Tailoring Light-Matter Interactions in Overcoupled Resonator for Biomolecule Recognition and Detection.

Plasmonic nanoantennas provide unique opportunities for precise control of light-matter coupling in surface-enhanced infrared absorption (SEIRA) spectroscopy, but most of the resonant systems realized so far suffer from the obstacles of low sensitivity, narrow bandwidth, and asymmetric Fano resonance perturbations. Here, we demonstrated an overcoupled resonator with a high plasmon-molecule coupling coefficient (µ) (OC-Hµ resonator) by precisely controlling the radiation loss channel, the resonator-oscillator coupling channel, and the frequency detuning channel. We observed a strong dependence of the sensing performance on the coupling state, and demonstrated that OC-Hµ resonator has excellent sensing properties of ultra-sensitive (7.25% nm-1), ultra-broadband (3-10 µm), and immune asymmetric Fano lineshapes. These characteristics represent a breakthrough in SEIRA technology and lay the foundation for specific recognition of biomolecules, trace detection, and protein secondary structure analysis using a single array (array size is 100 × 100 µm2). In addition, with the assistance of machine learning, mixture classification, concentration prediction and spectral reconstruction were achieved with the highest accuracy of 100%. Finally, we demonstrated the potential of OC-Hµ resonator for SARS-CoV-2 detection. These findings will promote the wider application of SEIRA technology, while providing new ideas for other enhanced spectroscopy technologies, quantum photonics and studying light-matter interactions.

Infrared routing and switching with tunable spectral bandwidth using arrays of metallic nanoantennas.

We study infrared routing and switching with tunable spectral bandwidth using in-plane scattering of light by flat Au nanoantenna arrays. The base dimensions of these nanoantennas are approximately 250 by 850 nm, while their heights vary from 20 to 150 nm. Our results show that, with the increase in height, the arrays become more efficient scatterers while their spectra broaden within the 1-1.6µm range. Our findings demonstrate that such processes strongly depend on the incident light polarization. For a given polarization, the incident light is efficiently scattered in only two opposite directions along the plane of the arrays, with insignificant transmission. Switching such a polarization by 90∘, however, suppresses this process, allowing the light to mostly pass through the arrays with minimal scattering. These unique characteristics suggest a tunable beam splitter application in the 1-1.6µm range and even longer wavelengths.

Focusing Surface Acoustic Waves with a Plasmonic Hypersonic Lens.

Plasmonic nanoantennas have proven to be efficient transducers of electromagnetic to mechanical energy and vice versa. The sudden thermal expansion of these structures after an ultrafast optical pulsed excitation leads to the emission of hypersonic acoustic waves to the supporting substrate, which can be detected by another antenna that acts as a high-sensitivity mechanical probe due to the strong modulation of its optical response. Here, we propose and experimentally demonstrate a nanoscale acoustic lens comprised of 11 gold nanodisks whose collective oscillation at gigahertz frequencies gives rise to an interference pattern that results in a diffraction-limited surface acoustic beam of about 340 nm width, with an amplitude contrast of 60%. Via spatially decoupled pump-probe experiments, we were able to map the radiated acoustic energy in the proximity of the focal area, obtaining a very good agreement with the continuum elastic theory.

Uncooled High Detectivity Mid-Infrared Photoconductor Using HgTe Quantum Dots and Nanoantennas.

Using a metal/insulator/metal (MIM) structure with a gold nanoantenna array made by electron beam lithography, the responsivity of a HgTe colloidal quantum dot film is enhanced in the mid-infrared. Simulations indicate that the spatially averaged peak spectral absorption of an 80 nm film is 60%, enhanced 23-fold compared to that of the same film on a bare sapphire substrate. The field intensity enhancement is focused near the antenna tips, being 20-fold 100 nm away, which represents only 1% of the total area and up to 1000-fold at the tips. The simulated polarized absorption spectra are in good agreement with the experiments, with a strong resonance around 4 µm. A responsivity of 0.6 A/W is obtained at a 1 V bias. Noise measurements separate the 1/f noise from the generation-recombination white noise and give a spatially averaged photoconductive gain of 0.3 at 1 V bias. The spatially averaged peak detectivity is improved 15-fold compared to the same film on a sapphire substrate without an MIM structure. The experimental peak detectivity reaches 9 × 109 Jones at 2650 cm-1 and 80 kHz, decreasing at lower frequencies. The MIM structure also enhances the spatially averaged peak photoluminescence of the CQD film by 16-fold, which is a potential Purcell enhancement. The good agreement between simulations and measurements confirms the viability of lithographically designed nanoantenna structures for vastly improving the performance of mid-IR colloidal quantum dot photoconductors. Further improvements will be possible by matching the optically enhanced and current collection areas.

