Single-crystal high entropy perovskite oxide epitaxial films
Abstract
Examples of single-crystal epitaxial thin films of a high entropy perovskite oxide are synthesized. Pulsed laser deposition is used to grow the configurationally disordered $$AB{\mathrm{O}}_{3}$$ perovskite $$\mathrm{Ba}(\mathrm{Z}{\mathrm{r}}_{0.2}\mathrm{S}{\mathrm{n}}_{0.2}\mathrm{T}{\mathrm{i}}_{0.2}\mathrm{H}{\mathrm{f}}_{0.2}\mathrm{N}{\mathrm{b}}_{0.2}){\mathrm{O}}_{3}$$ epitaxially on $$\mathrm{SrTi}{\mathrm{O}}_{3}$$ and MgO substrates. X-ray diffraction and scanning transmission electron microscopy demonstrate that the films are single phase with excellent crystallinity and atomically abrupt interfaces to the underlying substrates. Atomically resolved electron-energy-loss spectroscopy mapping shows a uniform and random distribution of all $B$-site cations. The ability to stabilize perovskites with this level of configurational disorder offers new possibilities for designing materials from a much broader combinatorial cation pallet while providing a fresh avenue for fundamental studies in strongly correlated quantum materials where local disorder can play a critical role in determining macroscopic properties.
- Authors:
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); ORNL Laboratory Directed Research and Development (LDRD) Program; Gordon and Betty Moore Foundation (United States)
- OSTI Identifier:
- 1457481
- Alternate Identifier(s):
- OSTI ID: 1460198
- Grant/Contract Number:
- AC05-00OR22725; GBMF4416
- Resource Type:
- Published Article
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Name: Physical Review Materials Journal Volume: 2 Journal Issue: 6; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; synthesis; thermal conductivity; perovskite; thin films; thermoreflectance; laser ablation
Citation Formats
Sharma, Yogesh, Musico, Brianna L., Gao, Xiang, Hua, Chengyun, May, Andrew F., Herklotz, Andreas, Rastogi, Ankur, Mandrus, David, Yan, Jiaqiang, Lee, Ho Nyung, Chisholm, Matthew F., Keppens, Veerle, and Ward, T. Zac. Single-crystal high entropy perovskite oxide epitaxial films. United States: N. p., 2018.
Web. doi:10.1103/PhysRevMaterials.2.060404.
Sharma, Yogesh, Musico, Brianna L., Gao, Xiang, Hua, Chengyun, May, Andrew F., Herklotz, Andreas, Rastogi, Ankur, Mandrus, David, Yan, Jiaqiang, Lee, Ho Nyung, Chisholm, Matthew F., Keppens, Veerle, & Ward, T. Zac. Single-crystal high entropy perovskite oxide epitaxial films. United States. doi:10.1103/PhysRevMaterials.2.060404.
Sharma, Yogesh, Musico, Brianna L., Gao, Xiang, Hua, Chengyun, May, Andrew F., Herklotz, Andreas, Rastogi, Ankur, Mandrus, David, Yan, Jiaqiang, Lee, Ho Nyung, Chisholm, Matthew F., Keppens, Veerle, and Ward, T. Zac. Wed .
"Single-crystal high entropy perovskite oxide epitaxial films". United States. doi:10.1103/PhysRevMaterials.2.060404.
