Department of Chemistry, Duke University, Durham, North Carolina 27708, USA.
J Chem Phys. 2011 Apr 14;134(14):144102. doi: 10.1063/1.3575588.
In this paper, we introduce a trajectory-based nonadiabatic dynamics algorithm which aims to correct the well-known overcoherence problem in Tully's popular fewest-switches surface hopping algorithm. Our simultaneous-trajectory surface hopping algorithm propagates a separate classical trajectory on each energetically accessible adiabatic surface. The divergence of these trajectories generates decoherence, which collapses the particle wavefunction onto a single adiabatic state. Decoherence is implemented without the need for any parameters, either empirical or adjustable. We apply our algorithm to several model problems and find a significant improvement over the traditional algorithm.
在本文中，我们介绍了一种基于轨迹的非绝热动力学算法，旨在纠正图利（Tully）广受欢迎的少数跃迁表面跳跃算法中的著名过度相干问题。我们的同时轨迹表面跳跃算法在每个可及的绝热表面上传播单独的经典轨迹。这些轨迹的发散产生退相干，从而将粒子波函数折叠到单个绝热态上。退相干是在不需要任何经验或可调参数的情况下实现的。我们将我们的算法应用于几个模型问题，并发现与传统算法相比有了显著的改进。
