Thomas Siegfried

Plasmonic Radiance: Probing Structure at the Ångström Scale with Visible Light

Plasmonic modes with long radiative lifetimes combine strong nanoscale light confinement with a narrow spectral line width carrying the signature of Fano resonances, making them very promising for nanophotonic applications such as sensing, lasing, and switching. Their coupling to incident radiation, also known as radiance, determines their optical properties and optimal use in applications. In this work, we theoretically and experimentally demonstrate that the radiance of a plasmonic mode can be classified into three different regimes. In the weak coupling regime, the line shape exhibits remarkable sensitivity to the dielectric environment. We show that geometrical displacements and deformations at the Ångström scale can be detected optically by measuring the radiance. In the intermediate regime, the electromagnetic energy stored in the mode is maximal, with large electric field enhancements that can be exploited in surface enhanced spectroscopy applications. In the strong coupling regime, the interaction can result in hybridized modes with tunable energies.

Fabrication of sub-10 nm gap arrays over large areas for plasmonic sensors

We report a high-throughput method for the fabrication of metallic nanogap arrays with high-accuracy over large areas. This method, based on shadow evaporation and interference lithography, achieves sub-10 nm gap sizes with a high accuracy of ±1.5 nm. Controlled fabrication is demonstrated over mm2 areas and for periods of 250 nm. Experiments complemented with numerical simulations indicate that the formation of nanogaps is a robust, self-limiting process that can be applied to wafer-scale substrates. Surface-enhanced Raman scattering (SERS) experiments illustrate the potential for plasmonic sensing with an exceptionally low standard-deviation of the SERS signal below 3% and average enhancement factors exceeding 1 × 106.

Gap Plasmons and Near-Field Enhancement in Closely Packed Sub-10 nm Gap Resonators

Pairs of metal nanoparticles with a sub-10 nm gap are an efficient way to achieve extreme near-field enhancement for sensing applications. We demonstrate an attractive alternative based on Fabry-Perot type nanogap resonators, where the resonance is defined by the gap width and vertical elongation instead of the particle geometry. We discuss the crucial design parameters for such gap plasmons to produce maximum near-field enhancement for surface-enhanced Raman scattering and show compatibility of the pattern processing with low-cost and low-resolution lithography. We find a minimum critical metal thickness of 80 nm and observe that the mode coupling from the far field increases by tapering the gap opening. We also show the saturation of the Raman signal for nanogap periodicities below 1 μm, demonstrating efficient funneling of light into such nanogap arrays.

Engineering Metal Adhesion Layers That Do Not Deteriorate Plasmon Resonances

Adhesion layers, required to stabilize metallic nanostructures, dramatically deteriorate the performances of plasmonic sensors, by severely damping the plasmon modes. In this article, we show that these detrimental effects critically depend on the overlap of the electromagnetic near-field of the resonant plasmon mode with the adhesion layer and can be minimized by careful engineering of the latter. We study the dependence of the geometrical parameters such as layer thickness and shape on the near-field of localized plasmon resonances for traditional adhesion layers such as Cr, Ti, and TiO2. Our experiments and simulations reveal a strong dependence of the damping on the layer thickness, in agreement with the exponential decay of the plasmon near-field. We developed a method to minimize the damping by selective deposition of thin adhesion layers (<1 nm) in a manner that prevents the layer to overlap with the hotspots of the plasmonic structure. Such a designed structure enables the use of standard Cr and Ti adhesion materials to fabricate robust plasmonic sensors without deteriorating their sensitivity.

Metal Double Layers with Sub-10 nm Channels

Double-layer plasmonic nanostructures are fabricated by depositing metal at normal incidence onto various resist masks, forming an antenna layer on top of the resist post and a hole layer on the substrate. Antenna plasmon resonances are found to couple to the hole layer, inducing image charges which enhance the near-field for small layer spacings. For continued evaporation above the resist height, a sub-10 nm gap channel develops due to a self-aligned process and a minimal undercut of the resist sidewall. For such double layers with nanogap channels, the average surface-enhanced Raman scattering intensity is improved by a factor in excess of 60 in comparison to a single-layer antenna with the same dimensions. The proposed design principle is compatible with low-cost fabrication, straightforward to implement, and applicable over large areas. Moreover, it can be applied for any particular antenna shape to improve the signals in surface-enhanced spectroscopy applications.

Fano resonant plasmonic systems: Functioning principles and applications

Keywords: Nanophotonics ; Plasmonics Reference EPFL-CONF-187056 Record created on 2013-06-17, modified on 2017-05-10

Large-scale sub-100 nm compound plasmonic grating arrays to control the interaction between localized and propagating plasmons

Abstract. Compound plasmonic resonances arise due to the interaction between discrete and continuous metallic nanostructures. Such combined nanostructures provide a versatility and tunability beyond that of most other metallic nanostructures. In order to observe such resonances and their tunability, multiple nanostructure arrays composed of periodic metallic gratings of varying width and an underlying metallic film should be studied. Large-area compound plasmonic structures composed of various Au grating arrays with sub-100 nm features spaced nanometers above an Au film were fabricated using extreme ultraviolet interference lithography. Reflection spectra, via both numerical simulations and experimental measurements over a wide range of incidence angles and excitation wavelengths, show the existence of not only the usual propagating and localized plasmon resonances, but also compound plasmonic resonances. These resonances exhibit not only propagative features, but also a spectral evolution with varying grating width. Additionally, a reduction of the width of the grating elements results in coupling with the localized dipolar resonance of the grating elements and thus plasmon hybridization. This newly acquired perspective on the various interactions present in such a plasmonic system will aid in an increased understanding of the mechanisms at play when designing plasmonic structures composed of both discrete and continuous elements.

Surface second harmonic generation from sub-10 nm gap plasmonic gratings

Sub-10 nm gap plasmonic gratings are experimentally studied for second harmonic generation (SHG) and a model is developed to explain the optimum in transmitted SHG, showing the interplay between the grating width and field enhancement.

Large area periodic nanogap arrays for Raman and fluorescence enhancement: Modeling and performance

We will discuss the use of dense periodic nanogap arrays for plasmonic sensing applications. A high-throughput fabrication process will be presented, that yields nanogap arrays with periodicities above 150 nm, and with accurately controlled gap widths of ±1.5 nm over mm2 large areas.

Minimizing quenching of plasmonic sensors caused by adhesion layers

Adhesion layers necessary for the robustness of plasmonic sensors are commonly used at dimensions where the electric near-field intensity can be strongly quenched. We have found that by minimizing the layer thickness to roughly 0.5 nm and by additionally controlling the geometric design of the layer, quenching can by reduced by a factor of up to 7.