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Abstract Due to its non‐invasive nature, ultrasound has been widely used for neuromodulation in biological systems, where its application influences the synaptic weights and the process of neurotransmitter delivery. However, such modulation has not been emulated in physical devices. Memristors are ideal electrical components for artificial synapses, but up till now they are hardly reported to respond to ultrasound signals. Here we design and fabricate a HfOx‐based memristor on 64°Y‐X LiNbO3 single crystal substrate, and successfully realize artificial synapses modulation by shear‐horizontal surface acoustic wave (SH‐SAW). It is a prominent short‐term resistance modulation, where ultrasound has been shown to cause resistance drop for various resistance states, which could fully recover after the ultrasound is shut off. The physical mechanism illustrates that ultrasound induced polarization potential in the HfOx dielectric layer acts on the Schottky barrier, leading to the resistance drop. The emulation of neuron firing frequency modulation through ultrasound signals is demonstrated. Moreover, the joint application of ultrasound and electric voltage yields fruitful functionalities, such as the enhancement of resistance window and synaptic plasticity through ultrasound application. All these promising results provide a new strategy for artificial synapses modulation, and also further advance neuromorphic devices toward system applications.

Abstract The scale-free ferroelectric polarization of fluorite MO2 (M = Hf, Zr) due to flat polar phonon bands are promising for nonvolatile memories. Defects are also widely introduced to improve the emergent ferroelectricity. However, their roles are still not fully understood at the atomic-level. Here, we report a significant effect of point-defect-driven flattening of polar phonon bands with more polar modes and polarization contribution in doped MO2. The polar phonon bands in La-doped MO2 (M = Hf, Zr) can be significantly flattened, compared with pure ones. However, the lower energy barrier with larger polarization of V O -only doped MO2 compared with La-doped cases suggest that V O and local lattice distortion should be balanced for high-performance fluorite ferroelectricity. The work is believed to bridge the relation between point defects and the generally enhanced induced ferroelectricity in fluorite ferroelectrics at the atomic-level and inspire their further property optimization via defect-engineering.

Abstract Lead halide perovskites have recently emerged as promising X/γ-ray scintillators. However, the small Stokes shift of exciton luminescence in perovskite scintillators creates problems for the light extraction efficiency and severely impedes their applications in hard X/γ-ray detection. Dopants have been used to shift the emission wavelength, but the radioluminescence lifetime has also been unwantedly extended. Herein, we demonstrate the intrinsic strain in 2D perovskite crystals as a general phenomenon, which could be utilized as self-wavelength shifting to reduce the self-absorption effect without sacrificing the radiation response speed. Furthermore, we successfully demonstrated the first imaging reconstruction by perovskites for application of positron emission tomography. The coincidence time resolution for the optimized perovskite single crystals (4 × 4 × 0.8 mm3) reached 119 ± 3 ps. This work provides a new paradigm for suppressing the self-absorption effect in scintillators and may facilitate the application of perovskite scintillators in practical hard X/γ-ray detections.

Abstract Two‐dimensional material‐based field‐effect transistors (2DM‐FETs) are playing a revolutionary role in electronic devices. However, before electronic design automation (EDA) for 2DM‐FETs can be achieved, it remains necessary to determine how to incorporate contact transports into model. Reported methods compromise between physical intelligibility and model compactness due to the heterojunction nature. To address this, quasi‐Fermi‐level phase space theory (QFLPS) is generalized to incorporate contact transports using the Landauer formula. It turns out that the Landauer‐QFLPS model effectively overcomes the issue of concern. The proposed new formula can describe 2DM‐FETs with Schottky or Ohmic contacts with superior accuracy and efficiency over previous methods, especially when describing non‐monotonic drain conductance characteristics. A three‐bit threshold inverter quantizer (TIQ) circuit is fabricated using ambipolar black phosphorus and it is demonstrated that the model accurately predicts circuit performance. The model could be very effective and valuable in the development of 2DM‐FET‐based integrated circuits.

Abstract The exchange bias (EB) effect plays an undisputed role in the development of highly sensitive, robust, and high-density spintronic devices in magnetic data storage. However, the weak EB field, low blocking temperature, as well as the lack of modulation methods, seriously limit the application of EB in van der Waals (vdW) spintronic devices. Here, we utilized pressure engineering to tune the vdW spacing of the two-dimensional (2D) FePSe3/Fe3GeTe2 heterostructures. The EB field (H EB, from 29.2 mT to 111.2 mT) and blocking temperature (T b, from 20 K to 110 K) are significantly enhanced, and a highly sensitive and robust spin valve is demonstrated. Interestingly, this enhancement of the EB effect was extended to exposed Fe3GeTe2, due to the single-domain nature of Fe3GeTe2. Our findings provide opportunities for the producing, exploring, and tuning of magnetic vdW heterostructures with strong interlayer coupling, thereby enabling customized 2D spintronic devices in the future.

