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<p>Two-dimensional hexagonal materials such as transition metal dichalcogenides exhibit valley degrees of freedom, offering fascinating potential for valley-based quantum computing and optoelectronics. In nonlinear optics, the K and K’ valleys provide excitation resonances that can be used for ultrafast control of excitons, Bloch oscillations, and Floquet physics. Under intense laser fields, however, the role of coherent carrier dynamics away from the K/K’ valleys is largely unexplored. In this study, we observe quantum interferences in high harmonic generation from monolayer WS<sub>2</sub> as laser fields drive electrons from the valleys across the full Brillouin zone. In the perturbative regime, interband resonances at the valleys enhance high harmonic generation through multi-photon excitations. In the strong-field regime, the high harmonic generation is sensitively controlled by quantum interferences of laser-field-driven electrons occupying various points in the Brillouin zone, including regions far from the K/K’ valleys. Our experimental observations are in strong agreement with quantum simulations, validating their interpretation. This work proposes new routes for harnessing laser-driven quantum interference in two-dimensional hexagonal systems and all-optical techniques to occupy and read-out electronic structures in the full Brillouin zone via strong-field nonlinear optics, advancing quantum technologies.</p>

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Quantum interference and occupation control in high harmonic generation from monolayer WS2

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月6日

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  • Minjeong Kim,
  • Taeho Kim,
  • Anna Galler,
  • Dasol Kim,
  • Alexis Chacon,
  • Xiangxin Gong,
  • Yuhui Yang,
  • Rouli Fang,
  • Kenji Watanabe,
  • Takashi Taniguchi,
  • B. J. Kim,
  • Sang Hoon Chae,
  • Moon-Ho Jo,
  • Angel Rubio,
  • Ofer Neufeld,
  • Jonghwan Kim

摘要

Two-dimensional hexagonal materials such as transition metal dichalcogenides exhibit valley degrees of freedom, offering fascinating potential for valley-based quantum computing and optoelectronics. In nonlinear optics, the K and K’ valleys provide excitation resonances that can be used for ultrafast control of excitons, Bloch oscillations, and Floquet physics. Under intense laser fields, however, the role of coherent carrier dynamics away from the K/K’ valleys is largely unexplored. In this study, we observe quantum interferences in high harmonic generation from monolayer WS2 as laser fields drive electrons from the valleys across the full Brillouin zone. In the perturbative regime, interband resonances at the valleys enhance high harmonic generation through multi-photon excitations. In the strong-field regime, the high harmonic generation is sensitively controlled by quantum interferences of laser-field-driven electrons occupying various points in the Brillouin zone, including regions far from the K/K’ valleys. Our experimental observations are in strong agreement with quantum simulations, validating their interpretation. This work proposes new routes for harnessing laser-driven quantum interference in two-dimensional hexagonal systems and all-optical techniques to occupy and read-out electronic structures in the full Brillouin zone via strong-field nonlinear optics, advancing quantum technologies.