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Surface-enhanced infrared absorption spectroscopy (SEIRA) has emerged as a powerful technique for ultrasensitive chemical-specific analysis. SEIRA can be realized by employing metasurfaces that can enhance light-matter interactions in the spectral bands of molecular vibrations. Increasing sample complexity emphasizes the need for metasurfaces that can operate simultaneously at different spectral bands, both accessing rich spectral information over a broad band, and resolving subtle differences in the absorption fingerprints through narrow-band resonances. Here, a novel concept of resonance-gradient metasurfaces is introduced, where the required spectral selectivity is achieved via local high-quality-factor (high-Q) resonances, while the continuous coverage of a broad band is enabled by the gradual adjustment of the unit-cell dimensions along the planar structure. The highly tailorable design of the gradient metasurfaces provides flexibility for shaping the spectral sampling density to match the relevant bands of target analytes while keeping a compact device footprint. The versatility of the gradient metasurfaces is demonstrated through several sensing scenarios, including polymer mixture deconvolution, detecting a multistep bioassay, and identification of the onset of vibrational strong coupling regime. The proposed gradient-resonance platform significantly contributes to the rapidly evolving landscape of nonlocal metasurfaces, enabling applications in molecular detection and analysis of fundamental light-matter interaction phenomena., (© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH.)

We hereby propose and theoretically investigate a new scheme for simultaneous generation and manipulation of terahertz (THz) waves through difference frequency generation facilitated by a metasurface-assisted nonlinear leaky waveguide antenna. The proposed structure integrates a nonlinear optical waveguide, composed of multiple Al x Ga 1-x As layers, with a THz leaky waveguide, wherein a bianisotropic metasurface realizes the radiating aperture. By explicitly utilizing the electric, magnetic, and magnetoelectric coupling responses of the metasurface, we demonstrate that the generated THz wave can be induced as a tightly confined, phase-matched guided mode for efficient generation of the THz wave. Additionally, this approach allows the THz wave to be transformed into a directive beam, radiating at a user-defined leakage rate and direction. Our numerical analyses suggest that THz beams ranging from 2.85 THz to 3.05 THz can be steered from 4 ∘ to 40 ∘ , utilizing the inherent beam-steering capabilities of the leaky-waveguide antenna. Within this THz frequency spectrum, the phase matching condition is achieved by adjusting the optical wavelengths between 1.6μm and 1.52μm. In particular, the nonlinear conversion efficiency is 2.9 × 10 -5 [1/W] at 3 THz.

This study investigated the influence of gas-injected nanobubbles on the morphology of particles during spray drying under various experimental conditions. The nanoparticle tracking system was used to measure the generation, size, and concentration of nanobubbles. Experiments were conducted at different temperatures (160°C-260°C) and feed rates (0.2-0.26 g/s) to examine the effect of nanobubbles on spray drying and present diverse results. The deionized (DI) water with generated nanobubbles had a particle concentration of 1.8 × 10 8 particles/mL and a mean particle size of 242.6 nm, which was ∼3.31 × 10 7 particles/mL higher untreated DI water. The maltodextrin solution containing nanobubbles also showed a significant increase in particle generation, with a concentration of 1.62 × 10 9 particles/mL. The viscosity of the maltodextrin solution containing nanobubbles decreased by ∼18%, from 9.3 mPa·s to 7.5 mPa·s. Overall, the size of the generated particles was similar regardless of nanobubble treatment, but there was a tendency for particle size to increase under specific temperature (260°C) and feed flow rate (0.32 g/s) conditions. Furthermore, it was observed that the Hausner ratio significantly varied with increasing temperature and feed flow rate, and these results were explained through scanning electron microscopy images. These findings confirm that the gas nanobubbles mixed in the feed can exert diverse effects on the spray drying system and powder characteristics depending on the operating conditions. This study suggests that nanobubbles can contribute to a more efficient process in spray drying and can influence the morphological characteristics of particles depending on the spray drying conditions., (The Authors. Published by Elsevier Inc. and Fass Inc. on behalf of the American Dairy Science Association®. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).)

Anisotropic planar polaritons - hybrid electromagnetic modes mediated by phonons, plasmons, or excitons - in biaxial two-dimensional (2D) van der Waals crystals have attracted significant attention due to their fundamental physics and potential nanophotonic applications. In this Perspective, we review the properties of planar hyperbolic polaritons and the variety of methods that can be used to experimentally tune them. We argue that such natural, planar hyperbolic media should be fairly common in biaxial and uniaxial 2D and 1D van der Waals crystals, and identify the untapped opportunities they could enable for functional (i.e. ferromagnetic, ferroelectric, and piezoelectric) polaritons. Lastly, we provide our perspectives on the technological applications of such planar hyperbolic polaritons., (© 2024. The Author(s).)

Transition metal dichalcogenide (TMD) layered semiconductors possess immense potential in the design of photonic, electronic, optoelectronic, and sensor devices. However, the sub-bandgap light absorption of TMD in the range from near-infrared (NIR) to short-wavelength infrared (SWIR) is insufficient for applications beyond the bandgap limit. Herein, we report that the sub-bandgap photoresponse of MoS 2 /Au heterostructures can be robustly modulated by the electrode fabrication method employed. We observed up to 60% sub-bandgap absorption in the MoS 2 /Au heterostructure, which includes the hybridized interface, where the Au layer was applied via sputter deposition. The greatly enhanced absorption of sub-bandgap light is due to the planar cavity formed by MoS 2 and Au; as such, the absorption spectrum can be tuned by altering the thickness of the MoS 2 layer. Photocurrent in the SWIR wavelength range increases due to increased absorption, which means that broad wavelength detection from visible toward SWIR is possible. We also achieved rapid photoresponse (~150 µs) and high responsivity (17 mA W -1 ) at an excitation wavelength of 1550 nm. Our findings demonstrate a facile method for optical property modulation using metal electrode engineering and for realizing SWIR photodetection in wide-bandgap 2D materials., (© 2023. The Author(s).)

