| XPK程序包：扩展唯象动力学方法(XPK)与常规动力学蒙特卡罗(KMC)方法的比较 |
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| 引用本文： | 申同昊,徐 昕.XPK程序包：扩展唯象动力学方法(XPK)与常规动力学蒙特卡罗(KMC)方法的比较[J].化学物理学报,2019,32(1):143-150. |
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| 作者姓名： | 申同昊 徐 昕 |
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| 作者单位： | 复旦大学化学系，能源材料化学协同创新中心，上海市分子催化和功能材料重点实验室，计算物质科学教育部重点实验室，上海 200438,复旦大学化学系，能源材料化学协同创新中心，上海市分子催化和功能材料重点实验室，计算物质科学教育部重点实验室，上海 200438 |
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| 摘 要： | 在常规的动力学蒙特卡罗方法(KMC)中，扩散过程的速率往往远大于化学反应，因而造成KMC方法在模拟表面化学体系演化时效率非常低下. 为了解决这一时间尺度分离问题，本文最近发展了扩展唯象动力学方法(XPK). 本文基于加氢反应体系模型，利用新发展的XPK程序包，对XPK方法与常规的KMC方法进行了细致的对比. 为了更全面地说明问题，测试中包含了两条不同的势能曲线，以及多种吸附物之间的相互作用. 对比的内容包括计算消耗、并行效率以及稳态的收敛行为等. 测试结果表明，相比于常规的KMC方法，XPK方法在兼顾精度的同时大大提高了模拟效率. 因而可以预期，XPK方法将成为多相催化理论研究的强有力工具. 特别是在表面吸附物种相互作用有决定性影响的情况下，XPK方法的优势尤其突出.
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| 关 键 词： | 动力学蒙特卡罗，扩展唯象动力学方法，表面反应，多相催化 |
| 收稿时间： | 2019/1/21 0:00:00 |
The XPK Package: A Comparison between the Extended Phenomenological Kinetic (XPK) Method and the Conventional Kinetic Monte Carlo (KMC) Method |
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| Tong-hao Shen and Xin Xu.The XPK Package: A Comparison between the Extended Phenomenological Kinetic (XPK) Method and the Conventional Kinetic Monte Carlo (KMC) Method[J].Chinese Journal of Chemical Physics,2019,32(1):143-150. |
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| Authors: | Tong-hao Shen and Xin Xu |
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| Institution: | Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, MOE Laboratory for Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200438, China and Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, MOE Laboratory for Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200438, China |
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| Abstract: | Recently, we proposed the extended phenomenological kinetics (XPK) method, which overcomes the notorious timescale separation difficulty between fast diffusion and slow chemical reactions in conventional kinetic Monte Carlo (KMC) simulations. In the present work, we make a comprehensive comparison, based on the newly developed XPK package, between the XPK method and the conventional KMC method using a model hydrogenation reaction system. Two potential energy surfaces with different lateral interactions have been designed to illustrate the advantages of the XPK method in computational costs, parallel efficiency and the convergence behaviors to steady states. The XPK method is shown to be efficient and accurate, holding the great promise for theoretical modelling in heterogeneous catalysis, in particular, when the role of the lateral interactions among adsorbates is crucial. |
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| Keywords: | Kinetic Monte Carlo Extended phenomenological kinetics Surface reaction Heterogeneous catalysis |
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