We
report that supramolecular polymer films composed of a 2:1 mixture
of monodiamidopyridine diketopyrrolopyrrole (DPP) electron donors
and perylene bisdiimide (PDI) electron acceptors undergo photoinduced
charge transfer in the solid state. Film formation is guided by complementary
noncovalent interactions programmed into the molecular components,
resulting in a film architecture comprised of polymer wires with order
across the molecular-to-macroscopic continuum. Using ultrafast transient
absorption spectroscopy, we show that recombination lifetimes increase
1000-fold compared to the same supramolecular polymers in solution.
Supramolecular donor–acceptor polymer films, such as these,
that are designed by considering structure and electron transfer dynamics
synergistically could lead to breakthroughs in organic optoelectronics