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@ARTICLE{Allum:646068,
author = {Allum, Felix and Lam, Chow-shing and Erk, Benjamin and
Bromberger, Hubertus and Bucksbaum, Philip and Britton,
Mathew and Burt, Michael and Ekanayake, Nagitha and
Gabalski, Ian and Garg, Diksha and Gougoula, Eva and
Heathcote, David and Howard, Andrew and Hockett, Paul and
Holland, David and Kumar, Sonu and Lee, Jason Wai Lung and
McManus, Joseph and Mikosch, Jochen and Milesevic, Dennis
and Minns, Russell and Papadopoulou, Christina and Passow,
Christopher and Razmus, Weronika and Roeder, Anja and
Rolles, Daniel and Rouzée, Arnaud and Schuurman, Michael
and Pinto Simao, Alcides and Stolow, Albert and Noor,
Atia-Tul and Unwin, James and Vallance, Claire and Walmsley,
Tiffany and Brouard, Mark and Forbes, Ruaridh},
title = {{F}ragmentation dynamics of {CS}2 dications and trications
following {S} 2p ionization},
journal = {The journal of chemical physics},
volume = {164},
number = {2},
issn = {0021-9606},
address = {Melville, NY},
publisher = {American Institute of Physics},
reportid = {PUBDB-2026-00708},
pages = {024304},
year = {2026},
abstract = {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.},
cin = {FS DOOR-User / FS-FLASH / FS-FLASH-O / FS-FLASH-D / FS-LA /
FS-CFEL-CMI / FS-SMP},
ddc = {530},
cid = {$I:(DE-H253)FS_DOOR-User-20241023$ /
I:(DE-H253)FS-FLASH-20140814 /
I:(DE-H253)FS-FLASH-O-20160930 /
I:(DE-H253)FS-FLASH-D-20160930 / I:(DE-H253)FS-LA-20130416 /
I:(DE-H253)FS-CFEL-CMI-20220405 /
I:(DE-H253)FS-SMP-20171124},
pnm = {631 - Matter – Dynamics, Mechanisms and Control
(POF4-631) / 6G2 - FLASH (DESY) (POF4-6G2) / FS-Proposal:
F-20200773 (F-20200773) / CALIPSOplus - Convenient Access to
Light Sources Open to Innovation, Science and to the World
(730872)},
pid = {G:(DE-HGF)POF4-631 / G:(DE-HGF)POF4-6G2 /
G:(DE-H253)F-20200773 / G:(EU-Grant)730872},
experiment = {EXP:(DE-H253)F-BL1-20150101},
typ = {PUB:(DE-HGF)16},
doi = {10.1063/5.0304278},
url = {https://bib-pubdb1.desy.de/record/646068},
}