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Re_LVC.pdf (677.55 kB)
Strong Influence of Decoherence Corrections and Momentum Rescaling in Surface Hopping Dynamics of Transition Metal Complexes
Preprints are manuscripts made publicly available before they have been submitted for formal peer review and publication. They might contain new research findings or data. Preprints can be a draft or final version of an author's research but must not have been accepted for publication at the time of submission.
submitted on 29.05.2019, 19:41 and posted on 30.05.2019, 16:15by Felix Plasser, Sebastian Mai, Maria Fumanal, Etienne Gindensperger, Chantal Daniel, Leticia Gonzalez
The reliability of different parameters in the surface hopping method is assessed for a vibronic coupling model of a challenging transition metal complex, where a large number of electronic states of different multiplicities are met within a small energy range. In particular, the effect of two decoherence correction schemes and of various strategies for momentum rescaling and treating frustrating hops during the dynamics is investigated and compared against an accurate quantum dynamics simulation. The results show that small differences in the surface hopping protocol can strongly affect the results. We find a clear preference for momentum rescaling along the nonadiabatic coupling vector and trace this effect back to an enhanced number of frustrated hops. Furthermore, reflection of the momentum after frustrated hops is shown to work better than to ignore the process completely. The study also highlights the importance of the decoherence correction but neither of the two methods employed, energy based decoherence and augmented fewest switches surface hopping, performs completely satisfactory. More generally, the study emphasises the importance of the often neglected parameters in surface hopping and shows that there is still need for simple, robust, and generally applicable correction schemes.