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RENiO3 Single Crystals (RE = Nd, Sm, Gd, Dy, Y, Ho, Er, Lu) Grown from Molten Salts under 2000 bar of Oxygen Gas Pressure


Klein, Yannick Maximilian; Kozłowski, Mirosław; Linden, Anthony; Lacorre, Philippe; Medarde, Marisa; Gawryluk, Dariusz Jakub (2021). RENiO3 Single Crystals (RE = Nd, Sm, Gd, Dy, Y, Ho, Er, Lu) Grown from Molten Salts under 2000 bar of Oxygen Gas Pressure. Crystal Growth & Design, 21(7):4230-4241.

Abstract

The electronic properties of transition-metal oxides with highly correlated electrons are of central importance in
modern condensed-matter physics and chemistry, both for their fundamental scientific interest and for their potential for advanced electronic applications. However, the design of materials with tailored properties has been restricted by the limited understanding of their structure−property relationships, which are particularly complex in the proximity of the regime where localized electrons become gradually mobile. RENiO3 perovskites, characterized by the presence of spontaneous metal to insulator transitions, are some of the most widely used model materials for the investigation of this region in theoretical studies. However, crucial experimental information needed to validate theoretical predictions is still lacking due to their challenging high-pressure synthesis, which has prevented to date the growth of sizable bulk single crystals with RE ≠ La, Pr, and Nd. Here we report the first successful growth of single crystals with RE = Nd, Sm, Gd, Dy, Y, Ho, Er, and Lu in sizes up to ∼75 μm, grown from molten salts in a temperature gradient under 2000 bar of oxygen gas pressure. The crystals display regular prismatic shapes with flat facets, and their crystal structures and metal−insulator and antiferromagnetic order transition temperatures are in excellent agreement with previously reported values obtained from polycrystalline samples. The availability of such crystals opens access to measurements that have hitherto been impossible to conduct. This should contribute to a better understanding of the fascinating properties of materials with highly correlated electrons and guide future efforts to engineer transition-metal oxides with tailored functional properties.

Abstract

The electronic properties of transition-metal oxides with highly correlated electrons are of central importance in
modern condensed-matter physics and chemistry, both for their fundamental scientific interest and for their potential for advanced electronic applications. However, the design of materials with tailored properties has been restricted by the limited understanding of their structure−property relationships, which are particularly complex in the proximity of the regime where localized electrons become gradually mobile. RENiO3 perovskites, characterized by the presence of spontaneous metal to insulator transitions, are some of the most widely used model materials for the investigation of this region in theoretical studies. However, crucial experimental information needed to validate theoretical predictions is still lacking due to their challenging high-pressure synthesis, which has prevented to date the growth of sizable bulk single crystals with RE ≠ La, Pr, and Nd. Here we report the first successful growth of single crystals with RE = Nd, Sm, Gd, Dy, Y, Ho, Er, and Lu in sizes up to ∼75 μm, grown from molten salts in a temperature gradient under 2000 bar of oxygen gas pressure. The crystals display regular prismatic shapes with flat facets, and their crystal structures and metal−insulator and antiferromagnetic order transition temperatures are in excellent agreement with previously reported values obtained from polycrystalline samples. The availability of such crystals opens access to measurements that have hitherto been impossible to conduct. This should contribute to a better understanding of the fascinating properties of materials with highly correlated electrons and guide future efforts to engineer transition-metal oxides with tailored functional properties.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > General Chemistry
Physical Sciences > General Materials Science
Physical Sciences > Condensed Matter Physics
Uncontrolled Keywords:General Materials Science, General Chemistry, Condensed Matter Physics
Language:English
Date:7 July 2021
Deposited On:29 Jul 2021 07:41
Last Modified:14 Jun 2024 03:38
Publisher:American Chemical Society (ACS)
ISSN:1528-7483
OA Status:Green
Publisher DOI:https://doi.org/10.1021/acs.cgd.1c00474
Project Information:
  • : FunderSNSF
  • : Grant ID51NF40-182892
  • : Project TitleNCCR MARVEL: Materials Revolution: Computational Design and Discovery of Novel Materials (phase II)
  • : FunderSNSF
  • : Grant ID461 206021_139082
  • : Project TitleR'Equip
  • Content: Accepted Version