Pol Van Dorpe

Symmetry Breaking in Plasmonic Nanocavities : Subradiant LSPR Sensing and a Tunable Fano Resonance

A metallic nanostructure consisting of a disk inside a thin ring supports superradiant and very narrow subradiant modes. Symmetry breaking in this structure enables a coupling between plasmon modes of differing multipolar order, resulting in a tunable Fano resonance. The LSPR sensitivities of the subradiant and Fano resonances are predicted to be among the largest yet for individual nanostructures.

Fano Resonances in Individual Coherent Plasmonic Nanocavities

We observe the appearance of Fano resonances in the optical response of plasmonic nanocavities due to the coherent coupling between their superradiant and subradiant plasmon modes. Two reduced-symmetry nanostructures probed via confocal spectroscopy, a dolmen-style slab arrangement and a ring/disk dimer, clearly exhibit the strong polarization and geometry dependence expected for this behavior at the individual nanostructure level, confirmed by full-field electrodynamic analysis of each structure. In each case, multiple Fano resonances occur as structure size is increased.

Tunability of Subradiant Dipolar and Fano-Type Plasmon Resonances in Metallic Ring/Disk Cavities: Implications for Nanoscale Optical Sensing

Plasmonic nanocavities consisting of the concentric arrangement of a disk and a ring sustain both subradiant and superradiant dipolar plasmon modes with large associated field enhancements and high refractive index sensitivities. In structures with broken symmetry, additionally a highly tunable Fano interference feature appears, which can be explained with a simple analytical harmonic oscillator model. The spectral tunability of these resonances from the visible to the mid-infrared is investigated, highlighting a potential for applications in surface enhanced spectroscopies.

Plasmonic Nanoclusters: Near Field Properties of the Fano Resonance Interrogated with SERS

While the far field properties of Fano resonances are well-known, clusters of plasmonic nanoparticles also possess Fano resonances with unique and spatially complex near field properties. Here we examine the near field properties of individual Fano resonant plasmonic clusters using surface-enhanced Raman scattering (SERS) both from molecules distributed randomly on the structure and from dielectric nanoparticles deposited at specific locations within the cluster. Cluster size, geometry, and interparticle spacing all modify the near field properties of the Fano resonance. For molecules, the spatially dependent SERS response obtained from near field calculations correlates well with the relative SERS intensities observed for individual clusters and for specific Stokes modes of a para-mercaptoaniline adsorbate. In all cases, the largest SERS enhancement is found when both the excitation and the Stokes shifted wavelengths overlap the Fano resonances. In contrast, for SERS from carbon nanoparticles we find that the dielectric screening introduced by the nanoparticle can drastically redistribute the field enhancement associated with the Fano resonance and lead to a significantly modified SERS response compared to what would be anticipated from the bare nanocluster.

Plasmon Line Shaping Using Nanocrosses for High Sensitivity Localized Surface Plasmon Resonance Sensing

The detection of small changes in the wavelength position of localized surface plasmon resonances in metal nanostructures has been used successfully in applications such as label-free detection of biomarkers. Practical implementations, however, often suffer from the large spectral width of the plasmon resonances induced by large radiative damping in the metal nanocavities. By means of a tailored design and using a reproducible nanofabrication process, high quality planar gold plasmonic nanocavities are fabricated with strongly reduced radiative damping. Moreover, additional substrate etching results in a large enhancement of the sensing volume and a subsequent increase of the sensitivity. Coherent coupling of bright and dark plasmon modes in a nanocross and nanobar is used to generate high quality factor subradiant Fano resonances. Experimental sensitivities for these modes exceeding 1000 nm/RIU with a Figure of Merit reaching 5 are demonstrated in microfluidic ensemble spectroscopy.

Experimental Realization of Subradiant, Superradiant, and Fano Resonances in Ring/Disk Plasmonic Nanocavities

Subradiant and superradiant plasmon modes in concentric ring/disk nanocavities are experimentally observed. The subradiance is obtained through an overall reduction of the total dipole moment of the hybridized mode due to antisymmetric coupling of the dipole moments of the parent plasmons. Multiple Fano resonances appear within the superradiant continuum when structural symmetry is broken via a nanometric displacement of the disk, due to coupling with higher order ring modes. Both subradiant modes and Fano resonances exhibit substantial reductions in line width compared to the parent plasmon resonances, opening up possibilities in optical and near IR sensing via plasmon line shape design.

