Exciton valley depolarization in monolayer transition-metal dichalcogenides
Abstract
The valley degree of freedom is a sought-after quantum number in monolayer transition-metal dichalcogenides. Similar to optical spin orientation in semiconductors, the helicity of absorbed photons can be relayed to the valley (pseudospin) quantum number of photoexcited electrons and holes. Also similar to the quantum-mechanical spin, the valley quantum number is not a conserved quantity. Valley depolarization of excitons in monolayer transition-metal dichalcogenides due to long-range electron-hole exchange typically takes a few ps at low temperatures. Exceptions to this behavior are monolayers MoSe2 and MoTe2 wherein the depolarization is much faster. Here, we elucidate the enigmatic anomaly of these materials, finding that it originates from Rashba-induced coupling of the dark and bright exciton branches next to their degeneracy point. When photoexcited excitons scatter during their energy relaxation between states next to the degeneracy region, they reach the light cone after losing the initial helicity. The valley depolarization is not as fast in monolayers WSe2, WS2, and MoS2, wherein the degeneracy is absent resulting in negligible Rashba-induced coupling between bright and dark excitons.
- Authors:
-
[1];
[1];
- Univ. of Rochester, NY (United States)
- Univ. of Toulouse (France)
- Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
- Publication Date:
- Research Org.:
- Univ. of Rochester, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); French National Research Agency (ANR); State of Florida
- OSTI Identifier:
- 1802616
- Alternate Identifier(s):
- OSTI ID: 1606584
- Grant/Contract Number:
- SC0014349; DMR-1503601
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 101; Journal Issue: 11; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Materials Science; Physics
Citation Formats
Yang, Min, Robert, Cedric, Lu, Zhengguang, Van Tuan, Dinh, Smirnov, Dmitry, Marie, Xavier, and Dery, Hanan. Exciton valley depolarization in monolayer transition-metal dichalcogenides. United States: N. p., 2020.
Web. doi:10.1103/physrevb.101.115307.
Yang, Min, Robert, Cedric, Lu, Zhengguang, Van Tuan, Dinh, Smirnov, Dmitry, Marie, Xavier, & Dery, Hanan. Exciton valley depolarization in monolayer transition-metal dichalcogenides. United States. https://doi.org/10.1103/physrevb.101.115307
Yang, Min, Robert, Cedric, Lu, Zhengguang, Van Tuan, Dinh, Smirnov, Dmitry, Marie, Xavier, and Dery, Hanan. Thu .
"Exciton valley depolarization in monolayer transition-metal dichalcogenides". United States. https://doi.org/10.1103/physrevb.101.115307. https://www.osti.gov/servlets/purl/1802616.
@article{osti_1802616,
title = {Exciton valley depolarization in monolayer transition-metal dichalcogenides},
author = {Yang, Min and Robert, Cedric and Lu, Zhengguang and Van Tuan, Dinh and Smirnov, Dmitry and Marie, Xavier and Dery, Hanan},
abstractNote = {The valley degree of freedom is a sought-after quantum number in monolayer transition-metal dichalcogenides. Similar to optical spin orientation in semiconductors, the helicity of absorbed photons can be relayed to the valley (pseudospin) quantum number of photoexcited electrons and holes. Also similar to the quantum-mechanical spin, the valley quantum number is not a conserved quantity. Valley depolarization of excitons in monolayer transition-metal dichalcogenides due to long-range electron-hole exchange typically takes a few ps at low temperatures. Exceptions to this behavior are monolayers MoSe2 and MoTe2 wherein the depolarization is much faster. Here, we elucidate the enigmatic anomaly of these materials, finding that it originates from Rashba-induced coupling of the dark and bright exciton branches next to their degeneracy point. When photoexcited excitons scatter during their energy relaxation between states next to the degeneracy region, they reach the light cone after losing the initial helicity. The valley depolarization is not as fast in monolayers WSe2, WS2, and MoS2, wherein the degeneracy is absent resulting in negligible Rashba-induced coupling between bright and dark excitons.},
doi = {10.1103/physrevb.101.115307},
journal = {Physical Review. B},
number = 11,
volume = 101,
place = {United States},
year = {Thu Mar 26 00:00:00 EDT 2020},
month = {Thu Mar 26 00:00:00 EDT 2020}
}
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Works referenced in this record:
Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons
journal, June 2017
- Zhou, You; Scuri, Giovanni; Wild, Dominik S.
- Nature Nanotechnology, Vol. 12, Issue 9
Exciton fine structure and spin decoherence in monolayers of transition metal dichalcogenides
journal, May 2014
- Glazov, M. M.; Amand, T.; Marie, X.
- Physical Review B, Vol. 89, Issue 20
Dark excitons and the elusive valley polarization in transition metal dichalcogenides
journal, February 2017
- Baranowski, M.; Surrente, A.; Maude, D. K.
