Physics

DNA strand displacement reactions provide a promising approach for implementing information processing and have been successfully used for encoding combinational logic. However, the construction of circuits with state-dependent behavior and clock-controlled operation remains a significant challenge. In this paper, we present a programmable DNA circuit platform capable of emulating digital sequential logic elements, including a Set-Reset (SR) latch, a clocked Data (D) flip-flop, and a two-bit binary counter. These molecular devices are realized through hierarchically designed DNA strand displacement modules. By encoding temporal information at the domain level and orchestrating reaction cascades on spatially confined DNA modules, we achieve reliable memory storage, clock-gated signal propagation, and input-dependent state transitions. Fluorescence-based kinetic measurements confirm the functional fidelity and timing accuracy of each logic element. Our work establishes a scalable methodology for constructing programmable, state-aware molecular logic systems, advancing the prospects of nanoscale processors and intelligent nanorobots.

The rapid growth of lithium-ion battery (LIB) deployment presents critical challenges in sustainable end-of-life management and raw material recovery. Conventional pyrometallurgical and hydrometallurgical methods suffer from high energy demand, lithium loss, and complex wastewater treatment. This study established a universal, highly efficient, and sustainable hydrothermal route for lithium extraction and material recovery from various spent lithium-ion battery cathodes using 1,2,4,5-benzenetetracarboxylic acid (BTCA). The optimized process achieved over 99% lithium leaching efficiency for lithium iron phosphate (LFP) and LiNi_<i>x</i>Mn_<i>y</i>Co_1-<i>x-</i><i>_y</i>O₂ (NMC), with transition metal coleaching below 1%. It was also broadly applicable to lithium manganese oxide, lithium cobalt oxide, and black mass, achieving 98.5%, 98.95%, and 94.06% leaching efficiencies, respectively. The extracted lithium was directly converted into battery-grade lithium sources, while transition metals were recovered as oxides. Unreacted BTCA was efficiently regenerated and reused without degradation. Electrochemical evaluation confirmed that cathode materials synthesized with recovered lithium exhibit comparable performance to commercial products. Compared to conventional hydrometallurgy, the BTCA-based process increased revenue by over 40% and reduced greenhouse gas emissions by up to 39%. This closed-loop, chemistry-agnostic strategy offered a scalable and economically viable solution for industrial LIB recycling, enabling resource circularity and reducing dependency on primary critical materials.

Next-generation human-machine interfaces and unclonable security systems demand materials that can convert a gentle touch into a bright, readable optical signal. Here, we realize this vision by fabricating a smart interactive terminal that recognizes handwritten digits with 99.35% accuracy and a dynamic anticounterfeiting platform that displays distinct, encrypted information under either optical or mechanical stimuli. The foundation of these breakthroughs is a simple yet powerful thermal activation (TA) strategy we developed for low-cost commercial ZnS/Cu phosphors. This treatment unlocks a five-time increase in mechanoluminescent (ML) brightness, extends afterglow persistence from 30 s to over 20 min, and drastically reduces the activation stress from 2.0 N to a gentle 0.5 N. Mechanistic studies reveal that these dramatic improvements stem from the activation of intrinsic sulfur vacancies within the material. This work not only demonstrates the seamless integration of high-performance ML materials into sophisticated mechano-optoelectronic systems but also provides a strategic reference for transforming commercial materials into key components for future intelligent interactive technologies.

