Suppressed terahertz dynamics of water confined in nanometer gaps.

Nanoconfined waters exhibit low static permittivity mainly due to interfacial effects that span about one nanometer. The characteristic length scale may be much longer in the terahertz (THz) regime where long-range collective dynamics occur; however, the THz dynamics have been largely unexplored because of the lack of a robust platform. Here, we use metallic loop nanogaps to sharply enhance light-matter interactions and precisely measure real and imaginary THz refractive indices of nanoconfined water at gap widths ranging from 2 to 20 nanometers, spanning mostly interfacial waters all the way to quasi-bulk waters. We find that, in addition to the well-known interfacial effect, the confinement effect also contributes substantially to the decrease in the complex refractive indices of the nanoconfined water by cutting off low-energy vibrational modes, even at gap widths as large as 10 nanometers. Our findings provide valuable insights into the collective dynamics of water molecules which is crucial to understanding water-mediated processes.

More Than 30 000-fold Field Enhancement of Terahertz Nanoresonators Enabled by Rapid Inverse Design.

The rapid development of 6G communications using terahertz (THz) electromagnetic waves has created a demand for highly sensitive THz nanoresonators capable of detecting these waves. Among the potential candidates, THz nanogap loop arrays show promising characteristics but require significant computational resources for accurate simulation. This requirement arises because their unit cells are 10 times smaller than millimeter wavelengths, with nanogap regions that are 1 000 000 times smaller. To address this challenge, we propose a rapid inverse design method using physics-informed machine learning, employing double deep Q-learning with an analytical model of the THz nanogap loop array. In ∼39 h on a middle-level personal computer, our approach identifies the optimal structure through 200 000 iterations, achieving an experimental electric field enhancement of 32 000 at 0.2 THz, 300% stronger than prior results. Our analytical model-based approach significantly reduces the amount of computational resources required, offering a practical alternative to numerical simulation-based inverse design for THz nanodevices.

Drift-dominant exciton funneling and trion conversion in 2D semiconductors on the nanogap.

Understanding and controlling the nanoscale transport of excitonic quasiparticles in atomically thin two-dimensional (2D) semiconductors are crucial to produce highly efficient nano-excitonic devices. Here, we present a nanogap device to selectively confine excitons or trions of 2D transition metal dichalcogenides at the nanoscale, facilitated by the drift-dominant exciton funneling into the strain-induced local spot. We investigate the spatiospectral characteristics of the funneled excitons in a WSe2 monolayer (ML) and converted trions in a MoS2 ML using hyperspectral tip-enhanced photoluminescence imaging with <15-nm spatial resolution. In addition, we dynamically control the exciton funneling and trion conversion rate by the gigapascal-scale tip pressure engineering. Through a drift-diffusion model, we confirm an exciton funneling efficiency of ∼25% with a significantly low strain threshold (∼0.1%), which sufficiently exceeds the efficiency of ∼3% in previous studies. This work provides a previously unexplored strategy to facilitate efficient exciton transport and trion conversion of 2D semiconductor devices.

High sensitivity bolometers based on metal nanoantenna dimers with a nanogap filled with vanadium dioxide.

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.

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.

Three-Dimensional Anisotropic Metamaterials as Triaxial Optical Inclinometers.

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.

High-density metallic nanogap arrays for the sensitive detection of single-walled carbon nanotube thin films.

We have investigated the extraordinary optical transmission of terahertz waves through an array of nanogaps with varying dimensions and periodicities, and used this platform to demonstrate terahertz sensing of a thin film of single-walled carbon nanotubes. We have used atomic layer lithography to fabricate periodic arrays of nanogap loops that have a gap size of 2 nm and a loop length of 100 µm (aspect ratio of 50,000). These sub-mm-scale loops of nanogaps can sustain terahertz electromagnetic resonances along the contour. We have characterized the transmission of terahertz waves through the nanogap arrays and investigated the influence of inter-gap electromagnetic coupling as the array periodicity shrinks from 100 µm to 4 µm. While the gaps occupy only 0.1% of the surface area, we have measured an amplitude (|E|) transmittance of over 50% due to the strong and broadband field enhancement inside the nanogaps. The absolute transmission through the 2 nm gaps along the rectangular loops can be boosted up to 25%, while it is only 1% for annular gaps with the same perimeter. Furthermore, the extremely tight field confinement and strong field enhancement near the 2 nm gap lead to 43% extinction of THz waves in a 10 nm-thick film of single-walled carbon nanotubes over the gaps. On the other hand, THz extinction by the same nanotube film on a bare glass substrate is only 2%. These nanogaps pave the way toward developing sensitive terahertz detectors for biological and chemical targets.

Squeezing millimeter waves through a single, nanometer-wide, centimeter-long slit.

We demonstrate broadband non-resonant squeezing of terahertz (THz) waves through an isolated 2-nm-wide, 2-cm-long slit (aspect ratio of 10(7)), representing a maximum intensity enhancement factor of one million. Unlike resonant nanogap structures, a single, effectively infinitely-long slit passes incident electromagnetic waves with no cutoff, enhances the electric field within the gap with a broad 1/f spectral response, and eliminates interference effects due to finite sample boundaries and adjacent elements. To construct such a uniform, isolated slit that is much longer than the millimeter-scale spot of a THz beam, we use atomic layer lithography to pattern vertical nanogaps in a metal film over an entire 4-inch wafer. We observe an increasing field enhancement as the slit width decreases from 20 nm to 2 nm, in agreement with numerical calculations.

