Optical Tweezing Terahertz Probing for a Single Metal Nanoparticle.

Recently, extensive research has been reported on the detection of metal nanoparticles using terahertz waves, due to their potential for efficient and nondestructive detection of chemical and biological samples without labeling. Resonant terahertz nanoantennas can be used to detect a small amount of molecules whose vibrational modes are in the terahertz frequency range with high sensitivity. However, the positioning of target molecules is critical to obtaining a reasonable signal because the field distribution is inhomogeneous over the antenna structure. Here, we combine an optical tweezing technique and terahertz spectroscopy based on nanoplasmonics, resulting in extensive controllable tweezing and sensitive detection at the same time. We observed optical tweezing of a gold nanoparticle and detected it with terahertz waves by using a single bowtie nanoantenna. Furthermore, the calculations confirm that molecular fingerprinting is possible by using our technique. This study will be a prestep of biomolecular detection using gold nanoparticles in terahertz spectroscopy.

Adaptive Gap-Tunable Surface-Enhanced Raman Spectroscopy.

Gap plasmon (GP) resonance in static surface-enhanced Raman spectroscopy (SERS) structures is generally too narrow and not tunable. Here, we present an adaptive gap-tunable SERS device to selectively enhance and modulate different vibrational modes via active flexible Au nanogaps, with adaptive optical control. The tunability of GP resonance is up to ∼1200 cm-1 by engineering gap width, facilitated by mechanical bending of a polyethylene terephthalate substrate. We confirm that the tuned GP resonance selectively enhances different Raman spectral regions of the molecules. Additionally, we dynamically control the SERS intensity through the wavefront shaping of excitation beams. Furthermore, we demonstrate simulation results, exhibiting the mechanical and optical properties of a one-dimensional flexible nanogap and their advantage in high-speed biomedical sensing. Our work provides a unique approach for observing and controlling the enhanced chemical responses with dynamic tunability.

Broadband high-performance terahertz polarizer based on a dense array of 5†nm gap slit antennas.

Critical factors for terahertz polarizers include broadband operation, high transmittance, and a good extinction ratio. In this paper, using a 5 nm-wide metallic slit array with a 200 nm periodicity as a wire grid polarizer, we achieved over 95% transmittance with an average extinction ratio of 40 dB, over the entire spectrum as defined by the terahertz time-domain spectroscopy (0.4 ∼ 2 THz). Theoretical calculations revealed that the slit array can show 100% transmission up to 5 THz, and wider bandwidths with a higher cutoff frequency can be achieved by reducing the slit periodicity. These results provide a novel approach for achieving a broadband THz polarizer and open a new path for seamless integration of the polarizers with nanophotonic applications.

Antenna-based reduced IR absorbers for high-performance microbolometers.

Absorbers for long-wavelength infrared (LWIR) are designed to have a reduced geometry fitted to a gold cross antenna and numerically studied. Compared to the square membrane geometry widely used in conventional microbolometers, the reduced geometry results in smaller thermal capacities of the vanadium dioxide (VO2) and silicon nitride (Si3N4) layers. However, near-field focusing by the cross antenna leads to a high LWIR absorption. Calculations show that the temperature change per incident energy increases with a decrease in the arm width, and the reduced absorber surpasses the square geometry for all incident angles and polarizations. The antenna-based reduced absorber studied here could serve as an alternative geometry for high-performance microbolometers.

Topological Control of 2D Perovskite Emission in the Strong Coupling Regime.

Momentum space topology can be exploited to manipulate radiation in real space. Here we demonstrate topological control of 2D perovskite emission in the strong coupling regime via polaritonic bound states in the continuum (BICs). Topological polarization singularities (polarization vortices and circularly polarized eigenstates) are observed at room temperature by measuring the Stokes parameters of photoluminescence in momentum space. Particularly, in symmetry-broken structures, a very large degree of circular polarization (DCP) of ∼0.835 is achieved in the perovskite emission, which is the largest in perovskite materials to our knowledge. In the strong coupling regime, lower polariton modes shift to the low-loss spectral region, resulting in strong emission enhancement and large DCP. Our reciprocity analysis reveals that DCP is limited by material absorption at the emission wavelength. Polaritonic BICs based on 2D perovskite materials combine unique topological features with exceptional material properties and may become a promising platform for active nanophotonic devices.

Topology-Changing Broadband Metamaterials Enabled by Closable Nanotrenches.

