Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92003-0365, USA.
J Chem Phys. 2011 May 7;134(17):174107. doi: 10.1063/1.3581093.
A biased potential molecular dynamics simulation approach, accelerated molecular dynamics (AMD), has been implemented in the framework of ab initio molecular dynamics for the study of chemical reactions. Using two examples, the double proton transfer reaction in formic acid dimer and the hypothetical adiabatic ring opening and subsequent rearrangement reactions in methylenecyclopropane, it is demonstrated that ab initio AMD can be readily employed to efficiently explore the reactive potential energy surface, allowing the prediction of chemical reactions and the identification of metastable states. An adaptive variant of the AMD method is developed, which additionally affords an accurate representation of both the free-energy surface and the mechanism associated with the chemical reaction of interest and can also provide an estimate of the reaction rate.
一种有偏向的分子动力学模拟方法——加速分子动力学（AMD），已被应用于从头算分子动力学框架中，用于研究化学反应。通过两个实例，即甲酸二聚体中的双质子转移反应和亚甲基环丙烷的假设绝热开环及随后的重排反应，证明了从头算 AMD 可以很容易地用于有效地探索反应势能面，从而可以预测化学反应并确定亚稳态。开发了 AMD 方法的自适应变体，该变体还可以准确地表示感兴趣的化学反应的自由能面和相关机制，并且还可以提供反应速率的估计。
