Theory of Atomic, Molecular, and Optical Processes

该提案涉及对科学技术中具有当前重要意义的广泛的原子、分子和光学（AMO）过程进行全面的理论研究。拟议的活动将建立在我们过去的努力和非微扰理论形式主义和高-精确计算方法，用于精确处理高激发态和多激发态的电子结构，以及强外场存在下原子和分子过程的多光子动力学和相干控制。探讨了高频真空紫外/极紫外波段高次谐波产生（HHG）谱的频率梳结构和各阶相干性。将为研究频率梳项目开发两种方法：（a）时间相关广义伪谱法，用于精确和有效地求解空间和时间相关薛定谔方程;（B）多模式Floquet理论。第二部分是研究里德伯原子中通过顺序跃迁或多光子绝热快速通过的布居转移的相干控制。在最后一部分，我们将介绍几个更长范围的计划，包括：（a）发展一种新的超球坐标下的TDGPS方法，用于外场存在下双电子原子双激发共振态和双光电离动力学的从头算6D处理;（B）无自相互作用含时密度泛函理论（TDDFT）在多电子里德堡原子动力学研究中的进一步发展。

This proposal addresses comprehensive theoretical investigation of a broad range ofatomic, molecular, and optical (AMO) processes of current significance in science andtechnology. The proposed activities will build on both of our past efforts and the newdevelopment of nonperturbative theoretical formalisms and high-precisioncomputational methods for accurate treatment of both the electronic structure of highlyand multiply excited states as well as the multiphoton dynamics and coherent control ofatomic and molecular processes in the presence of intense external fields.Emphasis in the first part of this proposal concerns the ab initio theoretical exploration ofthe frequency comb structure and coherence within each order of the high-orderharmonic generation (HHG) spectrum in the high-frequency VUV/XUV regime. Twoapproaches will be developed for the study of frequency comb projects: (a)time-dependent generalized pseudospectral method (TDGPS) for accurate and efficientsolution of the time-dependent Schrdinger equation (TDSE) in space and time, and (b)many-mode Floquet theory (MMFT). The second part of this proposal will deal with thestudy of the coherent control of population transfer in Rydberg atoms via sequentialtransitions or via multiphoton adiabatic rapid passage. In the last part of the proposal,several longer range projects will be presented, including (a) the development of a newTDGPS method in hyperspherical coordinates for fully ab initio 6D treatment of doublyexcited resonance states and double photoionization dynamics of two-electron atoms inthe presence of external fields, and (b) the further development of theself-interaction-free time-dependent density functional theory (TDDFT) for theexploration of many-electron Rydberg atom dynamics.