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Register a new userRevealing the Two-Electron Cusp in the Ground States of He and H2 via Quasifree Double Photoionization
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We report on kinematically complete measurements and ab initio non-perturbative calculations of double ionization of He and H2 by a single 800 eV circularly polarized photon. We confirm the quasifree mechanism of photoionization for H2 and show how it originates from the two-electron cusp in the ground state of a two-electron target. Our approach establishes a new method for mapping electrons relative to each other and provides valuable insight into photoionization beyond the electric-dipole approximation.
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The x-ray energies and transition rates associated with single and double electron radiative transitions from the double K hole state $2s2p$ to the $1s2s$ and $1s^{2}$ configurations of 11 He-like ions ($10!leq!Z!leq!47$) are evaluated using the fully relativistic multi-configuration Dirac-Fock method. An appropriate electron correlation model is constructed with the aid of the active space method, which allows the electron correlation effects to be studied efficiently. The contributions of electron correlation and the Breit interaction to the transition properties are analyzed in detail. It is found that the two-electron one-photon (TEOP) transition is correlation sensitive. The Breit interaction and electron correlation both contribute significantly to the radiative transition properties of the double K hole state of He-like ions. Good agreement between the present calculation and previous work is achieved. The calculated data will be helpful to future investigations on double K hole decay processes of He-like ions.
New sets of functions with arbitrary large finite cardinality are constructed for two-electron atoms. Functions from these sets exactly satisfy the Katos cusp conditions. The new functions are special linear combinations of Hylleraas- and/or Kinoshita-type terms. Standard variational calculation, leading to matrix eigenvalue problem, can be carried out to calculate the energies of the system. There is no need for optimization with constraints to satisfy the cusp conditions. In the numerical examples the ground state energy of the He atom is considered.
We apply a three-dimensional (3D) implementation of the time-dependent restricted-active-space self-consistent-field (TD-RASSCF) method to investigate effects of electron correlation in the ground state of Be as well as in its photoionization dynamics by short XUV pulses, including time-delay in photoionization. First, we obtain the ground state by propagation in imaginary time. We show that the flexibility of the TD-RASSCF on the choice of the active orbital space makes it possible to consider only relevant active space orbitals, facilitating the convergence to the ground state compared to the multiconfigurational time-dependent Hartree-Fock method, used as a benchmark to show the accuracy and efficiency of TD-RASSCF. Second, we solve the equations of motion to compute photoelectron spectra of Be after interacting with a short linearly polarized XUV laser pulse. We compare the spectra for different RAS schemes, and in this way we identify the orbital spaces that are relevant for an accurate description of the photoelectron spectra. Finally, we investigate the effects of electron correlation on the magnitude of the relative time-delay in the photoionization process into two different ionic channels. One channel, the ground state channel in the ion, is accessible without electron correlation. The other channel is only accessible when including electron correlation. The time-delay is highly sensitivity to the choice of the active space, and hence to the account of electron-electron correlation.
We experimentally investigate the effects of the linear photon momentum on the momentum distributions of photoions and photoelectrons generated in one-photon ionization in an energy range of 300 eV $leq~E_gamma~leq$ 40 keV. Our results show that for each ionization event the photon momentum is imparted onto the photoion, which is essentially the systems center of mass. Nevertheless, the mean value of the ion momentum distribution along the light propagation direction is backward-directed by $-3/5$ times the photon momentum. These results experimentally confirm a 90 year old prediction.
In this work, we apply the Monte Carlo wave packet method to study the ultrafast nuclear dynamics following inner-shell photoionization of N2 exposed to an ultrashort intense X-ray pulse. The photon energy of the X-ray pulse is large enough to remove a 1s electron from the N atom in N2. The intermediate state in N+2 is highly excited so that autoionization takes place from this state to the dissociative or non-dissociative electronic states of ungerade and gerade symmetries in N++2. The possible vibrational resonances allowed by the non-dissociative states prevents a direct extraction of the nuclear kinetic release (KER) spectrum from the nuclear wave packets in N++2. Therefore, we propose a hybrid technique by combining the advantages of two energy analysis strategies to obtain the final nuclear KER spectrum of the process. A femtosecond IR probe pulse, which couples the electronic states in N++2 together, is applied to achieve a time-resolved imaging and controlling of the ultrafast dynamics that takes place during double ionization of N2. The influence of the laser parameters including the peak intensity, pulse duration and pump-probe delay, on the nuclear dynamics is also investigated.
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