Topological wetting states of microdroplets on closed-loop structured surfaces: Breakdown of the Gibbs equation at the microscale.

Microdroplets are a class of soft matter that has been extensively employed for chemical, biochemical, and industrial applications. However, fabricating microdroplets with largely controllable contact-area shape and apparent contact angle, a key prerequisite for their applications, is still a challenge. Here, by engineering a type of surface with homocentric closed-loop microwalls/microchannels, we can achieve facile size, shape, and contact-angle tunability of microdroplets on the textured surfaces by design. More importantly, this class of surface topologies (with universal genus value = 1) allows us to reveal that the conventional Gibbs equation (widely used for assessing the edge effect on the apparent contact angle of macrodroplets) seems no longer applicable for water microdroplets or nanodroplets (evidenced by independent molecular dynamics simulations). Notably, for the flat surface with the intrinsic contact angle ~0°, we find that the critical contact angle on the microtextured counterparts (at edge angle 90°) can be as large as >130°, rather than 90° according to the Gibbs equation. Experiments show that the breakdown of the Gibbs equation occurs for microdroplets of different types of liquids including alcohol and hydrocarbon oils. Overall, the microtextured surface design and topological wetting states not only offer opportunities for diverse applications of microdroplets such as controllable chemical reactions and low-cost circuit fabrications but also provide testbeds for advancing the fundamental surface science of wetting beyond the Gibbs equation.

Robust DNA-Bridged Memristor for Textile Chips.

Electronic textiles may revolutionize many fields, such as communication, health care and artificial intelligence. To date, unfortunately, computing with them is not yet possible. Memristors are compatible with the interwoven structure and manufacturing process in textiles because of its two-terminal crossbar configuration. However, it remains a challenge to realize textile memristors owing to the difficulties in designing advanced memristive materials and achieving high-quality active layers on fiber electrodes. Herein we report a robust textile memristor based on an electrophoretic-deposited active layer of deoxyribonucleic acid (DNA) on fiber electrodes. The unique architecture and orientation of DNA molecules with the incorporation of Ag nanoparticles offer the best-in-class performances, e.g., both ultra-low operation voltage of 0.3 V and power consumption of 100 pW and high switching speed of 20 ns. Fundamental logic calculations such as implication and NAND are demonstrated as functions of textile chips, and it has been thus integrated with power-supplying and light emitting modules to demonstrate an all-fabric information processing system.

Influence of fullerenol on hIAPP aggregation: amyloid inhibition and mechanistic aspects.

Fullerenols have garnered significant scientific interest in nano-technology and biomedicine. A detailed understanding of their interactions with proteins is fundamentally important for their biomedical applications. Human islet amyloid polypeptide (hIAPP) is an intrinsically disordered protein and its aggregation is associated with type 2 diabetes. Here, we investigated the nano-bio-interactions of fullerenol with hIAPP and focused on the effect of C60(OH)24 on hIAPP aggregation by replica-exchange molecular dynamic simulations. Our simulations show that isolated hIAPP dimers transiently populated amyloid-precursor (ß-hairpin) containing ß-sheet structure, whereas C60(OH)24 completely suppressed this fibril-prone structure, thus inhibiting hIAPP aggregation. The simulation-predicted inhibitory effect of fullerenols was validated by atom force microscopy and thioflavin T fluorescence experiments. We find C60(OH)24 binds to hIAPP via hydrogen bonding interactions with polar residues T9, Q10, N14, N21, N22, N31, N35 and T36 as well as the collective van der Waals and hydrogen-bonding interaction with Y37. Molecular dynamic simulations show that C60(OH)24 destabilized the hIAPP protofibril by mostly binding to the 20SNNFGAILSS29 amyloid core region. This study not only helps to understand the mechanisms involved in hIAPP aggregation and amyloid inhibition, but also provides new clues for the development of therapeutic candidates against type 2 diabetes.

Directly probing the dissociation effects of graphene oxide nanosheets on hIAPP fibrils.

