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Upper-Bound Energy Minimization to Search for Stable Functional Materials with Graph Neural Networks

Jeffrey Law, Shubham Pandey, Prashun Gorai, Peter C. St. John

2022JACS Au25 citationsDOIOpen Access PDF

Abstract

, this upper bound energy can be quickly and accurately predicted with a scale-invariant graph neural network (GNN). We generate new structures via ionic substitution of known prototypes, and train our GNN on a new database of 128 000 DFT calculations comprising both fully relaxed and volume-only relaxed structures. By minimizing the predicted upper-bound energy, we discover new stable structures with over 99% accuracy (versus DFT). We demonstrate the method by finding promising new candidates for solid-state battery (SSB) electrolytes that not only possess the required stability, but also additional functional properties such as large electrochemical stability windows and high conduction ion fraction. We expect this proposed framework to be directly applicable to a wide range of design challenges in materials science.

Topics & Concepts

Density functional theoryUpper and lower boundsStability (learning theory)Computer scienceEnergy minimizationInvariant (physics)MinificationA priori and a posterioriEnergy functionalGraph theoryChemical stabilityComputational chemistryChemistryMathematicsPhysicsThermodynamicsMachine learningQuantum mechanicsCombinatoricsMathematical analysisEpistemologyPhilosophyProgramming languageMachine Learning in Materials ScienceFuel Cells and Related MaterialsElectrocatalysts for Energy Conversion
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