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  • Letter
  • Open Access

Exciton-magnon splitting in the van der Waals antiferromagnet MnPS3 unveiled by second-harmonic generation

Ziqian Wang1,*,†, Xiao-Xiao Zhang1,*, Yuki Shiomi2, Taka-hisa Arima1,3, Naoto Nagaosa1, Yoshinori Tokura1,4,5, and Naoki Ogawa1

  • 1RIKEN Center for Emergent Matter Science (CEMS), Wako, Saitama 351-0198, Japan
  • 2Department of Basic Science, University of Tokyo, Tokyo 153-8902, Japan
  • 3Department of Advanced Materials Science, University of Tokyo, Kashiwa, Chiba 277-8561, Japan
  • 4Department of Applied Physics, University of Tokyo, Tokyo 113-8656, Japan
  • 5Tokyo College, University of Tokyo, Tokyo 113-8656, Japan

  • *These authors contributed equally to this work.
  • †Corresponding author: ziqian.wang@riken.jp
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Phys. Rev. Research 5, L042032 – Published 30 November, 2023

DOI: https://doi.org/10.1103/PhysRevResearch.5.L042032

Abstract

Exciton-magnon pairwise excitation is promising to realize the direct and efficient photogeneration of magnons, especially in low-dimensional materials with large quasiparticle scattering cross sections. Using resonant second-harmonic generation spectroscopy, we identified exciton-magnon resonance in MnPS3 with possible splitting, in line with the exciton-induced modification of the magnon density of states based on our Koster-Slater-type theory. The substantial exciton-magnon interaction, favored by symmetry, sheds light on coherent cross control among charge, spin, and orbital degrees of freedom via quasiparticle correlations. Additionally, a large linear magnetoelectric effect of excitons is observed.

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Phys. Rev. Research 5, L042032– Published 30 November, 2023
  • Received 17 September 2022
  • Revised 1 September 2023
  • Accepted 5 October 2023
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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