Skip to main content

Research Repository

Advanced Search

Ultrafast isomerization in acetylene dication after carbon K-shell ionization

Li, Zheng; Inhester, Ludger; Liekhus-Schmaltz, Chelsea; Curchod, Basile F.E.; Snyder, James W.; Medvedev, Nikita; Cryan, James; Osipov, Timur; Pabst, Stefan; Vendrell, Oriol; Bucksbaum, Phil; Martinez, Todd J.

Ultrafast isomerization in acetylene dication after carbon K-shell ionization Thumbnail


Authors

Zheng Li

Ludger Inhester

Chelsea Liekhus-Schmaltz

James W. Snyder

Nikita Medvedev

James Cryan

Timur Osipov

Stefan Pabst

Oriol Vendrell

Phil Bucksbaum

Todd J. Martinez



Abstract

Ultrafast proton migration and isomerization are key processes for acetylene and its ions. However, the mechanism for ultrafast isomerization of acetylene [HCCH]2+ to vinylidene [H2CC]2+ dication remains nebulous. Theoretical studies show a large potential barrier ( > 2 eV) for isomerization on low-lying dicationic states, implying picosecond or longer isomerization timescales. However, a recent experiment at a femtosecond X-ray free-electron laser suggests sub-100 fs isomerization. Here we address this contradiction with a complete theoretical study of the dynamics of acetylene dication produced by Auger decay after X-ray photoionization of the carbon atom K shell. We find no sub-100 fs isomerization, while reproducing the salient features of the time-resolved Coulomb imaging experiment. This work resolves the seeming contradiction between experiment and theory and also calls for careful interpretation of structural information from the widely applied Coulomb momentum imaging method.

Citation

Li, Z., Inhester, L., Liekhus-Schmaltz, C., Curchod, B. F., Snyder, J. W., Medvedev, N., …Martinez, T. J. (2017). Ultrafast isomerization in acetylene dication after carbon K-shell ionization. Nature Communications, 8(1), Article 453. https://doi.org/10.1038/s41467-017-00426-6

Journal Article Type Article
Acceptance Date Jun 28, 2017
Online Publication Date Sep 6, 2017
Publication Date Sep 6, 2017
Deposit Date Nov 6, 2017
Publicly Available Date Mar 29, 2024
Journal Nature Communications
Publisher Nature Research
Peer Reviewed Peer Reviewed
Volume 8
Issue 1
Article Number 453
DOI https://doi.org/10.1038/s41467-017-00426-6

Files

Published Journal Article (1.7 Mb)
PDF

Publisher Licence URL
http://creativecommons.org/licenses/by/4.0/

Copyright Statement
Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.




You might also like



Downloadable Citations