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Development of Two-Dimenssional Raman Spectroscopy Based on Seventh Order Optical Nonlinear Phenomena

基于七阶光学非线性现象的二维拉曼光谱的发展

基本信息

批准号：
10440181
负责人：
TOMINAGA Keisuke
金额：
$ 9.02万
依托单位：
Kobe University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
1998
资助国家：
日本
起止时间：
1998 至 1999
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-10440181/
关键词：
two-dimensional Raman spectroscopy higher-order optical nonlinear phenomena ultrafast spectroscopy Ti : sapphire laser liquid dynamics

项目摘要

Two-dimensional Raman spectroscopy based on seventh order optical nonlinear phenomena has been developed experimentally and theoretically. We have constructed two short pulse laser system in order to perform the two-dimensional Raman experiment. One is a femtosecond dye laser system, which can produce two short pulses with different colors. The pulse width is about 100 fs. The other system is an intra-cavity dumped Ti : sapphire laser system, which produces a pulse width of 13 fs and energy of 67 nJ/pulse at 4 MHz. Currently, a multi-pass (six-pass) amplifier with a Ti : sapphire crystal is being designed and constructed to get a higher energy pulse. The purpose of this amplifier is to get a pulse with an energy more than sub microJ/pulse at 20 kHz. We are now constructing a detectionsystem inclusing optics for the seventh order nonlinear experiment. Theoretically, we have developed two different models to predict the two dimensional vibrational spectrum. One is to use perturbed states as stationary states and consider possible quantum pathways. By this method we show a physical picture ina qualitative level for the cross peaks in the seventh order two-dimensional Raman spectrum. The other method is to use unperturbed states as a basis set and solve a stochastic-Liouville equation. This method is capable of including more than two states in the formation quite easily, allowing us to apply optical nonlinear spectroscopy to dynamical studies of chemical reactions.

基于七阶光学非线性现象的二维拉曼光谱在实验和理论上得到了发展。为了进行二维拉曼实验，我们搭建了两套短脉冲激光系统。一种是飞秒染料激光系统，它可以产生两个不同颜色的短脉冲。脉冲宽度约为100 fs。另一个系统是腔内倒空钛宝石激光器系统，其在4 MHz下产生13 fs的脉冲宽度和67 nJ/脉冲的能量。目前，一个多通（六通）放大器与钛：蓝宝石晶体的设计和建造，以获得更高的能量脉冲。该放大器的目的是在20 kHz下获得能量大于亚微焦/脉冲的脉冲。我们正在为七阶非线性实验建立一个包括光学系统的探测系统。在理论上，我们发展了两种不同的模型来预测二维振动谱。一种是使用微扰态作为定态，并考虑可能的量子路径。用这种方法，我们在定性水平上给出了七阶二维拉曼谱中交叉峰的物理图象。另一种方法是以未扰动态为基组，求解随机刘维尔方程。这种方法能够包括两个以上的国家的形成相当容易，使我们能够应用光学非线性光谱的化学反应的动力学研究。