Necessary conditions for the emergence of homochirality via autocatalytic self-replication

Abstract

We analyze a recent proposal for spontaneous mirror symmetry breaking based on the coupling of first-order enantioselective autocatalysis and direct production of the enantiomers that invokes a critical role for intrinsic reaction noise. For isolated systems, the racemic state is the unique stable outcome for both stochastic and deterministic dynamics when the system is in compliance with the constraints dictated by the thermodynamics of chemical reaction processes. In open systems, the racemic outcome also results for both stochastic and deterministic dynamics when driving the auto-catalysis unidirectionally by external reagents. Nonracemic states can result in the latter only if the reverse reactions are strictly zero: these are kinetically controlled outcomes for small populations and volumes, and can be simulated by stochastic dynamics. However, the stability of the thermodynamic limit proves that the racemic outcome is the unique stable state for strictly irreversible externally driven autocatalysis. These findings contradict the suggestion that the inhibition requirement of the Frank autocatalytic model for the emergence of homochirality may be relaxed in a noise-induced mechanism.

Publication DOI: https://doi.org/10.1063/1.4961021
Divisions: College of Engineering & Physical Sciences > Systems analytics research institute (SARI)
Additional Information: Copyright 2016 Acoustical Society of America. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the Acoustical Society of America. The following article appeared in Stich, M., Ribó, J. M., Blackmond, D. G., & Hochberg, D. (2016). Necessary conditions for the emergence of homochirality via autocatalytic self-replication. Journal of Chemical Physics, 145, [074111] and may be found at http://link.aip.org/link/?JCP/145/7/074111
Uncontrolled Keywords: General Physics and Astronomy,Physical and Theoretical Chemistry
Publication ISSN: 1089-7690
Last Modified: 01 Oct 2024 17:04
Date Deposited: 31 Aug 2016 14:55
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Related URLs: http://www.scop ... tnerID=8YFLogxK (Scopus URL)
PURE Output Type: Article
Published Date: 2016-08-18
Accepted Date: 2016-08-02
Submitted Date: 2016-05-13
Authors: Stich, Michael (ORCID Profile 0000-0001-8862-1044)
Ribó, Josep M.
Blackmond, Donna G.
Hochberg, David

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