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Author(s): J. T. Heron (corresponding author) [1]; J. L. Bosse [2]; Q. He [3]; Y. Gao [4, 5]; M. Trassin [6]; L. Ye [2]; J. D. Clarkson [7]; C. Wang [...]

A few nanometer thick titanium adhesion layer was used to grow Pt electrodes by pulsed deposition on yttrium-stabilized zirconia (111). The Pt electrodes with ultrafast surface and perfect (111) monocrystalline orientation provide new route for the anisotropic characterization of multiferroic or magnetoelectric materials.

Multiferroic BiFeO3 (BFO)/La0.7.Sr0.3MnO3 heterostructured thin films were grown by pulsed laser deposition on polished spark plasma sintered LaAlO3 (LAO) polycrystalline substrates. Both polycrystalline LAO substrates and BFO films were locally characterized using electron backscattering diffraction, which confirmed the high-quality local epitaxial growth on each substrate grain. Piezoforce microscopy was used to image and switch the piezo-domains, and the results are consistent with the relative orientation of the ferroelectric variants with the surface normal. This high-throughput synthesis process opens the routes towards wide survey of electronic properties as a function of crystalline orientation in complex oxide thin film synthesis. [ABSTRACT FROM AUTHOR]

Epitaxial films of an alternative multiferroic material, GaFeO3 (GFO), were grown by pulsed laser deposition on yttrium-stabilized zirconia (001) and on conducting buffer layers of indium tin oxide (001). They present a perfect epitaxial growth along the GFO [010] axis and six crystallographic variants in the film’s plane. Their magnetic properties are close to those of the bulk with an out-of-plane [010] hard direction and a Curie temperature of ∼200 K. The films did exhibit ferroelectric properties when characterized by electrostatic force microscopy. [ABSTRACT FROM AUTHOR]

The manipulation of antiferromagnetic order in magnetoelectric Cr2O3 using electric field has been of great interest due to its potential in low-power electronics. The substantial leakage and low dielectric breakdown observed in twinned Cr2O3 thin films, however, hinders its development in energy efficient spintronics. To compensate, large film thicknesses (250 nm or greater) have been employed at the expense of device scalability. Recently, epitaxial V2O3 thin film electrodes have been used to eliminate twin boundaries and significantly reduce the leakage of 300 nm thick single crystal films. Here we report the electrical endurance and magnetic properties of thin (less than 100 nm) single crystal Cr2O3 films on epitaxial V2O3 buffered Al2O3 (0001) single crystal substrates. The growth of Cr2O3 on isostructural V2O3 thin film electrodes helps eliminate the existence of twin domains in Cr2O3 films, therefore significantly reducing leakage current and increasing dielectric breakdown. 60 nm thick Cr2O3 films show bulk-like resistivity (~ 1012 Ω cm) with a breakdown voltage in the range of 150–300 MV/m. Exchange bias measurements of 30 nm thick Cr2O3 display a blocking temperature of ~ 285 K while room temperature optical second harmonic generation measurements possess the symmetry consistent with bulk magnetic order. [ABSTRACT FROM AUTHOR]

We report direct experimental evidence for a room-temperature, ~130 µC/cm² ferroelectric polarization from the tetragonal-like BiFeO3 phase. The physical origin of this remarkable enhancement of ferroelectric polarization has been investigated by a combination of x-ray absorption spectroscopy, scanning transmission electron microscopy, and first principles calculations. A large strain-induced Fe-ion displacement relative to the oxygen octabedra, combined with the contribution of Bi 6s lone pair electrons, is the mechanism driving the large ferroelectric polarization in this tetragonal-like phase. [ABSTRACT FROM AUTHOR]

High-quality epitaxial thin films of Jeff = 1/2 Mott insulator Sr2IrO4 with increasing in-plane tensile strain have been grown on top of SrTiO3(001) substrates. Increasing the in-plane tensile strain up to ~0.3% was observed to drop the c/a tetragonality by 1.2%. X-ray absorption spectroscopy detected a strong reduction of the linear dichroism upon increasing in-plane tensile strain towards a reduced anisotropy in the local electronic structure. While the most relaxed thin film shows a consistent dependence with previously reported single crystal bulk measurements, electrical transport reveals a charge gap reduction from 200 meV down to 50 meV for the thinnest and most epitaxy-distorted film. We argue that the reduced tetragonality plays a major role in the change of the electronic structure, which is reflected in the change of the transport properties. Our work opens the possibility for exploiting epitaxial strain as a tool for both structural and functional manipulation of spin-orbit Mott systems. [ABSTRACT FROM AUTHOR]

