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Engineering exchange bias at the interface of self-polarized ultrathin ferroelectric Ba⁢Ti⁢O3 and ferromagnetic La0.67⁢Sr0.33⁢Mn⁢O3

Journal Article · · Physical Review Applied
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [4];  [7];  [8];  [9];  [5];  [10];  [4]
  1. Univ. of Cambridge (United Kingdom); Indian Institute of Science Education and Research (India)
  2. Indian Institute of Science Education and Research (India)
  3. Univ. of Cambridge (United Kingdom); Institute of Physics (Croatia)
  4. Univ. of Cambridge (United Kingdom)
  5. Purdue Univ., West Lafayette, IN (United States)
  6. Univ. of Cambridge (United Kingdom); Univ. of Tours (France)
  7. Univ. of Cambridge (United Kingdom); Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.; Univ. of Parma (Italy)
  8. Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.
  9. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  10. Univ. of Cambridge (United Kingdom); Nanjing Univ. of Aeronautics and Astronautics (China)

We investigate the emergence and optimization of conventional exchange bias (EB) in ultrathin (<10 nm) ferroelectric (FE) Ba⁢Ti⁢O3 (BTO)/ferromagnetic (FM) La0.67⁢Sr0.33⁢Mn⁢O3 (LSMO) epitaxial bilayers without an antiferromagnetic (AFM) material. The EB originates from the electronic orbital reconstruction at the FE-FM interface due to the ferroelectric polarization. We achieve maximum EB of approximately 42 Oe with single-domain polarization in nine-unit-cell-thick BTO, setting the BTO thickness above the critical threshold for ferroelectricity yet below the thickness of strain relaxation and multidomain breakdown. Furthermore, the LSMO layer needs to be thick enough to sustain both the FM layer and polarization-induced AFM spin configuration at the LSMO/BTO interface, yet as thin as possible to enable the EB loop shift. The temperature, training, field, and thickness dependence of the EB confirm that the LSMO/BTO interface exhibits conventional EB despite its unconventional origin. Using x-ray magnetic circular dichroism, scanning transmission electron microscopy, and density-functional-theory calculations, we confirm that the macroscopic EB effect originates from the interfacial AFM spin configuration in LSMO driven by FE-induced d-orbital modifications in interfacial Mn ions. Thus, we engineer strong interfacial EB coupling in artificial multiferroics without a conventional AFM material by controlling FE polarization, highlighting the potential for advanced spintronic applications.

Research Organization:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
Grant/Contract Number:
NA0003525
OSTI ID:
2584641
Journal Information:
Physical Review Applied, Journal Name: Physical Review Applied Journal Issue: 5 Vol. 22; ISSN 2331-7019
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (47)

Ultrathin Limit of Exchange Bias Coupling at Oxide Multiferroic/Ferromagnetic Interfaces journal July 2013
Magnetoelectric Coupling Induced by Interfacial Orbital Reconstruction journal September 2015
Hidden Interface Driven Exchange Coupling in Oxide Heterostructures journal May 2017
Tailoring Self-Polarization of BaTiO 3 Thin Films by Interface Engineering and Flexoelectric Effect journal November 2016
Exchange bias journal February 1999
Asymmetric shift of exchange bias loop in Ni-Ni(OH)2 core-shell nanoparticles journal November 2018
Atomic-Scale Control of Magnetism at the Titanite-Manganite Interfaces journal March 2019
Self-Polarization in Epitaxial Fully Matched Lead-Free Bismuth Sodium Titanate Based Ferroelectric Thin Films journal July 2018
Reversible Modulation of Orbital Occupations via an Interface-Induced Polar State in Metallic Manganites journal August 2014
Critical thickness for ferroelectricity in perovskite ultrathin films journal April 2003
Reversible electric control of exchange bias in a multiferroic field-effect device journal July 2010
Interface-induced room-temperature multiferroicity in BaTiO3 journal August 2011
Exchange bias in LaNiO3–LaMnO3 superlattices journal January 2012
Control of quantum magnets by atomic exchange bias journal December 2014
Signatures of enhanced out-of-plane polarization in asymmetric BaTiO3 superlattices integrated on silicon journal January 2022
Understanding and designing magnetoelectric heterostructures guided by computation: progresses, remaining questions, and perspectives journal May 2017
Oxygen-vacancy induced magnetic phase transitions in multiferroic thin films journal June 2020
Confinement of magnetism in atomically thin La0.7Sr0.3CrO3/La0.7Sr0.3MnO3 heterostructures journal May 2019
Atomic-scale engineering of ferroelectric-ferromagnetic interfaces of epitaxial perovskite films for functional properties journal September 2017
Re-epithelialization and immune cell behaviour in an ex vivo human skin model journal January 2020
Self-biased magnetoelectric switching at room temperature in three-phase ferroelectric–antiferromagnetic–ferrimagnetic nanocomposites journal May 2021
Strain engineering induced interfacial self-assembly and intrinsic exchange bias in a manganite perovskite film journal August 2013
Control of magnetism in Pb(Zr 0.2 Ti 0.8 )O 3 /La 0.8 Sr 0.2 MnO 3 multiferroic heterostructures (invited) journal April 2011
Exchange-biased magnetic tunnel junctions and application to nonvolatile magnetic random access memory (invited) journal April 1999
Exotic exchange bias at epitaxial ferroelectric-ferromagnetic interfaces journal July 2014
Induced Ti magnetization at La 0.7 Sr 0.3 MnO 3 and BaTiO 3 interfaces journal April 2016
Interface magnetization transition via minority spin injection journal December 2016
Interface control of bulk ferroelectric polarization journal May 2012
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
Interface-induced multiferroism by design in complex oxide superlattices journal June 2017
Advanced capabilities for materials modelling with Quantum ESPRESSO journal October 2017
Theory of the Role of Covalence in the Perovskite-Type Manganites [ La ,   M ( II ) ] Mn O 3 journal October 1955
Thickness-dependent polarization-induced intrinsic magnetoelectric effects in L a 0.67 S r 0.33 Mn O 3 / PbZ r 0.52 T i 0.48 O 3 heterostructures journal September 2019
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Coercivity in exchange-bias bilayers journal January 2001
Training of the exchange-bias effect: A simple analytic approach journal July 2004
Field-cooling dependence of exchange bias in a granular system of Fe nanoparticles embedded in an Fe oxide matrix journal August 2004
Critical thickness and orbital ordering in ultrathin La 0.7 Sr 0.3 MnO 3 films journal September 2008
Prediction of electrically induced magnetic reconstruction at the manganite/ferroelectric interface journal November 2009
Accuracy of the spin sum rule in XMCD for the transition-metal L edges from manganese to copper journal November 2009
Inducing exchange bias in La 0.67 Sr 0.33 MnO 3 − δ /SrTiO 3 thin films by strain and oxygen deficiency journal October 2013
Origin of the asymmetric exchange bias in BiFeO 3 / Bi 2 Fe 4 O 9 nanocomposite journal April 2014
Interface Ferromagnetism and Orbital Reconstruction in BiFeO 3 − La 0.7 Sr 0.3 MnO 3 Heterostructures journal July 2010
Depolarizing-Field Effects in Epitaxial Capacitor Heterostructures journal October 2019
Generalized Gradient Approximation Made Simple journal October 1996
Coercivity Enhancement in Exchange Biased Systems Driven by Interfacial Magnetic Frustration journal April 2000
Enhancement of Ferroelectricity in Strained BaTiO3 Thin Films journal November 2004