Long‐Lived Photocharges in Supramoelcular Polymers of Low‐Bandgap Chromophores

Photoinduced charge separation in supramolecular aggregates of π‐conjugated molecules is a fundamental photophysical process, and a key criterion for the development of advanced organic electronics materials. Here, we report on the self‐assembly of novel low‐bandgap chromophores into helical one‐dimensional aggregates due to intermolecular hydrogen‐bonding. The chromophores confined in these supramolecular polymers show strong excitonic coupling interactions and give rise to charge‐separated states with unusually long lifetimes of several hours and charge densities of up to 5 mol% after illumination with white light. Two‐contact devices exhibit increased photoconductivity and can even show Ohmic behavior. Our findings demonstrate that the confinement of organic semiconductors into one‐dimensional aggregates results in a considerable stabilization of charge carriers for a variety of π‐conjugated systems, which may have implications for the design of future organic electronic materials.