Probing the Origin of Interfacial Carriers in SrTiO3$-$LaCrO3 Superlattices

Comes, Ryan B.; Spurgeon, Steven R.; Kepaptsoglou, Despoina M.; Engelhard, Mark H.; Perea, Daniel E.; Kaspar, Tiffany C.; Ramasse, Quentin M.; Sushko, Peter V.; Chambers, Scott A.

doi:10.1021/acs.chemmater.6b04329

Title: Probing the Origin of Interfacial Carriers in SrTiO₃$$-$$LaCrO₃ Superlattices

Journal Article · Fri Jan 13 00:00:00 EST 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.6b04329· OSTI ID:1340608

^[1];

^[2]; Kepaptsoglou, Despoina M. ^[3]; Engelhard, Mark H. ^[4];

^[4]; Kaspar, Tiffany C. ^[2]; Ramasse, Quentin M. ^[3]; Sushko, Peter V. ^[2]; Chambers, Scott A. ^[2]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Auburn Univ., AL (United States). Dept. of Physics
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
SuperSTEM, Daresbury (United Kingdom). SciTech Daresbury Campus
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Emergent phenomena at complex oxide interfaces could provide the basis for a wide variety of next-generation devices, including photovoltaics and spintronics. To date, detailed characterization and computational modeling of interfacial defects, cation intermixing, and film stoichiometry have helped to explain many of the novel behaviors observed at a single heterojunction. Unfortunately, many of the techniques employed to characterize a single heterojunction are less effective for a superlattice made up of a repeating series of interfaces that induce collective interfacial phenomena throughout a film. These repeating interfaces present an untapped opportunity to introduce an additional degree of complexity, such as confined electric fields, that cannot be realized in a single heterojunction. In this work, we explore the properties of SrTiO₃–LaCrO₃ superlattices to understand the role of defects, including variations in cation stoichiometry of individual layers of the superlattice, intermixing across interfaces, and interfacial oxygen vacancies. Using X-ray photoelectron spectroscopy (XPS) and scanning transmission electron microscopy electron energy-loss spectroscopy (STEM-EELS), we quantify the stoichiometry of individual layers of the superlattice and determine the degree of intermixing in these materials. By comparing these results to both density functional theory (DFT) models and STEM-EELS measurements of the Ti and Cr valence in each layer of the superlattice, we correlate different types of defects with the associated materials properties of the superlattice. In conclusion, we show that a combination of ab initio modeling and complementary structural characterization methods can offer unique insight into structure–property relationships in many oxide superlattice systems.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1340608

Journal Information:: Chemistry of Materials, Vol. 29, Issue 3; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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Strain-induced indirect-to-direct bandgap transition in an np-type LaAlO ₃ /SrTiO ₃ (110) superlattice Wang, L.; Pan, W.; Hu, W. X. Physical Chemistry Chemical Physics, Vol. 21, Issue 13 https://doi.org/10.1039/c8cp07761d	journal	January 2019

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Title: Probing the Origin of Interfacial Carriers in SrTiO₃$$-$$LaCrO₃ Superlattices