Orbital control of metal-to-insulator transition in high-entropy nickelates

Cui, Ting; Lin, Ting; Jin, Qiao; Chen, Shengru; Hong, Haitao; Zhang, Qinghua; Fan, Yiyan; Rong, Dongke; Wang, Jiaou; Wang, Can; Gu, Lin; Jin, Kuijuan; Wang, Le; Guo, Er-Jia

doi:10.1103/physrevmaterials.7.115802

Title: Orbital control of metal-to-insulator transition in high-entropy nickelates

Journal Article · 14 November 2023 · Physical Review Materials

DOI: https://doi.org/10.1103/physrevmaterials.7.115802 · OSTI ID:2339615

Cui, Ting ^[1]; Lin, Ting ^[2];

^[2]; Chen, Shengru ^[1]; Hong, Haitao ^[1]; Zhang, Qinghua ^[2]; Fan, Yiyan ^[2]; Rong, Dongke ^[3]; Wang, Jiaou ^[4]; Wang, Can ^[5]; Gu, Lin ^[6]; Jin, Kuijuan ^[5];

^[7];

^[1]

Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China)
Chinese Academy of Sciences (CAS), Beijing (China)
Chinese Academy of Sciences (CAS), Beijing (China); China University of Geosciences (Beijing) (CUGB), (China)
Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics (IHEP)
Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China); Songshan Lake Materials Laboratory, Guangdong (China)
Tsinghua Univ., Beijing (China)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

High-entropy materials have emerged as a promising platform for exploring unique electronic and structural properties. In this study, we investigated the orbital control of the metal-to-insulator transition in thin films of high-entropy nickelates, which are composed of five rare-earth elements in equi-atomic concentrations. By manipulating the levels of misfit strain through substrate choice and film thickness, we modulated the electronic properties and examined the intricate interplay between strain, orbital interactions, and the metal-to-insulator transition. Compared to other nickelates thin films like NdNi O₃ and SmNi O₃, thin films of high-entropy nickelates exhibited remarkable resilience in maintaining control over their transport properties and orbital polarization, even in the presence of considerable A-site disorder. Further, this finding suggests that the electronic properties of A-site disordered high-entropy nickelates are still governed by the electronic bandwidth, primarily influenced by the Ni-O bonding geometry. This study provides valuable insights into the complex interplay among composition, structure, and electronic properties in perovskite oxides. These insights have the potential to guide the development of perovskite oxide materials with tailored electronic properties for a wide range of applications.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2339615

Report Number(s):: PNNL-SA--186623

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 11 Vol. 7; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (60)

