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Title: Template Engineering of Metal-to-Insulator Transitions in Epitaxial Bilayer Nickelate Thin Films

Abstract

Understanding metal-to-insulator phase transitions in solids has been a keystone not only for discovering novel physical phenomena in condensed matter physics but also for achieving scientific breakthroughs in materials science. In this work, we demonstrate that the transport properties (i.e., resistivity and transition temperature) in the metal-to-insulator transitions of perovskite nickelates are tunable via the epitaxial heterojunctions of LaNiO3 and NdNiO3 thin films. Here, a mismatch in the oxygen coordination environment and interfacial octahedral coupling at the oxide heterointerface allows us to realize an exotic phase that is unattainable in the parent compound. With oxygen vacancy formation for strain accommodation, the topmost LaNiO3 layer in LaNiO3/NdNiO3 bilayer thin films is structurally engineered and it electrically undergoes a metal-to-insulator transition that does not appear in metallic LaNiO3. Modification of the NdNiO3 template layer thickness provides an additional knob for tailoring the tilting angles of corner-connected NiO6 octahedra and the linked transport characteristics further. Our approaches can be harnessed to tune physical properties in complex oxides and to realize exotic physical phenomena through oxide thin-film heterostructuring.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5];  [4];  [5];  [6];  [7];  [8];  [9]; ORCiD logo [10]; ORCiD logo [11]; ORCiD logo [9]; ORCiD logo [8]; ORCiD logo [6];  [4];  [5]; ORCiD logo [4];  [3] more »; ORCiD logo [2]; ORCiD logo [7]; ORCiD logo [1] « less
  1. School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju 61005, Republic of Korea
  2. Department of Materials Science and Engineering, Pohang University of Science and Technology, Pohang 37673, Republic of Korea
  3. Department of Physics, University of Ulsan, Ulsan 44610, Republic of Korea
  4. Pohang Accelerator Laboratory, Pohang 37673, Republic of Korea
  5. Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
  6. Department of Electrical Engineering, Gachon University, Seongnam 13120, Republic of Korea
  7. Department of Physics, University of Ulsan and Energy Harvest-Storage Research Center (EHSRC), Ulsan 44610, Republic of Korea
  8. Department of Physics, Inha University, Incheon 22212, Republic of Korea
  9. Department of Physics, Pusan National University, Busan 46241, Republic of Korea
  10. Department of Physics, Soongsil University, Seoul 06978, Republic of Korea
  11. Department of Physics, Chung-Ang University, Seoul 06974, Republic of Korea
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF)
OSTI Identifier:
1858783
Alternate Identifier(s):
OSTI ID: 1840962
Grant/Contract Number:  
DEAC02-06CH11357; AC02-06CH11357; NRF-2018R1D1A1B07043155; NRF-2020R1F1A1057220; NRF-2019R1C1C1010345; NRF-2019R1A6A1A11053838; NRF-2020R1A4A1017915; 2017M3D1A1040834; NRF-2019K1A3A7A09033393; 2013M3A6B1078872; 2020R1A6C101A202
Resource Type:
Published Article
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Name: ACS Applied Materials and Interfaces Journal Volume: 13 Journal Issue: 45; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; heteroepitaxy; metal-to-insulator phase transition; oxide; template engineering; thin film

