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J Am Chem Soc. 2015 Mar 25;137(11):3755-8. doi: 10.1021/jacs.5b00313. Epub 2015 Mar 11.

Elucidation of two giants: challenges to thick-shell synthesis in CdSe/ZnSe and ZnSe/CdS core/shell quantum dots.

Journal of the American Chemical Society

Krishna P Acharya, Hue M Nguyen, Melissa Paulite, Andrei Piryatinski, Jun Zhang, Joanna L Casson, Hongwu Xu, Han Htoon, Jennifer A Hollingsworth

PMID: 25746140 DOI: 10.1021/jacs.5b00313

Abstract

Core/thick-shell giant quantum dots (gQDs) possessing type II electronic structures exhibit suppressed blinking and diminished nonradiative Auger recombination. We investigate CdSe/ZnSe and ZnSe/CdS as potential new gQDs. We show theoretically and experimentally that both can exhibit partial or complete spatial separation of an excited-state electron-hole pair (i.e., type II behavior). However, we reveal that thick-shell growth is challenged by competing processes: alloying and cation exchange. We demonstrate that these can be largely avoided by choice of shelling conditions (e.g., time, temperature, and QD core identity). The resulting CdSe/ZnSe gQDs exhibit unusual single-QD properties, principally emitting from dim gray states but having high two-exciton (biexciton) emission efficiencies, whereas ZnSe/CdS gQDs show characteristic gQD blinking suppression, though only if shelling is accompanied by partial cation exchange.

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