Femtosecond time-resolved geometry relaxation and ultrafast intramolecular energy redistribution in Ag2Au

Thorsten M. Bernhardt*, Jan Hagen, Liana D. Socaciu, Roland Mitrić, Andreas Heidenreich, Jérôme Le Roux, Denisia Popolan, Mihai Vaida, Ludger Wöste, Vlasta Bonaĉić-Koutecký, Joshua Jortner

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


The ultrafast dynamics of the bimetallic cluster Ag2Au is investigated by pump-probe negative ion-to-neutral-to-positive ion (NeNePo) spectroscopy. Preparation of the neutral cluster in a highly nonequilibrium state by electron detachment from the mass-selected anion, and subsequent probing of the neutral nuclear dynamics through two-photon ionization to the cationic state, leads to strongly probe-energy-dependent transient cation-abundance signals. The origin of this pronounced time and wavelength dependence of the ionization probability on the femtosecond scale is revealed by ab initio theoretical simulations of the transient spectra. Based on the analysis of underlying dynamics, two fundamental processes involving geometry relaxation from linear to triangular structure followed by ultrafast intramolecular vibrational energy redistribution (IVR) have been identified and for the first time experimentally observed in the frame of NeNePo spectroscopy under conditions close to zero electron kinetic energy.

Original languageEnglish
Pages (from-to)243-253
Number of pages11
Issue number2
StatePublished - Feb 2005


  • Femtochemistry
  • Gold
  • Mass spectrometry
  • Metal clusters
  • Silver


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