Pressure‐Induced Intersite BiM (M=Ru, Ir) Valence Transitions in Hexagonal Perovskites
Identifieur interne : 002970 ( Istex/Corpus ); précédent : 002969; suivant : 002971Pressure‐Induced Intersite BiM (M=Ru, Ir) Valence Transitions in Hexagonal Perovskites
Auteurs : Zixin Huang ; Josie E. Auckett ; Peter E. R. Blanchard ; Brendan J. Kennedy ; Wojciech Miiller ; Qingdi Zhou ; Maxim Avdeev ; Mark R. Johnson ; Mohamed Zbiri ; Gaston Garbarino ; William G. Marshall ; Qinfen Gu ; Chris D. LingSource :
- Angewandte Chemie International Edition [ 1433-7851 ] ; 2014-03-24.
Abstract
Pressure‐induced charge transfer from Bi to Ir/Ru is observed in the hexagonal perovskites Ba3+nBiM2+nO9+3n (n=0,1; M=Ir,Ru). These compounds show first‐order, circa 1 % volume contractions at room temperature above 5 GPa, which are due to the large reduction in the effective ionic radius of Bi when the 6s shell is emptied on oxidation, compared to the relatively negligible effect of reduction on the radii of Ir or Ru. They are the first such transitions involving 4d and 5d compounds, and they double the total number of cases known. Ab initio calculations suggest that magnetic interactions through very short (ca. 2.6 Å) MM bonds contribute to the finely balanced nature of their electronic states.
Url:
DOI: 10.1002/anie.201311159
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<front><div type="abstract" xml:lang="en">Pressure‐induced charge transfer from Bi to Ir/Ru is observed in the hexagonal perovskites Ba3+nBiM2+nO9+3n (n=0,1; M=Ir,Ru). These compounds show first‐order, circa 1 % volume contractions at room temperature above 5 GPa, which are due to the large reduction in the effective ionic radius of Bi when the 6s shell is emptied on oxidation, compared to the relatively negligible effect of reduction on the radii of Ir or Ru. They are the first such transitions involving 4d and 5d compounds, and they double the total number of cases known. Ab initio calculations suggest that magnetic interactions through very short (ca. 2.6 Å) MM bonds contribute to the finely balanced nature of their electronic states.</div>
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<titleGroup><title type="main" xml:lang="en">Pressure‐Induced Intersite BiM (M=Ru, Ir) Valence Transitions in Hexagonal Perovskites<link href="#nss"></link>
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<p>Pressure‐induced charge transfer from Bi to Ir/Ru is observed in the hexagonal perovskites Ba<sub>3+<i>n</i>
</sub>
BiM<sub>2+<i>n</i>
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<abstract type="graphical" xml:lang="en"><p><b>Pressure‐induced charge transfer</b>
from one element to another in three hexagonal perovskites represent the first such transitions involving 4d or 5d metals, and double the total number ever observed. Electrons can be “squeezed” from the 6s shell of Bi into the 4d or 5d shells of Ru/Ir, resulting in a 1 % volume reduction that becomes favorable above 5 GPa.<blockFixed type="graphic"><mediaResourceGroup><mediaResource alt="image" eRights="yes" copyright="WILEY-VCH" href="urn:x-wiley:14337851:media:ANIE201311159:content"></mediaResource>
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<abstract lang="en">Pressure‐induced charge transfer from Bi to Ir/Ru is observed in the hexagonal perovskites Ba3+nBiM2+nO9+3n (n=0,1; M=Ir,Ru). These compounds show first‐order, circa 1 % volume contractions at room temperature above 5 GPa, which are due to the large reduction in the effective ionic radius of Bi when the 6s shell is emptied on oxidation, compared to the relatively negligible effect of reduction on the radii of Ir or Ru. They are the first such transitions involving 4d and 5d compounds, and they double the total number of cases known. Ab initio calculations suggest that magnetic interactions through very short (ca. 2.6 Å) MM bonds contribute to the finely balanced nature of their electronic states.</abstract>
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