Design of new triphenylamine-sensitized solar cells: a theoretical approach.

This work reports a theoretical study of the photovoltaic properties of a series of original conjugated metal-free organic dyes containing the triphenylamine (TPA) moiety. These compounds have recently been develop for dye sensitized solar cells (DSSCs). Our (TD)DFT-based procedure made it possible to get insights into the geometrical and electronic structures of the dyes and to unravel the structural modifications optimizing the properties of TPA-based DSSCs. In particular, we aimed at improving the electron injection process as well as the light harvesting efficiency of the dyes. On the other hand, molecular dynamic (MD) investigations of the kinetics of the regeneration step have been performed for both "classical" (CHCl(3)/I(3)(-)/I(-)/Li(+)) and iodide imidazolium-based solvent-free electrolytes (DMII(+)/I(-)). The MD simulations helped to understand the regeneration mechanism for the solvent-free electrolyte: it combines the DMII(+)/DMII(0) couple to the I(3)(-)/I(-) redox system which acts as a "mediator".