Simulation, Design, and Discovery of Complex Materials

The competition between energetically comparable phases determines whether a material can be synthesized and whether it will exhibit favorable properties under relevant operating conditions. While electronic structure theory and simulation offer exciting possibilities for accelerating the design of new materials, they often neglect phase transitions and competing secondary phases. The overarching goal of this project is to understand how defects, disorder, and long-range interactions affect functionality and stability across a material’s phase diagram. Addressing this challenge, we will examine three key specific aims involving (1) connecting phase stability to emergent material functionality in multicomponent, disordered compounds, (2) building insights into defect- and disorder-driven vibrational behaviors, and (3) harnessing van der Waals-driven couplings in multiferroic materials. We will focus on bulk, multicomponent ceramics, layered magnetic materials, and materials with unique magnetic and/or phonon couplings. Central to this effort, will be the development and application of first-principles-derived methodologies to create realistic, materials-specific, predictive models that link phase-stability and material imperfections to functionality. This combined effort will provide crucial insights into materials behavior, with direct relevance to ORNL experimental synthesis and characterization efforts. This project will allow us to develop physical and chemical rules to accelerate the materials design and discovery process.