DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Switchable orbital polarization and magnetization in strained LaCo O 3 films

Abstract

Strain engineering of epitaxial heterostructures offers opportunities to control the orbital degree of freedom by lifting the degeneracy of eg states. In this work, we show that the orbital occupation in LaCoO3 (LCO) films can be switched between two degenerate eg bands with epitaxial strain. The orbital polarization of nearly -100% (or 100%) is controlled by depleting occupation of the dx2-y2 (or d(3z2-r2) orbital entirely in LCO for large compressive (or moderate tensile) strain. The change of electronic configuration associated with the spin-state transition modulates the magnetization of strained LCO films. Under compressive strain, LCO films exhibit a small magnetization without long-range ferromagnetic ordering. With tensile-strain increases, the magnetization of LCO films increases and reaches the maximum value when the bonding angle (Co-O-Co) is close to 180° and the in-plane bond length (Co-O) is unstretched. Our results highlight the role of octahedral distortion and spin-state crossover in tailoring the magnetic properties of cobaltite thin films, indicating an attractive route to deliberately control the orbital polarization that can be tuned to maximize the functionality of oxide heterostructures.

Authors:
 [1];  [2];  [3];  [4];  [2];  [5];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Martin Luther Univ. of Halle-Wittenberg (MLU), Halle (Germany)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1505601
Alternate Identifier(s):
OSTI ID: 1490921; OSTI ID: 1607130
Grant/Contract Number:  
AC02-06CH11357; AC02-06CH1135; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; X-ray scattering; Orbital polarization; ferroelastic materials; ferromagnetism; strain engineering

Citation Formats

Guo, Er-Jia, Desautels, Ryan D., Keavney, David, Herklotz, Andreas, Ward, T. Zac, Fitzsimmons, Michael R., and Lee, Ho Nyung. Switchable orbital polarization and magnetization in strained LaCoO3 films. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.014407.
Guo, Er-Jia, Desautels, Ryan D., Keavney, David, Herklotz, Andreas, Ward, T. Zac, Fitzsimmons, Michael R., & Lee, Ho Nyung. Switchable orbital polarization and magnetization in strained LaCoO3 films. United States. https://doi.org/10.1103/PhysRevMaterials.3.014407
Guo, Er-Jia, Desautels, Ryan D., Keavney, David, Herklotz, Andreas, Ward, T. Zac, Fitzsimmons, Michael R., and Lee, Ho Nyung. Tue . "Switchable orbital polarization and magnetization in strained LaCoO3 films". United States. https://doi.org/10.1103/PhysRevMaterials.3.014407. https://www.osti.gov/servlets/purl/1505601.
@article{osti_1505601,
title = {Switchable orbital polarization and magnetization in strained LaCoO3 films},
author = {Guo, Er-Jia and Desautels, Ryan D. and Keavney, David and Herklotz, Andreas and Ward, T. Zac and Fitzsimmons, Michael R. and Lee, Ho Nyung},
abstractNote = {Strain engineering of epitaxial heterostructures offers opportunities to control the orbital degree of freedom by lifting the degeneracy of eg states. In this work, we show that the orbital occupation in LaCoO3 (LCO) films can be switched between two degenerate eg bands with epitaxial strain. The orbital polarization of nearly -100% (or 100%) is controlled by depleting occupation of the dx2-y2 (or d(3z2-r2) orbital entirely in LCO for large compressive (or moderate tensile) strain. The change of electronic configuration associated with the spin-state transition modulates the magnetization of strained LCO films. Under compressive strain, LCO films exhibit a small magnetization without long-range ferromagnetic ordering. With tensile-strain increases, the magnetization of LCO films increases and reaches the maximum value when the bonding angle (Co-O-Co) is close to 180° and the in-plane bond length (Co-O) is unstretched. Our results highlight the role of octahedral distortion and spin-state crossover in tailoring the magnetic properties of cobaltite thin films, indicating an attractive route to deliberately control the orbital polarization that can be tuned to maximize the functionality of oxide heterostructures.},
doi = {10.1103/PhysRevMaterials.3.014407},
journal = {Physical Review Materials},
number = 1,
volume = 3,
place = {United States},
year = {Tue Jan 15 00:00:00 EST 2019},
month = {Tue Jan 15 00:00:00 EST 2019}
}

Journal Article:

Citation Metrics:
Cited by: 24 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Strain-driven magnetism in LaCoO 3 thin films
journal, January 2009


Effect of Interfacial Octahedral Behavior in Ultrathin Manganite Films
journal, April 2014

  • Moon, E. J.; Balachandran, P. V.; Kirby, B. J.
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl500235f

Spin State Transition in LaCoO 3 Studied Using Soft X-ray Absorption Spectroscopy and Magnetic Circular Dichroism
journal, October 2006


