ML-MCTDH-Aid: An auxiliary package for multilayer multiconfiguration time-dependent Hartree calculations

Abstract

The multilayer-multiconfiguration time-dependent Hartree (ML-MCTDH) method has garnered significant attention in the realm of theoretical chemistry owing to its powerful ability to perform numerically exact descriptions of multi-dimensional quantum dynamics and exhibit the remarkable performance in simulating the nonadiabatic dynamics of complex systems. Despite the availability of computational packages within the ML-MCTDH framework, executing these calculations seamlessly is not a straightforward task. Typically, substantial efforts are necessitated to configure the correct inputs for ML-MCTDH calculations, which require to correctly define several non-trivial parameters, to reasonably setup the optimal tree expansion of wavefunctions, and to properly select basis function numbers. To address these challenges, we have developed an auxiliary package named ML-MCTDH-Aid, which facilitates the setup of ML-MCTDH calculations using the Heidelberg MCTDH package in a user-friendly manner. This package is primarily tailored to handle the high-dimensional nonadiabatic dynamics governed by the Hamiltonian composed of several electronic states, several vibrational modes and their linear vibronic coupling terms. It automatically generates multiple essential input files, and all the calculations can be performed in an all-in-one black-box easy-to-use manner. To show the utility of the ML-MCTDH-Aid package, we provide a step-by-step tutorial that demonstrates running ML-MCTDH studies on three models. These examples illuminate how the utilization of the ML-MCTDH-Aid package significantly enhances the efficiency and effectiveness of ML-MCTDH calculations. This substantially boosts the accessibility of ML-MCTDH calculations in tackling the high-dimensional quantum dynamics of complex systems.