One of the most straightforward methods to actively control optical functionalities of metamaterials is to apply mechanical strain deforming the geometries. These deformations, however, leave symmetries and topologies largely intact, limiting the multifunctional horizon. Here, we present topology manipulation of metamaterials fabricated on flexible substrates by mechanically closing/opening embedded nanotrenches of various geometries. When an inner bending is applied on the substrate, the nanotrench closes and the accompanying topological change results in abrupt switching of metamaterial functionalities such as resonance, chirality, and polarization selectivity. Closable nanotrenches can be embedded in metamaterials of broadband spectrum, ranging from visible to microwave. The 99.9% extinction performance is robust, enduring more than a thousand bending cycles. Our work provides a wafer-scale platform for active quantum plasmonics and photonic application of subnanometer phenomena.

Effective-zero-thickness terahertz slot antennas using stepped structures.

Metallic nanostructures play an essential role in electromagnetic manipulations due to the localization and enhancement of electromagnetic waves in nanogaps. Scaling down the dimensions of the gap, such as the gap width and the thickness, is an effective way to enhance light-matter interaction with colossal field enhancement. However, reducing the thickness below 10 nanometers still suffers from fabrication difficulty and unintended direct transmission through metals. Here, we fabricate effective-zero-thickness slot antennas by stepping metals in the vicinity of the gaps to confine electromagnetic waves in tiny volumes. We analyze and simulate terahertz transmission, and demonstrate the absorption enhancement of molecules in the slot antennas. Our fabrication technique provides a simple but versatile tool for maximum field enhancement and molecular sensing.

Phonon-Polaritons in Lead Halide Perovskite Film Hybridized with THz Metamaterials.

In this work, we demonstrated a phonon-polariton in the terahertz (THz) frequency range, generated in a crystallized lead halide perovskite film coated on metamaterials. When the metamaterial resonance was in tune with the phonon resonance of the perovskite film, Rabi splitting occurred due to the strong coupling between the resonances. The Rabi splitting energy was about 1.1 meV, which is larger than the metamaterial and phonon resonance line widths; the interaction potential estimation confirmed that the strong coupling regime was reached successfully. We were able to tune the polaritonic branches by varying the metamaterial resonance, thereby obtaining the dispersion curve with a clear anticrossing behavior. Additionally, we performed in situ THz spectroscopy as we annealed the perovskite film and studied the Rabi splitting as a function of the films' crystallization coverage. The Rabi splitting versus crystallization volume fraction exhibited a unique power-law scaling, depending on the crystal growth dimensions.

Fabrication of vertical van der Waals gap array using single-and multi-layer graphene.

Arrays of van der Waals gaps were manufactured by synthesizing the vertically aligned graphene layer stacked between two copper (Cu) catalytic films. The Cu-graphene-Cu laminated structure was obtained by directly synthesizing graphene on a patterned Cu film followed by depositing a second copper layer for optical measurements. The synthesis of graphene on the Cu surface was optimized by adjusting the synthesis temperatures and pre-annealing time using plasma enhanced chemical vapor deposition (PECVD). Resonant Raman spectroscopy measurements reveal that graphene can be synthesized on both bulk Cu foil and relatively thin Cu film under the same growth mechanism using PECVD. Structural and optical characterizations of the array of graphene van der Waals gaps were implemented by the transmission electron microscope and terahertz-time domain spectroscopy (THz-TDS). In THz-TDS, the measured THz amplitude transmitted through the graphene van der Waals gap slit array was constant regardless of the gap width determined by the number of graphene layers between the Cu thin films in a single slit. These results imply that the optical dielectric constant of graphene at THz frequencies in the out-of-plane direction is linearly proportional to the gap width. Our results of the manufacturing method can be adopted to investigate mechanical, electrical, and optical properties of other 2D materials such as h-BN, MoS2, and others. Furthermore, metal-graphene-metal structures with vertical orientations can be used in many electronic, optic, and optoelectronic applications.

Copper-based etalon filter using antioxidant graphene layer.

Copper is a low-cost material compared to silver and gold, having high reflectivity in the near infrared spectral range as well as good electrical and thermal conductivity. Its properties make it a good candidate for metal-based low-cost multilayer thin-film devices and optical components. However, its high reflectance in the devices is reduced because copper is easily oxidized. Here, we suggest a copper-based Fabry-Perot optical filter consisting of a thin dielectric layer stacked between two copper films, which can realize low-cost production compared to a conventional silver-based etalon filter. The reduced performance due to the inherent oxidation of the copper surface can be overcome by passivating the copper films with monolayer graphene. The anti-oxidation of copper film is investigated by optical microscopy, x-ray photoelectron spectroscopy, and transmission measurement in UV-vi spectral ranges. Our results show that the graphene coating can be expanded for various metal-based optical devices in terms of anti-corrosion.

