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Cracks are formed along the photolithographically pre-determined lines with extremely high yield and repeatability, when Cu clusters are introduced between planarized Au thin films sequentially deposited on a PET substrate. These clusters act as nanometer-sized spacers preventing the formation of contiguous metallic bond between the adjacent Au layers which will render prepatterned-cracking impossible. While the effective gap width is initially zero in the optical sense from microwaves all the way to the visible, outer-bending the PET substrate allows the gap width tuning into the 100 nm range, with the stability and controllability in the ranges of 100 s and Angstrom-scale, respectively. It is anticipated that our wafer-scale prepatterned crack technology with an unprecedented mixture of macroscopic length and Angstrom-scale controllability will open-up many applications in optoelectronics, quantum photonics and photocatalysis.

Metallic nanogaps are being widely used for sensing applications, owing to their ability to confine and enhance electromagnetic field within the hot spots. Since the enhanced field does not confine itself perfectly within the gap, however, fringe fields well away from the gap are of potential use as well in real systems. Here, we extend the concept of near field absorption enhancement by quantitatively analyzing terahertz absorption behavior of water molecules outside the hot spots of sub-20 nm-wide, ∼100 μm-long nanotrenches. Contrary to point-gaps which show negligible field enhancement at distances larger than the gap width, our extended nanogap act as a line source, incorporating significant amount of absorption enhancement at much longer distances. We observe absorption enhancement factors of up to 3600 on top of a 5 nm-wide gap, and still well over 300 at 15 nm away. The finding is well supported by theoretical analyses including modal expansion calculations, Kirchhoff integral formalism and antenna theory. Our results provide means to quantitatively analyze light-matter interactions beyond the hot spot picture and enable application of nanogaps for sensitive surface analyses of various material systems.

A well-designed narrow gap between noble metal nanostructures plays a prominent role in surface-enhanced Raman scattering (SERS) to concentrate electromagnetic fields at the local point, called a "hot spot". However, SERS-active substrate fabrication remains a substantial hurdle due to the high process cost and the difficulty of engineering efficient plasmonic hot spots at the target area. In this study, we demonstrate a simple photolithographic method for generating ultrasensitive SERS hot spots at desired positions. The solid-state dewetting of a Ag thin film (thickness of ∼10 nm) using a continuous-wave laser (∼1 MW/cm

With recent advances in nanofabrication technology, various metallic gap structures with gap widths reaching a few to sub-nanometer, and even ‘zero-nanometer’, have been realized. At such regime, metallic gaps not only exhibit strong electromagnetic field confinement and enhancement, but also incorporate various quantum phenomena in a macroscopic scale, finding applications in ultrasensitive detection using nanosystems, enhancement of light–matter interactions in low-dimensional materials, and ultralow-power manipulation of electromagnetic waves, etc. Therefore, moving beyond nanometer to ‘zero-nanometer’ can greatly diversify applications of metallic gaps and may open the field of dynamic ‘gaptronics.’ In this paper, an overview is given on wafer-scale metallic gap structures down to zero-nanometer gap width limit. Theoretical description of metallic gaps from sub-10 to zero-nanometer limit, various wafer-scale fabrication methods and their applications are presented. With such versatility and broadband applicability spanning visible to terahertz and even microwaves, the field of ‘gaptronics’ can be a central building block for photochemistry, quantum optical devices, and 5/6G communications.

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.

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.

One critical factor for bolometer sensitivity is efficient electromagnetic heating of thermistor materials, which plasmonic nanogap structures can provide through the electric field enhancement. In this report, using finite element method simulation, electromagnetic heating of nanorod dimer antennas with a nanogap filled with vanadium dioxide (VO2) was studied for long-wavelength infrared detection. Because VO2 is a thermistor material, the electrical resistance between the two dimer ends depends on the dimer’s temperature. The simulation results show that, due to the high heating ability of the nanogap, the temperature rise is several times higher than expected from the areal coverage. This excellent performance is observed over various nanorod lengths and gap widths, ensuring wavelength tunability and ultrafast operating speed, thereby making the dimer structures a promising candidate for high sensitivity bolometers.