Raman spectroscopy enables the non-destructive characterization of chemical composition, crystallinity, defects, or strain in countless materials. However, the Raman response of surfaces or thin films is often weak and obscured by dominant bulk signals. Here we overcome this limitation by placing a transferable porous gold membrane, (PAuM) on the surface of interest. Slot-shaped nanopores in the membrane act as plasmonic antennas and enhance the Raman response of the surface or thin film underneath. Simultaneously, the PAuM suppresses the penetration of the excitation laser into the bulk, efficiently blocking its Raman signal. Using graphene as a model surface, we show that this method increases the surface-to-bulk Raman signal ratio by three orders of magnitude. We find that 90% of the Raman enhancement occurs within the top 2.5 nm of the material, demonstrating truly surface-sensitive Raman scattering. To validate our approach, we quantify the strain in a 12.5 nm thin Silicon film and analyze the surface of a LaNiO 3 thin film. We observe a Raman mode splitting for the LaNiO 3 surface-layer, which is spectroscopic evidence that the surface structure differs from the bulk. These results validate that PAuM gives direct access to Raman signatures of thin films and surfaces., (© 2024. The Author(s).)

Light is an effective tool to probe the polarization and domain distribution in ferroelectric materials passively, that is, non-invasively, for example, via optical second harmonic generation (SHG). With the emergence of oxide electronics, there is now a strong demand to expand the role of light toward active control of the polarization. In this work, optical control of the ferroelectric polarization is demonstrated in prototypical epitaxial PbZr x Ti 1-x O 3 (PZT)-based heterostructures. This is accomplished in three steps, using above-bandgap UV light, while tracking the response of the polarization with optical SHG. First, it is found that UV-light exposure induces a transient enhancement or suppression of the ferroelectric polarization in films with an upward- or downward-oriented polarization, respectively. This behavior is attributed to a modified charge screening driven by the separation of photoexcited charge carriers at the Schottky interface of the ferroelectric thin film. Second, by taking advantage of this optical handle on electrostatics, remanent optical poling from a pristine multi-domain into a single-domain configuration is accomplished. Third, via thermal annealing or engineered electrostatic boundary conditions, a complete reversibility of the optical poling is further achieved. Hence, this work paves the way for the all-optical control of the spontaneous polarization in ferroelectric thin films., (© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH.)

Material surfaces encompass structural and chemical discontinuities that often lead to the loss of the property of interest in so-called dead layers. It is particularly problematic in nanoscale oxide electronics, where the integration of strongly correlated materials into devices is obstructed by the thickness threshold required for the emergence of their functionality. Here we report the stabilization of ultrathin out-of-plane ferroelectricity in oxide heterostructures through the design of an artificial flux-closure architecture. Inserting an in-plane-polarized ferroelectric epitaxial buffer provides the continuity of polarization at the interface; despite its insulating nature, we observe the emergence of polarization in our out-of-plane-polarized model of ferroelectric BaTiO 3 from the very first unit cell. In BiFeO 3 , the flux-closure approach stabilizes a 251° domain wall. Its unusual chirality is probably associated with the ferroelectric analogue to the Dzyaloshinskii-Moriya interaction. We, thus, see that in an adaptively engineered geometry, the depolarizing-field-screening properties of an insulator can even surpass those of a metal and be a source of functionality. This could be a useful insight on the road towards the next generation of oxide electronics., (© 2023. The Author(s).)

In the room-temperature magnetoelectric multiferroic BiFeO 3 , the noncollinear antiferromagnetic state is coupled to the ferroelectric order, opening applications for low-power electric-field-controlled magnetic devices. While several strategies have been explored to simplify the ferroelectric landscape, here we directly stabilize a single-domain ferroelectric and spin cycloid state in epitaxial BiFeO 3 (111) thin films grown on orthorhombic DyScO 3 (011). Comparing them with films grown on SrTiO 3 (111), we identify anisotropic in-plane strain as a powerful handle for tailoring the single antiferromagnetic state. In this single-domain multiferroic state, we establish the thickness limit of the coexisting electric and magnetic orders and directly visualize the suppression of the spin cycloid induced by the magnetoelectric interaction below the ultrathin limit of 1.4 nm. This as-grown single-domain multiferroic configuration in BiFeO 3 thin films opens an avenue both for fundamental investigations and for electrically controlled noncollinear antiferromagnetic spintronics.

Improper ferroelectrics are expected to be more robust than conventional ferroelectrics against depolarizing field effects and to exhibit a much-desired absence of critical thickness. Recent studies, however, revealed the loss of ferroelectric response in epitaxial improper ferroelectric thin films. Here, we investigate improper ferroelectric hexagonal YMnO 3 thin films and find that the polarization suppression, and hence functionality, in the thinner films is due to oxygen off-stoichiometry. We demonstrate that oxygen vacancies form on the film surfaces to provide the necessary charge to screen the large internal electric field resulting from the positively charged YMnO 3 surface layers. Additionally, we show that by modifying the oxygen concentration of the films, the phase transition temperatures can be substantially tuned. We anticipate that our findings are also valid for other ferroelectric oxide films and emphasize the importance of controlling the oxygen content and cation oxidation states in ferroelectrics for their successful integration in nanoscale applications.

