Electrons as probes of dynamics in molecules and clusters : a contribution from Time Dependent Density Functional Theory

Abstract

Various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations exist. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the excitation dynamics. Such an analysis of electron signals covers total ionization, Photo-Electron Spectra, Photoelectron Angular Distributions, and ideally combined PES/PAD, with a long history in molecular physics, also increasingly used in cluster physics. Recent progress in the design of new light sources (high intensity and/or frequency, ultra short pulses) opens new possibilities for measurements and thus has renewed the interest on the analysis of dynamical scenarios through these observables, well beyond a simple access to a density of states. This, in turn, has motivated many theoretical investigations of the dynamics of electronic emission for molecules and clusters. A theoretical tool of choice is here Time-Dependent Density Functional Theory (TDDFT) propagated in real time and on a spatial grid, and augmented by a Self-Interaction Correction. This provides a pertinent, robust, and efficient description of electronic emission including the detailed pattern of PES and PAD. A direct comparison between experiments and well founded elaborate microscopic theories is thus readily possible, at variance with more demanding observables such as for example fragmentation or dissociation cross sections. The aim of this paper is to review the available experimental results motivating such studies, describe the theoretical tools developed on the basis of real-time and real-space TDDFT to address in a realistic manner the analysis of electronic emission following irradiation of clusters and molecules by various laser pulses, discuss representative results, and finally give some future directions of investigations.

arXiv comment104 pages, 63 figures, accepted in Physics Reports

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• Strong-field effects in the photo-emission spectrum of the C${}_{60}$ fullerene
• Photoionization of multishell fullerenes studied by ab initio and model approaches
• Forward-backward asymmetry of photoemission in C${}_{60}$ excited by few-cycle laser pulses
• Unexpected dipole instabilities in small molecules after ultrafast XUV irradiation
• The impact of the carrier envelope phase -- dependence on system and laser parameters
• Optimal control with non-adiabatic Molecular Dynamics: application to the Coulomb explosion of Sodium clusters
• Effects of electronic correlation on the high harmonic generation in helium: a time-dependent configuration interaction singles vs time-dependent full configuration interaction study