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Three dimensional band-filling control of complex oxides triggered by interfacial electron transfer.

ABSTRACT: The d-band-filling of transition metals in complex oxides plays an essential role in determining their structural, electronic and magnetic properties. Traditionally, at the oxide heterointerface, band-filling control has been achieved via electrostatic modification in the structure of field-effect transistors or electron transfer, which is limited to the quasi-two-dimension at the interface. Here we report a three-dimensional (3D) band-filling control by changing the local lattice coordination in a designed oxide heterostructure. At the LaCoO₃/LaTiO₃ heterointerface, due to the Fermi level mismatch, electrons transfer from LaTiO₃ to LaCoO₃. This triggers destabilisation of the CoO₆ octahedrons, i.e. the formation of lattice configurations with a reduced Co valence. The associated oxygen migration results in the 3D topotactic phase transition of LaCoO₃. Tuned by the thickness of LaTiO₃, different crystalline phases and band-fillings of Co occur, leading to the emergence of different magnetic ground states.

SUBMITTER: Meng M

PROVIDER: S-EPMC8079372 | biostudies-literature | 2021 Apr

REPOSITORIES: biostudies-literature

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Three dimensional band-filling control of complex oxides triggered by interfacial electron transfer.

Meng Meng M Sun Yuanwei Y Li Yuehui Y An Qichang Q Wang Zhenzhen Z Lin Zijian Z Yang Fang F Zhu Xuetao X Gao Peng P Guo Jiandong J

Nature communications 20210427 1

The d-band-filling of transition metals in complex oxides plays an essential role in determining their structural, electronic and magnetic properties. Traditionally, at the oxide heterointerface, band-filling control has been achieved via electrostatic modification in the structure of field-effect transistors or electron transfer, which is limited to the quasi-two-dimension at the interface. Here we report a three-dimensional (3D) band-filling control by changing the local lattice coordination i ...[more]

PMID: 33907193

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Project description:Formation of a transient [myoglobin (Mb), cytochrome b(5) (cyt b(5))] complex is required for the reductive repair of inactive ferri-Mb to its functional ferro-Mb state. The [Mb, cyt b(5)] complex exhibits dynamic docking (DD), with its cyt b(5) partner in rapid exchange at multiple sites on the Mb surface. A triple mutant (Mb(3M)) was designed as part of efforts to shift the electron-transfer process to the simple docking (SD) regime, in which reactive binding occurs at a restricted, reactive region on the Mb surface that dominates the docked ensemble. An electrostatically-guided brownian dynamics (BD) docking protocol was used to generate an initial ensemble of reactive configurations of the complex between unrelaxed partners. This ensemble samples a broad and diverse array of heme-heme distances and orientations. These configurations seeded all-atom constrained molecular dynamics simulations (MD) to generate relaxed complexes for the calculation of electron tunneling matrix elements (T(DA)) through tunneling-pathway analysis. This procedure for generating an ensemble of relaxed complexes combines the ability of BD calculations to sample the large variety of available conformations and interprotein distances, with the ability of MD to generate the atomic level information, especially regarding the structure of water molecules at the protein-protein interface, that defines electron-tunneling pathways. We used the calculated T(DA) values to compute ET rates for the [Mb(wt), cyt b(5)] complex and for the complex with a mutant that has a binding free energy strengthened by three D/E → K charge-reversal mutations, [Mb(3M), cyt b(5)]. The calculated rate constants are in agreement with the measured values, and the mutant complex ensemble has many more geometries with higher T(DA) values than does the wild-type Mb complex. Interestingly, water plays a double role in this electron-transfer system, lowering the tunneling barrier as well as inducing protein interface remodeling that screens the repulsion between the negatively-charged propionates of the two hemes.

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Three dimensional band-filling control of complex oxides triggered by interfacial electron transfer.

Publications

Three dimensional band-filling control of complex oxides triggered by interfacial electron transfer.

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