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Time-Dependent Density Functional Theory for Intense Laser-Matter Interaction


Ruggenthaler,  Michael
Division Prof. Dr. Christoph H. Keitel, MPI for Nuclear Physics, Max Planck Society;

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Ruggenthaler, M. (2009). Time-Dependent Density Functional Theory for Intense Laser-Matter Interaction. PhD Thesis, Ruprecht-Karls Universität, Heidelberg.

Cite as: https://hdl.handle.net/11858/00-001M-0000-0011-757C-3
In order to properly describe the dynamics of a many-particle system in strong, timedependent fields, a nonperturbative treatment of all constituents and of their correlation is needed. An ab initio solution of the time-dependent many-body Schr¨odinger equation is only feasible for simple systems. Hence, for many-electron systems in intense laser fields practicable methods for solving the quantum-mechanical many-body problem are required. An formally exact approach is the time-dependent density functional theory. In this work a mathematically rigorous formulation of the foundations of this theory is given. Further the non-locality in time of the exchange correlation functionals is examined, and we formally define the notion of “quantum memory”. We investigate the fundamental process of Rabi oscillations from a density functional point of view and find the few-level approximation to be in conflict with the basis of time-dependent density functional theory. Finally, we apply the theory to calculate the electron dynamics of C60 in intense laser pulses. Although the laser light is far off-resonant with respect to the collective modes of the C60 the multi-electron dynamics strongly influences the harmonic spectra. The efficiency of this multi-particle recollision process with respect to the usual single active electron approximation of high-order harmonic generation is estimated by two analytical models.