We introduce preliminary work aiming at developing a new generation of bio-enabled nanoscopic antennas which relies on quantum coherence to transform light energy into collective electronic excitations. The idea of super-radiant coupling between plasmons and molecular excited states has been discussed before, theoretically, in simplified contexts, e.g two state systems, in absence of geometric spatial symmetry considerations. Symmetry of molecular electronic states, and mesoscopic geometric constraints are factors that for the time being are easier to tackle experimentally. In our experiments, we decorate the surface of an icosahedral virus protein cage with organic dyes which interact strongly with the virus surface via intermolecular forces. We study the fluorescence emission under ultrafast pumping, in terms of intensity and lifetime as we increase the number of chromophores per particle. We find that, the initial increase in the number of chromophore, is accompanied by concentration quenching as one would expect from a dense chromophore system near thermodynamic equilibrium. However, above a threshold value (N = 135, 75% coverage), the intensity of fluorescence emission suddenly increases several times. The fluorescence lifetime is shorter than what we could measure with the current setup. We believe this to be a strong indication that collective relaxation tends to dominate emission when reaching near complete coverages. Control experiments that perturb the shell-chromophore interaction also destroy the suppression of fluorescence quenching effect. To study the near-field energy transfer between the chromophores excited state and the surface plasmon of a metal nanoparticle we encapsulate the later into a chromophore studded virus protein shell. Preliminary results show that the ratio of the integrated spectral density of emission from virus-like particles containing metal to the spectral density of emission from free dye depends on pump power. The same ratio is independent of pump power in the nanoparticle absence.
A new technique, the near-field correlation spectroscopy (NFCS), is introduced which will be useful for monitoring individual binding events between the biomolecular complex precursors and a functionalized nanoparticle core in a physiological fluid. From jumps in the measured correlation times of single particles trapped in nanoapertures in a metal film, one will be able to determine the rate of binding/dissociation events and, most importantly, the nature of the binding entity, for e.g. discriminate the arrival and binding of a pentamer from a hexamer of protein subunits. This report deals only with the initial steps that are required to implement the new technique.
We examine experimentally the modifications induced at the surface of silicon and IV-IV alloys by an excimer laser above the melting threshold fluence. Laser irradiation takes place under vacuum, or in the presence of a gas. The resulting processes are respectively: laser induced polarization, pulsed laser induced epitaxy, incorporation of atoms from the gas phase, and laser chemical etching. In turn, the laser induced surface modifications and the presence of adsorbates on the surface cause important changes in the melting/solidification cycle. We describe a model calculation which takes into account non-equilibrium heat diffusion, phase change, atom diffusion, segregation and desorption. The model is applied to the laser chemical etching process, and its results are compared to the experimental data. This simulation brings information on the segregation of chlorine and on the dynamics of desorption.
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