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Exploring a free energy landscape of frustrated system by means of multi-dimensional spectroscopes

利用多维光谱仪探索受挫系统的自由能景观

基本信息

批准号：
15205005
负责人：
TANIMURA Yoshitaka
金额：
$ 27.96万
依托单位：
Kyoto University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
财政年份：
2003
资助国家：
日本
起止时间：
2003 至 2006
项目状态：
已结题

项目摘要

The free energy landscape (FEL) is the conformational substates of the free energy as a function of macroscopic variables, which has been widely used to characterize the dynamical behavior of frustrated systems such as glasses and proteins. The aim of this research is to clarify some of postulation used to describe the dynamics of a frustrated system by exploring a possibility to measure the FEL directly by optical means. For this purpose, we consider a system consists of dipoles and employ a simple model to reduce the degrees of freedom. We calculated the FEL at various temperatures by generating all possible states and studied the dynamics of dipoles on the FEL by constructing the master equation for all states. For temperatures higher than the energy scale of dipole-dipole interactions. The free energy landscapes have quadratic shape. When the temperature drops, small notched structures appear on the free energy profiles because of the frustrated interactions among dipoles. From thi … More s approach, the new insight for electron transfer problem was obtained below the glass transition temperature, where the Marcus theory breaks down. The sensitivity of multidimensional spectroscopy is fully used to characterize the dynamics upon different FEL. Here, we calculated two-dimensional signals corresponding to infrared, far IR or THz spectroscopy defined by the four-body correlation functions of dipole operators. While the linear absorption signals decay in time in a similar manner regardless of the FEL profiles, the 2D signals exhibit prominent differences in those profiles. This indicates that, we may differentiate the profiles of FEL by changing two-time valuables involved in 2D spectroscopy. We also developed an efficient algorithm to study the dynamics of molecules on mulitidimensional spectroscopy from molecular dynamics simulation approach, which hybridizes the existing equilibrium and nonequilibrium methods of calculating multidimensional spectroscopy. As an application of this simulation method, we calculated two-dimensional Raman spectrum of various molecular liquids. Less

自由能景观（FEL）是自由能作为宏观变量的函数的构象子态，它已被广泛用于表征玻璃和蛋白质等阻挫体系的动力学行为。本研究的目的是通过探索用光学方法直接测量自由电子激光的可能性，来澄清一些用来描述受抑系统动力学的假设。为此，我们考虑一个系统由偶极子和采用一个简单的模型，以减少自由度。通过生成所有可能的态，计算了不同温度下的自由电子激光，并通过构造所有态的主方程，研究了自由电子激光上偶极子的动力学。对于温度高于偶极-偶极相互作用的能量标度。自由能景观具有二次形状。当温度降低时，由于偶极间的相互作用受阻，自由能剖面上出现了小的缺口结构。从这个 ...更多信息在Marcus理论失效的玻璃化转变温度以下，电子转移问题得到了新的认识。充分利用多维光谱的灵敏度来表征不同自由电子激光的动力学特性。在这里，我们计算了对应于红外，远红外或太赫兹光谱定义的偶极算子的四体相关函数的二维信号。虽然线性吸收信号在时间上以类似的方式衰减，而不管自由电子激光分布，2D信号在这些分布中表现出显著的差异。这表明，我们可以通过改变二维光谱中的二次值来区分自由电子激光的轮廓。我们还开发了一种有效的算法来研究分子动力学的多维光谱从分子动力学模拟方法，它混合了现有的平衡和非平衡计算多维光谱的方法。作为这种模拟方法的一个应用，我们计算了各种分子液体的二维拉曼光谱。少

项目成果

期刊论文数量（100）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Quantum dynamics of a system strongly coupled to a low temperature colored noise bath : reduced hierarchy_equations approach

与低温有色噪声浴强耦合的系统的量子动力学：简化的层次方程方法

DOI：
发表时间：
2005
期刊：
J. Phys. Soc. Jpn. 74
影响因子：
0
作者：
A. Ishizaki;Y. Tanimura
通讯作者：
Y. Tanimura

K.Okumura, Y.Tanimura: "Energy-level diagrams & their contribution to 5th-order Raman and 2nd-order infrared responses : 【triple bond】"Journal of Physical Chemistry. A107. 8092-8105 (2003)

K.Okumura、Y.Tanimura：“能级图及其对五阶拉曼和二阶红外响应的贡献：[三键]”物理化学杂志 A107（2003）。

DOI：
发表时间：
期刊：
影响因子：
0
作者：
通讯作者：

Modeling vibrational dephasing and energy relaxation processes of intermolecular anharmonic modes for multidimensional infrared spectrosconies

多维红外光谱分子间非简谐振动模式的振动相移和能量弛豫过程建模

DOI：
发表时间：
2006
期刊：
J.Chem.Phys. 125
影响因子：
0
作者：
Takeshi Mizunoya;Katsuhiro Sakurai;Riki Morioka;Yoshiro Higano;A.Ishizaki and Y.Tanimura
通讯作者：
A.Ishizaki and Y.Tanimura

Two-dimensional spectroscopy for two-dimensional rotator coupled to a Gaussian-Markovian noise bath

与高斯-马尔可夫噪声浴耦合的二维旋转器的二维光谱