Journal
PHYSICAL REVIEW LETTERS
Volume 117, Issue 27, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.117.277201
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Funding
- Max Planck Society
- European Research Council [ERC-2010-AdG-267374]
- Ministerio de Economia y Competitividad [FIS2013-46159-C3-1-P]
- Grupos Consolidados UPV/EHU [IT578-13]
- Laserlab-Europe III (EU-FP7) [284464]
- Alexander von Humboldt Foundation
- People Programme (Marie Curie Actions) of the European Union's Seventh Framework Programme FP7-PEOPLE-IEF Project [622934]
- Swiss National Science Foundation [PZ00P2_154867]
- Swiss National Science Foundation (SNF) [PZ00P2_154867] Funding Source: Swiss National Science Foundation (SNF)
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We report the spin-selective optical excitation of carriers in inversion-symmetric bulk samples of the transition metal dichalcogenide (TMDC) WSe2. Employing time-and angle-resolved photoelectron spectroscopy (trARPES) and complementary time-dependent density functional theory (TDDFT), we observe spin-, valley-, and layer-polarized excited state populations upon excitation with circularly polarized pump pulses, followed by ultrafast (< 100 fs) scattering of carriers towards the global minimum of the conduction band. TDDFT reveals the character of the conduction band, into which electrons are initially excited, to be two-dimensional and localized within individual layers, whereas at the minimum of the conduction band, states have a three-dimensional character, facilitating interlayer charge transfer. These results establish the optical control of coupled spin-, valley-, and layer-polarized states in centrosymmetric materials with locally broken symmetries and suggest the suitability of TMDC multilayer and heterostructure materials for valleytronic and spintronic device concepts.
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