Physics

Abstract Achieving precise drug delivery to the tumor site can minimize systemic side effects caused by off-target effects. As a therapy that depends on oxygen content, photodynamic therapy (PDT) is significantly constrained by the hypoxic nature of the tumor microenvironment (TME). Compared with the limited efficacy of single PDT, the combination of multiple treatment modalities can achieve synergistic enhancement and superior therapeutic outcomes. Since carbon radical therapy does not rely on oxygen as a reactive substrate, it is mechanistically complementary to oxygen-dependent PDT. In this work, we report a novel strategy for developing a theranostic nanoplatform for long-lasting PDT activated by 1530 nm laser irradiation and glutathione (GSH)-triggered carbon-centered radical synergistic therapy that responds specifically to the TME. This theranostic nanoplatform (UCNPs@WOR:AF@CDC, UWAC) comprises three components: GSH-responsive engineered vesicles (CDC), functionalized metal-organic frameworks (WOR) encapsulating lanthanide upconversion nanoparticles (UCNPs@WOR, UW), and carbon radical prodrugs (ART-Fe, AF). Lanthanide-based upconversion nanoparticles (UCNPs) could upconvert 1530 nm light to 1390 nm for attenuation-minimized second near-infrared (NIR-II) fluorescence imaging and to visible light that serves as the light source for photocatalysis for water oxidation. The 1530 nm light-activated generation of reactive oxygen species (ROS), enhanced by UW-mediated hydrolytic oxygen evolution, works in synergy with the GSH-triggered release of the carbon radical prodrug (AF) to achieve long-lasting therapeutic outcomes. Importantly, it could achieve tumor-specific drug release, triggered by the degradation of the engineered vesicles in response to elevated GSH levels. This work develops a novel theranostic nanoplatform, which could achieve GSH-activated drug delivery, deep-tissue penetration, and a long-lasting therapeutic effect.

Abstract The development of polarization-sensitive photodetectors based on low-dimensional materials with intrinsic lattice anisotropy has paved the way for next-generation polarizer-free and integration-friendly polarization-sensitive optoelectronic devices. Despite their superiority in miniaturization, the relatively low dichroic ratios (DRs) hinder further industrialization. In this work, low-dimensional derivatives of perovskite, quasi-1D yellow-phase (δ-phase) CsPbI3 single nanowires (NWs) are investigated for polarization-sensitive photodetection. Aberration-corrected transmission electron microscopy (TEM) and angle-resolved polarized Raman spectroscopy (ARPRS) reveal the pronounced crystallographic anisotropy of δ-CsPbI3. The pristine δ-CsPbI3 single NW photodetector exhibits a large DR of up to 8.3 under 405 nm illumination. To overcome the limited optoelectronic performance arising from the indirect bandgap nature of δ-CsPbI3, localized surface plasmon resonance (LSPR) is introduced by decorating the δ-CsPbI3 single NW with Au nanoparticles (NPs) via thermal evaporation. The Au-decorated device exhibits up to approximately 9-fold photocurrent enhancement compared with the pristine one, achieving a photoresponsivity (R) of 5.3 mA W–1 and a specific detectivity (D*) of 1.1 × 1010 Jones while retaining the high polarization sensitivity. In addition, the Au-decorated device demonstrates appreciable operational stability under ambient conditions, preserving 92% of its initial photocurrent after 400 switching cycles. This work unveils the great potential of the δ-CsPbI3 single NW for polarized light detection and demonstrates the feasibility of Au NP decoration regarding optoelectronic performance optimization, which can potentially be extended to other low-dimensional perovskite derivatives with analogous quasi-1D chain lattices.

