Super-Resolution Fluorescence Microscopy Study of the Production of K1 Capsules by Escherichia coli: Evidence for the Differential Distribution of the Capsule at the Poles and the Equator of the Cell.

The production of Escherichia coli K1 serotype capsule was investigated using direct stochastic optical reconstruction microscopy with live bacteria and graphene oxide-coated coverslips, overcoming many morphological artifacts found in other high-resolution imaging techniques. Super-resolution fluorescence images showed that the K1 capsular polysaccharide is not uniformly distributed on the cell surface, as previously thought. These studies demonstrated that on the cell surfaces the K1 capsule at the poles had bimodal thicknesses of 238 ± 41 and 323 ± 62 nm, whereas at the equator, there was a monomodal thickness of 217 ± 29 nm. This bimodal variation was also observed in high-pressure light-scattering chromatography measurements of purified K1 capsular polysaccharide. Particle tracking demonstrated that the formation of the capsule was dominated by the expansion of lyso-phosphatidylglycerol (lyso-PG) rafts that anchor the capsular polysaccharide in the outer membrane, and the expansion of these rafts across the cell surface was driven by new material transported through the capsular biosynthesis channels. The discovery of thicker capsules at the poles of the cell will have implications in mediating interactions between the bacterium and its immediate environment.

Reversible Thermoresponsive Peptide-PNIPAM Hydrogels for Controlled Drug Delivery.

Mixed thermoreversible gels were successfully fabricated by the addition of a thermosensitive polymer, poly(N-isopropylacrylamide) (PNIPAM), to fibrillar nanostructures self-assembled from a short peptide I3K. When the temperature was increased above the lower critical solution temperature of the PNIPAM, the molecules collapsed to form condensed globular particles, which acted as cross-links to connect different peptide nanofibrils and freeze their movements, resulting in the formation of a hydrogel. Since these processes were physically driven, such hydrogels could be reversibly switched between the sol and gel states as a function of temperature. As a model peptide, I3K was formulated with PNIPAM to produce a thermoreversible sol-gel system with a transition temperature of ∼33 °C, which is just below the body temperature. The antibacterial peptide of G(IIKK)3I-NH2 could be conveniently encapsulated in the hydrogel by the addition of the solution at lower temperatures in the sol phase and then increasing the temperature to be above 33 °C for gelation. The hydrogel gave a sustained and controlled linear release of G(IIKK)3I-NH2 over time. Using the peptide nanofibrils as three-dimensional scaffolds, such thermoresponsive hydrogels mimic the extracellular matrix and could potentially be used as injectable hydrogels for minimally invasive drug delivery or tissue engineering.

Determination of PMMA Residues on a Chemical-Vapor-Deposited Monolayer of Graphene by Neutron Reflection and Atomic Force Microscopy.

Chemical vapor deposition (CVD) is now a well-established method for creating monolayer graphene films. In this method, poly(methyl methacrylate) (PMMA) films are often coated onto monolayer graphene films to make them mechanically robust enough for transfer and further handling. However, it is found that PMMA is hard to remove entirely, and any residual polymers remaining can affect graphene's properties. We demonstrate here a method to determine the amount of PMMA remaining on the graphene sheet fabricated from CVD by a combined study of Raman scattering, atomic force microscopy, and neutron reflection. Neutron reflectivity is a powerful technique which is particularly sensitive to any interfacial structure, so it is able to investigate the density profile of the residual PMMA in the direction perpendicular to the graphene film surface. After the standard process of PMMA removal by acetone-IPA cleaning, we found that the remaining PMMA film could be represented as a two-layer model: an inner layer with a thickness of 17 Å and a roughness of 1 Å mixed with graphene and an outer diffuse layer with an average thickness of 31 Å and a roughness of 4 Å well mixed with water. On the basis of this model analysis, it was demonstrated that the remaining PMMA still occupied a significant fraction of the graphene film surface.

Analysis of the Tensile Properties and Probabilistic Characteristics of Large-Tow Carbon Fiber-Reinforced Polymer Composites.

