Transition metal dichalcogenides; transient absorption spectroscopy; spin and valley dynamics; layered materials; optoelectronics
Abstract :
[en] In monolayer (1L) transition metal dichalcogenides (TMDs) the valence and conduction bands are spin-split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark excitons, consisting of electrons and holes with opposite spin orientation, have lower energy than A excitons. The transition from bright to dark excitons involves the scattering of electrons from the upper to the lower conduction band at the K point of the Brillouin zone, with detrimental effects for the optoelectronic response of 1L-TMDs, since this reduces their light emission efficiency. Here, we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics in 1L-WS2. This occurs on a sub-ps time scale, and it is significantly dependent on temperature, indicative of phonon-assisted relaxation. Time-dependent ab initio calculations show that intravalley spin-flip scattering occurs on significantly longer time scales only at the K point, while the occupation of states away from the minimum of the conduction band significantly reduces the scattering time. Our results shed light on the scattering processes determining the light emission efficiency in optoelectronic and photonic devices based on 1L-TMDs.
Intravalley Spin-Flip Relaxation Dynamics in Single-Layer WS2
Publication date :
November 2018
Journal title :
NANO LETTERS
ISSN :
1530-6984
Publisher :
Amer Chemical Soc, Washington, Unknown/unspecified
Volume :
18
Issue :
11
Pages :
6882-6891
Peer reviewed :
Peer reviewed
Focus Area :
Physics and Materials Science
FnR Project :
FNR7731521 - #4;modelling Of Carrier Dynamics And Ultra-fast Spectroscopy In Two-dimensional Materials, 2014 (01/12/2014-31/03/2017) - Alejandro Molina-sánchez
Funders :
FNR - Fonds National de la Recherche [LU] Juan de la Cierva Program Early Postdoc Mobility program of the Swiss National Science Foundation EU Graphene Flagship ERC grant Hetero2D EPSRC - Engineering and Physical Sciences Research Council [GB] EU project MaX Materials design at the eXascale [H2020-EINFRA-2015-1] Nano science Foundries and Fine Analysis-Europe H2020-INFRAIA-2014-2015
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