Wireless-Channel Key Distribution Based on Laser Synchronization.

We propose and experimentally demonstrate a wireless-channel key distribution scheme based on laser synchronization induced by a common wireless random signal. Two semiconductor lasers are synchronized under injection of the drive signal after electrical-optical conversion and emit irregular outputs that are used to generate shared keys. Our proof-of-concept experiment using a complex drive signal achieved a secure key generation rate of up to 150 Mbit/s with a bit error rate below 3.8 × 10-3. Numerical simulation results show that the proposed scheme has the potential to achieve a distribution distance of several hundred meters. It is believed that common-signal-induced laser synchronization paves the way for high-speed wireless physical-layer key distribution.

Efficient Charge Separation and Transport in Fullerene-CuPcOC8 Donor-Acceptor Nanorod Enhancing Photocatalytic Hydrogen Generation.

Photocatalytic hydrogen generation via water decomposition is a promising avenue in the pursuit of large-scale, cost-effective renewable hydrogen energy generation. However, the design of an efficient photocatalyst plays a crucial role in achieving high yields in hydrogen generation. Herein, we have engineered a fullerene-2,3,9,10,16,17,23,24-octa(octyloxy)copper phthalocyanine (C60-CuPcOC8) photocatalyst, achieving both efficient hydrogen generation and high stability. The significant donor-acceptor (D-A) interactions facilitate the efficient electron transfer from CuPcOC8 to C60. The rate of photocatalytic hydrogen generation for C60-CuPcOC8 is 8.32 mmol·g-1·h-1, which is two orders of magnitude higher than the individual C60 and CuPcOC8. The remarkable increase in hydrogen generation activity can be attributed to the development of a robust internal electric field within the C60-CuPcOC8 assembly. It is 16.68 times higher than that of the pure CuPcOC8. The strong internal electric field facilitates the rapid separation within 0.6 ps, enabling photogenerated charge transfer efficiently. Notably, the hydrogen generation efficiency of C60-CuPcOC8 remains above 95%, even after 10 h, showing its exceptional photocatalytic stability. This study provides critical insight into advancing the field of photocatalysis.

Development towards high-resolution kHz-speed rotation-free volumetric imaging.

X-ray multi-projection imaging (XMPI) has the potential to provide rotation-free 3D movies of optically opaque samples. The absence of rotation enables superior imaging speed and preserves fragile sample dynamics by avoiding the centrifugal forces introduced by conventional rotary tomography. Here, we present our XMPI observations at the ID19 beamline (ESRF, France) of 3D dynamics in melted aluminum with 1000 frames per second and 8 µm resolution per projection using the full dynamical range of our detectors. Since XMPI is a method under development, we also provide different tests for the instrumentation of up to 3000 frames per second. As the high-brilliance of 4th generation light-sources becomes more available, XMPI is a promising technique for current and future X-ray imaging instruments.

A High-Tryptophan Diet Alleviated Cognitive Impairment and Neuroinflammation in APP/PS1 Mice through Activating Aryl Hydrocarbon Receptor via the Regulation of Gut Microbiota.

SCOPE: Recent studies have highlighted the vital role of gut microbiota in the pathogenesis of Alzheimer's disease (AD). However, the effect of the regulation of gut microbiota by dietary components on AD remains unknown. Thus, the study explored that a high-tryptophan (Trp) diet alleviates cognitive impairment by regulating microbiota. METHODS AND RESULTS: Male APP/PS1 mice are fed 0.5% Trp diet for 4 weeks, and then cognitive function, amyloid-ß (Aß) deposition, microglial activation, proinflammatory cytokines production, and gut microbiota are detected. Moreover, the level of aryl hydrocarbon receptor (AhR) and NF-κB pathway related protein are determined. The results show that high-Trp diet significantly alleviates cognitive impairment and Aß deposits. Moreover, high-Trp diet significantly inhibits activation of microglia, decreases the level of cluster of differentiation 11b (CD11b), and restrains the activation markers of microglia, such as cyclooxygenase-2 (Cox-2), interleukin (IL)-1ß, and IL-6. Notably, high-Trp diet significantly activates AhR, inhibits the phosphorylation of p65, and improves microbiota dysbiosis. CONCLUSIONS: These findings demonstrated that high-Trp diet exerts anti-inflammatory effects via upregulating AhR and suppressing NF-κB pathway, and its mechanisms may be mediated by regulating gut microbiota, suggesting that Trp diet may be a potential strategy for AD intervention.

