Valence-Ordered Thin-Film Nickelate with Tri-component Nickel Coordination Prepared by Topochemical Reduction
Source abstract
Abstract
The metal-hydride-based “topochemical reduction” process has produced several thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and nontrivial ground states. Here, by such an oxygen (de-)intercalation method we synthesis a 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 (4D-STEM), emerges from the intricate planes of {303} 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 nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents an interesting platform where mixed Ni valence can give rise to exotic phenomena.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Advanced Condensed Matter Physics · Catalytic Processes in Materials Science · Magnetic and transport properties of perovskites and related materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Laboratoire de Physique des Solides, CNRS, Université Paris-Saclay, Orsay 91400, France
Synchrotron SOLEIL, L’Orme des Merisiers, BP 48 St. Aubin, Gif sur Yvette 91192, France
Department of Physics, City University of Hong Kong, Kowloon, Hong Kong
City University of Hong Kong Shenzhen Research Institute, Shenzhen, Guangdong 518057, China
CPHT, Ecole Polytechnique, Palaiseau Cedex 91128, France
Department of Quantum Matter Physics, University of Geneva, Geneva 1211, Switzerland
Electron Spectrometry and Microscopy Laboratory (LSME), Institute of Physics (IPHYS), Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne 1015, Switzerland
LCPMR, Sorbonne Université, CNRS, Paris 75005, France
Funding
Research Grants Council, University Grants Committee · Schweizerischer Nationalfonds zur F?rderung der Wissenschaftlichen Forschung · Basic and Applied Basic Research Foundation of Guangdong Province · H2020 Research Infrastructures · National Natural Science Foundation of China · Seventh Framework Programme · Agence Nationale de la Recherche
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