Deformation of an inner valence molecular orbital in ethanol by an intense laser field
Deformation of an inner valence molecular orbital in ethanol by an intense laser field
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DOI：
10.1126/sciadv.aaw1885
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发表时间：
2019-05-01
期刊：
影响因子：
13.6
通讯作者：
Itakura, Ryuji
中科院分区：
文献类型：
--
作者：
Akagi, Hiroshi;Otobe, Tomohito;Itakura, Ryuji
价态分子轨道在化学反应中起着至关重要的作用。在这里，我们揭示了强激光场使乙醇分子的内价轨道（10a '）变形。我们测量反冲帧光电子角分布（RFPAD），这对应于轨道的电离概率的取向依赖性，使用光电子-光离子符合动量成像与圆偏振激光脉冲。从头算模拟表明，轨道的变形强烈依赖于激光场的方向和测量RFPAD不能复制不考虑轨道变形。我们的研究结果表明，在亚光周期时间尺度上，激光诱导的轨道变形发生在电子发射之前。
Valence molecular orbitals play a crucial role in chemical reactions. Here, we reveal that an intense laser field deforms an inner valence orbital (10a') in the ethanol molecule. We measure the recoil-frame photoelectron angular distribution (RFPAD), which corresponds to the orientation dependence of the ionization probability of the orbital, using photoelectron-photoion coincidence momentum imaging with a circularly polarized laser pulse. Ab initio simulations show that the orbital deformation depends strongly on the laser field direction and that the measured RFPAD cannot be reproduced without taking the orbital deformation into account. Our findings suggest that the laser-induced orbital deformation occurs before electron emission on a suboptical cycle time scale.