Limits to the strain engineering of layered square-planar nickelate thin films

Dan Ferenc Segedin; Berit H. Goodge; Grace A. Pan; Qi Song; Harrison LaBollita; Myung Chul Jung; Hesham El-Sherif; Spencer Doyle; Ari Turkiewicz; Nicole K. Taylor; Jarad A. Mason; Alpha T. N’Diaye; Hanjong Paik; Ismail El Baggari; Antia S. Botana; Lena F. Kourkoutis; Charles M. Brooks; Julia A. Mundy

doi:10.1038/s41467-023-37117-4

Limits to the strain engineering of layered square-planar nickelate thin films

Dan Ferenc Segedin, Berit H. Goodge, Grace A. Pan, Qi Song, Harrison LaBollita, Myung Chul Jung, Hesham El-Sherif, Spencer Doyle, Ari Turkiewicz, Nicole K. Taylor, Jarad A. Mason, Alpha T. N’Diaye, Hanjong Paik, Ismail El Baggari, Antia S. Botana, Lena F. Kourkoutis, Charles M. Brooks, Julia A. Mundy

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

Abstract

The layered square-planar nickelates, Nd_n+1Ni_nO_2n+2, are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd₆Ni₅O₁₂ thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd₄Ni₃O₁₀, and subsequent reduction to the square-planar phase, Nd₄Ni₃O₈. We synthesize our highest quality Nd₄Ni₃O₁₀ films under compressive strain on LaAlO₃ (001), while Nd₄Ni₃O₁₀ on NdGaO₃ (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd₄Ni₃O₁₀ on SrTiO₃ (001). Films reduced on LaAlO₃ become insulating and form compressive strain-induced c-axis canting defects, while Nd₄Ni₃O₈ films on NdGaO₃ are metallic. This work provides a pathway to the synthesis of Nd_n+1Ni_nO_2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.

Original language	English (US)
Article number	1468
Journal	Nature communications
Volume	14
Issue number	1
DOIs	https://doi.org/10.1038/s41467-023-37117-4
State	Published - Dec 2023
Externally published	Yes

ASJC Scopus subject areas

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
General
Physics and Astronomy(all)

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10.1038/s41467-023-37117-4

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Ferenc Segedin, D., Goodge, B. H., Pan, G. A., Song, Q., LaBollita, H., Jung, M. C., El-Sherif, H., Doyle, S., Turkiewicz, A., Taylor, N. K., Mason, J. A., N’Diaye, A. T., Paik, H., El Baggari, I., Botana, A. S., Kourkoutis, L. F., Brooks, C. M., & Mundy, J. A. (2023). Limits to the strain engineering of layered square-planar nickelate thin films. Nature communications, 14(1), [1468]. https://doi.org/10.1038/s41467-023-37117-4

Ferenc Segedin, D, Goodge, BH, Pan, GA, Song, Q, LaBollita, H, Jung, MC, El-Sherif, H, Doyle, S, Turkiewicz, A, Taylor, NK, Mason, JA, N’Diaye, AT, Paik, H, El Baggari, I, Botana, AS, Kourkoutis, LF, Brooks, CM & Mundy, JA 2023, 'Limits to the strain engineering of layered square-planar nickelate thin films', Nature communications, vol. 14, no. 1, 1468. https://doi.org/10.1038/s41467-023-37117-4

@article{2b2a31305ee2416792447bf6089c2489,

title = "Limits to the strain engineering of layered square-planar nickelate thin films",

abstract = "The layered square-planar nickelates, Ndn+1NinO2n+2, are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd6Ni5O12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd4Ni3O10, and subsequent reduction to the square-planar phase, Nd4Ni3O8. We synthesize our highest quality Nd4Ni3O10 films under compressive strain on LaAlO3 (001), while Nd4Ni3O10 on NdGaO3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd4Ni3O10 on SrTiO3 (001). Films reduced on LaAlO3 become insulating and form compressive strain-induced c-axis canting defects, while Nd4Ni3O8 films on NdGaO3 are metallic. This work provides a pathway to the synthesis of Ndn+1NinO2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.",

author = "{Ferenc Segedin}, Dan and Goodge, {Berit H.} and Pan, {Grace A.} and Qi Song and Harrison LaBollita and Jung, {Myung Chul} and Hesham El-Sherif and Spencer Doyle and Ari Turkiewicz and Taylor, {Nicole K.} and Mason, {Jarad A.} and N{\textquoteright}Diaye, {Alpha T.} and Hanjong Paik and {El Baggari}, Ismail and Botana, {Antia S.} and Kourkoutis, {Lena F.} and Brooks, {Charles M.} and Mundy, {Julia A.}",