Background: A motor unit (MU) is formed by a single alpha motor neuron (MN) and the muscle fibers it innervates. The MU is essential for all voluntary movements. Functional deficits in the MU result in neuromuscular disorders (NMDs). The pathological mechanisms underlying most NMDs remain poorly understood, in part due to the lack of in vitro models that can comprehensively recapitulate multistage intercellular interactions and physiological function of the MU., Results: We have designed a novel three-dimensional (3D) bilayer hydrogel tri-culture system where architecturally organized MUs can form in vitro. A sequential co-culture procedure using the three cell types of a MU, MN, myoblast, and Schwann cell was designed to construct a co-differentiating tri-culture on a bilayer hydrogel matrix. We utilized a µ-molded hydrogel with an additional Matrigel layer to form the bilayer hydrogel device. The µ-molded hydrogel layer provides the topological cues for myoblast differentiation. The Matrigel layer, with embedded Schwann cells, not only separates the MNs from myoblasts but also provides a proper micro-environment for MU development. The completed model shows key MU features including an organized MU structure, myelinated nerves, aligned myotubes innervated on clustered neuromuscular junctions (NMJs), MN-driven myotube contractions, and increases in cytosolic Ca 2+ upon stimulation., Conclusions: This organized and functional in vitro MU model provides an opportunity to study pathological events involved in NMDs and peripheral neuropathies, and can serve as a platform for physiological and pharmacological studies such as modeling and drug screening. Technically, the rational of this 3D bilayer hydrogel co-culture system exploits multiple distinct properties of hydrogels, facilitating effective and efficient co-culturing of diverse cell types for tissue engineering., (© 2023. Society of Chinese Bioscientists in America (SCBA).)

Infrared spectroscopy provides unique information on the composition and dynamics of biochemical systems by resolving the characteristic absorption fingerprints of their constituent molecules. Based on this inherent chemical specificity and the capability for label-free, noninvasive, and real-time detection, infrared spectroscopy approaches have unlocked a plethora of breakthrough applications for fields ranging from environmental monitoring and defense to chemical analysis and medical diagnostics. Nanophotonics has played a crucial role for pushing the sensitivity limits of traditional far-field spectroscopy by using resonant nanostructures to focus the incident light into nanoscale hot-spots of the electromagnetic field, greatly enhancing light-matter interaction. Metasurfaces composed of regular arrangements of such resonators further increase the design space for tailoring this nanoscale light control both spectrally and spatially, which has established them as an invaluable toolkit for surface-enhanced spectroscopy. Starting from the fundamental concepts of metasurface-enhanced infrared spectroscopy, a broad palette of resonator geometries, materials, and arrangements for realizing highly sensitive metadevices is showcased, with a special focus on emerging systems such as phononic and 2D van der Waals materials, and integration with waveguides for lab-on-a-chip devices. Furthermore, advanced sensor functionalities of metasurface-based infrared spectroscopy, including multiresonance, tunability, dielectrophoresis, live cell sensing, and machine-learning-aided analysis are highlighted., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Misfolded proteins associated with various neurodegenerative diseases often accumulate in tissues or circulate in biological fluids years before the clinical onset, thus representing ideal diagnostic targets. Real-time quaking-induced conversion (RT-QuIC), a protein-based seeded-amplification assay, holds great potential for early disease detection, yet challenges remain for routine diagnostic application. Chronic Wasting Disease (CWD), associated with misfolded prion proteins of cervids, serves as an ideal model for evaluating new RT-QuIC methodologies. In this study, we investigate the previously untested hypothesis that incorporating nanoparticles into RT-QuIC assays can enhance their speed and sensitivity when applied to biological samples. We show that adding 50 nm silica nanoparticles to RT-QuIC experiments (termed Nano-QuIC) for CWD diagnostics greatly improves the performance by reducing detection times 2.5-fold and increasing sensitivity 10-fold by overcoming the effect of inhibitors in complex tissue samples. Crucially, no false positives were observed with these 50 nm silica nanoparticles, demonstrating the enhanced reliability and potential for diagnostic application of Nano-QuIC in detecting misfolded proteins.

Nearly all biosensing platforms can be described using two fundamental steps-collection and detection. Target analytes must be delivered to a sensing element, which can then relay the transduced signal. For point-of-care technologies, where operation is to be kept simple, typically the collection step is passive diffusion driven-which can be slow or limiting under low concentrations. This work demonstrates an integration of both active collection and detection by using resonant wireless power transfer coupled to a nanogap capacitor. Nanoparticles suspended in deionized water are actively trapped using wireless dielectrophoresis and positioned within the most sensitive fringe field regions for wireless impedance-based detection. Trapping of 40 nm particles and larger is demonstrated using a 3.5 V RMS , 1 MHz radiofrequency signal delivered over a distance greater than 8 cm from the nanogap capacitor. Wireless trapping and release of 1 µm polystyrene beads is simultaneously detected in real-time over a distance of 2.5 cm from the nanogap capacitor. Herein, geometric scaling strategies coupled with optimal circuit design is presented to motivate combined collection and detection biosensing platforms amenable to wireless and/or smartphone operation., (© 2023. The Author(s).)

Subwavelength terahertz (THz) imaging methods are highly desirable for biochemical sensing as well as materials sciences, yet sensitive spectral fingerprinting is still challenging in the frequency domain due to weak light-matter interactions. Here, we demonstrate subwavelength THz resonance imaging (STRING) that overcomes this limitation to achieve ultrasensitive molecular fingerprinting. STRING combines individual ring-shaped coaxial single resonators with near-field spectroscopy, yielding considerable sensitivity gains from both local field enhancement and the near-field effect. As an initial demonstration, we obtained spectral fingerprints from isomers of α-lactose and maltose monohydrates, achieving sensitivity that was enhanced by up to 10 orders of magnitude compared to far-field THz measurements with pelletized samples. Our results show that the STRING platform could enable the development of THz spectroscopy as a practical and sensitive tool for the fingerprinting and spectral imaging of molecules and nanoparticles.

