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Register a new userQuantum Coherence in Photo-Ionization with Tailored XUV Pulses
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Added by
Stefanos Carlstr\\\"om
Publication date
2017
fields
Physics
and research's language is
English
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Ionization with ultrashort pulses in the extreme ultraviolet (XUV) regime can be used to prepare an ion in a superposition of spin--orbit substates. In this work, we study the coherence properties of such a superposition, created by ionizing xenon atoms using two phase-locked XUV pulses at different frequencies. In general, if the duration of the driving pulse exceeds the quantum beat period, dephasing will occur. If however, the frequency difference of the two pulses matches the spin--orbit splitting, the coherence can be efficiently increased and dephasing does not occur.
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We analyze the photoelectron angular distribution in two-pathway interference between non-resonant one-photon and resonant two-photon ionization of neon. We consider a bichromatic femtosecond XUV pulse whose fundamental frequency is tuned near the $2p^5 3s$ atomic states of neon. The time-dependent Schrodinger equation is solved and the results are employed to compute the angular distribution and the associated anisotropy parameters at the main photoelectron line. We also employ a time-dependent perturbative approach, which allows obtaining information on the process for a large range of pulse parameters, including the steady-state case of continuous radiation, i.e., an infinitely long pulse. The results from the two methods are in relatively good agreement over the domain of applicability of perturbation theory.
A new approach for few-femtosecond time-resolved photoelectron spectroscopy in condensed matter that balances the combined needs for both temporal and energy resolution is demonstrated. Here, the method is designed to investigate a prototypical Mott insulator, tantalum disulphide (1T-TaS2), which transforms from its charge-density-wave ordered Mott insulating state to a conducting state in a matter of femtoseconds. The signature to be observed through the phase transition is a charge-density-wave induced splitting of the Ta 4f core-levels, which can be resolved with sub-eV spectral resolution. Combining this spectral resolution with few-femtosecond time resolution enables the collapse of the charge ordered Mott state to be clocked. Precise knowledge of the sub-20-femtosecond dynamics will provide new insight into the physical mechanism behind the collapse and may reveal Mott physics on the timescale of electronic hopping.
We report the observation of multiple ionization of Argon through multi-XUV-photon absorption induced by an unprecedentedly powerful laser driven high-harmonic-generation source. Comparing the measured intensity dependence of the yield of the different Argon charge states with numerical calculations we can infer the different channels -direct and sequential- underlying the interaction. While such studies were feasible so far only with FEL sources, this work connects highly-non-linear-XUV-processes with the ultra-short time scales, inherent to the harmonic pulses, and highlights the advanced perspectives of emerging large scale laser research infrastructures.
We propose a new scenario to apply IR-pump-XUV-probe schemes to resolving strong field ionization induced and attosecond pulse driven electron-hole dynamics and coherence in real time. The coherent driving of both the infrared laser and the attoscond pulse correlates the dynamics of the core-hole and the valence-hole which leads to the otherwise forbidden absorption and emission of XUV photon. An analytical model is developed based on the strong-field approximation by taking into account of the essential multielectron configurations. The emission spectra from the core-valence transition and the core-hole recombination are found modulating strongly as functions of the time delay between the two pulses, which provides a unique insight into the instantaneous ionization and the interplay of the multi-electron-hole coherence.
We review the main aspects of multiple photoionization processes in atoms exposed to intense, short wavelength radiation. The main focus is the theoretical framework for the description of such processes as well as the conditions under which direct multiphoton multiple ionization processes can dominate over the sequential ones. We discuss in detail the mechanisms available in different wavelength ranges from the infrared to the hard X-rays. The effect of field fluctuations, present at this stage in all SASE free-electron-laser (FEL) facilities, as well as the effect of the interaction volume integration, are also discussed.
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