Physics

Monolithic three-dimensional (M3D) integration is a promising solution for next-generation integrated circuits, offering enhanced signal propagation, high integration density, and lower fabrication costs than planar architectures. Amorphous oxide semiconductors, with room-temperature deposition capability and large-scale uniformity, are well-suited for 3D applications, yet developing multitier high-performance oxide transistors compatible with traditional technologies remains challenging. Here, we present a threshold voltage modulation strategy for indium gallium zinc oxide (IGZO) transistors via channel thickness control and atomic-layer-deposited surface modification. A four-tier vertically stacked IGZO transistor array has been manufactured with sequential layer-by-layer integration; optimized transistors across the tiers exhibited a low subthreshold swing of 150 mV/dec and an on/off ratio exceeding 10 8 . Combined with via-hole interconnects, we demonstrated functional computing-in-memory 3D circuits featuring inverter modules (tier 1–2) and dynamic random access memory (DRAM) components (tier 3–4). The work advances oxide semiconductors’ applications in future advanced 3D circuits.

Metallic nanoparticles (NPs) enhance radiotherapy through photoelectric absorption and Auger electron cascades, yet the effective spatial range over which these low-energy electrons induce biological damage remains poorly defined. Quantifying nanoscale energy deposition is essential for rational therapeutic design and safe clinical translation. Here, we establish a self-assembled polyelectrolyte-nanoparticle-cell architecture enabling nanometer-precision control of NP-cell separation (25–100 nm) to directly probe distance-dependent radiation enhancement. Layer-by-layer assembly produced uniform interfaces confirmed by spectroscopy, ellipsometry, electron microscopy, atomic force microscopy, and microgravimetry. Using human microglial (HMC3) and diffuse intrinsic pontine glioma (SU-DIPG-IV) cells, we quantified intracellular reactive oxygen species generation and γH2AX-marked DNA double-strand breaks following 137 Cs γ-irradiation. Cells positioned 25.9 nm from the NP layer exhibited significantly increased DNA damage relative to NP-free controls, whereas damage progressively decreased with increasing separation, yielding a 250% differential effect between 25.9 and 97.5 nm. Modality-dependent attenuation profiles were observed across γ-ray, X-ray, and electron irradiation. These findings define the effective nanoscale interaction radius governing NP-mediated Auger enhancement and establish a technique for the interrogation of light–matter interactions for therapeutic energy deposition.

Pb–Sn mixed perovskites with an optimal bandgap of ∼1.25 eV are essential for high-efficiency all-perovskite tandem solar cells. However, the facile oxidation of Sn 2+ leads to detrimental Sn 4+ defects that cause severe nonradiative recombination and rapid degradation, hindering their commercialization. Here, we demonstrate a halide exchange strategy using inert metal chlorides (MnCl 2 /ZnCl 2 ) to simultaneously reduce the Sn 4+ concentration and form an inorganic protective layer in Pb–Sn perovskite solar cells (PSCs). The metal chlorides react with SnI 4 via ligand substitution, producing volatile SnCl 4, which reduces Sn 4+ concentrations, while forming MnI 2 /ZnI 2 passivation layers at the grain boundaries. In addition, the post-treatment induces partial dissolution-recrystallization, which enlarges the grain size and reduces residual stress. Furthermore, the inorganic passivation layer optimizes the energy-level alignment at the perovskite surface, facilitating carrier separation and extraction. As a result, the champion ZnCl 2 -modified device achieves a high power conversion efficiency (PCE) of 23.06% with an open-circuit voltage of 0.87 V and retains 90% of its initial PCE after 1000 h of continuous illumination in N 2 . This work establishes a novel inert metal chloride post-treatment strategy and elucidates the underlying reaction mechanisms in Pb–Sn mixed perovskites, thereby opening new avenues for developing highly efficient and stable tandem devices.

