Electron dynamics in water are of fundamental importance for a broad range of phenomena, but their real-time study faces numerous conceptual and methodological challenges. Here, we introduce attosecond size-resolved cluster spectroscopy and build up a molecular-level understanding of the attosecond electron dynamics in water. We measure the effect that the addition of single water molecules has on the photoionization time delays of water clusters. We find a continuous increase of the delay for clusters containing up to 4-5 molecules and little change towards larger clusters. We show that these delays are proportional to the spatial extension of the created electron hole, which first increases with cluster size and then partially localizes through the onset of structural disorder that is characteristic of large clusters and bulk liquid water. These results establish a previously unknown sensitivity of photoionization delays to electron-hole delocalization and reveal a direct link between electronic structure and attosecond photoemission dynamics. Our results offer novel perspectives for studying electron/hole delocalization and its attosecond dynamics.
Probing of Core Excitons in Solid NaF with Polarization-Selective Attosecond Time-Resolved Four-Wave Mixing Spectroscopy
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；University of Regensburg（雷根斯堡大学）；Lund University（隆德大学）
Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule
Shanghai Jiao Tong University（上海交通大学）；RIKEN Center for Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所交叉理论数学科学中心（iTHEMS））；RIKEN Center for Computational Science (R-CCS)（理化学研究所计算科学中心（R-CCS））；The University of Tokyo（东京大学）
Exceptionally strong correlation-driven charge migration and attosecond transient absorption spectroscopy
我们从理论上研究了多原子分子（C $_2$ H $_4$ BrI）迅速双电离后的电荷迁移，发现对于双电离，相关驱动的电荷迁移似乎特别突出，即，我们观察到特别丰富的动力学仅由电子-电子相互作用驱动，即使在电子从外价轨道发射的情况下。这些强关联电子动力学在理论上确定的时间分辨瞬态吸收截面见证。引人注目的是，在截面的功能可以追溯到电子空穴人口和时间依赖的部分电荷，因此，可以解释与令人惊讶的容易。值得注意的是，通过利用元素特定的核心到价跃迁，可以在时间和空间上跟踪空穴布居动态。有了这个，我们不仅报告了相关性驱动的电荷迁移的高度相关性，但我们的研究结果也突出了阿秒瞬态吸收光谱（ATAS）作为监测超快电子动力学在复杂的分子系统中最有前途的技术之一的突出作用。
Exploring the attosecond laser-driven electron dynamics in the hydrogen molecule with different real-time time-dependent configuration interaction approaches
