Abstract Increasing larval settlement can substantially accelerate coral reef restoration by overcoming a key bottleneck in coral population recovery. Successful settlement depends on biological and chemical cues associated with microbial biofilms and crustose coralline algae that are often reduced or absent on degraded reefs. Here, we present two complementary nanocarrier strategies for delivering a single defined bacterial settlement signal, lipopolysaccharides (LPS), from hydrogel coatings applied to coral settlement surfaces. One platform presents LPS at the hydrogel surface using liposome nanoparticles, while the other encapsulates LPS in silica nanoparticles embedded in the hydrogel matrix for gradual release. Both systems increased settlement of Montipora capitata larvae by >5-fold compared to uncoated control surfaces. Because this approach relies on a single cue derived from cultured bacteria, it offers a potentially scalable alternative to live biofilms or complex natural extracts. These results establish a promising biomaterials strategy for enhancing coral recruitment and supporting reef restoration.
Abstract We investigate how the assembly of magnetic nanoparticles embedded in a semi-crystalline polymer governs heat generation when submitted to a high-frequency alternating magnetic field by simultaneously monitoring temperature and structural anisotropy through infrared thermography and time-resolved ultra-small-angle X-ray scattering, respectively. A polypropylene matrix is used as a host system to disentangle intrinsic magnetic heating from structural contributions, thereby isolating the additional heat generated by dipolar chain formation above the polymer melting point during successive heating cycles. In contrast, reorienting the chain axis perpendicular to the applied field is found to significantly reduce heat generation. These in situ measurements are complemented by X-ray tomography and scanning electron microscopy experiments, providing a comprehensive view of the underlying mechanisms. Overall, this work establishes a direct relationship between nanoparticle organization and hyperthermia performance, opening new routes for the rational design of functional nanocomposites.
Abstract Developing sustainable electrocatalysts from waste resources offers an attractive route toward clean energy storage and environmental remediation. Herein, an all-in-waste strategy is reported to upcycle sewage sludge and straw into single-atom catalysts for rechargeable zinc–air batteries. High-energy mechanical shearing coupled with self-atmosphere pyrolysis transforms the waste into hierarchical porous carbon hosting Fe1–N4 active sites. The resulting sludge–straw-C catalyst achieves an oxygen reduction reaction kinetic current density of 4.5 mA cm–2 at 0.75 V, outperforming single-precursor counterparts by 4.1 to 5.6 times. Furthermore, it reduces the oxygen evolution reaction overpotential at 10 mA cm–2 to 390 mV, a decrease of 120–150 mV. Integrated into rechargeable zinc–air batteries, this catalyst delivers a peak power density of 160 mW cm–2 and stable cycling over 800 hours. This work provides a scalable and reagent-free route for transforming environmental pollutants into value-added energy materials.
Abstract We report a combined computational−experimental study that identifies and explains the enhanced spin splitting in single-layered (n = 1) two-dimensional (2D) lead−iodide hybrid perovskites. We develop a high-throughput screening workflow for experimentally synthesized 2D hybrid perovskites and identify 12 compounds with spin splitting, among which (2-BrPEA)2PbI4 exhibits the largest splitting energy. To establish a unified structure-splitting relationship, we introduce a root-mean-square deviation (RMSD)-based descriptor defined as the deviation between a structure and its inverted counterpart, which correlates with spin-splitting energy more strongly than conventional bond-angle metrics. Notably, although the reported room-temperature structure of (2-BrPEA)2PbI4 is nominally centrosymmetric, it shows strong circularly polarized luminescence (CPL) at room temperature, comparable to the benchmark (4AMP)PbI4. Ab initio molecular dynamics (AIMD) simulations further reveal thermally activated dynamical distortions that transiently break inversion symmetry and amplify spin splitting, establishing lattice dynamics as a key driver of room-temperature spin functionality in 2D hybrid perovskites.
