Sizing up excitons in core–shell quantum dots via shell-dependent photoluminescence blinking

Fisher, Aidan A E and Osborne, Mark A (2017) Sizing up excitons in core–shell quantum dots via shell-dependent photoluminescence blinking. ACS Nano, 11 (8). pp. 7829-7840. ISSN 1936-0851

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Semiconductor nanocrystals or quantum dots (QDs) are now widely used across solar cell, display, and bioimaging technologies. While advances in multishell, alloyed, and multinary core–shell QD structures have led to improved light-harvesting and photoluminescence (PL) properties of these nanomaterials, the effects that QD-capping have on the exciton dynamics that govern PL instabilities such as blinking in single-QDs is not well understood. We report experimental measurements of shell-size-dependent absorption and PL intermittency in CdSe-CdS QDs that are consistent with a modified charge-tunnelling, self-trapping (CTST) description of the exciton dynamics in these nanocrystals. By introducing an effective, core-exciton size, which accounts for delocalization of charge carriers across the QD core and shell, we show that the CTST models both the shell-depth-dependent red-shift of the QD band gap and changes in the on/off-state switching statistics that we observe in single-QD PL intensity trajectories. Further analysis of CdSe-ZnS QDs, shows how differences in shell structure and integrity affect the QD band gap and PL blinking within the CTST framework.

Item Type: Article
Keywords: charge transfer; core−shell nanocrystals; photoluminescence intermittency; semiconductor quantum dots; single molecule spectroscopy; stochastic simulation
Schools and Departments: School of Life Sciences > Chemistry
Research Centres and Groups: Energy and Materials Chemistry
Subjects: Q Science
Q Science > QC Physics > QC0170 Atomic physics. Constitution and properties of matter Including molecular physics, relativity, quantum theory, and solid state physics
Q Science > QD Chemistry > QD0146 Inorganic chemistry
Q Science > QD Chemistry > QD0450 Physical and theoretical chemistry
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Depositing User: Mark Osborne
Date Deposited: 20 Jul 2017 08:00
Last Modified: 02 Jul 2019 15:15

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