The spread of SARS-CoV-2 led to the emergence of several variants of concern (VOCs). The spike glycoprotein, responsible for engaging the viral receptor, exhibits the highest density of mutations, suggesting an ongoing evolution to optimize viral entry. This study characterizes the bond formed by virion mimics carrying the SARS-CoV-2 spike protein and the plasma membrane of host cells in the early stages of virus entry. Contrary to the traditional analysis of isolated ligand-receptor pairs, we utilized well-defined biomimetic models and biochemical and biophysical techniques to characterize the multivalent interaction of VOCs with the complex cell membrane. We observed an overall increase in the binding affinity for newer VOCs. By progressively reducing the system complexity, we identify heparan sulfate (HS) as a main driver of this variation, with a 10-fold increase in affinity for Omicron BA.1 over that of the original strain. These results demonstrate the essential role of coreceptors, particularly HS, in the modulation of SARS-CoV-2 infection and highlight the importance of multiscale biophysical and biochemical assays that account for membrane complexity to fully characterize and understand the role of molecular components and their synergy in viral attachment and entry.

Solid state nanopores have emerged as an important electrical label-free single-molecule detection platform. While much effort has been spent on analyzing the current trace to determine size, shape and charge of the translocating species, a less studied aspect is the number of events and how this relates to analyte concentration. In this work we systematically investigate how the event frequency depends on voltage applied across the pore and show that this dependence can be utilized to determine target concentration. Importantly, this method does not require any calibration or any additional species added to the solution. Data analysis algorithms are introduced to accurately count events also for high voltages (up to 1 V). For double stranded DNA as model analyte, we find a linear relation between event frequency and voltage for pores 10 nm or more in diameter. For smaller pores, the majority of events are dockings rather than translocations and the linear relation is lost, in agreement with theory. Our model also predicts that the electrophoretic mobility of the species will influence event frequency, while diffusivity does not, which we confirm by using two different sizes of DNA. The analyte concentration determination is found to be remarkably accurate (10% error) when taking the average of multiple (∼4) experiments. If based on a single experiment, the predictive power is lower, but the method still provides a useful estimate (<30% error). This study should be useful as a guide when performing experiments at higher voltages and may serve as a method to extract analyte concentration in bioanalytical applications of nanopore sensors.

As demand for immersive experiences grows, displays are moving closer to the eye with smaller sizes and higher resolutions. However, shrinking pixel emitters reduce intensity, making them harder to perceive. Electronic Papers utilize ambient light for visibility, maintaining optical contrast regardless of pixel size, but cannot achieve high resolution. We show electrically tunable meta-pixels down to 560 nm in size (>45,000 PPI) consisting of WO3 nanodiscs, allowing one-to-one pixel-photodetector mapping on the retina when the display size matches the pupil diameter, which we call Retina Electronic Paper. Our technology also supports video display (25 Hz), high reflectance ( 80 optical contrast ( 50 display.

Reflective pixels made by plasmonic metasurfaces and tuned by electrochromics exhibit significant potential to be used as flexible, polychromatic, electronic paper.

Recent years have shown many advances in the development of tunable structural colors by combining nanostructures with electrochromic materials. One main goal is to develop energy saving color displays that rely on ambient light instead of being emissive. However, all displays need to be pixelated to show arbitrary images and few studies have addressed the challenge of preparing and controlling individual electrochromic pixels. Herein, a very simple method to reach this milestone by using passive matrix addressing is presented, which requires no additional electronic components in the pixels. It is shown that the common transparent conductor indium tin oxide (ITO) in non‐aqueous electrolytes exhibits the diode‐like behavior (threshold in voltage in relation to current and coloration) necessary to prevent significant cross‐talk between pixels. The chemical nature of the redox activity that enables this behavior is attributed to omnipresent oxygen and the formation of superoxide ions. Additionally, it is shown that a gel‐like electrolyte can be prepared by optical lithography, which makes the concept compatible with patterning of pixels at high resolution. This method for preparing pixelated displays should be compatible with practically any type of electrochromic surface in both reflective and transmissive configurations. Also, the counter electrode maintains excellent transparency since it simply consists of ITO. The results should prove very useful as the research field of tunable structural colors moves from proof‐of‐concept to real devices.