Atomic layer lithography of wafer-scale nanogap arrays for extreme confinement of electromagnetic waves.

Squeezing light through nanometre-wide gaps in metals can lead to extreme field enhancements, nonlocal electromagnetic effects and light-induced electron tunnelling. This intriguing regime, however, has not been readily accessible to experimentalists because of the lack of reliable technology to fabricate uniform nanogaps with atomic-scale resolution and high throughput. Here we introduce a new patterning technology based on atomic layer deposition and simple adhesive-tape-based planarization. Using this method, we create vertically oriented gaps in opaque metal films along the entire contour of a millimetre-sized pattern, with gap widths as narrow as 9.9 Å, and pack 150,000 such devices on a 4-inch wafer. Electromagnetic waves pass exclusively through the nanogaps, enabling background-free transmission measurements. We observe resonant transmission of near-infrared waves through 1.1-nm-wide gaps (λ/1,295) and measure an effective refractive index of 17.8. We also observe resonant transmission of millimetre waves through 1.1-nm-wide gaps (λ/4,000,000) and infer an unprecedented field enhancement factor of 25,000.

Colossal absorption of molecules inside single terahertz nanoantennas.

Molecules have extremely small absorption cross sections in the terahertz range even under resonant conditions, which severely limit their detectability, often requiring tens of milligrams. We demonstrate that nanoantennas tailored for the terahertz range resolves the small molecular cross section problem. The extremely asymmetric electromagnetic environment inside the slot antenna, which finds the electric field being enhanced by thousand times with the magnetic field changed little, forces the molecular cross section to be enhanced by >10(3) accompanied by a colossal absorption coefficient of ~170,000 cm(-1). Tens of nanograms of small molecules such as 1,3,5-trinitroperhydro-1,3,5-triazine (RDX) and lactose drop-cast over an area of 10 mm(2), with only tens of femtograms of molecules inside the single nanoslot, can readily be detected. Our work enables terahertz sensing of chemical and biological molecules in ultrasmall quantities.

Selective enhanced resonances of two asymmetric terahertz nano resonators.

We studied the electromagnetic interaction between two asymmetric terahertz nano resonators, rectangular holes which have a few hundred micron lengths but nanoscale widths. We report that the dominant resonant transmission of the structures can be modulated by the horizontal distance between two rectangles due to the different oscillation strength of the asymmetric coupling at two different resonance frequencies. Our results are significant for an optimum design of rectangular holes in terahertz frequency regime for applications such as sensitive nanoparticle detection and terahertz filters.

Electrical control of terahertz nano antennas on VO2 thin film.

We demonstrate an active metamaterial device that allows to electrically control terahertz transmission over more than one order of magnitude. Our device consists of a lithographically defined gold nano antenna array fabricated on a thin film of vanadium dioxide (VO(2)), a material that possesses an insulator to metal transition. The nano antennas let terahertz (THz) radiation funnel through when the VO(2) film is in the insulating state. By applying a dc-bias voltage through our device, the VO(2) becomes metallic. This electrically shorts the antennas and therefore switches off the transmission in two distinct regimes: reversible and irreversible switching.

Terahertz pinch harmonics enabled by single nano rods.

A pinch harmonic (or guitar harmonic) is a musical note produced by lightly pressing the thumb of the picking hand upon the string immediately after it is picked [J. Chem. Educ. 84, 1287 (2007)]. This technique turns off the fundamental and all overtones except those with a node at that location. Here we present a terahertz analogue of pinch harmonics, whereby a metallic nano rod placed at a harmonic node on a terahertz nanoresonator suppresses the fundamental mode, making the higher harmonics dominant. Strikingly, a skin depth-wide nano rod placed at the mid-point turns off all resonances. Our work demonstrates that terahertz electromagnetic waves can be tailored by nanoparticles strategically positioned, paving important path towards terahertz switching and detection applications.

Controlling terahertz radiation with nanoscale metal barriers embedded in nano slot antennas.

Nanoscale metallic barriers embedded in terahertz (THz) slot antennas are shown to provide unprecedented control of the transition state arising at the crossover between the full- and half-wavelength resonant modes of such antennas. We demonstrate strong near-field coupling between two paired THz slot antennas separated by a 5 nm wide nanobarrier, almost fully inducing the shift to the resonance of the double-length slot antenna. This increases by a factor of 50 the length-scale needed to observe similar coupling strengths in conventional air-gap antennas (around 0.1 nm), making the transition state readily accessible to experiment. Our measurements are in good agreement with a quantitative theoretical modeling, which also provides a simple physical picture of our observations.

A reel-wound carbon nanotube polarizer for terahertz frequencies.

Utilizing highly oriented multiwalled carbon nanotube aerogel sheets, we fabricated micrometer-thick freestanding carbon nanotube (CNT) polarizers. Simple winding of nanotube sheets on a U-shaped polyethylene reel enabled rapid and reliable polarizer fabrication, bypassing lithography or chemical etching processes. With the remarkable extinction ratio reaching ∼37 dB in the broad spectral range from 0.1 to 2.0 THz, combined with the extraordinary gravimetric mechanical strength of CNTs, and the dispersionless character of freestanding sheets, the commercialization prospects for our CNT terahertz polarizers appear attractive.