Light propagation and nonlinear optical respnose in silver cluster-porphyrin nanostructures

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The goal of this project is to develop novel optimally designed nanostructures by selfassembling ordered arrays of silver clusters at selected porphyrin templates for the application in nanooptical devices such as sensors. We will theoretically investigate the fundamental aspects of the interaction of these hybrid quantum systems with localized electromagnetic fields and will develop strategies for the control of coherent light propagation and localization. Specifically designed porphyrin oligomers with optimal structures as well as extended one-dimensional and two-dimensional porphyrin polymers will be used as templates to stabilize ordered arrays of sizeselected silver nanoclusters. We will focus on “molecule-like” clusters with sizes <2 nm which exhibit discrete electronic states, localized absorption and emission and relatively long nonradiative excited state lifetimes. Based on the methodology developed in the first phase of the project, we will use time-dependent density functional theory (TDDFT) combined with computational electrodynamics in order to simulate the nonlinear optical response as well as the coherent light propagation and localization in these systems. The optimal control will be used to manipulate the light propagation, which is the basis for the development of functional nanooptical devices. The ultimate goal of the project is to design novel nanooptical sensors for the detection of specific (bio)molecules. The coherent spatio-temporal light localization at the binding site for the analyte molecule will be utilized in order to increase the detection selectivity and sensitivity far beyond the current cababilities.