“…In general, the V oc is mainly governed by the molecular frontier orbital energy levels,i.e., the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels,a nd the J sc is mainly dominated by the absorption capability of the active layer, and both of them have been extensively well studied and achieved great successes through systematic design of photovoltaic materials. [1,31,32] On the other hand, the FF as an equally important third parameter in determining PCE, which is more sensitive and determined by comprehensive and complicated courses,i ncluding charge generation, transport, recombination, and extraction, is still ac hallenging issue. [33][34][35][36] So far,toboost the FF of OSCs,alot of works have been focused on device engineering to simultaneously improve the corresponding charge generation, transport and extraction, as well as reduce charge recombination, including the modification of interlayer [17,28,30,37] and the optimization of bulk heterojunction (BHJ) active layer morphologies.…”