How to remove the spurious resonances from ring polymer molecular dynamics

半经典物理学 恒温器 分子动力学 量子 统计物理学 朗之万动力 伦纳德琼斯势 物理 量子动力学 虚假关系 量子隧道 经典力学 量子力学 数学 热力学 统计
作者
Mariana Rossi,Michele Ceriotti,David E. Manolopoulos
出处
期刊:Journal of Chemical Physics [American Institute of Physics]
卷期号:140 (23) 被引量:252
标识
DOI:10.1063/1.4883861
摘要

Two of the most successful methods that are presently available for simulating the quantum dynamics of condensed phase systems are centroid molecular dynamics (CMD) and ring polymer molecular dynamics (RPMD). Despite their conceptual differences, practical implementations of these methods differ in just two respects: the choice of the Parrinello-Rahman mass matrix and whether or not a thermostat is applied to the internal modes of the ring polymer during the dynamics. Here we explore a method which is halfway between the two approximations: we keep the path integral bead masses equal to the physical particle masses but attach a Langevin thermostat to the internal modes of the ring polymer during the dynamics. We justify this by showing analytically that the inclusion of an internal mode thermostat does not affect any of the desirable features of RPMD: thermostatted RPMD (TRPMD) is equally valid with respect to everything that has actually been proven about the method as RPMD itself. In particular, because of the choice of bead masses, the resulting method is still optimum in the short-time limit, and the transition state approximation to its reaction rate theory remains closely related to the semiclassical instanton approximation in the deep quantum tunneling regime. In effect, there is a continuous family of methods with these properties, parameterised by the strength of the Langevin friction. Here we explore numerically how the approximation to quantum dynamics depends on this friction, with a particular emphasis on vibrational spectroscopy. We find that a broad range of frictions approaching optimal damping give similar results, and that these results are immune to both the resonance problem of RPMD and the curvature problem of CMD.
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