Thrombolytic therapy is limited by rapid enzyme deactivation, off-target bleeding, and inefficient thrombus targeting. Here, we report a DNA-programmed gold nanoparticle (AuNP) platform that enables precise spatial control of tissue plasminogen activator orientation and thrombin-responsive regulation for synergistic thrombolysis and anticoagulation. By fine-tuning the polyA chain length and hybridization density, we identified the poly20A configuration as optimal for maximizing tPA (tissue plasminogen activator) loading and enzymatic accessibility. Embedded tPA exhibited superior stability and activity retention compared with exposed tPA, maintaining a 1.4-fold higher catalytic efficiency and enhanced resistance to PAI-1 inhibition. The thrombin-responsive DNA interface enabled targeted activation at thrombus sites, achieving a dose-dependent thrombolytic response. In vitro and in vivo studies demonstrated potent thrombus dissolution and thrombin inhibition, leading to a 75% reduction in thrombus area, 80% survival rate, and minimal hemorrhagic risk in mouse pulmonary embolism and femoral vein thrombosis models. This dual-function system, combining site-specific thrombin binding and protected tPA delivery, establishes a programmable and modular nanoplatform for precision thrombolysis and anticoagulation, offering a generalizable strategy for targeted vascular nanotherapeutics.

Abstract We investigate the quasinormal modes (QNMs) of a massive scalar field in the background of a regular black hole arising from the proper-time flow in asymptotically safe gravity. This quantum-corrected geometry, characterized by a deformation parameter \( q \), smoothly interpolates between a near-extremal regular black hole and the Schwarzschild solution. Employing both the WKB approximation with Padé resummation and time-domain integration, we compute the complex frequencies for various values of the scalar field mass \( \mu \), multipole number \( \ell \), and deformation parameter \( q \). We observe that the real parts of the QNMs increase with the field mass, while the imaginary parts exhibit behavior indicative of long-lived modes. Although quasi-resonances are not detected in the time-domain profiles due to the dominance of late-time tails, we find that the asymptotic decay follows an oscillatory slowly decaying behavior with the power-law envelope.

Light-driven micro/nanorobots require semiconductor materials with efficient light harvesting and well-defined structural asymmetry to achieve high-performance propulsion. However, most reported systems rely on inorganic semiconductors with rigid band structures and limited stability, while polymeric semiconductors have been restricted by the lack of controllable asymmetric architectures. Here, we report a kinetically programmed one-pot strategy for constructing asymmetric polymeric semiconductor nanorobots with tunable island architectures. By regulating interfacial free energy and competitive nucleation kinetics, mesoporous aminophenol-formaldehyde resin/silica Janus nanoparticles with single-, dual-, and multi-island configurations are precisely synthesized. The resulting asymmetric nanostructures support synergistic light- and fuel-driven self-diffusiophoretic propulsion, allowing programmable motion behaviors. Benefiting from the autonomous motion and photocatalytic activity, the polymeric semiconductor nanorobots exhibit enhanced interaction with bacteria, deep biofilm penetration, and efficient diffusion of reactive oxygen species. This work establishes a general strategy for asymmetric polymeric semiconductor construction and highlights its potential in active antimicrobial and wound-healing nanomedicine.

Multielemental catalysts (MECs) offer broad compositional freedom for tuning catalytic performance, yet practical optimization is often limited by trial-and-error synthesis and testing. Here we implement a transferable, reproducible closed-loop discovery workflow on a fully commercial robotic automation stack and couple it with machine-learning-guided optimization to accelerate MEC development for tetracycline degradation in a peroxymonosulfate (PMS)-based Fenton-like system. An adaptive-learning genetic algorithm (GA) was used to design an initial campaign of 144 MECs to train a multilayer perceptron (MLP) surrogate model. The GA-MLP closed loop then proposed and experimentally validated 25 additional candidates, identifying four high-performing MECs and increasing tetracycline degradation efficiency from ∼78% in the initial data set to 93% for the best catalyst. To substantiate the executability and reproducibility of the digital recipe, inductively coupled plasma optical emission spectrometry confirmed that recommended precursor ratios were translated into measured catalyst compositions with minor deviations, and catalysts prepared robotically and manually under identical protocols exhibited consistent degradation performance. Finally, SHapley Additive exPlanations (SHAP) analysis enabled model interpretation and revealed nonlinear composition-performance contributions, providing quantitative guidance for metal fraction and promoter loading windows. This work demonstrates a reproducible, automation-ready strategy for sample-efficient optimization of multielement catalysts for advanced oxidation processes in environmental applications.

