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Uniform shape monodisperse single chain nanocrystals by living aqueous catalytic polymerization.

ABSTRACT: The preparation of polymer nanoparticles with a uniform size and shape, beyond spheres, is an unresolved problem. Here we report a living aqueous catalytic polymerization, resulting in particles grown by a single active site and composed of a single ultra high molecular weight polyethylene (UHMWPE) chain. The control on a molecular level (M_w/M_n?=?1.1-1.2) and at the same time on a particle level (PDI??10 wt-% (N???10¹⁹ particles L^-1) polymer content. Key to this robust procedure to single chain nanoparticles are long-lived water-stable Ni(II) catalysts that do not undergo any chain transfer. These findings are a relevant step towards polymer materials based on nanoparticle assembly.

SUBMITTER: Schnitte M

PROVIDER: S-EPMC6565736 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Uniform shape monodisperse single chain nanocrystals by living aqueous catalytic polymerization.

Schnitte Manuel M Staiger Anne A Casper Larissa A LA Mecking Stefan S

Nature communications 20190613 1

The preparation of polymer nanoparticles with a uniform size and shape, beyond spheres, is an unresolved problem. Here we report a living aqueous catalytic polymerization, resulting in particles grown by a single active site and composed of a single ultra high molecular weight polyethylene (UHMWPE) chain. The control on a molecular level (M<sub>w</sub>/M<sub>n</sub> = 1.1-1.2) and at the same time on a particle level (PDI < 0.05) together with the immediate deposition of the growing chain on the ...[more]

PMID: 31197178

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Project description:Ligand-capped nanocrystals (NCs) of lead halide perovskites, foremost fully inorganic CsPbX3 NCs, are the latest generation of colloidal semiconductor quantum dots. They offer a set of compelling characteristics-large absorption cross section, as well as narrow, fast, and efficient photoluminescence with long exciton coherence times-rendering them attractive for applications in light-emitting devices and quantum optics. Monodisperse and shape-uniform, broadly size-tunable, scalable, and robust NC samples are paramount for unveiling their basic photophysics, as well as for putting them into use. Thus far, no synthesis method fulfilling all these requirements has been reported. For instance, long-chain zwitterionic ligands impart the most durable surface coating, but at the expense of reduced size uniformity of the as-synthesized colloid. In this work, we demonstrate that size-selective precipitation of CsPbBr3 NCs coated with a long-chain sulfobetaine ligand, namely, 3-(N,N-dimethyloctadecylammonio)-propanesulfonate, yields monodisperse and sizable fractions (>100 mg inorganic mass) with the mean NC size adjustable in the range between 3.5 and 16 nm and emission peak wavelength between 479 and 518 nm. We find that all NCs exhibit an oblate cuboidal shape with the aspect ratio of 1.2 × 1.2 × 1. We present a theoretical model (effective mass/k·p) that accounts for the anisotropic NC shape and describes the size dependence of the first and second excitonic transition in absorption spectra and explains room-temperature exciton lifetimes. We also show that uniform zwitterion-capped NCs readily form long-range ordered superlattices upon solvent evaporation. In comparison to more conventional ligand systems (oleic acid and oleylamine), supercrystals of zwitterion-capped NCs exhibit larger domain sizes and lower mosaicity. Both kinds of supercrystals exhibit superfluorescence at cryogenic temperatures-accelerated collective emission arising from the coherent coupling of the emitting dipoles.

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Uniform shape monodisperse single chain nanocrystals by living aqueous catalytic polymerization.

Publications

Uniform shape monodisperse single chain nanocrystals by living aqueous catalytic polymerization.

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