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

Title: Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO3

Abstract

The origin of strain-induced ferromagnetism, which is robust regardless of the type and degree of strain in LaCoO3 (LCO) thin films, is enigmatic despite intensive research efforts over the past decade. Here, by combining scanning transmission electron microscopy with ab initio density functional theory plus U calculations, we report that the ferromagnetism does not emerge directly from the strain itself but rather from the creation of compressed structural units within ferroelastically formed twin-wall domains. The compressed structural units are magnetically active with the rocksalt-type high-spin/low-spin order. Our study highlights that the ferroelastic nature of ferromagnetic structural units is important for understanding the intriguing ferromagnetic properties in LCO thin films.

Authors:
 [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Sungkyunkwan Univ., Suwon (Korea)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1798486
Alternate Identifier(s):
OSTI ID: 1817600
Report Number(s):
BNL-221687-2021-JAAM
Journal ID: ISSN 1530-6984; TRN: US2210681
Grant/Contract Number:  
SC0012704; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 21; Journal Issue: 9; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Epitaxial thin film; Complex oxides; Ferromagnetism; Electron microscopy; Thin films; Layers; Lattices; Magnetic properties; Epitaxy

Citation Formats

Yoon, Sangmoon, Gao, Xiang, Ok, Jong Mok, Liao, Zhaoliang, Han, Myung-Geun, Zhu, Yimei, Ganesh, Panchapakesan, Chisholm, Matthew F., Choi, Woo Seok, and Lee, Ho Nyung. Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO3. United States: N. p., 2021. Web. doi:10.1021/acs.nanolett.1c00756.
Yoon, Sangmoon, Gao, Xiang, Ok, Jong Mok, Liao, Zhaoliang, Han, Myung-Geun, Zhu, Yimei, Ganesh, Panchapakesan, Chisholm, Matthew F., Choi, Woo Seok, & Lee, Ho Nyung. Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO3. United States. https://doi.org/10.1021/acs.nanolett.1c00756
Yoon, Sangmoon, Gao, Xiang, Ok, Jong Mok, Liao, Zhaoliang, Han, Myung-Geun, Zhu, Yimei, Ganesh, Panchapakesan, Chisholm, Matthew F., Choi, Woo Seok, and Lee, Ho Nyung. Fri . "Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO3". United States. https://doi.org/10.1021/acs.nanolett.1c00756. https://www.osti.gov/servlets/purl/1798486.
@article{osti_1798486,
title = {Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO3},
author = {Yoon, Sangmoon and Gao, Xiang and Ok, Jong Mok and Liao, Zhaoliang and Han, Myung-Geun and Zhu, Yimei and Ganesh, Panchapakesan and Chisholm, Matthew F. and Choi, Woo Seok and Lee, Ho Nyung},
abstractNote = {The origin of strain-induced ferromagnetism, which is robust regardless of the type and degree of strain in LaCoO3 (LCO) thin films, is enigmatic despite intensive research efforts over the past decade. Here, by combining scanning transmission electron microscopy with ab initio density functional theory plus U calculations, we report that the ferromagnetism does not emerge directly from the strain itself but rather from the creation of compressed structural units within ferroelastically formed twin-wall domains. The compressed structural units are magnetically active with the rocksalt-type high-spin/low-spin order. Our study highlights that the ferroelastic nature of ferromagnetic structural units is important for understanding the intriguing ferromagnetic properties in LCO thin films.},
doi = {10.1021/acs.nanolett.1c00756},
journal = {Nano Letters},
number = 9,
volume = 21,
place = {United States},
year = {Fri Apr 30 00:00:00 EDT 2021},
month = {Fri Apr 30 00:00:00 EDT 2021}
}

Works referenced in this record:

Stress-Strain Behavior During Compression of Polycrystalline La1-xCaxCoO3 Ceramics
journal, March 2005


Reversal of the Lattice Structure in SrCoO x Epitaxial Thin Films Studied by Real-Time Optical Spectroscopy and First-Principles Calculations
journal, August 2013


