A workflow for identifying viable crystal structures with partially occupied sites applied to the solid electrolyte cubic Li7La3Zr2O12
A workflow for identifying viable crystal structures with partially occupied sites applied to the solid electrolyte cubic Li7La3Zr2O12
To date, experimental and theoretical works have been unable to uncover the ground-state configuration of the solid electrolyte cubic Li7La3Zr2O12(c-LLZO). Computational studies rely on an initial low-energy structure as a reference point. Here, we present a methodology for identifying energetically favorable configurations of c-LLZO for a crystallographically predicted structure. We begin by eliminating structures that involve overlapping Li atoms based on nearest neighbor counts. We further reduce the configuration space by eliminating symmetry images from all remaining structures. Then, we perform a machine learning-based energetic ordering of all remaining structures. By considering the geometrical constraints that emerge from this methodology, we determine that a large portion of previously reported structures may not be feasible or stable. The method developed here could be extended to other ion conductors. We provide a database containing all of the generated structures with the aim of improving accuracy and reproducibility in future c-LLZO research.
10257-10262
Holland, Julian
53181e22-5e9c-4e4b-b940-c63e34276c2b
Demeyere, Tom
f8ede386-230e-4329-a235-3abf78011d0e
Bhandari, Arihant
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Hanke, Felix
71211026-de4c-4ce2-96e4-a4e734578050
Milman, Victor
da6e2d9c-f740-40d5-8fc4-af6f7016bdb8
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
2023
Holland, Julian
53181e22-5e9c-4e4b-b940-c63e34276c2b
Demeyere, Tom
f8ede386-230e-4329-a235-3abf78011d0e
Bhandari, Arihant
f2f12a89-273f-4c5e-a52e-e21835aaacfc
Hanke, Felix
71211026-de4c-4ce2-96e4-a4e734578050
Milman, Victor
da6e2d9c-f740-40d5-8fc4-af6f7016bdb8
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Holland, Julian, Demeyere, Tom, Bhandari, Arihant, Hanke, Felix, Milman, Victor and Skylaris, Chris-Kriton
(2023)
A workflow for identifying viable crystal structures with partially occupied sites applied to the solid electrolyte cubic Li7La3Zr2O12.
The Journal of Physical Chemistry Letters, 14 (45), .
(doi:10.1021/acs.jpclett.3c02064).
Abstract
To date, experimental and theoretical works have been unable to uncover the ground-state configuration of the solid electrolyte cubic Li7La3Zr2O12(c-LLZO). Computational studies rely on an initial low-energy structure as a reference point. Here, we present a methodology for identifying energetically favorable configurations of c-LLZO for a crystallographically predicted structure. We begin by eliminating structures that involve overlapping Li atoms based on nearest neighbor counts. We further reduce the configuration space by eliminating symmetry images from all remaining structures. Then, we perform a machine learning-based energetic ordering of all remaining structures. By considering the geometrical constraints that emerge from this methodology, we determine that a large portion of previously reported structures may not be feasible or stable. The method developed here could be extended to other ion conductors. We provide a database containing all of the generated structures with the aim of improving accuracy and reproducibility in future c-LLZO research.
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holland-et-al-2023-a-workflow-for-identifying-viable-crystal-structures-with-partially-occupied-sites-applied-to-the
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Accepted/In Press date: 31 October 2023
e-pub ahead of print date: 8 November 2023
Published date: 2023
Additional Information:
Funding Information:
We would like to thank Davide Sarpa, Jacek Dziedzic, Benedict Saunders, and Brad Ayers for proofreading the manuscript, calculation assistance, and aesthetic choices. We also thank Dr. Johan Carlsson, Dr. Hamidreza Hajiyani, and Elizabeth Ojogbede for providing expert advice and probing questions that resulted in a stronger piece of research. We thank Dr. Samantha Kanza for their assistance with data processing. We thank Dr. Mark Light for providing guidance with terminology. We are grateful to the U.K. Materials and Molecular Modelling Hub for its computational resources, which are partially funded by EPSRC (EP/P020194/1 and EP/T022213/1). The authors acknowledge the use of the IRIDIS High Performance Computing Facility and associated support services at the University of Southampton in the completion of this work. We are grateful for computational support from the UK national high performance computing service, ARCHER2, for which access was obtained via the UKCP consortium and funded by EPSRC grant ref EP/X035891/1 and EP/X035956/1. J.H. would like to thank BIOVIA for an EPSRC iCASE Ph.D. funding. This work was also supported by the Faraday Institution (Grant FIRG059).
Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.
Identifiers
Local EPrints ID: 484344
URI: http://eprints.soton.ac.uk/id/eprint/484344
ISSN: 1948-7185
PURE UUID: 24f7c3f8-8dd5-4cfd-a953-36082b97d4b9
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Date deposited: 15 Nov 2023 18:16
Last modified: 18 Mar 2024 04:17
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Author:
Julian Holland
Author:
Tom Demeyere
Author:
Arihant Bhandari
Author:
Felix Hanke
Author:
Victor Milman
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