Memristive switching in the surface of a charge-density-wave topological semimetal.

Owing to the outstanding properties provided by nontrivial band topology, topological phases of matter are considered as a promising platform towards low-dissipation electronics, efficient spin-charge conversion, and topological quantum computation. Achieving ferroelectricity in topological materials enables the non-volatile control of the quantum states, which could greatly facilitate topological electronic research. However, ferroelectricity is generally incompatible with systems featuring metallicity due to the screening effect of free carriers. In this study, we report the observation of memristive switching based on the ferroelectric surface state of a topological semimetal (TaSe4)2I. We find that the surface state of (TaSe4)2I presents out-of-plane ferroelectric polarization due to surface reconstruction. With the combination of ferroelectric surface and charge-density-wave-gapped bulk states, an electric-switchable barrier height can be achieved in (TaSe4)2I-metal contact. By employing a multi-terminal-grounding design, we manage to construct a prototype ferroelectric memristor based on (TaSe4)2I with on/off ratio up to 103, endurance over 103 cycles, and good retention characteristics. The origin of the ferroelectric surface state is further investigated by first-principles calculations, which reveals an interplay between ferroelectricity and band topology. The emergence of ferroelectricity in (TaSe4)2I not only demonstrates it as a rare but essential case of ferroelectric topological materials, but also opens new routes towards the implementation of topological materials in functional electronic devices.

Neuromorphic electro-stimulation based on atomically thin semiconductor for damage-free inflammation inhibition.

Inflammation, caused by accumulation of inflammatory cytokines from immunocytes, is prevalent in a variety of diseases. Electro-stimulation emerges as a promising candidate for inflammatory inhibition. Although electroacupuncture is free from surgical injury, it faces the challenges of imprecise pathways/current spikes, and insufficiently defined mechanisms, while non-optimal pathway or spike would require high current amplitude, which makes electro-stimulation usually accompanied by damage and complications. Here, we propose a neuromorphic electro-stimulation based on atomically thin semiconductor floating-gate memory interdigital circuit. Direct stimulation is achieved by wrapping sympathetic chain with flexible electrodes and floating-gate memory are programmable to fire bionic spikes, thus minimizing nerve damage. A substantial decrease (73.5%) in inflammatory cytokine IL-6 occurred, which also enabled better efficacy than commercial stimulator at record-low currents with damage-free to sympathetic neurons. Additionally, using transgenic mice, the anti-inflammation effect is determined by ß2 adrenergic signaling from myeloid cell lineage (monocytes/macrophages and granulocytes).

Non-volatile rippled-assisted optoelectronic array for all-day motion detection and recognition.

In-sensor processing has the potential to reduce the energy consumption and hardware complexity of motion detection and recognition. However, the state-of-the-art all-in-one array integration technologies with simultaneous broadband spectrum image capture (sensory), image memory (storage) and image processing (computation) functions are still insufficient. Here, macroscale (2 × 2 mm2) integration of a rippled-assisted optoelectronic array (18 × 18 pixels) for all-day motion detection and recognition. The rippled-assisted optoelectronic array exhibits remarkable uniformity in the memory window, optically stimulated non-volatile positive and negative photoconductance. Importantly, the array achieves an extensive optical storage dynamic range exceeding 106, and exceptionally high room-temperature mobility up to 406.7 cm2 V-1 s-1, four times higher than the International Roadmap for Device and Systems 2028 target. Additionally, the spectral range of each rippled-assisted optoelectronic processor covers visible to near-infrared (405 nm-940 nm), achieving function of motion detection and recognition.

Programmable supramolecular chirality in non-equilibrium systems affording a multistate chiroptical switch.

The dynamic regulation of supramolecular chirality in non-equilibrium systems can provide valuable insights into molecular self-assembly in living systems. Herein, we demonstrate the use of chemical fuels for regulating self-assembly pathway, which thereby controls the supramolecular chirality of assembly in non-equilibrium systems. Depending on the nature of different fuel acids, the system shows pathway-dependent non-equilibrium self-assembly, resulting in either dynamic self-assembly with transient supramolecular chirality or kinetically trapped self-assembly with inverse supramolecular chirality. More importantly, successive conducting of chemical-fueled process and thermal annealing process allows for the sequential programmability of the supramolecular chirality between four different chiral hydrogels, affording a new example of a multistate supramolecular chiroptical switch that can be recycled multiple times. The current finding sheds new light on the design of future supramolecular chiral materials, offering access to alternative self-assembly pathways and kinetically controlled non-equilibrium states.

