Exploring cesium-tellurium phase space via high-throughput calculations beyond semi-local density-functional theory

• Published in: The Journal of chemical physics Vol. 156; no. 10; p. 104108
• Main Authors: Saßnick, Holger-Dietrich, Cocchi, Caterina
• Format: Journal Article
• Language: English
• Published: United States 14.03.2022
• ISSN: 1089-7690
• DOI: 10.1063/5.0082710

Boosted by the relentless increase in available computational resources, high-throughput calculations based on first-principles methods have become a powerful tool to screen a huge range of materials. The backbone of these studies is well-structured and reproducible workflows efficiently returning the desired properties given chemical compositions and atomic arrangements as sole input. Herein, we present a new workflow designed to compute the stability and the electronic properties of crystalline materials from density-functional theory using the strongly constrained and appropriately normed approximation (SCAN) for the exchange-correlation potential. We show the performance of the developed tool exploring the binary Cs-Te phase space that hosts cesium telluride, a semiconducting material widely used as a photocathode in particle accelerators. Starting from a pool of structures retrieved from open computational material databases, we analyze formation energies as a function of the relative Cs content and for a few selected crystals, we investigate the band structures and density of states unraveling interconnections among the structure, stoichiometry, stability, and electronic properties. Our study contributes to the ongoing research on alkali-based photocathodes and demonstrates that high-throughput calculations based on state-of-the-art first-principles methods can complement experiments in the search for optimal materials for next-generation electron sources.