Photogenerated charge carriers play a pivotal role in driving chemical transformations during photocatalysis. However, the structural complexity of photocatalysts presents challenges in establishing nanoscale correlation between carrier dynamics and photocatalytic activity. Here we integrate single-molecule fluorescence imaging with femtosecond interferometric scattering microscopy to resolve the carrier dynamics and specific reaction rate of hydroxyl radical oxidation at the individual structural features (that is, basal plane, edge and wrinkle) in 2D layered indium selenide (InSe). We find a positive linear correlation between the specific reaction rate and the carrier lifetime, but only a weak correlation with the carrier concentration. Moreover, both basal planes and edges exhibit peak lifetimes and specific reaction rates in three-layer InSe. These spatially resolved, correlative single-molecule superlocalization and ultrafast measurements are a powerful tool for investigations of structure–function correlation. Monitoring charge carrier dynamics and photocatalytic reaction rates in individual photocatalyst particles is a challenging task that can help us to understand structure–reactivity relationships. Here single-molecule fluorescence imaging is coupled with femtosecond interferometric scattering microscopy to investigate these properties in 2D InSe flakes.
Fullerene-based electron transport layers (ETLs) are commonly used in tin-based perovskite solar cells for high power conversion efficiency, but they suffer from high cost, complex synthesis, low electron mobilities and limited interaction with the perovskite. To tackle these issues, we use non-fullerene ETLs, that is, fluorinated triple-acceptor polymers (P1, P2 and P3), which offer lower cost, simpler synthesis, higher electron mobility and greater structural flexibility. These polymers form continuous, conformal interfaces with tin perovskite layers, enabling stronger, more uniform interactions, especially over large areas. Notably, P3 achieves optimal energy-level alignment and efficient electron transfer, resulting in efficiencies of 16.06% (certified at 15.90%) for 0.04-cm2 and 14.67% (certified at 14.51%) 1-cm2 devices, outperforming fullerene-based cells. Both devices retain over 85% of their initial efficiency after 550 h under continuous 1-sun illumination owing to the hydrophobicity of P3's long-alkyl side chains and fluorine substituents. This study shows the potential of non-fullerene ETLs for tin perovskite photovoltaics.
With the rapid advancement of modern information technologies, oscillators are essential for communication and neuromorphic computing, motivating the development of NDR-based resonant tunneling devices for self-sustained oscillation. Here, we fabricate highly aligned Gr/hBN/Gr resonant tunneling transistors using a tear-and-stack technique and achieve gate-tunable NDR. By systematically varying the graphene layer number, twist angle, hBN thickness, and junction-to-external resistance ratio, we show that momentum-conserving tunneling is the key mechanism of NDR, while band-structure engineering and voltage-division effects critically modulate its behavior. Finally, we integrate the device into an LC circuit and demonstrate a tunable oscillator with an ultralow startup voltage of 1.3 V, highlighting the potential of graphene resonant tunneling devices for next generation low power, low phase noise oscillator applications.
Neuromorphic computing is an ideal approach for achieving complex pattern recognition works; however, it is usually incompatible with digital logic processing units, limiting its application scope. Leveraging an opto-ferroelectric coupling enhanced effect, we herein achieve the light-controlled mode switchover between logic processing and neuromorphic computing in a ferroelectric transistor with α-In2Se3/h-BN as gate dielectrics and MoS2 as channel. Under dark conditions, the transistor operates in digital logic mode with a high current on/off ratio of 109, ultra-low subthreshold swing (SS) of 33 mV/dec, and low leakage current of 5.6 × 10-13 A, which is promising for logic processing applications. The inverter and NOR circuits with high noise margin and low power consumption were further implemented via interconnecting n- and p-type transistors. Under light conditions, the ferroelectric polarization field of α-In2Se3 is significantly enhanced, leading to an enlarged hysteresis window (ΔV) and switching the transistor into an optoelectronic synapse mode for neuromorphic computing, which can support image classification with an accuracy of up to 94.43% and a low energy consumption of 0.47 pJ/spike. This work provides an opto-ferroelectric coupling-enhanced transistor that addresses the incompatibility issue between digital logic and neuromorphic computing units, offering a new pathway for next-generation computing devices.
