Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule.
Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule.
复制标题
阿秒光谱揭示了ICl分子中依赖于取向的核-孔动力学。
DOI：
10.1038/s41467-020-19496-0
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发表时间：
2020-11-16
影响因子：
16.6
通讯作者：
Neumark DM
中科院分区：
文献类型：
--
作者：
Marroux HJB;Fidler AP;Ghosh A;Kobayashi Y;Gokhberg K;Kuleff AI;Leone SR;Neumark DM
移除分子核心壳层中的电子会产生瞬时态，这种瞬态的存在时间在几飞秒到阿秒之间。由于这些短寿命，这些状态的时间分辨研究具有挑战性，并且仅由电子相关驱动的复杂分子动力学很难观察到。在这里，我们利用碘在55 eV左右的4d - 16p跃迁的阿秒瞬态吸收，获得了一氯化碘的几飞秒核心激发态寿命。核级配体场分裂允许沿着和垂直于ICl分子轴排列的激发态直接进入。平行于键的核孔态的寿命分别为3.5±0.4 fs和4.3±0.4 fs，垂直于键的核孔态的寿命分别为6.5±0.6 fs和6.9±0.6 fs，而核运动基本上在这个时间尺度上是冻结的。理论表明，与共价键平行的核心空位的寿命急剧下降是ICl与邻近的Cl原子非局域相互作用的表现。本文报道了利用阿秒瞬态吸收光谱测量ICl分子核孔态寿命的研究。他们发现寿命取决于轨道相对于分子轴的排列。
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, we obtain few-femtosecond core-excited state lifetimes of iodine monochloride by using 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 ± 0.4 fs and 4.3 ± 0.4 fs are obtained for core-hole states parallel to the bond and 6.5 ± 0.6 fs and 6.9 ± 0.6 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. Here the authors report a study measuring lifetimes of core-hole states of ICl molecule using attosecond transient absorption spectroscopy. They find that lifetimes depend on the alignment of the orbital relative to the molecular axis.
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影响因子：
2.9
作者：
Bernhardt, Birgitta;Beck, Annelise R.;Leone, Stephen R.
通讯作者：
Leone, Stephen R.
影响因子：
4.4
作者：
LEFEBVREBRION, H;GIUSTISUZOR, A;RASEEV, G
通讯作者：
RASEEV, G
影响因子：
2.9
作者：
NAHON, L;MORIN, P
通讯作者：
MORIN, P
影响因子：
2.3
作者：
Olney, TN;Cooper, G;Brion, CE
通讯作者：
Brion, CE
影响因子：
3.3
作者：
Cao, Wei;Warrick, Erika R.;Leone, Stephen R.
通讯作者：
Leone, Stephen R.