Large-tow carbon fiber-reinforced polymer composites (CFRP) have great application potential in civil engineering due to their low price, but their basic mechanical properties are still unclear. The tensile properties of large-tow CFRP rods and plates were investigated in this study. First, the tensile properties of unidirectional CFRP rods and plates were studied, and the test results of the relevant mechanical properties were statistically analyzed. The tensile strength of the CFRP rod and plate are 2005.97 MPa and 2069.48 MPa. Second, the surface of the test specimens after failure was observed using a scanning electron microscope to analyze the type of failure and damage evolution process. Finally, the probabilistic characteristics of the mechanical properties were analyzed using normal, lognormal, and Weibull distributions for parameter fitting. Quasi-optimality tests were performed, and a probability distribution model was proposed for the mechanical properties of large-tow CFRP rods and plates.

U-shaped convolutional transformer GAN with multi-resolution consistency loss for restoring brain functional time-series and dementia diagnosis.

Introduction: The blood oxygen level-dependent (BOLD) signal derived from functional neuroimaging is commonly used in brain network analysis and dementia diagnosis. Missing the BOLD signal may lead to bad performance and misinterpretation of findings when analyzing neurological disease. Few studies have focused on the restoration of brain functional time-series data. Methods: In this paper, a novel U-shaped convolutional transformer GAN (UCT-GAN) model is proposed to restore the missing brain functional time-series data. The proposed model leverages the power of generative adversarial networks (GANs) while incorporating a U-shaped architecture to effectively capture hierarchical features in the restoration process. Besides, the multi-level temporal-correlated attention and the convolutional sampling in the transformer-based generator are devised to capture the global and local temporal features for the missing time series and associate their long-range relationship with the other brain regions. Furthermore, by introducing multi-resolution consistency loss, the proposed model can promote the learning of diverse temporal patterns and maintain consistency across different temporal resolutions, thus effectively restoring complex brain functional dynamics. Results: We theoretically tested our model on the public Alzheimer's Disease Neuroimaging Initiative (ADNI) dataset, and our experiments demonstrate that the proposed model outperforms existing methods in terms of both quantitative metrics and qualitative assessments. The model's ability to preserve the underlying topological structure of the brain functional networks during restoration is a particularly notable achievement. Conclusion: Overall, the proposed model offers a promising solution for restoring brain functional time-series and contributes to the advancement of neuroscience research by providing enhanced tools for disease analysis and interpretation.

Promoted Na Solubility and Modified Band Structure for Achieving Exceptional Average ZT by Extra Mn Doping in PbTe.

Na doping strategy provides an effective avenue to upgrade the thermoelectric performance of PbTe-based materials by optimizing electrical properties. However, the limited solubility of Na inherently restricts the efficiency of doping, resulting in a relatively low average ZT, which poses challenges for the development and application of subsequent devices. Herein, to address this issue, the introduced spontaneous Pb vacancies and additional Mn doping synergistically promote Na solubility with a further modified valence band structure. Furthermore, the induced massive point defects and multiscale microstructure greatly strengthen the scattering of phonons over a wide frequency range, leading to a remarkable ultralow lattice thermal conductivity of ∼0.42 W m-1 K-1. As a result, benefiting from the significantly enhanced Seebeck coefficient and superior thermal transports, a high peak ZT of ∼2.1 at 773 K and an excellent average ZT of ∼1.4 between 303 and 823 K are simultaneously achieved in Pb0.93Na0.04Mn0.02Te. This work proposes a simple and constructive method to obtain high-performance PbTe-based materials and is promising for the development of thermoelectric power generation devices.

Hybrid mesh for magnetotelluric forward modeling based on the finite element method.

Unstructured tetrahedral grids have been applied in magnetotelluric (MT) forward modeling using the finite element (FE) method because of their adaptability to complex anomalies. However, high-quality results require an extreme refinement of the near-surface area, which leads to excessive meshes and an increased degree of freedom (DoF) of the governing equation of the finite element system. To reduce the computational cost, we have developed a hybrid mesh based on triangular prisms and tetrahedrons. The required elements in the near-surface area are reduced because the quality of the triangular prism is not limited by the element aspect ratio. The deep area is discretized by tetrahedral elements to ensure the flexibility of the unstructured grids. The superiority of this hybrid mesh has been tested on a layered model, the DTM1 model and terrain relief models. The results show that the modeling efficiency has been improved, especially for high-frequency data. The accuracy of the modeling using the hybrid mesh is significantly higher than that of the tetrahedral mesh with a similar DoF. Usage of the hybrid mesh can be easily adapted to complex geoelectric models with strong terrain fluctuations, which requires less computational cost than using conventional unstructured elements.

