Atomistic Simulations, Italian Institute of Technology, via Morego 30, 16163 Genova, Italy.
Department of Chemistry and Applied Biosciences, ETH Zurich, 8092 Zurich, Switzerland.
Phys Rev Lett. 2020 Jul 10;125(2):026001. doi: 10.1103/PhysRevLett.125.026001.
We present a method to sample reactive pathways via biased molecular dynamics simulations in trajectory space. We show that the use of enhanced sampling techniques enables unconstrained exploration of multiple reaction routes. Time correlation functions are conveniently computed via reweighted averages along a single trajectory and kinetic rates are accessed at no additional cost. These abilities are illustrated analyzing a model potential and the umbrella inversion of NH_{3} in water. The algorithm allows a parallel implementation and promises to be a powerful tool for the study of rare events.
我们提出了一种通过在轨迹空间中进行有偏分子动力学模拟来采样反应途径的方法。我们表明，使用增强采样技术可以不受限制地探索多种反应途径。通过在单个轨迹上进行重新加权平均，可以方便地计算时间相关函数，并且不需要额外的成本即可获得动力学速率。我们通过分析模型势能和 NH_{3}在水中的伞式反转来说明这些能力。该算法允许并行实现，并有望成为研究稀有事件的有力工具。
