Topotactic fluorination of intermetallics as an efficient route towards quantum materials

Jean-Baptiste Vaney, Baptiste Vignolle, Alain Demourgues, Etienne Gaudin, Etienne Durand, Christine Labrugère, Fabio Bernardini, Andrés Cano and Sophie Tencé ()
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Jean-Baptiste Vaney: CNRS, Université Bordeaux, Bordeaux INP, ICMCB, UMR 5026
Baptiste Vignolle: CNRS, Université Bordeaux, Bordeaux INP, ICMCB, UMR 5026
Alain Demourgues: CNRS, Université Bordeaux, Bordeaux INP, ICMCB, UMR 5026
Etienne Gaudin: CNRS, Université Bordeaux, Bordeaux INP, ICMCB, UMR 5026
Etienne Durand: CNRS, Université Bordeaux, Bordeaux INP, ICMCB, UMR 5026
Christine Labrugère: CNRS, Univ. Bordeaux, PLACAMAT UMS 3626
Fabio Bernardini: Dipartimento di Fisica, Università di Cagliari
Andrés Cano: CNRS, Université Grenoble Alpes, Institut Néel
Sophie Tencé: CNRS, Université Bordeaux, Bordeaux INP, ICMCB, UMR 5026

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Intermetallics represent an important family of compounds, in which insertion of light elements (H, B, C, N) has been widely explored for decades to synthesize novel phases and promote functional materials such as permanent magnets or magnetocalorics. Fluorine insertion, however, has remained elusive so far since the strong reactivity of this atypical element, the most electronegative one, tends to produce the chemical decomposition of these systems. Here, we introduce a topochemical method to intercalate fluorine atoms into intermetallics, using perfluorocarbon reactant with covalent C-F bonds. We demonstrate the potential of this approach with the synthesis of non-stoichiometric mixed anion (Si-F) LaFeSiFx single-crystals, which are further shown to host FeSi-based superconductivity. Fluorine topochemistry on intermetallics is thus proven to be an effective route to provide functional materials where the coexistence of ionic and metallo-covalent blocks, and their interactions through inductive effects, is at the root of their functional properties.

Date: 2022
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DOI: 10.1038/s41467-022-29043-8

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