We calculate the emission times of the radiation in high-order harmonic generation using the Gabor transform of numerical data obtained from solving the time-dependent Schrödinger equation in one, two, and three dimensions. Both atomic and molecular systems, including nuclear motion, are investigated. Lewenstein model calculations are used to gauge the performance of the Gabor method. The resulting emission times are compared against the classical simple man's model as well as against the more accurate quantum orbit model based on complex trajectories. The influence of the range of the binding potential (long or short) on the level of agreement is assessed. Our analysis reveals that the short-trajectory harmonics are emitted slightly earlier than predicted by the quantum orbit model. This partially explains recent experimental observations for atoms and molecules. Furthermore, we observe a distinct signature of two-center interference in the emission times for H 2 and D 2 .

Recently, a method to image molecular electronic wave functions using high harmonic generation (HHG) was introduced by Itatani et al. [Nature 432, 876 (2004)]. We show that, while the tomographic reconstruction of general orbitals with arbitrary symmetry cannot be performed with long laser pulses, this becomes possible when extremely short pulses are used. An alternative reconstruction equation based on momentum matrix elements, rather than on dipole matrix elements, is proposed. We present simulations of the procedure for 2D model systems based on numerical solutions of the time-dependent Schrödinger equation, and present results from further post-processing of the reconstructed orbitals.

Accurate molecular imaging via high-order harmonic generation relies on comparing harmonic emission from a laser-irradiated molecule and an adequate reference system. However, an ideal reference atom with the same ionization properties as the molecule is not always available. We show that for suitably designed, very short laser pulses, a one-to-one mapping from high-order harmonic frequencies to electron momenta in above-threshold ionization exists. Comparing molecular and atomic momentum distributions then provides the electron recollision amplitude in the molecule for enhanced molecular imaging. The method retrieves the molecular recombination transition moments highly accurately, even with suboptimal reference atoms.