Abstract Achieving sustainable energy conversion hinges on the rational design of oxygen evolution reaction (OER) electrocatalysts that deliver both high efficiency and low cost. Herein, we report a phosphorus-doped iron-cobalt sulfide/molybdenum sulfide heterostructure on nickel foam (P-FeCoS2@MoS2/NF) as an effective OER electrocatalyst in both alkaline freshwater and alkaline seawater. During the sulfurization and phosphorization steps, MoS2 nanosheets are vertically grown on the surface of FeCoS2 nanorods derived from FeCo-layered double hydroxide, forming a heteroatom-P doped core–shell architecture. The core–shell structure prevents the restacking of MoS2 nanosheets and exposes an abundant active surface. The heterointerface induces strong electronic coupling and boosts the active sites to improve the catalytic performance. Experimental characterization confirms the successful formation of the heterostructure and the uniform distribution of phosphorus. Owing to the synergistic effects of a hierarchical structure, the formation of heterointerfaces, and phosphorus doping, P-FeCoS2@MoS2/NF exhibits exceptional OER activity, requiring overpotentials of 220 and 226 mV to reach 10 mA cm–2 in the alkaline electrolyte and alkaline seawater electrolyte, respectively, together with excellent catalytic stability. The low Tafel slope and diminished interfacial charge-transfer resistance in both electrolytes elucidate the rapid reaction kinetics during the OER operation. Post-OER analysis demonstrates the preserved morphology and surface chemistry, underscoring its structural robustness. This work offers a multi-step compositional and structural engineering approach for designing advanced metal sulfide-based heterostructure electrocatalysts for hydrogen production.

Abstract Nonradical peroxymonosulfate (PMS) activation provides a selective route for micropollutant degradation, yet the orbital-level origin of oxidant speciation at single-atom sites remains unclear. Herein, an asymmetric Fe single-atom catalyst (Fe–N3–VN–C) is synthesized via molten-salt-assisted pyrolysis of a zeolitic imidazolate framework precursor, where NaCl etching enriches pyrrolic-N anchors and stabilizes low-coordination Fe centers. Fe–N3–VN–C exhibits efficient degradation of electron-rich micropollutants, exemplified by sulfamethoxazole, over a wide pH range of 3.5–9.5 and in wastewater matrices. The study through quenching experiments and electron paramagnetic resonance spectroscopy indicates singlet oxygen (1O2) as the dominant reactive species, with only minor radical contributions. The density functional theory calculations reveal that asymmetric coordination induces Fe 3d electron delocalization, which reinforces Fe 3d–O 2p coupling, strengthens Fe–O covalency, accelerates interfacial charge transfer, and stabilizes Fe–O intermediates. In addition, adjacent pyrrolic N cooperates with Fe to polarize adsorbed pollutants, forming a dual-site center that promotes selective 1O2 generation. This work establishes Fe 3d electron delocalization as a key electronic origin of nonradical PMS activation and provides a mechanistic basis for designing single-atom catalysts for practical water purification.

Abstract Organic photodetectors (OPDs) are attracting increasing interest as receivers for visible light communication (VLC) systems due to their high sensitivity, low-cost fabrication, and mechanical flexibility. Recent efforts have focused on self-powered OPDs that can simultaneously enable data reception and energy harvesting. Here, we systematically investigate the effect of charge transport layer (CTL) composition on the dynamic performance of self-powered PM6:Y6 OPDs. Frequency response measurements show that devices employing inorganic CTLs deliver a significantly higher 3-dB bandwidth of 1.85 MHz compared to 1.10 MHz for organic CTLs, while OPDs with organic CTLs yield superior photovoltaic efficiency. In VLC demonstrations, OPDs with inorganic CTLs achieve a record usable modulation bandwidth of 52.9 MHz, substantially higher than previously reported values (∼30 MHz). Importantly, these OPDs support a record high-speed data transfer rate of 160 Mbs–1 while simultaneously harvesting 10 mW cm–2 of electrical power. Transient photocurrent and capacitance-voltage (C-V) analyses indicate that the enhanced response speed in inorganic CTL devices arises from faster charge extraction and reduced trap-related charge accumulation. These findings underscore the critical role of CTL selection in advancing self-powered OPDs for integrated high-speed optical communication and energy harvesting.

