Flexoelectric Domain Walls Originated from Structural Phase Transition in Epitaxial BiVO4 Films.

Polar domain walls in centrosymmetric ferroelastics induce inhomogeneity that is the origin of advantageous multifunctionality. In particular, polar domain walls promote charge-carrier separation and hence are promising for energy conversion applications that overcome the hurdles of the rate-limiting step in the traditional photoelectrochemical water splitting processes. Yet, while macroscopic studies investigate the materials at the device scale, the origin of this phenomenon in general and the emergence of polar domain walls during the structural phase transition in particular has remained elusive, encumbering the development of this attractive system. Here, it is demonstrated that twin domain walls arise in centrosymmetric BiVO4 films and they exhibit localized piezoelectricity. It is also shown that during the structural phase transition from the tetragonal to monoclinic, the symmetry reduction is accompanied by an emergence of strain gradient, giving rise to flexoelectric effect and the polar domain walls. These results not only expose the emergence of polar domain walls at centrosymmetric systems by means of direct observation, but they also expand the realm of potential application of ferroelastics, especially in photoelectrochemistry and local piezoelectricity.

Superconductor-superconductor bilayers for enhancing single-photon detection.

Here, we optimized ultrathin films of granular NbN on SiO2 and of amorphous αW5Si3. We showed that hybrid superconducting nanowire single-photon detectors (SNSPDs) made of 2 nm thick αW5Si3 films over 2 nm thick NbN films exhibit advantageous coexistence of timing (<5 ns reset time and 52 ps timing jitter) and efficiency (>96% quantum efficiency) performance. We discuss the governing mechanism of this hybridization via the proximity effect. Our results demonstrate saturated SNSPDs performance at 1550 nm optical wavelength and suggest that such hybridization can significantly expand the range of available superconducting properties, impacting other nano-superconducting technologies. Lastly, this hybridization may be used to tune properties, such as the amorphous character of superconducting films.

Eight-fold signal amplification of a superconducting nanowire single-photon detector using a multiple-avalanche architecture.

Superconducting nanowire avalanche single-photon detectors (SNAPs) with n parallel nanowires are advantageous over single-nanowire detectors because their output signal amplitude scales linearly with n. However, the SNAP architecture has not been viably demonstrated for n > 4. To increase n for larger signal amplification, we designed a multi-stage, successive-avalanche architecture which used nanowires, connected via choke inductors in a binary-tree layout. We demonstrated an avalanche detector with n = 8 parallel nanowires and achieved eight-fold signal amplification, with a timing jitter of 54 ps.

Chain-Like Semiconductive Fillers for Dielectric Enhancement and Loss Reduction of Polymer Composites.

Dielectric loss is a crucial factor in determining the long-term endurance for security and energy loss of dielectric composites. Here, chain-like semiconductive fibers of titanium oxide, indium, and niobium-doped titanium oxide are used for enhancing the complex dielectric properties of a polymer through composite construction, which involves significant interface enhancements. The chain-like fibers significantly enhance the dielectric constant owing to the special morphology of the fillers and their interfacial polarization, especially at higher temperatures. The dielectric loss and electrical conductivity of the composites are substantially reduced across the entire investigated temperature range, achieved by passivating the fiber surface with an alumina shell using atomic layer deposition. The as-deposited alumina shell transformed from an amorphous to a crystalline phase through thermal annealing results in a porous shell and more effective suppression of the loss tangent and electrical conductivity. A plausible mechanism for loss suppression is associated with carrier movement along the surface of the fibers and bulk, leading to a higher loss tangent. The alumina shell blocks the carrier transport path, particularly at the interfaces, resulting in a reduced interfacial polarization contribution and energy storage loss. This study provides a method for inhibiting dielectric loss by fabricating fillers with special surfaces.

Ultralow-power in-memory computing based on ferroelectric memcapacitor network.

Analog storage through synaptic weights using conductance in resistive neuromorphic systems and devices inevitably generates harmful heat dissipation. This thermal issue not only limits the energy efficiency but also hampers the very-large-scale and highly complicated hardware integration as in the human brain. Here we demonstrate that the synaptic weights can be simulated by reconfigurable non-volatile capacitances of a ferroelectric-based memcapacitor with ultralow-power consumption. The as-designed metal/ferroelectric/metal/insulator/semiconductor memcapacitor shows distinct 3-bit capacitance states controlled by the ferroelectric domain dynamics. These robust memcapacitive states exhibit uniform maintenance of more than 104 s and well endurance of 109 cycles. In a wired memcapacitor crossbar network hardware, analog vector-matrix multiplication is successfully implemented to classify 9-pixel images by collecting the sum of displacement currents (I = C × dV/dt) in each column, which intrinsically consumes zero energy in memcapacitors themselves. Our work sheds light on an ultralow-power neural hardware based on ferroelectric memcapacitors.

Unexpected controllable pair-structure in ferroelectric nanodomains.

