Epitaxial stabilization of ultra thin films of high entropy perovskite
Abstract
High entropy oxides (HEOs) are a class of materials, containing equimolar portions of five or more transition metal and/or rare-earth elements. We report here about the layer-by-layer growth of HEO [(La0.2Pr0.2Nd0.2Sm0.2Eu0.2)NiO3] thin films on NdGaO3 substrates by pulsed laser deposition. The combined characterizations with in situ reflection high energy electron diffraction, atomic force microscopy, and x-ray diffraction affirm the single crystalline nature of the film with smooth surface morphology. The desired +3 oxidation of Ni has been confirmed by an element sensitive x-ray absorption spectroscopy measurement. Temperature dependent electrical transport measurements revealed a first order metal-insulator transition with the transition temperature very similar to the undoped NdNiO3. Furthermore, since both these systems have a comparable tolerance factor, this work demonstrates that the electronic behaviors of A-site disordered perovskite-HEOs are primarily controlled by the average tolerance factor.
- Authors:
-
- Indian Inst. of Science, Bengaluru (India)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Office of Basic Energy Sciences (BES). Scientific User Facilities Division; Government of India, Department of Science and Technology; USDOE
- OSTI Identifier:
- 1761513
- Alternate Identifier(s):
- OSTI ID: 1600046
- Grant/Contract Number:
- AC02-06CH11357; DST/NM/NS/2018/246; SR/NM/Z-07/2015
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Physics Letters
- Additional Journal Information:
- Journal Volume: 116; Journal Issue: 7; Journal ID: ISSN 0003-6951
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Atomic force microscopy; electron diffraction; epitaxy; thin films; x-ray absorption spectroscopy; phase transitions; perovskites; x-ray diffraction; entropy; pulsed laser deposition
Citation Formats
Patel, Ranjan Kumar, Ojha, Shashank Kumar, Kumar, Siddharth, Saha, Akash, Mandal, Prithwijit, Freeland, J. W., and Middey, S. Epitaxial stabilization of ultra thin films of high entropy perovskite. United States: N. p., 2020.
Web. doi:10.1063/1.5133710.
Patel, Ranjan Kumar, Ojha, Shashank Kumar, Kumar, Siddharth, Saha, Akash, Mandal, Prithwijit, Freeland, J. W., & Middey, S. Epitaxial stabilization of ultra thin films of high entropy perovskite. United States. https://doi.org/10.1063/1.5133710
Patel, Ranjan Kumar, Ojha, Shashank Kumar, Kumar, Siddharth, Saha, Akash, Mandal, Prithwijit, Freeland, J. W., and Middey, S. Tue .
"Epitaxial stabilization of ultra thin films of high entropy perovskite". United States. https://doi.org/10.1063/1.5133710. https://www.osti.gov/servlets/purl/1761513.
@article{osti_1761513,
title = {Epitaxial stabilization of ultra thin films of high entropy perovskite},
author = {Patel, Ranjan Kumar and Ojha, Shashank Kumar and Kumar, Siddharth and Saha, Akash and Mandal, Prithwijit and Freeland, J. W. and Middey, S.},
abstractNote = {High entropy oxides (HEOs) are a class of materials, containing equimolar portions of five or more transition metal and/or rare-earth elements. We report here about the layer-by-layer growth of HEO [(La0.2Pr0.2Nd0.2Sm0.2Eu0.2)NiO3] thin films on NdGaO3 substrates by pulsed laser deposition. The combined characterizations with in situ reflection high energy electron diffraction, atomic force microscopy, and x-ray diffraction affirm the single crystalline nature of the film with smooth surface morphology. The desired +3 oxidation of Ni has been confirmed by an element sensitive x-ray absorption spectroscopy measurement. Temperature dependent electrical transport measurements revealed a first order metal-insulator transition with the transition temperature very similar to the undoped NdNiO3. Furthermore, since both these systems have a comparable tolerance factor, this work demonstrates that the electronic behaviors of A-site disordered perovskite-HEOs are primarily controlled by the average tolerance factor.},
doi = {10.1063/1.5133710},
journal = {Applied Physics Letters},
number = 7,
volume = 116,
place = {United States},
year = {Tue Feb 18 00:00:00 EST 2020},
month = {Tue Feb 18 00:00:00 EST 2020}
}
Web of Science
Works referenced in this record:
Transition from Curie-Weiss to enhanced Pauli paramagnetism in
journal, January 2003
- Zhou, J. -S.; Goodenough, J. B.; Dabrowski, B.