Detection of terahertz (THz) radiation has many potential applications, but presently available detectors are limited in many aspects of their performance, including sensitivity, speed, bandwidth and operating temperature. Most do not allow the characterization of THz polarization states. Recent observation of THz-driven luminescence in quantum dots offers a possible detection mechanism via field-driven interdot charge transfer. We demonstrate a room-temperature complementary metal-oxide-semiconductor THz camera and polarimeter based on quantum-dot-enhanced THz-to-visible upconversion mechanism with optimized luminophore geometries and fabrication designs. Besides broadband and fast responses, the nanoslit-based sensor can detect THz pulses with peak fields as low as 10 kV cm -1 . A related coaxial nanoaperture-type device shows a to-date-unexplored capability to simultaneously record the THz polarization state and field strength with similar sensitivity., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

Cellular retinoic acid-binding protein 1 (CRABP1) binds retinoic acid (RA) specifically in the cytoplasm with unclear functions. CRABP1 is highly and specifically expressed in spinal motor neurons (MNs). Clinical and pre-clinical data reveal a potential link between CRABP1 and MN diseases, including the amyotrophic lateral sclerosis (ALS). We established a sequenced MN-muscle co-differentiation system to engineer an in vitro functional 3D NMJ model for molecular studies and demonstrated that CRABP1 in MNs contributes to NMJ formation and maintenance. Consistently, Crabp1 knockout (CKO) mice exhibited an adult-onset ALS-like phenotype with progressively deteriorated NMJs, characterized with behavioral, EchoMRI, electrophysiological, histological, and immunohistochemical studies at 2-20-months old. Mechanistically, CRABP1 suppresses CaMKII activation to regulate neural Agrn expression and downstream muscle LRP4-MuSK signaling, thereby maintaining NMJ. A proof-of-concept was provided by specific re-expression of CRABP1 to rescue Agrn expression and the phenotype. This study identifies CRABP1-CaMKII-Agrn signaling as a physiological pre-synaptic regulator in the NMJ. This study also highlights a potential protective role of CRABP1 in the progression of NMJ deficits in MN diseases., (© 2022. The Author(s), under exclusive licence to ADMC Associazione Differenziamento e Morte Cellulare.)

Diagnostic tools for the detection of protein-misfolding diseases (i.e., proteopathies) are limited. Gold nanoparticles (AuNPs) facilitate sensitive diagnostic techniques via visual color change for the identification of a variety of targets. In parallel, recently developed quaking-induced conversion (QuIC) assays leverage protein-amplification and fluorescent signaling for the accurate detection of misfolded proteins. Here, we combine AuNP and QuIC technologies for the visual detection of amplified misfolded prion proteins from tissues of wild white-tailed deer infected with chronic wasting disease (CWD), a prion disease of cervids. Our newly developed assay, MN-QuIC, enables both naked-eye and light-absorbance measurements for detection of misfolded prions. MN-QuIC leverages basic laboratory equipment that is cost-effective and portable, thus facilitating real-time prion diagnostics across a variety of settings. In addition to laboratory-based tests, we deployed to a rural field-station in southeastern Minnesota and tested for CWD on site. We successfully demonstrated that MN-QuIC is functional in a non-traditional laboratory setting by performing a blinded analysis in the field and correctly identifying all CWD positive and CWD not-detected deer at the field site in 24 h, thus documenting the portability of the assay. White-tailed deer tissues used to validate MN-QuIC included medial retropharyngeal lymph nodes, parotid lymph nodes, and palatine tonsils. Importantly, all of the white-tailed deer (n = 63) were independently tested using ELISA, IHC, and/or RT-QuIC technologies and results secured with MN-QuIC were 95.7% and 100% consistent with these tests for positive and non-detected animals, respectively. We hypothesize that electrostatic forces help govern the AuNP/prion interactions and conclude that MN-QuIC has great potential for sensitive, field-deployable diagnostics for CWD, with future potential diagnostic applications for a variety of proteopathies., (© 2022. The Author(s).)

The ability to control the light polarization state is critically important for diverse applications in information processing, telecommunications, and spectroscopy. Here, we propose that a stack of anisotropic van der Waals materials can facilitate the building of optical elements with Jones matrices of unitary, Hermitian, non-normal, singular, degenerate, and defective classes. We show that the twisted stack with electrostatic control can function as arbitrary-birefringent wave-plate or arbitrary polarizer with tunable degree of non-normality, which in turn give access to plethora of polarization transformers including rotators, pseudorotators, symmetric and ambidextrous polarizers. Moreover, we discuss an electrostatic-reconfigurable stack which can be tuned to operate as four different polarizers and be used for Stokes polarimetry.

Open-channel microfluidics enables precise positioning and confinement of liquid volume to interface with tightly integrated optics, sensors, and circuit elements. Active actuation via electric fields can offer a reduced footprint compared to passive microfluidic ensembles and removes the burden of intricate mechanical assembly of enclosed systems. Typical systems actuate via manipulating surface wettability (i.e., electrowetting), which can render low-voltage but forfeits open-microchannel confinement. The dielectric polarization force is an alternative which can generate open liquid microchannels (sub-100 µm) but requires large operating voltages (50-200 V RMS ) and low conductivity solutions. Here we show actuation of microchannels as narrow as 1 µm using voltages as low as 0.5 V RMS for both deionized water and physiological buffer. This was achieved using resonant, nanoscale focusing of radio frequency power and an electrode geometry designed to abate surface tension. We demonstrate practical fluidic applications including open mixing, lateral-flow protein labeling, filtration, and viral transport for infrared biosensing-known to suffer strong absorption losses from enclosed channel material and water. This tube-free system is coupled with resonant wireless power transfer to remove all obstructing hardware - ideal for high-numerical-aperture microscopy. Wireless, smartphone-driven fluidics is presented to fully showcase the practical application of this technology., (© 2022. The Author(s).)