Despite extensive progress in iron-based superconductors, how interlayer coupling affects superconductivity remains a key unresolved issue. Here, using angle-resolved photoemission spectroscopy, we successfully resolve the electronic structure of a surface-decoupled FeAs monolayer in KCa 2 Fe 4 As 4 F 2, a rare example in iron pnictides. This allows for a direct, side-by-side comparison between the basic FeAs unit and its bulk bilayer counterpart within a single sample. Two distinct superconducting phases are identified: a bulk bilayer phase with Tc ∼ 34 K and a surface-decoupled monolayer phase with a smaller gap vanishing at ∼18 K. In addition to probable enhanced fluctuations in single-layer FeAs, we propose that this Tc difference may originate from either interfacial effect, such as phonon-mediated assistance from the CaF layers or electronic interlayer hopping within the bilayer unit. Our work offers a refined framework for understanding the superconductivity in multilayer iron-based superconductors.

ABSTRACT Checkpoint immunotherapy shows great promise to treat malignancies by reinvigorating immune cells and activating antitumor immune response. However, traditional checkpoint inhibitors suffer from low response rates, poor tumor‐targeting efficiency, and drug resistance. We herein report a self‐assembled lysosome targeting chimera nanoplatform (nano‐SALTAC) with cancer‐specific endocytic receptor‐driven protein degradation for activatable checkpoint cancer photo‐immunotherapy. This nano‐SALTAC is self‐assembled from two chimeric peptides, CP LDLR , and CP PD‐L1 , which consist of the photosensitizer (protoporphyrin IX, PpIX), the cathepsin B (CatB)‐cleavable substrate, the GSGS linker, and the low‐density lipoprotein receptor (LDLR)‐/programmed cell death ligand 1 (PD‐L1)‐targeting peptides. After systemic administration, nano‐SALTAC passively targets tumor cells, drives efficient cell internalization, and induces subsequent lysosome degradation of PD‐L1 via cancer‐specific endocytic receptor LDLR. Notably, the PD‐L1 degradation efficiency is optimizable via adjusting the self‐assembly ratio of CP LDLR /CP PD‐L1 . The cancer‐overexpressed CatB further induces the disassociation of nano‐SALTAC to release the photosensitizer fragment. Under localized photoirradiation, nano‐SALTAC generates 1 O 2 to induce immunogenic cell death, thereby synergizing with PD‐L1 degradation to boost antitumor immune responses and inhibit tumor growth. Thus, such a self‐assembled LYTAC strategy provides an easily formulated nanoplatform capable of improving cancer specificity and optimizing protein degradation efficiency for cancer therapy.

ABSTRACT Accurate spectral analysis in compact platforms is essential for portable sensing, integrated photonics, and on‐chip materials characterization. Single‐detector computational spectrometers offer an appealing route toward extreme miniaturization, but their performance is fundamentally constrained by the intrinsic structure of bias‐dependent responsivity curves: these responses evolve smoothly and non‐orthogonally with wavelength, producing highly correlated photocurrent patterns that collapse the effective rank of the responsivity matrix. Such low‐rank encoding leads to ill‐conditioned inverse problems, making the reconstruction of multi‐peak or densely spaced spectra particularly fragile to noise and device imperfections. Here, we overcome this long‐standing limitation by introducing gate‐tunable band‐profile modulation in an in‐plane dual‐bottom‐gate black phosphorus photodetector. Independent gate control forms a reconfigurable local potential barrier that generates strongly wavelength‐dependent photocurrent maps, substantially enhancing spectral discriminability and improving the effective rank and numerical conditioning of the responsivity matrix. Leveraging this encoding mechanism, a single detector enables high‐accuracy single‐peak identification over a 500‐nm near‐infrared band and reliable one‐to‐eight‐peak reconstruction within a calibrated window. We further demonstrate robust graphene layer‐number identification, including regimes where Raman spectroscopy becomes ambiguous. This work establishes band‐profile engineering as a general device‐level strategy for advancing single‐detector computational spectrometers and enabling compact, high‐fidelity spectral sensing.

