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Title: Exciton valley depolarization in monolayer transition-metal dichalcogenides

Journal Article · · Physical Review. B

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.

Research Organization:
Univ. of Rochester, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); French National Research Agency (ANR); State of Florida
Grant/Contract Number:
SC0014349; DMR-1503601
OSTI ID:
1802616
Alternate ID(s):
OSTI ID: 1606584
Journal Information:
Physical Review. B, Vol. 101, Issue 11; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 18 works
Citation information provided by
Web of Science

References (73)

Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons journal June 2017
Exciton fine structure and spin decoherence in monolayers of transition metal dichalcogenides journal May 2014
Dark excitons and the elusive valley polarization in transition metal dichalcogenides journal February 2017
Valley dynamics probed through charged and neutral exciton emission in monolayer WSe 2 journal August 2014
Carrier and Polarization Dynamics in Monolayer MoS 2 journal January 2014
Probing many-body interactions in monolayer transition-metal dichalcogenides journal February 2019
Polarization and time-resolved photoluminescence spectroscopy of excitons in MoSe 2 monolayers journal March 2015
Magnetic brightening and control of dark excitons in monolayer WSe2 journal June 2017
Emerging Photoluminescence in Monolayer MoS2 journal April 2010
Spin and pseudospins in layered transition metal dichalcogenides journal April 2014
Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum journal March 2019
Resonant Spin Amplification in n -Type GaAs journal May 1998
Optical polarization and intervalley scattering in single layers of MoS2 and MoSe2 journal April 2016
Valley depolarization in monolayer WSe2 journal October 2015
In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules journal July 2017
Optical Orientation and Femtosecond Relaxation of Spin-Polarized Holes in GaAs journal September 2002
Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer WSe 2 journal August 2019
k · p theory for two-dimensional transition metal dichalcogenide semiconductors journal April 2015
Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide journal September 2016
Resonance Profiles of Valley Polarization in Single-Layer MoS 2 and MoSe 2 journal October 2018
Large spin splitting in the conduction band of transition metal dichalcogenide monolayers journal December 2013
Ultrafast valley relaxation dynamics in monolayer MoS 2 probed by nonequilibrium optical techniques journal December 2015
Probing the Interlayer Exciton Physics in a MoS 2 /MoSe 2 /MoS 2 van der Waals Heterostructure journal September 2017
Marrying Excitons and Plasmons in Monolayer Transition-Metal Dichalcogenides journal November 2017
Spin relaxation via exchange with donor impurity-bound electrons journal June 2015
Exciton valley dynamics in monolayer Mo 1-x W x Se 2 (x = 0, 0.5, 1) journal October 2017
Atomically Thin MoS2 A New Direct-Gap Semiconductor journal September 2010
Low-temperature photocarrier dynamics in monolayer MoS 2 journal September 2011
Low-temperature spin relaxation in n -type GaAs journal December 2002
Ultrafast Coulomb-Induced Intervalley Coupling in Atomically Thin WS 2 journal April 2016
Theory of intervalley Coulomb interactions in monolayer transition-metal dichalcogenides journal August 2016
Valley-selective circular dichroism of monolayer molybdenum disulphide journal January 2012
Nuclear Dynamic Polarization by Optical Electronic Saturation and Optical Pumping in Semiconductors journal March 1968
Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides journal May 2014
Exciton spin dynamics in quantum wells journal June 1993
Two-dimensional Fröhlich interaction in transition-metal dichalcogenide monolayers: Theoretical modeling and first-principles calculations journal August 2016
Spin-Orbit Coupling, Quantum Dots, and Qubits in Monolayer Transition Metal Dichalcogenides journal March 2014
Spin–flip processes and radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers journal August 2016
Spintronics: Fundamentals and applications journal April 2004
Colloquium : Excitons in atomically thin transition metal dichalcogenides journal April 2018
Observation of exciton-phonon coupling in MoSe 2 monolayers journal July 2018
Coulomb interaction in monolayer transition-metal dichalcogenides journal September 2018
Exciton radiative lifetime in transition metal dichalcogenide monolayers journal May 2016
Intrinsic transport properties of electrons and holes in monolayer transition-metal dichalcogenides journal July 2014
Solution of few-body problems with the stochastic variational method II: Two-dimensional systems journal October 2008
Theory of Spin-Dependent Phonon-Assisted Optical Transitions in Silicon journal July 2010
Observation of Exciton–Exciton Interaction Mediated Valley Depolarization in Monolayer MoSe 2 journal December 2017
Optical generation of excitonic valley coherence in monolayer WSe2 journal August 2013
Optical Spin Injection and Spin Lifetime in Ge Heterostructures journal April 2012
Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry journal July 2013
Binding energies and structures of two-dimensional excitonic complexes in transition metal dichalcogenides journal March 2016
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
Theory and application of explicitly correlated Gaussians journal May 2013
Virtual Trions in the Photoluminescence of Monolayer Transition-Metal Dichalcogenides journal May 2019
Spin and energy relaxation in germanium studied by spin-polarized direct-gap photoluminescence journal July 2013
Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides journal March 2016
Precise solution of few-body problems with the stochastic variational method on a correlated Gaussian basis journal December 1995
Exciton formation assisted by longitudinal optical phonons in monolayer transition metal dichalcogenides journal September 2016
Phonon-limited mobility in n -type single-layer MoS 2 from first principles journal March 2012
Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides journal September 2015
Spin Accumulation and Dynamics in Inversion-Symmetric van der Waals Crystals journal June 2018
Excitons and trions in monolayer transition metal dichalcogenides: A comparative study between the multiband model and the quadratic single-band model journal July 2017
Exciton valley dynamics probed by Kerr rotation in WSe 2 monolayers journal October 2014
Temporal and spatial valley dynamics in two-dimensional semiconductors probed via Kerr rotation journal February 2017
Valley excitons in two-dimensional semiconductors journal December 2014
Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe 2 journal November 2019
Control of the Exciton Radiative Lifetime in van der Waals Heterostructures journal August 2019
Strain effects on the spin-orbit-induced band structure splittings in monolayer MoS 2 and graphene journal October 2013
Control of valley polarization in monolayer MoS2 by optical helicity journal June 2012
Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer MoS 2 journal May 2014
Valley polarization in MoS2 monolayers by optical pumping journal June 2012
Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers journal October 2017
Excitonic properties of semiconducting monolayer and bilayer MoT e 2 journal October 2016

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