Room-temperature valence transition in a strain-tuned perovskite oxide

Vipul Chaturvedi, Supriya Ghosh, Dominique Gautreau, William M. Postiglione, John E. Dewey, Patrick Quarterman, Purnima P. Balakrishnan, Brian J. Kirby, Hua Zhou, Huikai Cheng, Amanda Huon, Timothy Charlton, Michael R. Fitzsimmons, Caroline Korostynski, Andrew Jacobson, Lucca Figari, Javier Garcia Barriocanal, Turan Birol, K. Andre Mkhoyan and Chris Leighton ()
Additional contact information
Vipul Chaturvedi: University of Minnesota
Supriya Ghosh: University of Minnesota
Dominique Gautreau: University of Minnesota
William M. Postiglione: University of Minnesota
John E. Dewey: University of Minnesota
Patrick Quarterman: NIST Center for Neutron Research, National Institute of Standards and Technology
Purnima P. Balakrishnan: NIST Center for Neutron Research, National Institute of Standards and Technology
Brian J. Kirby: NIST Center for Neutron Research, National Institute of Standards and Technology
Hua Zhou: Advanced Photon Source, Argonne National Laboratory
Huikai Cheng: Thermo Fisher Scientific
Amanda Huon: Neutron Scattering Division, Oak Ridge National Lab
Timothy Charlton: Neutron Scattering Division, Oak Ridge National Lab
Michael R. Fitzsimmons: Neutron Scattering Division, Oak Ridge National Lab
Caroline Korostynski: University of Minnesota
Andrew Jacobson: University of Minnesota
Lucca Figari: University of Minnesota
Javier Garcia Barriocanal: University of Minnesota
Turan Birol: University of Minnesota
K. Andre Mkhoyan: University of Minnesota
Chris Leighton: University of Minnesota

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Cobalt oxides have long been understood to display intriguing phenomena known as spin-state crossovers, where the cobalt ion spin changes vs. temperature, pressure, etc. A very different situation was recently uncovered in praseodymium-containing cobalt oxides, where a first-order coupled spin-state/structural/metal-insulator transition occurs, driven by a remarkable praseodymium valence transition. Such valence transitions, particularly when triggering spin-state and metal-insulator transitions, offer highly appealing functionality, but have thus far been confined to cryogenic temperatures in bulk materials (e.g., 90 K in Pr1-xCaxCoO3). Here, we show that in thin films of the complex perovskite (Pr1-yYy)1-xCaxCoO3-δ, heteroepitaxial strain tuning enables stabilization of valence-driven spin-state/structural/metal-insulator transitions to at least 291 K, i.e., around room temperature. The technological implications of this result are accompanied by fundamental prospects, as complete strain control of the electronic ground state is demonstrated, from ferromagnetic metal under tension to nonmagnetic insulator under compression, thereby exposing a potential novel quantum critical point.

Date: 2022
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DOI: 10.1038/s41467-022-35024-8

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