Engineering Near-Field SEIRA Enhancements in Plasmonic Resonators.
ABSTRACT: Engineering of the optical resonances in plasmonic resonators arrays is achieved by virtue of the intrinsic properties to the constituent structures such as composition, size and shape and by controlling the inter-resonator interactions by of virtue the array geometrical arrangement. The nanoscale confinement of the plasmonic field enhances light-matter interactions enabling, for instance, the surface enhanced infrared absorption (SEIRA) effect. However, the subwavelength confinement also poses an experimental challenge for discriminating the response stemming from the individual resonators and from the collective response in densely packed arrays. In this work, the photothermal induced resonance (PTIR) technique is leveraged to obtain nanoscale images and spectra of near-field SEIRA hot spots observed in isolated plasmonic resonators of different shapes and in selected resonators within closely packed plasmonic arrays informing on whether the interactions with neighboring resonators are beneficial or otherwise. Results are correlated with far-field spectra and theoretical calculations.
Project description:Localizing light to nanoscale volumes through nanoscale resonators that are low loss and precisely tailored in spectrum to properties of matter is crucial for classical and quantum light sources, cavity QED, molecular spectroscopy, and many other applications. To date, two opposite strategies have been identified: to use either plasmonics with deep subwavelength confinement yet high loss and very poor spectral control or instead microcavities with exquisite quality factors yet poor confinement. In this work we realize hybrid plasmonic-photonic resonators that enhance the emission of single quantum dots, profiting from both plasmonic confinement and microcavity quality factors. Our experiments directly demonstrate how cavity and antenna jointly realize large cooperative Purcell enhancements through interferences. These can be controlled to engineer arbitrary Fano lineshapes in the local density of optical states.
Project description:Enhanced light-matter interactions are the basis of surface-enhanced infrared absorption (SEIRA) spectroscopy, and conventionally rely on plasmonic materials and their capability to focus light to nanoscale spot sizes. Phonon polariton nanoresonators made of polar crystals could represent an interesting alternative, since they exhibit large quality factors, which go far beyond those of their plasmonic counterparts. The recent emergence of van der Waals crystals enables the fabrication of high-quality nanophotonic resonators based on phonon polaritons, as reported for the prototypical infrared-phononic material hexagonal boron nitride (h-BN). In this work we use, for the first time, phonon-polariton-resonant h-BN ribbons for SEIRA spectroscopy of small amounts of organic molecules in Fourier transform infrared spectroscopy. Strikingly, the interaction between phonon polaritons and molecular vibrations reaches experimentally the onset of the strong coupling regime, while numerical simulations predict that vibrational strong coupling can be fully achieved. Phonon polariton nanoresonators thus could become a viable platform for sensing, local control of chemical reactivity and infrared quantum cavity optics experiments.
Project description:Arrays of sub-wavelength, sub-10?nm air-gap plasmonic ring resonators are fabricated using nanoimprinting. In near infra-red (NIR) range, the resonator supports a single dipole mode which is excited and identified via simple normal illumination and explored through transmission measurements. By controlling both lateral and vertical confinement via a metal edge, the mode volume is successfully reduced down to 1.3?×?10(-5) ?0(3). The advantage of such mode confinement is demonstrated by applying the resonators biosensing. Using bovine serum albumin (BSA) molecules, a dramatic enhancement of surface sensitivity up to 69?nm/nm is achieved as the modal height approaches the thickness of the adsorbed molecule layers.
Project description:We demonstrate parallel transduction of thermally driven mechanical motion of an array of gold-coated silicon nitride nanomechanical beams, by using near-field confinement in plasmonic metal-insulator-metal resonators supported in the gap between the gold layers. The free-space optical readout, enabled by the plasmonic resonances, allows for addressing multiple mechanical resonators in a single measurement. Light absorbed in the metal layer of the beams modifies their mechanical properties, allowing photothermal tuning of the eigenfrequencies. The appearance of photothermally driven parametric amplification indicates the possibility of plasmonic mechanical actuation.
Project description:Photothermal induced resonance (PTIR), also known as AFM-IR, is a scanning probe technique that provides sample composition information with a lateral resolution down to 20 nm. Interest in PTIR stems from its ability to identify unknown samples at the nanoscale thanks, in first approximation, to the direct comparability of PTIR spectra with far-field infrared databases. The development of rapidly tuning quantum cascade lasers has increased the PTIR throughput considerably, making nanoscale hyperspectral imaging within a reasonable time frame possible. Consequently, a better understanding of PTIR signal generation and of the fine details of PTIR analysis has become of paramount importance for extending complex IR analysis methods developed in the far-field, e.g., for classification and hyperspectral imaging, to nanoscale PTIR spectra. Here we calculate PTIR spectra via thin-film optics, to identify subtle changes (band shifts, deviation from linear approximation, etc.) for common sample parameters in the case of PTIR with total internal reflection illumination. Results show signal intensity linearity and small band shifts as long as the sample is prepared correctly, with band shifts typically smaller than macroscale attenuated total reflection (ATR) spectroscopy. Finally, a generally applicable algorithm to retrieve the pure imaginary component of the refractive index (i.e., the chemically specific information) is provided to overcome the PTIR spectra nonlinearity.
