Visualizing Intramolecular Vibrational Redistribution in Cyclotrimethylene Trinitramine (RDX) Crystals by Multiplex Coherent Anti-Stokes Raman Scattering
Visualizing Intramolecular Vibrational Redistribution in Cyclotrimethylene Trinitramine (RDX) Crystals by Multiplex Coherent Anti-Stokes Raman Scattering
复制标题
通过多重相干反斯托克斯拉曼散射可视化环三亚甲基三硝胺 (RDX) 晶体中的分子内振动再分布
DOI：
10.1021/acs.jpca.7b00069
复制
发表时间：
2017-04-06
影响因子：
2.9
通讯作者：
Yang, Yanqiang
中科院分区：
文献类型：
--
作者：
Yu, Guoyang;Zeng, Yangyang;Yang, Yanqiang
用飞秒时间分辨多重相干反斯托克斯拉曼散射(CARS)技术研究了1，3，5-三硝基-1，3，5-三氮杂环己烷(RDX)分子通过振动耦合产生的分子内振动重分布(IVR)。在多重CARS实验中，利用超连续谱(SC)作为宽带斯托克斯光，相干地集体激发多个振动模，观察到这些振动模之间的振动耦合产生的量子拍频。RDX的IVR通过这些振动耦合的拓扑图被可视化，通过对拓扑图的分析，确认了两个振动模式与大多数其他振动模式存在耦合作用，并被认为与这些振动模式有能量传递的趋势。我们认为，466 cM(-1)处的模式是RDX分子外向内能量传递的门户，672 cM(-1)处的模式是IVR中能量传递的重要转换点。
The femtosecond time-resolved multiplex coherent anti-Stokes Raman scattering (CARS) technique has been performed to investigate intramolecular vibrational redistribution (IVR) through vibrational couplings in 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) molecules. In the multiplex CARS experiment, the supercontinuum (SC) was used as broad-band Stokes light to coherently and collectively excite multiple vibrational modes, and quantum beats arising from vibrational couplings among these modes were observed. The IVR of RDX is visualized by a topological graph of these vibrational couplings, and with analysis of the topological graph, two vibrational modes, both of which are assigned to ring bending, are confirmed to have coupling interactions with most of the other vibrational modes and are considered to have a tendency of energy transfer with these vibrational modes. We suggest that the mode at 466 cm(-1) is a portal of energy transfer from outside to inside of the RDX molecule and the mode at 672 cm(-1) is, an important transit point of energy transfer in the IVR.