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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
Title: Jahn-Teller distortion and dissociation of CCl 4 + by transient X-ray spectroscopy simultaneously at the carbon K- and chlorine L-edge
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 ± 2 fs. The resultant symmetry-broken covalently bonded form subsequently separates to a noncovalently bound complex between CCl 3 + and Cl over 90 ± 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.  more » « less
Award ID(s):
1852537
PAR ID:
10354729
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Chemical Science
Volume:
13
Issue:
32
ISSN:
2041-6520
Page Range / eLocation ID:
9310 to 9320
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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