Journal article : Letter
Imaging three-dimensional molecular structure and dynamics with multiparticle covariance and cumulant Coulomb explosion analysis
- Abstract:
-
Coulomb explosion imaging (CEI) provides a direct means of imaging molecular geometry by correlating fragment ion momenta following the fragmentation of a molecular polycation. Here, we demonstrate the use of three-body covariance and four-body cumulant analysis to extract three-dimensional (3D) structural information from the X-ray-induced Coulomb explosion of tert-butyl iodide (C4H9I). Site-selective ionization at the iodine 4d edge with intense femtosecond soft X-ray pulses from an X-ray free-electron laser (XFEL) enables rapid charge buildup and molecular breakup. By correlating ionic fragments in the molecular frame, we isolate complete dissociation channels and reveal subtle structural changes, such as umbrella-type motion of the branched alkyl chain, during the ionization process. Comparison with point-charge simulations of the Coulomb explosion shows close agreement, validating the approach. These results establish covariance/cumulant mapping as a powerful strategy for imaging complex three-dimensional molecular structures and point the way toward time-resolved CEI using both XFEL and tabletop sources for capturing ultrafast structural dynamics.
- Publication status:
- Published
- Peer review status:
- Peer reviewed
Actions
Access Document
- Files:
-
-
(Preview, Accepted manuscript, pdf, 1.9MB, Terms of use)
-
(Preview, Supplementary materials, pdf, 4.2MB, Terms of use)
-
- Publisher copy:
- 10.1021/acs.jpclett.6c00162
Authors
- Funder identifier:
- 10.13039/501100000275
- Grant:
- RPG-2021-257
- Funder identifier:
- 10.13039/100006151
- Grant:
- DE-FG02-86ER13491
- Funder identifier:
- https://ror.org/001aqnf71
- Grant:
- EP/R010609/1
- Funder identifier:
- https://ror.org/0439y7842
- Grant:
- EP/V026690/1
- Publisher:
- American Chemical Society
- Journal:
- Journal of Physical Chemistry Letters More from this journal
- Article number:
- acs.jpclett.6c00162
- Publication date:
- 2026-03-10
- Acceptance date:
- 2026-02-19
- DOI:
- EISSN:
-
1948-7185
- ISSN:
-
1948-7185
- Language:
-
English
- Subtype:
-
Letter
- Pubs id:
-
2388473
- Local pid:
-
pubs:2388473
- Deposit date:
-
2026-03-12
- ARK identifier:
Terms of use
- Copyright holder:
- Cheng et al
- Copyright date:
- 2026
- Rights statement:
- © 2026 The Authors. Published by American Chemical Society
- Notes:
- The author accepted manuscript (AAM) of this paper has been made available under the University of Oxford's Open Access Publications Policy, and a CC BY public copyright licence has been applied.
- Licence:
- CC Attribution (CC BY)
If you are the owner of this record, you can report an update to it here: Report update to this record