手性自催化:镜像对称破缺中的反应噪声、微观可逆性和手性抑制
Chiral autocatalysis: reaction noise, micro-reversibility and chiral inhibition in mirror symmetry breaking
摘要:
应用详细平衡原理所规定的约束,我们分析了最近提出的自发镜像对称性破缺(SMSB)的提议,该提议基于与对映体线性衰变耦合的对映选择性自催化作用以及反应噪音的存在。我们发现外消旋状态是确定性以及随机动力学的最终稳定结果,以及良好的混合和小的空间耦合系统。即使在明显的非平衡条件下,自催化循环由外部试剂不可逆地驱动时,也会产生外消旋产物。我们的研究结果表明,一阶自动催化耦合到涉及\textit{non-linear}异手性动力学的反应是一个必要的先决条件,任何机制声称导致分子的同手性。
英文摘要:
Applying the constraints dictated by the principle of detailed balance, we analyze a recent proposal for spontaneous mirror symmetry breaking (SMSB) based on enantioselective autocatalysis coupled to a linear decay of the enantiomers and in the presence of reaction noise. We find the racemic state is the final stable outcome for both deterministic as well as for stochastic dynamics, and for both well-mixed and small spatially-coupled systems. The racemic outcome results even when the autocatalytic cycles are driven irreversibly by external reagents, in manifestly non-equilibrium conditions. Our findings suggest that first-order autocatalysis coupled to reactions involving \textit{non-linear} heterochiral dynamics is a necessary pre-condition for any mechanism purporting to lead to molecular homochirality.
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