Large magnetoelectric coupling in multiferroic oxide heterostructures assembled via epitaxial lift-off

Pesquera, David; Khestanova, Ekaterina; Ghidini, M.; Zhang, S.; Rooney, Aidan; Maccherozzi, Francesco; Riego, Patricia; Farokhipoor, Saeedeh; Kim, J.; Moya, Xavier; Vickers, M. E.; Stelmashenko, Nadia; Haigh, Sarah J.; Dhesi, S. S.; Mathur, N. D.

doi:10.1038/s41467-020-16942-x

Cited by 61 publications

(65 citation statements)

References 84 publications

(145 reference statements)

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“…Mechanical and electric-field manipulation of micrometer-sized freestanding flakes in electron-microscopy experiments [35,36] and straining experiments on polymersupported ultrathin perovskite membranes (restricted to films <10 nm in thickness) [37,38] have demonstrated their exceptional flexibility. Whereas transfer to polymers or electroactive substrates has been exploited to tune magnetic properties, [38][39][40] test the resilience of ferroelectric properties, [41][42][43] or induce ferroelectricity in non-polar materials, [44] deterministic strain control of properties has not been demonstrated on single-crystal ferroelectric membranes.…”

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confidence: 99%

Beyond Substrates: Strain Engineering of Ferroelectric Membranes

et al. 2020

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Integrating the diverse functionalities of complex oxides into semiconductor [1-7] and flexible [8-12] electronics is a major technological challenge that has motivated extensive work. But despite considerable effort, the structural, chemical, and thermal mismatches between such substrates and complex-oxide materials often yield films with considerably worse crystal quality than that attained on single-crystal perovskite substrates. Alternative strategies for hetero-integration via substrate release and transfer, mimicking the fabrication processes of van-der-Waals heterostructures, [13-15] are just now beginning to yield single-crystal oxide films on arbitrary substrates, [16-21] thus circumventing the constraints of epitaxial growth. Moreover, these detached films no longer experience mechanical constraint from the substrate, giving more flexibility in structural manipulation and heterostructure assembly. Strain control over the lattice structure is particularly impactful in ferroelectrics where the polarization is directly connected to structural distortions. [22,23] In thin films, strain can define the optimal operating temperature regime [24-26] or domain configuration [27-29] that will boost electro-mechanical or thermal functionalities, Strain engineering in perovskite oxides provides for dramatic control over material structure, phase, and properties, but is restricted by the discrete strain states produced by available high-quality substrates. Here, using the ferroelectric BaTiO 3 , production of precisely strain-engineered, substratereleased nanoscale membranes is demonstrated via an epitaxial lift-off process that allows the high crystalline quality of films grown on substrates to be replicated. In turn, fine structural tuning is achieved using interlayer stress in symmetric trilayer oxide-metal/ferroelectric/oxide-metal structures fabricated from the released membranes. In devices integrated on silicon, the interlayer stress provides deterministic control of ordering temperature (from 75 to 425 °C) and releasing the substrate clamping is shown to dramatically impact ferroelectric switching and domain dynamics (including reducing coercive fields to <10 kV cm −1 and improving switching times to <5 ns for a 20 µm diameter capacitor in a 100-nm-thick film). In devices integrated on flexible polymers, enhanced room-temperature dielectric permittivity with large mechanical tunability (a 90% change upon ±0.1% strain application) is demonstrated. This approach paves the way toward the fabrication of ultrafast CMOS-compatible ferroelectric memories and ultrasensitive flexible nanosensor devices, and it may also be leveraged for the stabilization of novel phases and functionalities not achievable via direct epitaxial growth. Perovskite ABO 3 oxides can display an immense number of phases and functions by merely changing the A-and B-site cations. Even within a single chemistry, multiple phases can be in competition, and their stability can be tuned statically by fixing The ORCID identification number(s) for the ...

