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Vibronic Coupling through the Continuum in the e+CO2 System

Jan Dvořák, Miloš Ranković, Karel Houfek, Pamir Nag, Roman Čurík, Juraj Fedor, and Martin Čížek
Phys. Rev. Lett. 129, 013401 – Published 27 June 2022

Abstract

We report two-dimensional electron energy-loss spectra of CO2. The high-resolution experiment reveals a counterintuitive fine structure at energy losses where CO2 states form a vibrational pseudocontinuum. Guided by the symmetry of the system, we constructed a four-dimensional nonlocal model for the vibronic dynamics involving two shape resonances (forming a Renner-Teller Πu doublet at the equilibrium geometry) coupled to a virtual Σg+ state. The model elucidates the extremely non-Born-Oppenheimer dynamics of the coupled nuclear motion and explains the origin of the observed structures. It is a prototype of the vibronic coupling of metastable states in continuum.

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  • Received 11 February 2022
  • Revised 20 April 2022
  • Accepted 20 May 2022

DOI:https://doi.org/10.1103/PhysRevLett.129.013401

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

Published by the American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Jan Dvořák1, Miloš Ranković2, Karel Houfek1, Pamir Nag2, Roman Čurík2, Juraj Fedor2,*, and Martin Čížek1,†

  • 1Charles University, Faculty of Mathematics and Physics, Institute of Theoretical Physics, V Holešovičkách 2, 180 00 Prague 8, Czech Republic
  • 2J. Heyrovský Institute of Physical Chemistry, Czech Academy of Sciences, Dolejškova 2155/3, 182 23 Prague 8, Czech Republic

  • *Corresponding author. juraj.fedor@jh-inst.cas.cz
  • Corresponding author. martin.cizek@mff.cuni.cz

See Also

Vibrational excitation in the e+CO2 system: Nonlocal model of ΣΠ vibronic coupling through the continuum

Jan Dvořák, Karel Houfek, and Martin Čížek
Phys. Rev. A 105, 062821 (2022)

Article Text

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Issue

Vol. 129, Iss. 1 — 1 July 2022

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