@article{osti_1457481,
title = {Single-crystal high entropy perovskite oxide epitaxial films},
author = {Sharma, Yogesh and Musico, Brianna L. and Gao, Xiang and Hua, Chengyun and May, Andrew F. and Herklotz, Andreas and Rastogi, Ankur and Mandrus, David and Yan, Jiaqiang and Lee, Ho Nyung and Chisholm, Matthew F. and Keppens, Veerle and Ward, T. Zac},
abstractNote = {Examples of single-crystal epitaxial thin films of a high entropy perovskite oxide are synthesized. Pulsed laser deposition is used to grow the configurationally disordered $AB{\mathrm{O}}_{3}$ perovskite $\mathrm{Ba}(\mathrm{Z}{\mathrm{r}}_{0.2}\mathrm{S}{\mathrm{n}}_{0.2}\mathrm{T}{\mathrm{i}}_{0.2}\mathrm{H}{\mathrm{f}}_{0.2}\mathrm{N}{\mathrm{b}}_{0.2}){\mathrm{O}}_{3}$ epitaxially on $\mathrm{SrTi}{\mathrm{O}}_{3}$ and MgO substrates. X-ray diffraction and scanning transmission electron microscopy demonstrate that the films are single phase with excellent crystallinity and atomically abrupt interfaces to the underlying substrates. Atomically resolved electron-energy-loss spectroscopy mapping shows a uniform and random distribution of all $B$-site cations. The ability to stabilize perovskites with this level of configurational disorder offers new possibilities for designing materials from a much broader combinatorial cation pallet while providing a fresh avenue for fundamental studies in strongly correlated quantum materials where local disorder can play a critical role in determining macroscopic properties.},
doi = {10.1103/PhysRevMaterials.2.060404},
journal = {Physical Review Materials},
number = 6,
volume = 2,
place = {United States},
year = {2018},
month = {6}
}
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1103/PhysRevMaterials.2.060404
DOI: 10.1103/PhysRevMaterials.2.060404
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 14 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Thin film substrates from the Raman spectroscopy point of view: Thin film substrates-Raman spectroscopy point of view
journal, April 2014
- Gasparov, L.; Jegorel, T.; Loetgering, L.
- Journal of Raman Spectroscopy, Vol. 45, Issue 6
Tetrahedron-tiling method for crystal structure prediction
journal, July 2017
- Hong, Qi-Jun; Yasi, Joseph; van de Walle, Axel
- Physical Review Materials, Vol. 1, Issue 2
Predictions of new perovskite compounds by combining machine learning and density functional theory
journal, April 2018
- Balachandran, Prasanna V.; Emery, Antoine A.; Gubernatis, James E.
- Physical Review Materials, Vol. 2, Issue 4
Giant Enhancement of Exchange Coupling in Entropy-Stabilized Oxide Heterostructures
journal, October 2017
- Meisenheimer, P. B.; Kratofil, T. J.; Heron, J. T.
- Scientific Reports, Vol. 7, Issue 1
Synthesis and microstructure of the (Co,Cr,Fe,Mn,Ni) 3 O 4 high entropy oxide characterized by spinel structure
journal, April 2018
- Dąbrowa, Juliusz; Stygar, Mirosław; Mikuła, Andrzej
- Materials Letters, Vol. 216
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976
- Shannon, R. D.
- Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767
Perovskite Oxides: Preparation, Characterizations, and Applications in Heterogeneous Catalysis
journal, August 2014
- Zhu, Junjiang; Li, Hailong; Zhong, Linyun
- ACS Catalysis, Vol. 4, Issue 9
Chemical ordering suppresses large-scale electronic phase separation in doped manganites
journal, April 2016
- Zhu, Yinyan; Du, Kai; Niu, Jiebin
- Nature Communications, Vol. 7, Issue 1
Temperature Dependence of the Raman Spectrum of BaTi
journal, October 1965
- Perry, C. H.; Hall, D. B.
- Physical Review Letters, Vol. 15, Issue 17
Quantum Critical Behavior in a Concentrated Ternary Solid Solution
journal, May 2016
- Sales, Brian C.; Jin, Ke; Bei, Hongbin
- Scientific Reports, Vol. 6, Issue 1
Local structure of the Mg x Ni x Co x Cu x Zn x O( x =0.2) entropy-stabilized oxide: An EXAFS study
journal, April 2017
- Rost, Christina M.; Rak, Zsolt; Brenner, Donald W.
- Journal of the American Ceramic Society, Vol. 100, Issue 6
Analysis of heat flow in layered structures for time-domain thermoreflectance
journal, December 2004
- Cahill, David G.
- Review of Scientific Instruments, Vol. 75, Issue 12
Room temperature lithium superionic conductivity in high entropy oxides
journal, January 2016
- Bérardan, D.; Franger, S.; Meena, A. K.