Advances and Applications of Metal-Organic Frameworks (MOFs) in Emerging Technologies: A Comprehensive Review.

Metal-organic frameworks (MOFs) that are the wonder material of the 21st century consist of metal ions/clusters coordinated to organic ligands to form one- or more-dimensional porous structures with unprecedented chemical and structural tunability, exceptional thermal stability, ultrahigh porosity, and a large surface area, making them an ideal candidate for numerous potential applications. In this work, the recent progress in the design and synthetic approaches of MOFs and explore their potential applications in the fields of gas storage and separation, catalysis, magnetism, drug delivery, chemical/biosensing, supercapacitors, rechargeable batteries and self-powered wearable sensors based on piezoelectric and triboelectric nanogenerators are summarized. Lastly, this work identifies present challenges and outlines future opportunities in this field, which can provide valuable references.

Tuneable Anisotropic Plasmonics with Shape-Symmetric Conducting Polymer Nanoantennas.

A wide range of nanophotonic applications rely on polarization-dependent plasmonic resonances, which usually requires metallic nanostructures that have anisotropic shape. This work demonstrates polarization-dependent plasmonic resonances instead by breaking symmetry via material permittivity. The study shows that molecular alignment of a conducting polymer can lead to a material with polarization-dependent plasma frequency and corresponding in-plane hyperbolic permittivity region. This result is not expected based only on anisotropic charge mobility but implies that also the effective mass of the charge carriers becomes anisotropic upon polymer alignment. This unique feature is used to demonstrate circularly symmetric nanoantennas that provide different plasmonic resonances parallel and perpendicular to the alignment direction. The nanoantennas are further tuneable via the redox state of the polymer. Importantly, polymer alignment could blueshift the plasma wavelength and resonances by several hundreds of nanometers, forming a novel approach toward reaching the ultimate goal of redox-tunable conducting polymer nanoantennas for visible light.

Multimode hybrid gold-silicon nanoantennas for tailored nanoscale optical confinement.

High-index dielectric nanoantennas, which provide an interplay between electric and magnetic modes, have been widely used as building blocks for a variety of devices and metasurfaces, both in linear and nonlinear regimes. Here, we investigate hybrid metal-semiconductor nanoantennas, consisting of a multimode silicon nanopillar core coated with a gold layer, that offer an enhanced degree of control over the mode selection and confinement, and emission of light on the nanoscale exploiting high-order electric and magnetic resonances. Cathodoluminescence spectra revealed a multitude of resonant modes supported by the nanoantennas due to hybridization of the Mie resonances of the core and the plasmonic resonances of the shell. Eigenmode analysis revealed the modes that exhibit enhanced field localization at the gold interface, together with high confinement within the nanopillar volume. Consequently, this architecture provides a flexible means of engineering nanoscale components with tailored optical modes and field confinement for a plethora of applications, including sensing, hot-electron photodetection and nanophotonics with cylindrical vector beams.

Spin-polarization control of in-plane scattering in arrays of asymmetric U-shaped nanoantennas.

We study projection-enabled enhancement of asymmetric optical responses of plasmonic metasurfaces for photon-spin control of their far field scattering. Such a process occurs by detecting the light scattered by arrays of asymmetric U-shaped nanoantennas along their planes (in-plane scattering). The nanoantennas are considered to have relatively long bases and two unequal arms. Therefore, as their view angles along the planes of the arrays are changed, they offer an extensive range of shape and size projections, providing a wide control over the contributions of plasmonic near fields and multipolar resonances to the far field scattering of the arrays. We show that this increases the degree of the asymmetric spin-polarization responses of the arrays to circularly polarized light, offering a large amount of chirality. In particular, our results show the in-plane scattering of such metasurfaces can support opposite handedness, offering the possibility of photon spin-dependent directional control of energy routing.

Boosting Plant Photosynthesis with Carbon Dots: A Critical Review of Performance and Prospects.