Strain Control of Oxygen Vacancies in Epitaxial Strontium Cobaltite Films Petrie, Jonathan R.; Mitra, Chandrima; Jeen, Hyoungjeen Advanced Functional Materials, Vol. 26, Issue 10 https://doi.org/10.1002/adfm.201504868	journal	January 2016
Tuning Bifunctional Oxygen Electrocatalysts by Changing the A-Site Rare-Earth Element in Perovskite Nickelates Wang, Le; Stoerzinger, Kelsey A.; Chang, Lei Advanced Functional Materials, Vol. 28, Issue 39 https://doi.org/10.1002/adfm.201803712	journal	August 2018
Electric-Field Control of the Metal-Insulator Transition in Ultrathin NdNiO3 Films Scherwitzl, Raoul; Zubko, Pavlo; Lezama, I. Gutierrez Advanced Materials, Vol. 22, Issue 48 https://doi.org/10.1002/adma.201003241	journal	October 2010
Tuning the Structure of Nickelates to Achieve Two-Dimensional Electron Conduction Kumah, Divine P.; Disa, Ankit S.; Ngai, Joseph H. Advanced Materials, Vol. 26, Issue 12 https://doi.org/10.1002/adma.201304256	journal	February 2014
Strain‐Engineered Metal‐to‐Insulator Transition and Orbital Polarization in Nickelate Superlattices Integrated on Silicon Chen, Binbin; Gauquelin, Nicolas; Jannis, Daen Advanced Materials, Vol. 32, Issue 50 https://doi.org/10.1002/adma.202004995	journal	November 2020
Tuning the Electronic Structure of LaNiO ₃ through Alloying with Strontium to Enhance Oxygen Evolution Activity Liu, Jishan; Jia, Endong; Wang, Le Advanced Science, Vol. 6, Issue 19 https://doi.org/10.1002/advs.201901073	journal	August 2019
Designing Magnetism in High Entropy Oxides Mazza, Alessandro R.; Skoropata, Elizabeth; Sharma, Yogesh Advanced Science, Vol. 9, Issue 10 https://doi.org/10.1002/advs.202200391	journal	February 2022
Epitaxial Design of Complex Nickelates as Electrocatalysts for the Oxygen Evolution Reaction Choi, Min‐Ju; Wang, Le; Stoerzinger, Kelsey A. Advanced Energy Materials, Vol. 13, Issue 22 https://doi.org/10.1002/aenm.202300239	journal	April 2023
Lanthanide nickelates for their application on Solid Oxide Cells Morales-Zapata, M. A.; Larrea, A.; Laguna-Bercero, M. A. Electrochimica Acta, Vol. 444 https://doi.org/10.1016/j.electacta.2023.141970	journal	March 2023
High entropy oxides-exploring a paradigm of promising catalysts: A review Albedwawi, Shaima H.; AlJaberi, Asala; Haidemenopoulos, Gregory N. Materials & Design, Vol. 202 https://doi.org/10.1016/j.matdes.2021.109534	journal	April 2021
Orientations-Dependent Metal-to-Insulator Transition in Solution-Deposited High-Entropy Nickelate Thin Films Tang, Xianwu; Hu, Ling; Zhu, Xiaoguang Crystal Growth & Design, Vol. 22, Issue 12 https://doi.org/10.1021/acs.cgd.2c00945	journal	November 2022
Spatially Controlled Octahedral Rotations and Metal–Insulator Transitions in Nickelate Superlattices Chen, Binbin; Gauquelin, Nicolas; Green, Robert J. Nano Letters, Vol. 21, Issue 3 https://doi.org/10.1021/acs.nanolett.0c03850	journal	January 2021
Understanding the Electronic Structure Evolution of Epitaxial LaNi_1–xFe_xO₃ Thin Films for Water Oxidation Wang, Le; Adiga, Prajwal; Zhao, Jiali Nano Letters, Vol. 21, Issue 19 https://doi.org/10.1021/acs.nanolett.1c02901	journal	September 2021
Oxygen Vacancy Induced Room-Temperature Metal–Insulator Transition in Nickelate Films and Its Potential Application in Photovoltaics Wang, Le; Dash, Sibashisa; Chang, Lei ACS Applied Materials & Interfaces, Vol. 8, Issue 15 https://doi.org/10.1021/acsami.6b00650	journal	April 2016
Strain Effect on Oxygen Evolution Reaction Activity of Epitaxial NdNiO ₃ Thin Films Wang, Le; Stoerzinger, Kelsey A.; Chang, Lei ACS Applied Materials & Interfaces, Vol. 11, Issue 13 https://doi.org/10.1021/acsami.8b21301	journal	March 2019
