title: Development of calculation and analysis methods for the dynamic first hyperpolarizability based on the ab initio molecular orbital-quantum master equation method.
abstract: We develop novel calculation and analysis methods for the dynamic first hyperpolarizabilities β [the second-order nonlinear optical (NLO) properties at the molecular level] in the second-harmonic generation based on the quantum master equation method combined with the ab initio molecular orbital (MO) configuration interaction method. As examples, we have evaluated off-resonant dynamic β values of donor (NH(2))- and/or acceptor (NO(2))-substituted benzenes using these methods, which are shown to reproduce those by the conventional summation-over-states method well. The spatial contributions of electrons to the dynamic β of these systems are also analyzed using the dynamic β density and its partition into the MO contributions. The present results demonstrate the advantage of these methods in unraveling the mechanism of dynamic NLO properties and in building the structure-dynamic NLO property relationships of real molecules.
authors.affiliation: Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan. rkishi@cheng.es.osaka-u.ac.jp
authors.forename: Ryohei
authors.initials: R
authors.lastname: Kishi
authors.forename: Hiroaki
authors.initials: H
authors.lastname: Fujii
authors.forename: Shingo
authors.initials: S
authors.lastname: Kishimoto
authors.forename: Yusuke
authors.initials: Y
authors.lastname: Murata
authors.forename: Soichi
authors.initials: S
authors.lastname: Ito
authors.forename: Katsuki
authors.initials: K
authors.lastname: Okuno
authors.forename: Yasuteru
authors.initials: Y
authors.lastname: Shigeta
authors.forename: Masayoshi
authors.initials: M
authors.lastname: Nakano