2026-10-12T10:16:28Z https://api.figshare.com/v2/oai

oai:figshare.com:article/33763300 2026-09-14T21:49:37Z portal_1197 item_type_3 month_year_09_2026

Data for Improved on-the-fly MCTDH simulations with many-body-potential tensor decomposition and projection diabatisation Scott Habershon (1263891) Gareth Richings (24877405) Christopher Robertson (6095033) Hartree-Fock approximation Algorithms Potential energy surfaces Migrated from ePrints 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. The figures are provided as pdfs, but can also be generated by using the program "gnuplot". Relevant *.gnu files are provided in each directory. 2026-09-14T21:49:37Z Dataset Dataset 10.82444/warw.33763300.v1 https://figshare.com/articles/dataset/Data_for_Improved_on-the-fly_MCTDH_simulations_with_many-body-potential_tensor_decomposition_and_projection_diabatisation/33763300 CC BY 4.0