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Impulsive control of the atomic dipole response in the time and frequency domain


Blättermann,  Alexander
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Blättermann, A. (2016). Impulsive control of the atomic dipole response in the time and frequency domain. PhD Thesis, Ruprecht-Karls-Universität, Heidelberg.

Cite as: https://hdl.handle.net/11858/00-001M-0000-0029-5CB2-0
The dipole response of an excited quantum system gives direct insight into the electron dynamics triggered by the incoming light. Spectroscopy techniques such as (attosecond) transient absorption spectroscopy make use of the fact that the dipole response leaves its characteristic fingerprint on the transmitted light. In this work, a general and comprehensive model is introduced, which allows for an analytic description of dipole dynamics triggered and modified by two ultrashort light pulses in both time and frequency domains. Based on this description, a two-dimensional spectral representation of time delay–resolved absorption data is developed. The power of the method to separate different pathways of light–matter interaction, which allows for their individual investigation, is demonstrated experimentally by studying electronic wave packet dynamics in doubly excited helium and inner-valence excited xenon. Furthermore, an in situ technique for characterization of the intense dressing laser pulse that drives (nonlinear) quantum dynamics in time-resolved absorption experiments is derived from the same analytic model and demonstrated experimentally. The possibility to characterize these ultrashort strong-field laser pulses directly within the spectroscopy target enhances the scope of transient absorption spectroscopy as it allows for the precise measurement and control of electron dynamics and increases the comparability between experiment and theory.