Deb Pratiti, Cao Michael C, Han Yimo, Holtz Megan E, Xie Saien, Park Jiwoong, Hovden Robert, Muller David A
School of Applied and Engineering Physics, Cornell University, Ithaca, USA.
School of Applied and Engineering Physics, Cornell University, Ithaca, USA.; Department of Chemistry, Pritzker School of Molecular Engineering, and James Franck Institute, University of Chicago, Chicago, IL 60637, USA.
Ultramicroscopy. 2020 Aug;215:113019. doi: 10.1016/j.ultramic.2020.113019. Epub 2020 May 26.
Friedel's law guarantees an inversion-symmetric diffraction pattern for thin, light materials where a kinematic approximation or a single-scattering model holds. Typically, breaking Friedel symmetry is ascribed to multiple scattering events within thick, non-centrosymmetric crystals. However, two-dimensional (2D) materials such as a single monolayer of MoS can also violate Friedel's law, with unexpected contrast between conjugate Bragg peaks. We show analytically that retaining higher order terms in the power series expansion of the scattered wavefunction can describe the anomalous contrast between hkl and hkl¯peaks that occurs in 2D crystals with broken in-plane inversion symmetry. These higher-order terms describe multiple scattering paths starting from the same atom in an atomically thin material. Furthermore, 2D materials containing heavy elements, such as WS, always act as strong phase objects, violating Friedel's law no matter how high the energy of the incident electron beam. Experimentally, this understanding can enhance diffraction-based techniques to provide rapid imaging of polarity, twin domains, in-plane rotations, or other polar textures in 2D materials.
弗里德尔定律保证了对于薄的轻质材料,在运动学近似或单散射模型成立的情况下会出现反演对称的衍射图案。通常,弗里德尔对称性的破坏归因于厚的非中心对称晶体中的多次散射事件。然而,二维(2D)材料,如单层MoS,也会违反弗里德尔定律,共轭布拉格峰之间会出现意想不到的对比度。我们通过分析表明,在散射波函数的幂级数展开中保留高阶项,可以描述在具有面内反演对称性破坏的二维晶体中hkl和hkl¯峰之间出现的反常对比度。这些高阶项描述了从原子级薄材料中的同一个原子开始的多次散射路径。此外,含有重元素的二维材料,如WS,总是表现为强相位物体,无论入射电子束的能量有多高,都会违反弗里德尔定律。在实验上,这种理解可以增强基于衍射的技术,以快速成像二维材料中的极性、孪晶畴、面内旋转或其他极性纹理。