Dataset Information

Solvent Mixing To Induce Molecular Motor Aggregation into Bowl-Shaped Particles: Underlying Mechanism, Particle Nature, and Application To Control Motor Behavior.

ABSTRACT: Control over dynamic functions in larger assemblies is key to many molecular systems, ranging from responsive materials to molecular machines. Here we report a molecular motor that forms bowl-shaped particles in water and how confinement of the molecular motor affects rotary motion. Studying the aggregation process in a broader context, we provide evidence that, in the case of bowl-shaped particles, the structures are not the product of self-assembly, but a direct result of the mixing a good solvent and a (partial) non-solvent and highly independent of the molecular design. Under the influence of the non-solvent, droplets are formed, of which the exterior is hardened due to the increase in the glass transition temperature by the external medium, while the interior of the droplets remains plasticized by the solvent, resulting in the formation of stable bowl-shaped particles with a fluid interior, a glass-like exterior, and a very specific shape: dense spheres with a hole in their side. Applying this to a bulky first-generation molecular motor allowed us to change its isomerization behavior. Furthermore, the motor shows in situ photo-switchable aggregation-induced emission. Strong confinement prohibits the thermal helix inversion step while altering the energy barriers that determine the rotary motion, such that it introduces a reverse trans- cis isomerization upon heating. These studies show a remarkable control of forward and backward rotary motion by simply changing solvent ratios and extent of confinement.

SUBMITTER: Franken LE

PROVIDER: S-EPMC6026844 | biostudies-literature | 2018 Jun

REPOSITORIES: biostudies-literature

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Solvent Mixing To Induce Molecular Motor Aggregation into Bowl-Shaped Particles: Underlying Mechanism, Particle Nature, and Application To Control Motor Behavior.

Franken Linda E LE Wei Yuchen Y Chen Jiawen J Boekema Egbert J EJ Zhao Depeng D Stuart Marc C A MCA Feringa Ben L BL

Journal of the American Chemical Society 20180619 25

Control over dynamic functions in larger assemblies is key to many molecular systems, ranging from responsive materials to molecular machines. Here we report a molecular motor that forms bowl-shaped particles in water and how confinement of the molecular motor affects rotary motion. Studying the aggregation process in a broader context, we provide evidence that, in the case of bowl-shaped particles, the structures are not the product of self-assembly, but a direct result of the mixing a good sol ...[more]

PMID: 29879351

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Project description:A time series of experiments at high temperature have been performed to investigate the influence of particle settling on magma mixing. A natural rhyolite glass was held above a natural basalt glass in a platinum crucible. After melting of the glasses at superliquidus temperatures, a platinum sphere was placed on the upper surface of the rhyolitic melt and sank into the experimental column (rhyolitic melt above basaltic melt). Upon falling through the rhyolitic-basaltic melt interface, the Pt sphere entrained a filament of rhyolitic melt in its further fall. The quenched products of the experiments were imaged using X-ray microCT methods. The images of our time series of experiments document the formation of a rhyolite filament as it is entrained into the underlying basalt by the falling platinum sphere. When the Pt particle reached the bottom of the crucible, the entrained rhyolitic filament started to ascend buoyantly up to the initial rhyolitic-basaltic interface. This generated a significant thickness increase of a comingled "melange" layer at the interface due to "liquid rope coiling" and piling up of the filament. As a consequence, the basalt/rhyolite interface was greatly enlarged and diffusive hybridisation greatly accelerated. Further, bubbles, originating at the interface, are observed to have risen into the overlying rhyolite dragging basalt filaments with them. Upon crossing the basalt/rhyolite interface, the bubbles have non-spherical shapes as they adapt to the differing surface tensions of basaltic and rhyolitic melts. Major element profiles, measured across the rhyolite filaments, exhibit asymmetrical shapes from the rhyolite into the basalt. Na and Ti reveal uphill diffusion from the rhyolite towards the interface in the filament cross sections. These results reveal the potential qualitative complexity of the mingling process between rhyolitic and basaltic magmas in the presence of sinking crystals. They imply that crystal-rich magma mingling may be expected to be accelerated with respect to crystal-poor systems. We urge the further fluid dynamic analysis of these phenomena, obtainable for the first time using detailed tomographic imaging.

Dataset Information

Solvent Mixing To Induce Molecular Motor Aggregation into Bowl-Shaped Particles: Underlying Mechanism, Particle Nature, and Application To Control Motor Behavior.

Publications

Solvent Mixing To Induce Molecular Motor Aggregation into Bowl-Shaped Particles: Underlying Mechanism, Particle Nature, and Application To Control Motor Behavior.

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