Mechanically induced homochirality in nucleated enantioselective polymerization

Celia Blanco, Michael Stich, David Hochberg*

*Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review


    Understanding how biological homochirality may have emerged during chemical
    evolution remains a challenge for origin of life research. In keeping with this goal, we introduce and solve numerically a kinetic rate equation model of nucleated cooperative enantioselective polymerization in closed systems. The microreversible scheme includes (i) solution phase racemization of the monomers, (ii) linear chain growth by stepwise monomer attachment, in both the nucleation and elongation phases, and (iii) annealing or fusion of homochiral chains. Mechanically induced breakage of the longest chains maintains the system out of equilibrium and drives a breakage-fusion recycling mechanism. Spontaneous mirror symmetry breaking (SMSB) can be achieved starting from small initial enantiomeric excesses due to the intrinsic statistical fluctuations about the idealized racemic composition. The subsequent chiral amplification confirms the model’s capacity for absolute asymmetric synthesis, and without chiral cross-inhibition and without explicit autocatalysis.
    Original languageEnglish
    Pages (from-to)942–955
    Number of pages14
    JournalJournal of Physical Chemistry: Part B
    Issue number5
    Early online date10 Jan 2017
    Publication statusPublished - 9 Feb 2017

    Bibliographical note

    This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry B, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see DOI 10.1021/acs.jpcb.6b10705.


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