Self-powered photodetectors with low dark current and high sensitivity are highly desirable for advanced optoelectronic applications. Herein, we report a novel temperature-sensitive photodetector based on a CH3NH3PbI3/VO2 composite film, which integrates the strong visible-light absorption of perovskite and the reversible metal-insulator transition (MIT) of VO2. Operating under zero bias, the device exhibits excellent self-powered performance, achieving a high responsivity of 538 mAW(-1) and a broad spectral response ranging from 450 to800nm. Notably, a unique reversible dark current polarity reversal is observed at temperatures below 306.3 K, where the dark current direction is opposite to that of the photocurrent. Temperature-dependent characterizations reveal enhanced photocurrent dynamics near the phase transition regions of both CH3NH3PbI3 and VO2. At 300 K, the device attains a detectivity of 3.2 x 10(12 )Jones and an on-off ratio of 342. This work proposes a novel strategy leveraging the synergistic effect of dual phase-transition materials, realizes a temperature-tunable self-powered mechanism induced by spin-coating-induced perovskite inhomogeneity, and bridges the gap between phase-transition materials and hybrid perovskite systems, paving the way for multifunctional photodetectors in dual-parameter sensing and adaptive optical systems.
advancement of cryogenic electronics for space exploration and quantum computing is critically limited by the absence of reliable p-channel transistors, which often suffer from low on-off ratios and significant hysteresis at low temperatures. Here, we report highperformance, wafer-scale p-type tellurium oxide (TeOX) thin film transistors (TFTs) fabricated via e-beam evaporation and low-temperature annealing (< 150 degrees C). Through precise modulation of oxygen content, we achieve a high field-effect mobility of 30 cm 2 V(-1)s(-1) and a record-high on-off ratio of 10(10) at 10 K, with negligible hysteresis and high reliability. The exceptional performance is attributed to bandgap engineering via oxygen composition-which effectively suppresses the off-state current-and to enhanced crystallinity achieved through optimized annealing. This breakthrough underscores the potential of oxygen-modulated TeOx for energy-efficient and highly reliable CMOS integrated circuits in extreme cryogenic environments.
Ferroelectric reconfigurable field-effect transistors (Fe-RFETs) and negative capacitance field-effect transistors (NC-FETs) have emerged as promising candidates for overcoming the performance and energy-efficiency limitations of conventional CMOS scaling. In this work, a systematic device and circuit-level investigation of gate-allaround (GAA)-structure FET, NC-FET, Fe-RFET, and NC-Fe-RFET are carried out using TCAD simulations. The electrical characteristics of the four devices are first analyzed and compared. Further, logic functions including NAND, NOR, XOR, and XNOR are implemented and evaluated in terms of delay, power consumption, energy consumption, area, and figure of merit (FoM). The results indicate that Fe-RFET-based logic functions achieve superior FoM due to the reduced delay and compact area, while the NC-Fe-RFET-based logic functions show the lowest power consumption. Besides, a Fe-RFET-based full adder is designed and simulated to assess system-level performance. Compared with the GAAFET-based full adder, the proposed Fe-RFET implementation exhibits significantly reduced propagation delay (40 ps), power consumption (10.4 nW), and energy per operation (0.08 fJ), leading to a substantial FoM improvement of over 30 dB. These results demonstrate the strong potential of Fe-RFETs for high-performance and energy-efficient reconfigurable logic and arithmetic circuits.
The escalating demand for memory scaling requires switching mechanisms that remain reliable at atomic thickness while operating with minimal energy consumption. Sliding ferroelectricity provides a promising platform for this challenge: the spontaneous interfacial polarization emerging at superlubric, atomically thin van der Waals interfaces endows exceptional fatigue resistance, ultrafast switching and ultralow coercive fields. Nevertheless, the intrinsically weak polarization of sliding ferroelectrics limits the available signal window, necessitating new physical mechanisms that can transduce subtle polarization variations into pronounced resistance contrasts. Here, we address this challenge by introducing momentum-conserving resonant tunneling between lattice-aligned graphene electrodes. The resulting resonant sliding ferroelectric tunnel junction achieves a tunneling electroresistance (TER) ratio of up to 225.65
Uncontrolled proton activity in aqueous electrolytes triggers detrimental side reactions that compromise the stability of zinc (Zn) metal anodes. To address this challenge, we propose a full-process proton regulation strategy enabled by the unique β-1,4-glycosidic framework of chitosan oligosaccharide (COS). The rigid COS backbone effectively constrains proton generation and transport in the electrolyte, while its preferential interfacial adsorption constructs an ultrathin molecular barrier that inhibits proton consumption at the Zn surface. This dual-function molecular architecture synergistically realizes "generation-transport-consumption" proton regulation, thereby delivering exceptional electrochemical performance: long-term cycling stability over 8,000 h in Zn||Zn symmetric cells, an average Coulombic efficiency of 99.84% over 2,300 cycles in Zn||Cu cells, and superior cycling stability for more than 2,000 cycles at 2 A g-1 in Zn||MnO2 full cells. This work reveals glycosidic frameworks as a universal and transferable design principle for aqueous batteries, shifting electrolyte design from functional group-centric optimization to framework-enabled regulation toward sustainable, high-performance energy storage.