ABSTRACT Purely organic room‐temperature phosphorescence (RTP) materials based on four‐coordinated boron are predominantly centered on the boron difluoride (BF 2 ) unit, leveraging its strong rigidification effect. Herein, a diphenylboron (BPh 2 ) and heavy‐atom synergistic strategy, constructing a BF 2 ‐free four‐coordinated boron RTP material (PMB‐Br), is presented. The introduction of the bromine atom endows the powder samples with green phosphorescence featuring a lifetime of 1.72 ms. Theoretical calculations reveal that the bromine atom intramolecularly enhances the key spin‐orbit coupling (SOC) constant to 16.13 cm −1 , providing the core driving force for efficient intersystem crossing; simultaneously, it intermolecularly cooperates with BPh 2 to construct a rigid network that stabilizes the excitons. A comparison with the isostructural BF 2 analogue (PMB‐BF 2 , SOC of merely 0.63 cm −1 ) demonstrates that the BPh 2 unit, due to its ability to induce an S 1 (CT)/T 2 (CT+LE) excited‐state configuration, possesses a more pronounced synergy with the heavy‐atom effect to enhance SOC. Based on this, a complementary dual‐pathway model for four‐coordinated boron RTP is tentatively proposed. Alongside the rigidification‐predominated BF 2 ‐based strategy, the BPh 2 pathway exemplifies a potential complementary SOC–predominated strategy, providing a new perspective for the future exploration beyond the established BF 2 ‐centric design paradigm.

ABSTRACT Photocatalytic technology stands as a pivotal avenue for addressing global energy and environmental challenges, but its practical use is hindered by insufficient efficiency and unclear mechanisms of reaction active sites. Emerging research has unveiled that upon exposure to light, photocatalysts undergo in situ structural evolutions, including light‐driven structural construction, real‐time reconstruction of structures and active sites during catalysis, and unavoidable photoinduced destruction. These phenomena are intimately linked to the generation, transformation, and deactivation of active sites. A comprehensive understanding of these light‐induced structural evolutions is indispensable for the rational design of high‐performance photocatalytic systems, but a holistic review synthesizing structural and active site transformations remains lacking. This review aims to bridge this gap by systematically summarizing recent research progress, including the impact of light on structure and catalytic sites throughout the lifecycle of photocatalysts, strategies for regulating structural evolution processes, related characterization and calculation methods. Finally, challenges and prospects in the research of photocatalysts are proposed, and some insights for improving photocatalytic efficiency and practical applications are provided. This review is the first to propose a unified framework linking photoexcitation, structural evolution, dynamic active sites and performance improvement, aiming to upgrade photocatalysis research from static material screening to dynamic system engineering.

ABSTRACT Carbon coating is a key strategy to enhance electron transport for polyanionic cathode materials. However, current carbon‐coating methods face challenges in simultaneously achieving ultrathin, continuous, and highly conductive coatings with low carbon content, to enable efficient coupled ion–electron transport. As for Na 4 Fe 3 (PO 4 ) 2 P 2 O 7 (NFPP), it still suffers from the above issues, limiting its electrochemical performance and industrial application. Commercial atomic layer deposition (ALD) technology is highly precise but unsuitable for carbon coatings and requires costly specialized equipment. Here, a precursor‐induced quasi‐ALD carbon deposition strategy is proposed to fabricate high‐power, stable NFPP@C‐FAC cathodes, using molecular‐level coupling of Fe and C sources. The obtained carbon matrix exhibits an ultrathin, uniform coating with an ultra‐low carbon content of 1.5% and few defects. These properties increase the electronic conductivity and the interfacial Na + diffusion kinetics, thereby improving the coupled ion–electron transport, as confirmed by DFT calculations. NFPP@C‐FAC demonstrates excellent rate performance (58 mAh g −1 at 200 C) and exceptional cycling stability, with 83.2% capacity retention after 20 000 cycles at 20 C. Moreover, NFPP@C‐FAC exhibits superior performance over a wide temperature range, which shows 90% capacity retention at −20°C compared to room temperature, with a single‐phase solid‐solution reaction mechanism confirmed by in situ XRD.

