Two blinking mechanisms in highly confined AgInS2 and AgInS2/ZnS quantum dots evaluated by single particle spectroscopy

B. Cichy, R. Rich, A. Olejniczak, Zygmunt Gryczynski, W. Strek

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Abstract

Ternary AgInS2 quantum dots (QDs) have been found as promising cadmium-free, red-shifted, and tunable luminescent bio-probes with efficient Stokes and anti-Stokes excitations and luminescence lifetimes (ca. 100 ns) convenient for time resolved techniques like fluorescence life-time imaging. Although the spectral properties of the AgInS2 QDs are encouraging, the complex recombination kinetics in the QDs being still far from understood, limits their full utility. In this paper we report on a model describing the recombination pathways responsible for large deviations from the first-order decay law observed commonly in the ternary chalcogenides. The presented results were evaluated by means of individual AgInS2 QD spectroscopy aided by first principles calculations including the electronic structure and structural reconstruction of the QDs. Special attention was devoted to study the impact of the surface charge state on the excited state relaxation and effect of its passivation by Zn2+ ion alloying. Two different blinking mechanisms related to defect-assisted charge imbalance in the QD responsible for fast non-radiative relaxation of the excited states as well as surface recharging of the QD were found as the major causes of deviations from the first-order decay law. Careful optimization of the AgInS2 QDs would help to fabricate new red-shifted and tunable fluorescent bio-probes characterized by low-toxicity, high quantum yield, long luminescence lifetime, and time stability, leading to many novel in vitro and in vivo applications based on fluorescence lifetime imaging (FLIM) and time-gated detection.

Original languageEnglish
Pages (from-to)4151-4159
Number of pages9
JournalNanoscale
Volume8
Issue number7
DOIs
StatePublished - 21 Feb 2016

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Semiconductor quantum dots
Spectroscopy
Excited states
Luminescence
Fluorescence
Imaging techniques
Chalcogenides
Quantum yield
Surface charge
Cadmium
Alloying
Passivation
Electronic structure
Toxicity
Ions
Defects
Kinetics

Cite this

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title = "Two blinking mechanisms in highly confined AgInS2 and AgInS2/ZnS quantum dots evaluated by single particle spectroscopy",
abstract = "Ternary AgInS2 quantum dots (QDs) have been found as promising cadmium-free, red-shifted, and tunable luminescent bio-probes with efficient Stokes and anti-Stokes excitations and luminescence lifetimes (ca. 100 ns) convenient for time resolved techniques like fluorescence life-time imaging. Although the spectral properties of the AgInS2 QDs are encouraging, the complex recombination kinetics in the QDs being still far from understood, limits their full utility. In this paper we report on a model describing the recombination pathways responsible for large deviations from the first-order decay law observed commonly in the ternary chalcogenides. The presented results were evaluated by means of individual AgInS2 QD spectroscopy aided by first principles calculations including the electronic structure and structural reconstruction of the QDs. Special attention was devoted to study the impact of the surface charge state on the excited state relaxation and effect of its passivation by Zn2+ ion alloying. Two different blinking mechanisms related to defect-assisted charge imbalance in the QD responsible for fast non-radiative relaxation of the excited states as well as surface recharging of the QD were found as the major causes of deviations from the first-order decay law. Careful optimization of the AgInS2 QDs would help to fabricate new red-shifted and tunable fluorescent bio-probes characterized by low-toxicity, high quantum yield, long luminescence lifetime, and time stability, leading to many novel in vitro and in vivo applications based on fluorescence lifetime imaging (FLIM) and time-gated detection.",
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Two blinking mechanisms in highly confined AgInS2 and AgInS2/ZnS quantum dots evaluated by single particle spectroscopy. / Cichy, B.; Rich, R.; Olejniczak, A.; Gryczynski, Zygmunt; Strek, W.

In: Nanoscale, Vol. 8, No. 7, 21.02.2016, p. 4151-4159.

Research output: Contribution to journalArticleResearchpeer-review

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T1 - Two blinking mechanisms in highly confined AgInS2 and AgInS2/ZnS quantum dots evaluated by single particle spectroscopy

AU - Cichy, B.

AU - Rich, R.

AU - Olejniczak, A.

AU - Gryczynski, Zygmunt

AU - Strek, W.

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