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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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Item Permalink: http://hdl.handle.net/21.11116/0000-0005-9E99-D Version Permalink: http://hdl.handle.net/21.11116/0000-0005-9E9B-B
Genre: Journal Article

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Knaflič, T.1, Author
Jeglič, P.1, Author
Komelj, M.1, Author
Zorko, A.1, Author
Biswas, P. K.1, Author
Ponomaryov, A. N.1, Author
Zvyagin, S. A.1, Author
Reehuis, M.1, Author
Hoser, A.1, Author
Geiß, M.1, Author
Janek, J.1, Author
Adler, P.2, Author              
Felser, C.3, Author              
Jansen, M.4, Author              
Arčon, D.1, Author
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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 Abstract: 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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Language(s): eng - English
 Dates: 2020
 Publication Status: Published online
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Title: Physical Review B
  Abbreviation : Phys. Rev. B
Source Genre: Journal
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Publ. Info: Woodbury, NY : American Physical Society
Pages: - Volume / Issue: 101 (2) Sequence Number: 024419 Start / End Page: 1 - 13 Identifier: ISSN: 1098-0121
CoNE: https://pure.mpg.de/cone/journals/resource/954925225008