Abstract
Ab initio multiple-spawning (AIMS) describes the nonadiabatic dynamics of molecules by expanding nuclear wave functions in a basis of traveling multidimensional Gaussians called trajectory basis functions (TBFs). New TBFs can be spawned whenever nuclear amplitude is transferred between electronic states due to nonadiabatic transitions. While the adaptive size of the TBF basis grants AIMS its characteristic accuracy in describing nonadiabatic processes, it also leads to a fast and uncontrolled growth of the number of TBFs, penalizing computational efficiency. A different flavor of AIMS, called AIMS with informed stochastic selections (AIMSWISS), has recently been proposed to reduce the number of TBFs dramatically. Herein, we test the performance of AIMSWISS for a series of challenging nonadiabatic processes-photodynamics of two-dimensional model systems, 1,2-dithiane and chromium (0) hexacarbonyl-and show that this method is robust and extends the range of molecular systems that can be simulated within the multiple-spawning framework.
| Original language | English |
|---|---|
| Pages (from-to) | 12011-12018 |
| Number of pages | 8 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 13 |
| Issue number | 51 |
| DOIs | |
| Publication status | Published - 29 Dec 2022 |
Bibliographical note
Funding Information:This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant agreement No. 803718, project SINDAM) and the EPSRC Grant EP/V026690/1. This work has made use of the Hamilton HPC Service of Durham University.
Publisher Copyright:
© 2022 The Authors. Published by American Chemical Society.