Growth Anisotropy and Morphology Evolution of Line Defects in Monolayer MoS₂: Atomic-Level Observation, Large-Scale Statistics, and Mechanism Understanding

Understanding the growth behavior and morphology evolution of defects in 2D transition metal dichalcogenides is significant for the performance tuning of nanoelectronic devices. Here, the low-voltage aberration-corrected transmission electron microscopy with an in situ heating holder and a fast frame rate camera to investigate the sulfur vacancy lines in monolayer MoS2 is applied. Vacancy concentration-dependent growth anisotropy is discovered, displaying first lengthening and then broadening of line defects as the vacancy densifies. With the temperature increase from 20 degrees C to 800 degrees C, the defect morphology evolves from a dense triangular network to an ultralong linear structure due to the temperature-sensitive vacancy migration process. Atomistic dynamics of line defect reconstruction on the millisecond time scale are also captured. Density functional theory calculations, Monte Carlo simulation, and configurational force analysis are implemented to understand the growth and reconstruction mechanisms at relevant time and length scales. Throughout the work, high-resolution imaging is closely combined with quantitative analysis of images involving thousands of atoms so that the atomic-level structure and the large-area statistical rules are obtained simultaneously. The work provides new ideas for balancing the accuracy and universality of discoveries in the TEM study and will be helpful to the controlled sculpture of nanomaterials