skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Atomic-scale determination of spontaneous magnetic reversal in oxide heterostructures

Abstract

Interfaces between transition metal oxides are known to exhibit emerging electronic and magnetic properties. Here we report intriguing magnetic phenomena for La 2/3 Sr 1/3 MnO 3 films on an SrTiO 3 (001) substrate (LSMO/STO), where the interface governs the macroscopic properties of the entire monolithic thin film. The interface is characterized on the atomic level utilizing scanning transmission electron microscopy and electron energy loss spectroscopy (STEM-EELS), and density functional theory (DFT) is employed to elucidate the physics. STEM-EELS reveals mixed interfacial stoichiometry, subtle lattice distortions, and oxidation-state changes. Magnetic measurements combined with DFT calculations demonstrate that a unique form of antiferromagnetic exchange coupling appears at the interface, generating a novel exchange spring-type interaction that results in a remarkable spontaneous magnetic reversal of the entire ferromagnetic film, and an inverted magnetic hysteresis, persisting above room temperature. Formal oxidation states derived from electron spectroscopy data expose the fact that interfacial oxidation states are not consistent with nominal charge counting. The present work demonstrates the necessity of atomically resolved electron microscopy and spectroscopy for interface studies. Theory demonstrates that interfacial nonstoichiometry is an essential ingredient, responsible for the observed physical properties. The DFT-calculated electrostatic potential is flat in both the LSMO andmore » STO sides (no internal electric field) for both Sr-rich and stoichiometric interfaces, while the DFT-calculated charge density reveals no charge transfer/accumulation at the interface, indicating that oxidation-state changes do not necessarily reflect charge transfer and that the concept of polar mismatch is not applicable in metal−insulator polar−nonpolar interfaces.« less

Authors:
; ; ; ; ; ; ; ; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1511530
Grant/Contract Number:  
S0002136; AC02-98CH10886; FG02-09ER46554
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 21; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Saghayezhian, M., Kouser, Summayya, Wang, Zhen, Guo, Hangwen, Jin, Rongying, Zhang, Jiandi, Zhu, Yimei, Pantelides, Sokrates T., and Plummer, E. W. Atomic-scale determination of spontaneous magnetic reversal in oxide heterostructures. United States: N. p., 2019. Web. doi:10.1073/pnas.1819570116.
Saghayezhian, M., Kouser, Summayya, Wang, Zhen, Guo, Hangwen, Jin, Rongying, Zhang, Jiandi, Zhu, Yimei, Pantelides, Sokrates T., & Plummer, E. W. Atomic-scale determination of spontaneous magnetic reversal in oxide heterostructures. United States. doi:10.1073/pnas.1819570116.
Saghayezhian, M., Kouser, Summayya, Wang, Zhen, Guo, Hangwen, Jin, Rongying, Zhang, Jiandi, Zhu, Yimei, Pantelides, Sokrates T., and Plummer, E. W. Wed . "Atomic-scale determination of spontaneous magnetic reversal in oxide heterostructures". United States. doi:10.1073/pnas.1819570116.
@article{osti_1511530,
title = {Atomic-scale determination of spontaneous magnetic reversal in oxide heterostructures},
author = {Saghayezhian, M. and Kouser, Summayya and Wang, Zhen and Guo, Hangwen and Jin, Rongying and Zhang, Jiandi and Zhu, Yimei and Pantelides, Sokrates T. and Plummer, E. W.},
abstractNote = {Interfaces between transition metal oxides are known to exhibit emerging electronic and magnetic properties. Here we report intriguing magnetic phenomena for La 2/3 Sr 1/3 MnO 3 films on an SrTiO 3 (001) substrate (LSMO/STO), where the interface governs the macroscopic properties of the entire monolithic thin film. The interface is characterized on the atomic level utilizing scanning transmission electron microscopy and electron energy loss spectroscopy (STEM-EELS), and density functional theory (DFT) is employed to elucidate the physics. STEM-EELS reveals mixed interfacial stoichiometry, subtle lattice distortions, and oxidation-state changes. Magnetic measurements combined with DFT calculations demonstrate that a unique form of antiferromagnetic exchange coupling appears at the interface, generating a novel exchange spring-type interaction that results in a remarkable spontaneous magnetic reversal of the entire ferromagnetic film, and an inverted magnetic hysteresis, persisting above room temperature. Formal oxidation states derived from electron spectroscopy data expose the fact that interfacial oxidation states are not consistent with nominal charge counting. The present work demonstrates the necessity of atomically resolved electron microscopy and spectroscopy for interface studies. Theory demonstrates that interfacial nonstoichiometry is an essential ingredient, responsible for the observed physical properties. The DFT-calculated electrostatic potential is flat in both the LSMO and STO sides (no internal electric field) for both Sr-rich and stoichiometric interfaces, while the DFT-calculated charge density reveals no charge transfer/accumulation at the interface, indicating that oxidation-state changes do not necessarily reflect charge transfer and that the concept of polar mismatch is not applicable in metal−insulator polar−nonpolar interfaces.},
doi = {10.1073/pnas.1819570116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 21,
volume = 116,
place = {United States},
year = {2019},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1819570116

