Journal
NANO LETTERS
Volume 19, Issue 6, Pages 4083-4090Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b01485
Keywords
Transition metal dichalcogenides; monolayer MoSe2; time-resolved Kerr rotation; spin lifetime; electron-phonon coupling
Categories
Funding
- European Union [785219]
- Helmholtz Nanoelectronic Facility (HNF)57 at the Forschungszentrum Julich
- Belgian FNRS [T.1077.15-1/7]
- Communaute Francaise de Belgique (ARC AIMED) [15/19-09]
- Ramon y Cajal program [RYC-2016-19344]
- CERCA programme of the Generalitat de Catalunya [2017SGR1506]
- Severo Ochoa programme (MINECO) [SEV-2017-0706]
- EC [H2020-INFRAEDI-2018-2020 MaX, 824143]
- FRS-FNRS [G.A. 2.5020.11]
- Walloon Region [G.A. 1117545]
- PRACE-3IP DECI [653838]
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We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe2. These long lifetimes are accompanied by an intriguing temperature-dependence of the Kerr amplitude, which increases with temperature up to 50 K and then abruptly switches sign. Using ab initio simulations, we explain the latter behavior in terms of the intrinsic electron-phonon coupling and the activation of transitions to secondary valleys. The phonon-assisted scattering of the photoexcited electron-hole pairs prepares a valley spin polarization within the first few ps after laser excitation. The sign of the total valley magnetization, and thus the Kerr amplitude, switches as a function of temperature, as conduction and valence band states exhibit different phonon-mediated intervalley scattering rates. However, the electron-phonon scattering on the ps time scale does not provide an explanation for the long spin lifetimes. Hence, we deduce that the initial spin polarization must be transferred into spin states, which are protected from the intrinsic electron-phonon coupling, and are most likely resident charge carriers, which are not part of the itinerant valence or conduction band states.
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