A High-Entropy Oxide as High-Activity Electrocatalyst for Water Oxidation Kante, Mohana V.; Weber, Moritz L.; Ni, Shu ACS Nano https://doi.org/10.1021/acsnano.2c08096	journal	March 2023
Towards 3D Mapping of BO ₆ Octahedron Rotations at Perovskite Heterointerfaces, Unit Cell by Unit Cell He, Qian; Ishikawa, Ryo; Lupini, Andrew R. ACS Nano, Vol. 9, Issue 8 https://doi.org/10.1021/acsnano.5b03232	journal	July 2015
Understanding the Role of Entropy in High Entropy Oxides Aamlid, Solveig S.; Oudah, Mohamed; Rottler, Jörg Journal of the American Chemical Society, Vol. 145, Issue 11 https://doi.org/10.1021/jacs.2c11608	journal	March 2023
Enhanced Bifunctional Oxygen Catalysis in Strained LaNiO ₃ Perovskites Petrie, Jonathan R.; Cooper, Valentino R.; Freeland, John W. Journal of the American Chemical Society, Vol. 138, Issue 8 https://doi.org/10.1021/jacs.5b11713	journal	February 2016
Strongly correlated perovskite fuel cells Zhou, You; Guan, Xiaofei; Zhou, Hua Nature, Vol. 534, Issue 7606 https://doi.org/10.1038/nature17653	journal	May 2016
Interlayer coupling through a dimensionality-induced magnetic state Gibert, M.; Viret, M.; Zubko, P. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11227	journal	April 2016
Heterointerface engineered electronic and magnetic phases of NdNiO3 thin films Liu, Jian; Kargarian, Mehdi; Kareev, Mikhail Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3714	journal	November 2013
Orbital reflectometry of oxide heterostructures Benckiser, Eva; Haverkort, Maurits W.; Brück, Sebastian Nature Materials, Vol. 10, Issue 3 https://doi.org/10.1038/nmat2958	journal	February 2011
Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy Aetukuri, Nagaphani B.; Gray, Alexander X.; Drouard, Marc Nature Physics, Vol. 9, Issue 10 https://doi.org/10.1038/nphys2733	journal	September 2013
Perovskite nickelates as bio-electronic interfaces Zhang, Hai-Tian; Zuo, Fan; Li, Feiran Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09660-6	journal	April 2019
Complete phase diagram of rare-earth nickelates from first-principles Varignon, Julien; Grisolia, Mathieu N.; Íñiguez, Jorge npj Quantum Materials, Vol. 2, Issue 1 https://doi.org/10.1038/s41535-017-0024-9	journal	April 2017
Length scales of interfacial coupling between metal and insulator phases in oxides Domínguez, Claribel; Georgescu, Alexandru B.; Mundet, Bernat Nature Materials, Vol. 19, Issue 11 https://doi.org/10.1038/s41563-020-0757-x	journal	August 2020
Competition between strain and dimensionality effects on the electronic phase transitions in NdNiO3 films Wang, Le; Ju, Sheng; You, Lu Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep18707	journal	December 2015
Epitaxial stabilization of ultra thin films of high entropy perovskite Patel, Ranjan Kumar; Ojha, Shashank Kumar; Kumar, Siddharth Applied Physics Letters, Vol. 116, Issue 7 https://doi.org/10.1063/1.5133710	journal	February 2020
Electronic conduction in : the dependence on the oxygen stoichiometry Gayathri, N.; Raychaudhuri, A. K.; Xu, X. Q. Journal of Physics: Condensed Matter, Vol. 10, Issue 6 https://doi.org/10.1088/0953-8984/10/6/015	journal	February 1998
Rare-earth nickelates R NiO ₃ : thin films and heterostructures Catalano, S.; Gibert, M.; Fowlie, J. Reports on Progress in Physics, Vol. 81, Issue 4 https://doi.org/10.1088/1361-6633/aaa37a	journal	February 2018
