Crystal structure evolution induced by the Jahn-Teller effect in mixed-valence silver fluoride Ag$_3$F$_5$

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Main Authors: Korotin, Dmitry M., Novoselov, Dmitry Y., Plotnikov, Yaroslav M., Anisimov, Vladimir I.
Format: Preprint
Published: 2024
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author Korotin, Dmitry M.
Novoselov, Dmitry Y.
Plotnikov, Yaroslav M.
Anisimov, Vladimir I.
author_facet Korotin, Dmitry M.
Novoselov, Dmitry Y.
Plotnikov, Yaroslav M.
Anisimov, Vladimir I.
contents The silver fluoride Ag$_3$F$_5$ consists structurally of square-planar units formed by four fluoride ions coordinated to a central silver ion, which possesses a partially filled $d$-subshell and the formal valence of +5/3. In this study, we demonstrate that the previously published crystal structure of Ag$_3$F$_5$ is unstable due to the Jahn-Teller effect, arising from the presence of two energetically degenerate $d_{x^2-y^2}$ states sharing a single electron hole. Through a full structural relaxation within the DFT+U framework, we identified a new crystal structure for Ag$_3$F$_5$ with reduced symmetry and an energy gain of 151~meV per formula unit relative to the published structure. In this relaxed structure, magnetic chains are formed by silver ions with an electronic hole occupying the $d_{x^2-y^2}$ orbital. These results highlight the crucial role of electron correlation effects and related structural distortions in determining the properties of such materials.
format Preprint
id arxiv_https___arxiv_org_abs_2411_07905
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Crystal structure evolution induced by the Jahn-Teller effect in mixed-valence silver fluoride Ag$_3$F$_5$
Korotin, Dmitry M.
Novoselov, Dmitry Y.
Plotnikov, Yaroslav M.
Anisimov, Vladimir I.
Strongly Correlated Electrons
The silver fluoride Ag$_3$F$_5$ consists structurally of square-planar units formed by four fluoride ions coordinated to a central silver ion, which possesses a partially filled $d$-subshell and the formal valence of +5/3. In this study, we demonstrate that the previously published crystal structure of Ag$_3$F$_5$ is unstable due to the Jahn-Teller effect, arising from the presence of two energetically degenerate $d_{x^2-y^2}$ states sharing a single electron hole. Through a full structural relaxation within the DFT+U framework, we identified a new crystal structure for Ag$_3$F$_5$ with reduced symmetry and an energy gain of 151~meV per formula unit relative to the published structure. In this relaxed structure, magnetic chains are formed by silver ions with an electronic hole occupying the $d_{x^2-y^2}$ orbital. These results highlight the crucial role of electron correlation effects and related structural distortions in determining the properties of such materials.
title Crystal structure evolution induced by the Jahn-Teller effect in mixed-valence silver fluoride Ag$_3$F$_5$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2411.07905