Physics

Hard carbons (HCs) are promising anodes for sodium-ion batteries (SIBs) but suffer from irreversible Na⁺ trapping, inadequate rate capability, and compromised low-temperature performance, primarily due to microstructural defects and suboptimal surface chemistry. Herein, an in situ-transformation carbonization strategy is proposed to synthesize surface low-concentration N, P-doped hard carbons (NP-HCs) for high-rate and low-temperature SIBs. A heteroatom-enriched polyphosphazene is conformally coated onto poplar wood precursors, with triethylamine playing a dual-function role in facilitating polymerization and precursor modification. This strategy endows the NP-HCs with a tailored interfacial environment for fast Na⁺ desolvation and transport, while establishing a bulk environment featuring abundant closed pores and expanded interlayer spacings. Consequently, NP-HCs deliver an ultrahigh reversible capacity of 428.8 mAh g^-1 and outstanding rate capability (272.6 mAh g^-1 at 10 C). Notably, remarkable low-temperature performance is achieved, with exceptional rate capability and cycling stability (93.1% capacity retention over 1200 cycles) at -20°C, underscoring their robustness under extreme conditions. Operando/ex situ characterizations coupled with computational studies reveal Na-storage mechanisms and accelerated kinetics, offering critical insights for high-performance HCs.

Lithium-rich manganese-based oxides (LRMO) suffer from rapid capacity decay, mainly driven by interfacial instability and bulk structural degradation associated with Jahn-Teller (J-T) distortion in Mn³⁺-rich regions. Such distortion accelerates surface oxygen activity, triggers nonuniform cathode electrolyte interphase (CEI) formation along with promoted parasitic reactions. Herein, we develop an electrolyte‑induced interfacial/bulk dual regulation strategy that enables negligible capacity decay in Li‑rich cathodes via coordinated interfacial/bulk regulation. In situ characterizations combined with interfacial compositional analyses confirm the dynamic formation of a thin, uniform, and robust LiF/LiBO₂-rich CEI, which stabilizes surface oxygen species and suppresses interfacial side reactions. Meanwhile, local structural analyses combined with theoretical calculations reveal that fluorinated molecules regulate Mn into a low-spin configuration, thereby alleviating J-T distortion and preventing bulk structural degradation. Benefiting from this dual induced interfacial-bulk stabilization effect, LRMO||Li cells deliver an initial capacity of 219.6 mAh g^-1 and retain 97.6% of their capacity after 400 cycles. This work provides a new pathway toward electrolyte-mediated dual stabilization and demonstrates the feasibility of mitigating capacity decay in Li-rich cathodes via electrolyte-induced interfacial/bulk regulation.

The application of organic electronics relies on reliable material manufacture. Owing to their multiscale structural characteristics, organic electronic materials face great opportunities and challenges in some unique applications compared with silicon-based semiconductors. Understanding the relationships among material structure, processing and properties is highly desirable for the multiscale manufacturing of organic functional devices. Recently, researchers have made significant progress in this field, achieving reliable fabrication across multiple scales, from molecular-scale devices to micro/milli-scale wearable systems and macroscale organic solar cell modules, to meet the specific requirements of various application scenarios. This review aims to summarize the latest advancements in multiscale manufacturing of organic electronic materials. It introduces multiscale structures and properties of organic semiconductors, with an emphasis on elucidating the structure-property relationship. Subsequently, different technologies for multiscale manufacturing and their advanced applications in organic electronics are discussed. Finally, potential challenges and prospects for the multiscale manufacture of organic electronic materials are proposed. This review could help in choosing appropriate manufacturing technologies to achieve optimal performance of organic electronic devices based on the properties of organic materials.

