Advances in nonlinear metasurfaces for imaging, quantum, and sensing applications.

Metasurfaces, composed of artificial meta-atoms of subwavelength size, can support strong light-matter interaction based on multipolar resonances and plasmonics, hence offering the great capability of empowering nonlinear generation. Recently, owing to their ability to manipulate the amplitude and phase of the nonlinear emission in the subwavelength scale, metasurfaces have been recognized as ultra-compact, flat optical components for a vast range of applications, including nonlinear imaging, quantum light sources, and ultrasensitive sensing. This review focuses on the recent progress on nonlinear metasurfaces for those applications.

Energy landscape of conformational changes for a single unmodified protein.

Resolving the free energy landscapes that govern protein biophysics has been obscured by ensemble averaging. While the folding dynamics of single proteins have been observed using fluorescent labels and/or tethers, a simpler and more direct measurement of the conformational changes would not require modifications to the protein. We use nanoaperture optical tweezers to resolve the energy landscape of a single unmodified protein, Bovine Serum Albumin (BSA), and quantify changes in the three-state conformation dynamics with temperature.

Optical scattering methods for the label-free analysis of single biomolecules.

Single-molecule techniques to analyze proteins and other biomolecules involving labels and tethers have allowed for new understanding of the underlying biophysics; however, the impact of perturbation from the labels and tethers has recently been shown to be significant in several cases. New approaches are emerging to measure single proteins through light scattering without the need for labels and ideally without tethers. Here, the approaches of interference scattering, plasmonic scattering, microcavity sensing, nanoaperture optical tweezing, and variants are described and compared.

Structural Flexibility and Disassembly Kinetics of Single Ferritin Molecules Using Optical Nanotweezers.

Ferritin, a spherical protein shell assembled from 24 subunits, functions as an efficient iron storage and release system through its channels. Understanding how various chemicals affect the structural behavior of ferritin is crucial for unravelling the origins of iron-related diseases in living organisms including humans. In particular, the influence of chemicals on ferritin's dynamics and iron release is barely explored at the single-protein level.

Electrical Transport and Dynamics of Confined DNA through Highly Conductive 2D Graphene Nanochannels.

Confining DNA in nanochannels is an important approach to studying its structure and transportation dynamics. Graphene nanochannels are particularly attractive for studying DNA confinement due to their atomic flatness, precise height control, and excellent mechanical strength. Here, using femtosecond laser etching and wetting transfer, we fabricate graphene nanochannels down to less than 4.

Label-Free Tracking of Proteins through Plasmon-Enhanced Interference.

Single unmodified biomolecules in solution can be observed and characterized by interferometric imaging approaches; however, Rayleigh scattering limits this to larger proteins (typically >30 kDa). We observe real-time image tracking of unmodified proteins down to 14 kDa using interference imaging enhanced by surface plasmons launched at an aperture in a metal film. The larger proteins show slower diffusion, quantified by tracking.

Simultaneous Determination of the Size and Shape of Single α-Synuclein Oligomers in Solution.

Soluble oligomers of amyloid-forming proteins are implicated as toxic species in the context of several neurodegenerative diseases. Since the size and shape of these oligomers influence their toxicity, their biophysical characterization is essential for a better understanding of the structure-toxicity relationship. Amyloid oligomers are difficult to characterize by conventional approaches due to their heterogeneity in size and shape, their dynamic aggregation process, and their low abundance.

Optical Monitoring of Iron Loading into Single, Native Ferritin Proteins.

Ferritin is a protein that stores and releases iron to prevent diseases associated with iron dysregulation in plants, animals, and bacteria. The conversion between iron-loaded holo-ferritin and empty apo-ferritin is an important process for iron regulation. To date, studies of ferritin have used either ensemble measurements to quantify the characteristics of a large number of proteins or single-molecule approaches to interrogate labeled or modified proteins.

Localized Nanopore Fabrication via Controlled Breakdown.

Nanopore sensors provide a unique platform to detect individual nucleic acids, proteins, and other biomolecules without the need for fluorescent labeling or chemical modifications. Solid-state nanopores offer the potential to integrate nanopore sensing with other technologies such as field-effect transistors (FETs), optics, plasmonics, and microfluidics, thereby attracting attention to the development of commercial instruments for diagnostics and healthcare applications. Stable nanopores with ideal dimensions are particularly critical for nanopore sensors to be integrated into other sensing devices and provide a high signal-to-noise ratio.

Flatband mode in photonic moiré superlattice for boosting second-harmonic generation with monolayer van der Waals crystals.

We theoretically investigate boosting second-harmonic generation (SHG) of monolayer van der Waals crystals by employing flatband modes hosted by photonic moiré superlattices. Such a system with high quality factor and a monolayer crystal accommodated on the top of it, provides a unique opportunity to enhance and manipulate SHG emission. We show that employing a doubly resonant diagram on such a moiré superlattice system not only boosts the SHG, but also tunes the directional emission of the second-harmonic wave.

Effects of off-axis translocation through nanopores on the determination of shape and volume estimates for individual particles.

