Interplay of polarization geometry and rotational dynamics in high-order harmonic generation from coherently rotating linear molecules.

Recent reports on intense-field pump-probe experiments for high-order harmonic generation (HHG) from coherently rotating linear molecules have revealed remarkable characteristic effects of the simultaneous variation of the polarization geometry and the time delay on the high-order harmonic signals. We analyze the effects and give a unified theoretical account of the experimental observations. Furthermore, characteristic behavior at critical polarization angles are found that can help to identify the molecular orbital symmetry in connection with the problem of molecular imaging from the HHG data.

Origin of anomalous spectra of dynamic alignments observed in N2 and O2.

Recent pump-probe experiments with intense femtosecond laser pulses and diatomic molecules N2 and O2, have revealed the presence of Raman-forbidden anomalous series and lines in the Fourier spectrum of HHG (high harmonic generation) signals. A theoretical analysis of the problem is made by deriving a general expression of the angle dependent HHG operator that governs the dynamic alignment signals in linear molecules, and applying them to the experiments in N2 and O2. A unified interpretation of the origin of the observed Raman-allowed and the anomalous spectral features is given.

Field-free alignment of molecules observed with high-order harmonic generation.

High-order harmonic generation is demonstrated to provide a sensitive way for an extensive study of dynamic processes in the field-free alignment of strong-field-induced molecular rotational wave packets. The time-dependent harmonic signal observed from field-free-aligned N2, O2, and CO2 has been found to include two sets of beat frequency for pairs of coherently populated rotational states. One of them is the well-known frequency component characterizing the field-free alignment of molecules, and the other is ascribed to the beat that arises from coherence embedded in the wave packet.