Abstract The Jahn-Teller (JT) effect involves the ions M with a degenerate electronic state distorting the corner-sharing MO6 octahedra to lift the degeneracy, inducing strong coupling of electrons to lattice, and mediating the exotic properties in perovskite oxides. Conversely, the anti-Jahn–Teller (AJT) effect refers to the deformation against the Jahn-Teller-distorted MO6 octahedra. However, it is difficult to experimentally execute both effects descending from the fine-tuning of crystal structures. We propose the AJT can be introduced by THz laser illumination at 11.71 THz in a candidate superconducting perovskite material BaBiO3 near room temperature. The illumination coherently drives the infrared-active phonon that excites the Raman breathing mode through the quadratic-linear nonlinear interaction. The process is characterized by the emergence of an AJT effect, accompanied by an insulator-to-metal transition occurring on the picosecond timescale. This study underlines the important role of crystal structure engineering by coherent phonon excitation in designing optoelectronic devices.

Abstract Increasing both clean water and green energy demands for survival and development are the grand challenges of our age. Here, we successfully fabricate a novel multifunctional 3D graphene-based catalytic membrane (3D-GCM) with active metal nanoparticles (AMNs) loading for simultaneously obtaining the water purification and clean energy generation, via a “green” one-step laser scribing technology. The as-prepared 3D-GCM shows high porosity and uniform distribution with AMNs, which exhibits high permeated fluxes (over 100 L m−2 h−1) and versatile super-adsorption capacities for the removal of tricky organic pollutants from wastewater under ultra-low pressure-driving (0.1 bar). After adsorption saturating, the AMNs in 3D-GCM actuates the advanced oxidization process to self-clean the fouled membrane via the catalysis, and restores the adsorption capacity well for the next time membrane separation. Most importantly, the 3D-GCM with the welding of laser scribing overcomes the lateral shear force damaging during the long-term separation. Moreover, the 3D-GCM could emit plentiful of hot electrons from AMNs under light irradiation, realizing the membrane catalytic hydrolysis reactions for hydrogen energy generation. This “green” precision manufacturing with laser scribing technology provides a feasible technology to fabricate high-efficient and robust 3D-GCM microreactor in the tricky wastewater purification and sustainable clean energy production as well.

HfO2-based ferroelectric films are attracting a great deal of attention. Here, the authors conclude that the performance degradation and the possible rejuvenation are ascribed to the reversible transition between polar and antipolar phases.

Abstract The wake‐up phenomenon widely exists in hafnia‐based ferroelectric capacitors, which causes device parameter variation over time. Crystallization at a higher temperature has been reported to be effective in eliminating wake‐up, but high temperature may yield the monoclinic phase or generate more oxygen vacancies. In this work, a unidirectional annealing method is proposed for the crystallization of Hf0.5Zr0.5O2 (HZO) superlattice ferroelectrics, which involves heating from the Pt/ZrO2 interface side. It is demonstrated that 600 °C annealing only leads to a moderate content of monoclinic phase in HZO, and the TiN/HZO/Pt capacitor exhibits wake‐up free nature and a switchable remnant polarization value of 27.4 µC cm−2. On the other hand, heating from the TiN/HfO2 side, or using 500 °C annealing temperature, could yield ferroelectric devices that require a wake‐up process. The special configuration of Pt/ZrO2 is verified by comparative studies with several other superlattice structures and HZO solid‐state solutions. It is discovered that heating from the Pt/HfO2 side at 600 °C leads to high leakage current and a memristor behavior. The mechanisms of ferroelectric phase stabilization and memristor formation have been discussed. The unidirectional heating method can also be useful for other hafnia‐based ferroelectric devices.

Understanding the mechanism of the formation and rupture of conductive filaments in HfO2-based memristors is essential to solve the problem of scalability of the devices. Here, Zhang et al. visualize this process by tracking atomic-scale evolution of conductive filaments during resistive switching cycles.

Lead halide perovskites are widely used e.g. in solar cells and LEDs, but devices based on thermal properties have received little attention. Here, the authors take advantage of the thermal properties to fabricate an optoacoustic transducer with both broad bandwidth and high conversion efficiency.

Abstract The adjustable conductance of a two‐terminal memristor in a crossbar array can facilitate vector‐matrix multiplication in one step, making the memristor a promising synapse for efficiently implementing neuromorphic computing. To achieve controllable and gradual switching of multi‐level conductance, important for neuromorphic computing, a theoretical design of a superlattice‐like (SLL) structure switching layer for the multi‐level memristor is proposed and validated, refining the growth of conductive filaments (CFs) and preventing CFs from the abrupt formation and rupture. Ti/(HfOx/AlOy)SLL/TiN memristors are shown with transmission electron microscopy , X‐ray photoelectron spectroscopy , and ab initio calculation findings corroborate the SLL structure of HfOx/AlOy film. The optimized SLL memristor achieves outstanding conductance modulation performance with linearly synaptic weight update (nonlinear factor α = 1.06), and the convolutional neural network based on the SLL memristive synapse improves the handwritten digit recognition accuracy to 94.95%. Meanwhile, this improved synaptic device has a fast operating speed (30 ns), a long data retention time (≥ 104 s at 85 ℃), scalability, and CMOS process compatibility. Finally, its physical nature is explored and the CF evolution process is characterized using nudged elastic band calculations and the conduction mechanism fitting. In this work, as an example the HfOx/AlOy SLL memristor provides a design viewpoint and optimization strategy for neuromorphic computing.

