TY  - JOUR
AU  - Livshits, Ester
AU  - Bittner, Dror M.
AU  - Trost, Florian
AU  - Meister, Severin
AU  - Lindenblatt, Hannes
AU  - Treusch, Rolf
AU  - Gope, Krishnendu
AU  - Pfeifer, Thomas
AU  - Baer, Roi
AU  - Moshammer, Robert
AU  - Strasser, Daniel
TI  - Symmetry-breaking dynamics of a photoionized carbon dioxide dimer
JO  - Nature Communications
VL  - 15
IS  - 1
SN  - 2041-1723
CY  - [London]
PB  - Nature Publishing Group UK
M1  - PUBDB-2024-05371
SP  - 6322
PY  - 2024
AB  - Photoionization can initiate structural reorganization of molecular matter and drive formation of new chemical bonds. Here, we used time-resolved extreme ultraviolet (EUV) pump – EUV probe Coulomb explosion imaging of carbon dioxide dimer ion (CO<sub>2</sub>)<sub>2</sub><sup>+</sup>dynamics, that combined with ab initio molecular dynamics simulations, revealed unexpected asymmetric structural rearrangement. We show that ionization by the pump pulse induces rearrangement from the slipped-parallel (C<sub>2h</sub>) geometry of the neutral CO<sub>2</sub> dimer towards a T-shaped (C<sub>2v</sub>) structure on the  100 fs timescale, although the most stable slipped-parallel (C<sub>2h</sub>) structure of the ionic dimer. Moreover, we find that excited states of the ionized CO<sub>2</sub> dimer can exhibit formation of a CO<sub>3</sub> moiety in the CO<sub>2</sub>O<sub>4</sub><sup>+</sup> complex that can persist even after a suitably time-delayed second photoionization in a metastable CO<sub>2</sub>O<sub>4</sub><sup>+</sup> dication. Our results suggest that charge asymmetry plays an important role in the ionization-induced dynamics in such dimers that are present in C<sub>2</sub> rich environments. 
LB  - PUB:(DE-HGF)16
C6  - pmid:39060261
UR  - <Go to ISI:>//WOS:001279103300003
DO  - DOI:10.1038/s41467-024-50759-2
UR  - https://bib-pubdb1.desy.de/record/612518
ER  -