The aggregation of human islet amyloid polypeptides (hIAPP) to mature fibrils is considered as the main cause of type II diabetes. Therefore destroying the pre-formed hIAPP fibrils is expected to be a promising strategy for therapeutic treatments. In this work, the dissociation effects of graphene oxide (GO) nanosheets on hIAPP mature fibrils are investigated. The results clearly demonstrate that hIAPP fibrils can be quickly adsorbed on the GO surface and efficiently broken into short fragments. Meanwhile, the ß-sheet structures of hIAPP fibrils are greatly destroyed. Particularly, in situ atomic force microscopy was applied to monitor the real-time interaction between hIAPP fibrils and GO nanosheets. It provides distinct evidence that the disruption of hIAPP fibrils by GO nanosheets mainly occurs at the GO edges. Size-dependent experiments further justify the interfere of edge contribution, which suggest small-sized GO nanosheets exhibit better dissociation ability than large-sized ones. Therefore, this study not only provides valuable information that GO nanosheets (especially small-sized ones) can act as efficient nanoblades to break hIAPP fibrils, but also suggests a powerful and widely available methodology for investigating real-time interaction between nanomaterials and biomolecules.

Toward precise site-controlling of self-assembled Ge quantum dots on Si microdisks.

A feasible route is developed toward precise site-controlling of quantum dots (QDs) at the microdisk periphery, where most microdisk cavity modes are located. The preferential growth of self-assembled Ge QDs at the periphery of Si microdisks is discovered. Moreover, both the height and linear density of Ge QDs can be controlled by tuning the amount of deposited Ge and the microdisk size. The inherent mechanisms of these unique features are discussed, taking into account both the growth kinetics and thermodynamics. By growing Ge on the innovative Si microdisks with small protrusions at the disk periphery, the positioning of Ge QDs at the periphery can be exactly predetermined. Such a precise site-controlling of Ge QDs at the periphery enables the location of the QD right at the field antinodes of the cavity mode of the Si microdisk, thereby achieving spatial matching between QD and cavity mode. These results open a promising door to realize the semiconductor QD-microdisk systems with both spectral and spatial matching between QDs and microdisk cavity modes, which will be the promising candidates for exploring the fundamental features of cavity quantum electrodynamics and the innovative optoelectronic devices based on strong light-matter interaction.

Promising features of low-temperature grown Ge nanostructures on Si(001) substrates.

High-quality Ge nanostructures are obtained by molecular beam epitaxy of Ge on Si(001) substrates at 200 °C and ex situ annealing at 400 °C. Their structural properties are comprehensively characterized by atomic force microscopy, transmission electron microscopy and Raman spectroscopy. It is disclosed that they are almost defect free except for some defects at the Ge/Si interface and in the subsequent Si capping layer. The misfit strain in the nanostructure is substantially relaxed. Dramatically strong photoluminescence (PL) from the Ge nanostructures is observed. Detailed analyses on the power- and temperature-dependent PL spectra, together with a self-consistent calculation, indicate the confinement and the high quantum efficiency of excitons within the Ge nanostructures. Our results demonstrate that the Ge nanostructures obtained via the present feasible route may have great potential in optoelectronic devices for monolithic optical-electronic integration circuits.

Effects of hydroxylated carbon nanotubes on the aggregation of Aß16-22 peptides: a combined simulation and experimental study.

The pathogenesis of Alzheimer's disease (AD) is associated with the aggregation of amyloid-ß (Aß) peptides into toxic aggregates with ?-sheet character. In a previous computational study, we showed that pristine single-walled carbon nanotubes (SWCNTs) can inhibit the formation of ß-sheet-rich oligomers in the central hydrophobic core fragment of Aß (Aß16-22). However, the poor solubility of SWCNTs in water hinders their use in biomedical applications and nanomedicine. Here, we investigate the influence of hydroxylated SWCNT, a water-soluble SWCNT derivative, on the aggregation of Aß16-22 peptides using all-atom explicit-water replica exchange molecular dynamics simulations. Our results show that hydroxylated SWCNTs can significantly inhibit ß-sheet formation and shift the conformations of Aß16-22 oligomers from ordered ß-sheet-rich structures toward disordered coil aggregates. Detailed analyses of the SWCNT-Aß interaction reveal that the inhibition of ß-sheet formation by hydroxylated SWCNTs mainly results from strong electrostatic interactions between the hydroxyl groups of SWCNTs and the positively charged residue K16 of Aß16-22 and hydrophobic and aromatic stacking interactions between SWCNTs and F19 and F20. In addition, our atomic force microscopy and thioflavin T fluorescence experiments confirm the inhibitory effect of both pristine and hydroxylated SWCNTs on Aß16-22 fibrillization, in support of our previous and present replica exchange molecular dynamics simulation results. These results demonstrate that hydroxylated SWCNTs efficiently inhibit the aggregation of Aß16-22; in addition, they offer molecular insight into the inhibition mechanism, thus providing new clues for the design of therapeutic drugs against amyloidosis.