Nanophotonic devices, which control light in subwavelength volumes and enhance light-matter interactions, have opened up exciting prospects for biosensing. Numerous nanophotonic biosensors have emerged to address the limitations of the current bioanalytical methods in terms of sensitivity, throughput, ease-of-use and miniaturization. In this Review, we provide an overview of the recent developments of label-free nanophotonic biosensors using evanescent-field-based sensing with plasmon resonances in metals and Mie resonances in dielectrics. We highlight the prospects of achieving an improved sensor performance and added functionalities by leveraging nanostructures and on-chip and optoelectronic integration, as well as microfluidics, biochemistry and data science toolkits. We also discuss open challenges in nanophotonic biosensing, such as reducing the overall cost and handling of complex biological samples, and provide an outlook for future opportunities to improve these technologies and thereby increase their impact in terms of improving health and safety., (© 2022. Springer Nature Limited.)

The front cover artwork is provided by Prof. Sang-Hyun Oh's group at the University of Minnesota. The image shows the optical trapping of chiral nanoparticles using coaxial nano-optical tweezers, devices capable of harnessing light to manipulate objects a few nanometers in size. Read the full text of the Review at 10.1002/cphc.202100004., (© 2021 Wiley-VCH GmbH.)

Optical tweezers were developed in 1970 by Arthur Ashkin as a tool for the manipulation of micron-sized particles. Ashkin's original design was then adapted for a variety of purposes, such as trapping and manipulation of biological materials [1] and the laser cooling of atoms. [2,3] More recent development has led to nano-optical tweezers, for trapping particles on the scale of only a few nanometers, and holographic tweezers, which allow for dynamic control of multiple traps in real-time. These alternatives to conventional optical tweezers have made it possible to trap single molecules and to perform a variety of studies on them. Presented here is a review of recent developments in nano-optical tweezers and their current and future applications., (© 2021 Wiley-VCH GmbH.)

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.

On-chip integration of plasmonics and electronics can benefit a broad range of applications in biosensing, signal processing, and optoelectronics. A key requirement is a chip-scale manufacturing method. Here, we demonstrate a split-trench resonator platform that combines a high-quality-factor resonant plasmonic biosensor with radio frequency (RF) nanogap tweezers. The split-trench resonator can simultaneously serve as a dielectrophoretic trap and a nanoplasmonic sensor. Trapping is accomplished by applying an RF electrical bias across a 10 nm gap, thereby either attracting or repelling analytes. Trapped analytes are detected in a label-free manner using refractive-index sensing, enabled by interference between surface-plasmon standing waves in the trench and light transmitted through the gap. This active sample concentration mechanism enables detection of nanoparticles and proteins at a concentration as low as 10 pM. We can manufacture centimeter-long split-trench cavity resonators with high throughput via photolithography and atomic layer deposition, toward practical applications in biosensing, spectroscopy, and optoelectronics.

Graphene is now a crucial component of many device designs in electronics and optics. Just like the noble metals, this single layer of carbon atoms in a honeycomb lattice can support surface plasmons, which are central to several sensing technologies in the mid-infrared regime. As with classical metal plasmons, periodic corrugations in the graphene sheet itself can be used to launch these surface waves; however, as graphene plasmons are tightly confined, the role of unwanted surface roughness, even at a nanometer scale, cannot be ignored. In this work, we revisit our previous numerical experiments on metal plasmons launched by vanishingly small grating structures, with the addition of graphene to the structure. These simulations are conducted with a recently devised, rapid, and robust high-order spectral scheme of the authors, and with it we carefully demonstrate how the plasmonic response of a perfectly flat sheet of graphene can be significantly altered with even a tiny corrugation (on the order of merely 5 nm). With these results, we demonstrate the primary importance of fabrication techniques that produce interfaces whose deviations from flat are on the order of angstroms.

Two-dimensional (2D) materials are promising candidates for building ultrashort-channel devices because their thickness can be reduced down to a single atomic layer. Here, we demonstrate an ultraflat nanogap platform based on atomic layer deposition (ALD) and utilize the structure to fabricate 2D material-based optical and electronic devices. In our method, ultraflat metal surfaces, template-stripped from a Si wafer mold, are separated by an Al 2 O 3 ALD layer down to a gap width of 10 nm. Surfaces of both electrodes are vertically aligned without a height difference, and each electrode is ultraflat with a measured root-mean-square roughness as low as 0.315 nm, smaller than the thickness of monolayer graphene. Simply by placing 2D material flakes on top of the platform, short-channel field-effect transistors based on black phosphorus and MoS 2 are fabricated, exhibiting their typical transistor characteristics. Furthermore, we use the same platform to demonstrate photodetectors with a nanoscale photosensitive channel, exhibiting higher photosensitivity compared to microscale gap channels. Our wafer-scale atomic layer lithography method can benefit a diverse range of 2D optical and electronic applications.

Although van der Waals-layered transition metal dichalcogenides from transient absorption spectroscopy have successfully demonstrated an ideal carrier multiplication (CM) performance with an onset of nearly 2E g , interpretation of the CM effect from the optical approach remains unresolved owing to the complexity of many-body electron-hole pairs. We demonstrate the escalated photocurrent with excitation photon energy by fabricating the dual-gate p-n junction of a MoTe 2 film on a transparent substrate. Electrons and holes were efficiently extracted by eliminating the Schottky barriers in the metal contact and minimizing multiple reflections. The photocurrent was elevated proportionately to the excitation photon energy. The boosted quantum efficiency confirms the multiple electron-hole pair generation of >2E g , consistent with CM results from an optical approach, pushing the solar cell efficiency beyond the Shockley-Queisser limit.