Non-dispersive infrared gas sensors, renowned for their high selectivity and high reliability, are extensively employed in applications of smart agriculture. In particular, a stable and high-emission infrared source component plays a critical role in the proper functioning of non-dispersive infrared systems. However, current infrared sources usually have shortcomings in poor temperature homogeneity within the active area and low-power consumption. Here, we demonstrate a wafer scale, in situ integrated infrared source combined with an Al@NF-based radiation layer, achieving a high emissivity of 0.8 at 4.26 mu m. Through iterative optimization of the microheater pattern, the temperature homogeneity reaches an impressive 90%. In the integrated Al@NF-infrared source sensing system, the power density is reduced from 386.8 to 256.7 mW/mm2; meanwhile, its operational efficiency is increased eighteenfold, from 0.39% to 7.24%. The developed device enables precise tracking of greenhouse gas concentrations under controlled greenhouse conditions. The findings pave the way for low-power non-dispersive infrared systems and provide a new hardware model for smart agriculture.
The polarization of HfO2-based ferroelectrics originates from the metastable orthorhombic phase formed during the tetragonal to monoclinic phase transition and is typically controlled by tuning the phase content. However, another way to control polarization via modulating ferroelectric domain orientations remains underexplored. This work uncovers a hidden tetragonal-orthorhombic phase transition pathway to engineer domain orientations and further polarization in polycrystalline Hf0.5Zr0.5O2 using single-crystalline TiN substrates. Specifically, (001)O and/or (010)O domains, which fully contribute to remanent polarization under an electric field, are controllable in Hf0.5Zr0.5O2 on TiN (001) and (111), enhancing remanent polarization compared to that on TiN (110). The key is the hidden transition from the tetragonal phase's longest c-axis to the orthorhombic phase's shorter bO/cO-axis, alongside the reported one to the longest aO-axis, assisted by periodic dislocations at the TiN/Hf0.5Zr0.5O2 interface. These findings shed light on governing the polarization of Hf0.5Zr0.5O2 films by controlling the interface dislocations and further domain orientations.
Ferroelectric materials are promising for developing non-volatile memory, neuromorphic computing, and photovoltaic technologies. Taking advantage of variable switching kinetics provides an important strategy for designing multifunctional ferroelectric devices. However, the conventional ferroelectrics due to the unmovable atomic species generally own a single switching kinetics, thus versatile and configurable switching kinetics still remain challenging. In this work, we systematically investigate the switching kinetics of the van der Waals ferroionic CuInP2S6 through polarization-determined ferroelectric photovoltaic behaviors. Based on the time- and field-dependent polarization switching and numerical simulation, we discover three switching modes, including intralayer switching, interlayer switching and intralayer-interlayer coupling switching in CuInP2S6. Through designing the poling voltage amplitude and width, we achieve the configurable kinetic control of polarization switching in CuInP2S6, enabling tunable binary, gradual and accumulative switching with defined poling voltages in a single device. The work demonstrated here is instructive for the development of nanoscale multifunctional ferroelectric devices.
Computer vision systems that lack color sensitivity may encounter challenges in object identification, particularly when the target object's pattern resembles the background. To enhance neural network color sensitivity while maintaining low power consumption and fast data processing, we present a switchable photodetection-synaptic transistor (SPST) based on a two-dimensional (2D) perovskite ferroelectric (PMA)2PbCl4 film for constructing self-powered optoelectronic synapses with color perception capabilities, with applications for in-sensor memory and neuromorphic computing. The SPST can be switched to photodetection mode or optoelectronic synapse modes by controlling its gate voltage, and, compared with the neural network based on an electrical synapse, the processing time and power consumption of the neural network based on the SPST are reduced by 56.52% and 91.43%, respectively. Compared to the traditional architecture based on electrical synapses, the classification accuracies for different targets improve to 98.53% (from 10.2%) and 99.47% (from 12.98%) after 5 training epochs.
Tin-based perovskites, renowned for their eco-friendliness, intrinsic high hole mobility, and low effective mass, hold great potential for p-type thin-film transistors (TFTs). However, their propensity for rapid crystallization and oxidation severely limits stability and carrier mobility. Here, we strategically enhance perovskite TFT performance by incorporating 2-thiopheneethylamine thiocyanate (TEASCN) into 3D tin-based perovskites. The induction of the pseudo-halide SCN − into a bilayer quasi-2D perovskite intermediate phase, combined with the strong interaction between sulfur-bearing thiophene rings (TEA + ) and Sn-I octahedra, effectively reorients perovskite crystallization while inhibiting Sn 2+ oxidation and reducing trap density. Consequently, TEASCN-based TFTs achieve an average hole mobility of more than 60 square centimeters per volt per second and an on/off current ratio surpassing 10 8 , standing out among state-of-the-art p-type perovskite TFTs. Furthermore, unencapsulated devices preserve 84% of their initial mobility after 30 days in an N 2 atmosphere, underscoring their remarkable stability. This work opens a straightforward path toward high-mobility and highly stable tin-based perovskite transistors.
