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Abstract Organic semiconductors (OSCs) are featured by weak spin-orbit coupling due to their light chemical element composition, which enables them to maintain spin orientation for a long spin lifetime and show significant potential in room-temperature spin transport. Carrier mobility and spin lifetime are the two main factors of the spin transport performance of OSCs, however, their ambiguous mechanisms with molecular structure make the development of spintronic materials really stagnant. Herein, the effects of halogen substitution in bay-annulated indigo-based polymers on carrier mobility and spin relaxation have been systematically investigated. The enhanced carrier mobility with an undiminished spin lifetime contributes to a 3.7-fold increase in spin diffusion length and a record-high magnetoresistance of 8.7% at room temperature. By analyzing the spin-orbit coupling and hyperfine interaction, it was found that the distance of the substitution site from the conjugated center and the nitrogen atoms in the molecules play crucial roles in spin relaxation. Based on the above results, we proposed a molecular design strategy of halogen substitution far from conjugate center to enhance spin transport efficiency, presenting a promising avenue for advancing the field of organic spintronics.

Abstract Developing highly active materials that efficiently utilize solar spectra is crucial for photocatalysis, but still remains a challenge. Here, we report a new donor-acceptor (D-A) covalent organic framework (COF) with a wide absorption range from 200 nm to 900 nm (ultraviolet-visible-near infrared light). We find that the thiophene functional group is accurately introduced into the electron acceptor units of TpDPP-Py (TpDPP: 5,5’-(2,5-bis(2-ethylhexyl)−3,6-dioxo-2,3,5,6-tetrahydropyrrolo [3,4-c]pyrrole-1,4-diyl)bis(thiophene-2-carbaldehyde), Py: 1,3,6,8-tetrakis(4-aminophenyl)pyrene) COFs not only significantly extends its spectral absorption capacity but also endows them with two-photon and three-photon absorption effects, greatly enhancing the utilization rate of sunlight. The selective coupling of benzylamine as the target reactant is used to assess the photocatalytic activity of TpDPP-Py COFs, showing high photocatalytic conversion of 99% and selectivity of 98% in 20 min. Additionally, the TpDPP-Py COFs also exhibit the universality of photocatalytic selective coupling of other imine derivatives with ~100% conversion efficiency. Overall, this work brings a significant strategy for developing COFs with a wide absorption range to enhance photocatalytic activity.

Abstract Stretchable neuromorphic optoelectronics present tantalizing opportunities for intelligent vision applications that necessitate high spatial resolution and multimodal interaction. Existing neuromorphic devices are either stretchable but not reconcilable with multifunctionality, or discrete but with low-end neurological function and limited flexibility. Herein, we propose a defect-tunable viscoelastic perovskite film that is assembled into strain-insensitive quasi-continuous microsphere morphologies for intrinsically stretchable neuromorphic vision-adaptive transistors. The resulting device achieves trichromatic photoadaptation and a rapid adaptive speed (

Abstract Challenges associated with stretchable optoelectronic devices, such as pixel size, power consumption and stability, severely brock their realization in high-resolution digital imaging. Herein, we develop a universal detachable interface technique that allows uniform, damage-free and reproducible integration of micropatterned stretchable electrodes for pixel-dense intrinsically stretchable organic transistor arrays. Benefiting from the ideal heterocontact and short channel length (2 μm) in our transistors, switching current ratio exceeding 106, device density of 41,000 transistors/cm2, operational voltage down to 5 V and excellent stability are simultaneously achieved. The resultant stretchable transistor-based image sensors exhibit ultrasensitive X-ray detection and high-resolution imaging capability. A megapixel image is demonstrated, which is unprecedented for stretchable direct-conversion X-ray detectors. These results forge a bright future for the stretchable photonic integration toward next-generation visualization equipment.

Abstract Nanoclusters with atomically precise structures and discrete energy levels are considered as nanoscale semiconductors for artificial intelligence. However, nanocluster electronic engineering and optoelectronic behavior have remained obscure and unexplored. Hence, we create nanocluster photoreceptors inspired by mantis shrimp visual systems to satisfy the needs of compact but multi-task vision hardware and explore the photo-induced electronic transport. Wafer-scale arrayed photoreceptors are constructed by a nanocluster-conjugated molecule heterostructure. Nanoclusters perform as an in-sensor charge reservoir to tune the conductance levels of artificial photoreceptors by a light valve mechanism. A ligand-assisted charge transfer process takes place at nanocluster interface and it features an integration of spectral-dependent visual adaptation and circular polarization recognition. This approach is further employed for developing concisely structured, multi-task, and compact artificial visual systems and provides valuable guidelines for nanocluster neuromorphic devices.