A model-driven approach for fast modeling of three-dimensional laser point cloud in large substation.

Using point cloud to reconstruct the 3D model of a substation is crucial for smart grid operation. Its main objective is to swiftly capture equipment point cloud data and align each device's model within the large and noisy point cloud scene of the substation. However, substation reconstruction needs improvement due to the low efficiency of traditional noise-resistant clustering methods and challenges in accurately classifying similar-looking electrical equipment. This paper proposes an automatic modeling framework for large-scale substation point cloud scenes. Firstly, we reduce the substation scene's dimensionality to improve clustering efficiency and establish relationships between data dimensions using a re-clustering algorithm. Next, a neural network is developed to identify various device types within clusters, even with limited subdivisions. Finally, a model library is employed to register standard models onto the target device's point cloud, obtaining device types and orientations. Real substation data processing demonstrates the ability to rapidly extract devices from complex and noisy point cloud scenes, effectively avoiding missegmentation issues. The automatic modeling approach achieves a precise substation calculation rate of 92.86%.

Band engineering enhances thermoelectric performance of Ag-doped Sn0.98Se.

Ag doping can effectively increase the carrier concentration ofp-type SnSe polycrystalline, thereby enhancing the thermoelectric (TE) performance. However, the key role of the transport valence band in Ag-doped SnSe remains unclear. Particularly, understanding the influence of evaluating the optimal balance between band convergence and carrier mobility on weighted mobility is a primary consideration in designing high-performance TE materials. Here, we strongly confirm through theoretical and experimental evidence that Ag-doped Sn0.98Se can promote the evolution of valence bands and achieve band convergence and density of states distortion. The significantly increased carrier concentration and effective mass result in a dramatic increase in weighted mobility, which favors the achievement of superior power factors. Furthermore, the Debye model reveals the reasons for the evolution of lattice thermal conductivity. Eventually, a superior average power factor and averagezTvalue are obtained in the Ag-doped samples in both directions over the entire test temperature range. This strategy of improving TE performance through band engineering provides an effective way to advance TEs.

High-Power Factor Enabled by Efficient Manipulation Interaxial Angle for Enhancing Thermoelectrics of GeTe-Cu2Te Alloys.

The emerged strategy of manipulating the rhombohedral crystal structure provides another new degree of freedom for optimizing the thermoelectric properties of GeTe-based compounds. However, the concept is difficult to be effectively measured and often depends on heavy doping that scatters carriers severely. Herein, we synergistically manipulate lattice distortion and vacancy concentration to promote the excellent electrical transport of GeTe-Cu2Te alloys and quantify the interaxial angle-dependent density of state effective mass. Distinct from the conventional electronic coupling effect, about 2% substitution of Zr4+ significantly increases the interaxial angle, thereby enhancing the band convergence effect and improving the Seebeck coefficient. In addition, Ge-compensation attenuates the mobility deterioration, leading to improved power factor over the whole temperature range, especially exceeding ∼22 µW cm-1 K-2 at 300 K. Furthermore, the Debye-Callaway model elucidates low lattice thermal conductivity due to strong phonon scattering from Zr/Ge substitutional defects. As a result, the highest figure of merit zT of ∼1.6 (at 650 K) and average zTave of ∼0.9 (300-750 K) are obtained in (Ge1.01Zr0.02Te)0.985(Cu2Te)0.015. This work demonstrates the effective band modulation of Zr on GeTe-based materials, indicating that the modification of the interaxial angle is a deep pathway to improve thermoelectrics.

Multifunctional GeMnTe2 Synergistically Optimizes Thermoelectric Properties of SnTe-In2Te3 Alloys.

