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An important goal in molecular physics and chemistry today is to obtain structure-dependent information about molecular function to obtain a deeper understanding into chemical reactions. However, until now, asymmetric tops, which comprise the widest and most general class of molecules, remain principally unexplored. This gap is particularly evident in high harmonic generation (HHG). HHG has successfully obtained structural information about electron hole pairs or orbitals for simple linear molecules. Unfortunately, for more complicated molecules, the emission from different molecular directions interfere, concealing individual angular signatures. Here we introduce a method to extract orientation-dependent information from asymmetric tops and apply it to the sulfur dioxide (SO2) molecule. We use the rotational revival structure to decompose the angular contributions of HHG emission. This method also extends HHG-based tomographic imaging into three dimensions and makes it applicable to a much wider class of systems than previously envisioned. Our results suggest that HHG is a powerful tool to probe electron orbital structure and dynamics of complex molecules.
This paper has been withdrawn by the authors because the wave packet propagation used in the ion-dynamics calculation did not allow for electron-nuclei correlation. Hence, the conclusion that the ion-dynamics model is not in agreement with experiment is not substantiated.
We investigate the orientation dependence of molecular high-order harmonic generation (HHG) both numerically and analytically. We show that the molecular recollision electronic wave packets (REWPs) in the HHG are closely related to the ionization pot
High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular geometries
We investigate how short and long electron trajectory contributions to high harmonic emission and their interferences give access to intra-molecular dynamics. In the case of unaligned molecules, we show experimental evidences that the long trajectory
We investigate the orientation dependence of high-order harmonic generation (HHG) from H$_2^+$ with different internuclear distances irradiated by intense laser fields both numerically and analytically. The calculated molecular HHG spectra are found