Strongly Localized ohmic Absorption of Terahertz Radiation in Nanoslot Antennas.

Ohmic absorption of light is an indication of a light-matter interaction within metals, where many interesting phenomena and application potentials can be found. To realize the ohmic absorption of light at long wavelengths, where metals are highly reflective, one can use a metamaterial absorber design to concentrate the electromagnetic field within a thin metal film. This concept has enabled thinning of perfect absorbers from a quarter-wave thickness to several tens of nanometers, greatly improving the utility and efficiency of light-metal interactions. Further improvements on the performance are expected if the absorption can be additionally focused laterally, which is a possibility not yet explored. In this study, we report that nanoslot antennas can be a unique ohmic absorber of the low-frequency radiations, where it can incorporate 70% of incident light to ohmic absorption, focused laterally onto 1% of the unit cell area. The inductive field that drives both field enhancement and ohmic absorption is localized within a skin depth distance from the slots with amplitude being as large as 30% of the incident field. Mode-matching calculations and terahertz spectroscopy measurements confirm the inductive and localized nature of the absorption. The strong confinement of the inductive field and of the resulting ohmic absorption is expected to open a new venue in nanocalorimetry, optical nonlinearities of metals, and bolometer applications.

Electromagnon with Sensitive Terahertz Magnetochromism in a Room-Temperature Magnetoelectric Hexaferrite.

An electromagnon in the magnetoelectric (ME) hexaferrite Ba_{0.5}Sr_{2.5}Co_{2}Fe_{24}O_{41} (Co_{2}Z-type) single crystal is identified by time-domain terahertz (THz) spectroscopy. The associated THz resonance is active on the electric field (E^{ω}) of the THz light parallel to the c axis (∥ [001]), whose spectral weight develops at a markedly high temperature, coinciding with a transverse conical magnetic order below 410 K. The resonance frequency of 1.03 THz at 20 K changes -8.7% and +5.8% under external magnetic field (H) of 2 kOe along [001] and [120], respectively. A model Hamiltonian describing the conical magnetic order elucidates that the dynamical ME effect arises from antiphase motion of spins which are coupled with modulating electric dipoles through the exchange striction mechanism. Moreover, the calculated frequency shift points to the key role of the Dzyaloshinskii-Moriya interaction that is altered by static electric polarization change under different H.

Terahertz Nanoprobing of Semiconductor Surface Dynamics.

Most semiconductors have surface dynamics radically different from its bulk counterpart due to surface defect, doping level, and symmetry breaking. Because of the technical challenge of direct observation of the surface carrier dynamics, however, experimental studies have been allowed in severely shrunk structures including nanowires, thin films, or quantum wells where the surface-to-volume ratio is very high. Here, we develop a new type of terahertz (THz) nanoprobing system to investigate the surface dynamics of bulk semiconductors, using metallic nanogap accompanying strong THz field confinement. We observed that carrier lifetimes of InP and GaAs dramatically decrease close to the limit of THz time resolution (∼1 ps) as the gap size decreases down to nanoscale and that they return to their original values once the nanogap patterns are removed. Our THz nanoprobing system will open up pathways toward direct and nondestructive measurements of surface dynamics of bulk semiconductors.

Terahertz field enhancement in asymmetric and tapered nano-gaps.

We investigate field enhancement inside metal-insulator-metal gaps with asymmetric thicknesses and tapered shapes in the terahertz regime. Finite-difference time-domain simulations were conducted for calculation of field enhancement factor. The calculation indicates that for asymmetric sample, field enhancement increases proportionally with the decrease of the thinner of the two metal film thicknesses surrounding the gap. Concomitantly, angle variation has little effect on the field enhancement if the thickness of the narrowest gap region is fixed. A model based on the capacitor concept is proposed for intuitive understanding of the phenomena.

Nanoscale Single-Element Color Filters.

Visible-light filters constructed from nanostructured materials typically consist of a metallic grating and rely on the excitation of surface plasmon polaritons (SPPs). In order to operate at full efficiency, the number of grating elements needs to be maximized such that light can couple more efficiently to the SPPs through improved diffraction. Such conditions impose a limitation on the compactness of the filter since a larger number of grating elements represents a larger effective size. For emerging applications involving nanoscale transmitters or receivers, a device that can filter localized excitations is highly anticipated but is challenging to realize through grating-type filters. In this work, we present the design of an optical filter operating with a single element, marking a departure from diffractive plasmonic coupling. Our device consists of a ZnO nanorod enclosed by two layers of Ag film. For diffraction-limited light focused on the nanorod, narrow passbands can be realized and tuned via variation of the nanorod diameter across the visible spectrum. The spectral and spatial filtering originates from scattering cancellation localized at the nanorod due to the cavity and nanorod exhibiting opposite effective dipole moments. This ability to realize high-performance optical filtering at the ultimate size introduces intriguing possibilities for nanoscale near-field communication or ultrahigh resolution imaging pixels.