Abstract Controlling polymorphism in ceramic microarchitectures is essential for linking processing, structure, and function yet remains difficult for ceramics produced by two-photon lithography (TPL). During thermal conversion, crystallite growth typically promotes the thermodynamically stable monoclinic (m) phase, restricting access to tetragonal (t)-ZrO2. Here, we show that infrared (IR) flash annealing stabilizes t-ZrO2 microarchitectures over a broad 600–1000 °C treatment window. Rapid IR heating (20 °C s–1) limits crystallite growth and suppresses the t-to-m transformation commonly observed near 750 °C under slower annealing. Scanning transmission electron microscopy (STEM) confirms crystallite-size-dependent t-stabilization during rapid IR heating, while Europium (Eu3+) serves as an embedded optical probe of local symmetry, providing distinct photoluminescence signatures without destructive preparation. Flash thermal processing controls polymorphism, while luminescent symmetry probing enables its non-destructive diagnosis in 3D ceramic microarchitectures, providing a transferable approach for studying phase evolution in lanthanide-doped ceramics.
Abstract X-ray dosimetry and imaging have been utilized in a wide range of applications. However, the complex components of detection, memory, and computing units of commercial detection systems inevitably make it structurally complex and energy consuming. Here, a multimodal two-terminal perovskite device is demonstrated that can measure real-time dose rate and record the accumulated dose of X-ray pulse signals concurrently by decoupling volatile electronic and non-volatile ionic variables of the conductance (G). The device delivers an X-ray sensitivity of 1159 μC Gy–1 cm–2, a limit of detection (LoD) of 27.9 nGy s–1, a limit of memory (LoM) of 0.32 μGy s–1, as well as multiple non-volatile storage states of around 40 nS. As a proof-of-concept, a perovskite crossbar array integrates the functions of sensitive X-ray detection, multi-state data memorization, as well as image pre-processing, offering a promising platform toward intelligent, robust, and lightweight radiation imaging systems.
Abstract Light-responsive photovoltaic biointerfaces convert optical energy into signals capable of modulating cellular activity. However, how these interfacial signals are generated, transmitted, and interpreted by living tissue remains a matter of ongoing debate. This Perspective argues that photovoltaic devices for wireless cellular modulation should not be treated as a simple electrode but as a dynamic interfacial electrochemical system in which light absorption, charge separation, ionic transport, capacitive charging, Faradaic reactions, photothermal effects, and cellular adaptation are inseparably coupled. We examine how material architecture—from conjugated polymers and bilayer heterojunctions to bulk heterojunctions and nanoparticles—governs both signal generation and biological outcome. We further highlight the need to replace isolated photovoltaic figures of merit with functional bioelectronic metrics that integrate the cellular response. Ultimately, understanding how distinct interfacial pathways translate photogenerated signals into biological responses will be essential for the rational design, evaluation, and clinical translation of next-generation photovoltaic biointerfaces.
Abstract We have developed a one-pot, two-stage method for the synthesis of highly monodispersed fluorescent polystyrene nanoparticles with surface carboxyl functional groups. The fluorescent nanoparticles have a tunable size range of 150−300 nm and excellent photo/chemical stability. Through conjugating antibodies to the surface carboxyl groups, various lateral flow immunoassays (LFIAs) using the fluorescent nanoparticles as the reporters have been developed, achieving a visual limit of detection (LOD) of 39 mIU mL−1 using human chorionic gonadotropin as the model sample. This LOD is 8-fold and 64-fold better as compared to LFIAs using AuNPs and free dye as reporters, respectively. The LODs of our optimized LFIAs are 3 pg mL−1 for HIV-1 p24, 4 ng mL−1 for Zika NS1, and 1 and 0.5 ng mL−1 for Staphylococcus aureus enterotoxin types A and B, respectively. These LOD values are below the clinical cutoffs and are comparable to ELISA results reported in the literature.
