In this work, we present all-oxide p-n junction core-shell nanowires (NWs) as fast and stable self-powered photodetectors. Hydrothermally grown n-type ZnO NWs were conformal covered by different thicknesses (up to 420 nm) of p-type copper oxide layers through metalorganic chemical vapor deposition (MOCVD).The ZnO NWs exhibit a single crystalline Wurtzite structure, preferentially grown along the [002] direction, and energy gap Eg=3.24 eV. Depending on the deposition temperature, the copper oxide shell exhibits either a crystalline cubic structure of pure Cu2O phase (MOCVD at 250 C) or a cubic structure of Cu2O with the presence of CuO phase impurities (MOCVD at 300 C), with energy gap of 2.48 eV.The electrical measurements indicate the formation of a p-n junction after the deposition of the copper oxide layer. The core-shell photodetectors present a photoresponsivity at 0V bias voltage up to 7.7 µA/W and time response ≤0.09 s, the fastest ever reported for oxide photodetectors in the visible range, and among the fastest including photodetectors with response limited to the UV region. The bare ZnO NWs have slow photoresponsivity, without recovery after the end of photo-stimulation. The fast time response for the core-shell structures is due to the presence of the p-n junctions, which enables fast exciton separation and charge extraction. Additionally, the suitable electronic structure of the ZnO-Cu2O heterojunction enables self-powering of the device at 0V bias voltage. These results represent a significant advancement in the development of low-cost, high efficiency and self-powered photodetectors, highlighting the need of fine tuning the morphology, composition and electronic properties of p-n junctions to maximize device performances.
Control of interactions between nanomaterials and cells remains a biomedical challenge. A strategy is proposed to modulate the intralysosomal distribution of nanoparticles through the design of 3D suprastructures built by hydrophilic nanocrystals (NCs) coated with alkyl chains. The intracellular fate of two water‐dispersible architectures of self‐assembled hydrophobic magnetic NCs: hollow deformable shells (colloidosomes) or solid fcc particles (supraballs) is compared. These two self‐assemblies display increased cellular uptake by tumor cells compared to dispersions of the water‐soluble NC building blocks. Moreover, the self‐assembly structures increase the NCs density in lysosomes and close to the lysosome membrane. Importantly, the structural organization of NCs in colloidosomes and supraballs are maintained in lysosomes up to 8 days after internalization, whereas initially dispersed hydrophilic NCs are randomly aggregated. Supraballs and colloidosomes are differently sensed by cells due to their different architectures and mechanical properties. Flexible and soft colloidosomes deform and spread along the biological membranes. In contrast, the more rigid supraballs remain spherical. By subjecting the internalized suprastructures to a magnetic field, they both align and form long chains. Overall, it is highlighted that the mechanical and topological properties of the self‐assemblies direct their intracellular fate allowing the control intralysosomal density, ordering, and localization of NCs.
Mucins are multifunctional glycosylated proteins that are increasingly investigated as building blocks of novel biomaterials. An attractive feature is their ability to modulate the immune response, in part by engaging with sialic acid binding receptors on immune cells. Once assembled into hydrogels, bovine submaxillary mucins (Muc gels) were shown to modulate the recruitment and activation of immune cells and avoid fibrous encapsulation in vivo. However, nothing is known about the early immune response to Muc gels. This study characterizes the response of macrophages, important orchestrators of the material-mediated immune response, over the first 7 days in contact with Muc gels. The role of mucin-bound sialic acid sugar residues was investigated by first enzymatically cleaving the sugar and then assembling the mucin variants into covalently cross-linked hydrogels with rheological and surface nanomechanical properties similar to nonmodified Muc gels. Results with THP-1 and human primary peripheral blood monocytes derived macrophages showed that Muc gels transiently activate the expression of both pro-inflammatory and anti-inflammatory cytokines and cell surface markers, for most makers with a maximum on the first day and loss of the effect after 7 days. The activation was sialic acid-dependent for a majority of the markers followed. The pattern of gene expression, protein expression, and functional measurements did not strictly correspond to M1 or M2 macrophage phenotypes. This study highlights the complex early events in macrophage activation in contact with mucin materials and the importance of sialic acid residues in such a response. The enzymatic glyco-modulation of Muc gels appears as a useful tool to help understand the biological functions of specific glycans on mucins which can further inform on their use in various biomedical applications.
Surface science, which spans the fields of chemistry, physics, biology and materials science, requires information to be obtained on the local properties and property variations across a surface. This has resulted in the development of different scanning probe methods that allow the measurement of local chemical composition and local electrical and mechanical properties. These techniques have led to rapid advancement in fundamental science with applications in areas such as composite materials, corrosion protection and wear resistance. In this perspective article, we focussed on the branch of scanning probe methods that allows the determination of surface nanomechanical properties. We discussed some different AFM-based modes that were used for these measurements and provided illustrative examples of the type of information that could be obtained. We also discussed some of the difficulties encountered during such studies.
Healthy material alternatives based on renewable resources and sustainable technologies have the potential to disrupt the environmentally damaging production and consumption practices established throughout the modern industrial era. In this study, a mycelium–nanocellulose biocomposite with hybrid properties is produced by the agitated liquid culture of a white‐rot fungus (Trametes ochracea) with nanocellulose (NC) comprised as part of the culture media. Mycelial development proceeds via the formation of pellets, where NC is enriched in the pellets and depleted from the surrounding liquid media. Micrometer‐scale NC elements become engulfed in mycelium, whereas it is hypothesized that the nanometer‐scale fraction becomes integrated within the hyphal cell wall, such that all NC in the system is essentially surface‐modified by mycelium. The NC confers mechanical strength to films processed from the biocomposite, whereas the mycelium screens typical cellulose–water interactions, giving fibrous slurries that dewater faster and films that exhibit significantly improved wet resistance in comparison to pure NC films. The mycelium–nanocellulose biocomposites are processable in the ways familiar to papermaking and are suggested for diverse applications, including packaging, filtration, and hygiene products.
Mucins are high molar mass glycoproteins that assume an extended conformation and can assemble into mucus hydrogels that protect our mucosal epithelium. In nature, the challenging task of generating a mucus layer, several hundreds of micrometers in thickness, from micrometer-sized cells is elegantly solved by the condensation of mucins inside vesicles and their on-demand release from the cells where they suddenly expand to form the extracellular mucus hydrogel. We aimed to recreate and control the process of compaction for mucins, the first step toward a better understanding of the process and creating biomimetic in vivo delivery strategies of macromolecules. We found that by adding glycerol to the aqueous solvent, we could induce drastic condensation of purified mucin molecules, reducing their size by an order of magnitude down to tens of nanometers in diameter. The condensation effect of glycerol was fully reversible and could be further enhanced and partially stabilized by cationic cross-linkers such as calcium and polylysine. The change of structure of mucins from extended molecules to nano-sized particles in the presence of glycerol translated into macroscopic rheological changes, as illustrated by a dampened shear-thinning effect with increasing glycerol concentration. This work provides new insight into mucin condensation, which could lead to new delivery strategies mimicking cell release of macromolecules condensed in vesicles such as mucins and heparin.
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