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

Bartel, Christopher J; Millican, Samantha L; Deml, Ann M; Rumptz, John R; Tumas, William; Weimer, Alan W; Lany, Stephan; Stevanović, Vladan et al. · Nat Commun · 2018

basic_science · Level V

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Abstract

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<sup>-1</sup> (~1 kcal mol<sup>-1</sup>) 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.