6}$ and highlight the crucial role of contributions from cross-coupling between polarization and magnetic nonlinear susceptibilities. Our work paves the way for systematic studies of light-matter couplings in quantum magnets and for establishing 2DCS as a versatile tool for probing fractional excitations of exotic magnetic quantum phases.

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Cited by 2 Pith papers

Reviewed papers in the Pith corpus that reference this work. Sorted by Pith novelty score. Full citation record

  1. Two-dimensional nonlinear dynamical response of the magnetoelectrically driven dimerized spin-$1{/}2$ chain

    cond-mat.str-el 2025-07 conditional novelty 6.0 of 10

    The 2D nonlinear response of a magnetoelectrically coupled dimerized spin-1/2 chain shows a galvanoelectric line whose width measures spinon scattering rates, plus RPA vertex corrections that create bound states and t...

  2. Extracting Nonlinear Dynamical Response Functions from Time Evolution

    cond-mat.str-el 2025-07 conditional novelty 6.0 of 10

    Functional derivatives evaluated with frequency-localized test pulses extract full nonlinear response functions from real-time evolution, validated up to third order in optical responses.

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