ACS Applied Electronic Materials最新文献

The integration of two-dimensional (2D) materials with metal halide perovskites offers a multidimensional approach for simultaneously addressing the interfacial, electronic, ionic, and stability-related limitations of conventional perovskite solar cells. Despite demonstrating the power conversion efficiencies of over 26%, their practical commercialization remains hindered by factors such as severe environmental instability, ion migration, interfacial recombination, and thermal degradation. Recent studies demonstrate that graphene, transition metal dichalcogenides (TMDs), MXenes, layered 2D perovskites, and related architectures can modify charge transfer, interfacial energetics, defect populations, crystallization behavior, and ionic transport through cooperative interfacial effects. This review highlights the recent progress in multidimensional 2D-perovskite heterostructures by focusing on interfacial engineering, charge-transfer dynamics, defect passivation mechanisms, and performance-enhancement pathways. There is particular emphasis on graphene-assisted transport layers, TMD-based heterointerfaces, MXene-enabled architectures, graded quasi-2D systems, and van der Waals (vdW) heterostructures. Furthermore, the review also addresses the challenges associated with synthesizing these solar cells, such as scalability, phase instability, interfacial reconstruction, and long-term reliability under operational conditions. The review concludes by discussing promising opportunities in flexible photovoltaics, tandem solar cells, and multifunctional optoelectronic systems. Collectively, synergistic 2D-perovskite heterostructures exhibit a promising route to more efficient, stable, and commercially viable next-generation solar-energy technologies. This review integrates material-specific architectures with their underlying physicochemical mechanisms, enabling a comparative assessment of interfacial engineering, charge-transfer pathways, defect regulation, ion migration, crystallization, and device stability across different 2D-perovskite systems.

All-inorganic cesium lead bromide (CsPbBr₃) nanocrystals (NCs) have recently attracted extensive attention due to their high photoluminescence quantum yield (PLQY), tunable bandgap, and promising applications in photodetectors. However, the stability of photodetector devices is still limited by the defect states, lattice microstrain, and phase instability. In this work, we investigate the effects of A-site cation doping (K⁺, Rb⁺, and FA⁺) on the structural, optical, and photodetection properties of CsPbBr₃ NCs, leading to stable photodetectors. By combining the Williamson–Hall method and DFT calculations, it has been confirmed that moderate A-site doping can preserve the cubic perovskite phase while inducing slight lattice contraction, reducing dislocation density, and enhancing crystallinity. As a result, the microstrain of 5% Rb⁺-doped (nominal precursor concentrations) CsPbBr₃ lattice is stable around 0.0028, while its PLQY increases to 98.7% (solution) and the slow-decay lifetime extends to 81.65 ns. The photodetector devices based on doped CsPbBr₃ NCs exhibit enhanced responsivity around 6.99 A/W at a high incident power of 28.1 mW, and the detectivity is stabilized around 4.9 × 10¹⁰ Jones at the light intensity from 5.6 to 22.5 mW. These findings provide clear evidence that rational A-site cation engineering is an effective strategy to optimize the optoelectronic performance of CsPbBr₃ NCs for high-performance photodetectors.

Flexible thermoelectric generators (f-TEGs) are a promising technology for harvesting low-grade waste heat to provide supplemental electrical power for flexible electronics. However, the large-scale market adoption of f-TEGs remains limited by the lack of manufacturing approaches that can simultaneously enable low thermal budget processing, mechanical flexibility, and high thermoelectric performance (ZT). Conventional sintering approaches utilize prolonged bulk-thermal exposures, thereby limiting design freedom and form factor flexibility. Moreover, the interdependence of electrical conductivity, Seebeck coefficient, and thermal conductivity in thermoelectric materials limits integration of conductive pathways that aid in selective energy delivery. Here, we report a scalable, energy-efficient fabrication strategy that combines flash sintering with MXene (Ti₃C₂) incorporation to produce high-density, thick (>200 µm) p-type Bi_0.5Sb_1.5Te₃ (BST) thermoelectric films. Homogeneous MXene incorporation functions as a conductive nanoadditive, enabling efficient pulsed-light xenon energy delivery and uniform densification across thick films within milliseconds under ambient conditions. Subsequent topical MXene deposition introduces high-aspect-ratio BST/MXene heterointerfaces, enabling energy-barrier scattering that decouples electrical conductivity and Seebeck coefficient. The optimized BST−MXene flash-sintered films exhibit a power factor of 2100 µW/mK² and a room-temperature ZT of 0.52, a ∼126% improvement over pristine BST films. Leveraging the flash-sintering MXene additive manufacturing process, a five-leg flexible thermoelectric generator is fabricated, delivering a maximum power output of 171.7 µW and a power density of 2.45 mW/cm² at a temperature difference of 30 K with stability under bending tests. MXene-assisted flash sintering enables rapid, scalable fabrication of high-performance flexible thermoelectric devices.

