Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
A combined theoretical study of the entire "light to free charge carrier" kinetics on hybrid inorganic-organic interfaces describes a huge challenge. This is mainly due to the manifold of interdependent subprocesses. While especially a proper study of the initial short time scale quantum dynamics demands for very expensive methods including e.g. a non-Markovian electron-vibration interaction, the long time scale kinetics, however, are very sensitive to a realistic size of the model system. In order to meet both grades, we set up an open system dynamics study based on a stochastic Schrödinger equation method. As the number of system states increases the preserved scaling benefit of this wave function approach becomes apparent.
After an introducing overview of the inorganic-organic hybrid system under consideration the excitation energy and charge transfer processes of interest are presented. The main part of the presentation gives insight into the combined coherent and dissipative hole motion in a huge organic para-sexiphenyl cluster. An initial study has the focus on solely the organic part. The required energies, vibronic couplings and transfer parameters are calculated on ab-initio level. Then we attend to the actual hybrid interface system by placing the molecular cluster on a ZnO surface. By means of an installed electronic excess charge distribution in the inorganic counterpart, the hole motion becomes subject to a realistic Coulomb attraction across the interface. In order to clarify the principles of the aspired electron-hole pair separation across such interfaces, it is fundamental to understand how the hole overcomes this existing barrier.
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