15 January 2013 | Hualing Zeng1, Gui-Bin Liu1,4,5, Junfeng Dai2,1, Yajun Yan3, Bairen Zhu1, Ruicong He1, Lu Xie1, Shijie Xu1, Xianhui Chen3, Wang Yao1,4 & Xiaodong Cui1
This study investigates the optical properties of WS2 and WSe2 monolayers and multilayers, focusing on the impact of symmetry variations and spin-valley coupling. The efficiency of second harmonic generation (SHG) shows a dramatic even-odd oscillation with the number of layers, indicating the presence or absence of inversion symmetry. Photoluminescence (PL) measurements reveal a crossover from an indirect band gap semiconductor in multilayers to a direct-gap one in monolayers. A hot luminescence peak (B) is observed at ~0.4 eV above the prominent band edge peak (A) in all samples, with the magnitude of A-B splitting being independent of the number of layers and coinciding with the spin-valley coupling strength in monolayers. Ab initio calculations confirm that this thickness-independent splitting pattern is a direct consequence of the strong spin-valley coupling, which suppresses interlayer hopping at the valence band edge near K points due to the sign change of the spin-valley coupling in the 2H stacking order. The study highlights the unique properties of tungsten dichalcogenides, making them promising materials for spintronics and valley-based electronics.This study investigates the optical properties of WS2 and WSe2 monolayers and multilayers, focusing on the impact of symmetry variations and spin-valley coupling. The efficiency of second harmonic generation (SHG) shows a dramatic even-odd oscillation with the number of layers, indicating the presence or absence of inversion symmetry. Photoluminescence (PL) measurements reveal a crossover from an indirect band gap semiconductor in multilayers to a direct-gap one in monolayers. A hot luminescence peak (B) is observed at ~0.4 eV above the prominent band edge peak (A) in all samples, with the magnitude of A-B splitting being independent of the number of layers and coinciding with the spin-valley coupling strength in monolayers. Ab initio calculations confirm that this thickness-independent splitting pattern is a direct consequence of the strong spin-valley coupling, which suppresses interlayer hopping at the valence band edge near K points due to the sign change of the spin-valley coupling in the 2H stacking order. The study highlights the unique properties of tungsten dichalcogenides, making them promising materials for spintronics and valley-based electronics.