Co-encapsulation of curcumin and anthocyanins in bovine serum album-fucoidan nanocomplex with a two-step pH-driven method.

BACKGROUND: Curcumin (CUR) and anthocyanins (ACN) are recommended due to their bioactivities. However, their nutritional values and health benefits are limited by their low oral bioavailability. The incorporation of bioactive substances into polysaccharide-protein composite nanoparticles is an effective way to enhance their bioavailability. Accordingly, this study explored the fabrication of bovine serum albumin (BSA)-fucoidan (FUC) hybrid nanoparticles using a two-step pH-driven method for the delivery of CUR and ACN. RESULTS: Under a 1:1 weight ratio of BSA to FUC, the point of zero charge moved from pH ⁓ 4.7 for BSA to around 2.5 for FUC-coated BSA, and the formation of BSA-FUC nanocomplex was pH-dependent by showing the maximum CUR emission wavelength shifting from 546 nm (CUR-loaded BSA-FUC at pH 4.7) and 544 nm (CUR/ACN-loaded BSA-FUC nanoparticles at pH 4.7) to 540 nm (CUR-loaded BSA-FUC at pH 6.0) and 539 nm (CUR/ACN-loaded BSA-FUC nanoparticles at pH 6.0). Elevated concentrations of NaCl from 0 to 2.5 mol L-1 caused particle size increase from about 250 to about 800 nm, but showing no effect on the encapsulation efficiency of CUR. The CUR and ACN entrapped, respectively, in the inner and outer regions of the BSA-FUC nanocomplex were released at different rates. After incubation for 10 h, more than 80% of ACN was released, while less than 25% of CUR diffused into the receiving medium, which fitted well to Logistic and Weibull models. CONCLUSION: In summary, the BSA-FUC nanocomposites produced by a two-step pH-driven method could be used for the co-delivery of hydrophilic and hydrophobic nutraceuticals. © 2023 Society of Chemical Industry.

Security optimization of synchronization in DFB lasers under constant-amplitude random-phase drive light by reducing drive-response correlation.

Common-signal-induced laser synchronization promoted a promising paradigm of high-speed physical key distribution. Constant-amplitude and random-phase (CARP) light was proposed as the common drive signal to enhance security by reducing the correlation between the drive and the laser response in intensity. However, the correlation in light phase is not examined. Here, we numerically reveal that the correlation coefficient of the CARP light phase and the response laser intensity (denoted as CCR-φD) can reach a value close to 0.6. Effects of parameters including optical frequency detuning, and modulation depth and noise bandwidth and transparency carrier density for CARP light generation are investigated in detail. By optimizing the optical frequency, modulation depth, and noise bandwidth, respectively, CCR-φD can be reduced to 0.32, 0.18, and 0.10. In the meantime, CCR-φD can be further reduced through secondary optimizing of parameters. CCR-φD can be further reduced by increasing transparent carrier density provided response laser synchronization is achieved. This work gives a new insight about the laser synchronization induced by common CARP light, and also contributes a suggestion of security improvement for physical key distribution based on laser synchronization.

Revealing the origins of vortex cavitation in a Venturi tube by high speed X-ray imaging.

