结合元动力学与分子动力学模拟的晶体生长微观速率常数

Dániel Kozma, G. Tóth
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引用次数: 1

摘要

晶体生长的原子模拟可分为两个步骤:微观速率常数的确定和介观动力学蒙特卡罗模拟。我们提出了一种测定晶体生长动力学速率常数的方法。我们对氩的平衡液晶界面进行了经典分子动力学研究。用元动力学方法研究了晶体生长的自由能面。在界面处选择一个晶体原子,并通过添加排斥高斯势将其置换到液相中。用高斯势的最大势能密度计算了该过程的激活自由能。利用过渡态理论计算了不同界面结构下的速率常数。为了模拟真实结晶,我们在计算两个相反的速率常数时采用了温差,并将其应用于动力学蒙特卡罗模拟。我们的技术的新颖之处在于它可以用于缓慢的结晶过程,而简单的轨迹跟踪只能应用于快速反应。我们的方法为确定晶体生长的基本速率常数提供了可能,这对于计算机辅助晶体设计的长期目标似乎是必要的。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Microscopic Rate Constants of Crystal Growth from Molecular Dynamic Simulations Combined with Metadynamics
Atomistic simulation of crystal growth can be decomposed into two steps: the determination of the microscopic rate constants and a mesoscopic kinetic Monte Carlo simulation. We proposed a method to determine kinetic rate constants of crystal growth. We performed classical molecular dynamics on the equilibrium liquid/crystal interface of argon. Metadynamics was used to explore the free energy surface of crystal growth. A crystalline atom was selected at the interface, and it was displaced to the liquid phase by adding repulsive Gaussian potentials. The activation free energy of this process was calculated as the maximal potential energy density of the Gaussian potentials. We calculated the rate constants at different interfacial structures using the transition state theory. In order to mimic real crystallization, we applied a temperature difference in the calculations of the two opposite rate constants, and they were applied in kinetic Monte Carlo simulation. The novelty of our technique is that it can be used for slow crystallization processes, while the simple following of trajectories can be applied only for fast reactions. Our method is a possibility for determination of elementary rate constants of crystal growth that seems to be necessary for the long-time goal of computer-aided crystal design.
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