- Journal of Materials Chemistry A, Vol. 4, Issue 24
A ferroelectric quantum phase transition inside the superconducting dome of Sr1−xCaxTiO3−δ
journal, April 2017
- Rischau, Carl Willem; Lin, Xiao; Grams, Christoph P.
- Nature Physics, Vol. 13, Issue 7
Topological crystalline metal in orthorhombic perovskite iridates
journal, March 2015
- Chen, Yige; Lu, Yuan-Ming; Kee, Hae-Young
- Nature Communications, Vol. 6, Issue 1
Pulse accumulation, radial heat conduction, and anisotropic thermal conductivity in pump-probe transient thermoreflectance
journal, November 2008
- Schmidt, Aaron J.; Chen, Xiaoyuan; Chen, Gang
- Review of Scientific Instruments, Vol. 79, Issue 11
Lower limit to the thermal conductivity of disordered crystals
journal, September 1992
- Cahill, David G.; Watson, S. K.; Pohl, R. O.
- Physical Review B, Vol. 46, Issue 10, p. 6131-6140
Strain Doping: Reversible Single-Axis Control of a Complex Oxide Lattice via Helium Implantation
journal, June 2015
- Guo, Hangwen; Dong, Shuai; Rack, Philip D.
- Physical Review Letters, Vol. 114, Issue 25
Perovskite oxides – a review on a versatile material class for solar-to-fuel conversion processes
journal, January 2017
- Kubicek, Markus; Bork, Alexander H.; Rupp, Jennifer L. M.
- Journal of Materials Chemistry A, Vol. 5, Issue 24
Origin of ferroelectricity in perovskite oxides
journal, July 1992
- Cohen, Ronald E.
- Nature, Vol. 358, Issue 6382
Multiferroic crossover in perovskite oxides
journal, April 2016
- Weston, L.; Cui, X. Y.; Ringer, S. P.
- Physical Review B, Vol. 93, Issue 16
Abnormal Poisson's ratio and Linear Compressibility in Perovskite Materials
journal, May 2012
- Huang, C. W.; Ren, Wei; Nguyen, Viet Cuong
- Advanced Materials, Vol. 24, Issue 30
Thermal conductivity of perovskite ferroelectrics
journal, September 2008
- Tachibana, Makoto; Kolodiazhnyi, Taras; Takayama-Muromachi, Eiji
- Applied Physics Letters, Vol. 93, Issue 9
Restoration of quantum critical behavior by disorder in pressure-tuned (Mn,Fe)Si
journal, August 2017
- Goko, Tatsuo; Arguello, Carlos J.; Hamann, Andreas
- npj Quantum Materials, Vol. 2, Issue 1
Thermal conductance of epitaxial interfaces
journal, February 2003
- Costescu, Ruxandra M.; Wall, Marcel A.; Cahill, David G.
- Physical Review B, Vol. 67, Issue 5
Effects of chemical and hydrostatic pressures on structural, magnetic, and electronic properties of double perovskites
journal, November 2014
- Zhao, Hong Jian; Liu, Xiao Qiang; Chen, Xiang Ming
- Physical Review B, Vol. 90, Issue 19
Magnetic Oxide Heterostructures
journal, July 2014
- Bhattacharya, Anand; May, Steven J.
- Annual Review of Materials Research, Vol. 44, Issue 1
Origin of morphotropic phase boundaries in ferroelectrics
journal, January 2008
- Ahart, Muhtar; Somayazulu, Maddury; Cohen, R. E.
- Nature, Vol. 451, Issue 7178
Entropy-stabilized oxides
journal, September 2015
- Rost, Christina M.; Sachet, Edward; Borman, Trent
- Nature Communications, Vol. 6, Issue 1
Colossal magnetoresistant materials: the key role of phase separation
journal, April 2001
- Dagotto, Elbio; Hotta, Takashi; Moreo, Adriana
- Physics Reports, Vol. 344, Issue 1-3
Experimental metrology to obtain thermal phonon transmission coefficients at solid interfaces
journal, May 2017
- Hua, Chengyun; Chen, Xiangwen; Ravichandran, Navaneetha K.
