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Efficient Stochastic Simulations of Complex Reaction Networks on Surfaces

机译:基于maTLaB的复杂反应网络的有效随机模拟   面

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摘要

Surfaces serve as highly efficient catalysts for a vast variety of chemicalreactions. Typically, such surface reactions involve billions of moleculeswhich diffuse and react over macroscopic areas. Therefore, stochasticfluctuations are negligible and the reaction rates can be evaluated using rateequations, which are based on the mean-field approximation. However, in casethat the surface is partitioned into a large number of disconnected microscopicdomains, the number of reactants in each domain becomes small and it stronglyfluctuates. This is, in fact, the situation in the interstellar medium, wheresome crucial reactions take place on the surfaces of microscopic dust grains.In this case rate equations fail and the simulation of surface reactionsrequires stochastic methods such as the master equation. However, in the caseof complex reaction networks, the master equation becomes infeasible becausethe number of equations proliferates exponentially. To solve this problem, weintroduce a stochastic method based on moment equations. In this method thenumber of equations is dramatically reduced to just one equation for eachreactive species and one equation for each reaction. Moreover, the equationscan be easily constructed using a diagrammatic approach. We demonstrate themethod for a set of astrophysically relevant networks of increasing complexity.It is expected to be applicable in many other contexts in which problems thatexhibit analogous structure appear, such as surface catalysis in nanoscalesystems, aerosol chemistry in stratospheric clouds and genetic networks incells.
机译:表面可作为多种化学反应的高效催化剂。通常,这种表面反应涉及数十亿个在宏观区域上扩散和反应的分子。因此,随机波动可以忽略不计,反应速率可以使用基于平均场近似的速率方程式进行评估。然而,在将表面划分为大量不连续的微观区域的情况下,每个区域中的反应物的数量变小并且强烈波动。实际上,这就是星际介质中微小粉尘颗粒表面发生一些关键反应的情况,在这种情况下,速率方程失败了,而表面反应的模拟则需要诸如主方程之类的随机方法。但是,在复杂的反应网络中,主方程变得不可行,因为方程的数量呈指数增长。为了解决这个问题,我们引入了一种基于矩方程的随机方法。在这种方法中,方程式的数量显着减少为每个反应物种只有一个方程式,每个反应只有一个方程式。此外,可以使用图解方法轻松构造方程式。我们证明了一套方法的复杂性与天文学相关的网络越来越复杂。它有望适用于出现类似结构问题的许多其他情况,例如纳米尺度系统中的表面催化,平流层云中的气溶胶化学和遗传网络内的细胞。

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  • 作者

    Barzel, B.; Biham, O.;

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  • 年度 2007
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  • 原文格式 PDF
  • 正文语种 {"code":"en","name":"English","id":9}
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