The nature of non-FRET photoluminescence quenching in nanoassemblies from semiconductor quantum dots and dye molecules

Literature Information

Publication Date 2018-06-21
DOI 10.1039/C8CP02846J
Impact Factor 3.676
Authors

Aleksander P. Stupak, Thomas Blaudeck, Eduard I. Zenkevich, Stefan Krause, Christian von Borczyskowski


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Abstract

Nanoassemblies formed via self-assembly based on colloidal CdSe quantum dots (QDs) and porphyrin (H2P) dye molecules show Fluorescence Resonant Energy Transfer (FRET) and non-FRET quenching of QD photoluminescence (PL). We present a procedure to unravel and quantify these two relaxation pathways via dynamic and static PL quenching experiments. Accordingly, FRET amounts at maximum to 10% of the total quenching efficiency. Since the degree of ligand coverage is inhomogeneously distributed across the QD ensemble PL quantum yields vary broadly. The attachment of H2P molecules occurs preferentially to those QDs with low ligand coverage. Along with that, nanoassembly formation deviates strongly from Poisson statistics. Like FRET, non-FRET depends on the QD size. We assign non-FRET quenching to the formation of specific new Cd2+ trap states following depletion of several ligands by the spacious dye molecules. While FRET follows quantitatively the Förster model, non-FRET appears on time scales of 1–3 ns in new and enhanced non-radiative near-band-edge QD PL decay channels caused by a trapping of the electrons in long-lived intra-gap states which then manifests itself in a subsequent weak PL emission. We assign the related intra-band emission to a recombination of deep-trap electrons and shallow-trap holes.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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