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Beyond Substrates: Strain Engineering of Ferroelectric Membranes

et al. 2020

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“…One of the main challenges in working with BFO films is preparation of the film and selection of suitable substrate. There are several working deposition methods, all with their own capabilities and limitations, like molecular beam epitaxy (MBE), metal-organic vapor deposition (MOCVD) and pulsed layer deposition (PLD) [7], but these all struggle when trying to deposit a uniform and precisely detailed thin layer of BFO at low temperatures. The only method that is able to clear all these requirements is atomic layer deposition (ALD) [8][9][10][11][12], which is the reason why it is used to prepare BFO layers in this paper.…”

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“…Preparation of functional oxides on flexible substrates is on of the great technological challenges because of this film's brittleness. There are several approaches for preparation of the flexible structures, among them are heteroepitaxy on organic or inorganic flexible substrates [19], and epitaxial lift-off [7]. The epitaxial lift-of advance is possible growth of structurally perfect film.…”

Section: Introductionmentioning

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Crack resistance of bismuth ferrite films obtained on a flexible substrate

et al. 2021

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Ultrathin BiOx and FeOx layers were obtained by Atomic Layer Deposition (ALD) on the surface of a flexible Kapton substrate (poly (4,4’-oxydiphenylene-pyromellitimide)) at a temperature of 250 °C. The layer thickness was 50 - 100 nm. Surface morphology, electrical polarization, and mechanical properties were investigated by Atomic Force Microscope, Piezoelectric Force Microscopy and Force Modulation Microscopy. Chemical analysis was performed by X-ray Photoelectron Spectroscopy, where the formation of Bi2O3 and Fe2O3 phases, as well as intermediate phases in the Bi-Fe-O system, was observed. With a small increase in the Bi content of the film, the BFO / Kapton structure becomes more crack resistant. Modification of the Kapton surface with bismuth and iron oxides showed that such a composition exhibits multiferroic behavior.

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“…Such techniques are rapidly emerging as an approach for tuning the lattice distortion and strain in ferroelectrics [35]- [41]. Several sacrificial layers have been developed, such as water soluble Sr3Al2O6 [37], acid solution soluble La0.67Sr0.33MnO3 (LSMO) [38], and graphene for mechanical exfoliation [40], leading to freestanding ferroelectric films down to the monolayer limit [27], as well as integration of single-crystalline membranes [40], and flexible layers with super-elasticity [41]. We demonstrate that quantitatively different features are obtained in freestanding BFO membranes versus their clamped counterparts, both in quasistatic measurements of the energetics (coercive field from hysteresis measurements) and dynamical measurements (pulsed switching studies) of the switching process.…”

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“…[38] to completely lift-off the Pt/SRO/BFO/SRO stack from the STO substrate. A supportive PDMS layer is used to then transfer the stack to a Pt/Si (001) substrate.…”

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The role of lattice dynamics in ferroelectric switching

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Parsonnet

Chen

et al. 2021

Preprint

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Reducing the switching energy of ferroelectric thin films remains an important goal in the pursuit of ultralow power ferroelectric memories and magnetoelectric spin-orbit logic devices. Here, we elucidate the fundamental role of lattice dynamics in ferroelectric switching by combining thermodynamic calculations, experiments, and phase-field simulations on both freestanding BiFeO3 membranes and films clamped to a substrate. We observe a distinct evolution of the ferroelectric domain pattern, from striped, 71° ferroelastic domains (spacing of ~100 nm) in clamped BiFeO3 films, to large (10’s of micrometers) 180° domains or even single domain structures, in freestanding films. Through the use of piezoresponse force microscopy, X-ray diffraction, polarization-electric field hysteresis loops, and high-speed pulsed ferroelectric switching experiments, it is found that removing the constraints imposed by the requirement of macroscopic continuity of deformation (also known as the von Mises criterion in the deformation of solids)[1]–[3] to the substrate, we can realize a ~40% reduction of the switching voltage and a consequent ~60% gain in the switching speed. The work highlights the critical role of mechanics and the clamping effect from the substrate in setting the energetics and dynamics of switching in ferroelectrics.

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Large magnetoelectric coupling in multiferroic oxide heterostructures assembled via epitaxial lift-off

Cited by 61 publications

References 84 publications

Beyond Substrates: Strain Engineering of Ferroelectric Membranes

Beyond Substrates: Strain Engineering of Ferroelectric Membranes

Crack resistance of bismuth ferrite films obtained on a flexible substrate

The role of lattice dynamics in ferroelectric switching

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