11 April 2013 | Hualing Zeng, Gui-Bin Liu, Junfeng Dai, Yajun Yan, Bairen Zhu, Ruicong He, Lu Xie, Shijie Xu, Xianhui Chen, Wang Yao, Xiaodong Cui
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.