Charge doping effects on magnetic properties of single-crystal La 1 − x Sr x ( Cr 0.2 Mn 0.2 Fe 0.2 Co 0.2 Ni 0.2 ) O 3 ( 0 ≤ x ≤ 0.5 ) high-entropy perovskite oxides Mazza, Alessandro R.; Skoropata, Elizabeth; Lapano, Jason Physical Review B, Vol. 104, Issue 9 https://doi.org/10.1103/PhysRevB.104.094204	journal	September 2021
Weak ferromagnetism in Tb(Fe0.2Mn0.2Co0.2Cr0.2Ni0.2)O3 high-entropy oxide perovskite thin films Farhan, Alan; Stramaglia, Federico; Cocconcelli, Maria Physical Review B, Vol. 106, Issue 6 https://doi.org/10.1103/PhysRevB.106.L060404	journal	August 2022
Systematic study of insulator-metal transitions in perovskites RNiO3 (R=Pr,Nd,Sm,Eu) due to closing of charge-transfer gap Torrance, J.; Lacorre, P.; Nazzal, A. Physical Review B, Vol. 45, Issue 14 https://doi.org/10.1103/PhysRevB.45.8209	journal	April 1992
Neutron-diffraction study of R NiO 3 ( R =La,Pr,Nd,Sm): Electronically induced structural changes across the metal-insulator transition García-Muñoz, J. L.; Rodríguez-Carvajal, J.; Lacorre, P. Physical Review B, Vol. 46, Issue 8 https://doi.org/10.1103/PhysRevB.46.4414	journal	August 1992
Resisitivity, thermopower, and susceptibility of R NiO 3 ( R =La,Pr) Xu, X. Q.; Peng, J. L.; Li, Z. Y. Physical Review B, Vol. 48, Issue 2 https://doi.org/10.1103/PhysRevB.48.1112	journal	July 1993
Influence of carrier injection on the metal-insulator transition in electron- and hole-doped R 1 − x A x NiO 3 perovskites García-Muñoz, J. L.; Suaaidi, M.; Martínez-Lope, M. J. Physical Review B, Vol. 52, Issue 18 https://doi.org/10.1103/PhysRevB.52.13563	journal	November 1995
Metal-insulator transitions in NdNiO 3 thin films Catalan, G.; Bowman, R. M.; Gregg, J. M. Physical Review B, Vol. 62, Issue 12 https://doi.org/10.1103/PhysRevB.62.7892	journal	September 2000
Resonant x-ray scattering experiments on electronic orderings in NdNiO 3 single crystals Lorenzo, J. E.; Hodeau, J. L.; Paolasini, L. Physical Review B, Vol. 71, Issue 4 https://doi.org/10.1103/PhysRevB.71.045128	journal	January 2005
Role of magnetic and orbital ordering at the metal-insulator transition in NdNiO 3 Scagnoli, V.; Staub, U.; Mulders, A. M. Physical Review B, Vol. 73, Issue 10 https://doi.org/10.1103/PhysRevB.73.100409	journal	March 2006
Fermi surfaces, electron-hole asymmetry, and correlation kink in a three-dimensional Fermi liquid LaNiO 3 Eguchi, R.; Chainani, A.; Taguchi, M. Physical Review B, Vol. 79, Issue 11 https://doi.org/10.1103/PhysRevB.79.115122	journal	March 2009
Quantifying octahedral rotations in strained perovskite oxide films May, S. J.; Kim, J. -W.; Rondinelli, J. M. Physical Review B, Vol. 82, Issue 1 https://doi.org/10.1103/PhysRevB.82.014110	journal	July 2010
Confinement-induced metal-to-insulator transition in strained LaNiO 3 /LaAlO 3 superlattices Blanca-Romero, Ariadna; Pentcheva, Rossitza Physical Review B, Vol. 84, Issue 19 https://doi.org/10.1103/PhysRevB.84.195450	journal	November 2011
Structural origins of the properties of rare earth nickelate superlattices Hwang, Jinwoo; Son, Junwoo; Zhang, Jack Y. Physical Review B, Vol. 87, Issue 6 https://doi.org/10.1103/PhysRevB.87.060101	journal	February 2013
Strain-controlled oxygen vacancy formation and ordering in CaMnO 3 Aschauer, Ulrich; Pfenninger, Reto; Selbach, Sverre M. Physical Review B, Vol. 88, Issue 5 https://doi.org/10.1103/PhysRevB.88.054111	journal	August 2013
Orbital polarization in strained LaNiO 3 : Structural distortions and correlation effects Peil, Oleg E.; Ferrero, Michel; Georges, Antoine Physical Review B, Vol. 90, Issue 4 https://doi.org/10.1103/PhysRevB.90.045128	journal	July 2014
