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Molecular materials have emerged as highly tunable materials for photovoltaicand light-harvesting applications. The most severe challenge of this class ofmaterials is the trapping of charge carriers in bound electron-hole pairs,which severely limits the free charge carrier generation. Here, we demonstratea significant modification of the exciton dynamics of thin films of endohedralmetallofullerene complexes upon alkali metal intercalation. For the exemplarycase of Sc$_3$N@C$_{80}$ thin films, we show that potassium intercalationresults in an additional relaxation channel for the optically excitedcharge-transfer excitons that prevents the trapping of excitons in a long-livedFrenkel exciton-like state. Instead, K intercalation leads to an ultrafastexciton dissociation coinciding most likely with the generation of free chargecarriers. In this way, we propose alkali metal doping of molecular films as anovel approach to enhance the light to-charge carrier conversion efficiency inphotovoltaic materials.

Ultrafast charge carrier separation in Potassium-intercalated endohedral metallofullerene Sc$_3$N@C$_{80}$ thin films