Controlling the surface chemistry of biobased nanomaterials is crucial for unlocking their full potential in advanced applications. However, the impact of such chemical modifications on nanoscale morphology remains poorly understood. In this work, we investigate the sequential deacetylation of chitin nanocrystals (ChNCs) into chitosan nanocrystals (ChsNCs), a transformation that significantly alters their ultrastructural properties through the introduction of amine functionalities. By combining bulk and nanoscale characterization techniques─including electron diffraction, cryo-transmission electron microscopy (cryoTEM), and scattering-type scanning near-field optical microscopy (s-SNOM)─we can track the chemical and structural evolution during the deacetylation process. Our findings demonstrate that partially deacetylated ChNCs (20-60% degree of deacetylation) exhibit chitosan-rich surface patches, revealing nanoscale heterogeneity in surface modification. Furthermore, we observed that such a patchy distribution is accompanied by a decrease in nanocrystal bundling, suggesting changes in interparticle interactions. Finally, at higher degrees of deacetylation, ChsNCs exhibit mobile chitosan chains surrounding cores composed of chitosan-rich or residual chitin regions. We believe that our results provide critical insights into the nanostructural identity of ChsNCs, with implications for understanding and tuning their structure-property-function relationships, which are critical for the fabrication of chitin-derived biomaterials.

Magic-sized clusters (MSCs) represent the missing molecular link between precursors and colloidal semiconductor nanocrystals; yet their synthetic fragility and limited compositional scope have hindered systematic exploration. Stoichiometric MSCs with precise metal-chalcogen parity are particularly elusive, restricting access to well-defined families and their emergent functions. Here, we report the synthesis of Mn²⁺-doped (CdS)₁₃ MSCs (denoted as Mn²⁺:(CdS)₁₃) and their directed self-assembly into suprastructures (SSs) featuring a distinct nanohexagonal morphology. Comprehensive optical spectroscopic and mass spectrometric analyses confirm that the MSCs retain their atomically precise (CdS)₁₃ frameworks within the SSs. The ordered assembly markedly enhances orange photoluminescence, yielding quantum efficiencies up to 57% through the reduction of surface defect states. Extending this strategy, we synthesize SSs based on alloy Mn²⁺:(Zn_<i>x</i>Cd_1-<i>x</i>S)₁₃ clusters, enabling atomic-level control of composition. These cluster-assembled materials serve as highly active photocatalysts for solar-driven hydrogen evolution, with alloyed systems reaching rates of ∼100 mmol g^-1 h^-1 and exhibiting up to 3.5-fold enhancement over unalloyed analogues due to atomic-level synergistic effects. This work establishes a general platform for generating doped and alloyed stoichiometric MSCs and demonstrates how the hierarchical assembly of atomically precise clusters can unlock emergent photophysical and catalytic properties.

Charge interactions at the sensing interface are pivotal for efficient signal transduction. However, in biofluids, charge screening and nonspecific adsorption induced by counterions and biomolecules can negatively affect the signal transduction between the interface and electrode. In this work, we demonstrate that counterion screening and nonspecific adsorption can be mitigated by regulating the surface charge density and composition of the sensing interface, thereby improving signal transduction performance. We constructed an interfacial model with an adjustable surface charge based on a hybrid phospholipid monolayer (HPM) to investigate the interactions between interfacial charge distribution, counterion screening, and nonspecific adsorption. The signal transduction capacity of the sensing interface was enhanced by doping unsaturated long-chain molecules within the HPM. Molecular dynamics simulations and density-functional theory calculations confirmed that an appropriate surface charge density and the doping of conjugated molecules are crucial for efficient signal transduction. We applied this sensing interface for the highly sensitive detection of myocardial injury biomarkers (MIBs), achieving a detection limit (LoD) as low as 0.92 pg/mL. Our findings reveal the underlying mechanism of efficient signal transduction at the sensing interface, highlighting the relationships between the interface composition and performance in electrical biosensing.