SnTe-In2Te3 alloys ensure excellent electrical properties in the whole temperature region due to the resonant level. Nevertheless, temperature-sensitive resonance states and single phonon scattering restrict further improvement of thermoelectric performance. Consequently, it is anticipated that additional electrically independent scattering sources should be introduced to impede phonon transport. Here, the SnTe-In2Te3-GeMnTe2 alloy is prepared by further solidifying cubic GeMnTe2, which demonstrates multiple modulation effects. The highly redissolved Mn2+ promotes the valence band convergence, enhances the Seebeck coefficient at higher temperature, and balances the possible weakened resonance level effect at higher carrier concentrations, and a high average power factor (1.94 mW m-1 K-2) is realized over the entire temperature range. Additionally, compensatory vacancies, substitutions, and Ge/Mn precipitates are easily constructed with GeMnTe2 alloying, leading to a further reduction in lattice thermal conductivity, which reaches κl ∼ 0.6 W m-1 K-1 at 850 K. Ultimately, a high peak zT of ∼1.25 (850 K) and a zTave of 0.72 (300-850 K) are realized in (SnTe)2.91(In2Te3)0.03(Ge0.5Mn0.5Te)1.2, and the maximum thermoelectric conversion efficiency of ∼2.8% (ΔT ∼ 450 K) is achieved. The present results indicate multiple effects of GeMnTe2 in enhancing the thermoelectric performance of SnTe-In2Te3 alloys.

Enzyme-Triggered Morphological Transition of Peptide Nanostructures for Tumor-Targeted Drug Delivery and Enhanced Cancer Therapy.

The use of smart drug carriers to realize cancer-targeted drug delivery is a promising method to improve the efficiency of chemotherapy and reduce its side effects. A surfactant-like peptide, Nap-FFGPLGLARKRK, was elaborately designed for cancer-targeted drug delivery based on an enzyme-triggered morphological transition of the self-assembled nanostructures. The peptide has three functional motifs: the aromatic motif of Nap-FF- to promote peptide self-assembly, the enzyme-cleavable segment of -GPLGLA- to introduce enzyme sensitivity, and the positively charged -RKRK- segment to balance the molecular amphiphilicity as well as to facilitate interaction with cell membranes. The peptide self-assembles into long fibrils with hydrophobic inner cores, which can encapsulate a high amount of anticancer drug doxorubicin (DOX). By having enzyme responsibility, these fibrils can be degraded into thinner ones by the cancer-overexpressed matrix metalloproteinase-7 (MMP7) at tumor sites and precipitate out to give sustained release of DOX, resulting in cancer-targeted drug delivery and selective cancer killing. In vivo antitumor experiments with mice confirm the high efficiency of such enzyme-responsive peptidic drug carriers in successfully suppressing the tumor growth and metastasis while greatly reducing the side effects. The study demonstrates the feasibility of using enzyme-sensitive peptide nanostructures for efficient and targeted drug delivery, which have great potential in biomedical cancer treatment.

Graphene Oxide-Assisted Accumulation and Layer-by-Layer Assembly of Antibacterial Peptide for Sustained Release Applications.

Fabrication of antibacterial materials with sustained release of active components is of great importance for long-term antibacterial applications. Graphene oxide (GO) has been found to be an excellent carrier for accumulating the antibacterial peptide of G(IIKK)4I-NH2 and mediating its loading into the layer-by-layer (LBL) films for sustained release applications. G(IIKK)4I-NH2 takes random coiled conformation in monomeric state below 0.17 mM but self-assembles into supramolecular aggregates with α-helical secondary structure at higher concentrations. It can bind onto GO surface in both monomeric and aggregate states to form stable GO@G(IIKK)4I-NH2 composites. Upon binding, the local amphiphilic environment of GO surface induces a conformational transition of G(IIKK)4I-NH2 monomers from random coils to α-helix. The aggregate binding enhances the loading amount greatly. GO (1 mg) can load as high as 1.7 mg of peptide at saturation. This enables the GO@G(IIKK)4I-NH2 composites to serve as reservoirs for sustained release of active G(IIKK)4I-NH2 monomers. Moreover, G(IIKK)4I-NH2 itself shows low efficiency in LBL assembly, whereas the GO@G(IIKK)4I-NH2 composites are ideal LBL assembling units with highly enhanced loading efficiency of G(IIKK)4I-NH2. The LBL films involving degradable poly(ß-amino esters) can realize sustained release of G(IIKK)4I-NH2 for bacteria killing in a well-controlled manner. This study demonstrates an efficient strategy for fabrication of long-durable antibacterial materials and surface coatings by using GO as the carrier for drug accumulation and loading.

