论文标题

热声子和热应力在二硫化钼的微拉曼光谱中的影响

Effects of hot phonons and thermal stress in micro-Raman spectra of molybdenum disulphide

论文作者

Sokalski, Peter, Han, Zherui, Fleming, Gabriella Coloyan, Smith, Brandon, Sullivan, Sean E., Huang, Rui, Ruan, Xiulin, Shi, Li

论文摘要

微拉曼光谱已成为探测新兴功能材料(例如二维(2D)分层结构)中嗜热物理行为的重要工具。聚焦的拉曼激发激光束的局部加热有望在材料中产生应力和非平衡温度分布。在这里,我们研究了热光音子在二硫化钼(MOS2)的拉曼光谱中的影响,并将其与热诱导的压缩应力引起的作用,从而导致聚焦的拉曼激光斑点拉曼频率蓝移。由于在微拉曼测量中考虑了应力效应,因此发现热光音子和声音子浴之间的非平衡程度比在悬浮石墨烯的先前微摩曼测量中观察到的声音浴比。与布里鲁因区和声音声子中的其他光学声子相比,该观察结果与基于第一原理的理论预测对过度人口中心的光学声子的理论预测一致。这些发现提供了对这种新兴的2D金属二甲基化金属元素(TMD)电子和光电材料中能量放松过程的详细见解,并阐明了该和其他2D材料中热传输的微拉曼测量中的一个重要问题。

Micro-Raman spectroscopy has become an important tool in probing thermophysical behavior in emerging functional materials such as two-dimensional (2D) layered structures. Localized heating by the focused Raman excitation laser beam is expected to produce both stress and nonequilibrium temperature distributions in the material. Here we investigate the effects of hot optical phonons in the Raman spectra of molybdenum disulphide (MoS2) and distinguish them from those caused by thermally-induced compressive stress, which causes a Raman frequency blue shift in the focused Raman laser spot. With the stress effect accounted for in micro-Raman measurements, the degree of nonequilibrium between the hot optical phonons and the acoustic phonon bath is found to be much smaller than those observed in prior micro-Raman measurements of suspended graphene. The observation agrees with a first-principles based theoretical prediction of overpopulated zone-center optical phonons compared to other optical phonons in the Brillouin zone and acoustic phonons. The findings provide detailed insight into the energy relaxation processes in this emerging 2D transition metal dichalcogenide (TMD) electronic and optoelectronic material and clarify an important question in micro-Raman measurements of thermal transport in this and other 2D materials.

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