Citation Formats

Lee, Jongmin, Kim, Gi-Yeop, Jeong, Seyeop, Yang, Mihyun, Kim, Jong-Woo, Cho, Byeong-Gwan, Choi, Yongseong, Kim, Sangmo, Choi, Jin San, Lee, Tae Kwon, Kim, Jiwoong, Lee, Dong Ryeol, Chang, Seo Hyoung, Park, Sungkyun, Jung, Jong Hoon, Bark, Chung Wung, Koo, Tae-Young, Ryan, Philip J., Ihm, Kyuwook, Kim, Sanghoon, Choi, Si-Young, Kim, Tae Heon, and Lee, Sanghan. Template Engineering of Metal-to-Insulator Transitions in Epitaxial Bilayer Nickelate Thin Films. United States: N. p., 2021. Web. doi:10.1021/acsami.1c13675.
Lee, Jongmin, Kim, Gi-Yeop, Jeong, Seyeop, Yang, Mihyun, Kim, Jong-Woo, Cho, Byeong-Gwan, Choi, Yongseong, Kim, Sangmo, Choi, Jin San, Lee, Tae Kwon, Kim, Jiwoong, Lee, Dong Ryeol, Chang, Seo Hyoung, Park, Sungkyun, Jung, Jong Hoon, Bark, Chung Wung, Koo, Tae-Young, Ryan, Philip J., Ihm, Kyuwook, Kim, Sanghoon, Choi, Si-Young, Kim, Tae Heon, & Lee, Sanghan. Template Engineering of Metal-to-Insulator Transitions in Epitaxial Bilayer Nickelate Thin Films. United States. https://doi.org/10.1021/acsami.1c13675
Lee, Jongmin, Kim, Gi-Yeop, Jeong, Seyeop, Yang, Mihyun, Kim, Jong-Woo, Cho, Byeong-Gwan, Choi, Yongseong, Kim, Sangmo, Choi, Jin San, Lee, Tae Kwon, Kim, Jiwoong, Lee, Dong Ryeol, Chang, Seo Hyoung, Park, Sungkyun, Jung, Jong Hoon, Bark, Chung Wung, Koo, Tae-Young, Ryan, Philip J., Ihm, Kyuwook, Kim, Sanghoon, Choi, Si-Young, Kim, Tae Heon, and Lee, Sanghan. Fri . "Template Engineering of Metal-to-Insulator Transitions in Epitaxial Bilayer Nickelate Thin Films". United States. https://doi.org/10.1021/acsami.1c13675.
@article{osti_1858783,
title = {Template Engineering of Metal-to-Insulator Transitions in Epitaxial Bilayer Nickelate Thin Films},
author = {Lee, Jongmin and Kim, Gi-Yeop and Jeong, Seyeop and Yang, Mihyun and Kim, Jong-Woo and Cho, Byeong-Gwan and Choi, Yongseong and Kim, Sangmo and Choi, Jin San and Lee, Tae Kwon and Kim, Jiwoong and Lee, Dong Ryeol and Chang, Seo Hyoung and Park, Sungkyun and Jung, Jong Hoon and Bark, Chung Wung and Koo, Tae-Young and Ryan, Philip J. and Ihm, Kyuwook and Kim, Sanghoon and Choi, Si-Young and Kim, Tae Heon and Lee, Sanghan},
abstractNote = {Understanding metal-to-insulator phase transitions in solids has been a keystone not only for discovering novel physical phenomena in condensed matter physics but also for achieving scientific breakthroughs in materials science. In this work, we demonstrate that the transport properties (i.e., resistivity and transition temperature) in the metal-to-insulator transitions of perovskite nickelates are tunable via the epitaxial heterojunctions of LaNiO3 and NdNiO3 thin films. Here, a mismatch in the oxygen coordination environment and interfacial octahedral coupling at the oxide heterointerface allows us to realize an exotic phase that is unattainable in the parent compound. With oxygen vacancy formation for strain accommodation, the topmost LaNiO3 layer in LaNiO3/NdNiO3 bilayer thin films is structurally engineered and it electrically undergoes a metal-to-insulator transition that does not appear in metallic LaNiO3. Modification of the NdNiO3 template layer thickness provides an additional knob for tailoring the tilting angles of corner-connected NiO6 octahedra and the linked transport characteristics further. Our approaches can be harnessed to tune physical properties in complex oxides and to realize exotic physical phenomena through oxide thin-film heterostructuring.},
doi = {10.1021/acsami.1c13675},
journal = {ACS Applied Materials and Interfaces},
number = 45,
volume = 13,
place = {United States},
year = {Fri Nov 05 00:00:00 EDT 2021},
month = {Fri Nov 05 00:00:00 EDT 2021}
}

