Formation of Pyrophosphates across Grain Boundaries Induces the Formation of Mismatched but Oriented Interfaces in Silver Phosphate Polypods

Abstract Interfaces and their misfit defects determine the material properties of a wide range of applications, such as electronic devices, photocatalysts, and structural materials. However, current atomic-level understanding of interfacial structures is limited. Here we reveal that a special interfacial structure, a mismatched but oriented interface formed by two differently structured facets, gives rise to Ag3PO4 polypods at room temperature in aqueous solution. Transmission and scanning electron microscopy results suggest that interfaces of {100} and {110}({100}/(110}), {100}/{111}, {110}/{111}, and {100}/{100} have certain orientation relationships, corresponding to the energy minima and coincident site lattices of interfacial atoms, as demonstrated by molecular dynamics simulations. Density functional theory calculations indicates that the formation of pyrophosphate and/or phosphates rotation across the interface, as well as deformation of Ag-O bonds, compensates for the lattice mismatch at the interfaces. Our work opens a new avenue for a much wider range of interfacial structures, allows for a higher diversity of structures, and shines light on tailoring crystal structures, morphologies, and their resulting properties.