In this Letter, we demonstrate a reversible strong coupling regime between a dipolar surface plasmon resonance and a molecular excited state. This reversible state is experimentally observed on silver nanoparticle arrays embedded in a polymer film containing photochromic molecules. Extinction measurements reveal a clear Rabi splitting of 294 meV, corresponding to ~13% of the molecular transition energy. We derived an analytical model to confirm our observations, and we emphasize the importance of spectrally matching the polymer absorption with the plasmonic resonance to observe coupled states. Finally, the reversibility of this coupling is illustrated by cycling the photochromic molecules between their two isomeric forms.

We present a new kind of UV-cured holographic grating that consists of polymer slices alternated with pure nematic films. By preventing the appearance of the nematic phase during the curing process, it is possible to avoid the formation of liquid-crystal droplets and obtain a sharp and uniform morphology, which reduces scattering losses and increases diffraction efficiency.

We present a detailed study on the resonant gain (RG) phenomena occurring in two nanostructures, in which the presence of dielectric singularities is used to reach a huge amplification of the emitted photons resonantly interacting with the system. The presence of gain molecules in the considered nanoresonator systems makes it possible to obtain optical features that are able to unlock several applications. Two noticeable cases have been investigated: a 1D nanoresonator based on hyperbolic metamaterials and a 3D metal/dielectric spherical multishell. The former has been designed in the framework of the effective medium theory, in order to behave as an epsilon-near-zero-and-pole metamaterial, showing extraordinary light confinement and collimation. Such a peculiarity represents the key to lead to a RG behavior, a condition in which the system is demonstrated to behave as a self-amplifying perfect lens. Very high enhancement and spectral sharpness of 1 nm of the emitted light are demonstrated by means of a transfer matrix method simulation. The latter system consists of a metal/doped-dielectric multishell. A dedicated theoretical approach has been set up to finely engineer its doubly tunable resonant nature. The RG condition has been demonstrated also in this case. Finite element method-based simulations, together with an analytical model, clarify the electric field distribution inside the multishell and suggest the opportunity to use this device as a self-enhanced loss compensated multishell, being a favorable scenario for low-threshold SPASER action. Counterintuitively, exceeding the resonant gain amount of molecules in both systems causes a significant drop in the amplitude of the resonance.

5 pagesInternational audienceWe study theoretically the polarizability of a single metallic nanoparticle immersed into an externally pumped, active gain medium able to couple to the plasmon resonance. Within the frame of a simple long-wavelength, macroscopic description, and under steady-state conditions, we show that localized plasmons can be strongly amplified, until becoming singular for a specific amount of surrounding gain; however, we find that such gain-assisted singular plasmons exhibit spectrally spread imaginary responses and are therefore intrinsically different from singular plasmons in idealized, lossless metals. More generally, we carry a systematic study of how the plasmonic response transforms under changes in the amount of gain, and show that the coupled particle and activemedium act as a self-tuned Fano resonant system. The resulting plasmons exhibit strongly distorted line shapes with unusual but interesting features. One particularly attractive situation is that of "conjugate plasmons," which, at resonance, display a strong real response in association with minimal losses. These findings could have some applications in plasmonics, nanoantennas, nanosensing, and optical metamaterials

The plasmonic response of a metal nanoparticle in the presence of surrounding gain elements is studied, using a space and time-dependent model, which integrates a quantum formalism to describe the gain and a classical treatment for the metal. Our model fully takes into account the influence of the system geometry (nanosphere) and offers for the first time, the possibility to describe the temporal evolution of the fields and the coupling among the multipolar modes of the particle. We calculate the lasing threshold value for all multipoles of the spaser, and demonstrate that the dipolar one is lowest. The onset of the lasing instability, in the linear regime, is then studied both with and without external field forcing. We also study the behaviour of the system below the lasing threshold, with the external field, demonstrating the existence of an amplification regime where the nanoparticle’s plasmon is strongly enhanced as the threshold is approached. Finally, a qualitative discussion is provided on later, non-linear stages of the dynamics and the approach to the steady-state of the spaser; in particular, it is shown that, for the considered geometry, the spasing is necessarily multi-modal and multipolar modes are always activated.

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The last few years have seen a growing interest in the ability of metallic nanoparticles (MNPs) to control temperature at the nanoscale. Under a suitable optical radiation, MNPs feature an enhanced light absorption/scattering, thus turning into an ideal nano-source of heat, remotely controllable by means of light. In this framework, we report our recent efforts on modeling and characterizing the photo-thermal effects observed in gold nanoparticles (GNPs) dispersed in thermotropic Liquid Crystals (LCs). Photo-induced temperature variations in GNPs dispersed in Nematic LCs (NLCs) have been studied by implementing an ad hoc theoretical model based on the thermal heating equation applied to an anisotropic medium. Theoretical predictions have been verified by performing photo-heating experiments on a sample containing a small percentage of GNPs dispersed in NLCs. Both theory and experiments represent an important achievement in understanding the physics of heat transfer at the nanoscale, with applications ranging from photonics to nanomedicine.

Inherent optical losses of plasmonic materials represent a crucial issue for optoplasmonics, whereas the realization of hierarchical plasmonic nanostructures implemented with gain functionalities is a promising and valuable solution to the problem. Here we demonstrate that porous silica capsules embedding gold nanoparticles (Au NPs) and fabricated at a scale intermediate between the single plasmonic nanostructure and bulk materials show remarkable form–function relations. At this scale, in fact, the plasmon–gain interplay is dominated by the location of the gain medium with respect to the spatial distribution of the local field. In particular, the hollow spherical cavities of these structures allow regions of uniform plasmonic field where the energy transfer occurring between chromophoric donors and the surrounding plasmonic acceptors gives rise to a broadband attenuation of losses.