Electron transfer and protein transfer reactions in salvation and protein environments

救赎和蛋白质环境中的电子转移和蛋白质转移反应

• 批准号: 10206210
• 负责人: TANIMURA Yoshitaka
• 金额: $ 10.94万
• 依托单位: Okazaki National Research Institutes
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research on Priority Areas (B)
• 财政年份: 1998
• 资助国家: 日本
• 起止时间: 1998 至 2000
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-10206210/
• 关键词: Two-dimensional Spectroscopy; Fifth-order optical process; Qauntum Brownian model; Inhomogeneous; Fokker-Planck equation; Tunneling process; ブラウン運動; トンネル現象; 2次元赤外分光

We employ various statistical mechanical models, such as a quantum Brownian oscillator system with nonlinear system-bath interactions and a quantum dissipative rotator to study dynamics of molecules in condensed phases and we demonstrate how the differences of models reveal on two-dimensional spectroscopy as profiles of signals. Calculations of multi-time correlation functions of molecular coordinate, which are the observables of two-dimensional spectroscopy, are based on newly developed path-integral and quantum Fokker-Planck formalisms. For nonlinear system-bath coupling model, we calculate the three and four-time correlation functions, which corresponds to fifth-order Raman and infrared photon echo measurements, by solving Gaussian-Markovian Fokker-Planck equation and show an interesting change of signal profiles corresponding to the homogeneous and inhomogeneous distribution of system oscillators which are set by a noise correlation time. For damped rotator case, we obtained analytical solution of multi-time correlation functions by using analytical expression of generating functional and show that quantum effects play a minor role in two-time correlation functions, but play a major role In four-time correlation functions.Our results in three years (1998-2001) are published as nine scientific papers of JCP and CPL, etc.

我们使用不同的统计力学模型，如具有非线性系统-浴相互作用的量子布朗振子系统和量子耗散旋转子来研究凝聚相中分子的动力学，并展示了模型的差异是如何在二维光谱上揭示信号轮廓的。分子坐标的多时间关联函数是二维光谱学的观察量，它的计算是基于新发展的路径积分和量子福克-普朗克公式。对于非线性的系统-浴场耦合模型，通过求解高斯-马尔可夫福克-普朗克方程，计算了对应于五阶拉曼和红外光子回波测量的三倍和四倍关联函数，并显示了与系统振子的均匀和非均匀分布对应的有趣的信号轮廓的变化，该分布由噪声关联时间决定。对于有阻尼项的旋转体情况，我们利用生成泛函的解析表达式得到了多时间关联函数的解析解，表明量子效应在二时间关联函数中起次要作用，而在四时间关联函数中起主要作用。我们三年(1998-2001)的结果以JCP和CPL等9篇科学论文的形式发表。

项目成果

K.Okumura, A.Tokmakov, Tanimura: "Structural information from two-dimensional fifth-order Raman spectroscopy"J.Chem.Phys.. 111. 492-503 (1999)

K.Okumura、A.Tokmakov、Tanimura：“二维五阶拉曼光谱的结构信息”J.Chem.Phys.. 111. 492-503 (1999)

K. Okumura, D. M. Jonas, and Tanimura: "Multi-dimensional vibrational spectroscopy measured from different phase-matching conditions"Chem. Phys.. 266. 237-250 (2001)

K. Okumura、D. M. Jonas 和 Tanimura：“从不同相位匹配条件测量的多维振动光谱”Chem。

Y.Tanimura: "The 5th-and 7th-order 2D Roman spectroscopy for intramolecular vibrational modes"Proc.of Two-Dimensional Correlation Spectroscopy (AIP). (2000)

Y.Tanimura：“分子内振动模式的 5 阶和 7 阶 2D Roman 光谱”Proc.of 二维相关光谱 (AIP)。

Y.Tanimura, T.Steffen: "The Fifth and Seventh Order 2D Raman spectroscopy for harmonic system with Nonlinear system-bath interactions:Gaussian-Markovian case"J.Phys.Soc.Jpn.. 69. 4095-4106 (2000)

Y.Tanimura, T.Steffen：“具有非线性系统-浴相互作用的调和系统的五阶和七阶二维拉曼光谱：高斯-马尔可夫案例”J.Phys.Soc.Jpn.. 69. 4095-4106 (2000)

Y.Suzuki, Y.Tanimura: "Quantum theory of 2D rotator in a dissipative environment:Application to infrared spectroscopy"J.Phys.Soc.Jpn.. 70. 1167-1170 (2001)

Y.Suzuki、Y.Tanimura：“耗散环境中二维旋转器的量子理论：在红外光谱中的应用”J.Phys.Soc.Jpn.. 70. 1167-1170 (2001)