Attosecond X-ray spectroscopy reveals the competing stochastic and ballistic dynamics of a bifurcating Jahn–Teller dissociation

Danylo Matselyukh, Vít Svoboda and Hans Jakob Wörner ()
Additional contact information
Danylo Matselyukh: ETH Zürich
Vít Svoboda: ETH Zürich
Hans Jakob Wörner: ETH Zürich

Nature Communications, 2025, vol. 16, issue 1, 1-7

Abstract: Abstract A fundamental approach to understanding chemical processes involves two key concepts: reaction paths and vibrational wavepackets. Collecting sufficient observables to experimentally determine these paths still challenges the latest advances in ultrafast science. Simultaneously observing the coherent nature of the wavepacket following them is even more challenging. Here, exploiting the sub-femtosecond time resolution (σ = 1 fs) of attosecond soft-X-ray-absorption spectroscopy, we overcome both of these challenges and observe a Jahn-Teller-mediated chemical reaction in its entirety—from initial symmetry breaking to beyond dissociation. We find that the Jahn-Teller effect in $${{{{{{\rm{SiH}}}}}^{+}_{4}}}$$ SiH 4 + immediately bifurcates the reaction into two channels: ballistic dissociation into $${{{{{{\rm{SiH}}}}}^{+}_{3}}}$$ SiH 3 + and H in 22.9 ± 0.5 fs in which the vibrational wavepacket is preserved, and—after an induction time of 11 ± 3.4 fs—a stochastic dissociation into $${{{{{{\rm{SiH}}}}}^{+}_{2}}}$$ SiH 2 + and H2 with a timescale of 140 ± 19 fs in which the wavepacket dephases. We find that adiabatic ab-initio molecular dynamics simulations correctly reproduce the ballistic channel, but fail with the stochastic channel. These unprecedented insights into an ultrafast Jahn-Teller-mediated chemical reaction establish the unique potential of our experimental scheme for investigating chemical processes, particularly ones containing non-adiabatic dynamics or involving hydrogen atoms, which are notoriously difficult to detect with other methods, such as electron or X-ray diffraction.

Date: 2025
References: Add references at CitEc
Citations:

Downloads: (external link)
https://www.nature.com/articles/s41467-025-61512-8 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-61512-8

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-025-61512-8

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().