- 2D Materials, Vol. 4, Issue 2
Valley dynamics probed through charged and neutral exciton emission in monolayer
journal, August 2014
- Wang, G.; Bouet, L.; Lagarde, D.
- Physical Review B, Vol. 90, Issue 7
Carrier and Polarization Dynamics in Monolayer
journal, January 2014
- Lagarde, D.; Bouet, L.; Marie, X.
- Physical Review Letters, Vol. 112, Issue 4
Probing many-body interactions in monolayer transition-metal dichalcogenides
journal, February 2019
- Van Tuan, Dinh; Scharf, Benedikt; Wang, Zefang
- Physical Review B, Vol. 99, Issue 8
Polarization and time-resolved photoluminescence spectroscopy of excitons in MoSe 2 monolayers
journal, March 2015
- Wang, G.; Palleau, E.; Amand, T.
- Applied Physics Letters, Vol. 106, Issue 11
Magnetic brightening and control of dark excitons in monolayer WSe2
journal, June 2017
- Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang
- Nature Nanotechnology, Vol. 12, Issue 9
Emerging Photoluminescence in Monolayer MoS2
journal, April 2010
- Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
- Nano Letters, Vol. 10, Issue 4, p. 1271-1275
Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014
- Xu, Xiaodong; Yao, Wang; Xiao, Di
- Nature Physics, Vol. 10, Issue 5
Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum
journal, March 2019
- Scharf, Benedikt; Van Tuan, Dinh; Žutić, Igor
- Journal of Physics: Condensed Matter, Vol. 31, Issue 20
Resonant Spin Amplification in -Type GaAs
journal, May 1998
- Kikkawa, J. M.; Awschalom, D. D.
- Physical Review Letters, Vol. 80, Issue 19
Optical polarization and intervalley scattering in single layers of MoS2 and MoSe2
journal, April 2016
- Kioseoglou, G.; Hanbicki, A. T.; Currie, M.
- Scientific Reports, Vol. 6, Issue 1
Valley depolarization in monolayer WSe2
journal, October 2015
- Yan, Tengfei; Qiao, Xiaofen; Tan, Pingheng
- Scientific Reports, Vol. 5, Issue 1
In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
journal, July 2017
- Wang, G.; Robert, C.; Glazov, M. M.
- Physical Review Letters, Vol. 119, Issue 4
Optical Orientation and Femtosecond Relaxation of Spin-Polarized Holes in GaAs
journal, September 2002
- Hilton, D. J.; Tang, C. L.
- Physical Review Letters, Vol. 89, Issue 14
Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer
journal, August 2019
- Molas, M. R.; Slobodeniuk, A. O.; Kazimierczuk, T.
- Physical Review Letters, Vol. 123, Issue 9
k · p theory for two-dimensional transition metal dichalcogenide semiconductors
journal, April 2015
- Kormányos, Andor; Burkard, Guido; Gmitra, Martin
- 2D Materials, Vol. 2, Issue 2
Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
journal, September 2016
- Plechinger, Gerd; Nagler, Philipp; Arora, Ashish
- Nature Communications, Vol. 7, Issue 1
Resonance Profiles of Valley Polarization in Single-Layer and
journal, October 2018
- Tornatzky, Hans; Kaulitz, Anne-Marie; Maultzsch, Janina
- Physical Review Letters, Vol. 121, Issue 16
Large spin splitting in the conduction band of transition metal dichalcogenide monolayers
journal, December 2013
- Kośmider, K.; González, J. W.; Fernández-Rossier, J.
- Physical Review B, Vol. 88, Issue 24
Ultrafast valley relaxation dynamics in monolayer probed by nonequilibrium optical techniques
journal, December 2015
- Dal Conte, S.; Bottegoni, F.; Pogna, E. A. A.
- Physical Review B, Vol. 92, Issue 23
Probing the Interlayer Exciton Physics in a MoS 2 /MoSe 2 /MoS 2 van der Waals Heterostructure
journal, September 2017
- Baranowski, M.; Surrente, A.; Klopotowski, L.
- Nano Letters, Vol. 17, Issue 10
Marrying Excitons and Plasmons in Monolayer Transition-Metal Dichalcogenides
journal, November 2017
- Van Tuan, Dinh; Scharf, Benedikt; Žutić, Igor
- Physical Review X, Vol. 7, Issue 4
Spin relaxation via exchange with donor impurity-bound electrons
journal, June 2015
- Qing, Lan; Li, Jing; Appelbaum, Ian
- Physical Review B, Vol. 91, Issue 24
Exciton valley dynamics in monolayer Mo 1-x W x Se 2 (x = 0, 0.5, 1)
journal, October 2017
- Ye, Jialiang; Niu, Binghui; Li, Ying
- Applied Physics Letters, Vol. 111, Issue 15
Atomically Thin A New Direct-Gap Semiconductor
journal, September 2010
- Mak, Kin Fai; Lee, Changgu; Hone, James
- Physical Review Letters, Vol. 105, Issue 13, Article No.136805
Low-temperature photocarrier dynamics in monolayer MoS 2
journal, September 2011
- Korn, T.; Heydrich, S.; Hirmer, M.