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Hidden Magnetic Configuration in Epitaxial La 1 x Sr x MnO 3 Films
journal, December 2010


Quenching of the Hopkinson maximum under contamination in the system Gd(0001)/W(110)
journal, May 1990


Magnetism and structural distortion in the La 0.7 Sr 0.3 Mn O 3 metallic ferromagnet
journal, June 1996


Strain-dependent magnetic phase diagram of epitaxial La0.67Sr0.33MnO3 thin films
journal, April 2000

  • Tsui, F.; Smoak, M. C.; Nath, T. K.
  • Applied Physics Letters, Vol. 76, Issue 17
  • DOI: 10.1063/1.126363

Interlayer coupling through a dimensionality-induced magnetic state
journal, April 2016

  • Gibert, M.; Viret, M.; Zubko, P.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11227

Physics of Ultrathin Films and Heterostructures of Rare-Earth Nickelates
journal, July 2016


Enhanced Local Magnetization by Interface Engineering in Perovskite-Type Correlated Oxide Heterostructures
journal, January 2015

  • Huijben, Mark; Liu, Yaohua; Boschker, Hans
  • Advanced Materials Interfaces, Vol. 2, Issue 3
  • DOI: 10.1002/admi.201400416

Interface-induced phenomena in magnetism
journal, June 2017


Tailoring Magnetic Interlayer Coupling in La 0.7 Sr 0.3 MnO 3 / SrRuO 3 Superlattices
journal, April 2010


Structural phases driven by oxygen vacancies at the La 0.7 Sr 0.3 MnO 3 /SrTiO 3 hetero-interface
journal, January 2015

  • Nord, M.; Vullum, P. E.; Moreau, M.
  • Applied Physics Letters, Vol. 106, Issue 4
  • DOI: 10.1063/1.4906920

Impact of interfacial coupling of oxygen octahedra on ferromagnetic order in La0.7Sr0.3MnO3/SrTiO3 heterostructures
journal, January 2017

  • Li, Xiaoyan; Lindfors-Vrejoiu, Ionela; Ziese, Michael
  • Scientific Reports, Vol. 7, Issue 1
  • DOI: 10.1038/srep40068

Avoiding the Polarization Catastrophe in LaAlO 3 Overlayers on SrTiO 3 ( 001 ) through Polar Distortion
journal, March 2009


Polar oxide surfaces
journal, July 2000


XSEDE: Accelerating Scientific Discovery
journal, September 2014

  • Towns, John; Cockerill, Timothy; Dahan, Maytal
  • Computing in Science & Engineering, Vol. 16, Issue 5
  • DOI: 10.1109/MCSE.2014.80

