Abstract

Charge-carrier dynamics of CdS quantum dot (QD) and CdS/CdSe type-I and CdS/CdTe type-II core–shell nanocrystals (NCs) sensitized with a Re(I)–polypyridyl complex have been carried with special emphasis on studies on carrier delocalization and the role of Re-complex as a hole acceptor and sensitizer molecule. Our investigation confirmed photoexcited hole transfer from CdS and CdS/CdSe to the Re-complex, while no hole transfer was observed in the CdS/CdTe–Re-complex system. This was rationalized by the evaluation of the relative energy levels, which revealed that such hole migration was not energetically favorable due to low-lying highest occupied molecular orbital (HOMO) of the Re-complex as compared with the valence band (VB) of CdTe shell; however, luminescence quenching from upper excited states of Re-complex was observed in the presence of all three QD and core–shell systems, which has been attributed to electron injection from hot state (energetically higher than the LUMO state) of the Re-complex to ...

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