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Chiral shape fluctuations and the origin of chirality in cholesteric phases of DNA origamis

Maxime M. C. Tortora, Garima Mishra, Domen PreŇ°ern and Jonathan P.K. Doye

Sci. Adv. 6, eaaw8331 (2020)


Lyotropic cholesteric liquid crystal (LCLC) phases are commonly observed in many biological and synthetic polymer solutions, which are characterised by a complex interplay between thermal fluctuations, entropic and enthalpic forces. The elucidation of the link between local molecular features and macroscopic chiral structure, and of the relative roles of these competing microscopic contributions on cholesteric organisation, remains a major open question in liquid crystal science. Here, we provide theoretical evidence of a novel mechanism of chirality amplification in LCLC phases of DNA origami filaments, whereby the emergence of phase chirality is governed by long-ranged helical fluctuations in their molecular backbone conformations, which may be attributed to the internal mechanical stresses underlying the origami folding process. Our results compare favourably to recent experimental studies of cholesteric phases of DNA origamis and demonstrate the importance of intra-molecular mechanics for the supra-molecular self-assembly of LCLCs, with potential implications for a broad class of experimentally-relevant colloidal systems.

The full paper is available from Science Advances and arXiv.org.