The imminent inability of silicon-based memory devices to satisfy Moore's Law is approaching rapidly. Controllable nanodomains of ferroic systems are anticipated to enable future high-density nonvolatile memory and novel electronic devices. We find via piezoresponse force microscopy (PFM) studies on lead zirconate titanate (PZT) films an unexpected nanostructuring of ferroelectric-ferroelastic domains. These consist of c-nanodomains within a-nanodomains in proximity to a-nanodomains within c-domains. These structures are created and annihilated as pairs, controllably. We treat these as a new kind of vertex-antivertex pair and consider them in terms of the Srolovitz-Scott 4-state Potts model, which results in pairwise domain vertex instabilities that resemble the vortex-antivortex mechanism in ferromagnetism, as well as dislocation pairs (or disclination pairs) that are well-known in nematic liquid crystals. Finally, we show that these nanopairs can be scaled up to form arrays that are engineered at will, paving the way toward facilitating them to real technologies.

Engineering Individual Oxygen Vacancies: Domain-Wall Conductivity and Controllable Topological Solitons.

Nanoscale devices that utilize oxygen vacancies in two-dimensional metal-oxide structures garner much attention due to conductive, magnetic, and even superconductive functionalities they exhibit. Ferroelectric domain walls have been a prominent recent example because they serve as a hub for topological defects and hence are attractive for next-generation data technologies. However, owing to the light weight of oxygen atoms and localized effects of their vacancies, the atomic-scale electrical and mechanical influence of individual oxygen vacancies has remained elusive. Here, stable individual oxygen vacancies were engineered in situ at domain walls of seminal titanate perovskite ferroics. The atomic-scale electric-field, charge, dipole-moment, and strain distribution around these vacancies were characterized by combining advanced transmission electron microscopy and first-principle methodologies. The engineered vacancies were used to form quasi-linear quadrupole topological defects. Significant intraband states were found in the unit cell of the engineered vacancies, proposing a meaningful domain-wall conductivity for miniaturized data-storage applications. Reduction of the Ti ion as well as enhanced charging and electric-field concentration were demonstrated near the vacancy. A 3-5% tensile strain was observed at the immediate surrounding unit cells of the vacancies. Engineering individual oxygen vacancies and topological solitons thus offers a platform for predetermining both atomic-scale and global functional properties of device miniaturization in metal oxides.

Bundles of polytwins as meta-elastic domains in the thin polycrystalline simple multi-ferroic system PZT.

We used enhanced piezo-response force microscopy (E-PFM) to investigate both ferroelastic and ferroelectric nanodomains in thin films of the simple multi-ferroic system PbZr(0.3)Ti(0.7)O(3) (PZT). We show how the grains are organized into a new type of elastic domain bundles of the well-known periodic elastic twins. Here we present these bundle domains and discuss their stability and origin. Moreover, we show that they can arrange in such a way as to release strain in a more effective way than simple twinning. Finally, we show that these bundle domains can arrange to form the macroscopic ferroelectric domains that constitute the basis of ferroelectric-based memory devices.

Formation and manipulation of domain walls with 2 nm domain periodicity in BaTiO3 without contact electrodes.

Interfaces at the two-dimensional limit in oxide materials exhibit a wide span of functionality that differs significantly from the bulk behavior. Among such interfaces, domain walls in ferroelectrics draw special attention because they can be moved deterministically with external voltage, while they remain at place after voltage removal, paving the way to novel neuromorphic and low-power data-processing technologies. Ferroic domains arise to release strain, which depends on material thickness, following Kittel's scaling law. Hence, a major hurdle is to reduce the device footprint for a given thickness, i.e., to form and move high-density domain walls. Here, we used transmission electron microscopy to produce domain walls with periodicity as high as 2 nm without the use of contact electrodes, while observing their formation and dynamics in situ in BaTiO3. Large-area coverage of the engineered domain walls was demonstrated. The domain-wall density was found to increase with increasing effective stress, until arriving at a saturation value that reflects 150-fold effective stress enhancement. Exceeding this value resulted in strain release by domain rotation. In addition to revealing this multiscale strain-releasing mechanism, we offer a device design that allows controllable switching of domain-walls with 2 nm periodicity, reflecting a potential 144 Tb per inch2 neuromorphic network.

Giant Superelastic Piezoelectricity in Flexible Ferroelectric BaTiO3 Membranes.

Mechanical displacement in commonly used piezoelectric materials is typically restricted to linear or biaxial in nature and to a few percent of the material dimensions. Here, we show that free-standing BaTiO3 membranes exhibit nonconventional electromechanical coupling. Under an external electric field, these superelastic membranes undergo controllable and reversible "sushi-rolling-like" 180° folding-unfolding cycles. This crease-free folding is mediated by charged ferroelectric domains, leading to giant >3.8 and 4.6 µm displacements for a 30 nm thick membrane at room temperature and 60 °C, respectively. Further increasing the electric field above the coercive value changes the fold curvature, hence augmenting the effective piezoresponse. Finally, it is found that the membranes fold with increasing temperature followed by complete immobility of the membrane above the Curie temperature, allowing us to model the ferroelectric domain origin of the effect.