Abstract
Achieving high charge recombination probability has been the major challenge for the practical utilization of molecule-based solar harvesting. Molecular switches were introduced to stabilize the charge separation state in donor-acceptor systems, but it is difficult to seamlessly incorporate the ON/OFF switching actions into the optoelectronic conversion cycle. Here we present a self-adaptive system in which the donor and acceptor are bridged by a switchable moiety that enables a complete charge separation repeatedly. Calculations are presented for a platinum(II) terpyridyl complex with an azobenzene bridge. The charge transfer induced by light extracts electrons from the azobenzene group, automatically triggering a trans → cis isomerization. The resulting conformation suppresses charge recombination. Energized charges are trapped in the acceptor, ready for charge collection by electrodes. The bridge then goes through inverse isomerization to restore the conjugation and conductance. This self-adaptive design provides a novel way to improve the performance of optoelectronic conversion and realize practical solar-harvesting applications in organic molecular systems.
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