Beyond Charge Transfer: The Impact of Auger Recombination and FRET on PL Quenching in an rGO-QDs System

PL intensity quenching and the PL lifetime reduction of fluorophores located close to graphene derivatives are generally explained by charge and energy transfer processes. Analyzing the PL from PbS QDs in rGO/QD systems, we observed a substantial reduction in average PL lifetimes with an increase in...

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Published inNanomaterials (Basel, Switzerland) Vol. 11; no. 6; p. 1623
Main Authors Babaev, Anton A, Sokolova, Anastasiia V, Cherevkov, Sergei A, Berwick, Kevin, Baranov, Alexander V, Fedorov, Anatoly V, Litvin, Aleksandr P
Format Journal Article
LanguageEnglish
Published Switzerland MDPI AG 21.06.2021
MDPI
Subjects
Auger recombination
Augers
Charge transfer
Chemical compounds
Current carriers
Energy charge
Energy transfer
Fluorescence
Fluorescence resonance energy transfer
Fluorophores
Graphene
Lifetime
Mathematical models
PL lifetime
Quantum dots
Quenching
Recombination
reduced graphene oxide
Reduction
Service life assessment
Simulation
spectroscopy
United States > US
quantum dots
PL lifetime
reduced graphene oxide
spectroscopy
Auger recombination
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Summary:PL intensity quenching and the PL lifetime reduction of fluorophores located close to graphene derivatives are generally explained by charge and energy transfer processes. Analyzing the PL from PbS QDs in rGO/QD systems, we observed a substantial reduction in average PL lifetimes with an increase in rGO content that cannot be interpreted solely by these two processes. To explain the PL lifetime dependence on the rGO/QD component ratio, we propose a model based on the Auger recombination of excitations involving excess holes left in the QDs after the charge transfer process. To validate the model, we conducted additional experiments involving the external engineering of free charge carriers, which confirmed the role of excess holes as the main QD PL quenching source. A mathematical simulation of the model demonstrated that the energy transfer between neighboring QDs must also be considered to explain the experimental data carefully. Together, Auger recombination and energy transfer simulation offers us an excellent fit for the average PL lifetime dependence on the component ratio of the rGO/QD system.
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content type line 23
ISSN:2079-4991
2079-4991
DOI:10.3390/nano11061623