Coonjobeeharry, J;
Spinlove, KE;
Sanz Sanz, C;
Sapunar, M;
Došlić, N;
Worth, GA;
(2022)
Mixed-quantum-classical or fully-quantized dynamics? A unified code to compare methods.
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences
, 380
(2223)
, Article 20200386. 10.1098/rsta.2020.0386.
Preview |
Text
Paper_v2.pdf - Accepted Version Download (3MB) | Preview |
Abstract
Three methods for non-adiabatic dynamics are compared to highlight their capabilities. Multi-configurational time-dependent Hartree is a full grid-based solution to the time-dependent Schrödinger equation, variational multi-configurational Gaussian (vMCG) uses a less flexible but unrestricted Gaussian wavepacket basis, and trajectory surface hopping (TSH) replaces the nuclear wavepacket with a swarm of classical trajectories. Calculations with all methods using a model Hamiltonian were performed. The vMCG and TSH were also then run in a direct dynamics mode, with the potential energy surfaces calculated on-the-fly using quantum chemistry calculations. All dynamics calculations used the Quantics package, with the TSH calculations using a new interface to a surface hopping code. A novel approach to calculate adiabatic populations from grid-based quantum dynamics using a time-dependent discrete variable representation is presented, allowing a proper comparison of methods. This article is part of the theme issue 'Chemistry without the Born-Oppenheimer approximation'.
| Type: | Article |
|---|---|
| Title: | Mixed-quantum-classical or fully-quantized dynamics? A unified code to compare methods |
| Location: | England |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1098/rsta.2020.0386 |
| Publisher version: | https://doi.org/10.1098/rsta.2020.0386 |
| Language: | English |
| Additional information: | This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third-party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
| Keywords: | MCTDH, direct dynamics, non-adiabatic dynamics, surface hopping, vMCG |
| UCL classification: | UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry UCL > Provost and Vice Provost Offices > UCL BEAMS UCL |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10146394 |
Archive Staff Only
 |
View Item |
