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Unveiling the X-ray-Induced Rabi Dynamics in Resonant Auger Fragment Spectra
School of Physics and Information Technology, Shaanxi Normal University, Xi’an 710119, China.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Theoretical Chemistry and Biology.ORCID iD: 0000-0003-1269-8760
School of Physics and Information Technology, Shaanxi Normal University, Xi’an 710119, China; School of Physics and Optoelectronic Engineering, Ludong University, Yantai 264025, China.
School of Physics and Information Technology, Shaanxi Normal University, Xi’an 710119, China.
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2025 (English)In: The Journal of Physical Chemistry Letters, E-ISSN 1948-7185, Vol. 16, no 36, p. 9561-9567Article in journal (Refereed) Published
Abstract [en]

Vibrationally resolved resonant Auger spectroscopy (RAS) on bound-continuum transitions enables highly sensitive probing of ultrafast dissociation in molecular core-excited states, where a distinct fragment band arises from Auger decay in dissociation fragments. Here, we theoretically investigate fragment band formation driven by ultrashort X-ray pulses. Unlike conventional molecular bands, fragment RAS peaks exhibit an insensitivity to strong X-ray Rabi oscillations. Numerical simulations on water molecules reveal that combining RAS with a fragment's kinetic energy release spectra enables clear observation of Rabi oscillation when the pulse broadening is smaller than the fragment's vibrational frequencies. This work establishes a framework for controlling ultrafast electron-nuclear dynamics in fragmentation by using X-ray pulses.

Place, publisher, year, edition, pages
American Chemical Society (ACS) , 2025. Vol. 16, no 36, p. 9561-9567
National Category
Atom and Molecular Physics and Optics Condensed Matter Physics
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URN: urn:nbn:se:kth:diva-370401DOI: 10.1021/acs.jpclett.5c02116ISI: 001564350200001PubMedID: 40907039Scopus ID: 2-s2.0-105015753739OAI: oai:DiVA.org:kth-370401DiVA, id: diva2:2001818
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QC 20250929

Available from: 2025-09-29 Created: 2025-09-29 Last updated: 2025-09-29Bibliographically approved

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Kimberg, Victor

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