Using quantum dynamics simulations to follow the competition between charge migration and charge transfer in polyatomic molecules

Research output: Contribution to journalArticle

Authors

Colleges, School and Institutes

Abstract

Recent work, particularly by Cederbaum and co-workers, has identified the phenomenon of charge migration, whereby charge flow occurs over a static molecular framework after the creation of an electronic wavepacket. In a real molecule, this charge migration competes with charge transfer, whereby the nuclear motion also results in the re-distribution of charge. To study this competition, quantum dynamics simulations need to be performed. To break the exponential scaling of standard grid-based algorithms, approximate methods need to be developed that are efficient yet able to follow the coupled electronic-nuclear motion of these systems. Using a simple model Hamiltonian based on the ionisation of the allene molecule, the performance of different methods based on Gaussian Wavepackets is demonstrated.

Details

Original languageEnglish
JournalChemical Physics
Early online date8 Oct 2016
Publication statusE-pub ahead of print - 8 Oct 2016

Keywords

  • Charge migration, Charge transfer, Quantum dynamics simulation, MCTDH, GWP method, Ehrenfest dynamics