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Register a new userMultiple ionization of argon via xuv-photon absorption induced by 20-gigawatt high-harmonic pulses
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Paraskevas Tzallas Dr
Publication date
2018
fields
Physics
and research's language is
English
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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.
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We present an experimental study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from non-resonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$ and $f$ partial wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the VUV polarization. The comparison between the present results and two previous sets of theoretical calculations [Pan, C. & Starace, A. F. (1991). $textit{Physical Review A}$, 44(1), 324., and Moccia, R., Rahman, N. K., & Rizzo, A. (1983). $textit{Journal of Physics B: Atomic and Molecular Physics}$, 16(15), 2737.] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.
We investigate the interaction of Xe with isolated attosecond XUV pulses. Specifically, we calculate the ion yields and determine the pathways leading to the formation of ionic charged states up to Xe$^{5+}$. To do so, in our formulation we account for single-photon absorption, sequential multi-photon absorption, direct two-photon absorption, single and double Auger decays, and shake-off. We compare our results for the ion yields and for ion yield ratios with recent experimental results obtained for 93 eV and 115 eV attosecond XUV pulses. In particular, we investigate the role that a sequence of two single-photon ionization processes plays in the formation of Xe$^{4+}$. We find that each one of these two processes ionizes a core electron and thus leads to the formation of a double core-hole state. Remarkably, we find that the formation of Xe$^{5+}$ involves a direct two-photon absorption process and the absorption of a total of three photons.
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.
High-harmonics generation spectroscopy is a promising tool for resolving electron dynamics and structure in atomic and molecular systems. This scheme, commonly described by the strong field approximation, requires a deep insight into the basic mechanism that leads to the harmonics generation. Recently, we have demonstrated the ability to resolve the first stage of the process -- field induced tunnel ionization -- by adding a weak perturbation to the strong fundamental field. Here we generalize this approach and show that the assumptions behind the strong field approximation are valid over a wide range of tunnel ionization conditions. Performing a systematic study -- modifying the fundamental wavelength, intensity and atomic system -- we observed a good agreement with quantum path analysis over a range of Keldysh parameters. The generality of this scheme opens new perspectives in high harmonics spectroscopy, holding the potential of probing large, complex molecular systems.
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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