Generation and Evolution of Spin-, Valley-, and Layer-Polarized Excited Carriers in Inversion-Symmetric WSe2

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 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