Controlling the Interference of Multiple Molecular Orbitals in High-Harmonic Generation

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

“…Detailed calculations show that the difference arises from the photorecombination dipole moment of HOMO that undergoes a sudden phase variation at the position of the structural minimum. [5] Thus, the minimum observed in CO 2 is mostly dynamical but its position is affected by structural properties as well.…”

“…[15,16,19] Most remarkably, the strong laser field does not lead to a measurable distortion of the electronic wave functions within the accuracy of current experiments, even in polarizable systems like xenon [20] or in molecules with appreciable extension along the direction of the laser field like CO 2 . [4,5] The second step, propagation of the electron wavepacket, is largely dominated by the laser field and is well described by classical equations as evidenced by, e.g. the chirp of attosecond pulses.…”

“…The experiment is thus repeated in each half-cycle of the laser field and the temporal information is read on the photon energy axis, exploiting the one-to-one relationship between transit time and emitted photon energy. [17] Recent experiments show that strongfield ionization does not exclusively prepare the ground state of the cation [4][5][6]28] but that excited states can also be populated. The probability of accessing a certain ionic state is exponentially sensitive to I p [29] but also to the shape of orbitals, [30] which can enhance the contribution of a deeply bound orbital.…”

“…The last few years have seen first successes in the observation of electronic dynamics on this time scale. [3][4][5][6][7] These techniques will enable a new experimental access to electronic structure and electron correlation, which is one of the most challenging problems in chemistry and physics.…”

“…This has been used to track the motion of protons on the attosecond time scale [17,18] and to study electron rearrangement following temporally confined ionization. [4][5][6] The most unusual aspect of these new methods is certainly the possibility to measure attosecond dynamics using multifemtosecond pulses. [2] This property originates in the extreme nonlinearity of the laser-matter interaction at high intensities.…”