An Optoelectronic Synapse Based on Two-Dimensional Violet Phosphorus Heterostructure.

Neuromorphic computing can efficiently handle data-intensive tasks and address the redundant interaction required by von Neumann architectures. Synaptic devices are essential components for neuromorphic computation. 2D phosphorene, such as violet phosphorene, show great potential in optoelectronics due to their strong light-matter interactions, while current research is mainly focused on synthesis and characterization, its application in photoelectric devices is vacant. Here, the authors combined violet phosphorene and molybdenum disulfide to demonstrate an optoelectronic synapse with a light-to-dark ratio of 106 , benefiting from a significant threshold shift due to charge transfer and trapping in the heterostructure. Remarkable synaptic properties are demonstrated, including a dynamic range (DR) of > 60 dB, 128 (7-bit) distinguishable conductance states, electro-optical dependent plasticity, short-term paired-pulse facilitation, and long-term potentiation/depression. Thanks to the excellent DR and multi-states, high-precision image classification with accuracies of 95.23% and 79.65% is achieved for the MNIST and complex Fashion-MNIST datasets, which is close to the ideal device (95.47%, 79.95%). This work opens the way for the use of emerging phosphorene in optoelectronics and provides a new strategy for building synaptic devices for high-precision neuromorphic computing.

2D materials readiness for the transistor performance breakthrough.

As the size of the transistor scales down, this strategy has confronted challenges because of the fundamental limits of silicon materials. Besides, more and more energy and time are consumed by the data transmission out of transistor computing because of the speed mismatching between the computing and memory. To meet the energy efficiency demands of big data computing, the transistor should have a smaller feature size and store data faster to overcome the energy burden of computing and data transfer. Electron transport in two-dimensional (2D) materials is constrained within a 2D plane and different materials are assembled by the van der Waals force. Owning to the atomic thickness and dangling-bond-free surface, 2D materials have demonstrated advantages in transistor scaling-down and heterogeneous structure innovation. In this review, from the performance breakthrough of 2D transistors, we discuss the opportunities, progress and challenges of 2D materials in transistor applications.

An ultrafast bipolar flash memory for self-activated in-memory computing.

In-memory computing could enhance computing energy efficiency by directly implementing multiply accumulate (MAC) operations in a crossbar memory array with low energy consumption (around femtojoules for a single operation). However, a crossbar memory array cannot execute nonlinear activation; moreover, activation processes are power-intensive (around milliwatts), limiting the overall efficiency of in-memory computing. Here we develop an ultrafast bipolar flash memory to execute self-activated MAC operations. Based on atomically sharp van der Waals heterostructures, the basic flash cell has an ultrafast n/p program speed in the range of 20-30 ns and an endurance of 8 × 106 cycles. Utilizing sign matching between the input voltage signal and the storage charge type, our bipolar flash can realize a rectified linear unit activation function during the MAC process with a power consumption for each operation of just 30 nW (or 5 fJ of energy). Using a convolutional neural network, we find that the self-activated MAC method has a simulated accuracy of 97.23%, tested on the Modified National Institute of Standards and Technology dataset, which is close to the conventional method where the MAC and activation operations are separated.

A Full-Device Autonomous Self-Healing Stretchable Soft Battery from Self-Bonded Eutectogels.

Next-generation energy storage devices should be soft, stretchable, and self-healable. Previously reported self-healable batteries mostly possess limited stretchability and rely on healable electrodes or electrolytes rather than achieving full-device self-healability. Herein, an all-component self-bonding strategy is reported to obtain an all-eutectogel soft battery (AESB) that simultaneously achieves full-cell autonomous self-healability and omnidirectional intrinsic stretchability (>1000% areal strain) over a broad temperature range (-20~60 °C). Without requiring any external stimulus, the five-layered soft battery can efficiently recover both its mechanical and electrochemical performance at full-cell level. The developed AESB can be easily configured into various 3D architectures with highly interfacial compatible eutectogel electrodes, electrolyte, and substrate, presenting an excellent opportunity for the development of embodied energy technologies. The present work provides a general and user-friendly soft electronic material platform for fabricating a variety of intrinsic self-healing stretchable multi-layered electronics, which are promising beyond the field of energy storage, such as displays, sensors, circuits, and soft robots.

Supramolecular Gel-Derived Highly Efficient Bifunctional Catalysts for Omnidirectionally Stretchable Zn-Air Batteries with Extreme Environmental Adaptability.