Enhanced Optical Trapping and Arrangement of Nano-Objects in a Plasmonic Nanocavity

Gentle manipulation of micrometer-sized dielectric objects with optical forces has found many applications in both life and physical sciences. To further extend optical trapping toward the true nanometer scale, we present an original approach combining self-induced back action (SIBA) trapping with the latest advances in nanoscale plasmon engineering. The designed resonant trap, formed by a rectangular plasmonic nanopore, is successfully tested on 22 nm polystyrene beads, showing both single- and double-bead trapping events. The mechanism responsible for the higher stability of the double-bead trapping is discussed, in light of the statistical analysis of the experimental data and numerical calculations. Furthermore, we propose a figure of merit that we use to quantify the achieved trapping efficiency and compare it to prior optical nanotweezers. Our approach may open new routes toward ultra-accurate immobilization and arrangement of nanoscale objects, such as biomolecules.

Fluorescence near gold nanoparticles for DNA sensing.

We investigated fluorescence quenching and enhancement near gold nanoparticles (GNP) of various sizes using fluorescently labeled hairpin DNA probes of different lengths. A closed hairpin caused intimate contact between the fluorophore and the gold, resulting in an efficient energy transfer (quenching). Upon hybridization with complementary DNA, the DNA probes were stretched yielding a strong increase in fluorescence signal. By carefully quantifying the amount of bound fluorescent probes and the GNP concentrations, we were able to determine the quenching and enhancement efficiencies. We also studied the size and distance dependence theoretically, using both FDTD simulations and the Gersten-Nitzan model and obtained a good agreement between experiments and theory. On the basis of experimental and theoretical studies, we report over 96.8% quenching efficiency for all particle sizes tested and a maximal signal increase of 1.23 after DNA hybridization. The described results also demonstrate the potential of gold nanoparticles for label free DNA sensing.

Boosting the figure-of-merit of LSPR-based refractive index sensing by phase-sensitive measurements.

Localized surface plasmon resonances possess very interesting properties for a wide variety of sensing applications. In many of the existing applications, only the intensity of the reflected or transmitted signals is taken into account, while the phase information is ignored. At the center frequency of a (localized) surface plasmon resonance, the electron cloud makes the transition between in- and out-of-phase oscillation with respect to the incident wave. Here we show that this information can experimentally be extracted by performing phase-sensitive measurements, which result in linewidths that are almost 1 order of magnitude smaller than those for intensity based measurements. As this phase change is an intrinsic property of a plasmon resonance, this opens up many possibilities for boosting the figure-of-merit (FOM) of refractive index sensing by taking into account the phase of the plasmon resonance. We experimentally investigated this for two model systems: randomly distributed gold nanodisks and gold nanorings on top of a continuous gold layer and a dielectric spacer and observed FOM values up to 8.3 and 16.5 for the respective nanoparticles.

Fabrication, Characterization, and Optical Properties of Gold Nanobowl Submonolayer Structures

We report on a versatile method to fabricate hollow gold nanobowls and complex gold nanobowls (with a core) based on an ion milling and a vapor HF etching technique. Two different sized hollow gold nanobowls are fabricated by milling and etching submonolayers of gold nanoshells deposited on a substrate, and their sizes and morphologies are characterized by scanning electron microscopy (SEM) and atomic force microscopy (AFM). Optical properties of hollow gold nanobowls with different sizes are investigated experimentally and theoretically, showing highly tunable plasmon resonance ranging from the visible to the near-infrared region. Additionally, finite difference time domain (FDTD) calculations show an enhanced localized electromagnetic field around hollow gold nanobowl structures, which indicates a potential application in surface-enhanced Raman scattering (SERS) spectroscopy for biomolecular detection. Finally, we demonstrate the fabrication of complex gold nanobowls with a gold nanoparticle core which offers the capability to create plasmon hybridized nanostructures.