[OsF6]x−: Molecular Models for Spin-Orbit Entangled Phenomena

Kasper S. Pedersen; Daniel N. Woodruff; Saurabh Kumar Singh; Alain Tressaud; Etienne Durand; Mihail Atanasov; Panagiota Perlepe; Katharina Ollefs; Fabrice Wilhelm; Corine Mathonière; Frank Neese; Andrei Rogalev; Jesper Bendix; Rodolphe Clérac

doi:10.1002/chem.201702894

[OsF₆]^x−: Molecular Models for Spin-Orbit Entangled Phenomena

Kasper S. Pedersen
, Daniel N. Woodruff
, Saurabh Kumar Singh
, Alain Tressaud
, Etienne Durand
, Mihail Atanasov
, Panagiota Perlepe
, Katharina Ollefs
, Fabrice Wilhelm
, Corine Mathonière
, Frank Neese
, Andrei Rogalev
, Jesper Bendix
, Rodolphe Clérac

Nanoporous Materials Genome Center

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

Heavy 5d elements, like osmium, feature strong spin-orbit interactions which are at the origin of exotic physical behaviors. Revealing the full potential of, for example, novel osmium oxide materials (“osmates”) is however contingent upon a detailed understanding of the local single-ion properties. Herein, two molecular osmate analogues, [OsF₆]²⁻ and [OsF₆]⁻, are reported as model systems for Os⁴⁺ and Os⁵⁺ centers found in oxides. Using X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) techniques, combined with state-of-the-art ab initio calculations, their ground state was elucidated; mirroring the osmium electronic structure in osmates. The realization of such molecular model systems provides a unique chemical playground to engineer materials exhibiting spin-orbit entangled phenomena.

Original language	English (US)
Pages (from-to)	11244-11248
Number of pages	5
Journal	Chemistry - A European Journal
Volume	23
Issue number	47
DOIs	https://doi.org/10.1002/chem.201702894
State	Published - Aug 22 2017

Bibliographical note

Funding Information:
The authors thank E. Lebraud, S. Exiga, M. Rouzi?res, and P. Voisin for technical and experimental assistance. The X-ray spectroscopy experiments were performed at the European Synchrotron Radiation Facility (ESRF, Grenoble, France). K.S.P. and R.C. thank the Danish Research Council for Independent Research for a DFF-Sapere Aude Research Talent grant (4090-00201), the University of Bordeaux, the R?gion Nouvelle Aquitaine, the CNRS and the GdR MCM-2: Magn?tisme et Commutation Mol?culaires.

Publisher Copyright:
© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

5d elements
X-ray spectroscopy
ab initio calculations
magnetism
osmium
spin-orbit interaction

Publisher link

10.1002/chem.201702894

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@article{fd5ec6b305f4432c972f0d40c76986b7,

title = "[OsF6]x−: Molecular Models for Spin-Orbit Entangled Phenomena",

abstract = "Heavy 5d elements, like osmium, feature strong spin-orbit interactions which are at the origin of exotic physical behaviors. Revealing the full potential of, for example, novel osmium oxide materials (“osmates”) is however contingent upon a detailed understanding of the local single-ion properties. Herein, two molecular osmate analogues, [OsF6]2− and [OsF6]−, are reported as model systems for Os4+ and Os5+ centers found in oxides. Using X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) techniques, combined with state-of-the-art ab initio calculations, their ground state was elucidated; mirroring the osmium electronic structure in osmates. The realization of such molecular model systems provides a unique chemical playground to engineer materials exhibiting spin-orbit entangled phenomena.",

keywords = "5d elements, X-ray spectroscopy, ab initio calculations, magnetism, osmium, spin-orbit interaction",

author = "Pedersen, \{Kasper S.\} and Woodruff, \{Daniel N.\} and Singh, \{Saurabh Kumar\} and Alain Tressaud and Etienne Durand and Mihail Atanasov and Panagiota Perlepe and Katharina Ollefs and Fabrice Wilhelm and Corine Mathoni{\`e}re and Frank Neese and Andrei Rogalev and Jesper Bendix and Rodolphe Cl{\'e}rac",

