Exploiting Quantum Interference in Dye Sensitized Solar Cells

A strategy to hinder the charge recombination process in dye sensitized solar cells is developed in analogy with similar approaches to modulate charge transport across nanostructures. The system studied is a TiO2 (anatase) chromophore interface, with an unsaturated carbon bridge connecting the two subunits. A theory for nonadiabatic electron transfer is employed in order to take explicitly into account the contribution from the bridge states mediating the process. If a cross-conjugated fragment is present in the bridge, it is possible to suppress the charge recombination by negative interference of the possible tunnelling path. Calculations carried out on realistic molecules at the OFT level of theory show how the recombination lifetime can be modulated by changes in the electron-withdrawing (donating) character of the groups connected to the cross-conjugated bridge. Tight binding calculations are employed to support the interpretation of the atomistic simulations.