期刊
NANO LETTERS
卷 20, 期 11, 页码 8053-8058出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c02972
关键词
two-dimensional materials; nonlinear optics; time-resolved THG; real-time TDDFT simulations
类别
资金
- Beijing Natural Science Foundation [JQ19004]
- Beijing Excellent Talents Training Support [2017000026833ZK11]
- National Natural Science Foundation of China [51991340, 51991342]
- National Key R&D Program of China [2016YFA0300903, 2016YFA0300804]
- Key R&D Program of Guangdong Province [2020B010189001, 2019B010931001, 2018B010109009, 2018B030327001]
- Beijing Municipal Science & Technology Commission [Z191100007219005]
- Beijing Graphene Innovation Program [Z181100004818003]
- Bureau of Industry and Information Technology of Shenzhen (Graphene platform) [201901161512]
- Guangdong Innovative and Entrepreneuri a l Research Team Program [2016ZT06D348]
- Science, Technology and Innovat ion Commission of Shenzhen Municipality [KYTDPT20181011104202253]
The modulation of optical harmonic generation in two-dimensional (2D) materials is of paramount importance in nanophotonic and nano-optoelectronic devices for their applications in optical switching and communication. However, an effective route with ultrafast modulation speed, ultrahigh modulation depth, and broad operation wavelength range is awaiting a full exploration. Here, we report that an optical pump can dynamically modulate the third harmonic generation (THG) of a graphene monolayer with a relative modulation depth above 90% at a time scale of 2.5 ps for a broad frequency ranging from near-infrared to ultraviolet. Our observation, together with the real-time, time-dependent density functional theory (TDDFT) simulations, reveals that this modulation process stems from nonlinear dynamics of the photoexcited carriers in graphene. The superior performance of the nonlinear all-optical modulator based on 2D materials paves the way for its potential applications including nanolasers and optical communication circuits.
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