Large Fluorescence Enhancement via Lossless All-Dielectric Spherical Mesocavities.

Nano- and microparticles are popular media to enhance optical signals, including fluorescence from a dye proximal to the particle. Here we show that homogeneous, lossless, all-dielectric spheres with diameters in the mesoscale range, between nano- (≲100 nm) and micro- (≳1 μm) scales, can offer surprisingly large fluorescence enhancements, up to ∼ 10. With the absence of nonradiative Ohmic losses inherent to plasmonic particles, we show that can increase, decrease or even stay the same with increasing intrinsic quantum yield , for suppressed, enhanced or intact radiative decay rates of a fluorophore, respectively.

Thermal degradation of optical resonances in plasmonic nanoparticles.

The dependence of plasmon resonance excitations in ultrafine (3-7 nm) gold nanoparticles on heating and melting is investigated. An integrated approach is adopted, where molecular dynamics simulations of the spatial and temporal development of the atoms constituting the nanoparticles generate trajectories out of which system conformations are sampled and extracted for calculations of plasmonic excitation cross sections which then are averaged over the sample configurations for the final result. The calculations of the plasmonic excitations, which take into account the temperature- and size-dependent relaxation of the plasmons, are carried out with a newly developed Extended Discrete Interaction Model (Ex-DIM) and complemented by multilayered Mie theory.

Atomistic description of plasmonic generation in alloys and core shell nanoparticles.

Using the extended discrete interaction model we investigate the tunabilty of surface plasmon resonances in alloys and core-shell nanoparticles made from silver and gold in the small (1-15 nm) nanoscale regime where classical models based on the bulk dielectric constant may not apply. We show that the surface plasmon resonance of these alloys and core-shell particles to a large extent follow Vegard's law irrespective of the geometry of the nanoparticle. The evolution of the polarizability with size demonstrates a highly non-linear behaviour of the polarizability with the ratio of the constituents and geometry in alloys and core-shell nanoparticles, with the exception of the longitudinal surface plasmon resonance in nanorods and, partly, nanodisc alloys.

Plasmonic nano-shells: atomistic discrete interaction versus classic electrodynamics models.

Using the extended discrete interaction model and Mie theory, we investigate the tunability of the optical polarizability of small metallic nano-shells. We show that the spectral positions of symmetric and antisymmetric dipolar plasmon resonances vary with the ratio of particle radius to hole radius in a manner similar to one predicted for uniform metallic nano-shells using a semiclassical approach of two coupled harmonic oscillators. We show that, according to the extended discrete interaction model, the dipolar plasmon resonances are also present for nano-shells in the 2-13 nm size region and show the same functional dependence seen for larger nano-shells.

Engineering novel tunable optical high-Q nanoparticle array filters for a wide range of wavelengths.

The interaction of non-monochromatic radiation with arrays comprising plasmonic and dielectric nanoparticles has been studied using the finite-difference time-domain electrodynamics method. It is shown that LiNbO, TiO, GaAs, Si, and Ge all-dielectric nanoparticle arrays can provide a complete selective reflection of an incident plane wave within a narrow spectral line of collective lattice resonance with a Q-factor of 10 or larger at various spectral ranges, while plasmonic refractory TiN and chemically stable Au nanoparticle arrays provide high-Q resonances with moderate reflectivity. Arrays with fixed dimensional parameters make it possible to fine-tune the position of a selected resonant spectral line by tilting the array relative to the direction of the incident radiation.

Collective lattice resonances in arrays of dielectric nanoparticles: a matter of size.

Collective lattice resonances (CLRs) in finite-sized $ 2D $2D arrays of dielectric nanospheres have been studied via the coupled dipole approximation. We show that even for sufficiently large arrays, up to $ 100 \times 100 $100×100 nanoparticles (NPs), electric or magnetic dipole CLRs may differ significantly from the ones calculated for infinite arrays with the same NP sizes and interparticle distances. The discrepancy is explained by the existence of a sufficiently strong cross-interaction between electric and magnetic dipoles induced at NPs in finite-sized lattices, which is ignored for infinite arrays.