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一种用于益生元同手性进化的扩展模型:一种自下而上探索生命起源的方法。

An extended model for the evolution of prebiotic homochirality: a bottom-up approach to the origin of life.

作者信息

Gleiser Marcelo, Walker Sara Imari

机构信息

Department of Physics and Astronomy, Dartmouth College Hanover, Hanover, NH 03755, USA.

出版信息

Orig Life Evol Biosph. 2008 Aug;38(4):293-315. doi: 10.1007/s11084-008-9134-5. Epub 2008 May 9.

Abstract

A generalized autocatalytic model for chiral polymerization is investigated in detail. Apart from enantiomeric cross-inhibition, the model allows for the autogenic (non-catalytic) formation of left and right-handed monomers from a substrate with reaction rates epsilon L and epsilon R, respectively. The spatiotemporal evolution of the net chiral asymmetry is studied for models with several values of the maximum polymer length, N. For N = 2, we study the validity of the adiabatic approximation often cited in the literature. We show that the approximation obtains the correct equilibrium values of the net chirality, but fails to reproduce the short time behavior. We show also that the autogenic term in the full N = 2 model behaves as a control parameter in a chiral symmetry-breaking phase transition leading to full homochirality from racemic initial conditions. We study the dynamics of the N--> infinity model with symmetric (epsilon L = epsilon R) autogenic formation, showing that it only achieves homochirality for epsilon > epsilon c, where epsilon c is an N-dependent critical value. For epsilon <or= epsilon c we investigate the behavior of models with several values of N, showing that the net chiral asymmetry grows as tanh(N). We show that for a given symmetric autogenic reaction rate, the net chirality and the concentrations of chirally pure polymers increase with the maximum polymer length in the model. We briefly discuss the consequences of our results for the development of homochirality in prebiotic Earth and possible experimental verification of our findings.

摘要

详细研究了一种用于手性聚合的广义自催化模型。除了对映体交叉抑制外,该模型还允许从底物分别以反应速率εL和εR自发生成左旋和右旋单体。针对具有几个最大聚合物长度N值的模型,研究了净手性不对称的时空演化。对于N = 2,我们研究了文献中经常引用的绝热近似的有效性。我们表明,该近似获得了净手性的正确平衡值,但未能重现短时间行为。我们还表明,完整的N = 2模型中的自发生成项在手性对称性破缺相变中表现为控制参数,从外消旋初始条件导致完全同手性。我们研究了具有对称(εL = εR)自发生成的N→∞模型的动力学,表明只有当ε>εc时它才会实现同手性,其中εc是一个与N有关的临界值。对于ε≤εc,我们研究了具有几个N值的模型的行为,表明净手性不对称随tanh(N)增长。我们表明,对于给定的对称自发生成反应速率,模型中的净手性和手性纯聚合物的浓度随最大聚合物长度增加。我们简要讨论了我们的结果对前生物地球中同手性发展的影响以及对我们发现的可能实验验证。

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