Electron-enhanced atomic layer deposition (EE-ALD) of amorphous, tunable titanium carbonitride (TiCxNy) films was obtained at low temperatures. The TiCxNy EE-ALD was achieved using sequential exposures of tetrakis(dimethylamido)titanium (TDMAT) and low-energy electrons in the presence of a continuous NH3 reactive background gas (RBG). The composition of the TiCxNy films was tuned by varying the NH3 background pressure and the electron exposure time. The TiCxNy EE-ALD was performed by utilizing a hollow cathode plasma electron source (HC-PES). The HC-PES delivered a high electron flux into background gases at pressures up to several mTorr. TDMAT was used as the source of Ti, C, and N. The NH3 RBG served as both a source of additional N and a method for the removal of C from the TiCxNy films. The TiCxNy EE-ALD film growth was monitored using in situ ellipsometry. The TiCxNy EE-ALD was conducted at low temperatures that never exceeded 130 °C, using NH3 pressures from 0 to 3 mTorr. The C content in the TiCxNy films could be tuned using the NH3 RBG pressure. Lower NH3 pressures led to the incorporation of more C into the TiCxNy films. The C:Ti ratio varied from ∼0.3 to ∼0.05 versus NH3 RBG pressure, as measured by X-ray photoelectron spectroscopy (XPS), at a constant electron exposure time of 10 s. Electron exposure time was also used to modulate the C content in the TiCxNy films. Shorter electron exposures led to more C incorporation. The C:Ti ratio varied from ∼2 to ∼0.1 versus electron exposure time, as measured by XPS at a constant NH3 background pressure of 2 mTorr. In situ 4-wavelength and ex situ spectroscopic ellipsometry were able to estimate electrical resistivities for the TiCxNy films. Resistivity was reduced from >2000 μΩ cm to ∼200 μΩ cm with decreasing C content. X-ray reflectivity (XRR) measurements were able to determine film densities. The film density for TiN films was 4.6 g/cm3, and the film density decreased with increasing C content. The C content in the TiCxNy films could also be varied using a CH4 RBG. Carbon could be added by carbon EE-chemical vapor deposition (EE-CVD) using electron exposures together with a CH4 RBG. The carbon could also be removed by carbon EE-chemical vapor etching (EE-CVE) using electron exposures together with NH3 RBG. The C content in the TiCxNy films was difficult to control using a supercycle approach with TiN EE-ALD and carbon EE-CVD.

Efficient, flexible, and solution-processable organic polymeric scintillators are urgently needed for diverse applications. However, conventional organic scintillators face intrinsic limitations in their exciton utilization efficiency and X-ray absorption capability. Herein, we introduce a design strategy for high-performance polymer scintillators by covalently integrating multiresonance thermally activated delayed fluorescence emitters into a bromine-functionalized copolymer matrix through facile free-radical copolymerization. The resulting copolymer scintillators exhibit enhanced exciton utilization through efficient reverse intersystem crossing and markedly improved X-ray absorption, owing to bromine incorporation. The optimized material achieves bright radioluminescence peaked at 500 nm, with a narrow full width at half-maximum of 46 nm. This scintillator achieves a high spatial resolution of 10 lp/mm, as determined by a standard line-pair test pattern, along with an exceptionally low detection limit of 301 nGy/s. Practical X-ray imaging applications confirm its capability to distinctly visualize intricate internal structures, validating its potential for clinical and industrial applications. This work establishes a versatile molecular design strategy for the development of advanced organic scintillators.

To realize highly optimized properties and performance of semiconductor photocatalysts, precise control over their composition and the site occupancy of multiple cations and anions is essential. This study demonstrates that Bi2YO4Cl, a multicationic oxyhalide photocatalyst, exhibits markedly higher activity when isovalent Bi-for-Y substitution is suppressed by simply controlling the precursor stoichiometry. The flux synthesis of Bi2YO4Cl under stoichiometric conditions induces the partial substitution of Bi3+ into Y3+ sites, creating localized states near the valence band maximum, which act as hole traps and hinder efficient charge carrier utilization. Using an excess of Y2O3 during the synthesis suppresses the undesired Bi-for-Y substitution, leading to markedly higher H2 and O2 evolution rates under visible-light irradiation. This study highlights the critical importance of precise cation placement for maximizing the photocatalytic performance of multicationic photocatalysts.

