TY - JOUR

T1 - Non-normality and non-monotonic dynamics in complex reaction networks

AU - Nicolaou, Zachary G.

AU - Nishikawa, Takashi

AU - Nicholson, Schuyler B.

AU - Green, Jason R.

AU - Motter, Adilson E.

N1 - Publisher Copyright:
© 2020 authors. Published by the American Physical Society.

PY - 2020/10/12

Y1 - 2020/10/12

N2 - Complex chemical reaction networks, which underlie many industrial and biological processes, often exhibit non-monotonic changes in chemical species concentrations. Such non-monotonic dynamics are in principle possible even in a linear model if the matrix defining the model is 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, at variance with the dominance of a single giant component observed in typical random reaction networks. The exact linearity of the master equation enables development of a rigorous theory and simulations for dynamical networks of unprecedented sizes (approaching 105 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.

AB - Complex chemical reaction networks, which underlie many industrial and biological processes, often exhibit non-monotonic changes in chemical species concentrations. Such non-monotonic dynamics are in principle possible even in a linear model if the matrix defining the model is 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, at variance with the dominance of a single giant component observed in typical random reaction networks. The exact linearity of the master equation enables development of a rigorous theory and simulations for dynamical networks of unprecedented sizes (approaching 105 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.

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U2 - 10.1103/PhysRevResearch.2.043059

DO - 10.1103/PhysRevResearch.2.043059

M3 - Article

AN - SCOPUS:85098617546

SN - 2643-1564

VL - 2

JO - Physical Review Research

JF - Physical Review Research

IS - 4

M1 - 043059

ER -