Hydrodynamic cavitation is useful in many processing applications, for example, in chemical reactors, water treatment and biochemical engineering. An important type of hydrodynamic cavitation that occurs in a Venturi tube is vortex cavitation known to cause luminescence whose intensity is closely related to the size and number of cavitation events. However, the mechanistic origins of bubbles constituting vortex cavitation remains unclear, although it has been concluded that the pressure fields generated by the cavitation collapse strongly depends on the bubble geometry. The common view is that vortex cavitation consists of numerous small spherical bubbles. In the present paper, aspects of vortex cavitation arising in a Venturi tube were visualized using high-speed X-ray imaging at SPring-8 and European XFEL. It was discovered that vortex cavitation in a Venturi tube consisted of angulated rather than spherical bubbles. The tangential velocity of the surface of vortex cavitation was assessed considering the Rankine vortex model.

Chaos synchronization of VCSELs with common injection of polarization-random light.

We propose and numerically demonstrate chaos synchronization of two vertical-cavity surface-emitting lasers (VCSELs) induced by common injection of constant-amplitude random-polarization light for physical key distribution. Results show that synchronization is sensitive to polarization rotation of injection light, and synchronization coefficients larger than 0.9 can be achieved as the rotation-degree mismatch is smaller than ±10°. Therefore, polarization rotation degree can serve as a hardware key parameter. Furthermore, each laser's output has no correlation to the constant amplitude of the injected light. Their components with identical polarization state, e.g. x or y polarization of VCSEL, also have low correlation coefficient smaller than 0.2. It is therefore believed that this synchronization scheme can provide a security-enhanced method of physical key distribution.

Enzymatically Activatable Polymers for Disease Diagnosis and Treatment.

The irregular expression or activity of enzymes in the human body leads to various pathological disorders and can therefore be used as an intrinsic trigger for more precise identification of disease foci and controlled release of diagnostics and therapeutics, leading to improved diagnostic accuracy, sensitivity, and therapeutic efficacy while reducing systemic toxicity. Advanced synthesis strategies enable the preparation of polymers with enzymatically activatable skeletons or side chains, while understanding enzymatically responsive mechanisms promotes rational incorporation of activatable units and predictions of the release profile of diagnostics and therapeutics, ultimately leading to promising applications in disease diagnosis and treatment with superior biocompatibility and efficiency. By overcoming the challenges, new opportunities will emerge to inspire researchers to develop more efficient, safer, and clinically reliable enzymatically activatable polymeric carriers as well as prodrugs.

Online dynamic flat-field correction for MHz microscopy data at European XFEL.

The high pulse intensity and repetition rate of the European X-ray Free-Electron Laser (EuXFEL) provide superior temporal resolution compared with other X-ray sources. In combination with MHz X-ray microscopy techniques, it offers a unique opportunity to achieve superior contrast and spatial resolution in applications demanding high temporal resolution. In both live visualization and offline data analysis for microscopy experiments, baseline normalization is essential for further processing steps such as phase retrieval and modal decomposition. In addition, access to normalized projections during data acquisition can play an important role in decision-making and improve the quality of the data. However, the stochastic nature of X-ray free-electron laser sources hinders the use of standard flat-field normalization methods during MHz X-ray microscopy experiments. Here, an online (i.e. near real-time) dynamic flat-field correction method based on principal component analysis of dynamically evolving flat-field images is presented. The method is used for the normalization of individual X-ray projections and has been implemented as a near real-time analysis tool at the Single Particles, Clusters, and Biomolecules and Serial Femtosecond Crystallography (SPB/SFX) instrument of EuXFEL.

Enhancing the Gene Transfection of Poly(ß-amino ester)/DNA Polyplexes by Modular Manipulation of Amphiphilicity.