An acoustic plasmon mode in a graphene-dielectric-metal structure has recently been spotlighted as a superior platform for strong light-matter interaction. It originates from the coupling of graphene plasmon with its mirror image and exhibits the largest field confinement in the limit of a sub-nm-thick dielectric. Although recently detected in the far-field regime, optical near-fields of this mode are yet to be observed and characterized. Here, we demonstrate a direct optical probing of the plasmonic fields reflected by the edges of graphene via near-field scattering microscope, revealing a relatively small propagation loss of the mid-infrared acoustic plasmons in our devices that allows for their real-space mapping at ambient conditions even with unprotected, large-area graphene grown by chemical vapor deposition. We show an acoustic plasmon mode that is twice as confined and has 1.4 times higher figure of merit in terms of the normalized propagation length compared to the graphene surface plasmon under similar conditions. We also investigate the behavior of the acoustic graphene plasmons in a periodic array of gold nanoribbons. Our results highlight the promise of acoustic plasmons for graphene-based optoelectronics and sensing applications.

Plasmonic enhancement of nonlinear optical processes confront severe limitations arising from the strong dispersion of metal susceptibilities and small interaction volumes that hamper the realization of desirable phase-matching-like conditions. Maximizing nonlinear interactions in nanoscale systems require simultaneous excitation of resonant modes that spatially and constructively overlap at all wavelengths involved in the process. Here, we present a hybrid rectangular patch antenna design for optimal second-harmonic generation (SHG) that is characterized by a non-centrosymmetric dielectric/ferroelectric material at the plasmonic hot spot. The optimization of the rectangular patch allows for the independent tuning of various modes of resonances that can be used to enhance the SHG process. We explore the angular dependence of SHG in these hybrid structures and highlight conditions necessary for the maximal SHG efficiency. Furthermore, we propose a novel configuration with a periodically poled ferroelectric layer for an orders-of-magnitude enhanced SHG at normal incidence. Such a platform may enable the development of integrated nanoscale light sources and on-chip frequency converters., Competing Interests: The authors declare no competing financial interest., (© 2020 American Chemical Society.)

Polaritons in two-dimensional materials provide extreme light confinement that is difficult to achieve with metal plasmonics. However, such tight confinement inevitably increases optical losses through various damping channels. Here we demonstrate that hyperbolic phonon polaritons in hexagonal boron nitride can overcome this fundamental trade-off. Among two observed polariton modes, featuring a symmetric and antisymmetric charge distribution, the latter exhibits lower optical losses and tighter polariton confinement. Far-field excitation and detection of this high-momenta mode become possible with our resonator design that can boost the coupling efficiency via virtual polariton modes with image charges that we dub 'image polaritons'. Using these image polaritons, we experimentally observe a record-high effective index of up to 132 and quality factors as high as 501. Further, our phenomenological theory suggests an important role of hyperbolic surface scattering in the damping process of hyperbolic phonon polaritons.

With advances in nanofabrication techniques, extreme-scale nanophotonic devices with critical gap dimensions of just 1-2 nm have been realized. The plasmonic response in these extreme-scale gaps is significantly affected by nonlocal electrodynamics, quenching field enhancement and blue-shifting the resonance with respect to a purely local behavior. The extreme mismatch in lengthscales, ranging from millimeter-long wavelengths to atomic-scale charge distributions, poses a daunting computational challenge. In this paper, we perform computations of a single nanoslit using the hybridizable discontinuous Galerkin method to solve Maxwell's equations augmented with the hydrodynamic model for the conduction-band electrons in noble metals. This method enables the efficient simulation of the slit while accounting for the nonlocal interactions between electrons and the incident light. We study the impact of gap width, film thickness and electron motion model on the plasmon resonances of the slit for two different frequency regimes: (1) terahertz frequencies, which lead to 1000-fold field amplitude enhancements that saturate as the gap shrinks; and (2) the near- and mid-infrared regime, where we show that narrow gaps and thick films cluster Fabry-Pérot (FP) resonances towards lower frequencies, derive a dispersion relation for the first FP resonance, in addition to observing that nonlocality boosts transmittance and reduces enhancement.

Tuning the properties of optical metamaterials in real time is one of the grand challenges of photonics. Being able to do so will enable a class of adaptive photonic materials for use in applications such as surface enhanced Raman spectroscopy and reflectors/absorbers. One strategy to achieving this goal is based on the electrovariable self-assembly and disassembly of two-dimensional nanoparticle arrays at a metal | liquid interface. As expected, the structure results in plasmonic coupling between NPs in the array but perhaps as importantly between the array and the metal surface. In such a system, the density of the nanoparticle array can be reversibly controlled by the variation of electrode potential. Theory suggests that due to a collective plasmon-coupling effect  less than 1 V variation of electrode potential can give rise to a dramatic simultaneous change in optical reflectivity from ∼93% to ∼1% and the amplification of the SERS signal by up to 5 orders of magnitude. This is experimentally demonstrated using a platform based on the voltage-controlled assembly of 40 nm Au-nanoparticle arrays at a TiN/Ag electrode in contact with an aqueous electrolyte. We show that all the physics underpinning the behavior of this platform works precisely as suggested by the proposed theory, setting the electrochemical nanoplasmonics as a promising direction in photonics research.

Advances in mid-IR lasers, detectors, and nanofabrication technology have enabled new device architectures to implement on-chip sensing applications. In particular, direct integration of plasmonic resonators with a dielectric waveguide can generate an ultra-compact device architecture for biochemical sensing via surface-enhanced infrared absorption (SEIRA) spectroscopy. A theoretical investigation of such a hybrid architecture is imperative for its optimization. In this work, we investigate the coupling mechanism between a plasmonic resonator array and a waveguide using temporal coupled-mode theory and numerical simulation. The results conclude that the waveguide transmission extinction ratio reaches maxima when the resonator-waveguide coupling rate is maximal. Moreover, after introducing a model analyte in the form of an oscillator coupled with the plasmonics-waveguide system, the transmission curve with analyte absorption can be fitted successfully. We conclude that the extracted sensing signal can be maximized when analyte absorption frequency is the same as the transmission minima, which is different from the plasmonic resonance frequency. This conclusion is in contrast to the dielectric resonator scenario and provides an important guideline for design optimization and sensitivity improvement of future devices.

