Exploring the Spatial Control of Topotactic Phase Transitions Using Vertically Oriented Epitaxial Interfaces

Wenrui Zhang; Jie Zhang; Shaobo Cheng; Christopher M. Rouleau; Kim Kisslinger; Lihua Zhang; Yimei Zhu; Thomas Z. Ward; Gyula Eres

doi:10.1007/s40820-021-00752-x

Exploring the Spatial Control of Topotactic Phase Transitions Using Vertically Oriented Epitaxial Interfaces

Wenrui Zhang, Jie Zhang, Shaobo Cheng, Christopher M. Rouleau, Kim Kisslinger, Lihua Zhang, Yimei Zhu, Thomas Z. Ward, Gyula Eres

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3 Scopus citations

Abstract

Engineering oxygen vacancy formation and distribution is a powerful route for controlling the oxygen sublattice evolution that affects diverse functional behavior. The controlling of the oxygen vacancy formation process is particularly important for inducing topotactic phase transitions that occur by transformation of the oxygen sublattice. Here we demonstrate an epitaxial nanocomposite approach for exploring the spatial control of topotactic phase transition from a pristine perovskite phase to an oxygen vacancy-ordered brownmillerite (BM) phase in a model oxide La_0.7Sr_0.3MnO₃ (LSMO). Incorporating a minority phase NiO in LSMO films creates ultrahigh density of vertically aligned epitaxial interfaces that strongly influence the oxygen vacancy formation and distribution in LSMO. Combined structural characterizations reveal strong interactions between NiO and LSMO across the epitaxial interfaces leading to a topotactic phase transition in LSMO accompanied by significant morphology evolution in NiO. Using the NiO nominal ratio as a single control parameter, we obtain intermediate topotactic nanostructures with distinct distribution of the transformed LSMO-BM phase, which enables systematic tuning of magnetic and electrical transport properties. The use of self-assembled heterostructure interfaces by the epitaxial nanocomposite platform enables more versatile design of topotactic phase structures and correlated functionalities that are sensitive to oxygen vacancies.[Figure not available: see fulltext.]

Original language	English
Article number	2
Journal	Nano-Micro Letters
Volume	14
Issue number	1
DOIs	https://doi.org/10.1007/s40820-021-00752-x
State	Published - Dec 2022

Funding

This work was supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. Part of this research was performed at the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, which is a DOE Office of Science User Facility. The electron microscopy work done at Brookhaven National Laboratory was supported by the U.S. DOE-BES, the Center for Functional Nanomaterials, a DOE Office of Science User Facility, and Materials Science and Engineering Division, under Contract No. DE-SC0012704. W. Z. acknowledges the support by National Natural Science Foundation of China (Grant No. 62004200) and Zhejiang Provincial Natural Science Foundation (Grant No. LZ21F040001). S. C. acknowledges the support by Q-MEEN-C, an Energy Frontier Research Center funded by the U.S. DOE-BES under award No. DE-SC0019273.

Funders	Funder number
U.S. DOE-BES
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering	DE-SC0012704
National Natural Science Foundation of China	62004200
Natural Science Foundation of Zhejiang Province	LZ21F040001, DE-SC0019273

Keywords

Epitaxial interface
Functional oxides
Nanocomposite
Oxygen vacancy
Topotactic phase transition

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10.1007/s40820-021-00752-x

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title = "Exploring the Spatial Control of Topotactic Phase Transitions Using Vertically Oriented Epitaxial Interfaces",