Project description:Plasmonic structures can provide deep-subwavelength electromagnetic fields that are useful for enhancing light-matter interactions. However, because these localized modes are also dissipative, structures that offer the best compromise between field confinement and loss have been sought. Metallic wedge waveguides were initially identified as an ideal candidate but have been largely abandoned because to date their experimental performance has been limited. We combine state-of-the-art metallic wedges with integrated reflectors and precisely placed colloidal quantum dots (down to the single-emitter level) and demonstrate quantum-plasmonic waveguides and resonators with performance approaching theoretical limits. By exploiting a nearly 10-fold improvement in wedge-plasmon propagation (19 ?m at a vacuum wavelength, ?vac, of 630 nm), efficient reflectors (93%), and effective coupling (estimated to be >70%) to highly emissive (~90%) quantum dots, we obtain Ag plasmonic resonators at visible wavelengths with quality factors approaching 200 (3.3 nm line widths). As our structures offer modal volumes down to ~0.004?vac(3) in an exposed single-mode waveguide-resonator geometry, they provide advantages over both traditional photonic microcavities and localized-plasmonic resonators for enhancing light-matter interactions. Our results confirm the promise of wedges for creating plasmonic devices and for studying coherent quantum-plasmonic effects such as long-distance plasmon-mediated entanglement and strong plasmon-matter coupling.
Project description:We investigated nonlinear photoemission from plasmonic films with femtosecond, mid-infrared pulses at 3.1??m wavelength. Transition between regimes of multi-photon-induced and tunneling emission is demonstrated at an unprecedentedly low intensity of <1?GW/cm(2). Thereby, strong-field nanophysics can be accessed at extremely low intensities by exploiting nanoscale plasmonic field confinement, enhancement and ponderomotive wavelength scaling at the same time. Results agree well with quantum mechanical modelling. Our scheme demonstrates an alternative paradigm and regime in strong-field physics.
Project description:Fano resonance refers to an interference between localized and continuum states that was firstly reported for atomic physics and solid-state quantum devices. In recent years, Fano interference gained more and more attention for its importance in metamaterials, nanoscale photonic devices, plasmonic nanoclusters and surface-enhanced Raman scattering (SERS). Despite such interest in nano-optics, no experimental evidence of Fano interference was reported up to now for purely nanomechanical resonators, even if classical mechanical analogies were referred from a theoretical point of view. Here we demonstrate for the first time that harmonic nanomechanical resonators with relatively high quality factors, such as cantilevers vibrating in vacuum, can show characteristic Fano asymmetric curves when coupled in arrays. The reported findings open new perspectives in fundamental aspects of classical nanomechanical resonators and pave the way to a new generation of chemical and biological nanoresonator sensors with higher parallelization capability.
Project description:Metamaterials and plasmonics are powerful tools for unconventional manipulation and harnessing of light. Metamaterials can be engineered to possess intriguing properties lacking in natural materials, such as negative refractive index. Plasmonics offers capabilities of confining light in subwavelength dimensions and enhancing light-matter interactions. Recently, the technological potential of graphene-based plasmonics has been recognized as the latter features large tunability, higher field-confinement and lower loss compared with metal-based plasmonics. Here, we introduce hybrid structures comprising graphene plasmonic resonators coupled to conventional split-ring resonators, thus demonstrating a type of highly tunable metamaterial, where the interaction between the two resonances reaches the strong-coupling regime. Such hybrid metamaterials are employed as high-speed THz modulators, exhibiting ?60% transmission modulation and operating speed in excess of 40?MHz. This device concept also provides a platform for exploring cavity-enhanced light-matter interactions and optical processes in graphene plasmonic structures for applications including sensing, photo-detection and nonlinear frequency generation.
Project description:Plasmonic superlattice membrane exhibits remarkable functional properties that are emerging from engineered assemblies of well-defined "meta-atoms," which is featured as a conceptual new category of two-dimensional optical metamaterials. The ability to build plasmonic membranes over macroscopic surfaces but with nanoscale ordering is crucial for systematically controlling the light-matter interactions and represents considerable advances for the bottom-up fabrication of soft optoelectronic devices and circuits. Through rational design, novel nanocrystals, and by engineering the packing orders, the hybridized plasmon signature can be customized, promoting controllable near-field confinement for surface-enhanced Raman scattering (SERS) based detection. However, building such 2D architectures has proven to be remarkably challenging due to the complicated interparticle forces and multiscale interactions during self-assembly. Here, we report on the fabrication of ultralong-nanobrick-based giant plasmonic superlattice membranes as high-performance SERS substrates for ultrasensitive and label-free protein detection. Using aspect-ratio controllable short-to-ultralong nanobricks as building blocks, we construct three distinctive plasmonic membranes by polymer-ligand-based strategy in drying-mediated self-assembly at the air/water interfaces. The plasmonic membranes exhibit monolayered morphology with nanoscale assembled ordering but macroscopic lateral dimensions, inducing enhanced near-field confinement and uniform hot-spot distribution. By choosing 4-aminothiophenol and bovine serum albumin (BSA) as a model analyte, we establish an ultrasensitive assay for label-free SERS detection. The detection limit of BSA can reach 15 nM, and the enhancement factor reached 4.3 × 105, enabling a promising avenue for its clinical application in ultrasensitive biodiagnostics.