Multi-exciton dissociation (MED) is an important charge multiplication mechanism for improving the power efficiency in quantum dot (QD) based energy applications. To achieve high efficiency via MED process, charge transfer rates need to outcompete the ultrafast exciton annihilation rates. In model systems composed of QDs and molecular acceptors, the electron transfer dynamics in MED process have been well studied, whereas measurements and knowledge on the much slower hole transfer dynamics are insufficient. Here we have designed a QD-dye system where a new redox-active dye anchored on the QD surface is utilized in transient absorption measurements to monitor the hole transfer kinetics from a QD to its ligand shell. The coupling between Auger-type excitonic dynamics and hole transfer dynamics has been systematically compared across CdSe QDs of different volumes and quasi-type II CdSe/CdS core/shell QDs with varying shell thickness. The size and composition of the QDs are tuned to vary the rate of Auger dynamics and the electronic coupling between ligands and QDs. The results provide mechanistic insights on the design rules of optimal QD-ligand system for hole extraction under multiexcitonic conditions. <br/>

Probing multi-excitonic hole transfer dynamics in quantum confined semiconductor nanocrystals

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.