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Register a new userMulti-electron dynamics in the tunnel ionization of correlated quantum systems
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Added by
Maximilian Hollstein
Publication date
2015
fields
Physics
and research's language is
English
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The importance of multi-electron dynamics during the tunnel ionization of a correlated quantum system is investigated. By comparison of the solution of the time-dependent Schru007fodinger equation (TDSE) with the time-dependent configuration interaction singles approach (TDCIS), we demonstrate the importance of a multi-electron description of the tunnel ionization process especially for weakly confined quantum systems. Within this context, we observe that adiabatic driving by an intense light field can even enhance the correlations between still trapped electrons.
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Modern intense ultrafast pulsed lasers generate an electric field of sufficient strength to permit tunnel ionization of the valence electrons in atoms. This process is usually treated as a rapid succession of isolated events, in which the states of the remaining electrons are neglected. Such electronic interactions are predicted to be weak, the exception being recollision excitation and ionization caused by linearly-polarized radiation. In contrast, it has recently been suggested that intense field ionization may be accompanied by a two-stage `shake-up reaction. Here we report a unique combination of experimental techniques that enables us to accurately measure the tunnel ionization probability for argon exposed to 50 femtosecond laser pulses. Most significantly for the current study, this measurement is independent of the optical focal geometry, equivalent to a homogenous electric field. Furthermore, circularly-polarized radiation negates recollision. The present measurements indicate that tunnel ionization results in simultaneous excitation of one or more remaining electrons through shake-up. From an atomic physics standpoint, it may be possible to induce ionization from specific states, and will influence the development of coherent attosecond XUV radiation sources. Such pulses have vital scientific and economic potential in areas such as high-resolution imaging of in-vivo cells and nanoscale XUV lithography.
The probability of multiple ionization of krypton by 50 femtosecond circularly polarized laser pulses, independent of the optical focal geometry, has been obtained for the first time. The excellent agreement over the intensity range 10 TWcm-2 to 10 PWcm-2 with the recent predictions of A. S. Kornev et al [Phys. Rev. A v.68, art.043414 (2003)] provides the first experimental confirmation that non-recollisional electronic excitation can occur in strong field ionization. This is particularly true for higher stages of ionization, when the laser intensity exceeds 1 PWcm-2 as the energetic departure of the ionized electron(s) diabatically distorts the wavefunctions of the bound electrons. By scaling the probability of ionization by the focal volume, we discusses why this mechanism was not apparent in previous studies.
The average dwell time of an electron in a potential barrier formed by an external electric field and the potential of a helium atom is evaluated within a semi classical one-dimensional tunneling approach. The tunneling electron is considered to interact with a nuclear charge screened by the electron in the helium ion. It is found that screening leads to smaller average dwell times of the tunneling electron. The dissipative effect of the environment on the tunneling electron is taken into account within a semiclassical model involving a velocity dependent frictional force and is found to change the average dwell time significantly.
A generalized ADK (Ammosov-Delone-Krainov) theory for ionization of open shell atoms is compared to ionization experiments performed on the transition metal atoms V, Ni, Pd, Ta, and Nb. Our theory is found to be in good agreement for V, Ni, Pd, and Ta, whereas conventional ADK theory overestimates ionization by orders of magnitude. The key to understanding the observed ionization reduction is the angular momentum barrier. Our analysis shows that the determination of the angular momentum barrier in open shell atoms is nontrivial. The Stark shift is identified as the second dominant effect responsible for ionization suppression. Finally, these two effects cannot explain the Nb data. An analysis of the electron spins suggests that Pauli blocking might be responsible for the suppression of tunneling in Nb.
Multi-electron dynamics in atoms and molecules very often occur on sub- to few-femtosecond timescales. The available intensities of extreme-ultraviolet (XUV) attosecond pulses have previously only allowed the time-resolved investigation of two-photon, two-electron interactions. Here we demonstrate attosecond control over double and triple ionization of argon atoms involving the absorption of up to five XUV photons. In an XUV-pump XUV-probe measurement using a pair of attosecond pulse trains (APTs), the Ar$^{2+}$ ion yield exhibits a weak delay dependence, showing that its generation predominantly results from the sequential emission of two electrons by photoabsorption from the two APTs. In contrast, the Ar$^{3+}$ ion yield exhibits strong modulations as a function of the delay, which is a clear signature of the simultaneous absorption of at least two XUV photons. The experimental results are well reproduced by numerical calculations that provide detailed insights into the ionization dynamics. Our results open up new opportunities for the investigation and control of multi-electron dynamics and complex electron correlation mechanisms on extremely short timescales.
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