Theoretical Study on the Dynamics of Molecules Under Strong Laser Field

强激光场下分子动力学的理论研究

• 批准号: 63044013
• 负责人: FUJIMURA Yuichi
• 金额: $ 1.92万
• 依托单位: Faculty of Science, Tohoku University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for international Scientific Research
• 财政年份: 1988
• 资助国家: 日本
• 起止时间: 1988 至 1990
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-63044013/
• 关键词: Strong Laser Field; Dressed State; Nuclear Wave Packet; Dynamic Stark Effect; Multiphoton Process; 01Coherent, Nonlinear Molecule-Radiation Field Interaction; レ-ザ化学

The purpose of this research project was to develop a fundamental theory toward the laser control of chemical reactions through the nonlinear, coherent interactions between molecules and strong laser fields. We were concerned with main subjects such as photon statistical effects on time evolution of molecules, bath-induced multiphoton process, spectral band theory of multi-level molecules under strong laser fields, restriction of intramolecular vibrational redistribution (IVR) by using coherent lasers, and photo dissociation mechanism under strong, nonstationary laser fields. We have treated the molecule-radiation intevactions not only under isolated condition but also in the presence of the heat bath. Through most of the research projects, theoretical treatments of dynamics of molecules under strong laser fields have been developed without invoking the perturbation theory in the dressed state representation. Especially, the laser phase has been shown to make an important role in contr … More olling IVR by using stationary laser fields. The emission multiplet structure of a multi-level molecule under strong laser field can not be interpreted in terms of the simple extension of two level molecule because of presence of interference effects between the dressed states. The theoretical treatment of photodissociation above threshold under nonstationary, strong laser field has been established based on the method of the nuclear wave packet propagation. Theory of laser-controlled chemical reaction of polyatomic molecules except simple diatoomic molecule ions, however, could not be developed within the term of this program because of the time restriction. We continue developing the theory of the laser controlling chemical reaction toward application to chemical reactions of interest such as intramolecular proton transfer, isomerization etc. We are convinced that the results obtained in this research project could provide important clue to performing experiments of the laser-controlled chemical reactions. Less

该研究项目的目的是通过分子与强激光场之间的非线性，连贯的相互作用来开发一种基本理论，以对化学反应进行激光控制。我们关注的是主要受试者，例如光子统计对分子时间演变的影响，浴诱导的多光子过程，在强激光场下的多级分子的光谱带理论，限制了分子内振动重新分布（IVR），使用相干激光器使用相对性激光以及在强度的机械机构下进行了强度的机构。我们已经处理了分子辐射的内膜，不仅在孤立的条件下，而且在存在热浴的情况下。通过大多数研究项目，已经开发了强度激光领域下分子动力学的理论治疗，而没有在穿着状态表示中调用扰动理论。尤其是，已经证明激光阶段在对照中发挥了重要作用……通过使用固定激光场更多的IVR。由于穿着状态之间存在干扰效应，因此无法根据两个级分子的简单扩展来解释多级分子的发射多重结构。基于核波包传播的方法，已经建立了在非平稳性激光场下高于阈值的光解离的理论处理。但是，由于时间限制，在该程序的任期内无法开发多原子分子的激光控制的化学反应理论。我们继续发展对应用化学反应的激光理论，以应用于感兴趣的化学反应，例如分子内质子转移，异构化等。我们坚信，该研究项目中获得的结果可以为执行激光控制化学反应的实验提供重要的线索。较少的

项目成果

S. H. Lin: "Theory of Multiphoton Processes by the Fourier-expansion Density Matrix Method." J. Chem. Phys.92. 2910-2916 (1990)

S. H. Lin：“傅里叶展开密度矩阵法的多光子过程理论”。

Y. Ohtsuki: "Band Structure of Stationary Emission Spectra from a Three-level Molecule Pumped by Strong Radiation Fields." J. Chem. Phys.93. 3012-3032 (1990)

Y. Ohtsuki：“强辐射场泵浦的三能级分子的固定发射光谱的能带结构。”

H. Kono: "Theory of Resonance Secondary Emission in Femtosecond Laser Excitation : On the Connection with Wave Packet Dynamics." J. Chem. Phys.91. 5960-5973 (1989)

H. Kono：“飞秒激光激发中的共振二次发射理论：与波包动力学的联系。”

Y. Nomura: "Effects of Photon Field Coherence on Selective Excitation of a Molecule." Trends in Chem. Phys.1. 31-36 (1990)

Y. Nomura：“光子场相干性对分子选择性激发的影响。”

H. Kono: Adv. Chem. Phys. (John Wiley & Sons, Inc.). A Theoretical Study of Origins of Resonance Raman Resonance Fluorescence Using a Split-up of the Emission Correlation Function., 403-462 (80,)

H.科诺：Adv。