- Applied Physics Letters, Vol. 99, Issue 10
Low-temperature spin relaxation in n -type GaAs
journal, December 2002
- Dzhioev, R. I.; Kavokin, K. V.; Korenev, V. L.
- Physical Review B, Vol. 66, Issue 24
Ultrafast Coulomb-Induced Intervalley Coupling in Atomically Thin WS 2
journal, April 2016
- Schmidt, Robert; Berghäuser, Gunnar; Schneider, Robert
- Nano Letters, Vol. 16, Issue 5
Theory of intervalley Coulomb interactions in monolayer transition-metal dichalcogenides
journal, August 2016
- Dery, Hanan
- Physical Review B, Vol. 94, Issue 7
Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012
- Cao, Ting; Wang, Gang; Han, Wenpeng
- Nature Communications, Vol. 3, Issue 1
Nuclear Dynamic Polarization by Optical Electronic Saturation and Optical Pumping in Semiconductors
journal, March 1968
- Lampel, Georges
- Physical Review Letters, Vol. 20, Issue 10
Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides
journal, May 2014
- Yu, Hongyi; Liu, Gui-Bin; Gong, Pu
- Nature Communications, Vol. 5, Issue 1
Exciton spin dynamics in quantum wells
journal, June 1993
- Maialle, M. Z.; de Andrada e. Silva, E. A.; Sham, L. J.
- Physical Review B, Vol. 47, Issue 23
Two-dimensional Fröhlich interaction in transition-metal dichalcogenide monolayers: Theoretical modeling and first-principles calculations
journal, August 2016
- Sohier, Thibault; Calandra, Matteo; Mauri, Francesco
- Physical Review B, Vol. 94, Issue 8
Spin-Orbit Coupling, Quantum Dots, and Qubits in Monolayer Transition Metal Dichalcogenides
journal, March 2014
- Kormányos, Andor; Zólyomi, Viktor; Drummond, Neil D.
- Physical Review X, Vol. 4, Issue 1
Spin–flip processes and radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers
journal, August 2016
- Slobodeniuk, A. O.; Basko, D. M.
- 2D Materials, Vol. 3, Issue 3
Spintronics: Fundamentals and applications
journal, April 2004
- Žutić, Igor; Fabian, Jaroslav; Das Sarma, S.
- Reviews of Modern Physics, Vol. 76, Issue 2
Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018
- Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
- Reviews of Modern Physics, Vol. 90, Issue 2
Observation of exciton-phonon coupling in monolayers
journal, July 2018
- Shree, S.; Semina, M.; Robert, C.
- Physical Review B, Vol. 98, Issue 3
Coulomb interaction in monolayer transition-metal dichalcogenides
journal, September 2018
- Van Tuan, Dinh; Yang, Min; Dery, Hanan
- Physical Review B, Vol. 98, Issue 12
Exciton radiative lifetime in transition metal dichalcogenide monolayers
journal, May 2016
- Robert, C.; Lagarde, D.; Cadiz, F.
- Physical Review B, Vol. 93, Issue 20
Intrinsic transport properties of electrons and holes in monolayer transition-metal dichalcogenides
journal, July 2014
- Jin, Zhenghe; Li, Xiaodong; Mullen, Jeffrey T.
- Physical Review B, Vol. 90, Issue 4
Solution of few-body problems with the stochastic variational method II: Two-dimensional systems
journal, October 2008
- Varga, Kálmán
- Computer Physics Communications, Vol. 179, Issue 8
Theory of Spin-Dependent Phonon-Assisted Optical Transitions in Silicon
journal, July 2010
- Li, Pengke; Dery, Hanan
- Physical Review Letters, Vol. 105, Issue 3
Observation of Exciton–Exciton Interaction Mediated Valley Depolarization in Monolayer MoSe 2
journal, December 2017
- Mahmood, Fahad; Alpichshev, Zhanybek; Lee, Yi-Hsien
- Nano Letters, Vol. 18, Issue 1
Optical generation of excitonic valley coherence in monolayer WSe2
journal, August 2013
- Jones, Aaron M.; Yu, Hongyi; Ghimire, Nirmal J.
- Nature Nanotechnology, Vol. 8, Issue 9
Optical Spin Injection and Spin Lifetime in Ge Heterostructures
journal, April 2012
- Pezzoli, F.; Bottegoni, F.; Trivedi, D.
