Combined static and dynamic intramicellar fluorescence quenching: effects on stationary and time-resolved Stern–Volmer experiments

Literature Information

Publication Date 2019-04-29
DOI 10.1039/C8CP07486K
Impact Factor 3.676
Authors

Tim Kohlmann, Martin Goez


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Abstract

We have conducted a theoretical and experimental study of Stern–Volmer experiments in micellar systems for the important case that fluorophore and quencher remain confined to their micelle during the luminescence decay (the “immobile probe/immobile quencher” scenario) and exhibit static quenching followed by dynamic quenching. By a comparative mathematical analysis, we have exposed inherent physical and mathematical contradictions of earlier theories. We present a general framework that allows a very simple derivation of consistent solutions. Even with the correct model, strong parameter correlations severely compromise fit uniqueness when the stationary luminescence is the only observable, but these correlations can be removed by parallel absorption measurements and do not occur in time-resolved luminescence experiments. The application of our protocol to pyrene quenching by substituted viologens in SDS micelles revealed a linear dependence of the apparent aggregation number of the surfactant on the equilibrium constant of formation of ground-state complexes, which can be quantitatively explained by a preference of the quencher for micelles containing the fluorophore. The complex formation is entropy controlled, as evidenced by a driving force that decreases linearly with the number of free rotors in the viologen sidechains.

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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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