Crystal Growth and Phase Formation of High-Entropy Rare-Earth Aluminum Perovskites

Matheus Pianassola; Bryan C. Chakoumakos; Charles L. Melcher; Mariya Zhuravleva

doi:10.1021/acs.cgd.2c01130

Crystal Growth and Phase Formation of High-Entropy Rare-Earth Aluminum Perovskites

Matheus Pianassola, Bryan C. Chakoumakos, Charles L. Melcher, Mariya Zhuravleva

Single Crystal Diffraction

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

We demonstrate for the first time the crystal growth of high-entropy rare-earth (RE) aluminum perovskites (REAlO₃) using the micro-pulling-down method to inform future exploration of functional crystals. To determine how composition affects phase formation, we formulate equiatomic compositions containing five REs from the following list: Lu, Yb, Tm, Er, Y, Ho, Dy, Tb, Gd, Eu, Sm, Nd, Pr, Ce, La. To test whether combinations of REs with similar ionic radii may favor a single phase, compositions containing REs with consecutive or nonconsecutive ionic radius values were formulated. Powder and single-crystal X-ray diffraction indicate that crystals containing only REs with similar ionic radii that form orthorhombic single-RE REAlO₃ are a single phase. Crystals containing REs with dissimilar ionic radii or mixtures of REs that form orthorhombic, rhombohedral, and tetragonal single-RE REAlO₃ are a mixture of phases. The elemental distribution in single-phase crystals analyzed via electron probe microanalysis confirms no evidence of preferential incorporation of any of the constituent REs. The distribution and composition of secondary phases were analyzed via scanning electron microscopy and energy dispersive spectroscopy; secondary phases were seen as a small region in the center of the crystals with branching features closer to the outer surface.

Original language	English
Pages (from-to)	480-488
Number of pages	9
Journal	Crystal Growth and Design
Volume	23
Issue number	1
DOIs	https://doi.org/10.1021/acs.cgd.2c01130
State	Published - Jan 4 2023

Funding

This work was supported by the National Science Foundation (DMR 1846935). Powder XRD was performed at the Institute for Advanced Materials & Manufacturing (IAMM) Diffraction Facility, located at the University of Tennessee, Knoxville. Electron microprobe measurements were performed at the Electron Microprobe Laboratory in the Department of Earth and Planetary Sciences at the University of Tennessee, Knoxville with the assistance of Molly McCanta and Allan Patchen. A portion of this research used resources at the Spallation Neutron Source, a Department of Energy Office of Science User Facility operated by the Oak Ridge National Laboratory.

Funders	Funder number
Department of Earth and Planetary Sciences at the University of Tennessee
Institute for Advanced Materials & Manufacturing
National Science Foundation	DMR 1846935
Office of Science
Oak Ridge National Laboratory
University of Tennessee

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title = "Crystal Growth and Phase Formation of High-Entropy Rare-Earth Aluminum Perovskites",

abstract = "We demonstrate for the first time the crystal growth of high-entropy rare-earth (RE) aluminum perovskites (REAlO3) using the micro-pulling-down method to inform future exploration of functional crystals. To determine how composition affects phase formation, we formulate equiatomic compositions containing five REs from the following list: Lu, Yb, Tm, Er, Y, Ho, Dy, Tb, Gd, Eu, Sm, Nd, Pr, Ce, La. To test whether combinations of REs with similar ionic radii may favor a single phase, compositions containing REs with consecutive or nonconsecutive ionic radius values were formulated. Powder and single-crystal X-ray diffraction indicate that crystals containing only REs with similar ionic radii that form orthorhombic single-RE REAlO3 are a single phase. Crystals containing REs with dissimilar ionic radii or mixtures of REs that form orthorhombic, rhombohedral, and tetragonal single-RE REAlO3 are a mixture of phases. The elemental distribution in single-phase crystals analyzed via electron probe microanalysis confirms no evidence of preferential incorporation of any of the constituent REs. The distribution and composition of secondary phases were analyzed via scanning electron microscopy and energy dispersive spectroscopy; secondary phases were seen as a small region in the center of the crystals with branching features closer to the outer surface.",

author = "Matheus Pianassola and Chakoumakos, {Bryan C.} and Melcher, {Charles L.} and Mariya Zhuravleva",

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AB - We demonstrate for the first time the crystal growth of high-entropy rare-earth (RE) aluminum perovskites (REAlO3) using the micro-pulling-down method to inform future exploration of functional crystals. To determine how composition affects phase formation, we formulate equiatomic compositions containing five REs from the following list: Lu, Yb, Tm, Er, Y, Ho, Dy, Tb, Gd, Eu, Sm, Nd, Pr, Ce, La. To test whether combinations of REs with similar ionic radii may favor a single phase, compositions containing REs with consecutive or nonconsecutive ionic radius values were formulated. Powder and single-crystal X-ray diffraction indicate that crystals containing only REs with similar ionic radii that form orthorhombic single-RE REAlO3 are a single phase. Crystals containing REs with dissimilar ionic radii or mixtures of REs that form orthorhombic, rhombohedral, and tetragonal single-RE REAlO3 are a mixture of phases. The elemental distribution in single-phase crystals analyzed via electron probe microanalysis confirms no evidence of preferential incorporation of any of the constituent REs. The distribution and composition of secondary phases were analyzed via scanning electron microscopy and energy dispersive spectroscopy; secondary phases were seen as a small region in the center of the crystals with branching features closer to the outer surface.

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Crystal Growth and Phase Formation of High-Entropy Rare-Earth Aluminum Perovskites

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