Poly(ß-amino ester)s (PAEs) have been widely developed for gene delivery, and hydrophobic modification can further enhance their gene transfection efficiency. However, systematic manipulation of amphiphilicity of PAEs through copolymerization with hydrophobic monomers is time-consuming and, to some extent, uncontrollable. Here, a modular strategy is developed to manipulate the amphiphilicity of the PAE/DNA polyplexes. A hydrophobic polymer (DD-C12-122) and a hydrophilic polymer (DD-90-122) are synthesized separately and used as a hydrophobic module and a hydrophilic module, respectively. The amphiphilicity of polyplexes could be manipulated by changing the ratio of the hydrophobic module and hydrophilic module. Using the modular strategy, the PAE/DNA polyplexes with the highest gene transfection efficiency and safety profile as well as possible mechanisms are identified. The modular strategy provides a novel way to engineer the hydrophobicity of PAEs to improve their gene transfection and can be easily generalized and potentially extended to other polymeric gene delivery systems.

Interfullerene Electronic Interactions and Excited-State Dynamics in Fullerene Dumbbell Conjugates.

Several dumbbell conjugates featuring M3N@Ih-C80 (M = Sc, Y) and C60 were prepared to systematically investigate interfullerene electronic interactions and excited state dynamics. From electrochemical investigations, we concluded that the redox potentials of our M3N@Ih-C80 (M = Sc, Y) dumbbells depend largely on the interfullerene electronic interactions. Assisted by DFT calculation, the unique role of metal atoms was highlighted. Most importantly, ultrafast spectroscopy experiments revealed symmetry-breaking charge separation in Sc3N@C80-dumbbell to yield an unprecedented (Sc3N@C80)•+-(Sc3N@C80)•- charge separated state. This is, to the best of our knowledge, the first time that symmetry-breaking charge separation following photoexcitation is corroborated in a fullerene system. As such, our work shed light on the significance of interfullerene electronic interactions and their uniqueness for modulating excited state properties.

Programmable Complex Shape Changing of Polysiloxane Main-Chain Liquid Crystalline Elastomers.

Liquid crystal elastomers (LCEs) are shape-morphing materials whose large and reversible shape transformations are caused by the coupling between the mobile anisotropic properties of liquid crystal (LC) units and the rubber elastic of polymer networks. Their shape-changing behaviors under certain stimuli are largely directed by the LC orientation; therefore, various strategies have been developed to spatially modulate the LC alignments. However, most of these methods are limited as they require complex fabrication technologies or have intrinsic limitations in applicability. To address this issue, programmable complex shape changes in some LCE types, such as polysiloxane side-chain LCEs, thiol-acrylate main-chain LCEs, etc., were achieved by using a mechanical alignment programming process coupled with two-step crosslinking. Here, we report a polysiloxane main-chain LCE with programmable 2- and 3D shape-changing abilities that were created by mechanically programming the polydomain LCE with two crosslinking steps. The resulting LCEs exhibited a reversible thermal-induced shape transformation between the initial and programmed shapes due to the two-way memory between the first and second network structures. Our findings expand on the applications of LCE materials in actuators, soft robotics, and smart structures where arbitrary and easily programmed shape morphing is needed.

Effect of gastrodin against cognitive impairment and neurodegeneration in APP/PS1 mice via regulating gut microbiota-gut-brain axis.

Gastrodin (Gas) has exhibited protective activity in neurological disorders. Here, we investigated the neuroprotective effect and potential mechanisms of Gas against cognitive impairment via regulating gut microbiota. APPswe/PSEN1dE9 transgenic (APP/PS1) mice were treated intragastrically with Gas for 4 weeks, and then cognitive deficits, deposits of amyloid-ß (Aß) and phosphorylation of tau were analyzed. The expression levels of insulin-like growth factor-1 (IGF-1) pathway-related proteins, such as cAMP response element-binding protein (CREB), were detected. Meanwhile, gut microbiota composition was evaluated. Our results showed that Gas treatment significantly improved cognitive deficits and Aß deposition in APP/PS1 mice. Moreover, Gas treatment increased the level of Bcl-2 and decreased level of Bax and ultimately inhibited neuronal apoptosis. Gas treatment markedly increased the expression levels of IGF-1 and CREB in APP/PS1 mice. Moreover, Gas treatment improved abnormal composition and structure of gut microbiota in APP/PS1 mice. These findings revealed that Gas actively participated in regulating the IGF-1 pathway to inhibit neuronal apoptosis via the gut-brain axis and that it can be considered a new therapeutic strategy against Alzheimer's disease.

