Yu Guoyang, Zeng Yangyang, Guo Wencan, Wu Honglin, Zhu Gangbei, Zheng Zhaoyang, Zheng Xianxu, Song Yunfei, Yang Yanqiang
National Key Laboratory of Shock Wave and Detonation Physics, Institute of Fluid Physics, China Academy of Engineering Physics , Mianyang 621900, People's Republic of China.
J Phys Chem A. 2017 Apr 6;121(13):2565-2571. doi: 10.1021/acs.jpca.7b00069. Epub 2017 Mar 24.
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 is a portal of energy transfer from outside to inside of the RDX molecule and the mode at 672 cm is an important transit point of energy transfer in the IVR.
飞秒时间分辨多路相干反斯托克斯拉曼散射（CARS）技术已被用于研究1,3,5-三硝基-1,3,5-三氮杂环己烷（RDX）分子中通过振动耦合的分子内振动再分布（IVR）。在多路CARS实验中，超连续谱（SC）被用作宽带斯托克斯光，以相干且集体地激发多个振动模式，并观察到这些模式之间振动耦合产生的量子拍。RDX的IVR通过这些振动耦合的拓扑图可视化，通过对拓扑图的分析，确认了两个均归属于环弯曲的振动模式与大多数其他振动模式具有耦合相互作用，并被认为具有与这些振动模式进行能量转移的趋势。我们认为，466 cm处的模式是能量从RDX分子外部向内部转移的门户，而672 cm处的模式是IVR中能量转移的重要过渡点。
