Full Ab Initio Many-Electron Simulation of Attosecond Molecular Pump–Probe Spectroscopy,Journal of Chemical Theory and Computation

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Full Ab Initio Many-Electron Simulation of Attosecond Molecular Pump–Probe Spectroscopy
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2018-09-04 00:00:00 , DOI: 10.1021/acs.jctc.8b00479
M. Ruberti ₁ , P. Decleva ₂ , V. Averbukh ₁

Affiliation

Here, we present an ab initio approach to full simulation of an attosecond molecular pump–probe experiment. Sequential molecular double ionization by the pump and probe laser pulses with controlled delay is described from first-principles with a full account of the continuum dynamics of the photoelectrons. Many-electron bound-continuum dynamics is simulated using the time-dependent (TD) molecular B-spline algebraic diagrammatic construction (ADC) method. Our calculations give a quantitative prediction about the creation of a coherent superposition of molecular ionic states in the photoionization process and simulate the probe of the ensuing attosecond dynamics by a second ionizing pulse within a single first-principles many-electron framework. We therefore demonstrate the capability to simulate and interpret the results of a prototypical molecular pump–probe experiment of interest in attoscience. As a particular example, we simulate and elucidate the interpretation of a pump–probe experiment in CO₂ aimed at measuring strong field-induced hole dynamics via photoionization yields.

中文翻译：

阿秒分子泵浦-探针光谱的全从头算多电子模拟

在这里，我们提出了一个从头开始的方法来全面模拟一个阿秒分子泵浦-探针实验。从第一性原理出发，充分考虑了光电子的连续动力学，描述了由泵浦和探测激光脉冲以受控延迟进行的连续分子双电离。使用时间依赖（TD）分子B样条代数图解构造（ADC）方法模拟多电子束缚连续谱动力学。我们的计算给出了有关在光电离过程中分子离子态的相干叠加的定量预测，并通过单个第一原理多电子框架内的第二个电离脉冲来模拟随后的阿秒动力学的探测。因此，我们证明了模拟和解释原子科学感兴趣的原型分子泵-探针实验结果的能力。作为一个特定的示例，我们模拟并阐明了CO中泵浦探针实验的解释_图2旨在通过光电离产量来测量强磁场诱导的空穴动力学。

更新日期：2018-09-04

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