Open system dynamics using Gaussian-based multiconfigurational time-dependent Hartree wavefunctions: Application to...

A variational approach for the quantum dynamics of statistical mixtures is developed, which is based upon the representation of the natural states of the mixture in terms of hybrid Gaussian-based Multiconfiguration Time-Dependent Hartree (G-MCTDH) wavefunctions. The method, termed ρG-MCTDH, is combined with a treatment of dissipation and decoherence based on the nonstochastic open-system Schrödinger equations. The performance and the convergence properties of the approach are illustrated for a two-dimensional tunneling system, where the primary tunneling coordinate, represented by flexible single-particle functions, is resonantly coupled to a second harmonic mode, represented by Gaussian wave packets. The harmonic coordinate is coupled to the environment and two different processes are studied: (i) vibrational relaxation at zero temperature described by a master equation in the Lindblad form and (ii) thermalization induced by the Caldeira-Leggett master equation. In the second case, the evolution from a quantum tunneling regime to a quasistationary classical-limit distribution, driven by the heat bath, is visualized using a flux analysis.