%0 Journal Article
%A Livshits, Ester
%A Bittner, Dror M.
%A Trost, Florian
%A Meister, Severin
%A Lindenblatt, Hannes
%A Treusch, Rolf
%A Gope, Krishnendu
%A Pfeifer, Thomas
%A Baer, Roi
%A Moshammer, Robert
%A Strasser, Daniel
%T Symmetry-breaking dynamics of a photoionized carbon dioxide dimer
%J Nature Communications
%V 15
%N 1
%@ 2041-1723
%C [London]
%I Nature Publishing Group UK
%M PUBDB-2024-05371
%P 6322
%D 2024
%X 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. 
%F PUB:(DE-HGF)16
%9 Journal Article
%$ pmid:39060261
%U <Go to ISI:>//WOS:001279103300003
%R 10.1038/s41467-024-50759-2
%U https://bib-pubdb1.desy.de/record/612518