note = "Funding Information: D.F.S. and B.H.G. contributed equally to this work. We thank Jennifer E. Hoffman and Michael Hayward for fruitful discussions. We thank H. Hijazi at the Rutgers University Laboratory of Surface Modification for assistance in Rutherford backscattering spectrometry. This project was primarily supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0021925. Materials growth and electron microscopy were supported in part by the Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials (PARADIM) under NSF Cooperative Agreement No. DMR-2039380. Electron microscopy was primarily performed at the Cornell Center for Materials Research (CCMR) Shared Facilities, which are supported by the NSF MRSEC Program (No. DMR-1719875). Additional electron microscopy was performed using the MIT.nano facilities at the Massachusetts Institute of Technology and at Harvard University{\textquoteright}s Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), supported by the NSF division of Electrical, Communications and Cyber Systems (ECCS) under NSF Grant No. 2025158. This work made use of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract No. DE-AC02-05CH11231. D.F.S. acknowledges support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under award no. DE-SC0021925 and from the NSF Graduate Research Fellowship no. DGE-1745303. B.H.G. and L.F.K acknowledge support from PARADIM and the Packard Foundation. G.A.P. acknowledges support from the Paul & Daisy Soros Fellowship for New Americans and from the NSF Graduate Research Fellowship Grant No. DGE-1745303. Q.S. was supported by the STC Center for Integrated Quantum Materials, NSF Grant No. DMR-1231319. H.E.S. and I.E. were supported by the Rowland Institute at Harvard. J. A. Mason acknowledges support from the Arnold and Mabel Beckman Foundation through a Beckman Young Investigator grant. H.L. and A.S.B. acknowledge support from NSF Grant No. DMR 2045826. J.A. Mundy acknowledges support from the Packard Foundation and the Gordon and Betty Moore Foundation{\textquoteright}s EPiQS Initiative, grant GBMF6760. Publisher Copyright: {\textcopyright} 2023, The Author(s).",

year = "2023",

month = dec,

doi = "10.1038/s41467-023-37117-4",

language = "English (US)",

volume = "14",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

number = "1",

}

TY - JOUR

T1 - Limits to the strain engineering of layered square-planar nickelate thin films

AU - Ferenc Segedin, Dan

AU - Goodge, Berit H.

AU - Pan, Grace A.

AU - Song, Qi

AU - LaBollita, Harrison

AU - Jung, Myung Chul

AU - El-Sherif, Hesham

AU - Doyle, Spencer

AU - Turkiewicz, Ari

AU - Taylor, Nicole K.

AU - Mason, Jarad A.

AU - N’Diaye, Alpha T.

AU - Paik, Hanjong

AU - El Baggari, Ismail

AU - Botana, Antia S.

AU - Kourkoutis, Lena F.

AU - Brooks, Charles M.

AU - Mundy, Julia A.

N1 - Funding Information: D.F.S. and B.H.G. contributed equally to this work. We thank Jennifer E. Hoffman and Michael Hayward for fruitful discussions. We thank H. Hijazi at the Rutgers University Laboratory of Surface Modification for assistance in Rutherford backscattering spectrometry. This project was primarily supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0021925. Materials growth and electron microscopy were supported in part by the Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials (PARADIM) under NSF Cooperative Agreement No. DMR-2039380. Electron microscopy was primarily performed at the Cornell Center for Materials Research (CCMR) Shared Facilities, which are supported by the NSF MRSEC Program (No. DMR-1719875). Additional electron microscopy was performed using the MIT.nano facilities at the Massachusetts Institute of Technology and at Harvard University’s Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), supported by the NSF division of Electrical, Communications and Cyber Systems (ECCS) under NSF Grant No. 2025158. This work made use of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract No. DE-AC02-05CH11231. D.F.S. acknowledges support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under award no. DE-SC0021925 and from the NSF Graduate Research Fellowship no. DGE-1745303. B.H.G. and L.F.K acknowledge support from PARADIM and the Packard Foundation. G.A.P. acknowledges support from the Paul & Daisy Soros Fellowship for New Americans and from the NSF Graduate Research Fellowship Grant No. DGE-1745303. Q.S. was supported by the STC Center for Integrated Quantum Materials, NSF Grant No. DMR-1231319. H.E.S. and I.E. were supported by the Rowland Institute at Harvard. J. A. Mason acknowledges support from the Arnold and Mabel Beckman Foundation through a Beckman Young Investigator grant. H.L. and A.S.B. acknowledge support from NSF Grant No. DMR 2045826. J.A. Mundy acknowledges support from the Packard Foundation and the Gordon and Betty Moore Foundation’s EPiQS Initiative, grant GBMF6760. Publisher Copyright: © 2023, The Author(s).

PY - 2023/12

Y1 - 2023/12

N2 - The layered square-planar nickelates, Ndn+1NinO2n+2, are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd6Ni5O12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd4Ni3O10, and subsequent reduction to the square-planar phase, Nd4Ni3O8. We synthesize our highest quality Nd4Ni3O10 films under compressive strain on LaAlO3 (001), while Nd4Ni3O10 on NdGaO3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd4Ni3O10 on SrTiO3 (001). Films reduced on LaAlO3 become insulating and form compressive strain-induced c-axis canting defects, while Nd4Ni3O8 films on NdGaO3 are metallic. This work provides a pathway to the synthesis of Ndn+1NinO2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.

AB - The layered square-planar nickelates, Ndn+1NinO2n+2, are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd6Ni5O12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd4Ni3O10, and subsequent reduction to the square-planar phase, Nd4Ni3O8. We synthesize our highest quality Nd4Ni3O10 films under compressive strain on LaAlO3 (001), while Nd4Ni3O10 on NdGaO3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd4Ni3O10 on SrTiO3 (001). Films reduced on LaAlO3 become insulating and form compressive strain-induced c-axis canting defects, while Nd4Ni3O8 films on NdGaO3 are metallic. This work provides a pathway to the synthesis of Ndn+1NinO2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.

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JO - Nature Communications

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Limits to the strain engineering of layered square-planar nickelate thin films

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