| Authors: | Asif Iqbal Bhatti, Sandeep Kumar, Catharina Jaeken, Michael Sluydts, Danny E.P. Vanpoucke, and Stefaan Cottenier |
| Journal: | Journal of Materials Chemistry A 13, 526-539 (2025) |
| doi: | 10.1039/D4TA06603K |
| IF(2024): | 10.7 |
| export: | bibtex |
| pdf: | <J.Mat.Chem.A> |
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| Graphical Abstract: Schematic representation of the LPS material and the variation of results obtained due to slight changes in settings within a High Throughput workflow. |
Abstract
High-throughput computational screening has become a powerful tool in materials science for identifying promising candidates for specific applications. However, the effectiveness of these methods relies heavily on the accuracy and appropriateness of the underlying models and assumptions. In this study, we use the popular argyrodite solid-state electrolyte family Li6PS5X (X = Cl, Br, I) as a case study to critically examine key steps in high-throughput workflows and highlight potential pitfalls. We demonstrate some of these pitfalls by highlighting the importance of careful structural considerations, including symmetry breaking and site disorder, and examine the difference between 0 K thermodynamic stability and finite-temperature stability based on temperature-dependent Gibbs free energy calculations. Furthermore, we explore the implications of these findings for the ranking of candidate materials in a mini-throughput study in a search space of isovalent analogs to Li6PS5Cl. As a result of these findings, our work underscores the need for balanced trade-offs between computational efficiency and accuracy in high-throughput screenings, and offers guidance for designing more robust workflows that can better bridge the gap between computational predictions and experimental realities.