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Attosecond spectroscopy reveals spontaneous symmetry breaking in molecular photoionization

Li, Mingxuan LU ; Zhao, Leshi ; Wang, Huiyong LU ; Li, Jialong LU ; Wang, Wentao ; Cai, Jiaao ; Hong, Xiaochun ; Shi, Xiaosen ; Zhang, Ming and Zhao, Xinning , et al. (2025) In Science Advances 11(38). p.1-8
Abstract

Spontaneous symmetry breaking, driven by nonadiabatic electron-nuclear coupling, can lead to geometric com plexity in molecules and solids. While structural distortion from symmetry breaking occurs in femtoseconds, the timescale to lift electronic state degeneracy has remained elusive. We use the vibrationally resolved attosecond chronoscope to capture the electronic symmetry breaking induced by the Renner-Teller effect in bent CO2 mole cules after photoionization by an extreme ultraviolet photon by measuring attosecond ionization delays. Relative photoionization delays between the four cation states are observed, with vibrational state–dependent delays, we analyze the evolution of the degenerate A2Πu... (More)

Spontaneous symmetry breaking, driven by nonadiabatic electron-nuclear coupling, can lead to geometric com plexity in molecules and solids. While structural distortion from symmetry breaking occurs in femtoseconds, the timescale to lift electronic state degeneracy has remained elusive. We use the vibrationally resolved attosecond chronoscope to capture the electronic symmetry breaking induced by the Renner-Teller effect in bent CO2 mole cules after photoionization by an extreme ultraviolet photon by measuring attosecond ionization delays. Relative photoionization delays between the four cation states are observed, with vibrational state–dependent delays, we analyze the evolution of the degenerate A2Πu state to the nondegenerate A′ and A″ states due to molecular bend ing. With the help of theoretical analysis, we show that the relative photoionization delays of up to 72 as between the vibrational levels originate from the symmetry breaking–induced shape resonance. This study offers funda mental insights by resolving the coupled electron and structural dynamics simultaneously.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Science Advances
volume
11
issue
38
pages
8 pages
publisher
American Association for the Advancement of Science (AAAS)
external identifiers
  • scopus:105016637417
  • pmid:40971424
ISSN
2375-2548
DOI
10.1126/sciadv.adw5415
language
English
LU publication?
yes
additional info
Publisher Copyright: Copyright © 2025 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).
id
07836943-206b-440f-8dcd-83bd8f5f16fc
date added to LUP
2025-11-19 23:10:57
date last changed
2025-11-20 09:41:21
@article{07836943-206b-440f-8dcd-83bd8f5f16fc,
  abstract     = {{<p>Spontaneous symmetry breaking, driven by nonadiabatic electron-nuclear coupling, can lead to geometric com plexity in molecules and solids. While structural distortion from symmetry breaking occurs in femtoseconds, the timescale to lift electronic state degeneracy has remained elusive. We use the vibrationally resolved attosecond chronoscope to capture the electronic symmetry breaking induced by the Renner-Teller effect in bent CO<sub>2</sub> mole cules after photoionization by an extreme ultraviolet photon by measuring attosecond ionization delays. Relative photoionization delays between the four cation states are observed, with vibrational state–dependent delays, we analyze the evolution of the degenerate A<sup>2</sup>Π<sub>u</sub> state to the nondegenerate A′ and A″ states due to molecular bend ing. With the help of theoretical analysis, we show that the relative photoionization delays of up to 72 as between the vibrational levels originate from the symmetry breaking–induced shape resonance. This study offers funda mental insights by resolving the coupled electron and structural dynamics simultaneously.</p>}},
  author       = {{Li, Mingxuan and Zhao, Leshi and Wang, Huiyong and Li, Jialong and Wang, Wentao and Cai, Jiaao and Hong, Xiaochun and Shi, Xiaosen and Zhang, Ming and Zhao, Xinning and Weissenbilder, Robin and Busto, David and Gisselbrecht, Mathieu and Ueda, Kiyoshi and Luo, Sizuo and Li, Zheng and Ding, Dajun}},
  issn         = {{2375-2548}},
  language     = {{eng}},
  month        = {{09}},
  number       = {{38}},
  pages        = {{1--8}},
  publisher    = {{American Association for the Advancement of Science (AAAS)}},
  series       = {{Science Advances}},
  title        = {{Attosecond spectroscopy reveals spontaneous symmetry breaking in molecular photoionization}},
  url          = {{http://dx.doi.org/10.1126/sciadv.adw5415}},
  doi          = {{10.1126/sciadv.adw5415}},
  volume       = {{11}},
  year         = {{2025}},
}