Implementation of the time-dependent configuration-interaction singles method for atomic strong-field processes

Journal Article · Sun Aug 15 00:00:00 EDT 2010 · Physical Review. A

DOI:https://doi.org/10.1103/PHYSREVA.82.023406· OSTI ID:21448523

Greenman, Loren; Kamarchik, Eugene; Mazziotti, David A ^[1]; Ho, Phay J ^[2]; Pabst, Stefan ^[2]; Santra, Robin ^[2]

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1. Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637 (United States)
2. Argonne National Laboratory, Argonne, Illinois 60439 (United States)

We present an implementation of the time-dependent configuration-interaction singles (TDCIS) method for treating atomic strong-field processes. In order to absorb the photoelectron wave packet when it reaches the end of the spatial grid, we add to the exact nonrelativistic many-electron Hamiltonian a radial complex absorbing potential (CAP). We determine the orbitals for the TDCIS calculation by diagonalizing the sum of the Fock operator and the CAP using a flexible pseudospectral grid for the radial degree of freedom and spherical harmonics for the angular degrees of freedom. The CAP is chosen such that the occupied orbitals in the Hartree-Fock ground state remain unaffected. Within TDCIS, the many-electron wave packet is expanded in terms of the Hartree-Fock ground state and its single excitations. The virtual orbitals satisfy nonstandard orthogonality relations, which must be taken into consideration in the calculation of the dipole and Coulomb matrix elements required for the TDCIS equations of motion. We employ a stable propagation scheme derived by second-order finite differencing of the TDCIS equations of motion in the interaction picture and subsequent transformation to the Schroedinger picture. Using the TDCIS wave packet, we calculate the expectation value of the dipole acceleration and the reduced density matrix of the residual ion. The technique implemented will allow one to study electronic channel-coupling effects in strong-field processes.

• OSTI ID: 21448523
• Journal Information: Physical Review. A, Vol. 82, Issue 2; Other Information: DOI: 10.1103/PhysRevA.82.023406; (c) 2010 The American Physical Society; ISSN 1050-2947
• Country of Publication: United States
• Language: English

Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
74 ATOMIC AND MOLECULAR PHYSICS
CONFIGURATION INTERACTION
DEGREES OF FREEDOM
DENSITY MATRIX
DIPOLES
ELECTRONS
EQUATIONS OF MOTION
EXCITATION
EXPECTATION VALUE
HAMILTONIANS
HARTREE-FOCK METHOD
IONS
MATRIX ELEMENTS
POTENTIALS
SCHROEDINGER PICTURE
SPHERICAL HARMONICS
TIME DEPENDENCE
WAVE PACKETS
APPROXIMATIONS
CALCULATION METHODS
CHARGED PARTICLES
DIFFERENTIAL EQUATIONS
ELEMENTARY PARTICLES
ENERGY-LEVEL TRANSITIONS
EQUATIONS
FERMIONS
FUNCTIONS
LEPTONS
MATHEMATICAL OPERATORS
MATRICES
MULTIPOLES
PARTIAL DIFFERENTIAL EQUATIONS
QUANTUM OPERATORS