ABSTRACT Chirality transfer enables molecular asymmetry to propagate from discrete building blocks into hierarchical assemblies, providing a fundamental framework for engineering functional nanostructures. However, conventional supramolecular co‐assembly typically necessitates stoichiometric or excess guest loading to achieve effective chirality transfer, a requirement that often compromises structural fidelity and chiroptical efficiency due to inefficient stereochemical communication. Here, we report a sub‐stoichiometric co‐assembly strategy wherein trace amounts of an achiral modulator (berberine, BBR) cooperatively intercalate within a chiral supramolecular framework (LPF/DPF; left‐/right‐handed phenylalanine‐based gelators) to induce potent chiroptical amplification. We demonstrate that a minimal guest‐to‐host mole ratio of 0.2 is sufficient to capture and amplify host chirality, yielding luminescence dissymmetry factors (| g lum | ≈ 0.08) an order of magnitude higher than those produced by stoichiometric equivalents. Mechanistic investigations reveal that sparse intercalation at this sub‐stoichiometric threshold preserves the underlying hydrogen‐bonded network while enforcing a precise helical registry through synergistic π–π and electrostatic interactions that ensures thermodynamic stability (Δ G °). While stoichiometric excess results in kinetically trapped, non‐helical aggregates, this sub‐stoichiometric control establishes a robust design principle for translating molecular‐scale interactions into high‐performance chiroptical materials with minimal guest loading.

ABSTRACT The vast, unexplored synthesis space of LNMCO cathode materials contains potential solutions to the long‐standing trade‐off between energy density and stability. To navigate this high‐dimensional space, a predictive tool capable of accurately mapping the complex relationships between synthesis parameters and electrochemical performance is essential. Here, a cascaded neural network (CaNN) architecture was designed to simulate the material synthesis workflow. This model synchronously maps 37 process dimensions within the composition‐processing‐structure‐property‐performance (CPSPP) paradigm. By utilizing a cascaded structure, the output of upstream prediction tasks serves as the input for downstream tasks, enabling the capture of hierarchical dependencies that govern material properties. This design choice proved highly effective, achieving superior predictive accuracy with an overall coefficient of determination ( R 2 ) of 0.85. Furthermore, SHAP analysis was integrated to open the model's “black box,” demonstrating a mechanism‐informed approach where predictions align closely with the underlying physical laws of structural inheritance. Experimental validation of nine candidates spanning diverse compositions and synthesis routes confirms the predictive accuracy of the strategy (prediction errors < 10%), establishing a “CaNN modeling → Latin Hypercube Sampling → Wa Screening → Experiments validation” framework for the accelerated discovery of high‐performance cathode materials.

ABSTRACT A stable symbiosis within the microbiome‐host axis is essential for human health. However, preventing microbiome dysbiosis using biomaterials remains challenging due to their unpredictable influence on microbiome evolution. Inspired by the defensive niche of symbiotic mucosa, we have developed a biointerface that forms an engineered mucosa‐inspired dynamic niche to prevent pathogenic dysbiosis. This biointerface features a dynamic zwitterionic network that emulates the mucosa's biophysical defensive functions. Notably, by leveraging its dynamic niche, the biointerface restricts microbial attachment and aggregation, thereby preventing biofilm formation. Comprehensive metagenomic analyses reveal that microbial communities adapt to this biofilm‐preventive dynamic biointerface compositionally and functionally. In particular, Gram‐negative bacteria were relatively reduced, along with decreased abundance of pathways associated with virulence and biofilm formation. Consequently, the mucosa‐inspired biointerface intrinsically prevents the development of pathogenic dysbiosis. This study demonstrates the groundbreaking potential of material‐based niche engineering to guide the ecological shifts of microbial communities from the material scale.

ABSTRACT Mechanical recycling of mixed post‐consumer apolar/polar polymers, due to their mis‐matched polarity and inherent immiscibility, is typically a downcycling process yielding brittle materials. An emerging method that can enhance recycling of such mixtures into dynamically crosslinked, high‐performance thermosets is a dynamic crosslinker (DC) platform; however, current DCs typically require an external catalyst and, due to their insufficiently high peak activation temperature ( T a <190°C), are limited to a subset of applicable polymers and unsuitable for industrial melt‐extrusion processing of high melting temperature ( T m ) polymers. Herein, we report a trifunctional DC incorporating three sought‐after properties: thermally robust pyridotriazole cores as the high‐ T a (245°C) crosslinking sites compatible with reactive extrusion up to 270°C; dynamic siloxane linkages as the robust yet exchangeable bonds; and pyridine/ester functionalities as the internal catalysis sites devoid of external catalysts. Overall, this self‐catalyzed, high‐ T a DC can compatibilize waste plastic mixtures containing high T m polymers and impart the recycled mixtures with superior thermoset properties such as enhanced creep resistance and thermomechanical stability while being melt‐(re)processable.

