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  Spin-dimer ground state driven by consecutive charge and orbital ordering transitions in the anionic mixed-valence compound Rb4O6

Knaflič, T., Jeglič, P., Komelj, M., Zorko, A., Biswas, P. K., Ponomaryov, A. N., et al. (2020). Spin-dimer ground state driven by consecutive charge and orbital ordering transitions in the anionic mixed-valence compound Rb4O6. Physical Review B, 101(2): 024419, pp. 1-13. doi:10.1103/PhysRevB.101.024419.

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Knaflič, T.1, Autor
Jeglič, P.1, Autor
Komelj, M.1, Autor
Zorko, A.1, Autor
Biswas, P. K.1, Autor
Ponomaryov, A. N.1, Autor
Zvyagin, S. A.1, Autor
Reehuis, M.1, Autor
Hoser, A.1, Autor
Geiß, M.1, Autor
Janek, J.1, Autor
Adler, P.2, Autor           
Felser, C.3, Autor           
Jansen, M.4, Autor           
Arčon, D.1, Autor
Affiliations:
1External Organizations, ou_persistent22              
2Peter Adler, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863435              
3Claudia Felser, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863429              
4Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863425              

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 Zusammenfassung: Recently, a Verwey-type transition in the mixed-valence alkali sesquioxide Cs4O6 was deduced from the charge ordering of molecular peroxide O-2(2-) and superoxide O-2(-) anions accompanied by the structural transformation and a dramatic change in electronic conductivity [Adler et al., Sci. Adv. 4, eaap7581 (2018)]. Here, we report that in the sister compound Rb4O6, a similar Verwey-type charge ordering transition is strongly linked to O-2(-) orbital and spin dynamics. On cooling, a powder neutron diffraction experiment reveals a charge ordering and a cubic-to-tetragonal transition at T-CO = 290 K, which is followed by a further structural instability at T-s = 92 K that involves an additional reorientation of magnetic O-2(-) anions. Magnetic resonance techniques supported by density functional theory computations suggest the emergence of a peculiar type of pi*-orbital ordering of the magnetically active O-2(-) units, which promotes the formation of a quantum spin state composed of weakly coupled spin dimers. These results reveal that as in 3d transition-metal compounds, also in the pi* open-shell alkali sesquioxides the interplay between Jahn-Teller-like electron-lattice coupling and Kugel-Khomskii-type superexchange determines the nature of orbital ordering and the magnetic ground state.

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Sprache(n): eng - English
 Datum: 2020
 Publikationsstatus: Online veröffentlicht
 Seiten: -
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: -
 Identifikatoren: ISI: 000509474400006
DOI: 10.1103/PhysRevB.101.024419
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Titel: Physical Review B
  Kurztitel : Phys. Rev. B
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Woodbury, NY : American Physical Society
Seiten: - Band / Heft: 101 (2) Artikelnummer: 024419 Start- / Endseite: 1 - 13 Identifikator: ISSN: 1098-0121
CoNE: https://pure.mpg.de/cone/journals/resource/954925225008