Dynamic Multi-Mode Mie Model for Gain-Assisted Metal Nano-Spheres.

Coupling externally pumped gain materials with plasmonic spherical particles, even in the simplest case of a single spherical nanoparticle in a uniform gain medium, generates an incredibly rich variety of electrodynamic phenomena. The appropriate theoretical description of these systems is dictated by the quantity of the included gain and the size of the nano-particle. On the one hand, when the gain level is below the threshold separating the absorption and the emission regime, a steady-state approach is a rather adequate depiction, yet a time dynamic approach becomes fundamental when this threshold is exceeded. On the other hand, while a quasi-static approximation can be used to model nanoparticles when they are much smaller than the exciting wavelength, a more complete scattering theory is necessary to discuss larger nanoparticles. In this paper, we describe a novel method including a time-dynamical approach to the Mie scattering theory, which is able to account for all the most enticing aspects of the problem without any limitation in the particle's size. Ultimately, although the presented approach does not fully describe the emission regime yet, it does allow us to predict the transient states preceding emission and represents an essential step forward in the direction of a model able to adequately describe the full electromagnetic phenomenology of these systems.

Optical vortices generated by edge dislocations in electro-convective instability arrays of nematic liquid crystals.

We demonstrated by means of interferometry that optical vortices can be generated by diffraction of a laser beam from a birefringent nematic liquid crystal that spontaneously creates a periodic array of electro-convective domains and edge dislocations under an applied electric field. The diffracted beam of order m produced by an elementary dislocation comprises a number |m| of distinct optical vortices, each with unit topological charge. Birefringent liquid crystal arrays provide a fast, convenient, and promising way of generating and studying optical vortices. The used materials are inexpensive, fabrication processes are simple, and both input polarization and applied field can be used as external controls to switch the optical vortices on and off.

Interface of physics and biology: engineering virus-based nanoparticles for biophotonics.

Virus-based nanoparticles (VNPs) have been used for a wide range of applications, spanning basic materials science and translational medicine. Their propensity to self-assemble into precise structures that offer a three-dimensional scaffold for functionalization has led to their use as optical contrast agents and related biophotonics applications. A number of fluorescently labeled platforms have been developed and their utility in optical imaging demonstrated, yet their optical properties have not been investigated in detail. In this study, two VNPs of varying architectures were compared side-by-side to determine the impact of dye density, dye localization, conjugation chemistry, and microenvironment on the optical properties of the probes. Dyes were attached to icosahedral cowpea mosaic virus (CPMV) and rod-shaped tobacco mosaic virus (TMV) through a range of chemistries to target particular side chains displayed at specific locations around the virus. The fluorescence intensity and lifetime of the particles were determined, first using photochemical experiments on the benchtop, and second in imaging experiments using tissue culture experiments. The virus-based optical probes were found to be extraordinarily robust under ultrashort, pulsed laser light conditions with a significant amount of excitation energy, maintaining structural and chemical stability. The most effective fluorescence output was achieved through dye placement at optimized densities coupled to the exterior surface avoiding conjugated ring systems. Lifetime measurements indicate that fluorescence output depends not only on spacing the fluorophores, but also on dimer stacking and configurational changes leading to radiationless relaxation-and these processes are related to the conjugation chemistry and nanoparticle shape. For biological applications, the particles were also examined in tissue culture, from which it was found that the optical properties differed from those found on the benchtop due to effects from cellular processes and uptake kinetics. Data indicate that fluorescent cargos are released in the endolysosomal compartment of the cell targeted by the virus-based optical probes. These studies provide insight into the optical properties and fates of fluorescent proteinaceous imaging probes. The cellular release of cargo has implications not only for virus-based optical probes, but also for drug delivery and release systems.

Plasmon mediated super-absorber flexible nanocomposites for metamaterials.

A flexible host has been selected to achieve, for the first time, functional nanocomposites based on CdSe@ZnS core-shell type quantum dots (QDs) and Au nanoparticles (NPs), simultaneously dispersed in a polymer matrix. Coherent interactions between QDs and plasmonic Au NPs embedded in PDMS films have been demonstrated to lead to a relevant enhancement of the absorption cross-section of the QDs, remarkably modifying the optical response of the entire system. Optical and time resolved spectroscopy studies revealed an active gain-plasmon feedback behind the super-absorbing overall effect.

Blue-shifted random-laser-mode selection in gain-assisted anisotropic complex fluids.

Random laser action in organic materials is of great topical interest that is fueled by the rapid development of active compounds and new dye molecules. We propose a pure-diffusive model to describe the strong connection established between a dye-host interaction and the scattering when considering an anisotropic complex fluid. The model considers multiple scattering induced by dielectric tensor fluctuations and a suitable quantistic description for light amplification in order to explain the generation of the narrow-band blue-shifted lasing mode experimentally observed in such systems. We also find that the introduction of a strong intermolecular force field provides the condition to enhance diffusive processes. The agreement between experimental observations and simulations advances the understanding of the physical mechanism behind mode selection in these systems.