Wedekind Jan, Strey Reinhard, Reguera David
Institut für Physikalische Chemie, Universität zu Köln, D-50939 Köln, Germany.
J Chem Phys. 2007 Apr 7;126(13):134103. doi: 10.1063/1.2713401.
We present a new method to analyze molecular and Brownian dynamics simulations of activated processes based on the concept of mean first-passage times. The new method provides a simple and efficient strategy to evaluate reaction rates and it facilitates the localization of the transition state directly from the kinetics of the system without the need of thermodynamical considerations. It also provides a more rigorous value of the steady-state transition rate and gives valuable information about many important characteristics of the process. We illustrate the power of this new technique by its application to the study of nucleation in rare gases.
我们提出了一种基于平均首次通过时间概念来分析活化过程的分子动力学和布朗动力学模拟的新方法。这种新方法提供了一种简单而有效的策略来评估反应速率,并且无需热力学考量就能直接从系统动力学中确定过渡态的位置。它还给出了稳态过渡速率的更精确值,并提供了有关该过程许多重要特征的有价值信息。我们通过将这种新技术应用于稀有气体中的成核研究来说明其强大功能。