论文标题
Jahn-Teller的失真和CCL $ _4^+$的分离，同时在碳K和氯L-EDGE上同时X射线光谱
Jahn-Teller Distortion and Dissociation of CCl$_4^+$ by Transient X-ray Spectroscopy Simultaneously at the Carbon K- and Chlorine L-Edge
论文作者
论文摘要
X射线瞬态吸收光谱（XTA）和理论计算用于研究由800 nm强场电离制备的CCL $ _4^+$。 XTA同时探测碳K-EDGE（280-300 eV）和氯L-EDGE（195-220 eV）的原子。通过轨道优化的密度功能理论（OO-DFT）计算的实验与X射线光谱的比较表明，电离后，CCL $ _4^+$在6 $ \ pm 2 fs中从初始四面体结构（T $ _D $）中驱动的Jahn-Teller畸变驱动的对称破坏。随后，所得的对称性破裂形式随后将CCL $ _3^+$和CL之间的非共价结合复合物与90美元$ \ pm $ 10 fs分开，理论再次预测了这一点。最后，在超过800 fs之后，观察到了原子CL的L边缘信号，表明解离为免费的CCL $ _3^+$和Cl。 Jahn-Teller对CCL $ _4^+$的对称形式形式的结果以及Cl-Ccl $ _3^+$复合物的形成表征了以前未观察到的新物种，沿着路线解离。
X-ray Transient Absorption Spectroscopy (XTAS) and theoretical calculations are used to study CCl$_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.
