Quantum Many-Body Effects in Defective Transition-Metal-Oxide Superlattices

Juan A. Santana; Rohan Mishra; Jaron T. Krogel; Albina Y. Borisevich; Paul R.C. Kent; Sokrates T. Pantelides; Fernando A. Reboredo

doi:10.1021/acs.jctc.7b00483

Quantum Many-Body Effects in Defective Transition-Metal-Oxide Superlattices

Juan A. Santana, Rohan Mishra, Jaron T. Krogel, Albina Y. Borisevich, Paul R.C. Kent, Sokrates T. Pantelides, Fernando A. Reboredo

Computational Chemistry and Nanomaterial

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Strong electronic correlations, interfaces, and defects, and disorder each individually challenge the theoretical methods for predictions of materials properties. These challenges are all simultaneously present in complex transition-metal-oxide interfaces and superlattices, which are known to exhibit unique and unusual properties caused by multiple coupled degrees of freedom and strong electronic correlations. Here we show that ab initio quantum Monte Carlo (QMC) solutions of the many-electron problem are now possible for the full complexity of these systems. Within a single nonempirical theoretical approach, we unambiguously establish the site-specific stability of oxygen vacancies in the (LaFeO₃)₂/(SrFeO₃) superlattice, accounting for experimental data, and predict their migration pathways. QMC calculations are now capable of playing a major role in the elucidation of many-body phenomena in complex oxides previously out of reach of first-principles theories.

Original language	English
Pages (from-to)	5604-5609
Number of pages	6
Journal	Journal of Chemical Theory and Computation
Volume	13
Issue number	11
DOIs	https://doi.org/10.1021/acs.jctc.7b00483
State	Published - Nov 14 2017

Funding

This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). *E-mail: [email protected]. ORCID Juan A. Santana: 0000-0003-2349-6312 Rohan Mishra: 0000-0003-1261-0087 Albina Y. Borisevich: 0000-0002-3953-8460 Author Contributions The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript. Funding The work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences Materials Sciences & Engineering Division (BES-MSED). P.R.C.K. was supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Work at Vanderbilt was supported by Department of Energy BES-MSED grant DE-FG02-09ER46554. Work at Washington University was supported by the Consortium for Clean Coal Utilization (CCCU). Computational resources were provided by the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory and the National Energy Research Scientific Computing Center, supported by the Office of Science of the U.S. Department of Energy under contract numbers DE-AC05-00OR22725 and DE-AC02-05CH11231, and the Extreme Science and Engineering Discovery Environment, which is supported by National Science Foundation under grant number ACI-1053575. Notes The authors declare no competing financial interest.

Funders	Funder number
BES-MSED
Basic Energy Sciences Materials Sciences & Engineering Division
Consortium for Clean Coal Utilization
Department of Energy BES-MSED	DE-FG02-09ER46554
Extreme Science and Engineering Discovery Environment
Scientific User Facilities Division
National Science Foundation	ACI-1053575
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Council for Christian Colleges and Universities
National Energy Research Scientific Computing Center	DE-AC05-00OR22725, DE-AC02-05CH11231

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title = "Quantum Many-Body Effects in Defective Transition-Metal-Oxide Superlattices",

abstract = "Strong electronic correlations, interfaces, and defects, and disorder each individually challenge the theoretical methods for predictions of materials properties. These challenges are all simultaneously present in complex transition-metal-oxide interfaces and superlattices, which are known to exhibit unique and unusual properties caused by multiple coupled degrees of freedom and strong electronic correlations. Here we show that ab initio quantum Monte Carlo (QMC) solutions of the many-electron problem are now possible for the full complexity of these systems. Within a single nonempirical theoretical approach, we unambiguously establish the site-specific stability of oxygen vacancies in the (LaFeO3)2/(SrFeO3) superlattice, accounting for experimental data, and predict their migration pathways. QMC calculations are now capable of playing a major role in the elucidation of many-body phenomena in complex oxides previously out of reach of first-principles theories.",

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AU - Pantelides, Sokrates T.

AU - Reboredo, Fernando A.

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AB - Strong electronic correlations, interfaces, and defects, and disorder each individually challenge the theoretical methods for predictions of materials properties. These challenges are all simultaneously present in complex transition-metal-oxide interfaces and superlattices, which are known to exhibit unique and unusual properties caused by multiple coupled degrees of freedom and strong electronic correlations. Here we show that ab initio quantum Monte Carlo (QMC) solutions of the many-electron problem are now possible for the full complexity of these systems. Within a single nonempirical theoretical approach, we unambiguously establish the site-specific stability of oxygen vacancies in the (LaFeO3)2/(SrFeO3) superlattice, accounting for experimental data, and predict their migration pathways. QMC calculations are now capable of playing a major role in the elucidation of many-body phenomena in complex oxides previously out of reach of first-principles theories.

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Quantum Many-Body Effects in Defective Transition-Metal-Oxide Superlattices

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