- Physical Review B, Vol. 67, Issue 2
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
Phase engineering of rare earth nickelates by digital synthesis
journal, August 2018
- Middey, S.; Meyers, D.; Kumar Patel, Ranjan
- Applied Physics Letters, Vol. 113, Issue 8
Pure electronic metal-insulator transition at the interface of complex oxides
journal, June 2016
- Meyers, D.; Liu, Jian; Freeland, J. W.
- Scientific Reports, Vol. 6, Issue 1
Multicomponent equiatomic rare earth oxides
journal, August 2016
- Djenadic, Ruzica; Sarkar, Abhishek; Clemens, Oliver
- Materials Research Letters, Vol. 5, Issue 2
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
Structural, magnetic and electronic properties of perovskites (R = rare earth)
journal, February 1997
- Medarde, María Luisa
- Journal of Physics: Condensed Matter, Vol. 9, Issue 8
Physics of Ultrathin Films and Heterostructures of Rare-Earth Nickelates
journal, July 2016
- Middey, S.; Chakhalian, J.; Mahadevan, P.
- Annual Review of Materials Research, Vol. 46, Issue 1
Heterointerface engineered electronic and magnetic phases of NdNiO3 thin films
journal, November 2013
- Liu, Jian; Kargarian, Mehdi; Kareev, Mikhail
- Nature Communications, Vol. 4, Issue 1
Strongly correlated oxides for energy harvesting
journal, August 2018
- Matsuno, Jobu; Fujioka, Jun; Okuda, Tetsuji
- Science and Technology of Advanced Materials, Vol. 19, 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
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
Novel Electronic Behavior Driving Metal-Insulator Transition
journal, July 2015
- Upton, M. H.; Choi, Yongseong; Park, Hyowon
- Physical Review Letters, Vol. 115, Issue 3
Neutron-diffraction study of the magnetic ordering in the insulating regime of the perovskites R ( R =Pr and Nd)
journal, July 1994
- García-Muñoz, J. L.; Rodríguez-Carvajal, J.; Lacorre, P.
- Physical Review B, Vol. 50, Issue 2
High entropy oxides for reversible energy storage
journal, August 2018
- Sarkar, Abhishek; Velasco, Leonardo; Wang, Di
- Nature Communications, Vol. 9, Issue 1
Coexisting first- and second-order electronic phase transitions in a correlated oxide
journal, July 2018
- Post, K. W.; McLeod, A. S.; Hepting, M.
- Nature Physics, Vol. 14, Issue 10
Tuning bad metal and non-Fermi liquid behavior in a Mott material: Rare-earth nickelate thin films
journal, November 2015
- Mikheev, Evgeny; Hauser, Adam J.; Himmetoglu, Burak
- Science Advances, Vol. 1, Issue 10
Atomic-scale control of competing electronic phases in ultrathin LaNiO3
journal, April 2014
- King, P. D. C.; Wei, H. I.; Nie, Y. F.
- Nature Nanotechnology, Vol. 9, Issue 6
Origin of the pre-peak features in the oxygen K-edge x-ray absorption spectra of LaFeO 3 and LaMnO 3 studied by Ga substitution of the transition metal ion
journal, July 2011
- Lafuerza, S.; Subías, G.; García, J.
