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催化反应网络中普遍存在的“玻璃态”弛豫。

Ubiquitous "glassy" relaxation in catalytic reaction networks.

作者信息

Awazu Akinori, Kaneko Kunihiko

机构信息

Department of Mathematical and Life Sciences, Hiroshima University, Kagami-yama 1-3-1, Higashi-Hiroshima 739-8526, Japan.

出版信息

Phys Rev E Stat Nonlin Soft Matter Phys. 2009 Oct;80(4 Pt 1):041931. doi: 10.1103/PhysRevE.80.041931. Epub 2009 Oct 30.

Abstract

Study of reversible catalytic reaction networks is important not only as an issue for chemical thermodynamics but also for protocells. From extensive numerical simulations and theoretical analysis, slow relaxation dynamics to sustain nonequlibrium states are commonly observed. These dynamics show two types of salient behaviors that are reminiscent of glassy behavior: slow relaxation along with the logarithmic time dependence of the correlation function and the emergence of plateaus in the relaxation-time course. The former behavior is explained by the eigenvalue distribution of a Jacobian matrix around the equilibrium state that depends on the distribution of kinetic coefficients of reactions. The latter behavior is associated with kinetic constraints rather than metastable states and is due to the absence of catalysts for chemicals in excess and the negative correlation between two chemical species. Examples are given and generality is discussed with relevance to bottleneck-type dynamics in biochemical reactions as well.

摘要

可逆催化反应网络的研究不仅对化学热力学很重要,对原始细胞也很重要。通过广泛的数值模拟和理论分析,通常会观察到维持非平衡态的缓慢弛豫动力学。这些动力学表现出两种显著行为,让人联想到玻璃态行为:相关函数的对数时间依赖性导致的缓慢弛豫以及弛豫时间过程中平台的出现。前一种行为可以通过平衡态附近雅可比矩阵的本征值分布来解释,该分布取决于反应动力学系数的分布。后一种行为与动力学约束而非亚稳态有关,是由于缺乏过量化学物质的催化剂以及两种化学物质之间的负相关。文中给出了示例,并讨论了与生化反应中的瓶颈型动力学相关的普遍性。

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