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  From antiferromagnetic and hidden order to Pauli paramagnetism in UM2Si2 compounds with 5f electron duality

Amorese, A., Sundermann, M., Leedahl, B., Marino, A., Takegami, D., Gretarsson, H., et al. (2020). From antiferromagnetic and hidden order to Pauli paramagnetism in UM2Si2 compounds with 5f electron duality. Proceedings of the National Academy of Sciences of the United States of America, 1-8. doi:10.1073/pnas.2005701117.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0007-7138-B Version Permalink: http://hdl.handle.net/21.11116/0000-0007-810D-9
Genre: Journal Article

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 Creators:
Amorese, Andrea1, Author              
Sundermann, Martin1, Author              
Leedahl, Brett1, Author              
Marino, Andrea1, Author              
Takegami, Daisuke1, Author              
Gretarsson, Hlynur1, Author              
Gloskovskii, Andrei2, Author
Schlueter, Christoph2, Author
Haverkort, Maurits W.2, Author
Huang, Yingkai2, Author
Szlawska, Maria2, Author
Kaczorowski, Dariusz2, Author
Ran, Sheng2, Author
Maple, M. Brian2, Author
Bauer, Eric D.2, Author
Leithe-Jasper, Andreas3, Author              
Philipp, Hansmann1, Author              
Thalmeier, Peter4, Author              
Tjeng, Liu Hao5, Author              
Severing, Andrea1, Author              
Affiliations:
1Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863445              
2External Organizations, ou_persistent22              
3Andreas Leithe-Jasper, Chemical Metal Science, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863406              
4Peter Thalmeier, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863457              
5Liu Hao Tjeng, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863452              

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 Abstract: The interplay of band-formation and electron-correlation effects in uranium heavy fermion compounds is the subject of an ongoing debate. Here unexpected insight has been gained from advanced spectroscopies on isostructural members of the UM2Si2 family with different properties. The antiferromagnetic (M = Pd,Ni), hidden order (M = Ru), and Pauli-paramagnetic (M = Fe) compounds all exhibit atomic-like U 5f2 multiplet states with singlet–singlet (quasi-doublet) symmetry while the U 5f3 weight increases from Pd→Ni→Ru→Fe, indicating increasing itineracy. This reveals the dual nature of the U-5f electrons throughout the family; the local aspects persist in the hidden-order compound URu2Si2 and surprisingly even in the highly itinerant Pauli paramagnet UFe2Si2. This study gives guidelines for the theoretical treatment of U intermetallic systems.Using inelastic X-ray scattering beyond the dipole limit and hard X-ray photoelectron spectroscopy we establish the dual nature of the U 5f electrons in UM2Si2 (M = Pd, Ni, Ru, Fe), regardless of their degree of delocalization. We have observed that the compounds have in common a local atomic-like state that is well described by the U 5f2 configuration with the Γ1(1) and Γ2 quasi-doublet symmetry. The amount of the U 5f3 configuration, however, varies considerably across the UM2Si2 series, indicating an increase of U 5f itineracy in going from M = Pd to Ni to Ru and to the Fe compound. The identified electronic states explain the formation of the very large ordered magnetic moments in UPd2Si2 and UNi2Si2, the availability of orbital degrees of freedom needed for the hidden order in URu2Si2 to occur, as well as the appearance of Pauli paramagnetism in UFe2Si2. A unified and systematic picture of the UM2Si2 compounds may now be drawn, thereby providing suggestions for additional experiments to induce hidden order and/or superconductivity in U compounds with the tetragonal body-centered ThCr2Si2 structure.All data are available upon request.

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Language(s): eng - English
 Dates: 2020-11-172020-11-17
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1073/pnas.2005701117
 Degree: -

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Title: Proceedings of the National Academy of Sciences of the United States of America
  Other : PNAS
  Other : Proceedings of the National Academy of Sciences of the USA
  Abbreviation : Proc. Natl. Acad. Sci. U. S. A.
Source Genre: Journal
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Affiliations:
Publ. Info: Washington, D.C. : National Academy of Sciences
Pages: 202005701 Volume / Issue: - Sequence Number: - Start / End Page: 1 - 8 Identifier: ISSN: 0027-8424
CoNE: https://pure.mpg.de/cone/journals/resource/954925427230