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Generation of High Power Infrared Short Pulse by Cr:Forsterite and Development of Two-Dimensional Vibrational Spectroscopy

Cr:镁橄榄石产生高功率红外短脉冲及二维振动光谱学的发展

基本信息

批准号：
12304036
负责人：
TOMINAGA Keisuke
金额：
$ 8.65万
依托单位：
Kobe University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
财政年份：
2000
资助国家：
日本
起止时间：
2000 至 2002
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-12304036/
关键词：
high-power infrared short pulse infrared nonlinear spectroscopy two-dimensional vibrational spectroscopy infrared photon echo infrared transient grating vibrational dephasing vibrational population relaxation solvation dynamics フェムト秒固体レーザー

项目摘要

We have developed high power, infrared (IR) short pulse and third order optical nonlinear spectroscopy in the infrared region using the IR pulse. The infrared pulses are generated by some optical nonlinear processes such as difference frequency mixing and optical parametric generation/amplification with an all-solid-state laser. Group velocity dispersion in the pulse is compensated by inserting a silicon plate in the optical path. The pulse width is measured to be 55 fs with an energy of more than microJ/pulse by an autocorrelation method, which is the shortest pulse of the infrared pulse with such a high energy to our knowledge. Using this pulse we have constructed optical systems of nonlinear spectroscopy such as time-integrated and frequency-resolved transient grating, time-integrated and frequency-resolved 2- and 3-pulse photon echo. These techniques are multi-dimensional methods in time and/or frequency, and the frequency-resolved 3-pulse photon echo is a homodyne detected vibrational version of 2D NMR. We have applied these techniques to several vibrational modes such as three-atom ions (OCN^- and SCN^-) in polar solvents, the -N=C=N- anti-stretching modes of large organic molecules, the C=O stretching modes of metal porphyrines, the CN stretching modes of cyano-iron complexes, and the OH stretching mode of hydrogen bonding liquids. We discuss vibrational dynamics of these modes including vibrational population relaxation, pure vibrational dephasing, dynamical fluctuation and spectral diffusion, inhomogeneity of the transition frequency, and so on.

利用红外脉冲，我们发展了高功率、红外短脉冲和红外区三阶非线性光学光谱技术。利用全固态激光器，通过差频混频、光参量产生/放大等光学非线性过程产生红外脉冲。在光路中插入硅片补偿了脉冲的群速度色散，用自相关法测得脉冲宽度为55 fs，能量超过微焦耳/脉冲，是迄今为止已知的最短的高能量红外脉冲。利用该脉冲，我们建立了时间积分和频率分辨的瞬态光栅、时间积分和频率分辨的二脉冲和三脉冲光子回波等非线性光谱光学系统。这些技术是时间和/或频率上的多维方法，并且频率分辨的3脉冲光子回波是2D NMR的零差检测振动版本。我们已经将这些技术应用于几种振动模式，例如极性溶剂中的三原子离子（OCN^-和SCN^-），大有机分子的-N=C=N-反伸缩模式，金属卟啉的C=O伸缩模式，氰基铁络合物的CN伸缩模式和氢键液体的OH伸缩模式。我们讨论了这些模式的振动动力学，包括振动布居弛豫、纯振动退相、动力学涨落和光谱扩散、跃迁频率的不均匀性等。