Configuration-interaction-based time-dependent orbital approach for ab initio treatment of electronic dynamics in a strong optical laser field
- Argonne National Laboratory, Argonne, Illinois 60439 (United States)
- Department of Electrical Engineering and Computer Science and Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)
The time-dependent configuration interaction singles (TDCIS) method - an ab initio electronic-structure technique with predictive character - is reformulated in terms of an effective one-electron theory with coupled channels. In this form, the TDCIS equations of motion may be evaluated using standard wave-packet propagation techniques in real space. The time-dependent orbital formulation of TDCIS has computational and conceptual advantages for studying strong-field phenomena in many-electron systems. A simplified version of this theory, referred to as the determinantal single-active-electron (d-SAE) method, is derived. TDCIS and d-SAE are tested by their application to a one-dimensional two-electron model in a strong laser field. The numerically exact time-dependent dipole moment of the interacting system is found to be very well reproduced with TDCIS. The d-SAE method is less accurate, but still provides superior performance in comparison to the standard single-active-electron approach.
- OSTI ID:
- 20863940
- Journal Information:
- Physical Review. A, Vol. 74, Issue 4; Other Information: DOI: 10.1103/PhysRevA.74.043420; (c) 2006 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA); ISSN 1050-2947
- Country of Publication:
- United States
- Language:
- English
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