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This review article focuses on the latest achievements in the creation of a class of electrotuneable optical metamaterials for switchable mirrors/windows, variable colour mirrors, optical filters, and SERS sensors, based on the voltage-controlled self-assembly of plasmonic nanoparticles at liquid/liquid or solid/liquid electrochemical interfaces. Practically, these experimental systems were navigated by physical theory, the role of which was pivotal in defining the optimal conditions for their operation, but which itself was advanced in feedback with experiments. Progress and problems in the realisation of the demonstrated effects for building the corresponding devices are discussed. To put the main topic of the review in a wider perspective, the article also discusses a few other types of electrovariable metamaterials, as well as some of those that are controlled by chemistry.

It is not uncommon for students to view laboratory instruments as black boxes. Unfortunately, this can often result in poor experimental results and interpretation. To tackle this issue, a laboratory course was designed to enable students not only to critically think about operating principles of the instrument but also to improve interpretation skills. Students were required to build their own visible spectrometer using interlocking building bricks with simple optical elements and a Raspberry Pi computer. Experiments were then conducted to explore the instrumental capabilities while, at the same time, using Python programming to plot data, perform linear least-squares fitting, and calculate errors. Instrument response and spectral measurements were followed by kinetic studies, enabling the students to tackle a "real" problem by extracting rate constants. The main learning outcomes were that the students would gain a better understanding of instrumental components and at the same time learn valuable analytical techniques such as calibration, determination of the limits of linearity, and dynamic range. These outcomes were achieved by applying a problem based learning approach.

Recent innovations in single-cell technologies have opened up exciting possibilities for profiling the omics of individual cells. Minimally invasive analysis tools that probe and remove the contents of living cells enable cells to remain in their standard microenvironment with little impact on their viability. This negates the requirement of lysing cells to access their contents, an advancement from previous single-cell manipulation methods. These novel methods have the potential to be used for dynamic studies on single cells, with many already providing high intracellular spatial resolution. In this article, we highlight key technological advances that aim to remove the contents of living cells for downstream analysis. Recent applications of these techniques are reviewed, along with their current limitations. We also propose recommendations for expanding the scope of these technologies to achieve comprehensive single-cell tracking in the future, anticipating the discovery of subcellular mechanisms and novel therapeutic targets and treatments, ultimately transforming the fields of spatial transcriptomics and personalised medicine. [ABSTRACT FROM AUTHOR]

Here, we introduce high-strength carbon nanofibers (CNFs) into optimized polymer–nanoparticle composite formulations [modified SiO2 nanoparticles/high-density polyethylene (HDPE)] to generate superhydrophobic surface coatings that are directly integrated into HDPE substrates. This is achieved through the use of a parallel plate hot pressing process and a unique design approach that considers the chemical properties of individual formulation components within a ternary system. Subsequently, this enables the generation of resilient, high-functioning, nano/microscale materials while increasing potential lifetimes, through integrating self-cleaning functionality into the polymer. The most encouraging nanocomposite surface coating was found to surpass 100 abrasion cycles while retaining its high water repellency, displaying a static contact angle of 150 ± 3° and tilting angle of 18 ± 7° after 4 weeks of continual submersion (from values of 156 ± 3 and 5 ± 1°, respectively), under a hydrostatic pressure of 7.85 kPa (80 cm depth), where it was found to remain fully functional as a self-cleaning coating. [ABSTRACT FROM AUTHOR]

Low-dimensional van der Waals (vdW) materials can harness tightly confined polaritonic waves to deliver unique advantages for nanophotonic biosensing. The reduced dimensionality of vdW materials, as in the case of two-dimensional graphene, can greatly enhance plasmonic field confinement, boosting sensitivity and efficiency compared to conventional nanophotonic devices that rely on surface plasmon resonance in metallic films. Furthermore, the reduction of dielectric screening in vdW materials enables electrostatic tunability of different polariton modes, including plasmons, excitons, and phonons. One-dimensional vdW materials, particularly single-walled carbon nanotubes, possess unique form factors with confined excitons to enable single-molecule detection as well as in vivo biosensing. We discuss basic sensing principles based on vdW materials, followed by technological challenges such as surface chemistry, integration, and toxicity. Finally, we highlight progress in harnessing vdW materials to demonstrate new sensing functionalities that are difficult to perform with conventional metal/dielectric sensors. [ABSTRACT FROM AUTHOR]

