Abstract
In this review, we report on recent progress in the generation and application of multichromatic polarization-tailored pulse sequences for the coherent control of multiphoton ionization (MPI) dynamics and present unpublished experimental results that complement our previous findings. Specifically, we utilize single-color, bichromatic, and trichromatic polarization-controlled pulse sequences generated by spectral amplitude, phase and polarization modulation of a carrier-envelope phase (CEP)-stable white light supercontinuum for MPI. The analysis of the number of ionization pathways and the number of distinct final free electron states shows that both increase significantly, but scale differently with the number of absorbed photons and the number of pulses in the sequence. In our experiments, ultrafast polarization shaping is combined with high-resolution photoelectron tomography to generate, control, and reconstruct three-dimensional photoelectron momentum distributions from atomic and molecular MPI. We discuss the use of polarization-controlled single-color and bichromatic pulse sequences in perturbative and non-perturbative coherent control of coupled electron-nuclear dynamics in molecules, atomic spin-orbit wave packet dynamics and the directional photoemission from atoms and chiral molecules. We compare the coherent control of CEP-insensitive intraband multipath interference in the MPI with a fixed number of photons with CEP-sensitive interband multipath interference in the ionization with a different number of photons. The generation and control of free electron vortices with even-numbered rotational symmetry by MPI with single-color pulse sequences is contrasted with the bichromatic control of CEP-sensitive electron vortices with odd-numbered rotational symmetry. To illustrate the potential of multichromatic pulse sequences for coherent control, we present a trichromatic scheme for shaper-based quantum state holography.
Highlights
The basic principles of coherent control have been established more than 30 years ago [1,2,3,4,5,6]
We have reported on coherent control of multiphoton ionization (MPI) dynamics of atomic and molecular model systems using fully coherent polarization-tailored single-color, bichromatic and trichromatic pulse sequences
Building on previous experiments with single-color pulse sequences, we have shown that the advanced polarization shaping of carrier-envelope phase (CEP)-stable supercontinua enables the generation of unprecedented bichromatic laser fields such as propeller-shaped circularly polarized (CRCP) pulses or Lissajous-like orthogonal linearly polarized (OLP) pulses
Summary
The basic principles of coherent control have been established more than 30 years ago [1,2,3,4,5,6]. Polarization-tailored multicolor femtosecond laser fields have opened up new perspectives in numerous applications ranging from HHG [67,68,69,70,71,72, 74, 75] over the coherent control of ultrafast electron dynamics in atoms and molecules [73, 76,77,78] to the manipulation of coherent excitations in nanostructures [79, 80]. The use of advanced polarization-shaped pulses for the generation of free electron wave packets by MPI has necessitated 3D detection to characterize the full 3D photoelectron momentum distribution (PMD).
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