Jiang Wenyu, Armstrong Gregory S J, Tong Jihong, Xu Yidan, Zuo Zitan, Qiang Junjie, Lu Peifen, Clarke Daniel D A, Benda Jakub, Fleischer Avner, Ni Hongcheng, Ueda Kiyoshi, van der Hart Hugo W, Brown Andrew C, Gong Xiaochun, Wu Jian
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai, China.
Centre for Theoretical Atomic, Molecular and Optical Physics, School of Mathematics and Physics, Queen's University Belfast, University Road, Belfast, BT7 1NN, Northern Ireland, UK.
Nat Commun. 2022 Aug 29;13(1):5072. doi: 10.1038/s41467-022-32753-8.
Attosecond chronoscopy is central to the understanding of ultrafast electron dynamics in matter from gas to the condensed phase with attosecond temporal resolution. It has, however, not yet been possible to determine the timing of individual partial waves, and steering their contribution has been a substantial challenge. Here, we develop a polarization-skewed attosecond chronoscopy serving as a partial wave meter to reveal the role of each partial wave from the angle-resolved photoionization phase shifts in rare gas atoms. We steer the relative ratio between different partial waves and realize a magnetic-sublevel-resolved atomic phase shift measurement. Our experimental observations are well supported by time-dependent R-matrix numerical simulations and analytical soft-photon approximation analysis. The symmetry-resolved, partial-wave analysis identifies the transition rate and phase shift property in the attosecond photoelectron emission dynamics. Our findings provide critical insights into the ubiquitous attosecond optical timer and the underlying attosecond photoionization dynamics.
阿秒时间分辨技术对于理解从气体到凝聚相物质中具有阿秒时间分辨率的超快电子动力学至关重要。然而，目前尚无法确定各个分波的时间，并且控制它们的贡献一直是一项重大挑战。在此，我们开发了一种偏振倾斜的阿秒时间分辨技术，作为一种分波计，以从稀有气体原子的角分辨光电离相移中揭示每个分波的作用。我们控制不同分波之间的相对比例，并实现了磁子能级分辨的原子相移测量。我们的实验观测结果得到了含时R矩阵数值模拟和解析软光子近似分析的有力支持。这种对称分辨的分波分析确定了阿秒光电子发射动力学中的跃迁速率和相移特性。我们的研究结果为普遍存在的阿秒光学定时器以及潜在的阿秒光电离动力学提供了关键见解。
