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research article

Core-Valence Attosecond Transient Absorption Spectroscopy of Polyatomic Molecules

Golubev, Nikolay V.  
•
Vaníček, Jiří  
•
Kuleff, Alexander I.
September 16, 2021
Physical Review Letters

Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we report an extension of the theory underlying the attosecond transient absorption spectroscopy (ATAS) for the case of molecules, including a full account for the coupled electron-nuclear dynamics in the initially created wave packet, and apply it to probe the oscillations of the positive charge created after outer-valence ionization of the propiolic acid molecule. By taking advantage of element-specific core-to-valence transitions induced by x-ray radiation, we show that the resolution of ATAS makes it possible to trace the dynamics of electron density with atomic spatial resolution.

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Type
research article
DOI
10.1103/PhysRevLett.127.123001
Author(s)
Golubev, Nikolay V.  
Vaníček, Jiří  
Kuleff, Alexander I.
Date Issued

2021-09-16

Published in
Physical Review Letters
Volume

127

Issue

12

Article Number

123001

Subjects

Ultrafast phenomena

•

Molecular spectra

•

Quantum dynamics

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCPT  
FunderGrant Number

ETH Board of the Swiss Federal Institutes of Technology

Branco Weiss Fellowship—Society in Science

FNS-NCCR

NCCR MUST

Other foundations

DFG QUTIF

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Available on Infoscience
September 24, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/181583
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