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| Format: | Preprint |
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2023
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| Online-Zugang: | https://arxiv.org/abs/2308.02855 |
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| _version_ | 1866910383587983360 |
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| author | Raji, Aravind Dong, Zhengang Porée, Victor Subedi, Alaska Li, Xiaoyan Mundet, Bernat Varbaro, Lucia Domínguez, Claribel Hadjimichael, Marios Feng, Bohan Nicolaou, Alessandro Rueff, Jean-Pascal Li, Danfeng Gloter, Alexandre |
| author_facet | Raji, Aravind Dong, Zhengang Porée, Victor Subedi, Alaska Li, Xiaoyan Mundet, Bernat Varbaro, Lucia Domínguez, Claribel Hadjimichael, Marios Feng, Bohan Nicolaou, Alessandro Rueff, Jean-Pascal Li, Danfeng Gloter, Alexandre |
| contents | The metal-hydride-based topochemical reduction process has produced novel thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and non-trivial ground states. Here, by such an oxygen (de-) intercalation method we synthesis a novel samarium nickelate with ordered nickel valences associated with tri-component coordination configurations. This structure, with a formula of Sm$_{9}$Ni$_{9}$O$_{22}$ as revealed by four-dimensional scanning transmission electron microscopy, emerges from the intricate planes of {303}$_{\text{pc}}$ ordered apical oxygen vacancies. X-ray spectroscopy measurements and ab-initio calculations show the coexistence of square-planar, pyramidal and octahedral Ni sites with mono-, bi- and tri-valences. It leads to an intense orbital polarization, charge-ordering, and a ground state with a strong electron localization marked by the disappearance of ligand-hole configuration at low-temperature. This new nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents a unique platform where mixed Ni valence can give rise to exotic phenomena. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2308_02855 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Emergent electronic landscapes in a novel valence-ordered nickelate with tri-component nickel coordination Raji, Aravind Dong, Zhengang Porée, Victor Subedi, Alaska Li, Xiaoyan Mundet, Bernat Varbaro, Lucia Domínguez, Claribel Hadjimichael, Marios Feng, Bohan Nicolaou, Alessandro Rueff, Jean-Pascal Li, Danfeng Gloter, Alexandre Materials Science The metal-hydride-based topochemical reduction process has produced novel thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and non-trivial ground states. Here, by such an oxygen (de-) intercalation method we synthesis a novel samarium nickelate with ordered nickel valences associated with tri-component coordination configurations. This structure, with a formula of Sm$_{9}$Ni$_{9}$O$_{22}$ as revealed by four-dimensional scanning transmission electron microscopy, emerges from the intricate planes of {303}$_{\text{pc}}$ ordered apical oxygen vacancies. X-ray spectroscopy measurements and ab-initio calculations show the coexistence of square-planar, pyramidal and octahedral Ni sites with mono-, bi- and tri-valences. It leads to an intense orbital polarization, charge-ordering, and a ground state with a strong electron localization marked by the disappearance of ligand-hole configuration at low-temperature. This new nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents a unique platform where mixed Ni valence can give rise to exotic phenomena. |
| title | Emergent electronic landscapes in a novel valence-ordered nickelate with tri-component nickel coordination |
| topic | Materials Science |
| url | https://arxiv.org/abs/2308.02855 |