Metal nanostructures supporting plasmonic resonances offer pronounced modifications of an electromagnetic environment for efficient light harvesting in solar energy conversion applications. Since t...

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.

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

Terahertz (THz) nanoantennas have significant potential for versatile applications in THz spectroscopy because of their capability for strong electromagnetic field localization. Electron-beam lithography or focused ion beam machining is typically employed to fabricate nanoantenna structures. These nanolithography methods present limitations in the widespread utilization of THz nanoantennas because of their high cost and low productivity. In this work, we proposed graphene-based crack lithography as a high throughput fabrication method for nanoantenna structures. A double-layer graphene interface was introduced to enable independent control of the nanoantenna dimensions and provide graphene-based nanoantenna structures. We analyzed the underlying mechanism of graphene-based cracking and developed an analytical model governing the geometric parameters of the fabricated nanostructures. As a vital application of the fabricated nanoantenna structures, we demonstrated the highly sensitive detection of d -Glucose molecules. Graphene-based crack lithography can provide a cost-effective method for generating nanoantenna structures with the desired characteristics and can accelerate the development of practical applications of electromagnetic metamaterials.

Through the manipulation of metallic structures, light–matter interaction can enter into the realm of quantum mechanics. For example, intense terahertz pulses illuminating a metallic nanotip can promote terahertz field–driven electron tunneling to generate enormous electron emission currents in a subpicosecond time scale. By decreasing the dimension of the metallic structures down to the nanoscale and angstrom scale, one can obtain a strong field enhancement of the incoming terahertz field to achieve atomic field strength of the order of V/nm, driving electrons in the metal into tunneling regime by overcoming the potential barrier. Therefore, designing and optimizing the metal structure for high field enhancement are an essential step for studying the quantum phenomena with terahertz light. In this review, we present several types of metallic structures that can enhance the coupling of incoming terahertz pulses with the metals, leading to a strong modification of the potential barriers by the terahertz electric fields. Extreme nonlinear responses are expected, providing opportunities for the terahertz light for the strong light–matter interaction. Starting from a brief review about the terahertz field enhancement on the metallic structures, a few examples including metallic tips, dipole antenna, and metal nanogaps are introduced for boosting the quantum phenomena. The emerging techniques to control the electron tunneling driven by the terahertz pulse have a direct impact on the ultrafast science and on the realization of next-generation quantum devices.

A pair of parallel metallic plates with nanometer-scale separations, or a ‘metallic nanotrench’, creates strongly enhanced electric field with uniform spatial distribution when a long wavelength radiation is incident. This property is not only useful for quantitative analysis of light-matter interactions, but also for potential electrochemical studies on nanoconfined molecules. Here, we show our progress on realizing sub-10 nm-wide metallic nanotrenches filled with various liquids to study interaction of nano-confined molecules with terahertz radiation. Large height-to-width aspect ratio and strong field enhancement of the nanotrenches enable sensitive detection of the nano-confined molecules, from which optical properties of the molecules can be determined. We demonstrate fabrication of the nanotrenches with widths as small as 2 nm, and study changes in their terahertz optical properties upon integration with various liquids. Also, we discuss anomalous optical properties of water molecules confined within sub-10 nm-wide metallic nanotrenches.

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.

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.

