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@ARTICLE{Kilaj:465265,
author = {Kilaj, Ardita and Käser, Silvan and Wang, Jia and Stranak,
Patrik and Schwilk, Max and Xu, Lei and von Lilienfeld, O.
Anatole and Küpper, Jochen and Meuwly, Markus and
Willitsch, Stefan},
title = {{C}onformational and state-specific effects in reactions of
2,3-dibromobutadiene with {C}oulomb-crystallized calcium
ions},
journal = {Physical chemistry, chemical physics},
volume = {25},
number = {20},
issn = {1463-9076},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {PUBDB-2021-03818, arXiv:2303.11813},
pages = {13933 - 13945},
year = {2023},
abstract = {Recent advances in experimental methodology enabled studies
of the quantum-state- and conforma- tional dependence of
chemical reactions under precisely controlled conditions in
the gas phase. Here, we generated samples of selected gauche
and s-trans 2,3-dibromobutadiene (DBB) by electrostatic
deflection in a molecular beam and studied their reaction
with Coulomb crystals of laser-cooled Ca$^+$ ions in an ion
trap. The rate coefficients for the total reaction were
found to strongly depend on both the conformation of DBB and
the electronic state of Ca$^+$. In the (4p) $^2P_{1/2}$ and
(3d) $^2D_{3/2}$ excited states of Ca$^+$, the reaction is
capture-limited and faster for the gauche conformer due to
long-range ion-dipole interactions. In the (4s) $^2S_{1/2}$
ground state of Ca$^+$, the reaction rate for s-trans DBB
still conforms with the capture limit, while that for gauche
DBB is strongly suppressed. The exper- imental observations
were analysed with the help of adiabatic capture theory,
ab-initio calculations, and reactive molecular dynamics
simulations on a machine-learned full-dimensional potential
en- ergy surface of the system. The theory yields
near-quantitative agreement for s-trans-DBB, but
overestimates the reactivity of the gauche- conformer
compared to the experiment. The present study points to the
important role of molecular geometry even in strongly
reactive exothermic systems and illustrates striking
differences in the reactivity of individual conformers in
gas-phase ion-molecule reactions.},
cin = {FS-CFELCMI / UNI/EXP / UNI/CUI},
ddc = {540},
cid = {I:(DE-H253)FS-CFELCMI-20150527 /
$I:(DE-H253)UNI_EXP-20120731$ /
$I:(DE-H253)UNI_CUI-20121230$},
pnm = {631 - Matter – Dynamics, Mechanisms and Control
(POF4-631) / DFG project 390715994 - EXC 2056: CUI: Advanced
Imaging of Matter (390715994) / Ex-Net-0002-Phase2-3 -
Advanced Imaging of Matter: Structure, Dynamics and Control
on the Atomic Scale - AIM $(2018_Ex-Net-0002-Phase2-3)$},
pid = {G:(DE-HGF)POF4-631 / G:(GEPRIS)390715994 /
$G:(DE-HGF)2018_Ex-Net-0002-Phase2-3$},
experiment = {EXP:(DE-H253)CFEL-Exp-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {37190820},
UT = {WOS:000988047600001},
eprint = {2303.11813},
howpublished = {arXiv:2303.11813},
archivePrefix = {arXiv},
SLACcitation = {$\%\%CITATION$ = $arXiv:2303.11813;\%\%$},
doi = {10.1039/D3CP01416A},
url = {https://bib-pubdb1.desy.de/record/465265},
}