Orbital Order and Possible Superconductivity in LaNiO 3 / LaMO 3 Superlattices Chaloupka, Jiří; Khaliullin, Giniyat Physical Review Letters, Vol. 100, Issue 1 https://doi.org/10.1103/PhysRevLett.100.016404	journal	January 2008
Metal-Insulator Transition in Ultrathin LaNiO 3 Films Scherwitzl, R.; Gariglio, S.; Gabay, M. Physical Review Letters, Vol. 106, Issue 24 https://doi.org/10.1103/PhysRevLett.106.246403	journal	June 2011
Asymmetric Orbital-Lattice Interactions in Ultrathin Correlated Oxide Films Chakhalian, J.; Rondinelli, J. M.; Liu, Jian Physical Review Letters, Vol. 107, Issue 11 https://doi.org/10.1103/PhysRevLett.107.116805	journal	September 2011
Site-Selective Mott Transition in Rare-Earth-Element Nickelates Park, Hyowon; Millis, Andrew J.; Marianetti, Chris A. Physical Review Letters, Vol. 109, Issue 15 https://doi.org/10.1103/PhysRevLett.109.156402	journal	October 2012
Mott Electrons in an Artificial Graphenelike Crystal of Rare-Earth Nickelate Middey, S.; Meyers, D.; Doennig, D. Physical Review Letters, Vol. 116, Issue 5 https://doi.org/10.1103/PhysRevLett.116.056801	journal	February 2016
Structural “ δ Doping” to Control Local Magnetization in Isovalent Oxide Heterostructures Moon, E. J.; He, Q.; Ghosh, S. Physical Review Letters, Vol. 119, Issue 19 https://doi.org/10.1103/PhysRevLett.119.197204	journal	November 2017
Switchable orbital polarization and magnetization in strained LaCo O 3 films Guo, Er-Jia; Desautels, Ryan D.; Keavney, David Physical Review Materials, Vol. 3, Issue 1 https://doi.org/10.1103/PhysRevMaterials.3.014407	journal	January 2019
Unexpected crystalline homogeneity from the disordered bond network in La ( C r 0.2 M n 0.2 F e 0.2 C o 0.2 N i 0.2 ) O 3 films Brahlek, Matthew; Mazza, Alessandro R.; Pitike, Krishna Chaitanya Physical Review Materials, Vol. 4, Issue 5 https://doi.org/10.1103/PhysRevMaterials.4.054407	journal	May 2020
Property and cation valence engineering in entropy-stabilized oxide thin films Kotsonis, George N.; Meisenheimer, Peter B.; Miao, Leixin Physical Review Materials, Vol. 4, Issue 10 https://doi.org/10.1103/PhysRevMaterials.4.100401	journal	October 2020
Tuning bad metal and non-Fermi liquid behavior in a Mott material: Rare-earth nickelate thin films Mikheev, Evgeny; Hauser, Adam J.; Himmetoglu, Burak Science Advances, Vol. 1, Issue 10 https://doi.org/10.1126/sciadv.1500797	journal	November 2015
High-entropy materials for catalysis: A new frontier Sun, Yifan; Dai, Sheng Science Advances, Vol. 7, Issue 20 https://doi.org/10.1126/sciadv.abg1600	journal	May 2021
Dimensionality Control of Electronic Phase Transitions in Nickel-Oxide Superlattices Boris, A. V.; Matiks, Y.; Benckiser, E. Science, Vol. 332, Issue 6032 https://doi.org/10.1126/science.1202647	journal	May 2011
A Perovskite Oxide Optimized for Oxygen Evolution Catalysis from Molecular Orbital Principles Suntivich, J.; May, K. J.; Gasteiger, H. A. Science, Vol. 334, Issue 6061 https://doi.org/10.1126/science.1212858	journal	October 2011
Sum Rules and Fundamental Spectra of Magnetic X-Ray Dichroism in Crystal Field Symmetry van der Laan, G. Journal of the Physical Society of Japan, Vol. 63, Issue 6 https://doi.org/10.1143/JPSJ.63.2393	journal	June 1994

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36 MATERIALS SCIENCE
high-entropy nickelates
metal-insulator transition
orbital polarization
strain

Title: Orbital control of metal-to-insulator transition in high-entropy nickelates

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