International audience

Owing to their stable three-dimensional cross-linked network and excellent mechanical and electrical insulation properties, anhydride-cured epoxy resins are widely used in dry-type transformers. 1,5,7-triazidobicyclo[4.4.0]deca-5-ene (TBD), a common catalyst for the ring-opening reaction of anhydrides and transesterification reactions, is widely applied in anhydride-cured epoxy resins. However, the high crystallinity of TBD results in poor compatibility with epoxy-anhydride thermosets, causing precipitation during mixing and nonuniform curing of the resin. In addition, the strong basicity of TBD induces excessive reactivity, undesirably narrowing the processing window. To overcome these limitations, a thermally latent catalyst (PTBD) was designed and synthesized. PTBD remains chemically inert at room temperature, significantly extending the processing window. Upon heating to 120 °C, PTBD dissociates into TBD, which efficiently catalyzes the transesterification reaction, thereby imparting excellent dynamic reversibility to the cured resin. This study achieves the synergistic enhancement of processability (processing window exceeding 190 min at 80 °C), mechanical performance (tensile strength up to 102.82 MPa) and degradability (complete degradation at 130 °C for 4 h) in epoxy resin systems.

The efficient construction of molecular complexity from simple building blocks is a significant goal in catalysis, and the controlled ring-opening functionalization of strained carbocycles provides a powerful strategy to achieve it. However, selective catalytic strategies for ring-opening difunctionalization of methylenecyclobutanes (MCBs) remain elusive. Here, we report a nickel-catalyzed method that enables the 1,4-dicarbofunctionalization and 1,4-hydrocarbofunctionalization of MCBs via selective C-C bond cleavage. This protocol exploits the strain energy and dual reactivity of MCBs to deliver nonadjacent C(sp³)/C(sp²) frameworks in good to excellent yields under mild conditions. A broad substrate scope, scalability to the gram scale, and versatile downstream transformations demonstrate the synthetic utility of this approach. Mechanistic studies, including control, isotope-labeling experiments, and DFT calculations, reveal a distinct cooperative pathway involving strain-driven β-carbon elimination, offering new opportunities for catalyst-controlled activation of MCBs.

FLT3-ITD inhibitors are approved for acute myeloid leukemia (AML) treatment but relapse is common. In this study, the combined inhibition of FLT3-ITD signal and protein translation by QUIZartinib and Omacetaxine Mepesuccinate (QUIZOM) synergistically suppressed the most critical FLT3-ITD survival signals including mitochondrial respiration and proteostasis, which induced apoptosis and pro-inflammatory response. In a Phase 2 trial (NCT03135054) involving 40 chemo-refractory/unfit FLT3-ITD AML patients, QUIZOM achieved a composite complete remission (CRc) of 83%, a median leukemia-free survival (LFS) of 10 months (Range: 0.7-68.2 months) and a median overall survival (OS) of 12.9 months (Range: 1.8-69.2 months). 13/33 (39%) received allogeneic HSCT after a median of 143 days (Range: 53-367 days). Higher CRc rates were observed in patients with NPM1 mutations, DNMT3A mutations, and wild-type WT1. Single-cell RNA-sequencing of QUIZOM cohort revealed positive correlation between pro-inflammatory response in blasts, CD8 + T activation and clinical responsiveness. Further, we identified a leukemic stem cell (LSC) subpopulation with activated JNK/JUN/HSPA1B axis via PLD1-driven phosphatidylcholine metabolism, which promoted proteostasis and drove QUIZOM resistance. PLD1-inhibitor remodeled phospholipid metabolism, induced ferroptosis and restored QUIZOM response in LSC. Our findings provided the therapeutic and resistant mechanisms of QUIZOM and paved the way for targeted interventions in this AML subtype.

