Silicon- (Si-) based optoelectronic synaptic devices mimicking biological synaptic functionalities may be critical to the development of large-scale integrated optoelectronic artificial neural networks. As a type of important Si materials, Si nanocrystals (NCs) have been successfully employed to fabricate optoelectronic synaptic devices. In this work, organometal halide perovskite with excellent optical asborption is employed to improve the performance of optically stimulated Si-NC-based optoelectronic synaptic devices. The improvement is evidenced by the increased optical sensitivity and decreased electrical energy consumption of the devices. It is found that the current simulation of biological synaptic plasticity is essentially enabled by photogating, which is based on the heterojuction between Si NCs and organometal halide perovskite. By using the synaptic plasticity, we have simulated the well-known biased and correlated random-walk (BCRW) learning.

In quantum mechanics, a norm-squared wave function can be interpreted as the probability density that describes the likelihood of a particle to be measured in a given position or momentum. This statistical property is at the core of the fuzzy structure of microcosmos. Recently, hybrid neural structures raised intense attention, resulting in various intelligent systems with far-reaching influence. Here, we propose a probability-density-based deep learning paradigm for the fuzzy design of functional metastructures. In contrast to other inverse design methods, our probability-density-based neural network can efficiently evaluate and accurately capture all plausible metastructures in a high-dimensional parameter space. Local maxima in probability density distribution correspond to the most likely candidates to meet the desired performances. We verify this universally adaptive approach in but not limited to acoustics by designing multiple metastructures for each targeted transmission spectrum, with experiments unequivocally demonstrating the effectiveness and generalization of the inverse design.

In the photoreduction of CO₂ to CO, the competitive H₂ evolution is always inevitable due to the approximate reduction potentials of H⁺/H₂ and CO₂/CO, which results in poor selectivity for CO production. Herein, imidazolium-type ionic liquid- (IL-) modified rhenium bipyridine-based porous organometallic polymers (Re-POMP-IL) were designed as efficient and selective photocatalysts for visible-light CO₂ photoreduction to CO based on the affinity of IL with CO₂. Photoreduction studies demonstrated that CO₂ photoreduction promoted by Re-POMP-IL functioning as the catalyst exhibits excellent CO selectivity up to 95.5% and generate 40.1 mmol CO/g of Re-POMP-IL1.0 (obtained by providing equivalent [(5,5{}^{\prime }-divinyl-2,2{}^{\prime }-bipyridine)Re(CO)₃Cl] and 3-ethyl-1-vinyl-1H-imidazol-3-ium bromide) at 12 h, outperforming that attained with the corresponding Re-POMP analogue without IL, which highlights the crucial role of IL. Notably, CO₂ adsorption, light harvesting, and transfer of photogenerated charges as key steps for CO₂RR were studied by employing POMPs modified with different amounts of IL as photocatalysts, among which the CO₂ affinity as an important factor for POMPs catalyzed CO₂ reduction is revealed. Overall, this work provides a practical pathway to improve the CO₂ photoreduction efficiency and CO selectivity by employing IL as a regulator.

The drug-eluting stent (DES) has become one of the most successful and important medical devices for coronary heart disease, but yet suffers from insufficient endothelial cell (EC) growth and intima repair, eventually leading to treatment failure. Although biomacromolecules such as vascular endothelial growth factor (VEGF) would be promising to promote the intima regeneration, combining hydrophilic and vulnerable biomacromolecules with hydrophobic drugs as well as preserving the bioactivity after harsh treatments pose a huge challenge. Here, we report on a design of hierarchical capillary coating, which composes a base solid region and a top microporous region for incorporating rapamycin and VEGF, respectively. The top spongy region can guarantee the efficient, safe, and controllable loading of VEGF up to 1  μg/cm² in 1 minute, providing a distinctive real-time loading capacity for saving the bioactivity. Based on this, we demonstrate that our rapamycin-VEGF hierarchical coating impressively promoted the competitive growth of endothelial cells over smooth muscle cells (ratio of EC/SMC~25) while relieving the adverse impact of rapamycin to ECs. We further conducted the real-time loading of VEGF on stents and demonstrate that the hierarchical combination of rapamycin and VEGF showed remarkable endothelium regeneration while maintaining a very low level of in-stent restenosis. This work paves an avenue for the combination of both hydrophobic and hydrophilic functional molecules, which should benefit the next generation of DES and may extend applications to diversified combination medical devices.

