Many-electron dynamics in molecules by B-spline algebraic diagrammatic construction method

阿秒或少飞秒激光脉冲诱导的多电子动力学的理论描述是当今AMO物理学的关键挑战之一。最近，我们发展了一种新的第一性原理计算技术，B-样条代数图构造(ADC)，它有望解决这个问题。该方法基于电子-电子相互作用的多体格林函数方法和有效的B样条单电子基函数。该方法已成功地应用于He、Ne等原子的测量。和小分子(如二氧化碳)，提供了有价值的洞察动力学的高次谐波产生(HHG)和阿秒电子空穴动力学在这些系统中，但需要进一步发展，才能应用于感兴趣的多原子分子，如甘氨酸。在目前的PHD研究过程中，我们将探索使用B-样条单电子基的改进，如混合B-样条基/高斯基和多中心B-样条基，在B-Spline ADC内准确和有效地描述多中心体系中的多电子动力学。我们将把改进的技术应用于各种阿秒抽运-探测空穴迁移光谱的完全模拟，包括我们团队开发的那些，例如单光子激光使能俄歇光谱和关联驱动空穴动力学的HHG光谱。

Theoretical description of many-electron dynamics induced by attosecond or few-femtosecond laser pulses is one of the key challenges of the present-day AMO physics. Recently, we have developed a new first-principles computational technique that holds high promise for solving this problem, B-spline algebraic diagrammatic construction (ADC). This method is based on the many-body Green's function approach to electron-electron interaction and the efficient B-spline single-electron basis. The method has been applied successfully to atoms (He, Ne, etc.) and small molecules (e.g. CO2), providing valuable insight into dynamics of high-order harmonic generation (HHG) and attosecond electron hole dynamics in these systems, but needs further development before it can be applied to the polyatomic molecules of interest, such as glycine. In the course of the present PhD research, we will explore using modifications of the B-spline single-electron basis, such as hybrid B-spline/Gaussian basis and multi-centre B-spline basis for accurate and efficient description of many-electron dynamics in multi-centre systems within the B-spline ADC. We will apply the modified technique to full modelling of a variety of attosecond pump-probe spectroscopies of hole migration, including the ones developed by our group, such as single-photon laser-enable Auger spectroscopy and HHG spectroscopy of correlation-driven hole dynamics.