Competing Pathways for Nucleation of the Double Perovskite Structure in the Epitaxial Synthesis of La 2 MnNiO 6

Spurgeon, Steven R.; Du, Yingge; Droubay, Timothy; Devaraj, Arun; Sang, Xiahan; Longo, Paolo; Yan, Pengfei; Kotula, Paul G.; Shutthanandan, Vaithiyalingam; Bowden, Mark E.; LeBeau, James M.; Wang, Chongmin; Sushko, Peter V.; Chambers, Scott A.

doi:10.1021/acs.chemmater.6b00829

Title: Competing Pathways for Nucleation of the Double Perovskite Structure in the Epitaxial Synthesis of La ₂ MnNiO ₆

Journal Article · Tue Jun 14 00:00:00 EDT 2016 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.6b00829· OSTI ID:1327135

Spurgeon, Steven R.; Du, Yingge; Droubay, Timothy; Devaraj, Arun; Sang, Xiahan; Longo, Paolo; Yan, Pengfei; Kotula, Paul G.; Shutthanandan, Vaithiyalingam; Bowden, Mark E.; LeBeau, James M.; Wang, Chongmin; Sushko, Peter V.; Chambers, Scott A.

Over the past decades a confluence of advanced synthesis techniques, data-driven characterization, and rapid increases in computing power has sparked a renaissance in materials engineering. The emerging “materials-by-design” approach, while radically transforming the development of multicomponent systems, has tended to overlook the complex kinetic pathways that define materials synthesis. Although we are able to envision almost limitless materials combinations, we are unable to synthesize all of them in practice, since existing characterization and modeling approaches often fail to capture the inherent complexity of such systems. There is currently a disconnect between highly local structural characterization and macroscale properties measurements, resulting in oversimplified or incomplete structure-property models. Here we describe a multi-technique approach that combines aberration-corrected transmission electron microscopy with emerging oxide atom probe tomography to measure chemical ordering and extended defects in the model complex oxide, La2MnNiO6. We visualize cation ordering, as well as a three-dimensional network of secondary phases, which we describe in terms of ab initio structure calculations. We propose a defect model in which these phases alter their surrounding octahedral environment, severely disrupting cation superexchange. Through this array of experimental and theoretical techniques, we uncover fundamental structure-property relationships and illustrate a new approach to engineer complex, multicomponent systems.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1327135

Report Number(s):: PNNL-SA-115671; 48341; KC0203020

Journal Information:: Chemistry of Materials, Vol. 28, Issue 11; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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