We demonstrate high-harmonic spectroscopy in many-electron molecules using time-dependent density-functional theory. We show that a weak attosecond-pulse-train ionization seed that is properly synchronized with the strong driving mid-infrared laser field can produce experimentally relevant high-harmonic generation (HHG) signals, from which we extract both the spectral amplitude and the target-specific phase (group delay). We also show that further processing of the HHG signal can be used to achieve molecular-frame resolution, i.e., to resolve the contributions from rescattering on different sides of an oriented molecule. In this framework, we investigate transient two-center interference in CO2 and OCS, and how subcycle polarization effects shape the oriented/aligned angle-resolved spectra. (C) 2019 Author(s).
Publication Source (Journal or Book title)
Mauger, F., Abanador, P. M., Lopata, K., & Schafer, K. J. (2019). High-harmonic spectroscopy of transient two-center interference calculated with time-dependent density-functional theory. STRUCTURAL DYNAMICS-US, 6 (4) https://doi.org/10.1063/1.5111349