ABSTRACT The nonvolatile control of magnetic structures in 2D ferromagnets is essential for advancing spintronics. Here, gate‐tunable lithium intercalation is demonstrated as an effective strategy for modulating the magnetic properties of Fe 3 GaTe 2 in a pronounced thickness‐dependent manner. In flakes thicker than 27 nm, partial Li intercalation induces a functional ferromagnetic–antiferromagnetic vertical heterostructure, evidenced by an enhanced coercive field and a giant exchange bias of ∼0.31 T. Conversely, in flakes thinner than 20 nm, full Li penetration leads to a mixed‐phase transition, resulting in reduced coercivity and no exchange bias is observed. Real‐space magnetic force microscopy (MFM) imaging, combined with in situ atomic force microscopy (AFM) and scanning transmission electron microscopy (STEM), directly reveals the thickness‐dependent evolution of magnetic domains and lattice distortions, providing a structural basis for the observed modulation. Density functional theory (DFT) calculations support these findings, confirming a lithium‐induced ferromagnetic‐to‐antiferromagnetic phase transition accompanied by lattice expansion. These results highlight the exceptional magnetic tunability of Fe 3 GaTe 2 via ionic control and establish gate‐controlled intercalation as a reconfigurable platform for engineering topological spin textures and energy‐efficient magnetic memory devices.

ABSTRACT Conventional fossil fuel combustion intensifies environmental problems, while elevated operating temperatures severely limit the power output and durability of photovoltaic technologies. Hydrogel‐driven photovoltaic thermal management exploits the intrinsic water‐retention and evaporation properties of hydrogels to overcome the limitations of conventional cooling. This strategy provides an innovative solution to temperature‐induced performance degradation in photovoltaic systems. This review summarizes recent progress in hydrogel‐driven photovoltaic thermal management. First, this review compares existing photovoltaic cooling technologies and finds superior performance for hydrogel‐based passive evaporative cooling. This performance originates from hydrophilic functional groups in hydrogel networks and reduced effective evaporation enthalpy. Then, this review analyzes hydrogel material design strategies from four aspects: polymer network mechanisms, three‐dimensional network structures, functional components, and macroscopic composite architectures. Next, this review discusses system integration and configuration strategies for hydrogel‐driven photovoltaic cooling, including closely attached configurations, packed bed structures, heat sink coupled systems, and multifunctional cogeneration designs. These systems demonstrate the potential for coordinated energy and water utilization. Finally, this review summarizes key technical challenges and proposes future research directions.

ABSTRACT Utilizing photo‐generated carriers to boost charge–discharge process is of significance in photo‐assisted lithium‐oxygen batteries (PLOBs), while this poses a great challenge for low‐cost multinary metal oxides (MMOs) photoelectrodes on the unfavorable conduction band that is generally lower than the reduction potential of Li 2 O 2 to Li. The present work demonstrates a universal strategy of laser subtracting bulk MMOs, yielding gram‐scale MMOs nanocrystals with a favorable band position that allows for photo‐generated electrons to participate in photo‐assisted reduction of oxygen. The extreme conditions manufacturing endows the MMO nanocrystals with unique surface states with abundant Lewis acid‐base sites, which is experimentally verified to be favorable for acceleration of electrochemical reaction kinetics in PLOBs. Exemplified by photoelectrodes comprising laser‐subtracted BiVO 4 (BVO) NCs with elevated conduction band and tailored surface states, which achieve a high discharge potential of 3.25 V and low charge potential of 2.98 V (0.1 mA cm −2 ) with a round‐trip efficiency of 109%, and excellent cycling stability over 255 cycles with only 0.027% capacity decay per cycle, surpassing previously reported metal oxide‐based cathodes in PLOBs. Such a laser‐subtracting strategy was further found to be general in yielding many other MMOs NCs with activated photo‐assisted discharge behaviors, thus paving an efficient way to discover potential bifunctional photoelectrodes for PLOBs based on laser‐matter interactions.

ABSTRACT Photo‐driven carbene cross‐linking represents an emerging, versatile strategy for advanced polymer engineering. By harnessing photogenerated free carbenes from rationally designed diazo and diazirine precursors, this approach enables precise covalent bonding through efficient C─H/X─H (X = N, O, S, etc.) insertion mechanisms. Going beyond a conventional summary, this review establishes a critical bridge between micro‐level photochemistry and macroscopic material performance. We systematically outline fundamental molecular design guidelines, highlighting how the precise regulation of carbene spin states (singlet vs. triplet) and the strategic selection between aryl diazo esters (ADEs) and trifluoromethyl aryl diazirines (TADs) directly dictate oxygen tolerance, lithographic resolution, and ultimate device fidelity. Guided by these foundational principles, we comprehensively review recent breakthroughs of carbene cross‐linkers in high‐resolution surface patterning and robust interfacial adhesion across diverse substrates. The technology's unique combination of spatiotemporal control, substrate independence, and mild processing conditions establishes a versatile platform for next‐generation polymer manufacturing and advanced functional material design.