- Journal of Physics: Condensed Matter, Vol. 23, Issue 32
Evolution of electronic structure across the rare-earth RNiO3 series
journal, April 2016
- Freeland, John W.; van Veenendaal, Michel; Chakhalian, Jak
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 208
Critical features of colossal magnetoresistive manganites
journal, February 2006
- Tokura, Y.
- Reports on Progress in Physics, Vol. 69, Issue 3
Epitaxial strain modulated electronic properties of interface controlled nickelate superlattices
journal, July 2018
- Middey, S.; Meyers, D.; Ojha, Shashank Kumar
- Physical Review B, Vol. 98, Issue 4
Oxide Electronics Utilizing Ultrafast Metal-Insulator Transitions
journal, August 2011
- Yang, Zheng; Ko, Changhyun; Ramanathan, Shriram
- Annual Review of Materials Research, Vol. 41, Issue 1
Tunable Charge and Spin Order in Thin Films and Superlattices
journal, November 2014
- Hepting, M.; Minola, M.; Frano, A.
- Physical Review Letters, Vol. 113, Issue 22
Experimental versus x-ray absorption of iron-doped zirconia: Trends in O -edge spectra as a function of iron doping
journal, November 2014
- Douma, D. H.; Ciprian, R.; Lamperti, A.
- Physical Review B, Vol. 90, Issue 20
High‐Entropy Oxides: Fundamental Aspects and Electrochemical Properties
journal, March 2019
- Sarkar, Abhishek; Wang, Qingsong; Schiele, Alexander
- Advanced Materials, Vol. 31, Issue 26
Direct Observation of Charge Order in an Epitaxial Film
journal, March 2002
- Staub, U.; Meijer, G. I.; Fauth, F.
- Physical Review Letters, Vol. 88, Issue 12
Entropy-stabilized oxides
journal, September 2015
- Rost, Christina M.; Sachet, Edward; Borman, Trent
- Nature Communications, Vol. 6, Issue 1
Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates
journal, April 2018
- Middey, S.; Meyers, D.; Kareev, M.
- Physical Review Letters, Vol. 120, Issue 15
Structural and transport properties of epitaxial PrNiO3 thin films grown by molecular beam epitaxy
journal, March 2013
- Feigl, L.; Schultz, B. D.; Ohya, S.
- Journal of Crystal Growth, Vol. 366
Orbital reflectometry of superlattices
journal, May 2015
- Wu, M.; Benckiser, E.; Audehm, P.
- Physical Review B, Vol. 91, Issue 19
Electronic transitions in strained SmNiO 3 thin films
journal, November 2014
- Catalano, S.; Gibert, M.; Bisogni, V.
- APL Materials, Vol. 2, Issue 11
Phase stability and distortion in high-entropy oxides
journal, March 2018
- Anand, G.; Wynn, Alex P.; Handley, Christopher M.
- Acta Materialia, Vol. 146
R perovskites ( R =Pr,Nd): Nickel valence and the metal-insulator transition investigated by x-ray-absorption spectroscopy
journal, December 1992
- Medarde, M.; Fontaine, A.; García-Muñoz, J. L.
- Physical Review B, Vol. 46, Issue 23
Phase diagram of compressively strained nickelate thin films
journal, September 2013
- Disa, A. S.; Kumah, D. P.; Ngai, J. H.
- APL Materials, Vol. 1, Issue 3
Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate
journal, October 2014
- Middey, S.; Rivero, P.; Meyers, D.
- Scientific Reports, Vol. 4, Issue 1
Role of magnetic and orbital ordering at the metal-insulator transition in
journal, March 2006
- Scagnoli, V.; Staub, U.; Mulders, A. M.
- Physical Review B, Vol. 73, Issue 10
Metal-insulator transitions
journal, October 1998
- Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
- Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
Rare-earth nickelates R NiO 3 : thin films and heterostructures
journal, February 2018
- Catalano, S.; Gibert, M.; Fowlie, J.
