Building Thermodynamic Models for Accelerated Materials Realization

Abstract: New materials with better functional properties are the building blocks of interdisciplinary energy, health, and electronics solutions. However, experimental realization of new materials remains a complex challenge due to syntheses with multiple tuning parameters. Leveraging computation to understand the experimental environment, particularly through thermodynamic phase diagrams sourced from first principles density functional theory (DFT) calculations, has emerged as a promising optimization device. Here, we show how to use aqueous electrochemical phase diagrams (Pourbaix diagrams) to understand traditional corrosion applications, as well as the hydrothermal synthesis of thermoelectric bismuth oxychalcogenides. Diagrams constructed with multiple degrees-of-freedom, including multiple nonstandard states, aqueous complexes, and solid compounds, describe system evolution as functions of pH, reagent concentration, and solution potential. Further, we revisit Pourbaix diagram construction to introduce a new, high-throughput descriptor of aqueous ion formation: the maximum driving force (MDF). Finally, we will introduce the ALab, an autonomous solid-state laboratory whose work on new materials discovery, synthesis science, and automated characterization analysis is revolutionizing the field of synthesis science. Together, these topics underscore the process and capabilities of thermodynamic models as integral tools to accelerate and rationalize materials discovery.

Bio: Lauren Walters is a postdoctoral scholar in Gerbrand Ceder’s group at Lawrence Berkeley National Laboratory. She graduated with her BS and MS in polymer science and engineering from Case Western Reserve University in 2017, and her PhD from Northwestern University in 2022. She previously worked in the Materials Theory and Design group under the mentorship of James Rondinelli on computational structure-property relationships, materials discovery for metal-insulator transition materials, and thermodynamic models for corrosion science and hydrothermal synthesis. Her current research focuses on accelerating new materials discovery via thermodynamic models. Her work has been shared in a number of different peer reviewed journals and conferences, resulting in awards such as the MRS Graduate Student Silver award and the Weertman Doctoral Fellowship. Teaching and mentorship constitute a core part of Lauren’s work as a scientist; she has completed four teaching assistantships, won TA of the year awards, earned a SEARLE Center Teaching Program certificate, and is eagerly awaiting the start of her fifth undergraduate researcher to work under her guidance starting in summer 2024