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HERO ID
6650195
Reference Type
Journal Article
Title
Trap Passivation in Indium-Based Quantum Dots through Surface Fluorination: Mechanism and Applications
Author(s)
Kim, TaeGon; Zherebetskyy, D; Bekenstein, Y; Oh, MH; Wang, LinW; Jang, E; Alivisatos, AP; ,
Year
2018
Is Peer Reviewed?
1
Journal
ACS Nano
ISSN:
1936-0851
EISSN:
1936-086X
Publisher
AMER CHEMICAL SOC
Location
WASHINGTON
Page Numbers
11529-11540
PMID
30335943
DOI
10.1021/acsnano.8b06692
Web of Science Id
WOS:000451789200092
Abstract
Treatment of InP colloidal quantum dots (QDs) with hydrofluoric acid (HF) has been an effective method to improve their photoluminescence quantum yield (PLQY) without growing a shell. Previous work has shown that this can occur through the dissolution of the fluorinated phosphorus and subsequent passivation of indium on the reconstructed surface by excess ligands. In this article, we demonstrate that very significant luminescence enhancements occur at lower HF exposure though a different mechanism. At lower exposure to HF, the main role of the fluoride ions is to directly passivate the surface indium dangling bonds in the form of atomic ligands. The PLQY enhancement in this case is accompanied by red shifts of the emission and absorption peaks rather than blue shifts caused by etching as seen at higher exposures. Density functional theory shows that the surface fluorination is thermodynamically preferred and that the observed spectral characteristics might be due to greater exciton delocalization over the outermost surface layer of the InP QDs as well as alteration of the optical oscillator strength by the highly electronegative fluoride layer. Passivation of surface indium with fluorides can be applied to other indium-based QDs. PLQY of InAs QDs could also be increased by an order of magnitude via fluorination. We fabricated fluorinated InAs QD-based electrical devices exhibiting improved switching and higher mobility than those of 1,2-ethanedithiol cross-linked QD devices. The effective surface passivation eliminates persistent photoconductivity usually found in InAs QD-based solid films.
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