High-pressure behavior of a linear chain alkane, tricosane
High-pressure behavior of a linear chain alkane, tricosane
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DOI：
10.1063/1.5143450
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发表时间：
2020-03
影响因子：
3.2
通讯作者：
Abhisek Basu;Patrick P Murphy;M. Mookherjee;B. Haberl;R. Boehler
中科院分区：
文献类型：
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作者：
Abhisek Basu;Patrick P Murphy;M. Mookherjee;B. Haberl;R. Boehler
探索烃在压力下的行为对于理解其在行星科学中的作用以及探索新的有机化学具有重要意义。在这项研究中，我们利用拉曼光谱研究了一种线性链烃，三聚糖（C23H48）的高压行为。我们将三聚糖压缩到23gpa，并没有发现在本研究中探索的条件下压力诱导非晶化的任何证据。压缩后，我们在100-300 cm−1的低能区观察到新的模态。为了理解这些新模式在高压下的出现，我们使用了互补从头计算，并探索了链构型（线性和弯曲）对预测拉曼光谱的影响。我们发现在高压下观察到的这些新模式可以用三聚糖链的弯曲构型来更好地解释。因此，基于高压拉曼光谱，三聚糖的线性链很可能在压力下发生弯曲，即发生压力诱导的反式间扭转变。这种弯曲区域（即扭结）也可能在与类木行星内部相关的极端条件下，作为大链碳氢化合物分解成小链长度的位点。探索烃在压力下的行为对于理解其在行星科学中的作用以及探索新的有机化学具有重要意义。在这项研究中，我们利用拉曼光谱研究了一种线性链烃，三聚糖（C23H48）的高压行为。我们将三聚糖压缩到23gpa，并没有发现在本研究中探索的条件下压力诱导非晶化的任何证据。压缩后，我们在100-300 cm−1的低能区观察到新的模态。为了理解这些新模式在高压下的出现，我们使用了互补从头计算，并探索了链构型（线性和弯曲）对预测拉曼光谱的影响。我们发现在高压下观察到的这些新模式可以用三聚糖链的弯曲构型来更好地解释。因此，基于高压拉曼光谱，三聚糖的线性链很可能在压力下弯曲，即它经历了压力诱导的弯曲。
Exploring the behavior of hydrocarbon under pressure is important for understanding its role in planetary sciences and also for exploring novel organic chemistry. In this study, we explored the high-pressure behavior of a linear-chain hydrocarbon, tricosane (C23H48), using Raman spectroscopy. We compressed tricosane up to 23 GPa and did not find any evidence for pressure-induced amorphization within the conditions explored in this study. Upon compression, we observe new modes in the low energy region 100–300 cm−1. In order to understand the appearance of these new modes at high pressures, we used complementary ab initio calculations and explored the effect of chain configurations (linear and bent) on the predicted Raman spectra. We find that these new modes observed at higher pressures are better explained by bent configuration of tricosane chains. Thus, based on high-pressure Raman spectra, it is very likely that a linear chain of tricosane is bent under pressure, i.e., it undergoes a pressure-induced trans-gauche transformation. It is also likely that such bent regions (i.e., kinks) will act as sites along which large chain hydrocarbons could dissociate into smaller chain lengths at extreme conditions relevant to the interiors of Jovian planets.Exploring the behavior of hydrocarbon under pressure is important for understanding its role in planetary sciences and also for exploring novel organic chemistry. In this study, we explored the high-pressure behavior of a linear-chain hydrocarbon, tricosane (C23H48), using Raman spectroscopy. We compressed tricosane up to 23 GPa and did not find any evidence for pressure-induced amorphization within the conditions explored in this study. Upon compression, we observe new modes in the low energy region 100–300 cm−1. In order to understand the appearance of these new modes at high pressures, we used complementary ab initio calculations and explored the effect of chain configurations (linear and bent) on the predicted Raman spectra. We find that these new modes observed at higher pressures are better explained by bent configuration of tricosane chains. Thus, based on high-pressure Raman spectra, it is very likely that a linear chain of tricosane is bent under pressure, i.e., it undergoes a pressure-induced tr...