ABSTRACT Achieving robust underwater adhesion remains challenging due to the interference of interfacial water and insufficient cohesion within conventional adhesives. Inspired by the sandcastle worm's cement forming via liquid–liquid phase separation (LLPS), we developed a novel class of tannic acid/polyethylene glycol/Laponite (TA/PEG/Lap, TPL) composite adhesives to effectively enhance interfacial water repulsion and underwater adhesion. TA and PEG self‐assembled into a dynamic adhesive coacervate matrix via LLPS, while Laponite nanoclays were subsequently introduced as reinforcement fillers and catalysts to trigger polyphenol oxidation, thereby transforming TPL from dynamic soft gel to mechanically robust solid. Specifically, the initially self‐healing TPL can adapt to the irregular surface topography by repelling interfacial water and forming adhesion, thereafter self‐cure to strengthen the mechanical interlocking with irregular substrate surfaces, and eventually realize robust underwater adhesion. Leveraging the transient network reversibility and self‐driven crosslinking stability, the TPL formulations can be processed into injectable, sprayable, coatable, or scaffold forms, offering robust adhesion, fault tolerance, eco‐compatibility, long‐term stability, fire resistance, and antibacterial activity. Overall, this work establishes a paradigm shift in bioinspired design of robust underwater adhesives and highlights the potential of TPL systems for multi‐scenario and multi‐functional applications, including acute hemostasis, soil fixation, infrastructure crack repair, and other underwater sealing tasks.

ABSTRACT Photocatalytic CO 2 reduction (CO 2 RR) involves a cascade of intrinsically coupled processes, rendering the independent optimization of catalytic kinetics and thermodynamics challenging. In this study, we introduce a structural regulation strategy via steric‐driven interlayer slipping engineering of metalloporphyrin‐based covalent organic frameworks (COFs) to decouple and simultaneously optimize the catalytic microenvironment and the spin state of the active metal center. Through regulating the length of alkoxy side‐chains, conventional AA stacking is transformed into a moderately serrated slipped configuration (AA*). Kinetically, the resulting slipped nanochannels enhance local hydrophobicity and spatial confinement, thereby greatly enriching in‐channel CO 2 concentration and suppressing hydrogen evolution. Thermodynamically and electronically, this interlayer slipping reconstructs the ligand field of catalytic Co sites and maximizes vertical π–d exchange interactions. As a result, this triggers a collective spin transition from isolated low‐spin ( S = 1/2) monomers to a high‐spin ( S = 3/2) state, which significantly prolongs charge carrier lifetimes and optimizes the adsorption and activation of the *COOH intermediate. Consequently, the optimized CoP‐COFs deliver a record CO production rate of 71.4 mmol g −1 h −1 with 90% selectivity among porphyrin‐based COF photocatalysts. This work establishes stacking engineering as a versatile strategy for decoupling entangled reaction steps to enable efficient solar fuel production.

ABSTRACT Multimodal physiological monitoring using in‐ear devices is an excellent solution for nonintrusive and noninvasive health monitoring. However, the small size of the ear canal, variation in its morphology in different individuals, and ear wax introduce challenges such as a non‐conformal interface between the sensors and the skin due to the complex ear canal geometry, device fitting issues, biofouling blockage layers, hearing blockage by the device and discomfort. Here, we report a multimodal self‐cleansing, in‐ear nonintrusive and configurable electronic (SCIENCE) device which adapts to various canal geometries and performs active wax cleaning at the sensor‐canal interfaces. Triggered by immersing the sensor in water, the small cylindrical device with a diameter of 2 mm expands once in the ear, and it converts to a spindle shape with a center diameter that can reach 9 mm, thus leading to adaptive contact with the ear canal and forming a stable sensor‐canal interface. The proposed in‐ear device was also endowed with wax cleaning capability to automatically break the biofouling barrier and decrease the sensor‐skin interface impedance by 20%. SCIENCE is integrated with miniaturized circuits and enables simultaneous mobile and wireless recording of electroencephalography (EEG), electrocardiography (ECG), and core body temperature.

