With an impending surge in the global demand for energy, there is a need for disruptive solar energy harvesting approaches, and superstructures that undergo long-distance photoinduced charge separation are one solution to this challenge. We have recently developed a supramolecular system composed of diketopyrrolopyrrole (DPP) electron donors and perylene derived bismide (PDI) electron acceptors, which forms 2:1 helical heteroaggregate supramolecular polymers as a result of triple H-bonding and ?���? stacking orthogonal to the H-bonding axis (Fig. 1 A). 1 Here we report that fluorescence quenching arises with assembly of the DPP and PDI into superstructures upon cooling (Fig. 1 B). 2Ultrafast transient absorption spectroscopy reveals that electron transfer could proceed from the upper SOMO (-3.24 eV) of photoexcited DPP into the PDI LUMO (-3.63eV), or alternatively hole transfer from the lower SUMO (-5.35 eV) of the photoexcited PDI into the DPP HOMO (-5.98eV) with driving forces of -0.39 eV and -0.63eV, respectively (Fig. 1 C). This route towards functional hierarchical superstructures could lead to new materials for artificial photosynthesis and organic electronics. 

Cooperatively assembling donor-acceptor superstructures direct energy into an emergent charge separated state

248th National Meeting (2014)

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