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Spin-orbit coupling in a half-filled 𝑡2⁢𝑔 shell: The case of 5⁢𝑑3 K2⁢ReCl6
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Number of Authors: 122024 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 109, no 15, article id 155149Article in journal (Refereed) Published
Abstract [en]

The half-filled 𝑡2⁢𝑔 shell of the configuration usually, in 𝐿⁢𝑆 coupling, hosts a 𝑆=3/2 ground state with quenched orbital moment. This state is not Jahn-Teller active. Sufficiently large spin-orbit coupling 𝜁 has been predicted to change this picture by mixing in orbital moment, giving rise to a sizable Jahn-Teller distortion. In 5⁢𝑑3K2⁢ReCl6 we study the electronic excitations using resonant inelastic x-ray scattering and optical spectroscopy. We observe on-site intra-𝑡2⁢𝑔 excitations below 2 eV and corresponding overtones with two intra-𝑡2⁢𝑔 excitations on adjacent sites, the Mott gap at 2.7 eV, 𝑡2⁢𝑔-to-𝑒𝑔 excitations above 3 eV, and charge-transfer excitations at still higher energy. The intra-𝑡2⁢𝑔 excitation energies are a sensitive measure of 𝜁 and Hund's coupling 𝐽H. The sizable value of 𝜁≈0.29eV places K2⁢ReCl6 into the intermediate coupling regime, but 𝜁/𝐽H≈0.6 is not sufficiently large to drive a pronounced Jahn-Teller effect. We discuss the ground state wave function in a Kanamori picture and find that the 𝑆=3/2 multiplet still carries about 97% of the weight. However, the finite admixture of orbital moment allows for subtle effects. We discuss small temperature-induced changes of the optical data and find evidence for a lowering of the ground state by about 3 meV below the structural phase transitions.

Place, publisher, year, edition, pages
2024. Vol. 109, no 15, article id 155149
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Condensed Matter Physics
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URN: urn:nbn:se:su:diva-232529DOI: 10.1103/PhysRevB.109.155149ISI: 001229774400001Scopus ID: 2-s2.0-85190890367OAI: oai:DiVA.org:su-232529DiVA, id: diva2:1890381
Available from: 2024-08-19 Created: 2024-08-19 Last updated: 2024-08-19Bibliographically approved

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Hermanns, Maria

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