Investigation of the aggregation process of amyloid-ß-(16-22) peptides and the dissolution of intermediate aggregates.

The aggregation processes of amyloid-ß-(16-22) peptides (Aß16-22) are investigated by atomic force microscopy (AFM). It is found that Aß16-22 peptides quickly aggregate from monomers to oligomers and flakelike structures and finally to fibrils. In particular, unusual morphology change is observed in an early stage of aggregation; that is, the originally formed flakelike structures would disappear in the following aggregation processes. To determine the evolution of the flakelike structures, in situ AFM imaging is carried out in liquid to reveal the real-time morphology change of Aß16-22. The results provide clear evidence that the flakelike structures are in an unstable intermediate state, which would be dissolved into oligomers or short protofibrils for reorganization. Further fluorescence and attenuated total reflectance Fourier transform infrared (ATR-FTIR) experiments on thioflavin T(ThT) suggest that those flakelike structures contain ß-sheet components.

Conidia Fusion: A Mechanism for Fungal Adaptation to Nutrient-Poor Habitats.

Conidia fusion (CF) is a commonly observed structure in fungi. However, it has not been systematically studied. This study examined 2457 strains of nematode-trapping fungi (NTF) to explore the species specificity, physiological period, and physiological significance of CF. The results demonstrated that only six species of Arthrobotrys can form CF among the sixty-five tested NTF species. The studies on the model species Arthrobotrys oligospora (DL228) showed that CF occurred in both shed and unshed plus mature and immature conidia. Additionally, the conidia fusion rate (CFR) increased significantly with the decrease of nutrient concentration in habitats. The studies on the conidia fusion body (CFB) produced by A. oligospora (DL228) revealed that the more conidia contained in the CFB, the faster and denser the mycelia of the CFB germinated in weak nutrient medium and soil plates. On the one hand, rapid mycelial extension is beneficial for the CFB to quickly find new nutrient sources in habitats with uneven nutrient distribution. On the other hand, dense mycelium increases the contact area with the environment, improving the nutrient absorption efficiency, which is conducive to improving the survival rate of conidia in the weak nutrient environment. In addition, all species that form CF produce smaller conidia. Based on this observation, CF may be a strategy to balance the defects (nutrient deficiency) caused by conidia miniaturization.

Fabrication of crystal α-Si3N4/Si-SiOx core-shell/Au-SiOx peapod-like axial double heterostructures for optoelectronic applications.

Novel crystal α-Si(3)N(4)/Si-SiO(x) core-shell/Au-SiO(x) peapod-like axial double heterostructural nanowires were obtained by directly annealing a Au covered SiO(2) thin film on a Si substrate. Our extensive electron microscopic investigation revealed that the α-Si(3)N(4) sections with a mathematical left angle bracket 101 mathematical right angle bracket growth direction were grown first, followed by growth of the Si-SiO(x) core-shell sections and finally growth of the Au-SiO(x) peapod-like sections. Through a series of systematically comparative experiments, a temperature-dependent multi-step vapor-liquid-solid growth mechanism is proposed. Room temperature photoluminescence measurement of individual nanowires reveals two emission peaks (410 and 515 nm), indicating their potential applications in light sources, laser or light emitting display devices.

Photoelectrical Properties Investigated on Individual Si Nanowires and Their Size Dependence.

Periodically ordered arrays of vertically aligned Si nanowires (Si NWs) are successfully fabricated with controllable diameters and lengths. Their photoconductive properties are investigated by photoconductive atomic force microscopy (PCAFM) on individual nanowires. The results show that the photocurrent of Si NWs increases significantly with the laser intensity, indicating that Si NWs have good photoconductance and photoresponse capability. This photoenhanced conductance can be attributed to the photoinduced Schottky barrier change, confirmed by I-V curve analyses. On the other hand, electrostatic force microscopy (EFM) results indicate that a large number of photogenerated charges are trapped in Si NWs under laser irradiation, leading to the lowering of barrier height. Moreover, the size dependence of photoconductive properties is studied on Si NWs with different diameters and lengths. It is found that the increasing magnitude of photocurrent with laser intensity is greatly relevant to the nanowires' diameter and length. Si NWs with smaller diameters and shorter lengths display better photoconductive properties, which agrees well with the size-dependent barrier height variation induced by photogenerated charges. With optimized diameter and length, great photoelectrical properties are achieved on Si NWs. Overall, in this study the photoelectrical properties of individual Si NWs are systematically investigated by PCAFM and EFM, providing important information for the optimization of nanostructures for practical applications.