Neuromorphic devices require reliable charge trapping mechanisms to emulate synaptic functionalities such as hysteresis, memory retention, and weight modulation; however, conventional oxide semiconductor-based devices often suffer from limited stability due to the absence of well-defined trapping layers. Here, we demonstrate that defect-engineered hexagonal boron nitride (hBN) grown by plasma-enhanced chemical vapor deposition (PECVD) can serve as an effective charge-trapping interlayer in indium-gallium-zinc oxide (IGZO) synaptic transistors. The PECVD-grown hBN exhibits significant structural disorder, oxygen-related bonding, increased Urbach energy, and reduced film density, indicating the presence of abundant defect-induced localized states that provide energetically favorable sites for charge trapping and retention. When the hBN film is integrated with the IGZO semiconducting channel layer, it significantly enhances the charge trapping efficiency, resulting in a pronounced increase in the hysteresis window from 0.8 to 4.7 V, along with improved synaptic characteristics such as enhanced potentiation/depression behavior and stable long-term memory retention. These results highlight the potential of PECVD-grown defect-rich hBN as a functional charge-trapping layer for high-performance oxide semiconductor-based neuromorphic devices.

Accompanying the rapid growth of wearable electronics, flexible hydrogel pressure sensors have garnered significant attention due to their promising application in health monitoring and human–machine interfaces. However, traditional hydrogels suffer from water evaporation under ambient conditions, resulting in structural changes and functional decline. In this work, a series of polyacrylamide/gelatin (PAMg) hydrogels with different diameters of microcolumn structure were fabricated via a straightforward template method. The obtained PAMg hydrogels were further treated with composite polyols to improve weather resistance. Using the as-prepared PAMg hydrogel as a sensing medium, sandwich-structured hydrogel pressure sensors were assembled. Combined with equivalent circuit simulation and in situ structural characterization, the obvious variations in electric double-layer capacitance at the hydrogel–electrode interface and induced capacitance between electrodes, which originate from the microcolumn deformation under loading, effectively enhance the capacitance sensing performance of the sensors. Investigations of the effect of microcolumn diameter on sensing performance reveal that the decrease in microcolumn diameter can improve the sensitivity of the sensor. Nevertheless, an excessively small microcolumn diameter leads to insufficient mechanical strength of the microcolumns and results in collapse during tests. Notably, the sensor based on PAMg hydrogels with 600 μm microcolumn diameter exhibits a stable capacitance response over a wide strain and pressure range from 0.01% strain (0.15 kPa) to 50% strain (150 kPa) as well as excellent fatigue resistance (1000 cycles). Moreover, these sensors illustrate precise electrical response to various external stimuli, including static force, temperature, joint movement, etc. Meanwhile, the sensors possess outstanding environmental tolerance and anti-overload capability, thereby enhancing their practical utility.

With the development of wearable electronics, Internet of Things devices, and integrated sensor systems, flexible and miniaturized energy-storage technologies are increasingly sought. In the present work, we present a scalable approach to manufacture flexible micro-supercapacitors (MSCs) using a commercial carbon ink doped with 5 wt % polyaniline (PANI) through semi-automatic screen printing on polyethylene terephthalate (PET) substrates. Rheological tests show that the PANI–carbon ink is highly shear-thinning, highlighting that the presence of PANI maintains the flow properties needed for the screen-printing process and also allows well-defined interdigitated electrode structures to be achieved. The hybrid electrode exhibits a maximum areal capacitance of 11.68 mF cm^–2 and an areal energy density of 0.584 µWh cm^–2. The power-law and Dunn analysis results support mixed surface and diffusion charge storage with a greater capacitive component at higher scan rates. After 15,000 GCD cycles, the capacitance retained by the MSC is about 94% with a calculated coulombic efficiency of 98.24% at the 15,000th cycle. The flexibility is shown by maintaining 98.2% capacitance retention under bending. Moreover, series connections of MSCs increase the operating voltage to 0.6–1.2 V, parallel connections boost the charge-storage capacity and the integrated devices can drive a red LED. These findings illustrate a scalable way to make redox-active polymers a part of commercial screen-printing inks for mechanically flexible, practically integrated microscale energy-storage devices.

In the rapidly evolving fields of flexible electronics and biomedical devices, traditional flexible electronic materials are prone to functional degradation during service, primarily due to mechanical wear and the propagation of microcracks. This degradation not only reduces operational lifespan and increases maintenance costs but also introduces potential safety hazards. Such passive failure mechanisms have become critical bottlenecks constraining the high-quality development of related disciplines. In response, self-healing materials—an important subclass of intelligent materials—have been developed. These materials are capable of autonomously detecting damage and initiating repair processes, either without external intervention or under mild stimuli, thereby enabling simultaneous restoration of structural integrity and functional performance. However, materials relying on a single self-healing mechanism inevitably suffer an inherent trade-off between mechanical robustness and self-healing efficiency. This review systematically summarizes extrinsic and intrinsic self-healing mechanisms, with a particular focus on multi-mechanism synergistic strategies. These synergistic systems effectively balance mechanical strength, healing speed, and cyclic stability, demonstrating significant advantages in applications such as flexible sensors, electronic skins, and conductive devices. This paper aims to provide key guidance for the molecular design, performance modulation, and engineering applications of advanced self-healing materials for next-generation flexible electronics.