- Physical Review Letters, Vol. 108, Issue 15
Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry
journal, July 2013
- Song, Yang; Dery, Hanan
- Physical Review Letters, Vol. 111, Issue 2
Binding energies and structures of two-dimensional excitonic complexes in transition metal dichalcogenides
journal, March 2016
- Kidd, Daniel W.; Zhang, David K.; Varga, Kálmán
- Physical Review B, Vol. 93, Issue 12
Spin and valley dynamics of excitons in transition metal dichalcogenide monolayers: Spin and valley dynamics of excitons in transition metal dichalcogenide monolayers
journal, October 2015
- Glazov, M. M.; Ivchenko, E. L.; Wang, G.
- physica status solidi (b), Vol. 252, Issue 11
Theory and application of explicitly correlated Gaussians
journal, May 2013
- Mitroy, Jim; Bubin, Sergiy; Horiuchi, Wataru
- Reviews of Modern Physics, Vol. 85, Issue 2
Virtual Trions in the Photoluminescence of Monolayer Transition-Metal Dichalcogenides
journal, May 2019
- Van Tuan, Dinh; Jones, Aaron M.; Yang, Min
- Physical Review Letters, Vol. 122, Issue 21
Spin and energy relaxation in germanium studied by spin-polarized direct-gap photoluminescence
journal, July 2013
- Pezzoli, Fabio; Qing, Lan; Giorgioni, Anna
- Physical Review B, Vol. 88, Issue 4
Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016
- Mak, Kin Fai; Shan, Jie
- Nature Photonics, Vol. 10, Issue 4
Precise solution of few-body problems with the stochastic variational method on a correlated Gaussian basis
journal, December 1995
- Varga, K.; Suzuki, Y.
- Physical Review C, Vol. 52, Issue 6
Exciton formation assisted by longitudinal optical phonons in monolayer transition metal dichalcogenides
journal, September 2016
- Thilagam, A.
- Journal of Applied Physics, Vol. 120, Issue 12
Phonon-limited mobility in -type single-layer MoS from first principles
journal, March 2012
- Kaasbjerg, Kristen; Thygesen, Kristian S.; Jacobsen, Karsten W.
- Physical Review B, Vol. 85, Issue 11
Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides
journal, September 2015
- Dery, Hanan; Song, Yang
- Physical Review B, Vol. 92, Issue 12
Spin Accumulation and Dynamics in Inversion-Symmetric van der Waals Crystals
journal, June 2018
- Guimarães, M. H. D.; Koopmans, B.
- Physical Review Letters, Vol. 120, Issue 26
Excitons and trions in monolayer transition metal dichalcogenides: A comparative study between the multiband model and the quadratic single-band model
journal, July 2017
- Van der Donck, M.; Zarenia, M.; Peeters, F. M.
- Physical Review B, Vol. 96, Issue 3
Exciton valley dynamics probed by Kerr rotation in monolayers
journal, October 2014
- Zhu, C. R.; Zhang, K.; Glazov, M.
- Physical Review B, Vol. 90, Issue 16
Temporal and spatial valley dynamics in two-dimensional semiconductors probed via Kerr rotation
journal, February 2017
- Huang, Jiani; Hoang, Thang B.; Ming, Tian
- Physical Review B, Vol. 95, Issue 7
Valley excitons in two-dimensional semiconductors
journal, December 2014
- Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong
- National Science Review, Vol. 2, Issue 1
Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe 2
journal, November 2019
- Lu, Zhengguang; Rhodes, Daniel; Li, Zhipeng
- 2D Materials, Vol. 7, Issue 1
Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
journal, August 2019
- Fang, H. H.; Han, B.; Robert, C.
- Physical Review Letters, Vol. 123, Issue 6
Strain effects on the spin-orbit-induced band structure splittings in monolayer MoS and graphene
journal, October 2013
- Cheiwchanchamnangij, Tawinan; Lambrecht, Walter R. L.; Song, Yang
- Physical Review B, Vol. 88, Issue 15
Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012
- Mak, Kin Fai; He, Keliang; Shan, Jie
- Nature Nanotechnology, Vol. 7, Issue 8
Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer
journal, May 2014
- Yu, T.; Wu, M. W.
- Physical Review B, Vol. 89, Issue 20
Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012
- Zeng, Hualing; Dai, Junfeng; Yao, Wang
- Nature Nanotechnology, Vol. 7, Issue 8
Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers
journal, October 2017
- Robert, C.; Amand, T.; Cadiz, F.
- Physical Review B, Vol. 96, Issue 15
Excitonic properties of semiconducting monolayer and bilayer
journal, October 2016
- Robert, C.; Picard, R.; Lagarde, D.
- Physical Review B, Vol. 94, Issue 15
Exciton formation assisted by longitudinal optical phonons in monolayer transition metal dichalcogenides
journal, September 2016
- Thilagam, A.
- Journal of Applied Physics, Vol. 120, Issue 12