Ultrafast charge carrier separation in Potassium-intercalated endohedral metallofullerene Sc₃N@C₈₀ thin films

Molecular materials have emerged as highly tunable materials for photovoltaic and light-harvesting applications. The most severe challenge of this class of materials is the trapping of charge carriers in bound electron-hole pairs, which severely limits the free charge carrier generation. Here, we demonstrate a significant modification of the exciton dynamics of thin films of endohedral metallofullerene complexes upon alkali metal intercalation. For the exemplary case of Sc$_3$N@C$_{80}$ thin films, we show that potassium intercalation results in an additional relaxation channel for the optically excited charge-transfer excitons that prevents the trapping of excitons in a long-lived Frenkel exciton-like state. Instead, K intercalation leads to an ultrafast exciton dissociation coinciding most likely with the generation of free charge carriers. In this way, we propose alkali metal doping of molecular films as a novel approach to enhance the light to-charge carrier conversion efficiency in photovoltaic materials.