kmos: A lattice kinetic Monte Carlo framework
kmos: A lattice kinetic Monte Carlo framework
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DOI：
10.1016/j.cpc.2014.04.003
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发表时间：
2014-07-01
影响因子：
6.3
通讯作者：
Reuter, Karsten
中科院分区：
文献类型：
--
作者：
Hoffmann, Max J.;Matera, Sebastian;Reuter, Karsten
动力学蒙特卡罗（kMC）模拟已经成为多相催化和其他材料应用中微观动力学建模的关键工具。系统，其中所有的基本反应的位点特异性允许映射到离散的活性位点的晶格，可以在特别有效的晶格kMC方法内解决。为此，我们描述了多功能的kmos软件包，它提供了一个最用户友好的实施，执行和评价晶格kMC模型的任意复杂性在一至三维晶格系统，涉及多个活性位点的周期性或非周期性安排，以及网站解决成对和高阶横向相互作用。从概念上讲，kmos实现了最大的运行时性能，这是基本上独立的晶格大小，通过生成代码的效率确定的本地更新的可用事件，是一个定义的kMC模型优化。对于这个模型定义以及所有运行时和评估方面的控制，kmos提供了一个高级应用程序编程接口。通过脚本或图形用户界面交互使用，可视化模型几何形状，晶格占据和选定的基本反应速率，同时允许实时更改模拟参数。我们展示了kmos的性能和缩放与应用程序的kMC模型的表面催化过程中，对于给定的操作，条件（温度和分压的所有反应物）中央模拟结果是催化活性和选择性，表面组成，并在反应网络中发生的个别基本过程的机理洞察。
Kinetic Monte Carlo (kMC) simulations have emerged as a key tool for microkinetic modeling in heterogeneous catalysis and other materials applications. Systems, where site-specificity of all elementary reactions allows a mapping onto a lattice of discrete active sites, can be addressed within the particularly efficient lattice kMC approach. To this end we describe the versatile kmos software package, which offers a most user-friendly implementation, execution, and evaluation of lattice kMC models of arbitrary complexity in one- to three-dimensional lattice systems, involving multiple active sites in periodic or aperiodic arrangements, as well as site-resolved pairwise and higher-order lateral interactions. Conceptually, kmos achieves a maximum runtime performance which is essentially independent of lattice size by generating code for the efficiency-determining local update of available events that is optimized for a defined kMC model. For this model definition and the control of all runtime and evaluation aspects kmos offers a high-level application programming interface. Usage proceeds interactively, via scripts, or a graphical user interface, which visualizes the model geometry, the lattice occupations and rates of selected elementary reactions, while allowing on-the-fly changes of simulation parameters. We demonstrate the performance and scaling of kmos with the application to kMC models for surface catalytic processes, where for given operation,conditions (temperature and partial pressures of all reactants) central simulation outcomes are catalytic activity and selectivities, surface composition, and mechanistic insight into the occurrence of individual elementary processes in the reaction network.