Unveiling the Photoinduced Electron‐Donating Character of MoS2 in Covalently Linked Hybrids Featuring Perylenediimide

Abstract The covalent functionalization of MoS 2 with a perylenediimide (PDI) is reported and the study is accompanied by detailed characterization of the newly prepared MoS 2 ‐PDI hybrid material. Covalently functionalized MoS 2 interfacing organic photoactive species has shown electron and/or energy accepting, energy reflecting or bi‐directional electron accepting features. Herein, a rationally designed PDI, unsubstituted at the perylene core to act as electron acceptor, forces MoS 2 to fully demonstrate for the first time its electron donor capabilities. The photophysical response of MoS 2 ‐PDI is visualized in an energy‐level diagram, while femtosecond transient absorption studies disclose the formation of MoS 2 .+ ‐PDI .− charge separated state. The tunable electronic properties of MoS 2 , as a result of covalently linking photoactive organic species with precise characteristics, unlock their potentiality and enable their application in light‐harvesting and optoelectronic devices.