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  • Title: Development of Polar Order by Liquid-Crystal Self-Assembly of Weakly Bent Molecules.
    Author: Alaasar M, Prehm M, Poppe S, Tschierske C.
    Journal: Chemistry; 2017 Apr 24; 23(23):5541-5556. PubMed ID: 28195374.
    Abstract:
    Organic ferroelectrics are of growing importance for multifunctional materials. Here we provide an understanding of the distinct stages of the development of sterically induced polar order in liquid-crystalline (LC) soft matter. Three series of weakly bent molecules derived from 4-cyanoresorcinol as the bent core unit with laterally fluorinated azobenzene wings have been synthesized, and the effects of the position of fluorine substitution, alkyl-chain length, and temperature on the LC self-assembly and polar order were studied. In the LC phases a paraelectric-ferroelectric transition took place as the size of the polar domains gradually increased, thereby crossing a permittivity maximum, similar to inorganic solid-state ferroelectrics. An increase in polar coherence length simultaneously led to a transition from synpolar to antipolar domain correlation in the high-permittivity paraelectric range. Associated with the emergence of polar order was the development of a tilted organization of the molecules and a growing coherence of tilt. This led to a transition from non-tilted via tilt-randomized uniaxial to long-range-tilted biaxial smectic phases, and to surface-stabilized symmetry breaking with the formation of chiral conglomerates and field-induced tilt. Moreover, there is a remarkably strong effect of the position of fluorination; polar order is favored by peripheral core substitution and is suppressed by inside-directed fluorination.
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