Time-Dependent Quantum Chemistry and Time-Resolved Electron Dynamics

瞬态量子化学和时间分辨电子动力学

• 批准号: RGPIN-2015-05369
• 负责人: NguyenDang, ThanhTung
• 金额: $ 2.04万
• 依托单位: Université Laval
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2019
• 资助国家: 加拿大
• 起止时间: 2019-01-01 至 2020-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=682906
• 关键词: Time; Dependent; Quantum; Chemistry; Resolved

The general objective of the present research program is to further the development of ab-initio time-dependent Quantum Chemistry through the completion of MEDYS (Many-Electron DYnamicS), a set of codes for the direct computation of time-dependent many-electron wavefunctions including electron correlation effects, and capable of treating large amplitude electronic motions (strong-field-driven ionization and electron recollision). Using the developed methodology, fundamental problems in intense-field attosecond photophysics/chemistry will be addressed. These include in particular: The role of electron correlation in strong-field ionizations, its interplay with field-induced many-electron state mixing, and symmetry conservation principles in laser-driven time-dependent electron dynamics. These studies will directly find applications in problems dealing with the quantum dynamic imaging of molecules. We will explore the possibility of developing a molecular orbital tomography scheme based on Laser-Induced Electron Diffraction (LIED) and Ultrafast Photoelectron Holography. We will further studies on ultrafast pump-probe spectroscopy of laser-induced transition states of a molecule dissociating under the influence of an intense Infra-red (IR) laser pulse. **

本研究计划的总体目标是通过完成MEDYS（多电子动力学）来进一步发展从头算含时量子化学，MEDYS是一套直接计算含时多电子波函数的代码，包括电子相关效应，并能够处理大幅度电子运动（强场驱动电离和电子电离）。使用开发的方法，将解决强场阿秒光物理/化学中的基本问题。其中特别包括：电子关联在强场电离中的作用，它与场诱导多电子态混合的相互作用，以及激光驱动含时电子动力学中的对称性守恒原理。这些研究将直接应用于处理分子的量子动力学成像问题。我们将探讨基于激光诱导电子衍射（LIED）和超快光电子全息术发展分子轨道层析成像方案的可能性。我们将进一步研究在强红外激光脉冲作用下分子离解的激光诱导过渡态的超快泵浦-探测光谱。**