Experimental and theoretical Raman spectroscopy of isotopically pure and diluted ice VI
Experimental and theoretical Raman spectroscopy of isotopically pure and diluted ice VI
复制标题
同位素纯冰和稀释冰的实验和理论拉曼光谱 VI
DOI：
10.1021/acs.jpcc.2c05133
复制
发表时间：
2022
期刊：
影响因子：
3.7
通讯作者：
Takuma Yagasaki. Shoichi Yamaguchi
中科院分区：
文献类型：
--
作者：
Tetsuyuki Takayama;Kota Kishi;Takuhiro Otosu;Takuma Yagasaki. Shoichi Yamaguchi
我们提出了一个实验和理论的拉曼光谱研究同位素纯和稀释冰六在室温下1 GPa。在实验中，我们测量了在金刚石砧细胞中加压的多晶冰VI的oh -拉伸拉曼光谱。在分子动力学（MD）模拟和光谱图的基础上，我们还获得了冰六和冰六的理论拉曼光谱。我们发现理论拉曼光谱与实验数据吻合良好，证明了光谱图和MD模拟不仅在环境条件下，而且在高压条件下的适用性和准确性。特别是，理论计算成功地再现了实验观测到的冰VI比冰Ih更宽的带宽。通过对MD轨迹的分析，我们将这种带宽差异归因于oh -拉伸频率的位点依赖性，特别是在冰VI中发生。本研究表明，振动光谱中实验和理论的结合对于获得复杂分子系统的微观理解是多么强大。
We present an experimental and theoretical Raman spectroscopic study of isotopically pure and diluted ice VI at 1 GPa at room temperature. In the experiment, we measured the OH-stretch Raman spectra of polycrystalline ice VI pressurized in a diamond anvil cell. We also obtained the theoretical Raman spectra of ice VI as well as ice Ihon the basis of molecular dynamics (MD) simulations and a spectroscopic map. We find that the theoretical Raman spectra are in good agreement with the experimental data, which proves the applicability and accuracy of the spectroscopic map and the MD simulations not only in the ambient condition but also at the high pressure. In particular, the theoretical calculation successfully reproduces the experimental observation of the broader bandwidth of ice VI as opposed to ice Ih. Through the analysis of the MD trajectories, we attribute this bandwidth difference to the site dependence of the OH-stretch frequency that takes place specifically in ice VI. The present study demonstrates how powerful the combination of experiment and theory in vibrational spectroscopy can be for gaining a microscopic understanding of complex molecular systems.