ABSTRACT Self‐assembled monolayers (SAMs) have become pivotal hole‐selective layers for efficient inverted perovskite solar cells (PSCs), yet conventional single‐component SAMs suffer from severe intermolecular aggregation, insufficient thermal anchoring, and weak crystallization templating, which severely limit efficiency and operational stability, especially in flexible configurations. Herein, we demonstrate a rationally designed molecular engineering approach for constructing robust buried bottom interfaces via multifunctional SAMs featuring bidentate phosphonic acid anchors, electron‐donating methoxy groups. Such elaborate molecular design enables strengthened interfacial binding, optimized energy‐level alignment, suppressed self‐aggregation, and oriented perovskite crystallization with relieved residual tensile strain. As a result, rigid PSCs achieve a champion efficiency of 27.15% (certified 26.51%), and flexible PSCs exhibit a remarkable efficiency of 25.37% with outstanding mechanical robustness. Moreover, the optimized devices deliver exceptional operational stability, retaining 97.5% of initial performance after 1000 h of continuous operation under ISOS‐L‐2 protocols. This work provides a universal molecular engineering paradigm toward high‐performance and ultra‐stable flexible perovskite photovoltaics via robust buried interface engineering.

ABSTRACT Although vanadium‐based oxides are promising cathodes for aqueous zinc‐ion batteries (AZIBs), their rigid crystalline lattices suffer from sluggish ion diffusion and rapid capacity decay caused by vanadium dissolution. Here, we report an organic‐driven topological amorphization strategy to construct a resilient and kinetically accelerated cathode. Using levamisole hydrochloride (LMS) as a dual‐functional modulator, strong Lewis's acid‐base interactions (V─N/V─S coordination) generate localized tensile stress that progressively disrupts the long‐range periodic lattice. This targeted lattice cleavage transforms crystalline VO 2 into a short‐range ordered amorphous sponge (denoted as L‐VO 2 ‐0.1), while preserving nanoclustered motifs interconnected through flexible organic “hinges”. The resulting topological architecture simultaneously reconciles the stability‐kinetics trade‐off, where the isotropic 3D open framework enables fast, sterically unimpeded Zn 2+ transport with capacitor‐like kinetics, while the dynamic organic hinges efficiently accommodate volume strain and thermodynamically suppress vanadium dissolution. Consequently, the L‐VO 2 ‐0.1 cathode delivers 481.6 mAh g −1 at 0.5 A g −1 and sustains 12 000 cycles at an extreme rate of 20 A g −1 with 83.5% capacity retention. Furthermore, a dual‐cathode pouch cell achieves a commercial‐grade absolute capacity of 1.15 Ah and a high areal capacity of 7.9 mAh cm −2 under a stringent mass loading (>20 mg cm −2 ), enabling feasible routes toward scalable, durable energy storage devices.

ABSTRACT Aerogels have emerged as a unique class of ultralight porous materials that combine exceptional thermal insulation with low density, high porosity, and remarkable structural versatility, enabling broad opportunities across aerospace, energy, electronics, environmental remediation, and wearable technologies. However, their widespread adoption has been constrained by the high cost, limited scalability, and energy‐intensive nature of conventional manufacturing processes, particularly supercritical CO 2 drying. This review highlights recent advances in scalable and cost‐effective aerogel fabrication, including ambient‐pressure drying, templating strategies, top‐down manufacturing, chemical vapor deposition, and solution spinning, which collectively enable enhanced performance while significantly reducing production complexity and cost. We further present a unified perspective on the thermal transport physics of porous materials by systematically discussing the mechanisms of solid conduction, gas conduction, convection, and thermal radiation, and comparing aerogels with other porous architectures such as cellular foams. These fundamental insights establish rational design principles for engineering next‐generation aerogels with tailored thermal functionalities. Finally, we showcase emerging applications that extend well beyond thermal insulation, including moisture‐ and water‐driven energy harvesting, oil–water separation, high‐temperature acoustic insulation, and thermoregulating smart textiles. By bridging scalable manufacturing, fundamental thermal science, and emerging multifunctional applications, this work provides a comprehensive framework for the rational design and commercialization of next‐generation aerogels, paving the way toward their widespread adoption in advanced materials and engineering systems.

