skip to main content

DOE PAGESDOE PAGES

Title: Towards spin-polarized two-dimensional electron gas at a surface of an antiferromagnetic insulating oxide

Here, the surfaces of transition-metal oxides with the perovskite structure are fertile grounds for the discovery of novel electronic and magnetic phenomena. In this article, we combine scanning transmission electron microscopy (STEM) with density functional theory (DFT) calculations to obtain the electronic and magnetic properties of the (001) surface of a (LaFeO 3) 8/(SrFeO 3) 1 superlattice film capped with four layers of LaFeO 3. Simultaneously acquired STEM images and electron-energy-loss spectra reveal the surface structure and a reduction in the oxidation state of iron from Fe 3+ in the bulk to Fe 2+ at the surface, extending over several atomic layers, which signals the presence of oxygen vacancies. The DFT calculations confirm the reduction in terms of oxygen vacancies and further demonstrate the stabilization of an exotic phase in which the surface layer is half metallic and ferromagnetic, while the bulk remains antiferromagnetic and insulating. Based on the calculations, we predict that the surface magnetism and conductivity can be controlled by tuning the partial pressure of oxygen.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [3] ;  [6] ;  [6] ;  [7] ;  [3]
  1. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Washington Univ., St. Louis, MO (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Institute for Basic Science (IBS), Suwon (Republic of Korea); Sungkyunkwan Univ., (SKKU), Suwon (Republic of Korea)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Washington Univ., St. Louis, MO (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States); Korea Institute of Science and Technology, Seoul (Republic of Korea)
  6. Argonne National Lab. (ANL), Argonne, IL (United States)
  7. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725; FG02-09ER46554; AC02-05CH11231; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 94; Journal Issue: 4; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
OSTI Identifier:
1329163
Alternate Identifier(s):
OSTI ID: 1263724; OSTI ID: 1352677

Mishra, Rohan, Kim, Young -Min, He, Qian, Huang, Xing, Kim, Seong Keun, Susner, Michael A., Bhattacharya, Anand, Fong, Dillon D., Pantelides, Sokrates T., and Borisevich, Albina Y.. Towards spin-polarized two-dimensional electron gas at a surface of an antiferromagnetic insulating oxide. United States: N. p., Web. doi:10.1103/PhysRevB.94.045123.
Mishra, Rohan, Kim, Young -Min, He, Qian, Huang, Xing, Kim, Seong Keun, Susner, Michael A., Bhattacharya, Anand, Fong, Dillon D., Pantelides, Sokrates T., & Borisevich, Albina Y.. Towards spin-polarized two-dimensional electron gas at a surface of an antiferromagnetic insulating oxide. United States. doi:10.1103/PhysRevB.94.045123.
Mishra, Rohan, Kim, Young -Min, He, Qian, Huang, Xing, Kim, Seong Keun, Susner, Michael A., Bhattacharya, Anand, Fong, Dillon D., Pantelides, Sokrates T., and Borisevich, Albina Y.. 2016. "Towards spin-polarized two-dimensional electron gas at a surface of an antiferromagnetic insulating oxide". United States. doi:10.1103/PhysRevB.94.045123. https://www.osti.gov/servlets/purl/1329163.
@article{osti_1329163,
title = {Towards spin-polarized two-dimensional electron gas at a surface of an antiferromagnetic insulating oxide},
author = {Mishra, Rohan and Kim, Young -Min and He, Qian and Huang, Xing and Kim, Seong Keun and Susner, Michael A. and Bhattacharya, Anand and Fong, Dillon D. and Pantelides, Sokrates T. and Borisevich, Albina Y.},
abstractNote = {Here, the surfaces of transition-metal oxides with the perovskite structure are fertile grounds for the discovery of novel electronic and magnetic phenomena. In this article, we combine scanning transmission electron microscopy (STEM) with density functional theory (DFT) calculations to obtain the electronic and magnetic properties of the (001) surface of a (LaFeO3)8/(SrFeO3)1 superlattice film capped with four layers of LaFeO3. Simultaneously acquired STEM images and electron-energy-loss spectra reveal the surface structure and a reduction in the oxidation state of iron from Fe3+ in the bulk to Fe2+ at the surface, extending over several atomic layers, which signals the presence of oxygen vacancies. The DFT calculations confirm the reduction in terms of oxygen vacancies and further demonstrate the stabilization of an exotic phase in which the surface layer is half metallic and ferromagnetic, while the bulk remains antiferromagnetic and insulating. Based on the calculations, we predict that the surface magnetism and conductivity can be controlled by tuning the partial pressure of oxygen.},
doi = {10.1103/PhysRevB.94.045123},
journal = {Physical Review B},
number = 4,
volume = 94,
place = {United States},
year = {2016},
month = {7}
}

Works referenced in this record:

Inner shell edge profiles in electron energy loss spectroscopy
journal, January 1985

Generalized Gradient Approximation Made Simple
journal, October 1996
  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Projector augmented-wave method
journal, December 1994

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998
  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Atomic Control of the SrTiO3 Crystal Surface
journal, December 1994

Two-dimensional electron gas with universal subbands at the surface of SrTiO3
journal, January 2011
  • Santander-Syro, A. F.; Copie, O.; Kondo, T.
  • Nature, Vol. 469, Issue 7329, p. 189-193
  • DOI: 10.1038/nature09720

Special points for Brillouin-zone integrations
journal, June 1976
  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994

Highly conductive nanolayers on strontium titanate produced by preferential ion-beam etching
journal, July 2005
  • Reagor, David W.; Butko, Vladimir Y.
  • Nature Materials, Vol. 4, Issue 8, p. 593-596
  • DOI: 10.1038/nmat1402

Design principles for oxygen-reduction activity on perovskite oxide catalysts for fuel cells and metal–air batteries
journal, June 2011
  • Suntivich, Jin; Gasteiger, Hubert A.; Yabuuchi, Naoaki
  • Nature Chemistry, Vol. 3, Issue 7, p. 546-550
  • DOI: 10.1038/nchem.1069