The self-assembled monolayer modification of electrodes - some recent advances in biological application

The modification of an electrode surface at the molecular level using the technique of depositing self-assembled monolayers (SAM) is a typical example of the techniques used in nanotechnology, from the process &quot;bottom up&quot;, which is to create a nanostructure by successive additions of molecular or atomic entities on a surface. This article presents some recent advances in the field, with examples: the development of systems Sat hybridized with biomolecules, nanoparticles or nanotubes in bioelectronics, the use of switchable electrodes to study the adhesion and migration of biological cells , and the integration of molecular son in the SAM to recognize and allow the transduction of a biological response allowing the practice of electrochemistry in a complex biological environment.<br /

Direct-laser writing for subnanometer focusing and single-molecule imaging

Two-photon direct laser writing is an additive fabrication process that utilizes two-photon absorption of tightly focused femtosecond laser pulses to implement spatially controlled polymerization of a liquid-phase photoresist. Two-photon direct laser writing is capable of nanofabricating arbitrary three-dimensional structures with nanometer accuracy. Here, we explore direct laser writing for high-resolution optical microscopy by fabricating unique 3D optical fiducials for single-molecule tracking and 3D single-molecule localization microscopy. By having control over the position and three-dimensional architecture of the fiducials, we improve axial discrimination and demonstrate isotropic subnanometer 3D focusing (<0.8 nm) over tens of micrometers using a standard inverted microscope. We perform 3D single-molecule acquisitions over cellular volumes, unsupervised data acquisition and live-cell single-particle tracking with nanometer accuracy

Ultrafast generation of highly crystalline graphene quantum dots from graphite paper via laser writing

Graphene quantum dots (GQDs) are attractive fluorescent nanoparticles that have wide applicability, are inexpensive, nontoxic, photostable, water-dispersible, biocompatible and environmental-friendly. Various strategies for the synthesis of GQDs have been reported. However, simple and efficient methods of producing GQDs with control over the size of the GQDs, and hence their optical properties, are sorely needed. Herein, an ultra-fast and efficient laser writing technique is presented as a means to produce GQDs with homogeneous size from graphene produced by the instantaneous photothermal gasification and recrystallization mechanism. Controlling the laser scan speed and output power, the yield of GQDs can reach to be about 31.458 mg/s, which shows promising potential for large-scale production. The entire process eliminates the need for chemical solvents or any other reagents. Notably, the prepared laser writing produced GQDs (LWP-GQDs) exhibit blue fluorescence under UV irradiation of 365 nm and the Commission Internationale de L'Eclairage (CIE) chromaticity coordinates is measured at (0.1721, 0.123). Overall, this method exhibits superior advantages over the complex procedures and low yields required by other existing methods, and thus has great potential for the commercial applications

Synthesis of hierarchical metal nanostructures with high electrocatalytic surface areas

3D interconnected structures can be made with molecular precision or with micrometer size. However, there is no strategy to synthesize 3D structures with dimensions on the scale of tens of nanometers, where many unique properties exist. Here, we bridge this gap by building up nanosized gold cores and nickel branches that are directly connected to create hierarchical nanostructures. The key to this approach is combining cubic crystal–structured cores with hexagonal crystal–structured branches in multiple steps. The dimensions and 3D morphology can be controlled by tuning at each synthetic step. These materials have high surface area, high conductivity, and surfaces that can be chemically modified, which are properties that make them ideal electrocatalyst supports. We illustrate the effectiveness of the 3D nanostructures as electrocatalyst supports by coating with nickel-iron oxyhydroxide to achieve high activity and stability for oxygen evolution reaction. This work introduces a synthetic concept to produce a new type of high-performing electrocatalyst support

The T cell receptor displays lateral signal propagation involving non-engaged receptors

T cells are highly sensitive to low levels of antigen, but how this sensitivity is achieved is currently unknown. Here, we imaged proximal TCR-CD3 signal propagation with single molecule localization microscopy (SMLM) in T cells activated with nanoscale clusters of TCR stimuli. We observed the formation of large TCR-CD3 clusters that exceeded the area of the ligand clusters, and required multivalent interactions facilitated by TCR-CD3 phosphorylation for assembly. Within these clustered TCR-CD3 domains, TCR-CD3 signaling spread laterally for ∼500 nm, far beyond the activating site, via non-engaged receptors. Local receptor density determined the functional cooperativity between engaged and non-engaged receptors, but lateral signal propagation was not influenced by the genetic deletion of ZAP70. Taken together, our data demonstrates that clustered ligands induced the clustering of non-ligated TCR-CD3 into domains that cooperatively facilitate lateral signal propagation

