Quantum interference and occupation control in high harmonic generation from monolayer WS2
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.
Authors
- Xiangxin Gong (ORCID: https://orcid.org/0000-0002-5744-6260)
- D.S. Kim (ORCID: https://orcid.org/0000-0002-2250-9380)
- Ofer Neufeld (ORCID: https://orcid.org/0000-0002-5477-2108)
- B. J. Kim (ORCID: https://orcid.org/0000-0002-3584-6853)
- Takashi Taniguchi (ORCID: https://orcid.org/0000-0002-1467-3105)
- Kenji Watanabe (ORCID: https://orcid.org/0000-0003-3701-8119)
- Moon‐Ho Jo (ORCID: https://orcid.org/0000-0002-3160-358X)
- Sang Hoon Chae (ORCID: https://orcid.org/0000-0002-9612-5371)
- Anna Galler (ORCID: https://orcid.org/0000-0002-8596-7784)
- Ángel Rubio (ORCID: https://orcid.org/0000-0003-2060-3151)
- Alexis Chacón (ORCID: https://orcid.org/0000-0002-9279-4463)
- Minjeong Kim (ORCID: https://orcid.org/0000-0001-7676-0370)
- Taeho Kim (ORCID: https://orcid.org/0000-0003-2335-0532)
- Yufan Yang (ORCID: https://orcid.org/0000-0001-7460-8164)
- Jonghwan Kim (ORCID: https://orcid.org/0000-0002-7646-3269)
- Rouli Fang (ORCID: https://orcid.org/0000-0003-3800-0180)
Institutions
- Universidad de Panamá (PA)
- Pohang University of Science and Technology (KR)
- Universidad Autónoma de Chiriquí (PA)
- Nanyang Technological University (SG)
- Technion – Israel Institute of Technology (IL)
- National Institute for Materials Science (JP)
- Graz University of Technology (AT)
- Institute for Basic Science (KR)
- Secretaría Nacional de Ciencia, Tecnología e Innovación (PA)
- Max Planck Institute for the Structure and Dynamics of Matter (DE)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-11-06
- DOI
- https://doi.org/10.1038/s41467-025-65725-9
- Citations
- 3
- Primary Topic
- Strong Light-Matter Interactions
- Type
- article
- Field-Weighted Citation Impact
- 3.74
Funders
- Flatiron Health
- National Research Foundation
- Deutsche Forschungsgemeinschaft
- Ministry of Education, Culture, Sports, Science and Technology
- Austrian Science Fund
- National Research Foundation of Korea
- Ministry of Education, India
- Bộ Giáo dục và Ðào tạo
- Iran Telecommunication Research Center
- Institute for Basic Science
- Ministry of Science and ICT, South Korea
- Japan Society for the Promotion of Science
- Institute for Information and Communications Technology Promotion
- Core Research for Evolutional Science and Technology