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Main Authors: Laurent, Gabin, Göppel, Tobias, Lacoste, David, Gerland, Ulrich
Format: Preprint
Published: 2023
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Online Access:https://arxiv.org/abs/2311.04677
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author Laurent, Gabin
Göppel, Tobias
Lacoste, David
Gerland, Ulrich
author_facet Laurent, Gabin
Göppel, Tobias
Lacoste, David
Gerland, Ulrich
contents RNA in extant biological systems is homochiral; it consists exclusively of D-ribonucleotides rather than L-ribonucleotides. How the homochirality of RNA emerged is not known. Here, we use stochastic simulations to quantitatively explore the conditions for RNA homochirality to emerge in the prebiotic scenario of an RNA reactor, in which RNA strands react in a non-equilibrium environment. These reactions include the hybridization, dehybridization, template-directed ligation, and cleavage of RNA strands. The RNA reactor is either closed, with a finite pool of ribonucleotide monomers of both chiralities (D and L), or the reactor is open, with a constant inflow of a racemic mixture of monomers. For the closed reactor, we also consider the interconversion between D and L monomers via a racemization reaction. We first show that template-free polymerization is unable to reach a high degree of homochirality, due to the lack of autocatalytic amplification. In contrast, in the presence of template-directed ligation, with base pairing and stacking between bases of the same chirality thermodynamically favored, a high degree of homochirality can arise and be maintained, provided the non equilibrium environment overcomes product inhibition, for instance via temperature cycling. Furthermore, if the experimentally observed kinetic stalling of ligation after chiral mismatches is also incorporated, the RNA reactor can evolve towards a fully homochiral state, in which one chirality is entirely lost. This is possible because the kinetic stalling after chiral mismatches effectively implements a chiral cross-inhibition process. Taken together, our model supports a scenario where the emergence of homochirality is assisted by template-directed ligation and polymerization in a non equilibrium RNA reactor.
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publishDate 2023
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spellingShingle Emergence of homochirality via template-directed ligation in an RNA reactor
Laurent, Gabin
Göppel, Tobias
Lacoste, David
Gerland, Ulrich
Biological Physics
RNA in extant biological systems is homochiral; it consists exclusively of D-ribonucleotides rather than L-ribonucleotides. How the homochirality of RNA emerged is not known. Here, we use stochastic simulations to quantitatively explore the conditions for RNA homochirality to emerge in the prebiotic scenario of an RNA reactor, in which RNA strands react in a non-equilibrium environment. These reactions include the hybridization, dehybridization, template-directed ligation, and cleavage of RNA strands. The RNA reactor is either closed, with a finite pool of ribonucleotide monomers of both chiralities (D and L), or the reactor is open, with a constant inflow of a racemic mixture of monomers. For the closed reactor, we also consider the interconversion between D and L monomers via a racemization reaction. We first show that template-free polymerization is unable to reach a high degree of homochirality, due to the lack of autocatalytic amplification. In contrast, in the presence of template-directed ligation, with base pairing and stacking between bases of the same chirality thermodynamically favored, a high degree of homochirality can arise and be maintained, provided the non equilibrium environment overcomes product inhibition, for instance via temperature cycling. Furthermore, if the experimentally observed kinetic stalling of ligation after chiral mismatches is also incorporated, the RNA reactor can evolve towards a fully homochiral state, in which one chirality is entirely lost. This is possible because the kinetic stalling after chiral mismatches effectively implements a chiral cross-inhibition process. Taken together, our model supports a scenario where the emergence of homochirality is assisted by template-directed ligation and polymerization in a non equilibrium RNA reactor.
title Emergence of homochirality via template-directed ligation in an RNA reactor
topic Biological Physics
url https://arxiv.org/abs/2311.04677