All-Dielectric Silicon Nanogap Antennas To Enhance the Fluorescence of Single Molecules.

Plasmonic antennas have a profound impact on nanophotonics as they provide efficient means to manipulate light and enhance light-matter interactions at the nanoscale. However, the large absorption losses found in metals can severely limit the plasmonic applications in the visible spectral range. Here, we demonstrate the effectiveness of an alternative approach using all-dielectric nanoantennas based on silicon dimers to enhance the fluorescence detection of single molecules. The silicon antenna design is optimized to confine the near-field intensity in the 20 nm nanogap and reach a 270-fold fluorescence enhancement in a nanoscale volume of λ(3)/1800 with dielectric materials only. Our conclusions are assessed by combining polarization resolved optical spectroscopy of individual antennas, scanning electron microscopy, numerical simulations, fluorescence lifetime measurements, fluorescence burst analysis, and fluorescence correlation spectroscopy. This work demonstrates that all-silicon nanoantennas are a valid alternative to plasmonic devices for enhanced single molecule fluorescence sensing, with the additional key advantages of reduced nonradiative quenching, negligible heat generation, cost-efficiency, and complementary metal-oxide-semiconductor (CMOS) compatibility.

High-resolution imaging and spectroscopy of multipolar plasmonic resonances in aluminum nanoantennas.

We report on the high resolution imaging of multipolar plasmonic resonances in aluminum nanoantennas using electron energy loss spectroscopy (EELS). Plasmonic resonances ranging from near-infrared to ultraviolet (UV) are measured. The spatial distributions of the multipolar resonant modes are mapped and their energy dispersion is retrieved. The losses in the aluminum antennas are studied through the full width at half-maximum of the resonances, unveiling the weight of both interband and radiative damping mechanisms of the different multipolar resonances. In the blue-UV spectral range, high order resonant modes present a quality factor up to 8, two times higher than low order resonant modes at the same energy. This study demonstrates that near-infrared to ultraviolet tunable multipolar plasmonic resonances in aluminum nanoantennas with relatively high quality factors can be engineered. Aluminum nanoantennas are thus an appealing alternative to gold or silver ones in the visible and can be efficiently used for UV plasmonics.

Plasmonic-Enhanced Tunable Near-Infrared Photoresponse for Narrowband Organic Photodetectors.

Near-infrared (NIR) narrowband organic photodetectors (OPDs) can be essential building blocks for emerging applications including wireless optical communication and light detection, but further improvement of their performances remains to be a great challenge. Herein, a light manipulation strategy combining solution-processable gold nanorings (AuNRs)-based hole transporting layer (HTL) and an optical microcavity is proposed to achieve high-performance NIR narrowband OPDs. Optical microcavities with a Fabry-Pérot resonator structure, guided by theoretical simulation, are coupled with PM6:BTP-eC9-based OPDs to exhibit highly tunable NIR selectivity. The further integration of AuNRs array with NIR-customized localized surface plasmon resonance in the HTL of the NIR narrowband OPDs enables evident NIR absorption enhancement, yielding a specific detectivity exceeding 1013 Jones (1.5 × 1012 Jones, calculated from noise spectral density) at 820 nm, along with a finely selective photoresponse (full width at half-maximum of 80 nm) and a 3-fold increase in photocurrent intensity. Finally, the practical application of our OPDs is demonstrated in an NIR communication system. These results reveal the great potential of an appropriate optical design for developing highly performing NIR narrowband OPDs.

Intense Bessel-like beams arising from pyramid-shaped microtips.

We show both numerically and experimentally that intense, narrow, and low-divergence beams of light are produced at the apex of dielectric pyramid-shaped microtips. These beams exhibit a Bessel transverse profile but are narrower than the usual Bessel beam, allowing for a significant enhancement of the light intensity inside the beam. They are generated by axicon-like structures with submicrometric height imprinted in glass by combining optical lithography and chemical etching. The resulting beams are experimentally imaged using fluorescence microscopy, in remarkable agreement with numerical computations.

Stabilization of Copper-Based Biochips with Alumina for Biosensing Application.

