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Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates

The lacunar-spinel chalcogenides exhibit magnetic centers in the form of transition-metal tetrahedra. On the basis of density-functional computations, the electronic ground state of an Mo(4)(13+) tetrahedron has been postulated as single-configuration a(1)(2) e(4) t(2)(5), where a(1), e, and t(2) ar...

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Autores principales: Petersen, Thorben, Prodan, Lilian, Geirhos, Korbinian, Nakamura, Hiroyuki, Kézsmárki, István, Hozoi, Liviu
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9918447/
https://www.ncbi.nlm.nih.gov/pubmed/36765082
http://dx.doi.org/10.1038/s41598-023-28656-3
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author Petersen, Thorben
Prodan, Lilian
Geirhos, Korbinian
Nakamura, Hiroyuki
Kézsmárki, István
Hozoi, Liviu
author_facet Petersen, Thorben
Prodan, Lilian
Geirhos, Korbinian
Nakamura, Hiroyuki
Kézsmárki, István
Hozoi, Liviu
author_sort Petersen, Thorben
collection PubMed
description The lacunar-spinel chalcogenides exhibit magnetic centers in the form of transition-metal tetrahedra. On the basis of density-functional computations, the electronic ground state of an Mo(4)(13+) tetrahedron has been postulated as single-configuration a(1)(2) e(4) t(2)(5), where a(1), e, and t(2) are symmetry-adapted linear combinations of single-site Mo t(2g) atomic orbitals. Here we unveil the many-body tetramer wave-function: we show that sizable correlations yield a weight of only 62% for the a(1)(2) e(4) t(2)(5) configuration. While spin–orbit coupling within the peculiar valence orbital manifold is still effective, the expectation value of the spin–orbit operator and the g factors deviate from figures describing nominal t(5) j(eff) = 1/2 moments. As such, our data documents the dressing of a spin–orbit j(eff) = 1/2 object with intra-tetramer excitations. Our results on the internal degrees of freedom of these magnetic moments provide a solid theoretical starting point in addressing the intriguing phase transitions observed at low temperatures in these materials.
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spelling pubmed-99184472023-02-12 Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates Petersen, Thorben Prodan, Lilian Geirhos, Korbinian Nakamura, Hiroyuki Kézsmárki, István Hozoi, Liviu Sci Rep Article The lacunar-spinel chalcogenides exhibit magnetic centers in the form of transition-metal tetrahedra. On the basis of density-functional computations, the electronic ground state of an Mo(4)(13+) tetrahedron has been postulated as single-configuration a(1)(2) e(4) t(2)(5), where a(1), e, and t(2) are symmetry-adapted linear combinations of single-site Mo t(2g) atomic orbitals. Here we unveil the many-body tetramer wave-function: we show that sizable correlations yield a weight of only 62% for the a(1)(2) e(4) t(2)(5) configuration. While spin–orbit coupling within the peculiar valence orbital manifold is still effective, the expectation value of the spin–orbit operator and the g factors deviate from figures describing nominal t(5) j(eff) = 1/2 moments. As such, our data documents the dressing of a spin–orbit j(eff) = 1/2 object with intra-tetramer excitations. Our results on the internal degrees of freedom of these magnetic moments provide a solid theoretical starting point in addressing the intriguing phase transitions observed at low temperatures in these materials. Nature Publishing Group UK 2023-02-10 /pmc/articles/PMC9918447/ /pubmed/36765082 http://dx.doi.org/10.1038/s41598-023-28656-3 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Petersen, Thorben
Prodan, Lilian
Geirhos, Korbinian
Nakamura, Hiroyuki
Kézsmárki, István
Hozoi, Liviu
Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
title Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
title_full Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
title_fullStr Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
title_full_unstemmed Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
title_short Dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
title_sort dressed j(eff)-1/2 objects in mixed-valence lacunar spinel molybdates
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9918447/
https://www.ncbi.nlm.nih.gov/pubmed/36765082
http://dx.doi.org/10.1038/s41598-023-28656-3
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