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Probing Dynamic Processes of the Initial Stages of Cu(100) Surface Oxidation by in situ Environmental TEM and Multiscale Simulations

Corrosion is one of the biggest challenges facing the safe and reliable use of metals and alloys, especially under elevated temperatures. Understanding the microscopic mechanisms for surface oxidation is critical to unveil the mysteries of corrosion, and will also facilitate research in fields such as environmental stability, high-temperature corrosion, and catalytic reactions. The process of surface oxidation can be divided into three stages, namely oxygen chemisorption, oxide nucleation and growth, and bulk oxide growth. Despite numerous studies focusing on the initial stage of oxidation that commences with oxygen chemisorption on clean metal surfaces and ends with oxide nucleation and growth, this stage remains poorly understood due to the lack of experimental methods available for studying this stage. For example, surface science techniques such as Scanning Tunneling Microscopy (STM) and atomistic simulations have shown that after oxygen chemisorption, clean Cu(100) surfaces will undergo several surface reconstructions, demonstrating c (2×2) reconstruction and missing row reconstruction (MRR) structures[1]. However, characterization of the atomic mechanisms forming reconstructions, as well as determination of whether reconstruction is necessary for oxide nucleation, have not been conclusively investigated, given the lack of direct experimental observation. In this work, using state-of-the-art Environmental TEM (ETEM) (Hitachi H-9500 operating at 300 keV) and multiscale atomistic simulation, we explore the dynamic processes of the initial