From quantum control of electron hole dynamics in polyatomic molecules towards attosecond pulse shaping

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Attosecond Science has emerged with the discovery of coherent electron-ion collisions induced by a strong laser field, usually referred to as re-collisions . Within one optical period an electron is removed from an atom or molecule, accelerated by the oscillating laser field, and driven back to re-collide and radiatively recombine with the parent ion. This process - high harmonic generation (HHG) - produces tens of eV-broad coherent spectra and has two crucial applications. First, high harmonic emission is used to generate attosecond pulses of light, which can then be used in time-resolved pump-probe experiments. Second, ultra-broad coherent harmonic spectrum carries attosecond information about the underlying nonlinear response, which can be extracted. Our proposal contributes to both applications. Its main objective is to lay the theoretical foundation for attosecond “pulse shapers” in XUV domain. We will develop methods for controlling the properties (spectral phases, amplitudes and polarizations) of attosecond pulses as they are produced by controlling electron-hole dynamics between ionization and recombination. The latter will be achieved by controlling laser-induced transitions between different electronic states of the ion on attosecond time scale and/or controlling the ionization regime. We expect that our approaches will contribute to the development of HHG spectroscopy of multielectron dynamics, with application to shaped attosecond XUV pulses that will open new ways of controlling matter on attosecond time scale.