Investigation of the Dissociation Mechanism of Single-Walled Carbon Nanotube on Mature Amyloid-ß Fibrils at Single Nanotube Level.

Amyloid fibrils originating from the fibrillogenesis of misfolded amyloid proteins are associated with the pathogenesis of many neurodegenerative diseases, such as Alzheimer's, Parkinson's, and Huntington's diseases. Carbon nanotubes have been extensively applied in our life and industry due to their unique chemical and physical properties. Nonetheless, the details between carbon nanotubes and mature amyloid fibrils remain elusive. In this study, we explored the interplay between single-walled carbon nanotubes (SWCNTs) and preformed amyloid-ß (Aß) fibrils by atomic force microscopy at the single SWCNT level, together with ThT fluorescence, cellular viability assays, infrared spectroscopy, and molecular dynamics (MD) simulations. The results demonstrated that SWCNTs could partially destroy the preformed Aß fibrils and form the Aß-surrounded-SWCNTs conjugates, as well as reduce the ß-sheet structures. Peak force quantitative nanomechanical measurements revealed that the conjugates have lower Young's modulus than fibrils. Furthermore, our MD simulation demonstrated that the dissociation ability was dependent on the binding sites of Aß fibrils. Overall, this study provides an insight into the dissociation mechanism between SWCNT and Aß fibrils, which could be beneficial for the study of bionanomaterials and the development of other potential drug candidates for amyloidosis.

Fabrication of High-Quality and Strain-Relaxed GeSn Microdisks by Integrating Selective Epitaxial Growth and Selective Wet Etching Methods.

GeSn is a promising material for the fabrication of on-chip photonic and nanoelectronic devices. Processing techniques dedicated to GeSn have thus been developed, including epitaxy, annealing, ion implantation, and etching. In this work, suspended, strain-relaxed, and high-quality GeSn microdisks are realized by a new approach without any etching to GeSn alloy. The GeSn alloy was grown on pre-patterned Ge (001) substrate by molecular beam epitaxy at low temperatures. The transmission electron microscopy and scanning electron microscopy were carried out to determine the microstructures of the GeSn samples. The microdisks with different diameters of Ge pedestals were fabricated by controlling the selective wet etching time, and micro-Raman results show that the microdisks with different dimensions of the remaining Ge pedestals have different extents of strain relaxation. The compressive strain of microdisks is almost completely relaxed under suitable conditions. The semiconductor processing technology presented in this work can be an alternative method to fabricate innovative GeSn and other materials based micro/nano-structures for a range of Si-compatible photonics, 3D-MOSFETs, and microelectromechanical device applications.

Highly Efficient Charge Collection in Bulk-Heterojunction Organic Solar Cells by Anomalous Hole Transfer and Improved Interfacial Contact.

The dilute donor-fullerene bulk heterojunction (BHJ) has been proven to be an efficient architecture of organic solar cells. However, the hole-extraction pathway and the origin of the high open-circuit voltage ( VOC) in this peculiar architecture remains elusive. Direct evidence is provided here that the photogenerated holes can be extracted via the acceptor phase even under the operating conditions. Meanwhile VOC is found to be closely correlated with the surface composition at the MoO3/BHJ interface. Extending these findings into device optimization, more than 37% enhancement is achieved in a prototype BHJ device. These results evoke renewed insight into the underlying physics in organic solar cells.

Label-free imaging of amyloid plaques in Alzheimer's disease with stimulated Raman scattering microscopy.

One of the key pathological features of Alzheimer's disease (AD) is the existence of extracellular deposition of amyloid plaques formed with misfolded amyloid-ß (Aß). The conformational change of proteins leads to enriched contents of ß sheets, resulting in remarkable changes of vibrational spectra, especially the spectral shifts of the amide I mode. Here, we applied stimulated Raman scattering (SRS) microscopy to image amyloid plaques in the brain tissue of an AD mouse model. We have demonstrated the capability of SRS microscopy as a rapid, label-free imaging modality to differentiate misfolded from normal proteins based on the blue shift (~10 cm-1) of amide I SRS spectra. Furthermore, SRS imaging of Aß plaques was verified by antibody staining of frozen thin sections and fluorescence imaging of fresh tissues. Our method may provide a new approach for studies of AD pathology, as well as other neurodegenerative diseases associated with protein misfolding.