ABSTRACT The development of Fe‐rich 2:17‐type SmCo permanent magnets is crucial for achieving high performance, yet it has been persistently plagued by an inescapable performance trade‐off. The high degree of order in the Fe‐rich solid solution severely impedes the disordering phase transition and subsequent Cu segregation, leading to defective cellular structures and poor squareness and magnetic energy product. Herein, a novel cyclic heat treatment strategy is introduced that overturns the conventional paradigm of simply prolonging the solid solution time. By utilizing the existing nanoscale cellular structure as a precursor for secondary solution treatment, this strategy ingeniously engineers a rapid and complete boundary‐initiated disordering pathway. Driven by Sm diffusion, the process rapidly consumes the ordered intracellular, leading to significant reduction in the degree of order within the solid solution. This optimized precursor enables the formation of a highly continuous and uniform cellular architecture with ideal Cu distribution during aging. Consequently, the magnet exhibits an ultra‐high squareness of 87.8%, ultimately resulting in a recorded magnetic energy product of 282.9 kJ/m 3 and intrinsic coercivity of 1846.7 kA/m. This work provides a new insight into regulating phase transition kinetics and paves the way for the development of permanent magnets with higher performance.

ABSTRACT Dynamic multicolor room‐temperature phosphorescent carbon dots (RTP CDs) hold great promise for applications in programmable photonic encryption. However, their intrinsic confinement effects inevitably lead to exciton localization, making it difficult to regulate emissive behavior within extended conjugated systems. Herein, an exciton delocalization‐mediated strategy was employed to realize tunable RTP emission ranging from blue to red in CDs@boron oxide (PACDs@B 2 O 3 , 23NA‐CDs@B 2 O 3 , 18NA‐CDs@B 2 O 3 , and ND‐CDs@B 2 O 3 ), and time‐dependent dynamic RTP emission was further demonstrated in both 18NA‐CDs@B 2 O 3 and ND‐CDs@B 2 O 3 . Combined characterizations show that regulating the benzene‐ring structures of the precursors effectively extends the π‐conjugated system of the carbon core in the CDs, thereby markedly promoting exciton delocalization and reducing the energy gap between singlet and triplet states, leading to a redshifted RTP emission. Furthermore, exciton delocalization between graphitic domains with different conjugation sizes enables cascade energy transfer from larger domains to smaller ones, resulting in dynamic RTP emission. The successful application of dynamic multicolor RTP CDs@B 2 O 3 in programmable photonic encryption clearly demonstrates their broad application potential. This work opens up a new avenue for the on‐demand design of dynamic multicolor RTP materials.

ABSTRACT Developing new mechanoluminescence (ML) materials serves as a powerful approach for probing the fundamental mechanism of interfacial interactions dominated resultant ML. Herein, a novel resultant ML composite, Mg 3 (PO 4 ) 2 :Eu/polydimethylsiloxane (PDMS), was developed, exhibiting bright green emission with outstanding durability over thousands of stretching cycles. Spectroscopic analyses in terms of photoluminescence (PL), cathodoluminescence, x‐ray excited luminescence, and ML reveal that the green emission should be attributed to the generation of dynamic Eu 2+ triggered by free electrons, providing solid evidence for the hypothesis that the interfacial peeling process generates free electrons. Thermoluminescence spectroscopy results further confirm that the interfacial peeling involves a high‐energy process capable of inducing new radiation defects within the phosphor lattice, based on which the interfacial high‐energy driven resultant ML model is proposed. Moreover, the multi‐mode luminescence, combining ultraviolet‐induced red PL and green ML, is utilized for advanced encryption and self‐powered mechanics sensing.