Gold nanoparticles possess unique photothermal properties and have gained considerable interest in biomedical research, particularly for photothermal therapy (PTT). This study focuses on evaluating the photothermal properties of gold nanorods (AuNRs) supported on glass substrates upon excitation with near-infrared (NIR) light. Two aspect ratios of AuNRs were electrostatically immobilized onto glass with controlled coverage. In situ X-ray diffraction (XRD) was performed to evaluate the photothermal behavior and morphological changes of the supported AuNRs during NIR laser irradiation. The XRD data sets were corroborated with scanning electron microscopy and Vis-NIR spectroscopy characterization. XRD revealed a linear temperature increase with laser power, aligning with theoretical predictions, and a slope dependent on the AuNR coverage, until the onset of morphology transformations around 120 degrees C. This study provides valuable insights into the photothermal properties of supported AuNRs, crucial for their application in PTT.

The possibility to detect and analyze single or few biological molecules is very important for understanding interactions and reaction mechanisms. Ideally, the molecules should be confined to a nanoscale volume so that the observation time by optical methods can be extended. However, it has proven difficult to develop reliable, non-invasive trapping techniques for biomolecules under physiological conditions. Here we present a platform for long-term tether-free (solution phase) trapping of proteins without exposing them to any field gradient forces. We show that a responsive polymer brush can make solid state nanopores switch between a fully open and a fully closed state with respect to proteins, while always allowing the passage of solvent, ions and small molecules. This makes it possible to trap a very high number of proteins (500-1000) inside nanoscale chambers as small as one attoliter, reaching concentrations up to 60 gL-1. Our method is fully compatible with parallelization by imaging arrays of nanochambers. Additionally, we show that enzymatic cascade reactions can be performed with multiple native enzymes under full nanoscale confinement and steady supply of reactants. This platform will greatly extend the possibilities to optically analyze interactions involving multiple proteins, such as the dynamics of oligomerization events.

Electrochromic materials and their implementation with structural colors are currently being intensely researched because of their promising applications as non-emissive display devices utilizing ambient light. In particular, several fully inorganic devices that rely on electrochromic tungsten trioxide (WO3) have been presented. For preparing nanoscale films of this material, sputtering is the most established technique, but electrodeposition has recently been shown to be capable of achieving exceptionally high electro-optical modulation contrast without the need for expensive equipment. In this work, we investigate the possibilities of electrodeposited WO3 and present a systematic comparison with sputtered WO3 with respect to performance in electrochromic devices. Importantly, we show that "ultralarge" electro-optical modulation (∼95% change in transmission) is possible for both types of films. However, it is only the sputtered films that enable such high contrast in a stable electrolyte such as LiClO4 in propylene carbonate. The electrodeposited films are less uniform and difficult to make thicker than ∼500 nm. We find no evidence that the electrochromic properties of the electrodeposited WO3 are intrinsically better than those of sputtered WO3. However, the electrodeposited films are much rougher and/or porous on the nanoscale, which increases the switching speed considerably. We conclude that electrodeposited WO3 is mainly useful in applications in which high contrast is not essential while switching speed is. As an example, we present the first electrodeposited WO3 integrated with structural colors by sandwiching the material between two metal films. By electrical control, the reflective colors can then be tuned at least one order of magnitude faster (a few seconds) than previously reported while having fair color quality and without any loss of brightness.

Low-cost, flexible and thin display technology is becoming an interesting field of research as it can accompany the wide range of sensors being developed. Here, the synthesis of poly(dimethylpropylene-dioxythiophene) (PProDOT-Me-2) by combining vapor phase polymerization and screen printing is presented. A multilayer architecture using poly(3,4-ethylenedioxythiophene) (PEDOT) and PProDOT-Me-2 to allow for electrochromic switching of PProDOT-Me-2, thereby eliminating the need for a supporting transparent conductive (metal oxide) layer is introduced. Furthermore, the technology is adapted to a blended architecture, which removes the additional processing steps and results in improved color contrast ( increment E* > 25). This blend architecture is extended to other conductive polymers, such as PEDOT and polypyrrole (PPy), to highlight the ability of the technique to adjust the color of all-printed electrochromic displays. As a result, a green color is obtained when combining the blue and yellow states of PEDOT and PPy, respectively. This technology has the potential to pave the way for all-printed multicolored electrochromic displays for further utilization in printed electronic systems in various Internet of Things applications.

