Ultrafast Science / 2021 / Article / Fig 1

Research Article

Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry

Figure 1

Threefold control of molecular attosecond interferometry. (a) Control of molecular rotation. Experimental yield of the harmonic 25th from CO2 as a function of the alignment and generation pulse delay . The two figures in the bottom sketch the calculated rotational wave packet at the alignment ( ps) and antialignment ( ps) moments. (b) Control of attosecond electron wave packet. The arms on the left and right sides of the electron wave packet are constructed by the adjacent half-cycles of the laser. Two symmetric trajectories are generated by using only the fundamental laser pulse (red trajectories), while adding the second-harmonic pulse can break the symmetry (blue trajectories) and introduce the even harmonics and THz emissions. is the direction of molecular axis with respect to the generation pulse polarization. (c) Control of hole formation. The calculated HOMO, HOMO-1, and HOMO-2 orbitals are shown with their binding energies, respectively [22]. Ionization of molecules is strongly dependent on the molecular orbitals involved. The angle-resolved hole wave packet in the molecular frame can be reconstructed by EWPs propagating in opposite directions to exhibit the deformation of a hole and therefore, under different azimuth angle , form molecular attosecond interferometry (data from H28).