ABSTRACT We introduce a copper‐nicotinate (Cu‐NA) framework as a halogenide‐stabilized Cu + /Cu 0 pre‐catalyst for electrocatalytic CO 2 reduction with high C 2+ selectivity in a “neutral” electrolyte. Alkaline electrolytes (1 M KOH) primarily lead to H 2 and CH 4 formation due to rapid catalyst restructuring and carbonate precipitation, causing flooding of the gas‐diffusion electrode. Replacing the electrolyte with 1 M KCl induces a severe change in selectivity. Cu‐NA in KCl delivers >70% Faradaic efficiency for C 2+ products at a current density of 500 mA cm −2 with a C 2+ /C 1 ratio exceeding 14. Operando Raman spectroscopy detected strong CO ads accumulation and time‐dependent CO ads band shifts characteristic of high CO ads coverage conducive to C‐C coupling. Scanning electrochemical microscopy (SECM) measurements confirm that the local pH converges to highly alkaline values at high current densities in both electrolytes, ruling out pH as the origin of the selectivity switch. Post‐reaction XPS and XRD show that KCl preserves a Cu + ‐rich Cu/Cu 2 O surface and introduces surface‐bound chloride that suppresses HER, mitigates Cu dissolution/redeposition, and stabilizes the Cu + /Cu 0 interface essential for C 2+ formation. Anions can be used as active regulators of catalyst speciation and selectivity, offering a simple yet powerful design principle for CO 2 to C 2+ conversion at high current densities.

ABSTRACT Polyanionic ca–thode systems offer long cycle life and tunable redox potential due to their three–dimensional rigid skeleton. Here, we design a new Na 2 Fe 2 P 2 O 7 SO 4 cathode with a sulfate–pyrophosphate double anion for the first time. [SO 4 ] 2− and [P 2 O 7 ] 4− tetrahedra are coupled into the FeO 6 /FeO 4 polyhedral skeleton, and in situ biomass carbon coating constructs a highly conductive network with continuous 3D Na + migration channels. Using density functional theory and the climbing–image–driven elastic band method, the effects of different anion compositions on structural stability and sodium ion diffusion are evaluated. Our findings reveal that the composite anion displays the lowest migration energy barrier, thereby confirming the efficacy of the dual–anion synergy strategy in optimizing diffusion kinetics. The resulting Na 2 Fe 2 P 2 O 7 SO 4 /C–BM–2 delivers an initial discharge capacity of 124.70 mAh g −1 (0.05 C), a reversible capacity of 88.15 mAh g −1 at 1 C, and retains 64.43% after 10 000 cycles at 20 C. At −25°C, capacity retention reaches 95.46% after 1000 cycles at 0.5 C. This dual–anion–regulated material provides an innovative design for high‐energy, wide–temperature, long–life polyanion cathodes, particularly suitable for large–scale energy storage sodium–ion batteries requiring safety and durability.

ABSTRACT Metal–organic frameworks (MOFs) offer unique chemical selectivity for surface‐enhanced Raman scattering (SERS), yet their intrinsically weak light–matter coupling fundamentally limits sensitivity and has long hindered their practical deployment as plasmon‐free SERS substrates. Here, we report a photonic‐crystal strategy that fundamentally amplifies charge‐transfer (CT)‐mediated SERS in MOFs by exploiting slow photons at the photonic stop‐band edge. Using UiO‐66(Zr) nanocrystals as the model MOF, the assembled ordered MOF photonic crystals (PhCs) with tunable Bragg reflection are precisely aligned to the excitation wavelength. The resulting slow‐light effect dramatically increases photon residence time and local electromagnetic field within the MOF pore domains. This slow‐photon confinement synergistically couples with CT processes between MOFs and analyte molecules, resulting in a tenfold enhancement in SERS intensity compared with disordered MOF assemblies and an enhancement factor up to 5.15 × 10 8 without any plasmonic components. By leveraging the intrinsic band‐structure tunability of MOFs, selective CT‐SERS is further demonstrated across different molecular systems and environments. The optimized MOF‐PhCs substrate enables ppb‐level detection and multicomponent discrimination of lung‐cancer‐associated volatile organic compounds, which are digitally encoded into machine‐readable Raman barcodes. This work establishes slow‐photon‐regulated MOF photonic crystals as a versatile platform for plasmon‐free, chemically programmable, and functionally integrated SERS sensing.