Various material properties change considerably when material is thinned down to nanometer thicknesses. Accordingly, researchers have been trying to obtain homogeneous thin films with nanometer thickness but depositing homogeneous few nanometers thick gold film is challenging as it tends to form islands rather than homogenous film. Recently, studies have revealed that treating the substrate with an organic buffer, (3-mercaptopropyl) trimethoxysilane (MPTMS) enables deposition of ultra-thin gold film having thickness as low as 5 nm. Different aspects of MPTMS treatment for ultra-thin gold films like its effect on the structure and optical properties at visible wavelengths have been investigated. However, the effect of the MPTMS treatment on electrical conductivity of ultra-thin gold film at terahertz frequency remains unexplored. Here, we measure the complex conductivity of nanometer-thick gold films deposited onto an MPTMS-coated silicon substrate using terahertz time-domain spectroscopy. Following the MPTMS treatment of the substrate, the conductivity of the films was found to increase compared to those deposited onto uncoated substrate for gold films having the thickness less than 11 nm. We observed 5-fold enhancement in the conductivity for a 7 nm-thick gold film. We also demonstrate the fabrication of nanoslot-antenna arrays in 8.2-nm-thick gold films. The nanoslot-antenna with MPTMS coating has resonance at around 0.5 THz with an electric field enhancement of 44, whereas the nanoslot-antenna without MPTMS coating does not show resonant properties. Our results demonstrate that gold films deposited onto MPTMS-coated silicon substrates are promising advanced materials for fabricating ultra-thin terahertz plasmonic devices.

A novel plasmonic interferometric sensor intended for application to biochemical sensing has been investigated experimentally and theoretically. The sensor was included a slit surrounded by rectangular grooves using a thick gold film. A three-dimensional finite difference time-domain commercial software package was applied to simulate the structure. The Focused ion beam milling has been used as a mean to fabricate series of rectangular plasmonic interferometer with varying slit-groove distance L. Oscillation behavior is shown by transmission spectra in a broadband wavelength range between 400 nm and 800 nm in the distance between slit and grooves. Red-shifted interference spectrum is the result of increasing refractive indices. The proposed structure is functional from visible to near-infrared wavelength range and yields a sensitivity of 4923 nm/RIU and a figure of merit as high as 214 at 729 nm wavelength. In conclusion, this study indicates the possibility of fabricating a low cost, compact, and real-time high-throughput plasmonic interferometer.

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.

The function of nanophotonic devices, such as metamaterials for the visible range, photonic and plasmonic crystals, nanoscale waveguides, resonators, switches or optical antennas relies essentially on our ability to tailor and control electromagnetic fields on a subwavelength scale, in much the same way as the wavefunction of electronic nanostructures is localized on an atomic scale. Unlike matter waves, these localized electromagnetic waves are vectorial in nature, and their orientation and magnitude varies on a sub-wavelength scale. Therefore it is vital for a complete description of light in nano-scale devices to map the field vectors with subwavelength resolution. Experimental techniques aimed at probing the field intensity, e.g. aperture-less or aperture-based near-field microscopies, are rapidly improving, but the local orientation of the electromagnetic polarization vector, a fundamental property of the local electromagnetic field, could not be accessed experimentally. Yet, the orientation of the field vector is a key quantity in many thousands of theoretical studies on nano-optics, nanophotonic devices and optical sciences in general. Evidently, the ability to experimentally probe electromagnetic field vectors with nanometer resolution is of fundamental importance for understanding and improving nano-optical devices and for reconciling experiment and theory in the bourgeoning field of nanophotonics. In this chapter, we describe and demonstrate the local field polarization vector detection using the gold nanoparticle (GNP) attached tip as the local field scatterer acting as a nanometer-scaled polarizer. For a suitably small GNP, the far-field scattering is dominated by the electric dipole radiation. Dipole radiation conserve its polarization state into the farfield region enabling characterization of the dipole moment induced at the GNP by measuring the far-field polarization state. And also the dipole moment is determined by the local electric field via polarizability tensor of GNP. Therefore, by characterizing the polarizability tensor of GNP and the polarization state of far-field scattered light, the local electric field vector can be reconstructed. In doing that, the different scattering shape of GNP, the polarizability tensor, is carefully measured and considered to get a consistant result independently of the tip shape. Mapping the local polarization vector in the near-field demands a careful consideration of the surface effect. For example, far field detected light is a complex mixture of the scattered light from GNP and its reflected light at the sample surface which interfere each other strongly depending on the polarization. This so called image dipole effect should be taken into account to correctly address the reconstructed local field vectors in near-field region. In the last section of this chaper, we discuss the limitations of our method and give suggestions to improve the functionality of the polarization vector microscopy.

