Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2
Abstract
Optical selection rules fundamentally determine the optical transitions between energy states in a variety of physical systems, from hydrogen atoms to bulk crystals such as gallium arsenide. These rules are important for optoelectronic applications such as lasers, energy-dispersive X-ray spectroscopy, and quantum computation. Recently, single-layer transition metal dichalcogenides have been found to exhibit valleys in momentum space with nontrivial Berry curvature and excitons with large binding energy. However, there has been little study of how the unique valley degree of freedom combined with the strong excitonic effect influences the nonlinear optical excitation. Here in this paper, we report the discovery of nonlinear optical selection rules in monolayer WS2, an important candidate for visible 2D optoelectronics because of its high quantum yield and large direct bandgap. We experimentally demonstrated this principle for second-harmonic generation and two-photon luminescence (TPL). Moreover, the circularly polarized TPL and the study of its dynamics evince a sub-ps interexciton relaxation (2p → 1s). The discovery of this new optical selection rule in a valleytronic 2D system not only considerably enhances knowledge in this area but also establishes a foundation for the control of optical transitions that will be crucial for valley optoelectronic device applications such as 2Dmore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States). NSF Nanoscale Science and Engineering Center (NSEC)
- Univ. of California, Berkeley, CA (United States). NSF Nanoscale Science and Engineering Center (NSEC); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Material Sciences Division
- Univ. of California, Berkeley, CA (United States). NSF Nanoscale Science and Engineering Center (NSEC); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Material Sciences Division; King Abdulaziz Univ., Jeddah (Saudi Arabia). Dept. of Physics
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1415947
- Grant/Contract Number:
- AC02-05CH11231; SC0001293
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Light, Science & Applications
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 12; Journal ID: ISSN 2047-7538
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Nonlinear optics; Optical materials and structures; Nonlinear optical selection rule; 2D materials; 2p–1s exciton relaxation; Valley exciton
Citation Formats
Xiao, Jun, Ye, Ziliang, Wang, Ying, Zhu, Hanyu, Wang, Yuan, and Zhang, Xiang. Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2. United States: N. p., 2015.
Web. doi:10.1038/lsa.2015.139.
Xiao, Jun, Ye, Ziliang, Wang, Ying, Zhu, Hanyu, Wang, Yuan, & Zhang, Xiang. Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2. United States. https://doi.org/10.1038/lsa.2015.139
Xiao, Jun, Ye, Ziliang, Wang, Ying, Zhu, Hanyu, Wang, Yuan, and Zhang, Xiang. Fri .
"Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2". United States. https://doi.org/10.1038/lsa.2015.139. https://www.osti.gov/servlets/purl/1415947.
@article{osti_1415947,
title = {Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2},
author = {Xiao, Jun and Ye, Ziliang and Wang, Ying and Zhu, Hanyu and Wang, Yuan and Zhang, Xiang},
abstractNote = {Optical selection rules fundamentally determine the optical transitions between energy states in a variety of physical systems, from hydrogen atoms to bulk crystals such as gallium arsenide. These rules are important for optoelectronic applications such as lasers, energy-dispersive X-ray spectroscopy, and quantum computation. Recently, single-layer transition metal dichalcogenides have been found to exhibit valleys in momentum space with nontrivial Berry curvature and excitons with large binding energy. However, there has been little study of how the unique valley degree of freedom combined with the strong excitonic effect influences the nonlinear optical excitation. Here in this paper, we report the discovery of nonlinear optical selection rules in monolayer WS2, an important candidate for visible 2D optoelectronics because of its high quantum yield and large direct bandgap. We experimentally demonstrated this principle for second-harmonic generation and two-photon luminescence (TPL). Moreover, the circularly polarized TPL and the study of its dynamics evince a sub-ps interexciton relaxation (2p → 1s). The discovery of this new optical selection rule in a valleytronic 2D system not only considerably enhances knowledge in this area but also establishes a foundation for the control of optical transitions that will be crucial for valley optoelectronic device applications such as 2D valley-polarized THz sources with 2p-1s transitions, optical switches, and coherent control for quantum computing.},
doi = {10.1038/lsa.2015.139},
journal = {Light, Science & Applications},
number = 12,
volume = 4,
place = {United States},
year = {2015},
month = {12}
}
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