abstract = "Engineering oxygen vacancy formation and distribution is a powerful route for controlling the oxygen sublattice evolution that affects diverse functional behavior. The controlling of the oxygen vacancy formation process is particularly important for inducing topotactic phase transitions that occur by transformation of the oxygen sublattice. Here we demonstrate an epitaxial nanocomposite approach for exploring the spatial control of topotactic phase transition from a pristine perovskite phase to an oxygen vacancy-ordered brownmillerite (BM) phase in a model oxide La0.7Sr0.3MnO3 (LSMO). Incorporating a minority phase NiO in LSMO films creates ultrahigh density of vertically aligned epitaxial interfaces that strongly influence the oxygen vacancy formation and distribution in LSMO. Combined structural characterizations reveal strong interactions between NiO and LSMO across the epitaxial interfaces leading to a topotactic phase transition in LSMO accompanied by significant morphology evolution in NiO. Using the NiO nominal ratio as a single control parameter, we obtain intermediate topotactic nanostructures with distinct distribution of the transformed LSMO-BM phase, which enables systematic tuning of magnetic and electrical transport properties. The use of self-assembled heterostructure interfaces by the epitaxial nanocomposite platform enables more versatile design of topotactic phase structures and correlated functionalities that are sensitive to oxygen vacancies.[Figure not available: see fulltext.]",

keywords = "Epitaxial interface, Functional oxides, Nanocomposite, Oxygen vacancy, Topotactic phase transition",

author = "Wenrui Zhang and Jie Zhang and Shaobo Cheng and Rouleau, {Christopher M.} and Kim Kisslinger and Lihua Zhang and Yimei Zhu and Ward, {Thomas Z.} and Gyula Eres",

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AU - Zhang, Wenrui

AU - Zhang, Jie

AU - Cheng, Shaobo

AU - Rouleau, Christopher M.

AU - Kisslinger, Kim

AU - Zhang, Lihua

AU - Zhu, Yimei

AU - Ward, Thomas Z.

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N2 - Engineering oxygen vacancy formation and distribution is a powerful route for controlling the oxygen sublattice evolution that affects diverse functional behavior. The controlling of the oxygen vacancy formation process is particularly important for inducing topotactic phase transitions that occur by transformation of the oxygen sublattice. Here we demonstrate an epitaxial nanocomposite approach for exploring the spatial control of topotactic phase transition from a pristine perovskite phase to an oxygen vacancy-ordered brownmillerite (BM) phase in a model oxide La0.7Sr0.3MnO3 (LSMO). Incorporating a minority phase NiO in LSMO films creates ultrahigh density of vertically aligned epitaxial interfaces that strongly influence the oxygen vacancy formation and distribution in LSMO. Combined structural characterizations reveal strong interactions between NiO and LSMO across the epitaxial interfaces leading to a topotactic phase transition in LSMO accompanied by significant morphology evolution in NiO. Using the NiO nominal ratio as a single control parameter, we obtain intermediate topotactic nanostructures with distinct distribution of the transformed LSMO-BM phase, which enables systematic tuning of magnetic and electrical transport properties. The use of self-assembled heterostructure interfaces by the epitaxial nanocomposite platform enables more versatile design of topotactic phase structures and correlated functionalities that are sensitive to oxygen vacancies.[Figure not available: see fulltext.]

AB - Engineering oxygen vacancy formation and distribution is a powerful route for controlling the oxygen sublattice evolution that affects diverse functional behavior. The controlling of the oxygen vacancy formation process is particularly important for inducing topotactic phase transitions that occur by transformation of the oxygen sublattice. Here we demonstrate an epitaxial nanocomposite approach for exploring the spatial control of topotactic phase transition from a pristine perovskite phase to an oxygen vacancy-ordered brownmillerite (BM) phase in a model oxide La0.7Sr0.3MnO3 (LSMO). Incorporating a minority phase NiO in LSMO films creates ultrahigh density of vertically aligned epitaxial interfaces that strongly influence the oxygen vacancy formation and distribution in LSMO. Combined structural characterizations reveal strong interactions between NiO and LSMO across the epitaxial interfaces leading to a topotactic phase transition in LSMO accompanied by significant morphology evolution in NiO. Using the NiO nominal ratio as a single control parameter, we obtain intermediate topotactic nanostructures with distinct distribution of the transformed LSMO-BM phase, which enables systematic tuning of magnetic and electrical transport properties. The use of self-assembled heterostructure interfaces by the epitaxial nanocomposite platform enables more versatile design of topotactic phase structures and correlated functionalities that are sensitive to oxygen vacancies.[Figure not available: see fulltext.]

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Exploring the Spatial Control of Topotactic Phase Transitions Using Vertically Oriented Epitaxial Interfaces

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