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Anisotropic Polyethylene Nanocrystals Labeled with a Single Fluorescent Dye Molecule : Towards Monitoring of Nanoparticle Orientation

Anisotropic Polyethylene Nanocrystals Labeled with a Single Fluorescent Dye Molecule : Towards Monitoring of Nanoparticle Orientation

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SCHEINHARDT, Benjamin, Justyna TRZASKOWSKI, Moritz C. BAIER, Beate STEMPFLE, Alex OPPERMANN, Dominik WÖLL, Stefan MECKING, 2013. Anisotropic Polyethylene Nanocrystals Labeled with a Single Fluorescent Dye Molecule : Towards Monitoring of Nanoparticle Orientation. In: Macromolecules. 46(19), pp. 7902-7910. ISSN 0024-9297. eISSN 1520-5835

@article{Scheinhardt2013Aniso-24501, title={Anisotropic Polyethylene Nanocrystals Labeled with a Single Fluorescent Dye Molecule : Towards Monitoring of Nanoparticle Orientation}, year={2013}, doi={10.1021/ma401828k}, number={19}, volume={46}, issn={0024-9297}, journal={Macromolecules}, pages={7902--7910}, author={Scheinhardt, Benjamin and Trzaskowski, Justyna and Baier, Moritz C. and Stempfle, Beate and Oppermann, Alex and Wöll, Dominik and Mecking, Stefan} }

Trzaskowski, Justyna Oppermann, Alex Wöll, Dominik Mecking, Stefan The three-dimensional orientation monitoring of anisotropic nanoparticles during dynamic processes is a fundamental issue. Herein we show that incorporation of a single fluorescent reporter molecule is a promising concept toward this goal. As a model system, shape anisotropic single lamella polyethylene (PE) nanocrystals bearing one single fluorescent reporter molecule were prepared via ring-opening metathesis polymerization (ROMP) of highly ring-strained trans-cyclooctene (trCOE) using a mixture of a dye-functionalized ruthenium-based initiator (1; perylene diimide (PDI) substituted Hoveyda–Grubbs second generation Ru alkylidene) and an appropriate excess of the unlabeled analogue (2; Hoveyda–Grubbs second generation Ru alkylidene) in aqueous microemulsion as a key step and subsequent exhaustive hydrogenation (>99.9%) of the main-chain unsaturated polymer in the nanoparticles to yield nanocrystals of high molecular weight, strictly linear PE (Mn = 8 × 105 g mol–1; Mw/Mn = 1.4). TEM and AFM show a particle thickness of ca. 12 nm with a lateral extension of typically 45 nm. Comparable initiation kinetics of both complexes 1 and 2, which is a key requirement for this approach, were revealed by fluorescence spectroscopy studies (ΔH‡ = 57.4 kJ mol–1, ΔS‡ = −73.0 J mol–1 K–1 for 1 vs ΔH‡ = 63.6 kJ mol–1, ΔS‡ = −80.8 J mol–1 K–1 for 2 for the initiation with n-butyl vinyl ether, respectively). The labeled nanocrystals were characterized by means of single molecule fluorescence spectroscopy. Orientational analysis via defocused wide-field fluorescence microscopy (DWFM) revealed a fixed orientation of the chromophores within the nanocrystals, with their long molecular axis predominantly oriented parallel to the polar axis of the nanoparticles. Scheinhardt, Benjamin 2013-09-30T12:30:08Z Anisotropic Polyethylene Nanocrystals Labeled with a Single Fluorescent Dye Molecule : Towards Monitoring of Nanoparticle Orientation deposit-license Stempfle, Beate Trzaskowski, Justyna Oppermann, Alex eng Baier, Moritz C. Scheinhardt, Benjamin 2013 Wöll, Dominik Macromolecules ; 46 (2013), 19. - S. 7902-7910 Mecking, Stefan Stempfle, Beate Baier, Moritz C. 2013-09-30T12:30:08Z

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