Transient Nonlinear Optics of Two-Dimensional Materials

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School of Electrical Engineering | Doctoral thesis (article-based) | Defence date: 2022-03-04
Degree programme
80 + app. 114
Aalto University publication series DOCTORAL THESES, 31/2022
Two-dimensional (2D) layered materials with remarkable optical and electronic properties, are promising for a variety of applications in the area of electronics, photonics, and optoelectronics. Recently, increasing efforts are targeted toward the nonlinear optical properties of 2D materials, which are not only fascinating in terms of fundamental physics, but also intriguing for various potential applications. Beneficial from their atomically thin nature, 2D materials are the ideal material to address the subjects on how the materials respond to the light excitation without considering phase-matching effects. In this thesis, I devote main efforts to studying the relation between carrier dynamics and nonlinear optical responses in 2D materials and to developing potential applications in the area of ultrafast nonlinear optics. Details are expressed as below: 1. Transient linear optical absorption of monolayer MoS2 is studied in the sub-bandgap region from 860 nm to 1400 nm. A significant absorption enhancement of up to 4.2% is observed due to the pump-induced absorption at the excited carrier states. 2. Transient second-harmonic generations in transition metal dichalcogenide monolayers are investigated in a broadband energy range. The pump modified excitonic oscillation strength enables to enhance the SHG at dark exciton states and bleach the SHG at bright exciton states. The enhancement of SHG is achieved as high as 386 times. Further, the SHG modulation has been realized with a modulation depth of up to 60% and a response time of ~600 fs. 3. Transient higher-order harmonic generations are finally studied. Broadband third-harmonic spectroscopy displays a series of electronic states in monolayer MoS2 with high signal contrast up to 800 times. The ultrafast photocarrier dynamics of electronic states in MoS2 are explored by transient third-harmonic generation. Further, the all-optical modulation of high-harmonic generation in monolayer MoS2 is demonstrated with a modulation depth up to 90%, offering a promising platform for the ultrafast optical signal processing of nonlinear optics.
Supervising professor
Sun, Zhipei, Prof., Aalto University, Department of Electronics and Nanoengineering, Finland
Nonlinear Optics, Two-Dimensional Materials, Pump-Probe Spectroscopy, Excitonic States, Harmonic Generations, Ultrafast All-Optical Modulation
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  • [Publication 1]: Yadong Wang, Masood Ghotbi, Susobhan Das, Yunyun Dai, Shisheng Li, Xuerong Hu, Xuetao Gan, Jianlin Zhao, and Zhipei Sun, Difference frequency generation in monolayer MoS2. Nanoscale, 12 (38), 19638 (2020).
    Full text in Acris/Aaltodoc:
    DOI: 10.1039/d0nr01994a View at publisher
  • [Publication 2]: Yadong Wang, Biqiang Jiang, Susobhan Das, Qiang Zhao, Xuetao Gan, and Jianlin Zhao, All-optically controlled slow and fast lights in graphene-coated tilted fiber Bragg grating. Applied Physics Express, 12 (7), 072010 (2019).
    Full text in Acris/Aaltodoc:
    DOI: 10.7567/1882-0786/ab281b View at publisher
  • [Publication 3]: Yadong Wang, Susobhan Das, Fadil Iyikanat, Yunyun Dai, Shisheng Li, Xiangdong Guo, Xiaoxia Yang, Jinluo Cheng, Xuerong Hu, Masood Ghotbi, Fangwei Ye, Harri Lipsanen, Shiwei Wu, Tawfique Hasan, Xuetao Gan, Kaihui Liu, Dong Sun, Qing Dai, F. Javier García de Abajo, Jianlin Zhao and Zhipei Sun, Giant all-optical modulation of second-harmonic generation mediated by dark excitons. ACS Photonics, 8 (8), 2320 (2021).
    Full text in Acris/Aaltodoc:
    DOI: 10.1021/acsphotonics.1c00466 View at publisher
  • [Publication 4]: Yadong Wang, Fadil Iyikanat, Habib Rostami, Xueyin Bai, Xuerong Hu, Susobhan Das, Yunyun Dai, Luojun Du, Yi Zhang, Shisheng Li, Harri Lipsanen, F. Javier García de Abajo, and Zhipei Sun, Probing Electronic States in Monolayer Semiconductors through Static and Transient Third-Harmonic Spectroscopies. Advanced Materials, 2107104 (2021).