Correlation between magnetism and “dark stripes” in strained La 1−x Sr x CoO 3 epitaxial films (0 ≤ x ≤ 0.1)
journal, December 2015

  • Lan, Q. Q.; Shen, X.; Yang, H. W.
  • Applied Physics Letters, Vol. 107, Issue 24
  • DOI: 10.1063/1.4937562

Reversible redox reactions in an epitaxially stabilized SrCoOx oxygen sponge
journal, August 2013

  • Jeen, Hyoungjeen; Choi, Woo Seok; Biegalski, Michael D.
  • Nature Materials, Vol. 12, Issue 11
  • DOI: 10.1038/nmat3736

Ferroelastic Behavior of LaCoO3-Based Ceramics
journal, September 2001


Temperature- and pressure-driven spin-state transitions in LaCoO 3
journal, February 2007


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


Oxygen Vacancy Ordering Modulation of Magnetic Anisotropy in Strained LaCoO 3– x Thin Films
journal, October 2018

  • Zhang, Ningbin; Zhu, Yinlian; Li, Da
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 44
  • DOI: 10.1021/acsami.8b13674

Dimensionality Controlled Octahedral Symmetry-Mismatch and Functionalities in Epitaxial LaCoO 3 /SrTiO 3 Heterostructures
journal, June 2015


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

Strain-sensitive spin-state ordering in thin films of perovskite LaCoO 3
journal, November 2015


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

Ferroelasticity
journal, September 1984


TEM observations of rhombohedral and monoclinic domains in LaCoO 3 -based ceramics
journal, March 2008


Strain-induced high-temperature perovskite ferromagnetic insulator
journal, March 2018

  • Meng, Dechao; Guo, Hongli; Cui, Zhangzhang
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 12
  • DOI: 10.1073/pnas.1707817115

Strain control of oxygen kinetics in the Ruddlesden-Popper oxide La1.85Sr0.15CuO4
journal, January 2018


Spin state transition and covalent bonding in LaCoO 3
journal, November 2012


Suppression of spin-state transition in epitaxially strained LaCoO 3
journal, November 2008


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


Phase transitions in ferroelastic and co-elastic crystals
journal, April 1990


High‐Pressure Neutron Diffraction Study of LaCoO 3
journal, January 2019

  • Capone, Mara; Ridley, Christopher J.; Funnell, Nicholas P.
  • physica status solidi (a), Vol. 216, Issue 6
  • DOI: 10.1002/pssa.201800736

Thermally induced insulator-metal transition in LaCoO 3 :   A view based on the Mott transition
journal, July 1998


Calculation of critical layer thickness versus lattice mismatch for Ge x Si 1− x /Si strained‐layer heterostructures
journal, August 1985

  • People, R.; Bean, J. C.
  • Applied Physics Letters, Vol. 47, Issue 3
  • DOI: 10.1063/1.96206

Suppressed Dependence of Polarization on Epitaxial Strain in Highly Polar Ferroelectrics
journal, May 2007


Oxygen Diode Formed in Nickelate Heterostructures by Chemical Potential Mismatch
journal, March 2018


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


Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCo O 3 δ thin films
journal, March 2020


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


Structural and Magnetic Properties of LaCoO 3 /SrTiO 3 Multilayers
journal, July 2016

  • Zhang, Hongrui; Zhang, Jing; Yang, Huaiwen
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 28
  • DOI: 10.1021/acsami.6b03756

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


Valence-state reflectometry of complex oxide heterointerfaces
journal, September 2016


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

Room‐Temperature Ferromagnetic Insulating State in Cation‐Ordered Double‐Perovskite Sr 2 Fe 1+ x Re 1− x O 6 Films
journal, November 2018

  • Sohn, Changhee; Skoropata, Elizabeth; Choi, Yongseong
  • Advanced Materials, Vol. 31, Issue 4
  • DOI: 10.1002/adma.201805389

Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure
journal, May 2019


Nanoscale ferroelastic twins formed in strained LaCoO 3 films
journal, March 2019