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

Abstract

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 Schr\odinger 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.