Theory of ultrafast exciton interaction and spectroscopy at atomically thin semiconductor monolayer/organic molecule interfaces (B12)

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A many body theory for the optical dynamics at TMDC-semiconductor/organic molecule interfaces (TMDC: transition metal dichalcogenide) on a mesoscopic scale is developed. The focus is on the dynamics during and after short pulse excitation of hybrid inorganic/organic system (HIOS) excitons and describes their formation, nonlinear interaction and decay as function of geometry, level alignment, exciton-vibron interaction, disorder, and doping. For this, HIOS-Bloch equations are used to explore the conditions where the HIOS coupling for charge and excitation transfer is relevant in comparison to internal interactions of the individual constituents. The predicted HIOS dynamics is used to analyze time resolved (non-)linear optical spectroscopy and in electron spectroscopy.