ABSTRACT Osteoarthritis (OA) is a multifactorial degenerative joint disease characterized by irreversible cartilage deterioration associated with chronic inflammation, oxidative stress, tissue acidosis, and abnormal mechanical loading. During OA progression, inflammation‐associated metabolic reprogramming and hypoxia‐enhanced glycolysis promote lactate accumulation and local acidosis. OA‐associated acidosis may function as an exacerbating factor within this pathological microenvironment by engaging acid‐sensing pathways and contributing to chondrocyte senescence, apoptosis, and SASP‐associated inflammatory amplification, thereby exacerbating cartilage degeneration. Accordingly, therapeutic strategies that actively neutralize pathological acidity while concurrently modulating inflammatory and oxidative stress cascades may provide a more robust, disease‐modifying approach for OA intervention. Herein, we designed a nanoreactor termed OLDH‐DP@POM by integrating mildly alkaline layered double hydroxide (LDH) nanosheets with active acid‐neutralizing capability and anchoring polyoxometalates (POM) with antioxidant activity, thereby enabling coordinated regulation of pathological acidosis and oxidative stress. Meanwhile, lubrication‐enhancing zwitterionic poly(2‐methacryloyloxyethyl phosphorylcholine) (PMPC) polymer brushes were grafted, endowing the nanoreactor with superior joint lubrication and chondroprotective capability. Both in vitro and in vivo results demonstrated that OLDH‐DP@POM effectively neutralized local acidosis at osteoarthritic lesions, substantially ameliorated synovial inflammation, suppressed Piezo‐mediated mechanotransduction, delayed chondrocyte senescence, and ultimately attenuated cartilage degeneration. Overall, this work provides a promising nanotherapeutic platform for disease‐modifying treatment of OA.

ABSTRACT Circularly polarized organic light‐emitting diodes (CP‐OLEDs) have attracted great attention because of their promising applications in 3D displays. However, developing high‐performance CP‐OLEDs typically face the challenge of integrating large‐scale availability of emitters, device efficiency, color purity, and brightness, especially in the deep‐blue spectral region. Herein, we developed a novel strategy to successfully realize the diastereoselective and gram‐scale synthesis of helically chiral tetradentate Pt(II) complexes with high configurational stabilities through a central chirality adaptively induced helical chirality (CAIH) approach. The bulky central chiral moiety facilitates the suppression of intermolecular interactions and increases the color purity and molecular rigidity. R,M ‐PtCam2 showed a quantum efficiency of 99% and high color purity, with a full‐width at half‐maximum (FWHM) of 19.8 nm. R,M ‐PtCam2/ P ‐PtCam2‐based deep‐blue OLEDs successfully displayed obvious and mirror‐image CP electroluminescence signals. R,M ‐PtCam2 CP‐OLED exhibited a high color purity (FWHM = 24 nm) and a high maximum brightness of up to 51592 cd/m 2 ; moreover, it also achieved a maximum external quantum efficiency (EQE) of 33.2%, along with a record‐high EQE of 30.9% at 1000 cd/m 2 for all reported deep‐blue CP‐OLEDs with CIE y < 0.20. This study provides a molecular design strategy to prepare robust helically chiral Pt(II) emitters for high‐performance deep‐blue phosphorescent CP‐OLEDs.

ABSTRACT Conventional self‐assembled monolayers (SAMs) are conformationally rigid. They cannot buffer interfacial strain during rapid perovskite crystallization, limiting both film quality and device stability. We introduce a conformational engineering strategy using 2‐benzhydrylidene‐succinic acid (BSA), a rigid diphenylmethylene anchor with flexible succinic acid chains to create an elastic buried interface. Atomic simulations show BSA acts as a compressible buffer, delaying stress accumulation by ∼6 Å under displacement. This dynamic strain dissipation improves heterojunction contact and enhances hole extraction and transport. BSA‐modified p‐i‐n devices reach 26.89% (0.045 cm 2 , certified 26.52%). Large‐area modules (22.95 cm 2 ) deliver 24.30% (certified 23.95%), which is among the highest certified values for this area. The devices retain 90% of initial efficiency after 316 h of diurnal cycling and 88% after 300 extreme transient thermal shock cycles from ‐20 °C to 100 °C. This conformational design integrates mechanical compliance with electronic functionality in scalable perovskite photovoltaics.

