论文标题
Attosend光谱揭示了ICL分子中依赖对齐的核心孔动力学
Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule
论文作者
论文摘要
位于分子核心壳中的电子的去除会产生瞬时状态，这些状态居住在几个飞秒之间。由于这些短寿命，这些状态的时间分辨研究具有挑战性，很难观察到仅由电子相关驱动的复杂分子动力学。在这里，碘单氯化物的核心兴奋的状态寿命很少，可以通过在55 eV左右的碘4D-16p过渡上获得attosent瞬时吸收。核心水平的配体场分裂允许直接访问沿着ICL分子轴对准并垂直于ICL分子轴的激发状态。对于平行于键的核心孔状态，获得了3.5 fs和4.3 fs的寿命，垂直状态为6.5 fs和6.9 fs，而在此时间表上，核运动基本上是冻结的。理论表明，平行于共价键的核心胶合体的寿命急剧下降是与ICL相邻CL原子的非本地相互作用的表现。
The removal of electrons located in the core shells of molecules creates transient states that live between a few femtoseconds to attoseconds. Owing to these short lifetimes, time-resolved studies of these states are challenging and complex molecular dynamics driven solely by electronic correlation are difficult to observe. Here, few-femtosecond core-excited state lifetimes of iodine monochloride are obtained by attosecond transient absorption on iodine 4d-16p transitions around 55 eV. Core-level ligand field splitting allows direct access of excited states aligned along and perpendicular to the ICl molecular axis. Lifetimes of 3.5 fs and 4.3 fs are obtained for core-hole states parallel to the bond and 6.5 fs and 6.9 fs for perpendicular states, while nuclear motion is essentially frozen on this timescale. Theory shows that the dramatic decrease of lifetime for core-vacancies parallel to the covalent bond is a manifestation of non-local interactions with the neighboring Cl atom of ICl.