Recent advances in nanofabrication technologies have enabled new ways to produce structural colors. By combining nanofabrication methods, it is possible to integrate electrochromic materials with the nanostructures, which enable electrical tuning of the colors and thus new types of reflective displays. Previous work has shown high quality colors and high switching contrast in general. However, so far the intensity modulation has always been more limited in the blue. In this work we prepare blue structural colors and synthesize films of an electrochromic polymer (PProDOP) that is optimized for high contrast in this spectral region. A protocol for electropolymerization of PProDOP on gold surfaces is presented. The polymer films are shown to follow Lambert-Beer behavior and can provide up to 75% contrast (difference in transmittivity). On blue nanostructures, the reflectivity can be modulated with a contrast of 50%, which is a considerable improvement in comparison with previous work. The results presented here should be useful for electrochromic or other electro-optical devices operating in the blue spectral region.

Dynamically tunable reflective structural colors are attractive for reflective displays (electronic paper). However, it is challenging to tune a thin layer of structural color across the full red–green–blue (RGB) basis set of colors at video rates and with long‐term stability. In this work, this is achieved through a hybrid cavity built from metal–insulator–metal (MIM) “nanocaves” and an electrochromic polymer (PProDOTMe 2 ). The reflective colors are modulated by electrochemically doping/dedoping the polymer. Compared with traditional subpixel‐based systems, this hybrid structure provides high reflectivity (>40%) due to its “monopixel” nature and switches at video rates. The polymer bistability helps deliver ultralow power consumption (≈2.5 mW cm −2 ) for video display applications and negligible consumption (≈3 µW cm −2 ) for static images, compatible with fully photovoltaic powering. In addition, the color uniformity of the hybrid material is excellent (over cm −2 ) and the scalable fabrication enables large‐area production.

In nanobiotechnology, the importance of controlling interactions between biological molecules and surfaces is paramount. In recent years, many devices based on nanostructured silicon materials have been presented, such as nanopores and nanochannels. However, there is still a clear lack of simple, reliable, and efficient protocols for preventing and controlling biomolecule adsorption in such structures. In this work, we show a simple method for passivation or selective biofunctionalization of silica, without the need for polymerization reactions or vapor-phase deposition. The surface is simply exposed stepwise to three different chemicals over the course of ∼1 h. First, the use of aminopropylsilatrane is used to create a monolayer of amines, yielding more uniform layers than conventional silanization protocols. Second, a cross-linker layer and click chemistry are used to make the surface reactive toward thiols. In the third step, thick and dense poly(ethylene glycol) brushes are prepared by a grafting-to approach. The modified surfaces are shown to be superior to existing options for silica modification, exhibiting ultralow fouling (a few ng/cm2) after exposure to crude serum. In addition, by including a fraction of biotinylated polymer end groups, the surface can be functionalized further. We show that avidin can be detected label-free from a serum solution with a selectivity (compared to nonspecific binding) of more than 98% without the need for a reference channel. Furthermore, we show that our method can passivate the interior of 150 nm × 100 nm nanochannels in silica, showing complete elimination of adsorption of a sticky fluorescent protein. Additionally, our method is shown to be compatible with modifications of solid-state nanopores in 20 nm thin silicon nitride membranes and reduces the noise in the ion current. We consider these findings highly important for the broad field of nanobiotechnology, and we believe that our method will be very useful for a great variety of surface-based sensors and analytical devices.

Surface plasmon resonance is a very well-established surface sensitive technique for label-free analysis of biomolecular interactions, generating thousands of publications each year. An inconvenient effect that complicates interpretation of SPR results is the "bulk response" from molecules in solution, which generate signals without really binding to the surface. Here we present a physical model for determining the bulk response contribution and verify its accuracy. Our method does not require a reference channel or a separate surface region. We show that proper subtraction of the bulk response reveals an interaction between poly(ethylene glycol) brushes and the protein lysozyme at physiological conditions. Importantly, we also show that the bulk response correction method implemented in commercial instruments is not generally accurate. Using our method, the equilibrium affinity between polymer and protein is determined to be KD = 200 μM. One reason for the weak affinity is that the interaction is relatively short-lived (1/koff < 30 s). Furthermore, we show that the bulk response correction also reveals the dynamics of self-interactions between lysozyme molecules on surfaces. Besides providing new insights on important biomolecular interactions, our method can be widely applied to improve the accuracy of SPR data generated by instruments worldwide.

