Details

Autor(en) / Beteiligte

• Krause, Pascal
• Klamroth, Tillmann
• Saalfrank, Peter

Titel

Molecular response properties from explicitly time-dependent configuration interaction methods

Ist Teil von

• The Journal of chemical physics, 2007-07, Vol.127 (3), p.034107-034107-10

Ort / Verlag

United States: American Institute of Physics

Erscheinungsjahr

2007

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• 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 Schrödinger equation) to time-dependent perturbations of arbitrary shape and strength. Three variants are used to solve the time-dependent electronic Schrödinger 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.