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research article

Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules

Ji, Jia-Bao
•
Guo, Zhaoheng  
•
Driver, Taran
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November 14, 2025
Physical Review X

Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, the spectral congestion of valence photoelectron spectra sets fundamental limits to the complexity of systems that can be studied, and the delocalization of valence electron wave functions blurs the spatial origin of the photoelectron wave packet. Using attosecond x-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: The photoelectron spectra remain atomlike, the measurements become element specific, and the observed scattering dynamics originate from a pointlike source when multicenter interference effects are negligible. We exploit these unique features to reveal the effects of changing functional groups (C-H vs N) and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N − 1 s and C − 1 s core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wave function with the replacement of C-H groups by N atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter.

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Type
research article
DOI
10.1103/dp5w-qxqc
Author(s)
Ji, Jia-Bao
Guo, Zhaoheng  

École Polytechnique Fédérale de Lausanne

Driver, Taran
Trevisan, Cynthia S.
Cesar, David
Cheng, Xinxin
Duris, Joseph
Franz, Paris L.
Glownia, James
Gong, Xiaochun
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Date Issued

2025-11-14

Publisher

American Physical Society (APS)

Published in
Physical Review X
Volume

15

Issue

4

Article Number

041031

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LUXS  
FunderFunding(s)Grant NumberGrant URL

SLAC National Accelerator Laboratory

U.S. Department of Energy

Office of Science

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Available on Infoscience
November 17, 2025
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/255879
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