Quenched Stochastic Optical Reconstruction Microscopy (qSTORM) with Graphene Oxide.

Quenched Stochastic Optical Reconstruction Microscopy (qSTORM) was demonstrated with graphene oxide sheets, peptides and bacteria; a method of contrast enhancement with super-resolution fluorescence microscopy. Individual sheets of graphene oxide (GO) were imaged with a resolution of 16 nm using the quenching of fluorescence emission by GO via its large Resonant Energy Transfer (RET) efficiency. The method was then extended to image self-assembled peptide aggregates (resolution 19 nm) and live bacterial cells (resolution 55 nm, the capsular structure of E. coli from urinary tract infections) with extremely low backgrounds and high contrasts (between one and two orders of magnitude contrast factor improvements that depended on the thickness of the graphene oxide layer used). Graphene oxide films combined with STORM imaging thus provide an extremely convenient method to image samples with large backgrounds due to non-specifically bound fluorophores (either due to excess labelling or autofluorescent molecules), which is a common occurrence in studies of both biological cells and soft-condensed matter. The GO quenches the fluorescence across a thin layer at distances of less than 15 nm. Graphene oxide films coated with thin layers (≤15 nm) of polystyrene, polymethylmethacrylate and polylysine are shown to be effective in producing high contrast qSTORM images, providing a convenient modulation of sample/substrate interactions. The GO coatings can also provide an increased image resolution and a factor of 2.3 improvement was observed with the peptide fibres using a feature of interest metric,when there was a large non-specifically bound background.

Interfacial Adsorption of Monoclonal Antibody COE-3 at the Solid/Water Interface.

Spectroscopic ellipsometry (SE) and neutron reflection (NR) data for the adsorption of a monoclonal antibody (mAb, termed COE-3, pI 8.44) at the bare SiO2/water interface are compared here to the simulations based on Derjaguin-Landau-Verwey-Overbeek theory. COE-3 adsorption was characterized by an initial rapid increase in the surface-adsorbed amount (Γ) followed by a plateau. Only the initial rate of the increase in Γ was strongly correlated with the bulk concentration (0.002-0.2 mg/mL), with Γ at the plateau being about 2.2 mg/m2 (pH 5.5). Simulations captured COE-3 adsorption at equilibrium most accurately, the point at which the outgoing flux of molecules within the adsorbed plane matched the adsorption flux. Increasing the buffer pH from 5.5 to 9 increased Γ at equilibrium to ∼3 mg/m2 (0.02 mg/mL COE-3), revealing a dominant role for lateral repulsion between adsorbed mAb molecules. In contrast, increasing the buffer ionic strength (pH 6) reduced Γ, which was captured by simulations accounting for electrostatic screening by ions, in addition to mAb/SiO2 attractive forces and lateral repulsion. NR data at the same bulk concentrations corroborated the SE data, albeit with slightly higher Γ due to longer adsorption times for data acquisition; for example, at pH 9, Γ was 3.6 mg/m2 (0.02 mg/mL COE-3), equivalent to a relatively high volume fraction of 0.5. An adsorbed monolayer with a thickness of 50-52 Å was consistently determined by NR, corresponding to the short axial lengths of fragment antigen-binding and fragment crystallization and implying minimal structural perturbation. Thus, the simulations enabled a mechanistic interpretation of the experimental data of mAb adsorption at the SiO2/water interface.

Coadsorption of a Monoclonal Antibody and Nonionic Surfactant at the SiO2/Water Interface.

