Publication date: 11th March 2026
Reducing voltage losses is essential for advancing the efficiency of organic solar cells (OSCs), yet state-of-the-art non-fullerene acceptors (NFAs) still exhibit substantially larger non-radiative losses than their inorganic counterparts. Here, we identify intermolecular charge-transfer (iCT) states as a key intrinsic factor limiting radiative recombination in Y-series NFAs. Using an oligomer-based model strategy, we demonstrate that the formation of an iCT state, strongly hybridized with the local exciton, suppresses the radiative decay rate without increasing the non-radiative decay rate and reduces the oscillator strength of the lowest excited state. This hybridization leads to a diminished photoluminescence quantum yield (PLQY) and prolonged emission lifetimes, consistent with the emergence of partially dark excitonic states. Guided by this mechanistic insight, we develop a molecular design strategy based on side-to-tail coupling to promote J-type excitonic interactions while suppressing dark iCT formation. Devices employing this design achieve a voltage loss less than the 0.45 eV, among the lowest reported for OSCs to date. These results establish controlled excitonic coupling as a powerful design principle for minimizing voltage losses and advancing next-generation high-efficiency OSCs.
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