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

Vipul Chaturvedi, Supriya Ghosh, Dominique M 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, Chris Leighton

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

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.

Original languageEnglish (US)
Article number7774
JournalNature communications
Volume13
Issue number1
DOIs
StatePublished - Dec 2022

Bibliographical note

Funding Information:
We gratefully acknowledge helpful comments and input from R. Fernandes. Work at the University of Minnesota (UMN) was primarily funded by the Department of Energy (DOE) through the UMN Center for Quantum Materials under Grant Number DE-SC0016371 (CL). Electron microscopy by SG and KAM was supported by the National Science Foundation (NSF) through the UMN MRSEC under DMR-2011401 (KAM). Parts of the work were performed in the Characterization Facility, UMN, which receives partial support from the NSF through the MRSEC and NNCI programs. Part of this work also used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Aspects of this work additionally used resources of the Advanced Photon Source, a DOE Office of Science User Facility operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Certain commercial equipment, instruments, or materials are identified in this paper to foster understanding. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the materials or equipment identified are necessarily the best available for the purpose.

Funding Information:
We gratefully acknowledge helpful comments and input from R. Fernandes. Work at the University of Minnesota (UMN) was primarily funded by the Department of Energy (DOE) through the UMN Center for Quantum Materials under Grant Number DE-SC0016371 (CL). Electron microscopy by SG and KAM was supported by the National Science Foundation (NSF) through the UMN MRSEC under DMR-2011401 (KAM). Parts of the work were performed in the Characterization Facility, UMN, which receives partial support from the NSF through the MRSEC and NNCI programs. Part of this work also used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Aspects of this work additionally used resources of the Advanced Photon Source, a DOE Office of Science User Facility operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Certain commercial equipment, instruments, or materials are identified in this paper to foster understanding. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the materials or equipment identified are necessarily the best available for the purpose.

Publisher Copyright:
© 2022, The Author(s).

MRSEC Support

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  • Journal Article

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