Artificially augmented photosynthesis in nano-bionic plants requires tunable nano-antenna structures with physiochemical and optoelectronic properties, as well as unique light conversion capabilities. The use of nanomaterials to promote light capture across photosystems, primarily by carbon dots, has shown promising results in enhancing photosynthesis through tunable uptake, translocation, and biocompatibility. Carbon dots possess the ability to perform both down and up-light conversions, making them effective light promoters for harnessing solar energy beyond visible light wavelengths.This review presents and discusses the recent progress in fabrication, chemistry, and morphology, as well as other properties such as photoluminescence and energy conversion efficiency of nano-antennas based on carbon dots. The performance of artificially boosted photosynthesis is discussed and then correlated with the conversion properties of carbon dots and how they are applied to plant models. The challenges related to the nanomaterial delivery and the performance evaluation practices in modified photosystems, consideration of the reliability of this approach, and the potential avenues for performance improvements through other types of nano-antennas based on alternative nanomaterials are also critically evaluated. It is anticipated that this review will stimulate more high-quality research in plant nano-bionics and provide avenues to enhance photosynthesis for future agricultural applications.

Next-Generation Reconfigurable Nanoantennas and Polarization of Light.

This study is aimed at the design, calibration, and development of a near-infrared (NIR) liquid crystal multifunctional automated optical polarimeter, which is aimed at the study and characterization of the polarimetric properties of polymer optical nanofilms. The characterization of these novel nanophotonic structures has been achieved, in terms of Mueller matrix and Stokes parameter analyses. The nanophotonic structures of this study consisted of (a) a matrix consisting of two different polymer domains, namely polybutadiene (PB) and polystyrene (PS), functionalized with gold nanoparticles; (b) cast and annealed Poly (styrene-b-methyl methacrylate) (PS-PMMA) diblock copolymers; (c) a matrix of a block copolymer (BCP) domain, PS-b-PMMA or Poly (styrene-block-methy methacrylate), functionalized with gold nanoparticles; and (d) different thicknesses of PS-b-P2VP diblock copolymer functionalized with gold nanoparticles. In all cases, backscattered infrared light was studied and related to the polarization figures-of-merit (FOM). The outcome of this study indicates that functionalized polymer nanomaterials, depending upon their structure and composition, exhibit promising optical characteristics, modulating and manipulating the polarimetric properties of light. The fabrication of technologically useful, tunable, conjugated polymer blends with an optimized refractive index, shape, size, spatial orientation, and arrangement would lead to the development of new nanoantennas and metasurfaces.

Construction of Hollow Carbon Nanofibers with Graphene Nanorods as Nano-Antennas for Lower-Frequency Microwave Absorption.

Electromagnetic (EM) wave absorbers at a lower-frequency region (2-8 GHz) require higher attenuation ability to achieve efficient absorption. However, the impedance match condition and attenuation ability are usually inversely related. Herein, one-dimensional hollow carbon nanofibers with graphene nanorods are prepared based on coaxial electrospinning technology. The morphology of graphene nanorods can be controlled by the annealing process. As the annealing time increased from 2 to 8 h, graphene nanospheres grew into graphene nanorods, which were catalyzed by Co catalysts derived from ZIF-67 nanoparticles. These nanorods can play the role of nano-antennas, which can guide EM waves into materials to enhance impedance match conditions. As a result, the carbon nanofibers with graphene nanorods possess a larger impedance match area with higher attenuation ability. The minimum reflection loss reaches -57.1 dB at a thickness of 4.6 mm, and the effective absorption bandwidth can cover almost both the S and C bands (2.4-8 GHz). This work contributes a meaningful perspective into the modulation of microwave absorption performance in the lower-frequency range.

Spatially Resolved Nonlinear Plasmonics.

Nonlinear optical plasmonics investigates the emission of plasmonic nanoantennas with the aid of nonlinear spectroscopy. Here we introduce nonlinear spatially resolved spectroscopy (NSRS) which is capable of imaging the k-space as well as spatially resolving the THG signal of gold nanoantennas and investigating the emission of individual antennas by wide-field illumination of entire arrays. Hand in hand with theoretical simulations, we demonstrate our ability of imaging various oscillation modes inside the nanostructures and therefore spatial emission hotspots. Upon increasing intensity of the femtosecond excitation, an individual destruction threshold can be observed. We find certain antennas becoming exceptionally bright. By investigating those samples taking structural SEM images of the nanoantenna arrays afterward, our spatially resolved nonlinear image can be correlated with this data proving that antennas had deformed into a peanut-like shape. Thus, our NSRS setup enables the investigation of a nonlinear self-enhancement process of nanoantennas under critical laser excitation.

Ultrasensitive Molecular Fingerprint Retrieval Using Strongly Detuned Overcoupled Plasmonic Nanoantennas.