Refractometric sensors utilizing surface plasmon resonance (SPR) should satisfy a series of performance metrics, bulk sensitivity, thin-film sensitivity, refractive-index resolution, and high-Q-factor resonance, as well as practical requirements such as manufacturability and the ability to separate optical and fluidic paths via reflection-mode sensing. While many geometries such as nanohole, nanoslit, and nanoparticles have been employed, it is nontrivial to engineer nanostructures to satisfy all of the aforementioned requirements. We combine gold nanohole arrays with a water-index-matched Cytop film to demonstrate reflection-mode, high- Q -factor ( Q exp = 143) symmetric plasmonic sensor architecture. Using template stripping with a Cytop film, we can replicate a large number of index-symmetric nanohole arrays, which support sharp plasmonic resonances that can be probed by light reflected from their backside with a high extinction amplitude. The reflection geometry separates the optical and microfluidic paths without sacrificing sensor performance as is the case of standard (index-asymmetric) nanohole arrays. Furthermore, plasmon hybridization caused by the array refractive-index symmetry enables dual-mode detection that allows distinction of refractive-index changes occurring at different distances from the surface, making it possible to identify SPR response from differently sized particles or to distinguish binding events near the surface from bulk index changes. Due to the unique combination of a dual-mode reflection-configuration sensing, high-Q plasmonic modes, and template-stripping nanofabrication, this platform can extend the utility of nanohole SPR for sensing applications involving biomolecules, polymers, nanovesicles, and biomembranes.

With advances in nanofabrication techniques, extreme-scale nanophotonic devices with critical gap dimensions of just 1-2 nm have been realized. Plasmons in such ultranarrow gaps can exhibit nonlocal response, which was previously shown to limit the field enhancement and cause optical properties to deviate from the local description. Using atomic layer lithography, we create mid-infrared-resonant coaxial apertures with gap sizes as small as 1 nm and observe strong evidence of nonlocality, including spectral shifts and boosted transmittance of the cutoff epsilon-near-zero mode. Experiments are supported by full-wave 3-D nonlocal simulations performed with the hybridizable discontinuous Galerkin method. This numerical method captures atomic-scale variations of the electromagnetic fields while efficiently handling extreme-scale size mismatch. Combining atomic-layer-based fabrication techniques with fast and accurate numerical simulations provides practical routes to design and fabricate highly-efficient large-area mid-infrared sensors, antennas, and metasurfaces.

A label-free, non-dispruptive, and real-time analytical device to monitor the dynamic features of biomolecules and their interactions with neighboring molecules is an essential prerequisite for biochip- and diagonostic assays. To explore one of the central questions on the lipid-lipid interactions in the course of the liquid-ordered (l o ) domain formation, called rafts, we developed a method of reconstituting continuous but spatially heterogeneous lipid membrane platforms with molayer-bilayer juntions (MBJs) that enable to form the l o domains in a spatiotemporally controlled manner. This allows us to detect the time-lapse dynamics of the lipid-lipid interactions during raft formation and resultant membrane phase changes together with the raft-associated receptor-ligand binding through the surface plasmon resonance (SPR). For cross-validation, using epifluorescence microscopy, we demonstrated the underlying mechanisms for raft formations that the infiltration of cholesterols into the sphingolipid-enriched domains plays a crucial roles in the membrane phase-separation. Our membrane platform, being capable of monitoring dynamic interactions among lipids and performing the systematic optical analysis, will unveil physiological roles of cholesterols in a variety of biological events., (Copyright © 2019 Elsevier B.V. All rights reserved.)

We present the photonic printing that can display different color images depending on the optical polarization of incident light. The dynamic selection among different images becomes possible by using anisotropic Fabry-Perot resonators that incorporate a layer of liquid crystal molecules aligned by directional molecular registration (DMR) as polarization-dependent color pixels. Using the new device platform, we demonstrate a prototype of an anticounterfeiting label with inherent anti-replicability that results from the molecular-level origin of security images. In addition, this concept is extended to polarization-selective holography. Our molecular-level approach enables to develop a new class of security labels and holographic storage media.

One of the fundamental hurdles in plasmonics is the trade-off between electromagnetic field confinement and the coupling efficiency with free-space light, a consequence of the large momentum mismatch between the excitation source and plasmonic modes. Acoustic plasmons in graphene, in particular, have an extreme level of field confinement, as well as an extreme momentum mismatch. Here, we show that this fundamental compromise can be overcome and demonstrate a graphene acoustic plasmon resonator with nearly perfect absorption (94%) of incident mid-infrared light. This high efficiency is achieved by utilizing a two-stage coupling scheme: free-space light coupled to conventional graphene plasmons, which then couple to ultraconfined acoustic plasmons. To realize this scheme, we transfer unpatterned large-area graphene onto template-stripped ultraflat metal ribbons. A monolithically integrated optical spacer and a reflector further boost the enhancement. We show that graphene acoustic plasmons allow ultrasensitive measurements of absorption bands and surface phonon modes in ångström-thick protein and SiO 2 layers, respectively. Our acoustic plasmon resonator platform is scalable and can harness the ultimate level of light-matter interactions for potential applications including spectroscopy, sensing, metasurfaces and optoelectronics.

Much of the functionality of multicellular systems arises from the spatial organization and dynamic behaviours within and between cells. Current single-cell genomic methods only provide a transcriptional 'snapshot' of individual cells. The real-time analysis and perturbation of living cells would generate a step change in single-cell analysis. Here we describe minimally invasive nanotweezers that can be spatially controlled to extract samples from living cells with single-molecule precision. They consist of two closely spaced electrodes with gaps as small as 10-20 nm, which can be used for the dielectrophoretic trapping of DNA and proteins. Aside from trapping single molecules, we also extract nucleic acids for gene expression analysis from living cells without affecting their viability. Finally, we report on the trapping and extraction of a single mitochondrion. This work bridges the gap between single-molecule/organelle manipulation and cell biology and can ultimately enable a better understanding of living cells.

