Issue 17, 2023

Imperfections are not 0 K: free energy of point defects in crystals

Abstract

Defects determine many important properties and applications of materials, ranging from doping in semiconductors, to conductivity in mixed ionic–electronic conductors used in batteries, to active sites in catalysts. The theoretical description of defect formation in crystals has evolved substantially over the past century. Advances in supercomputing hardware, and the integration of new computational techniques such as machine learning, provide an opportunity to model longer length and time-scales than previously possible. In this Tutorial Review, we cover the description of free energies for defect formation at finite temperatures, including configurational (structural, electronic, spin) and vibrational terms. We discuss challenges in accounting for metastable defect configurations, progress such as machine learning force fields and thermodynamic integration to directly access entropic contributions, and bottlenecks in going beyond the dilute limit of defect formation. Such developments are necessary to support a new era of accurate defect predictions in computational materials chemistry.

Graphical abstract: Imperfections are not 0 K: free energy of point defects in crystals

Article information

Article type
Tutorial Review
Submitted
05 juin 2023
First published
11 août 2023
This article is Open Access
Creative Commons BY license

Chem. Soc. Rev., 2023,52, 5812-5826

Imperfections are not 0 K: free energy of point defects in crystals

I. Mosquera-Lois, S. R. Kavanagh, J. Klarbring, K. Tolborg and A. Walsh, Chem. Soc. Rev., 2023, 52, 5812 DOI: 10.1039/D3CS00432E

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