Department of Chemistry, Ludwig-Maximilians-Universität München, Butenandtstr. 5-13, 81377, Munich, Germany.
Max-Planck-Institute for Astronomy, Königstuhl 17, 69117, Heidelberg, Germany.
Orig Life Evol Biosph. 2022 Sep;52(1-3):75-91. doi: 10.1007/s11084-022-09627-6. Epub 2022 Aug 19.
To understand chiral symmetry breaking on the molecular level, we developed a method to efficiently investigate reaction kinetics of single molecules. The model systems include autocatalysis as well as a reaction cascade to gain further insight into the prebiotic origin of homochirality. The simulated reactions start with a substrate and only a single catalyst molecule, and the occurrence of symmetry breaking was examined for its degree of dependence on randomness. The results demonstrate that interlocking processes, which e.g., form catalysts, autocatalytic systems, or reaction cascades that build on each other and lead to a kinetic acceleration, can very well amplify a statistically occurring symmetry breaking. These results suggest a promising direction for the experimental implementation and identification of such processes, which could have led to a shift out of thermodynamic equilibrium in the emergence of life.
为了在分子水平上理解手性对称破缺，我们开发了一种高效的方法来研究单个分子的反应动力学。模型系统包括自催化以及反应级联，以深入了解手性的前生物起源。模拟反应从一个底物和单个催化剂分子开始，并检查对称性破缺的程度与其随机性的依赖关系。结果表明，互锁过程（例如形成催化剂、自催化系统或相互依存并导致动力学加速的反应级联）可以很好地放大统计上发生的对称性破缺。这些结果为实验实施和识别此类过程提供了一个很有前途的方向，这些过程可能导致生命出现时从热力学平衡中转移。
