The interfaces between solids, nanoparticles, and liquids play a fundamental role in determining the properties of materials. With an understanding of the microscopic structure of heterogeneous interfaces, researchers can predict the properties of optimal materials for many applications, including photoelectrochemical water splitting, solar cells, clean fuel production, and energy storage.

However, the properties of interfaces are seldom explicitly included in ab initio models, due to the complexity and cost of the associated calculations. With this INCITE project, researchers from the University of Chicago and the University of California, Davis, aim to tackle the characterization and control of heterogeneous interfaces at the atomic and molecular scale from a computational standpoint

The research team will use the Qbox and WEST codes, which have been optimized for Mira, to investigate the properties of interfaces present in materials of interest to solar energy conversion processes. This includes performing ab initio calculations of electronic and vibrational spectra, integrated with large-scale ab initio molecular dynamics simulations, to study realistic interfaces that can be compared directly to experimental results.

The main objective of the project is to calculate the physical properties of aqueous interfaces with solid oxides and semiconductors, and of inorganic interfaces at the nanoscale. The results can be used to interpret experiments and to optimize materials properties to improve solar energy applications, including photoeletrochemical water splitting and third-generation solar cells. This work will help establish a robust strategy to enable the comparison of ab initio data with experiments carried out at light sources, such as Argonne’s Advanced Photon Source. Ultimately, the results could lead to analysis tools for spectroscopic data that can be used by theorists and experimentalists alike.