School of Engineering, Indian Institute of Technology Mandi, Kamand, H.P. 175005, India.
Nanoscale. 2018 Aug 30;10(34):16321-16331. doi: 10.1039/c8nr02246a.
A scalable approach is needed in the formation of atomically flat edges with specific terminations to enhance local properties for optoelectronic, nanophotonic and energy applications. We demonstrate point defect clustering-driven faceted void formations with luminescent enhanced edges in WS2 monolayers during large-scale CVD growth and controlled annealing. With the aid of aberration-corrected scanning transmission electron microscopy (AC-STEM) high angle annular dark field (HAADF) imaging, we probed atomic terminations of S and W to explain observed luminescence enhancement in alternate edges. Faceted void formation in monolayer WS2 was found to be sensitive to annealing temperature, time, gas environment and precursor supply. Our observations of areal coverage evolution over time revealed competition between monolayer WS2 growth and void formation at 850 °C. While the initial stage was dominated by monolayer growth, defect generation and void growth dominated at later stages and provided an optimum processing window for monolayer WS2 as well as faceted void growth. Growth of faceted voids not only followed the geometry of monolayer facets but also showed similar atomic terminations at the edges and thus enabled local manipulation of photoluminescence enhancement with an order of magnitude increase in intensity. The developed CVD processing enabled multi-fold increase in the luminescent active edge length through the formation of faceted voids within the WS2 monolayer.
需要一种可扩展的方法来形成具有特定末端的原子级平坦边缘,以增强光电、纳米光子学和能源应用的局部性质。我们在大规模 CVD 生长和控制退火过程中,展示了点缺陷团聚驱动的层状 WS2 中单原子层中具有发光增强边缘的面心空隙形成。借助校正像差的扫描透射电子显微镜(AC-STEM)高角度环形暗场(HAADF)成像,我们探测了 S 和 W 的原子末端,以解释在交替边缘观察到的发光增强。发现单层 WS2 中的面心空隙形成对退火温度、时间、气体环境和前驱体供应敏感。我们对随时间变化的面积覆盖率的观察揭示了 850°C 时单层 WS2 生长和空隙形成之间的竞争。虽然初始阶段主要由单层生长主导,但缺陷生成和空隙生长在后期主导,为单层 WS2 以及面心空隙生长提供了最佳的处理窗口。面心空隙的生长不仅遵循了单层的几何形状,而且在边缘处也表现出相似的原子末端,从而能够局部操纵光致发光增强,强度提高了一个数量级。所开发的 CVD 处理方法通过在 WS2 单层中形成面心空隙,使发光活性边缘长度增加了多倍。