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Decoupling the high-temperature spin-state and insulator-metal transitions in LaCoO3 via heteroepitaxial strain

Jierui Liang, Vipul Chaturvedi, Nileena Nandakumaran, Paromita Dutta, Lucca Figari, Turan Birol, and Chris Leighton*

  • Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455, USA

  • *Contact author: leighton@umn.edu

Phys. Rev. Materials 10, L091404 – Published 23 September, 2026

DOI: https://doi.org/10.1103/j12p-j8my

Abstract

LaCoO3 is a prototypical perovskite oxide, exhibiting simultaneous ∼500−K insulator-metal and spin-state transitions, which have been intensively studied. As is often the case, understanding which of the various coupled degrees of freedom primarily drives the insulator-metal transition (IMT) in LaCoO3 has proven challenging. We show here that heteroepitaxial strain in thin-film LaCoO3 can be used to entirely decouple the high-temperature spin-state and insulator-metal transitions, providing important insight. Specifically, the IMT is found to occur independent of the strain-tuned spin state, establishing that it is the IMT in bulk LaCoO3 that fundamentally drives the high-temperature spin-state transition, not the inverse. The strain dependence of the IMT temperature in thin-film LaCoO3 is then shown to be remarkably consistent with the trend versus cell volume across the bulk RCoO3 series (R=rare-earth). Density-functional theory results on bulk RCoO3 and biaxially strained LaCoO3 support interpretation of these results in terms of trends in electronic bandwidths and orbital degeneracy.

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