Holzmeier F, Joseph J, Houver J C, Lebech M, Dowek D, Lucchese R R
Université Paris-Saclay, CNRS, Institut des Sciences Moléculaires d'Orsay, 91405, Orsay, France.
Université Paris-Saclay, Synchrotron SOLEIL, 91190, Saint Aubin, France.
Nat Commun. 2021 Dec 20;12(1):7343. doi: 10.1038/s41467-021-27360-y.
Characterizing time delays in molecular photoionization as a function of the ejected electron emission direction relative to the orientation of the molecule and the light polarization axis provides unprecedented insights into the attosecond dynamics induced by extreme ultraviolet or X-ray one-photon absorption, including the role of electronic correlation and continuum resonant states. Here, we report completely resolved experimental and computational angular dependence of single-photon ionization delays in NO molecules across a shape resonance, relying on synchrotron radiation and time-independent ab initio calculations. The angle-dependent time delay variations of few hundreds of attoseconds, resulting from the interference of the resonant and non-resonant contributions to the dynamics of the ejected electron, are well described using a multichannel Fano model where the time delay of the resonant component is angle-independent. Comparing these results with the same resonance computed in e-NO scattering highlights the connection of photoionization delays with Wigner scattering time delays.
将分子光电离中的时间延迟表征为相对于分子取向和光偏振轴的出射电子发射方向的函数，为极端紫外或X射线单光子吸收所诱导的阿秒动力学提供了前所未有的见解，包括电子关联和连续共振态的作用。在此，我们报告了基于同步辐射和与时间无关的从头算计算，完全解析了NO分子在形状共振过程中单光子电离延迟的实验和计算角度依赖性。由共振和非共振对出射电子动力学贡献的干涉导致的几百阿秒的角度相关时间延迟变化，使用多通道法诺模型得到了很好的描述，其中共振分量的时间延迟与角度无关。将这些结果与在电子-NO散射中计算的相同共振进行比较，突出了光电离延迟与维格纳散射时间延迟之间的联系。
