Probing the Origin of Interfacial Carriers in SrTiO3$$-$$LaCrO3 Superlattices
Abstract
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 layermore »
- Authors:
-
[1];
[2];
[4];
- 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)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1340608
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 3; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 97 MATHEMATICS AND COMPUTING; 36 MATERIALS SCIENCE; Complex oxides; superlattices; x-ray photoelectron spectroscopy; x-ray absorption spectroscopy; scanning transmission electron microscopy
Citation Formats
Comes, Ryan B., Spurgeon, Steven R., Kepaptsoglou, Despoina M., Engelhard, Mark H., Perea, Daniel E., Kaspar, Tiffany C., Ramasse, Quentin M., Sushko, Peter V., and Chambers, Scott A. Probing the Origin of Interfacial Carriers in SrTiO3$-$LaCrO3 Superlattices. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.6b04329.
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. Probing the Origin of Interfacial Carriers in SrTiO3$-$LaCrO3 Superlattices. United States. https://doi.org/10.1021/acs.chemmater.6b04329
Comes, Ryan B., Spurgeon, Steven R., Kepaptsoglou, Despoina M., Engelhard, Mark H., Perea, Daniel E., Kaspar, Tiffany C., Ramasse, Quentin M., Sushko, Peter V., and Chambers, Scott A. Fri .
"Probing the Origin of Interfacial Carriers in SrTiO3$-$LaCrO3 Superlattices". United States. https://doi.org/10.1021/acs.chemmater.6b04329. https://www.osti.gov/servlets/purl/1340608.
@article{osti_1340608,
title = {Probing the Origin of Interfacial Carriers in SrTiO3$-$LaCrO3 Superlattices},
author = {Comes, Ryan B. and Spurgeon, Steven R. and Kepaptsoglou, Despoina M. and Engelhard, Mark H. and Perea, Daniel E. and Kaspar, Tiffany C. and Ramasse, Quentin M. and Sushko, Peter V. and Chambers, Scott A.},
abstractNote = {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.},
doi = {10.1021/acs.chemmater.6b04329},
journal = {Chemistry of Materials},
number = 3,
volume = 29,
place = {United States},
year = {Fri Jan 13 00:00:00 EST 2017},
month = {Fri Jan 13 00:00:00 EST 2017}
}
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Works referencing / citing this record:
Strain-induced indirect-to-direct bandgap transition in an np-type LaAlO 3 /SrTiO 3 (110) superlattice
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