Using quantum dynamics simulations to follow the competition between charge migration and charge transfer in polyatomic molecules
2017 (English)In: Chemical Physics, ISSN 0301-0104, E-ISSN 1873-4421, Vol. 482, 52-63 p.Article in journal (Refereed) Published
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.
Place, publisher, year, edition, pages
ELSEVIER SCIENCE BV , 2017. Vol. 482, 52-63 p.
Charge migration, Charge transfer, Quantum dynamics simulation, MCTDH, GWP method, Ehrenfest dynamics
IdentifiersURN: urn:nbn:se:uu:diva-319137DOI: 10.1016/j.chemphys.2016.10.007ISI: 000394634700007OAI: oai:DiVA.org:uu-319137DiVA: diva2:1086246