Triplet generation at the CdTe quantum dot/anthracene interface mediated by hot and thermalized electron exchange for...

Triplet energy transfer (TET) from semiconductor quantum dots (QDs) to molecular triplets has potential applications in photon up-conversion and singlet oxygen generation. Here, we have constructed a complex consisting of CdTe QDs as the donor and 9-anthracenecarboxylic acid (ACA) as the triplet acceptor, and studied the TET pathways and enhanced singlet oxygen generation properties. The results from steady-state and time-resolved spectroscopy demonstrate efficient TET with a total efficiency of over 80% from photoexcited CdTe QDs to ACA. Dynamical analysis clearly indicates two distinctive TET channels - hot electron exchange and thermalized electron exchange - mediating the TET process in the CdTe QDs-ACA complex. The TET efficiencies from hot electron exchange at high energetic levels and thermalized electron exchange on the lowest exciton state can reach ∼27% and ∼85%, respectively, following 530 nm excitation. This efficient TET endows the CdTe QDs-ACA complex with a good capability of generating singlet oxygen species with a yield of up to ∼59%. These findings contribute further insights to the mechanisms of interfacial TET processes and are significant in designing efficient TET systems based on semiconductor nanoparticles and triplet molecules.