3 research outputs found
Jahn-Teller Distortion and Dissociation of CCl 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 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 undergoes symmetry breaking driven by Jahn-Teller
distortion away from the initial tetrahedral structure (T) in 62 fs.
The resultant symmetry-broken covalently bonded form subsequently separates to
a noncovalently bound complex between CCl and Cl over 9010 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 and Cl.
The results for Jahn-Teller distortion to the symmetry-broken form of CCl
and formation of the Cl -- CCl complex characterize previously unobserved
new species along the route to dissociation
Correction: Jahn-Teller distortion and dissociation of CCl4 + by transient X-ray spectroscopy simultaneously at the carbon K- and chlorine L-edge.
[This corrects the article DOI: 10.1039/D2SC02402K.]
Jahn-Teller distortion and dissociation of CCl4 + 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 CCl4 + 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, CCl4 + undergoes symmetry breaking driven by Jahn-Teller distortion away from the initial tetrahedral structure (Td) in 6 ± 2 fs. The resultant symmetry-broken covalently bonded form subsequently separates to a noncovalently bound complex between CCl3 + 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 CCl3 + and Cl. The results for Jahn-Teller distortion to the symmetry-broken form of CCl4 + and formation of the Cl-CCl+ 3 complex characterize previously unobserved new species along the route to dissociation