Polarized molecular wires for efficient photo-generation of free electric charge carriers†

In this study, five all-organic polarized molecular wires (PMWs) for photovoltaic applications are introduced and investigated by means of theoretical chemistry methods. Structurally based on polarized pyrrole and isoindole moieties, the proposed systems demonstrate efficient and ultrafast charge separation upon light absorption. The relevant PMW properties are evaluated using semi-empirical and ab initio quantum-chemical calculations, as well as nonadiabatic molecular dynamics simulations. For each system, the individual mechanism of charge carrier separation is identified and characterized, with all proposed wires exhibiting remarkable charge carrier separation efficiencies and rates. Furthermore, the designed PMW structures enable their straightforward incorporation into more extended molecular frameworks.