ABSTRACT Driven by the pursuit of superior therapeutic efficacy and patient autonomy, healthcare is shifting toward proactive “active rehabilitation”. Conductive composite hydrogels, featuring tissue‐mimetic mechanics and multi‐modal sensing capabilities, have emerged as ideal bio‐electronic interfaces for these systems. This review systematically provides a comprehensive overview of hydrogel‐interfaced active rehabilitation systems, progressing from fundamental material design and system architecture to applications. We first outline strategies to enhance hydrogels' biocompatibility, mechanical properties, environmental robustness, self‐adhesion, and conductivity. Next, we delineate the closed‐loop architecture comprising perception, decision, and execution layers, and trace two end‐to‐end demonstrations from ionic‐to‐electronic transduction through algorithmic decoding to physical feedback. Furthermore, we highlight applications in limb motor recovery, swallowing, language, and cognitive rehabilitation, and neural, bone, and tendon regeneration. Finally, we discuss persistent challenges in signal decoupling, material trade‐offs, energy autonomy, and clinical validation, and envision future directions toward AI‐driven personalization, variable‐stiffness hydrogels, self‐powered integration, and standardized benchmarking.

ABSTRACT Intermediate‐valence copper (Cu + ) is essential for preserving C─O bonds during the electrochemical reduction of CO 2 to ethanol, yet its progressive over‐reduction to Cu 0 under operating potentials inevitably dictates C─O bond cleavage and shifts selectivity toward ethylene. Herein, we propose an interfacial dynamic oxygen exchange strategy to stabilize Cu + sites and steer the ethanol reaction pathway. We realize this mechanism by engineering a few‐layer ceria‐coated cuprous oxide (Cu 2 O@CeO 2 ) catalyst featuring an oxygen vacancy‐rich heterointerface (Ce−O V −Cu). Operando spectroscopic measurements and density functional theory calculations reveal that these interfacial oxygen vacancies act as core mediators; by continuously capturing and migrating oxygen species derived from CO 2 , they effectively arrest the reduction of adjacent Cu + siteversuss. Crucially, this dynamic interface dictates the asymmetric C─C coupling of *CH 2 and *CHO, successfully preserving the C−O bond during the subsequent protonation of *CH 2 CHO to *CH 3 CHO. Consequently, the optimized catalyst delivers an outstanding ethanol Faradaic efficiency of 68.5% at −1.1 V versus RHE and exhibits robust operational stability exceeding 150 h, substantially outperforming pristine Cu 2 O. This study establishes vacancy‐mediated dynamic oxygen exchange as a robust strategy for preserving key oxygen‐containing functional groups in highly selective CO 2 ‐to‐ethanol electrosynthesis.

ABSTRACT Conventional artificial vision systems process dynamic scenes inefficiently by reconstructing motion from discrete frames, which requires post‐processing. In contrast, real‐world environments containing multiple moving objects demand sensor‐level discrimination. This work presents a memristive motion‐streak neuron that performs spatiotemporal encoding by integrating an Al/InGaZnO/Al optomemristor with an Ag/HfO 2 /Pt dynamic memristor, whose relaxation dynamics provide temporal memory. In this system, the presence time of moving objects is detected by decay of the output current, allowing motion direction and speed to be directly inferred from the relaxation behavior. The integrated memristor pixel array enables processing of continuous movements and achieves 96.2% classification accuracy for multiple objects. Also, integrating the motion‐streak neuron with the resistor–capacitor kernel further encodes temporal intervals between optical events, enabling recognition of complex movement patterns. This dynamic processing diminishes computational overhead and provides a hardware solution for next‐generation vision systems.

