Abstract
The ultrafast relaxation of small clusters immediately after ionization and photodetachment is theoretically studied. Microscopic models are proposed to describe the non-equilibrium dynamics of the clusters. As an example of strong structural response we determine for Ag3 the time scale for the change from a linear to triangular structure after the photodetachment process Ag− 3 → Ag3. We show that the time-dependent change of the ionization potential reflects in detail the internal degrees of freedom, in particular coherent and incoherent motion. We demonstrate that the time scales for bond breaking and formation are temperature dependent. We compare with experiment and point out the general significance of our results. We also study the ultrafast fragmentation dynamics of small Hgn clusters. We determine the fragmentation-time distributions induced by ionization. A dramatic change in the non-equilibrium fragmentation behavior occurs when the temperature before ionization reaches the melting point of the neutral clusters. This new effect could one allow to determine “melting points” of small clusters by pump&probe experiments. The ultrafast dynamics depends nonlinearly on the initial atomic positions and velocities, reflecting the intrinsic chaotic behavior of small clusters. The application of the theoretical models presented here, to the study of other relevant processes like control of chemical reactions, is discussed.
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Garcia, M.E., Jeschke, H.O., Bennemann, K.H. (1999). Ultrafast Structural Response and Nonlinear Fragmentation Dynamics of Small Clusters Induced by Optical Excitation. In: Jellinek, J. (eds) Theory of Atomic and Molecular Clusters. Springer Series in Cluster Physics. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-58389-6_8
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DOI: https://doi.org/10.1007/978-3-642-58389-6_8
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