Most existing stretchable batteries can generally only be stretched uniaxially and suffer from poor mechanical and electrochemical robustness to withstand extreme mechanical and environmental challenges. A highly efficient bifunctional electrocatalyst is herein developed via the unique self-templated conversion of a guanosine-based supramolecular hydrogel and presents a fully integrated design strategy to successfully fabricate an omnidirectionally stretchable and extremely environment-adaptable Zn-air battery (ZAB) through the synergistic engineering of active materials and device architecture. The electrocatalyst demonstrates a very low reversible overpotential of only 0.68 V for oxygen reduction/evolution reactions (ORR/OER). This ZAB exhibits superior omnidirectional stretchability with a full-cell areal strain of >1000% and excellent durability, withstanding more than 10 000 stretching cycles. Promisingly, without any additional pre-treatment, the ZAB exhibits outstanding ultra-low temperature tolerance (down to -60 °C) and superior waterproofness, withstanding continuous water rinsing (>5 h) and immersion (>3 h). The present work offers a promising strategy for the design of omnidirectionally stretchable and high-performance energy storage devices for future on-skin wearable applications.

Low-molecular-weight supramolecular adhesives based on non-covalent self-assembly of a small molecular gelator.

Currently developed adhesives are overwhelmingly polymeric in nature. Herein, we highlight for the first time the potential of supramolecular eutectogels assembled from small molecules as robust low-molecular-weight (LMW) supramolecular adhesives in air, water and organic solvents, and under low temperatures. These supramolecular eutectogels were produced from commercial alkyl trimethyl ammonium bromide (CnTAB) in emerging deep eutectic solvents (DESs), which demonstrated rapid (∼2 min), robust, and tunable adhesion to both hydrophilic and hydrophobic surfaces at room temperature in air. Moreover, high adhesion performance was maintained even in liquid nitrogen (-196 °C), underwater, and in organic solvents. A study of the structure-property relationship of these adhesives and molecular dynamics (MD) simulations further clarified the assembly and adhesion mechanism of the C12TAB molecules in DESs. Compared with traditional polymer adhesives and several existing examples of LMW supramolecular adhesives with solvent-free dry network structures, the spontaneous self-assembly of LMW gelators in versatile DESs provides a new strategy for the facile construction of high-strength supramolecular adhesives with gel network structures for a diverse range of harsh environments.

An application-specific image processing array based on WSe2 transistors with electrically switchable logic functions.

With the rapid development of artificial intelligence, parallel image processing is becoming an increasingly important ability of computing hardware. To meet the requirements of various image processing tasks, the basic pixel processing unit contains multiple functional logic gates and a multiplexer, which leads to notable circuit redundancy. The pixel processing unit retains a large optimizing space to solve the area redundancy issues in parallel computing. Here, we demonstrate a pixel processing unit based on a single WSe2 transistor that has multiple logic functions (AND and XNOR) that are electrically switchable. We further integrate these pixel processing units into a low transistor-consumption image processing array, where both image intersection and image comparison tasks can be performed. Owing to the same image processing power, the consumption of transistors in our image processing unit is less than 16% of traditional circuits.

All-in-one two-dimensional retinomorphic hardware device for motion detection and recognition.

With the advent of the Internet of Things era, the detection and recognition of moving objects is becoming increasingly important1. The current motion detection and recognition (MDR) technology based on the complementary metal oxide semiconductor (CMOS) image sensors (CIS) platform contains redundant sensing, transmission conversion, processing and memory modules, rendering the existing systems bulky and inefficient in comparison to the human retina. Until now, non-memory capable vision sensors have only been used for static targets, rather than MDR. Here, we present a retina-inspired two-dimensional (2D) heterostructure based retinomorphic hardware device with all-in-one perception, memory and computing capabilities for the detection and recognition of moving trolleys. The proposed 2D retinomorphic device senses an optical stimulus to generate progressively tuneable positive/negative photoresponses and memorizes it, combined with interframe differencing computations, to achieve 100% separation detection of moving trichromatic trolleys without ghosting. The detected motion images are fed into a conductance mapped neural network to achieve fast trolley recognition in as few as four training epochs at 10% noise level, outperforming previous results from similar customized datasets. The prototype demonstration of a 2D retinomorphic device with integrated perceptual memory and computation provides the possibility of building compact, efficient MDR hardware.

Programmable Transient Supramolecular Chiral G-quadruplex Hydrogels by a Chemically Fueled Non-equilibrium Self-Assembly Strategy.

