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

对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前AMO物理学的主要挑战之一。最近，我们开发了一种新的第一性原理计算技术，b样条代数图构造（ADC），它对解决这个问题具有很高的希望。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。该方法已成功应用于原子（He， Ne等）和小分子（如CO2），为这些系统中的高次谐波产生（HHG）和阿秒电子空穴动力学提供了有价值的见解，但在应用于感兴趣的多原子分子（如甘氨酸）之前还需要进一步发展。在本博士的研究过程中，我们将探索利用b样条单电子基的修改，如混合b样条/高斯基和多中心b样条基，在b样条ADC内准确有效地描述多中心系统中的多电子动力学。我们将把改进的技术应用于各种空穴迁移的阿秒泵浦探测光谱的全面建模，包括我们小组开发的那些，如单光子激光激活俄歇光谱和相关驱动空穴动力学的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.