Journal Article:
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https://doi.org/10.1021/acsami.1c13675

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Works referenced in this record:

Template engineering of Co-doped BaFe2As2 single-crystal thin films
journal, February 2010

  • Lee, S.; Jiang, J.; Zhang, Y.
  • Nature Materials, Vol. 9, Issue 5
  • DOI: 10.1038/nmat2721

Nanoscale Domain Control in Multiferroic BiFeO3 Thin Films
journal, September 2006

  • Chu, Y.-H.; Zhan, Q.; Martin, L. W.
  • Advanced Materials, Vol. 18, Issue 17, p. 2307-2311
  • DOI: 10.1002/adma.200601098

Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3
journal, August 2004

  • Muller, David A.; Nakagawa, Naoyuki; Ohtomo, Akira
  • Nature, Vol. 430, Issue 7000
  • DOI: 10.1038/nature02756

Long-Range Domain Structure and Symmetry Engineering by Interfacial Oxygen Octahedral Coupling at Heterostructure Interface
journal, June 2016

  • Liao, Zhaoliang; Green, Robert J.; Gauquelin, Nicolas
  • Advanced Functional Materials, Vol. 26, Issue 36
  • DOI: 10.1002/adfm.201602155

Structural, magnetic and electronic properties of perovskites (R = rare earth)
journal, February 1997


Physics of Ultrathin Films and Heterostructures of Rare-Earth Nickelates
journal, July 2016


Oxygen Vacancy Induced Room-Temperature Metal–Insulator Transition in Nickelate Films and Its Potential Application in Photovoltaics
journal, April 2016

  • Wang, Le; Dash, Sibashisa; Chang, Lei
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 15
  • DOI: 10.1021/acsami.6b00650

A correlated nickelate synaptic transistor
journal, October 2013

  • Shi, Jian; Ha, Sieu D.; Zhou, You
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3676

Catalytic Hydrogen Doping of NdNiO 3 Thin Films under Electric Fields
journal, November 2020

  • Sidik, Umar; Hattori, Azusa N.; Rakshit, Rupali
  • ACS Applied Materials & Interfaces, Vol. 12, Issue 49
  • DOI: 10.1021/acsami.0c15724

Octahedral Tilting in Perovskites. I. Geometrical Considerations
journal, February 1997


Connecting bulk symmetry and orbital polarization in strained RNiO 3 ultrathin films
journal, November 2013


Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling
journal, March 2016

  • Liao, Z.; Huijben, M.; Zhong, Z.
  • Nature Materials, Vol. 15, Issue 4
  • DOI: 10.1038/nmat4579

Systematic study of insulator-metal transitions in perovskites RNiO3 (R=Pr,Nd,Sm,Eu) due to closing of charge-transfer gap
journal, April 1992


Conductivity and Local Structure of LaNiO 3 Thin Films
journal, March 2017

  • Fowlie, Jennifer; Gibert, Marta; Tieri, Giulio
  • Advanced Materials, Vol. 29, Issue 18
  • DOI: 10.1002/adma.201605197

Multiple strain-induced phase transitions in LaNi O 3 thin films
journal, July 2016


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
  • DOI: 10.1038/nnano.2014.59

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
  • DOI: 10.1016/j.elspec.2015.07.006

Asymmetric Orbital-Lattice Interactions in Ultrathin Correlated Oxide Films
journal, September 2011


Oxide Electronics Utilizing Ultrafast Metal-Insulator Transitions
journal, August 2011


Control of octahedral connectivity in perovskite oxide heterostructures: An emerging route to multifunctional materials discovery
journal, March 2012

  • Rondinelli, James M.; May, Steven J.; Freeland, John W.
  • MRS Bulletin, Vol. 37, Issue 3
  • DOI: 10.1557/mrs.2012.49