Magic-size metal chalcogenide clusters of molecular size exhibit well-defined structure and unique properties that might be further expanded with the incorporation or substitution of a second metal. We report the postmodification of magic-size clusters synthesized in polymer thin films via exposure to volatile metal organic precursors commonly utilized for atomic layer deposition. Exposure of In₆S₆(CH₃)₆ clusters to dimethylcadmium results in exposure-dependent incorporation of Cd²⁺, which extends the optical absorbance of the clusters into the visible spectrum. The mechanism for Cd²⁺ incorporation is consistent with Cd²⁺ replacement of In³⁺ that includes methyl ligand removal to maintain charge neutrality. Even for clusters embedded in a polymer matrix, ligand loss leads to sintering and transformation into larger nanoscale aggregates with zinc blende-type structure. The extent of Cd incorporation can be modulated by varying the process temperature and volatile metal organic exposure as well as the choice of volatile metal organic precursor. A computational thermodynamic analysis of heteroatom incorporation for several metals and chemistries reveals that both the stability of the substituted cluster and the favorability of reaction byproducts jointly determine the favorability of cation incorporation.

Spinal cord injury (SCI) is a devastating trauma to the central nervous system, causing permanent functional nerve defects. A key therapeutic challenge is the inhibition of the secondary injury cascade, specifically the progressive neural damage from iron overload-induced ferroptosis and oxidative stress. To target these dual mechanisms, we developed a dual-functional, iron-scavenging, and hydrogen-releasing microneedle patch (MN/MON@AB) composed of ammonia borane (AB)-loaded, amino-functionalized mesoporous organosilica nanoparticles (MON-NH₂) embedded in a biodegradable silk fibroin array. This system functions via a dual-target mechanism: amino groups chelate excess iron ions to suppress the Fenton reaction, while AB provides sustained release of molecular hydrogen (H₂) in the acidic injury microenvironment to neutralize reactive oxygen species (ROS). MN/MON@AB has been found to reduce the intracellular Fe²⁺ levels by 46.7%, nearly doubling the expression of the key ferroptosis regulator GPX4, and largely alleviating lipid peroxidation <i>in vitro</i>. In a murine SCI model, the patch significantly reduced spinal iron deposition (<i>p</i> < 0.0001) and promoted marked locomotor recovery (<i>p</i> < 0.001). Featuring combined localized iron chelation and sustained antioxidant delivery, the present strategy offers a broadly applicable and pioneering therapeutic platform for treating acute neural injuries and subsequent neurodegenerative processes.

High-performance thermal regulators are essential for human survival in cold environments. However, conventional fibrous materials suffer from large diameters and low porosity, resulting in heavy weight and limited insulation. While aerogels are renowned for their low density and high porosity, their brittleness and poor mechanical properties severely hinder practical application. Herein, a porous-core/dense-shell nanofiber inspired by polar bear hair is engineered for multimodal thermal regulation via coaxial electrospinning based on fast-slow phase separation. Controlling polymer-solvent-water interactions within the coaxial jet induces rapid phase separation in the core and delayed phase separation in the shell, yielding porous-core/dense-shell nanofibers that self-assemble into aerogels (CSNA). The core/shell nanofibers and bonding networks endow CSNA with mechanical robustness, withstanding 20,000 times its weight without fracture. Meanwhile, the polar-bear-hair-inspired structure, featuring nanoscale fiber diameter, small pore size, and high porosity, synergistically achieves an ultralight density (5.5 mg cm^-3) and low thermal conductivity (26.45 mW m^-1 K^-1), enabling warmth retention that matches down at one-third the thickness. Furthermore, carbon-black-doped CSNA exhibits efficient Joule heating and photothermal conversion, enabling on-demand switching between passive and active warming modes under cold conditions. This strategy offers a promising approach for fabricating high-strength nanofibrous aerogels, showing great potential for next-generation thermal-regulation textiles.

