LAUSR

Singlet fission is a process by which an organic semiconductor is able to generate two triplet excitons from a single photon. If charges from the triplets can be successfully harvested without heavy losses in energy, then this process can enable a single‐junction solar cell to surpass the Shockley–Queisser limit. While singlet fission processes are commonly observed in several materials, harvesting the resulting triplets is difficult and has been demonstrated with only a few transport materials. Here, transient absorption spectroscopy is used to investigate singlet fission and carrier transfer processes at the AgBiS2/pentacene (AgBiS2/Pc) heterojunction. The successful transfer of triplets from pentacene to AgBiS2 and the transfer of holes from AgBiS2 to pentacene is observed. Further singlet fission in pentacene by modifying the crystallinity of the pentacene layer and have fabricated the first singlet fission AgBiS2/Pc solar cell is enhanced. Singlet fission devices exhibit higher external quantum efficiency compared with the control devices, and thus demonstrating the significant contribution of charges from the singlet fission process.