
1.NSF Nanoscale Science and Engineering Center (NSEC), University of California at Berkeley, Berkeley, CA, USA
2.Material Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA
3.Department of Physics, King Abdulaziz University, Jeddah, Saudi Arabia
X Zhang, Email: xiang@berkeley.edu
Published:2015-12,
Published Online:06 September 2015,
Received:14 August 2015,
Revised:03 September 2015,
Accepted:05 September 2015
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Xiao, J. et al. Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2. Light: Science & Applications, 4, e366 (2015).
Xiao, J. et al. Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2. Light: Science & Applications, 4, e366 (2015). DOI: 10.1038/lsa.2015.139.
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
we report the discovery of nonlinear optical selection rules in monolayer WS
2
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 (2
p
→ 1
s
). 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 2
p
–1
s
transitions
optical switches
and coherent control for quantum computing.
nonlinear optical selection rule2D materials2p–1s exciton relaxationvalley exciton
Hilton DJ, Tang CL. Optical orientation and femtosecond relaxation of spin-polarized hole in GaAs.Phys Rev Lett2002;89: 146601..
Gerardot BD, Brunner D, Dalgarno PA, Öhberg P, Seidl Set al. Optical pumping of a single hole spin in a quantum dot.Nature2008;451: 441–444..
Chuang SL. Physics of Photonic Devices. Hoboken, NJ: Wiley; 2009.
Yao W, Xiao D, Niu Q. Valley-dependent optoelectronics from inversion symmetry breaking.Phys Rev B2008;77: 235406..
Mak KF, He K, Shan J, Heinz TF. Control of valley polarization in monolayer MoS2by optical helicity.Nat Nanotechnol2012;7: 494–498..
Cao T, Wang G, Han WP, Ye HQ, Zhu CRet al. Valley-selective circular dichroism of monolayer molybdenum disulphide.Nat Commun2012;3: 887..
Zeng HL, Dai JF, Yao W, Xiao D, Cui XD. Valley polarization in MoS2monolayers by optical pumping.Nat Nanotechnol2012;7: 490–493..
Liu GB, Xiao D, Yao YG, Xu XD, Yao W. Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides.Chem Soc Rev2015;44: 2643–2663..
Ye ZL, Cao T, O'Brien K, Zhu HY, Yin XBet al. Probing excitonic dark states in single-layer tungsten disulphide.Nature2014;513: 214–218..
Baugher BWH, Churchill HOH, Yang YF, Jarillo-Herrero P. Optoelectronic devices based on electrically tunable p-n diodes in a monolayer dichalcogenide.Nat Nanotechnol2014;9: 262–267..
Mak KF, McGill KL, Park J, McEuen PL. The valley Hall effect in MoS2transistors.Science2014;344: 1489–1492..
He KL, Kumar N, Zhang L, Wang ZF, Mak KFet al. Tight bound excitons in monolayer WSe2.Phys Rev Lett2014;113: 026803..
Chernikov A, Berkelbach TC, Hill HM, Rigosi A, Li Yet al. Exciton binding energy and nonhydrogenic Rydberg series in monolayer WS2.Phys Rev Lett2014;113: 076802..
Zhu BR, Chen X, Cui XD. Exciton binding energy of monolayer WS2.Sci Rep2015;5: 9218..
Lin YX, Ling X, Yu LL, Huang SX, Hsu ALet al. Dielectric screening of excitons and trions in single-layer MoS2.Nano Lett2014;14: 5569–5576..
Ye Y, Wong ZJ, Lu XF, Zhu HY, Chen XHet al. Monolayer excitonic laser. 2015; arXiv: 1503.06141.
Wang G, Marie X, Gerber I, Amand T, Lagarde Det al. Giant enhancement of the optical second-harmonic emission of WSe2monolayers by laser excitation at exciton resonances.Phys Rev Lett2015;114: 097403..
Seyler KL, Schaibley JR, Gong P, Rivera P, Jones AMet al. Electrical control of second-harmonic generation in a WSe2monolayer transistor.Nat Nanotechnol2015;10: 407–411..
Behnia K. Condensed-matter physics: polarized light boosts valleytronics.Nat Nanotechnol2012;7: 488–489..
Zaslow B, Zandler ME. Two-dimensional analog to the hydrogen atom.Am J Phys1967;35: 1118–1119..
Qiu DY, da Jornada FH, Louie SG. Optical spectrum of MoS2: many-body effects and diversity of exciton states.Phys Rev Lett2013;111: 216805..
Simon HJ, Bloembergen N. Second-harmonic light generation in crystals with natural optical activity.Phys Rev1968;171: 1104–1114..
Bloembergen N. Conservation laws in nonlinear optics.J Opt Soc Am1980;70: 1429–1436..
Boyd RW. Nonlinear Optics. Burlington, MA: Academic Press; 2008.
Kioseoglou G, Hanbicki AT, Currie M, Friedman AL, Gunlycke Det al. Valley polarization and intervalley scattering in monolayer MoS2.Appl Phys Lett2012;101: 221907..
Snoke DW, Rühle WW, Köhler K, Ploog K. Spin flip of excitons in GaAs quantum wells.Phys Rev B1997;55: 13789–13794..
Lakowicz JR. Topics in Fluorescence Spectroscopy Ch. 3. New York: Kluwer Academic Publishers; 2002.
Hong XP, Kim J, Shi SF, Zhang Y, Jin CHet al. Ultrafast charge transfer in atomically thin MoS2/WS2heterostructures.Nat Nanotechnol2014;9: 682–686..
Shi HY, Yan RS, Bertolazzi S, Brivio J, Gao Bet al. Exciton dynamics in suspended monolayer and few-layer MoS22D crystals.ACS Nano2013;7: 1072–1080..
Kumar N, Cui QN, Ceballos F, He DW, Wang YSet al. Exciton-exciton annihilation in MoSe2monolayers.Phys Rev B2014;89: 125427..
Yu T, Wu MW. Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer MoS2.Phys Rev B2014;89: 205303..
Slavcheva G, Kavokin AV. Polarization selection rules in exciton-based terahertz lasers.Phys Rev B2013;88: 085321..
Fleischhauer M, Imamoglu A, Marangos JP. Electromagnetically induced transparency: optics in coherent media.Rev Mod Phys2005;77: 633..
Silberberg Y. Quantum coherent control for nonlinear spectroscopy and microscopy.Annu Rev Phys Chem2009;60: 277–292..
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