Subwavelength Terahertz Resonance Imaging (STRING) for Molecular Fingerprinting.

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.

A room-temperature polarization-sensitive CMOS terahertz camera based on quantum-dot-enhanced terahertz-to-visible photon upconversion.

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.

Terahertz and infrared nonlocality and field saturation in extreme-scale nanoslits.

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.

Modeling and observation of mid-infrared nonlocality in effective epsilon-near-zero ultranarrow coaxial apertures.

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.

High-Contrast Infrared Absorption Spectroscopy via Mass-Produced Coaxial Zero-Mode Resonators with Sub-10 nm Gaps.

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 104∼105. These single nanometer gap ZMR devices can be mass-produced via batch processing and offer promising routes for broad applications of SEIRA.

High-Throughput Fabrication of Resonant Metamaterials with Ultrasmall Coaxial Apertures via Atomic Layer Lithography.

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 ∼ 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 ≫ period, making this fabrication method ideal for manufacturing resonant metamaterials.

Numerical design of electrical-mechanical traps.

We present a coupled immersed interface method-boundary element method (IIM-BEM) numerical technique that predicts the behaviour of deformable cells under the effect of both hydrodynamic and electrical forces. This technique is applied to the study of a hybrid electrical-mechanical trap for single-cell trapping. We report on the effect of different combinations of electrode positions and mechanical properties of the trap on the maximum loading and unloading Reynolds numbers. We also report on the effect that cells moving with the flow have on cells which have been already trapped in a cavity.