Significant augmentation of second harmonic generation using Fano resonances in plasmonic heptamers made of silver is theoretically and experimentally demonstrated. The geometry is engineered to ...simultaneously produce a Fano resonance at the fundamental wavelength, resulting in a strong localization of the fundamental field close to the system, and a higher order scattering peak at the second harmonic wavelength. These results illustrate the versatility of Fano resonant structures to engineer specific optical responses both in the linear and nonlinear regimes thus paving the way for future investigations on the role of dark modes in nonlinear and quantum optics.
The optical properties of plasmonic nanostructures supporting Fano resonances are investigated with an electromagnetic theory. Contrary to the original work of Fano, this theory includes losses in ...the materials composing the system. As a result, a more general formula is obtained for the response of the system and general conclusions for the determination of the resonance parameters are drawn. These predictions are verified with surface integral numerical calculations in a broad variety of plasmonic nanostructures including dolmens, oligomers, and gratings. This work presents a robust and consistent analysis of plasmonic Fano resonances and enables the control of their line shape based on Maxwell’s equations. The insights into the physical understanding of Fano resonances gained this way will be of great interest for the design of plasmonic systems with specific spectral responses for applications such as sensing and optical metamaterials.
Fano resonances in hybridized systems formed from the interaction of bright modes only are reported. Despite precedent works, we demonstrate theoretically and experimentally that Fano resonances can ...be obtained by destructive interference between two bright dipolar modes out of phase. A simple oscillator model is provided to predict and fit the far-field scattering. The predictions are verified with numerical calculations using a surface integral equation method for a wide range of geometrical parameters. The validity of the model is then further demonstrated with experimental dark-field scattering measurements on actual nanostructures in the visible range. A remarkable set of properties like crossings, avoided crossings, inversion of subradiant and superradiant modes and a plasmonic equivalent of a bound state in the continuum are presented. The nanostructure, that takes advantage of the combination of Fano resonance and nanogap effects, also shows high tunability and strong near-field enhancement. Our study provides a general understanding of Fano resonances as well as a simple tool for engineering their spectral features.
Predetermined and selective placement of nanoparticles onto large-area substrates with nanometre-scale precision is essential to harness the unique properties of nanoparticle assemblies, in ...particular for functional optical and electro-optical nanodevices. Unfortunately, such high spatial organization is currently beyond the reach of top-down nanofabrication techniques alone. Here, we demonstrate that topographic features comprising lithographed funnelled traps and auxiliary sidewalls on a solid substrate can deterministically direct the capillary assembly of Au nanorods to attain simultaneous control of position, orientation and interparticle distance at the nanometre level. We report up to 100% assembly yield over centimetre-scale substrates. We achieve this by optimizing the three sequential stages of capillary nanoparticle assembly: insertion of nanorods into the traps, resilience against the receding suspension front and drying of the residual solvent. Finally, using electron energy-loss spectroscopy we characterize the spectral response and near-field properties of spatially programmable Au nanorod dimers, highlighting the opportunities for precise tunability of the plasmonic modes in larger assemblies.
Plasmonics has emerged as an important research field in nanoscience and nanotechnology. Recently, significant attention has been devoted to the observation and the understanding of nonlinear optical ...processes in plasmonic nanostructures, giving rise to the new research field called nonlinear plasmonics. This review provides a comprehensive insight into the physical mechanisms of one of these nonlinear optical processes, namely, second harmonic generation (SHG), with an emphasis on the main differences with the linear response of plasmonic nanostructures. The main applications, ranging from the nonlinear optical characterization of nanostructure shapes to the optimization of laser beams at the nanoscale, are summarized and discussed. Future directions and developments, made possible by the unique combination of SHG surface sensitivity and field enhancements associated with surface plasmon resonances, are also addressed.
The optical trapping of Au nanoparticles with dimensions as small as 10 nm in the gap of plasmonic dipole antennas is demonstrated. Single nanoparticle trapping events are recorded in real time by ...monitoring the Rayleigh scattering spectra of individual plasmonic antennas. Numerical simulations are also performed to interpret the experimental results, indicating the possibility to trap nanoparticles only a few nanometers in size. This work unveils the potential associated with the integration of plasmonic trapping with localized surface plasmon resonance based sensing techniques, in order to deliver analyte to specific, highly sensitive regions (“hot spots”).
Plasmonic effects associated with metallic nanostructures have been widely studied for color generation. It became apparent that highly saturated and bright colors are hard to obtain, and very small ...nanostructures need to be fabricated. To address this issue, in this study, we employ metal–insulator–metal sandwich nanodisks that support enhanced in-phase electric dipole modes, which are blue-shifted with respect to a single metal disk. The blue shift enables the generation of short wavelength colors with larger nanostructures. The radiation modes hybridize with the Wood’s anomaly in periodic structures, creating narrow and high-resonance peaks in the reflection and deep valleys in the transmission spectra, thus producing vivid complementary colors in both cases. Full colors can be achieved by tuning the radius of the nanodisks and the periodicity of the arrays. Good agreement between simulations and experiments is demonstrated and analyzed in CIE1931, sRGB, and HSV color spaces. The presented method has potential for applications in imaging, data storage, ultrafine displays, and plasmon-based biosensors.
We investigate optical second-harmonic generation (SHG) from metasurfaces where noncentrosymmetric V-shaped gold nanoparticles are ordered into regular array configurations. In contrast to ...expectations, a substantial enhancement of the SHG signal is observed when the number density of the particles in the array is reduced. More specifically, by halving the number density, we obtain over 5-fold enhancement in SHG intensity. This striking result is attributed to favorable interparticle interactions mediated by the lattice, where surface-lattice resonances lead to spectral narrowing of the plasmon resonances. Importantly, however, the results cannot be explained by the improved quality of the plasmon resonance alone. Instead, the lattice interactions also lead to further enhancement of the local fields at the particles. The experimental observations agree very well with results obtained from numerical simulations including lattice interactions.
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.