Plasmonic gap governs much of the electromagnetic response of metamaterials. Meanwhile, nano and subnanometric gap control achieved by exceptional advancement of nanotechnology has paved the way for quantum plasmonics. However, practical applications have been hindered by difficulties of active nano-control over a broad spectral range. We report on mechanically nano-controllable plasmonic metamaterials fabricated on flexible substrate with a broad spectral response from the visible to the terahertz waves. By closing and opening the metallic nanogap via macroscopic control, we observed both classical and quantum plasmonic responses. Using our devices functioning between the two extreme regimes of classical gaps and full-contact mode, we achieve unprecedented performances of light modulation in a broad spectral range.

A metallic nano-trench is a unique optical structure capable of ultrasensitive detection of molecules, active modulation as well as potential electrochemical applications. Recently, wet-etching the dielectrics of metal–insulator–metal structures has emerged as a reliable method of creating optically active metallic nano-trenches with a gap width of 10 nm or less, opening a new venue for studying the dynamics of nanoconfined molecules. Yet, the high surface tension of water in the process of drying leaves the nano-trenches vulnerable to collapsing, limiting the achievable width to no less than 5 nm. In this work, we overcome the technical limit and realize metallic nano-trenches with widths as small as 1.5 nm. The critical point drying technique significantly alleviates the stress applied to the gap in the drying process, keeping the ultra-narrow gap from collapsing. Terahertz spectroscopy of the trenches clearly reveals the signature of successful wet etching of the dielectrics without apparent damage to the gap. We expect that our work will enable various optical and electrochemical studies at a few-molecules-thick level.

Metallic nanostructures have important roles in electromagnetic field manipulations due to the localization of electromagnetic waves, for which fabrication techniques in nanotechnology have been developed. To achieve higher field enhancement, it is required to decrease the dimensions of the nanostructures such as thickness or width of the gap. Here, we fabricated the slant nano-antennas where a portion of metals on each side is overlapped. The slant nano-antennas realize higher electromagnetic field enhancement while keeping background noise almost zero.

We demonstrated a switchable terahertz (THz) resonator by bending it outward with different radius curvatures (RCs), accordingly changing the shape of a diabolo array to a bowtie array. The resonance frequency switched to 0.5 THz and 1.08 THz as the flexible substrate of the resonator was flattened and bent. We analyzed the electrical properties in the I- V curve and optical properties in THz transmission spectra for the cases on flattening/bending/re-flattening after bending the resonator. A switchable THz resonator remains functional even though the operation originates from distorting the metallic array.

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.

We demonstrate photoexcited carrier response of metallic nanogap-patterned semiconductor using optical pump-terahertz probe spectroscopy. Metallic nanogap facilitates observing surface carrier dyna...

Understanding light interaction with metallic structures provides opportunities of manipulation of light, and is at the core of various research areas including terahertz (THz) optics from which diverse applications are now emerging. For instance, THz waves take full advantage of the interaction to have strong field enhancement that compensates their relatively low photon energy. As the THz field enhancement have boosted THz nonlinear studies and relevant applications, further understanding of light interaction with metallic structures is essential for advanced manipulation of light that will bring about subsequent development of THz optics. In this review, we discuss THz wave interaction with deep sub-wavelength nano structures. With focusing on the THz field enhancement by nano structures, we review fundamentals of giant field enhancement that emerges from non-resonant and resonant interactions of THz waves with nano structures in both sub- and super- skin-depth thicknesses. From that, we introduce surprisingly simple description of the field enhancement valid over many orders of magnitudes of conductivity of metal as well as many orders of magnitudes of the metal thickness. We also discuss THz interaction with structures in angstrom scale, by reviewing plasmonic quantum effect and electron tunneling with consequent nonlinear behaviors. Finally, as applications of THz interaction with nano structures, we introduce new types of THz molecule sensors, exhibiting ultrasensitive and highly selective functionalities.

