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

已经研究了理论和计算的各种物理和化学现象，用于包括树突系统和激光领域在内的超分子系统之间的相互作用。成就描述如下。1。我们已经开发了一种一般计算方法，该方法处理了与各种量子场相互作用的多状态模型，并研究了多光子过程的影响，这是非线性光学效应对这种动力学的影响。特别是，我们开发了一种新的方法，该方法治疗了使用量子主方程方法在动力学上分子振动和碰撞引起的弛豫效应。对于与两种量子场相互作用的二聚体模型系统，发现二聚体系统激发状态种群的塌陷恢复现象在振荡放大器中受到显着影响，并通过分子间偶极 - 偶极 - 偶极 - 复兴时间受到影响。事实证明，二聚体系统的纯相和种群松弛破坏了……二聚体电子状态之间的相干性更多，导致分子非线性光学效应的显着衰减。现在正在研究对外部量子场的令人兴奋的放松率和外部量子场的量子统计数据，现在正在研究树突系统的动态和非线性光学现象。2。我们已经研究了光收集和动态的非线性光学现象，包括树突状系统的超分子系统，包括树突状系统，以阐明结构预处理。已经开发了一种新型的计算方法，该方法已经开发出了单位分子聚集体模型系统的动态非线性光学性能，并应用于具有各种令人兴奋的迁移速率的纳米级树突状聚集系统非线性光谱的计算。事实证明，由激动人心的迁移造成的纯粹的塑料已被发现显着增加了频谱宽度并降低了峰值。为了治疗实际的超分子系统，例如树突聚合物，我们开发了一种基于从头算分子轨道轨道构型相互作用（CI）的量子主方程方法（CI），并阐明了有效的定向能量迁移起源于通过Meta-辅助固定的苯甲酸苯甲酸苯二氨基化的πConjugation的部分渗透。我们还开始研究开放式分子作为超分子系统的单位（构建基块），从理论上发现非线性光学效应显着取决于旋转状态和偏差特征。预计这种有吸引力的结果将是非线性光学材料领域的新型系统。较少的

项目成果

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

1.3.3.12, dendritic polymer

1.3.3.12、树枝状聚合物

• 发表时间: 2005
• 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;Ryohei Kishi;Masayoshi Nakano;岸亮平;R.Kishi
• 通讯作者: R.Kishi

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。

M.Nakano: "Monte Carlo wave-function approach to the quantum-phase dynamics of a dissipative molecular system interacting with a single-mode amplitude-squeezed field"J.Chem.Phys.. 119. 12106-12118 (2003)

M.Nakano：“蒙特卡罗波函数方法研究与单模振幅压缩场相互作用的耗散分子系统的量子相动力学”J.Chem.Phys.. 119. 12106-12118 (2003)

M.Nakano: "Advances in Multiphoton Processes and Spectroscopy"World Scientific. 146 (2003)

M.Nakano：“多光子过程和光谱学的进展”世界科学。