Thiemann Fabian L, Scalliet Camille, Müller Erich A, Michaelides Angelos
IBM Research Europe, Daresbury WA4 4AD, United Kingdom.
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, United Kingdom.
Proc Natl Acad Sci U S A. 2025 Mar 4;122(9):e2416932122. doi: 10.1073/pnas.2416932122. Epub 2025 Feb 28.
Two-dimensional (2D) materials display nanoscale dynamic ripples that significantly impact their properties. Defects within the crystal lattice are the elementary building blocks to tailor the material's morphology. While some studies have explored the link between defective structures and rippling dynamics in 2D materials, a comprehensive understanding of this relationship has yet to be achieved. Here, we address this using machine learning-driven molecular dynamics simulations. Specifically, we find that above a critical concentration of defects, free-standing graphene sheets undergo a dynamic transition from freely propagating to static ripples. Our computational approach captures the dynamics with atomic resolution, and reveals that the transition is driven by elastic interactions between defects. The strength of these interactions is found to vary across defect types and we identify a unifying set of principles driving the dynamic-to-static transition in 2D materials. Our work not only rationalizes puzzling experimental results for defective 2D materials, but also paves the way to design two-dimensional devices with tailored rippling dynamics. These insights could lay the foundations for a class of disorder-based catalytic and interfacial materials.
二维(2D)材料呈现出纳米级的动态涟漪,这对其性能有显著影响。晶格中的缺陷是定制材料形态的基本构建单元。虽然一些研究探索了二维材料中缺陷结构与涟漪动力学之间的联系,但尚未实现对这种关系的全面理解。在这里,我们使用机器学习驱动的分子动力学模拟来解决这个问题。具体而言,我们发现,当缺陷浓度超过临界值时,独立的石墨烯片会经历从自由传播到静态涟漪的动态转变。我们的计算方法以原子分辨率捕捉动力学,并揭示这种转变是由缺陷之间的弹性相互作用驱动的。发现这些相互作用的强度因缺陷类型而异,并且我们确定了一组统一的原理来驱动二维材料中的动态到静态转变。我们的工作不仅解释了有缺陷的二维材料令人困惑的实验结果,还为设计具有定制涟漪动力学的二维器件铺平了道路。这些见解可为一类基于无序的催化和界面材料奠定基础。