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Development of Various Two-Dimensional Vibrational Spectroscopy and Its Application for Practical Use

各种二维振动光谱的发展及其实际应用

基本信息

批准号：
13554019
负责人：
TOMINAGA Keisuke
金额：
$ 8.96万
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：
2001
资助国家：
日本
起止时间：
2001 至 2003
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-13554019/
关键词：
2D Vibrational Spectroscopy IR Photon Echo IR Transient Grating IR Short Pulse Femtosecond Solid State Laser Anharmonicity Vibrational Dephasing Vibrational Population Relaxation 赤外非線形分光

项目摘要

By using a infrared short pulse with a duration of 55 fs and energy more than 1 μJ/pulse, which is the shortest IR pulse with a high energy, we have developed third order optical nonlinear spectroscopy and applied to vibrational dynamics in condensed phases. The examples are three-pulse photon echo method, wavelength-resolved three-pulse photon echo method, and wavelength-resolved transient grating method. In these methods we can plot a signal as a function of multi-dimensional coordinates such as delay time and frequency. Especially, wavelength-resolved three-pulse photon echo method is a vibrational analogue of two-dimensional NMR. We applied these methods to several vibrational modes in condensed phases to obtain, for example, the time-correlation function of the transition frequency fluctuation, lifetime of the vibrational excited state, reorientational time, and anharmonicity. The examples are the anti-symmetric stretching modes of OCN^-and SCN^-in methanol, the anti-symmetric CN … More stretching mode of Fe(CN)_6^<4->, the CO stretching mode of coordinated to Ruporphyryine, anti-symmetric -N=C=N-stretching mode, and the OH stretching mode of water in a reverse micelle. One of the problems to be overcome for practical use is to obtain very stable IR pulse. At first, we thought that IR short pulse should have an enough high energy, but we found that rather than that shot-to-shot stability of the pulse is more important that the high energy. The present system uses superfluorescence for optical parametric generation (OPG), and this method easily introduces un-stable nature in the pulse. Therefore, we have constructed a new system which uses white light for OPG, and difference frequency mixing set up to generate IR pulses. We have obtained idler pulses in the near IR region from 1.7 to 2.4 mm, signal pulses in the near IR region from 1.1 to 1.5 mm, and IR pulse in the mid-IR region from 3.0 to 5.0 mm. A shot-to-shot stability of the mid IR pulse is about 0.3%, which is almost the best performance ever recorded. Less

利用脉宽为55 fs、能量大于1 μJ/pulse的最短高能红外脉冲，发展了三阶非线性光学光谱，并应用于凝聚相振动动力学研究。实例有三脉冲光子回波法、波长分辨三脉冲光子回波法和波长分辨瞬态光栅法。在这些方法中，我们可以将信号绘制为多维坐标（例如延迟时间和频率）的函数。特别是波长分辨三脉冲光子回波法是二维核磁共振的振动模拟。我们将这些方法应用于凝聚相中的几种振动模式，以获得例如跃迁频率波动的时间相关函数、振动激发态的寿命、再取向时间和非谐性。这些例子是OCN^-和SCN^-在甲醇中的反对称伸缩模，反对称CN ^-和SCN^-在甲醇中的反对称伸缩模。 ...更多信息反胶束中Fe（CN）_6 ~（2-）的伸缩模<4->、Ruphyryine配位的CO伸缩模、反对称-N=C= N-伸缩模和水的OH伸缩模。实际应用中需要克服的问题之一是获得非常稳定的红外脉冲。起初，我们认为红外短脉冲应该有足够高的能量，但我们发现，而不是拍到拍脉冲的稳定性更重要的是高能量。目前的系统利用超荧光产生光参量，这种方法容易在脉冲中引入不稳定性。因此，我们建立了一个新的系统，使用白色光的OPG，差频混合设置产生红外脉冲。我们已经获得了空闲脉冲在近红外区域从1.7到2.4毫米，信号脉冲在近红外区域从1.1到1.5毫米，和IR脉冲在中红外区域从3.0到5.0毫米。一个拍摄到拍摄的中红外脉冲的稳定性约为0.3%，这几乎是有史以来最好的性能记录。少