Field-Free Spin-Orbit Torque Magnetization Switching in a Single-Phase Ferromagnetic and Spin Hall Oxide.

Current-induced spin-orbit torque (SOT) offers substantial promise for the development of low-power, nonvolatile magnetic memory. Recently, a single-phase material concurrently exhibiting magnetism and the spin Hall effect has emerged as a scientifically and technologically interesting platform for realizing efficient and compact SOT systems. Here, we demonstrate external-magnetic-field-free switching of perpendicular magnetization in a single-phase ferromagnetic and spin Hall oxide SrRuO3. We delicately altered the local lattices of the top and bottom surface layers of SrRuO3, while retaining a quasi-homogeneous, single-crystalline nature of the SrRuO3 bulk. This leads to unbalanced spin Hall effects between the top and bottom layers, enabling net SOT performance within single-layer ferromagnetic SrRuO3. Notably, our SrRuO3 exhibits the highest SOT efficiency and lowest power consumption among all known single-layer systems under field-free conditions. Our method of artificially manipulating the local atomic structures will pave the way for advances in spin-orbitronics and the exploration of new SOT materials.

Flexoelectricity-Driven Mechanical Switching of Polarization in Metastable Ferroelectrics.

Flexoelectricity-based mechanical switching of ferroelectric polarization has recently emerged as a fascinating alternative to conventional polarization switching using electric fields. Here, we demonstrate hyperefficient mechanical switching of polarization exploiting metastable ferroelectricity that inherently holds a unique mechanical response. We theoretically predict that mechanical forces markedly reduce the coercivity of metastable ferroelectricity, thus greatly bolstering flexoelectricity-driven mechanical polarization switching. As predicted, we experimentally confirm the mechanical polarization switching via an unusually low mechanical force (100 nN) in metastable ferroelectric CaTiO_{3}. Furthermore, the use of low mechanical forces narrows the width of mechanically writable nanodomains to sub-10 nm, suggesting an ultrahigh data storage density of ≥1 Tbit cm^{-2}. This Letter sheds light on the mechanical switching of ferroelectric polarization as a viable key element for next-generation efficient nanoelectronics and nanoelectromechanics.

Ferroelectrically tunable magnetic skyrmions in ultrathin oxide heterostructures.

Magnetic skyrmions are topologically protected whirling spin texture. Their nanoscale dimensions, topologically protected stability and solitonic nature, together are promising for future spintronics applications. To translate these compelling features into practical spintronic devices, a key challenge lies in achieving effective control of skyrmion properties, such as size, density and thermodynamic stability. Here, we report the discovery of ferroelectrically tunable skyrmions in ultrathin BaTiO3/SrRuO3 bilayer heterostructures. The ferroelectric proximity effect at the BaTiO3/SrRuO3 heterointerface triggers a sizeable Dzyaloshinskii-Moriya interaction, thus stabilizing robust skyrmions with diameters less than a hundred nanometres. Moreover, by manipulating the ferroelectric polarization of the BaTiO3 layer, we achieve local, switchable and nonvolatile control of both skyrmion density and thermodynamic stability. This ferroelectrically tunable skyrmion system can simultaneously enhance the integratability and addressability of skyrmion-based functional devices.

Tunneling Hot Spots in Ferroelectric SrTiO3.

Strontium titanate (SrTiO3) is the "silicon" in the emerging field of oxide electronics. While bulk properties of this material have been studied for decades, new unexpected phenomena have recently been discovered at the nanoscale, when SrTiO3 forms an ultrathin film or an atomically sharp interface with other materials. One of the striking discoveries is room-temperature ferroelectricity in strain-free ultrathin films of SrTiO3 driven by the TiSr antisite defects, which generate a local dipole moment polarizing the surrounding nanoregion. Here, we demonstrate that these polar defects are not only responsible for ferroelectricity, but also propel the appearance of highly conductive channels, "hot spots", in the ultrathin SrTiO3 films. Using a combination of scanning probe microscopy experimental studies and theoretical modeling, we show that the hot spots emerge due to resonant tunneling through localized electronic states created by the polar defects and that the tunneling conductance of the hot spots is controlled by ferroelectric polarization. Our finding of the polarization-controlled defect-assisted tunneling reveals a new mechanism of resistive switching in oxide heterostructures and may have technological implications for ferroelectric tunnel junctions. It is also shown that the conductivity of the hot spots can be modulated by mechanical stress, opening a possibility for development of conceptually new electronic devices with mechanically tunable resistive states.

Electron-Lattice Coupling in Correlated Materials of Low Electron Occupancy.