Colloquium : Opportunities in nanomagnetism
journal, January 2006


Hidden Interface Driven Exchange Coupling in Oxide Heterostructures
journal, May 2017

  • Chen, Aiping; Wang, Qiang; Fitzsimmons, Michael R.
  • Advanced Materials, Vol. 29, Issue 26
  • DOI: 10.1002/adma.201700672

Insulator-metal transition and giant magnetoresistance in La 1 x Sr x MnO 3
journal, May 1995


Atomic-resolution imaging of oxidation states in manganites
journal, February 2009


Field-dependent ac susceptibility of amorphous ( Fe 1 x Mn x ) 75 P 16 B 6 Al 3 : Weakly frustrated regime
journal, October 1995


Unravelling the role of the interface for spin injection into organic semiconductors
journal, June 2010

  • Barraud, Clément; Seneor, Pierre; Mattana, Richard
  • Nature Physics, Vol. 6, Issue 8
  • DOI: 10.1038/nphys1688

Electron Accumulation and Emergent Magnetism in LaMnO 3 / SrTiO 3 Heterostructures
journal, October 2017


Magnetization switching and inverted hysteresis in perpendicular antiferromagnetic superlattices
journal, May 2014

  • Charilaou, M.; Bordel, C.; Hellman, F.
  • Applied Physics Letters, Vol. 104, Issue 21
  • DOI: 10.1063/1.4880821

Termination control of the interface dipole in La 0.7 Sr 0.3 MnO 3 / Nb : SrTiO 3 (001) Schottky junctions
journal, February 2009


Critical Neutron Scattering in SrTi O 3 and KMn F 3
journal, December 1972


All-oxide–based synthetic antiferromagnets exhibiting layer-resolved magnetization reversal
journal, July 2017


Giant Magnetoresistance in Ferromagnet/Superconductor Superlattices
journal, February 2005


Colossal magnetoresistance magnetic tunnel junctions grown by molecular-beam epitaxy
journal, April 2000

  • O’Donnell, J.; Andrus, A. E.; Oh, S.
  • Applied Physics Letters, Vol. 76, Issue 14
  • DOI: 10.1063/1.126210

Exchange-spring behavior in epitaxial hard/soft magnetic bilayers
journal, November 1998


Magnetic Oxide Heterostructures
journal, July 2014


Inverted hysteresis and giant exchange bias in La0.7Sr0.3MnO3/SrRuO3 superlattices
journal, August 2010

  • Ziese, M.; Vrejoiu, I.; Hesse, D.
  • Applied Physics Letters, Vol. 97, Issue 5
  • DOI: 10.1063/1.3470101

Interfacial Coupling-Induced Ferromagnetic Insulator Phase in Manganite Film
journal, June 2016


Atomic-scale control of magnetic anisotropy via novel spin–orbit coupling effect in La 2/3 Sr 1/3 MnO 3 /SrIrO 3 superlattices
journal, May 2016

  • Yi, Di; Liu, Jian; Hsu, Shang-Lin
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 23
  • DOI: 10.1073/pnas.1524689113

Observation of complete inversion of the hysteresis loop in a bimodal magnetic thin film
journal, March 2017


A novel hysteresis loop and indirect exchange coupling in Co/Pt/Gd/Pt multilayer films
journal, September 1993

  • Takanashi, K.; Kurokawa, H.; Fujimori, H.
  • Applied Physics Letters, Vol. 63, Issue 11
  • DOI: 10.1063/1.110756

Robust isothermal electric control of exchange bias at room temperature
journal, June 2010

  • He, Xi; Wang, Yi; Wu, Ning
  • Nature Materials, Vol. 9, Issue 7
  • DOI: 10.1038/nmat2785

The Origin of Oxygen Vacancies Controlling La 2/3 Sr 1/3 MnO 3 Electronic and Magnetic Properties
journal, January 2016

