Scale-invariant machine-learning model accelerates the discovery of quaternary chalcogenides with ultralow lattice thermal conductivity

Koushik Pal*, Cheol Woo Park, Yi Xia, Jiahong Shen, Chris Wolverton

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

We design an advanced machine-learning (ML) model based on crystal graph convolutional neural network that is insensitive to volumes (i.e., scale) of the input crystal structures to discover novel quaternary chalcogenides, AMM′Q3 (A/M/M' = alkali, alkaline earth, post-transition metals, lanthanides, and Q = chalcogens). These compounds are shown to possess ultralow lattice thermal conductivity (κl), a desired requirement for thermal-barrier coatings and thermoelectrics. Upon screening the thermodynamic stability of ~1 million compounds using the ML model iteratively and performing density-functional theory (DFT) calculations for a small fraction of compounds, we discover 99 compounds that are validated to be stable in DFT. Taking several DFT-stable compounds, we calculate their κl using Peierls–Boltzmann transport equation, which reveals ultralow κl (<2 Wm−1K−1 at room temperature) due to their soft elasticity and strong phonon anharmonicity. Our work demonstrates the high efficiency of scale-invariant ML model in predicting novel compounds and presents experimental-research opportunities with these new compounds.

Original languageEnglish (US)
Article number48
Journalnpj Computational Materials
Volume8
Issue number1
DOIs
StatePublished - Dec 2022

ASJC Scopus subject areas

  • Modeling and Simulation
  • Materials Science(all)
  • Mechanics of Materials
  • Computer Science Applications

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