论文标题
复杂反应网络中的非正常和非单调动力学
Non-normality and non-monotonic dynamics in complex reaction networks
论文作者
论文摘要
基于许多工业和生物学过程的复杂化学反应网络通常在化学物种浓度中表现出非单调的变化,通常使用非线性模型进行描述。即使在线性模型中,如果定义模型的矩阵是非正常的,则这些非单调动力学也是可能的,其特征是必然是非正交的特征向量值集。但是,非正式对非单调行为负责的程度仍然是一个悬而未决的问题。在这里,使用主方程对反应动力学进行建模,我们得出了观察单个物种非单调动力学的一般条件,确定非正态性促进了非单调性,但并不需要它。相比之下,我们表明非正常性是在Rényi熵中观察到的非单调动力学的要求。使用氢燃烧作为示例应用,我们证明了在实验条件下的非单调动力学由线性连接组件的线性链支持,与在典型的随机反应网络中观察到的单个巨型组件的优势相反。主方程的确切线性性使得对前所未有的大小的动态网络进行了严格的理论和模拟的开发(接近$ 10^5 $动力学变量,即使对于只有20个反应和少于100个原子的网络)。我们的结论有望在其他燃烧过程中得出,我们开发的一般理论适用于所有化学反应网络,包括生物学反应网络。
Complex chemical reaction networks, which underlie many industrial and biological processes, often exhibit non-monotonic changes in chemical species concentrations, typically described using nonlinear models. Such non-monotonic dynamics are in principle possible even in linear models if the matrices defining the models are non-normal, as characterized by a necessarily non-orthogonal set of eigenvectors. However, the extent to which non-normality is responsible for non-monotonic behavior remains an open question. Here, using a master equation to model the reaction dynamics, we derive a general condition for observing non-monotonic dynamics of individual species, establishing that non-normality promotes non-monotonicity but is not a requirement for it. In contrast, we show that non-normality is a requirement for non-monotonic dynamics to be observed in the Rényi entropy. Using hydrogen combustion as an example application, we demonstrate that non-monotonic dynamics under experimental conditions are supported by a linear chain of connected components, in contrast with the dominance of a single giant component observed in typical random reaction networks. The exact linearity of the master equation enables development of rigorous theory and simulations for dynamical networks of unprecedented size (approaching $10^5$ dynamical variables, even for a network of only 20 reactions and involving less than 100 atoms). Our conclusions are expected to hold for other combustion processes, and the general theory we develop is applicable to all chemical reaction networks, including biological ones.