- Reports on Progress in Physics, Vol. 81, Issue 4
The 2016 oxide electronic materials and oxide interfaces roadmap
journal, October 2016
- Lorenz, M.; Ramachandra Rao, M. S.; Venkatesan, T.
- Journal of Physics D: Applied Physics, Vol. 49, Issue 43
Progress in perovskite nickelate research
journal, July 2008
- Catalan, G.
- Phase Transitions, Vol. 81, Issue 7-8
Neutron-diffraction study of R ( R =La,Pr,Nd,Sm): Electronically induced structural changes across the metal-insulator transition
journal, August 1992
- García-Muñoz, J. L.; Rodríguez-Carvajal, J.; Lacorre, P.
- Physical Review B, Vol. 46, Issue 8
A new class of high-entropy perovskite oxides
journal, January 2018
- Jiang, Sicong; Hu, Tao; Gild, Joshua
- Scripta Materialia, Vol. 142
Stable metal–insulator transition in epitaxial SmNiO3 thin films
journal, June 2012
- Ha, Sieu D.; Otaki, Miho; Jaramillo, R.
- Journal of Solid State Chemistry, Vol. 190
Metal−Insulator Transitions, Structural and Microstructural Evolution of RNiO 3 (R = Sm, Eu, Gd, Dy, Ho, Y) Perovskites: Evidence for Room-Temperature Charge Disproportionation in Monoclinic HoNiO 3 and YNiO 3
journal, May 1999
- Alonso, José A.; Martínez-Lope, María J.; Casais, María T.
- Journal of the American Chemical Society, Vol. 121, Issue 20
Single-crystal high entropy perovskite oxide epitaxial films
journal, June 2018
- Sharma, Yogesh; Musico, Brianna L.; Gao, Xiang
- Physical Review Materials, Vol. 2, Issue 6
Rationalizing strain engineering effects in rare-earth nickelates
journal, November 2013
- Bruno, F. Y.; Rushchanskii, K. Z.; Valencia, S.
- Physical Review B, Vol. 88, Issue 19
Measurement of a solid-state triple point at the metal–insulator transition in VO2
journal, August 2013
- Park, Jae Hyung; Coy, Jim M.; Kasirga, T. Serkan
- Nature, Vol. 500, Issue 7463
Domain wall nanoelectronics
journal, February 2012
- Catalan, G.; Seidel, J.; Ramesh, R.
- Reviews of Modern Physics, Vol. 84, Issue 1
High-entropy oxides: An emerging prospect for magnetic rare-earth transition metal perovskites
journal, March 2019
- Witte, Ralf; Sarkar, Abhishek; Kruk, Robert
- Physical Review Materials, Vol. 3, Issue 3
Anomalous electron transport in epitaxial films
journal, June 2019
- Ojha, Shashank Kumar; Ray, Sujay; Das, Tanmoy
- Physical Review B, Vol. 99, Issue 23
Metal-Insulator Transition in Ultrathin Films
journal, June 2011
- Scherwitzl, R.; Gariglio, S.; Gabay, M.
- Physical Review Letters, Vol. 106, Issue 24
Long-Range Antiferromagnetic Order in a Rocksalt High Entropy Oxide
journal, April 2019
- Zhang, Junjie; Yan, Jiaqiang; Calder, Stuart
- Chemistry of Materials, Vol. 31, Issue 10
Publisher’s Note: Strain-modulated Mott transition in EuNiO ultrathin films [Phys. Rev. B 88 , 075116 (2013)]
journal, August 2013
- Meyers, D.; Middey, S.; Kareev, M.
- Physical Review B, Vol. 88, Issue 7
Strain-mediated metal-insulator transition in epitaxial ultrathin films of NdNiO3
journal, June 2010
- Liu, Jian; Kareev, M.; Gray, B.
- Applied Physics Letters, Vol. 96, Issue 23
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