Tailoring light-matter interactions via plasmonic nanoantennas (PNAs) has emerged as a breakthrough technology for spectroscopic applications. The detuning between molecular vibrations and plasmonic resonances, as a fundamental and inevitable optical phenomenon in light-matter interactions, reduces the interaction efficiency, resulting in a weak molecule sensing signal at the strong detuning state. Here, it is demonstrated that the low interaction efficiency from detuning can be tackled by overcoupled PNAs (OC-PNAs) with a high ratio of the radiative to intrinsic loss rates, which can be used for ultrasensitive spectroscopy at strong plasmonic-molecular detuning. In OC-PNAs, the ultrasensitive molecule signals are achieved within a wavelength detuning range of 248 cm-1 , which is 173 cm-1 wider than previous works. Meanwhile, the OC-PNAs are immune to the distortion of molecular signals and maintain a lineshape consistent with the molecular signature fingerprint. This strategy allows a single device to enhance and capture the full and complex fingerprint vibrations in the mid-infrared range. In the proof-of-concept demonstration, 13 kinds of molecules with some vibration fingerprints strongly detuning by the OC-PNAs are identified with 100% accuracy with the assistance of machine-learning algorithms. This work gains new insights into detuning-state nanophotonics for potential applications including spectroscopy and sensors.

One-Shot Laser-Pulse Modification of Bare and Silica-Coated Gold Nanoparticles of Various Morphologies.

Gold nanoparticles are widely used in laser biomedical applications due to their favorable properties, mainly localized plasmon resonance. However, laser radiation can cause a change in the shape and size of plasmonic nanoparticles, thus resulting in an unwanted reduction of their photothermal and photodynamic efficiency due to a drastic alteration of optical properties. Most previously reported experiments were carried out with bulk colloids where different particles were irradiated by different numbers of laser pulses, thus making it difficult to accurately evaluate the laser power photomodification (PM) threshold. Here, we examine the one-shot nanosecond laser-pulse PM of bare and silica-coated gold nanoparticles moving in a capillary flow. Four types of gold nanoparticles, including nanostars, nanoantennas, nanorods, and SiO2@Au nanoshells, were fabricated for PM experiments. To evaluate the changes in the particle morphology under laser irradiation, we combine measurements of extinction spectra with electron microscopy. A quantitative spectral approach is developed to characterize the laser power PM threshold in terms of normalized extinction parameters. The experimentally determined PM threshold increases in series were as follows: nanorods, nanoantennas, nanoshells, and nanostars. An important observation is that even a thin silica shell significantly increases the photostability of gold nanorods. The developed methods and reported findings can be useful for the optimal design of plasmonic particles and laser irradiation parameters in various biomedical applications of functionalized hybrid nanostructures.

Hybrid Plasmonic Nanostructures for Enhanced Single-Molecule Detection Sensitivity.

Biosensing applications based on fluorescence detection often require single-molecule sensitivity in the presence of strong background signals. Plasmonic nanoantennas are particularly suitable for these tasks, as they can confine and enhance light in volumes far below the diffraction limit. The recently introduced antenna-in-box (AiB) platforms achieved high single-molecule detection sensitivity at high fluorophore concentrations by placing gold nanoantennas in a gold aperture. However, hybrid AiB platforms with alternative aperture materials such as aluminum promise superior performance by providing better background screening. Here, we report on the fabrication and optical characterization of hybrid AiBs made of gold and aluminum for enhanced single-molecule detection sensitivity. We computationally optimize the optical properties of AiBs by controlling their geometry and materials and find that hybrid nanostructures not only improve signal-to-background ratios but also provide additional excitation intensity and fluorescence enhancements. We further establish a two-step electron beam lithography process to fabricate hybrid material AiB arrays with high reproducibility and experimentally validate the higher excitation and emission enhancements of the hybrid nanostructures as compared to their gold counterpart. We foresee that biosensors based on hybrid AiBs will provide improved sensitivity beyond the capabilities of current nanophotonic sensors for a plethora of biosensing applications ranging from multicolor fluorescence detection to label-free vibrational spectroscopy.

Universal Narrowband Wavefront Shaping with High Quality Factor Meta-Reflect-Arrays.

Optical metasurfaces offer unprecedented flexibility in light wave manipulation but suffer weak resonant enhancement. Tackling this problem, we experimentally unveil a new phase gradient metasurface platform made entirely from individually addressable high quality factor (high-Q) silicon meta-atoms. Composed of pairs of nearly identical nanoblocks, these meta-atoms support dipolar-guided-mode resonances that, due to the controlled suppression of radiation loss, serve as highly sensitive phase pixels when placed above a mirror. A key novelty of this platform lies in the vanishingly small structural perturbations needed to produce universal phase fronts. Having fabricated elements with Q-factor ∼380 and spaced by λ/1.2, we achieve strong beam steering, up to 59% efficient, to angles 32.3°, 25.3°, and 20.9°, with variations in nanoantenna volume fractions across the metasurfaces of ≤2.6%, instead of >50% required by traditional versions. Aside from extreme sensitivity, the metasurfaces exhibit near-field intensity enhancement over 1000×. Taken together, these properties represent an exciting prospect for dynamic and nonlinear wave shaping.

