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  • Letter
  • Open Access

Attosecond photoionization delays in molecules: The role of nuclear motion

Adrián J. Suñer-Rubio1, Christoph Lemell2, Roger Y. Bello3, Joachim Burgdörfer2, Alicia Palacios1,4,5, and Fernando Martín1,6

  • 1Departamento de Química, Módulo 13, Universidad Autónoma de Madrid, 28049 Madrid, Spain
  • 2Institute for Theoretical Physics, Vienna University of Technology, Wiedner Hauptstr. 8-10, A-1040 Vienna, Austria
  • 3Departamento de Química Física Aplicada, Módulo 14, Universidad Autónoma de Madrid (UAM), 28049 Madrid, Spain
  • 4Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid (UAM), 28049 Madrid, Spain
  • 5Institute of Advanced Research in Chemical Sciences (IAdChem), Universidad Autónoma de Madrid (UAM), 28049 Madrid, Spain
  • 6Instituto Madrileño de Estudios Avanzados IMDEA Nanociencia, Cantoblanco, 28049 Madrid, Spain

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Phys. Rev. Research 6, L022066 – Published 20 June, 2024

DOI: https://doi.org/10.1103/PhysRevResearch.6.L022066

Abstract

Molecular photoionization delays are often analyzed by assuming that nuclei remain fixed during the ionization process since they move much more slowly than electrons. However, recent high-energy resolution and multicoincidence experiments have shown that nuclear motion can have a significant and visible effect on the measured ionization delays on the attosecond time scale. To analyze this behavior, we have chosen the simplest of all molecules, H2+, and performed nearly exact calculations of streaking and RABBIT (reconstruction of attosecond beatings by interferences in two-photon transitions) spectra by solving the time-dependent Schrödinger equation in full dimensionality, and retrieved the corresponding photoionization delays. We show that, when two-center effects are at play, nuclear motion is responsible for a substantial increase of the photoionization delays, in particular of the so-called continuum-continuum delays. The magnitude of such an increase is comparable to the absolute values of the measured delays.

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Phys. Rev. Research 6, L022066– Published 20 June, 2024
  • Received 25 January 2024
  • Accepted 22 April 2024
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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.

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