Time-Domain Rotational Raman Spectroscopy of the Ethylene Dimer and Trimer by Coulomb Explosion Imaging of Rotational Wave Packets,The Journal of Physical Chemistry A

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Time-Domain Rotational Raman Spectroscopy of the Ethylene Dimer and Trimer by Coulomb Explosion Imaging of Rotational Wave Packets
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2023-05-23 , DOI: 10.1021/acs.jpca.3c02149
Kenta Mizuse _{1,

2} , Koyomi Takano ₂ , Eri Kakizaki ₂ , Yuya Tobata ₁ , Yasuhiro Ohshima ₁

Affiliation

We report rotational Raman spectroscopy of the ethylene dimer and trimer, based on time-resolved Coulomb explosion imaging of rotational wave packets. Rotational wave packets were created in the gas-phase ethylene clusters upon nonresonant ultrashort pulse irradiation. The subsequent rotational dynamics were traced as spatial distribution of monomer ions ejected from the clusters via the Coulomb explosion process induced by a strong probe pulse. The observed images of monomer ions show multiple kinetic energy components. The time-dependence of the angular distribution for each component was analyzed, and the Fourier transformation spectra, which correspond to rotational spectra, were obtained. A lower kinetic energy component was mainly attributed to a signal from the dimer and a higher energy component mainly from the trimer. We have successfully observed rotational wave packets up to a delay time of ∼20 ns and achieved a spectral resolution of 70 MHz after Fourier transformation. Owing to this higher resolution than the previous studies, improved rotational and centrifugal distortion constants were obtained from the spectra. In addition to improving the spectroscopic constants, this study opens the way for rotational spectroscopy of larger molecular clusters than dimers through Coulomb explosion imaging of rotational wave packets. Details of spectral acquisition and analyses of each kinetic energy component are also reported.

中文翻译：

通过旋转波包的库仑爆炸成像对乙烯二聚体和三聚体进行时域旋转拉曼光谱分析

我们报告了乙烯二聚体和三聚体的旋转拉曼光谱，该光谱基于旋转波包的时间分辨库仑爆炸成像。在非共振超短脉冲照射下，在气相乙烯团簇中产生旋转波包。随后的旋转动力学被追踪为单体离子的空间分布，单体离子通过强探测脉冲引起的库仑爆炸过程从簇中喷射出来。观察到的单体离子图像显示出多个动能分量。分析了每个分量的角度分布的时间依赖性，并获得了对应于旋转光谱的傅里叶变换光谱。较低的动能成分主要归因于来自二聚体的信号，而较高的能量成分主要来自三聚体。我们已经成功地观察到延迟时间长达 ~20 ns 的旋转波包，并在傅立叶变换后实现了 70 MHz 的光谱分辨率。由于比以前的研究分辨率更高，从光谱中获得了改进的旋转和离心畸变常数。除了提高光谱常数外，这项研究还通过旋转波包的库仑爆炸成像，为比二聚体更大的分子簇的旋转光谱学开辟了道路。还报告了每个动能分量的光谱采集和分析的详细信息。从光谱中获得了改进的旋转和离心畸变常数。除了提高光谱常数外，这项研究还通过旋转波包的库仑爆炸成像，为比二聚体更大的分子簇的旋转光谱学开辟了道路。还报告了每个动能分量的光谱采集和分析的详细信息。从光谱中获得了改进的旋转和离心畸变常数。除了提高光谱常数外，这项研究还通过旋转波包的库仑爆炸成像，为比二聚体更大的分子簇的旋转光谱学开辟了道路。还报告了每个动能分量的光谱采集和分析的详细信息。

更新日期：2023-05-23

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