Competition between strain and dimensionality effects on the electronic phase transitions in NdNiO3 films
journal, December 2015

  • Wang, Le; Ju, Sheng; You, Lu
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep18707

Tuning magnetic anisotropy by interfacially engineering the oxygen coordination environment in a transition metal oxide
journal, March 2016

  • Kan, Daisuke; Aso, Ryotaro; Sato, Riko
  • Nature Materials, Vol. 15, Issue 4
  • DOI: 10.1038/nmat4580

The missing memristor found
journal, May 2008

  • Strukov, Dmitri B.; Snider, Gregory S.; Stewart, Duncan R.
  • Nature, Vol. 453, Issue 7191
  • DOI: 10.1038/nature06932

Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates
journal, April 2018


Metal–insulator-transition engineering by modulation tilt-control in perovskite nickelates for room temperature optical switching
journal, September 2018

  • Liao, Zhaoliang; Gauquelin, Nicolas; Green, Robert J.
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 38
  • DOI: 10.1073/pnas.1807457115

Low-dimensional Mott material: Transport in ultrathin epitaxial LaNiO3 films
journal, February 2010

  • Son, Junwoo; Moetakef, Pouya; LeBeau, James M.
  • Applied Physics Letters, Vol. 96, Issue 6
  • DOI: 10.1063/1.3309713

Direct Evidence of the Competing Nature between Electronic and Lattice Breathing Order in Rare-Earth Nickelates
journal, March 2020


Strain-driven disproportionation at a correlated oxide metal-insulator transition
journal, March 2020


Doped holes in edge-shared CuO 2 chains and the dynamic spectral weight transfer in X-ray absorption spectroscopy
journal, July 2002


Metal-insulator transitions in NdNiO 3 thin films
journal, September 2000


Effects of Nonequilibrium Growth, Nonstoichiometry, and Film Orientation on the Metal-to-Insulator Transition in NdNiO 3 Thin Films
journal, December 2014

  • Breckenfeld, Eric; Chen, Zuhuang; Damodaran, Anoop. R.
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 24
  • DOI: 10.1021/am506436s

Correlation between stoichiometry, strain, and metal-insulator transitions of NdNiO 3 films
journal, March 2015

  • Hauser, Adam J.; Mikheev, Evgeny; Moreno, Nelson E.
  • Applied Physics Letters, Vol. 106, Issue 9
  • DOI: 10.1063/1.4914002

Metal-insulator transitions
journal, October 1998

  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/RevModPhys.70.1039

Rare-earth nickelates R NiO 3 : thin films and heterostructures
journal, February 2018


Polar metals by geometric design
journal, April 2016


Interface Physics in Complex Oxide Heterostructures
journal, March 2011


Progress in perovskite nickelate research
journal, July 2008


Neutron-diffraction study of R NiO 3 ( 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
  • DOI: 10.1103/PhysRevB.46.4414

Influence of tensile-strain-induced oxygen deficiency on metal-insulator transitions in NdNiO3−δ epitaxial thin films
journal, July 2017


Non-stoichiometry-induced metal-to-insulator transition in nickelate thin films grown by pulsed laser deposition
journal, December 2018


Superconductivity in an infinite-layer nickelate
journal, August 2019


Charge order and antiferromagnetism in epitaxial ultrathin films of EuNiO 3
journal, December 2015


Tuning the magnetic properties of La Co O 3 thin films by epitaxial strain
journal, January 2008


The classification of tilted octahedra in perovskites
journal, November 1972

  • Glazer, A. M.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 11
  • DOI: 10.1107/S0567740872007976

Oxygen Diode Formed in Nickelate Heterostructures by Chemical Potential Mismatch
journal, March 2018


Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates
journal, October 2016

  • Bisogni, Valentina; Catalano, Sara; Green, Robert J.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13017

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
  • DOI: 10.1063/1.3451462

Elastic Constants of Strontium Titanate (SrTi O 3 )
journal, June 1958