The shape recovery ability of shape-memory alloys vanishes below a critical size (~50 nm), which prevents their practical applications at the nanoscale. In contrast, ferroic materials, even when scaled down to dimensions of a few nanometers, exhibit actuation strain through domain switching, though the generated strain is modest (~1%). Here, we develop freestanding twisted architectures of nanoscale ferroic oxides showing shape-memory effect with a giant recoverable strain (>8%). The twisted geometrical design amplifies the strain generated during ferroelectric domain switching, which cannot be achieved in bulk ceramics or substrate-bonded thin films. The twisted ferroic nanocomposites allow us to overcome the size limitations in traditional shape-memory alloys and open new avenues in engineering large-stroke shape-memory materials for small-scale actuating devices such as nanorobots and artificial muscle fibrils., (© 2023. The Author(s).)

The ability to sensitively image electric fields is important for understanding many nanoelectronic phenomena, including charge accumulation at surfaces 1 and interfaces 2 and field distributions in active electronic devices 3 . A particularly exciting application is the visualization of domain patterns in ferroelectric and nanoferroic materials 4,5 , owing to their potential in computing and data storage 6-8 . Here, we use a scanning nitrogen-vacancy (NV) microscope, well known for its use in magnetometry 9 , to image domain patterns in piezoelectric (Pb[Zr 0.2 Ti 0.8 ]O 3 ) and improper ferroelectric (YMnO 3 ) materials through their electric fields. Electric field detection is enabled by measuring the Stark shift of the NV spin 10,11 using a gradiometric detection scheme 12 . Analysis of the electric field maps allows us to discriminate between different types of surface charge distributions, as well as to reconstruct maps of the three-dimensional electric field vector and charge density. The ability to measure both stray electric and magnetic fields 9,13 under ambient conditions opens opportunities for the study of multiferroic and multifunctional materials and devices 8,14 ., Competing Interests: Competing interestsThe authors declare no competing interests., (© The Author(s) 2023.)

Magnetic skyrmions are compact chiral spin textures that exhibit a rich variety of topological phenomena and hold potential for the development of high-density memory devices and novel computing schemes driven by spin currents. Here, we demonstrate the room-temperature interfacial stabilization and current-driven control of skyrmion bubbles in the ferrimagnetic insulator Tm 3 Fe 5 O 12 coupled to Pt, showing the current-induced motion of individual skyrmion bubbles. The ferrimagnetic order of the crystal together with the interplay of spin-orbit torques and pinning determine the skyrmion dynamics in Tm 3 Fe 5 O 12 and result in a strong skyrmion Hall effect characterized by a negative deflection angle and hopping motion. Further, we show that the velocity and depinning threshold of the skyrmion bubbles can be modified by exchange coupling Tm 3 Fe 5 O 12 to an in-plane magnetized Y 3 Fe 5 O 12 layer, which distorts the spin texture of the skyrmions and leads to directional-dependent rectification of their dynamics. This effect, which is equivalent to a magnetic ratchet, is exploited to control the skyrmion flow in a racetrack-like device., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

Ferroic order is characterized by hystereses with two remanent states and therefore inherently binary. The increasing interest in materials showing non-discrete responses, however, calls for a paradigm shift towards continuously tunable remanent ferroic states. Device integration for oxide nanoelectronics furthermore requires this tunability at the nanoscale. Here we demonstrate that we can arbitrarily set the remanent ferroelectric polarization at nanometric dimensions. We accomplish this in ultrathin epitaxial PbZr 0.52 Ti 0.48 O 3 films featuring a dense pattern of decoupled nanometric 180° domains with a broad coercive-field distribution. This multilevel switching is achieved by driving the system towards the instability at the morphotropic phase boundary. The phase competition near this boundary in combination with epitaxial strain increases the responsiveness to external stimuli and unlocks new degrees of freedom to nano-control the polarization. We highlight the technological benefits of non-binary switching by demonstrating a quasi-continuous tunability of the non-linear optical response and of tunnel electroresistance., (© 2022. The Author(s).)

In order to bring the diverse functionalities of transition metal oxides into modern electronics, it is imperative to integrate oxide films with controllable properties onto the silicon platform. Here, we present asymmetric LaMnO 3 /BaTiO 3 /SrTiO 3 superlattices fabricated on silicon with layer thickness control at the unit-cell level. By harnessing the coherent strain between the constituent layers, we overcome the biaxial thermal tension from silicon and stabilize c-axis oriented BaTiO 3 layers with substantially enhanced tetragonality, as revealed by atomically resolved scanning transmission electron microscopy. Optical second harmonic generation measurements signify a predominant out-of-plane polarized state with strongly enhanced net polarization in the tricolor superlattices, as compared to the BaTiO 3 single film and conventional BaTiO 3 /SrTiO 3 superlattice grown on silicon. Meanwhile, this coherent strain in turn suppresses the magnetism of LaMnO 3 as the thickness of BaTiO 3 increases. Our study raises the prospect of designing artificial oxide superlattices on silicon with tailored functionalities., (© 2022. The Author(s).)