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 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 switche...

Descripción completa

Detalles Bibliográficos
Autores: Ersfeld, Manfred, Volmer, Frank, Melo, Pedro Miguel M. C. de, Winter, Robin de, Heithoff, Maximilian, Zanolli, Zeila, Stampfer, Christoph, Verstraete, Matthieu J., Beschoten, Bernd
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2019
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/201047
Acceso en línea:http://hdl.handle.net/10261/201047
Access Level:acceso abierto
id ES_16d279726d6df02cc6bc9bc9cd096f2d
oai_identifier_str oai:digital.csic.es:10261/201047
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
title Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
spellingShingle Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
Ersfeld, Manfred
title_short Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
title_full Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
title_fullStr Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
title_full_unstemmed Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
title_sort Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2
dc.creator.none.fl_str_mv Ersfeld, Manfred
Volmer, Frank
Melo, Pedro Miguel M. C. de
Winter, Robin de
Heithoff, Maximilian
Zanolli, Zeila
Stampfer, Christoph
Verstraete, Matthieu J.
Beschoten, Bernd
author Ersfeld, Manfred
author_facet Ersfeld, Manfred
Volmer, Frank
Melo, Pedro Miguel M. C. de
Winter, Robin de
Heithoff, Maximilian
Zanolli, Zeila
Stampfer, Christoph
Verstraete, Matthieu J.
Beschoten, Bernd
author_role author
author2 Volmer, Frank
Melo, Pedro Miguel M. C. de
Winter, Robin de
Heithoff, Maximilian
Zanolli, Zeila
Stampfer, Christoph
Verstraete, Matthieu J.
Beschoten, Bernd
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Agencia Estatal de Investigación (España)
European Commission
Helmholtz Association
Fonds de la Recherche Scientifique (Fédération Wallonie-Bruxelles)
Communauté Française de Belgique
Agence Nationale de la Recherche (France)
Ministerio de Economía y Competitividad (España)
Generalitat de Catalunya
Ministerio de Ciencia, Innovación y Universidades (España)
National Fund for Scientific Research (Belgium)
Fonds de la Recherche Scientifique (Fédération Wallonie-Bruxelles)
Beschoten, Bernd [0000-0003-2359-2718]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
description 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.
publishDate 2019
dc.date.none.fl_str_mv 2019
2020
2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/201047
url http://hdl.handle.net/10261/201047
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/EC/H2020/785219
SEV-2017-0706/AEI/10.13039/501100011033
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/RYC-2016-19344
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/SEV-2017-0706
info:eu-repo/grantAgreement/EC/H2020/824143
info:eu-repo/grantAgreement/EC/H2020/653838
https://doi.org/10.1021/acs.nanolett.9b01485

dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869403880563933184
spelling Spin states protected from intrinsic electron–phonon coupling reaching 100 ns lifetime at room temperature in MoSe2Ersfeld, ManfredVolmer, FrankMelo, Pedro Miguel M. C. deWinter, Robin deHeithoff, MaximilianZanolli, ZeilaStampfer, ChristophVerstraete, Matthieu J.Beschoten, BerndWe 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.This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 785219. It was also supported by the Helmholtz Nanoelectronic Facility (HNF)57 at the Forschungszentrum Jülich. P.M.M.C.M. and M.J.V. acknowledge funding by the Belgian FNRS (PDR G.A. T.1077.15-1/7) and the Communauté Francaise de Belgique (ARC AIMED G.A. 15/19-09). ̧ Z.Z. acknowledges financial support by the Ramon y Cajal program (RYC-2016-19344), the CERCA programme of the Generalitat de Catalunya (grant 2017SGR1506), the Severo Ochoa programme (MINECO, SEV-2017-0706), and the EC H2020-INFRAEDI-2018-2020 MaX “Materials Design at the Exascale” CoE (grant No. 824143). Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by FRS-FNRS G.A. 2.5020.11; the Zenobe Tier-1 supercomputer is funded by the Walloon Region under G.A. 1117545 and by a PRACE-3IP DECI grant 2DSpin on Beskow (G.A. 653838 of H2020).Peer reviewedAmerican Chemical SocietyAgencia Estatal de Investigación (España)European CommissionHelmholtz AssociationFonds de la Recherche Scientifique (Fédération Wallonie-Bruxelles)Communauté Française de BelgiqueAgence Nationale de la Recherche (France)Ministerio de Economía y Competitividad (España)Generalitat de CatalunyaMinisterio de Ciencia, Innovación y Universidades (España)National Fund for Scientific Research (Belgium)Fonds de la Recherche Scientifique (Fédération Wallonie-Bruxelles)Beschoten, Bernd [0000-0003-2359-2718]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202020202019info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/201047reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/H2020/785219SEV-2017-0706/AEI/10.13039/501100011033info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/RYC-2016-19344info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/SEV-2017-0706info:eu-repo/grantAgreement/EC/H2020/824143info:eu-repo/grantAgreement/EC/H2020/653838https://doi.org/10.1021/acs.nanolett.9b01485Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2010472026-05-22T06:33:51Z
score 15,81155