Accurately Controlling Angle-Resolved Second Harmonic Generation by Stacking Orders from a MoS2 Homobilayer,The Journal of Physical Chemistry C

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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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