  • Guo, Haizhong; Wang, Jia-ou; He, Xu
  • Advanced Materials Interfaces, Vol. 3, Issue 5
  • DOI: 10.1002/admi.201500753

Interface Physics in Complex Oxide Heterostructures
journal, March 2011


Visualizing the interfacial evolution from charge compensation to metallic screening across the manganite metal–insulator transition
journal, March 2014

  • Mundy, Julia A.; Hikita, Yasuyuki; Hidaka, Takeaki
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4464

Thermal hysteresis of the initial permeability of soft ferrites at transition temperatures
journal, June 1993


Symmetry and lattice mismatch induced strain accommodation near and away from correlated perovskite interfaces
journal, September 2014

  • Vailionis, A.; Boschker, H.; Liao, Z.
  • Applied Physics Letters, Vol. 105, Issue 13
  • DOI: 10.1063/1.4896969

Preventing the Reconstruction of the Polar Discontinuity at Oxide Heterointerfaces
journal, March 2012

  • Boschker, H.; Verbeeck, J.; Egoavil, R.
  • Advanced Functional Materials, Vol. 22, Issue 11
  • DOI: 10.1002/adfm.201102763

Nearly total spin polarization in La2/3Sr1/3MnO3 from tunneling experiments
journal, January 2003

  • Bowen, M.; Bibes, M.; Barthélémy, A.
  • Applied Physics Letters, Vol. 82, Issue 2
  • DOI: 10.1063/1.1534619

Termination layer dependence of Schottky barrier height for La 0.6 Sr 0.4 MnO 3 / Nb : SrTiO 3 heterojunctions
journal, June 2010


Giant sharp and persistent converse magnetoelectric effects in multiferroic epitaxial heterostructures
journal, April 2007

  • Eerenstein, W.; Wiora, M.; Prieto, J. L.
  • Nature Materials, Vol. 6, Issue 5
  • DOI: 10.1038/nmat1886

Exchange bias in LaNiO3–LaMnO3 superlattices
journal, January 2012

  • Gibert, Marta; Zubko, Pavlo; Scherwitzl, Raoul
  • Nature Materials, Vol. 11, Issue 3
  • DOI: 10.1038/nmat3224

Grain size effect on the Néel temperature and magnetic properties of nanocrystalline NiFe2O4 spinel
journal, January 2002

  • Chinnasamy, C. N.; Narayanasamy, A.; Ponpandian, N.
  • Journal of Magnetism and Magnetic Materials, Vol. 238, Issue 2-3
  • DOI: 10.1016/S0304-8853(01)00928-3

A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004


Why some interfaces cannot be sharp
journal, January 2006

  • Nakagawa, Naoyuki; Hwang, Harold Y.; Muller, David A.
  • Nature Materials, Vol. 5, Issue 3, p. 204-209
  • DOI: 10.1038/nmat1569

Anomalous Spontaneous Reversal in Magnetic Heterostructures
journal, April 2006


Superconducting Interfaces Between Insulating Oxides
journal, August 2007


Exchange bias
journal, February 1999


Lattice Effects on the Magnetoresistance in Doped LaMn O 3
journal, July 1995


Optimized fabrication of high-quality La 0.67 Sr 0.33 MnO 3 thin films considering all essential characteristics
journal, April 2011


Orbital-Occupancy versus Charge Ordering and the Strength of Electron Correlations in Electron-Doped CaMnO 3
journal, July 2007


Direct imaging of the coexistence of ferromagnetism and superconductivity at the LaAlO3/SrTiO3 interface
journal, September 2011

  • Bert, Julie A.; Kalisky, Beena; Bell, Christopher
  • Nature Physics, Vol. 7, Issue 10, p. 767-771
  • DOI: 10.1038/nphys2079

Anomalously deep polarization in SrTi O 3 (001) interfaced with an epitaxial ultrathin manganite film
journal, October 2016