Disordered enthalpy-entropy descriptor for high-entropy ceramics discovery

Simon Divilov; Hagen Eckert; David Hicks; Corey Oses; Cormac Toher; Rico Friedrich; Marco Esters; Michael J Mehl; Adam C Zettel; Yoav Lederer; Eva Zurek; Jon-Paul Maria; Donald W Brenner; Xiomara Campilongo; Suzana Filipović; William G Fahrenholtz; Caillin J Ryan; Christopher M DeSalle; Ryan J Crealese; Douglas E Wolfe; Arrigo Calzolari; Stefano Curtarolo

doi:10.1038/s41586-023-06786-y

Disordered enthalpy-entropy descriptor for high-entropy ceramics discovery

Nature. 2024 Jan;625(7993):66-73. doi: 10.1038/s41586-023-06786-y. Epub 2024 Jan 3.

Authors

Simon Divilov^#^{1

2}, Hagen Eckert^#^{1

2}, David Hicks^#^{1

2}, Corey Oses^#^{1

2}, Cormac Toher^#^{2

3}, Rico Friedrich^{2

4

5}, Marco Esters^{1

2}, Michael J Mehl^{1

2}, Adam C Zettel^{1

2}, Yoav Lederer^{2

6}, Eva Zurek⁷, Jon-Paul Maria⁸, Donald W Brenner⁹, Xiomara Campilongo², Suzana Filipović^{10

11}, William G Fahrenholtz¹⁰, Caillin J Ryan¹², Christopher M DeSalle¹², Ryan J Crealese¹², Douglas E Wolfe¹², Arrigo Calzolari^{1

2

13}, Stefano Curtarolo^{14

15}

Affiliations

¹ Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC, USA.
² Center for Autonomous Materials Design, Duke University, Durham, NC, USA.
³ Department of Materials Science and Engineering and Department of Chemistry and Biochemistry, The University of Texas at Dallas, Richardson, TX, USA.
⁴ Institute of Ion Beam Physics and Materials Research, Helmholtz-Zentrum Dresden-Rossendorf, Dresden, Germany.
⁵ Theoretical Chemistry, Technical University of Dresden, Dresden, Germany.
⁶ Department of Physics, NRCN, Beer-Sheva, Israel.
⁷ Department of Chemistry, State University of New York at Buffalo, Buffalo, NY, USA.
⁸ Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, USA.
⁹ Department of Materials Science and Engineering, North Carolina State University, Raleigh, NC, USA.
¹⁰ Department of Materials Science and Engineering, Missouri University of Science and Technology, Rolla, MO, USA.
¹¹ Institute of Technical Sciences of the Serbian Academy of Sciences and Arts, Belgrade, Serbia.
¹² Applied Research Laboratory, The Pennsylvania State University, University Park, PA, USA.
¹³ CNR-NANO Research Center S3, Modena, Italy.
¹⁴ Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC, USA. stefano@duke.edu.
¹⁵ Center for Autonomous Materials Design, Duke University, Durham, NC, USA. stefano@duke.edu.

^# Contributed equally.

Abstract

The need for improved functionalities in extreme environments is fuelling interest in high-entropy ceramics^1-3. Except for the computational discovery of high-entropy carbides, performed with the entropy-forming-ability descriptor⁴, most innovation has been slowly driven by experimental means^1-3. Hence, advancement in the field needs more theoretical contributions. Here we introduce disordered enthalpy-entropy descriptor (DEED), a descriptor that captures the balance between entropy gains and enthalpy costs, allowing the correct classification of functional synthesizability of multicomponent ceramics, regardless of chemistry and structure. To make our calculations possible, we have developed a convolutional algorithm that drastically reduces computational resources. Moreover, DEED guides the experimental discovery of new single-phase high-entropy carbonitrides and borides. This work, integrated into the AFLOW computational ecosystem, provides an array of potential new candidates, ripe for experimental discoveries.