Temporal coherent control of resonant two-photon double ionization of the hydrogen molecule via doubly excited states
Abstract
Here, 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 $$\hat k$$ either parallel or perpendicular to the molecular axis $$\hat R$$. For $$\hat k$$∥ $$\hat R$$ and a pulse carrier frequency of 36 eV resonantly populating the Q21Π$$^+_u$$ (1) doubly excited state as well as other 1Π$$^+_u$$ 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 1P$$^ o_ {±1}$$ doubly excited states; 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 $$\hat k$$⟂$$\hat R$$ and a broadband pulse carrier frequency of 30 eV populating the Q11Π$$^+_u$$(1), Q11Σ$$^+_u$$(1), Q21Π$$^+_u$$(1) , and Q11Σ$$^+_u$$ (2) doubly excited states, the momentum distribution is shown to exhibit dynamical electron vortices with four spiral arms, which originates from the interplay between the 1Δ$$^+_ g$$ ,1Π$$^+_ g$$, and 1Σ$$^+_ g$$ 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.
- Authors:
-
- Univ. of Nebraska, Lincoln, NE (United States)
- Publication Date:
- Research Org.:
- Univ. of Nebraska, Lincoln, NE (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Nebraska Research Initiative
- OSTI Identifier:
- 1850232
- Grant/Contract Number:
- FG03-96ER14646; SC0021054; TG-PHY-120003
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 103; Journal Issue: 5; Journal ID: ISSN 2469-9926
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; atomic and molecular processes in external fields; autoionization; auger processes; coherent control; electron correlation calculation for atoms and ions; multiphoton or tunneling ionization and excitation; single-and few-photon ionization and excitation; ultrafast phenomena
Citation Formats
Ngoko Djiokap, J. M., and Starace, Anthony F. Temporal coherent control of resonant two-photon double ionization of the hydrogen molecule via doubly excited states. United States: N. p., 2021.
Web. doi:10.1103/physreva.103.053110.
Ngoko Djiokap, J. M., & Starace, Anthony F. Temporal coherent control of resonant two-photon double ionization of the hydrogen molecule via doubly excited states. United States. https://doi.org/10.1103/physreva.103.053110
Ngoko Djiokap, J. M., and Starace, Anthony F. Tue .
"Temporal coherent control of resonant two-photon double ionization of the hydrogen molecule via doubly excited states". United States. https://doi.org/10.1103/physreva.103.053110. https://www.osti.gov/servlets/purl/1850232.
@article{osti_1850232,
title = {Temporal coherent control of resonant two-photon double ionization of the hydrogen molecule via doubly excited states},
author = {Ngoko Djiokap, J. M. and Starace, Anthony F.},
abstractNote = {Here, 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 $\hat k$ either parallel or perpendicular to the molecular axis $\hat R$. For $\hat k$∥ $\hat R$ and a pulse carrier frequency of 36 eV resonantly populating the Q21Π$^+_u$ (1) doubly excited state as well as other 1Π$^+_u$ 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 1P$^ o_ {±1}$ doubly excited states; 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 $\hat k$⟂$\hat R$ and a broadband pulse carrier frequency of 30 eV populating the Q11Π$^+_u$(1), Q11Σ$^+_u$(1), Q21Π$^+_u$(1) , and Q11Σ$^+_u$ (2) doubly excited states, the momentum distribution is shown to exhibit dynamical electron vortices with four spiral arms, which originates from the interplay between the 1Δ$^+_ g$ ,1Π$^+_ g$, and 1Σ$^+_ g$ 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.},
doi = {10.1103/physreva.103.053110},
journal = {Physical Review A},
number = 5,
volume = 103,
place = {United States},
year = {Tue May 11 00:00:00 EDT 2021},
month = {Tue May 11 00:00:00 EDT 2021}
}
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