Auger ionization beats photo-oxidation of semiconductor quantum dots: extended stability of single-molecule photoluminescence

Angewandte Chemie
Shin-Ichi YamashitaVasudevanpillai Biju

Abstract

Despite the bright and tuneable photoluminescence (PL) of semiconductor quantum dots (QDs), the PL instability induced by Auger recombination and oxidation poses a major challenge in single-molecule applications of QDs. The incomplete information about Auger recombination and oxidation is an obstacle in the resolution of this challenge. Here, we report for the first time that Auger-ionized QDs beat self-sensitized oxidation and the non-digitized PL intensity loss. Although high-intensity photoactivation insistently induces PL blinking, the transient escape of QDs into the ultrafast Auger recombination cycle prevents generation of singlet oxygen ((1) O2 ) and preserves the PL intensity. By the detection of the NIR phosphorescence of (1) O2 and evaluation of the photostability of single QDs in aerobic, anaerobic, and (1) O2 scavenger-enriched environments, we disclose relations of Auger ionization and (1) O2 -mediated oxidation to the PL stability of single QDs, which will be useful during the formulation of QD-based single-molecule imaging tools and single-photon devices.

References

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Aug 25, 2010·ACS Nano·Morihiko HamadaVasudevanpillai Biju
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Aug 15, 2013·Angewandte Chemie·Edakkattuparambil Sidharth ShibuVasudevanpillai Biju

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Citations

Mar 4, 2017·Advanced Materials·Haiyan QinXiaogang Peng
Jul 25, 2015·Nanoscale·Vasudevanpillai BijuShin-ichi Wakida
Jul 14, 2019·Analytical and Bioanalytical Chemistry·Xiangyu JiaoXueji Zhang
Nov 30, 2018·The Journal of Physical Chemistry Letters·Bin LiSuotang Jia

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