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Jahn-Teller Distortion and Dissociation of CCl$_4^+$ by Transient X-ray Spectroscopy Simultaneously at the Carbon K- and Chlorine L-Edge by Ross, Andrew D.; Hait, Diptarka; Scutelnic, Valeriu; Haugen, Eric A.; Ridente, Enrico; Balkew, Mikias B.; Neumark, Daniel M.; Head-Gordon, Martin; Leone, Stephen R. is a scholarly article available to read on EtoBox.

What is Jahn-Teller Distortion and Dissociation of CCl$_4^+$ by Transient X-ray Spectroscopy Simultaneously at the Carbon K- and Chlorine L-Edge about?

X-ray Transient Absorption Spectroscopy (XTAS) and theoretical calculations are used to study CCl$_4^+$ prepared by 800 nm strong-field ionization. XTAS simultaneously probes atoms at the carbon K-edge (280-300 eV) and chlorine L-edge (195-220 eV). Comparison of experiment to X-ray spectra computed by orbital-optimized density functional theory (OO-DFT) indicates that after ionization, CCl$_4^+$ undergoes symmetry breaking driven by Jahn-Teller distortion away from the initial tetrahedral structure (T$_d$) in 6$\pm$2 fs. The resultant symmetry-broken covalently bonded form subsequently separates to a noncovalently bound complex between CCl$_3^+$ and Cl over 90$\pm$10 fs, which is again predicted by theory. Finally, after more than 800 fs, L-edge signals for atomic Cl are observed, indicating dissociation to free CCl$_3^+$ and Cl. The results for Jahn-Teller distortion to the symmetry-broken form of CCl$_4^+$ and formation of the Cl -- CCl$_3^+$ complex characterize previously unobserved new species along the route to dissociation.

Author

Ross, Andrew D.; Hait, Diptarka; Scutelnic, Valeriu; Haugen, Eric A.; Ridente, Enrico; Balkew, Mikias B.; Neumark, Daniel M.; Head-Gordon, Martin; Leone, Stephen R.

Published

2022

Language

EN