In correlated materials including transition metal oxides, electronic properties and functionalities are modulated and enriched by couplings between the electron and lattice degrees of freedom. These couplings are controlled by external parameters such as chemical doping, pressure, magnetic and electric fields, and light irradiation. However, the electron-lattice coupling relies on orbital characters, i.e., symmetry and occupancy, of t2g and eg orbitals, so that a large electron-lattice coupling is limited to eg electron system, whereas t2g electron system exhibits an inherently weak coupling. Here, we design and demonstrate a strongly enhanced electron-lattice coupling in electron-doped SrTiO3, that is, the t2g electron system. In ultrathin films of electron-doped SrTiO3 [i.e., (La0.25Sr0.75)TiO3], we reveal the strong electron-lattice-orbital coupling, which is manifested by extremely increased tetragonality and the corresponding metal-to-insulator transition. Our findings open the way of an active tuning of the charge-lattice-orbital coupling to obtain new functionalities relevant to emerging nanoelectronic devices.

Sharpened VO2 Phase Transition via Controlled Release of Epitaxial Strain.

Phase transitions in correlated materials can be manipulated at the nanoscale to yield emergent functional properties, promising new paradigms for nanoelectronics and nanophotonics. Vanadium dioxide (VO2), an archetypal correlated material, exhibits a metal-insulator transition (MIT) above room temperature. At the thicknesses required for heterostructure applications, such as an optical modulator discussed here, the strain state of VO2 largely determines the MIT dynamics critical to the device performance. We develop an approach to control the MIT dynamics in epitaxial VO2 films by employing an intermediate template layer with large lattice mismatch to relieve the interfacial lattice constraints, contrary to conventional thin film epitaxy that favors lattice match between the substrate and the growing film. A combination of phase-field simulation, in situ real-time nanoscale imaging, and electrical measurements reveals robust undisturbed MIT dynamics even at preexisting structural domain boundaries and significantly sharpened MIT in the templated VO2 films. Utilizing the sharp MIT, we demonstrate a fast, electrically switchable optical waveguide. This study offers unconventional design principles for heteroepitaxial correlated materials, as well as novel insight into their nanoscale phase transitions.

Flexoelectric rectification of charge transport in strain-graded dielectrics.

Flexoelectricity is emerging as a fascinating means for exploring the physical properties of nanoscale materials. Here, we demonstrated the unusual coupling between electronic transport and the mechanical strain gradient in a dielectric epitaxial thin film. Utilizing the nanoscale strain gradient, we showed the unique functionality of flexoelectricity to generate a rectifying diode effect. Furthermore, using conductive atomic force microscopy, we found that the flexoelectric effect can govern the local transport characteristics, including spatial conduction inhomogeneities, in thin-film epitaxy systems. Consideration of the flexoelectric effect will improve understanding of the charge conduction mechanism at the nanoscale and may facilitate the advancement of novel nanoelectronic device design.

Mixed Triboelectric and Flexoelectric Charge Transfer at the Nanoscale.

The triboelectric effect is a ubiquitous phenomenon in which the surfaces of two materials are easily charged during the contact-separation process. Despite the widespread consequences and applications, the charging mechanisms are not sufficiently understood. Here, the authors report that, in the presence of a strain gradient, the charge transfer is a result of competition between flexoelectricity and triboelectricity, which could enhance charge transfer during triboelectric measurements when the charge transfers of both effects are in the same direction. When they are in the opposite directions, the direction and amount of charge transfer could be modulated by the competition between flexoelectric and triboelectric effects, which leads to a distinctive phenomenon, that is, the charge transfer is reversed with varying forces. The subsequent results on the electrical power output signals from the triboelectrification support the proposed mechanism. Therefore, the present study emphasizes the key role of the flexoelectric effect through experimental approaches, and suggests that both the amount and direction of charge transfer can be modulated by manipulating the mixed triboelectric and flexoelectric effects. This finding may provide important information on the triboelectric effect and can be further extended to serve as a guideline for material selection during a nanopatterned device design.

Stabilizing hidden room-temperature ferroelectricity via a metastable atomic distortion pattern.

Nonequilibrium atomic structures can host exotic and technologically relevant properties in otherwise conventional materials. Oxygen octahedral rotation forms a fundamental atomic distortion in perovskite oxides, but only a few patterns are predominantly present at equilibrium. This has restricted the range of possible properties and functions of perovskite oxides, necessitating the utilization of nonequilibrium patterns of octahedral rotation. Here, we report that a designed metastable pattern of octahedral rotation leads to robust room-temperature ferroelectricity in CaTiO3, which is otherwise nonpolar down to 0 K. Guided by density-functional theory, we selectively stabilize the metastable pattern, distinct from the equilibrium pattern and cooperative with ferroelectricity, in heteroepitaxial films of CaTiO3. Atomic-scale imaging combined with deep neural network analysis confirms a close correlation between the metastable pattern and ferroelectricity. This work reveals a hidden but functional pattern of oxygen octahedral rotation and opens avenues for designing multifunctional materials.

Colossal flexoresistance in dielectrics.

