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  Generation and evolution of spin-, valley- and layer-polarized excited carriers in inversion-symmetric WSe2

Bertoni, R., Nicholson, C., Waldecker, L., Hübener, H., Monney, C., De Giovannini, U., et al. (2016). Generation and evolution of spin-, valley- and layer-polarized excited carriers in inversion-symmetric WSe2. Physical Review Letters, 117(27): 277201. doi:10.1103/PhysRevLett.117.277201.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002A-E779-A Version Permalink: http://hdl.handle.net/21.11116/0000-0004-8FD1-F
Genre: Journal Article

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PhysRevLett.117.277201.pdf (Publisher version), 898KB
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2016_Bertoni_TMDC_dichroism_SI_rev.pdf (Supplementary material), 228KB
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http://arxiv.org/abs/1606.03218 (Preprint)
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 Creators:
Bertoni, Roman1, Author              
Nicholson, Christopher1, Author              
Waldecker, Lutz1, Author              
Hübener, Hannes2, Author
Monney, Claude3, Author
De Giovannini, Umberto2, Author
Puppin, Michele1, Author              
Hoesch, Moritz4, Author
Springate, Emma5, Author
Chapman, Richard T.5, Author
Cacho, Cephise5, Author
Wolf, Martin1, Author              
Rubio, Angel2, 6, 7, Author              
Ernstorfer, Ralph1, Author              
Affiliations:
1Physical Chemistry, Fritz Haber Institute, Max Planck Society, ou_634546              
2Nano-Bio Spectroscopy Group and ETSF, Universidad del País Vasco, CFM CSIC-UPV/EHU, 20018 San Sebastian, Spain, ou_persistent22              
3University of Zurich, Department of Physics, Winterthurerstrasse 190, 8057 Zürich, Switzerland, ou_persistent22              
4Diamond Light Source, Harwell Campus, Didcot OX11 0DE, United Kingdom, ou_persistent22              
5Central Laser Facility, STFC Rutherford Appleton Laboratory, Harwell Campus, Didcot OX11 0QX, United Kingdom, ou_persistent22              
6Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
7Center for Free-Electron Laser Science, Notkestraße 85, 22761 Hamburg, Germany, ou_persistent22              

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Free keywords: Condensed Matter; Mesoscale and Nanoscale Physics; Materials Science
 Abstract: Manipulation of spin and valley degrees of freedom is a key step towards realizing novel quantum technologies, for which atomically thin transition metal dichalcogenides (TMDCs) have been established as promising candidates. In monolayer TMDCs, the lack of inversion symmetry gives rise to a spin-valley correlation of the band structure allowing for valley-selective electronic excitation with circularly polarized light. Here we show that, even in centrosymmetric samples of 2H-WSe2, circularly polarized light can generate spin-, valley- and layer-polarized excited states in the conduction band. Employing time- and angle-resolved photoemission spectroscopy (trARPES) with spin-selective excitation, the dynamics of valley and layer pseudospins of the excited carriers are investigated. Complementary time-dependent density functional theory (TDDFT) calculations of the excited state populations reveal a strong circular dichroism of the spin-, valley- and layer-polarizations and a pronounced 2D character of the excited states in the K valleys. We observe scattering of carriers towards the global minimum of the conduction band on a sub-100 femtosecond timescale to states with three-dimensional character facilitating inter-layer charge transfer. Our results establish the optical control of coupled spin-, valley- and layer-polarized states in centrosymmetric materials and suggest the suitability of TMDC multilayer materials for valleytronic and spintronic device concepts.

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Language(s): eng - English
 Dates: 2016-07-182016-12-302016-12-30
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: arXiv: 1606.03218
DOI: 10.1103/PhysRevLett.117.277201
 Degree: -

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Project name : This work was funded by the Max Planck Society, the European Research Council (ERC-2010-AdG-267374), by the Ministerio de Economía y Competitividad (FIS2013- 46159-C3-1-P), and Grupos Consolidados UPV/EHU (IT578-13). Access to the Artemis Facility was funded by Laserlab-Europe III (EU-FP7, grant agreement No. 284464). R. B. thanks the Alexander von Humboldt Foundation for financial support. H. H. acknowledges support from the People Programme (Marie Curie Actions) of the European Union ’ s Seventh Framework Programme FP7-PEOPLE-2013-IEF Project No. 622934. C. M. acknowledges support by the Swiss National Science Foundation under Grant No. PZ00P2_154867.
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Title: Physical Review Letters
  Abbreviation : Phys. Rev. Lett.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Physical Society
Pages: - Volume / Issue: 117 (27) Sequence Number: 277201 Start / End Page: - Identifier: ISSN: 0031-9007
CoNE: /journals/resource/954925433406_1