Femtosecond Drift Photocurrents Generated by an Inversely Designed Plasmonic Antenna.

Photocurrents play a crucial role in various applications, including light detection, photovoltaics, and THz radiation generation. Despite the abundance of methods and materials for converting light into electrical signals, the use of metals in this context has been relatively limited. Nanostructures supporting surface plasmons in metals offer precise light manipulation and induce light-driven electron motion. Through the inverse design optimization of a gold nanostructure, we demonstrate enhanced volumetric, unidirectional, intense, and ultrafast photocurrents via a magneto-optical process derived from the inverse Faraday effect. This is achieved through fine-tuning the amplitude, polarization, and gradients in the local light field. The virtually instantaneous process allows dynamic photocurrent modulation by varying optical pulse duration, potentially yielding nanosources of intense, ultrafast, planar magnetic fields and frequency-tunable THz emission. These findings open avenues for ultrafast magnetic material manipulation and hold promise for nanoscale THz spectroscopy.

Effects of Surface Topography and Cellular Biomechanics on Nanopillar-Induced Bactericidal Activity.

Bacteria are mechanically resistant biological structures that can sustain physical stress. Experimental data, however, have shown that high-aspect-ratio nanopillars deform bacterial cells upon contact. If the deformation is sufficiently large, it lyses the bacterial cell wall, ultimately leading to cell death. This has prompted a novel strategy, known as mechano-bactericide technology, to fabricate antibacterial surfaces. Although adhesion forces were originally proposed as the driving force for mechano-bactericidal action, it has been recently shown that external forces, such as capillary forces arising from an air-water interface at bacterial surfaces, produce sufficient loads to rapidly kill bacteria on nanopillars. This discovery highlights the need to theoretically examine how bacteria respond to external loads and to ascertain the key factors. In this study, we developed a finite element model approximating bacteria as elastic shells filled with cytoplasmic fluid brought into contact with an individual nanopillar or nanopillar array. This model elucidates that bacterial killing caused by external forces on nanopillars is influenced by surface topography and cell biomechanical variables, including the density and arrangement of nanopillars, in addition to the cell wall thickness and elastic modulus. Considering that surface topography is an important design parameter, we performed experiments using nanopillar arrays with precisely controlled nanopillar diameters and spacing. Consistent with model predictions, these demonstrate that nanopillars with a larger spacing increase bacterial susceptibility to mechanical puncture. The results provide salient insights into mechano-bactericidal activity and identify key design parameters for implementing this technology.

Spatially-Localized Functionalization on Nanostructured Surfaces for Enhanced Plasmonic Sensing Efficacy.

This work demonstrates the enhancement in plasmonic sensing efficacy resulting from spatially-localized functionalization on nanostructured surfaces, whereby probe molecules are concentrated in areas of high field concentration. Comparison between SERS measurements on nanostructured surfaces (arrays of nanodisks 110 and 220 nm in diameter) with homogeneous and spatially-localized functionalization with thiophenol demonstrates that the Raman signal originates mainly from areas with high field concentration. TERS measurements with 10 nm spatial resolution confirm the field distribution profiles predicted by the numerical modeling. Though this enhancement in plasmonic sensing efficacy is demonstrated with SERS, results apply equally well to any type of optical/plasmonic sensing on functionalized surfaces with nanostructuring.

Surface micropatterning for the formation of an in vitro functional endothelial model for cell-based biosensors.

Label-free biosensing, such as with surface plasmon resonance (SPR), is a highly efficient method for monitoring the responses of living cells exposed to pharmacological agents and biochemical stimuli in vitro. Conventional cell culture protocols used in cell-based biosensing generally provide little direct control over cell morphologies and phenotypes. Surface micropatterning techniques have been exploited for the controlled immobilization and establishment of well-defined cell morphologies and phenotypes. In this article, surface adhesion micropatterns are used to control the adhesion of endothelial cells within adjacent hexagonal microstructures to promote the emergence of a well-controlled and standardized cell layer phenotype onto SPR sensor surfaces. We show that the formation of cell-cell junctions can be controlled by tuning the inter-cellular spacing in groups of 3 neighbouring cells. Fluorescence microscopy was used to confirm the formation of vascular endothelium cadherin junctions, a structural marker of a functional endothelium. In order to confirm the functionality of the proposed model, the response to thrombin, a modulator of endothelium integrity, was monitored by surface plasmon resonance imaging (SPRI). Experiments demonstrate the potential of the proposed model as a primary biological signal transducer for SPRI-based analysis, with potential applications in cell biology, pharmacology and diagnostic.