Biofunctionalization of artificial nerve implants by incorporation of specific bioactive factors has greatly enhanced the success of grafting procedures for peripheral nerve regeneration. However, most studies on novel biofunctionalized implants have emphasized the promotion of neuronal and axonal repair over vascularization, a process critical for long-term functional restoration. We constructed a dual-biofunctionalized chitosan/collagen composite scaffold with Ile-Lys-Val-Ala-Val (IKVAV) and vascular endothelial growth factor (VEGF) by combining solution blending, in situ lyophilization, and surface biomodification. Immobilization of VEGF and IKVAV on the scaffolds was confirmed both qualitatively by staining and quantitatively by ELISA. Various single- and dual-biofunctionalized scaffolds were compared for the promotion of endothelial cell (EC) and Schwann cell (SC) proliferation as well as the induction of angiogenic and neuroregeneration-associated genes by these cells in culture. The efficacy of these scaffolds for vascularization was evaluated by implantation in chicken embryos, while functional repair capacity in vivo was assessed in rats subjected to a 10 mm sciatic nerve injury. Dual-biofunctionalized scaffolds supported robust EC and SC proliferation and upregulated the expression levels of multiple genes and proteins related to neuroregeneration and vascularization. Dual-biofunctionalized scaffolds demonstrated superior vascularization induction in embryos and greater promotion of vascularization, myelination, and functional recovery in rats. These findings support the clinical potential of VEGF/IKVAV dual-biofunctionalized chitosan/collagen composite scaffolds for facilitating peripheral nerve regeneration, making it an attractive candidate for repairing critical nerve defect. The study may provide a critical experimental and theoretical basis for the development and design of new artificial nerve implants with excellent biological performance.

Noninvasive in vivo imaging of hepatic glutathione (GSH) levels is essential to early diagnosis and prognosis of acute hepatitis. Although GSH-responsive fluorescence imaging probes have been reported for evaluation of hepatitis conditions, the low penetration depth of light in liver tissue has impeded reliable GSH visualization in the human liver. We present a liver-targeted and GSH-responsive trimodal probe (GdNPs-Gal) for rapid evaluation of lipopolysaccharide- (LPS-) induced acute liver inflammation via noninvasive, real-time in vivo imaging of hepatic GSH depletion. GdNPs-Gal are formed by molecular coassembly of a GSH-responsive Gd(III)-based MRI probe (1-Gd) and a liver-targeted probe (1-Gal) at a mole ratio of 5/1 (1-Gd/1-Gal), which shows high r_1 relaxivity with low fluorescence and fluorine magnetic resonance spectroscopic (¹⁹F-MRS) signals. Upon interaction with GSH, 1-Gd and 1-Gal are cleaved and GdNPs-Gal rapidly disassemble into small molecules 2-Gd, 2-Gal, and 3, producing a substantial decline in r_1 relaxivity with compensatory enhancements in fluorescence and ¹⁹F-MRS. By combining in vivo magnetic resonance imaging (¹H-MRI) with ex vivo fluorescence imaging and ¹⁹F-MRS analysis, GdNPs-Gal efficiently detect hepatic GSH using three independent modalities. We noninvasively visualized LPS-induced liver inflammation and longitudinally monitored its remediation in mice after treatment with an anti-inflammatory drug, dexamethasone (DEX). Findings highlight the potential of GdNPs-Gal for in vivo imaging of liver inflammation by integrating molecular coassembly with GSH-driven disassembly, which can be applied to other responsive molecular probes for improved in vivo imaging.