Abstract Achieving fail-safe normally-off operation without plasma-induced damage remains a significant challenge in β-Ga2O3-based high-power electronics. We demonstrate a forward metal-assisted chemical (f-MAC) etching that functions as a damage-free and self-aligned process for recessed-gate β-Ga2O3 metal–semiconductor field-effect transistors. The asymmetric work functions of a Ti Ohmic electrode and buried Pt gate electrode establish a built-in electric field that separates photogenerated electron−hole pairs and drives the localized etching of β-Ga2O3, generating a recessed gate structure. A vertical etching rate of 7.9 nm/min enables a channel thickness reduction from 402 to 230 nm, shifting the threshold voltage from −9.14 to +1.55 V to achieve enhancement-mode operation. The device demonstrates a 33.7% reduction in subthreshold swing and a 5.26-fold enhancement in the on/off current ratio owing to the strengthened channel modulation and defect-preferential nature of f-MAC etching, establishing f-MAC etching as a promising damage-free fabrication process for high-performance β-Ga2O3 high-power electronics.
Abstract Future sustainable agriculture requires root-zone systems that conserve water, retain nutrients, support beneficial microbes, withstand drought and salinity, and degrade safely in soil. Hydrogels are a promising material platform because their hydrated polymer networks can be tuned in chemistry, mechanics, transport, architecture, and degradation. This viewpoint frames agricultural hydrogels as adaptive rhizosphere interfaces, with exchange at the root-soil interface as the central design target. We organize this opportunity around three directions: water resilience, nutrient efficiency, and biotic integration. Water resilience demands root-zone moisture regulation under soil confinement, salinity, and wet−dry cycling. Nutrient efficiency requires reversible ion retention and synchronized release under plant demand. Biotic integration requires hydrated, permeable, and biodegradable microhabitats that support plant−microbe interactions. We argue that hydrogel design must move beyond swelling capacity and release curves toward the field materials engineering, including soil-confined testing, multifunctional trade-offs, scalable forms, and safe end-of-life behavior for practical climate-resilient and resource-efficient agriculture.
Abstract Developing organic−inorganic hybrid nanomaterials generating multiple optical signals remains challenging due to inherent design complexities. Herein, we present organic-SiO2 nanohybrids exhibiting size-dependent room-temperature phosphorescence (RTP) and structural color. By employing a covalent anchoring strategy, silanized organic phosphors are incorporated into the SiO2 matrix, protecting triplet excitons and enabling multicolor aqueous RTP emission with a maximum lifetime of 314.81 ms. Notably, as particle size increases, organic-SiO2 RTP nanohybrids exhibit an approximately 2-fold enhancement in RTP lifetime and generate a red-shifted structural color signal through self-assembly. The long-lived luminescence and excellent biocompatibility of NPA@SiO2 (H-120) enable in vivo afterglow imaging without additional covering treatments. Within 0.5 h after tail vein injection at an ultralow chromophore dose (0.25 mg kg−1), tumor sites in mice are precisely localized via efficient cellular uptake, representing superior imaging performance. Furthermore, the unique multiplexed optical features of organic-SiO2 nanohybrids provide significant advantages for anti-counterfeiting labeling and multi-level encryption applications.
Abstract Synthesis of amino acids via electrocatalytic C−N coupling is considered a promising and green approach. Whether C−N coupling relies on cooperative sites (bonded or nonbonded) is an open question and is crucial for the development of highly efficient catalysts. Here, Cu single-atomic site (SAS) catalysts with different site densities were synthesized via an ion exchange approach, and the impact of site proximity on Faradaic efficiency of alanine (FEalanine) was probed. The FEalanine is positively correlated with Cu SAS loadings. An FEalanine of 42% can be achieved at 15 wt % loading. Remarkably, it is revealed that fully isolated Cu SASs (at 1 wt % loading) do not result in alanine. This suggests that the presence of adjacent-site configurations is probably essential for the C−N coupling. It is speculated that fully isolated Cu SASs prefer to adsorb pyruvic acid rather than nitrate, thus failing to form the key intermediate hydroxylamine.
