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Raman spectrometry study of phonon anharmonicity of hafnia at elevated temperaturesud

机译:高温下elevated的声子非谐性的拉曼光谱研究

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摘要

Raman spectra of monoclinic hafnium oxide (HfO_2) were measured at temperatures up to 1100 K. Raman peak shifts and broadenings are reported. Phonon dynamics calculations were performed with the shell model to obtain the total and partial phonon density of states, and to identify the individual motions of Hf and O atoms in the Raman modes. Correlating these motions to the thermal peak shifts and broadenings, it was found that modes involving changes in oxygen-oxygen bond length were the most anharmonic. The hafnium-dominated modes were more quasiharmonic and showed less broadening with temperature. Comparatively, the oxygen-dominated modes were more influenced by the cubic term in the interatomic potential than the hafnium-dominated modes. An approximately quadratic correlation was found between phonon-line broadening and softening.
机译:在高达1100 K的温度下测量了单斜晶氧化oxide(HfO_2)的拉曼光谱。据报道,拉曼峰移动并变宽。用壳模型进行声子动力学计算,以获得状态的总声子密度和部分声子密度,并确定拉曼模式中Hf和O原子的单个运动。将这些运动与热峰位移和增宽相关联,发现涉及氧-氧键长变化的模式是最不谐和的。 ha主导的模式更准谐波,并且随温度的展宽较小。相比之下,氧占主导地位的模式在原子间电势中受立方项的影响要大于the占主导地位的模式。发现声子线变宽和变软之间存在近似二次相关性。

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