Time-resolved spectroscopy at surfaces and adsorbate dynamics: insights from a model-system approach

Abstract

We introduce a model description of femtosecond laser induced desorption at surfaces. The substrate part of the system is taken into account as a (possibly semi-infinite) linear chain. Here, being especially interested in the early stages of dissociation, we consider a finite-size implementation of the model (i.e., a finite substrate), for which an exact numerical solution is possible. By time-evolving the many-body wave function, and also using results from a time-dependent density functional theory description for electron-nuclear systems, we analyze the competition between several surface-response mechanisms and electronic correlations in the transient and longer time dynamics under the influence of dipole-coupled fields. Our model allows us to explore how coherent multiple-pulse protocols can impact desorption in a variety of prototypical experiments.

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• Time resolved multi-photon effects in the fluorescence spectra of two-level systems at rest and in motion
• Time-Dependent Multi-Component Density Functional Theory for Coupled Electron-Positron Dynamics
• Photon pumping, photodissociation and dissipation at interplay for the fluorescence of a molecule in a cavity