Ultrasmall fluorescent core-shell nanoparticles (NPs) with a silica core and poly(ethylene glycol) ligand shell are the earliest example of hybrid NPs that have received U.S. investigational new drug FDA approval. They are among only a few inorganic NPs translated to safety, diagnostic, and therapeutic human clinical trials. Despite these achievements, little is known about the exact structure of their 3-4 nm sized silica cores. We report the surprising discovery of a well-defined pentagonal bipyramidal core structure preferentially formed in the aqueous synthesis built from seven primary silica NPs. A combination of reverse-phase high-performance liquid chromatography, cryogenic transmission electron microscopy, and coarse-grained simulations provides fundamental insights into this magic-size cluster formation and its unusual stability. Results rationalize the successful NP synthesis scale-up from 1 mL to 50 L, provide clues to the recent discovery of their self-therapeutic properties in oncology via ferroptosis, an iron-dependent cell death mechanism, and promise improved control of particle size distribution via chromatographic separations.

Inadequate control over particle size and intermediate adsorption leads to low active site density and sluggish reaction kinetics, which remain critical challenges for the development of high-performance nanozymes. Here, we report a one-pot strategy that simultaneously enables IrO_<i>x</i> nucleation, metal organic framework (MOF) formation, and cobalt (Co) doping, thus constructing in situ confined Co-doped IrO_<i>x</i> (CoIrO_<i>x</i>) cluster complexes within MOFs (denoted as CoIrO_<i>x</i>/CoIr-MOFs). Systematic characterization revealed that MOF nanosheets grown on the preferentially nucleated CoIrO_<i>x</i> surface inhibit their excessive growth and aggregation, ultimately confining ultrafine CoIrO_<i>x</i> uniformly within the interlayer regions and forming tight interfaces. Moreover, Co doping into the IrO_<i>x</i> lattice weakens the adsorption energy of the OH* intermediates, thereby reducing the overpotential for oxygen reduction and the energy barrier of the rate-determining step. Concurrently, it enhances the substrate affinity of the catalytic sites. The as-prepared CoIrO_<i>x</i>/CoIr-MOFs can directly catalyze oxygen or hydrogen peroxide to generate reactive oxygen species (ROS), exhibiting multienzymes (oxidase, peroxidase, and laccase) like activities that enable different signal transduction. As a proof of concept for the rational design of the nanozyme, CoIrO_<i>x</i>/CoIr-MOFs constructed a triple-modal sensing platform. Its highly efficient detection performance for glutathione (GSH) stems from the excellent catalytic properties of CoIrO_<i>x</i>/CoIr-MOFs under the synergistic regulation of in situ confinement and Co doping. This work provides a foundational design strategy for metal oxide/MOF heterostructures with excellent catalytic performance and supports the further applications of advanced nanozyme in catalysis and biosensing.

Photoinduced hot electrons are central to plasmon-driven catalysis. Atomically thin Ti₃C₂O₂, with high carrier density and broad optical absorption, offers a promising platform for plasmon-driven reactions. However, comprehensive investigations of its plasmon resonance, hot-carrier generation, and plasmonic catalytic performance remain limited. In this work, real-time time-dependent density functional theory (rt-TDDFT) was employed to study Ti₃C₂O₂'s plasmon excitation and hot-carrier generation from nonradiative plasmon damping. The temporal evolution of the dipole moment reveals plasmon resonance in Ti₃C₂O₂, followed by strong plasmon damping that redistributes the stored energy to generate hot carriers. Ti₃C₂O₂ with low oxygen vacancy concentration (O_v-Ti₃C₂O₂) exhibits plasmonic behavior resembling the pristine surface, and the plasmon-generated hot electrons can markedly reduce the dissociation barrier of CO₂ at the oxygen vacancy. These findings provide fundamental insights into the plasmonic properties of Ti₃C₂O₂ and how they drive its catalytic performance in surface reactions, which is valuable for advancing plasmon-driven catalysis.

