Abstract
We use time-delayed, counter-rotating, circularly polarized few-cycle attosecond nonoverlapping pulses to study the temporal coherent control of the resonant process of two-photon double ionization (TPDI) of hydrogen molecule via doubly excited states for pulse propagation direction along either parallel or perpendicular to the molecular axis . For and a pulse carrier frequency of 36 eV resonantly populating the doubly excited state as well as other doubly excited states, we find that the indirect ionization pathway through these doubly excited states changes the character of the kinematical vortex-shaped momentum distribution produced by the two direct ionization pathways from fourfold to twofold rotational symmetry. This result is similar to what found in TPDI of the He atom involving doubly excited states [Ngoko Djiokap and Starace, J. Opt. 19, 124003 (2017)]; however, angular distributions exhibiting a quantum beat effect between the ground state and a doubly excited state seen for the He atom are observed here for its molecular counterpart with an anomaly in shape and magnitude, not in frequency. The sixfold differential probability integrated over the azimuthal angle of the photoelectron pair shows that this anomaly is due to autoionization decays and quantum beats between doubly excited states. For and a broadband pulse carrier frequency of 30 eV populating the , , , and doubly excited states, the momentum distribution is shown to exhibit dynamical electron vortices with four spiral arms, which originates from the interplay between the , , and dynamical ionization amplitudes. Our treatment within either the adiabatic-nuclei approximation or fixed-nuclei approximation shows that the latter provides a very good account for this correlated process.
- Received 23 October 2020
- Revised 24 March 2021
- Accepted 22 April 2021
DOI:https://doi.org/10.1103/PhysRevA.103.053110
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