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.
Nanoparticles , Terahertz Spectroscopy , Spectrum Analysis , Terahertz Spectroscopy/methods
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.
Quantum Dots , Temperature , Photons , Semiconductors , Luminescence
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 VRMS) and low conductivity solutions. Here we show actuation of microchannels as narrow as 1 µm using voltages as low as 0.5 VRMS 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.
Electrowetting , Microfluidics , Surface Tension , Water , Wettability
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.
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.
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.
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.
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 2Eg, 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 MoTe2 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 >2Eg, consistent with CM results from an optical approach, pushing the solar cell efficiency beyond the Shockley-Queisser limit.
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.
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.
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 SiO2 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.
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 µm2, 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.
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.
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.
Biosensing Techniques/methods , Lipid Bilayers/chemistry , Membrane Lipids/chemistry , Spectroscopy, Fourier Transform Infrared , Circular Dichroism , Lipid Bilayers/metabolism , Membrane Lipids/metabolism , Membrane Proteins/chemistry , Membrane Proteins/metabolism , Peptides/chemistry , Peptides/metabolism , Protein Binding , Reproducibility of Results
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.
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 Al2O3 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 Al2O3 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 104â¼105. These single nanometer gap ZMR devices can be mass-produced via batch processing and offer promising routes for broad applications of SEIRA.
We demonstrate the integration of a black phosphorus photodetector in a hybrid, three-dimensional architecture of silicon photonics and metallic nanoplasmonics structures. This integration approach combines the advantages of the low propagation loss of silicon waveguides, high-field confinement of a plasmonic nanogap, and the narrow bandgap of black phosphorus to achieve high responsivity for detection of telecom-band, near-infrared light. Benefiting from an ultrashort channel (â¼60 nm) and near-field enhancement enabled by the nanogap structure, the photodetector shows an intrinsic responsivity as high as 10 A/W afforded by internal gain mechanisms, and a 3 dB roll-off frequency of 150 MHz. This device demonstrates a promising approach for on-chip integration of three distinctive photonic systems, which, as a generic platform, may lead to future nanophotonic applications for biosensing, nonlinear optics, and optical signal processing.
We combine atomic layer lithography and glancing-angle ion polishing to create wafer-scale metamaterials composed of dense arrays of ultrasmall coaxial nanocavities in gold films. This new fabrication scheme makes it possible to shrink the diameter and increase the packing density of 2 nm-gap coaxial resonators, an extreme subwavelength structure first manufactured via atomic layer lithography, both by a factor of 100 with respect to previous studies. We demonstrate that the nonpropagating zeroth-order Fabry-Pérot mode, which possesses slow light-like properties at the cutoff resonance, traps infrared light inside 2 nm gaps (gap volume â¼ λ(3)/10(6)). Notably, the annular gaps cover only 3% or less of the metal surface, while open-area normalized transmission is as high as 1700% at the epsilon-near-zero (ENZ) condition. The resulting energy accumulation alongside extraordinary optical transmission can benefit applications in nonlinear optics, optical trapping, and surface-enhanced spectroscopies. Furthermore, because the resonance wavelength is independent of the cavity length and dramatically red shifts as the gap size is reduced, large-area arrays can be constructed with λresonance â« period, making this fabrication method ideal for manufacturing resonant metamaterials.
Gold/chemistry , Nanostructures/chemistry , Nanotechnology/methods , Light , Nanostructures/ultrastructure , Optics and Photonics
In this work, we present an infrared plasmonic biosensor for chemical-specific detection and monitoring of biomimetic lipid membranes in a label-free and real-time fashion. Lipid membranes constitute the primary biological interface mediating cell signaling and interaction with drugs and pathogens. By exploiting the plasmonic field enhancement in the vicinity of engineered and surface-modified nanoantennas, the proposed biosensor is able to capture the vibrational fingerprints of lipid molecules and monitor in real time the formation kinetics of planar biomimetic membranes in aqueous environments. Furthermore, we show that this plasmonic biosensor features high-field enhancement extending over tens of nanometers away from the surface, matching the size of typical bioassays while preserving high sensitivity.
Biosensing Techniques , Membrane Lipids/isolation & purification , Nanostructures/chemistry , Kinetics , Membrane Lipids/chemistry , Spectrophotometry, Infrared , Surface Plasmon Resonance , Water/chemistry