ABSTRACT Biomass‐derived materials are promising candidates for sustainable plastics, yet the long‐standing trade‐off between high performance and efficient, facile chemical recyclability remains unresolved. Here, we present an aromatic nitrogen heterocycle–encoded coupling mechanism that overcomes this limitation in a fully biomass‐derived polyester material. We utilize abundant biomass feedstocks, including dimethyl pyridine‐3,5‐dicarboxylate, succinic acid, and 1,4‐butanediol—to craft the biomass‐derived polyester material (PABP) through a simple melt polymerization process. Pyridine units embedded in the polyester backbone simultaneously enhance chain packing and intermolecular interactions while enabling hydrogen‐bond‐assisted nucleophile activation. This dual role yields biomass‐derived polyesters with high mechanical strength (64 MPa), low oxygen permeability (0.096 barrer), and effective ultraviolet shielding (84.6%). After biaxial stretching, the PABP‐2 shows further improved performance, reaching a tensile strength of 136 MPa, an oxygen permeability of 0.095 barrer, and low haze (19.4%), surpassing most reported biaxial‐stretched counterparts. Crucially, the same heterocyclic nitrogen atoms facilitate chemical recycling by promoting ester bond cleavage under mild conditions. This enables rapid depolymerization, with monomers recovered in high yield (>89.0%) and purity (>95.2%). Monomers are repolymerized to regenerate materials with properties comparable to the original polyester. This work establishes a general strategy for coupling high performance with easy recyclability in sustainable materials.

ABSTRACT Magnetic soft materials derive their programmable shape morphing from spatially encoded magnetic anisotropy, which typically requires the controlled reorientation of magnetic particles during fabrication. Magnetic fluids or suspensions, in which magnetic particles possess high rotational freedom, offer a promising platform for constructing and programming such materials. However, the intrinsic fluidity of magnetic suspensions also leads to severe magnetofluidic instabilities, preventing precise magnetic programming. Here, we introduce capillary locking as a general physical strategy to stabilize magnetic fluids in open systems. By infiltrating a magnetic polymer solution containing hard‐magnetic microparticles into an interconnected porous scaffold, capillary forces at solid–liquid–air interfaces immobilize the fluid while preserving the rotational freedom of the magnetic particles. This interfacial confinement suppresses magnetically induced flow and surface instabilities without encapsulation, enabling stable magnetic domain programming under weak magnetic fields. The capillary locked magnetic phase can be reversibly liquefied and resolidified through solvent exchange, allowing repeated reprogramming and fabrication of flexible magnetic composites with programmable magneto‐mechanical responses. Owing to the open porous architecture, the system further supports solvent‐assisted processing, modular assembly, and material recycling. These results establish capillary locking as a universal route for constructing reprogrammable magnetic soft materials from inherently unstable magnetic fluids.

ABSTRACT Balancing ordered molecular packing in cathode interlayers with the suppression of trap states along the electron transport pathway continues to be a major hurdle for high‐performance organic solar cells (OSCs). Here, a molecular design strategy that enables vertical ordering across the entire interlayer in a chlorinated perylene diimide (PDI‐2Cl) cathode interlayer is reported. Compared with a naphthalene diimide analogue (NDI‐2Cl), PDI‐2Cl possesses a larger conjugated core and stronger intermolecular π‑‐π interactions, leading to highly ordered packing that persists uniformly from the interface to the interior of the interlayer, as directly revealed by depth‑dependent GIWAXS. This structural superiority reduces energetic disorder and suppresses trap‑assisted recombination. Consequently, OSCs incorporating the PDI‐2Cl interlayer achieve a power conversion efficiency of 20.0%, substantially outperforming the NDI‐2Cl‑based counterpart (18.4%). This work highlights that engineering depth‑stable full‑layer ordering in cathode interlayers is an effective strategy to minimize transport‑pathway trap states and enhance device performance.