Variational calculation of static and dynamic vibrational nonlinear optical properties.
The vibrational configuration interaction method used to obtain static vibrational (hyper)polarizabilities is extended to dynamic nonlinear optical properties in the infinite optical frequency approximation. Illustrative calculations are carried out on H(2)O and NH(3). The former molecule is weakly anharmonic while the latter contains a strongly anharmonic umbrella mode. The effect on vibrational (hyper)polarizabilities due to various truncations of the potential energy and property surfaces involved in the calculation are examined.
Luis
Josep M
JM
Institute of Computational Chemistry, University of Girona, Campus de Montilivi, 17071 Girona, Catalonia, Spain. josepm.luis@udg.edu
Torrent-Sucarrat
Miquel
M
Christiansen
Ove
O
Kirtman
Bernard
B