Phosphocholine-Functionalized Zwitterionic Highly Branched Poly(ß-amino ester)s for Cytoplasmic Protein Delivery.

Proteins have tremendous potential for vaccine development and disease treatment, but multiple extracellular and intracellular biological barriers must be overcome before they can exert specific biological functions in the target tissue. The use of polymers as carriers would greatly improve their bioavailability and therapeutic efficiency. Nevertheless, effective protein packaging and cell membrane penetration without causing cytotoxicity is particularly challenging, due largely to the simultaneous distribution of positive and negative charges on protein surface. Here, phosphocholine-functionalized zwitterionic poly(ß-amino ester)s, HPAE-D-(±), are developed for cytoplasmic protein delivery. The zwitterionic phosphocholine is capable of binding to both proteins and the cell membrane to facilitate protein packaging and nanoparticle cellular uptake. Compared to amine-functionalized HPAE-E-(+) and carboxylic acid-functionalized HPAE-C-(-), HPAE-D-(±) exhibits much higher cytoplasmic protein delivery efficiency and lower cytotoxicity. In addition, HPAE-D-(±) are readily degraded in aqueous solution. This strategy may be extended to other zwitterions and polymers, thus having profound implications for the development of safe and efficient protein delivery systems.

Carbon microspheres built of La2O3 quantum dots-implanted nanorods: Superb hosts with ultra-long Li2Sn-catalysis durability.

Practical utilization of Li-sulfur batteries (LSBs) is still hindered by the sulfur cathode side due to its inferior electrical conductivity, huge volume expansion and adverse polysulfide shuttling effects. Though using polar catalysts coupled with mesoporous carbons may well surmount these barriers, such unsheltered catalysts rarely survive due to oversaturated polysulfide adsorption and extra sulfuration side reactions. To overcome above constrains, we herein propose to implant highly reactive nanocatalysts into carbon matrix with few nanometers insertion depth for mechanical protection. As a paradigm study, we have embedded La2O3-quantum dots (QDs) into carbon nanorods, which are then assembled into carbon microspheres (CMs). As evaluated, La2O3 QDs-CMs can help elevate the cathode redox reaction kinetics and sulfur utilization ratios, delivering a large capacity of 1392 mAh g-1 at 0.25C and high-capacity retention of 76% after total cycling. The thin carbon layers on La2O3 QDs exert a key role in impeding excess polysulfide accumulation on catalysts and thus prevent their deactivation/failure. Our strategy may guide a smart way to make catalysts-involved sulfur cathode systems with ultra-long working durability for LSBs applications.

Self-powered, light-controlled, bioresorbable platforms for programmed drug delivery.

Degradable polymer matrices and porous scaffolds provide powerful mechanisms for passive, sustained release of drugs relevant to the treatment of a broad range of diseases and conditions. Growing interest is in active control of pharmacokinetics tailored to the needs of the patient via programmable engineering platforms that include power sources, delivery mechanisms, communication hardware, and associated electronics, most typically in forms that require surgical extraction after a period of use. Here we report a light-controlled, self-powered technology that bypasses key disadvantages of these systems, in an overall design that is bioresorbable. Programmability relies on the use of an external light source to illuminate an implanted, wavelength-sensitive phototransistor to trigger a short circuit in an electrochemical cell structure that includes a metal gate valve as its anode. Consequent electrochemical corrosion eliminates the gate, thereby opening an underlying reservoir to release a dose of drugs by passive diffusion into surrounding tissue. A wavelength-division multiplexing strategy allows release to be programmed from any one or any arbitrary combination of a collection of reservoirs built into an integrated device. Studies of various bioresorbable electrode materials define the key considerations and guide optimized choices in designs. In vivo demonstrations of programmed release of lidocaine adjacent the sciatic nerves in rat models illustrate the functionality in the context of pain management, an essential aspect of patient care that could benefit from the results presented here.

