title: Field-induced surface hopping method for probing transition state nonadiabatic dynamics of Ag3.
abstract: We present the simulation of time-resolved photoelectron spectra of Ag(3) involving excitation from the linear transition state, where nonadiabatic relaxation takes place in a complex manifold of electronic states. Thus, we address ultrafast processes reachable by negative ion-to neutral-to positive ion (NeNePo) spectroscopy starting from the linear Ag anionic species. For this purpose we use our newly developed field-induced surface hopping method (FISH) augmented for the description of photoionization processes. Furthermore we employ our method for nonadiabatic molecular dynamics "on the fly" in the framework of time-dependent density functional theory generalized for open shell systems. Our presented approach is generally applicable for the prediction of time-resolved photoelectron spectra and their analysis in systems with complex electronic structure as well as many nuclear degrees freedom. This theoretical development should serve to stimulate new ultrafast experiments.
authors.affiliation: Freie Universität Berlin, Fachbereich Physik, Arnimallee 14, D-14195 Berlin, Germany. mitric@zedat.fu-berlin.de
authors.forename: Roland
authors.initials: R
authors.lastname: Mitrić
authors.forename: Jens
authors.initials: J
authors.lastname: Petersen
authors.forename: Matthias
authors.initials: M
authors.lastname: Wohlgemuth
authors.forename: Ute
authors.initials: U
authors.lastname: Werner
authors.forename: Vlasta
authors.initials: V
authors.lastname: Bonačić-Koutecký
mesh_terms: D056951:Photoelectron Spectroscopy; D011789:Quantum Theory; D012834:Silver / Q000737:chemistry*; D013499:Surface Properties; D013997:Time Factors
chemical_list: D012834:Silver