Modeling for Structural Engineering and Synthesis of Two-Dimensional WSe2 Using a Newly Developed ReaxFF Reactive Force Field
Modeling for Structural Engineering and Synthesis of Two-Dimensional WSe2 Using a Newly Developed ReaxFF Reactive Force Field
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DOI：
10.1021/acs.jpcc.0c09155
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发表时间：
2020-12
影响因子：
3.7
通讯作者：
Nadire Nayir;Yuanxi Wang;S. Shabnam;D. R. Hickey;L. Miao;Xiaotian Zhang;S. Bachu;N. Alem;J. Red
中科院分区：
文献类型：
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作者：
Nadire Nayir;Yuanxi Wang;S. Shabnam;D. R. Hickey;L. Miao;Xiaotian Zhang;S. Bachu;N. Alem;J. Red
原子模拟技术已成为一种不可或缺的工具，以获得一个基本的理解的二维（2D）感兴趣的材料的生长和结构特征，从而加快在同一领域的实验研究。这里提出的一个新的ReaxFF反应力场是第一个全面的经验势，它被明确设计用于捕获2D WSe 2固相化学的最突出的特征，例如作为局部几何形状和硫属元素化学势的函数的缺陷形成，空位迁移和相变，从而使得能够在比第一原理理论可获得的长得多的大长度尺度和时间尺度上对2D WSe 2进行成本有效和可靠的表征。这种潜力，验证使用广泛的第一性原理能量学数据的周期性和非周期性的系统和实验测量，可以准确地描述单层变形和空位能量之间的机械化学耦合，提供有价值的原子洞察力的形态演变的单层在不同的环境中的加载条件和各种浓度和分布的缺陷。由于了解生长如何受到局部化学环境的影响对于制造高效和功能性原子薄的2D WSe 2至关重要，因此新的ReaxFF描述能够以低计算成本使用与实验条件密切匹配的反应环境来研究2D WSe 2单晶的边缘控制生长。
Atomistic simulation techniques have become an indispensable tool to acquire a fundamental understanding of growth and structural characteristics of two-dimensional (2D) materials of interest, thereby accelerating experimental research in the same field. A new ReaxFF reactive force field presented here is the first comprehensive empirical potential that is explicitly designed to capture the most prominent features of 2D WSe2solid-phase chemistry, such as defect formation as a function of local geometry and chalcogen chemical potential, vacancy migration and phase transition, thus enabling cost-effective and reliable characterization of 2D WSe2at large length scales and time scales much longer than what is accessible by first-principles theory. This potential, validated using extensive first-principles energetics data on both periodic and nonperiodic systems and experimental measurements, can accurately describe the mechanochemical coupling between monolayer deformations and vacancy energetics, providing valuable atomistic insights into the morphological evolution of a monolayer in different environments in terms of loading conditions and various concentrations and distributions of defects. Since understanding how growth is affected by the local chemical environment is vital to fabricating efficient and functional atomically thin 2D WSe2, the new ReaxFF description enables investigations of edge-controlled growth of single crystals of 2D WSe2using reactive environments closely matching experimental conditions at a low computational cost.