The non-volatile spontaneous ferroelectric polarization field serves as a cornerstone for applying ferroelectric materials in electronic devices, yet it is frequently mitigated by charge trapping at defect sites. Achieving an effective transition between ferroelectric polarization and charge trapping is challenging due to the inherent opposition of the two mechanisms and the uncontrollable charge trapping types in ferroelectric materials. Here, we realized a polarity-dependent ferroelectric transition in two-dimensional ferroelectric heterojunction transistor by integrating a hybrid organic-inorganic ferroelectric layer embedded with electron trapping sites. Through theoretical calculations and experimental validation, we demonstrate a ferroelectric manifestation and elimination mechanism based on the polarity of the semiconductor layer. The electron-majority n-type semiconductor exhibits charge trapping behavior, while the electron-minority p-type transistor exhibits the ferroelectric control mechanism. Leveraging the mechanism transition, our bipolar heterojunction transistor enables synergistic heterogeneous control of non-volatile memory and volatile synaptic weight modulation within a single bipolar ferroelectric transistor. Based on the experimentally extracted parameters from the transistors, the device-informed simulation achieves a recognition accuracy of 92.9% and a 20.7-fold improvement in training efficiency of the transfer learning network.
Hafnium zirconium oxide with antiferroelectric polarizations holds great promise for emerging applications such as neuromorphic computing, energy-efficient storage, and nonvolatile memory, owing to its tunable phase transitions, fast switching speed, improved endurance, and excellent compatibility with silicon-based processes. In practical memory applications, however, the moderate residual polarizations of antiferroelectric hafnium zirconium oxide films pose greater challenges for nondestructive readout than their ferroelectric counterparts, particularly when relying solely on electrical pulses applied via metal electrodes. Here, we introduce graphite nanosheets as photoactive top electrodes for Hf0.1Zr0.9O2-based nonvolatile memories, enabling nondestructive optical readout through the photo-pyroelectric effect. The optothermally active van der Waals graphite nanosheet top electrode triggers nonpolar-to-polar state transition, thereby inducing a pyroelectric response in the Hf0.1Zr0.9O2 layer. This mechanism enables self-powered and nondestructive photo-pyroelectric sensing capabilities, as well as voltage-programmable in-memory logic functionalities-circumventing the destructive readout issues faced by traditional hafnium-based ferroelectrics. Our work paves the way for hafnium-zirconium-oxide-based, photonic-compatible memory architectures for post-Moore electronics.
Topological polar structures in ferroelectric thin films have become an emerging research field for exotic phenomena. Due to the prerequisite of the intricate balance among the intrinsic dipolar anisotropy, the imposed electric and mechanical boundary, the topological polar domains are predominantly formed within complex oxides. Here, combining the microscopic polarization measurement via Piezoresponse Force Microscopy and the atomic displacement mapping via Scanning Transmission Electron Microscopy, we report the direct observation of atomically thin topological polar textures in twisted boron nitride system, which is well confined at the twisted interface. Leveraging the advantages of the sliding switching mechanism and atomically thin nature, we demonstrate nonvolatile manipulation of the topological polar textures, which is crucial for potential applications. This result provides opportunities to create truly 2D topological polar textures with dynamical controllability, which would render the exploration on the previously unknown physical phenomena and functional devices feasible.
The emergence of sliding ferroelectricity is found in non-ferroelectric two-dimensional materials, which brings novel ferroelectric phenomena and expands the potential for advancing ferroelectric devices. Experimental studies have largely focused on sliding ferroelectricity with fixed twist angles owing to the limitations of preparation methods with controlled angles. However, how to modulate the ferroelectric properties in the sliding materials is still challenging. In this work, the out-of-plane ferroelectric properties of typical bilayer MoS2/WS2 heterostructure are reported by precisely controlling twist angles. The experimental results demonstrate that the second-harmonic generation response, indicative of symmetry breaking, decreases as the twist angle increases. In addition, the switching voltage of ferroelectric polarization exhibits the opposite trend with increasing the twist angle. According to experimental studies and theoretical calculations, the tunability of ferroelectric properties arises from the distortion of polar symmetry regions induced by Moiré patterns at different twist angles. Furthermore, the ferroelectric semiconductor field-effect transistors yield the twist angles dependent electrical properties, achieving a large ferroelectric memory window of ≈14 V. The study opens the door to significantly modulating the sliding ferroelectricity via designing twist angles, which will enrich the framework of twistronics and expand the promising applications in the emerging sliding ferroelectric devices.