Atomic-scale observation of geometric frustration in a fluorine-intercalated infinite layer nickelate superlattice
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arXiv
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| Autori principali: | , , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2024
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| _version_ | 1866912006158680064 |
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| author | Yang, Chao Ortiz, Roberto A. Wang, Hongguang Sigle, Wilfried Anggara, Kelvin Benckiser, Eva Keimer, Bernhard van Aken, Peter A. |
| author_facet | Yang, Chao Ortiz, Roberto A. Wang, Hongguang Sigle, Wilfried Anggara, Kelvin Benckiser, Eva Keimer, Bernhard van Aken, Peter A. |
| contents | Anion doping offers immense potential for tailoring material properties, but achieving precise control over anion incorporation remains a challenge due to complex synthesis processes and limitations in local dopant detection. Here, we investigate the F-ion intercalation within an infinite layer NdNiO2+x/SrTiO3 superlattice film using a two-step synthesis approach. We employ advanced four-dimensional scanning transmission electron microscopy (4D-STEM) coupled with electron energy loss spectroscopy to map the F distribution and its impact on the atomic and electronic structure. Our observations reveal a striking geometric reconstruction of the infinite layer structure upon fluorination, resulting in a more distorted orthorhombic phase compared to the pristine perovskite. Notably, F-ion intercalation occurs primarily at the apical sites of the polyhedron, with some occupation of basal sites in localized regions. This process leads to the formation of two distinct domains within the nickelate layer, reflecting a competition between polyhedral distortion and geometric frustration-induced neodymium (Nd) displacement near 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 within the infinite layer structure with distinct F-ion configurations. These findings provide crucial insights into understanding and manipulating anion doping at the atomic level, paving the way for the development of novel materials with precisely controlled functionalities. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2408_14157 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Atomic-scale observation of geometric frustration in a fluorine-intercalated infinite layer nickelate superlattice Yang, Chao Ortiz, Roberto A. Wang, Hongguang Sigle, Wilfried Anggara, Kelvin Benckiser, Eva Keimer, Bernhard van Aken, Peter A. Materials Science Mesoscale and Nanoscale Physics Anion doping offers immense potential for tailoring material properties, but achieving precise control over anion incorporation remains a challenge due to complex synthesis processes and limitations in local dopant detection. Here, we investigate the F-ion intercalation within an infinite layer NdNiO2+x/SrTiO3 superlattice film using a two-step synthesis approach. We employ advanced four-dimensional scanning transmission electron microscopy (4D-STEM) coupled with electron energy loss spectroscopy to map the F distribution and its impact on the atomic and electronic structure. Our observations reveal a striking geometric reconstruction of the infinite layer structure upon fluorination, resulting in a more distorted orthorhombic phase compared to the pristine perovskite. Notably, F-ion intercalation occurs primarily at the apical sites of the polyhedron, with some occupation of basal sites in localized regions. This process leads to the formation of two distinct domains within the nickelate layer, reflecting a competition between polyhedral distortion and geometric frustration-induced neodymium (Nd) displacement near 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 within the infinite layer structure with distinct F-ion configurations. These findings provide crucial insights into understanding and manipulating anion doping at the atomic level, paving the way for the development of novel materials with precisely controlled functionalities. |
| title | Atomic-scale observation of geometric frustration in a fluorine-intercalated infinite layer nickelate superlattice |
| topic | Materials Science Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2408.14157 |