skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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 » valley-polarized THz sources with 2p-1s transitions, optical switches, and coherent control for quantum computing.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3]
  1. Univ. of California, Berkeley, CA (United States). NSF Nanoscale Science and Engineering Center (NSEC)
  2. 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
  3. 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) (SC-22)
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. doi: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. doi: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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 22 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Giant Enhancement of the Optical Second-Harmonic Emission of WSe 2 Monolayers by Laser Excitation at Exciton Resonances
journal, March 2015


Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014


Valley polarization and intervalley scattering in monolayer MoS 2
journal, November 2012

  • Kioseoglou, G.; Hanbicki, A. T.; Currie, M.
  • Applied Physics Letters, Vol. 101, Issue 22
  • DOI: 10.1063/1.4768299

Dielectric Screening of Excitons and Trions in Single-Layer MoS 2
journal, September 2014

  • Lin, Yuxuan; Ling, Xi; Yu, Lili
  • Nano Letters, Vol. 14, Issue 10
  • DOI: 10.1021/nl501988y

Quantum Coherent Control for Nonlinear Spectroscopy and Microscopy
journal, May 2009


Exciton-exciton annihilation in MoSe 2 monolayers
journal, March 2014


Polarization selection rules in exciton-based terahertz lasers
journal, August 2013


Two-Dimensional Analog to the Hydrogen Atom
journal, December 1967

  • Zaslow, B.; Zandler, Melvin E.
  • American Journal of Physics, Vol. 35, Issue 12
  • DOI: 10.1119/1.1973790

Electromagnetically induced transparency: Optics in coherent media
journal, July 2005

  • Fleischhauer, Michael; Imamoglu, Atac; Marangos, Jonathan P.
  • Reviews of Modern Physics, Vol. 77, Issue 2
  • DOI: 10.1103/RevModPhys.77.633

Optoelectronic devices based on electrically tunable p–n diodes in a monolayer dichalcogenide
journal, March 2014

  • Baugher, Britton W. H.; Churchill, Hugh O. H.; Yang, Yafang
  • Nature Nanotechnology, Vol. 9, Issue 4
  • DOI: 10.1038/nnano.2014.25

Exciton Binding Energy of Monolayer WS2
journal, March 2015

  • Zhu, Bairen; Chen, Xi; Cui, Xiaodong
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep09218

Optical Orientation and Femtosecond Relaxation of Spin-Polarized Holes in GaAs
journal, September 2002


Electrical control of second-harmonic generation in a WSe2 monolayer transistor
journal, April 2015

  • Seyler, Kyle L.; Schaibley, John R.; Gong, Pu
  • Nature Nanotechnology, Vol. 10, Issue 5
  • DOI: 10.1038/nnano.2015.73

Polarized light boosts valleytronics
journal, July 2012


Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014

  • Hong, Xiaoping; Kim, Jonghwan; Shi, Su-Fei
  • Nature Nanotechnology, Vol. 9, Issue 9
  • DOI: 10.1038/nnano.2014.167

Valley-dependent optoelectronics from inversion symmetry breaking
journal, June 2008


Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States
journal, November 2013


Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

  • Ye, Ziliang; Cao, Ting; O’Brien, Kevin
  • Nature, Vol. 513, Issue 7517
  • DOI: 10.1038/nature13734

Conservation laws in nonlinear optics*
journal, January 1980


Spin flip of excitons in GaAs quantum wells
journal, May 1997


The valley Hall effect in MoS2 transistors
journal, June 2014


Monolayer excitonic laser
journal, October 2015


Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

  • Cao, Ting; Wang, Gang; Han, Wenpeng
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1882

Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides
journal, January 2015

  • Liu, Gui-Bin; Xiao, Di; Yao, Yugui
  • Chemical Society Reviews, Vol. 44, Issue 9
  • DOI: 10.1039/C4CS00301B

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2
journal, August 2014


Second-Harmonic Light Generation in Crystals with Natural Optical Activity
journal, July 1968


Optical pumping of a single hole spin in a quantum dot
journal, January 2008

  • Gerardot, Brian D.; Brunner, Daniel; Dalgarno, Paul A.
  • Nature, Vol. 451, Issue 7177
  • DOI: 10.1038/nature06472

Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012


Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012

  • Zeng, Hualing; Dai, Junfeng; Yao, Wang
  • Nature Nanotechnology, Vol. 7, Issue 8
  • DOI: 10.1038/nnano.2012.95

Exciton Dynamics in Suspended Monolayer and Few-Layer MoS 2 2D Crystals
journal, January 2013

  • Shi, Hongyan; Yan, Rusen; Bertolazzi, Simone
  • ACS Nano, Vol. 7, Issue 2
  • DOI: 10.1021/nn303973r

    Works referencing / citing this record:

    Nonlinear optics of two‐dimensional transition metal dichalcogenides
    journal, July 2019


    Tight-binding modeling of excitonic response in van der Waals stacked 2D semiconductors
    journal, January 2019

    • Yip, Cho Tung; Lo, Tsz Wing; Zhu, Si-Cong
    • Nanoscale Horizons, Vol. 4, Issue 4
    • DOI: 10.1039/c9nh00042a

    Nonlinear optical selection rules of excitons in monolayer transition metal dichalcogenides
    journal, June 2019


    Nonlinear optics of two‐dimensional transition metal dichalcogenides
    journal, July 2019


    Tight-binding modeling of excitonic response in van der Waals stacked 2D semiconductors
    journal, January 2019

    • Yip, Cho Tung; Lo, Tsz Wing; Zhu, Si-Cong
    • Nanoscale Horizons, Vol. 4, Issue 4
    • DOI: 10.1039/c9nh00042a

    Temperature-driven evolution of critical points, interlayer coupling, and layer polarization in bilayer Mo S 2
    journal, April 2018


    Nonlinear optical selection rules of excitons in monolayer transition metal dichalcogenides
    journal, June 2019