Explicit atomistic modelling of solid–solid interfaces: from construction to design

Solid–solid interfaces play a critical role in the performance of energy storage systems, catalysts, and electronic devices, yet their atomic-scale structure and behaviour remain challenging to probe experimentally. Explicit atomistic modelling provides a powerful approach for investigating interfaces by directly constructing and simulating contacting phases, enabling the calculation of interfacial energetics, electronic structure, charge transfer, stability, and transport processes. This Review summarises the methodology and applications of explicit interface modelling, including interface construction strategies, properties accessible from atomistic simulations, and recent advances enabled by machine-learned interatomic potentials that extend simulations to larger time and length scales. We also discuss how computational results can be interpreted and validated using experimental characterisation techniques, and highlight current challenges and emerging opportunities in predictive interface modelling and materials design.