Deep potential molecular dynamics simulations of low-temperature plasma-surface interactions

Machine learning approaches to potential generation for molecular dynamics (MD) simulations of low-temperature plasma-surface interactions could greatly extend the range of chemical systems that can be modeled. Empirical potentials are difficult to generalize to complex combinations of multiple elements with interactions that might include covalent, ionic, and metallic bonds. This work demonstrates that a specific machine learning approach, Deep Potential Molecular Dynamics (DeepMD), can generate potentials that provide a good model of plasma etching in the Si-Cl-Ar system. Comparisons are made between MD results using DeepMD models and empirical potentials, as well as experimental measurements. Pure Si properties predicted by the DeepMD model are in reasonable agreement with experimental results. Simulations of Si bombardment by Ar⁺ ions demonstrate the ability of the DeepMD method to predict sputtering yields as well as the depth of the amorphous-crystalline interface. Etch yields as a function of flux ratio and ion energy for simultaneous Cl₂ and Ar⁺ impacts are in good agreement with previous simulation results and experiment. Predictions of etch yields and etch products during plasma-assisted atomic layer etching of Si-Cl₂-Ar are shown to be in good agreement with MD predictions using empirical potentials and with experiment. Finally, good agreement was also seen with measurements for the spontaneous etching of Si by Cl atoms at 300 K. Further, the demonstration that DeepMD can reproduce results from MD simulations using empirical potentials is a necessary condition to future efforts to extend the method to a much wider range of systems for which empirical potentials may be difficult or impossible to obtain.. Authors: Kounis-Melas, Andreas [Princeton Univ., NJ (United States)] (ORCID:0009000185326469); Vella, Joseph R. [Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)] (ORCID:0000000286668719); Panagiotopoulos, Athanassios Z. [Princeton Univ., NJ (United States)] (ORCID:0000000281526615); Graves, David B. [Princeton Univ., NJ (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)] (ORCID:0000000222886768). DOE Contract: AC02-09CH11466. Subjects: 70 PLASMA PHYSICS AND FUSION TECHNOLOGY; Artificial neural networks; Atomic energy; Crystallography; Density functional theory; Force field; Machine learning; Molecular dynamics; Plasma material interactions; Plasma processing; Thermal effects