Time Evolution of ML-MCTDH Wavefunctions II: Application of the Projector Splitting Integrator

Abstract

The multi-layer multiconfiguration time-dependent Hartree (ML-MCTDH) approach suffers from numerical instabilities whenever the wavefunction is weakly entangled. These instabilities arise from singularities in the equations of motion (EOMs) and necessitate the use of a regularization parameter. The Projector Splitting Integrator (PSI) has previously been presented as an approach for evolving ML-MCTDH wavefunctions that is free of singularities. Here we will discuss the implementation of the multi-layer PSI with a particular focus on how the steps required relate to those required to implement standard ML-MCTDH. We demonstrate the efficiency and stability of the PSI for large ML-MCTDH wavefunctions containing up to hundreds of thousands of nodes by considering a series of spin-boson models with up to $10^6$ bath modes, and find that for these problems the PSI requires roughly 3-4 orders of magnitude fewer Hamiltonian evaluations and 2-3 orders of magnitude fewer Hamiltonian applications than standard ML-MCTDH, and 2-3/1-2 orders of magnitude fewer evaluations/applications than approaches that use improved regularization schemes. Finally, we consider a series of significantly more challenging multi-spin-boson models that require much larger numbers of single-particle functions with wavefunctions containing up to $\sim 1.3\times 10^9$ parameters to obtain accurate dynamics.

Main paper: 17 pages, 7 figures. Supplemental information (for paper I and paper II of the series): 22 pages, 2 figures

References in corpus (8)

• Full dimensional (15D) quantum-dynamical simulation of the protonated water-dimer II: infrared spectrum and vibrational dynamics
• Full dimensional (15D) quantum-dynamical simulation of the protonated water-dimer I: Hamiltonian setup and analysis of the ground vibrational state
• Time Dependent Variational Principle with Ancillary Krylov Subspace
• Dynamics, Synchronization and Quantum Phase Transitions of Two Dissipative Spins
• Time-dependent variational principle in matrix-product state manifolds: pitfalls and potential
• The quantum phase transition and correlations in the multi-spin-boson model
• Time Evolution of ML-MCTDH Wavefunctions I: Gauge Conditions, Basis Functions, and Singularities
• Quantum Phase Transition of Many Interacting Spins Coupled to a Bosonic Bath: static and dynamical properties