The light-harvesting microcrystals were prepared with solvent evaporation–induced self-assembly. In a typical preparation, 30 μl of 2 mM OPV in chlorobenzene was first mixed with 30 μl of C60 chlorobenzene solution to form a homogeneous mixture, which was then placed in a 50-ml closed beaker containing 3 ml of cyclohexane anti-solvent. In the whole procedures, a solvent atmosphere was kept and the evaporation speed of the solvent (i.e., the saturation degree of the solution) can be well controlled. A large number of doped microcrystals were finally obtained after 12 to 24 hours. The C60 doping concentrations in OPV were adjusted by changing the concentrations of C60 chlorobenzene solution from 0, 1 mM, 2 mM, 5 mM to 10 mM. The actual doping concentrations of C60 in light-harvesting microcrystals were determined to be 0, 0.6 mol%, 1.7 mol%, 2.8 mol%, and 5.6 mol%, respectively.

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