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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ultrafast X-ray Photoelectron Imaging of Attosecond Electron Dynamics in Molecular Coherent Excitation
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Ultrafast X-ray Photoelectron Imaging of Attosecond Electron Dynamics in Molecular Coherent Excitation

机译：超快X射线光电子电子成像在分子相干激发中的attosecond电子动力学

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摘要

Ultrafast photoelectron imaging allows to measure information about coherent electron dynamic processes in materials or chemical compounds on femtosecond to attosecond time scales. We show that molecular time-resolved photoelectron diffraction produced by a time-delayed soft X-ray attosecond pulse can be used to monitor the ultrafast coherent excitation induced by a resonant UV pump pulse with variable carrier-envelope phases. Asymmetric diffraction angular patterns illustrate coherent electron dynamics of charge migration with spatiotemporal resolution on the attosecond and angstrom scale. This allows the temporal reconstruction of phases and amplitudes of electronic states and geometry of molecules as a function of time delay of the probe pulse and carrier-envelope phases of the pump pulse. Results are obtained from solutions of time-dependent Schrodinger equations of the hydrogen molecular ion, and analyzed by ultrafast photoelectron diffraction models for coherent superposition of electronic states. The present demonstration provides a guiding principle for monitoring ultrafast spatiotemporal coherent electron dynamics and imaging molecular electronic structure in complex systems by ultrafast pump-probe experiments and their dependence on carrier-envelope phases and time delays.
机译：UltraFast光电子成像允许测量关于在飞秒上的材料或化学化合物中的相干电子动力过程的信息，以抵押时间尺度。我们表明，通过延迟软X射线抗脉冲产生的分子时间分辨光电子衍射可用于监测具有可变载体包络相位的谐振UV泵脉冲引起的超快相干激发。不对称衍射角度图案示出了在attosecond和埃尺度上具有时空分辨率的电荷迁移的相干电子动力学。这允许作为泵脉冲的探针脉冲和载体包络相的时间延迟的函数和分子的几何形状的阶段重建和分子的几何形状。结果是从氢分子离子的时间依赖性Schrodinger方程的溶液中获得，并通过超氮育光电子衍射模型进行分析，用于电子状态的相干叠加。本示威提供了通过超薄泵探针实验及其对载体包络阶段和时间延迟的复杂系统中超快时空相干电子动力学和成像分子电子结构的指导原理。

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