Theory of Nonlinear Spectroscopy of Quantum Magnets

Fuente: arXiv
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Hauptverfasser: Srivastava, Anubhav, Birnkammer, Stefan, Sim, GiBaik, Knap, Michael, Knolle, Johannes
Format: Preprint
Veröffentlicht: 2025
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author Srivastava, Anubhav
Birnkammer, Stefan
Sim, GiBaik
Knap, Michael
Knolle, Johannes
author_facet Srivastava, Anubhav
Birnkammer, Stefan
Sim, GiBaik
Knap, Michael
Knolle, Johannes
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2502_17554
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Theory of Nonlinear Spectroscopy of Quantum Magnets
Srivastava, Anubhav
Birnkammer, Stefan
Sim, GiBaik
Knap, Michael
Knolle, Johannes
Strongly Correlated Electrons
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.
title Theory of Nonlinear Spectroscopy of Quantum Magnets
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2502.17554