Large-Area Au-Nanoparticle-Functionalized Si Nanorod Arrays for Spatially Uniform Surface-Enhanced Raman Spectroscopy.

In this study, large-area hexagonal-packed Si nanorod (SiNR) arrays in conjunction with Au nanoparticles (AuNPs) were fabricated for surface-enhanced Raman spectroscopy (SERS). We have achieved ultrasensitive molecular detection with high reproducibility and spatial uniformity. A finite-difference time-domain simulation suggests that a wide range of three-dimensional electric fields are generated along the surfaces of the SiNR array. With the tuning of the gap and diameter of the SiNRs, the produced long decay length (>130 nm) of the enhanced electric field makes the SERS substrate a zero-gap system for ultrasensitive detection of large biomolecules. In the detection of R6G molecules, our SERS system achieved an enhancement factor of >107 with a relative standard deviation as small as 3.9-7.2% over 30 points across the substrate. More significantly, the SERS substrate yielded ultrasensitive Raman signals on long amyloid-ß fibrils at the single-fibril level, which provides promising potentials for ultrasensitive detection of amyloid aggregates that are related to Alzheimer's disease. Our study demonstrates that the SiNRs functionalized with AuNPs may serve as excellent SERS substrates in chemical and biomedical detection.

Interaction Dynamics in Inhibiting the Aggregation of Aß Peptides by SWCNTs: A Combined Experimental and Coarse-Grained Molecular Dynamic Simulation Study.

The aggregation of amyloid-ß peptides (Aß) is considered as the main possible cause of Alzheimer's disease (AD). How to suppress the formation of toxic Aß aggregates has been an intensive concern over the past several decades. Increasing evidence shows that whether carbon nanomaterials can suppress or promote the aggregation depends on their physicochemical properties. However, their interaction dynamics remains elusive as amyloid fibrillation is a complex multistep process. In this paper, we utilized atomic force microscopy (AFM), electrostatic force microscopy (EFM), ThT/fluorescence spectroscopy, and cell viability measurements, combined with coarse-grained molecular dynamic (MD) simulations to study the dynamic interaction of full length Aß with single-walled carbon nanotubes (SWCNT). At the single SWCNTs scale, it is found that the presence of SWCNTs would result in rapid and spontaneous adsorption of Aß1-40 peptides on their surface and stacking into nonfibrillar aggregates with reduced toxicity, which plays an important role in inhibiting the formation of toxic oligomers and mature fibrils. Our results provide new clues for studying the interaction in amyloid/SWCNTs system as well as for seeking amyloidosis inhibitors with carbon nanomaterials.

Highly Efficient Destruction of Amyloid-ß Fibrils by Femtosecond Laser-Induced Nanoexplosion of Gold Nanorods.

Alzheimer's disease (AD) is associated with the aggregation of the amyloid-beta (Aß) peptides into toxic aggregates. How to inhibit the aggregation of Aß peptides has been extensively studied over recent decades. The investigation on eliminating preformed fibrils, however, has rarely been reported. In this paper, near-infrared femtosecond (fs) laser is applied for the destruction of preformed Aß fibrils in conjunction with gold nanorods (AuNRs). Our results demonstrate that the 800 nm fs-laser irradiation can locally trigger the explosion of AuNRs due to the strong localized surface plasmon resonance effect. As a result, the majority of Aß fibrils are efficiently destroyed into small fragments by the irradiation of fs-laser with a light dose less than 75 J·cm-2. Meanwhile, significant reduction of ß-sheet structures is observed by thioflavin T (ThT) fluorescence measurements. In contrast, the destruction effect by continuous wave (cw) laser irradiation is much weaker with equivalent power density and irradiation time. Furthermore, the laser-induced destruction of fibrils by Au nanoparticles (AuNPs) is also investigated, which reveals that most of the Aß fibrils remain well under the surface explosion of spherical AuNPs. Overall, our results provide a novel design for the fast destruction of amyloid fibrils locally and biocompatibly, which may have remarkable potentials in the therapy of AD.