Ab initio molecular orbitalconfiguration interaction based quantum master equation (MOQME) approach to the dynamic first hyperpolarizabilities of asymmetric πconjugated systems
Abstract
In this study, we apply the ab initio molecular orbital  configuration interaction based quantum master equation (MOQME) approach to the calculation and analysis of the dynamic first hyperpolarizabilities (β) of asymmetric πconjugated molecules. In this approach, we construct the excited state models by the ab initio configuration interaction singles method. Then, time evolutions of system reduced density matrix ρ(t) and system polarization p(t) are calculated by the QME approach. Dynamic β in the second harmonic generation is calculated based on the nonperturbative definition of nonlinear optical susceptibility, using the frequency domain system polarization p(ω). Spatial contributions of electrons to β are analyzed based on the dynamic hyperpolarizability density map, which visualizes the secondorder response of charge density oscillating with a frequency of 2ω. We apply the present method to the calculation of the dynamic β of a series of donor/acceptor substituted polyene oligomers, and then discuss the applicability of the MOQME method to the calculation and analysis of dynamic NLO properties of molecular systems.
 Authors:
 Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 5608531 (Japan)
 Publication Date:
 OSTI Identifier:
 22390932
 Resource Type:
 Journal Article
 Resource Relation:
 Journal Name: AIP Conference Proceedings; Journal Volume: 1642; Journal Issue: 1; Conference: ICCMSE2010: International Conference of Computational Methods in Sciences and Engineering 2010, Kos (Greece), 38 Oct 2010; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; ASYMMETRY; CHARGE DENSITY; CONFIGURATION INTERACTION; DENSITY MATRIX; ELECTRONS; EXCITED STATES; HARMONIC GENERATION; MOLECULAR ORBITAL METHOD; NONLINEAR PROBLEMS; POLARIZATION; QUANTUM MECHANICS
Citation Formats
Kishi, Ryohei, Fujii, Hiroaki, Minami, Takuya, Shigeta, Yasuteru, and Nakano, Masayoshi. Ab initio molecular orbitalconfiguration interaction based quantum master equation (MOQME) approach to the dynamic first hyperpolarizabilities of asymmetric πconjugated systems. United States: N. p., 2015.
Web. doi:10.1063/1.4906735.
Kishi, Ryohei, Fujii, Hiroaki, Minami, Takuya, Shigeta, Yasuteru, & Nakano, Masayoshi. Ab initio molecular orbitalconfiguration interaction based quantum master equation (MOQME) approach to the dynamic first hyperpolarizabilities of asymmetric πconjugated systems. United States. doi:10.1063/1.4906735.
Kishi, Ryohei, Fujii, Hiroaki, Minami, Takuya, Shigeta, Yasuteru, and Nakano, Masayoshi. 2015.
"Ab initio molecular orbitalconfiguration interaction based quantum master equation (MOQME) approach to the dynamic first hyperpolarizabilities of asymmetric πconjugated systems". United States.
doi:10.1063/1.4906735.
@article{osti_22390932,
title = {Ab initio molecular orbitalconfiguration interaction based quantum master equation (MOQME) approach to the dynamic first hyperpolarizabilities of asymmetric πconjugated systems},
author = {Kishi, Ryohei and Fujii, Hiroaki and Minami, Takuya and Shigeta, Yasuteru and Nakano, Masayoshi},
abstractNote = {In this study, we apply the ab initio molecular orbital  configuration interaction based quantum master equation (MOQME) approach to the calculation and analysis of the dynamic first hyperpolarizabilities (β) of asymmetric πconjugated molecules. In this approach, we construct the excited state models by the ab initio configuration interaction singles method. Then, time evolutions of system reduced density matrix ρ(t) and system polarization p(t) are calculated by the QME approach. Dynamic β in the second harmonic generation is calculated based on the nonperturbative definition of nonlinear optical susceptibility, using the frequency domain system polarization p(ω). Spatial contributions of electrons to β are analyzed based on the dynamic hyperpolarizability density map, which visualizes the secondorder response of charge density oscillating with a frequency of 2ω. We apply the present method to the calculation of the dynamic β of a series of donor/acceptor substituted polyene oligomers, and then discuss the applicability of the MOQME method to the calculation and analysis of dynamic NLO properties of molecular systems.},
doi = {10.1063/1.4906735},
journal = {AIP Conference Proceedings},
number = 1,
volume = 1642,
place = {United States},
year = 2015,
month = 1
}

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