The development of optoelectronic devices requires breakthroughs in new material systems and novel device mechanisms, and the demand recently changes from the detection of signal intensity and responsivity to the exploration of sensitivity of polarized state information. Two-dimensional (2D) materials are a rich family exhibiting diverse physical and electronic properties for polarization device applications, including anisotropic materials, valleytronic materials, and other hybrid heterostructures. In this review, we first review the polarized-light-dependent physical mechanism in 2D materials, then present detailed descriptions in optical and optoelectronic properties, involving Raman shift, optical absorption, and light emission and functional optoelectronic devices. Finally, a comment is made on future developments and challenges. The plethora of 2D materials and their heterostructures offers the promise of polarization-dependent scientific discovery and optoelectronic device application.

This review article surveys the recent experimental findings that suggest alternative chemical models of directed chirality amplification at the early, prebiotic Earth. It is believed that the chirality amplification step followed the initial emergence of small enantiomeric imbalance and preceded (as a necessary condition) the occurrence of homochiral biopolymers, assembled from enantiomerically pure building blocks. This work focuses on the chemical nature of possible mechanisms of primordial chirality enhancement, without going into detail of the preceding and subsequent phases of origination of biological homochirality and life on Earth. These mechanisms are discussed through the prism of integrity of biological natural selection and chemical kinetic selection.

Numerous experiments have demonstrated that the metal atom is the active center of monoatomic catalysts for hydrogen evolution reaction (HER), while the active sites of nonmetal doped atoms are often neglected. By combining theoretical prediction and experimental verification, we designed a unique ternary Ru-N₄-P coordination structure constructed by monodispersed Ru atoms supported on N,P dual-doped graphene for highly efficient hydrogen evolution in acid solution. The density functional theory calculations indicate that the charge polarization will lead to the most charge accumulation at P atoms, which results in a distinct nonmetallic P active sites with the moderate H\ast adsorption energy. Notably, these P atoms mainly supply highly efficient catalytic sites with ultrasmall absorption energy of 0.007 eV. Correspondingly, the Ru-N₄-P demonstrated outstanding HER performance not only in an acidic condition but also in alkaline environment. Notably, the performance of Ru-NPC catalyst at high current is even superior to the commercial Pt/C catalysts, whether in acidic or alkaline medium. Our in situ synchrotron radiation infrared spectra demonstrate that a P-H_ads intermediate is continually emerging on the Ru-NPC catalyst, actively proving the nonmetallic P catalytically active site in HER that is very different with previously reported metallic sites.

Mg-based micromotors have emerged as an extremely attractive artificial micro/nanodevice, but suffered from uncontrollable propulsion and limited motion lifetime, restricting the fulfillment of complex tasks. Here, we have demonstrated Mg-based micromotors composed of Mg microspheres asymmetrically coated with Pt and temperature-sensitive poly(N-isopropylacrylamide) (PNIPAM) hydrogel layers in sequence. They can implement different motion behaviors stemming from the driving mechanism transformation when encountering catalyzed substrates such as H₂O₂ and respond to both H₂O₂ concentration and temperature in aqueous environment. The as-constructed Mg-based micromotors are self-propelled by Pt-catalyzed H₂O₂ decomposition following the self-consuming Mg-H₂O reaction. In this case, they could further generate bilateral bubbles and thus demonstrate unique self-limitation motion like hovering when the phase transformation of PNIPAM is triggered by decreasing temperature or when the H₂O₂ concentration after permeating across the PNIPAM hydrogel layer is high enough to facilitate bubble nucleation. Our work for the first time provides a stimuli-induced “hovering” strategy for self-propelled micromotors, which endows Mg-based micromotors with an intelligent response to the surroundings besides the significant extension of their motion lifetime.