Elucidation of Two Giants: Challenges to Thick-shell Synthesis in CdSe/ZnSe and ZnSe/CdS Core/Shell Quantum Dots

Acharya, Krishna P.; Nguyen, Hue M.; Paulite, Melissa; Piryatinski, Andrei; Zhang, Jun; Casson, Joanna Lee; Xu, Hongwu; Htoon, Han; Hollingsworth, Jennifer Ann

doi:10.1021/jacs.5b00313

Title: Elucidation of Two Giants: Challenges to Thick-shell Synthesis in CdSe/ZnSe and ZnSe/CdS Core/Shell Quantum Dots

Journal Article · Fri Mar 06 00:00:00 EST 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b00313· OSTI ID:1329561

Acharya, Krishna P. ^[1]; Nguyen, Hue M. ^[1]; Paulite, Melissa ^[1]; Piryatinski, Andrei ^[2]; Zhang, Jun ^[3]; Casson, Joanna Lee ^[4]; Xu, Hongwu ^[3]; Htoon, Han ^[5]; Hollingsworth, Jennifer Ann ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Materials Physics and Applications Division, Center for Integrated Nanotechnologies
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division, Physics of Condensed Matter & Complex Systems
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Earth & Environmental Science Division, Earth System Observations
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Chemistry Division, Physical Chemistry & Applied Spectroscopy
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Materials Physics and Applications Division: Center for Integrated Nanotechnologies

Core/thick-shell "giant" quantum dots (gQDs) possessing type II electronic structures exhibit suppressed blinking and diminished nonradiative Auger recombination. Here 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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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396; 2009LANL1096

OSTI ID:: 1329561

Report Number(s):: LA-UR-15-20906

Journal Information:: Journal of the American Chemical Society, Vol. 137, Issue 11; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 54 works

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