Multibridge channel field-effect transistors (MBC-FETs) based on two-dimensional (2D) semiconductors emerge as promising candidates for achieving the ultimate scaling of transistors at advanced technology nodes. Here, the MBC-FETs based on 2D group IV-VI materials are designed by vertically stacking multiple conductive channels and gate electrodes. Concurrently, the operational mechanism underlying the device's tailored transport behaviors is comprehensively analyzed by integrating the characterizations of potential difference, local device density of states, transmission spectra, and projected device density of states. The double-gate double-channel MBC-FETs with 96.2 mV/dec subthreshold swing (SS) achieve YES, NAND, and NOR logic operations via precise electrode doping concentration control and programmable bias voltage. Moreover, the triple-gate double-channel MBC-FETs (SS = 81 mV/dec) enable the implementation of Y = A̅, NAND, and Y = B̅ logic operations. This work paves the way for developing MBC-FETs-based multifunctional logic devices for next-generation integrated circuits and continuing Moore's Law.

Chirality plays an essential role in emergent quantum phenomena owing to its interplay with spin and photon degrees of freedom. In this work, a pair of chiral enantiomeric cocrystals were fabricated, where right-handed and left-handed cocrystals present significantly different spin polarization. The distinct chiral lattice structure predominantly accounts for the observed variations in magnetization; only the right-handed cocrystal undergoes a chiral inversion upon cooling. Due to the temperature-triggered chiral lattice structural phase transition, spin polarization of the right-handed cocrystal increases nonlinearly and rapidly with decreasing temperature. Moreover, the spin degeneracy lifting induced by the chiral lattice is also affected by chiral inversion, leading to a mirror response in the magnetic field control of circularly polarized transmittance. In addition, the phase transition temperature of the chiral lattice can be effectively tuned by circularly polarized light. Overall, this study provides deeper insight into the dynamic chiral lattice dependent spin and optics in homochiral cocrystals.

Late-stage hydrogen isotope exchange and dearomatization reactions under D₂ have recently been used for preparing labeled compounds using metal nanoparticle catalysts. In the case of dearomatization, lower rates are usually observed under D₂ compared to H₂ as a result of a kinetic isotope effect. Here, we report the synthesis of NHC-stabilized PdNPs, their characterization, and their use for the reduction of 2-phenylpyridine to 2-phenylpiperidine or 2-phenylpiperidine-<i>d</i>₆, which reveals an unexpected preference for D₂ over H₂. This effect is observed using NPs stabilized by polyvinylpyrrolidone (Pd@PVP) but is more pronounced in the presence of NHC ligands (Pd@NHC). DFT calculations reveal that the phenomenon arises from a higher surface concentration of deuterides relative to hydrides in both systems, which is enhanced by the electronic influence of NHC ligands. This study provides the first report and mechanistic insight into an unusual isotopic effect in NP-catalyzed deuteration, highlighting the pivotal role of ligand-NP interactions.

Dimensionality fundamentally dictates the behavior of quantum systems, and dimensional crossover serves as a key bridge to understand the pronounced differences between distinct dimensional regimes. However, achieving continuous control over such a crossover within a real material remains challenging. Here, we demonstrate a gate-tunable dimensional crossover of quantum confined Dirac Fermions in graphene/transition metal dichalcogenide heterostructure quantum dots (QDs). By adjusting the electrostatic gate, we modulate the potential depth of an elongated QD, which exhibits distinct confinement sizes along two perpendicular directions, thereby enabling precise tuning of the confined carrier wavelength with respect to these two distinct size dimensions. Scanning tunneling microscopy measurements reveal a clear evolution from one-dimensional confinement, characterized by strongly anisotropic wave function distributions, to two-dimensional behavior. This establishes a direct and tunable means to control dimensional crossover in situ via electrostatic gating, providing a new platform for exploring dimension-driven quantum phenomena.

