Abstract
High harmonic spectroscopy gives access to molecular structure with Angström resolution. Such information is encoded in the destructive interferences occurring between the harmonic emissions from the different parts of the molecule. By solving the time-dependent Schrödinger equation, either numerically or with the molecular strong-field approximation, we show that the electron dynamics in the emission process generally results in a strong spectral smoothing of the interferences, blurring the structural information. However we identify specific generation conditions where they are unaffected. These findings have important consequences for molecular imaging and orbital tomography using high harmonic spectroscopy.
Highlights
High Harmonic Spectroscopy (HHS) is a powerful technique in which the process of High Harmonic Generation (HHG) is used to probe the structure and dynamics of the generating medium with Angström and attosecond resolution
It is crucial to disentangle the different effects in order to access this rich information[11,12,13]. This was generally performed by recording the dependence on the laser parameters, since it was widely accepted that structural interferences do not depend on them[14]
This appears clearly in the Quantitative ReScattering theory (QRS)[15] where the harmonic dipole is expressed as the product of the returning Electron Wave-Packet (EWP), containing all the laser parameters, and the target-specific field-free recombination dipole, only dependent on the EWP energy and recollision direction
Summary
High Harmonic Spectroscopy (HHS) is a powerful technique in which the process of High Harmonic Generation (HHG) is used to probe the structure and dynamics of the generating medium with Angström and attosecond resolution. We study the signatures of the electron dynamics on the structural interference occurring in the harmonic emission from diatomic molecules.
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