ABSTRACT Achieving compositionally homogeneous mixed‐halide (I − and Br − ) wide‐bandgap (WBG) perovskite films is crucial for high‐performance perovskite/crystalline silicon tandem solar cells (TSCs), yet the disparate crystallization kinetics of iodide‐ and bromide‐rich phases readily induce halide segregation and inhomogeneous elemental distribution, thereby compromising the performance of TSCs. Herein, we employ 3,4,5‐trifluorobenzeneboronic acid (3FBBA) as a multifunctional modulator that synergistically interacts with both organic cations and lead‐halide octahedra via complementary hydrogen‐bonding and coordination interactions, by which 3FBBA fundamentally modulates the formation mechanism of α ‐phase perovskite. It transforms the spontaneous, uncontrolled direct crystallization pathway into a well‐regulated phase‐transition process mediated by highly ordered intermediate phases. These well‐structured intermediates act as well‐defined pre‐structural frameworks to guide the formation of high‐quality α ‐phase perovskite. Benefiting from this strategy, the resultant WBG perovskite films possess enlarged grain size and reduced defect density, which suppress nonradiative recombination loss and accelerate charge transfer kinetics. As a consequence, a single‐junction 1.66 eV WBG perovskite solar cell (PSC) achieves a high‐power conversion efficiency (PCE) of 24.09%, while a two‐terminal perovskite/silicon TSC delivers a champion PCE of 33.6%. Notably, the unencapsulated TSC maintains over 90% of its initial PCE throughout 571 h of continuous maximum power point tracking (MPPT) under ambient atmospheric conditions.

ABSTRACT Efficient wide‐bandgap (WBG) perovskite top cells are essential for high‐performance perovskite/silicon tandem solar cells (TSCs), yet their fabrication in humid ambient air remains difficult because moisture‐ and oxygen‐induced reactions deteriorate film quality and stability. Here, 4‐[[4,6‐bis(octylthio)‐1,3,5‐triazin‐2‐yl]amino]‐2,6‐bis(1,1‐dimethylethyl)‐phenol (BTDP) is introduced into the perovskite precursor to enable WBG perovskite formation under high‐humid ambient air conditions. BTDP scavenges superoxide radical anions, inhibits I − oxidation to I 2 , absorbs ultraviolet light, coordinates with Pb 2+ to regulate crystallization and forms a hydrophobic barrier at surfaces and grain boundaries. With this strategy, blade‐coated WBG perovskite solar cells (PSCs) fabricated at 60% relative humidity deliver a power conversion efficiency (PCE) of 23.45%, which represents the highest PCE reported for air‐processed WBG PSCs with bandgap ≥1.68 eV. Mini‐modules with an aperture area of 14.81 cm 2 reach 20.12% efficiency. Moreover, the method enables ambient‐air fabrication of two‐terminal perovskite/tunnel oxide passivated contact (TOPCon) TSCs with a certified efficiency of 32.59%, among the highest PCEs reported for two‐terminal perovskite/TOPCon TSCs. This study provides a scalable route to efficient, stable single‐junction and tandem perovskite photovoltaics.

ABSTRACT The lack of mechanistic guidelines hinders rational anionic doping in layered oxide cathodes for sodium‐ion batteries (SIBs). Using O3‐type Na(NiFeMn) 1/3 O 2 as a model and combining experiments with density functional theory (DFT) calculations, we reveal that doping effects are governed by two intrinsic dopant properties: valence‐electron configuration and ionic radius. For radius‐matched dopants, electron‐donating F reduces Fe 3 + , enhancing high‐voltage and air stability, whereas electron‐withdrawing N oxidizes Ni 2 + , accelerating degradation. Oversized (Cl, Br) or mismatched (B) dopants cause structural collapse. This dual‐parameter framework enables predictive design of stable, high‐performance cathodes.

ABSTRACT Effective tuning of the Schottky barrier, which determines charge transport across the metal‐semiconductor interface, is essential for optimizing the performance of electronics and optoelectronic devices. However, interfacial disorders and orbital overlap between metals and semiconductors induce Fermi‐level pinning (FLP), making the Schottky barrier height (SBH) largely insensitive to metal work function. Here, we demonstrate that depositing an ultrathin inorganic molecular crystal layer of Sb 2 O 3 between metal and 2D semiconductors can eliminate FLP, enabling highly tunable SBH modulation. Owing to its van der Waals structure, Sb 2 O 3 introduces no excess defects and protects the fragile 2D channel from metal deposition damage, yielding a clean, defect‐free interface. Incorporation of Sb 2 O 3 tunneling layer significantly reduces the SBH in 2D MoS 2 transistors, and the polarity of 2D WSe 2 ‐based FET can be switched from n‐type to p ‐type via adjusting the contact metal work function. The pinning factor turns from −0.11 to around −0.93, approaching the ideal Mott‐Schottky limit. This scalable strategy offers broad applicability in high‐performance 2D electronics.