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Engineering exchange bias at the interface of self-polarized ultrathin ferroelectric BaTiO3 and ferromagnetic La0.67Sr0.33MnO3

Tuhin Maity1,2,3,*,¶, Manisha Bansal2,¶, Nives Strkalj1,4, Kapildeb Dolui1, Di Zhang5, Zihao He5, Guillaume F. Nataf1,§, Adam Lovett1, Massimo Ghidini1,6,7 et al.

Sarnjeet S. Dhesi6, Ping Lu8, Haiyan Wang5, Weiwei Li1,9,†, and Judith L. MacManus-Driscoll1,‡

  • *Contact author: tuhin@iisertvm.ac.in
  • †Contact author: wl337@nuaa.edu.cn
  • ‡Contact author: jld35@cam.ac.uk
  • §Present address: GREMAN UMR7347, CNRS, University of Tours, INSA Centre Val de Loire, 37000 Tours, France
  • These authors contributed equally.
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Phys. Rev. Applied 22, 054035 – Published 13 November, 2024

DOI: https://doi.org/10.1103/PhysRevApplied.22.054035

Abstract

We investigate the emergence and optimization of conventional exchange bias (EB) in ultrathin (<10 nm) ferroelectric (FE) BaTiO3 (BTO)/ferromagnetic (FM) La0.67Sr0.33MnO3 (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.

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Phys. Rev. Applied 22, 054035– Published 13 November, 2024
  • Received 20 March 2024
  • Revised 11 September 2024
  • Accepted 4 October 2024
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