The integration of nanoplasmonic devices with a silicon photonic platform affords a new approach for efficient light delivery by combining the high field enhancement of plasmonics and the ultralow propagation loss of dielectric waveguides. Such a hybrid integration obviates the need for a bulky free-space optics setup and can lead to fully integrated, on-chip optical sensing systems. Here, we demonstrate ultracompact plasmonic resonators directly patterned atop a silicon waveguide for mid-infrared spectroscopic chemical sensing. The footprint of the plasmonic nanorod resonators is as small as 2 μm 2 , yet they can couple with the mid-infrared waveguide mode efficiently. The plasmonic resonance is directly measured through the transmission spectrum of the waveguide with a coupling efficiency greater than 70% and a field intensity enhancement factor of over 3600 relative to the evanescent waveguide field intensity. Using this hybrid device and a tunable mid-infrared laser source, surface-enhanced infrared absorption spectroscopy of both a thin poly(methyl methacrylate) film and an octadecanethiol monolayer is successfully demonstrated.

Nanoplasmonic structures can tightly confine light onto a material's surface to probe biomolecular interactions not easily accessed by other sensing techniques. New and exciting developments in nanofabrication processes, nano-optical trapping, graphene devices, mid-infrared spectroscopy, and metasurfaces will greatly empower the performance and functionalities of nanoplasmonic sensors.

rHIgM22 is a recombinant human monoclonal IgM designed to promote remyelination, and it is currently in Phase I clinical trials in patients with multiple sclerosis (MS). In animal models of demyelination, a single low dose of rHIgM22 stimulates oligodendrocyte maturation, induces remyelination, preserves axons, and slows the decline of locomotor deficits. Natural autoantibodies like rHIgM22 typically bind to multiple antigens with weak affinity. rHIgM22 binds to oligodendrocytes and myelin. Because the antigens for rHIgM22 is prevalent within and exclusive to central nervous system (CNS) myelin, we used CNS myelin particles in combination with surface plasmon resonance to determine the kinetic and affinity constants for the interaction of rHIgM22 to myelin. We found that both the serum and recombinant forms of the antibody bind to myelin with very small dissociation constants in the 100 pM range, which is highly unusual for natural autoantibodies. The extraordinary affinity between rHIgM22 and myelin may explain why such a low effective dose can stimulate CNS repair in animal models of demyelination and underlie the accumulation of rHIgM22 in the CSF in treated MS patients by targeting myelin.

A rapid, label-free, and broadly applicable chemical analysis platform for nanovesicles and subcellular components is highly desirable for diagnostic assays. We demonstrate an integrated nanogap plasmonic sensing platform that combines subvolt dielectrophoresis (DEP) trapping, gold nanoparticles (AuNPs), and a lineated illumination scheme for real-time, surface-enhanced Raman spectroscopy (SERS) imaging of biological nanoparticles. Our system is capable of isolating suspended sub-100 nm vesicles and imaging the Raman spectra of their cargo within seconds, 100 times faster than conventional point-scan Raman systems. Bare AuNPs are spiked into solution and simultaneously trapped with the nanovesicles along the gap to boost local optical fields. In addition, our platform offers simultaneous and delay-free spatial and temporal multiplexing functionality. These nanogap devices can be mass-produced via atomic layer lithography and provide a practical platform for high-speed SERS analysis of biological nanoparticles.

Waveguide-integrated plasmonics is a growing field with many innovative concepts and demonstrated devices in the visible and near-infrared. Here, we extend this body of work to the mid-infrared for the application of surface-enhanced infrared absorption (SEIRA), a spectroscopic method to probe molecular vibrations in small volumes and thin films. Built atop a silicon-on-insulator (SOI) waveguide platform, two key plasmonic structures useful for SEIRA are examined using computational modeling: gold nanorods and coaxial nanoapertures. We find resonance dips of 90% in near diffraction-limited areas due to arrays of our structures and up to 50% from a single resonator. Each of the structures is evaluated using the simulated SEIRA signal from poly(methyl methacrylate) and an octadecanethiol self-assembled monolayer. The platforms we present allow for a compact, on-chip SEIRA sensing system with highly efficient waveguide coupling in the mid-IR.

We present optical trapping with a 10 nm gap resonant coaxial nanoaperture in a gold film. Large arrays of 600 resonant plasmonic coaxial nanoaperture traps are produced on a single chip via atomic layer lithography with each aperture tuned to match a 785 nm laser source. We show that these single coaxial apertures can act as efficient nanotweezers with a sharp potential well, capable of trapping 30 nm polystyrene nanoparticles and streptavidin molecules with a laser power as low as 4.7 mW. Furthermore, the resonant coaxial nanoaperture enables real-time label-free detection of the trapping events via simple transmission measurements. Our fabrication technique is scalable and reproducible, since the critical nanogap dimension is defined by atomic layer deposition. Thus our platform shows significant potential to push the limit of optical trapping technologies.

Poloxamer 188 (P188), a poly(ethylene oxide)- b-poly(propylene oxide)- b-poly(ethylene oxide) triblock copolymer, protects cell membranes against various external stresses, whereas poly(ethylene oxide) (PEO; 8600 g/mol) homopolymer lacks protection efficacy. As part of a comprehensive effort to elucidate the protection mechanism, we used surface plasmon resonance (SPR) to obtain direct evidence of binding of the polymers onto supported lipid bilayers. Binding kinetics and coverage of P188 and PEO were examined and compared. Most notably, PEO exhibited membrane association comparable to that of P188, evidenced by comparable association rate constants and coverage. This result highlights the need for additional mechanistic understanding beyond simple membrane association to explain the differential efficacy of P188 in therapeutic applications.

A multitude of biological processes are enabled by complex interactions between lipid membranes and proteins. To understand such dynamic processes, it is crucial to differentiate the constituent biomolecular species and track their individual time evolution without invasive labels. Here, we present a label-free mid-infrared biosensor capable of distinguishing multiple analytes in heterogeneous biological samples with high sensitivity. Our technology leverages a multi-resonant metasurface to simultaneously enhance the different vibrational fingerprints of multiple biomolecules. By providing up to 1000-fold near-field intensity enhancement over both amide and methylene bands, our sensor resolves the interactions of lipid membranes with different polypeptides in real time. Significantly, we demonstrate that our label-free chemically specific sensor can analyze peptide-induced neurotransmitter cargo release from synaptic vesicle mimics. Our sensor opens up exciting possibilities for gaining new insights into biological processes such as signaling or transport in basic research as well as provides a valuable toolkit for bioanalytical and pharmaceutical applications.

