期刊
NANO LETTERS
卷 22, 期 21, 页码 8455-8462出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c02711
关键词
All-Optical Control; Static High-Harmonic Generation; Transient High-Harmonic Generation; Interband Carrier Transition; Electronic States; Real-Time Quantitative Theory of Nonlinear Optics
类别
资金
- Aalto Centre for Quantum Engineering, Academy of Finland [314810, 333982, 336144, 336818]
- Academy of Finland Flagship Programme [320167]
- Foundation for Aalto University Science and Technology [630001]
- ERC [834742-ATOP, 789104-eNANO]
- Spanish MCINN [PID2020-112625GB-I00, CEX2019-000910-S]
- Generalitat de Catalunya (CERCA )
- Fundacios Cellex
- Generalitat de Catalunya ( AGAUR)
We demonstrate optically controlled high-harmonic generation (HHG) in monolayer semiconductors by engineering interband polarization. Our experiments reveal efficient control of HHG in the excitonic spectral region with high modulation depths and ultrafast response speeds. Time-domain theory of the nonlinear optical susceptibilities in monolayer semiconductors further supports our findings.
High-harmonic generation (HHG), an extreme nonlinear optical phenomenon beyond the perturbation regime, is of great significance for various potential applications, such as high-energy ultrashort pulse generation with outstanding spatiotemporal coherence. However, efficient active control of HHG is still challenging due to the weak light-matter interaction displayed by currently known materials. Here, we demonstrate optically controlled HHG in monolayer semiconductors via the engineering of interband polarization. We find that HHG can be efficiently controlled in the excitonic spectral region with modulation depths up to 95% and ultrafast response speeds of several picoseconds. Quantitative time-domain theory of the nonlinear optical susceptibilities in monolayer semiconductors further corroborates these experimental observations. Our demonstration not only offers an in-depth understanding of HHG but also provides an effective approach toward active optical devices for strong-field physics and extreme nonlinear optics.
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