High-refractive-index silicon nanoresonators are promising low-loss alternatives to plasmonic particles in CMOS-compatible nanophotonics applications. However, complex 3D particle morphologies are challenging to realize in practice, thus limiting the range of achievable optical functionalities. Using 3D film structuring and a novel gradient mask transfer technique, the first intrinsically chiral dielectric metasurface is fabricated in the form of a monolayer of twisted silicon nanocrescents that can be easily detached and dissolved into colloidal suspension. The metasurfaces exhibit selective handedness and a circular dichroism as large as 160° µm due to pronounced differences in induced current loops for left-handed and right-handed polarization. The detailed morphology of the detached particles is analyzed using high-resolution transmission electron microscopy. Furthermore, it is shown that the particles can be manipulated in solution using optical tweezers. The fabrication and detachment method can be extended to different nanoparticle geometries and paves the way for a wide range of novel nanophotonic experiments and applications of high-index dielectrics.
In comparison to nanoplasmonic structures, resonant high-index dielectric nanoantennas hold several advantages that may benefit nanophotonic applications, including CMOS compatibility and low ohmic losses. One such application area might be label-free refractometric sensing, where changes in individual antenna resonance properties are used to quantify changes in the surrounding refractive index, for example, due to biomolecular binding. Here, we analyze and compare the sensing performance of silicon and gold nanodisks using a common and unbiased testing framework. We find that the all-dielectric system is fully capable of effectively monitoring small changes in bulk refractive index and biomolecular coverage, but the sensitivity is five to ten times lower than the plasmonic counterpart. However, this drawback is partly compensated for by a more linear response to adsorbate layer thickness changes and an approximately four times smaller susceptibility to photothermal heating. Finally, dielectric sensors may show promise if certain strategies are employed to improve their performance, which could thus bridge the gap between the two systems.
Optically thin perfect light absorbers could find many uses in science and technology. However, most physical realizations of perfect absorption for the optical range rely on plasmonic excitations in nanostructured metallic metasurfaces, for which the absorbed light energy is quickly lost as heat due to rapid plasmon decay. Here we show that a silicon metasurface excited in a total internal reflection configuration can absorb at least 97% of incident near-infrared light due to interferences between coherent electric and magnetic dipole scattering from the silicon nanopillars that build up the metasurface and the reflected wave from the supporting glass substrate. This "near-perfect" absorption phenomenon loads more than 50 times more light energy into the semiconductor than what would be the case for a uniform silicon sheet of equal surface density, irrespective of incident polarization. We envisage that the concept could be used for the development of novel light harvesting and optical sensor devices.
Plasmonic gold nanorods are prime candidates for a variety of biomedical, spectroscopy, data storage, and sensing applications. It was recently shown that gold nanorods optically trapped by a focused circularly polarized laser beam can function as extremely efficient nanoscopic rotary motors. The system holds promise for applications ranging from nanofluidic flow control and nanorobotics to biomolecular actuation and analysis. However, to fully exploit this potential, one needs to be able to control and understand heating effects associated with laser trapping. We investigated photothermal heating of individual rotating gold nanorods by simultaneously probing their localized surface plasmon resonance spectrum and rotational Brownian dynamics over extended periods of time. The data reveal an extremely slow nanoparticle reshaping process, involving migration of the order of a few hundred atoms per minute, for moderate laser powers and a trapping wavelength close to plasmon resonance. The plasmon spectroscopy and Brownian analysis allows for separate temperature estimates based on the refractive index and the viscosity of the water surrounding a trapped nanorod. We show that both measurements yield similar effective temperatures, which correspond to the actual temperature at a distance of the order 10-15 nm from the particle surface. Our results shed light on photothermal processes on the nanoscale and will be useful in evaluating the applicability and performance of nanorod motors and optically heated nanoparticles for a variety of applications.
Anisotropic media induce changes in the polarization state of transmitted and reflected light. Here we combine this effect with the refractive index sensitivity typical of plasmonic nanoparticles to experimentally demonstrate self-referenced single wavelength refractometric sensing based on polarization conversion. We fabricated anisotropic plasmonic metasurfaces composed of gold dimers and, as a proof of principle, measured the changes in the rotation of light polarization induced by biomolecular adsorption with a surface sensitivity of 0.2 ng cm(-2). We demonstrate the possibility of miniaturized sensing and we show that experimental results can be reproduced by analytical theory. Various ways to increase the sensitivity and applicability of the sensing scheme are discussed.
enable realization of large-scale nanostructured HID materials with well-defined physical and optical properties. Electron beam lithography has been the method of choice for proof-of-concept metasurface applications, but simpler and cheaper fabrication methods are needed to upscale new ideas into commercial devices. Several such methodologies have indeed been proposed, each technique with its own advantages and drawbacks. [19] For example, dewetting [20] and laser ablation methods from bulk HID materials [6,21] can easily be upscaled, but they are difficult to control and result in a large degree of particle heterogeneity. Nanoimprint lithography [22] and laser assisted deposition [23] are more precise, but the first requires the use of expensive masks and the latter is not yet upscalable.
The ability to differentiate chiral molecules of different handedness is of great importance for chemical and life sciences. Since most of the relevant chiral molecules have their chiral transitions in the UV region, detecting their circular dichroism (CD) signal is associated with practical experimental challenges of performing optical measurements in that spectral range. To address this problem, here, we study the possibility of shifting CD signal of a model chiral medium by reaching the strong coupling regime with an optical microcavity.Specifically, we show that by strongly coupling chiral plasmonic nanoparticles to a non-chiral Fabry-Pérot microcavity one can imprint the hybrid mode splitting, the hallmark of strongly coupled systems, on the CD spectrum of the coupled system and thereby effectively shift the chiral resonance of the model system to lower energies. We first predict the effect using analytical transfer-matrix method as well as numerical finite-difference time-domain (FDTD) simulations. Furthermore, we confirm the validity of theoretical predictions in a proof-ofprinciple experiment involving chiral plasmonic nanoparticles coupled to a Fabry-Pérot microcavity.
Plasmonic optical antennas and metamaterials with an ability to boost light-matter interactions for particular incidence or emission angles could find widespread use in solar harvesting, biophotonics, and in improving photon source performance at optical frequencies. However, directional plasmonic structures have generally large footprints or require complicated geometries and costly nanofabrication technologies. Here, we present a directional metasurface realized by breaking the out-of-plane symmetry of its individual elements: tilted subwavelength plasmonic gold nanopillars. Directionality is caused by the complex charge oscillation induced in each individual nanopillar, which essentially acts as a tilted dipole above a dielectric interface. The metasurface is homogeneous over a macroscopic area and it is fabricated by a combination of facile colloidal lithography and off-normal metal deposition. Fluorescence excitation and emission from dye molecules deposited on the metasurface is enhanced in specific directions determined by the tilt angle of the nanopillars. We envisage that these directional metasurfaces can be used as cost-effective substrates for surface-enhanced spectroscopies and a variety of nanophotonic applications.
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