Electric double-layer transistors (EDLTs) have attracted considerable attention owing to their ultrahigh interfacial capacitance and low-voltage operation. However, existing models usually rely on idealized ionic assumptions, leaving the influence of non-ideal ionic interactions on device behavior poorly understood. Here, we develop an electrical model for a-IGZO EDLTs that incorporates ionic-size asymmetry (ξ), finite ion-size effects (γ), and short-range correlations (α). This framework enables a unified description of interfacial charge accumulation, voltage partitioning, and transistor characteristics by self-consistently coupling the two EDLs formed within the electrolyte with the electrostatic response of the semiconductor channel. The results show that non-ideal ionic effects regulate device operation by modifying interfacial charge accumulation, electrostatic screening, and voltage partitioning. Specifically, ξ fundamentally alters the voltage partitioning between the two EDL interfaces, while γ determines the onset of steric saturation and limits the maximum attainable interfacial charge density. More importantly, increasing α significantly enhances the interfacial charge density and semiconductor surface potential, yet reduces the drain current by compressing the effective channel-driving potential through nonlinear voltage redistribution. These findings demonstrate that enhanced interfacial charge accumulation does not necessarily translate into improved transistor conduction. The proposed model identifies voltage partitioning as a key mechanism governing electrolyte-gated transistor operation, establishing a direct physical link between microscopic ionic interactions and macroscopic device performance.

Organic memristors are attracting increasing interest due to their potential in low-cost, flexible, and neuromorphic electronics. Despite ongoing research, the underlying switching mechanisms are not yet fully understood and require further systematic investigation. Herein, we present an ITO/PEDOT: PSS (+DMSO+TsOH) (PPDT)/PVA–PEG-H₂SO₄ ion-gel (IG)/Ag-based memristor that uniquely couples capacitive and filamentary switching through deliberate layer engineering. By tailoring active layer thickness, we unlock tunable transitions from capacitive-dominated to filament-assisted conduction, manifested as reversible shifts from nonpinched to pinched hysteresis loops, polarity reversal, and adjustable ON/OFF ratios. This dual-mode behavior is a direct consequence of protonic transport in the ion-gel matrix, which synergistically interacts with Ag⁺-driven filament formation and is stabilized by conductivity-enhanced PEDOT: PSS. Unlike conventional reports, this study integrates a β-controlled hysteresis framework that quantitatively links loop evolution with structural and electrical parameters, providing a unified description that bridges the gap between capacitive and resistive switching in polymer devices. We have also demonstrated (i) control of memristive state, (ii) the establishment of a generalized β-model for hysteresis tuning, and (iii) the fabrication of organic memristors that are stable, repeatable, and cost-effective. These developments elucidate fundamental switching principles and provide a scalable approach for fabricating multifunctional organic memories, making them appealing alternatives for intelligent, adaptable systems, reconfigurable storage, and adaptive computing.

Thermal–tactile sensing is a key capability for robotic perception, enabling temperature estimation and material discrimination during physical interaction. In soft robotic manipulation, the integration of compliant sensing technologies is essential to preserve the intrinsic adaptability of deformable end-effectors while providing meaningful information about the environment and manipulated objects. This requirement calls for sensing materials that combine mechanical compliance with stable thermal transduction and straightforward integration into soft robotic bodies. Here, we report an AC-driven thermal–tactile sensing platform based on eco-friendly ionogel that combines stable ionic sensing, dedicated signal-conditioning electronics, and deployment in robotic manipulation tasks. The ionogel is fabricated through a simple water-based solvent-casting process using natural-derived choline lactate, poly(vinyl alcohol), and poly(vinyl pyrrolidone), yielding a compliant material with temperature–dependent ionic conductivity. Unlike conventional DC-operated ionic sensors, the proposed approach exploits alternating-current excitation to mitigate polarization, ionic accumulation, and electrochemical degradation. A complete sensing unit comprising the ionogel element, compliant electrodes, encapsulation, and portable electronics was developed and characterized. The sensor exhibited reversible thermal responses from –22 to 56 °C, with a theoretical resolution of ∼0.1 °C and pressure cross-sensitivity below ∼0.05 °C/N, while maintaining robust operation under repeated measurements. The sensing platform was integrated into a Pisa/IIT SoftHand mounted on a robotic manipulator. The resulting system successfully performed temperature estimation and material recognition tasks based on thermal conductivity signatures acquired during physical interaction. These results demonstrate how ionic thermal sensing materials can be translated from material-level characterization to system-level robotic perception, providing a sustainable thermal–tactile sensing strategy for soft robotic manipulation.