Metal nanoparticles that can couple light into tightly confined surface plasmons bridge the size mismatch between the wavelength of light and nanostructures are one of the smallest building blocks of nano-optics. However, plasmonic nanoparticles have been primarily studied to concentrate or scatter incident light as an ultrasmall antenna, while studies of their intrinsic plasmonic light emission properties have been limited. Although light emission from plasmonic structures can be achieved by inelastic electron tunneling, this strategy cannot easily be applied to isolated single nanoparticles due to the difficulty in making electrical connections without disrupting the particle plasmon mode. Here, we solve this problem by placing gold nanoparticles on a graphene tunnel junction. The monolayer graphene provides a transparent counter electrode for tunneling while preserving the ultrasmall footprint and plasmonic mode of nanoparticle. The tunneling electrons excite the plasmonic mode, followed by radiative decay of the plasmon. We also demonstrate that a dielectric overlayer atop the graphene tunnel junction can be used to tune the light emission. We show the simplicity and scalability of this approach by achieving electroluminescence from single nanoparticles without bulky contacts as well as millimeter-sized arrays of nanoparticles.

We present a wafer-scale array of resonant coaxial nanoapertures as a practical platform for surface-enhanced infrared absorption spectroscopy (SEIRA). Coaxial nanoapertures with sub-10 nm gaps are fabricated via photolithography, atomic layer deposition of a sacrificial Al 2 O 3 layer to define the nanogaps, and planarization via glancing-angle ion milling. At the zeroth-order Fabry-Pérot resonance condition, our coaxial apertures act as a "zero-mode resonator (ZMR)", efficiently funneling as much as 34% of incident infrared (IR) light along 10 nm annular gaps. After removing Al 2 O 3 in the gaps and inserting silk protein, we can couple the intense optical fields of the annular nanogap into the vibrational modes of protein molecules. From 7 nm gap ZMR devices coated with a 5 nm thick silk protein film, we observe high-contrast IR absorbance signals drastically suppressing 58% of the transmitted light and infer a strong IR absorption enhancement factor of 10 4 ∼10 5 . These single nanometer gap ZMR devices can be mass-produced via batch processing and offer promising routes for broad applications of SEIRA.

The many unique properties of graphene, such as the tunable optical, electrical, and plasmonic response make it ideally suited for applications such as biosensing. As with other surface-based biosensors, however, the performance is limited by the diffusive transport of target molecules to the surface. Here we show that atomically sharp edges of monolayer graphene can generate singular electrical field gradients for trapping biomolecules via dielectrophoresis. Graphene-edge dielectrophoresis pushes the physical limit of gradient-force-based trapping by creating atomically sharp tweezers. We have fabricated locally backgated devices with an 8-nm-thick HfO 2 dielectric layer and chemical-vapor-deposited graphene to generate 10× higher gradient forces as compared to metal electrodes. We further demonstrate near-100% position-controlled particle trapping at voltages as low as 0.45 V with nanodiamonds, nanobeads, and DNA from bulk solution within seconds. This trapping scheme can be seamlessly integrated with sensors utilizing graphene as well as other two-dimensional materials.

Split-ring resonators (SRRs) present an attractive avenue for the development of micro/nano scale inclinometers for applications like medical microbots, military hardware, and nanosatellite systems. However, the 180° isotropy of their two-dimensional structure presents a major hurdle. In this paper, we present the design of a three-dimensional (3D) anisotropic SRR functioning as a microscale inclinometer enabling it to remotely sense rotations from 0° to 360° along all three axes (X, Y, and Z), by employing the geometric property of a 3D structure. The completely polymeric composition of the cubic structure renders it transparent to the Terahertz (THz) light, providing a transmission response of the tilted SRRs patterned on its surface that is free of any distortion, coupling, and does not converge to a single point for two different angular positions. Fabrication, simulation, and measurement data have been presented to demonstrate the superior performance of the 3D micro devices.

A high spatial resolution, cyclical thinning method for realizing black phosphorus (BP) heterostructures is reported. This process utilizes a cyclic technique involving BP surface oxidation and vacuum annealing to create BP flakes as thin as 1.6 nm. The process also utilizes a spatially patternable mask created by evaporating Al that oxidizes to form Al 2 O 3 , which stabilizes the unetched BP regions and enables the formation of lateral heterostructures with spatial resolution as small as 150 nm. This thinning/patterning technique has also been used to create the first-ever lateral heterostructure BP metal oxide semiconductor field-effect transistor (MOSFET), in which half of a BP flake was thinned in order to increase its band gap. This heterostructure MOSFET showed an ON/OFF current ratio improvement of 1000× compared to homojunction MOSFETs.

We present a novel plasmonic antenna structure, a split-wedge antenna, created by splitting an ultrasharp metallic wedge with a nanogap perpendicular to its apex. The nanogap can tightly confine gap plasmons and boost the local optical field intensity in and around these opposing metallic wedge tips. This three-dimensional split-wedge antenna integrates the key features of nanogaps and sharp tips, i.e., tight field confinement and three-dimensional nanofocusing, respectively, into a single platform. We fabricate split-wedge antennas with gaps that are as small as 1 nm in width at the wafer scale by combining silicon V-grooves with template stripping and atomic layer lithography. Computer simulations show that the field enhancement and confinement are stronger at the tip-gap interface compared to what standalone tips or nanogaps produce, with electric field amplitude enhancement factors exceeding 50 when near-infrared light is focused on the tip-gap geometry. The resulting nanometric hotspot volume is on the order of λ 3 /10 6 . Experimentally, Raman enhancement factors exceeding 10 7 are observed from a 2 nm gap split-wedge antenna, demonstrating its potential for sensing and spectroscopy applications.