Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 8, Issue 14, Pages 3179-3184Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b01503
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Funding
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- Ontario Research Fund Research Excellence Program
- IBM Canada Research and Development Center
- IBM Canada Research and Development Center through the Southern Ontario Smart Computing Innovation Platform (SOSCIP) postdoctoral fellowship
- Ontario Government
- Federal Economic Development Agency for Southern Ontario
- Canada Foundation for Innovation under the auspices of Compute Canada
- Government of Ontario
- Ontario Research Fund - Research Excellence
- University of Toronto
- University of Ottawa Research Chair in Quantum Theory of Materials, Nanostructures and Devices
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It has previously been found that Auger processes can lead to femtosecond carrier trapping in quantum dots, limiting their performance in optoelectronic applications that rely on radiative recombination. Using atomistic simulations, we investigate whether a shell can protect carriers from Auger-assisted trapping. For these studies we investigate CdSe/CdS core shell quantum dots having total diameters reaching up to 10 nm. We find trapping lifetimes as fast as 1 ps for 2 nm shells, and we report that shells as thick as 6 nm are required to suppress trapping fully. The most efficient recombination mechanism is found to proceed through shallow empty traps, suggesting it can be suppressed by filling the traps through doping or external electrochemical potential. Our findings suggest that to achieve efficient light emission, surface traps have to be completely eliminated, even in thick-shell quantum dots.
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