Stabilization of a non-superconducting, orthorhombic phase by over-hydrogenating LaFeSiH

Fuente: arXiv
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Autores principales: Hansen, M. F., Lepoittevin, C., Vaney, J. -B., Boullay, P., Nassif, V., Sulpice, A., Mayaffre, H., Julien, M. -H., Tencé, S., Toulemonde, P.
Formato: Preprint
Publicado: 2026
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author Hansen, M. F.
Lepoittevin, C.
Vaney, J. -B.
Boullay, P.
Nassif, V.
Sulpice, A.
Mayaffre, H.
Julien, M. -H.
Tencé, S.
Toulemonde, P.
author_facet Hansen, M. F.
Lepoittevin, C.
Vaney, J. -B.
Boullay, P.
Nassif, V.
Sulpice, A.
Mayaffre, H.
Julien, M. -H.
Tencé, S.
Toulemonde, P.
contents Chemical composition provides a powerful route to tune the electronic ground state of iron-based superconductors and other quantum materials, yet access to highly doped phases remains limited. Here we demonstrate that high-pressure thermal decomposition of hydrogen-rich precursors enables over-hydrogenation of LaFeSi. Using anthracene, we synthesize tetragonal superconducting LaFeSiH, including a single hydrogen site, while ammonia borane yields a structurally distorted over-hydrogenated phase, LaFeSiH1+x, with an orthorhombic structure. Chemical analysis reveal excess hydrogen (x ~ 0.6), implying a second H site in LaFeSiH1.6 whose localization and occupancy are determined by neutron diffraction. In contrast to metallic LaFeSi and superconducting LaFeSiH, orthorhombic LaFeSiH1.6 exhibits semiconductor-like behavior. Upon hydrogen release near 100 °C, it transforms into tetragonal superconducting LaFeSiH1+δ (δ << 0.6). These results establish the chemical flexibility of the layered LaFeSiX (X = H, O, F) family and provide access to a high hydrogen-doping regime, creating new opportunities to investigate superconductivity in Fe-based silicides.
format Preprint
id arxiv_https___arxiv_org_abs_2604_20716
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Stabilization of a non-superconducting, orthorhombic phase by over-hydrogenating LaFeSiH
Hansen, M. F.
Lepoittevin, C.
Vaney, J. -B.
Boullay, P.
Nassif, V.
Sulpice, A.
Mayaffre, H.
Julien, M. -H.
Tencé, S.
Toulemonde, P.
Superconductivity
Chemical composition provides a powerful route to tune the electronic ground state of iron-based superconductors and other quantum materials, yet access to highly doped phases remains limited. Here we demonstrate that high-pressure thermal decomposition of hydrogen-rich precursors enables over-hydrogenation of LaFeSi. Using anthracene, we synthesize tetragonal superconducting LaFeSiH, including a single hydrogen site, while ammonia borane yields a structurally distorted over-hydrogenated phase, LaFeSiH1+x, with an orthorhombic structure. Chemical analysis reveal excess hydrogen (x ~ 0.6), implying a second H site in LaFeSiH1.6 whose localization and occupancy are determined by neutron diffraction. In contrast to metallic LaFeSi and superconducting LaFeSiH, orthorhombic LaFeSiH1.6 exhibits semiconductor-like behavior. Upon hydrogen release near 100 °C, it transforms into tetragonal superconducting LaFeSiH1+δ (δ << 0.6). These results establish the chemical flexibility of the layered LaFeSiX (X = H, O, F) family and provide access to a high hydrogen-doping regime, creating new opportunities to investigate superconductivity in Fe-based silicides.
title Stabilization of a non-superconducting, orthorhombic phase by over-hydrogenating LaFeSiH
topic Superconductivity
url https://arxiv.org/abs/2604.20716