The temporal and spatial control of natural systems has aroused great interest for the creation of synthetic mimics. By using boronic ester based dynamic covalent chemistry and coupling it with an internal pH feedback system, we have developed a new chemically fueled reaction network for non-equilibrium supramolecular chiral G-quadruplex hydrogels with programmable lifetimes from minutes, to hours, to days, as well as high transparency and conductivity, excellent injectability, and rapid self-healing properties. The system can be controlled by the kinetically controlled in situ formation and dissociation of dynamic boronic ester bonds between the cis-diol of guanosine (G) and 5-fluorobenzoxaborole (B) in the presence of chemical fuels (KOH and 1,3-propanesultone), thereby leading to a precipitate-solution-gel-precipitate cycle under non-equilibrium conditions. A combined experimental-computational approach showed the underlying mechanism of the non-equilibrium self-assembly involves aggregation and disaggregation of right-handed helical G-quadruplex superstructures. The proposed dynamic boronic ester-based non-equilibrium self-assembly strategy offers a new option to design next-generation adaptive and interactive smart materials.

Super-stretchable and extreme temperature-tolerant supramolecular-polymer double-network eutectogels with ultrafast in situ adhesion and flexible electrochromic behaviour.

The current tough and stretchable gels with various integrated functions are mainly based on polymer hydrogels. By introducing a non-covalent supramolecular self-assembled network into a covalently cross-linked polymer network in the presence of eco-friendly and cost-effective deep eutectic solvents (DESs), we developed a new small molecule-based supramolecular-polymer double-network (SP-DN) eutectogel platform. This exciting material exhibits high stretchability and toughness (>18 000% areal strain), spontaneous self-healing ability, ultrafast (∼5 s) in situ underwater and low-temperature (-80 °C) adhesion, and unusual boiling water-resistance, as well as strong base-, strong acid- (even aqua regia), ultra-low-temperature- (liquid nitrogen, -196 °C), and high-temperature- (200 °C) resistance. All these outstanding properties strongly recommend the SP-DN eutectogels as a quasi-solid electrolyte for soft electrochromic devices, which exhibited exceptional flexibility and consistent electrochromic behaviours in harsh mechanical or temperature environments. The experimental and simulation results uncovered the assembly mechanism of the SP-DN eutectogels. Unlike polymer hydrogels, the obtained SP-DN eutectogels showed high molecular design freedom and structural versatility. The findings of this work offer a promising strategy for developing the next generation of mechanically robust and functionally integrated soft materials with high environmental adaptability.

Controllable Doping in 2D Layered Materials.

For each generation of semiconductors, the issue of doping techniques is always placed at the top of the priority list since it determines whether a material can be used in the electronic and optoelectronic industry or not. When it comes to 2D materials, significant challenges have been found in controllably doping 2D semiconductors into p- or n-type, let alone developing a continuous control of this process. Here, a unique self-modulated doping characteristic in 2D layered materials such as PtSSe, PtS0.8 Se1.2 , PdSe2 , and WSe2 is reported. The varying number of vertically stacked-monolayers is the critical factor for controllably tuning the same material from p-type to intrinsic, and to n-type doping. Importantly, it is found that the thickness-induced lattice deformation makes defects in PtSSe transit from Pt vacancies to anion vacancies based on dynamic and thermodynamic analyses, which leads to p- and n-type conductance, respectively. By thickness-modulated doping, WSe2 diode exhibits a high rectification ratio of 4400 and a large open-circuit voltage of 0.38 V. Meanwhile, the PtSSe detector overcomes the shortcoming of large dark-current in narrow-bandgap optoelectronic devices. All these findings provide a brand-new perspective for fundamental scientific studies and applications.

Ultrathin Multibridge Channel Transistor Enabled by van der Waals Assembly.

Multibridge channel field-effect transistors (MBCFETs) enable improved gate control and flow of a large drive current and they are regarded as promising candidates for next-generation transistor architecture. However, in achieving a larger drive current with a thinner channel, limitations arise from the decrease in mobility when the thickness of the Si nanosheet is less than 5 nm. In addition, an increase in the leakage current is unavoidable when a large number of channels are stacked. Here, a 2D ultrathin MBCFET is demonstrate, constructed based on 2 nm/2 nm MoS2 channels. The normalized drive current (23.11 µA*µm µm-1 ) in each level channel of this MBCFET exceeds that of the latest seven-level-stacked Si MBCFET, while the leakage current is only 0.4% of this value, with the subthreshold swing reaching 60 mV dec-1 and an on/off ratio reaching up to 4 × 108 at room temperature. Furthermore, the drive current of this 2D ultrathin MBCFET can be further increased by regulating the polarity of the operation voltage to reduce the injection barrier. The combination of 2D materials and an MBC structure has the potential for use in high-performance and low-power-consumption electronics.

