Theoretical Studies of Electron Dynamics in Nanometer-Sized Molecules

纳米分子中电子动力学的理论研究

基本信息

批准号：
17550024
负责人：
NOBUSADA Katsuyuki
金额：
$ 1.73万
依托单位：
Institute for Molecular Science
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2005
资助国家：
日本
起止时间：
2005 至 2006
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-17550024/
关键词：
electron dynamics optical response quantum dissipation

项目摘要

Dynamics in molecular systems is classified into two categories: one is nuclear (or ion) dynamics and the other one is electron dynamics. Chemical reaction dynamics is a typical example of the nuclear dynamics. On the other hand, the electron dynamics is related to linear and nonlinear optical response, electron charge transfer, or electronic conduction in molecular junctions. Despite their importance, the electron dynamics has not yet been studied theoretically because the electron dynamics is an ultrafast process and it is difficult to take account of electron correlation accurately. We have theoretically demonstrated that circularly polarized laser pulses induce electric currents and magnetic moments in ring-shaped molecules Na_<10> and benzene. The time-dependent adiabatic local density approximation was employed for this purpose, solving the time-dependent Kohn-Sham equation in real-space and real-time. It has been found that the electric currents are induced efficiently and persist continuously even after the laser pulses were switched off provided the frequency of the applied laser pulse is in tune with the excitation energy of the electronic excited state with the dipole strength for each molecular system. The electric currents were definitely revealed to be a second order nonlinear optical response to the magnitude of the electric field. The magnetic dipole moments inevitably accompany the ring currents, so that the molecules are magnetized. The production of the electric currents and the magnetic moments in the present procedure is found to be much more efficient than that utilizing static magnetic fields. We then proceeded to develop a numerical method based on quantum Liouville equation in order to discuss electron dynamics in quantum dissipative systems.

分子系统动力学分为两类：一类是核（或离子）动力学，另一类是电子动力学。化学反应动力学是核动力学的典型例子。另一方面，电子动力学与分子结中的线性和非线性光学响应、电子电荷转移或电子传导有关。尽管电子动力学很重要，但尚未在理论上进行研究，因为电子动力学是一个超快的过程，并且很难准确地考虑电子相关性。我们从理论上证明了圆偏振激光脉冲在环形分子Na_<10>和苯中感应出电流和磁矩。为此，采用了时间相关的绝热局域密度近似，实时求解了时间相关的 Kohn-Sham 方程。已经发现，即使在激光脉冲关闭后，只要所施加的激光脉冲的频率与电子激发态的激发能量以及每个分子系统的偶极子强度相一致，电流就会被有效地感应并持续存在。。电流被明确地揭示为对电场强度的二阶非线性光学响应。磁偶极矩不可避免地伴随着环电流，从而使分子被磁化。发现本过程中电流和磁矩的产生比利用静磁场产生的效率高得多。然后，我们继续开发一种基于量子刘维尔方程的数值方法，以讨论量子耗散系统中的电子动力学。

项目成果

期刊论文数量（12）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Efficient Numerical Method for Calculating Exciton States in Quantum Boxes

计算量子盒中激子态的有效数值方法

DOI：
发表时间：
2007
期刊：
Phys. Lett. A (in press)
影响因子：
0
作者：
Y.Kubota;K.Nobusada
通讯作者：
K.Nobusada

Gold-Thiolate Core-in-Cage Cluster [Au25 (SCH3) 18] Shows Localized Spins in Charged States

金硫醇笼核心簇 [Au25 (SCH3) 18] 显示带电状态下的局部自旋

DOI：
发表时间：
2007
期刊：
Phys. Lett. A (in press)
影响因子：
0
作者：
T.Iwasa;K.Nobusada
通讯作者：
K.Nobusada

Electronic structure calculations at constant chemical potential toward the application to electrochemistry

恒定化学势下的电子结构计算及其在电化学中的应用

DOI：
发表时间：
2007
期刊：
Comp. Phys. Comm. (in press)
影响因子：
0
作者：
K.Shiratori;K.Nobusada
通讯作者：
K.Nobusada

Photoinduced electric currents in ring-shaped molecules by circularly polarized laser pulses

DOI：
10.1103/physreva.75.032518
发表时间：
2007-03
期刊：
Physical Review A
影响因子：
2.9
作者：
K. Nobusada;K. Yabana
通讯作者：
K. Nobusada;K. Yabana

Electric currents in ring-shaped molecules induced by circularly polarized laser pulses

圆偏振激光脉冲在环形分子中引起的电流

DOI：
发表时间：
2007
期刊：
Computational Physics Communications 177
影响因子：
0
作者：
Hada;T;et. al.;羽田亨;K. Nobusada and K. Yabana;T. Otobe and K. Yabana;寺澤敏夫;K. Nobusada and K. Yabana
通讯作者：
K. Nobusada and K. Yabana