Abstract Perylenediimides (PDIs), which feature strong visible-light absorption, π-electron-deficient planes, and photochemical characteristics, offer a versatile platform for developing tunable and efficient metal−organic framework (MOF) materials through modulation of their bay-substituent groups. Herein, we report two structurally modified MOFs, MOF-Cl4 and MOF-Br2, whose PDI components feature different halogen substitution patterns in their bay regions, imparting differential halogen-controlled photochromism. Notably, MOF-Cl4 exhibited high photosensitivity, whereas MOF-Br2 was found to be almost photochemically inert. Furthermore, both MOFs could be readily photoexcited to generate their respective excited states or radical anions. Interestingly, experimental and theoretical calculations revealed that these excited states or radical anions demonstrated halogen-controlled photocatalytic activities in the oxysulfonylation of alkynes and the aerobic oxidation of enamines. The photocatalytic performance of MOF-Cl4 proved superior to that of MOF-Br2, a difference primarily attributed to the divergent SOMO-1 and optical bandgap of the PDI ligands and MOF materials, induced by the halogen substitution patterns.
Abstract Garnet-type Li7La3Zr2O12 (LLZO) is a promising solid electrolyte, but its highly conductive cubic phase is metastable at room temperature. We investigate lithium-ion migration mechanisms in LLZO using machine-learning molecular dynamics (MLMD), which achieves near-AIMD accuracy while enabling nanosecond-scale simulations at significantly reduced computational cost. Li-site supervalent doping (Fe, Ga, Al, B, and Zn) stabilizes the cubic phase by reducing the energy difference between tetragonal and cubic phases. In tetragonal LLZO, supervalent doping enhances Li-ion transport through vacancy-mediated hopping. In contrast, cubic LLZO possesses a disordered Li sublattice, making transport relatively insensitive to doping and susceptible to migration pathway disruption. Overall, Li-site supervalent doping improves conductivity by stabilizing the cubic phase and activating transport in tetragonal LLZO, rather than increasing intrinsic mobility in cubic LLZO. These results highlight MLMD as a powerful tool for probing ion transport and provide optimal doping strategies to introduce Li vacancies while preserving well-connected migration pathways.
Abstract Electrochemical biosensors hold immense promise for sensitive, point-of-care detection of clinically relevant biomarkers from liquid biopsies; however, their performance is fundamentally constrained by charge screening and steric hindrance at the biointerface, particularly under physiological conditions where the Debye length is <1 nm. Herein, we establish a rational framework for engineering high-performance electrochemical biointerfaces by independently tuning two key parameters: linker-based bioreceptor spacing and probe loading density. This strategy is enabled by a modular nanobody−MXene platform, combining 2D MXene nanosheets with covalently conjugated nanobodies. Using anti-GFP nanobodies as model bioreceptors, we identified an intermediate linker regime that maximized signal transduction and a low-density probe regime that mitigated steric hindrance while enhancing dynamic range and sensitivity. Applied to a VHH72 nanobody−MXene biosensor, this framework enabled the detection of SARS-CoV-2 S1 with a 12 pM limit of detection, high specificity, and robust performance in saliva. Collectively, this work establishes a dual-parameter framework for advancing next-generation electrochemical biosensors.
Abstract Biomaterials, particularly hydrogels, are being engineered for tissue engineering, drug delivery, and medical implants. While natural and synthetic polymers offer distinct advantages like the biocompatibility of collagen or the precise tunability of polyethylene glycol, advancements in chemical synthesis have enabled the development of bioinspired synthetic hydrogels that bridge these categories. Bioactive peptides can recruit growth factors, promote angiogenesis, and reprogram macrophages toward a healing phenotype, while proteins can produce hydrogels with tunable mechanical properties. Significant needs in soft tissue repair remain: nonhealing chronic wounds, scarring, fibrosis, corneal blindness, and heart failure urgently require improved therapies. This Perspective article discusses current state-of-the-art peptide-based hydrogels, focusing on applications for skin, cornea, and heart repair. Despite progress, challenges remain regarding optimal material properties, clinical scalability, and regulatory hurdles. Future advancements are expected to leverage emerging technologies such as OMICS, spatial transcriptomics, and artificial intelligence to create personalized, iterative designs for next-generation regenerative therapies.
