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

Nat Commun. 2023 Mar 16;14(1):1468. doi: 10.1038/s41467-023-37117-4.

Authors

Dan Ferenc Segedin^#¹, Berit H Goodge^#^{2

3}, Grace A Pan¹, Qi Song¹, Harrison LaBollita⁴, Myung-Chul Jung⁴, Hesham El-Sherif⁵, Spencer Doyle¹, Ari Turkiewicz¹, Nicole K Taylor⁶, Jarad A Mason⁷, Alpha T N'Diaye⁸, Hanjong Paik^{9

10}, Ismail El Baggari⁵, Antia S Botana⁴, Lena F Kourkoutis^{2

3}, Charles M Brooks¹, Julia A Mundy¹¹

Affiliations

¹ Department of Physics, Harvard University, Cambridge, MA, USA.
² School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA.
³ Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY, USA.
⁴ Department of Physics, Arizona State University, Tempe, AZ, USA.
⁵ The Rowland Institute, Harvard University, Cambridge, MA, USA.
⁶ School of Engineering and Applied Science, Harvard University, Cambridge, MA, USA.
⁷ Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA.
⁸ Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
⁹ Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials (PARADIM), Cornell University, Ithaca, NY, USA.
¹⁰ School of Electrical and Computer Engineering, University of Oklahoma, Norman, OK, USA.
¹¹ Department of Physics, Harvard University, Cambridge, MA, USA. mundy@fas.harvard.edu.

^# Contributed equally.

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.