Data for Improved on-the-fly MCTDH simulations with many-body-potential tensor decomposition and projection diabatisation

We have recently demonstrated how potential energy surface (PES) interpolation methods such as kernel ridge regression (KRR), can be combined with accurate wavefunction time-propagation methods, specifically the multi-configuration time-dependent Hartree (MCTDH) method, to generate a new "on-the-fly" MCTDH scheme (DD-MCTDH) which does not require the pre-fitting of the PES which is normally required by MCTDH. Specifically, we have shown how our DD-MCTDH strategy can be used to model non-adiabatic dynamics in a 4-mode/2-state model of pyrazine, with \emph{ab initio} electronic structure calculations performed directly during propagation, requiring around 100 hours of computer wall-time.

In this Article, we show how the efficiency and accuracy of DD-MCTDH can be dramatically improved further still by: (i) using systematic tensor decompositions of the KRR PES, and (ii) using a novel scheme for diabatisation within the framework of configuration interaction (CI) methods which only requires local adiabatic electronic states, rather than non-adiabatic coupling matrix elements. The result of these improvements is that our latest version of DD-MCTDH can perform a 12-mode/2-state simulation of pyrazine, with PES evaluations at CAS level, in just 29-90 hours on a standard desktop computer; this work therefore represents an enormous step towards direct quantum dynamics with MCTDH.<br><br>This zip file contains data from: Improved on-the-fly MCTDH simulations with many-body-potential tensor decomposition and projection diabatisation The four directories contain the datasets for the 7 figures in the manuscript.