Dynamics of diatomic molecules in intense laser fields: Alignment, Ionization and Fragmentation of dimers: Die Dynamik zweiatomiger Moleküle in intensiven Laserfeldern

A realistic description of ionization in intense laser fields is implemented into the Non-Adiabatic Quantum Molecular Dynamics (NA-QMD) formalism. First, the error of a finite basis expansion is considered and a new measure is proposed for time-dependent calculations. This is used to investigate systematically the influence of the used basis set in calculations on the hydrogen atom in intense laser fields. Second, absorbing boundary conditions in basis expansion are introduced via an imaginary potential into the effective one-particle Hamiltonian. It is shown that the used form of the absorber potential is valid in many-electron time-dependent density functional theory calculations, i.e. that only ionized states are affected by the absorbing potential. The absorber is then tested on reference calculations that exist for H and aligned H+2 in intense laser fields. Excellent agreement is found. Additionally, an approximative treatment of the missing electron-nuclear correlations is proposed. It is found in calculations on H+2 that a qualitative improvement of the description of nuclear dynamics results. The extension of the NA-QMD formalism is then used to investigate the alignment behavior of diatomic molecules. Recent experiments on H+2 and H2 are reviewed and explained. It is found that dynamic alignment, i.e. the laser induced rotation of the molecule, plays a central role. The alignment behavior of H+2 and H2 and its intensity dependence is investigated after that. A drastic difference between H+2 and H2 is found in NA-QMD as well as model calculations. Then, the focus is on an astonishing new effect that has been found in N2 calculations. This effect which is called "rotational destabilization" is studied on the model system H+2. Yet, it might be observable only in heavy dimers and might have already been found in an experiment on I2