Understanding Surface/Interface‐Induced Chemical and Physical Properties at Atomic Level by First Principles Investigations

ABSTRACT The scientific trajectory in contemporary materials research has transitioned toward surface and interface engineering as critical determinants of functional performance, facilitating atomic‐level precision in modulating physical and chemical properties for advanced applications spanning functional device architectures, catalytic systems, and electrochemical technologies. However, persistent challenges in atomic‐scale characterization and the resource‐intensive nature of empirical optimization necessitate systematic implementation of first‐principles calculations to elucidate fundamental mechanisms underlying experimental observations and enable rational design of surface/interface modifications. This review examines three advancements in ab initio calculations for interfacial engineering: (1) revealing the mechanism of selective assembly and activation phenomena on surfaces, (2) theoretical predictions of interface engineering strategies, and (3) developing material databases with ionic/van der Waals components. We further address computational challenges while proposing quantum‐mechanical methods to design next‐gen materials with customized interfacial properties.