Theory of Atomic, Molecular, and Optical Processes

University Of Kansas Center For Research Inc, Lawrence KS

Investigators

Abstract

This proposal addresses comprehensive theoretical investigation of a broad range of atomic, molecular, and optical (AMO) processes of current significance in science and technology. The proposed activities will build on both of our past efforts and the new development of nonperturbative theoretical formalisms and high-precision computational methods for accurate treatment of both the electronic structure of highly and multiply excited states as well as the multiphoton dynamics and coherent control of atomic and molecular processes in the presence of intense external fields. Emphasis in the first part of this proposal concerns the ab initio theoretical exploration of the frequency comb structure and coherence within each order of the high-order harmonic generation (HHG) spectrum in the high-frequency VUV/XUV regime. Two approaches will be developed for the study of frequency comb projects: (a) time-dependent generalized pseudospectral method (TDGPS) for accurate and efficient solution 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 the study of the coherent control of population transfer in Rydberg atoms via sequential transitions 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 new TDGPS method in hyperspherical coordinates for fully ab initio 6D treatment of doubly excited resonance states and double photoionization dynamics of two-electron atoms in the presence of external fields, and (b) the further development of the self-interaction-free time-dependent density functional theory (TDDFT) for the exploration of many-electron Rydberg atom dynamics.