Plastic solar cells bear the potential for large‐scale power generation based on materials that provide the possibility of flexible, lightweight, inexpensive, efficient solar cells. Since the discovery of the photoinduced electron transfer from a conjugated polymer to fullerene molecules, followed by the introduction of the bulk heterojunction (BHJ) concept, this material combination has been extensively studied in organic solar cells, leading to several breakthroughs in efficiency, with a power conversion efficiency approaching 5 %. This article reviews the processes and limitations that govern device operation of polymer:fullerene BHJ solar cells, with respect to the charge‐carrier transport and photogeneration mechanism. The transport of electrons/holes in the blend is a crucial parameter and must be controlled (e.g., by controlling the nanoscale morphology) and enhanced in order to allow fabrication of thicker films to maximize the absorption, without significant recombination losses. Concomitantly, a balanced transport of electrons and holes in the blend is needed to suppress the build‐up of the space–charge that will significantly reduce the power conversion efficiency. Dissociation of electron–hole pairs at the donor/acceptor interface is an important process that limits the charge generation efficiency under normal operation condition. Based on these findings, there is a compromise between charge generation (light absorption) and open‐circuit voltage (VOC) when attempting to reduce the bandgap of the polymer (or fullerene). Therefore, an increase in VOC of polymer:fullerene cells, for example by raising the lowest unoccupied molecular orbital level of the fullerene, will benefit cell performance as both fill factor and short‐circuit current increase simultaneously.

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The origin of the enhanced performance of bulk heterojunction solar cells based on slowly dried films of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61-butyric acid methyl ester is investigated, combining charge transport measurements with numerical device simulations. Slow drying leads to a 33-fold enhancement of the hole mobility up to 5.0×10−7m2V−1s−1 in the P3HT phase of the blend, thereby balancing the transport of electrons and holes in the blend. The resulting reduction of space-charge accumulation enables the use of thick films (∼300nm), absorbing most of the incoming photons, without losses in the fill factor and short-circuit current of the device.

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