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

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 () and Jonghwan Kim ()
Additional contact information
Minjeong Kim: Pohang University of Science and Technology
Taeho Kim: Pohang University of Science and Technology
Anna Galler: Graz University of Technology
Dasol Kim: Pohang University of Science and Technology
Alexis Chacon: Pohang University of Science and Technology
Xiangxin Gong: Nanyang Technological University
Yuhui Yang: Nanyang Technological University
Rouli Fang: Nanyang Technological University
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
B. J. Kim: Pohang University of Science and Technology
Sang Hoon Chae: Nanyang Technological University
Moon-Ho Jo: Pohang University of Science and Technology
Angel Rubio: Max Planck Institute for the Structure and Dynamics of Matter
Ofer Neufeld: Faculty of Chemistry
Jonghwan Kim: Pohang University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-65725-9

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