Strong demand for plasmonic devices with an enormously enhanced electric field and desired resonance frequencies has led to extensive investigations of metallic slot structures. While strong field enhancement can be achieved by reducing the width of the slot, the effect of the gap surface plasmon limits the maximum achievable field enhancement at higher frequencies. Specifically, the effect of the gap surface plasmon becomes stronger as the gap width decreases and strongly suppresses the transmission while causing a red-shift of the resonance. Here, we overcome these issues and realize strong field enhancements at higher frequencies, by managing the metal thickness of the nanoslots. We show that, as the nanoslots become as thin as 10 nm, they show a giant electric field enhancement of up to 7600. Moreover, the resonances are strongly blue-shifted to above 1 THz from 0.33 THz. Our work provides a novel route to achieving high field enhancements at desired frequencies, as well as a means by which to charact...

Slot-type nanogaps have been widely utilized in transmission geometry because of their advantages of exclusive light funneling and exact quantification of near-field enhancement at the gap. For further application of the nanogaps in electromagnetic interactions with various target materials, complementary studies on both transmission and reflection properties of the nanogaps are necessary. Here, we observe an anomalous extinction of terahertz waves interacting with rectangular ring-shaped sub-30 nm wide gaps. Substrate works as an index matching layer for the nanogaps, leading to a stronger field enhancement and increased nonlinearity at the gap under substrate-side illumination. This effect is expressed in reflection as a larger dip at the resonance, caused by destructive interference of the diffracted field from the gap with the reflected beam from the metal. The resulting extinction at the resonance is larger than 60% of the incident power, even without any absorbing material in the whole nanogap structure. The extinction even decreases in the presence of an absorbing medium on top of the nanogaps, suggesting that transmission and reflection from nanogaps might not necessarily represent the absorption of the whole structure.

Terahertz (THz) nanogap structures have emerged as versatile platforms for THz science and applications by virtue of their strong in-gap field enhancements and accompanying high levels of sensitivity to gap environments. However, despite their potential, reliable fabrication methods by which to create THz structures with sub-10 nm gaps remain limited. In this work, we fabricated THz split-ring resonator (SRR) arrays featuring a sub-10 nm split gap. Our fabrication method, involving photolithography, argon ion milling, and atomic layer deposition, is a high-throughput technique that is also applicable to the fabrication of other THz structures with sub-10 nm gaps. Through THz-time domain spectroscopy and a numerical simulation, we identified the fundamental magnetic resonances of the nanogap SRRs, at which the electric field enhancement factor is experimentally estimated to be around 7000. This substantial field enhancement makes SRRs with a sub-10 nm gap suitable for the study of high-field phenomena and ...

Split-ring resonator (SRR) based metamaterials have been studied for the development of highly sensitive, small-sized, low-power chemical and biomolecular sensors. However, the anisotropic behavior arising from their two-dimensional (2D) structure presents substantial challenges leading to ambiguity in their transmission spectra. In this paper, we present the design of a three-dimensional (3D) isotropic octagram split-ring resonator (OSRR) demonstrating a three-dimensionally coupled resonance behavior that overcomes the anisotropic response of conventional 2D SRRs, leading to a strong, distortion-free, and polarization-invariant transmission response. The OSRR undergoes 3D coupling through the splits at the corners of the 3D structure (cube), which remains invariant under any polarization along the coordinate axes. The strong coupling between resonant segments provides the OSRR with 25 times higher sensitivity than the corresponding 2D structure, allowing the resonant frequency to be reliably monitored fo...