Theoretical study on nonlinear and quantum optical phenomena of dendritic systems interacting with quantum laser field

树突系统与量子激光场相互作用的非线性和量子光学现象的理论研究

• 批准号: 14340184
• 负责人: NAKANO Masayoshi
• 金额: $ 10.3万
• 依托单位: Osaka University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2002
• 资助国家: 日本
• 起止时间: 2002 至 2005
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-14340184/
• 关键词: quantum field; dendrimer; nonlinear optics; exciton; relaxtion; energy migration; coherency; dissipation; マスター方程式; ナノスター; モンテカルロ波動関数法; モンテカルロ波動関数; スクイズド光; コヒーレント; エキシトンダイナミクス; エキシトン-フォノンカップリング; スクイーズド

Various physical and chemical phenomena for the interaction between supramolecular systems including dendritic systems and laser fields have been investigated theoretically and computationaly. The achievements are described as follows.1.We have developed a general calculation method treating multi-state model interacting with various quantum fields and investigated the effects of multi-photon process, which is one of nonlinear optical effects, on such dynamics. In particular, we have developed a novel method treating relaxation effects caused by molecular vibration and collision on the dynamics using a quantum master equation approach. For a dimer model system interacting with a two-mode quantum field, the collapse-revival phenomena of excited state population for dimer systems are found to be remarkably affected in oscillation amplitude and revival time by the intermolecular dipole-dipole interaction. The pure-phase and population relaxations of dimer systems are turned out to destroy … More the coherency between dimer electronic states, leading to the significant attenuation of molecular nonlinear optical effects. Several additional effects, i.e., exciton relaxation rates and quantum statistics of external quantum fields, on the dynamics and nonlinear optical phenomena of dendritic systems are now being investigated.2.We have studied light harvesting and dynamic nonlinear optical phenomena of supramolecular systems including dendritic systems in order to elucidate the structure-property relationship. A novel calculation method of dynamic nonlinear optical properties of one-exciton molecular aggregate model systems have been developed and applied to the calculation of nonlinear optical spectra of nanostar dendritic aggregate systems with various exciton migration rates. The pure-dephasing caused by the exciton migration originating in the exciton-phonon coupling has been turned out to significantly increase the spectrum width and decrease the peak. In order to treat real supermolecular systems, e.g., dendrimers, we have developed a quantum master equation method based on the ab initio molecular orbital configuration interaction (CI) and have clarified that the efficient directed energy migration originates in the partial penetration of πconjugation through meta-substituted benzene ring. We have also started to examine the open-shell molecules as a unit (building block) of supramolecular systems, and have theoretically found that the nonlinear optical effects significantly depend on the spin state and diradical character. This attractive result is expected to be a novel class of systems in the field of nonlinear optical materials. Less

从理论上和计算上研究了包括树枝状系统在内的超分子系统与激光场之间相互作用的各种物理和化学现象，取得的成果如下： 1.我们发展了一种处理与各种量子场相互作用的多态模型的通用计算方法。并研究了多光子过程（非线性光学效应之一）对这种动力学的影响，特别是，我们开发了一种利用量子主方程方法处理分子振动和碰撞对动力学造成的弛豫效应的新方法。对于相互作用的二聚体模型系统在双模量子场中，发现二聚体系统的激发态布居的塌缩-复活现象在振荡幅度和复活时间上受到分子间偶极子-偶极子相互作用的特别影响。二聚体系统的纯相和布居弛豫。结果破坏了二聚体电子态之间的相干性，导致分子非线性光学效应的显着衰减，即激子弛豫率和外部量子场的量子统计。树枝状系统的动力学和非线性光学现象正在研究中。2.我们研究了包括树枝状系统在内的超分子系统的光收集和动态非线性光学现象，以阐明动态非线性光学性质的结构-性质关系。开发了一种单激子分子聚集体模型系统，并将其应用于计算具有不同激子迁移速率的纳米星树枝状聚集体系统的非线性光谱。激子-声子耦合产生的激子迁移已被证明可以显着增加谱宽并降低峰值。为了处理真实的超分子系统，例如树枝状聚合物，我们开发了一种基于从头算的量子主方程方法。分子轨道构型相互作用（CI）并阐明了有效的定向能量迁移源于π共轭通过间位取代苯环的部分渗透。开壳层分子作为超分子系统的单元（构建块），并在理论上发现非线性光学效应显着依赖于自旋态和双自由基特征，这一引人注目的结果有望成为超分子系统领域的一类新型系统。非线性光学材料。

项目成果

Quantum Master Equation Approach to the Second Hyperpolarizability of Nanostar Dendritic Systems

纳米星树突系统第二次超极化的量子主方程方法

• 发表时间: 2005
• 期刊: J.Phys.Chem.B 109
• 作者: M.Nakano;B.Champagne;M.Nakano;M.Nakano
• 通讯作者: M.Nakano

Theoretical study on on the Second Hyperpolarizability(γ) of a Homogeneous Molecule in the Bond Dissociation Process : Enhancement of γ in the intermediate Correlation

