Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry
Optimal phases of even harmonics determined by molecular attosecond interferometry with THz phase reference. (a) Experimental dependence of high-harmonic and terahertz spectroscopy (HATS) on the alignment angle and two-color relative phase. Intensity modulations of different harmonics are normalized under each alignment angle , respectively. The black dashed line is the fit of modulation of THz yields. (b) Comparison between the observed optimal phases (OPs) with the parallel (green solid lines), 45-degree (blue solid lines), and perpendicular (violet solid lines) alignments, as well as the calculated OPs considering only the HOMO (black dashed lines), HOMO-1 (light-gray dashed lines), and HOMO-2 (gray dotted lines) channels via the SFA method and the calculated OPs (red open circles) via the time-dependent Hartree-Fock (TDHF) method with parallel alignment. The scales of the error bar are indicated by the horizontal lines. (c) Calculated high-harmonic spectra from parallel-aligned CO2 when the HOMO, HOMO-1, and HOMO-2 are involved based on the TDHF method. The blue and red bars represent the intensities of odd and even harmonics under two-color fields with the phase delay , respectively. The green solid lines show the calculated results under the fundamental field. The black arrow indicates the intensity minimum induced by the interference between HOMO and HOMO-2 channels.