Abstract The miniaturization of integrated circuits is increasingly limited by parasitic resistance−capacitance (RC) delay. Metal−organic frameworks (MOFs) are promising low-dielectric-constant (low-k) materials, yet simultaneously achieving ultralow k and mechanical robustness remains challenging. Here, we propose an antianisotropic growth strategy to fabricate compact MIL-53(Al) thin films via microwave-assisted hydrothermal conversion of an atomic layer-deposited Al2O3 layer. By combining a metal species modulator to reduce the grain length-to-width ratio with a pH modulator to boost nucleation, this synergistic approach enables nanoscale-controlled growth. The optimized microstructure enhanced the elastic modulus by 45.9% while maintaining an ultralow k of 1.98 at 1 MHz. The breakdown field increased approximately 4-fold, resulting in a projected lifetime of 5.55 years at 1 MV cm−1. The antianisotropic growth strategy enables MOF films to combine ultralow k with robust mechanical properties and reliability, offering a practical strategy for high-performance dielectrics in next-generation interconnect technologies.
Abstract The functional properties of ferroelectric materials are strongly influenced by their polarization orientation; as such, precise characterization of polarization vectors is important to ferroelectrics research. Here, we develop a fully automated three-dimensional piezoresponse force microscopy (Auto-3DPFM) technique, which integrates all essential steps in interferometric PFM for 3D polarization vector characterization, including laser alignment, tip calibration and approach, image acquisition, polarization vector reconstruction, and visualization. The automation reduces the experimental burden of ferroelectric polarization vector characterization, while continual calibration ensures consistency and reproducibility of 3D polarization reconstruction. An algorithmic workflow is also developed to identify domain walls and calculate their characteristic angles via a spatial vector-angle-difference method, presenting one capability enabled by Auto-3DPFM and inaccessible through traditional PFM techniques. When integrated with machine learning and adaptive sampling strategies in self-driving labs, Auto-3DPFM serves as a valuable tool for advancing ferroelectric physics and microelectronics development.
Abstract Artificial intelligence-assisted design of electromagnetic wave absorbing coatings is often restricted to geometry or topology optimization within fixed materials. Here, we present a modular particle swarm optimization−proximal policy optimization (PSO−PPO) framework for radar-absorbing metastructures that combines a progressive feature fusion surrogate for 8−18 GHz reflection-loss prediction, a ResNet-based empirical filter for low-performance patterns, and reinforcement learning optimization in a mixed discrete-continuous design space. For broadband single-layer optimization, the framework identifies a generated-material M2/Pt metasurface absorber with a 1.30 mm thickness and a CST-validated effective bandwidth of 6.32 GHz, with field simulations indicating absorption from multiple localized resonances and dielectric loss. The same strategy is extended to multilayer inverse design for prescribed single-peak Gaussian spectra, yielding target responses at 10, 12, and 16 GHz with mean absolute errors (MAEs) of 1.64−2.19 dB. This work demonstrates an efficient route for automated absorber optimization and customized spectral regulation.
Abstract The production of high-quality monolayer MXene nanosheets is constrained by the trade-off between delamination efficiency and structural damage. Here, we report a cavitation-free, high-speed shear emulsification strategy for the rapid, low-damage delamination of multilayer Ti3C2Tx MXene. Continuous fluid shear promotes interlayer sliding and separation, enabling an 82% monolayer yield within 10 min while retaining an average lateral size of approximately 5 μm and a film conductivity of 10,800 S cm–1, outperforming conventional ultrasonic delamination. Structural and spectroscopic analyses show that crystallinity and surface terminations are retained, enabling assembly into dense lamellar films. These films exhibit electromagnetic interference (EMI) shielding effectiveness above 60 dB and an infrared emissivity of 0.11. Furthermore, the process is readily scalable to hundred-gram-level delamination, highlighting its potential for the large-scale production of high-quality MXene for multifunctional applications.