In recent years, hafnia-based ferroelectrics have attracted enormous attention due to their capability of maintaining ferroelectricity below 10 nm thickness and excellent compatibility with microelectronics flow lines. However, the physical origin of their ferroelectricity is still not fully clear, although it is commonly attributed to a polar Pca 2 _1 orthorhombic phase. The high-temperature paraelectric phases (the tetragonal phase or the cubic phase) do not possess a soft mode at the Brillouin zone center, thus the ferroelectric distortion has to be explained in terms of trilinear coupling among three phonon modes in the tetragonal phase. It is necessary to explore new materials with possible ferroelectricity due to the polar Pca 2 _1 phase, which in turn should be very helpful in evaluating the microscopic theory for ferroelectric hafnia. In this work, based on the idea of the Materials Genome Engineering, a series of hafnia-like ferroelectrics have been found, exemplified by LaSeCl, LaSeBr, LuOF and YOF, which possess adequate spontaneous polarization values and also relatively favorable free energies for the polar phase. Their common features and individual differences are discussed in detail. In particular, a promising potential ferroelectric material, Pca 2 _1 phase LuOF, is predicted and recommended for further experimental synthesis and investigation.

Abstract The growing demand for scalable solar‐blind image sensors with remarkable photosensitive properties has stimulated the research on more advanced solar‐blind photodetector (SBPD) arrays. In this work, the authors demonstrate ultrahigh‐performance metal‐semiconductor‐metal (MSM) SBPDs based on amorphous (a‐) Ga2O3 via a post‐annealing process. The post‐annealed MSM a‐Ga2O3 SBPDs exhibit superhigh sensitivity of 733 A/W and high response speed of 18 ms, giving a high gain‐bandwidth product over 104 at 5 V. The SBPDs also show ultrahigh photo‐to‐dark current ratio of 3.9 × 107. Additionally, the PDs demonstrate super‐high specific detectivity of 3.9 × 1016 Jones owing to the extremely low noise down to 3.5 fW Hz−1/2, suggesting high signal‐to‐noise ratio. Underlying mechanism for such superior photoelectric properties is revealed by Kelvin probe force microscopy and first principles calculation. Furthermore, for the first time, a large‐scale, high‐uniformity 32 × 32 image sensor array based on the post‐annealed a‐Ga2O3 SBPDs is fabricated. Clear image of target object with high contrast can be obtained thanks to the high sensitivity and uniformity of the array. These results demonstrate the feasibility and practicality of the Ga2O3 PDs for applications in solar‐blind imaging, environmental monitoring, artificial intelligence and machine vision.

Abstract Memristive logic device is a promising unit for beyond von Neumann computing systems and 2D materials are widely used because of their controllable interfacial properties. Most of these 2D memristive devices, however, are made from semiconducting chalcogenides which fail to gate the off‐state current. To this end, a crossbar device using 2D HfSe2 is fabricated, and then the top layers are oxidized into “high‐k” dielectric HfSexOy via oxygen plasma treatment, so that the cell resistance can be remarkably increased. This two‐terminal Ti/HfSexOy/HfSe2/Au device exhibits excellent forming‐free resistive switching performance with high switching speed (

Ionic migration degrades not only the characteristics of halide perovskite solar cells, but also those of perovskite X-ray detectors. Here Yang et al. employ heteroepitaxial BiOBr to passivate Cs2AgBiBr6 double perovskite, which suppresses ionic migration and obtain high performance X-ray detectors.

The exact composition and structure of conductive filaments in hafnia-based memristors are still not fully understood, but recent theoretical investigations reveal that hexagonal HfOx phases close to the h.c.p. Hf structure are probable filament candidates. In this work we list h.c.p. Hf, Hf6O, Hf3O and Hf2O as possible phases for the filament in hafnia memristors. Their differences in lattice parameters, electronic structures and O charge states are studied in details. Migration of O ions for both in-plane and out-of-plane directions in these phases is investigated using first-principles calculations. Both single-phase supercells and filament-in-dielectric models are used for migration barrier calculations, while the latter is proven to be more accurate for the c-direction. The migration of O ions is fastest in metal Hf, while slowest in Hf2O. The existence of O interstitials in Hf tends to hinder the transport of O.