Hydrophilic Mechano-Bactericidal Nanopillars Require External Forces to Rapidly Kill Bacteria.

Nanopillars have been shown to mechanically damage bacteria, suggesting a promising strategy for future antibacterial surfaces. However, the mechanisms underlying this phenomena remain unclear, which ultimately limits translational potential toward real-world applications. Using real-time and end-point analysis techniques, we demonstrate that in contrast to initial expectations, bacteria on multiple hydrophilic "mechano-bactericidal" surfaces remained viable unless exposed to a moving air-liquid interface, which caused considerable cell death. Reasoning that normal forces arising from surface tension may underlie this mechano-bactericidal activity, we developed computational and experimental models to estimate, manipulate, and recreate the impact of these forces. Our experiments together demonstrate that a critical level of external force acting on cells attached to nanopillar surfaces can rapidly deform and rupture bacteria. These studies provide fundamental physical insight into how nanopillar surfaces can serve as effective antibacterial materials and suggest use-conditions under which such nanotechnology approaches may provide practical value.

An electrically induced probe of the modes of a plasmonic multilayer stack.

A new single-image acquisition technique for the determination of the dispersion relation of the propagating modes of a plasmonic multilayer stack is introduced. This technique is based on an electrically-driven, spectrally broad excitation source which is nanoscale in size: the inelastic electron tunnel current between the tip of a scanning tunneling microscope (STM) and the sample. The resulting light from the excited modes of the system is collected in transmission using a microscope objective. The energy-momentum dispersion relation of the excited optical modes is then determined from the angle-resolved optical spectrum of the collected light. Experimental and theoretical results are obtained for metal-insulator-metal (MIM) stacks consisting of a silicon oxide layer (70, 190 or 310 nm thick) between two gold films (each with a thickness of 30 nm). The broadband characterization of hybrid plasmonic-photonic transverse magnetic (TM) modes involved in an avoided crossing is demonstrated and the advantages of this new technique over optical reflectivity measurements are evaluated.

Nanoplasmonics-enhanced label-free imaging of endothelial cell monolayer integrity.

Surface plasmon resonance imaging (SPRI) is a powerful label-free imaging modality for the analysis of morphological dynamics in cell monolayers. However, classical plasmonic imaging systems have relatively poor spatial resolution along one axis due to the plasmon mode attenuation distance (tens of µm, typically), which significantly limits their ability to resolve subcellular structures. We address this limitation by adding an array of nanostructures onto the metal sensing surface (25 nm thick, 200 nm width, 400 nm period grating) to couple localized plasmons with propagating plasmons, thereby reducing attenuation length and commensurately increasing spatial imaging resolution, without significant loss of sensitivity or image contrast. In this work, experimental results obtained with both conventional unstructured and nanostructured gold film SPRI sensor chips show a clear gain in spatial resolution achieved with surface nanostructuring. The work demonstrates the ability of the nanostructured SPRI chips to resolve fine morphological detail (intercellular gaps) in experiments monitoring changes in endothelial cell monolayer integrity following the activation of the cell surface protease-activated receptor 1 (PAR1) by thrombin. In particular, the nanostructured chips reveal the persistence of small intercellular gaps (<5 µm2) well after apparent recovery of cell monolayer integrity as determined by conventional unstructured surface based SPRI. This new high spatial resolution plasmonic imaging technique uses low-cost and reusable patterned substrates and is likely to find applications in cell biology and pharmacology by allowing label-free quantification of minute cell morphological activities associated with receptor dependent intracellular signaling activity.

Directional surface enhanced Raman scattering on gold nano-gratings.

Directional plasmon excitation and surface enhanced Raman scattering (SERS) emission were demonstrated for 1D and 2D gold nanostructure arrays deposited on a flat gold layer. The extinction spectrum of both arrays exhibits intense resonance bands that are redshifted when the incident angle is increased. Systematic extinction analysis of different grating periods revealed that this band can be assigned to a propagated surface plasmon of the flat gold surface that fulfills the Bragg condition of the arrays (Bragg mode). Directional SERS measurements demonstrated that the SERS intensity can be improved by one order of magnitude when the Bragg mode positions are matched with either the excitation or the Raman wavelengths. Hybridized numerical calculations with the finite element method and Fourier modal method also proved the presence of the Bragg mode plasmon and illustrated that the enhanced electric field of the Bragg mode is particularly localized on the nanostructures regardless of their size.