Resistive pulses generated by nanoparticles that translocate through a nanopore contain multi-parametric information about the physical properties of those particles. For example, non-spherical particles sample several different orientations during translocation, producing fluctuations in blockade current that relate to their shape. Due to the heterogenous distribution of electric field from the center to the wall of a nanopore while a particle travels through the pore, its radial position influences the blockade current, thereby affecting the quantification of parameters related to the particle's characteristics.

Rewritable Nanoplasmonics through Room-Temperature Phase Manipulations of Vanadium Dioxide.

The interactions between light and plasmonic charge oscillations in conducting materials are important venues for realizing nanoscale light manipulations. Conventional metal-based plasmonic devices lack tunability due to the fixed material permittivities. Here, we show that reconfigurable plasmonic functionalities can be achieved using the spatially controlled phase transitions in strongly correlated oxide films.

Surface coatings for solid-state nanopores.

Since their introduction in 2001, solid-state nanopores have been increasingly exploited for the detection and characterization of biomolecules ranging from single DNA strands to protein complexes. A major factor that enables the application of nanopores to the analysis and characterization of a broad range of macromolecules is the preparation of coatings on the pore wall to either prevent non-specific adhesion of molecules or to facilitate specific interactions of molecules of interest within the pore. Surface coatings can therefore be useful to minimize clogging of nanopores or to increase the residence time of target analytes in the pore.

Estimation of Shape, Volume, and Dipole Moment of Individual Proteins Freely Transiting a Synthetic Nanopore.

This paper demonstrates that high-bandwidth current recordings in combination with low-noise silicon nitride nanopores make it possible to determine the molecular volume, approximate shape, and dipole moment of single native proteins in solution without the need for labeling, tethering, or other chemical modifications of these proteins. The analysis is based on current modulations caused by the translation and rotation of single proteins through a uniform electric field inside of a nanopore. We applied this technique to nine proteins and show that the measured protein parameters agree well with reference values but only if the nanopore walls were coated with a nonstick fluid lipid bilayer.

Fluid surface coatings for solid-state nanopores: comparison of phospholipid bilayers and archaea-inspired lipid monolayers.

In the context of sensing and characterizing single proteins with synthetic nanopores, lipid bilayer coatings provide at least four benefits: first, they minimize unwanted protein adhesion to the pore walls by exposing a zwitterionic, fluid surface. Second, they can slow down protein translocation and rotation by the opportunity to tether proteins with a lipid anchor to the fluid bilayer coating. Third, they provide the possibility to impart analyte specificity by including lipid anchors with a specific receptor or ligand in the coating.

Formation of Single Nanopores with Diameters of 20-50 nm in Silicon Nitride Membranes Using Laser-Assisted Controlled Breakdown.

Nanopores with diameters from 20 to 50 nm in silicon nitride (SiN ) windows are useful for single-molecule studies of globular macromolecules. While controlled breakdown (CBD) is gaining popularity as a method for fabricating nanopores with reproducible size control and broad accessibility, attempts to fabricate large nanopores with diameters exceeding ∼20 nm via breakdown often result in undesirable formation of multiple nanopores in SiN membranes. To reduce the probability of producing multiple pores, we combined two strategies: laser-assisted breakdown and controlled pore enlargement by limiting the applied voltage.

Hyperspectral imaging using the single-pixel Fourier transform technique.

Hyperspectral imaging technology is playing an increasingly important role in the fields of food analysis, medicine and biotechnology. To improve the speed of operation and increase the light throughput in a compact equipment structure, a Fourier transform hyperspectral imaging system based on a single-pixel technique is proposed in this study. Compared with current imaging spectrometry approaches, the proposed system has a wider spectral range (400-1100 nm), a better spectral resolution (1 nm) and requires fewer measurement data (a sample rate of 6.

Precise fabrication of a 5 nm graphene nanopore with a helium ion microscope for biomolecule detection.

We report a scalable method to fabricate high-quality graphene nanopores for biomolecule detection using a helium ion microscope (HIM). HIM milling shows promising capabilities for precisely controlling the size and shape, and may allow for the potential production of nanopores at wafer scale. Nanopores could be fabricated at different sizes ranging from 5 to 30 nm in diameter in few minutes.

Monitoring tetracycline through a solid-state nanopore sensor.

Antibiotics as emerging environmental contaminants, are widely used in both human and veterinary medicines. A solid-state nanopore sensing method is reported in this article to detect Tetracycline, which is based on Tet-off and Tet-on systems. rtTA (reverse tetracycline-controlled trans-activator) and TRE (Tetracycline Responsive Element) could bind each other under the action of Tetracycline to form one complex.

Ultra-strong enhancement of electromagnetic fields in an L-shaped plasmonic nanocavity.

Enhancements up to four orders of magnitude for electric intensity and three orders of magnitude for magnetic intensity are realized in a novel 2D L-shaped nanocavity. This structure makes full use of the dimension confinement, cavity resonance and tip enhancement to increase the electromagnetic intensity. An impedance matching model is developed to design this cavity by regarding the cavity as a load impedance where electromagnetic fields are maximally enhanced when maximum electromagnetic energy is delivered to the load impedance.