Hematopoietic stem cells (HSCs) survive many types of cellular stress but often lose their regenerative and lymphopoietic capacities as a result. Such functional decline also occurs with age, and dysfunctional HSCs with impaired mitochondria accumulate during aging. However, the molecular link between HSC stress response and age-related functional decline remains poorly understood. Here we show that multiple stress responses converge on the RIPK3-MLKL axis to induce age-related changes in HSCs. The necroptosis effector MLKL is readily activated by inflammation and replication stress and accumulates in HSC mitochondria. Consequently, activated MLKL does not cause cell death but impairs HSC self-renewal and lymphoid differentiation. Such MLKL-mediated functional decline also occurs in HSCs during organismal aging, with activated MLKL primarily mediating age-related mitochondrial damage and reduced glycolytic flux. Collectively, our results establish the RIPK3-MLKL axis as a key mediator of HSC aging and identify a necroptosis-independent role of MLKL in mitochondrial damage.

The single-pass transmembrane receptor guanylyl cyclase A (GC-A), also known as natriuretic peptide receptor A (NPR-A) or NPR1, regulates blood pressure through vasodilation and natriuresis, making it a promising therapeutic target for hypertension and heart failure. We describe two monoclonal antibodies, XX16 and REGN5308, that differentially activate GC-A. Using cryo-electron microscopy and molecular dynamics simulations, we reveal that XX16 stabilizes GC-A in an active conformation even without its ligand ANP, whereas REGN5308 requires ANP to fully promote receptor activation. Both antibodies increase ANP binding affinity to GC-A and enhance GC-A-mediated cGMP signaling, although XX16 exerts a stronger stabilizing influence on ATP and GTP binding. In a mouse model of obesity-induced hypertension, XX16 treatment significantly reduces blood pressure, underscoring its therapeutic potential. These findings outline the structural and functional basis of GC-A activation by antibody positive allosteric modulators, offering strategies for durable antihypertensive therapies and improved management of cardiovascular diseases.

Angular momentum removal is a fundamental requirement for star and planet formation, yet the mechanisms driving this process remain debated. Magnetohydrodynamic disk winds, launched along magnetic field lines from extended disk regions, offer a promising solution, particularly in regions where magnetorotational turbulence is weak. Here we present high-resolution Atacama Large Millimeter/submillimeter Array observations of the Class 0 protostar HOPS 358, revealing a rotating, nested outflow structure traced by H₂CO, SO, and CH₃OH emission. The outflow preserves the disk's rotational sense and is aligned with the disk axis, providing direct observational evidence for a magnetically launched disk wind. From the measured kinematics, we derive a dimensionless magnetic lever arm of approximately 2.3 and constrain the wind-launching region to radii of 10-18 astronomical units within the planet-forming zone. These results demonstrate that magnetohydrodynamic disk winds operate during the deeply embedded phase, efficiently extracting angular momentum while shaping disk evolution and establishing initial conditions for planet formation.

Nitrogen-fixing nodule symbiosis is an ecologically and economically important trait in legumes and some related species. A critical step in the evolution of nodulation is the recruitment of NODULE INCEPTION (NIN); a homolog of the nitrate-sensing NIN-LIKE PROTEIN (NLP) transcription factors. However, whether adaptations have occurred in the NIN protein upon its recruitment in symbiosis remains elusive. Here we show that non-symbiotic NIN orthologs can function in intracellular infection and even nodule initiation, indicating that these properties of NIN predate the evolution of nodulation. Concurrent with the evolution of nodulation, symbiotic NIN proteins were optimized for their role in symbiosis by acquiring nitrate independent functionality, including constitutive nuclear localization. A single amino acid substitution in the non-symbiotic Arabidopsis AtNLP2 enhances its nuclear localization under low nitrate conditions, making it functionally comparable to the symbiotic Parasponia PanNIN. Our study provides insight in the evolutionary trajectory and molecular adaptation that allowed NIN to function as the central regulator of nitrogen-fixing nodule symbiosis.