TagPaint: Covalent labelling of genetically encoded protein tags for DNA-PAINT imaging

Recently, DNA-PAINT single-molecule localization microscopy (SMLM) has shown great promise for quantitative imaging; however, labelling strategies thus far have relied on multivalent and affinity-based approaches. Here, the covalent labelling of expressed protein tags (SNAP tag and Halo tag) with single DNA-docking strands and application of SMLM via DNA-PAINT is demonstrated. tagPAINT is then used for T-cell receptor signalling proteins at the immune synapse as a proof of principle

Self-assembled monolayers: a journey from fundamental tools for understanding interfaces to commercial sensing technologies

Self-assembled monolayers were first described in the 1980s and have now become ubiquitous in many interfacial technologies. In this account, we discuss different self-assembled monolayer systems, outlining their positives and negatives. We then overview other researchers’ work and our own group’s journey in using self-assembled monolayers to develop new concepts in sensing and addressing general challenges faced by many types of sensors. Finally, we reflect on some of the challenges monolayer chemistry needs to address to facilitate further use of this powerful surface chemistry in commercial devices

How Do Cells Make Decisions: Engineering Micro- and Nanoenvironments for Cell Migration

Cell migration contributes to cancer metastasis and involves cell adhesion to the extracellular matrix (ECM), force generation through the cell's cytoskeletal, and finally cell detachment. Both adhesive cues from the ECM and soluble cues from neighbouring cells and tissue trigger intracellular signalling pathways that are essential for cell migration. While the machinery of many signalling pathways is relatively well understood, how hierarchies of different and conflicting signals are established is a new area of cellular cancer research. We examine the recent advances in microfabrication, microfluidics, and nanotechnology that can be utilized to engineer micro- and nanoscaled cellular environments. Controlling both adhesive and soluble cues for migration may allow us to decipher how cells become motile, choose the direction for migration, and how oncogenic transformations influences these decision-making processes

Injectable hydrogel with MSNs/microRNA-21-5p delivery enables both immunomodification and enhanced angiogenesis for myocardial infarction therapy in pigs

Current therapeutic strategies such as angiogenic therapy and anti-inflammatory therapy for treating myocardial infarction have limited success. An effective approach may benefit from resolution of excessive inflammation combined with enhancement of angiogenesis. Here, we developed a microRNA-21-5p delivery system using functionalized mesoporous silica nanoparticles (MSNs) with additional intrinsic therapeutic effects. These nanocarriers were encapsulated into an injectable hydrogel matrix (Gel@MSN/miR-21-5p) to enable controlled on-demand microRNA-21 delivery triggered by the local acidic microenvironment. In a porcine model of myocardial infarction, we demonstrated that the released MSN complexes notably inhibited the inflammatory response by inhibiting the polarization of M1 macrophage within the infarcted myocardium, while further microRNA-21-5p delivery by MSNs to endothelial cells markedly promoted local neovascularization and rescued at-risk cardiomyocytes. The synergy of anti-inflammatory and proangiogenic effects effectively reduced infarct size in a porcine model of myocardial infarction

Small zinc doped iron oxide tracers for magnetic particle imaging

Magnetic particle imaging (MPI) has garnered significant attention in biomedical imaging research due to its excellent signal intensity that is generated directly from superparamagnetic iron oxide nanoparticles (SPIONs). Small nanoparticle tracers with high saturation magnetisation are crucial for MPI as they can prolong circulation, crossing the blood brain barrier and enhance cellular uptake. In this work, we demonstrate small zinc doped iron oxide nanoparticles (Zn-IONPs) are excellent MPI tracers. Our Zn-IONPs exhibited up to 37 % and 64% enhancement in saturation magnetisation (Msat) value and MPI signal intensity respectively compared to Fe3O4 of the same size. As a result, the polymer encapsulated Zn-IONPs achieved up to 2.7-fold enhancement in MPI signal intensity compared to VivoTrax. Furthermore, these polymer encapsulated NPs were also determined to be non-toxic hence making these Zn-IONPs ideal for many biomedical applications in MPI where small size is critical to prolong circulation time and crossing the blood brain barrier