Abstract
This brief review illustrates on a few typical applications fully fledged dynamical simulations of finite electronic systems (atoms, molecules, clusters) using time-dependent density-functional theory (TDDFT). It concentrates on aspects which are different from nuclear applications. These are: the correct handling of electron emission, the self-interaction correction, the enormous versatility of laser excitation to probe systems properties, and with it the exploitation of detailed observables of electron emission as photo-electron angular distributions and photo-electron spectra (PES). Finally, we demonstrate the impact of electronic dissipation putting question marks on the reliability of TDDFT simulations over long times.
Highlights
Far-off equilibrium dynamics in quantum many-body systems is since numerous decades a challenging task much studied in experimental and theoretical investigations
We illustrate the importance of self-interaction correction (SIC) for time-dependent density functional theory (TDDFT) on the example of the Na5 cluster irradiated by a femtosecond laser pulse with full width at half maximum of intensity (FWHM) of 10 fs, intensity I = 2.2 × 1011 W/cm2, and frequency ωlas = 10.9 eV, well above ionization threshold and far away from dominant eigenfrequencies of the system
We have presented a couple of typical applications of timedependent density functional theory (TDDFT) to electronic dynamics in clusters and molecules, as triggered by laser pulses
Summary
Far-off equilibrium dynamics in quantum many-body systems is since numerous decades a challenging task much studied in experimental and theoretical investigations. The theoretical description of such far-off equilibrium situations is demanding It requires large phase spaces and must cover vastly different time scales ranging from basic processes of excitation over collisional redistribution with subsequent relaxation to ionic motion and possible coupling to environment. TDLDA is plagued by a self-interaction error [23] which arises because the local approximation of Coulomb exchange spoils the subtle balance with the direct Coulomb term (which was still maintained in full Hartree-Fock calculations) This is disastrous for simulation of emission properties because the ionization potentials in terms of the energy of the highest occupied single-electron orbital are underestimated. We illustrate the capabilities of short laser pulses and discuss the impact of dissipation
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