High Harmonic Generation from Multiple Orbitals in N2
High Harmonic Generation from Multiple Orbitals in N2
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DOI：
10.1126/science.1162780
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发表时间：
2008-11-21
期刊：
影响因子：
56.9
通讯作者：
Guhr, Markus
中科院分区：
文献类型：
--
作者：
McFarland, Brian K.;Farrell, Joseph P.;Guhr, Markus
分子电子态的能量低于最高占据分子轨道（HOMO）应该有助于激光驱动的高次谐波产生（HHG），但以前没有观察到这种行为。我们对垂直于激光偏振排列的 N-2 分子的 HHG 光谱的测量显示，在旋转半复兴处有最大值。该特征表明占据 N-2 HOMO（称为 HOMO-1）正下方轨道的电子的影响。对较低轨道的这种观察对于理解激光激发分子中的亚飞秒/亚埃电子运动至关重要。
Molecular electronic states energetically below the highest occupied molecular orbital ( HOMO) should contribute to laser- driven high harmonic generation (HHG), but this behavior has not been observed previously. Our measurements of the HHG spectrum of N-2 molecules aligned perpendicular to the laser polarization showed a maximum at the rotational half- revival. This feature indicates the influence of electrons occupying the orbital just below the N-2 HOMO, referred to as the HOMO-1. Such observations of lower- lying orbitals are essential to understanding subfemtosecond/subangstrom electronic motion in laser- excited molecules.