均质分子键解离过程中第二超极化率(γ)的理论研究：中间相关性中γ的增强

• 发表时间: 2004
• 期刊: Journal of Nonlinear Optical Physics and Materials 13
• 作者: M.Nakano;B.Champagne;M.Nakano;M.Nakano;B.Champagne;M.Takahata;R.Kishi;M.Nakano;M.Nakano;M.Nakano;R.Kishi;M.Nakagawa;S.Yamada;M.Takahata;M.Nakano;S.Ohta;Benoit Champagne;Masayoshi Nakano;Benoit Champagne;M.Takahata;Ryohei Kishi;Masayoshi Nakano;Masayoshi Nakano;Ryohei Kishi;Nozomi Nakagawa;Satoru Yamada;Masayoshi Nakano;Suguru Ohta;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;Satoru Yamada;Kizashi Yamaguchi;Masayoshi Nakano;Ryoichi Kishi;Satoru Yamada;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;S.Yamada;K.Yamaguchi;M.Nakano;R.Kishi;M.Nakano;M.Nakano;M.Nakano;M.Nakano;Masayoshi Nakano;Satoru Yamada;Kizashi Yamaguchi;Masayoshi Nakano;Ryohei Kishi;Masayoshi Nakano;Masayoshi Nakano
• 通讯作者: Masayoshi Nakano

Basis set and electron correlation effects on the polarizability and second hyperpolarizability of model open-shell p-conjugated systems

基组和电子关联对开壳层 p 共轭体系模型极化率和二次超极化率的影响

• 期刊: J.Chem.Phys. (in press)
• 作者: M.Nakano;B.Champagne;M.Nakano;M.Nakano;B.Champagne;M.Takahata;R.Kishi;M.Nakano;M.Nakano;M.Nakano;R.Kishi;M.Nakagawa;S.Yamada;M.Takahata;M.Nakano;S.Ohta;Benoit Champagne;Masayoshi Nakano;Benoit Champagne;M.Takahata;Ryohei Kishi;Masayoshi Nakano;Masayoshi Nakano;Ryohei Kishi;Nozomi Nakagawa;Satoru Yamada;Masayoshi Nakano;Suguru Ohta;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;Satoru Yamada;Kizashi Yamaguchi;Masayoshi Nakano;Ryoichi Kishi;Satoru Yamada;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;S.Yamada;K.Yamaguchi;M.Nakano;R.Kishi;M.Nakano;M.Nakano;M.Nakano;M.Nakano;Masayoshi Nakano;Satoru Yamada;Kizashi Yamaguchi;Masayoshi Nakano;Ryohei Kishi;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;H.Fujita;M.Takahata;M.Nakano;M.Nakano;M.Takahata;M.Nakano;M.Takahata;M.Takahata;M.Nakano;S.Yamada;M.Nakano;M.Nakano;M.Nakano;M.Nakano;M.Takahata;M.Nakano;M.Takahata;M.Nakano;M.Nakano;M.Nakano;H.Fujita;M.Nakano;M.Takahata;M.Nakano;M.Takahata;M.Nakano;S.Yamada;M.Nakano;M.Nakano;H.Fujita;M.Nakano;M.Takahata;M.Nakano;M.Nakano;M.Nakano;M.Nakano;M.Nakano;Hiroya Nitta;Suguru Ohta;Benoit Champagne
• 通讯作者: Benoit Champagne

Monte Carlo Wave-Function(MCWF) Approach to Dissipative Quantum Systems Interacting with a Single-Mode Quantized Field

与单模量化场相互作用的耗散量子系统的蒙特卡罗波函数 (MCWF) 方法

• 发表时间: 2003
• 期刊: Int. J. Quantum Chem. 95
• 作者: M.Nakano;B.Champagne;M.Nakano;M.Nakano;B.Champagne;M.Takahata;R.Kishi;M.Nakano;M.Nakano;M.Nakano;R.Kishi;M.Nakagawa;S.Yamada;M.Takahata;M.Nakano;S.Ohta;Benoit Champagne;Masayoshi Nakano;Benoit Champagne;M.Takahata;Ryohei Kishi;Masayoshi Nakano;Masayoshi Nakano;Ryohei Kishi;Nozomi Nakagawa;Satoru Yamada;Masayoshi Nakano;Suguru Ohta;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;Satoru Yamada;Kizashi Yamaguchi;Masayoshi Nakano;Ryoichi Kishi;Satoru Yamada;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;S.Yamada;K.Yamaguchi;M.Nakano;R.Kishi;M.Nakano;M.Nakano;M.Nakano;M.Nakano;Masayoshi Nakano;Satoru Yamada;Kizashi Yamaguchi;Masayoshi Nakano;Ryohei Kishi;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;Masayoshi Nakano;M.Nakano;M.Nakano;H.Fujita;M.Takahata;M.Nakano;M.Nakano
• 通讯作者: M.Nakano

M.Takahata: "Asymmetric structural effects on exciton migration of dendritic molecular aggregates"Synthetic Metals. 137. 875-876 (2003)

M.Takahata：“树枝状分子聚集体激子迁移的不对称结构效应”合成金属。