Structure and Properties of Functional Oxide Thin Films: Insights From Electronic-Structure Calculations
journal, July 2011


First-Order Localized-Electron Collective-Electron Transition in LaCo O 3
journal, March 1967


Different Look at the Spin State of Co 3 + Ions in a CoO 5 Pyramidal Coordination
journal, May 2004


Nanoscale Spin-State Ordering in LaCoO 3 Epitaxial Thin Films
journal, April 2014

  • Kwon, Ji-Hwan; Choi, Woo Seok; Kwon, Young-Kyun
  • Chemistry of Materials, Vol. 26, Issue 8
  • DOI: 10.1021/cm5003115

Interfacial Symmetry Control of Emergent Ferromagnetism at the Nanoscale
journal, August 2016


Critical thickness and orbital ordering in ultrathin La 0.7 Sr 0.3 MnO 3 films
journal, September 2008


Sum Rules and Fundamental Spectra of Magnetic X-Ray Dichroism in Crystal Field Symmetry
journal, June 1994

  • van der Laan, G.
  • Journal of the Physical Society of Japan, Vol. 63, Issue 6
  • DOI: 10.1143/JPSJ.63.2393

Ferroelasticity and related properties of crystals
journal, January 1982


Mechanical properties of LaCoO3 based ceramics
journal, January 2000


Monoclinic Ferroelastic Domains in LaCoO3-Based Perovskites
journal, December 2007

  • Vullum, P. E.; Holmestad, R.; Lein, H. L.
  • Advanced Materials, Vol. 19, Issue 24
  • DOI: 10.1002/adma.200700021

Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling
journal, March 2016

  • Liao, Z.; Huijben, M.; Zhong, Z.
  • Nature Materials, Vol. 15, Issue 4
  • DOI: 10.1038/nmat4579

Reversible strain effect on the magnetization of LaCoO 3 films
journal, March 2009


Tuning the magnetic properties of La Co O 3 thin films by epitaxial strain
journal, January 2008


Ferromagnetism and Charge Order from a Frozen Electron Configuration in Strained Epitaxial LaCoO 3
journal, May 2018


Bulk modulus anomaly in R Co O 3 ( R = La , Pr, and Nd)
journal, June 2005


In-situ neutron diffraction of LaCoO 3 perovskite under uniaxial compression. II. Elastic properties
journal, July 2014

  • Lugovy, Mykola; Aman, Amjad; Chen, Yan
  • Journal of Applied Physics, Vol. 116, Issue 1
  • DOI: 10.1063/1.4884336

In Situ Observation of Oxygen Vacancy Dynamics and Ordering in the Epitaxial LaCoO 3 System
journal, June 2017


Spin-Orbital Superstructure in Strained Ferrimagnetic Perovskite Cobalt Oxide
journal, July 2013


Pressure-induced intermediate-to-low spin state transition in LaCoO 3
journal, April 2003


Ferromagnetism in La Co O 3
journal, July 2004


Ferromagnetic order in epitaxially strained La Co O 3 thin films
journal, April 2007


Tensile-Strain-Dependent Spin States in Epitaxial LaCoO 3 Thin Films
journal, May 2018


Electric-field control of tri-state phase transformation with a selective dual-ion switch
journal, May 2017

  • Lu, Nianpeng; Zhang, Pengfei; Zhang, Qinghua
  • Nature, Vol. 546, Issue 7656
  • DOI: 10.1038/nature22389

Structural phenomena associated with the spin-state transition in LaCoO 3
journal, September 2002


Strain-Induced Spin States in Atomically Ordered Cobaltites
journal, January 2012

  • Choi, Woo Seok; Kwon, Ji-Hwan; Jeen, Hyoungjeen
  • Nano Letters, Vol. 12, Issue 9
  • DOI: 10.1021/nl302562f

Influence of rare-earth ion radii on the low-spin to intermediate-spin state transition in lanthanide cobaltite perovskites:  LaCoO 3 versus HoCoO 3
journal, December 2003


Correlating interfacial octahedral rotations with magnetism in (LaMnO3+δ)N/(SrTiO3)N superlattices
journal, July 2014

  • Zhai, Xiaofang; Cheng, Long; Liu, Yang
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5283

Absorption of circularly polarized x rays in iron
text, January 1987


Works referencing / citing this record:

Structural, electronic, transport and magnetic studies of LaCo 1 − x Ni x O 3 (x = 0, 0.3) thin films
journal, December 2019

  • Kumar, Ashok; Kumar, Vinod; Shukla, Dinesh
  • Journal of Applied Physics, Vol. 126, Issue 23
  • DOI: 10.1063/1.5119435

Maximization of ferromagnetism in LaCo O 3 films by competing symmetry
journal, November 2019