Surface plasmon resonance devices typically rely on the use of gold-coated surfaces, but the use of more abundant metals is desirable for the long-term development of plasmonic biochips. As a substitute for gold, thin copper films have been deposited on glass coverslips by thermal evaporation. As expected, these films immersed in a water solution initially exhibit an intense plasmonic resonance comparable to gold. However, without protection, an angle-resolved optical analysis shows a rapid degradation of the copper, characterized by a continuous angular shift of the plasmonic resonance curve. We show that copper films protected with a thin layer of aluminum oxide of a few nanometers can limit the oxidation rate for a sufficient time to perform some standard measurements. As the process is simple and compatible with the current biochip production technique, such an approach could pave the way for the production of alternative and more sustainable biochips.

Detecting a Zeptogram of Pyridine with a Hybrid Plasmonic-Photonic Nanosensor.

Thanks to their small sensing volume, nanosensors based on localized surface plasmon resonances (LSPR) allow the detection of minute amounts of analytes, down to the single-molecule limit. However, the detected analytes are often large molecules, such as proteins. The detection of small molecules remains largely unexplored. Here, we use a hybrid photonic-plasmonic nanosensor to detect a small target molecule (pyridine). The sensor's design is based on a dielectric photonic microstructure acting as an antenna, which efficiently funnels light toward a plasmonic transducer and enhances the detection efficiency. This sensor exhibits a limit of detection as small as 10-14 mol L-1. Using a calibration procedure based on electrodynamical numerical simulations, we compute the number of detected molecules. This yields a limit of detection in mass of 4 zeptograms (1 zg = 10-21 g), a record value for plasmonic molecular sensors. Our system can hence be seen as an optical molecular weighing scale, enabling room temperature detection of mass at the zeptogram scale.

Large-Scale and Low-Cost Fabrication of Silicon Mie Resonators.

High index dielectric nanoparticles have been proposed for many different applications. However, widespread utilization in practice also requires large-scale production methods for crystalline silicon nanoparticles, with engineered optical properties in a low-cost manner. Here, we demonstrate a facile, low-cost, and large-scale fabrication method of crystalline silicon colloidal Mie resonators in water, using a blender. The obtained nanoparticles are polydisperse with an almost spherical shape and the diameters controlled in the range 100-200 nm by a centrifugation process. Then the size distribution of silicon nanoparticles enables broad extinction from UV to near-infrared, confirmed by Mie theory when considering the size distribution in the calculations. Thanks to photolithographic and drop-cast deposition techniques to locate the position on a substrate of the colloidal nanoparticles, we experimentally demonstrate that the individual silicon nanoresonators show strong electric and magnetic Mie resonances in the visible range.

All-Dielectric Colored Metasurfaces with Silicon Mie Resonators.

The photonic resonances hosted by nanostructures provide vivid colors that can be used as color filters instead of organic colors and pigments in photodetectors and printing technology. Metallic nanostructures have been widely studied due to their ability to sustain surface plasmons that resonantly interact with light. Most of the metallic nanoparticles behave as point-like electric multipoles. However, the needs of an another degree of freedom to tune the color of the photonic nanostructure together with the use of a reliable and cost-effective material are growing. Here, we report a technique to imprint colored images based on silicon nanoparticles that host low-order electric and magnetic Mie resonances. The interplay between the electric and magnetic resonances leads to a large palette of colors. This all-dielectric fabrication technique offers the advantage to use cost-effective, reliable, and sustainable materials to provide vivid color spanning the whole visible spectrum. The interest and potential of this all-dielectric printing technique are highlighted by reproducing at a micrometer scale a Mondrian painting.

Optimized 2D array of thin silicon pillars for efficient antireflective coatings in the visible spectrum.

Light reflection occuring at the surface of silicon wafers is drastically diminished by etching square pillars of height 110 nm and width 140 nm separated by a 100 nm gap distance in a square lattice. The design of the nanostructure is optimized to widen the spectral tolerance of the antireflective coatings over the visible spectrum for both fundamental polarizations. Angle and polarized resolved optical measurements report a light reflection remaining under 5% when averaged in the visible spectrum for both polarizations in a wide angular range. Light reflection remains almost insensitive to the light polarization even in oblique incidence.