Generalized analytical model based on harmonic coupling for hybrid plasmonic modes: comparison with numerical and experimental results.

Metal nanoparticle arrays have proved useful for different applications due to their ability to enhance electromagnetic fields within a few tens of nanometers. This field enhancement results from the excitation of various plasmonic modes at certain resonance frequencies. In this article, we have studied an array of metallic nanocylinders placed on a thin metallic film. A simple analytical model is proposed to explain the existence of the different types of modes that can be excited in such a structure. Owing to the cylinder array, the structure can support localized surface plasmon (LSP) modes. The LSP mode couples to the propagating surface plasmon (PSP) mode of the thin film to give rise to the hybrid lattice plasmon (HLP) mode and anti-crossing phenomenon. Due to the periodicity of the array, the Bragg modes (BM) are also excited in the structure. We have calculated analytically the resonance frequencies of the BM, LSP and the corresponding HLP, and have verified the calculations by rigorous numerical methods. Experimental results obtained in the Kretschmann configuration also validate the proposed analytical model. The dependency of the resonance frequencies of these modes on the structural parameters such as cylinder diameter, height and the periodicity of the array is shown. Such a detailed study can offer insights on the physical phenomenon that governs the excitation of various plasmonic modes in the system. It is also useful to optimize the structure as per required for the different applications, where such types of structures are used.

Transmission and reflection characteristics of metal-coated optical fiber tip pairs.

The optical transmission and reflection in between two metalized optical fiber tips is studied in the optical near-field and far-field domains. In addition to aluminum-coated tips for near-field scanning optical microscopy (NSOM), specifically developed gold-coated fiber tips cut by focused ion beam are investigated. Transverse transmission maps of subwavelength width clearly indicate optical near-field coupling between the tips for short tip distances and become essentially Gaussian-shaped for larger distances in the far-field regime. Moreover, concentric reflection fringes observed for NSOM-type tips illustrate the influence of the receiving fiber tip on the emission pattern of the source tip.

Norovirus capsid proteins self-assemble through biphasic kinetics via long-lived stave-like intermediates.

The self-assembly kinetics for a norovirus capsid protein were probed by time-resolved small-angle X-ray scattering and then analyzed by singular value decomposition and global fitting. Only three species contribute to the total scattering intensities: dimers, intermediates comprising some 11 dimers, and icosahedral T = 3 capsids made up of 90 dimers. Three-dimensional reconstructions of the intermediate robustly show a stave-like shape consistent with an arrangement of two pentameric units connected by an interstitial dimer. Upon triggering of self-assembly, the biphasic kinetics consist of a fast step in which dimers are assembled into intermediates, followed by a slow step in which intermediates interlock into capsids. This simple kinetic model reproduces experimental data with an excellent agreement over 6 decades in time and with nanometer resolution. The extracted form factors are robust against changes in experimental conditions. These findings challenge and complement currently accepted models for the assembly of norovirus capsids.

Unusual self-assembly properties of Norovirus Newbury2 virus-like particles.

In the Caliciviridae family of nonenveloped, positive-stranded RNA viruses, Noroviruses are major causes of human and animal gastroenteritis worldwide. The Norovirus T=3 icosahedral capsid is made of 180 copies of the VP1 protein, as exemplified in the crystal structure of the virus-like particle (VLP) of the human Norwalk virus (NV). It was previously shown that the ca 40-nm recombinant NV VLP can be disassembled and reassembled in vitro. Here we report on the disassembly and self-assembly properties for the related (VP1 sequence identity of 50%) bovine Newbury2 Norovirus (NB2) VLP. Using a panel of biophysical techniques, we show that while the NB2 VLP displays disassembly properties similar to the NV VLP, NB2-VP1 shows remarkable self-assembly properties heretofore unreported for NV-VP1 or any other calicivirus capsid protein. These properties include the capabilities of self-assembling not only into regular T=3 capsids but also into larger VLP (up to 76 nm in diameter) and of tolerating substitution of the spike domain for that of a distantly related Calicivirus. In conditions favoring the natural, T=3 capsid, NB2-VP1 reproducibly assembles by an apparent two-phase process. Our results establish a robust new system with which to probe the dynamics of viral capsid self-assembly.