Chemical design of electronic and magnetic energy scales of tetravalent praseodymium materials

Arun Ramanathan, Jensen Kaplan, Dumitru-Claudiu Sergentu, Jacob A. Branson, Mykhaylo Ozerov, Alexander I. Kolesnikov, Stefan G. Minasian, Jochen Autschbach, John W. Freeland, Zhigang Jiang, Martin Mourigal and Henry S. La Pierre ()
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Arun Ramanathan: Georgia Institute of Technology
Jensen Kaplan: Georgia Institute of Technology
Dumitru-Claudiu Sergentu: University of Rennes, CNRS ISCR (Institut des Sciences Chimiques de Rennes) - UMR 6226
Jacob A. Branson: University of California
Mykhaylo Ozerov: Florida State University
Alexander I. Kolesnikov: Oak Ridge National Laboratory
Stefan G. Minasian: Lawrence Berkeley National Laboratory
Jochen Autschbach: University at Buffalo, State University of New York
John W. Freeland: Argonne National Laboratory
Zhigang Jiang: Georgia Institute of Technology
Martin Mourigal: Georgia Institute of Technology
Henry S. La Pierre: Georgia Institute of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Lanthanides in the trivalent oxidation state are typically described using an ionic picture that leads to localized magnetic moments. The hierarchical energy scales associated with trivalent lanthanides produce desirable properties for e.g., molecular magnetism, quantum materials, and quantum transduction. Here, we show that this traditional ionic paradigm breaks down for praseodymium in the tetravalent oxidation state. Synthetic, spectroscopic, and theoretical tools deployed on several solid-state Pr4+-oxides uncover the unusual participation of 4f orbitals in bonding and the anomalous hybridization of the 4f1 configuration with ligand valence electrons, analogous to transition metals. The competition between crystal-field and spin-orbit-coupling interactions fundamentally transforms the spin-orbital magnetism of Pr4+, which departs from the Jeff = 1/2 limit and resembles that of high-valent actinides. Our results show that Pr4+ ions are in a class on their own, where the hierarchy of single-ion energy scales can be tailored to explore new correlated phenomena in quantum materials.

Date: 2023
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DOI: 10.1038/s41467-023-38431-7

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