note = "Funding Information: The authors thank E. Lebraud, S. Exiga, M. Rouzi?res, and P. Voisin for technical and experimental assistance. The X-ray spectroscopy experiments were performed at the European Synchrotron Radiation Facility (ESRF, Grenoble, France). K.S.P. and R.C. thank the Danish Research Council for Independent Research for a DFF-Sapere Aude Research Talent grant (4090-00201), the University of Bordeaux, the R?gion Nouvelle Aquitaine, the CNRS and the GdR MCM-2: Magn?tisme et Commutation Mol?culaires. Publisher Copyright: {\textcopyright} 2017 Wiley-VCH Verlag GmbH \& Co. KGaA, Weinheim",

year = "2017",

month = aug,

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doi = "10.1002/chem.201702894",

language = "English (US)",

volume = "23",

pages = "11244--11248",

journal = "Chemistry - A European Journal",

issn = "0947-6539",

publisher = "John Wiley and Sons Inc.",

number = "47",

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T1 - [OsF6]x−

T2 - Molecular Models for Spin-Orbit Entangled Phenomena

AU - Pedersen, Kasper S.

AU - Woodruff, Daniel N.

AU - Singh, Saurabh Kumar

AU - Tressaud, Alain

AU - Durand, Etienne

AU - Atanasov, Mihail

AU - Perlepe, Panagiota

AU - Ollefs, Katharina

AU - Wilhelm, Fabrice

AU - Mathonière, Corine

AU - Neese, Frank

AU - Rogalev, Andrei

AU - Bendix, Jesper

AU - Clérac, Rodolphe

N1 - Funding Information: The authors thank E. Lebraud, S. Exiga, M. Rouzi?res, and P. Voisin for technical and experimental assistance. The X-ray spectroscopy experiments were performed at the European Synchrotron Radiation Facility (ESRF, Grenoble, France). K.S.P. and R.C. thank the Danish Research Council for Independent Research for a DFF-Sapere Aude Research Talent grant (4090-00201), the University of Bordeaux, the R?gion Nouvelle Aquitaine, the CNRS and the GdR MCM-2: Magn?tisme et Commutation Mol?culaires. Publisher Copyright: © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2017/8/22

Y1 - 2017/8/22

N2 - Heavy 5d elements, like osmium, feature strong spin-orbit interactions which are at the origin of exotic physical behaviors. Revealing the full potential of, for example, novel osmium oxide materials (“osmates”) is however contingent upon a detailed understanding of the local single-ion properties. Herein, two molecular osmate analogues, [OsF6]2− and [OsF6]−, are reported as model systems for Os4+ and Os5+ centers found in oxides. Using X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) techniques, combined with state-of-the-art ab initio calculations, their ground state was elucidated; mirroring the osmium electronic structure in osmates. The realization of such molecular model systems provides a unique chemical playground to engineer materials exhibiting spin-orbit entangled phenomena.

AB - Heavy 5d elements, like osmium, feature strong spin-orbit interactions which are at the origin of exotic physical behaviors. Revealing the full potential of, for example, novel osmium oxide materials (“osmates”) is however contingent upon a detailed understanding of the local single-ion properties. Herein, two molecular osmate analogues, [OsF6]2− and [OsF6]−, are reported as model systems for Os4+ and Os5+ centers found in oxides. Using X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) techniques, combined with state-of-the-art ab initio calculations, their ground state was elucidated; mirroring the osmium electronic structure in osmates. The realization of such molecular model systems provides a unique chemical playground to engineer materials exhibiting spin-orbit entangled phenomena.

KW - 5d elements

KW - X-ray spectroscopy

KW - ab initio calculations

KW - magnetism

KW - osmium

KW - spin-orbit interaction

UR - https://www.scopus.com/pages/publications/85026405833

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DO - 10.1002/chem.201702894

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JO - Chemistry - A European Journal

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