Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice

Abstract Anion doping offers immense potential for tailoring material properties, but precise control over anion incorporation remains challenging due to complex synthesis and limitations in dopant detection. This study investigates F-ion intercalation within an infinite-layer NdNiO2+x /SrTiO3 super...

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Main Authors: Chao Yang, Roberto A. Ortiz, Hongguang Wang, Wilfried Sigle, Kelvin Anggara, Eva Benckiser, Bernhard Keimer, Peter A. van Aken
Format: Article
Language:English
Published: Nature Portfolio 2025-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-58646-0
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author Chao Yang
Roberto A. Ortiz
Hongguang Wang
Wilfried Sigle
Kelvin Anggara
Eva Benckiser
Bernhard Keimer
Peter A. van Aken
author_facet Chao Yang
Roberto A. Ortiz
Hongguang Wang
Wilfried Sigle
Kelvin Anggara
Eva Benckiser
Bernhard Keimer
Peter A. van Aken
author_sort Chao Yang
collection DOAJ
description Abstract Anion doping offers immense potential for tailoring material properties, but precise control over anion incorporation remains challenging due to complex synthesis and limitations in dopant detection. This study investigates F-ion intercalation within an infinite-layer NdNiO2+x /SrTiO3 superlattice using a two-step process. We employ advanced four-dimensional scanning transmission electron microscopy (4D-STEM) coupled with electron energy loss spectroscopy (EELS) to map the F distribution and its impact on the atomic and electronic structure. Our observations reveal a fluorination-induced geometric reconstruction of the infinite layer structure, resulting in a more distorted orthorhombic phase compared to the pristine perovskite. F-ion are primarily located at apical polyhedral sites, with some basal sites occupation in localized regions, leading to the formation of two distinct domains. These domains reflect a competition between polyhedral distortion and Nd displacement at domain interfaces. Interestingly, we observe an anomalous structural distortion where basal site anions are displaced in the same direction as Nd atoms, potentially linked to the partial basal site F-ion occupation. This coexistence of diverse structural distortions signifies a locally disordered F-ion distribution with distinct configurations. These findings provide crucial insights into the mechanisms of anion doping at the atomic level, contributing to the design of materials with tailored functionalities.
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spelling doaj-art-c92a4d142acc49fb8397901fb4d569652025-08-20T01:54:25ZengNature PortfolioNature Communications2041-17232025-04-011611910.1038/s41467-025-58646-0Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlatticeChao Yang0Roberto A. Ortiz1Hongguang Wang2Wilfried Sigle3Kelvin Anggara4Eva Benckiser5Bernhard Keimer6Peter A. van Aken7Max Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchMax Planck Institute for Solid State ResearchAbstract Anion doping offers immense potential for tailoring material properties, but precise control over anion incorporation remains challenging due to complex synthesis and limitations in dopant detection. This study investigates F-ion intercalation within an infinite-layer NdNiO2+x /SrTiO3 superlattice using a two-step process. We employ advanced four-dimensional scanning transmission electron microscopy (4D-STEM) coupled with electron energy loss spectroscopy (EELS) to map the F distribution and its impact on the atomic and electronic structure. Our observations reveal a fluorination-induced geometric reconstruction of the infinite layer structure, resulting in a more distorted orthorhombic phase compared to the pristine perovskite. F-ion are primarily located at apical polyhedral sites, with some basal sites occupation in localized regions, leading to the formation of two distinct domains. These domains reflect a competition between polyhedral distortion and Nd displacement at domain interfaces. Interestingly, we observe an anomalous structural distortion where basal site anions are displaced in the same direction as Nd atoms, potentially linked to the partial basal site F-ion occupation. This coexistence of diverse structural distortions signifies a locally disordered F-ion distribution with distinct configurations. These findings provide crucial insights into the mechanisms of anion doping at the atomic level, contributing to the design of materials with tailored functionalities.https://doi.org/10.1038/s41467-025-58646-0
spellingShingle Chao Yang
Roberto A. Ortiz
Hongguang Wang
Wilfried Sigle
Kelvin Anggara
Eva Benckiser
Bernhard Keimer
Peter A. van Aken
Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice
Nature Communications
title Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice
title_full Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice
title_fullStr Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice
title_full_unstemmed Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice
title_short Atomic-scale observation of geometric reconstruction in a fluorine-intercalated infinite layer nickelate superlattice
title_sort atomic scale observation of geometric reconstruction in a fluorine intercalated infinite layer nickelate superlattice
url https://doi.org/10.1038/s41467-025-58646-0
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