Humoral immune-related adverse events, including hypogammaglobulinemia and B cell depletion, pose long-term infection risks after chimeric antigen receptor T cell therapy (CARTx) for hematologic malignancies. This prospective study evaluates the kinetics of pathogen-specific humoral immunity prior to and up to a year after CARTx targeting CD19 and CD20 (B cells) or BCMA (plasma cells) in 100 and 28 individuals, respectively. Antibodies are tested for 12 vaccine-preventable pathogens and using comprehensive high-throughput antibody profiling. A subset of 72 participants are evaluated for post-CARTx vaccine responses. Here, we show pathogen-specific humoral immunity does not significantly change after CD19-, CD20-, or BCMA-targeted CAR-T cell therapy (CARTx). However, seroprotective antibodies are absent for up to one-third of routine vaccine-preventable pathogens in CD19- and CD20-CARTx recipients and for nearly half of vaccine-preventable pathogens in BCMA-CARTx recipients by one-year post-CARTx. Pre-vaccination B cell count is the main predictor of vaccine response.

Lassa fever, a viral hemorrhagic fever caused by the arenavirus Lassa virus (LASV), affects thousands of individuals annually, highlighting the need for a vaccine. Yet, immunological correlates of viral load control remain poorly defined. Here we study vaccination-induced immunity in a surrogate LASV challenge model in mice. We find that LASV-cross-reactive B cell immunity induced by the glycoprotein of distantly related arenaviruses, such as lymphocytic choriomeningitis virus (LCMV), provides significant viral load control. Counter to common concepts, suppression of viremia is observed in the absence of CD8 T cells or neutralizing antibodies but correlates with non-neutralizing glycoprotein-specific antibody responses. Adoptive cell transfer experiments with monoclonal LCMV-specific B cells demonstrates that these cells suppress viral loads when previously activated by a heterologous cross-reactive glycoprotein and diversified by somatic hypermutation. These findings establish vaccination-induced B cell immunity to the LASV glycoprotein as a correlate of viral load control, independently of virus-neutralizing antibody titers at the time of challenge.

Ferroelectric materials with a switchable polarization are appealing for optoelectronic applications because of their above-bandgap photovoltage with a potential to exceed the Shockley-Queisser limit efficiency within classic p-n junctions. However, the intrinsic photovoltaic current in ferroelectrics remains far below the junction ones by orders, hindering their practical applications. Here we report an extremely large photovoltaic current density of 130 mA cm^-2 with a photovoltage of 1.31 V under 375 nm light illumination in single-domain lead titanate films. Its photoresponsivity surpasses all available ferroelectric materials by two orders of magnitude. Systematic investigations reveal that an interfacial Ta dopant layer during solution epitaxy drives a polarization converting of the film via the flexoelectric effect, where surface charged Pb vacancy layer was generated for polarization screening. These two layers produce a p-i-n structure throughout the film, accounting for the ultrahigh photovoltaic response. Furthermore, a self-powered X-ray detector made of such film was explored to achieve a sensitivity of 4.73 C Gy_air^-1 cm^-3, three orders of magnitude higher than that of commercial amorphous Se detectors. Our findings may pave the way for exploring novel detection and imaging devices based on ferroelectric materials.

While genetic screens have facilitated the dissection of protein function in animal development, advances in systematic point mutagenesis open new opportunities for forward genetics in mammalian cells. Here, we develop a CRISPR/Cas9-mediated base editing screen that allows functional screening of extensive collections of single amino acid substitutions of endogenous proteins. We demonstrate the application on the X-chromosomal Hprt and the autosomal Msh2 gene in diploid male and haploid mouse embryonic stem cells, respectively. Finally, we use this methodology to generate a sequence-function map of the transcriptional co-repressor SPEN in X chromosome inactivation. We demonstrate that the substitution of the SPEN RRM4-residue W522 abrogates X-linked gene repression by Xist RNA and impairs the establishment of H3K27me3 deposition. Our results demonstrate that screening in haploid cells allows efficient identification of mutations that would be recessive in diploid cells, suggesting applications across a wide range of areas.