Nanopores in solid-state membranes are promising for a wide range of applications including DNA sequencing, ultra-dilute analyte detection, protein analysis, and polymer data storage. Techniques to fabricate solid-state nanopores have typically been time consuming or lacked the resolution to create pores with diameters down to a few nanometres, as required for the above applications. In recent years, several methods to fabricate nanopores in electrolyte environments have been demonstrated. These in situ methods include controlled breakdown (CBD), electrochemical reactions (ECR), laser etching and laser-assisted controlled breakdown (la-CBD). These techniques are democratising solid-state nanopores by providing the ability to fabricate pores with diameters down to a few nanometres (i.e. comparable to the size of many analytes) in a matter of minutes using relatively simple equipment. Here we review these in situ solid-state nanopore fabrication techniques and highlight the challenges and advantages of each method. Furthermore we compare these techniques by their desired application and provide insights into future research directions for in situ nanopore fabrication methods. [ABSTRACT FROM AUTHOR]

Analytes with similar redox properties are normally difficult to distinguish through classic electrochemical methods. This becomes especially true for the on‐site detection in seawater where the high salinity and complex chemical components can impose severe interference. Hereby introducing numerous nanoscale heterojunctions in the Cu/CuO/reduced graphene oxide (rGO)/polypyrrole (PPy) and Cu/CuO/rGO/chitosan electrochemical sensors, tunable interfacial energy barriers to exponentially regulate the electrochemical signal can be constructed. Importantly, these energy barriers are independent to redox but closely related to the electrostatic interaction from absorbed charged analytes such as Hg2+ and Cu2+. Moreover, the similar sensing principle is also valid for the energy barriers in p‐n junctions as demonstrated in the Ni/NiO/ZnO/PPy sensor. The good anti‐interference properties and ultrahigh sensitivity of this sensing mode offers new opportunities in trace analyte detection in harsh environments such as seawater. [ABSTRACT FROM AUTHOR]

The ability to sense proteins and protein‐related interactions at the single‐molecule level is becoming of increasing importance to understand biological processes and diseases better. Single‐molecule sensors, such as nanopores have shown substantial promise for the label‐free detection of proteins; however, challenges remain due to the lack of selectivity and the need for relatively high analyte concentrations. An aptamer‐functionalized nanopore extended field‐effect transistor (nexFET) sensor is reported here, where protein transport can be controlled via the gate voltage that in turn improves single‐molecule sensitivity and analyte capture rates. Importantly, these sensors allow for selective detection, based on the choice of aptamer chemistry, and can provide a valuable addition to the existing methods for the analysis of proteins and biomarkers in biological fluids. [ABSTRACT FROM AUTHOR]

We present a method for improving detection efficiencies in single molecule confocal fluorescence spectroscopy with subfemtoliter probe volumes within microfluidic channels. Our approach is based on hydrodynamically focusing an analyte stream within a microfluidic channel down to a width on the same order of magnitude as that of the confocal probe volume. Experiments are performed in which fluorescently labeled polystyrene microspheres (930 nm diameter) are motivated through a microchannel and passed through a focused laser beam at a variety of flow rates (0.1-11 μL/min). Hydrodynamic focusing of the analyte stream is achieved by introduction of two sheath flow streams that flank the central analyte stream. Through variation of the relative flow rates in each input stream the analyte stream can be controlled with micron resolution. A maximum hydrodynamic focusing width of 3 μm was achieved within a 50 μm wide microfluidic channel; hence, a larger proportion of molecules traveling through the microfluidic device were detected. Furthermore, simple statistical methods are used to investigate the resulting fluorescence bursts and generate single-particle burst width and burst area distributions. From these data, the total detection efficiencies are shown to be an order of magnitude better than those achievable in conventional unfocused systems. [ABSTRACT FROM AUTHOR]

