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Optical Properties and Ultrafast Dynamics in Metal Cluster Hybrids with Diamondoids, and Conjugated π-Systems

Hybrids between metal clusters and sp3 or sp2 carbon nanostructures represent highly promising systems for the development of new optical, plasmonic and sensing materials. The functionality of these systems is governed by the interplay between the electronic structure,  ultrafast dynamical processes, such as internal conversion or intersystem crossing, and near-field enhancement effects. The goal of our project is to theoretically predict new hybrid systems with unique optical properties, which can be realized in collaboration with experimental partners. We will explore structural, optical and dynamical properties of small metal clusters (Ag, Au, Al) interacting with sp3 or sp2 hybridized organic systems including pure and functionalized diamondoids, multiporphyrin arrays and polycyclic aromatic hydrocarbons (PAHs). The hybrids between metal clusters and sp3 hybridized diamondoids allow for designing 3D scaffolds in which the optical properties of both subunits are largely preserved due to the relative inertness of diamondoids, and the presence of the metal nanocluster may lead to the enhancement of the absorption and emission in diamondoids. In contrast, in hybrids with sp2 hybridized porphyrin and PAH systems the resonance between the metal cluster excitations and tunable delocalized π-system excitations provides strong coupling and is expected to give rise to new collective phenomena. The nonradiative processes and excited state relaxation will be investigated using our field-induced surface hopping (FISH) method combined with ab initio and semiempirical methods for the electronic structure. The methodology will be extended in this project by including spin-orbit coupling in order to describe intersystem crossing dynamics. Furthermore, we will introduce the combination of electrodynamics with light-induced nonadiabatic dynamics in order to investigate the influence of the near-field enhancement on the radiative and nonradiative relaxation at the atomic level. The ultimate aim is to design novel hybrid systems with unique linear and nonlinear optical response in the context of plasmonic and sensing applications.

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