    DOI: 10.1002/adma.202107104 View at publisher
  • [Publication 5]: Jakub Bogusławski, Yadong Wang, Hui Xue, Xiaoxia Yang, Dong Mao, Xuetao Gan, Zhaoyu Ren, Jianlin Zhao, Qing Dai, Grzegorz Soboń, Jarosław Sotor, and Zhipei Sun, Graphene actively mode-locked lasers. Advanced Functional Materials, 28 (28), 1801539 (2018).
    Full text in Acris/Aaltodoc:
    DOI: 10.1002/adfm.201801539 View at publisher
  • [Publication 6]: Hui Xue, Yadong Wang, Yunyun Dai, Wonjae Kim, Henri Jussila, Mei Qi, Jannatul Susoma, Zhaoyu Ren, Qing Dai, Jianlin Zhao, Kari Holonen, Harri Lipsanen, Xiaomu Wang, Xuetao Gan, and Zhipei Sun, A MoSe2/WSe2 heterojunction-based photodetector at telecommunication wavelengths. Advanced Functional Materials, 28 (47), 1804388 (2018).
    Full text in Acris/Aaltodoc:
    DOI: 10.1002/adfm.201804388 View at publisher
  • [Publication 7]: Susobhan Das, Yadong Wang, Yunyun Dai, Shisheng Li, and Zhipei Sun, Ultrafast transient sub-bandgap absorption of monolayer MoS2. Light: Science& Applications, 10 (1), 27 (2021).
    Full text in Acris/Aaltodoc:
    DOI: 10.1038/s41377-021-00462-4 View at publisher
  • [Publication 8]: Yunyun Dai, Yadong Wang, Susohban Das, Hui Xue, Xueyin Bai, Eero Hulkko, Guangyu Zhang, Xiaoxia Yang, Qing Dai, and Zhipei Sun, Electrical Control of Interband Resonant Nonlinear Optics in Monolayer MoS2. ACS Nano, 14 (7), 8442 (2020).
    DOI: 10.1021/acsnano.0c02642 View at publisher
  • [Publication 9]: Yunyun Dai, Yadong Wang, Susobhan Das, Shisheng Li, Hui Xue, Ahmadi Mohsen, and Zhipei Sun, Broadband Plasmon-Enhanced Four-Wave Mixing in Monolayer MoS2. Nano Letters, 21 (14), 6321 (2021).
    Full text in Acris/Aaltodoc:
    DOI: 10.1021/acs.nanolett.1c02381 View at publisher
  • [Publication 10]: Anton Autere, Henri Jussila, Yunyun Dai, Yadong Wang, Harri Lipsanen, and Zhipei Sun, Nonlinear optics with 2D layered materials. Advanced Materials 30 (24), 1705963 (2018).
    Full text in Acris/Aaltodoc:
    DOI: 10.1002/adma.201705963 View at publisher
  • [Publication 11]: Diao Li, Hui Xue, Yadong Wang, Mei Qi, Wonjae Kim, Changfeng Li,Juha Riikonen, Zhaoyu Ren, Jintao Bai, Harri Lipsanen, and Zhipei Sun, Active synchronization and modulation of fiber lasers with a graphene electrooptic modulator. Optics Letters 43 (15), 3497 (2018).
    Full text in Acris/Aaltodoc:
    DOI: 10.1364/OL.43.003497 View at publisher
  • [Publication 12]: Diao Li, Hui Xue, Mei Qi, Yadong Wang, Sinan Aksimsek, Nikolai Chekurov, Wonjae Kim, Changfeng Li, Juha Riikonen, Fangwei Ye, Qing Dai, Zhaoyu Ren, Jintao Bai, Tawfique Hasan, Harri Lipsanen, and Zhipei Sun, Graphene actively Q-switched lasers. 2D Materials 4 (2), 025095 (2017).
    DOI: 10.1088/2053-1583/aa6e6b View at publisher