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Nowadays, it is still a great challenge to obtain high‐performance green‐solvent‐processed organic solar cells (OSCs). In this study, a ternary blend strategy (one donor and two acceptors, 1D/2A) is developed to solve the difficulty of film morphology modulation during the fabrication of high‐performance green‐solvent‐processed OSCs. A typical high‐performance halogenated‐solvent processable binary system D18:BTP‐eC9‐4F is selected as the host, its green‐solvents‐processed devices show an inferior power conversion efficiency (PCE) of ≈16%. SM16 with two 3D shape persistent end groups is selected as the third component due to its high fluorescence quantum yield, reduced intermolecular interaction, good solubility, and moderate crystallinity. As a result, the ternary devices display bicontinuous interpenetrating networks, reduced energy loss, and suppressed charge carrier recombination losses. Hence, an excellent PCE of 18.20% is achieved for the D18:BTP‐eC9‐4F:SM16 ternary devices, which is much higher than D18:BTP‐eC9‐4F‐based binary ones and also one of the highest PCEs for the green‐solvents‐processed OSCs. Besides, this strategy also demonstrates a good universality for other binary systems and becomes an effective pathway for the development of green‐solvent processable high‐performance OSCs. [ABSTRACT FROM AUTHOR]

The electron donor/acceptor (D/A) heterojunction is the core for photocharge generation and recombination in organic photovoltaics (OPVs). Developing practical methods for the D/A heterojunction modification remains challenging and is rarely discussed in OPV research. Herein, the roles of molecular doping at the D/A heterojunction in the charge‐transfer exciton dissociation and detailed energy loss are investigated, and new insights are gained into the functions of doping on the OPV performance. Heterojunction doping simultaneously enhances all three OPV parameters, especially the short‐circuit current (Jsc). It is shown that the Jsc improvement is due to the combined effects of strengthened electric field and reduced activation energy, which is regulated via an entropy‐related mechanism. The performance enhancement is further demonstrated in homojunction devices showing the great potential of interfacial doping to overcome the intrinsic limitation between high Jsc and open‐circuit voltage (Voc) in OPVs. [ABSTRACT FROM AUTHOR]