Regioisomeric Benzidine-Fullerenes: Tuning of the Diverse Hole-Distribution to Influence Charge Separation Patterns.

Understanding the influence of molecular structure on charge distribution and charge separation (CS) provides essential guidance for optoelectronic materials design. Here we propose a regioisomeric strategy to tune the diverse hole-distribution, and probe the influence on CS patterns. Para-, meta- and ortho-substituted benzidine-fullerene, named 1 p, 1 m and 1 o are designed. Following CS, hole-delocalization occurs in 1 p, while hole-localization exists in 1 m and 1 o. The rates of charge separation (4.02×1011  s-1 ) and recombination (9.8×109  s-1 ) of 1 p is about 20 and 12 times faster than 1 m and 1 o, indicating that para-determined delocalization promotes ultrafast CS, while meta- and ortho-generated localization contributes to long-lived CS states. Computational analysis further implies that localization results from the destruction of electronic conjugation for 1 m, and limitation of conformational relaxation for 1 o. Given that the universality and simplicity of regional isomerism, this work opens up new thoughts for molecular design with tunable charge separation patterns.

Fabrication of foxtail millet prolamin/caseinate/chitosan hydrochloride composite nanoparticles using antisolvent and pH-driven methods for curcumin delivery.

Co-assembled foxtail millet (FP)-sodium casein (NaCas) nanocomplex and NaCas coated FP nanoparticles (NPs) were produced by using pH-cycle and anti-solvent methods, respectively. Subsequently, the effects of chitosan hydrochloride (CHC) coating on the particle size, surface charge and physicochemical stability of the two different FP/NaCas nanoparticles (NPs) were evaluated. With the addition of CHC, the particle size of NaCas coated FP NPs and co-assembled FP-NaCas nanocomplex significantly increased from 128.3 nm and 69.5 nm to 183.5 nm and 113.8 nm, respectively. The stability of the two kinds of CHC coated FP-based NPs to different pH values and varying ionic strengths was different due to their different NP structures. Using different fabrication formulations, co-assembled FP-NaCas NPs entrapped curcumin in relatively hydrophilic microenvironment and showed higher curcumin retention rate in comparison with NaCas coated FP NPs in terms of long-term storage stability. The results revealed that the produced CHC coated FP/NaCas nanocomplexes could be very beneficial in entrapping and delivering bioactive substances.

Physical-layer key distribution based on commonly-driven laser synchronization with random modulation of drive light.

We propose and experimentally demonstrate a physical-layer key distribution scheme using commonly-driven laser synchronization with random modulation of drive light. Two parameter-matched semiconductor lasers injected by a common complex drive light are used as entropy sources for legitimate users. Legitimate users generate their own random signal by randomly time-division multiplexing of two random sequences with a certain duration according to individual control codes, and then independently modulate the drive light. Laser synchronization is achieved during time slots when the modulation sequences of two users are identical, and thus provide highly correlated randomness for extracting random numbers as shared keys. Experimental results show that the random modulation of the drive light reduces the correlation between the drive light and laser outputs. In addition, laser synchronization is sensitive to the modulation delay and then the latter can be used as an additional hardware parameter. These mean that security is enhanced. In addition, the proposed method has a short laser synchronization recovery time of lower than 1.1 ns, meaning a high rate of key distribution. The upper limit of final key rate of 2.55 Gb/s with a criterion of bit error rate of 1.68 × 10-3 is achieved in experiments. Our results provide a promising candidate for protecting the security of optical fiber communication.