A novel resonant mechanism involving the interference of a broadband plasmon with the narrowband vibration from molecules is presented. With the use of this concept, we demonstrate experimentally the enormous enhancement of the vibrational signals from less than one attomol of molecules on individual gold nanowires, tailored to act as plasmonic nanoantennas in the infrared. By detuning the resonance via a change in the antenna length, a Fano-type behavior of the spectral signal is observed, which is clearly supported by full electrodynamical calculations. This resonant mechanism can be a new paradigm for sensitive infrared identification of molecular groups.
High-permittivity dielectric particles with resonant magnetic properties are being explored as constitutive elements of new metamaterials and devices. Magnetic properties of low-loss dielectric nanoparticles in the visible or infrared are not expected due to intrinsic low refractive index of optical media in these regimes. Here we analyze the dipolar electric and magnetic response of lossless dielectric spheres made of moderate permittivity materials. For low material refractive index (<∼3) there are no sharp resonances due to strong overlapping between different multipole contributions. However, we find that Silicon particles with index of refraction∼3.5 and radius∼200 nm present strong electric and magnetic dipolar resonances in telecom and near-infrared frequencies, (i.e. at wavelengths≈1.2-2 mm) without spectral overlap with quadrupolar and higher order resonances. The light scattered by these Si particles can then be perfectly described by dipolar electric and magnetic fields.
The plasmon resonances of two closely spaced metallic particles have enabled applications including single-molecule sensing and spectroscopy, novel nanoantennas, molecular rulers, and nonlinear optical devices. In a classical electrodynamic context, the strength of such dimer plasmon resonances increases monotonically as the particle gap size decreases. In contrast, a quantum mechanical framework predicts that electron tunneling will strongly diminish the dimer plasmon strength for subnanometer-scale separations. Here, we directly observe the plasmon resonances of coupled metallic nanoparticles as their gap size is reduced to atomic dimensions. Using the electron beam of a scanning transmission electron microscope (STEM), we manipulate pairs of ~10-nm-diameter spherical silver nanoparticles on a substrate, controlling their convergence and eventual coalescence into a single nanosphere. We simultaneously employ electron energy-loss spectroscopy (EELS) to observe the dynamic plasmonic properties of these dimers before and after particle contact. As separations are reduced from 7 nm, the dominant dipolar peak exhibits a redshift consistent with classical calculations. However, gaps smaller than ~0.5 nm cause this mode to exhibit a reduced intensity consistent with quantum theories that incorporate electron tunneling. As the particles overlap, the bonding dipolar mode disappears and is replaced by a dipolar charge transfer mode. Our dynamic imaging, manipulation, and spectroscopy of nanostructures enables the first full spectral mapping of dimer plasmon evolution and may provide new avenues for in situ nanoassembly and analysis in the quantum regime.
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