Spin states protected from intrinsic electron-phonon coupling reaching 100 ns lifetime at room temperature in MoSe₂

We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe. 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...

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Detalles Bibliográficos
Autores: Ersfeld, Manfred, Volmer, Frank|||0000-0003-3526-2687, Melo, Pedro Miguel M. C. de, Winter, Robin de, Heithoff, Maximilian, Zanolli, Zeila|||0000-0003-0860-600X, Stampfer, Cristoph, Verstraete, Matthieu J.|||0000-0001-6921-5163, Beschoten, Bernd|||0000-0003-2359-2718
Tipo de recurso: artículo
Fecha de publicación:2019
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:215004
Acceso en línea:https://ddd.uab.cat/record/215004
https://dx.doi.org/urn:doi:10.1021/acs.nanolett.9b01485
Access Level:acceso abierto
Palabra clave:Transition metal dichalcogenides
Monolayer MoSe₂
Time-resolved Kerr rotation
Spin lifetime
Electron-phonon coupling
Descripción
Sumario:We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe. 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.