Symmetry Breaking Charge Separation in Linked Violanthrone Dimers

Symmetry-breaking charge separation (SBCS) has the potential to significantly enhance energy conversion efficiency. However, the role of molecular structure in mediating SBCS remains incompletely understood. Here, we report SBCS in novel violanthrone dimers where charge transfer (CT) and charge separation (CS) is tunable through molecular design. We show that in polar environments CT readily occurs even at large interchromophore distances and with flexible linkers. While CT character is observed in all the dimers studied, CS occurs most readily for the dimer with the shortest interchromophore separation.