Theory of Atomic, Molecular, and Optical Processes

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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.