During the formulation of therapeutic monoclonal antibodies (mAbs), nonionic surfactants are commonly added to attenuate structural rearrangement caused by adsorption/desorption at interfaces during processing, shipping, and storage. We examined the adsorption of a mAb (COE-3) at the SiO2/water interface in the presence of pentaethylene glycol monododecyl ether (C12E5), polysorbate 80 (PS80-20EO), and a polysorbate 80 analogue with seven ethoxylates (PS80-7EO). Spectroscopic ellipsometry was used to follow COE-3 dynamic adsorption, and neutron reflection was used to determine interfacial structure and composition. Neither PS80-20EO nor C12E5 had a notable affinity for COE-3 or the interface under the conditions studied and thus did not prevent COE-3 adsorption. In contrast, PS80-7EO did coadsorb but did not influence the dynamic process or the equilibrated amount of absorbed COE-3. Near equilibration, COE-3 underwent structural rearrangement and PS80-7EO started to bind the COE-3 interfacial layer and subsequently formed a well-defined surfactant bilayer via self-assembly. The resultant interfacial layer comprised an inner mAb layer of about 70 Å thickness and an outer surfactant layer of a further 70 Å, with distinct transitional regions across the mAb-surfactant and surfactant-bulk water boundaries. Once formed, such interfacial layers were very robust and worked to prevent further mAb adsorption, desorption, and structural rearrangement. Such robust interfacial layers could be anticipated to exist for formulated mAbs stored in type II glass vials; further research is required to understand the behavior of these layers for siliconized glass syringes.

Neutron Reflection Study of Surface Adsorption of Fc, Fab, and the Whole mAb.

Characterizing the influence of fragment crystallization (Fc) and antigen-binding fragment (Fab) on monoclonal antibody (mAb) adsorption at the air/water interface is an important step to understanding liquid mAb drug product stability during manufacture, shipping, and storage. Here, neutron reflection is used to study the air/water adsorption of a mAb and its Fc and Fab fragments. By varying the isotopic contrast, the adsorbed amount, thickness, orientation, and immersion of the adsorbed layers could be determined unambiguously. While Fc adsorption reached saturation within the hour, its surface adsorbed amount showed little variation with bulk concentration. In contrast, Fab adsorption was slower and the adsorbed amount was concentration dependent. The much higher Fc adsorption, as compared to Fab, was linked to its lower surface charge. Time and concentration dependence of mAb adsorption was dominated by Fab behavior, although both Fab and Fc behaviors contributed to the amount of mAb adsorbed. Changing the pH from 5.5 to 8.8 did not much perturb the adsorbed amount of Fc, Fab, or mAb. However, a small decrease in adsorption was observed for the Fc over pH 8-8.8 and vice versa for the Fab and mAb, consistent with a dominant Fab behavior. As bulk concentration increased from 5 to 50 ppm, the thicknesses of the Fc layers were almost constant at 40 Å, while Fab and mAb layers increased from 45 to 50 Å. These results imply that the adsorbed mAb, Fc, and Fab all retained their globular structures and were oriented with their short axial lengths perpendicular to the interface.

Direct exfoliation of graphite into graphene in aqueous solutions of amphiphilic peptides.

Different amphiphilic peptides were used to mediate the direct exfoliation of graphite into few-layered graphene flakes in aqueous solutions. Charge was found to be an important parameter in determining their graphite exfoliating efficiency. The anionic molecules were more favorable than the cationic ones leading to a higher efficiency. The gemini-type peptide IleIleIleCys-CysIleIleIle (I3C-CI3) exhibited the highest efficiency, which might be attributed to its specific physicochemical properties and interactions with graphene sheets. I3C-CI3 adsorbed onto the graphene surface as either monomers or self-assembled nanoaggregates. These adsorbed species increased both electrostatic and steric repulsions between the graphene/I3C-CI3 composites. More interestingly, the graphene/I3C-CI3 composites showed a reversible pH-dependent dispersion/aggregation. This behavior resulted from the pH-sensitive protonation of the peptide molecules and was rarely found in the graphene dispersions exfoliated by traditional surfactants. Moreover, the graphene/I3C-CI3 dispersion was used to fabricate free-standing macroscopic composite films that contained different nanostructures. The study expands the library of available agents for direct graphite exfoliation to produce graphene sheets. Employing peptide molecules as graphene exfoliating and stabilizing agents avoids the use of toxic reagents, which may allow fabrication of functional composite materials for biocompatible applications.