Ultrafast non-volatile flash memory based on van der Waals heterostructures.

Flash memory has become a ubiquitous solid-state memory device widely used in portable digital devices, computers and enterprise applications. The development of the information age has demanded improvements in memory speed and retention performance. Here we demonstrate an ultrafast non-volatile flash memory based on MoS2/hBN/multilayer graphene van der Waals heterostructures, which achieves an ultrafast writing/erasing speed of 20 ns through two-triangle-barrier modified Fowler-Nordheim tunnelling. Using detailed theoretical analysis and experimental verification, we postulate that a suitable barrier height, gate coupling ratio and clean interface are the main reasons for the breakthrough writing/erasing speed of our flash memory devices. Because of its non-volatility this ultrafast flash memory could provide the foundation for the next generation of high-speed non-volatile memory.

A Steep-Slope MoS2/Graphene Dirac-Source Field-Effect Transistor with a Large Drive Current.

In the continuous transistor feature size scaling down, the scaling of the supply voltage is stagnant because of the subthreshold swing (SS) limit. A transistor with a new mechanism is needed to break through the thermionic limit of SS and hold the large drive current at the same time. Here, by adopting the recently proposed Dirac-source field-effect transistor (DSFET) technology, we experimentally demonstrate a MoS2/graphene (1.8 nm/0.3 nm) DSFET for the first time, and a steep SS of 37.9 mV/dec at room temperature with nearly free hysteresis is observed. Besides, by bringing in the structure of gate-all-around (GAA), the MoS2/graphene DSFET exhibits a steeper SS of 33.5 mV/dec and a 40% increased normalized drive current up to 52.7 µA·µm/µm (VDS = 1 V) with a current on/off ratio of 108, which shows potential for low-power and high-performance electronics applications.

Self-healing mechanism and bioelectrochemical interface properties of core-shell guanosine-borate hydrogels.

The self-healing mechanism and bioelectrochemical interface properties of supramolecular gels have been rarely explored. In this context, we propose a constitutive "fibril-reorganization" model to reveal the self-healing mechanism of a series of core-shell structured guanosine-borate (GB) hydrogels and emphasize that interfibrillar interactions at the supramolecular polymer scale (G-quadruplex nanowires) drive the self-healing process of GB hydrogels. Structure-electrochemical sensing performance studies reveal that GB hydrogel nanofibers with relatively strong biomolecular affinity such as -SH modified GB hydrogel (GB-SH) show a high sensitivity of response and low limit of detection for tumour marker alpha-fetoprotein sensing (AFP; 0.076 pg mL-1). Guanosine/ferroceneboronic acid (GB-Fc) hydrogel nanofibers with superior conductivity and redox activity display the widest linear detection range for AFP (0.0005-100 ng mL-1). Structure-property correlations of GB hydrogels provide useful insight for the future design of advanced self-healing materials and electrochemical biosensors.

NiO nanoparticles decorated hexagonal Nickel-based metal-organic framework: Self-template synthesis and its application in electrochemical energy storage.

A one-pot solvothermal strategy and subsequent calcination were proposed for fabricating a composite of NiO nanoparticles on hexagonal Ni-based metal-organic framework (Ni-MOF) (Ni-MOF@NiO). The prepared NiO nanoparticles on the hexagonal Ni-MOF not only improves the electrical conductivity and increases redox active sites, but also prevents the agglomeration of NiO nanoparticles. In particular, highly dispersed and small-sized NiO nanoparticles on the hexagonal Ni-MOF facilitates the migration of electrolyte ions, and the pseudocapacitive performance is evaluated through electrochemical measurements. At 0.5 A g-1, the Ni-MOF@NiO composite shows a specific capacitance of up to 1192.7 F g-1 and a high capacity retention (93.23% over 5000 cycles) in 3 M KOH. Moreover, the Ni-MOF@NiO nanoparticles and activated carbon are assembled into aqueous devices with a maximum energy density of 62.2 Wh kg-1. These results indicate the potential of Ni-MOF@NiO composite as an electrode material for application in supercapacitors. Additionally, the method of synthesizing Ni-MOF@NiO in this study can be used to synthesize other MOF@metal oxide materials for electrochemical energy storage and other related applications.