Cálculos de (hiper)polarizabilidades dinâmicas das moléculas de ozônio, dióxido de enxofre, óxido nitroso e dióxido de carbono incluindo correções vibracionais e efeitos de correlação eletrônica
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2013-11-08
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Universidade Federal de Goiás
Resumo
This work presents results for the dynamic (hyper)polarizabilities of ozone, sulfur dioxide, nitrous
oxide and carbon dioxide molecules, with inclusion of vibrational corrections. The electronic contributions
for the properties of interest were computed analytically at the single and double coupled
cluster level through response theory. Ozone and sulfur dioxide were studied separately. For both
systems, contributions of connected triple excitations were also estimated by the multiplicative correction
scheme. The vibrational corrections were calculated by the perturbation theoretical method
(PT). The zero-point vibrational average correction, calculated only for ozone and sulfur dioxide,
proved to be small. Results also show that the pure vibrational correction is relevant for the following
nonlinear optical processes: dc-Pockels effect, intensity dependent refractive index, and dc-Kerr
effect. For the ozone molecule the dc-second harmonic generation effect also had a significant pure
vibrational correction. In addition, pure vibrational correction was calculated according to a variational
methodology proposed by our research group (VAR) for the four systems, and the results were
compared with the corresponding PT results. A comparison between PT and VAR results shows that
ozone is the system most sensitive to the method, while sulfur dioxide and carbon dioxide are the
most well behaved.
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NAVES, Emílio Santiago. Cálculos de (hiper)polarizabilidades dinâmicas das moléculas de ozônio, dióxido de enxofre, óxido nitroso e dióxido de carbono incluindo correções vibracionais e efeitos de correlação eletrônica, 2013. 109 f. Tese (Doutorado em Física) - Universidade Federal de Goiás, Goiânia, 2013.