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Formation Principles and Exciton Relaxation in Semiconductor Quantum Dot–Dye Nanoassemblies

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Quantum Dot Molecules

Part of the book series: Lecture Notes in Nanoscale Science and Technology ((LNNST,volume 14))

Abstract

In this chapter we discuss “bottom-up” non-covalent self-assembly principles which define a strategy for the formation of organic–inorganic nanoassemblies containing colloidal semiconductor quantum dots (QD) of different types (based on a CdSe core) and various heterocyclic molecules (dyes) with functionalized anchoring side substituents (meso-pyridyl substituted porphyrins and perylene diimides). Using a combination of ensemble and single molecule spectroscopy of “QD–Dye” nanoassemblies, we show that single functionalized molecules can be considered as extremely sensitive probes for studying the complex interface physics and chemistry (influence of the embedding environment and temperature) and related exciton relaxation processes in QDs. It will be quantitatively laid out that the major part of the observed QD photoluminescence (PL) quenching in nanoassemblies can be understood, on the one hand, in terms of exciton wave function tunneling under the condition of quantum confinement and, on the other hand, by the influence of ligand dynamics. In nanoassemblies, photoinduced Foerster-type energy transfer (FRET) QD → Dye is often only a small contribution to the PL quenching and is effectively suppressed already in slightly polar solvents which is often overlooked in literature. Finally we would like to point out that properties of “QD–Dye” nanoassemblies are not only interesting in themselves but also provide a valuable tool to study surface-related phenomena in QDs on an extremely low level of surface modification, thus providing the data for a further development of defined multi-component structures for exploitation as artificial light-harvesting complexes, electro- and photochemical devices or nanosensors.

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Acknowledgments

This work was supported by Volkswagen Foundation (Priority Program “Physics, Chemistry and Biology with Single Molecules”), DFG GRK 829/3 (“Accumulation of single molecules to nanostructures”), German Academic Exchange Service (DAAD, grant № A/08/08573, EZ), Belarussian Foundation for Basic Research (grant № Ф10СО-005), Belarussian State Program for Scientific Research “Convergence 3.2.08—Photophysics of Bioconjugates, Semiconductor and Metallic Nanostructures and Supramolecular Complexes and Their Biomedical Applications.” Prof. E. Zenkevich thanks B.I. Stepanov Institute of Physics NAS, Minsk, Belarus and the DFG FOR877 (“From local constraints to macroscopic transport”) for financial support. The first experiments in 2002 have only been possible by providing CdSe/ZnS QDs by Dr. A. Rogach (Ludwig-Maximilians-University Munich, Germany) and Dr. D. Talapin (University of Hamburg, Germany) which are gratefully acknowledged. We also thank Dr. A. Shulga (B.I. Stepanov Institute of Physics NAS, Minsk, Belarus) for the synthesis of all tetrapyrrole compounds including monomers and chemical dimers and Prof. F. Wuerthner (Wuerzburg University) for supplying all perylene diimide dyes. We thank Dr. Habil. E. Sagun, Dr. A. Stupak, Dr. V. Knyukshto, Dr. V. Galievsky, A. Stasheuski, and A. Yarovoi (B.I. Stepanov Institute of Physics NAS, Minsk, Belarus), who have performed many experiments in Minsk or in Chemnitz, Dr. T. Blaudeck (now at ENAS, Chemnitz), Dr. D. Kowerko (now at University of Zürich), S. Krause, Prof. M. Abdel-Mottaleb (now at Nile University, Centre for Nanotechnology, Cairo), K. Szwaykowska (now at California Institute of Technology), for performing mutual experiments, theoretical analysis, and fruitful discussions in Chemnitz. Titration and FRET experiments in TEHOS have been performed by F. Gerlach (now at Fibotec oberoptics GmbH, Meiningen, Germany). Dr. D. Kilin (now at the University of South Dakota, USA) has performed helpful calculations on QD–Dye nanoassemblies. We thank Prof. Dr. S.V. Gaponenko (B.I. Stepanov Institute of Physics, National Academy of Sciences, Minsk, Belarus) for fruitful discussion. We also thank Prof. F. Cichos (now at Molecular Nanophotonics, University of Leipzig, Germany) for stimulating and guiding many of the experiments.

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  1. Institute of Physics and Centre for Nanostructured Materials and Analytics (nanoMA), Chemnitz University of Technology, Reichenhainerstr. 70, Chemnitz, 09107, Germany

    Christian von Borczyskowski

  2. Department of Information Technologies and Robotics, National Technical University of Belarus, Prospect Nezavisimosti 65, Minsk, 220013, Belarus

    Eduard Zenkevich

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  1. Christian von Borczyskowski
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Correspondence to Christian von Borczyskowski .

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  1. State Key Laboratory of Electronic Thin, University of Electronic Science and Technology of China, Chengdu, People's Republic of China

    Jiang Wu

  2. State Key Laboratory of Electronic, University of Electronic Science and Technology, Chengdu, People's Republic of China

    Zhiming M. Wang

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von Borczyskowski, C., Zenkevich, E. (2014). Formation Principles and Exciton Relaxation in Semiconductor Quantum Dot–Dye Nanoassemblies. In: Wu, J., Wang, Z. (eds) Quantum Dot Molecules. Lecture Notes in Nanoscale Science and Technology, vol 14. Springer, New York, NY. https://doi.org/10.1007/978-1-4614-8130-0_4

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