Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2

Xiao, Jun; Ye, Ziliang; Wang, Ying; Zhu, Hanyu; Wang, Yuan; Zhang, Xiang

doi:10.1038/lsa.2015.139

Title: Nonlinear optical selection rule based on valley-exciton locking in monolayer ws₂

Journal Article · Fri Dec 18 00:00:00 EST 2015 · Light, Science & Applications

DOI:https://doi.org/10.1038/lsa.2015.139· OSTI ID:1415947

Xiao, Jun ^[1]; Ye, Ziliang ^[1]; Wang, Ying ^[1]; Zhu, Hanyu ^[1]; Wang, Yuan ^[2]; Zhang, Xiang ^[3]

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

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0001293

OSTI ID:: 1415947

Journal Information:: Light, Science & Applications, Vol. 4, Issue 12; ISSN 2047-7538

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 88 works

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Title: Nonlinear optical selection rule based on valley-exciton locking in monolayer ws₂