Surface plasmon resonance (SPR) is a highly useful technique in biology and is gradually becoming useful also for materials science. However, measurements to date have been performed almost exclusively on gold, which limits the possibility to probe chemical modifications of other metals. In this work we show that 20 nm Pd and Pt films work "fairly well" for quantitative SPR sensing of organic films despite the high light absorption. In the interval between total reflection and the SPR angle, high intensity changes occur when a film is formed on the surface. Fresnel models accurately describe the full angular spectra and our data analysis provides good resolution of surface coverage in air (a few ng cm-2). Overall, the Pd sensors behave quite similarly to 50 nm gold in terms of sensitivity and field extension, although the noise level in real-time measurements is ∼5 times higher. The Pt sensors exhibit a longer extension of the evanescent field and ∼10 times higher noise compared to gold. Yet, formation of organic layers a few nm in thickness can still be monitored in real-time. As a model system, we use thiolated poly(ethylene glycol) to make Pd and Pt protein repelling. Our findings show how SPR can be used for studying chemical modifications of two metals that are important in several contexts, for instance within heterogeneous catalysis. We emphasize the advantages of simple sample preparation and accurate quantitative analysis in the planar geometry by Fresnel models.

Plasmonic metasurfaces for color generation are emerging as important components for next generation display devices. Fabricating bright plasmonic colors economically and via easily scalable methods, however, remains difficult. Here, the authors demonstrate an efficient and scalable strategy based on colloidal lithography to fabricate silver‐based reflective metal–insulator–nanodisk plasmonic cavities that provide a cyan‐magenta‐yellow (CMY) color palette with high relative luminance. With the same basic structure, they exploit different mechanisms to efficiently produce a complete subtractive color palette. Finite‐difference time‐domain simulations reveal that these mechanisms include gap surface plasmon modes for thin insulators and hybridized modes between disk plasmons and Fabry–Pérot modes for thicker systems. To produce yellow hues, they take advantage of higher‐energy gap surface plasmon modes to allow resonance dips in the blue spectral region for comparably large nanodisks, thereby circumventing difficult fabrication of nanodisks less than 80 nm. It is anticipated that incorporation of these strategies can reduce fabrication constraints, produce bright saturated colors, and expedite large‐scale production.

The nuclear pore complex is a nanoscale assembly that achieves shuttle-cargo transport of biomolecules: a certain cargo molecule can only pass the barrier if it is attached to a shuttle molecule. In this review we summarize the most important efforts aiming to reproduce this feature in artificial settings. This can be achieved by solid state nanopores that have been functionalized with the most important proteins found in the biological system. Alternatively, the nanopores are chemically modified with synthetic polymers. However, only a few studies have demonstrated a shuttle-cargo transport mechanism and due to cargo leakage, the selectivity is not comparable to that of the biological system. Other recent approaches are based on DNA origami, though biomolecule transport has not yet been studied with these. The highest selectivity has been achieved with macroscopic gels, but they are yet to be scaled down to nano-dimensions. It is concluded that although several interesting studies exist, we are still far from achieving selective and efficient artificial shuttle-cargo transport of biomolecules. Besides being of fundamental interest, such a system could be potentially useful in bioanalytical devices.

AbstractInterfaces functionalized with polymers are known for providing excellent resistance towards biomolecular adsorption and for their ability to bind high amounts of protein while preserving their structure. However, making an interface that switches between these two states has proven challenging and concepts to date rely on changes in the physiochemical environment, which is static in biological systems. Here we present the first interface that can be electrically switched between a high‐capacity (>1 μg cm−2) multilayer protein binding state and a completely non‐fouling state (no detectable adsorption). Switching is possible over multiple cycles without any regeneration. Importantly, switching works even when the interface is in direct contact with biological fluids and a buffered environment. The technology offers many applications such as zero fouling on demand, patterning or separation of proteins as well as controlled release of biologics in a physiological environment, showing high potential for future drug delivery in vivo.