Terahertz quantum plasmonics at nanoscales and angstrom scales

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

Enhanced terahertz conductivity in ultra-thin gold film deposited onto (3-mercaptopropyl) trimethoxysilane (MPTMS)-coated Si substrates

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 ultrathin 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

High-Efficiency Photodetector Based On CVD-Grown WS2_2 Monolayer

Future generation technologies demand high efficiency photodetectors to enable sensing and switching devices for ultrafast communication and machine vision. This require direct-band gap materials with high photosensitivity, high detectivity and high quantum efficiency. Monolayered two- Dimensional (2D)-Semiconductors based photodetectors are the most promising materials for such applications, although experimental realization has been limited due to unavailability of high quality sample. In the current manuscript, we report about WS$_2$ based photodetector having sensitivity of 290 AW-1 upon 405 nm excitation and incident power density as low as 0.06 mW/cm$^2$. The fabricated device shows detectivity of 52*10^14 with external quantum efficiency of 89*10$^3$%. The observed superior photo-response parameters of CVD grown WS$_2$ based photodetector as compared to Si-detectors establishes it capability to replace the Si-photodetectors with monolayered ultrathin device having superior performance parameters.Comment: 26 Pages, 8 figure

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. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreemen

Near-maximum microwave absorption in a thin metal film at the pseudo-free-standing limit

Electromagnetic absorbers based on ultra-thin metallic film are desirable for many applications such as plasmonics, metamaterials, and long-wavelength detectors. A metallic film will achieve a maximum 50% of electromagnetic wave absorption, frequency independent, at a thickness defined by its conductivity, typically in the sub-Angstrom range for good metals if bulk conductivity is maintained throughout. This makes it extremely difficult to obtain substantial absorption from thin metal films, in contrast to 2D materials such as graphene. Luckily, however, from a practical point of view, metal conductivity is drastically reduced as the film becomes sub-100 nm, to make it a race between the thinnest possible metal thickness experimentally achievable vs the conductivity reduction. Here, we demonstrate a near-50% absorption at a gold film thickness of 6.5 nm, with conductivity much reduced from the bulk value, down to the range of 10(6) Siemens per meter. Studying the effect of the substrate thickness, we found that the common cover glass, with its thickness much smaller than the wavelength, achieves symmetric absorption of 44%, implying that a pseudo-free-standing limit is achieved. Our work may find applications in infrared sensing as in bolometers and biomedical sensing using microwaves

Angstrom-Scale Active Width Control of Nano Slits for Variable Plasmonic Cavity

Nanogap slits can operate as a plasmonic Fabry-Perot cavity in the visible and infrared ranges due to the gap plasmon with an increased wavenumber. Although the properties of gap plasmon are highly dependent on the gap width, active width tuning of the plasmonic cavity over the wafer length scale was barely realized. Recently, the fabrication of nanogap slits on a flexible substrate was demonstrated to show that the width can be adjusted by bending the flexible substrate. In this work, by conducting finite element method (FEM) simulation, we investigated the structural deformation of nanogap slit arrays on an outer bent polydimethylsiloxane (PDMS) substrate and the change of the optical properties. We found that the tensile deformation is concentrated in the vicinity of the gap bottom to widen the gap width proportionally to the substrate curvature. The width widening leads to resonance blueshift and field enhancement decrease. Displacement ratio ((width change)/(supporting stage translation)), which was identified to be proportional to the substrate thickness and slit period, is on the order of 10(-5) enabling angstrom-scale width control. This low displacement ratio comparable to a mechanically controllable break junction highlights the great potential of nanogap slit structures on a flexible substrate, particularly in quantum plasmonics

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. (C) 2022 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreemen

Ultra-Narrow Metallic Nano-Trenches Realized by Wet Etching and Critical Point Drying

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

Molecular lens of the nonresonant dipole force

A cylindrical molecular lens is formed by focusing a nanosecond IR laser pulse. Trajectories of a CS2 molecular beam deflected by the lens are traced using the velocity map imaging technique. The characteristic lens parameters including the focal length, minimum beam width, and distance to the minimum-width position are determined. The laser intensity dependence of the parameters is in good agreement with theoretical predictions. Exciting possibilities for molecular optics and a new type of optical chromatography are opened up.open394