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Accurately Controlling Angle-Resolved Second Harmonic Generation by Stacking Orders from a MoS2 Homobilayer
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-06-17 , DOI: 10.1021/acs.jpcc.2c02778
Chuan He 1 , Lipeng Zhu 2 , Yuanyuan Huang 1 , Wanyi Du 1 , Mei Qi 1 , Yixuan Zhou 1 , Qiyi Zhao 3 , Xinlong Xu 1
Affiliation  

As an efficient way to control crystal symmetry, the stacking order introduces a degree of freedom of twist angle, offering a powerful platform to engineer artificial vertically stacked van der Waals (vdW) structures for nonlinear twistoptics. Herein, we show that stacking orders of a MoS2 homobilayer results in strong tunability of interlayer coupling and second harmonic generation (SHG). The interlayer coupling exhibits a strong dependence on the alignment and staggering degree of the sulfur atoms in the two MoS2 layers. Controlling the in-plane and out-of-plane charge density symmetry by the stacking order can adjust the number and dispersion of second-order nonlinear coefficients in a MoS2 homobilayer. Besides, the angle-resolved SHG pattern of the MoS2 homobilayer with different stacking orders can be distinguished only under oblique incidence, which solves the experimental difficulty in distinguishing the SHG pattern of similar homobilayers such as 3R and 3R-like bilayers. Our results pave the way for the stacking engineering to tune the nonlinear optical response and the angle-dependent SHG pattern to probe the symmetry of stacked vdW structures.

中文翻译:

通过堆叠 MoS2 Homobilayer 的阶数准确控制角度分辨二次谐波的产生

作为控制晶体对称性的一种有效方法,堆叠顺序引入了扭转角的自由度,为设计用于非线性扭转光学的人工垂直堆叠范德华 (vdW) 结构提供了一个强大的平台。在这里,我们展示了 MoS 2同双层的堆叠顺序导致层间耦合和二次谐波产生 (SHG) 的强可调性。层间耦合表现出强烈依赖于两个MoS 2层中硫原子的排列和交错程度。通过堆叠顺序控制面内和面外电荷密度对称性可以调整MoS 2同质双层中二阶非线性系数的数量和色散。此外,MoS 的角度分辨 SHG 图案2不同堆叠顺序的同双层只有在斜入射下才能区分,这解决了区分类似同双层如3R和类3R双层的SHG模式的实验困难。我们的结果为堆叠工程调整非线性光学响应和角度相关的 SHG 图案以探索堆叠 vdW 结构的对称性铺平了道路。
更新日期:2022-06-17
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