Abstract Metal-nitrogen-carbon catalysts with hierarchically dispersed porosity are deemed as efficient geometry for oxygen reduction reaction (ORR). However, catalytic performance determined by individual and interacting sites originating from structural heterogeneity is particularly elusive and yet remains to be understood. Here, an efficient hierarchically porous Fe single atom catalyst (Fe SAs-HP) is prepared with Fe atoms densely resided at micropores and mesopores. Fe SAs-HP exhibits robust ORR performance with half-wave potential of 0.94 V and turnover frequency of 5.99 e−1s−1site−1 at 0.80 V. Theoretical simulations unravel a structural heterogeneity induced optimization, where mesoporous Fe-N4 acts as real active centers as a result of long-range electron regulation by adjacent microporous sites, facilitating O2 activation and desorption of key intermediate *OH. Multilevel operando characterization results identify active Fe sites undergo a dynamic evolution from basic Fe-N4 to active Fe-N3 under working conditions. Our findings reveal the structural origin of enhanced intrinsic activity for hierarchically porous Fe-N4 sites.

2D and 3D conductive MOFs have performed well in the fields of energy and catalysis. Here, authors synthesise a 1D conductive MOF in which DDA ligands are connected by double Cu ions, forming nanoribbon layers with π-d conjugated nanoribbon planes and out-of-plane π-π stacking, which facilitates charge transport along two dimensions.

Wearable and skin-like X-ray detectors need intrinsic flexibility and high sensitivity. Here Guo et al. develop a stretchable n-type polymer semiconductor with aligned nanofiber networks which achieve photosensitivity of 1.52×10^4 μC Gyair^-1 cm^−2 and low detection limit of 37.7 nGyair s^-1.

Here, the authors fabricate large area and highly aligned polymer semiconductor sub-microwires arrays via coaxial focused electrohydrodynamic jet printing technology, achieving high on/off ratio and average mobility that is 5x higher than that of thin film based organic field effect transistors.

Understanding the slow kinetics of hydrogen evolution reaction in neutral media is of fundamental importance for the rational design of high-performance electrocatalysts for hydrogen energy. Here, by studying Ru single atom and RuSe x cluster, the authors report how the rate of hydrogen evolution reaction activity in neutral media is governed by interfacial water.

Solution-based synthesis of covalent organic frameworks (COFs) often leads to insoluble powders or fragile films on solution surfaces. Here, the authors report large-area two-dimensional (2D) COF films with controllable thicknesses via vapour induced conversion.

Abstract In principle, polymerization tends to produce amorphous or poorly crystalline materials. Efficiently producing high-quality single crystals by polymerization in solvent remains as an unsolved issue in chemistry, especially for covalent organic frameworks (COFs) with highly complex structures. To produce μm-sized single crystals, the growth time is prolonged to >15 days, far away from the requirements in practical applications. Here, we find supercritical CO2 (sc-CO2) accelerates single-crystal polymerization by 10,000,000 folds, and produces two-dimensional (2D) COF single crystals with size up to 0.2 mm within 2~5 min. Although it is the fastest single-crystal polymerization, the growth in sc-CO2 leads to not only the largest crystal size of 2D COFs, but also higher quality with improved photoconductivity performance. This work overcomes traditional concept on low efficiency of single-crystal polymerization, and holds great promise for future applications owing to its efficiency, industrial compatibility, environmental friendliness and universality for different crystalline structures and linkage bonds.

Realizing organic p–n junctions based on ordered crystalline materials with dimensions comparable to the exciton diffusion length of most organic semiconductors remains a challenge. Here, the authors report a strategy to form molecular monolayer crystal-based p–n junctions with thickness below 5 nm.

The Bacillus haemolytic enterotoxin haemolysin BL has been shown to activate the NLRP3 inflammasome. Here the authors show that a non-haemolytic enterotoxin (NHE) from B. cereus can also activate the NLRP3 inflammasome with a similar mechanism of lytic pore formation.

Field effect transistors based on graphene hold promise for future sensing applications. Here, the authors report a free radical sensor in which the •OH radical cuts cysteamine to release Cd2 + from the electrolyte/graphene interface and selectively detects •OH with a concentration down to 10−9 M.