Electrophoretic mobility differences of biological molecules are frequently exploited to physically separate and subsequently identify the components of a mixture. We present a method to rapidly identify single molecules by measuring both their mobility and fluorescence emission under continuous flow without separation. Submicrometer fluidic channels were used to detect individual nucleic-acid-engineered fluorescent labels driven electrokinetically in free solution. Two separate focal volumes along the length of the fluidic channel collected spectral, spatial, and temporal information from the passage of fluorescent labels through the channel. One focal volume was defined by a focused 488-nm-wavelength laser and the other by a focused 568-nm laser. The subfemtoliter focal volumes resulted in signal-to-noise ratios sufficient for single-fluorophore detection, and the two excitation wavelengths enabled detection of multicolor fluorescent labels and discrimination of single-color detection events. Each fluorescent label was uniformly excited and analyzed as it passed through the channel. Flow control facilitated high throughput at low concentrations, as well as a balance of several experimental parameters. Two fluorescent labels were considered for identification by single-molecule mobility measurements. Approximately 81% of fluorescent labels of one variety and 77% of the other were found to be identifiable based on their mobility alone. As implemented, this method could be used in conjunction with spectral analysis of fluorescent labels to enhance the resolution of single-molecule identification. Ultimately, this technique could be used autonomously to detect biomolecules bound to fluorescent labels and to identify similarly labeled biomolecules by their mobility. [ABSTRACT FROM AUTHOR]

We present a nonlithographic approach for forming free standing nanochannels, made of a variety of materials, that can be easily integrated with microfabricated structures. The approach uses a deposited polymeric fiber as a sacrificial template around which a deposited coating forms a tube. We formed suspended nanochannels of silica glass spanning a trench on a silicon wafer and used these structures for detection of single fluorescently labeled proteins. This geometry provides excellent isolation of the molecules of interest and also separates them from surrounding material that could create unwanted background fluorescence. The same geometry provides a platform for observing motion and mechanical response of the suspended nanochannel, and we measured the mechanical resonance of a glass channel of the type used for the fluorescent detection. This type of structure provides a general approach for integrating fluid carrying nanochannels with microstructures. [ABSTRACT FROM AUTHOR]

There has been a significant drive to deliver nanotechnological solutions to biosensing, yet there remains an unmet need in the development of biosensors that are affordable, integrated, fast, capable of multiplexed detection, and offer high selectivity for trace analyte detection in biological fluids. Herein, some of these challenges are addressed by designing a new class of nanoscale sensors dubbed nanopore extended field-effect transistor (nexFET) that combine the advantages of nanopore single-molecule sensing, field-effect transistors, and recognition chemistry. We report on a polypyrrole functionalized nexFET, with controllable gate voltage that can be used to switch on/off, and slow down single-molecule DNA transport through a nanopore. This strategy enables higher molecular throughput, enhanced signal-to-noise, and even heightened selectivity via functionalization with an embedded receptor. This is shown for selective sensing of an anti-insulin antibody in the presence of its IgG isotype. [ABSTRACT FROM AUTHOR]

Mirror-on-mirror platforms based on arrays of metallic nanoparticles, arranged top-down or self-assembled on a thin metallic film, have interesting optical properties. Interaction of localized surface-plasmons in nanoparticles with propagating surface-plasmons in the film underpins the exotic features of such platforms. Here, we present a comprehensive theoretical framework which emulates such a system using a five-layer-stack model and calculate its reflectance, transmittance, and absorbance spectra. The theory rests on dipolar quasi-static approximations incorporating image-forces and effective medium theory. Systematically tested against full-wave simulations, this simple approach proves to be adequate within its obvious applicability limits. It is used to study optical signals as a function of nanoparticle dimensions, interparticle separation, metal film thickness, the gap between the film and nanoparticles, and incident light characteristics. Several peculiar features are found, e.g., quenching of reflectivity in certain frequency domains or shift of the reflectivity spectra. Schemes are proposed to tailor those as functions of the mentioned parameters. Calculating the system's optical responses in seconds, as compared to much longer running simulations, this theory helps to momentarily unravel the role of each system parameter in light reflection, transmission, and absorption, facilitating thereby the design and optimisation of novel mirror-on-mirror systems. [ABSTRACT FROM AUTHOR]

Compartmentalised structures based on droplet interface bilayers (DIBs), including multisomes and compartmentalised vesicles, are seen by many as the next generation of biomimetic soft matter devices. Herein, we outline a microfluidic approach for the construction of miniaturised multisomes of pL volumes in high-throughput and demonstrate their potential as vehicles for in situ chemical synthesis. [ABSTRACT FROM AUTHOR]