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Design of Viologen-Based Liquid Crystals Exhibiting Bicontinuous Cubic Phases and Their Redox-Active Behavior.

ABSTRACT: We have succeeded in developing viologen-based liquid-crystalline materials forming bicontinuous cubic phases. They are composed of amphiphilic zwitterions with a viologen ionic-head-group and sulfonyl-imide-type acids. In the bicontinuous cubic liquid-crystalline assemblies, the ionic-head groups of the amphiphiles align along a gyroid minimal surface, forming a 3D continuous viologen layer. The ionic state of the viologen-moieties can be tuned from a dication state (V2+) to a radical mono cation state (V1+•) by UV irradiation and/or electric field. This redox reaction proceeds in bulk, accompanying the change of their color from colorless to purple. Interestingly, they preserve the 3D molecular assembled structures beyond the redox reaction, which has been confirmed by polarizing optical microscopy and X-ray diffraction measurements.

SUBMITTER: Kobayashi T

PROVIDER: S-EPMC5706190 | biostudies-literature | 2017 Oct

REPOSITORIES: biostudies-literature

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Design of Viologen-Based Liquid Crystals Exhibiting Bicontinuous Cubic Phases and Their Redox-Active Behavior.

Kobayashi Tsubasa T Ichikawa Takahiro T

Materials (Basel, Switzerland) 20171027 11

We have succeeded in developing viologen-based liquid-crystalline materials forming bicontinuous cubic phases. They are composed of amphiphilic zwitterions with a viologen ionic-head-group and sulfonyl-imide-type acids. In the bicontinuous cubic liquid-crystalline assemblies, the ionic-head groups of the amphiphiles align along a gyroid minimal surface, forming a 3D continuous viologen layer. The ionic state of the viologen-moieties can be tuned from a dication state (<b>V<sup>2+</sup></b>) to a ...[more]

PMID: 29077001

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Project description:Nonlamellar lipid membranes are frequently induced by proteins that fuse, bend, and cut membranes. Understanding the mechanism of action of these proteins requires the elucidation of the membrane morphologies that they induce. While hexagonal phases and lamellar phases are readily identified by their characteristic solid-state NMR line shapes, bicontinuous lipid cubic phases are more difficult to discern, since the static NMR spectra of cubic-phase lipids consist of an isotropic (31)P or (2)H peak, indistinguishable from the spectra of isotropic membrane morphologies such as micelles and small vesicles. To date, small-angle X-ray scattering is the only method to identify bicontinuous lipid cubic phases. To explore unique NMR signatures of lipid cubic phases, we first describe the orientation distribution of lipid molecules in cubic phases and simulate the static (31)P chemical shift line shapes of oriented cubic-phase membranes in the limit of slow lateral diffusion. We then show that (31)P T2 relaxation times differ significantly between isotropic micelles and cubic-phase membranes: the latter exhibit 2 orders of magnitude shorter T2 relaxation times. These differences are explained by the different time scales of lipid lateral diffusion on the cubic-phase surface versus the time scales of micelle tumbling. Using this relaxation NMR approach, we investigated a DOPE membrane containing the transmembrane domain (TMD) of a viral fusion protein. The static (31)P spectrum of DOPE shows an isotropic peak, whose T2 relaxation times correspond to that of a cubic phase. Thus, the viral fusion protein TMD induces negative Gaussian curvature, which is an intrinsic characteristic of cubic phases, to the DOPE membrane. This curvature induction has important implications to the mechanism of virus-cell fusion. This study establishes a simple NMR diagnostic probe of lipid cubic phases, which is expected to be useful for studying many protein-induced membrane remodeling phenomena in biology.

Dataset Information

Design of Viologen-Based Liquid Crystals Exhibiting Bicontinuous Cubic Phases and Their Redox-Active Behavior.

Publications

Design of Viologen-Based Liquid Crystals Exhibiting Bicontinuous Cubic Phases and Their Redox-Active Behavior.

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