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Stimuli-Directed Dynamic Reconfiguration in Self-Organized Helical Superstructures Enabled by Chemical Kinetics of Chiral Molecular Motors.

ABSTRACT: Dynamic controllability of self-organized helical superstructures in spatial dimensions is a key step to promote bottom-up artificial nanoarchitectures and functional devices for diverse applications in a variety of areas. Here, a light-driven chiral overcrowded alkene molecular motor with rod-like substituent is designed and synthesized, and its thermal isomerization reaction exhibits an increasing structural entropy effect on chemical kinetic analysis in anisotropic achiral liquid crystal host than that in isotropic organic liquid. Interestingly, the stimuli-directed angular orientation motion of helical axes in the self-organized helical superstructures doped with the chiral motors enables the dynamic reconfiguration between the planar (thermostationary) and focal conic (photostationary) states. The reversible micromorphology deformation processes are compatible with the free energy fluctuation of self-organized helical superstructures and the chemical kinetics of chiral motors under different conditions. Furthermore, stimuli-directed reversible nonmechanical beam steering is achieved in dynamic hidden periodic photopatterns with reconfigurable attributes prerecorded with a corresponding photomask and photoinduced polymerization.

SUBMITTER: Sun J

PROVIDER: S-EPMC5827101 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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Stimuli-Directed Dynamic Reconfiguration in Self-Organized Helical Superstructures Enabled by Chemical Kinetics of Chiral Molecular Motors.

Sun Jian J Lan Ruochen R Gao Yanzi Y Wang Meng M Zhang Wanshu W Wang Ling L Zhang Lanying L Yang Zhou Z Yang Huai H

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20171201 2

Dynamic controllability of self-organized helical superstructures in spatial dimensions is a key step to promote bottom-up artificial nanoarchitectures and functional devices for diverse applications in a variety of areas. Here, a light-driven chiral overcrowded alkene molecular motor with rod-like substituent is designed and synthesized, and its thermal isomerization reaction exhibits an increasing structural entropy effect on chemical kinetic analysis in anisotropic achiral liquid crystal host ...[more]

PMID: 29619309

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Project description:Photon-to-matter chirality transfer offers both simplicity and universality to chiral synthesis, but its efficiency is typically low for organic compounds. Besides the fundamental importance of this process relevant for understanding the origin of homochirality on Earth, new pathways for imposing chiral bias during chemical process are essential for a variety of technologies from medicine to informatics. The strong optical activity of inorganic nanoparticles (NPs) affords photosynthetic routes to chiral superstructures using circularly polarized photons. Although plasmonic NPs are promising candidates for such synthetic routes due to the strong rotatory power of highly delocalized plasmonic states (Ma et al. Chem. Rev. 2017, 117 (12), 8041), realization of light-driven synthesis of chiral nanostructures has been more challenging for plasmonic NPs than for the semiconductor due to the short lifetime of the plasmonic states. Here we show that illumination of gold salt solutions with circularly polarized light induces the formation of NPs and their subsequent assembly into chiral nanostructures 10-15 nm in diameter. Despite their seemingly irregular shape, the resulting nanocolloids showed circular dichroism (CD) spectra with opposite polarity after exposure to photons with left and right circular polarization. The sign and spectral position of the CD peaks of illuminated dispersions matched those calculated for nanostructures with complex geometry identified from electron tomography images. Quantification of the complex shapes of NP assemblies using chirality measures revealed a direct correlation with the experimental spectra. The light-driven assembly of chiral nanostructures originates from the asymmetric displacement of NPs in dynamic assemblies by plasmonic fields followed by particle-to-particle attachment. The ability of gold NPs to "lock" the chirality of the incident photons in assembled nanostructures can be used to create a variety of chiral nanomaterials with plasmonic resonances.

Dataset Information

Stimuli-Directed Dynamic Reconfiguration in Self-Organized Helical Superstructures Enabled by Chemical Kinetics of Chiral Molecular Motors.

Publications

Stimuli-Directed Dynamic Reconfiguration in Self-Organized Helical Superstructures Enabled by Chemical Kinetics of Chiral Molecular Motors.

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