- Physical Review B, Vol. 95, Issue 20
Structural, magnetic, and electrical properties of single-crystalline
journal, September 2002
- Hemberger, J.; Krimmel, A.; Kurz, T.
- Physical Review B, Vol. 66, Issue 9
Controlled Jahn-Teller distortion in (MgCoNiCuZn)O-based high entropy oxides
journal, May 2017
- Berardan, D.; Meena, A. K.; Franger, S.
- Journal of Alloys and Compounds, Vol. 704
Percolative phase separation underlies colossal magnetoresistance in mixed-valent manganites
journal, June 1999
- Uehara, M.; Mori, S.; Chen, C. H.
- Nature, Vol. 399, Issue 6736
Phase stability and distortion in high-entropy oxides
journal, March 2018
- Anand, G.; Wynn, Alex P.; Handley, Christopher M.
- Acta Materialia, Vol. 146
Micro-Raman scattering and dielectric investigations of phase transition behavior in the BaTiO3–BaZrO3 system
journal, June 2001
- Dobal, P. S.; Dixit, A.; Katiyar, R. S.
- Journal of Applied Physics, Vol. 89, Issue 12
Rare earth and transition metal based entropy stabilised perovskite type oxides
journal, May 2018
- Sarkar, Abhishek; Djenadic, Ruzica; Wang, Di
- Journal of the European Ceramic Society, Vol. 38, Issue 5
A critical review of high entropy alloys and related concepts
journal, January 2017
- Miracle, D. B.; Senkov, O. N.
- Acta Materialia, Vol. 122
Ultrastable metal oxide nanotube arrays achieved by entropy-stabilization engineering
journal, March 2018
- Lei, Zhifeng; Liu, Xiongjun; Li, Rui
- Scripta Materialia, Vol. 146
A new class of high-entropy perovskite oxides
journal, January 2018
- Jiang, Sicong; Hu, Tao; Gild, Joshua
- Scripta Materialia, Vol. 142
Magnetic properties of tuned by the site-selected charge doping, oxygen disorder, and hydrostatic pressure
journal, November 2017
- Pietosa, J.; Kolesnik, S.; Puzniak, R.
- Physical Review Materials, Vol. 1, Issue 6
Perovskite-type oxides—The new approach to high- superconductivity
journal, July 1988
- Bednorz, J. Georg; Müller, K. Alex
- Reviews of Modern Physics, Vol. 60, Issue 3
Studies on the relaxor behavior of sol-gel derived Ba(Zr x Ti1− x )O3 (0.30≤x≤0.70) thin films
journal, January 2006
- Dixit, A.; Majumder, S. B.; Katiyar, R. S.
- Journal of Materials Science, Vol. 41, Issue 1
Soft modes and local structural transitions in Pb-free Ba(Ti0.8Zr0.2)O3-x (Ba0.7Ca0.3)TiO3 (x = 0.5): Pressure- and temperature-dependent Raman studies
journal, March 2013
- Seo, Yu-Seong; Ahn, Jai Seok; Jeong, Il-Kyoung
- Journal of the Korean Physical Society, Vol. 62, Issue 5
Improper electric polarization in simple perovskite oxides with two magnetic sublattices
journal, January 2017
- Zhao, Hong Jian; Bellaiche, L.; Chen, Xiang Ming
- Nature Communications, Vol. 8, Issue 1
Ultrasonic Velocities in BaTiO 3
journal, April 1973
- Kashida, Shoji; Hatta, Ichiro; Ikushima, Akira
- Journal of the Physical Society of Japan, Vol. 34, Issue 4
On the minimum limit to thermal conductivity of multi-atom component crystalline solid solutions based on impurity mass scattering
journal, September 2017
- Giri, Ashutosh; Braun, Jeffrey L.; Rost, Christina M.
- Scripta Materialia, Vol. 138
Nanocrystalline multicomponent entropy stabilised transition metal oxides
journal, February 2017
- Sarkar, Abhishek; Djenadic, Ruzica; Usharani, Nandhini J.
- Journal of the European Ceramic Society, Vol. 37, Issue 2