Molecular response properties from explicitly time-dependent configuration interaction methods.
In this paper we report the calculation of molecular electric response properties with the help of explicitly time-dependent configuration interaction (TD-CI) methods. These methods have the advantage of being applicable (within the limitations of the time-dependent Schrodinger equation) to time-dependent perturbations of arbitrary shape and strength. Three variants are used to solve the time-dependent electronic Schrodinger equation, namely, the TD-CIS (inclusion of single excitations only), TD-CISD (inclusion of single and double excitations), and TD-CIS(D) (single excitations and perturbative treatment of double excitations) methods and applied for illustration to small molecules, H(2) and H(2)O. In the calculation, slowly varying off-resonant electric fields are applied to the molecules and linear (polarizabilities) and nonlinear (hyperpolarizabilities, harmonic generation) response properties are determined from the time-dependent dipole moments.
Krause
Pascal
P
Theoretische Chemie, Institut für Chemie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, D-14476 Potsdam, Germany.
Klamroth
Tillmann
T
Saalfrank
Peter
P