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Alchemical screening of ionic crystals
JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift)
 
ID 3720366
Author(s) Solovyevaa, Alisa; von Lilienfeld, O. Anatole
Author(s) at UniBasel von Lilienfeld, Anatole
Year 2016
Title Alchemical screening of ionic crystals
Journal Physical Chemistry Chemical Physics
Volume 18
Number 45
Pages / Article-Number 31078-31091
Abstract We introduce alchemical perturbations as a rapid and accurate tool to estimate fundamental structural and energetic properties in pure and mixed ionic crystals. We investigated formation energies, lattice constants, and bulk moduli for all sixteen iso-valence-electron combinations of pure pristine alkali halides involving elements Me is an element of Na, K, Rb, Cs and X is an element of F, Cl, Br, I. For rock salt, zinc-blende, and cesium chloride symmetry, alchemical Hellmann-Feynman derivatives, evaluated along lattice scans of sixteen reference crystals, have been obtained for coupling to all respective 16 x 15 target crystals. Mean absolute errors (MAEs) are on par with the density functional theory level of accuracy for energies and bulk moduli. The predicted lattice constants are less accurate but reproduce qualitative trends. The reference salt NaCl affords the most accurate alchemical estimates of relative energies (MAE < 40 meV per atom). The best predictions of lattice constants are based on NaF as a reference salt (MAE < 0.5 angstrom), accounting only for qualitative trends. The best reference salt for the prediction of bulk moduli is CsCl (MAE < 0.4 x 10(11) dynes cm(-2)). The alchemical predictions distinguish competing rock salt and cesium chloride phases in binary and ternary solid mixtures with CsCl. Using pure RbI as a reference salt, they reproduce the reversal of the rock salt/cesium chloride stability trend for binary MeX1-xCsClx as well as for ternary MeX0.5-0.5x(Me`Y)(0.5-0.5x)CsClx mixtures.
Publisher Royal Society of Chemistry
ISSN/ISBN 1463-9076 ; 1463-9084
edoc-URL http://edoc.unibas.ch/53280/
Full Text on edoc Available
Digital Object Identifier DOI 10.1039/c6cp04258a
ISI-Number 000388943500024
Document type (ISI) Article
 
   

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19/04/2024