Large-scale atomistic simulations of nanostructured materials based on divide-and-conquer density functional theory
Large-scale atomistic simulations of nanostructured materials based on divide-and-conquer density functional theory
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DOI：
10.1140/epjst/e2011-01418-y
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发表时间：
2011-05
期刊：
影响因子：
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通讯作者：
F. Shimojo;S. Ohmura;A. Nakano;R. Kalia;P. Vashishta
中科院分区：
文献类型：
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作者：
F. Shimojo;S. Ohmura;A. Nakano;R. Kalia;P. Vashishta
基于分而治之 (DC) 方案的线性缩放算法旨在执行大规模分子动力学模拟，其中原子间力在密度泛函理论 (DFT) 框架下以量子力学方式计算。该方案应用于 Al/Fe2O3 界面的铝热反应。研究发现，协同金属-氧翻转机制增强了界面处的质量扩散和反应速率。基于传统DFT对水中铝颗粒进行了初步模拟，作为大规模DC-DFT模拟的目标系统。模拟中发现，铝表面上的一对路易斯酸和碱位点优先催化以低活化势垒机制产生氢气。
A linear-scaling algorithm based on a divide-and-conquer (DC) scheme is designed to perform large-scale molecular-dynamics simulations, in which interatomic forces are computed quantum mechanically in the framework of the density functional theory (DFT). This scheme is applied to the thermite reaction at an Al/Fe2O3interface. It is found that mass diffusion and reaction rate at the interface are enhanced by a concerted metal-oxygen flip mechanism. Preliminary simulations are carried out for an aluminum particle in water based on the conventional DFT, as a target system for large-scale DC-DFT simulations. A pair of Lewis acid and base sites on the aluminum surface preferentially catalyzes hydrogen production in a low activation-barrier mechanism found in the simulations.