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research article

Decoherence and revival in attosecond charge migration driven by non-adiabatic dynamics

Matselyukh, Danylo T.
•
Despre, Victor
•
Golubev, Nikolay, V
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August 4, 2022
Nature Physics

Attosecond charge migration is a periodic evolution of the charge density at specific sites of a molecule on a timescale defined by the energy intervals between the electronic states involved. Here we report the observation of charge migration in neutral silane (SiH4) in 690 as, its decoherence within 15 fs and its revival after 40-50 fs, using X-ray attosecond transient-absorption spectroscopy. We observe the migration of charge as pairs of quantum beats with a characteristic spectral phase in the transient spectrum, in agreement with theory. The decay and revival of the degree of electronic coherence is found to be a result of both adiabatic and non-adiabatic dynamics in the populated Rydberg and valence states. The experimental results are supported by fully quantum-mechanical ab initio calculations that include both electronic and nuclear dynamics, which additionally support the experimental evidence that conical intersections can mediate the transfer of electronic coherence from an initial superposition state to another one involving a different lower-lying state. X-ray ultrafast transient absorption spectroscopy captures the charge migration in neutral silane molecules, which shows in the spectra as pairs of quantum beats.

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Type
research article
DOI
10.1038/s41567-022-01690-0
Web of Science ID

WOS:000836090300001

Author(s)
Matselyukh, Danylo T.
•
Despre, Victor
•
Golubev, Nikolay, V
•
Kuleff, Alexander, I
•
Woerner, Hans Jakob
Date Issued

2022-08-04

Published in
Nature Physics
Volume

18

Start page

1206

End page

1213

Subjects

Physics, Multidisciplinary

•

Physics

•

si 2p

•

photoabsorption

•

ionization

•

valence

•

model

•

field

Peer reviewed

REVIEWED

Written at

EPFL

Available on Infoscience
August 15, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/190019
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