Heterogeneous interfaces between solids, nanoparticles, and liquids play a fundamental role in determining the properties of materials. With an understanding of the microscopic structure of solid-water and solid-electrolyte interfaces, researchers can better predict the properties of optimal materials for applications, such as water splitting, the production of clean fuels, 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 multiyear INCITE project, researchers are developing accurate and efficient computational methods to study the interfaces present in realistic materials. The team has optimized the Qbox and WEST codes for Mira to enable calculations of opto-electronic (e.g.,photoemission and absorption) and vibrational spectra (e.g., sum frequency generation) integrated with large-scale ab initio molecular dynamics simulations. This capability, combined with the petascale power of Mira, provides a practical time-to-solution for identifying vibrational signatures of specific reaction pathways that occur at interfaces and for sampling many configurations from Qbox for input to many-body GW calculations with WEST.

The team’s open-source computational protocols will enable accurate calculations of the electronic properties of electrolyte solutions and interfaces important to energy-related applications. Theorists and experimentalists alike can use analysis tools derived from the calculations to interpret experiments and to optimize materials properties to improve clean fuel production and solar energy applications. In addition, the 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.