Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry

• Published in: Nature communications Vol. 9; no. 1; pp. 4168 - 10
• Main Authors: Bartel, Christopher J., Millican, Samantha L., Deml, Ann M., Rumptz, John R., Tumas, William, Weimer, Alan W., Lany, Stephan, Stevanović, Vladan, Musgrave, Charles B., Holder, Aaron M.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 09.10.2018; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 639/301/1034; 639/705/531; Chemical reactions; Composition; Computer applications; Crystal structure; Equilibrium conditions; Gibbs energy; Humanities and Social Sciences; Inorganic compounds; materials chemistry; MATERIALS SCIENCE; multidisciplinary; Organic chemistry; Phase diagrams; Science; Science (multidisciplinary); Stability; statistics; Synthesis; Temperature; Temperature dependence; Temperature effects; theory and computation
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-018-06682-4

The Gibbs energy, G , determines the equilibrium conditions of chemical reactions and materials stability. Despite this fundamental and ubiquitous role, G has been tabulated for only a small fraction of known inorganic compounds, impeding a comprehensive perspective on the effects of temperature and composition on materials stability and synthesizability. Here, we use the SISSO (sure independence screening and sparsifying operator) approach to identify a simple and accurate descriptor to predict G for stoichiometric inorganic compounds with ~50 meV atom −1 (~1 kcal mol −1 ) resolution, and with minimal computational cost, for temperatures ranging from 300–1800 K. We then apply this descriptor to ~30,000 known materials curated from the Inorganic Crystal Structure Database (ICSD). Using the resulting predicted thermochemical data, we generate thousands of temperature-dependent phase diagrams to provide insights into the effects of temperature and composition on materials synthesizability and stability and to establish the temperature-dependent scale of metastability for inorganic compounds. Materials databases currently neglect the temperature effect on compound thermodynamics. Here the authors introduce a Gibbs energy descriptor enabling the high-throughput prediction of temperature-dependent thermodynamics across a wide range of compositions and temperatures for inorganic solids.