Cao Lingling, Stoltz Gabriel, Lelièvre Tony, Marinica Mihai-Cosmin, Athènes Manuel
CEA, DEN, Service de Recherches de Métallurgie Physique, F-91191 Gif-sur-Yvette, France.
Université Paris-Est, CERMICS (ENPC), INRIA, F-77455 Marne-la-Vallée, France.
J Chem Phys. 2014 Mar 14;140(10):104108. doi: 10.1063/1.4866811.
We propose an adiabatic reweighting algorithm for computing the free energy along an external parameter from adaptive molecular dynamics simulations. The adaptive bias is estimated using Bayes identity and information from all the sampled configurations. We apply the algorithm to a structural transition in a cluster and to the migration of a crystalline defect along a reaction coordinate. Compared to standard adaptive molecular dynamics, we observe an acceleration of convergence. With the aid of the algorithm, it is also possible to iteratively construct the free energy along the reaction coordinate without having to differentiate the gradient of the reaction coordinate or any biasing potential.
我们提出了一种绝热重加权算法，用于从自适应分子动力学模拟中计算沿外部参数的自由能。使用贝叶斯恒等式和来自所有采样构型的信息来估计自适应偏差。我们将该算法应用于团簇中的结构转变以及晶体缺陷沿反应坐标的迁移。与标准自适应分子动力学相比，我们观察到收敛加速。借助该算法，还可以沿反应坐标迭代构建自由能，而无需区分反应坐标的梯度或任何偏置势。
