Detailed insight in the processes that take place at the sensitized solid/liquid interface in DSSC is very valuable. We show how computer simulations based on atomistic models and density functional theory can provide an atomistic model of the interface that takes important components (oxide, dye, electrolyte) of the system explicitly into account. In particular, various binding modes of the N3 dye on anatase(101) have been computed and IR spectra are assigned. These results allow for predicting the more stable surface conformations, and clarifies the various carboxylate-Ti interactions. Extensive classical simulations of the TiO2-acetonitrile interface provide an explanation for the good performance of the acetonitrile/I3-/I- electrolyte. Free energy calculations in explicit solution suggest an efficient pathway for dye regeneration and an alternative mechanism for the formation of I3-. Novel simulation techniques, such as linear scaling DFT, can be used to study question that are out of the reach of more traditional approaches.

Towards an atomistic picture of the active interface in dye sensitized solar cells

245th National Meeting (2013)

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