Mandal Souvik, Gatti Fabien, Bindech Oussama, Marquardt Roberto, Tremblay Jean-Christophe
Laboratoire de Physique et Chimie Théoriques, UMR 7019 CNRS/Université de Lorraine, 1 Blvd. Arago, 57070 Metz, France.
Institut de Sciences Moléculaires d'Orsay, UMR 8214 CNRS/Université Paris-Saclay, Bât 520, rue André Rivière, 91405 Orsay CEDEX, France.
J Chem Phys. 2022 Mar 7;156(9):094109. doi: 10.1063/5.0079735.
In this paper, multidimensional dissipative quantum dynamics is studied within a system-bath approach in the Markovian regime using a model Lindblad operator. We report on the implementation of a Monte Carlo wave packet algorithm in the Heidelberg version of the Multi-Configuration Time-Dependent Hartree (MCTDH) program package, which is henceforth extended to treat stochastic dissipative dynamics. The Lindblad operator is represented as a sum of products of one-dimensional operators. The new form of the operator is not restricted to the MCTDH formalism and could be used with other multidimensional quantum dynamical methods. As a benchmark system, a two-dimensional coupled oscillators model representing the internal stretch and the surface-molecule distance in the O/Pt(111) system coupled to a Markovian bath of electron-hole-pairs is used. The simulations reveal the interplay between coherent intramolecular coupling due to anharmonic terms in the potential and incoherent relaxation due to coupling to an environment. It is found that thermalization of the system can be approximately achieved when the intramolecular coupling is weak.
在本文中，使用模型林德布拉德算符，在马尔可夫区域内的系统 - 浴方法框架下研究了多维耗散量子动力学。我们报告了在多组态含时哈特里（MCTDH）程序包的海德堡版本中蒙特卡罗波包算法的实现情况，该算法随后被扩展以处理随机耗散动力学。林德布拉德算符表示为一维算符乘积的总和。算符的这种新形式并不局限于MCTDH形式体系，可与其他多维量子动力学方法一起使用。作为一个基准系统，使用了一个二维耦合振子模型，该模型表示O/Pt(111)系统中的内部拉伸和表面 - 分子距离，并耦合到一个电子 - 空穴对的马尔可夫浴。模拟揭示了由于势中的非谐项引起的相干分子内耦合与由于与环境耦合导致的非相干弛豫之间的相互作用。研究发现，当分子内耦合较弱时，系统的热化可以近似实现。