Nanostructures for Solar Energy Harvesting.

Renewable energy sources are becoming more and more essential to energy production as societies evolve toward a fossil-fuel-free world. Solar energy is one of the most abundant sources of green energy. Nanoantennas can be used to improve and enhance the absorption of light into a photovoltaic cell in order to generate more current. In this study, different nanoantenna structures are analysed in tandem with a silicon solar cell in an effort to improve its output. The nanoantennas studied are metallic aperture nanoantennas made up of either silver, aluminium, gold or copper. The three geometries compared are rectangular, circular and triangular. The maximum field enhancement obtained is for an aluminium rectangular nanoantenna of 50 nm thickness. Despite this, the geometry with more improvements compared with a basic silicon cell was the circle geometry with a 100 nm radius.

Magnetoplasmonic Nanoantennas for On-Chip Reconfigurable Optical Wireless Communications.

On-chip wireless communications require optical nanoantennas with dynamically tunable radiation patterns, which may allow for higher integration with multiple nanoantennas instead of two fixed nanoantennas in existing approaches. In this paper, we introduce a concept to enable active manipulation of radiated beam steering using applied magnetic fields. The proposed system consists of a highly directive Yagi-Uda-like arrangement of magnetoplasmonic nanoribs made of Co6Ag94 and immersed in SiO2. Numerical demonstration of the tilting of the radiated beam from the nanoantenna on its plane is provided with full-wave electromagnetic simulations using the finite element method. The tilt direction of the radiated beam can be changed by reversing the magnetization direction, while the conventional plasmonic nanoantenna pattern is recovered by demagnetizing the system. The geometry of the nanoantenna can be tailored to work at optical or infrared wavelengths, but a proof of concept for λ = 700 nm is conducted for taking advantage of the high magneto-optical activity of Co6Ag94. The design was based on experimental data for materials that can be fabricated via nanolithography, thus permitting magnetically on-chip reconfigurable optical wireless communications.

Nonlinear Optical Signal Generation Mediated by a Plasmonic Azimuthally Chirped Grating.

Plasmonic gratings are simple and effective platforms for nonlinear signal generation since they provide a well-defined momentum for photon-plasmon coupling and local hot spots for frequency conversion. Here, a plasmonic azimuthally chirped grating (ACG), which provides spatially resolved broadband momentum for photon-plasmon coupling, was exploited to investigate the plasmonic enhancement effect in two nonlinear optical processes, namely two-photon photoluminescence (TPPL) and second harmonic generation (SHG). The spatial distributions of the nonlinear signals were determined experimentally by hyperspectral mapping with ultrashort pulsed excitation. The experimental spatial distributions of nonlinear signals agree very well with the analytical prediction based on photon-plasmon coupling with the momentum of the ACG, revealing the "antenna" function of the grating in plasmonic nonlinear signal generation. This work highlights the importance of the antenna effect of the gratings for nonlinear signal generation and provides insight into the enhancement mechanism of plasmonic gratings in addition to local hot spot engineering.

Bio-Inspired Nanomembranes as Building Blocks for Nanophotonics, Plasmonics and Metamaterials.

Nanomembranes are the most widespread building block of life, as they encompass cell and organelle walls. Their synthetic counterparts can be described as freestanding or free-floating structures thinner than 100 nm, down to monatomic/monomolecular thickness and with giant lateral aspect ratios. The structural confinement to quasi-2D sheets causes a multitude of unexpected and often counterintuitive properties. This has resulted in synthetic nanomembranes transiting from a mere scientific curiosity to a position where novel applications are emerging at an ever-accelerating pace. Among wide fields where their use has proven itself most fruitful are nano-optics and nanophotonics. However, the authors are unaware of a review covering the nanomembrane use in these important fields. Here, we present an attempt to survey the state of the art of nanomembranes in nanophotonics, including photonic crystals, plasmonics, metasurfaces, and nanoantennas, with an accent on some advancements that appeared within the last few years. Unlimited by the Nature toolbox, we can utilize a practically infinite number of available materials and methods and reach numerous properties not met in biological membranes. Thus, nanomembranes in nano-optics can be described as real metastructures, exceeding the known materials and opening pathways to a wide variety of novel functionalities.