Terahertz Quantum Plasmonics of Nanoslot Antennas in Nonlinear Regime.

Quantum tunneling in plasmonic nanostructures has presented an interesting aspect of incorporating quantum mechanics into classical optics. However, the study has been limited to the subnanometer gap regime. Here, we newly extend quantum plasmonics to gap widths well over 1 nm by taking advantage of the low-frequency terahertz regime. Enhanced electric fields of up to 5 V/nm induce tunneling of electrons in different arrays of ring-shaped nanoslot antennas of gap widths from 1.5 to 10 nm, which lead to a significant nonlinear transmission decrease. These observations are consistent with theoretical calculations considering terahertz-funneling-induced electron tunneling across the gap.

A Vanadium Dioxide Metamaterial Disengaged from Insulator-to-Metal Transition.

We report that vanadium dioxide films patterned with λ/100000 nanogaps exhibit an anomalous transition behavior at millimeter wavelengths. Most of the hybrid structure's switching actions occur well below the insulator to metal transition temperature, starting from 25 °C, so that the hysteresis curves completely separate themselves from their bare film counterparts. It is found that thermally excited intrinsic carriers are responsible for this behavior by introducing enough loss in the context of the radically modified electromagnetic environment in the vicinity of the nanogaps. This phenomenon newly extends the versatility of insulator to metal transition devices to encompass their semiconductor properties.

Terahertz-Triggered Phase Transition and Hysteresis Narrowing in a Nanoantenna Patterned Vanadium Dioxide Film.

We demonstrate that high-field terahertz (THz) pulses trigger transient insulator-to-metal transition in a nanoantenna patterned vanadium dioxide thin film. THz transmission of vanadium dioxide instantaneously decreases in the presence of strong THz fields. The transient THz absorption indicates that strong THz fields induce electronic insulator-to-metal transition without causing a structural transformation. The transient phase transition is activated on the subcycle time scale during which the THz pulse drives the electron distribution of vanadium dioxide far from equilibrium and disturb the electron correlation. The strong THz fields lower the activation energy in the insulating phase. The THz-triggered insulator-to-metal transition gives rise to hysteresis loop narrowing, while lowering the transition temperature both for heating and cooling sequences. THz nanoantennas enhance the field-induced phase transition by intensifying the field strength and improve the detection sensitivity via antenna resonance. The experimental results demonstrate a potential that plasmonic nanostructures incorporating vanadium dioxide can be the basis for ultrafast, energy-efficient electronic and photonic devices.

Ultrasensitive molecular absorption detection using metal slot antenna arrays.

We theoretically study the transmission reduction of light passing through absorptive molecules embedded in a periodic metal slot array in a near infrared wavelength regime. From the analytically solved transmitted light, we present a simple relation given by the attenuation length of light at the resonance wavelength of the slot antennas with respect to the spectral width of the resonant transmission peak. This relation clearly explains that the control of the transmission reduction even with very low absorptive materials is possible. We investigate also the transmission reduction by absorptive molecules in a real metallic slot antenna array on a dielectric substrate and compare the results with finite difference time domain calculations. In numerical calculations, we demonstrate that the same amount of transmission reduction by a bulk absorptive material can be achieved only with one-hundredth thickness of the same material when it is embedded in an optimized Fano-resonant slot antenna array. Our relation presented in this study can contribute to label-free chemical and biological sensing as an efficient design and performance criterion for periodic slot antenna arrays.

Selective electric and magnetic sensitivity of aperture probes.

We report the effect of geometrical factors governing the polarization profiles of near-field scanning optical microscope (NSOM) probes. The most important physical parameter controlling the selective electric or magnetic field sensitivity is found to be the width of the metal rim surrounding aperture. Probes with metal rim width w < λ/2 selectively senses the optical electric field, while those with w > λ/2 selectively senses the optical magnetic field. Intensity variation of optical Hertz standing wave formed upon reflection at oblique incidence shows a phase difference of π/2 between electric and magnetic probes: an analogue of the classical Wiener's experiment. Our work paves way towards electromagnetic engineering of nanostructures.