TY  - JOUR
AU  - Allum, Felix
AU  - Lam, Chow-shing
AU  - Erk, Benjamin
AU  - Bromberger, Hubertus
AU  - Bucksbaum, Philip
AU  - Britton, Mathew
AU  - Burt, Michael
AU  - Ekanayake, Nagitha
AU  - Gabalski, Ian
AU  - Garg, Diksha
AU  - Gougoula, Eva
AU  - Heathcote, David
AU  - Howard, Andrew
AU  - Hockett, Paul
AU  - Holland, David
AU  - Kumar, Sonu
AU  - Lee, Jason Wai Lung
AU  - McManus, Joseph
AU  - Mikosch, Jochen
AU  - Milesevic, Dennis
AU  - Minns, Russell
AU  - Papadopoulou, Christina
AU  - Passow, Christopher
AU  - Razmus, Weronika
AU  - Roeder, Anja
AU  - Rolles, Daniel
AU  - Rouzée, Arnaud
AU  - Schuurman, Michael
AU  - Pinto Simao, Alcides
AU  - Stolow, Albert
AU  - Noor, Atia-Tul
AU  - Unwin, James
AU  - Vallance, Claire
AU  - Walmsley, Tiffany
AU  - Brouard, Mark
AU  - Forbes, Ruaridh
TI  - Fragmentation dynamics of CS2 dications and trications following S 2p ionization
JO  - The journal of chemical physics
VL  - 164
IS  - 2
SN  - 0021-9606
CY  - Melville, NY
PB  - American Institute of Physics
M1  - PUBDB-2026-00708
SP  - 024304
PY  - 2026
AB  - We present the results from a detailed study of the fragmentation dynamics of and, formed in intense femtosecond soft x-ray pulses above the sulfur 2p edge, primarily through single core photoionization from the S 2p site, and subsequent Auger–Meitner decay(s). By combining three-dimensional velocity map imaging with covariance analysis, we determine the relative momenta of the ions produced in each two- and three-body fragmentation channel, at significantly higher ion count rates than conventional coincidence measurements. We shed new light on the wide range of fragmentation channels observed from the CS2 dication and trication, including channels that involve ionization-induced bond formation and fragmentations producing undetected neutral cofragments. In the latter case, a “native frames” approach is used to isolate contributions from concerted and sequential fragmentations and extract dynamical information about each step of a concerted fragmentation process. While dications often fragment sequentially, the trication is dominated by concerted fragmentation. The main trication fragmentation channel into S+ + C+ + S+ can be well-approximated by classical Coulombic simulations of the ground-state geometry distribution, reflecting both the nature of the trication potential energy surface and the rapid multiple ionization prior to substantial structural dynamics. This study demonstrates ways in which fundamental insights into the fragmentation dynamics of polycations following x-ray ionization may be extracted, which will be beneficial to future studies that employ time-resolved x-ray Coulomb explosion imaging to study ultrafast photochemistry.
LB  - PUB:(DE-HGF)16
DO  - DOI:10.1063/5.0304278
UR  - https://bib-pubdb1.desy.de/record/646068
ER  -