Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
In this work, we investigate the laser-induced electron migration in dye-sensitized solar cells at an atomistic level of theory. The electron dynamics is simulated with a time-dependent many-electron configuration interaction ansatz and a single active electron approach. This allows to determine for the first time the extent of many-body effects during the charge transfer process by comparison with a wave function reference. A recently developed toolset including electronic yields, electronic fluxes, and flux densities helps us to unravel the mechanistic pathway of the electron from the dye into the semiconductor. In this context, we introduce a new decomposition of the many-body wavefunction to shed light on electron-electron and hole-hole interactions during the charge migration. Additionally, we focus on the influence of different chromophore-substrate binding motifs. We observe comparable electron transfer mechanisms for the different binding modes on different time scales. Furthermore, we confirm that a single active electron approach is a well-suited and low-cost method to properly describe electron migration processes in systems of this type. Our novel decomposition technique of the electron flux density reveals the correlated nature of the many-body wave function.
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