Dielectrics have long been considered as unsuitable for pure electrical switches; under weak electric fields, they show extremely low conductivity, whereas under strong fields, they suffer from irreversible damage. Here, we show that flexoelectricity enables damage-free exposure of dielectrics to strong electric fields, leading to reversible switching between electrical states-insulating and conducting. Applying strain gradients with an atomic force microscope tip polarizes an ultrathin film of an archetypal dielectric SrTiO3 via flexoelectricity, which in turn generates non-destructive, strong electrostatic fields. When the applied strain gradient exceeds a certain value, SrTiO3 suddenly becomes highly conductive, yielding at least around a 108-fold decrease in room-temperature resistivity. We explain this phenomenon, which we call the colossal flexoresistance, based on the abrupt increase in the tunneling conductance of ultrathin SrTiO3 under strain gradients. Our work extends the scope of electrical control in solids, and inspires further exploration of dielectric responses to strong electromechanical fields.

Enhanced flexoelectricity at reduced dimensions revealed by mechanically tunable quantum tunnelling.

Flexoelectricity is a universal electromechanical coupling effect whereby all dielectric materials polarise in response to strain gradients. In particular, nanoscale flexoelectricity promises exotic phenomena and functions, but reliable characterisation methods are required to unlock its potential. Here, we report anomalous mechanical control of quantum tunnelling that allows for characterising nanoscale flexoelectricity. By applying strain gradients with an atomic force microscope tip, we systematically polarise an ultrathin film of otherwise nonpolar SrTiO3, and simultaneously measure tunnel current across it. The measured tunnel current exhibits critical behaviour as a function of strain gradients, which manifests large modification of tunnel barrier profiles via flexoelectricity. Further analysis of this critical behaviour reveals significantly enhanced flexocoupling strength in ultrathin SrTiO3, compared to that in bulk, rendering flexoelectricity more potent at the nanoscale. Our study not only suggests possible applications exploiting dynamic mechanical control of quantum effect, but also paves the way to characterise nanoscale flexoelectricity.

Oxygen Partial Pressure during Pulsed Laser Deposition: Deterministic Role on Thermodynamic Stability of Atomic Termination Sequence at SrRuO3/BaTiO3 Interface.

With recent trends on miniaturizing oxide-based devices, the need for atomic-scale control of surface/interface structures by pulsed laser deposition (PLD) has increased. In particular, realizing uniform atomic termination at the surface/interface is highly desirable. However, a lack of understanding on the surface formation mechanism in PLD has limited a deliberate control of surface/interface atomic stacking sequences. Here, taking the prototypical SrRuO3/BaTiO3/SrRuO3 (SRO/BTO/SRO) heterostructure as a model system, we investigated the formation of different interfacial termination sequences (BaO-RuO2 or TiO2-SrO) with oxygen partial pressure (PO2) during PLD. We found that a uniform SrO-TiO2 termination sequence at the SRO/BTO interface can be achieved by lowering the PO2 to 5 mTorr, regardless of the total background gas pressure (Ptotal), growth mode, or growth rate. Our results indicate that the thermodynamic stability of the BTO surface at the low-energy kinetics stage of PLD can play an important role in surface/interface termination formation. This work paves the way for realizing termination engineering in functional oxide heterostructures.

Flexoelectric control of defect formation in ferroelectric epitaxial thin films.

Flexoelectric control of defect formation and associated electronic function is demonstrated in ferroelectric BiFeO3 thin films. An intriguing, so far never demonstrated, effect of internal electric field (Eint ) on defect formation is explored by a means of flexoelectricity. Our study provides novel insight into defect engineering, as well as allows a pathway to design defect configuration and associated electronic function.

Flexoelectric effect in the reversal of self-polarization and associated changes in the electronic functional properties of BiFeO(3) thin films.

Flexoelectricity can play an important role in the reversal of the self-polarization direction in epitaxial BiFeO3 thin films. The flexoelectric and interfacial effects compete with each other to determine the self-polarization state. In Region I, the self-polarization is downward because the interfacial effect is more dominant than the flexoelectric effect. In Region II, the self-polarization is upward, because the flexoelectric effect becomes more dominant than the interfacial effect.

Giant flexoelectric effect through interfacial strain relaxation.

Interfacial strain gradients in oxide epitaxial thin films provide an interesting opportunity to study flexoelectric effects and their potential applications. Oxide epitaxial thin films can exhibit giant and tunable flexoelectric effects, which are six or seven orders of magnitude larger than those in conventional bulk solids. The strain gradient in an oxide epitaxial thin film can generate an electric field above 1 MV m(-1) by flexoelectricity, large enough to affect the physical properties of the film. Giant flexoelectric effects on ferroelectric properties are discussed in this overview of recent experimental observations.

Multilevel data storage memory using deterministic polarization control.

Multilevel non-volatile memory for high-density date storage is achieved by using the deterministic control of ferroelectric polarization. In a real ferroelectric thin-film system, eight stable and reproducible polarization states are realized (i.e., 3-bit data storage) by adjusting the displacement current. This approach can be used to triple or quadruple the memory density, even at existing feature scales.

Active control of ferroelectric switching using defect-dipole engineering.

Active control of defect structures and associated polarization switching in a ferroelectric material is achieved without compromising its ferroelectric properties. Based on dipolar interaction between defect dipole and polarization, the unique functionality of the defect dipole to control ferroelectric switching is visualized. This approach can provide a foundation for novel ferroelectric applications, such as high-density multilevel data storage.