Reliable, low-resistance contacts remain a central bottleneck in two-dimensional (2D) semiconductor devices, where Fermi-level pinning (FLP) at metal-semiconductor interfaces limits carrier injection and masks intrinsic transport. Here, we demonstrate that metallic van der Waals (vdW) contacts based on transferred NbSe₂ enable near-ideal p-type operation in WSe₂ field-effect transistors. Devices with NbSe₂ contacts exhibit clear p-type characteristics, ohmic behavior, and high on/off ratios, in contrast to conventional high-work-function metal contacts. Temperature-dependent measurements reveal a reduced Schottky barrier height of ∼0.06 eV, compared to ∼0.26 eV for Pt contacts. Four-point-probe measurements confirm a low contact resistance and channel-dominated transport, evidencing efficient carrier injection across the vdW interface. Furthermore, a dopant-free complementary metal-oxide-semiconductor (CMOS) inverter is realized by integrating p-type NbSe₂ and n-type Sb contacts on WSe₂. These results establish metallic vdW contacts as an effective strategy to suppress FLP and enable high-performance 2D electronics.

Strain engineering, as a key strategy for regulating two-dimensional (2D) material anisotropy, has demonstrated remarkable effectiveness in band engineering. However, systematic investigations of the third-order nonlinear-optical (NLO) response of low-symmetry materials under strain fields still pose a significant challenge. This study combines experimental and theoretical approaches to reveal for the first time the extreme sensitivity of third-harmonic generation (THG) anisotropy in quasi-one-dimensional-layered TiS₃ to uniaxial strain. Due to the anisotropic reconstruction of interband transition dipole moment, the THG anisotropy ratio reaches 316.90 ± 7.93 under 7.25% <i>a</i>-axis strain, which is the largest reported in 2D materials, to our best knowledge. Based on the excellent third-order nonlinear anisotropy and strain regulation characteristics of TiS₃, an all-optical Boolean logic gate based on NLO intensity encoding was further constructed. This work not only elucidates the strain-NLO coupling mechanism but also proposes a tunable nonlinear all-optical device based on anisotropic 2D materials.

Non-electrochemical lithium (Li) permeation into solid-state electrolytes (SSEs) poses a latent yet critical failure mode for all-solid-state lithium metal batteries (ASSLMBs). This work reveals severe Li self-permeation in the Li₃N SSE under pressure and heat, forming mixed conductive regions that undermine interfacial stability. To address this problem, we developed an anion-tuning strategy by doping Li₃N with LiF to obtain Li_2.9N_0.95F_0.05. Fluorine substitution elevates the interfacial energy between Li and SSE, effectively suppressing spontaneous Li permeation. Li_2.9N_0.95F_0.05 exhibits high ionic conductivity (5.8 × 10^-4 S cm^-1) and low activation energy (0.326 eV). Consequently, Li-symmetric cells achieve stable cycling for >1000 h at 0.2 mA cm^-2, and the ASSLMB employing Li_2.9N_0.95F_0.05 as SSE interlayers and LiCoO₂ cathodes retain 80% capacity after 120 cycles at 0.5 C, demonstrating engineering viability. This study provides an effective pathway to stabilize Li metal interfaces and advance the performance of ASSLMBs.

The activity-stability trade-off for IrO₂ constrains the development of proton exchange membrane water electrolyzers (PEMWEs). Conventionally, high IrO₂ crystallinity ensures oxygen evolution reaction (OER) stability while compromising activity, while amorphous structure offers high OER activity while sacrificing durability. Herein, we develop a kinetically constrained amorphization strategy using high-temperature thermal shock to precisely tune IrO₂ crystallinity, capturing an ideal intermediate state: low-crystallinity IrO₂ (LC-IrO₂). LC-IrO₂ merges the high activity of amorphous IrO₂ derived from the short-range order and the robust stability of crystalline IrO₂ with structural rigidity. Consequently, the LC-IrO₂ catalyst simultaneously achieves excellent catalytic activity and stability for acidic OER. A PEMWE using a LC-IrO₂ anode requires only 1.69 V to reach 1 A cm^-2 at 60 °C and maintains steady operation for 500 h with a negligible degradation rate. This study demonstrates kinetic crystallinity control as a new paradigm for electrocatalyst design.